Co-reporter:Lingang Yang, Hongli Guo, Lingzhi Wang, Jinlong Zhang
Microporous and Mesoporous Materials 2017 Volume 239() pp:173-179
Publication Date(Web):February 2017
DOI:10.1016/j.micromeso.2016.10.010
•A facile “template extracting” strategy to fabricate HPMO was presented.•PS particle is served as the sacrificial template and removed by extraction by selected solvent to obtain hollow particle.•Systematic characterizations clearly revealed that the HPMO particles have excellent monodispersity.•Multifunctional particles realize the application in magnetic separable environmental renovation and drug delivery system.A facile “template dissolving” strategy has been developed for the fabrication of hollow periodic mesoporous organosilica (HPMO) particles with perpendicularly ordered mesopores, where polystyrene (PS) is used as sacrifice template for the generation of hollow cavity. Systematic characterizations including transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray powder diffraction (XRD) and N2 adsorption/desorption analysis clearly reveal that the HPMO particles have an excellent monodispersity with a high specific surface area of 1246.7 m2 g−1, large pore volume of 1.38 cm3 g−1 and uniformly ordered mesopores of 2.48 nm. The pre-encapsulation of a core into PS (SiO2, Fe3O4@SiO2) results in a yolk-shell (Y-S) particle with high tunable shell thickness (30–60 nm) and cavity size (230–450 nm). The magnetically recyclable Fe3O4-YS-PMO was further utilized to adsorb 2, 4-dichlorophenol (2, 4-DCP) and the controlled release of camptothecin (CPT). Up to 81 mg of CPT was loaded per gram of the Fe3O4-YS-PMO particles, followed with a continuously release of 76% within 5 days.
Co-reporter:Waheed Iqbal, Lingzhi Wang, Xianjun Tan, Jinlong Zhang
Journal of Environmental Chemical Engineering 2017 Volume 5, Issue 4(Issue 4) pp:
Publication Date(Web):1 August 2017
DOI:10.1016/j.jece.2017.07.011
•Porous g-C3N4 is prepared by using starch as green template in situ gaseous template.•Porous g-C3N4 favours the separation of radiative charge carriers.•Samples enhanced visible light photocatalytic activity.•Optimized gaseous template contents have a significant influence on photooxidative chemical reaction.We report a facile and sustainable route to prepare the porous g-C3N4 by using starch as green in situ gaseous template and melamine as a precursor. The as-prepared g-C3N4 exhibited a porous thin sheet like structure with a larger surface area and showed an efficient separation efficiency for radiative charge carriers. The textural structure and morphology of the porous g-C3N4 materials were well characterized by TEM, SEM, XRD, BET, FT-IR, Raman, XPS, UV–vis DRS and PL spectroscopy. The starch mediated porous g-C3N4 photocatalyst demonstrated significantly an enhanced visible light photocatalytic performance and excellent physicochemical stability for the photodegradation of organic pollutants (including rhodamine B and phenol). The results revealed that, the optimized gaseous template contents had a significant influence on photooxidative chemical reaction of the as-prepared samples. The radical scavenging experiments proved that holes and O2− are the main reactive species responsible for the visible light degradation of rhodamine B. This simple, economical and green strategy using starch as gaseous porogen agent for the fabrication of porous g-C3N4 with excellent visible-light photocatalytic activity is desirable for environmental remediation and solar energy applications.Download high-res image (139KB)Download full-size image
Co-reporter:Dan Du, Wen Shi, Lingzhi Wang, Jinlong Zhang
Applied Catalysis B: Environmental 2017 Volume 200(Volume 200) pp:
Publication Date(Web):1 January 2017
DOI:10.1016/j.apcatb.2016.07.043
•The Fe3O4@void@TiO2 NPs show a remarkable performance for degrading TC.•The synergic effect between TiO2 shell and Fe3O4 core plays an important role.•The photo-Fenton-like catalyst can work under a wide pH range of 3–9.Herein, we demonstrate the yolk-shell structured Fe3O4@void@TiO2 sphere as an efficient heterogeneous catalyst for the photo-Fenton-like degradation of tetracycline (TC). The composite was synthesized by first successively coating amorphous SiO2 and TiO2 shells around a Fe3O4 core via the sol-gel strategy to form Fe3O4@SiO2@TiO2, then crystallizing TiO2 and removing SiO2 through calcination and the ultrasonic ammonia-etching treatment, respectively. The particles are monodisperse and uniform in size (ca. 180 nm), where the diameter of the core is ca. 100 nm and the thickness of the shell is ca. 10 nm. This composite possesses anatase TiO2 shell with high crystallinity, superparamagnetic core with a saturation magnetization value of 28.71 emu/g and high specific surface area of 101 m2 g−1. It shows extremely high activity towards the degradation of TC (40 mg/L) in a wide pH range as demonstrated by almost 100% elimination efficiency at pH = 3 and ca. 75% at pH = 9 within 6 min. Moreover, benefitting from the superparamagnetism of the core, this composite could be magnetically recovered and reapplied in the TC degradation without significant loss of activity after 5 recycling (ca. 10%). The degradation curve can be well fitted by pseudo-first order model, where a kinetic constant of 0.51 min−1 is achieved, much higher than those of Fe3O4@TiO2 (0.24 min−1), hollow TiO2 (0.17 min−1), Fe3O4@SiO2@TiO2 (0.14 min−1) and Fe3O4 (0.11 min−1). The high activity is attributed to the efficient enrichment and confinement of reactants (TC and hydroxyl radicals) in the nanocavity of the yolk-shell structure, and the efficient reduction of Fe3+ to Fe2+ by the photo-generated electrons from the TiO2 shell.Yolk-shell structured Fe3O4@void@TiO2asaphoto-Fenton-likecatalystshowsanexcellentperformanceforthedegradationofTC.Download high-res image (223KB)Download full-size image
Co-reporter:Yuanxin Deng, Mingyang Xing, Jinlong Zhang
Applied Catalysis B: Environmental 2017 Volume 211(Volume 211) pp:
Publication Date(Web):15 August 2017
DOI:10.1016/j.apcatb.2017.04.037
•An advanced TiO2/Fe2TiO5/Fe2O3 triple-heterojunction was successfully prepared.•Abundant phase interfaces enhance efficiencies of charges migration and separation.•High efficiency of Fe3+/Fe2+ cycle reaction on the catalyst surface.•Wide pH range of application.•Stable catalyst structure and PFR performance.The construction of catalysts with high efficiency and stability for heterogeneous Photo-Fenton reaction Heterogeneous (PFR) has been a major challenge for the degradation of organic pollutants. Here, we successfully develop an advanced TiO2/Fe2TiO5/Fe2O3 triple-heterojunction structure by using the mesoporous TiO2 spheres as the substrate via a simple ion-exchange method. The XRD and HRTEM results demonstrate the generation of Fe2TiO5 on the interface between TiO2 and Fe2O3, which can be used as a “bridge” to transfer the photo-excited electrons from TiO2 to Fe2O3. The as-prepared triple-heterojunction has abundant interphase boundaries which greatly improve the migration of photo-excited charges among different components. As a result, the prepared triple-heterojunction has a significantly enhanced PFR activity for the visible-light-driven degradation of methyl orange (MO) and colorless organic pollutant of phenol, compared with the single catalysts of Fe2O3 and TiO2, and the binary-heterojunction of TiO2/Fe2O3. Compared to the traditional Fe2O3 based PFR, the degradation rates of MO and phenol over triple-heterojunction can be increased from 4% to 87% within 10 min irradiation and from 38% to 100% within 60 min irradiation, respectively. And the total organic carbon (TOC) degradation rate of phenol can be up to 85%. Moreover, this advanced triple-heterojunction has a wide pH value range of application in PFR. Either at a pH of 4.0 or 7.0, it shows a much higher and more stable PFR activity for the degradation of MO than the catalysts of Fe2O3 and TiO2/Fe2O3. And the reaction rate of TiO2/Fe2TiO5/Fe2O3 almost keeps changeless even after 10th cycles, suggesting its vast application foreground in the environmental pollutant treatment.Download high-res image (207KB)Download full-size image
Co-reporter:Yuhang Wang;Sukhbaatar Lkhamjav;Bocheng Qiu
Research on Chemical Intermediates 2017 Volume 43( Issue 4) pp:2055-2066
Publication Date(Web):2017 April
DOI:10.1007/s11164-016-2746-x
Modification of brookite titanium dioxide (TiO2) for the treatment of typical pollutants is a great challenge, owing to its poor chemical stability and the difficulty involved in obtaining it. In this paper, we report a facile method to prepare Fe3+ modified brookite TiO2. The Fe3+ modified brookite TiO2 catalysts exhibit enhanced absorption in visible light region and efficient separation of photo-generated electrons and holes. Meanwhile, we investigate the effect of the modified contents of Fe3+ on the photocatalytic activity, and the optimum Fe3+ content is obtained at 2 wt% that shows the highest photocatalytic activity for the degradation of Rhodamine B both under UV and visible light irradiation. The traps induced by the Fe3+ doping have been well studied here, which are expected to contribute to the narrowing of the band gap of brookite and the separation of electrons and holes.
Co-reporter:Jingyan Si;Ya Liu;Shunzhou Chang;Di Wu
Research on Chemical Intermediates 2017 Volume 43( Issue 4) pp:2067-2080
Publication Date(Web):2017 April
DOI:10.1007/s11164-016-2747-9
AgBr@TiO2/GO (graphene oxide) ternary composite photocatalyst was synthesized by fabricating core–shell-structured AgBr@TiO2 and anchoring it onto the surface of GO. The obtained samples were characterized by transmission electron microscopy, X-ray diffraction analysis, X-ray photoelectron spectroscopy, ultraviolet–visible (UV–Vis) diffuse reflectance spectrum, and photoluminescence (PL) spectroscopy. It was found that the AgBr nanoparticles were prone to aggregation while the core–shell-structured AgBr@TiO2 possessed excellent dispersity. PL analysis revealed that the ternary-structured AgBr@TiO2/GO could effectively promote the separation rate of electron–hole pairs. Photocatalytic oxidation of benzyl alcohol to benzaldehyde under visible-light irradiation was selected as probe reaction to evaluate the photocatalytic activity of the different samples. It was found that the AgBr@TiO2/GO ternary composite exhibited evidently improved photocatalytic activity compared with AgBr, AgBr@TiO2, and AgBr/GO. On the basis of the experiment results, the photocatalytic oxidation mechanism of benzyl alcohol over AgBr@TiO2/GO is tentatively discussed.
Co-reporter:Wei Ming;Jingjing Feng;Shunzhou Chang
Research on Chemical Intermediates 2017 Volume 43( Issue 12) pp:7387-7398
Publication Date(Web):25 July 2017
DOI:10.1007/s11164-017-3082-5
Small-molecule thiols such as cysteine (Cys) and glutathione (GSH) are essential for maintaining the cellular redox environment and play important roles in regulating various cellular functions. Therefore, it is significant to quantitatively detect the small-molecule thiols in clinical chemistry and biochemistry. Here, we synthesized a new probe RT by using a rhodol-based fluorescent dye with long emission wavelength (λem = 635 nm) as the fluorophore and the DNBS group as the response unit. It was found that the probe RT showed high response speed and selectivity toward Cys and GSH over other amino acids. After reacting with Cys/GSH, it shows a strong red fluorescence, corresponding to a color change from colorless to purple, which can be easily discriminated by the naked eye. The detection limit of the probe RT is as low as 24 nM to Cys and 20 nM to GSH. All these advantages of the probe RT make it possible for the quantitative detection of small-molecule thiols such as Cys and GSH in living organisms.
Co-reporter:Mingyang Xing;Bocheng Qiu;Mengmeng Du;Qiaohong Zhu;Lingzhi Wang;Jinlong Zhang
Advanced Functional Materials 2017 Volume 27(Issue 35) pp:
Publication Date(Web):2017/09/01
DOI:10.1002/adfm.201702624
To the photocatalytic H2 evolution, the exposure of a reduction surface over a catalyst plays an important role for the reduction of hydrogen protons. Here, this study demonstrates the design of a noble-metal-free spatially separated photocatalytic system exposed with reduction surfaces (MnOx@CdS/CoP) for highly solar-light-driven H2 evolution activity. CoP and MnOx nanoparticles are employed as the electron and hole collectors, which are selectively anchored on the outer and inner surface of CdS shells, respectively. Under solar light irradiation, the photogenerated holes and electrons can directionally move to the MnOx and CoP, respectively, leading to the exposure of a reduction surface. As a result, the H2 evolution increases from 32.0 to 238.4 µmol h−1, which is even higher than the activity of platinum-loaded photocatalyst (MnOx@CdS/Pt). Compared to the pure CdS with serious photocorrosion, the MnOx@CdS/CoP maintains a changeless activity for the H2 evolution and rhodamine B degradation, even after four cycles. The research provides a new strategy for the preparation of spatially separated photocatalysts with a selective reduction surface.
Co-reporter:Dr. Bocheng Qiu;Dr. Qiaohong Zhu;Mengmeng Du;Linggang Fan; Dr. Mingyang Xing; Dr. Jinlong Zhang
Angewandte Chemie 2017 Volume 129(Issue 10) pp:2728-2732
Publication Date(Web):2017/03/01
DOI:10.1002/ange.201612551
AbstractHollow structures with an efficient light harvesting and tunable interior component offer great advantages for constructing a Z-scheme system. Controlled design of hollow cobalt sulfide (Co9S8) cubes embedded with cadmium sulfide quantum dots (QDs) is described, using hollow Co(OH)2 as the template and a one-pot hydrothermal strategy. The hollow CdS/Co9S8 cubes utilize multiple reflections of light in the cubic structure to achieve enhanced photocatalytic activity. Importantly, the photoexcited charge carriers can be effectively separated by the construction of a redox-mediator-free Z-scheme system. The hydrogen evolution rate over hollow CdS/Co9S8 is 134 and 9.1 times higher than that of pure hollow Co9S8 and CdS QDs under simulated solar light irradiation, respectively. Moreover, this is the first report describing construction of a hollow Co9S8 based Z-scheme system for photocatalytic water splitting, which gives full play to the advantages of light-harvesting and charges separation.
Co-reporter:
Chinese Journal of Chemistry 2017 Volume 35(Issue 2) pp:153-158
Publication Date(Web):2017/02/01
DOI:10.1002/cjoc.201600924
AbstractBi2WO6 was modified with MnOx via a photodeposition method. Multiple techniques including XRD, SEM, TEM, UV–vis and XPS were applied to investigate the structures, morphologies and optical characteristics of the as-prepared sample. The nanostructured composites were formed with MnOx loaded on the surface of flower-like Bi2WO6, where MnOx exists as a mixed-valence manganese of Mn3+ and Mn4+ as verified by XPS. The photocatalytic activity of the MnOx/Bi2WO6 composites was evaluated by using rhodamine B (RhB) as a target organic pollutant under visible light irradiation. The as-prepared MnOx/Bi2WO6 composites exhibited much higher photocatalytic activities than pure Bi2WO6. The enhanced activities were attributed to the interfacial transfer of photogenerated holes from Bi2WO6 to MnOx, leading to effective way to improve photocatalytic efficiency, which may be extended to a strategy for other semiconductor. Based on the experimental results, a possible mechanism of MnOx for the enhancement of visible light performance was proposed.
Co-reporter:Yulan Peng;Lingzhi Wang;Yongdi Liu;Haijun Chen;Juying Lei;Jinlong Zhang
European Journal of Inorganic Chemistry 2017 Volume 2017(Issue 40) pp:4797-4802
Publication Date(Web):2017/11/02
DOI:10.1002/ejic.201700930
A composite catalyst combining CoP with g-C3N4 was explored for the photocatalytic production of H2O2 under visible-light irradiation. The composite catalyst was fabricated by growth of CoP nanoparticles on the surface of g-C3N4. The CoP nanoparticles were well dispersed on the surface of g-C3N4 and could interact with g-C3N4 to improve charge separation and electron transfer. The composite catalyst showed superior catalytic activity compared with pure CoP or g-C3N4 under visible-light irradiation. The optimal catalyst with 1.76 wt.-% CoP loading exhibited the best photocatalytic efficiency with an H2O2 production of 140 µm in 2 h, which is about 4.6 and 23.3 times those of pure g-C3N4 and pure CoP, respectively. A possible mechanism for the visible-light-driven photocatalytic production of H2O2 is proposed. The composite catalyst exhibited stable performance without obvious loss of catalytic activity after seven successive runs, and thus has good application prospects in sustainable H2O2 production.
Co-reporter:Bocheng Qiu;Qiaohong Zhu;Mingyang Xing;Jinlong Zhang
Chemical Communications 2017 vol. 53(Issue 5) pp:897-900
Publication Date(Web):2017/01/10
DOI:10.1039/C6CC08311K
CdxZn1−xSe/CoP composites have been well studied as effervescent photocatalysts for H2 evolution. These composites are highly efficient at 45.1 mmol h−1 g−1 and have a high quantum yield of 11.8% at ∼520 nm. The tunable energy band of CdxZn1−xSe facilitates photo-electrons transferring to CoP via chemical bonds between components. Advances in CdxZn1−xSe/CoP for photocatalytic H2 evolution provide a new strategy for future splitting of seawater.
Co-reporter:Weijia Lv;Zhihang Liu;Jinjing Lan;Ziyu Liu;Wenxin Mi;Juying Lei;Lingzhi Wang;Yongdi Liu;Jinlong Zhang
Catalysis Science & Technology (2011-Present) 2017 vol. 7(Issue 23) pp:5687-5693
Publication Date(Web):2017/11/27
DOI:10.1039/C7CY01748K
Spurred by the threat of hexavalent chromium (Cr(VI)), the idea of reducing Cr(VI) into less toxic Cr(III) has been commonly studied. Here, we used a facile photodeposition method to modify inverse opal TiO2 (i.o.TiO2) with cobalt phosphate (Co-Pi), and the resulting composite was applied for photocatalytic reduction of Cr(VI). This is the first time that an inverse opal structure as well as a Co-Pi catalyst is applied in the photocatalytic reduction of Cr(VI). In addition, the combination of i.o.TiO2 and Co-Pi achieves high visible-light-driven photocatalytic activity, which is better than that of the pure Co-Pi catalyst and unmodified i.o.TiO2. Experimental results demonstrated that the Co-Pi in the composite could absorb a large amount of visible light and then inject electrons into the conduction band of i.o.TiO2 which subsequently participate in the reduction reaction of Cr(VI). Moreover, the inverse opal structure of the catalyst possesses the advantages of having a large surface area and efficient light harvesting ability, leading to the better catalytic activity of Co-Pi/i.o.TiO2 than Co-Pi/bulk TiO2 and Co-Pi/P25. It's also proved that this Co-Pi/i.o.TiO2 photocatalyst can efficiently remove organic pollutants together with Cr(VI). This study provides new insights into the design and fabrication of efficient photocatalysts for the removal of environmental pollutants under visible light.
Co-reporter:Waheed Iqbal;Bocheng Qiu;Juying Lei;Lingzhi Wang;Jinlong Zhang;Masakazu Anpo
Dalton Transactions 2017 vol. 46(Issue 32) pp:10678-10684
Publication Date(Web):2017/08/14
DOI:10.1039/C7DT00849J
The development of highly active, cost-effective, environmentally friendly and stable g-C3N4 based photocatalysts for H2 evolution is one of the most anticipated potential pathways for future hydrogen utilization. Herein, a facile gaseous bubble template approach was designed to prepare large-scale thin g-C3N4 nanosheets (g-C3N4 NSs) using melamine and ammonium sulphate as the bubble template. Through distinctive structural improvements for a large bandgap, excellent electron mobility, prolonged lifetime of the photogenerated charge carriers and a high specific surface area with highly accessible potential reaction sites, the as-synthesized g-C3N4 NSs demonstrated a high photocatalytic hydrogen evolution rate of 9871 μmol h−1 g−1 and efficient photocatalytic degradation of Rhodamine B (RhB) and phenol under simulated solar light irradiation.
Co-reporter:Yuhang Wang;Yuanxin Deng;Linggang Fan;Yu Zhao;Bin Shen;Di Wu;Yi Zhou;Chencheng Dong;Mingyang Xing;Jinlong Zhang
RSC Advances (2011-Present) 2017 vol. 7(Issue 39) pp:24064-24069
Publication Date(Web):2017/05/03
DOI:10.1039/C7RA02608K
As a novel material for water depollution, conjugated polydiphenylbutadiyne (PDPB) nanofibers have received attention due to their visible light responsive photocatalytic activity. In this study, we successfully prepared a PDPB/SnO2 p–n heterojunction by an in situ growth route. The XPS characterization indicates the generation of Sn–C bonds between SnO2 and PDPB, which would decrease the bandgap of SnO2 and promote the transference efficiency of electrons and holes between these two components. The PDPB could act as the sensitizer to enlarge the solar light absorption region of the heterojunction. The SnO2 provides a stable mesoporous structure and enhanced hydrophilic properties. The solar-driven photodegradation rate of Rhodamine B over the PDPB/SnO2 (ratio is 2 : 1) is 4 times higher than that of the pure SnO2 and 2 times higher than that of the pure PDPB nanofibers. Our strategy gives a facile strategy for the preparation of an organic–inorganic hybrid heterojunction with high solar light activity.
Co-reporter:Juying Lei;Fenghui Liu;Lingzhi Wang;Yongdi Liu;Jinlong Zhang
RSC Advances (2011-Present) 2017 vol. 7(Issue 44) pp:27377-27383
Publication Date(Web):2017/05/22
DOI:10.1039/C7RA03534A
New polymer composites consisting of poly(diphenylbutadiyne) (PDPB) and g-C3N4 have been successfully prepared. UV-vis diffuse reflectance spectra show that the existence of PDPB in composites can clearly increase the visible light absorption of the catalysts. Photoluminescence spectroscopy and photoelectrochemical measurements reveal that PDPB can effectively facilitate the charge carrier separation in the composites. Compared with pure g-C3N4 or pure PDPB, the composite catalysts exhibit observably enhanced visible-light photocatalytic activity for degradation of RhB and phenol. A possible mechanism for the charge separation and transfer in the composite catalysts is proposed. In addition, the composite catalysts show stable catalytic performance after five successive runs, displaying potential for applications in various fields of photocatalysis.
Co-reporter:Lingzhi Wang;Yin Xu;Xianjun Tan;Sen Tapas;Jinlong Zhang
RSC Advances (2011-Present) 2017 vol. 7(Issue 58) pp:36201-36207
Publication Date(Web):2017/07/20
DOI:10.1039/C7RA05547A
A sensitive and selective SERS sensor with easy and excellent recyclability is highly demanded because of its great potential application in complex detection environments. Here, using methylene blue (MB) as a model target, a semiconductor-based SERS substrate composed of a MoO3 nanorod core and a uniform molecule-imprinting polymethacrylic acid shell (MIP) with a thickness of 4 nm was designed and fabricated (MoO3@MIP) to achieve selective detection. The key to the successful coating of the ultrathin uniform MIP shell lies in the pretreatment of a MoO3 core with nitric acid, providing sufficient surficial hydroxyls for the anchoring of a polymer precursor. The molecule-imprinted voids for MB were formed simply via light irradiation as a result of photocatalytic degradation by a MoO3 semiconductor. This core–shell MIP composite shows a high SERS selectivity towards low-level MB in a mixed MB/CV solution. The enhanced factor (EF) is high, at 1.6 × 104. More importantly, the selective detection allows the further photocatalytic recycling of MoO3@MIP in an “aim-and-shoot” way, which well preserves the detection selectivity and sensitivity towards MB at least for 4 cycles. Based on decreased sensitivity with the increasing shell thickness (10–24 nm), a MIP-gating charge transfer mechanism is proposed to demonstrate the high EF instead of the molecule-enrichment effect. This “aim-and-shoot” strategy is expected to push forward the prosperous application of selective SERS for trace detection in versatile environments.
Co-reporter:Yulan Peng;Xiaojun Shen;Lingzhi Wang;Baozhu Tian;Yongdi Liu;Haijun Chen;Juying Lei;Jinlong Zhang
RSC Advances (2011-Present) 2017 vol. 7(Issue 72) pp:45742-45745
Publication Date(Web):2017/09/22
DOI:10.1039/C7RA08381E
A simple method has been developed to prepare porous TiO2 photocatalysts with different crystal phases and large surface area by calcining titanate nanofibers under different temperatures. All the products exhibited excellent photocatalytic activity for RhB degradation under ultraviolet light irradiation.
Co-reporter:Yi Zhou;Wenzhang Fang;Yuanxin Deng;Lihan Pan;Bin Shen;Hexing Li;Yun Hu;Haijun Chen;Mingyang Xing;Jinlong Zhang
RSC Advances (2011-Present) 2017 vol. 7(Issue 88) pp:55927-55934
Publication Date(Web):2017/12/07
DOI:10.1039/C7RA09903G
Managing air and water pollution is among the greatest challenges and a major issue for human civilizations in the 21st century. Semiconductors such as TiO2 are regarded as one of the most promising catalysts that can be used to realize the simultaneous and efficient treatment of multi-component wastewater and NO selective oxidation. However, the granular TiO2 always contains too many phase interfaces, which are harmful to the transfer of photo-excited electrons. Reduced TiO2 mesoporous single crystals (TiO2−x MSCs) with capacity of photoreduction and photooxidation were successfully synthesized by a facile hydrothermal treatment. The formation of Ti3+ impurity levels contribute to a narrowed band gap and enhanced visible light adsorption of TiO2−x. In addition, the mesoporous single crystal structure would provide a long-range order channel for the transfer of photo-generated electrons, which leads to the efficient photoreduction and photooxidation capacity of TiO2−x MSCs. The results revealed that Ti3+-MSCs exhibit outstanding photocatalytic decontamination performance in simultaneous photo-degradation of phenol and removal of Cr(VI) owing to high photo-generated charge separation rate and the synergistic effect of phenol and Cr(VI). In addition, in the absence of any noble metal, the as-prepared reduced Ti3+-MSCs still show high selectivity of NO2 in the NOx photo-oxidation process, owing to the extended wide-spectrum absorption of Ti3+-MSCs and the high-active holes on Ti3+-MSCs under solar light irradiation.
Co-reporter:Shenyuan Bao;Qiangfang Wu;Shunzhou Chang;Baozhu Tian;Jinlong Zhang
Catalysis Science & Technology (2011-Present) 2017 vol. 7(Issue 1) pp:124-132
Publication Date(Web):2017/01/04
DOI:10.1039/C6CY01980C
A Z-scheme heterogeneous photocatalyst CdS–Au–BiVO4 was synthesized for the first time by photo-reduction and deposition–precipitation methods. The microstructures and optical properties of the as-prepared samples were investigated by means of scanning electron microscopy (SEM), field emission scanning electron microscopy (FE-SEM), high resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and UV-vis diffuse reflectance spectroscopy (DRS). Due to the oriented accumulation of electrons on the {010} facets of BiVO4 crystals, Au nanoparticles were successfully anchored on the {010} facets of BiVO4 crystals via the photo-reduction process. CdS was further selectively deposited on the surface of Au nanoparticles, benefitting from the strong S–Au interaction. Photocatalytic degradations of tetracycline and Rhodamine B indicated that CdS–Au–BiVO4 exhibits much higher photocatalytic activity than BiVO4, Au–BiVO4, and CdS–BiVO4. Radical trapping experiments confirmed that in the case of CdS–Au–BiVO4, the main reactive species responsible for organic contaminant degradation are h+, ˙OH, and ˙O2−, while only h+ can be produced in the case of CdS–BiVO4. Based on the photoelectrochemical analysis and radical trapping experiments, it can be deduced that the Z-scheme structure of CdS–Au–BiVO4 not only decreases the recombination rate of photo-generated carriers but also makes the holes and electrons keep a higher redox ability.
Co-reporter:Fenghui Liu, Jie Yu, Guangyuan Tu, Ling Qu, Jiacheng Xiao, Yongdi Liu, Lingzhi Wang, Juying Lei, Jinlong Zhang
Applied Catalysis B: Environmental 2017 Volume 201(Volume 201) pp:
Publication Date(Web):1 February 2017
DOI:10.1016/j.apcatb.2016.08.001
•g-C3N4 was loaded into the Ti-incorporated mesoporous silica materials.•Ti moiety in Ti-SBA15-CN improves the charge separation of g-C3N4 under visible light.•Ti-SBA15-CN showed better photocatalytic activity than Ti-SBA15 and SBA15-CN.•Photocatalytic activity of Ti-SBA15-CN exhibited a rise with increasing of Ti content.•Synergism of photocatalytic Cr (VI) reduction and phenol degradation was observed.In this study, carbon nitride was loaded into the titanium incorporated SBA-15 mesoporous silica (denoted as Ti-SBA15-CN) by a two-step vapor condensation of dicyandiamide. The as-prepared sample was characterized by various spectroscopy techniques. Photocatalytic reduction of Cr (VI) in aqueous solution was investigated using Ti-SBA15-CN under visible-light irradiation. By introducing Ti into the SBA-15 framework structure, the visible light driven photocatalytic activity of the obtained Ti-SBA15-CN was higher than SBA15-CN and the photocatalytic activity exhibited a rise with the increase of Ti contents. It was because the presence of Ti moiety could promote the separation of the photo-generated charge carriers in carbon nitride, leading to the enhancement of the photocatalytic activity. The addition of phenol further enhanced the photocatalytic reduction of Cr (VI). Similarly, the presence of Cr (VI) promoted the degradation of phenol. The synergistic effect between the reduction of Cr (VI) and the degradation of phenol provided salutary method for purification of the complex waste water and environmental restoration.Download high-res image (156KB)Download full-size image
Co-reporter:Yulan Peng;Fenghui Liu;Lingzhi Wang;Yongdi Liu;Juying Lei;Jinlong Zhang
RSC Advances (2011-Present) 2017 vol. 7(Issue 83) pp:52626-52631
Publication Date(Web):2017/11/10
DOI:10.1039/C7RA08969D
In this work, graphene carbon nitride (g-C3N4, CN) is loaded into the carbon dots (CD) modified SBA-15 mesoporous silica by a precursor impregnation method. The obtained samples are characterized by various spectroscopy techniques and applied in the visible-light-driven photocatalytic degradation of phenol. The photocatalytic activity of the obtained SBA15–CN is 2 times as high as that of pure g-C3N4 due to the high dispersion of g-C3N4 into SBA-15 channels. For CD-SBA15–CN, the visible light driven photocatalytic activity is further increased, which is 4 times as high as that of pure g-C3N4. This promotion can be attributed to carbon dots with the ability to transfer photogenerated electrons as well as the compound catalyst having a bigger surface area and pore volume. When the weight ratio of CD-SBA15/g-C3N4 was 1 : 6, the catalyst (1 : 6 CD-SBA15–CN) performed best. The 1 : 6 CD-SBA15–CN photocatalyst had enhanced visible absorption and the interaction between CDs and g-C3N4 can further promote the separation of photo-generated electrons and holes, achieving the highest photocatalytic activity of CD-SBA15–CN compared to SBA15–CN and g-C3N4.
Co-reporter:Waheed Iqbal;Chunyang Dong;Mingyang Xing;Xianjun Tan;Jinlong Zhang
Catalysis Science & Technology (2011-Present) 2017 vol. 7(Issue 8) pp:1726-1734
Publication Date(Web):2017/04/21
DOI:10.1039/C7CY00286F
We report a facile and eco-friendly one-pot synthesis of well-adorned mesoporous g-C3N4 material through a bubble templating strategy and involving controlling the surface area from 17 to 195 m2 g−1 by simply adjusting the mass ratio of melamine/NH4Cl. Various characterization techniques were adopted to examine the structures and physicochemical properties of the as-prepared mpg-C3N4 samples. The results are a step forward to the bottleneck problems of producing mesoporous g-C3N4 materials with both a high BET surface area with well-adorned pore diameters and considerable pore volume by simply employing ammonium chloride as a gaseous bubble template and melamine as a g-C3N4 precursor. The obtained ammonium chloride-mediated mesoporous g-C3N4 photocatalyst demonstrated excellent photocatalytic performance compared with bulk g-C3N4 for the visible light photodegradation of RhB and phenol. The extraordinary photocatalytic activity and outstanding stability of the as-prepared mesoporous g-C3N4 were predominantly attributed to the exceptionally high surface area with ordered pore diameters, improved optical absorbance, and efficient charge separation. Our work not only exhibits the simplest, eco-friendly, and economical approach to fabricate highly efficient well-adorned mesoporous g-C3N4 photocatalysts, but also paves new opportunities for the rational design and synthesis of advanced photocatalysts with great potential in environmental remediation.
Co-reporter:Wen Shi, Dan Du, Bin Shen, Chuanfeng Cui, Liujia Lu, Lingzhi Wang, and Jinlong Zhang
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 32) pp:20831
Publication Date(Web):July 28, 2016
DOI:10.1021/acsami.6b07644
Yolk–shell (Y–S) structured Fe3O4@void@CdS nanoparticles (NPs) are synthesized through a one-pot coating-etching process with Fe3O4@SiO2 as the core, where the coating of an outer CdS shell from a chemical bath deposition (CBD) process is simultaneously accompanied by the gradual etching of an inner SiO2 shell. The as-prepared Fe3O4@void@CdS NPs (ca. 200 nm) possess good monodispersity and a uniform CdS shell of ca.15 nm. This composite exhibits excellent photo-Fenton (ph-F) activity toward the degradation of methylene blue (MB) in a wide pH working range of 4.5–11 under the visible light irradiation. A series of control experiments demonstrate the unique Y–S structure contributes to the enhanced activity, where the separation of hole–electron pair from CdS and the reduction of Fe2+ from Fe3+ are mutually promoted. The similar efficiency can also be achieved when the shell component changes to TiO2 or CeO2, demonstrating a general strategy for the design of robust ph-F agent.Keywords: Fe3O4@void@CdS; photo-Fenton; semiconductors; wide pH range; yolk−shell
Co-reporter:Lingang Yang, Chuanfeng Cui, Lingzhi Wang, Juying Lei, and Jinlong Zhang
ACS Applied Materials & Interfaces 2016 Volume 8(Issue 29) pp:19084-19091
Publication Date(Web):July 5, 2016
DOI:10.1021/acsami.6b05872
The rational design and controlled synthesis of a smart device with flexibly tailored response ability is all along desirable for bioapplication but long remains a considerable challenge. Here, a pH-stimulated valve system with a visualized “on–off” mode is constructed through a dual-shell fluorescence resonance energy transfer (FRET) strategy. The dual shells refer to carbon dots and fluorescent molecules embedded polymethacrylic acid (F-PMAA) layers successively coating around a SiO2 core (ca. 120 nm), which play the roles as energy donor and acceptor, respectively. The total thickness of the dual-shell in the solid composite is ca. 10 nm. The priorities of this dual-shell FRET nanovalve stem from three facts: (1) the thin shell allows the formation of efficient FRET system without chemical bonding between energy donor and acceptor; (2) the maximum emission wavelength of CD layer is tunable in the range of 400–600 nm, thus providing a flexible energy donor for a wide variety of energy acceptors; (3) the outer F-PMAA shell with a pH-sensitive swelling–shrinking (on–off) behavior functions as a valve for regulating the FRET process. As such, a sensitive and stable pH ratiometric sensor with a working pH range of 3–6 has been built by simply encapsulating pH-responsive fluorescein isothiocyanate (FITC) into PMAA; a pH-dependent swelling–shrinking shuttle carrier with a finely controllable molecule-release behavior has been further fabricated using rhodamine B isothiocyanate (RBITC) as the energy donor and model guest molecule. Significantly, the controlled releasing process is visually self-monitorable.
Co-reporter:Xianjun Tan, Lingzhi Wang, Chen Cheng, Xuefeng Yan, Bin Shen and Jinlong Zhang
Chemical Communications 2016 vol. 52(Issue 14) pp:2893-2896
Publication Date(Web):16 Dec 2015
DOI:10.1039/C5CC10020H
Plasmonic MoO3−x@MoO3 nanosheets obtained from surface oxidation of MoO3−x were employed as a SERS substrate for methylene blue detection. They exhibit extraordinary sensitivity comparable to noble metals, which is attributed to shell-isolated electromagnetic enhancing by the plasmonic MoO3−x core and elimination of the photocatalytic degradation by the MoO3 shell.
Co-reporter:Qiangfang Wu, Shenyuan Bao, Baozhu Tian, Yifei Xiao and Jinlong Zhang
Chemical Communications 2016 vol. 52(Issue 47) pp:7478-7481
Publication Date(Web):10 May 2016
DOI:10.1039/C6CC02737G
BiVO4 mesoporous single crystals (MSCs) were successfully prepared, for the first time, by a one-step hydrothermal method using the acidified BiVO4 precursor solution pre-impregnated silica as the template. It was revealed that the BiVO4 MSCs were formed by a double-diffusion mechanism. The O2 evolution rate over BiVO4 MSCs was improved nearly 10 times than that over BiVO4 bulk single crystals.
Co-reporter:Yi Zhou, Qiuying Yi, Mingyang Xing, Lu Shang, Tierui Zhang and Jinlong Zhang
Chemical Communications 2016 vol. 52(Issue 8) pp:1689-1692
Publication Date(Web):27 Nov 2015
DOI:10.1039/C5CC07567J
Sandwich structured graphene modified TiO2 mesoporous single crystals (GR-MSCs) were obtained by using the graphene embedded silica spheres as the hard template, via a hydrothermal treatment. The selective photocatalysis of TiO2 can be achieved by controlling the location of graphene in TiO2 mesoporous single crystals. The sandwich structured graphene–TiO2 composite has a photooxidation surface, and the core–shell structured TiO2@graphene has a photoreduction surface. It provides a new pathway to realize the selectivity of photocatalysis by controlling the location of graphene in TiO2 MSCs for the first time.
Co-reporter:Lingang Yang, Lingzhi Wang, Chuanfeng Cui, Juying Lei and Jinlong Zhang
Chemical Communications 2016 vol. 52(Issue 36) pp:6154-6157
Publication Date(Web):01 Apr 2016
DOI:10.1039/C6CC01917J
The Stöber process is revisited using vinyltriethoxysilane as the precursor, where a kinetics-controlled condensation of vinylsilanols, free from external fluorogens, unprecedentedly produces hydrophilic diamond-structured organosilica nanocrystals (ca. 2–6 nm) with finely tunable fluorescence (460–625 nm). The key to the synthesis lies in a slow successful condensation of vinylsilanols triggered and guided by the π–π stacking interaction of vinyl groups.
Co-reporter:Lingzhi Wang;Kaifeng Gan;Deli Lu;Jinlong Zhang
European Journal of Inorganic Chemistry 2016 Volume 2016( Issue 6) pp:890-896
Publication Date(Web):
DOI:10.1002/ejic.201501215
Abstract
A core–shell-structured magnetic Fe3O4@C composite has been prepared from Fe3O4@RF (RF = resorcinol-formaldehyde) through pyrolysis at 600 °C under a N2 atmosphere. The resultant products were characterized by transmission electron microscopy (TEM), powder X-ray powder diffraction (PXRD), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and thermogravimetric analysis (TGA). The Fe3O4@C composite has excellent particle monodispersity, a uniform particle diameter of ca. 200 nm, a magnetic saturation of 41.2 emu g–1, and a high specific surface area of 247.3 m2 g–1 owing to the existence of a bimodal micro-macroporous system. Moreover, the carbon shell is graphitized but has good hydrophilicity, which is attributed to the existence of remnant oxygen-containing groups. When applied as an adsorbent for the removal of 2,4-dichlorophenol from water, Fe3O4@C shows a good dispersivity (0.2 g L–1) and an average maximum adsorption capacity of 131.83 mg g–1 with a fluctuation of less than 17 % over a wide pH range from 1 to 11 and can be quickly recovered within 30 s by the application of an external magnetic field (800 G). The adsorption performance of Fe3O4@C is revealed to be attributed to π–π electron donor–acceptor interactions between the electron-rich conjugated aromatic groups of Fe3O4@C and electron-deficient 2,4-dichlorophenol. The high adsorption capacity and facile magnetic separation performance make our hydrophilic Fe3O4@C an ideal adsorbent for the removal of 2,4-dichlorophenol from wastewater.
Co-reporter:Chencheng Dong, Hui Song, Yi Zhou, Chunyang Dong, Bin Shen, Hua Yang, Masaya Matsuoka, Mingyang Xing and Jinlong Zhang
RSC Advances 2016 vol. 6(Issue 81) pp:77863-77869
Publication Date(Web):16 Aug 2016
DOI:10.1039/C6RA17884G
We employed a facile method to realize sulfur nanoparticles in situ growth on TiO2 mesoporous single crystals (MSCs). The prepared photocatalysts were characterized by XRD, Raman, UV-vis absorption spectra, XPS, TEM, FESEM, TG/DTA and photoluminescence (PL) emission spectra. The average sulfur particle size is around 8 nm, and we utilized various volumes of ammonium polysulfide ((NH4)2Sx) to tailor the loading of sulfur nanoparticles. When the loading content is 27.2 wt%, they exhibit the optimal photoactivity in degrading acid orange 7 (AO7). In comparison with the pure MSCs (P-TiO2 MSCs), the removal rate of 30S-TiO2 MSCs can be enhanced about 90% under solar light irradiation, and after 5 cycles it retains a high photocatalytic performance.
Co-reporter:Muhammad Nasir, Juying Lei, Waheed Iqbal, Jinlong Zhang
Applied Surface Science 2016 Volume 364() pp:446-454
Publication Date(Web):28 February 2016
DOI:10.1016/j.apsusc.2015.12.166
Highlights
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Sc and C co-doped TiO2 nanoparticles were synthesized by sol–gel method.
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Sc and C co-doping TiO2 decreased the crystal size and increased the surface area.
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Sc and C co-doping increase the lifetime of photo-generated electrons and holes.
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The co-doped samples show a remarkable increase in the visible light photoactivity.
Co-reporter:Yunchang Liu, Kaiqiang Xiang, Baozhu Tian, Jinlong Zhang
Tetrahedron Letters 2016 Volume 57(Issue 23) pp:2478-2483
Publication Date(Web):8 June 2016
DOI:10.1016/j.tetlet.2016.04.068
•A fluorescein-based fluorescent probe for detecting thiols is synthesized.•The probe shows good selectivity toward thiols compared with many other amino acids.•The probe can detect thiols even with the disturbance of quantity of other amino acids.•The color changes from colorless to yellow which can be checked by naked eyes.A new turn-on fluorescent probe for the selective detection of thiol over other amino acids was synthesized. Probe possesses the widely-used thiol-selective 2,4-dinitrobenzenesulfonyl (DNBS) group which can react with thiol and release the fluorescein which has strong fluorescence. Fluorescein, a well known xanthene fluorescent dye, has two states at different environment. Fluorescein is in the state of spirocyclization when connected with 2,4-dinitrobenzenesulfonyl (DNBS) group which has no fluorescence. However, it is in the state of open form when it reacts with thiol which has a strong fluorescence. The transition of the two states can be used to selectively detect thiol and the color can change from colorless to yellow which can be differentiated by naked eyes. Upon the titration of thiol, the absorption band at 454 nm rises gradually and the fluorescence emerges at 521 nm and the detection limit can be as low as 0.16 μM. All of such good properties prove it to be a good sensor for the selective detection of thiol and it shows a potential use in bioimaging applications.We designed a asymmetric fluorescein-based probe for the detection of thiol using 2,4-dinitrobenzenesulfonyl (DNBS) group as the detection group. The probe shows nonfluorescence when connected with 2,4-dinitrobenzenesulfonyl which destroys the π-conjugation and its fluorescence appears when the probe reacts with thiol.
Co-reporter:Yunchang Liu, Kaiqiang Xiang, Min Guo, Baozhu Tian, Jinlong Zhang
Tetrahedron Letters 2016 Volume 57(Issue 13) pp:1451-1455
Publication Date(Web):30 March 2016
DOI:10.1016/j.tetlet.2016.02.062
•A coumarin-based fluorescent probe for the detection of Pd0 is designed and synthesized.•The probe shows good selectivity towards Pd0 compared with many other ions.•The probe can detect Pd0 even with the disturbance of quantity of other metal ions.•The detection limit is as low as 0.34 nM which is lower than the specific threshold in drugs.A off–on coumarin-based fluorescent probe for the fast detection of Pd0 is designed and synthesized. The probe shows not only good selectivity but also fast response to Pd0 in phosphate buffered saline (PBS) solution. The absorption band at 412 nm rises sharply as well as the fluorescence at 450 nm after the addition of Pd0 within few minutes. The detection limit is as low as 0.34 nM. The probe shows nonfluorescence when it conjuncted with allyl carbonate ester which destroys the Intramolecular Charge Transfer (ICT) system. The effect of Pd0 to the probe can change the structure and make the departure of the conjuncted allyl carbonate ester. As a result, the fluorogen is exposed and it shows fluorescence.We design a fluorescent probe for the detection of palladium with the high sensitivity and selectivity. The probe shows nonfluorescence when connected with allyl carbonate ester which destroys the ICT system. The effect of palladium to the probe can change the structure. As a result, the fluorophore is exposed and it shows fluorescence.
Co-reporter:Hong Li;Lingzhi Wang;Yongdi Liu;Juying Lei
Research on Chemical Intermediates 2016 Volume 42( Issue 5) pp:3979-3998
Publication Date(Web):2016 May
DOI:10.1007/s11164-015-2294-9
Graphitic carbon nitride (g-C3N4), as a kind of polymeric semiconductor that has unique electronic structure and excellent chemical stability, has attracted increasing attention of researchers. Moreover, the raw materials for the preparation of g-C3N4 are various and easily accessible. All of these have provided favorable advantages for the fast development of g-C3N4. Compared to bulk g-C3N4, mesoporous g-C3N4 has more prominent natures, such as high specific surface area, large pore volume, and the increased amount of surface active sites. Therefore, great efforts have been devoted to develop mesoporous g-C3N4 (MCN). Up to now, many methods have been explored for the synthesis of MCN, such as hard-template method, soft-template method, template-free method, sol–gel method, and so on. Among these methods, the hard template method is used most widely. In this paper, the recent research on the synthesis of MCN was reviewed. In addition, the modifications to the obtained MCN, which lead to performance enhancement of the MCN for better applications, were also summarized.
Co-reporter:Qiuying Yi;Yi Zhou;Mingyang Xing;Jinlong Zhang
Research on Chemical Intermediates 2016 Volume 42( Issue 5) pp:4181-4189
Publication Date(Web):2016 May
DOI:10.1007/s11164-015-2268-y
Ti3+ and carbon co-doped TiO2 photocatalysts were prepared hydrothermally to introduce the carbon, and followed by simple vacuum activation to achieve the Ti3+ self-doping. The prepared co-doped photocatalysts were characterized by XRD, TEM, UV–Vis absorption spectra, EPR, and XPS. It was found that the co-doped TiO2 has dispersed nanoparticles and a narrower band-gap compared with the un-doped TiO2 and single-doped TiO2. The experimental results displayed that the coke carbon generated on the surface of co-doped TiO2 acts as a photosensitizer and has the photosensitization effect under solar light irradiation. Except for the carbon sensitization effect, the Ti3+ self-doping modification has a synergistic effect which is the reason for the effective photo-degradation of methyl orange under simulated solar light irradiation.
Co-reporter:Bocheng Qiu
The Journal of Physical Chemistry C 2016 Volume 120(Issue 22) pp:12125-12131
Publication Date(Web):May 24, 2016
DOI:10.1021/acs.jpcc.6b03800
The rational design and controllable synthesis of TiO2 and noble metal composite photocatalysts represent an unprecedented challenge for developing the solar-driven reduction of nitrobenzene (NB) to aminobenzene (AB), owing to the recombination over the interface between the noble metals and TiO2, which is harmful to the conversion efficiency of NB to AB. Here, we design a unique ternary structure (the high separation of TiO2 and Pt nanoparticles on the surface of reduced graphene oxide (RGO)) through the sol–gel and microwave-assisted strategies. The substrate of RGO can be used as an “electric wire” to effectively transfer the photogenerated electrons from the isolated TiO2 nanocrystals to the isolated Pt nanoparticles, which greatly decreases the interface recombination between TiO2 and Pt and further improves the conversion efficiency of NB to AB under the solar light irradiation. We anticipate our research provides a new way to overcome the interface recombination on the binary photocatalysts in the photocatalytic reaction.
Co-reporter:Chunyang Dong; Mingyang Xing;Jinlong Zhang
The Journal of Physical Chemistry Letters 2016 Volume 7(Issue 15) pp:2962-2966
Publication Date(Web):July 14, 2016
DOI:10.1021/acs.jpclett.6b01287
On the basis of the fact that the competitive adsorption between CO2 and H2O on the catalyst plays an important role in the CO2 photoreduction process, here we develop an economic NH4F-induced hydrophobic modification strategy to enhance the CO2 competitive adsorption on the mesoporous TiO2–SiO2 composite surface via a simple solvothermal method. After the hydrophobic modification, the CO2 photoreduction for the selective generation of CH4 over the noble-metal-free TiO2–SiO2 composite can be greatly enhanced (2.42 vs 0.10 μmol/g in 4h). The enhanced CO2 photoreduction efficiency is assigned to the rational hydrophobic modification on TiO2–SiO2 surface by replacing Si–OH to hydrophobic Si–F bonds, which will improve the CO2 competitive adsorption and trigger the eight-electron CO2 photoreduction on the reaction kinetics.
Co-reporter:Bocheng Qiu, Mingyang Xing and Jinlong Zhang
Journal of Materials Chemistry A 2015 vol. 3(Issue 24) pp:12820-12827
Publication Date(Web):07 May 2015
DOI:10.1039/C5TA02675J
We report three-dimensional (3D) graphene-based hybrids of Fe2O3 nanocrystals grown in situ on graphene aerogels (Fe2O3/GAs) by a Stöber-like method. Compared with other reported Fe2O3/3D-graphene, Fe2O3/GAs have outstanding mechanical strength, high elasticity, ultralow mass, excellent electrical conductivity, good oil absorption capacity and a dispersion of nanoparticles. They have a 3D network structure with a high surface area of 316 m2 g−1 and physicochemical stability. 3D-GAs can inhibit the loss of Fe2+ and stabilize the conversion of Fe3+/Fe2+ in the photo-Fenton reaction. Compared with Fe2O3 and Fe2O3/2D-graphene (Fe2O3/GR), Fe2O3/GAs exhibit an ultrastable, solar-driven Fenton activity over a wide pH range of 3.5–9.0 for the first time. In addition, the highly-dispersed, nanosized Fe2O3 on the surface of the GAs makes the composite highly suitable for use in electrochemical capacitors. Although the Fe2O3/GAs only contain 18.3 wt% Fe2O3, they still yield a high and stable capacitance (151.2 F g−1) at a high discharge current density of 10 A g−1, which is better than that of Fe2O3/GR (93.6 F g−1).
Co-reporter:Lingzhi Wang, Chen Cheng, Sen Tapas, Juying Lei, Masaya Matsuoka, Jinlong Zhang and Fan Zhang
Journal of Materials Chemistry A 2015 vol. 3(Issue 25) pp:13357-13364
Publication Date(Web):14 May 2015
DOI:10.1039/C5TA01652E
Periodic mesoporous organosilica embedded with carbon dots are adopted as the adsorbent for removal of the toxic organic pollutant 2,4-dichlorophenol and inorganic metal ions Hg(II), Cu(II), and Pb(II). The composite possesses an ordered 2D hexagonal mesostructure with a space group of p6mm, high specific surface area (∼468.46 m2 g−1), and uniform pore size (∼5.50 nm). The surface is covered by about 1–2 layers of carbon dot nanoparticles. The maximum adsorption capacity for 2,4-dichlorophenol is 99.70 mg g−1, and the distribution coefficient of metal ions between adsorbent and solution phases is in the range of 2.60–7.41, following the order of Hg(II) > Cu(II) > Pb(II). The Cu(II) and Pb(II) adsorption stays nearly fixed while Hg(II) adsorption is depressed by ∼45% in a mixed solution of metal ions. The Cu(II) and Hg(II) adsorption shows unapparent variation but Pb(II) adsorption is improved by ∼55% in a mixed solution of metal ion and 2,4-dichlorophenol. In contrast, all metal ions lead to the depression of 2,4-dichlorophenol adsorption by 37% (Pb(II)), 45% (Cu(II)), and 48% (Hg(II)). Finally, the n–π electron donor–acceptor interaction between O- and N-containing groups in mesoporous organosilica and the benzene ring in 2,4-dichlorophenol is revealed to be responsible for the enhanced adsorption of 2,4-dichlorophenol, while the electrostatic force and complex formation between metal ions and amide groups co-contribute to the improvement of metal ions adsorption.
Co-reporter:Dianyu Qi, Xuefeng Yan, Lingzhi Wang and Jinlong Zhang
Chemical Communications 2015 vol. 51(Issue 42) pp:8813-8816
Publication Date(Web):10 Apr 2015
DOI:10.1039/C5CC02468D
Here, using the (Au/TiO2)-catalyzed reduction of 4-nitrothiophenol as a probe reaction, a catalysis/SERS bifunctional composite fabricated by uniformly dispersing catalysis-active Au nanoclusters (∼2 nm) on a SERS-active TiO2 photonic microarray was successfully applied to the non-plasmonic SERS self-monitoring of a catalytic reaction for the first time, which is superiorly sensitive and interference-free.
Co-reporter:Juying Lei;Lingang Yang;Deli Lu;Xuefeng Yan;Chen Cheng;Yongdi Liu;Lingzhi Wang;Jinlong Zhang
Advanced Optical Materials 2015 Volume 3( Issue 1) pp:57-63
Publication Date(Web):
DOI:10.1002/adom.201400364
Co-reporter:Hong Li, Liang Zhou, Lingzhi Wang, Yongdi Liu, Juying Lei and Jinlong Zhang
Physical Chemistry Chemical Physics 2015 vol. 17(Issue 26) pp:17406-17412
Publication Date(Web):27 May 2015
DOI:10.1039/C5CP02554K
Well dispersed TiO2 nanocrystals with (001) facets were successfully grown in situ on g-C3N4 through a facial solvothermal method. The resultant TiO2/g-C3N4 composites exhibit remarkably higher efficiency for photocatalytic degradation of phenol as compared to pure catalysts (g-C3N4 or TiO2) or mechanically mixed TiO2/g-C3N4. The optimal composite with 11.2 wt% TiO2 showed the highest degradation rate constant, which is 2.8 times that of pure g-C3N4, 2.2 times that of pure TiO2, and 1.4 times that of mechanically mixed TiO2/g-C3N4. The enhanced photocatalytic activity is mainly attributed to the effective charge separation derived from two aspects: (1) well matched energy levels between TiO2 and g-C3N4 and (2) a uniform and close contact between TiO2 and g-C3N4 that resulted from the in situ growth of highly dispersed TiO2 nanocrystals. The TiO2/g-C3N4 hybrid material prepared in this study is expected to provide a good foundation for the further design and synthesis of advanced TiO2/g-C3N4-based functional materials, and the in situ growth method developed is hopeful to provide a new strategy for the synthesis of other semiconductor-modified g-C3N4 materials.
Co-reporter:Kaiqiang Xiang, Yunchang Liu, Changjiang Li, Baozhu Tian, Tianzhong Tong, Jinlong Zhang
Dyes and Pigments 2015 Volume 123() pp:78-84
Publication Date(Web):December 2015
DOI:10.1016/j.dyepig.2015.06.037
•A ratiometric fluorescence probe for H2S was synthesized using dicyanoisophorone as fluorophore.•The probe showed long emission wavelength (643 nm) and large stokes shift (163 nm).•The probe exhibited high response speed and selectivity toward H2S.•The probe showed high sensitivity toward HS− and the detection limit is as low as 0.13 μM.Developing probes for selective and sensitive detection of hydrogen sulfide (H2S) has received much research attention, because H2S is an environmental toxin as well as an important signaling molecule to regulate physiological and pathological processes. In this work, a new colorimetric and ratiometric fluorescent probe (Probe 1) for H2S detection was synthesized by employing dicyanoisophorone based fluorescence dye as a fluorophore and azide group as the response unit. The synthesized Probe 1 showed a long emission wavelength (λem = 643 nm) and large stokes shift (λem − λabs = 163 nm). Based on the H2S-induced reduction of azide group to amino group, Probe 1 showed high response speed, sensitivity, and selectivity toward HS− under room temperature. Moreover, Probe 1 can ratiometrically respond to HS− and the detection limit is as low as 0.13 μM. It was proved that Probe 1 is suitable for quantitatively detecting HS− ions in river water samples. The numerous advantages of Probe 1 make it be potentially used for quantitative detection of H2S in environment and living organisms.
Co-reporter:Juying Lei, Ying Chen, Fan Shen, Lingzhi Wang, Yongdi Liu, Jinlong Zhang
Journal of Alloys and Compounds 2015 Volume 631() pp:328-334
Publication Date(Web):15 May 2015
DOI:10.1016/j.jallcom.2015.01.080
•g-C3N4/TiO2 was prepared by a one-step preparation under mild conditions.•Photocatalysts showed excellent activity under both UV and visible light.•A neat surface modification process is proved, excluding influence of N doping.•Two photocatalytic mechanisms under different wavelengths are proposed.•A wide range of available wavelengths would greatly improve practicability of TiO2.g-C3N4 modified TiO2 composites were prepared through a simple calcination process of anatase and cyanamide. The as-prepared samples were characterized by X-ray diffraction (XRD), diffuse reflectance spectrophotometry (DRS), fourier transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), thermogravimetry differential thermal analysis (TG–DTA) and X-ray photoelectron spectroscopy (XPS), proving a successful modification of TiO2 with g-C3N4. Photodegradation of acid orange 7 (AO7) was used to evaluate the photocatalytic activities of the composites, showing excellent activity of them under both visible and UV light. In addition, base treatment was then introduced to investigate the interaction between g-C3N4 and TiO2. After removing the g-C3N4 modified on TiO2 by base, no nitrogen doping is found in TiO2 lattice, demonstrating the g-C3N4 was surface attached on TiO2 and attributing all improvement of photocatalytic activity of g-C3N4/TiO2 composite to the synergy between the two semiconductors.
Co-reporter:Kaiqiang Xiang, Yunchang Liu, Changjiang Li, Baozhu Tian and Jinlong Zhang
RSC Advances 2015 vol. 5(Issue 65) pp:52516-52521
Publication Date(Web):09 Jun 2015
DOI:10.1039/C5RA06144J
Developing probes for selective and sensitive detection of palladium in living organisms is of great importance. In this work, we synthesized a colorimetric and ratiometric fluorescent probe (Probe 1) with red light emission (λem = 643 nm) by employing an isophorone based fluorescent dye as the fluorophore and an allylcarbamate group as the response unit. Based on the Pd0-triggered cleavage reaction, Probe 1 showed high response speed, selectivity, and sensitivity towards palladium species. Upon addition of palladium, the absorption and emission spectra of Probe 1 exhibited obvious red-shifts, which can be easily discriminated by the naked eye. In terms of palladium, the detection limit is as low as 24.2 nM and the signal-to-noise ratio in fluorescence intensity can reach 85-fold. As a red emitting ratiometric sensor, Probe 1 can be potentially used for quantitative detection of palladium in living organisms.
Co-reporter:Dianyu Qi, Lingzhi Wang and Jinlong Zhang
RSC Advances 2015 vol. 5(Issue 91) pp:74557-74561
Publication Date(Web):28 Aug 2015
DOI:10.1039/C5RA11938C
In this study, hierarchical TiO2 with macro- and mesostructure is prepared and applied in dye-sensitized solar cell (DSSCs). To achieve the hierarchical structure, hard and soft templating is combined. Polystyrene spheres serve as the hard template for μm-scale macropores, and triblock copolymers act as the soft template of nm-scale mesopores. The prepared hierarchical TiO2 is analyzed by TEM, XRD and N2 sorption, and results indicate that meso/macroporous structure is successfully obtained. Mesoporous structure provides a larger surface area for dye adsorption, and macroporous structure induces a faster electron transportation property. Combining the advantages of mesopores and macropores, the prepared hierarchical TiO2 DSSCs show a higher photon to electron efficiency in comparison to individual mesoporous and macroporous samples.
Co-reporter:Wen Shi, Deli Lu, Lingzhi Wang, Fei Teng and Jinlong Zhang
RSC Advances 2015 vol. 5(Issue 128) pp:106038-106043
Publication Date(Web):08 Dec 2015
DOI:10.1039/C5RA22295H
A chelating-assistant growth route of CdS on the surface of Fe3O4@SiO2 nanoparticles (NPs) was used to form a magnetically recoverable photocatalyst. Characterization by transmission electron microscopy, X-ray powder diffraction, Raman spectroscopy and a vibrating sample magnetometer reveals monodispersed superparamagnetic Fe3O4@SiO2@CdS NPs (ca. 250 nm) have been formed with a uniform CdS shell thickness of ca. 20 nm, Brunauer–Emmett–Teller (BET) surface area of ca. 25.1 m2 g−1 and saturation magnetization of 22.02 emu g−1. This composite shows excellent photocatalytic activity towards the degradation of methylene blue (MB) under visible-light irradiation with a reaction constant of 1.95 × 10−2 min−1 in spite of the low weight percentage of CdS (9.15%) as determined by the energy-dispersive X-ray spectroscopy, which is higher than those observed on Fe3O4@CdS (53.30%, 1.22 × 10−2 min−1) and CdS NPs (3.33 × 10−3 min−1). Furthermore, Fe3O4@SiO2@CdS can be quickly magnetically recovered within 30 s by applying an external magnetic field near the solution after the photocatalytic process, which still preserves the excellent particle monodispersity with the slightly reduced CdS thickness (ca. 15 nm), while Fe3O4@CdS and CdS NPs are severely photo-corroded and aggregated. The maximized specific surface area from uniform coating and the efficient generation of activated oxygen species from CdS shells might be responsible for the enhanced photoactivity.
Co-reporter:Fan Shen, Li Zhou, Jiajia Shi, Mingyang Xing and Jinlong Zhang
RSC Advances 2015 vol. 5(Issue 7) pp:4918-4925
Publication Date(Web):01 Dec 2014
DOI:10.1039/C4RA10227D
SiO2/BiOX (X = Cl, Br, I) thin films, which were well adhered to glass substrates with SiO2 as the intermediate layer, were prepared via a simple sol–gel method. The prepared films were characterized using X-ray diffraction (XRD), scanning electron microscopy (SEM), UV-visible diffuse reflectance spectroscopy (UV-vis DRS), X-ray photoelectron spectroscopy (XPS) and Raman. The results suggest that the films have a tetragonal PbFCl-type structure and crystallized well. These films showed high and stable photocatalytic activities for the degradation of RhB under visible light. This method is cheap and convenient, the size and morphology of the product are uniform, the production cycle is short, and the process is applicable to large-scale applications. SiO2/BiOX (X = Cl, Br, I) films might have promising applications in photocatalysis, photovoltaic film devices, nano-coating, pearlescent pigments and other fields.
Co-reporter:Bocheng Qiu, Chengchao Zhong, Mingyang Xing and Jinlong Zhang
RSC Advances 2015 vol. 5(Issue 23) pp:17802-17808
Publication Date(Web):26 Jan 2015
DOI:10.1039/C4RA17151A
A green and facile approach is employed to prepare an efficient visible-light-driven photocatalyst by using mesocellular foams (MCF) as a matrix, glucose as a carbon-modified source and TiO2 as the catalytic active site, which is denoted as C-modified TiO2/MCF. Characterization results reveal that nano-sized TiO2 nanoparticles are loaded in the pore channels of MCF rather than being aggregated on the surface of the MCF. Furthermore, glucose selectively covers the surface of the TiO2/MCF composites during the stirring process due to the excellent adsorption capacity of MCF, and glucose then can be transformed into coke carbon through a hydrothermal process. In addition, a facile thermal treatment is adopted to enhance the visible light photocatalytic activity of the TiO2/MCF composites. It is believed that the post-thermal treatment plays a significant role in controlling the carbon diffusion from the surface to the bulk of TiO2. Compared to traditional C-TiO2 photocatalysts, the prepared C-doped catalyst exhibits stable carbon doping of TiO2, superior adsorption capacity and higher visible light photocatalytic activity owing to the special structure of the supported mesoporous catalyst. This study implies that the novel photocatalyst has good application prospects in photocatalytic water splitting, dye-sensitized solar cells and other fields.
Co-reporter:Deli Lu, Hong Chen, Xuefeng Yan, Lingzhi Wang, Jinlong Zhang
Journal of Photochemistry and Photobiology A: Chemistry 2015 Volume 299() pp:125-130
Publication Date(Web):15 February 2015
DOI:10.1016/j.jphotochem.2014.11.011
•A fluorescent resonance energy transfer (FRET) system was built for ratiometric sensing of Hg2+ using periodic mesoporous organosilica (PMO) nanoparticles as the scaffold.•Bis-silylated anthracene (Anth) and silylated Rhodamine 6G derivative containing spirolactam unit (R6G) were adopted as the energy donor and acceptor of FRET, which were arranged into the pore framework and channel, respectively.A fluorescent resonance energy transfer (FRET) system was built for ratiometric sensing of Hg2+ in water with periodic mesoporous organosilica (PMO) nanoparticles (NPs) as the scaffold. The silylated rhodamine 6G with a spiro-ring (R6G) as the energy acceptor was covalently attached on the pore walls of anthracene (Anth) encapsulated PMO NPs, which played the role of energy donor. In the presence of Hg2+, the fluorescence emission from R6G in the pore channel was observed by exciting Anth in the framework, which means the emission energy of Anth can effectively funnel into R6G and excite it. The successful FRET from Anth to R6G should be attributed to the shortened distance between them attributed to the nanometer-sized pore system of PMO matrix, which finally leads to the emission of original colorless R6G through a Hg2+-promoted ring-opening process of R6G derivative. An extremely low detection limit for Hg2+ (6 × 10−9 M) can be achieved. These results demonstrate that fluorescent PMOs have great potential as supporting materials for enhanced fluorescence chemosensors.
Co-reporter:Juying Lei;Ying Chen;Lingzhi Wang;Yongdi Liu
Journal of Materials Science 2015 Volume 50( Issue 9) pp:3467-3476
Publication Date(Web):2015 May
DOI:10.1007/s10853-015-8906-3
A TiO2-based catalyst modified with highly condensed g-C3N4 has been synthesized though a simple vacuum calcination method and applied for the photocatalytic degradation of azo dye acid orange 7 (AO7). The obtained catalyst was thoroughly characterized by an array of analytical techniques, among which X-ray diffraction, Fourier transform infrared spectroscopy, UV–vis diffuse reflectance spectra, and transmission electronic microscopy proved a successfully combination of the two composites. And elemental analysis revealed a C/N ratio close to the theoretical data of g-C3N4, indicating highly condensed g-C3N4 in the composited catalyst. The catalyst showed excellent photocatalytic activity toward degradation of AO7 under both visible and UV light, and in addition it had better photocatalytic performance than that of the catalyst prepared by calcination in air. The high photocatalytic activity could be attributed to two aspects: the suitable band gap positions for g-C3N4/TiO2 composite which could improve the separation efficiency of photo-generated electron–hole pairs and the high condensation degree of g-C3N4 resulting from the vacuum calcination which is advantageous for higher carrier mobility and lower HOMO levels.
Co-reporter:Bocheng Qiu ; Mingyang Xing ;Jinlong Zhang
Journal of the American Chemical Society 2014 Volume 136(Issue 16) pp:5852-5855
Publication Date(Web):April 8, 2014
DOI:10.1021/ja500873u
TiO2/graphene composites have been well studied as a solar light photocatalysts and electrode materials for lithium-ion batteries (LIBs). Recent reports have shown that ultralight 3D-graphene aerogels (GAs) can better adsorb organic pollutants and can provide multidimensional electron transport pathways, implying a significant potential application for photocatalysis and LIBs. Here, we report a simple one-step hydrothermal method toward in situ growth of ultradispersed mesoporous TiO2 nanocrystals with (001) facets on GAs. This method uses glucose as the dispersant and linker owing to its hierarchically porous structure and a high surface area. The TiO2/GAs reported here exhibit a highly recyclable photocatalytic activity for methyl orange pollutant and a high specific capacity in LIBs. The strong interaction between TiO2 and GAs, the facet characteristics, the high electrical conductivity, and the three-dimensional hierarchically porous structure of these composites results in highly active photocatalysis, a high rate capability, and stable cycling.
Co-reporter:Mingyang Xing, Wenzhang Fang, Xiaolong Yang, Baozhu Tian and Jinlong Zhang
Chemical Communications 2014 vol. 50(Issue 50) pp:6637-6640
Publication Date(Web):27 Mar 2014
DOI:10.1039/C4CC01341G
Highly-dispersed boron-doped graphene nanoribbons (B-GNRs), prepared by a simple vacuum activation method, exhibit p-type semiconductor properties and provide many more zigzag- and armchair-edges to facilitate control of the bandgap. B-GNRs are used for the photodegradation of Rhodamine B in order to demonstrate their excellent conductivity and photocatalytic activity.
Co-reporter:Deli Lu, Fei Teng, Yunchang Liu, Liujia Lu, Chen Chen, Juying Lei, Lingzhi Wang and Jinlong Zhang
RSC Advances 2014 vol. 4(Issue 36) pp:18660-18667
Publication Date(Web):01 Apr 2014
DOI:10.1039/C4RA01599A
A mesoporous shell containing a fluorescence resonance energy transfer (FRET) type of ratiometric Cu2+ fluorescent sensor was coated around a cetyltrimethylammonium bromide (CTAB) stabilized Fe3O4@SiO2 core. All of the units comprising the sensor composite, including the Cu2+ ligand, signal reference and reporter units, are independent of each other and without a direct covalent linkage between them, and are site-selectively self-assembled into the pore framework or channel of the mesoporous silica matrix through the electrostatic interaction between CTAB porogen and silicates. The coordination of Cu2+ and its ligand leads to the variation of fluorescence energy transfer efficiency between neighboring FRET pairs benefiting from the nanosized pore system of the mesoporous matrix, which finally results in the ratiometric detection of Cu2+. Investigation of Cu2+ adsorption performance indicated rapid removal efficiency, with a maximum adsorption capacity of 17.86 mg g−1. Fe3O4 nanoparticles were introduced as a core to make the sensor system magnetically recyclable after sensing and adsorption. Finally, the disassembly and reassembly of the Cu2+ sensor were achieved by extracting and reintroducing the units in CTAB micelles, making the sensing system reproducible.
Co-reporter:Zhenhao Xi, Changjiang Li, Lu Zhang, Mingyang Xing, Jinlong Zhang
International Journal of Hydrogen Energy 2014 Volume 39(Issue 12) pp:6345-6353
Publication Date(Web):15 April 2014
DOI:10.1016/j.ijhydene.2014.01.209
•Cu2O/TiO2 nanoparticles were prepared by solvothermal method.•H2 evolution rate under simulated solar irradiation was increasingly promoted.•A certain amount of Cu particles were formed on the surface of Cu2O/TiO2.•Photoactivity was accordingly further enhanced with forming Cu particles.•The Cu particles play a key role in enhancing the hydrogen production activity.Cu2O/TiO2 nanoparticles were prepared by solvothermal method, which formed the heterostructure of Cu2O/TiO2. Due to the heterostructure, the H2 evolution rate under simulated solar irradiation was increasingly promoted. Meanwhile a certain amount of Cu particles which were confirmed by Transmission Electro Microscopy (TEM) and X-Ray Photoelectron Spectroscopy (XPS), formed on the surface of Cu2O/TiO2, and the photoactivity was accordingly further enhanced. The stabilized activity was maintained after many times irradiation. It is interesting that after a few hours irradiation the amount of Cu particles on the surface kept unchanged in the presence of Cu2O and TiO2. The Cu particles that formed during hydrogen generation reaction play a key role in the further enhancement of the hydrogen production activity. In this study, it is the first time to study the details on the formation of the stable ternary structure under simulated solar irradiation and their synergistic effect on the photoactivity of the water splitting.
Co-reporter:Yongji Gu, Mingyang Xing, Jinlong Zhang
Applied Surface Science 2014 Volume 319() pp:8-15
Publication Date(Web):15 November 2014
DOI:10.1016/j.apsusc.2014.04.182
Highlights
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Graphene based doped TiO2 nanocomposites were prepared.
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The intimate contact between doped TiO2 and graphene is achieved simultaneously.
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These nanocomposites showed higher photocatalytic activity than TiO2 and doped TiO2.
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Photocatalytic mechanism was explained thoroughly.
Co-reporter:Haibei Liu;Fan Shen;Mingyang Xing;Jinlong Zhang;Masakazu Anpo
Catalysis Letters 2014 Volume 144( Issue 9) pp:1494-1498
Publication Date(Web):2014 September
DOI:10.1007/s10562-014-1308-3
Vacuum activation method was used to modify TiO2 to produce highly air stable V4+ and Ti3+ co-doped TiO2. The physicochemical properties of the catalysts were studied by a series of characterizations. The low valence Ti3+ and V4+ states were formed by vacuum activation and vanadium doping formed new impurity bands between CB and VB of TiO2, which narrowed the band gap and enhanced the absorption of visible light. Also, the V4+/V5+ and Ti3+/Ti4+ cations could reduce the e−/h+ pair recombination rate to give high quantum efficiency.
Co-reporter:Dianyu Qi ; Mingyang Xing ;Jinlong Zhang
The Journal of Physical Chemistry C 2014 Volume 118(Issue 14) pp:7329-7336
Publication Date(Web):March 17, 2014
DOI:10.1021/jp4123979
A novel hydrophobic photocatalyst carbon-doped TiO2/MCF-F was prepared by using silica mesoporous cellular foam (MCF) as host material, glucose as carbon source, and NH4F as hydrophobic modifying agent. It was confirmed that titania nanoparticles were loaded in pore of MCF by XRD, N2 sorption isotherms, and TEM. The loaded titania nanoparticles exhibited higher photocatalytic performance. UV–vis absorption spectra and XPS suggested carbon atoms were doped in the lattice of titania by replacing titanium atoms and narrowed the band gap so that visible light absorption and photocatalytic activity of the photocatalyst were highly promoted. On the other hand, water contact angle measurement and XPS proved that the photocatalyst was endowed with hydrophobic property, which was caused by Si–F bonds. Carbon-doped TiO2/MCF-F photocatalyst showed good adsorptive ability and photocatalytic activity in the photodegradation test of methyl orange under visible light.
Co-reporter:Zhidan Tian, Baozhu Tian, Jinlong Zhang
Dyes and Pigments 2013 Volume 99(Issue 3) pp:1132-1136
Publication Date(Web):December 2013
DOI:10.1016/j.dyepig.2013.06.013
Two new rhodamine dyes (Rh Q-H, Rh Q-Me) containing 1, 4-diethyl-1, 2, 3, 4-tetrahydroquinoxaline as an effective electron donor are designed and synthesized. The structures of the novel compounds are confirmed by 1H NMR, 13C NMR and ESI. Due to an excited-state intramolecular charge transfer (ICT), the new dyes exhibit longer absorption (>580 nm) and emission (>640 nm) compared with the model compounds, rhodamine 101 and rhodamine 6G. The new rhodamine dyes show large Stokes shift of 40–50 nm in commonly used solvents. Notably, when measured in a mixture of H2O/EtOH solution, significant stokes shift of 65–68 nm are achieved, which is among the largest Stokes shifts ever reported for rhodamine dyes.
Co-reporter:Lu Zhang, Zhenhao Xi, Mingyang Xing, Jinlong Zhang
International Journal of Hydrogen Energy 2013 Volume 38(Issue 22) pp:9169-9177
Publication Date(Web):26 July 2013
DOI:10.1016/j.ijhydene.2013.05.052
•Ternary P25/GO/Pt hybrid photocatalysts are prepared by different methods.•Comparison of property of the ternary P25/GO/Pt prepared by different methods.•The quantity of introduced GO and electronic transfer path play an important role.In this study, ternary P25/GO/Pt hybrid photocatalysts are prepared in different orders, using Degussa's TiO2 (P25), graphene oxide (GO), chloroplatinic acid as precursor. The prepared catalysts were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), fourier transform infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS). This work is first time to compare the hydrogen production of the ternary P25/GO/Pt hybrid photocatalysts prepared in different orders. We focus on studying the introduction of GO and find that the quantity of introduced GO and electronic transfer path play an important role in photocatalytic activity on ternary P25/GO/Pt hybrid catalysts. When the proper Pt particle loaded on the flat surface of GO which was 0.5wt% of P25, the highest H2 evolution was obtained.
Co-reporter:Cuiyun Zeng, Min Guo, Baozhu Tian, Jinlong Zhang
Chemical Physics Letters 2013 Volume 575() pp:81-85
Publication Date(Web):21 June 2013
DOI:10.1016/j.cplett.2013.05.007
Highlights•Ag/AgBr/RGO plasmonic photocatalyst was prepared by a facile multistep route.•Ag/AgBr/RGO exhibited strong light absorption in the visible region.•Ag/AgBr/RGO can effectively separate the photogenerated electrons and holes.•Ag/AgBr/RGO showed excellent visible light activity for the degradation of azo dyes.A novel visible light driven photocatalyst, reduced graphene oxide (RGO)-modified Ag/AgBr (Ag/AgBr/RGO), was synthesized by sequent double-jet precipitation, hydrothermal, and UV light reduction processes. The XPS and Raman results confirmed that part of GO was successfully reduced by hydrothermal treatment. Compared with Ag/AgBr, Ag/AgBr/RGO exhibited higher visible light photocatalytic activity for the degradation of methyl orange. The EIS analysis revealed that Ag/AgBr/RGO has better capability for charge transfer than Ag/AgBr. The excellent photocatalytic activity of Ag/AgBr/RGO is attributed to the strong visible light absorption of Ag nanoparticles and AgBr as well as the effective separation of photogenerated electrons and holes.Graphical abstract
Co-reporter:Rongfang Dong ; Baozhu Tian ; Cuiyun Zeng ; Taoyun Li ; Tingting Wang ;Jinlong Zhang
The Journal of Physical Chemistry C 2013 Volume 117(Issue 1) pp:213-220
Publication Date(Web):December 13, 2012
DOI:10.1021/jp311970k
Uniform cubic Ag@AgCl plasmonic photocatalyst was synthesized by a facile green route in the absence of organic solvent, in which a controllable double-jet precipitation technique was employed to fabricate homogeneous cubic AgCl grains and a photoreduction process was used to produce Ag nanoparticles (NPs) on the surface of AgCl. During the double-jet precipitation process, the presence of gelatin and Cl– ions at low concentration was necessary for the formation of cubic AgCl grains. Atomic force microscopy (AFM) was used to probe the morphological structure of Ag@AgCl grains for the first time, which showed that Ag NPs are anchored on the surface of AgCl grains like up-and-down mounds. Further characterization of the photocatalyst was also done by scanning electron microscopy (SEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and UV–visible diffuse reflectance spectroscopy (DRS). The as-prepared Ag@AgCl plasmonic photocatalyst exhibited excellent photocatalytic efficiency for the degradation of the azo dye acid orange 7 (AO7), phenol, and 2,4-dichlorophenol (2,4-DCP). The photocatalytic mechanism was studied by radical-trapping experiments and the electron spin resonance (ESR) technique with 5,5-dimethyl-1-pyrroline N-oxide (DMPO), and the results indicated that •O2– and Cl0 are responsible for the rapid degradation of organic pollutants under visible-light irradiation.
Co-reporter:Muhammad Nasir, Zhenhao Xi, Mingyang Xing, Jinlong Zhang, Feng Chen, Baozhu Tian, and Segomotso Bagwasi
The Journal of Physical Chemistry C 2013 Volume 117(Issue 18) pp:9520-9528
Publication Date(Web):April 16, 2013
DOI:10.1021/jp402575w
Different samples of Ce- and S-codoped TiO2 nanoparticles were prepared through simple sol–gel synthesis method by using cerium nitrate hexahydrate as cerium precursor, thiourea as sulfur, and tetrabutyl titanate (TBOT) as titanium precursor. Characterization of prepared samples were done by various techniques such as, X-ray diffraction (XRD), UV–visible diffuse reflectance spectroscopy, transmission electron microscopy, Fourier transformation infrared spectroscopy, photoluminescence spectroscopy, and X-ray photoelectron spectroscopy. The XRD showed the presence of only anatase TiO2 for the single sulfur-doped and cerium- and sulfur-codoped titania samples. XRD analysis also pointed out the decrease in the crystal size with the increase in Ce concentration in the samples. The BET analysis reported an increase in the surface area and decrease in the pore size with the increase in the Ce concentration. The PLS results of the samples first showed a decrease in the intensity of the spectra sync with the reduction of recombination centers when the Ce was introduced in codoped TiO2 with the maximum decrease for 0.04 Ce/S-codoped titania; with the further increase in the Ce concentration in the samples, the intensity of the spectra gradually increased coinciding with the increase in the recombination centers. The recombination centers exhibit a direct relationship with the photocatalytic activity of the samples, which could be evidenced by the decolorization of 25 mg/L solution of AO-7. The activity of codoped samples was first increased by the incorporation of Ce with the maximum degradation for 0.04 cerium- and sulfur-codoped titania. By the further increase in the Ce amount in the Ce- and S-codoped titania samples the activity was shown to decrease gradually.
Co-reporter:Jinlong Zhang
Research on Chemical Intermediates 2013 Volume 39( Issue 4) pp:1613-1614
Publication Date(Web):2013 April
DOI:10.1007/s11164-012-0893-2
Co-reporter:Ming-Yang Xing, Bing-Xing Yang, Huan Yu, Bao-Zhu Tian, Segomotso Bagwasi, Jin-Long Zhang, and Xue-Qing Gong
The Journal of Physical Chemistry Letters 2013 Volume 4(Issue 22) pp:3910-3917
Publication Date(Web):November 4, 2013
DOI:10.1021/jz4021102
Although the preparation of TiO2 exposed with high-energy facets is a challenge, these facets have a large application potential in the loading of Au nanoparticles. We successfully prepared TiO2 single crystals exposed with (001) and (110) facets as an ideal support to load the highly dispersed nanosized Au particles to improve the stability of Au on the catalyst surface and expand its photocatalytic applications. The transfer of photoexcited electrons from the higher-surface-energy facet, that is, (001) and (110), to the lower-energy facet of (101) could make the electrons aggregate on the (101) facet and leave holes on the (001) and (110) facets, which would promote the separation of electrons and holes. The highly dispersed Au nanoparticles also could capture the electrons from active facets and further improve the photocatalytic activity of TiO2. Systematic density functional theory calculation was also carried out to investigate the formation of (001) and (110) facets.Keywords: anatase; Au loading stability; density functional theory; high-energy facets; photocatalytic activity;
Co-reporter:Deli Lu ; Juying Lei ; Lingzhi Wang ;Jinlong Zhang
Journal of the American Chemical Society 2012 Volume 134(Issue 21) pp:8746-8749
Publication Date(Web):May 16, 2012
DOI:10.1021/ja301691j
Monodisperse and nanometer-sized periodic mesoporous organosilicas co-doped with fluorescence resonance energy transfer cascades composed of triple fluorophores at various ratios were prepared. These nanoparticles exhibit multifluorescent emissions by a single-wavelength excitation and were designed for the application as multichannelly traceable drug carriers. Different from the hydrophilic framework of inorganic mesoporous silica and hydrophobic framework of mesoporous carbon, these multifluorescent nanoparticles have intrinsically different and finely tunable pore surface polarities governed by the type and amount of fluorophore inside the framework. When applied as drug carriers, they can achieve synchronous or asynchronous release of different drugs by simply choosing different colored nanoparticles. These colorful mesoporous composites with finely tunable color-related drug release performance provide a strong barcoding system for the potential applications of fluorescent nanoparticles in effective screening of drugs and therapeutic protocols for diseases.
Co-reporter:Deli Lu, Juying Lei, Zhidan Tian, Lingzhi Wang, Jinlong Zhang
Dyes and Pigments 2012 Volume 94(Issue 2) pp:239-246
Publication Date(Web):August 2012
DOI:10.1016/j.dyepig.2012.01.004
Monodisperse mesoporous silica nanosphere (MSN) modified with anthracene derivative, 2-(3-(triethoxysilyl) propylamino)-N-(9-anthryl methyl) acetamide (SGAAn) has been fabricated as a fluorescent sensor (SGAAn-MSN) for the detection of metal ions, which shows an exclusive selectivity to Cu2+. Compared with SGAAn, SGAAn-MSN presents a higher sensitivity to Cu2+. The loading amount of SGAAn in MSN has a great influence on the detection sensitivity of SGAAn-MSN, which varies with the local concentration and accessibility of SGAAn in the pore channel of MSN. Interference studies indicate that the addition of other metal ions such as Ag+, Cd2+ and Pb2+ has a negligible effect on the selectivity of SGAAn-MSN to Cu2+. The possible mechanism for the sensing behavior of SGAAn-MSN to Cu2+ is proposed based on the relation between fluorescence quench degree and Cu2+ concentration.Highlights► Cu2+ fluorescence sensor based on MSN was fabricated. ► The sensor has high detection sensitivity to Cu2+. ► The improved sensitivity is attributed to the high local concentration of dye molecules in MSN. ► The dye molecules loading amount has a great influence on the detection sensitivity.
Co-reporter:Lu Zhang, Baozhu Tian, Feng Chen, Jinlong Zhang
International Journal of Hydrogen Energy 2012 Volume 37(Issue 22) pp:17060-17067
Publication Date(Web):November 2012
DOI:10.1016/j.ijhydene.2012.08.120
In this study, TiO2 photocatalysts with nickel sulfide cocatalyst are prepared by loading nickel sulfide on TiO2 with solvothermal synthesis approach. The materials were prepared by glycol solvothermal method using anatase, nickel nitrate, thiourea as precursor. The prepared catalysts were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), ultraviolet–visible diffuse reflectance spectroscopy (UV–vis DRS), and X-ray photoelectron spectroscopy (XPS). This is the first time to report that NiS is used as a cocatalyst with TiO2 for the photocatalytic production of H2. The results revealed that the structure and the amount of the cocatalyst loaded on TiO2 play important roles in the photocatalytic activity of NiS/TiO2 composite. The maximum evolution of H2 was obtained when NiS had hexagonal structure with content in the composite of 7 at% in relation to TiO2. The rate of H2 evolution was increased up to about 30 times than that of TiO2 alone.Highlights▶ TiO2 photocatalysts with nickel sulfide cocatalyst are prepared. ▶ To enhance photocatalytic H2 production of TiO2 by using NiS as cocatalyst. ▶ Structure and loading content of NiS play an important role on activity of NiS/TiO2.
Co-reporter:Yunfei Ma, Mingyang Xing, Jinlong Zhang, Baozhu Tian, Feng Chen
Microporous and Mesoporous Materials 2012 Volume 156() pp:145-152
Publication Date(Web):1 July 2012
DOI:10.1016/j.micromeso.2012.02.010
Well-ordered mesoporous TiO2 co-doped with nitrogen and ytterbium was successfully synthesized by an evaporation-induced self-assembly process. The as-prepared and calcined mesoporous TiO2 materials were characterized by X-ray diffraction, transmission electron microscope, UV–vis absorbance spectroscopy, X-ray photoelectron spectroscopy, fourier transform infrared and N2 adsorption–desorption measurements. After calcinations at 350 °C, the TiO2 co-doped with nitrogen and 3% ytterbium had the highest surface area (219 m2 g−1) and retained ordered structures. Under visible light irradiation, 75% of 20 mg/L phenol solution was degraded after 10 h and 10 mg/L rhodamine B (RhB) was decomposed completely after 4 h. The significant enhancement in the photocatalytic activity of the modified TiO2 is attributed to the synergistic effect of N and Yb. The N dopant extended the absorption to visible region and the Yb dopant was beneficial in stabilizing the mesoporous structure and restraining the recombination of photogenerated holes and electrons.Graphical abstractHighlights► Ordered mesoporous Yb, N co-doped TiO2 was successfully synthesized. ► The nitrogen dopant enhanced the absorption in the visible region. ► The ytterbium dopant stabilized the ordered mesoporous structure. ► The ytterbium dopant reduced the recombination of holes and electrons. ► The 3.0Yb/N-TiO2 showed higher visible photocatalytic activity than pure TiO2.
Co-reporter:Deli Lu, Lingang Yang, Zhidan Tian, Lingzhi Wang and Jinlong Zhang
RSC Advances 2012 vol. 2(Issue 7) pp:2783-2789
Publication Date(Web):08 Feb 2012
DOI:10.1039/C2RA01106A
Core-shell mesoporous silica nanospheres encapsulated with rhodamine 101 into the solid core and 8-aminoquinoline derivatives into the mesoporous shell were used as a ratiometric fluorescent sensor to detect metal ions, which shows a high selectivity and sensitivity to Zn2+. Concentrations as low as 5 × 10−8 M can be detected and the addition of other metal ions has a negligible influence on the fluorescence emission. Moreover, the dye-doped nanospheres show excellent photostability, no dye leaking and a good adsorption capacity to Zn2+, which make it repeatedly applicable for simultaneous heavy metal ion sensing and removal from polluted water.
Co-reporter:Segomotso Bagwasi, Baozhu Tian, Feng Chen, Jinlong Zhang
Applied Surface Science 2012 Volume 258(Issue 8) pp:3927-3935
Publication Date(Web):1 February 2012
DOI:10.1016/j.apsusc.2011.12.066
Abstract
Iodine doped titanium dioxide has been successfully prepared by simple hydrolysis of tetrabutyl titanate in the presence of iodic acid. The adopted method allowed for the production of spherical iodine doped titaniun dioxide nanoparticles with varied amount of iodine content. Analysis by X-ray diffraction, Raman, transmission electron microscopy as well as UV–vis DRS revealed that titanium dioxide nanostructures were doped with iodine which existed in two different valence states I5+ and I−. The iodine in the form of I5+ is believed to have doped into the lattice whereas I− was well dispersed on the surface of TiO2 probably as iodine adducts hence rendering it to be highly absorbing in visible light region. The I-TiO2 exhibited improved photocatalytic activity toward degradation of acid orange 7 (AO7), methyl orange (MO) and 2,4-dichlorophenol (2,4-DCP) under visible light over the pristine TiO2 prepared by the same method. High catalytic properties are attributed to iodine doping which led to high specific surface area, absorption in visible region as well as alleviation of charge carrier recombination. The most probable route undertaken in the degradation of AO7 is through indirect oxidation by the hydroxyl radicals.
Co-reporter:Ling-Zhi Wang, Lin Jiang, Cheng-Cheng Xu, and Jin-Long Zhang
The Journal of Physical Chemistry C 2012 Volume 116(Issue 31) pp:16454-16460
Publication Date(Web):July 18, 2012
DOI:10.1021/jp302289e
TiO2 was loaded on Cr-MCM-4s8 and Cr-KIT-6 mesoporous silica matrixes (TiO2/Cr-MCM-48 and TiO2/Cr-KIT-6) synthesized in alkaline and acidic conditions to achieve visible-light driven photocatalytic activity. The influences of pore ordering, Cr species, and content of mesoporous matrixes to the photocatalytic activity of TiO2 were carefully studied, where the Si/Cr ratio varies from 10 to 40 both in alkaline and acidic conditions. For the acidic conditions, Cr species are present as Cr(VI) in the samples synthesized with Si/Cr > 20 and as the mixture of Cr(VI) and Cr (III) in the samples synthesized with Si/Cr ≤ 20. However, for the alkaline conditions, Cr species are present as the mixture of Cr(VI) and Cr(III) in all of samples synthesized with Si/Cr = 10–40. Energy dispersive X-ray spectrum (EDX) and X-ray powder diffraction (XRD) indicate that the alkaline system leads to more introduction of Cr content but more deterioration of matrix ordering. UV–vis spectra and XRD patterns indicate that Cr(VI) and Cr(III) species exist as highly dispersive Cr–O–M (M = Si and Cr) in the framework and Cr2O3 crystal in the pore channel, respectively. For the photocatalytic application by adopting AO7 as the degradation target, all of TiO2 loaded composites show visible-light driven photocatalytic activity, which reaches the best at Si/Cr = 30. However, almost all of the TiO2 loaded on Cr-KIT-6 synthesized in acidic conditions show higher activities than those loaded on Cr-MCM-48 synthesized in alkaline conditions with the same Si/Cr ratio, which is attributed to the formation of less Cr2O3 crystal and better pore ordering of the matrix synthesized in the acidic conditions.
Co-reporter:Baozhu Tian;Jinlong Zhang
Catalysis Surveys from Asia 2012 Volume 16( Issue 4) pp:210-230
Publication Date(Web):2012 December
DOI:10.1007/s10563-012-9145-0
Semiconductor photocatalysis is considered to be one of the most promising technologies to solve the worldwide environmental and energy issues. In recent years, silver halide (AgX)-based photocatalytic materials have received increasing research attention owing to its excellent visible light-driven photocatalytic performances in the applications of organic pollutant degradation, H2/O2 generation, and disinfection. AgX-based materials used in photocatalytic fields can be classified into three categories: AgX (Ag/AgX), AgX composites, and supported AgX materials. For the AgX (Ag/AgX) photocatalysts, it has been widely accepted that the final photocatalytic performances of photocatalysts are severely dependent on their morphological structures as well as exposed crystal facets. As a result, considerable efforts have been devoted to fabricating different morphological AgX photocatalysts as well as exploring the relationship between the morphological structures and photocatalytic performances. In this review, we mainly introduce the recent developments made in fabricating morphology and facet-controllable AgX (Ag/AgX) photocatalytic materials. Moreover, this review also deals with the photocatalytic mechanism and applications of AgX (Ag/AgX) and supported AgX materials.
Co-reporter:Xiaojun Shen;Jinlong Zhang;Baozhu Tian;Masakazu Anpo
Journal of Materials Science 2012 Volume 47( Issue 15) pp:5743-5751
Publication Date(Web):2012 August
DOI:10.1007/s10853-012-6465-4
Titanium dioxide with different ratios of anatase to brookite has been prepared by a facile hydrothermal method in the presence of tartaric acid. The resulting samples were investigated by X-ray diffraction, Raman spectroscopy, scanning electron microscopy, transmission electron microscopy, UV–Vis diffuse reflectance spectra, and Brunauer–Emmett–Teller analysis. The contents of anatase and brookite in the TiO2 particles have been successfully controlled by simply adjusting molar ratio of tartaric acid to Ti in reaction system. The degradation of Rhodamine B in aqueous solutions reveals that the catalyst containing 78.7 % anatase and 21.3 % brookite has the highest photocatalytic activity. A proposed mechanism is discussed to interpret the evolution of the phases based on the effect of different C4H6O6/Ti molar ratios.
Co-reporter:Yanchao Jiao, Feng Chen, Bin Zhao, Hongyun Yang, Jinlong Zhang
Colloids and Surfaces A: Physicochemical and Engineering Aspects 2012 Volume 402() pp:66-71
Publication Date(Web):20 May 2012
DOI:10.1016/j.colsurfa.2012.03.020
A series of brookite and anatase TiO2 hybrids with different ratios were synthesized by in situ hydrolysis of tetrabutyl titanate (TBOT) on the pre-prepared brookite nanoflowers. The composition and content of the mixture were examined by X-ray diffraction (XRD). The morphology and construction of the hybrids were examined by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and high-resolution transmission electron microscopy (HRTEM), while BET was used to measure the specific surface area of all the samples. Anatase nano-grains grow on the surface of brookite petals, which builds special heterojunction on their interface and thus benefits the separation of photogenerated electrons and holes under UV irradiation. The TiO2 hybrids appeared superior photocatalytic activity to the single phase toward the degradation of methyl orange (MO) and 2,4-dichlorophenol (2,4-DCP). The hybrid contains 40% anatase and 60% brookite exhibited the highest activity, the degradation rate constants of which are 2.27 and 1.80 times higher than that of the corresponding physically mixed sample for the degradation of MO and 2,4-DCP, respectively.Graphical abstractHighlights► Brookite/anatase hybrids with superior photocatalytic activity were prepared. ► Hybrids have an optimal brookite/anatase ratio of 6/4 for photocatalytic activity. ► Special heterojunction forms from the in situ nucleation of anatase on brookite. ► The heterojunction benefits the separation of photogenerated carriers in hybrids.
Co-reporter:Haibei Liu, Yongmei Wu, and Jinlong Zhang
ACS Applied Materials & Interfaces 2011 Volume 3(Issue 5) pp:1757
Publication Date(Web):April 19, 2011
DOI:10.1021/am200248q
Carbon-modified vanadium-doped TiO2 was successfully prepared with the intention of enhancing the visible-light photocatalytic performance by expanding the absorption in the visible-light region and improving the quantum efficiency of the photocatalytic reaction. The physicochemical properties of the catalysts were characterized by XRD, Raman, TEM, XPS, UV–vis diffuse reflectance spectra. The result indicated that some vanadium ions substituted for Ti4+ in the lattice of TiO2, whereas all the carbon was modified on the surface of catalysts in the form of stable graphite-like carbonaceous species. Compared with vanadium doped TiO2 sample and carbon modified TiO2 sample, the 0.32C–0.5%V–TiO2 photocatalyst exhibited excellent visible light activity and the synergistic effects of vanadium and carbon was responsible for improving the photocatalytic activity.Keywords: carbon modified; photocatalytic activity; TiO2; vanadium doped
Co-reporter:Mingyang Xing, Jinlong Zhang, Feng Chen and Baozhu Tian
Chemical Communications 2011 vol. 47(Issue 17) pp:4947-4949
Publication Date(Web):21 Mar 2011
DOI:10.1039/C1CC10537J
This study reports a simple and economic method to modify Degussa P25 with a vacuum activated procedure, resulting in its high photo-activity and photosensitivity, which suggests this method to be a starting point for the extension of its application to photocatalysis.
Co-reporter:Yanchao Jiao, Bin Zhao, Feng Chen and Jinlong Zhang
CrystEngComm 2011 vol. 13(Issue 12) pp:4167-4173
Publication Date(Web):12 May 2011
DOI:10.1039/C0CE00932F
A feasible approach to synthesize pure brookite was achieved in an aqueous ammonia system via a hydrothermal process. By hydrothermal treatment of the titanate that directly hydrolyzed from tetrabutyl titanate (TBOT), a phase transition from titanate to TiO2 was observed with XRD. Anatase TiO2 was produced with an unobstructed closure of titanate layers. The phase transition process can be controlled by adding an electrolyte such as NaCl into the hydrothermal media. Na+ ions locally stop the direct closure of titanate layers at their adjacent position, which induce the formation of a brookite-like structure. The optimal hydrothermal reaction parameters for the crystal lattice formation of brookite in aqueous ammonia media were found to be 180 °C, 0.5 M NaCl and ≥72 h. The phase transition process of titanate precursor to TiO2 depends heavily on the electrolyte. Metal cations play a crucial role in conducting the transition procedure from layered titanate into brookite or anatase. Na+ is preferred to conduct the phase transition from titanate to brookite rather than K+ and Li+. Although anions do not determine the phase transition rule during the hydrothermal process, they are influential in the phase transition process, as they can promote the phase transition by interacting with the TiO6 octahedra.
Co-reporter:Sajjad Shamaila, Ahmed Khan Leghari Sajjad, Feng Chen, Jinlong Zhang
Journal of Colloid and Interface Science 2011 Volume 356(Issue 2) pp:465-472
Publication Date(Web):15 April 2011
DOI:10.1016/j.jcis.2011.01.015
A bismuth oxychloride (BiOCl) nanostructure is prepared by a new low temperature route using sodium dodecyl sulfate as template and urea as hydrolytic agent. A novel heterojunction is developed between BiOCl and tungsten oxide (WO3) to make it an efficient visible light photocatalyst. The catalysts were characterized by X-ray diffraction analysis, Raman spectroscopy, thermogravimetric analysis, energy-dispersive X-ray spectroscopy, scanning electron microscopy, transmission electron microscopy, and N2 sorption isotherms. The WO3/BiOCl heterojunction system extends the absorption edge to the visible region efficiently. BiOCl works as a main photocatalyst while WO3 acts as the photosensitizer absorbing visible light in the WO3/BiOCl composite. The individual BiOCl and WO3 show very low photocatalytic efficiency under visible light irradiation but their heterojunction provides unexpectedly high efficiency in decomposing rhodamine B as compared to Degussa P25, pure BiOCl, and WO3.Graphical abstractBiOCl prepared via new low temperature route is developed in a novel hetrerojunction of WO3/BiOCl as an efficient visible light active photocatalyst for environmental cleanup purposes.Research highlights► 2D nanoflakes of BiOCl are prepared by a new and facile low temperature route. ► A novel heterojunction is developed between BiOCl and WO3. ► The WO3/BiOCl heterojunction extends the absorption edge to the visible region. ► WO3 in this junction acts as the photosensitizer absorbing visible light. ► The WO3/BiOCl composite induces complete decomposition of RhB under visible light.
Co-reporter:Yuanlin Liu, Lingzhi Wang, Jinlong Zhang, Lijing Chen, Huasheng Xu
Microporous and Mesoporous Materials 2011 Volume 145(1–3) pp:150-156
Publication Date(Web):November 2011
DOI:10.1016/j.micromeso.2011.05.009
A layered mesoporous SAPO-34 with particle size of about 20 μm was synthesized by using as-synthesized SBA-15 as silica source. For comparison, another three synthesis system were adopted to form SAPO-34 by using stoichiometric equivalence of calcined SBA-15, physical mixture of calcined SBA-15 and P123, and physical mixture of colloidal silica and P123 as initial reactants, respectively. The result shows that SAPO-34 can be prepared by all of the synthesis systems, however, only the sample prepared with as-synthesized SBA-15 shows mesoporous structure as revealed by X-ray diffraction (XRD) and high resolution transmission electron microscopy (HRTEM). Compared with SAPO-34 prepared with conventional and the above three contrasting systems, the specific surface area of this sample is considerably improved due to the existence of mesoporous structure. For the application as the catalyst for methanol to olefins (MTO) reaction, the layered mesoporous SAPO-34 presents the longest single life among all of samples.Graphical abstractHighlights► Layered mesoporous SAPO-34 is fabricated using uncalcined SBA-15 as silica source. ► P123 in SBA-15 plays an important role for the formation of layered structure. ► The layered mesoporous SAPO-34 shows an improved selectivity to light olefins. ► The deactivation time for MTO is prolonged by using layered mesoporous SAPO-34.
Co-reporter:Baozhu Tian, Zhimang Shao, Yunfei Ma, Jinlong Zhang, Feng Chen
Journal of Physics and Chemistry of Solids 2011 Volume 72(Issue 11) pp:1290-1295
Publication Date(Web):November 2011
DOI:10.1016/j.jpcs.2011.07.024
Co-reporter:Yuanlin Liu, Lingzhi Wang, Jinlong Zhang
Materials Letters 2011 Volume 65(Issue 14) pp:2209-2212
Publication Date(Web):31 July 2011
DOI:10.1016/j.matlet.2011.04.064
A novel floral mesoporous SAPO-34 was synthesized via conventional hydrothermal method in the presence of NaF with F/Si = 0.02–0.2. X-ray diffraction (XRD) analysis shows that the crystallinity of SAPO-34 increases with the increasing F/Si ratio and reaches to the best at F/Si = 0.1. Further increasing of F/Si ratio leads to the decrease of the crystallinity and the ultimate phase transformation to SAPO-5. Scanning electron microscopy (SEM) analysis shows that the addition of NaF leads to the formation of floral SAPO-34 while the addition of other salts including NH4F, NH4Cl and NaCl leads to the formation of traditional cubic SAPO-34. N2 sorption isotherm and NH3 temperature programmed desorption (NH3-TPD) analyses indicate that floral SAPO-34 has the largest pore volume but lowest strong acidity compared with other samples with traditional cubic morphology. When applied to methanol to olefin (MTO) reactions, floral SAPO-34 shows the comparable yields of propylene and butylenes to other samples but lowest overall olefin yield, which is attributed to the synergistic effect of the largest pore volume and lowest strong acidity.Research Highlights► A floral mesoporous SAPO-34 is fabricated with the aid of NaF for MTO. ► The formation of floral structure is due to the eroding effect of fluoride ions. ► Floral SAPO-34 shows the highest selectivities for propylene and butylene in MTO.
Co-reporter:Xiaona Lu, Yunfei Ma, Baozhu Tian, Jinlong Zhang
Solid State Sciences 2011 Volume 13(Issue 3) pp:625-629
Publication Date(Web):March 2011
DOI:10.1016/j.solidstatesciences.2010.12.036
A series of uniform and transparent Fe-doped TiO2 films were prepared by autoclaved-sol method at low temperature. The as-prepared films were characterized by XRD, DRS, EPR and AFM. The photocatalytic activity was evaluated based on the degradation of Rhodamine B solution under visible light. It was found that all the films were composed of mixed-phase crystal of anatase and brookite. Fe3+ ions have been successfully doped into the TiO2 crystal lattice by substituting Ti4+, thus inducing significant absorption shift toward visible region compared with the pure TiO2 films. EPR result further illustrated the doped Fe ions entered into the TiO2 lattice. AFM reveals that doping of Fe ions increases the mean roughness and secondary particle size. The 0.5% Fe–TiO2 films demonstrated the highest photocatalytic activity under visible light due to the interaction of active sites, impurity energy level and contact surface area.Fe3+ ions have been successfully doped into the TiO2 crystal lattice by substituting Ti4+, thus inducing significant absorption shift toward visible region compared with the pure TiO2 films and higher photocatalytic activity.
Co-reporter:Huan Yu;Dr. Baozhu Tian;Dr. Jinlong Zhang
Chemistry - A European Journal 2011 Volume 17( Issue 20) pp:5499-5502
Publication Date(Web):
DOI:10.1002/chem.201003437
Co-reporter:Pengfei Ji, Mingyang Xing, Segomotso Bagwasi, Baozhu Tian, Feng Chen, Jinlong Zhang
Materials Research Bulletin 2011 46(11) pp: 1902-1907
Publication Date(Web):
DOI:10.1016/j.materresbull.2011.07.027
Co-reporter:Dr. Ming-Yang Xing;Dr. Dian-Yu Qi; Jin-Long Zhang; Feng Chen
Chemistry - A European Journal 2011 Volume 17( Issue 41) pp:11432-11436
Publication Date(Web):
DOI:10.1002/chem.201101654
Co-reporter:Ming-Yang Xing ; Wei-Kun Li ; Yong-Mei Wu ; Jin-Long Zhang ;Xue-Qing Gong
The Journal of Physical Chemistry C 2011 Volume 115(Issue 16) pp:7858-7865
Publication Date(Web):April 6, 2011
DOI:10.1021/jp111103r
A novel double hydrothermal method to prepare the boron and nitrogen codoped TiO2 is developed. Two different ways have been used for the synthesis of the catalysts, one through the addition of boron followed by nitrogen, and the other through the addition of nitrogen first and then by boron. The X-ray photoelectron spectroscopy analysis indicates the synergistic effect of boron and nitrogen with the formation of Ti−B−N−Ti and Ti−N−B−O compounds on the surface of catalysts when nitrogen is introduced to the materials first. When the boron is added first, only Ti−N−B−O species occurs on the surface of catalysts. The above two compounds are all thought to enhance the photocatalytic activities of codoped TiO2. Density functional theory simulations are also performed to investigate the B−N synergistic effect. For the (101) surface, the formation of Ti−B−N−Ti structures gives rise to the localized states within the TiO2 band gap.
Co-reporter:Bin Zhao, Feng Chen, Yanchao Jiao, Hongyun Yang, Jinlong Zhang
Journal of Molecular Catalysis A: Chemical 2011 Volume 348(1–2) pp:114-119
Publication Date(Web):1 September 2011
DOI:10.1016/j.molcata.2011.08.015
Ag0-loaded brookite/anatase composite was prepared via an alkalescent hydrothermal process. The photocatalytic performance of as-prepared catalysts was evaluated in terms of the degradation of methyl orange (MO). The physical features of the catalysts were measured with XRD, BET and HRTEM techniques. The phase content of brookite and anatase in the TiO2 can be controlled by fixing the concentration of the electrolyte in the hydrothermal system. The as-formed Ag0 clusters have an average diameter of ca. 1.5 nm and intersperse throughout the surface of both anatase nanoparticles and brookite nanorods. Ag0 has an optimal loading dosage of 2.0 mol%, with which the photocatalytic degradation of MO are 4.82 and 2.28 times of that with Ag0-free composite and P25 TiO2, respectively. The synergistic effect of hetero-junction in brookite/anatase composite and the schottky barrier at the interface of Ag0 and TiO2 significantly improved the separation of the photogenerated electrons and holes under UV irradiation and thus resulted in a much enhanced photocatalytic reactivity towards the degradation of MO.Graphical abstractHighlights► Ag0-loaded brookite/anatase TiO2 with uniform Ag0 size distribution was prepared. ► 2.0% Ag0-loaded brookite/anatase TiO2 has the highest photocatalytic reactivity. ► Hetero-junction in brookite/anatase composite benefits the charge separation. ► Schottky barrier between Ag0 and TiO2 further improved the charge separation.
Co-reporter:Guo-Dong Chen;Zhi-Dan Tian;Ling-Zhi Wang
Research on Chemical Intermediates 2011 Volume 37( Issue 8) pp:891-899
Publication Date(Web):2011 October
DOI:10.1007/s11164-011-0297-8
The fluorescent dye molecules, 4-piperidine-1,8-naphthalimide, were successfully fixed into the amino modified pore channel of mesoporous MCM-41 type materials by in situ reaction of 4-piperidinyl-1,8-naphthalic anhydride with the amino group. The formation of amide bonds on the pore surface was verified by infrared spectra. The maximum fluorescence emission peak of this hybrid material has a red shift of 13 nm compared to that of a naphthalimide derivative in ethanol solution. Moreover, the fluorescence intensity of dye molecules grafted into Ce-doped MCM-41 is higher than that in pure silica MCM-41. This phenomenon is attributed to the inhibited internal electron transfer from piperidine to naphthalimide groups by Ce4+, thus improving the fluorescence intensity of the naphthalimide group. The unique fluorescence behavior of the 1,8-naphthalimide derivative doped hybrid mesoporous material makes it a good candidate for the metal ions microdetection.
Co-reporter:Yuanlin Liu;Lingzhi Wang;Jinlong Zhang;Feng Chen
Research on Chemical Intermediates 2011 Volume 37( Issue 8) pp:949-959
Publication Date(Web):2011 October
DOI:10.1007/s11164-011-0302-2
Macroporous microspheres of SAPO-34 (MAMISAPO-34) were fabricated using polystyrene spheres (PS, 2 μm) as hard template. Cubic SAPO-34 (1 μm) synthesized by the conventional hydrothermal method was mixed with kaolin, silica sol, aluminium phosphate sol, template, and deionized water. Spray drying was then performed to prepare 30–50 μm microspheres which were converted to macroporous SAPO-34 by post-hydrothermal and calcination treatments. For comparison, 30–50 μm non-macroporous microspheres (NOMISAPO-34) were also obtained without using PS. XRD, NH3-TPD, and SEM analyses were used to characterize the macroporous and non-macroporous SAPO-34. The results showed that MAMISAPO-34 was more crystalline and had more strong acid sites than NOMISAPO-34. When used in MTO (methanol to olefins) reactions, MAMISAPO-34 had better catalytic performance than NOMISAPO-34, because of its greater crystallinity.
Co-reporter:Juying Lei, Lingzhi Wang, and Jinlong Zhang
ACS Nano 2011 Volume 5(Issue 5) pp:3447
Publication Date(Web):March 29, 2011
DOI:10.1021/nn103254g
A novel kind of monodisperse core−shell silica nanosphere composed of a fluorescent solid core and a mesoporous shell has been successfully fabricated. These nanospheres exhibit multifluorescent signals under a single-wavelength excitation as a result of the solid silica core that is doped with three kinds of dyes and that can produce effective fluorescence resonance energy transfer. The fluorescent signal of a single nanosphere is about 700 times brighter than its constituent fluorophores. X-ray diffraction, transmission electron microscopy, and N2 adsorption−desorption isotherms reveal that these nanospheres possess abundant mesopores in the shell. Combining the advantages of extremely bright multifluorescent signals excited with a single wavelength and an abundant mesoporous system, this core−shell silica nanosphere is designed for the simultaneous monitoring of fluorescence of in vivo multiple-target drug transport. Experiments on drug loading and release in addition to studies on cell uptake reveal that these nanospheres not only show good drug storage and sustained release capacity but also demonstrate biocompatibility and mutlifluorescent labeling capacity for biological systems.Keywords: core−shell nanoparticles; mesoporous silica; multifluorescence; transport carrier
Co-reporter:Jinlong Zhang, Yongmei Wu, Mingyang Xing, Sajjad Ahmed Khan Leghari and Shamaila Sajjad
Energy & Environmental Science 2010 vol. 3(Issue 6) pp:715-726
Publication Date(Web):17 May 2010
DOI:10.1039/B927575D
This paper presents a critical review of novel achievements in the modification of N–TiO2 photocatalytic systems aimed at enhancing TiO2 applications in the areas of energy conversion and environmental clean-up. Herein we studied the synthesis, physical properties, as well as synergism of modified N-doped TiO2. Based on the studies reported in the literature, metal, nonmetal and metal oxide modified N–TiO2 are very effective systems to extend the activating spectra to the visible range. Therefore, modified N–TiO2 play an important role in the development of efficient photocatalysts for future perspectives.
Co-reporter:Mingyang Xing, Yongmei Wu, Jinlong Zhang and Feng Chen
Nanoscale 2010 vol. 2(Issue 7) pp:1233-1239
Publication Date(Web):18 May 2010
DOI:10.1039/C0NR00078G
Single doped, co-doped and tri-doped TiO2 with B, N and Fe are successfully synthesized by using the hydrothermal method. The samples are characterized by X-ray diffraction (XRD), UV-vis diffuse reflectance spectroscopy (DRS), and X-ray photoelectron spectroscopy (XPS). The photocatalytic activities of the samples are evaluated for degradation of methyl-orange (MO, 20 mg L−1) in aqueous solutions under visible light (λ > 420 nm). The results of XRD suggest that all the catalysts present anatase crystal. All the doping catalysts show higher photoactivities than pure TiO2 under visible light irradiation. In the single nonmetal doped TiO2, the localized dopant levels near the valence band (VB) are responsible for the enhancement of photoactivies. Fe3+ impurity level formed under the conduction band (CB) induces the high photocatalytic activities of iron doped TiO2. In the co-doped and tri-doped catalysts, the B 2p and N 2p acceptor states contribute to the band gap narrowing by mixing with O 2p states combined with the overlapping of the conduction band by the iron “d” orbital, resulting in improvement of the photo-performance under visible light irradiation. Iron co-doped with boron catalyst shows low photoactivity under visible light due to the absence of Fe3+ impurity levels at the bottom of the conduction band. In addition, the XPS results indicate the presence of synergistic effects in co-doped and tri-doped catalysts, which contribute to the enhancement of photocatalytic activities.
Co-reporter:Juying Lei, Lingzhi Wang and Jinlong Zhang
Chemical Communications 2010 vol. 46(Issue 44) pp:8445-8447
Publication Date(Web):01 Oct 2010
DOI:10.1039/C0CC03310C
Incorporation of a dual-FRET dye pair into mesoporous silica nanoparticles yields sensitive and sensing-range tunable nanosensors with good reversibility that can be used for ratiometric pH measurements under a single-wavelength excitation.
Co-reporter:Lin Jiang, Lingzhi Wang and Jinlong Zhang
Chemical Communications 2010 vol. 46(Issue 42) pp:8067-8069
Publication Date(Web):24 Sep 2010
DOI:10.1039/C0CC01646B
Bi2WO6 nanoparticles loaded on a spherical MCM-48 mesoporous molecular sieve with a high photocatalytic activity in the visible-light range was synthesized for the first time using a facile one-step process.
Co-reporter:Chenxu He, Baozhu Tian, Jinlong Zhang
Journal of Colloid and Interface Science 2010 Volume 344(Issue 2) pp:382-389
Publication Date(Web):15 April 2010
DOI:10.1016/j.jcis.2010.01.002
A thermally stable SiO2-doped mesoporous TiO2 with high crystallinity was prepared by a templating method. The content of SiO2 dopant was varied from 3% to 20%. The gels were characterized by TG-DTA analysis. And the resultant catalysts were investigated by various physicochemical techniques, such as WAXRD, Raman spectroscopy, N2 adsorption–desorption, TEM, FT-IR, and XPS. The WAXRD, TEM, and Raman measurements suggest that the SiO2 dopant can enhance the thermal stability of the anatase phase remarkably. Rutile phase did not present at all even at 1000 °C when the SiO2 content was up to 15%. N2 adsorption–desorption results show that the SiO2-doped samples have uniform pore diameters and large specific surface area, which is beneficial for photocatalytic reaction. The photocatalytic activities of the samples were evaluated by degradation of Rhodamin-6G solution under UV irradiation. The results show that the SiO2-doped mesoporous TiO2 have better activity than commercial P25. Especially, the 15% SiO2-doped mesoporous TiO2 exhibited much higher photocatalytic activity than P25 in a large range of calcination temperatures, even at 900 °C. The excellent photocatalytic activity of the samples can be attributed to the high anatase crystallinity, large specific surface area, preserved surface hydroxyl groups and mesoporous channels.Mesoporous SiO2-doped TiO2 with large surface area was prepared, which exhibited much higher photocatalytic activity than P25 in a large range of calcination temperatures, even at 900 °C.
Co-reporter:Yongmei Wu, Jinlong Zhang, Ling Xiao, Feng Chen
Applied Surface Science 2010 Volume 256(Issue 13) pp:4260-4268
Publication Date(Web):15 April 2010
DOI:10.1016/j.apsusc.2010.02.012
Abstract
The nanoparticles of TiO2 modified with carbon and iron were synthesized by sol–gel followed solvothermal method at low temperature. Its chemical composition and optical absorption were investigated by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), photoluminescence emission spectroscopy (PL), UV–vis absorption spectroscopy, and electron paramagnetic resonance (EPR). It was found that carbon and iron modification causes the absorption edge of TiO2 to shift the visible light region. Fe(III) cation could be doped into the matrix of TiO2, by which could hinder the recombination rate of excited electrons/holes. Superior photocatalytic activity of TiO2 modified with carbon and iron was observed for the decomposition of acid orange 7 (AO7) under visible light irradiation. The synergistic effects of carbon and iron in modified TiO2 nanoparticles were responsible for improving visible light photocatalytic activity.
Co-reporter:Guodong Chen, Lin Jiang, Lingzhi Wang, Jinlong Zhang
Microporous and Mesoporous Materials 2010 Volume 134(1–3) pp:189-194
Publication Date(Web):October 2010
DOI:10.1016/j.micromeso.2010.05.025
Mesoporous ZSM-5 was synthesized by using dual templates and one step hydrothermal crystallization method under alkali conditions. Mesopores were created by using cetyltrimethylammonium bromide (CTAB) as the template and the crystallized pore wall framework was formed by using tetrapropylammonium bromide (TPAB) as the template. The specific influences of the polyethylene glycol (PEG) and ammonium fluoride (NH4F) addition, hydrothermal crystallization temperature, TPAB/Si and Al/Si ratio to the mesostructure and crystallinity of the obtained samples were carefully studied. In this system, PEG plays an important role in the maintenance of the mesoporous pore ordering and the zeolite crystallinity. Moreover, the study on the hydrothermal stability of the sample with best mesoporous pore ordering and zeolite crystallinity showed this kind mesoporous zeolite has extremely high hydrothermal stability in boiling water.
Co-reporter:Weiwei Zou, Jinlong Zhang, Feng Chen
Materials Letters 2010 Volume 64(Issue 15) pp:1710-1712
Publication Date(Web):15 August 2010
DOI:10.1016/j.matlet.2010.05.008
DDAT(S-1-Dodecyl-S′-(α, α′-dimethyl-α″-acetic acid) trithiocarbonate) modified TiO2 photocatalysts were prepared by hydrothermal treatment before TiO2 crystallization. The adsorption of DDAT onto the surface of titania nanoparticles led the shifting of the onset wavelength of the optical absorption in the visible range corresponding to ligand-to-metal charge transfer transition within the surface-modified complex. The interaction of TiO2 nanoparticles with DDAT was investigated by infrared spectra. The XRD indicated that the modification process could not influence the crystallite phase of TiO2. The photocatalytic studies suggested that the DDAT modified TiO2 photocatalysts showed enhanced photocatalytic efficiency of photodegradation of 2,4-dichlorophenol compared with the as-prepared TiO2 under visible-light irradiation.
Co-reporter:Pengfei Ji;Lingzhi Wang;Dr. Feng Chen;Dr. Jinlong Zhang
ChemCatChem 2010 Volume 2( Issue 12) pp:1552-1554
Publication Date(Web):
DOI:10.1002/cctc.201000191
Co-reporter:Sajjad Shamaila, Ahmed Khan Leghari Sajjad, Feng Chen, Jinlong Zhang
Materials Research Bulletin 2010 45(10) pp: 1375-1382
Publication Date(Web):
DOI:10.1016/j.materresbull.2010.06.047
Co-reporter:Shamaila Sajjad;Sajjad A. K. Leghari;Dr. Feng Chen;Dr. Jinlong Zhang
Chemistry - A European Journal 2010 Volume 16( Issue 46) pp:13795-13804
Publication Date(Web):
DOI:10.1002/chem.201001099
Abstract
A controllable and reproducible synthesis of highly ordered two-dimensional hexagonal mesoporous, crystalline bismuth-doped TiO2 nanocomposites with variable Bi ratios is reported here. Analyses by transmission electron microscopy, X-ray diffraction, Raman, and X-ray photoelectron spectroscopy reveal that the well-ordered mesostructure is doped with Bi, which exists as Bi3+ and Bi(3+x+). The Bi-doped mesoporous TiO2 (ms-TiO2) samples exhibit improved photocatalytic activities for simultaneous phenol oxidation and chromium reduction in aqueous suspension under visible and UV light over the pure ms-TiO2, P-25, and conventional Bi-doped titania. The high catalytic activity is due to both the unique structural characteristics and the Bi doping. This new material extends the spectral response from UV to the visible region, and reduces electron–hole recombination, which renders the 2.0 % Bi-doped ms-TiO2 photocatalyst highly responsive to visible light.
Co-reporter:Xiaona Lu, Baozhu Tian, Feng Chen, Jinlong Zhang
Thin Solid Films 2010 Volume 519(Issue 1) pp:111-116
Publication Date(Web):29 October 2010
DOI:10.1016/j.tsf.2010.07.071
A series of uniform and transparent boron-doped TiO2 films were synthesized from autoclaved-sol without organic solvent at low temperature. As-prepared B-TiO2 films with two layers were characterized by XRD, DRS, XPS and AFM. The photocatalytic characteristics were measured based on the degradation of Rhodamine B (RhB) solution under visible or UV light. The results indicated that the anatase phase was the main crystal form of the films, containing a small amount of brookite. The presence of boron caused a red shift in the absorption band of TiO2 films. The doped boron was mainly presented in the form of B2O3, O–Ti–B and O–Ti–B bonds, confirming that autoclaved-sol synthesis at low temperature allowed for incorporation of boron atoms into the TiO2 matrix. Transmission of the films was about 90% in the visible region. The 10% (atom) B-TiO2 film exhibited the best photocatalytic activity both in visible and UV light.
Co-reporter:Xiao-Li Yuan;Masakazu Anpo
Research on Chemical Intermediates 2010 Volume 36( Issue 1) pp:83-93
Publication Date(Web):2010 January
DOI:10.1007/s11164-010-0117-6
Fe3+ doped mesoporous TiO2 with ordered mesoporous structure were successfully prepared by the solvent evaporation-induced self-assembly process using P123 as soft template. The properties and structure of Fe3+ doped mesoporous TiO2 were characterized by means of XRD, EPR, BET, TEM, and UV–vis absorption spectra. The characteristic results clearly show that the amount of Fe3+ dopant affects the mesoporous structure as well as the visible light absorption of the catalysts. The photocatalytic activity of the prepared mesoporous TiO2 was evaluated from an analysis of the photodegradation of methyl orange under visible light irradiation. The results indicate that the sample of 0.50%Fe–MTiO2 exhibits the highest visible light photocatalytic activity compared with other catalysts.
Co-reporter:Wenjiao Wang;Jinlong Zhang;Feng Chen;Masakazu Anpo
Research on Chemical Intermediates 2010 Volume 36( Issue 2) pp:163-172
Publication Date(Web):2010 March
DOI:10.1007/s11164-010-0130-9
Ag nanoparticles encapsulated by TiO2 shells have the ability to catalyze redox reactions on their surface. By continually monitoring by use of UV–visible spectroscopy it was found that the surface charge of both TiO2-coated and uncoated colloidal silver particles changed after chemical electron injection. The charging and discharging process of Ag@TiO2 vary, depending on the different Ag content of the core–shell nanoparticles. In order to enhance the stability of Ag@TiO2 colloids, Fe3+ was doped into the lattice of the TiO2 shells. The experimental results showed that the Fe3+ ions have the capacity to store and transfer electrons. Furthermore, the charging and discharging rate can be controlled by changing the thickness of the TiO2 shells, because they are limited by the diffusion distance of electrons through the TiO2 shells.
Co-reporter:Chenxu He;Baozhu Tian;Jinlong Zhang
Research on Chemical Intermediates 2010 Volume 36( Issue 4) pp:349-359
Publication Date(Web):2010 June
DOI:10.1007/s11164-010-0145-2
N, B, Si-tridoped mesoporous TiO2, together with N-doped, N, B-codoped and N, Si-codoped TiO2, was prepared by a modified sol–gel method. The samples were characterized by wide-angle X-ray diffraction (WAXRD), N2 adsorption–desorption, transmission electron microscopy (TEM), Fourier transform infrared (FT-IR) spectroscopy, UV–visible adsorbance spectra (UV–vis) and X-ray photoelectron spectra (XPS). The N, B, Si-tridoped mesoporous TiO2 showed small crystallite size, large specific surface area (350 m2/g), uniform pore distribution (3.2 nm) and strong absorption in the visible light region. The photocatalytic activities of the samples were evaluated by the photodegradation of 2,4-dichlorophenol (2,4-DCP) aqueous solution. The N, B, Si-tridoping sample exhibited much higher photocatalytic activity compared with other synthesized photocatalysts. The high activity could be attributed to the strong absorption in the visible light region, large specific surface area, small crystallite size, large amount of surface hydroxyl groups, and mesoporosity.
Co-reporter:Lingzhi Wang, Juying Lei and Jinlong Zhang
Chemical Communications 2009 (Issue 16) pp:2195-2197
Publication Date(Web):02 Mar 2009
DOI:10.1039/B900200F
Bright and colourful nanocomposites are easily fabricated by doping and fixing one or two kinds of oligosilicate fluorescent dots encapsulated with dye molecules into the pore channels of mesoporous silica nanoparticles, which can engender abundant fluorescent signals with a single excitation wavelength.
Co-reporter:Guodong Chen, Lingzhi Wang, Jinlong Zhang, Feng Chen, Masakazu Anpo
Dyes and Pigments 2009 Volume 81(Issue 2) pp:119-123
Publication Date(Web):May 2009
DOI:10.1016/j.dyepig.2008.09.013
4-Piperazinyl-N-methyl-1,8-naphthalimide (PMN) was synthesized and encapsulated into mesoporous molecular sieves. The fluorescent emission spectra and fluorescence decay of PMN/M-MCM-41 (where M = Si, Ce, Al) were used to investigate the photophysical properties of the hybrid composites. The emission intensity of 4-piperazinyl-N-methyl-1,8-naphthalimide can be increased by decreasing the pH environment of the hybrid composites; the emission intensity varied with different MCM-41 hosts in the order: PMN/Al-MCM-41 > PMN/Si-MCM-41 > PMN/Ce-MCM-41; the fluorescence lifetime of PMN molecules followed the same order. The reasons for the improved fluorescence intensity and the prolonged lifetime of PMN in a low pH environment and Al-MCM-41 are discussed.
Co-reporter:Guodong Chen, Lingzhi Wang, Juying Lei, Jinlong Zhang
Microporous and Mesoporous Materials 2009 Volume 124(1–3) pp:204-209
Publication Date(Web):August–September 2009
DOI:10.1016/j.micromeso.2009.05.011
Co-reporter:Lingzhi Wang, Jinlong Zhang, Feng Chen
Microporous and Mesoporous Materials 2009 Volume 122(1–3) pp:229-233
Publication Date(Web):1 June 2009
DOI:10.1016/j.micromeso.2009.03.004
The hydrothermally stable MCM-48 mesoporous molecular sieve was successfully prepared at extremely low cost of cetyltrimethylammonium bromide (CTAB) by carefully adjusting the synthesis conditions. The increasing of the crystallization temperature from 373 K to 423 K can dramatically reduce the CTAB surfactant amount for the preparation of MCM-48 from 0.65 to 0.1 of the CTAB/Si ratio. The effect of increasing crystallization temperature on the formation process of MCM-48 at low CTAB cost was carefully studied. The influences of OH−/Si ratio and fluoride addition to the structure stability of the MCM-48 material synthesized at CTAB/Si = 0.1 and 423 K were systematically studied by XRD patterns. Moreover, the combination of increasing crystallization temperature and adding small amount of fluoride ions can considerably improve the structure stability of MCM-48 when reducing the CTAB cost.
Co-reporter:Chenxu He, Baozhu Tian, Jinlong Zhang
Microporous and Mesoporous Materials 2009 Volume 126(1–2) pp:50-57
Publication Date(Web):November 2009
DOI:10.1016/j.micromeso.2009.05.019
Highly ordered bicontinuous cubic mesoporous titania–silica binary oxides were synthesized via evaporation-induced self-assembly (EISA) method. X-ray diffraction (XRD), fourier transform infrared spectra (FT-IR), transmission electron microscopy (TEM), BET surface area and BJH pore-size distribution have been used to determine the mesostructrues and properties of the samples. The resultant materials are thermally stable (up to 600 °C), and show high surface areas (110–234 m2/g), uniform pore diameters (∼3.3 nm). And the pore wall framework is composed of anatase and minor rutile phases. The effects of acidity, water content in sol and heat treatment temperature on the formation and thermal stability of mesoporous structures were investigated. Photodegradation of Rhodamine B (RhB) under UV light irradiation shows that the sample has a comparable photocatalytic activity with Degussa P25, and higher activity than pure TiO2.
Co-reporter:Hongyuan Hao, Jinlong Zhang
Microporous and Mesoporous Materials 2009 Volume 121(1–3) pp:52-57
Publication Date(Web):1 May 2009
DOI:10.1016/j.micromeso.2009.01.002
The iron (III) and nitrogen co-doped mesoporous titania was prepared in the first time by modified sol–gel method, in which, the nitrogen-containing surfactant (dodecylamine) was introduced as a structure directing agent as well as a nitrogen dopant. The mesoporous materials were characterized by low angle and wide angle X-ray diffraction (XRD), N2 adsorption–desorption, UV–visible diffuse reflectance spectroscopy, transmission electron microscopy (TEM), X-band electron paramagnetic resonance (EPR), and X-ray photoelectron spectra (XPS). Characteristic results clearly show that the mesoporous architecture of nitrogen and Fe (III) co-doped TiO2 is composed of mixed-phase crystal textures of anatase and brookite. And the prepared sample has a larger specific area, small crystal size and an uniform pore distribution even after calcined 400 °C. The photocatalytic activity of samples was evaluated by the photodegradation of 2,4-dichlorophenol in solution under visible light irradiation. It was found that the photocatalytic activity of co-doped mesoporous TiO2 powders was higher than that of N-doped mesoporous TiO2 sample and P25.
Co-reporter:Hongyuan Hao, Jinlong Zhang
Materials Letters 2009 Volume 63(Issue 1) pp:106-108
Publication Date(Web):15 January 2009
DOI:10.1016/j.matlet.2008.09.020
Co-reporter:Zhimang Shao, Baozhu Tian, Jinlong Zhang
Materials Letters 2009 Volume 63(Issue 20) pp:1705-1708
Publication Date(Web):15 August 2009
DOI:10.1016/j.matlet.2009.05.019
To improve the photocatalytic activity of TiO2 on decomposing anionic surfactants, MgO-coated mesoporous TiO2 was fabricated by evaporation induced self-assembly (EISA) combined with impregnation method. MgO was uniformly dispersed on the surface of TiO2, which played the role of stabilizing the ordered mesostructure of TiO2 and improving the adsorption of anion surfactants, while inhibiting the crystallization of TiO2. The powders coated with 5 wt.% MgO showed the highest photocatalytic activity for the decomposition of sodium dodecylbenzenesulfonate-6 (DBS).
Co-reporter:Hong-Yuan Hao;Chen-Xu He;Bao-Zhu Tian
Research on Chemical Intermediates 2009 Volume 35( Issue 6-7) pp:
Publication Date(Web):2009 September
DOI:10.1007/s11164-009-0092-y
Mesoporous nanocrystalline Cd-doped titania was firstly prepared at low temperature by a modified sol–gel method, using dodecylamine as a template. The template could be easily removed by refluxing samples in nitric acid ethanol solution. The Fourier transform infrared spectrometer (FT-IR), low-angle and wide-angle X-ray diffraction (XRD), N2 adsorption–desorption, transmission electron microscopy (TEM), X-ray photoelectron spectra (XPS), and UV–visible diffuse reflectance spectroscopy were used for the characterization of catalysts. The characteristic results clearly showed that Cd2+ ions were doped into the titania lattice, and the mesoporous architecture of Cd-doped TiO2 was composed of mixed-phase crystal textures of anatase and brookite. The samples displayed high visible-light photocatalytic activity for photodegradating 2,4-dichlorophenol (2,4-DCP) solution. The high activities of samples were attributed to the bicrystalline framework, large BET surface area, small crystallite size, and Cd-doping.
Co-reporter:Weiwei Zou;Feng Chen;Masakazu Anpo
Research on Chemical Intermediates 2009 Volume 35( Issue 6-7) pp:
Publication Date(Web):2009 September
DOI:10.1007/s11164-009-0093-x
The surface of titanium dioxide nanoparticles has been chemically modified with toluene 2,4-di-isocyanate (TDI). The modified titanium dioxide can efficiently absorb visible irradiation. The samples were characterized by means of wide-angle X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FT-IR), diffuse reflectance UV–Vis spectroscopy (DRS), X-ray photoelectron spectroscopy (XPS), and thermogravimetric analysis (TGA). The as-prepared photocatalyst exhibited good photostability and photocatalytic performance in the degradation of organic compounds. For model organic pollutants, modified titanium dioxide had excellent visible-light photocatalytic performance and the surface chemistry linkage product had high photostability.
Co-reporter:Xiao-Li Yuan;Bao-Zhu Tian
Research on Chemical Intermediates 2009 Volume 35( Issue 6-7) pp:693-703
Publication Date(Web):2009 September
DOI:10.1007/s11164-009-0095-8
A simple synthetic method was employed to prepare mesoporous titania with anatase crystalline walls and high photocatalytic activity. The properties and structures of mesoporous titania were characterized by means of low angle and wide angle X-ray diffraction (XRD), Fourier transform (FT)-IR spectra, transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), and N2 adsorption–desorption. The characteristic results clearly show that crystallization rate of the mesoporous titania affects the stability of the mesoporous structure after reflux, and that the anatase crystal in the mesoporous wall of mesoporous titania can stabilize the mesoporous structure. The photocatalytic activity of titania powder was evaluated from an analysis of the photodegradation of methyl orange under UV irradiation. The results indicate that the titania powder with mesoporous structure shows the highest photocatalytic activity.
Co-reporter:Mingyang Xing, Jinlong Zhang and Feng Chen
The Journal of Physical Chemistry C 2009 Volume 113(Issue 29) pp:12848-12853
Publication Date(Web):June 15, 2009
DOI:10.1021/jp9034166
A simple method to prepare the N−TiO2 adsorbed with Fe3+ ions only on the surface of catalysts and modify the catalysts by a redox treatment (NaBH4 reduction and air oxidation treatment) was proposed. The samples were characterized by X-ray diffraction (XRD), UV−vis diffuse reflectance spectroscopy, FTIR, X-ray photoelectron spectroscopy (XPS), and high-resolution transmission electron micrograph (HRTEM). The photocatalytic activities of the samples were evaluated for degradation of methylene blue (MB) in aqueous solutions under visible light (λ > 420 nm). The results of XRD, FTIR, XPS, and HRTEM analysis indicated that the structure of Fe compounds changed from Fe2O3 to γ-FeOOH after redox treatment. Compared to N−TiO2 with Fe3+ ions, the catalysts after redox treatment showed higher photoactivity under visible light, and the formation of γ-FeOOH was responsible for the improvement of photocatalytic activity. Furthermore, to the catalysts after redox treatment, the mechanism for degradation of MB under visible light is an opening of a central aromatic ring attacked by OH• combined with a process of γ-FeOOH photoreductive dissolution.
Co-reporter:Yongmei Wu, Haibei Liu, Jinlong Zhang and Feng Chen
The Journal of Physical Chemistry C 2009 Volume 113(Issue 33) pp:14689-14695
Publication Date(Web):July 2, 2009
DOI:10.1021/jp904465d
N-doped TiO2 deposited with Au (Au/N−TiO2) was successfully prepared via hydrolysis of titanium sulfate and ammonia followed with a Au deposition−precipitation method. The resulting samples were characterized by X-ray diffraction (XRD), atomic absorption flame emission spectroscopy (AAS), UV−vis absorbance spectroscopy, X-ray photoelectron spectroscopy (XPS), N2 physical adsorption, high-resolution transmission electron microscopy (HRTEM), and photoluminescence (PL) spectra. The photocatalytic activities of the samples were evaluated for degradation of methyl orange (MO) under visible light and UV light irradiation. It was found that the Au/N−TiO2 samples presented much higher photocatalytic activity than N-doped TiO2 under both UV and visible light irradiation. Diffuse reflectance UV−vis spectra showed an extension of light absorption into the visible region for Au/N−TiO2, and PL analysis of the sample indicated that the electron−hole recombination has been effectively inhibited after Au particles deposition. XPS analysis displayed Au existing as Au0 on the surface of the N−TiO2 photocatalyst and nitrogen species in the form of N−Ti−O and Ti−O−N. The excellent photoactivities of Au/N−TiO2 compared with N-doped TiO2 could be explained by its appropriate Au particle sizes and cooperation effect between N species and metallic Au particles.
Co-reporter:Wenjiao Wang, Jinlong Zhang, Feng Chen, Dannong He, Masakazu Anpo
Journal of Colloid and Interface Science 2008 Volume 323(Issue 1) pp:182-186
Publication Date(Web):1 July 2008
DOI:10.1016/j.jcis.2008.03.043
Ag@TiO2 core–shell-type nanophotocatalysts have been prepared using a simple and convenient method. The products were characterized by TEM, XRD, and UV–vis spectra. To make the catalysts achieve the highest photocatalytic activity under UV light illumination, the Ag content of Ag@TiO2 was optimized. The results showed that Ag@TiO2-doped Fe3+ extend their absorption into the visible region. Among the Fe3+-doped samples, Ag@Fe–TiO2 with low Ag content showed higher photocatalytic activity under visible light illumination. An excessive added amount of Ag would reduce Fe3+ to Fe2+ and make them difficult to be incorporated into the lattice of titania. From the experiments, we found that Fe3+ ions could stabilize the Ag@TiO2 colloid by holding back the aggregation of the core–shell nanoparticles.Acting as an electron trap, the Ag core is protected by a TiO2 shell from corrosion or dissolution. Fe3+ doped on the Ag@TiO2 system can enhance the photocatalytic activity under visible light illumination.
Co-reporter:Yaofeng Shao, Lingzhi Wang, Jinlong Zhang, Masakazu Anpo
Microporous and Mesoporous Materials 2008 Volume 109(1–3) pp:271-277
Publication Date(Web):1 March 2008
DOI:10.1016/j.micromeso.2007.05.001
The hydrothermal stability of Cr-containing MCM-48 in boiling water was found to be higher than that of the pure silica MCM-48, which was first improved with the increasing Cr content at low Si/Cr ratio, then went to the maxima at Si/Cr = 50, and finally instead decreases with the increasing Si/Cr ratio. The Cr-MCM-48 sample synthesized at Si/Cr = 50 maintained their mesoporous structure after refluxing in boiling water for 36 h. The results of diffuse reflectance UV–vis and ESR spectra showed that the calcined Cr-MCM-48 contains Cr(V) and Cr(VI) at low Cr content. Chromium is present as Cr(V), Cr(VI) and Cr(III) species at the rich Cr content. Both of the Cr positioned on the surface of pore walls and in the framework provide the protection against water attack.
Co-reporter:Guodong Chen, Lingzhi Wang, Feng Chen, Jinlong Zhang, Mazakazu Anpo
Materials Letters 2008 Volume 62(Issue 27) pp:4245-4247
Publication Date(Web):31 October 2008
DOI:10.1016/j.matlet.2008.07.018
Mesoporous silica was synthesized by modified nonionic organosilicon surfactant under acidic condition for the first time. The XRD patterns, HRTEM image and corresponding BET characterization show that it has ordered 2-D hexagonal pore channel and ultra thick pore wall (about 6 nm). The calcination can result in the vanishment of organic composite and the linkage of the hydrolyzed silica source and the hydrophobic chain (polymethylsiloxane) of the silica-based template. Hence this recombination process tremendously enhances the pore wall of the resulting mesoporous material and causes a certain amount of micropores in the wall. The resulted mesoporous material has high hydrothermal stability due to its ultra thick pore wall and hydrophobic surface.
Co-reporter:Lingzhi Wang;Yaofeng Shao;Jinlong Zhang
Research on Chemical Intermediates 2008 Volume 34( Issue 2-3) pp:267-286
Publication Date(Web):2008 February
DOI:10.1163/156856708783623500
This is a review of our recent reports about improving the hydrothermal stability of MCM-48 mesoporous molecular sieves and the related works done by other groups. It presents the different effects of direct addition of various anions, including F−, SO42−, NO3− and Cl−, on the improvement of the hydrothermal stability of MCM-48. The different effects of anions on the improvement of the hydrothermal stability and the critical factors influencing the formation of hydrothermally stable MCM-48 are also explained by careful analysis and discussion.
Co-reporter:Baoping Zhang;Jinlong Zhang;Feng Chen
Research on Chemical Intermediates 2008 Volume 34( Issue 4) pp:375-380
Publication Date(Web):2008 April
DOI:10.1163/156856708784040669
A magnetic TiO2/ZnFe2O4 photocatalyst was prepared by a sol-gel method, and X-ray diffraction (XRD), magnetic and photocatalytic properties analysis were employed to characterize this photocatalyst. The XRD results show that ZnFe2O4 can prevent the transformation of titania from anatase to rutile. The magnetic properties analysis indicates that TiO2/ZnFe2O4 is of large saturation magnetization value and low coercivity. The photocatalytic experimental results show that TiO2/ZnFe2O4=3 and 4 are superior in photocatalytic reactivity to other proportions. TEM shows that TiO2/ZnFe2O4 has a fine core-shell fabric. After being used for four times during the photocatalytic reaction, the TiO2/ZnFe2O4 nanoparticles have good photocatalytic stability.
Co-reporter:Pengfei Ji, Jinlong Zhang, Feng Chen and Masakazu Anpo
The Journal of Physical Chemistry C 2008 Volume 112(Issue 46) pp:17809-17813
Publication Date(Web):2017-2-22
DOI:10.1021/jp8054087
Ordered nanocrystalline mesoporous cerium oxide was successfully synthesized using MCM-48 molecular sieves as a hard template. The long-range ordered mesostructure was characterized by low-angle and wide-angle X-ray diffraction (XRD), N2 adsorption−desorption technique, and transmission electron microscopy (TEM), and the obtained cerium oxide exhibited high similarity to the cubic Ia3d symmetry of the silica template. Due to smaller crystal size, the mesoporous materials have a blue shift in light absorption as compared with nonporous materials. X-ray photoelectron spectrum (XPS) and energy-dispersive X-ray spectrum (EDS) patterns confirm that mesoporous materials possess more surface vacancies than bulk CeO2. Photocatalytic degradation of azodye acid orange 7 under visible light illumination was used as a catalytic test reaction. The activity of mesoporous product in dye decolorization is substantially higher than those for a nonporous sample and TiO2 P25.
Co-reporter:Tianzhong Tong, Jinlong Zhang, Baozhu Tian, Feng Chen, Dannong He, Masakazu Anpo
Journal of Colloid and Interface Science 2007 Volume 315(Issue 1) pp:382-388
Publication Date(Web):1 November 2007
DOI:10.1016/j.jcis.2007.06.051
The Ce–TiO2 catalysts were prepared by controlled hydrolysis of Ti(OC4H9)4 with water generated “in situ” via an esterification reaction between acetic acid and ethanol, followed by hydrothermal treatment. The samples were characterized by X-ray diffraction (XRD), UV–vis diffuse reflectance spectroscopy (DRS), scanning electron microscopy (SEM), atomic absorption flame emission spectroscopy (AAS), and nitrogen adsorption–desorption methods. Both of undoped TiO2 and Ce–TiO2 samples exclusively consist of primary anatase crystallites, which further form spherical aggregates with diameters ranging from 100 to 500 nm. The photocatalytic activity of Ce–TiO2 was investigated for the photocatalytic degradation of Rhodamine B (RB) aqueous solution both under UV and visible light irradiation. Doping of Ce4+ effectively improves the photocatalytic activity under both UV light irradiation and visible light irradiation with an optimal doping concentration of 0.2 and 0.4%, respectively. The photocatalytic mechanisms of Ce–TiO2 catalysts were tentatively discussed.
Co-reporter:Yulong Li, Bin He, Jinlong Zhang
Dyes and Pigments 2007 Volume 75(Issue 1) pp:111-115
Publication Date(Web):2007
DOI:10.1016/j.dyepig.2006.05.026
A series of novel 9-(4-substituted)phenoxy-naphthaceno[5,6-bc]pyran-2,8-diones were synthesized and their structures were confirmed using elemental analysis and the IR, 1H NMR and MS spectra. The photochromism of these compounds was observed in DMSO, DMF, CH2Cl2, CHCl3, benzene and toluene. The trans forms had an absorption maximum in the range of 419–422 nm, while the ana forms had two large absorption maxima in the ranges 489–492 nm and 524–526 nm. The λmax and isosbestic points were affected little by the electronic properties of the substituents on the phenoxy group. However, the formation of the photostationary state was strongly influenced by the polarity of the substituents.
Co-reporter:Baozhu Tian, Tianzhong Tong, Feng Chen, Jinlong Zhang
Acta Physico-Chimica Sinica 2007 Volume 23(Issue 7) pp:978-982
Publication Date(Web):July 2007
DOI:10.1016/S1872-1508(07)60052-7
By using Au(S2O3)23– as the gold precursor, Au/TiO2 photocatalysts were prepared by water washing (W) and rotary evaporation (E) processes, respectively. The samples were characterized by UV-Vis diffuse reflectance spectroscopy (DRS), X-ray diffraction (XRD), transmission electron microscopy (TEM), and atomic absorption flame emission spectroscopy (AAS). The photocatalytic activity of the samples was evaluated from the analysis of the photodegradation of methyl orange (MO). By using the water washing treatment, well-dispersed gold nanoparticles with the diameter of 2–5 nm were formed on the surface of TiO2, whereas only the gold coating was formed for rotary evaporation processes. The photocatalytic activity of Au/TiO2 photocatalysts is related to the preparation process. With a similar gold loading, the photocatalysts prepared by water washing showed higher photocatalytic activity compared to the catalysts prepared by rotary evaporation.
Co-reporter:Li Han;Min-Zhao Xue;Da-Pu Wang;Yan-Gang Liu
Research on Chemical Intermediates 2007 Volume 33( Issue 7) pp:589-597
Publication Date(Web):2007 July
DOI:10.1163/156856707781749928
In this paper, the ESR and photoluminescence (PL) of BaFCl and BaFCl:Eu2+ radiated or un-radiated by X-ray were observed. The single electron in the color center could be produced in BaFCl without Eu2+. A series of traps of different energy level in BaFCl lattice were formed, and some shallow traps of them could be bleached by Vis-light, and the other deep traps could not. The bleaching effects on ESR and photostimulated luminescence (PSL) were investigated. An F-H-Eu2+ complex (F color center, H color center and Eu2+ complex) in the lattice of BaFCl:Eu2+ was suggested when the phosphor was X-ray irradiated. The Eu2+ located in the complex has only contribution to the ESR signal, but has no contribution to PL spectrum. The excitation of both F-center and located Eu2+ could decompose the complex to induce bleaching. The 440 nm light could excite the F-centers and the 220 nm and 270 nm could excite the located Eu2+, and the excitation disturbed the F-H-Eu2+ complex and caused a decrease of the PSL.
Co-reporter:Dongmei Li, Wenjuan Zhao, Xuedong Sun, Jinlong Zhang, Masakazu Anpo, Jincai Zhao
Dyes and Pigments 2006 Volume 68(Issue 1) pp:33-37
Publication Date(Web):January 2006
DOI:10.1016/j.dyepig.2004.12.015
Highly ordered MCM-41 has been synthesized and four coumarin derivative dyes were incorporated into it by impregnation method. The absorption and emission spectra of four coumarin derivatives in both toluene and MCM-41 were examined to explore the structural and environmental effects on the optical properties of these dyes. The spectra results indicated that dye molecules existed in monomer form within MCM-41. The maxima of absorption and emissions shifted to red compared with those in toluene due to the strong host–guest interactions. The shifts of emission maxima increased with increasing the volume of the dyes.
Co-reporter:Lingzhi Wang, Yaofeng Shao, Jinlong Zhang, Masakazu Anpo
Microporous and Mesoporous Materials 2006 Volume 95(1–3) pp:17-25
Publication Date(Web):18 October 2006
DOI:10.1016/j.micromeso.2006.04.016
MCM-48 mesoporous molecular sieve with thermal and hydrothermal stability can be conveniently prepared within only 24 h with the aid of promoter anions SO42-, NO3- or Cl− (referred as P). The influences of the P/Si ratio and OH−/Si ratio to the formation of MCM-48 were investigated here, where the P/Si and OH−/Si ranges were set between 0–0.3 and 0.45–0.55, respectively. The suitable P/Si range for the formation of MCM-48 mainly depends on the hydration energy of the promoter anion, which follows the order of SO42->Cl->NO3-. The lower the hydration energy is, the wider the P/Si range is. Moreover, the P/Si range also varies with the OH−/Si, which is wider when the OH−/Si is lower. The thermal and hydrothermal stability of MCM-48 can be considerably improved by directly adding promoter anions to the synthesis gel. The results show SO42- is the most effective promoter for the improvement of structure stability due to its extremely high hydration energy, which is followed by NO3- and Cl− successively. Each promoter added to the synthesis gel has an optimum P/Si ratio for the improvement of the stability since overmuch addition of promoters obstructs the electronic interaction between anion silicates and cation surfactants, leading to the formation of poor ordered MCM-48 materials.
Co-reporter:Qiaorong Sheng, Ye Cong, Shuai Yuan, Jinlong Zhang, Masakazu Anpo
Microporous and Mesoporous Materials 2006 Volume 95(1–3) pp:220-225
Publication Date(Web):18 October 2006
DOI:10.1016/j.micromeso.2006.05.033
A mesoporous TiO2 with crystalline framework was synthesized by nanocrystalline particle assembly using a double surfactant system. Hydrothermal treatment was adopted in order to improve the crystallinity of mesoporous framework. The XRD patterns, HRTEM and TEM images indicate that the as-synthesized product is mesoporous structure and the pore wall is crystalline structure. Nitrogen adsorption–desorption isotherm reveals that there is the bi-porous structure in the sample calcined at 523 K. A controlled calcination process using a slow and constant heating rate was adopted so that the mesoporous structure of the sample could be retained to 673 K.
Co-reporter:Qiaorong Sheng, Shuai Yuan, Jinlong Zhang, Feng Chen
Microporous and Mesoporous Materials 2006 Volume 87(Issue 3) pp:177-184
Publication Date(Web):9 January 2006
DOI:10.1016/j.micromeso.2005.06.036
A mesoporous TiO2 with high photocatalytic activity was synthesized by assembling nanocrystalline particles using dodecylamine (DDA) as organic linkers. The products were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), nitrogen adsorption–desorption isotherms and thermogravimetry-differential thermal analysis (TG-DTA). Low-angle XRD and TEM confirmed that the mesoporous TiO2 had a wormhole-like structure. Nitrogen adsorption–desorption isotherm showed products retained mesoporosity with a narrow pore size distribution (2.8–4.0 nm) and high surface areas (104.4–346.0 m2/g) to 673 K. TG-DTA analysis revealed that the surfactant had been removed partly in as-synthesized samples. The pH value affected the order of mesoporous structure. The ordered mesoporous structure would not retain at pH = 14. All calcined mesoporous TiO2 showed high photocatalytic activities on photodecomposition of cationic dye X-GL.
Co-reporter:Lingzhi Wang, Yaofeng Shao, Jinlong Zhang, Masakazu Anpo
Optical Materials 2006 Volume 28(Issue 10) pp:1232-1234
Publication Date(Web):July 2006
DOI:10.1016/j.optmat.2005.08.005
Fluorescein was first introduced to the large pore channel of SBA-15 by impregnation method. UV–Vis absorption, fluorescence emission and lifetime were used to characterize the host–guest composite. The existing forms of fluorescein in SBA-15 consist of monoanion and dianion. The emission spectrum of fluorescein in SBA-15 shifts to blue about 10 nm and the fluorescence lifetime is largely prolonged compared with that in ethanol. The prolonged lifetime in SBA-15 is attributed to the high dispersion of fluorescein molecules in SBA-15 and the formation of hydrogen bond with silanols on the surface of SBA-15.
Co-reporter:Lijun Zhou, Shanshan Yan, Baozhu Tian, Jinlong Zhang, Masakazu Anpo
Materials Letters 2006 Volume 60(Issue 3) pp:396-399
Publication Date(Web):February 2006
DOI:10.1016/j.matlet.2005.08.065
TiO2–SiO2 films were successfully deposited on modified poly (ethylene terephthalate) (PET) substrate as one of the thermal-sensitive material with different content of SiO2. The as-prepared films were characterized with Fourier transform infrared spectra (FTIR), X-ray diffraction (XRD), atomic force microscopy (AFM), respectively. At the ratio of Ti / Si = 1 : 1, the TiO2–SiO2 thin film showed the highest photocatalytic activity due to improving the ability of the surface adsorption and increasing surface hydroxyl group in the composite thin film. Moreover, the SiO2–TiO2 composite thin film showed the most surface roughness, which further confirms the film with the highest photocatalytic activity at the ratio of Si / Ti = 1 : 1. When the ratio of Si / Ti more than 1 : 1, the decrease in photocatalytic activity is due to reducing amount of the surface acidity sites and photocatalytic center.
Co-reporter:Yaofeng Shao, Lingzhi Wang, Jinlong Zhang, Masakazu Anpo
Journal of Photochemistry and Photobiology A: Chemistry 2006 Volume 180(1–2) pp:59-64
Publication Date(Web):15 May 2006
DOI:10.1016/j.jphotochem.2005.09.018
Photophysical and photochemical properties of rhodamine B molecules encapsulated into various mesoporous molecular sieves were investigated by absorption and emission spectra and fluorescence decay. The different fluorescence properties were observed within different RhB/Me-MCM-48 (Me = Ce, Fe, Cr) composites. There were larger blue shifts in fluorescence spectra when RhB included in Ce-MCM-48 than that in Fe-MCM-48 and Cr-MCM-48. However, the much larger electron transfer efficiencies from excited dye molecules to iron and chromium oxide occurred within the system of RhB/Fe-MCM-48 and RhB/Cr-MCM-48 than that within the system of RhB/Ce-MCM-48. The effects of Ce-containing amounts on the fluorescence properties were also investigated in detail.
Co-reporter:Jiefang Zhu, Feng Chen, Jinlong Zhang, Haijun Chen, Masakazu Anpo
Journal of Photochemistry and Photobiology A: Chemistry 2006 Volume 180(1–2) pp:196-204
Publication Date(Web):15 May 2006
DOI:10.1016/j.jphotochem.2005.10.017
Fe3+-doped anatase nanosized TiO2 photocatalysts have been prepared by combining sol–gel method with hydrothermal treatment. The samples were characterized by UV–vis diffuse reflectance spectroscopy, X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET)-specific surface area (SBET), transmission electron microscopy (TEM), atomic absorption flame emission spectroscopy (AAS), electron paramagnetic resonance (EPR) spectroscopy and X-ray photoelectron spectroscopy (XPS). From results of UV–vis diffuse reflectance spectroscopy, Fe3+-doped TiO2 extends its absorption to longer than 500 nm, which leads to an obvious photocatalatic activity under visible irradiation. From XRD, EPR, AAS and XPS, it was found that Fe exist in trivalent ionic state substituting Ti4+ in TiO2 lattice and its concentration decreases from the surface to the center of doped TiO2. The photocatalytic activity of prepared samples was investigated for the photocatalytic degradation of active yellow XRG dye. The photocatalytic activity of TiO2 doped with appropriate content of Fe3+ exceeded those of non-doped TiO2 and P25 both under UV and visible light irradiation.
Co-reporter:Wenjuan Zhao, Dongmei Li, Bin He, Jinlong Zhang, Jiazhen Huang, Lizhong Zhang
Dyes and Pigments 2005 Volume 64(Issue 3) pp:265-270
Publication Date(Web):March 2005
DOI:10.1016/j.dyepig.2004.06.002
Coumarin derivative encapsulated in various mesoporous sieves was prepared by impregnation method. The effects of pore size and Ti-containing amounts on the fluorescence properties were investigated. High dispersion of the dye molecules could be realized on the composite of mesoporous sieves, and the electron transfer from the excited dye molecule to titanium oxide occurred in the composite.
Co-reporter:Yaofeng Shao, Lingzhi Wang, Jinlong Zhang, Masakazu Anpo
Microporous and Mesoporous Materials 2005 Volume 86(1–3) pp:314-322
Publication Date(Web):28 November 2005
DOI:10.1016/j.micromeso.2005.07.043
The high quality MCM-48 has been easily synthesized at 120 °C for 24 h, and the results of which showed that not only long-range ordering of MCM-48, but also hydrothermal stability could be significantly improved by direct addition of NaF with F−/Si ratio of 0.1 and 0.2 to initial reacting gel without post-treatment and pH adjustment. The results of XRD, N2-adsorption and TEM analyses indicated that MCM-48, which was synthesized via appropriate procedure, maintained their structural integrity after boiling in water at 100 °C for at least 3 days. Additionally, the optimum condition was F−/Si ratio of 0.1 at a Na2O/SiO2 ratio of 0.25. The adding time of NaF was critical in the formation of this high quality MCM-48. When the addition of fluoride ions was 60 min earlier than that of surfactant, the mesoporous structure of the synthesized MCM-48 could be maintained after refluxing in boiling water for 3 days. When the additions of fluoride ions and surfactant were simultaneous, however, the structure of MCM-48 was collapsed after 12 h refluxing in boiling water. The result clearly showed that the long-range structural ordering and hydrothermal stability could be improved only when adding NaF at the early stage of hydrolysis and polymerization of silicate. The different effects of fluoride anions at the different reacting periods of synthesizing MCM-48 are also discussed.
Co-reporter:Dongmei Li, Jinlong Zhang, Masakazu Anpo
Optical Materials 2005 Volume 27(Issue 4) pp:671-673
Publication Date(Web):January 2005
DOI:10.1016/j.optmat.2004.04.016
Pyrylium salt 2,4-diphenyl-5,6,7,8-tetrahydro-chromenylium; perchlorate (S-2) was introduced into the three-dimensional channels of mesoporous molecular sieve MCM-48 by post-synthesis impregnation method. There were large blue shifts in absorption and fluorescence spectra when S-2 was included into MCM-48. The results indicate that the S-2 molecules exist in the monomer state in MCM-48 and form hydrogen bond with the surface silanols of MCM-48.
Co-reporter:Jiefang Zhu, Jinlong Zhang, Feng Chen, Masakazu Anpo
Materials Letters 2005 Volume 59(Issue 27) pp:3378-3381
Publication Date(Web):November 2005
DOI:10.1016/j.matlet.2005.05.072
A simple method for preparing high photoactive photocatalysts with anatase and TiO2 (B) has been developed by controlled hydrolysis of titanium butoxide with water generated “in situ” via an esterification reaction between acetic acid and ethanol. The existence of a very uncommon crystal phase, TiO2 (B) was verified by XRD, HRTEM and Raman. The photocatalytic activity of samples prepared was higher than that of Degussa P25 for the liquid phase photocatatlytic degradation of active yellow XRG dye, which is mostly due to the modified sol–gel process and bicrystalline structure containing anatase and TiO2 (B).
Co-reporter:Dongmei Li, Jinlong Zhang, Masakazu Anpo, Minzhao Xue, Yangang Liu
Materials Letters 2005 Volume 59(Issue 17) pp:2120-2123
Publication Date(Web):July 2005
DOI:10.1016/j.matlet.2005.02.044
Laser dye Coumarin-6 (C6) molecules were incorporated into the three-dimensional channels of mesoporous molecular sieve MCM-48. The photophysical and photochemical properties of C6 in MCM-48 were characterized by absorption, emission and electron paramagnetic resonance (EPR) spectra. The results indicated that MCM-48 exerted a significant influence on the photophysical and photochemical properties of the incorporated C6 molecules. Absorption maxima of C6 in MCM-48 exhibited large red-shift while emission exhibited relatively small red-shift compared with those in ethanol. A broad EPR signal with a g value of 2.003 indicates that electron transfer occur easily in the C6/MCM-48 composite.
Co-reporter:Xing-wang Bao, Shan-Shan Yan, Feng Chen, Jin-long Zhang
Materials Letters 2005 Volume 59(Issue 4) pp:412-415
Publication Date(Web):February 2005
DOI:10.1016/j.matlet.2004.09.035
Well-dispersed nanocrystalline TiO2 powders were prepared by hydrothermal method from aqueous peroxotitanium acid gel obtained by addition of H2O2 solution to freshly prepared and well-washed titanic acid gel. The obtained TiO2 powders were characterized by FT-IR spectrophotometer, X-ray diffraction (XRD), transmission electron microscope (TEM) and N2 adsorption. The powders obtained by hydrothermally treating at 393 K for 6 h showed the highest photocatalytic activity for the degradation of aqueous methyl orange solution.
Co-reporter:Lingzhi Wang, Yaofeng Shao, Jinlong Zhang
Materials Letters 2005 Volume 59(Issue 28) pp:3604-3607
Publication Date(Web):December 2005
DOI:10.1016/j.matlet.2005.06.033
The crystallization time for cubic Ia3d mesoporous MCM-48 molecular sieve was first reduced by combining slight increase of reaction temperature with addition of tiny fluoride ions to the synthesis system. The reaction time reduces with the increasing F− / Si ratio, but the high ratio of 0.4 will only lead to a disordered structure with poor crystallinity. The pore ordering is also considerably improved with the aid of fluoride ions even the reaction time is much shorter than those without any fluorides. The time-reduction action of fluoride ions on the synthesis of MCM-48 is attributed to the accelerated hydrolysis speed of silica source and condensation degree of silicates by fluoride ions.
Co-reporter:Xuedong Sun, Jinglong Zhang, Bin He
Journal of Photochemistry and Photobiology A: Chemistry 2005 Volume 172(Issue 3) pp:283-288
Publication Date(Web):5 June 2005
DOI:10.1016/j.jphotochem.2004.12.016
A series of meso-thienyl porphyrins were synthesized through Lindsey's procedure and characterized. Compared with H2TPP (tetraphenylporphyrin), the absorption and fluorescence spectra of thienyl porphyrins have red shift obviously which show that thienyl substituents at meso-position change the electronic structure of tetrapyrrole ring. With protonation using CF3COOH, the absorption bands of thienyl porphyrins are further red shifted. The absorption bands of meso-thienyl porphyrins change correspondingly with the variation of solvents’ properties, however the maxima emission wavelengths corresponding to Q* have little relation with solvents. And the fluorescence lifetime become so less even to 1.1 ns. The half-wave redox potential shows cathodic shift relative to H2TPP. These changes above are all ascribed to the introduction of thienyl group at meso-position and the possibility of more planarity of meso-thienyl porphyrins for the small size of thienyl group which is helpful to the extending π-delocalization of thienyl groups to the tetrapyrrole ring.
Co-reporter:Dongmei Li, Jinlong Zhang, Masakazu Anpo
Dyes and Pigments 2004 Volume 63(Issue 1) pp:71-76
Publication Date(Web):October 2004
DOI:10.1016/j.dyepig.2003.12.013
Benzopyrylium salt S-2 (2,4-diphenyl-5,6,7,8-tetrahedro-1-benzopyrylium perchlorate) was introduced into the channels of mesoporous molecular sieves Ti-HMS with different Ti content by impregnation method. The fluorescence properties (excitation, emission and lifetime) of S-2 in these sieves have been studied. The results indicated that S-2 molecules interact with the isolated framework Ti4+ on the internal surface of Ti-HMS and the amount of S-2 introduced increases with the increasing of isolated titanium content. The observed biexponential decay can be interpreted in terms of two absorbed site, the isolate Ti site and the silanol site. The S-2 molecules absorbed on the Ti site have longer lifetime.
Co-reporter:Shuai Yuan, Qiaorong Sheng, Jinlong Zhang, Feng Chen, Masakazu Anpo
Materials Letters 2004 Volume 58(22–23) pp:2757-2760
Publication Date(Web):September 2004
DOI:10.1016/j.matlet.2004.04.013
The effects of H+/Ti molar ratio on the formation of mesoporous structure and the phase transition have been investigated, and the mesoporous titania with bicrystalline framework consisting of anatase and rutile was characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), BET surface area, and BJH pore size distribution.
Co-reporter:Jiefang Zhu, Wei Zheng, Bin He, Jinlong Zhang, Masakazu Anpo
Journal of Molecular Catalysis A: Chemical 2004 Volume 216(Issue 1) pp:35-43
Publication Date(Web):1 July 2004
DOI:10.1016/j.molcata.2004.01.008
Iron-ion-doped anatase titanium (IV) dioxide (TiO2) samples were prepared by hydrothermal hydrolysis and crystallization in octanol-water solution. The samples were characterized by X-ray diffraction, BET-specific surface area determination, UV-Vis diffuse reflectance spectroscopy and electron paramagnetic resonance spectroscopy. UV-Vis diffuse reflectance spectra showed a slight shift to longer wavelengths and an extension of the absorption in the visible region for almost all the ion-doped samples, compared to the non-doped sample. The photocatalytic activity of those catalysts was investigated for the liquid phase photocatatlytic degradation of active yellow XRG dye diluted in water under UV and visible light irradiation. It was found that the catalysts doped with FeCl3 have better catalytic activity for photodegradation of XRG than those doped with FeCl2. The amount of doped iron ion plays a significant role in affecting its photocatalytic activity and iron doped with optimum content can enhance photocatalytic activity, especially under visible light irradiation.Iron-ion-doped anatase titanium (IV) dioxide (TiO2) were prepared by hydrothermal method in this paper. Absorption, crystal size, specific surface area and photocatalytic activity of TiO2 were obviously changed by doping. Iron doped with optimum content can enhance photocatalytic activity, especially under visible light irradiation.
Co-reporter:Mingyang Xing, Dianyu Qi, Jinlong Zhang, Feng Chen, Baozhu Tian, Segomotso Bagwas, Masakazu Anpo
Journal of Catalysis (October 2012) Volume 294() pp:37-46
Publication Date(Web):1 October 2012
DOI:10.1016/j.jcat.2012.07.004
NH4F was used instead of conventional organic silylation agent as the hydrophobic modifier to synthesize the super-hydrophobic mesocellular foams (MCF) loaded with nano-sized TiO2 photocatalysts in its pore channels, which could be considered as an extractant for organics. Compared to organosilane modified catalysts, NH4F-modified MCF/TiO2 has a more stable super-hydrophobic property and much higher photocatalytic activity. It was found that only using isopropanol as the solvent, the NH4F-modified catalyst showed super-hydrophobic property. It is believed that the solvent plays a role in controlling the exchange between surface OH groups and F ions. The special structure of supported mesoporous catalyst greatly facilitated the surface fluorination, which together with the Ti3+ generation led to its excellent adsorption capacity and UV/visible light photocatalytic activity. This novel super-hydrophobic mesoporous photocatalyst has a large application potential in the field of photocatalysis, shipbuilding, and other industries.Graphical abstractNH4F was used as hydrophobic modifier to synthesize the superhydrophobic mesocellular foams loaded with TiO2 photocatalyst, which could be considered as an extractant for organics and a high-performance photocatalyst.Download high-res image (275KB)Download full-size imageHighlights► Superhydrophobic mesoporous MCF as supports for TiO2 photocatalysts are prepared. ► NH4F is instead of unstable organic silylation agent as the hydrophobic modifier. ► Isopropanol is used as the only effective solvent to achieve the hydrophobicity. ► Low-temperature vacuum activation can produce Ti3+. ► Synergistic effect of Ti3+ and surface fluorination is responsible for its enhanced adsorption capacity and photocatalytic activity.
Co-reporter:Xiangqi Zhu, Jinlong Zhang, Feng Chen
Chemosphere (March 2010) Volume 78(Issue 11) pp:1350-1355
Publication Date(Web):1 March 2010
DOI:10.1016/j.chemosphere.2010.01.002
Bismuth titanate (Bi12TiO20) nanostructures with different morphologies were synthesized hydrothermally using Bi(NO3)3 and Ti(SO4)2 in the presence of polyethylene glycol (PEG). X-ray diffraction (XRD) proved that the samples were in pure cubic phase. UV–visible diffuse reflection spectra showed the band gap of Bi12TiO20 is about 2.7 eV. Brunauer–Emmett–Teller (BET) analysis proved that the Bi12TiO20 samples have higher surface areas than samples prepared by methods reported previously. Photocatalytic degradation of acid orange 7 (AO7) under visible light illumination was used to evaluate the photocatalytic ability of samples. The photocatalytic results showed Bi12TiO20 could degrade AO7 very efficiently and had higher photocatalytic activity than traditional N-doped TiO2. In addition, we have also discussed factors that have major effect on reaction efficiency. BET surface area played the most important role in the photocatalytic degradation of AO7. The crystallinity of the samples is another important factor which can also influence photocatalysis results.
Co-reporter:Penghua Wang, Juying Lei, Mingyang Xing, Lingzhi Wang, Yongdi Liu, Jinlong Zhang
Journal of Environmental Chemical Engineering (June 2015) Volume 3(Issue 2) pp:961-968
Publication Date(Web):1 June 2015
DOI:10.1016/j.jece.2015.03.012
•Rhombic anatase nanocrystals were synthesized by a facile green solvothermal approach.•Ammonium acetate and ethylenediamine act as structure directing agents.•The nanocrystals possess large percentage of {0 1 0} facets up to 73%.•The nanocrystals have small average particle size and large surface area.•The nanocrystals have superior photocatalytic activity to commercial anatase and P25.This work reports a facile green solvothermal approach to synthesize rhombic anatase TiO2 nanocrystals with small particle size of 50 nm and large percentage of {0 1 0} facets up to 73%. Tetrabutyl titanate (TBOT) is used as the titanium precursor while ethanol as the reaction solvent. The key strategy of this approach is to utilize ammonium acetate (AMAT) and ethylenediamine (EDA) in the non-aqueous system, where AMAT promotes the hydrolysis of TBOT and EDA serves as the capping agent. AMAT and EDA act synergistically to achieve a controlled growth of crystal structure of the anatase TiO2 nanocrystals with exposed {0 1 0} facets. The mechanism for the nanocrystal growth was proposed based on experimental evidence. And the photocatalytic activities of the resultant nanocrystals were evaluated by degradation of methyl orange. This nanocrystal exhibits a superior photocatalytic activity in reference to commercial anatase TiO2 and P25, owing to the large percentage of exposed {0 1 0} facets along with large surface area resulting from the small particle size.
Co-reporter:Mingyang Xing, Wenzhang Fang, Muhammad Nasir, Yunfei Ma, Jinlong Zhang, Masakazu Anpo
Journal of Catalysis (January 2013) Volume 297() pp:236-243
Publication Date(Web):1 January 2013
DOI:10.1016/j.jcat.2012.10.014
A series of TiO2 catalysts self-doped with Ti3+ were successfully synthesized by a simple one-step solvothermal method with low-cost NaBH4 added as a reductant. During NaBH4 reduction, large amounts of NaBO2 and carbonaceous impurities covered the surface of the TiO2 self-doped with Ti3+, resulting in an inhibition of visible-light absorption and photocatalytic activity. In the preparation, HCl solution was used to wash off the by-product NaBO2 and carbonaceous impurities coated on the surface of the catalysts. The samples were characterized by XRD, UV-DRS, ESR, XPS, and FT-IR analyses. After HCl washing, the photocatalytic activity of the Ti3+-doped TiO2 increased markedly, while the Ti3+ content remained the same. Furthermore, it was found that the visible-light photocatalytic activity of Ti3+-doped TiO2 depended on the amount of Ti3+ added, while there was no significant impact of Ti3+ doping on its UV-light photocatalytic activity.Graphical abstractTi3+ generation is responsible for the narrowing of the band gap, enhanced visible-light absorption, and photocatalytic activity.Download high-res image (77KB)Download full-size imageHighlights► TiO2 self-doped with Ti3+ are successfully synthesized by a simple solvothermal method. ► Low-cost NaBH4 is used as a reductant. ► HCl solution is used to wash out the by-product and carbonaceous impurities coated on the catalysts surface. ► Visible-light photocatalytic activity of Ti3+-doped TiO2 depends on the amount of Ti3+ added. ► There is no significant impact of Ti3+ doping on its UV-light photocatalytic activity.
Co-reporter:Bocheng Qiu, Qiaoying Li, Bin Shen, Mingyang Xing, Jinlong Zhang
Applied Catalysis B: Environmental (April 2016) Volume 183() pp:216-223
Publication Date(Web):April 2016
DOI:10.1016/j.apcatb.2015.10.053
Co-reporter:Yongmei Wu, Mingyang Xing, Jinlong Zhang, Feng Chen
Applied Catalysis B: Environmental (9 June 2010) Volume 97(Issues 1–2) pp:
Publication Date(Web):9 June 2010
DOI:10.1016/j.apcatb.2010.03.038
A visible light-active TiO2 photocatalyst modified by boron and carbon was synthesized by sol–gel followed solvothermal process. The resulting photocatalyst was characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), UV–vis absorption spectroscopy, and electron paramagnetic resonance (EPR). It was found that the boron and carbon modified TiO2 showed obvious absorption in the range 400–500 nm. XPS results suggested boron species entered into interstitial site of TiO2 matrix and formed the B–O–Ti bond, while carbon species were in the form of carbonates species. EPR results showed the existence of oxygen vacancy in carbon and boron modified TiO2. This may result in the sensitivity of the as-synthesized photocatalyst to visible light. The resulting boron and carbon modified TiO2 exhibited significantly higher photocatalytic activity than carbon modified TiO2 and undoped anatase TiO2 on the degradation of Acid Orange 7 (AO7) in aqueous solution under visible light irradiation. The presence of carbon originating from organic precursor has great influence on the surface properties of B-doped TiO2.
Co-reporter:Baozhu Tian, Jinlong Zhang, Tianzhong Tong, Feng Chen
Applied Catalysis B: Environmental (8 March 2008) Volume 79(Issue 4) pp:394-401
Publication Date(Web):8 March 2008
DOI:10.1016/j.apcatb.2007.11.001
Co-reporter:Ahmed Khan Leghari Sajjad, Sajjad Shamaila, Baozhu Tian, Feng Chen, Jinlong Zhang
Applied Catalysis B: Environmental (7 September 2009) Volume 91(Issues 1–2) pp:397-405
Publication Date(Web):7 September 2009
DOI:10.1016/j.apcatb.2009.06.005
Co-reporter:Ya Liu, Ping Zhang, Baozhu Tian, Jinlong Zhang
Catalysis Communications (5 October 2015) Volume 70() pp:30-33
Publication Date(Web):5 October 2015
DOI:10.1016/j.catcom.2015.07.018
•1D core–shell structural CdS@TiO2 was fabricated by a sol–gel method.•Thickness of TiO2 shell layer can be tuned by changing the additional amount of ammonia.•a-TiO2 shell layer promotes the separation of electron–hole pairs.•CdS@a-TiO2 showed improved activity for selectively oxidizing benzyl alcohol.One dimension (1D) core–shell structural CdS@TiO2 was fabricated by a modified sol–gel method. The thickness of amorphous TiO2 (a-TiO2) layer was adjusted by changing the amount of ammonia. Although a-TiO2 shell layer diminishes the visible light absorption in a certain extent, it largely increases the surface area of photocatalyst and effectively promotes the separation rate of photogenerated electron–hole pairs. It was revealed that a-TiO2 shell layer can effectively enhance the photocatalytic activity of CdS NRs for benzyl alcohol (BA) to benzaldehyde (BAD) transformation. Moreover, the core–shell structural CdS@a-TiO2 showed high stability and reusability for the selective oxidation of BA.Download high-res image (126KB)Download full-size image
Co-reporter:Liqin Guo, Feng Chen, Xiangqun Fan, Wandong Cai, Jinlong Zhang
Applied Catalysis B: Environmental (26 April 2010) Volume 96(Issues 1–2) pp:162-168
Publication Date(Web):26 April 2010
DOI:10.1016/j.apcatb.2010.02.015
Co-reporter:Sajjad Shamaila, Ahmed Khan Leghari Sajjad, Feng Chen, Jinlong Zhang
Catalysis Today (25 October 2011) Volume 175(Issue 1) pp:568-575
Publication Date(Web):25 October 2011
DOI:10.1016/j.cattod.2011.03.041
The mesoporous titania, designated MS-TiO2 was successfully prepared via a new combination of pluronic P123 and poly ethylene glycol templates and acetic acid as the hydrolytic retardant with extremely high crystallinity achieved during synthesis process. MS-TiO2 has remarkable thermal stability, biporous mesostructure and superior photocatalytical activity for phenol degradation and mineralization as compared to mesoporous TiO2 prepared using single template systems. The anatase–rutile phase transformation of the MS-TiO2 was not observed up to 800 °C. The mesoscale order of MS-TiO2 was retained after thermal treatment up to 450 °C as confirmed by low angle X-ray diffraction and transmission electron microscopy analyses. It maintained its pore properties at high temperature of 700 °C with a significant pore size 10.4 nm and pore volume 0.11 cm3/g. MS-TiO2 has biporous mesostructure with the small mesopore of 5.5 nm and the large mesopore of 8.7 nm in mean pore diameters. The MS-TiO2 showed higher photocatalytic activity for phenol degradation than mesoporous titania prepared using single templates and standard system of Degussa P25. The remarkably high catalytic activity of the MS-TiO2 is attributed to its high crystallinity and biporous mesostructure. The phenol mineralization was confirmed using high performance liquid chromatography and total organic carbon analyses.Graphical abstractDownload high-res image (196KB)Download full-size imageHighlights► Highly crystalline mesoporous titania in as prepared form is achieved by a new combination of dual-template system of triblock copolymer (P123) and poly ethylene glycol (PEG). ► The moment of anatase formation during the synthesis depends on both medium and type of surfactants used. ► This combination provides more hydrophobic contrast than single template system resulting in the thicker anatase walls which gives higher thermal stability. ► Excellent photocatalytic abilities for phenol degradation and mineralization as compared to Degussa P25 and mesoporous titania prepared by single templates.
Co-reporter:Sajjad Shamaila, Ahmed Khan Leghari Sajjad, Feng Chen, Jinlong Zhang
Applied Catalysis B: Environmental (10 February 2010) Volume 94(Issues 3–4) pp:272-280
Publication Date(Web):10 February 2010
DOI:10.1016/j.apcatb.2009.12.001
Co-reporter:Dianyu Qi ; Liujia Lu ; Lingzhi Wang ;Jinlong Zhang
Journal of the American Chemical Society () pp:
Publication Date(Web):June 24, 2014
DOI:10.1021/ja5052632
Highly sensitive surface-enhanced Raman scattering (SERS) detection was achieved on plasmon-free TiO2 photonic artificial microarray, which can be quickly recovered under simulated solar light irradiation and repeatedly used. The sensitive detection performance is attributed to the enhanced matter-light interaction through repeated and multiple light scattering in photonic microarray. Moreover, the SERS sensitivity is unprecedentedly found to be dependent on the different light-coupling performance of microarray with various photonic band gaps, where microarray with band gap center near to laser wavelength shows a lower SERS signal due to depressed light propagation, while those with band gap edges near to laser wavelength show higher sensitivity due to slow light effect.
Co-reporter:Lin Jiang, Lingzhi Wang and Jinlong Zhang
Chemical Communications 2010 - vol. 46(Issue 42) pp:NaN8069-8069
Publication Date(Web):2010/09/24
DOI:10.1039/C0CC01646B
Bi2WO6 nanoparticles loaded on a spherical MCM-48 mesoporous molecular sieve with a high photocatalytic activity in the visible-light range was synthesized for the first time using a facile one-step process.
Co-reporter:Dianyu Qi, Xuefeng Yan, Lingzhi Wang and Jinlong Zhang
Chemical Communications 2015 - vol. 51(Issue 42) pp:NaN8816-8816
Publication Date(Web):2015/04/10
DOI:10.1039/C5CC02468D
Here, using the (Au/TiO2)-catalyzed reduction of 4-nitrothiophenol as a probe reaction, a catalysis/SERS bifunctional composite fabricated by uniformly dispersing catalysis-active Au nanoclusters (∼2 nm) on a SERS-active TiO2 photonic microarray was successfully applied to the non-plasmonic SERS self-monitoring of a catalytic reaction for the first time, which is superiorly sensitive and interference-free.
Co-reporter:Yi Zhou, Qiuying Yi, Mingyang Xing, Lu Shang, Tierui Zhang and Jinlong Zhang
Chemical Communications 2016 - vol. 52(Issue 8) pp:NaN1692-1692
Publication Date(Web):2015/11/27
DOI:10.1039/C5CC07567J
Sandwich structured graphene modified TiO2 mesoporous single crystals (GR-MSCs) were obtained by using the graphene embedded silica spheres as the hard template, via a hydrothermal treatment. The selective photocatalysis of TiO2 can be achieved by controlling the location of graphene in TiO2 mesoporous single crystals. The sandwich structured graphene–TiO2 composite has a photooxidation surface, and the core–shell structured TiO2@graphene has a photoreduction surface. It provides a new pathway to realize the selectivity of photocatalysis by controlling the location of graphene in TiO2 MSCs for the first time.
Co-reporter:Juying Lei, Lingzhi Wang and Jinlong Zhang
Chemical Communications 2010 - vol. 46(Issue 44) pp:NaN8447-8447
Publication Date(Web):2010/10/01
DOI:10.1039/C0CC03310C
Incorporation of a dual-FRET dye pair into mesoporous silica nanoparticles yields sensitive and sensing-range tunable nanosensors with good reversibility that can be used for ratiometric pH measurements under a single-wavelength excitation.
Co-reporter:Mingyang Xing, Wenzhang Fang, Xiaolong Yang, Baozhu Tian and Jinlong Zhang
Chemical Communications 2014 - vol. 50(Issue 50) pp:NaN6640-6640
Publication Date(Web):2014/03/27
DOI:10.1039/C4CC01341G
Highly-dispersed boron-doped graphene nanoribbons (B-GNRs), prepared by a simple vacuum activation method, exhibit p-type semiconductor properties and provide many more zigzag- and armchair-edges to facilitate control of the bandgap. B-GNRs are used for the photodegradation of Rhodamine B in order to demonstrate their excellent conductivity and photocatalytic activity.
Co-reporter:Lingang Yang, Lingzhi Wang, Chuanfeng Cui, Juying Lei and Jinlong Zhang
Chemical Communications 2016 - vol. 52(Issue 36) pp:NaN6157-6157
Publication Date(Web):2016/04/01
DOI:10.1039/C6CC01917J
The Stöber process is revisited using vinyltriethoxysilane as the precursor, where a kinetics-controlled condensation of vinylsilanols, free from external fluorogens, unprecedentedly produces hydrophilic diamond-structured organosilica nanocrystals (ca. 2–6 nm) with finely tunable fluorescence (460–625 nm). The key to the synthesis lies in a slow successful condensation of vinylsilanols triggered and guided by the π–π stacking interaction of vinyl groups.
Co-reporter:Bocheng Qiu, Mingyang Xing and Jinlong Zhang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 24) pp:NaN12827-12827
Publication Date(Web):2015/05/07
DOI:10.1039/C5TA02675J
We report three-dimensional (3D) graphene-based hybrids of Fe2O3 nanocrystals grown in situ on graphene aerogels (Fe2O3/GAs) by a Stöber-like method. Compared with other reported Fe2O3/3D-graphene, Fe2O3/GAs have outstanding mechanical strength, high elasticity, ultralow mass, excellent electrical conductivity, good oil absorption capacity and a dispersion of nanoparticles. They have a 3D network structure with a high surface area of 316 m2 g−1 and physicochemical stability. 3D-GAs can inhibit the loss of Fe2+ and stabilize the conversion of Fe3+/Fe2+ in the photo-Fenton reaction. Compared with Fe2O3 and Fe2O3/2D-graphene (Fe2O3/GR), Fe2O3/GAs exhibit an ultrastable, solar-driven Fenton activity over a wide pH range of 3.5–9.0 for the first time. In addition, the highly-dispersed, nanosized Fe2O3 on the surface of the GAs makes the composite highly suitable for use in electrochemical capacitors. Although the Fe2O3/GAs only contain 18.3 wt% Fe2O3, they still yield a high and stable capacitance (151.2 F g−1) at a high discharge current density of 10 A g−1, which is better than that of Fe2O3/GR (93.6 F g−1).
Co-reporter:Mingyang Xing, Jinlong Zhang, Feng Chen and Baozhu Tian
Chemical Communications 2011 - vol. 47(Issue 17) pp:NaN4949-4949
Publication Date(Web):2011/03/21
DOI:10.1039/C1CC10537J
This study reports a simple and economic method to modify Degussa P25 with a vacuum activated procedure, resulting in its high photo-activity and photosensitivity, which suggests this method to be a starting point for the extension of its application to photocatalysis.
Co-reporter:Qiangfang Wu, Shenyuan Bao, Baozhu Tian, Yifei Xiao and Jinlong Zhang
Chemical Communications 2016 - vol. 52(Issue 47) pp:NaN7481-7481
Publication Date(Web):2016/05/10
DOI:10.1039/C6CC02737G
BiVO4 mesoporous single crystals (MSCs) were successfully prepared, for the first time, by a one-step hydrothermal method using the acidified BiVO4 precursor solution pre-impregnated silica as the template. It was revealed that the BiVO4 MSCs were formed by a double-diffusion mechanism. The O2 evolution rate over BiVO4 MSCs was improved nearly 10 times than that over BiVO4 bulk single crystals.
Co-reporter:Hong Li, Liang Zhou, Lingzhi Wang, Yongdi Liu, Juying Lei and Jinlong Zhang
Physical Chemistry Chemical Physics 2015 - vol. 17(Issue 26) pp:NaN17412-17412
Publication Date(Web):2015/05/27
DOI:10.1039/C5CP02554K
Well dispersed TiO2 nanocrystals with (001) facets were successfully grown in situ on g-C3N4 through a facial solvothermal method. The resultant TiO2/g-C3N4 composites exhibit remarkably higher efficiency for photocatalytic degradation of phenol as compared to pure catalysts (g-C3N4 or TiO2) or mechanically mixed TiO2/g-C3N4. The optimal composite with 11.2 wt% TiO2 showed the highest degradation rate constant, which is 2.8 times that of pure g-C3N4, 2.2 times that of pure TiO2, and 1.4 times that of mechanically mixed TiO2/g-C3N4. The enhanced photocatalytic activity is mainly attributed to the effective charge separation derived from two aspects: (1) well matched energy levels between TiO2 and g-C3N4 and (2) a uniform and close contact between TiO2 and g-C3N4 that resulted from the in situ growth of highly dispersed TiO2 nanocrystals. The TiO2/g-C3N4 hybrid material prepared in this study is expected to provide a good foundation for the further design and synthesis of advanced TiO2/g-C3N4-based functional materials, and the in situ growth method developed is hopeful to provide a new strategy for the synthesis of other semiconductor-modified g-C3N4 materials.
Co-reporter:Xianjun Tan, Lingzhi Wang, Chen Cheng, Xuefeng Yan, Bin Shen and Jinlong Zhang
Chemical Communications 2016 - vol. 52(Issue 14) pp:NaN2896-2896
Publication Date(Web):2015/12/16
DOI:10.1039/C5CC10020H
Plasmonic MoO3−x@MoO3 nanosheets obtained from surface oxidation of MoO3−x were employed as a SERS substrate for methylene blue detection. They exhibit extraordinary sensitivity comparable to noble metals, which is attributed to shell-isolated electromagnetic enhancing by the plasmonic MoO3−x core and elimination of the photocatalytic degradation by the MoO3 shell.
Co-reporter:Lingzhi Wang, Juying Lei and Jinlong Zhang
Chemical Communications 2009(Issue 16) pp:NaN2197-2197
Publication Date(Web):2009/03/02
DOI:10.1039/B900200F
Bright and colourful nanocomposites are easily fabricated by doping and fixing one or two kinds of oligosilicate fluorescent dots encapsulated with dye molecules into the pore channels of mesoporous silica nanoparticles, which can engender abundant fluorescent signals with a single excitation wavelength.
Co-reporter:Waheed Iqbal, Chunyang Dong, Mingyang Xing, Xianjun Tan and Jinlong Zhang
Catalysis Science & Technology (2011-Present) 2017 - vol. 7(Issue 8) pp:NaN1734-1734
Publication Date(Web):2017/03/07
DOI:10.1039/C7CY00286F
We report a facile and eco-friendly one-pot synthesis of well-adorned mesoporous g-C3N4 material through a bubble templating strategy and involving controlling the surface area from 17 to 195 m2 g−1 by simply adjusting the mass ratio of melamine/NH4Cl. Various characterization techniques were adopted to examine the structures and physicochemical properties of the as-prepared mpg-C3N4 samples. The results are a step forward to the bottleneck problems of producing mesoporous g-C3N4 materials with both a high BET surface area with well-adorned pore diameters and considerable pore volume by simply employing ammonium chloride as a gaseous bubble template and melamine as a g-C3N4 precursor. The obtained ammonium chloride-mediated mesoporous g-C3N4 photocatalyst demonstrated excellent photocatalytic performance compared with bulk g-C3N4 for the visible light photodegradation of RhB and phenol. The extraordinary photocatalytic activity and outstanding stability of the as-prepared mesoporous g-C3N4 were predominantly attributed to the exceptionally high surface area with ordered pore diameters, improved optical absorbance, and efficient charge separation. Our work not only exhibits the simplest, eco-friendly, and economical approach to fabricate highly efficient well-adorned mesoporous g-C3N4 photocatalysts, but also paves new opportunities for the rational design and synthesis of advanced photocatalysts with great potential in environmental remediation.
Co-reporter:Lingzhi Wang, Chen Cheng, Sen Tapas, Juying Lei, Masaya Matsuoka, Jinlong Zhang and Fan Zhang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 25) pp:NaN13364-13364
Publication Date(Web):2015/05/14
DOI:10.1039/C5TA01652E
Periodic mesoporous organosilica embedded with carbon dots are adopted as the adsorbent for removal of the toxic organic pollutant 2,4-dichlorophenol and inorganic metal ions Hg(II), Cu(II), and Pb(II). The composite possesses an ordered 2D hexagonal mesostructure with a space group of p6mm, high specific surface area (∼468.46 m2 g−1), and uniform pore size (∼5.50 nm). The surface is covered by about 1–2 layers of carbon dot nanoparticles. The maximum adsorption capacity for 2,4-dichlorophenol is 99.70 mg g−1, and the distribution coefficient of metal ions between adsorbent and solution phases is in the range of 2.60–7.41, following the order of Hg(II) > Cu(II) > Pb(II). The Cu(II) and Pb(II) adsorption stays nearly fixed while Hg(II) adsorption is depressed by ∼45% in a mixed solution of metal ions. The Cu(II) and Hg(II) adsorption shows unapparent variation but Pb(II) adsorption is improved by ∼55% in a mixed solution of metal ion and 2,4-dichlorophenol. In contrast, all metal ions lead to the depression of 2,4-dichlorophenol adsorption by 37% (Pb(II)), 45% (Cu(II)), and 48% (Hg(II)). Finally, the n–π electron donor–acceptor interaction between O- and N-containing groups in mesoporous organosilica and the benzene ring in 2,4-dichlorophenol is revealed to be responsible for the enhanced adsorption of 2,4-dichlorophenol, while the electrostatic force and complex formation between metal ions and amide groups co-contribute to the improvement of metal ions adsorption.
Co-reporter:Bocheng Qiu, Qiaohong Zhu, Mingyang Xing and Jinlong Zhang
Chemical Communications 2017 - vol. 53(Issue 5) pp:NaN900-900
Publication Date(Web):2016/12/12
DOI:10.1039/C6CC08311K
CdxZn1−xSe/CoP composites have been well studied as effervescent photocatalysts for H2 evolution. These composites are highly efficient at 45.1 mmol h−1 g−1 and have a high quantum yield of 11.8% at ∼520 nm. The tunable energy band of CdxZn1−xSe facilitates photo-electrons transferring to CoP via chemical bonds between components. Advances in CdxZn1−xSe/CoP for photocatalytic H2 evolution provide a new strategy for future splitting of seawater.
Co-reporter:Shenyuan Bao, Qiangfang Wu, Shunzhou Chang, Baozhu Tian and Jinlong Zhang
Catalysis Science & Technology (2011-Present) 2017 - vol. 7(Issue 1) pp:NaN132-132
Publication Date(Web):2016/11/18
DOI:10.1039/C6CY01980C
A Z-scheme heterogeneous photocatalyst CdS–Au–BiVO4 was synthesized for the first time by photo-reduction and deposition–precipitation methods. The microstructures and optical properties of the as-prepared samples were investigated by means of scanning electron microscopy (SEM), field emission scanning electron microscopy (FE-SEM), high resolution transmission electron microscopy (HR-TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and UV-vis diffuse reflectance spectroscopy (DRS). Due to the oriented accumulation of electrons on the {010} facets of BiVO4 crystals, Au nanoparticles were successfully anchored on the {010} facets of BiVO4 crystals via the photo-reduction process. CdS was further selectively deposited on the surface of Au nanoparticles, benefitting from the strong S–Au interaction. Photocatalytic degradations of tetracycline and Rhodamine B indicated that CdS–Au–BiVO4 exhibits much higher photocatalytic activity than BiVO4, Au–BiVO4, and CdS–BiVO4. Radical trapping experiments confirmed that in the case of CdS–Au–BiVO4, the main reactive species responsible for organic contaminant degradation are h+, ˙OH, and ˙O2−, while only h+ can be produced in the case of CdS–BiVO4. Based on the photoelectrochemical analysis and radical trapping experiments, it can be deduced that the Z-scheme structure of CdS–Au–BiVO4 not only decreases the recombination rate of photo-generated carriers but also makes the holes and electrons keep a higher redox ability.
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