Co-reporter:Cuncai Lv, Zhen Peng, Yaoxing Zhao, Zhipeng Huang and Chi Zhang
Journal of Materials Chemistry A 2016 vol. 4(Issue 4) pp:1454-1460
Publication Date(Web):22 Dec 2015
DOI:10.1039/C5TA08715E
The development of an effective, non-precious electrocatalyst for the hydrogen evolution reaction (HER) is highly desirable for the commercial application of hydrogen as a clean and renewable energy and remains a substantial challenge. Herein, a hierarchical nanowires array (HNA) of iron phosphide (FeP) nanowires coated with iron phosphide nanorods grown on a carbon fiber paper (CFP) was constructed which exhibited remarkable catalytic activity in the HER. The overpotential required for the current density of 20 mA cm−2 is as small as 45 and 221 mV in acidic and basic solution, respectively, corresponding to Tafel slopes of 53 and 134 mV dec−1. The effective catalytic activity of the CFP–FeP HNA in the HER, together with its long-term stability and nearly 100% faradaic efficiency in water electrolysis, make the CFP–FeP HNA one of the best non-noble electrocatalysts described to date. The prominent catalytic activity of CFP–FeP HNA is correlated to the large number of active sites for the HER, and the fast electron transport from the CFP to the FeP nanorods mediated by FeP nanowires.
Co-reporter:Lingliang Long, Yanjun Wu, Lin Wang, Aihua Gong, Rongfeng Hu, Chi Zhang
Analytica Chimica Acta 2016 Volume 908() pp:1-7
Publication Date(Web):18 February 2016
DOI:10.1016/j.aca.2015.12.016
•A novel design strategy for developing fluorescent sensors with zero background signals has been demonstrated.•As proof-of-principle study, a fluorescence sensor for Cu2+ has been developed.•Upon treatment with Cu2+, fluorescence intensity of the sensor enhanced up to 811-fold.•The sensor can be utilized as a simple tool to detect different concentration of Cu2+ in water samples and living cells.The reaction-based fluorescent sensors have attracted increasing attention in the past decades. However, the application of these sensors for accurate sensing was significantly retarded by the background fluorescence from the sensors themselves. In this work, we demonstrated a novel strategy that the background fluorescence of the sensor could be completely eliminated by the combined effect of multiple fluorescence quenching groups. Based on this new strategy, as proof-of-principle study, a fluorescent sensor (CuFS) for Cu2+ was judiciously developed. In CuFS, three types of fluorescence quenching groups were directly tethered to a commonly used coumarin fluorophore. The fluorescence of coumarin fluorophore in CuFS was completely suppressed by the combined effect of these fluorescence quenching groups. Upon treatment with 22 μM Cu2+, sensor CuFS achieved a dramatic fluorescence enhancement (fluorescence intensity enhanced up to 811-fold) centered at 469 nm. The detection limits was determined to be 12.3 nM. The fluorescence intensity enhancement also showed a good linearity with the Cu2+ concentration in the range of 12.3 nM to 2 μM. By fabricating test strips, sensor CuFS can be utilized as a simple tool to detect Cu2+ in water samples. Furthermore, the fluorescent sensor was successfully applied in detecting different concentration of Cu2+ in living cells.
Co-reporter:Jinhui Hao;Wenshu Yang;Zhipeng Huang
Advanced Materials Interfaces 2016 Volume 3( Issue 16) pp:
Publication Date(Web):
DOI:10.1002/admi.201600236
Bifunctional, binder-free, and non-precious-metal electrocatalysts with superwetting properties are of great significance for high-performance oxygen evolution reactions (OER) and hydrogen evolution reactions (HER). Herein, the fabrication of copper phosphide (Cu3P) microsheets through the phosphidation of CuCl microsheets deposited onto nickel foam, and the effective catalytic activity of the Cu3P microsheets in the HER and OER is demonstrated. Due to their hierarchical structure, the Cu3P microsheets are superhydrophilic and superaerophobic. A well-defined superhydrophilic surface enhances the electrolyte–electrode contact, and a superaerophobic surface facilitates bubbles extraction and efficiently minimizes the dead area of the electrode induced by bubble coverage. These two features are beneficial for the high activity and stability of the electrocatalysts during the OER and HER. The superhydrophilic and superaerophobic Cu3P microsheets prepared at 450 °C afford a current density of 10 mA cm–2 at an overpotential of 290 mV for the OER and 130 mV for the HER. This work highlights a simple, low-cost approach that can be easily scaled-up to construct high-performance electrocatalysts for the OER and HER.
Co-reporter:Qiang Zhou, Jun Qian, Chi Zhang
Journal of Molecular Structure 2016 Volume 1119() pp:340-345
Publication Date(Web):5 September 2016
DOI:10.1016/j.molstruc.2016.04.034
•Three interesting coordination compounds based on metalloligand and alkaline-earth ions have been synthesized.•The structures of the prepared compounds have been investigated by different spectroscopic techniques.•The magnetic property of coordination compound 2 has been studied.Based on metalloligand LCu ([Cu(2,4-pydca)2]2−, 2,4-pydca2− = pyridine-2,4-dicarboxylate) and alkaline-earth ions (Ca2+, Sr2+, and Ba2+), three interesting coordination compounds, [Ca(H2O)7][LCu·H2O]·H2O (1), {Sr[LCu·H2O]·4H2O}n (2), and {Ba[LCu·H2O]·8H2O}n (3), have been synthesized and well-characterized by elemental analysis, infrared spectroscopy, thermogravimetric and single-crystal X-ray diffraction analysis. X-ray crystallographic studies reveal that 1 features a discrete 0D coordination compound, while 2 and 3 exhibit the 2D network and 1D chain structures, respectively. Compound 2 is constructed from {LCu}2 dimers connected with {Sr2} units, which is fabricated by two Sr2+ ions bridged via two μ2-O bridges, while compound 3 is formed by 1D {Ba}n chain linked with metalloligands LCu and exhibits an interesting sandwich like chain structure. It is noted that the coordination numbers of alkaline-earth ions are in positive correlation with their radiuses. Moreover, the magnetic property of compound 2 has been studied.The reaction of metalloligand LCu and alkaline-earth ions (Ca2+, Sr2+, and Ba2+) gave rise to three interesting coordination compounds, [Ca(H2O)7][LCu·H2O]·H2O (1), {Sr[LCu·H2O]·4H2O}n (2), and {Ba[LCu·H2O]·8H2O}n (3), which exhibit discrete, 2D net, and 1D chain structures, respectively. All three compounds have been well-characterized by elemental analysis, infrared spectroscopy, thermogravimetric and single-crystal X-ray diffraction analysis. The magnetic property of compound 2 has also been studied.
Co-reporter:Cuncai Lv, Zhibo Chen, Zhongzhong Chen, Bin Zhang, Yong Qin, Zhipeng Huang and Chi Zhang
Journal of Materials Chemistry A 2015 vol. 3(Issue 34) pp:17669-17675
Publication Date(Web):24 Jul 2015
DOI:10.1039/C5TA03438H
Iron phosphide (FeP) was introduced onto silicon nanowires (SiNWs) via precursor loading and phosphorization. The resultant SiNWs/FeP shows remarkably enhanced photoelectrochemical hydrogen production in comparison with bare SiNWs. The solar power conversion efficiency of SiNWs/FeP is as high as 2.64%, which is 94% of that of SiNWs modified with Pt particles, and is larger than those of silicon-based photocathodes loaded with other non-precious electrocatalysts such as transition metals and their chalcogenides. The faster reaction rate of the hydrogen evolution reaction (HER) on the surface of the SiNWs/FeP than that of the bare SiNWs was confirmed by an electrochemistry impedance experiment (EIS). The investigations over the EIS spectra and the flat band potential show that the onset potential of cathodic photocurrent is mainly influenced by the reaction rate of the HER on the surface of the photocathode. The transient photocurrent experiments also suggest the faster kinetics of the HER on the surface of the SiNWs/FeP in comparison with that of the bare SiNWs. This result demonstrates a convenient approach to SiNWs loaded with a highly effective electrocatalyst and its promising application potential in photoelectrochemical hydrogen generation.
Co-reporter:Lingliang Long, Yanjun Wu, Lin Wang, Aihua Gong, Feilong Hu and Chi Zhang
Chemical Communications 2015 vol. 51(Issue 52) pp:10435-10438
Publication Date(Web):18 May 2015
DOI:10.1039/C5CC03972J
Herein, a novel signaling mechanism for constructing fluorescent probes was demonstrated for the first time based on modulation of the unique rotation of the N–N single bond in the acetohydrazide group. According to the new signaling mechanism, a fluorescent probe for hypochlorite was then judiciously developed.
Co-reporter:Jun Qian;Jingchun Hu;Hirofumi Yoshikawa;Jinfang Zhang;Kunio Awaga
European Journal of Inorganic Chemistry 2015 Volume 2015( Issue 12) pp:2110-2119
Publication Date(Web):
DOI:10.1002/ejic.201403223
Abstract
Three manganese–molybdenum/tungsten bimetallic coordination polymers, two 2D {{[μ4-M(CN)8]2[Mn(dmf)3]2[Mn(dmf)4]}·2DMF}n (M = W 1, Mo 2) and a 1D {{[μ4-Mo(CN)8][Mn(dmf)4]2}·(ClO4)}n (3), were constructed from the reaction of the (Bu3NH)3[M(CN)8] (M = W, Mo) and Mn(ClO4)2·6H2O molecular building blocks in DMF solvent in the presence (for 1 and 2) or absence (for 3) of the organic ligand bis(benzimidazol-2′-yl)pyridine. Single-crystal X-ray diffraction structure analysis indicated that compounds 1 and 2 both crystallize in the monoclinic crystal system with the P21/c space group and possess the same 2D network. The 2D layer structures of 1 and 2 have a (3,4)-connected 2-nodal topology with the point symbol {42·63·8}{42·6}. Compound 3 crystallizes in the tetragonal crystal system with the P42/m space group. All three compounds are further assembled into 3D supramolecular structures through intermolecular C–H···N or C–H···O hydrogen bonds. The magnetic susceptibility of compounds 1 and 3 was investigated in the temperature range of 2–300 K; these compounds exhibit typical ferrimagnetic properties.
Co-reporter:Zhipeng Huang, Cuncai Lv, Zhongzhong Chen, Zhibo Chen, Feng Tian, Chi Zhang
Nano Energy 2015 Volume 12() pp:666-674
Publication Date(Web):March 2015
DOI:10.1016/j.nanoen.2015.01.027
•The nanocomposite of diiron phosphide and nitrogen-doped graphene was conveniently synthesized.•The nanocomposite exhibits efficient electrocatalytic activity in hydrogen evolution reaction.•Diiron phosphide is the active component and nitrogen-doped graphene acts as a conductive support.A nanocomposite comprising diiron phosphide (Fe2P) nanoparticles and nitrogen-doped graphene (NGr) was synthesized by a facile one-pot reaction. Such a nanocomposite showed efficient electrocatalytic activity in hydrogen evolution reaction (HER) in both acidic and basic solutions. The optimal overpotential required for the current density of 20 mA cm−2 (η20) in acidic solution is 164 mV, which is favourably comparable to those of recently reported non-precious electrocatalysts; whereas in basic solution the value of η20 is 376 mV. The HER activity of Fe2P/NGr can be correlated to Fe2P nanoparticles in the nanocomposite, and NGr is beneficial to the electron transport from electrode to the catalyst. The faradaic efficiency of Fe2P/NGr nanocomposite in HER is nearly 100% in both acidic and basic solutions. The stability of Fe2P/NGr nanocomposite during HER has been demonstrated by potentiostatic electrolysis and accelerated degradation experiments. Tafel slope was determined to be 65 mV dec−1, which suggests that the HER processes might proceed along a Volmer–Heyrovsky mechanism. The catalytic activity of Fe2P/NGr nanocomposite is influenced by synthesis temperature, which may result in the differences in phase purity, particle size and specific surface areas of the composite material. The charged natures of Fe and P in Fe2P nanoparticle might be responsible for the HER activity of Fe2P/NGr nanocomposite.
Co-reporter:JIANGHUA LI
Journal of Chemical Sciences 2015 Volume 127( Issue 11) pp:1871-1882
Publication Date(Web):2015 November
DOI:10.1007/s12039-015-0966-z
Three Cu-based coordination polymers (CPs), including [Cu II(N- η1-NCS) 2(O- η1-DMF) 2(μ2-3,3’-bptz)] n (1), [Cu I(1,3- μ2-NCS)(μ2-3,3’-bptz)] n (2) and [(Cu I(1,3- μ2- NCS))(μ2-4,4’-bptz)] n (3) (DMF = N, N-dimethyl formamide, 3,3’-bptz = 3,6-bis(3-pyridyl)tetrazine and 4,4’-bptz = 3,6-bis(4-pyridyl)tetrazine) have been successfully constructed by solution diffusion reactions by using Cu(NO 3) 2⋅3H 2O or CuNCS and KNCS with 3,3’-bptz / 4,4’-bptz ligands, respectively. The resulting crystalline materials have been characterized by the single-crystal X-ray diffraction analyses, elemental analyses, FT-IR spectra, thermogravimetric analyses and powder X-ray diffraction (PXRD). Single crystal X-ray analyses revealed that CP 1 is organized in one-dimensional (1D) chain in which the Cu(II) ions are coordinated by η1-NCS − anions and η1-DMF molecules, and linked by μ2-3,3’-bptz bridging ligands. CPs 2 and 3 are structural isomers. CP 2 exhibits two-dimensional (2D) (4,4)-plane-like network in which Cu(I) ions are linked by μ2-NCS − and μ2-3,3’-bptz ligands. In CP 3, Cu(I) ions are connected by μ2-NCS − and μ2-4,4’-bptz ligands to form 2D saw-tooth wavy network. In addition, the photoluminescence properties of CPs 1-3 were also investigated in the solid state at room temperature.
Co-reporter:Zhipeng Huang, Maoying Li, Ding Jia, Peng Zhong, Feng Tian, Zhongzhong Chen, Mark G. Humphrey and Chi Zhang
Journal of Materials Chemistry A 2014 vol. 2(Issue 8) pp:1418-1426
Publication Date(Web):25 Nov 2013
DOI:10.1039/C3TC31919A
Semiconductor–semiconductor hetero-nanorods (Ag2Se–CdSe and Ag2Se–ZnSe) with high crystallinity have been synthesized by a facile and low-cost method. High resolution transmission electron microscopy investigations reveal that the growth follows a catalyst-assisted mechanism. A preliminary investigation of nonlinear optical properties shows that the hetero-nanorods exhibit significantly enhanced third-order nonlinear optical properties. The free carrier absorption cross-section of Ag2Se–CdSe hetero-nanorods is one order of magnitude higher than that of the corresponding single component CdSe nanocrystals. The results obtained in this study represent a new approach to the design and construction of metal selenide hetero-nanorods with high crystallinity and enhanced nonlinear optical capabilities.
Co-reporter:Lingliang Long, Liping Zhou, Lin Wang, Suci Meng, Aihua Gong, Chi Zhang
Analytica Chimica Acta 2014 Volume 812() pp:145-151
Publication Date(Web):17 February 2014
DOI:10.1016/j.aca.2013.12.024
•A fluorescence ratiometric probe for Fe3+ has been developed.•The probe was developed based on the Fe3+-mediated deprotection of acetal reaction.•Upon treatment with Fe3+, fluorescence ratio (I522/I390) of the probe displayed significant changes.•The probe can be used to monitor Fe3+ level in human blood serum.A simple and versatile ratiometric fluorescent Fe3+ detecting system, probe 1, was rationally developed based on the Fe3+-mediated deprotection of acetal reaction. Notably, this reaction was firstly employed to design fluorescent Fe3+ probe. Upon treatment with Fe3+, probe 1 showed ratiometric response, with the fluorescence spectra displaying significant red shift (up to 132 nm) and the emission ratio value (I522/I390) exhibiting approximately 2362-fold enhancement. In addition, the probe is highly sensitive (with the detection limit of 0.12 μM) and highly selective to Fe3+ over other biologically relevant metal ions. The sensing reaction product of the probe with Fe3+ was confirmed by NMR spectra and mass spectrometry. TD-DFT calculation has demonstrated that the ratiometric response of probe 1 to Fe3+ is due to the regulation of intramolecular charge transfer (ICT) efficiency. Moreover, the practical utility in fluorescence detection of Fe3+ in human blood serum was also conducted, and probe 1 represents the first ratiometric fluorescent probe that can be used to monitor Fe3+ level in human blood serum. Finally, probe 1 was further employed in living cell imaging with pancreatic cancer cells, in which it displayed low cytotoxicity, satisfactory cell permeability, and selective ratiometric response to Fe3+.
Co-reporter:Jun Qian, Jingchun Hu, Hirofumi Yoshikawa, Jinfang Zhang, Kunio Awaga, and Chi Zhang
Crystal Growth & Design 2014 Volume 14(Issue 5) pp:2288-2295
Publication Date(Web):April 17, 2014
DOI:10.1021/cg4019053
A three-dimensional (3D) manganese–tungsten bimetallic coordination polymer (CP) {{[μ5-W(CN)8]2[Mn(HMTA)1.5]2[Mn(HMTA)(H2O)2]}·2H2O}n (CP-1) (HMTA = hexamethylenetetramine) is constructed by the reaction of the molecular building block [W(CN)8]3– and tetradentate bridging ligand HMTA with d5 transition metal ion Mn2+. CP-1 has been unambiguously confirmed by Fourier-transform infrared spectroscopy, elemental analysis, thermogravimetric analysis, and single-crystal and powder X-ray diffraction. Crystallographic analysis reveals that, crystallizing in the monoclinic crystal system with P21/c space group, CP-1 possesses an infinite 3D framework and exhibits an unusual (4,5)-connected 4,5T7 topology with point symbol (32·62·72)(3·44·52·62·7)4. The extended 3D structure is constructed by two-dimensional (2D) cyano-bridged corrugated -W–Mn2–W–Mn2- layers pillared via the [Mn1(HMTA)(H2O)2] units. The magnetic investigation indicates ferrimagnetic behavior for CP-1 because of the antiferromagnetic coupling between WV (S = 1/2) and MnII (S = 5/2) centers mediated by cyano bridges.
Co-reporter:Hui Feng, Junli Wang, Weiling Fan, Chi Zhang
Materials Letters 2014 Volume 126() pp:67-70
Publication Date(Web):1 July 2014
DOI:10.1016/j.matlet.2014.04.037
•Matchstick-like Ag2S–ZnS hetero-nanorods were prepared by a two-step colloidal method.•The formation of Ag2S–ZnS hetero-nanorods followed a catalytic growth mechanism.•Ag2S nanocrystals served as an effective catalyst.•Dodecanethiol was used as a sulfur source and a solvent.•This method could be extended to producing ZnS nanorods without Ag2S heads.A two-step colloidal synthesis of highly uniform Ag2S–ZnS matchstick-like hetero-nanorods, composed of Ag2S head and ZnS rod-like stem, is reported. Dodecanethiol is used as a sulfur source and a solvent. Ag2S nanocrystals are first prepared, act as a catalyst to grow anisotropic ZnS nanorods, and finally remain at the tip of the resultant nanorods, leading to Ag2S–ZnS hetero-nanorods with a matchstick-like shape. By decreasing the amount of Ag precursor (AgNO3), uniform ZnS nanorods without Ag2S catalytic heads can be prepared. The disappearance of Ag2S heads is attributed to the diffusion of Ag+ ions from Ag2S into the growing ZnS nanorods. These hetero-nanorods combine narrow band gap semiconductor Ag2S (bulk Eg=0.9–1.1 eV) with wide band gap semiconductor ZnS (bulk Eg=3.77 eV) and may be promising optical and/or optoelectronic materials.
Co-reporter:Zhipeng Huang, Zhibo Chen, Zhongzhong Chen, Cuncai Lv, Hua Meng, and Chi Zhang
ACS Nano 2014 Volume 8(Issue 8) pp:8121
Publication Date(Web):July 28, 2014
DOI:10.1021/nn5022204
The exploitation of a low-cost catalyst is desirable for hydrogen generation from electrolysis or photoelectrolysis. In this study we have demonstrated that nickel phosphide (Ni12P5) nanoparticles have efficient and stable catalytic activity for the hydrogen evolution reaction. The catalytic performance of Ni12P5 nanoparticles is favorably comparable to those of recently reported efficient nonprecious catalysts. The optimal overpotential required for 20 mA/cm2 current density is 143 ± 3 mV in acidic solution (H2SO4, 0.5 M). The catalytic activity of Ni12P5 is likely to be correlated with the charged natures of Ni and P. Ni12P5 nanoparticles were introduced to silicon nanowires, and the power conversion efficiency of the resulting composite is larger than that of silicon nanowires decorated with platinum particles. This result demonstrates the promising application potential of metal phosphide in photoelectrochemical hydrogen generation.Keywords: electrocatalyst; electrolysis; hydrogen generation; nickel phosphide; photoelectrolysis; silicon nanowires
Co-reporter:Zhipeng Huang, Zhongzhong Chen, Zhibo Chen, Cuncai Lv, Mark G. Humphrey, Chi Zhang
Nano Energy 2014 Volume 9() pp:373-382
Publication Date(Web):October 2014
DOI:10.1016/j.nanoen.2014.08.013
•A convenient method is used to fabricate cobalt phosphide (Co2P) nanorods.•Co2P nanorods exhibit efficient electrocatalytic activity in hydrogen evolution reaction.•Co2P nanorods work stably in both acidic and basic solutions.Cobalt phosphide (Co2P) nanorods are found to exhibit efficient catalytic activity for the hydrogen evolution reaction (HER), with the overpotential required for the current density of 20 mA/cm2 as small as 167 mV in acidic solution and 171 mV in basic solution. In addition, the Co2P nanorods can work stably in both acidic and basic solution during hydrogen production. This performance can be favorably compared to typical high efficient non-precious catalysts, and suggests the promising application potential of Co2P nanorods in the field of hydrogen production. The HER process follows a Volmer–Heyrovsky mechanism, and the rates of the discharge step and desorption step appear to be comparable during the HER process. The similarity of charged natures of Co and P in the Co2P nanorods to those of the hydride-acceptor and proton-acceptor in highly efficient Ni2P catalysts, [NiFe] hydrogenase, and its analogues implies that the HER catalytic activity of the Co2P nanorods might be correlated with the charged natures of Co and P.
Co-reporter:Dr. Aijian Wang ;Yu Fang;Wang Yu;Dr. Lingliang Long;Dr. Yinglin Song;Wei Zhao;Dr. Marie P. Cifuentes;Dr. Mark G. Humphrey;Dr. Chi Zhang
Chemistry – An Asian Journal 2014 Volume 9( Issue 2) pp:639-648
Publication Date(Web):
DOI:10.1002/asia.201301379
Abstract
Allyloxyporphyrin-functionalized multiwalled carbon nanotubes (MWCNT-TPP) were synthesized by radical polymerization and characterized by FTIR, UV/Vis absorption, and X-ray photoelectron spectroscopy; elemental analysis; TEM; and thermogravimetric analysis. Z-scan studies revealed that this nanohybrid exhibits enhanced nonlinear optical (NLO) properties compared to a control sample consisting of a covalently unattached physical blend of MWCNTs and porphyrin, as well as to the separate MWCNTs and porphyrin. At the wavelengths used, the mechanism of enhanced optical limiting likely involves reverse saturable absorption, nonlinear scattering, and photoinduced electron/energy transfer between the MWCNTs and the porphyrin. The role of electron/energy transfer in the NLO performance of MWCNT-TPP was investigated by Raman and fluorescence spectroscopy.
Co-reporter:Zhipeng Huang, Peng Zhong, Chifang Wang, Xuanxiong Zhang, and Chi Zhang
ACS Applied Materials & Interfaces 2013 Volume 5(Issue 6) pp:1961
Publication Date(Web):February 22, 2013
DOI:10.1021/am3027458
The top of silicon nanowires (SiNWs) arrays was coated with reduced graphene oxide (rGO) by the facile spin-coating method. The resulting SiNWs/rGO composite exhibits enhanced photoelectrochemical properties, with short-circuit photocurrent density more than 4 times higher than that of the pristine SiNWs and more than 600 times higher than that of planar Si/rGO composite. The trapping and recombination of photogenerated carriers at the surface state of SiNWs were reduced after the application of rGO. The results of electrochemical impedance spectroscopy measurements suggest that the reduction of trapping and recombination of photogenerated carriers as well as remarkably enhancement of photoelectrochemical properties can be attributed to the low charge transfer resistance at the SiNWs–rGO interface and rGO–electrolyte interface. The method and results shown here indicate a convenient and applicable approach to further exploitation of high activity materials for photoelectrochemical applications.Keywords: graphene; nanowires; photocatalyst; photoelectrochemisty; silicon;
Co-reporter:Lingliang Long, Dongdong Zhang, Xiufen Li, Jinfang Zhang, Chi Zhang, Liping Zhou
Analytica Chimica Acta 2013 Volume 775() pp:100-105
Publication Date(Web):2 May 2013
DOI:10.1016/j.aca.2013.03.016
•A fluorescence ratiometric sensor for hypochlorite has been developed.•The sensor was designed based on novel dual-fluorophore response approach.•The sensor contains two fluorophores that responded simultaneously to hypochlorite at two separate optical windows.•Upon treatment with hypochlorite, fluorescence ratio (I578/I501) of the sensor displayed significant changes.•The sensor can also be applied in real samples.A fluorescence ratiometric sensor for OCl− has been developed based on a novel dual fluorophore response approach. The sensor molecule contains a coumarin fluorophore and a rhodamine fluorophore, and the two fluorophores are directly linked to an OCl− recognition group. The structure of the sensor was characterized by ESI-MS, NMR, and X-ray crystallographic analysis. Upon treatment with OCl−, both fluorophores in the sensor responded simultaneously at two separate optical windows, with large enhancement of the fluorescence ratio (I578/I501) from 0.01 to 39.55. The fluorescence ratios for the sensor showed a good linearity with the concentration of OCl− in the range of 0.2–40 μM and the detection limits is 0.024 μM (S N−1 = 3). Investigation of reaction products indicated that the sensor reaction with OCl− produced two new fluorescent molecules, which were responsible for the fluorescence changes in two optical windows. In addition, the sensor showed high selectivity to OCl− over other reactive oxygen species, reactive nitrogen species, cations, and anions. The sensor has also been successfully applied to detection of OCl− in natural water samples with satisfactory recovery.Graphical abstract
Co-reporter:Tingting You, Junli Wang, Hui Feng, Kangmin Chen, Weiling Fan, Chi Zhang and Runsheng Miao
Dalton Transactions 2013 vol. 42(Issue 21) pp:7724-7730
Publication Date(Web):13 Mar 2013
DOI:10.1039/C3DT50301A
Template growth and catalytic growth are two typical mechanisms for the solution-chemistry synthesis of one-dimensional (1D) II–VI semiconductor nanomaterials. Here, we systematically demonstrate the competition relationship between them by tuning the synthesis of 1D ZnS nanostructures in different chain-length primary alkyl-amines. The template growth, derived from the coordination effect of amines, produces ZnS nanobelts and will compete with the Ag2S-catalyzed mechanism as AgNO3 is added into these amines. In short-chain n-propylamine and n-butylamine the template growth is much stronger than the catalytic growth, leading to the morphology maintenance of ZnS nanobelts, whereas the latter replaces the former in long-chain n-octylamine and n-dodecylamine due to the decrease of coordination ability of amines, which yields ZnS nanowires instead of nanobelts. A balance of competition is built between these two mechanisms in middle-length n-hexylamine, producing a mixture of ZnS nanobelts and nanowires. The morphology and growth mechanism changes of ZnS nanostructures have been rationally investigated using various characterization techniques. Meanwhile, the optical properties of the products synthesized before and after adding AgNO3 are comparatively studied by UV-vis absorption and photoluminescence (PL) spectra.
Co-reporter:Lingliang Long, Liping Zhou, Lin Wang, Suci Meng, Aihua Gong, Fengyi Du and Chi Zhang
Organic & Biomolecular Chemistry 2013 vol. 11(Issue 47) pp:8214-8220
Publication Date(Web):15 Oct 2013
DOI:10.1039/C3OB41741G
In this work, compound 1 has been rationally designed and synthesized as a new fluorescent probe for biological thiols. Notably, probe 1 has almost no background fluorescence (Φf < 0.0001) in aqueous solutions; however, it exhibited fluorescence turn-on response to thiols with high sensitivity (a 246-fold fluorescence enhancement and a low detection limit of 0.22 μM for Cys). Moreover, probe 1 showed excellent thiol specificity over other biologically relevant species. The kinetic studies indicated that the probe responded to thiols rapidly, and the pseudo-first-order rate constants of probe 1 reaction with Cys, Hcy, and GSH were determined to be 1.85842, 0.67656, and 0.51519 min−1, respectively. A possible detection mechanism was proposed to involve the Michael addition of the thiol to the α,β-unsaturated ketone, followed by a cleavage of the hemiketal group, thereby leading to the formation of a fluorescent 7-hydroxyl coumarin derivative. Furthermore, the optical responses of probe 1 to thiols were studied by TD-DFT calculations. Finally, probe 1 has been successfully applied to the detection of biological thiols in human blood serum. And the intracellular imaging applications established that probe 1 can be used to detect different concentrations of intracellular thiols in living cells.
Co-reporter:Aijian Wang, Lingliang Long, Suci Meng, Xiufen Li, Wei Zhao, Yinglin Song, Marie P. Cifuentes, Mark G. Humphrey and Chi Zhang
Organic & Biomolecular Chemistry 2013 vol. 11(Issue 25) pp:4250-4257
Publication Date(Web):16 Apr 2013
DOI:10.1039/C3OB40323H
A novel porphyrin derivative bearing one D–π–A–π–D pyrimidine chromophore at the periphery was designed, prepared, and studied using the Z-scan technique, the results showing that this compound exhibits enhanced nonlinear optical (NLO) absorption, refraction and optical limiting responses. The significant NLO properties can be ascribed to an effective combination of distinct nonlinear mechanisms.
Co-reporter:Jun Qian, Jingchun Hu, Jinfang Zhang, Hirofumi Yoshikawa, Kunio Awaga, and Chi Zhang
Crystal Growth & Design 2013 Volume 13(Issue 12) pp:5211-5219
Publication Date(Web):September 25, 2013
DOI:10.1021/cg400909b
Aqueous solution was introduced into the self-assembly of water-insoluble (Bu3NH)3[M(CN)8] (M = W, Mo) and Mn(NO3)2·6H2O to afford two, three-dimensional (3D) coordination polymers (CPs), {[μ8-MV(CN)8MnII2(H2O)2(CH3OH)][NO3]}n (M = W 1, Mo 2), while polymer {[μ4-WV(CN)8MnII2(DMF)8](ClO4)}n (DMF = N,N-dimethylformamide) (3) was crystallized from the reaction of (Bu3NH)3[W(CN)8] and Mn(ClO4)2·6H2O in DMF. All three CPs 1, 2, and 3 have been well-characterized by elemental analysis, infrared spectra, single-crystal X-ray diffraction, as well as thermogravimetric analysis. The single-crystal X-ray structural analysis shows that both CPs 1 and 2 crystallize in the monoclinic crystal system with space group of C2/c and possess the infinite 3D framework in an unprecedented afm1 topology geometry, which is an unreported 4-nodal 4,4,8,8-coordinated net with point symbol {411.612.85}{417.610.8}{45.6}4. Polymer 3 crystallizes in the space group of P42/m as a 3D supermolecule structure, which is constructed by one-dimensional (1D) cationic {[μ4-WV(CN)8MnII2(DMF)8]+}n chains linked via the hydrogen bonds. Magnetic susceptibility measurements in the temperature range of 2–300 K reveal that CPs 1 and 2 exhibit the similar typical antiferromagnetic properties, while CP 3 shows the ferromagnetic property.
Co-reporter:Lingliang Long, Xiufen Li, Dongdong Zhang, Suci Meng, Jinfang Zhang, Xianglan Sun, Chi Zhang, Liping Zhou and Lin Wang
RSC Advances 2013 vol. 3(Issue 30) pp:12204-12209
Publication Date(Web):10 May 2013
DOI:10.1039/C3RA41329B
Two novel ratiometric sensors, 1a and 1b, for acidic pH have been rationally developed with 7-diethylamino-coumarin as the fluorophore and pyridine as the receptor. Both of the sensors exhibited a fluorescence ratiometric response to acidic pH. For sensor 1a, upon decreasing the pH from 8.35 to 2.36, the fluorescence emission spectra exhibited a large red shift from 529 to 616 nm, the emission ratio (I529:I616) changed dramatically from 8.58 to 0.09, and the pKa value was calculated to be 5.36. The emission ratio also displayed a good linearity with the pH in the range of 4.0 to 6.5, which is valuable for quantitative determination of pH in this acidic pH window. Similar behaviour was observed for sensor 1b. In addition, NMR experiments and theoretical calculations demonstrated that the ratiometric response of the sensors to acidic pH was due to H+ binding with the N of pyridine and the induced enhancement of the intramolecular charger transfer (ICT) process. The sensors have been successfully applied to quantitatively detect pH in biological fluids. The intracellular pH imaging experiments also proved that the sensors are suitable for detecting acidic pH fluctuations in living cells.
Co-reporter:Jianghua Li;Jinfang Zhang;Mark G. Humphrey
European Journal of Inorganic Chemistry 2013 Volume 2013( Issue 3) pp:328-346
Publication Date(Web):
DOI:10.1002/ejic.201200735
Abstract
This article provides a concise summary of recent research progress, including synthetic strategies, structural diversity, theoretical studies, and third-order nonlinear optical (NLO) properties, on Mo(W)/S(Se)/Ag heterobimetallic clusters. It offers a preliminary analysis of their metal-cation-directed synthesis, structures, and the subtle interplay of structural–functional relationships. Furthermore, DFT was used to provide an insight into the electronic transitions and spectral characterization of these clusters. Recent trends and perspectives of these clusters as NLO materials are also described.
Co-reporter:Lingliang Long, Liping Zhou, Lin Wang, Suci Meng, Aihua Gong, Fengyi Du and Chi Zhang
Analytical Methods 2013 vol. 5(Issue 23) pp:6605-6610
Publication Date(Web):27 Sep 2013
DOI:10.1039/C3AY41475B
A fluorescent ratiometric probe, compound 1, for cyanide has been rationally constructed based on an intramolecular charge transfer (ICT) mechanism. Upon treatment with cyanide, probe 1 exhibited a fluorescence ratiometric response, with the emission wavelength displaying a very large shift (up to 160 nm). When 2 equivalents of cyanide were added, the emission ratios (I458/I618) of probe 1 changed dramatically from 0.027 to 28.306. In addition, the emission ratios (I458/I618) showed good linearity with the cyanide concentration in the range of 0–6.0 μM, and the detection limit measured to be 0.126 μM. The NMR experiments and theoretical calculations confirmed that the ratiometric response of probe 1 to cyanide is due to the nucleophilic addition reaction of the cyanide with the vinyl malononitrile group of probe 1, which results in the inhibition of the ICT process in the probe. Importantly, probe 1 has been applied to detection of cyanide in a natural water sample with satisfactory recovery. Furthermore, the quantitative determination of endogenous cyanide in cassava root demonstrated that the probe can be employed to detect endogenous cyanide in real biological samples.
Co-reporter:Dr. Aijian Wang;Yu Fang;Dr. Lingliang Long;Dr. Yinglin Song;Wang Yu;Wei Zhao;Dr. Marie P. Cifuentes;Dr. Mark G. Humphrey;Dr. Chi Zhang
Chemistry - A European Journal 2013 Volume 19( Issue 42) pp:14159-14170
Publication Date(Web):
DOI:10.1002/chem.201302477
Abstract
Two multi-walled carbon nanotube (MWCNT)-based nanohybrids, MWCNT–ZnTPP and MWCNT–TPP (TPP=5-[4-{2-(4-formylphenoxy)- ethyloxy}phenyl]-10,15,20-triphenylporphyrin, ZnTPP=5-[4-{(4-formylphenyl)ethynyl}phenyl]-10,15,20-triphenylporphinatozinc(II)), were prepared directly from pristine MWCNTs through 1,3-dipolar cycloaddition reactions. Covalent attachment of the porphyrins to the surfaces of the MWCNTs was confirmed by Fourier transform infrared spectroscopy, ultraviolet/visible absorption, fluorescence, Raman, and X-ray photoelectron spectroscopy, elemental analysis, transmission electron microscopy, and thermogravimetric analysis. Attachment of the porphyrin moieties to the surface of the MWCNTs significantly improves the solubility and ease of processing of these MWCNT–porphyrin composite materials. Z-scan studies reveal that these MWCNT–porphyrin nanohybrids exhibit enhanced nonlinear optical properties under both nanosecond and picosecond laser pulses at λ=532 nm in comparison with free MWCNTs and the free porphyrin chromophores, whereas superior optical limiting performance was displayed by MWCNT–porphyrin composite materials rather than MWCNTs/ZnTPP and MWCNTs/TPP blends, which is consistent with a remarkable accumulation effect as a result of the covalent linkage between the porphyrin and the MWCNTs.
Co-reporter:Dr. Aijian Wang;Yu Fang;Dr. Lingliang Long;Dr. Yinglin Song;Wang Yu;Wei Zhao;Dr. Marie P. Cifuentes;Dr. Mark G. Humphrey;Dr. Chi Zhang
Chemistry - A European Journal 2013 Volume 19( Issue 42) pp:
Publication Date(Web):
DOI:10.1002/chem.201390164
Co-reporter:Zhipeng Huang, Chifang Wang, Lei Pan, Feng Tian, Xuanxiong Zhang, Chi Zhang
Nano Energy 2013 Volume 2(Issue 6) pp:1337-1346
Publication Date(Web):November 2013
DOI:10.1016/j.nanoen.2013.06.016
•A high efficiency and low-cost photocathode for hydrogen production is demonstrated.•Composite of silicon nanowires and molybdenum sulfide can be fabricated by a convenient method.•Electrochemical measurements reveal the origin of enhancement in photoelectrochemical performance.The composite of silicon nanowires (SiNWs) and MoS3 (SiNWs@MoS3) was fabricated by a convenient method. In comparison with SiNWs, SiNWs@MoS3 exhibits remarkably enhanced photocurrent during photoelectrochemical hydrogen production. The photoelectrochemical performance of SiNWs@MoS3 is comparable to that of the composite of SiNWs and Pt nanoparticles (SiNWs@PtNPs). Electrochemical impedance spectroscopy experiments suggest that the enhanced performance of SiNWs@MoS3 can be attributed to small charge transfer resistance (i.e. fast H+ reduction kinetics ) at SiNWs@MoS3/electrolyte interface, and the large electrochemically active surface area of SiNWs@MoS3.High efficient silicon nanowires (SiNWs)@MoS3photocathode was fabricated by a convenient method. The SiNWs@MoS3 exhibit remarkably enhanced photoelectrochemical hydrogen production, in comparison with the pristine silicon nanowires. The hydrogen production capability of silicon nanowires@MoS3 is also comparable to that of SiNWs@Pt nanoparticles. The superior photoelectrochemical hydrogen production ability of SiNWs@MoS3 can be ascribed to small charge transfer resistance (i.e. faradic reaction kinetics) at SiNWs@MoS3/electrolyte interface and large photoelectrochemical active area of SiNWs@MoS3.
Co-reporter:Junli Wang, Congming Yang, Zhipeng Huang, Mark G. Humphrey, Ding Jia, Tingting You, Kangmin Chen, Qing Yang and Chi Zhang
Journal of Materials Chemistry A 2012 vol. 22(Issue 19) pp:10009-10014
Publication Date(Web):13 Apr 2012
DOI:10.1039/C2JM00091A
Seed-catalyzed, heteroepitaxial growth of high aspect-ratio, uniform ZnSe nanowires is reported, in which Ag2Se nanoparticles serve as heterogeneous seeds and as epitaxial substrates. Due to the difference in solubility product constants (Ksp: Ag2Se ≪ ZnSe), Ag2Se is precipitated before ZnSe and in situ seeds and catalyzes the nanowire growth in a one-pot solution synthesis. The lattice match between metastable tetragonal Ag2Se{212} and cubic ZnSe{220} planes facilitates the heteroepitaxial growth of ZnSe nanowires. Conversion of small, uniform Ag particles, which are produced from the reduction of Ag+ ions by reductants/surfactants such as polyvinyl pyrrolidone (PVP) and oleylamine (OA), into Ag2Se with small size and high uniformity is shown to be an effective strategy to control the diameter size and distribution of ZnSe nanowires. The third-order nonlinear optical behavior of the as-prepared nanowires has been evaluated by Z-scan measurements.
Co-reporter:Zhipeng Huang, Ruxue Wang, Ding Jia, Li Maoying, Mark G. Humphrey, and Chi Zhang
ACS Applied Materials & Interfaces 2012 Volume 4(Issue 3) pp:1553
Publication Date(Web):February 13, 2012
DOI:10.1021/am201758z
A facile method for the low-cost and large-scale production of silicon nanowires has been developed. Silicon powders were subjected to sequential metal plating and metal-assisted chemical etching, resulting in well-defined silicon nanowires. The morphology and structure of the silicon nanowires were investigated, revealing that single-crystal silicon nanowires with average diameters of 79 ± 35 nm and length more than 10 μm can be fabricated. The silicon nanowires show excellent third-order nonlinear optical properties, with a third-order susceptibility much larger than that of bulk silicon, porous silicon, and silicon nanocrystals embedded in SiO2.Keywords: etching; nonlinear optics; silicon nanowire; synthesis;
Co-reporter:Jianghua Li, Suci Meng, Jinfang Zhang, Yinglin Song, Zhipeng Huang, Huajian Zhao, Hongyang Wei, Wenjiang Huang, Marie P. Cifuentes, Mark G. Humphrey and Chi Zhang
CrystEngComm 2012 vol. 14(Issue 8) pp:2787-2796
Publication Date(Web):03 Feb 2012
DOI:10.1039/C2CE06610F
Reactions of hexamethylenetetramine (hmt) and AgSCN in different solvents generated three distinct [AgSCN]n-based coordination polymers (CPs): [Ag(1,3-μ2-SCN)(μ2-hmt)]n (1), {[Ag(1,1,3-μ3-SCN)]2(μ2-hmt)}n (2) and [Ag(1,1,3-μ3-SCN)(μ4-hmt)0.5]n (3). The identities of the coordination polymers (CPs) 1–3 have been unambiguously established by elemental analysis, IR, UV-vis spectra and single-crystal X-ray diffraction studies. Interestingly, 1 displays a two-dimensional (2D) (4,4) network involving one-dimensional (1D) zigzag [Ag(1,3-μ2-SCN)]n chains bridged by μ2-hmt linkers. 2 and 3 are novel 2D and three-dimensional (3D) supramolecular isomers: 2 presents an unusual 2D threaded-loop type (3,4)-connected {(3·4·5)(52·7)}{(3·4·53·63·72)(3·54·63·72)} network containing puckered [Ag(1,1,3-μ3-SCN)]n networks linked by μ2-hmt bridges, while 3 exhibits a unique 3D pillared-layer (3,4,6)-connected (4·62)(66)2(42·610·83) framework in which the undulating [Ag(1,1,3-μ3-SCN)]n layers are supported by μ4-hmt pillars. 1–3 all possess good third-order nonlinear optical (NLO) properties. Density functional theory (DFT) and time-dependent density functional theory (TD-DFT) calculations have afforded insight into the electronic transitions and spectral characterization of these functionalized NLO molecular materials.
Co-reporter:Congming Yang, Junli Wang, Tingting You, Chi Zhang
Materials Letters 2012 80() pp: 29-32
Publication Date(Web):
DOI:10.1016/j.matlet.2012.04.074
Co-reporter:Jinfang Zhang, Suci Meng, Yinglin Song, Yimeng Zhou, Yuan Cao, Jianghua Li, Huajian Zhao, Jingchun Hu, Jinhua Wu, Mark G. Humphrey, and Chi Zhang
Crystal Growth & Design 2011 Volume 11(Issue 1) pp:100-109
Publication Date(Web):November 24, 2010
DOI:10.1021/cg1009779
An efficient route to construct three-dimensional (3-D) M/S/Cu nest-cluster-based coordination polymers has been developed. By this method, cyanide bridges have been successfully introduced to build three new non-interpenetrating 3-D nest-shaped-cluster [MoOS3Cu3]-based coordination polymers, 3∞{[(NO3)⊂(Me4N)3]⊂[MoOS3Cu3(CN)3]} (1) and 3∞{[(NH4)·2DMF]⊂[Mo2O2S6Cu6(CN)3(L)4]} (L1 = bipy = 4,4′-bipyridine, 2; L2 = bpee = 1,2-bis(4-pyridyl)ethene, 3). The structures of 1−3 have been established by elemental analysis, IR, UV−vis, and single-crystal X-ray crystallographic studies. 1 is the first non-interpenetrating 3-D 6-connected M/S/Cu coordination polymer and possesses an unprecedented dual-inclusive structure, rare “ACS” topology and huge free volume. 2 and 3 possess unusual non-interpenetrating 3-D pillar-layer-alternating honeycomb-like frameworks with diamondoid topologies. Nonlinear optical (NLO) properties of these clusters were investigated by Z-scan employing 5 ns pulses at 532 nm, with 1−3 showing strong third-order NLO properties. Time-dependent density functional theory (TD-DFT) studies have afforded insight into the electronic transitions and spectral characterization of these functionalized NLO molecular materials.
Co-reporter:Jun Qian, Huajian Zhao, Hongyang Wei, Jianghua Li, Jinfang Zhang, Hirofumi Yoshikawa, Kunio Awaga and Chi Zhang
CrystEngComm 2011 vol. 13(Issue 2) pp:517-523
Publication Date(Web):13 Sep 2010
DOI:10.1039/C0CE00227E
Treatment of molecular building block [W(CN)8]3− with Co(NO3)2·6H2O or Cu(ClO4)2·6H2O in different reaction conditions affords two 3D (three-dimensional) metalloligand-bridged coordination polymers {[WV(CN)8Co2(DMF)8][NO3]}n1 and {WIV(CN)8Cu2(py)8}n2, respectively. The single-crystal X-ray structural analysis shows that both polymers 1 and 2 crystallize in the tetragonal crystal system with space group of I41/a and possess the similar 3D framework in a diamondoid topology geometry, although [W(CN)8]3− ion was reduced into [W(CN)8]4− in polymer 2 during the reaction process. The magnetic studies on coordination polymers 1 and 2 indicate that polymer 1 shows the typical ferromagnetic property with an ordering temperature of about 5 K but polymer 2 exhibits paramagnetic behavior due to the diamagnetic octacyanometalate bridge –NC–WIV(S = 0)–CN–.
Co-reporter:Jinfang Zhang, Suci Meng, Yinglin Song, Junyi Yang, Hongyang Wei, Wenjiang Huang, Marie P. Cifuentes, Mark G. Humphrey and Chi Zhang
New Journal of Chemistry 2011 vol. 35(Issue 2) pp:328-338
Publication Date(Web):15 Nov 2010
DOI:10.1039/C0NJ00674B
The sequential addition to [WS4]2− of different solvent-coordinated ytterbium cations as templates and silver iodide as Ag+ source afforded the heterothiometallic clusters {[Yb(DMSO)7][Yb(DMSO)8][W6S24Ag6]}n1 (DMSO = dimethyl sulfoxide), {[Yb(DMF)8][W3S12Ag3]}n2 (DMF = N,N′-dimethylformamide) and {[Yb(HMP)4(NO3)2][WS4Ag]}n3 (HMP = hexamethylphosphoramide) with isomeric anionic skeletons and in high yields. 1–3 have been fully characterized by elemental analysis, IR and UV-vis spectroscopies, and single-crystal X-ray crystallographic studies. 1 possesses a 1D anionic helical chain with unusual hexavalent repeat units, a structure directed by the combination of seven- and eight-coordinated ytterbium cations, 2 exhibits an unusual 1D anionic zigzag chain, while 3 contains a 1D anionic linear chain. Z-scan studies (532 nm, 8 ns pulses) reveal that 1 and 2 possess strong third-order nonlinear optical properties. Density functional theory and time-dependent density functional theory calculations at the B3LYP/LanL2DZf+6-31G* level were performed on 1–3 to rationalize their experimental absorption spectra.
Co-reporter:Huiqi Pan, Xiukai Li, Zongjin Zhuang, Chi Zhang
Journal of Molecular Catalysis A: Chemical 2011 Volume 345(1–2) pp:90-95
Publication Date(Web):5 July 2011
DOI:10.1016/j.molcata.2011.05.024
Visible light-responsive g-C3N4/SiO2–HNb3O8 composite photocatalysts were prepared by a solid state-reaction method with melamine as a g-C3N4 precursor. The photocatalytic activities of the samples were evaluated for rhodamine B (RhB) degradation under visible light irradiation and the results were compared with those obtained over pure SiO2–HNb3O8 and g-C3N4. Techniques such as XRD, FT-IR, SEM, TEM, and UV–vis diffuse reflectance spectroscopy were adopted to explore the characteristics of samples. The g-C3N4/SiO2–HNb3O8 composite materials exhibited superior activities than pure SiO2–HNb3O8 and g-C3N4; the sample prepared with SiO2–HNb3O8 to melamine ratio being 1:2 and the heating duration being 4 h performed the best. The improved activity of g-C3N4/SiO2–HNb3O8 is attributed to the unique synergetic effect between SiO2–HNb3O8 and g-C3N4.Graphical abstractHighlights► g-C3N4/SiO2–HNb3O8 composites were prepared by solid state reaction. ► g-C3N4/SiO2–HNb3O8 composites are visible light active photocatalysts. ► g-C3N4/SiO2–HNb3O8 exhibited superior activity than SiO2–HNb3O8 and g-C3N4. ► The enhanced activity is ascribed to the synergism between the two components.
Co-reporter:Dr. Jinfang Zhang;Dr. Suci Meng;Dr. Yinglin Song;Huajian Zhao;Jianghua Li;Gaoju Qu;Liang Sun;Dr. Mark G. Humphrey;Dr. Chi Zhang
Chemistry - A European Journal 2010 Volume 16( Issue 47) pp:13946-13950
Publication Date(Web):
DOI:10.1002/chem.201001249
Co-reporter:Chi Zhang Dr.;Tsuyoshi Matsumoto Dr.;Marek Samoc Dr.;Simon Petrie Dr.;Suci Meng Dr.;T. ChristopherCorkery;Robert Stranger Dr.;Jinfang Zhang Dr.;MarkG. Humphrey Dr.;Kazuyuki Tatsumi Dr.
Angewandte Chemie International Edition 2010 Volume 49( Issue 25) pp:4209-4212
Publication Date(Web):
DOI:10.1002/anie.200907074
Co-reporter:Chi Zhang Dr.;Tsuyoshi Matsumoto Dr.;Marek Samoc Dr.;Simon Petrie Dr.;Suci Meng Dr.;T. ChristopherCorkery;Robert Stranger Dr.;Jinfang Zhang Dr.;MarkG. Humphrey Dr.;Kazuyuki Tatsumi Dr.
Angewandte Chemie 2010 Volume 122( Issue 25) pp:4305-4308
Publication Date(Web):
DOI:10.1002/ange.200907074
Co-reporter:Chi Zhang Dr.;Tsuyoshi Matsumoto Dr.;Marek Samoc Dr.;Simon Petrie Dr.;Suci Meng Dr.;T. ChristopherCorkery;Robert Stranger Dr.;Jinfang Zhang Dr.;MarkG. Humphrey Dr.;Kazuyuki Tatsumi Dr.
Angewandte Chemie 2010 Volume 122( Issue 25) pp:
Publication Date(Web):
DOI:10.1002/ange.201002348
Co-reporter:Chi Zhang Dr.;Tsuyoshi Matsumoto Dr.;Marek Samoc Dr.;Simon Petrie Dr.;Suci Meng Dr.;T. ChristopherCorkery;Robert Stranger Dr.;Jinfang Zhang Dr.;MarkG. Humphrey Dr.;Kazuyuki Tatsumi Dr.
Angewandte Chemie International Edition 2010 Volume 49( Issue 25) pp:
Publication Date(Web):
DOI:10.1002/anie.201002348
Co-reporter:Guo-dong Tang, Zheng-jing Jiang, Rong-qing Li, Jin-fang Zhang, Yu Zhang, Chi Zhang
Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy 2009 Volume 74(Issue 1) pp:228-232
Publication Date(Web):15 September 2009
DOI:10.1016/j.saa.2009.06.035
Theoretical calculations were carried out on some neutral nest-shaped heterothiometallic cluster compounds [MOS3Py5Cu3X] (M = Mo, W; X = F, Cl, Br, I) with the high first static hyperpolarizabilities β values. The geometries of these cluster compounds were optimized by the restricted DFT method at B3LYP level with LanL2DZ base set without any constrains. In order to understand the relationship between the first static hyperpolarizabilities and the compositions of these clusters, the frontier orbital compositions and energy gaps between the HOMO and LUMO orbitals were calculated and analysed. In these clusters the HOMO orbitals are mainly composed of halogen atoms and the first static hyperpolarizability increases from F to I atom. The LUMO orbitals of clusters [MoOS3Py5Cu3X] are comprised of Mo, O and S atoms while the LUMO orbitals of clusters [WOS3Py5Cu3X] composed of W atom and pyridine ring. The energy gaps between the HOMO and LUMO orbitals of the clusters [MoOS3Py5Cu3X] are smaller than those of the clusters [WOS3Py5Cu3X]. As a result the first static hyperpolarizability values of the clusters [MoOS3Py5Cu3X] are higher than those of the clusters [WOS3Py5Cu3X].
Co-reporter:Chi Zhang;Yuan Cao;Jinfang Zhang;Suci Meng;Tsuyoshi Matsumoto;Yinglin Song;Jing Ma;Zhaoxu Chen;Kazuyuki Tatsumi;Mark G. Humphrey
Advanced Materials 2008 Volume 20( Issue 10) pp:1870-1875
Publication Date(Web):
DOI:10.1002/adma.200702645
Co-reporter:Guodong Tang, Yuan Cao, Jinfang Zhang, Yu Zhang, Yinglin Song, Fengli Bei, Lude Lu, Chi Zhang
Synthetic Metals 2008 Volume 158(Issue 7) pp:264-272
Publication Date(Web):May 2008
DOI:10.1016/j.synthmet.2008.01.015
A series of new candidates as nonlinear optical materials, tetra-nuclear heterobimetallic clusters [MOS3M3′Y(PPh3)3] (M = Mo, M′ = Ag, Y = Br 1; M = W, M′ = Ag, Y = I 2; M = Mo, M′ = Cu, Y = I 3; M = W, M′ = Cu, Y = I 4), have been synthesized by newly developed ligand-redistribution reaction for third-order nonlinear optical (NLO) studies. Single-crystal X-ray diffraction shows that clusters [MoX(μ3-S)3(μ3-Br)(AgPPh3)3] 1 and [WX(μ3-S)3(μ3-I)(CuPPh3)3] 4 (X = O0.5S0.51, O 4) adopt an isomorphous neutral cubane-like skeleton. Their optical nonlinearities were measured by Z-scan technique with an 8 ns pulsed laser at 532 nm. These clusters were found to exhibit effective nonlinear absorption, self-focusing effects and large optical limiting capabilities. The effective NLO susceptibilities χ(3) and the corresponding second-order hyperpolarizabilities γ of these clusters are also reported. The influence of cluster composition on NLO properties has been discussed accordingly.
Co-reporter:Zhipeng Huang ; Chifang Wang ; Zhibo Chen ; Hua Meng ; Cuncai Lv ; Zhongzhong Chen ; Ruqu Han
ACS Applied Materials & Interfaces () pp:
Publication Date(Web):
DOI:10.1021/am501940x
Tungsten sulfides, including WS2 (crystalline) and WS3 (amorphous), were introduced to silicon nanowires, and both can promote the photoelectrochemical hydrogen production of silicon nanowires. In addition, more enhancement of energy conversion efficiency can be achieved by the loading of WS3, in comparison with loading of WS2. Polarization curves of WS3 and WS2 suggest that WS3 has higher catalytic activity in the hydrogen evolution reaction than WS2, affording higher energy conversion efficiency in silicon nanowires decorated with WS3. The higher electrocatalytic activity of WS3 correlates with the amorphous structure of WS3 and larger surface area of WS3, which result in more active sites in comparison with crystalline WS2.
Co-reporter:Zhipeng Huang, Maoying Li, Ding Jia, Peng Zhong, Feng Tian, Zhongzhong Chen, Mark G. Humphrey and Chi Zhang
Journal of Materials Chemistry A 2014 - vol. 2(Issue 8) pp:NaN1426-1426
Publication Date(Web):2013/11/25
DOI:10.1039/C3TC31919A
Semiconductor–semiconductor hetero-nanorods (Ag2Se–CdSe and Ag2Se–ZnSe) with high crystallinity have been synthesized by a facile and low-cost method. High resolution transmission electron microscopy investigations reveal that the growth follows a catalyst-assisted mechanism. A preliminary investigation of nonlinear optical properties shows that the hetero-nanorods exhibit significantly enhanced third-order nonlinear optical properties. The free carrier absorption cross-section of Ag2Se–CdSe hetero-nanorods is one order of magnitude higher than that of the corresponding single component CdSe nanocrystals. The results obtained in this study represent a new approach to the design and construction of metal selenide hetero-nanorods with high crystallinity and enhanced nonlinear optical capabilities.
Co-reporter:Tingting You, Junli Wang, Hui Feng, Kangmin Chen, Weiling Fan, Chi Zhang and Runsheng Miao
Dalton Transactions 2013 - vol. 42(Issue 21) pp:NaN7730-7730
Publication Date(Web):2013/03/13
DOI:10.1039/C3DT50301A
Template growth and catalytic growth are two typical mechanisms for the solution-chemistry synthesis of one-dimensional (1D) II–VI semiconductor nanomaterials. Here, we systematically demonstrate the competition relationship between them by tuning the synthesis of 1D ZnS nanostructures in different chain-length primary alkyl-amines. The template growth, derived from the coordination effect of amines, produces ZnS nanobelts and will compete with the Ag2S-catalyzed mechanism as AgNO3 is added into these amines. In short-chain n-propylamine and n-butylamine the template growth is much stronger than the catalytic growth, leading to the morphology maintenance of ZnS nanobelts, whereas the latter replaces the former in long-chain n-octylamine and n-dodecylamine due to the decrease of coordination ability of amines, which yields ZnS nanowires instead of nanobelts. A balance of competition is built between these two mechanisms in middle-length n-hexylamine, producing a mixture of ZnS nanobelts and nanowires. The morphology and growth mechanism changes of ZnS nanostructures have been rationally investigated using various characterization techniques. Meanwhile, the optical properties of the products synthesized before and after adding AgNO3 are comparatively studied by UV-vis absorption and photoluminescence (PL) spectra.
Co-reporter:
Analytical Methods (2009-Present) 2013 - vol. 5(Issue 23) pp:
Publication Date(Web):
DOI:10.1039/C3AY41475B
A fluorescent ratiometric probe, compound 1, for cyanide has been rationally constructed based on an intramolecular charge transfer (ICT) mechanism. Upon treatment with cyanide, probe 1 exhibited a fluorescence ratiometric response, with the emission wavelength displaying a very large shift (up to 160 nm). When 2 equivalents of cyanide were added, the emission ratios (I458/I618) of probe 1 changed dramatically from 0.027 to 28.306. In addition, the emission ratios (I458/I618) showed good linearity with the cyanide concentration in the range of 0–6.0 μM, and the detection limit measured to be 0.126 μM. The NMR experiments and theoretical calculations confirmed that the ratiometric response of probe 1 to cyanide is due to the nucleophilic addition reaction of the cyanide with the vinyl malononitrile group of probe 1, which results in the inhibition of the ICT process in the probe. Importantly, probe 1 has been applied to detection of cyanide in a natural water sample with satisfactory recovery. Furthermore, the quantitative determination of endogenous cyanide in cassava root demonstrated that the probe can be employed to detect endogenous cyanide in real biological samples.
Co-reporter:Lingliang Long, Yanjun Wu, Lin Wang, Aihua Gong, Feilong Hu and Chi Zhang
Chemical Communications 2015 - vol. 51(Issue 52) pp:NaN10438-10438
Publication Date(Web):2015/05/18
DOI:10.1039/C5CC03972J
Herein, a novel signaling mechanism for constructing fluorescent probes was demonstrated for the first time based on modulation of the unique rotation of the N–N single bond in the acetohydrazide group. According to the new signaling mechanism, a fluorescent probe for hypochlorite was then judiciously developed.
Co-reporter:Cuncai Lv, Zhibo Chen, Zhongzhong Chen, Bin Zhang, Yong Qin, Zhipeng Huang and Chi Zhang
Journal of Materials Chemistry A 2015 - vol. 3(Issue 34) pp:NaN17675-17675
Publication Date(Web):2015/07/24
DOI:10.1039/C5TA03438H
Iron phosphide (FeP) was introduced onto silicon nanowires (SiNWs) via precursor loading and phosphorization. The resultant SiNWs/FeP shows remarkably enhanced photoelectrochemical hydrogen production in comparison with bare SiNWs. The solar power conversion efficiency of SiNWs/FeP is as high as 2.64%, which is 94% of that of SiNWs modified with Pt particles, and is larger than those of silicon-based photocathodes loaded with other non-precious electrocatalysts such as transition metals and their chalcogenides. The faster reaction rate of the hydrogen evolution reaction (HER) on the surface of the SiNWs/FeP than that of the bare SiNWs was confirmed by an electrochemistry impedance experiment (EIS). The investigations over the EIS spectra and the flat band potential show that the onset potential of cathodic photocurrent is mainly influenced by the reaction rate of the HER on the surface of the photocathode. The transient photocurrent experiments also suggest the faster kinetics of the HER on the surface of the SiNWs/FeP in comparison with that of the bare SiNWs. This result demonstrates a convenient approach to SiNWs loaded with a highly effective electrocatalyst and its promising application potential in photoelectrochemical hydrogen generation.
Co-reporter:Lingliang Long, Liping Zhou, Lin Wang, Suci Meng, Aihua Gong, Fengyi Du and Chi Zhang
Organic & Biomolecular Chemistry 2013 - vol. 11(Issue 47) pp:NaN8220-8220
Publication Date(Web):2013/10/15
DOI:10.1039/C3OB41741G
In this work, compound 1 has been rationally designed and synthesized as a new fluorescent probe for biological thiols. Notably, probe 1 has almost no background fluorescence (Φf < 0.0001) in aqueous solutions; however, it exhibited fluorescence turn-on response to thiols with high sensitivity (a 246-fold fluorescence enhancement and a low detection limit of 0.22 μM for Cys). Moreover, probe 1 showed excellent thiol specificity over other biologically relevant species. The kinetic studies indicated that the probe responded to thiols rapidly, and the pseudo-first-order rate constants of probe 1 reaction with Cys, Hcy, and GSH were determined to be 1.85842, 0.67656, and 0.51519 min−1, respectively. A possible detection mechanism was proposed to involve the Michael addition of the thiol to the α,β-unsaturated ketone, followed by a cleavage of the hemiketal group, thereby leading to the formation of a fluorescent 7-hydroxyl coumarin derivative. Furthermore, the optical responses of probe 1 to thiols were studied by TD-DFT calculations. Finally, probe 1 has been successfully applied to the detection of biological thiols in human blood serum. And the intracellular imaging applications established that probe 1 can be used to detect different concentrations of intracellular thiols in living cells.
Co-reporter:Aijian Wang, Lingliang Long, Suci Meng, Xiufen Li, Wei Zhao, Yinglin Song, Marie P. Cifuentes, Mark G. Humphrey and Chi Zhang
Organic & Biomolecular Chemistry 2013 - vol. 11(Issue 25) pp:NaN4257-4257
Publication Date(Web):2013/04/16
DOI:10.1039/C3OB40323H
A novel porphyrin derivative bearing one D–π–A–π–D pyrimidine chromophore at the periphery was designed, prepared, and studied using the Z-scan technique, the results showing that this compound exhibits enhanced nonlinear optical (NLO) absorption, refraction and optical limiting responses. The significant NLO properties can be ascribed to an effective combination of distinct nonlinear mechanisms.
Co-reporter:Junli Wang, Congming Yang, Zhipeng Huang, Mark G. Humphrey, Ding Jia, Tingting You, Kangmin Chen, Qing Yang and Chi Zhang
Journal of Materials Chemistry A 2012 - vol. 22(Issue 19) pp:
Publication Date(Web):
DOI:10.1039/C2JM00091A
Co-reporter:Cuncai Lv, Zhen Peng, Yaoxing Zhao, Zhipeng Huang and Chi Zhang
Journal of Materials Chemistry A 2016 - vol. 4(Issue 4) pp:NaN1460-1460
Publication Date(Web):2015/12/22
DOI:10.1039/C5TA08715E
The development of an effective, non-precious electrocatalyst for the hydrogen evolution reaction (HER) is highly desirable for the commercial application of hydrogen as a clean and renewable energy and remains a substantial challenge. Herein, a hierarchical nanowires array (HNA) of iron phosphide (FeP) nanowires coated with iron phosphide nanorods grown on a carbon fiber paper (CFP) was constructed which exhibited remarkable catalytic activity in the HER. The overpotential required for the current density of 20 mA cm−2 is as small as 45 and 221 mV in acidic and basic solution, respectively, corresponding to Tafel slopes of 53 and 134 mV dec−1. The effective catalytic activity of the CFP–FeP HNA in the HER, together with its long-term stability and nearly 100% faradaic efficiency in water electrolysis, make the CFP–FeP HNA one of the best non-noble electrocatalysts described to date. The prominent catalytic activity of CFP–FeP HNA is correlated to the large number of active sites for the HER, and the fast electron transport from the CFP to the FeP nanorods mediated by FeP nanowires.
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