Wei Xiao

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Organization: Wuhan University
Department: School of Resource and Environmental Sciences
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Co-reporter:Jiong Wang, Xiaoming Ge, Zhaolin Liu, Larissa Thia, Ya Yan, Wei Xiao, and Xin Wang
Journal of the American Chemical Society 2017 Volume 139(Issue 5) pp:1878-1884
Publication Date(Web):January 18, 2017
DOI:10.1021/jacs.6b10307
Molecular Co2+ ions were grafted onto doped graphene in a coordination environment, resulting in the formation of molecularly well-defined, highly active electrocatalytic sites at a heterogeneous interface for the oxygen evolution reaction (OER). The S dopants of graphene are suggested to be one of the binding sites and to be responsible for improving the intrinsic activity of the Co sites. The turnover frequency of such Co sites is greater than that of many Co-based nanostructures and IrO2 catalysts. Through a series of carefully designed experiments, the pathway for the evolution of the Co cation-based molecular catalyst for the OER was further demonstrated on such a single Co-ion site for the first time. The Co2+ ions were successively oxidized to Co3+ and Co4+ states prior to the OER. The sequential oxidation was coupled with the transfer of different numbers of protons/hydroxides and generated an active Co4+═O fragment. A side-on hydroperoxo ligand of the Co4+ site is proposed as a key intermediate for the formation of dioxygen.
Co-reporter:Jing Zhou, Lifan Qin, Wei Xiao, Chen Zeng, Ni Li, Teng Lv, Hua Zhu
Applied Catalysis B: Environmental 2017 Volume 207(Volume 207) pp:
Publication Date(Web):15 June 2017
DOI:10.1016/j.apcatb.2017.01.083
•Oriented growth of layered-MnO2 nanosheets on α-MnO2 nanotubes is reported.•Epitaxial relationship in the resulting α-MnO2@L-MnO2 heteroepitaxy is rationalized.•Pt/α-MnO2@L-MnO2 show enhanced activity to room-temperature HCHO oxidation.•The exposed α-MnO2 {100} surface facilitates adsorption and activation of O2.•The exposed layered-MnO2 {001} surface is beneficial to desorption of resultant H2O.Construction of heterostructures with well-defined size, dimension, surface and interface is an effective approach to develop enhanced and unprecedented functionality. Herein, oriented growth of layered-MnO2 nanosheets (L-MnO2) over α-MnO2 nanotubes backbones is demonstrated. The epitaxial relationship in the resulting α-MnO2@L-MnO2 heteroepitaxy is rationalized as (110)(α-MnO2)||(001)(layered-MnO2). With loading of 1 wt% Pt nanoparticles over the MnO2 samples, the resulting Pt/MnO2 samples show catalytic activity toward room-temperature HCHO oxidation via “HCHO + O2 = CO2 + H2O”. Upon 1 h treatment, 92.1% HCHO becomes mineralized over the Pt/α-MnO2@L-MnO2, higher than that of 81.3% and 75.9% for the Pt/α-MnO2 and Pt/L-MnO2. The oxidation of HCHO was well fitted with the second-order kinetic model, with the rate constant of the Pt/α-MnO2@L-MnO2 exceeding that of the Pt/α-MnO2 and the Pt/L-MnO2 by 2.27 and 5.92 times. Density-Functional-Theory (DFT) simulations show that α-MnO2 {100} surface facilitates adsorption/activation of O2, and layered-MnO2 {001} surface is beneficial to desorption of resultant H2O. The α-MnO2@L-MnO2 heteroepitaxy simultaneously integrates exposed facets of α-MnO2 {100} surface and layered-MnO2 {001} surface, in which the synergetic effect of the two surfaces leads to significantly enhanced room-temperature HCHO oxidation activity. The present study provides a rational design of manganese oxide-based catalysts for advanced environmental and energy applications.Oriented growth of layered-MnO2 nanosheets over α-MnO2 nanotubes is demonstrated for construction of α-MnO2@L-MnO2 heteroepitaxy, which, with supported trace Pt nanoparticles, shows enhanced room-temperature HCHO oxidation.Download high-res image (100KB)Download full-size image
Co-reporter:Le Yu;Buyuan Guan;Xiong Wen (David) Lou
Advanced Energy Materials 2015 Volume 5( Issue 21) pp:
Publication Date(Web):
DOI:10.1002/aenm.201500981

Yolk-shelled particles with tailored physical and chemical properties are attractive for electrochemical energy storage. Starting with metal acetate hydroxide with tetragonal prism-like shapes, yolk-shelled Ni–Co mixed oxide nanoprisms with tunable composition have been prepared by simple thermal annealing in air. It is found that the yolk-shelled structure is formed due to the fast thermally driven contraction process. With the favorable porous structure and composition, these yolk-shelled Ni–Co oxide particles manifest greatly enhanced electrochemical properties when evaluated as electrodes for both hybrid supercapacitors and lithium ion batteries. In particular, the resultant Ni0.37Co oxide sample delivers very high specific capacitance of over 1000 F g−1 at a current density of 10 A g−1 with remarkably high capacitance retention of 98% after 15 000 cycles.

Co-reporter:Huayi Yin, Wei Xiao, Xuhui Mao, Hua Zhu and Dihua Wang  
Journal of Materials Chemistry A 2015 vol. 3(Issue 4) pp:1427-1430
Publication Date(Web):25 Nov 2014
DOI:10.1039/C4TA05244G
We present here a controllable and affordable preparation of porous nanostructured germaniums with interesting photo-responsive properties from GeO2 powder through an electrochemical reduction–alloying process in molten salt (reduction and alloying) and post zero-energy-consumption water etching (dealloying).
Co-reporter:Huayi Yin, Diyong Tang, Xuhui Mao, Wei Xiao and Dihua Wang  
Journal of Materials Chemistry A 2015 vol. 3(Issue 29) pp:15184-15189
Publication Date(Web):01 Jul 2015
DOI:10.1039/C5TA03728J
The use of lightweight elements/compounds and the employment of multi-electron reaction (MER) chemistry are two approaches used to develope high energy density materials for batteries. In this work, nanoscaled calcium hexaboride (CaB6) was prepared in one-step by the electro-reduction of solid calcium borate (CaB2O4) in molten CaCl2–NaCl. CaB2O4 was synthesized by a simple co-precipitation method. It was revealed that the electrolytic CaB6 delivers a specific capacity of 2400 mA h g−1 in 30% KOH solution though a multi-electron reaction mechanism. Its practical gravimetric energy is three times that of Zn. Decrease of particle size substantially improves both the electrochemical activity and discharge capacity of CaB6. The electrolysis of CaB2O4 in molten salt provides a straightforward and sustainable way to prepare high-capacity CaB6 using low-cost and environmentally friendly boron and calcium resources, which can be recycled from the used CaB6 primary batteries.
Co-reporter:Beihu Lu, Zuoan Xiao, Hua Zhu, Wei Xiao, Wenlong Wu, Dihua Wang
Journal of Power Sources 2015 Volume 298() pp:74-82
Publication Date(Web):1 December 2015
DOI:10.1016/j.jpowsour.2015.08.047
•Commercial activated carbons are re-activated in molten carbonates.•The origin and re-activated carbons are evaluated for supercapacitor.•Activated carbons after molten carbonate treatment show enhanced capacitive performance.•Rationalizations on mechanism and structure-activity correlations are provided.Simple, affordable and green methods to improve capacitive properties of commercial activated carbon (AC) are intriguing since ACs possess a predominant role in the commercial supercapacitor market. Herein, we report a green reactivation of commercial ACs by soaking ACs in molten Na2CO3–K2CO3 (equal in mass ratios) at 850 °C combining the merits of both physical and chemical activation strategies. The mechanism of molten carbonate treatment and structure-capacitive activity correlations of the ACs are rationalized. Characterizations show that the molten carbonate treatment increases the electrical conductivity of AC without compromising its porosity and wettability of electrolytes. Electrochemical tests show the treated AC exhibited higher specific capacitance, enhanced high-rate capability and excellent cycle performance, promising its practical application in supercapacitors. The present study confirms that the molten carbonate reactivation is a green and effective method to enhance capacitive properties of ACs.
Co-reporter:Liu Pi, Rui Jiang, Wangchi Zhou, Hua Zhu, Wei Xiao, Dihua Wang, Xuhui Mao
Applied Surface Science 2015 Volume 358(Part A) pp:231-239
Publication Date(Web):15 December 2015
DOI:10.1016/j.apsusc.2015.08.176

Highlights

Composite material consisting of photo-responsive C3N4 and biochar was studied.

Interconnection of C3N4 and biochar was fulfilled via a condensation reaction.

The adsorption properties of composite were governed by the biochar.

The composite exhibited decontamination capability even after saturated.

Adsorption and photo-induced regeneration were mutual beneficial in composite.

Co-reporter:Jing Zhou, Han Xiao, Bowen Zhou, Feifan Huang, Shoubin Zhou, Wei Xiao, Dihua Wang
Applied Surface Science 2015 Volume 358(Part A) pp:152-158
Publication Date(Web):15 December 2015
DOI:10.1016/j.apsusc.2015.07.187

Highlights

Hierarchical MoS2–rGO nanosheets with high MoS2 loading were prepared.

GO facilitates formation of well-dispersed ultrathin MoS2 nanosheets.

Enhanced HER and ORR activities are obtained in the hybrid material.

Rationalizations of structural and compositional natures on properties are performed.

Co-reporter:Yin Xu, Haochen Jiang, Xiaoxiao Li, Han Xiao, Wei Xiao and Tian Wu  
Journal of Materials Chemistry A 2014 vol. 2(Issue 33) pp:13345-13351
Publication Date(Web):18 Jun 2014
DOI:10.1039/C4TA02544J
Implementation of non-precious electrocatalysts towards the oxygen reduction reaction (ORR) is the central focus for fulfilling cost-affordable and high-performance fuel cells and metal/air batteries. Herein, we report a modified solvothermal approach for the preparation of composite carbonates between Mn and X (X = Co, Ni and Fe). Upon post-annealing treatment, the aforementioned carbonates are transformed into the corresponding micro/nano hierarchical structured mixed oxides with increased porosity. It is found that onion-like core–shell architectures appear in the Mn–Co and Mn–Ni systems because of volume shrinkage arising from the generation of chemical-level mixed oxides, while a less porous structure occurs in the Mn–Fe system with the formation of a physical-level mixture. The ORR activity of the prepared composite oxides in alkaline media is investigated by voltammetry under different hydrodynamic conditions. An enhanced ORR activity is observed in the Mn–Co mixed oxide, which is rationalized in terms of the unique microstructure and crystallographic phase. The present study suggests that proper mixing is an effective method for activating the ORR activity of manganese oxides, which is beneficial for developing non-precious electrocatalysts for fuel cells and metal/air batteries.
Co-reporter:Ying Wang, Jiaguo Yu, Wei Xiao and Qin Li  
Journal of Materials Chemistry A 2014 vol. 2(Issue 11) pp:3847-3855
Publication Date(Web):03 Feb 2014
DOI:10.1039/C3TA14908K
The construction and application of visible-light-driven photocatalysts falls in the central focus for the efficient utilization of renewable solar energy, which provides unprecedented opportunities for addressing the increasing concerns on energy and environmental sustainability. Herein, graphene based Au–TiO2 photocatalysts were fabricated by a simple, one-step microwave-assisted hydrothermal method, using Degussa P25 TiO2 powder (P25), graphene oxide and HAuCl4 aqueous solution as the raw materials. The effects of graphene introduction and gold loading on the photocatalytic hydrogen production rates of the as-prepared samples in a methanolic aqueous solution were investigated. The results indicated that Au–TiO2–graphene composite had a significantly increased visible light absorption and enhanced photocatalytic H2-production activity compared to the Au–TiO2 composite. In comparison, the pure TiO2, graphene–TiO2 and graphene–Au had no appreciable visible-light-driven H2 production. The enhanced photocatalytic H2-production activity of the Au–TiO2–graphene composite is ascribed to (1) the load of the Au nanoparticles which broadens the visible light response of TiO2 due to the surface plasmon resonance (SPR) effect, and (2) the introduction of graphene, which functions as rapid electron transfer units, facilitating the space separation of photoelectron and hole pairs. The proposed H2-production activity enhancement mechanism was further confirmed by the transient photocurrent response and electrochemical impedance spectroscopy (EIS) experiments.
Co-reporter:Jiaguo Yu, Ke Wang, Wei Xiao and Bei Cheng  
Physical Chemistry Chemical Physics 2014 vol. 16(Issue 23) pp:11492-11501
Publication Date(Web):17 Apr 2014
DOI:10.1039/C4CP00133H
Photocatalytic reduction of CO2 into renewable hydrocarbon fuels is an alternative way to develop reproducible energy, which is also a promising way to solve the problem of the greenhouse effect. In this work, graphitic carbon nitride (g-C3N4) was synthesized by directly heating thiourea at 550 °C and then a certain amount of Pt was deposited on it to form g-C3N4–Pt nanocomposites used as catalysts for photocatalytic reduction of CO2 under simulated solar irradiation. The main products of photocatalysis were CH4, CH3OH and HCHO. The deposited Pt acted as an effective cocatalyst, which not only influenced the selectivity of the product generation, but also affected the activity of the reaction. The yield of CH4 first increased upon increasing the amount of Pt deposited on the g-C3N4 from 0 to 1 wt%, then decreased at 2 wt% Pt loading. The production rates of CH3OH and HCHO also increased with the content of Pt increasing from 0 to 0.75 wt% and the maximum yield was observed at 0.75 wt%. The Pt nanoparticles (NPs) could facilitate the transfer and enrichment of photogenerated electrons from g-C3N4 to its surface for photocatalytic reduction of CO2. At the same time, Pt was also used a catalyst to promote the oxidation of products. The transient photocurrent response further confirmed the proposed photocatalytic reduction mechanism of CO2. This work indicates that the deposition of Pt is a good strategy to improve the photoactivity and selectivity of g-C3N4 for CO2 reduction.
Co-reporter:Feiyan Xu, Wei Xiao, Bei Cheng, Jiaguo Yu
International Journal of Hydrogen Energy 2014 Volume 39(Issue 28) pp:15394-15402
Publication Date(Web):23 September 2014
DOI:10.1016/j.ijhydene.2014.07.166
•Anatase and rutile bi-phase TiO2 nanofibers with changing rutile content prepared.•Bi-phase TiO2 nanofibers exhibited the enhanced H2-production performance.•A Z-scheme photocatalytic mechanism first proposed to explain the enhanced activity.Design and preparation of direct Z-scheme anatase/rutile TiO2 nanofiber photocatalyst to enhance photocatalytic H2-production activity via water splitting is of great importance from both theoretical and practical viewpoints. Herein, we develop a facile method for preparing anatase and rutile bi-phase TiO2 nanofibers with changing rutile content via a slow and rapid cooling of calcined electrospun TiO2 nanofibers. The phase structure and composition, surface morphology, specific surface area, surface chemical composition and element chemical states of TiO2 nanofibers were analyzed by X-ray powder diffraction (XRD), field emission scanning electron microscopy (FESEM), high-resolution transmission electron microscopy (HRTEM), nitrogen adsorption and X-ray photoelectron spectroscopy (XPS). By a rapid cooling of 500 °C-calcined electrospun TiO2 precursor, anatase/rutile bi-phase TiO2 nanofibers with a roughly equal weight ratio of 55 wt.% anatase and 45 wt.% rutile were prepared. The enhanced H2 production performance was observed in the above obtained anatase/rutile composite TiO2 nanofibers. A Z-scheme photocatalytic mechanism is first proposed to explain the enhanced photocatalytic H2-production activity of anatase/rutile bi-phase TiO2 nanofibers, which is different from the traditional heterojunction electron–hole separation mechanism. This report highlights the importance of phase structure and composition on optimizing photocatalytic activity of TiO2-based material.Direct Z-scheme anatase/rutile bi-phase TiO2 nanofiber photocatalyst, prepared by rapid cooling of calcined electrospun TiO2 nanofiber, exhibits enhanced H2-production activity.
Co-reporter:Dr. Qin Li;Huan Meng; Jiaguo Yu; Wei Xiao;Yingqiu Zheng;Juan Wang
Chemistry - A European Journal 2014 Volume 20( Issue 4) pp:1176-1185
Publication Date(Web):
DOI:10.1002/chem.201303446

Abstract

In response to the increasing concerns over energy and environmental sustainability, photocatalytic water-splitting technology has attracted broad attention for its application in directly converting solar energy to valuable hydrogen (H2) energy. In this study, high-efficiency visible-light-driven photocatalytic H2 production without the assistance of precious-metal cocatalysts was achieved on graphene–ZnxCd1−xS composites with controlled compositions. The graphene-ZnxCd1−xS composites were for the first time fabricated by a one-step hydrothermal method with thiourea as an organic S source. It was found that thiourea facilitates heterogeneous nucleation of ZnxCd1−xS and in situ growth of ZnxCd1−xS nanoparticles on graphene nanosheets. Such a scenario results in abundant and intimate interfacial contact between graphene and ZnxCd1−xS nanoparticles, efficient transfer of the photogenerated charge carriers, and enhanced photocatalytic activity for H2 production. The highest H2-production rate of 1.06 mmol h−1 g−1 was achieved on a graphene–Zn0.5Cd0.5S composite photocatalyst with a graphene content of 0.5 wt %, and the apparent quantum efficiency was 19.8 % at 420 nm. In comparison, the graphene–ZnxCd1−xS composite photocatalyst prepared by using an inorganic S source such as Na2S exhibited much lower activity for photocatalytic H2 production. In this case, homogeneous nucleation of ZnxCd1−xS becomes predominant and results in insufficient and loose contact with the graphene backbone through weak van der Waals forces and a large particle size. This study highlights the significance of the choice of S source in the design and fabrication of advanced graphene-based sulfide photocatalytic materials with enhanced activity for photocatalytic H2 production.

Co-reporter:Jiaguo Yu, Ying Wang and Wei Xiao  
Journal of Materials Chemistry A 2013 vol. 1(Issue 36) pp:10727-10735
Publication Date(Web):27 Jun 2013
DOI:10.1039/C3TA12218B
Ordered rutile TiO2 nanorods grown on transparent electro-conductive F-doped SnO2-coated (FTO) glass substrates were prepared by a simple hydrothermal method using tetrabutyl titanate as the precursor and then calcined at various temperatures. The prepared SnO2/TiO2 composite film samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The photoelectrocatalytic (PEC) activity was evaluated by PEC degradation of methylene blue (MB) aqueous solutions under UV-LED light irradiation. The results showed that rutile TiO2 nanorods with diameters of ca. 300–700 nm and lengths of ca. 5 μm vertically grew on the FTO substrate. The resulting rutile TiO2 arrays exhibited excellent stability upon annealing in a temperature range of 300–500 °C. The sample calcined at 400 °C exhibited the highest PEC activity due to the combined effects of several factors including its one-dimensional morphology, high crystallinity, close contact between the TiO2 nanorods and SnO2 layers, SnO2/TiO2 n–n heterojunction and the applied external electrostatic field. The proposed enhanced PEC mechanism was further confirmed by the transient photocurrent response and electrochemical impedance spectroscopy (EIS) experiments.
Co-reporter:Ruixue Chen, Jiaguo Yu and Wei Xiao  
Journal of Materials Chemistry A 2013 vol. 1(Issue 38) pp:11682-11690
Publication Date(Web):24 Jul 2013
DOI:10.1039/C3TA12589K
Hierarchically porous manganese dioxide (MnO2) microspheres were fabricated by a facile hydrothermal method using potassium permanganate as the precursor at different hydrothermal temperatures. The as-prepared samples were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), nitrogen adsorption–desorption isotherms and Fourier transform infrared (FTIR) spectroscopy. Adsorption of methyl blue (MB) onto the as-prepared samples from aqueous solutions was investigated and discussed. It was found that MnO2 microspheres were composed of two levels of hierarchical porous organization, viz., mesopores (2–50 nm) and macropores (>50 nm). The equilibrium adsorption data of MB on the as-prepared samples was well fitted with the Freundlich isotherm model. The sample obtained at 80 °C displayed the highest adsorption capacity with 259.2 mg g−1. In addition, adsorption data were fitted using the pseudo-second-order kinetics equation, suggesting that pseudo-second-order kinetics could well represent the adsorption kinetics. The adsorption between MB and MnO2 was mainly attributed to the strong electrostatic attraction force. The as-prepared hierarchically porous MnO2 microspheres turned out to be an effective adsorbent for the removal of MB from effluent because of their unique hierarchical porous microstructure and high specific surface areas.
Co-reporter:Peng Zhou, Xiaofeng Zhu, Jiaguo Yu, and Wei Xiao
ACS Applied Materials & Interfaces 2013 Volume 5(Issue 16) pp:8165
Publication Date(Web):August 5, 2013
DOI:10.1021/am402246b
Formaldehyde (HCHO), as the main indoor air pollutant, is highly needed to be removed by adsorption or catalytic oxidation from the indoor air. Herein, the F–, OH–, and Cl–-modified anatase TiO2 nanosheets (TNS) with exposed {001} facets were prepared by a simple hydrothermal and post-treatment method, and their HCHO adsorption performance and mechanism were investigated by the experimental analysis and theoretical simulations. Our results indicated that the adsorbed F–, OH–, and Cl– ions all could weaken the interaction between the HCHO and TNS surface, leading to the serious reduction of HCHO adsorption performance of TNS. However, different from F– and Cl– ions, OH– ion could induce the dissociative adsorption of HCHO by capturing one H atom from HCHO, resulting in the formation of one formyl group and one H2O-like group. This greatly reduced the total energy of the HCHO adsorption system. Thus, the adsorbed OH– ions could provide the additional active centers for HCHO adsorption. As a result, the NaOH-treated TNS showed the best HCHO adsorption performance mainly because its surface F– was replaced by OH–. This study will provide new insight into the design and fabrication of high performance adsorbents for removing indoor HCHO and, also, will enhance the understanding of the HCHO adsorption mechanism.Keywords: adsorption performance; dissociative adsorption; F ions; formaldehyde; hydroxyl group; TiO2 nanosheets;
Co-reporter:Jiaguo Yu, Xinyang Li, Zhihua Xu, and Wei Xiao
Environmental Science & Technology 2013 Volume 47(Issue 17) pp:9928-9933
Publication Date(Web):July 29, 2013
DOI:10.1021/es4019892
NaOH-modified ceramic honeycombs (Na–CH) were simply prepared by impregnating ceramic honeycombs (CH) into NaOH aqueous solution. It was clearly shown that the surface modification incurs higher specific surface area and smaller grain sizes of the CH without destruction of their integrity. Moreover, the introduced surface NaOH can trigger Cannizzaro disproportionation of surface-absorbed formaldehyde (HCHO) on Na–CH, resulting in catalytic transformation of HCHO into less-toxic formate and methoxy salts. The NaOH concentration during impregnating treatment has a great influence on HCHO adsorption and removal efficiency, while the impregnation time and temperature have little influence on the efficiency. When the CH was impregnated in 1 M NaOH aqueous solution for 0.5 h at room temperature, the HCHO removal efficiency at ambient temperature can reach about 80% with an initial HCHO concentration of 250 ppm. Moreover, the used Na–CH can be facilely regenerated via 1 min blow using a common electric hair dryer, with the generation of less toxic HCOOH and CH3OH and recovery of NaOH. Using such a mild, fast, and practical regeneration method, the regenerated Na–CH showed slight degradation in adsorption and removal capability toward HCHO. The enhanced performance of Na–CH obtained was attributed to the presence of NaOH and increase of specific surface area and surface hydroxyl groups. Considering no demand of noble metal for HCHO removal at ambient temperature and practical reusable capability of Na–CH under mild conditions, this work may provide some new insights into the design and fabrication of advanced catalysts for indoor air purification.
Co-reporter:Jiaguo Yu, Shuhan Wang, Jingxiang Low and Wei Xiao  
Physical Chemistry Chemical Physics 2013 vol. 15(Issue 39) pp:16883-16890
Publication Date(Web):14 Aug 2013
DOI:10.1039/C3CP53131G
Formaldehyde (HCHO) is a major indoor pollutant and long-term exposure to HCHO may cause health problems such as nasal tumors and skin irritation. Photocatalytic oxidation is considered as the most promising strategy for the decomposition of HCHO. Herein, for the first time, a direct g-C3N4–TiO2 Z-scheme photocatalyst without an electron mediator was prepared by a facile calcination route utilizing affordable P25 and urea as the feedstocks. Photocatalytic activities of the as-prepared samples were evaluated by the photocatalytic oxidation decomposition of HCHO in air. It was shown that the photocatalytic activity of the prepared Z-scheme photocatalysts was highly dependent on the g-C3N4 content. At the optimal g-C3N4 content (sample U100 in this study), the apparent reaction rate constant was 7.36 × 10−2 min−1 for HCHO decomposition, which exceeded that of pure P25 (3.53 × 10−2 min−1) by a factor of 2.1. The enhanced photocatalytic activity could be ascribed to the formation of a g-C3N4–TiO2 Z-scheme photocatalyst, which results in the efficient space separation of photo-induced charge carriers. Considering the ease of the preparation method, this work will provide new insights into the design of high-performance Z-scheme photocatalysts for indoor air purification.
Co-reporter:Dr. Zhihua Xu; Jiaguo Yu;Dr. Wei Xiao
Chemistry - A European Journal 2013 Volume 19( Issue 29) pp:9592-9598
Publication Date(Web):
DOI:10.1002/chem.201300438

Abstract

Mesoporous ferrihydrite/SiO2 composites were synthesized according to a water-in-oil microemulsion method and characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, thermogravimetry, nitrogen-adsorption/desorption, and by X-ray photoelectron spectroscopy. The as-prepared porous ferrihydrite/SiO2 composites showed an excellent adsorption performance for formaldehyde (HCHO) removal from indoor air at ambient temperature. It was found that the aging time during the synthesis had a significant impact on the pore structure, surface area, and HCHO adsorption of these materials. The ferrihydrite/SiO2 composite that was aged for 3 h in the presence of tetraethyl orthosilicate (TEOS) exhibited a relatively high HCHO adsorption capacity, as well as good recyclability, which was attributed to a relatively large BET surface area, optimal pore size, a suitable Si/Fe atomic ratio, and a synergistic effect between ferrihydrite and SiO2. This work not only demonstrates that porous ferrihydrite/SiO2 composites can act as an efficient adsorbent toward HCHO, but suggests a new route for the rational design of cost-effective and environmentally benign adsorbents with high performance for indoor air purification.

Co-reporter:Huayi Yin, Wei Xiao, Xuhui Mao, Hua Zhu and Dihua Wang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 4) pp:NaN1430-1430
Publication Date(Web):2014/11/25
DOI:10.1039/C4TA05244G
We present here a controllable and affordable preparation of porous nanostructured germaniums with interesting photo-responsive properties from GeO2 powder through an electrochemical reduction–alloying process in molten salt (reduction and alloying) and post zero-energy-consumption water etching (dealloying).
Co-reporter:Ruixue Chen, Jiaguo Yu and Wei Xiao
Journal of Materials Chemistry A 2013 - vol. 1(Issue 38) pp:NaN11690-11690
Publication Date(Web):2013/07/24
DOI:10.1039/C3TA12589K
Hierarchically porous manganese dioxide (MnO2) microspheres were fabricated by a facile hydrothermal method using potassium permanganate as the precursor at different hydrothermal temperatures. The as-prepared samples were characterized by X-ray diffraction (XRD), field-emission scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), nitrogen adsorption–desorption isotherms and Fourier transform infrared (FTIR) spectroscopy. Adsorption of methyl blue (MB) onto the as-prepared samples from aqueous solutions was investigated and discussed. It was found that MnO2 microspheres were composed of two levels of hierarchical porous organization, viz., mesopores (2–50 nm) and macropores (>50 nm). The equilibrium adsorption data of MB on the as-prepared samples was well fitted with the Freundlich isotherm model. The sample obtained at 80 °C displayed the highest adsorption capacity with 259.2 mg g−1. In addition, adsorption data were fitted using the pseudo-second-order kinetics equation, suggesting that pseudo-second-order kinetics could well represent the adsorption kinetics. The adsorption between MB and MnO2 was mainly attributed to the strong electrostatic attraction force. The as-prepared hierarchically porous MnO2 microspheres turned out to be an effective adsorbent for the removal of MB from effluent because of their unique hierarchical porous microstructure and high specific surface areas.
Co-reporter:Jiaguo Yu, Shuhan Wang, Jingxiang Low and Wei Xiao
Physical Chemistry Chemical Physics 2013 - vol. 15(Issue 39) pp:NaN16890-16890
Publication Date(Web):2013/08/14
DOI:10.1039/C3CP53131G
Formaldehyde (HCHO) is a major indoor pollutant and long-term exposure to HCHO may cause health problems such as nasal tumors and skin irritation. Photocatalytic oxidation is considered as the most promising strategy for the decomposition of HCHO. Herein, for the first time, a direct g-C3N4–TiO2 Z-scheme photocatalyst without an electron mediator was prepared by a facile calcination route utilizing affordable P25 and urea as the feedstocks. Photocatalytic activities of the as-prepared samples were evaluated by the photocatalytic oxidation decomposition of HCHO in air. It was shown that the photocatalytic activity of the prepared Z-scheme photocatalysts was highly dependent on the g-C3N4 content. At the optimal g-C3N4 content (sample U100 in this study), the apparent reaction rate constant was 7.36 × 10−2 min−1 for HCHO decomposition, which exceeded that of pure P25 (3.53 × 10−2 min−1) by a factor of 2.1. The enhanced photocatalytic activity could be ascribed to the formation of a g-C3N4–TiO2 Z-scheme photocatalyst, which results in the efficient space separation of photo-induced charge carriers. Considering the ease of the preparation method, this work will provide new insights into the design of high-performance Z-scheme photocatalysts for indoor air purification.
Co-reporter:Jiaguo Yu, Ke Wang, Wei Xiao and Bei Cheng
Physical Chemistry Chemical Physics 2014 - vol. 16(Issue 23) pp:NaN11501-11501
Publication Date(Web):2014/04/17
DOI:10.1039/C4CP00133H
Photocatalytic reduction of CO2 into renewable hydrocarbon fuels is an alternative way to develop reproducible energy, which is also a promising way to solve the problem of the greenhouse effect. In this work, graphitic carbon nitride (g-C3N4) was synthesized by directly heating thiourea at 550 °C and then a certain amount of Pt was deposited on it to form g-C3N4–Pt nanocomposites used as catalysts for photocatalytic reduction of CO2 under simulated solar irradiation. The main products of photocatalysis were CH4, CH3OH and HCHO. The deposited Pt acted as an effective cocatalyst, which not only influenced the selectivity of the product generation, but also affected the activity of the reaction. The yield of CH4 first increased upon increasing the amount of Pt deposited on the g-C3N4 from 0 to 1 wt%, then decreased at 2 wt% Pt loading. The production rates of CH3OH and HCHO also increased with the content of Pt increasing from 0 to 0.75 wt% and the maximum yield was observed at 0.75 wt%. The Pt nanoparticles (NPs) could facilitate the transfer and enrichment of photogenerated electrons from g-C3N4 to its surface for photocatalytic reduction of CO2. At the same time, Pt was also used a catalyst to promote the oxidation of products. The transient photocurrent response further confirmed the proposed photocatalytic reduction mechanism of CO2. This work indicates that the deposition of Pt is a good strategy to improve the photoactivity and selectivity of g-C3N4 for CO2 reduction.
Co-reporter:Jiaguo Yu, Ying Wang and Wei Xiao
Journal of Materials Chemistry A 2013 - vol. 1(Issue 36) pp:NaN10735-10735
Publication Date(Web):2013/06/27
DOI:10.1039/C3TA12218B
Ordered rutile TiO2 nanorods grown on transparent electro-conductive F-doped SnO2-coated (FTO) glass substrates were prepared by a simple hydrothermal method using tetrabutyl titanate as the precursor and then calcined at various temperatures. The prepared SnO2/TiO2 composite film samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). The photoelectrocatalytic (PEC) activity was evaluated by PEC degradation of methylene blue (MB) aqueous solutions under UV-LED light irradiation. The results showed that rutile TiO2 nanorods with diameters of ca. 300–700 nm and lengths of ca. 5 μm vertically grew on the FTO substrate. The resulting rutile TiO2 arrays exhibited excellent stability upon annealing in a temperature range of 300–500 °C. The sample calcined at 400 °C exhibited the highest PEC activity due to the combined effects of several factors including its one-dimensional morphology, high crystallinity, close contact between the TiO2 nanorods and SnO2 layers, SnO2/TiO2 n–n heterojunction and the applied external electrostatic field. The proposed enhanced PEC mechanism was further confirmed by the transient photocurrent response and electrochemical impedance spectroscopy (EIS) experiments.
Co-reporter:Ying Wang, Jiaguo Yu, Wei Xiao and Qin Li
Journal of Materials Chemistry A 2014 - vol. 2(Issue 11) pp:NaN3855-3855
Publication Date(Web):2014/02/03
DOI:10.1039/C3TA14908K
The construction and application of visible-light-driven photocatalysts falls in the central focus for the efficient utilization of renewable solar energy, which provides unprecedented opportunities for addressing the increasing concerns on energy and environmental sustainability. Herein, graphene based Au–TiO2 photocatalysts were fabricated by a simple, one-step microwave-assisted hydrothermal method, using Degussa P25 TiO2 powder (P25), graphene oxide and HAuCl4 aqueous solution as the raw materials. The effects of graphene introduction and gold loading on the photocatalytic hydrogen production rates of the as-prepared samples in a methanolic aqueous solution were investigated. The results indicated that Au–TiO2–graphene composite had a significantly increased visible light absorption and enhanced photocatalytic H2-production activity compared to the Au–TiO2 composite. In comparison, the pure TiO2, graphene–TiO2 and graphene–Au had no appreciable visible-light-driven H2 production. The enhanced photocatalytic H2-production activity of the Au–TiO2–graphene composite is ascribed to (1) the load of the Au nanoparticles which broadens the visible light response of TiO2 due to the surface plasmon resonance (SPR) effect, and (2) the introduction of graphene, which functions as rapid electron transfer units, facilitating the space separation of photoelectron and hole pairs. The proposed H2-production activity enhancement mechanism was further confirmed by the transient photocurrent response and electrochemical impedance spectroscopy (EIS) experiments.
Co-reporter:Yin Xu, Haochen Jiang, Xiaoxiao Li, Han Xiao, Wei Xiao and Tian Wu
Journal of Materials Chemistry A 2014 - vol. 2(Issue 33) pp:NaN13351-13351
Publication Date(Web):2014/06/18
DOI:10.1039/C4TA02544J
Implementation of non-precious electrocatalysts towards the oxygen reduction reaction (ORR) is the central focus for fulfilling cost-affordable and high-performance fuel cells and metal/air batteries. Herein, we report a modified solvothermal approach for the preparation of composite carbonates between Mn and X (X = Co, Ni and Fe). Upon post-annealing treatment, the aforementioned carbonates are transformed into the corresponding micro/nano hierarchical structured mixed oxides with increased porosity. It is found that onion-like core–shell architectures appear in the Mn–Co and Mn–Ni systems because of volume shrinkage arising from the generation of chemical-level mixed oxides, while a less porous structure occurs in the Mn–Fe system with the formation of a physical-level mixture. The ORR activity of the prepared composite oxides in alkaline media is investigated by voltammetry under different hydrodynamic conditions. An enhanced ORR activity is observed in the Mn–Co mixed oxide, which is rationalized in terms of the unique microstructure and crystallographic phase. The present study suggests that proper mixing is an effective method for activating the ORR activity of manganese oxides, which is beneficial for developing non-precious electrocatalysts for fuel cells and metal/air batteries.
Co-reporter:Huayi Yin, Diyong Tang, Xuhui Mao, Wei Xiao and Dihua Wang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 29) pp:NaN15189-15189
Publication Date(Web):2015/07/01
DOI:10.1039/C5TA03728J
The use of lightweight elements/compounds and the employment of multi-electron reaction (MER) chemistry are two approaches used to develope high energy density materials for batteries. In this work, nanoscaled calcium hexaboride (CaB6) was prepared in one-step by the electro-reduction of solid calcium borate (CaB2O4) in molten CaCl2–NaCl. CaB2O4 was synthesized by a simple co-precipitation method. It was revealed that the electrolytic CaB6 delivers a specific capacity of 2400 mA h g−1 in 30% KOH solution though a multi-electron reaction mechanism. Its practical gravimetric energy is three times that of Zn. Decrease of particle size substantially improves both the electrochemical activity and discharge capacity of CaB6. The electrolysis of CaB2O4 in molten salt provides a straightforward and sustainable way to prepare high-capacity CaB6 using low-cost and environmentally friendly boron and calcium resources, which can be recycled from the used CaB6 primary batteries.
Nickel alloy
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