Zn-doped TiO2 (Zn?TiO2) thin films were prepared by the sol?gel method on titanium substrates with heat treatment at different temperatures. The effects of heat treatment temperatures and Zn doping on the structure, p...Zn-doped TiO2 (Zn?TiO2) thin films were prepared by the sol?gel method on titanium substrates with heat treatment at different temperatures. The effects of heat treatment temperatures and Zn doping on the structure, photocathodic protection and photoelectrochemical properties of TiO2 thin films were investigated. It is indicated that the photoelectrical performance of the Zn?TiO2 films is enhanced with the addition of Zn element compared with the pure-TiO2 film and the largest decline by 897 mV in the electrode potential is achieved under 300 °C heat treatment. SEM?EDS analyses show that Zn element is unevenly distributed in Zn?TiO2 films; XRD patterns reveal that the grain size of Zn?TiO2 is smaller than that of pure-TiO2; FTIR results indicate that Zn - O bond forms on Zn?TiO2 surface. Ultraviolet visible absorption spectra prove that Zn?TiO2 shifts to visible light region.Mott?Shottky curves show that the flat-band potential of Zn?TiO2 is more negative and charge carrier density is bigger than that ofpure-TiO2, implying that under the synergy of the width of the space-charge layer, carrier density and flat-band potential, Zn?TiO2 with 300 °C heat treatment displays the best photocathodic protection performance.展开更多
Birnessite films on fluorine-doped tin oxide(FTO) coated glass were prepared by cathodic reduction of aqueous KMnO4. The deposited birnessite films were characterized with X-ray diffraction, Raman spectroscopy, scan...Birnessite films on fluorine-doped tin oxide(FTO) coated glass were prepared by cathodic reduction of aqueous KMnO4. The deposited birnessite films were characterized with X-ray diffraction, Raman spectroscopy, scanning electron microscopy and atomic force microscopy.The photoelectrochemical activity of birnessite films was investigated and a remarkable photocurrent in response to visible light was observed in the presence of phenol, resulting from localized manganese d–d transitions. Based on this result, the photoelectrocatalytic oxidation of phenol was investigated. Compared with phenol degradation by the electrochemical oxidation process or photocatalysis separately, a synergetic photoelectrocatalytic degradation effect was observed in the presence of the birnessite film coated FTO electrode.Photoelectrocatalytic degradation ratios were influenced by film thickness and initial phenol concentrations. Phenol degradation with the thinnest birnessite film and initial phenol concentration of 10 mg/L showed the highest efficiency of 91.4% after 8 hr. Meanwhile, the kinetics of phenol removal was fit well by the pseudofirst-order kinetic model.展开更多
Nanocomposites composed of one-dimensional(1D) CdS nanowires(NWs) and 1 T-MoS2 nanosheets have been fabricated through a two-step solvothermal process. 5 mol% of MoS2 loading results in the best optical properties...Nanocomposites composed of one-dimensional(1D) CdS nanowires(NWs) and 1 T-MoS2 nanosheets have been fabricated through a two-step solvothermal process. 5 mol% of MoS2 loading results in the best optical properties,photoelectrochemical(PEC) as well as photocatalytic activities for hydrogen evolution reaction(HER). Compared with pure CdS NWs, the optimized nanocomposite shows 5.5 times enhancement in photocurrent and 86.3 times increase for HER in the presence of glucose and lactic acid as hole scavengers.The enhanced PEC and HER activities are attributed to the intimate contact between MoS2 and CdS that efficiently enhances charge carrier separation. In addition, ultrafast transient absorption(TA) measurements have been used to probe the charge carrier dynamics and gain deeper insight into the mechanism behind the enhanced PEC and photocatalytic performance.展开更多
Crystal phase engineering on CulnS2(CIS)nanocrystals,especially polytypic structure,has become one of the research hotspots to design the advanced materials and devices for energy conversion and environment treatment....Crystal phase engineering on CulnS2(CIS)nanocrystals,especially polytypic structure,has become one of the research hotspots to design the advanced materials and devices for energy conversion and environment treatment.Here,the polytypic CIS nanosheets(NSs)including zincblende/wutzite and chalcopyrite/wurtzite types were first time achieved in a hot-injection system using oleic acid and liquid paraffin as the reaction media.As-obtained polytypic CIS NSs exhibit significantly enhanced light-absorption abillty and visible-light-driven photocatalytic performance originating from the rational hetero-crystalline interfaces and surface defect states,which efficiently inhibit the recombination of photo-generated carriers.Meanwhile,the polytypic CIS NSs were spin-coated onto the surface of fluorinated-tin oxide glass substrate and used as the photoelectrode,which shows an excellent photoelectrochemical(PEC)activity in aqueous solution.The present work not only provides a facile,rapid,low-cost,and environmental-friendly synthesis strategy to design the crystal phase and defect structure of ternary chalcogenides,but also demonstrates the relationships between the polytypic structure and photocatalytic/photoelectrochemical properties.展开更多
Supertetrahedral zinc-gallium-tin sulfide cluster modified with reduced graphene oxide protective layer was first synthesized, which exhibited an excellent photoelectrochemical performance and enhanced stability in co...Supertetrahedral zinc-gallium-tin sulfide cluster modified with reduced graphene oxide protective layer was first synthesized, which exhibited an excellent photoelectrochemical performance and enhanced stability in comparison to supertetrahedral clusters.展开更多
Developing a high-quality photoelectrode for photoelectrochemical applications is still an ongoing challenge. In this study, we prepared the g-C_(3)N_(4) film on the indium tin oxide(ITO) glass through conventional co...Developing a high-quality photoelectrode for photoelectrochemical applications is still an ongoing challenge. In this study, we prepared the g-C_(3)N_(4) film on the indium tin oxide(ITO) glass through conventional coating, liquid-based growth, in-situ calcination, and vapor deposition methods, respectively. These electrodes were characterized and used as photoanodes to degrade methylene blue(MB) in water. Among these methods, the in-situ calcination method was most appropriate for preparing the continuous and organized g-C_(3)N_(4) film electrodes with uniform g-C_(3)N_(4) coverage and strong adhesion to the ITO substrate.It also had the highest activity in the photocatalytic(PC), electrochemical(EC), and photoelectrocatalytic(PEC) degradation processes of MB. In the PEC reaction, at an applied potential of 1.0 V and a light intensity of 0.96 W/cm^(2), the removal rate of MB was 62.5%, which was much higher than those in the PC and EC reactions. The high degradation rate was due to the synergistic effect of PEC degradation, wherein the PC and EC reactions promote and optimize each other. In the PC reaction, MB was degraded by-CH_(3) elimination, while the EC degradation pathway mainly included the conversion of sulfhydryl into sulfoxide and the opening of the central aromatic ring. Both methyl loss and aromatic ring opening occurred in the PEC reaction. Moreover, some monocyclic compounds were formed, and MB showed more complete degradation in the PEC reaction.展开更多
基金Project(cstc2011jj A50008)supported by the Natural Science Foundation of Chongqing,ChinaProject(14ZB0025)supported by Education Department of Sichuan Province,China
文摘Zn-doped TiO2 (Zn?TiO2) thin films were prepared by the sol?gel method on titanium substrates with heat treatment at different temperatures. The effects of heat treatment temperatures and Zn doping on the structure, photocathodic protection and photoelectrochemical properties of TiO2 thin films were investigated. It is indicated that the photoelectrical performance of the Zn?TiO2 films is enhanced with the addition of Zn element compared with the pure-TiO2 film and the largest decline by 897 mV in the electrode potential is achieved under 300 °C heat treatment. SEM?EDS analyses show that Zn element is unevenly distributed in Zn?TiO2 films; XRD patterns reveal that the grain size of Zn?TiO2 is smaller than that of pure-TiO2; FTIR results indicate that Zn - O bond forms on Zn?TiO2 surface. Ultraviolet visible absorption spectra prove that Zn?TiO2 shifts to visible light region.Mott?Shottky curves show that the flat-band potential of Zn?TiO2 is more negative and charge carrier density is bigger than that ofpure-TiO2, implying that under the synergy of the width of the space-charge layer, carrier density and flat-band potential, Zn?TiO2 with 300 °C heat treatment displays the best photocathodic protection performance.
基金supported by the National Basic Research Program(973)of China(No.2014CB846001)the NationalNatural Science Foundation of China(Nos.41230103,41402032&41402301)
文摘Birnessite films on fluorine-doped tin oxide(FTO) coated glass were prepared by cathodic reduction of aqueous KMnO4. The deposited birnessite films were characterized with X-ray diffraction, Raman spectroscopy, scanning electron microscopy and atomic force microscopy.The photoelectrochemical activity of birnessite films was investigated and a remarkable photocurrent in response to visible light was observed in the presence of phenol, resulting from localized manganese d–d transitions. Based on this result, the photoelectrocatalytic oxidation of phenol was investigated. Compared with phenol degradation by the electrochemical oxidation process or photocatalysis separately, a synergetic photoelectrocatalytic degradation effect was observed in the presence of the birnessite film coated FTO electrode.Photoelectrocatalytic degradation ratios were influenced by film thickness and initial phenol concentrations. Phenol degradation with the thinnest birnessite film and initial phenol concentration of 10 mg/L showed the highest efficiency of 91.4% after 8 hr. Meanwhile, the kinetics of phenol removal was fit well by the pseudofirst-order kinetic model.
基金financially supported by the National Natural Science Foundation of China (51402126)support from Delta Dental Health Associates, NASA through MACES (NNX15AQ01A)UCSC Committee on Research Special Research Grant
文摘Nanocomposites composed of one-dimensional(1D) CdS nanowires(NWs) and 1 T-MoS2 nanosheets have been fabricated through a two-step solvothermal process. 5 mol% of MoS2 loading results in the best optical properties,photoelectrochemical(PEC) as well as photocatalytic activities for hydrogen evolution reaction(HER). Compared with pure CdS NWs, the optimized nanocomposite shows 5.5 times enhancement in photocurrent and 86.3 times increase for HER in the presence of glucose and lactic acid as hole scavengers.The enhanced PEC and HER activities are attributed to the intimate contact between MoS2 and CdS that efficiently enhances charge carrier separation. In addition, ultrafast transient absorption(TA) measurements have been used to probe the charge carrier dynamics and gain deeper insight into the mechanism behind the enhanced PEC and photocatalytic performance.
基金This work was financially supported by the Joint Foundation of National Natural Science Foundation of China(No.U1764254)321 Talent Project of Nanjing,China(No.631783)and 111 Project,China(No.D17003)
文摘Crystal phase engineering on CulnS2(CIS)nanocrystals,especially polytypic structure,has become one of the research hotspots to design the advanced materials and devices for energy conversion and environment treatment.Here,the polytypic CIS nanosheets(NSs)including zincblende/wutzite and chalcopyrite/wurtzite types were first time achieved in a hot-injection system using oleic acid and liquid paraffin as the reaction media.As-obtained polytypic CIS NSs exhibit significantly enhanced light-absorption abillty and visible-light-driven photocatalytic performance originating from the rational hetero-crystalline interfaces and surface defect states,which efficiently inhibit the recombination of photo-generated carriers.Meanwhile,the polytypic CIS NSs were spin-coated onto the surface of fluorinated-tin oxide glass substrate and used as the photoelectrode,which shows an excellent photoelectrochemical(PEC)activity in aqueous solution.The present work not only provides a facile,rapid,low-cost,and environmental-friendly synthesis strategy to design the crystal phase and defect structure of ternary chalcogenides,but also demonstrates the relationships between the polytypic structure and photocatalytic/photoelectrochemical properties.
文摘Supertetrahedral zinc-gallium-tin sulfide cluster modified with reduced graphene oxide protective layer was first synthesized, which exhibited an excellent photoelectrochemical performance and enhanced stability in comparison to supertetrahedral clusters.
基金financial support from the National Natural Science Foundation of China(No.51978658)。
文摘Developing a high-quality photoelectrode for photoelectrochemical applications is still an ongoing challenge. In this study, we prepared the g-C_(3)N_(4) film on the indium tin oxide(ITO) glass through conventional coating, liquid-based growth, in-situ calcination, and vapor deposition methods, respectively. These electrodes were characterized and used as photoanodes to degrade methylene blue(MB) in water. Among these methods, the in-situ calcination method was most appropriate for preparing the continuous and organized g-C_(3)N_(4) film electrodes with uniform g-C_(3)N_(4) coverage and strong adhesion to the ITO substrate.It also had the highest activity in the photocatalytic(PC), electrochemical(EC), and photoelectrocatalytic(PEC) degradation processes of MB. In the PEC reaction, at an applied potential of 1.0 V and a light intensity of 0.96 W/cm^(2), the removal rate of MB was 62.5%, which was much higher than those in the PC and EC reactions. The high degradation rate was due to the synergistic effect of PEC degradation, wherein the PC and EC reactions promote and optimize each other. In the PC reaction, MB was degraded by-CH_(3) elimination, while the EC degradation pathway mainly included the conversion of sulfhydryl into sulfoxide and the opening of the central aromatic ring. Both methyl loss and aromatic ring opening occurred in the PEC reaction. Moreover, some monocyclic compounds were formed, and MB showed more complete degradation in the PEC reaction.