Photoelectrochemical(PEC) cathodic protection is considered as an environment friendly method for metals anticorrosion. In this technology, a n-type semiconductor photoanode provides the photogenerated electrons for m...Photoelectrochemical(PEC) cathodic protection is considered as an environment friendly method for metals anticorrosion. In this technology, a n-type semiconductor photoanode provides the photogenerated electrons for metal to achieve cathodic protection. Comparing with traditional PEC photoanode for water splitting, it requires the photoanode providing a suitable cathodic potential for the metal, instead of pursuit ultimate photon to electric conversion efficiency, thus it is a more possible PEC technology for engineering application. To date, great efforts have been devoted to developing novel n-type semiconductors and advanced modification method to improve the performance on PEC cathodic protection metals. Herein, recent progresses in this field are summarized. We highlight the fabrication process of PEC cathodic protection thin film, various nanostructure controlling, doping, compositing methods and their operation mechanism. Finally, the current challenges and future potential works on improving the PEC cathodic protection performance are discussed.展开更多
Photoelectrochemical(PEC)water splitting is recognized as a sustainable strategy for hydrogen generation due to its abundant hydrogen source,utilization of inexhaustible solar energy,high-purity product,and environmen...Photoelectrochemical(PEC)water splitting is recognized as a sustainable strategy for hydrogen generation due to its abundant hydrogen source,utilization of inexhaustible solar energy,high-purity product,and environment-friendly process.To actualize a practical PEC water splitting,it is paramount to develop efficient,stable,safe,and low-cost photoelectrode materials.Recently,graphitic carbon nitride(g-C3N4)has aroused a great interest in the new generation photoelectrode materials because of its unique features,such as suitable band structure for water splitting,a certain range of visible light absorption,nontoxicity,and good stability.Some inherent defects of g-C3N4,however,seriously impair further improvement on PEC performance,including low electronic conductivity,high recombination rate of photogenerated charges,and limited visible light absorption at long wavelength range.Construction of g-C3N4-based nanosized heteroarrays as photoelectrodes has been regarded as a promising strategy to circumvent these inherent limitations and achieve the high-performance PEC water splitting due to the accelerated exciton separation and the reduced combination of photogenerated electrons/holes.Herein,we summarize in detail the latest progress of g-C3N4-based nanosized heteroarrays in PEC water-splitting photoelectrodes.Firstly,the unique advantages of this type of photoelectrodes,including the highly ordered nanoarray architectures and the heterojunctions,are highlighted.Then,different g-C3N4-based nanosized heteroarrays are comprehensively discussed,in terms of their fabrication methods,PEC capacities,and mechanisms,etc.To conclude,the key challenges and possible solutions for future development on g-C3N4-based nanosized heteroarray photoelectrodes are discussed.展开更多
Solar energy driven photoelectrochemical(PEC) water splitting is a clean and powerful approach for renewable hydrogen production. The design and construction of metal oxide based nanoarray photoanodes is one of the pr...Solar energy driven photoelectrochemical(PEC) water splitting is a clean and powerful approach for renewable hydrogen production. The design and construction of metal oxide based nanoarray photoanodes is one of the promising strategies to make the continuous breakthroughs in solar to hydrogen conversion efficiency of PEC cells owing to their owned several advantages including enhanced reactive surface at the electrode/electrolyte interface, improved light absorption capability, increased charge separation efficiency and direct electron transport pathways. In this Review, we first introduce the structure,work principle and their relevant efficiency calculations of a PEC cell. We then give a summary of the state-of the-art research in the preparation strategies and growth mechanism for the metal oxide based nanoarrays, and some details about the performances of metal oxide based nanoarray photoanodes for PEC water splitting. Finally, we discuss key aspects which should be addressed in continued work on realizing high-efficiency metal oxide based nanoarray photoanodes for PEC solar water splitting systems.展开更多
Nanomaterial shapes can have profound effects on material properties, and therefore offer an efficient way to improve the performances of designed materials and devices. The rational fabrication of multidimensional ar...Nanomaterial shapes can have profound effects on material properties, and therefore offer an efficient way to improve the performances of designed materials and devices. The rational fabrication of multidimensional architectures such as one dimensional （1D）-two dimensional （2D） hybrid nanomaterials can integrate the merits of individual components and provide enhanced functionality. However, it is still very challenging to fabricate 1D/2D architectures because of the different growth mechanisms of the nanostructures. Here, we present a new solvent- mediated, surface reaction-driven growth route for synthesis of CdS nanowire （NW）/CdIn2S4 nanosheet （NS） 1D/2D architectures. The as-obtained CdS NW/ CdIn2S4 NS structures exhibit much higher visible-light-responsive photocatalytic activities for water splitting than the individual components. The CdS NW/CdIn2S4 NS heterostructure was further fabricated into photoelectrodes, which achieved a considerable photocurrent density of 2.85 mA·cm^-2 at 0 V vs. the reversible hydrogen electrode （RHE） without use of any co-catalysts. This represents one of the best results from a CdS-based photoelectrochemical （PEC） cell. Both the multidimensional nature and type II band alignment of the 1D/2D CdS/CdIn2S4 heterostructure contribute to the enhanced photocatalyfic and photoelectrochemical activity. The present work not only provides a new strategy for designing multidimensional 1D/2D heterostructures, but also documents the development of highly efficient energy conversion catalysts.展开更多
Electrochemical water splitting is an efficient and clean strategy to produce sustainable energy produc- tions （especially hydrogen） from earth-abundant water. Recently, layered double hydroxide （LDH）-based materi...Electrochemical water splitting is an efficient and clean strategy to produce sustainable energy produc- tions （especially hydrogen） from earth-abundant water. Recently, layered double hydroxide （LDH）-based materi- als have gained increasing attentions as promising electrocatalysts for water splitting. Designing LDHs into hierarchical architectures （e.g., core-shell nanoarrays） is one of the most promising strategies to improve their electrocatalytic performances, owing to the abundant exposure of active sites. This review mainly focuses on recent progress on the synthesis of hierarchical LDH-based core-shell nanoarrays as high performance electrocatalysts for electrochemical water splitting. By classifying different nanostructured materials combined with LDHs, a number of LDH-based core-shell nanoarrays have been developed and their synthesis strategies, structural characters and electrochemical performances are rationally described. Moreover, further developments and challenges in devel- oping promising electrocatalysts based on hierarchical nanostructured LDHs are covered from the viewpoint of fundamental research and practical applications.展开更多
Sustainable development and continued prosperity of humanity hinge on the availability of renewable energy sources on a terawatts scale. In the long run, solar energy is the only source that can meet this daunting dem...Sustainable development and continued prosperity of humanity hinge on the availability of renewable energy sources on a terawatts scale. In the long run, solar energy is the only source that can meet this daunting demand. Widespread utilization of solar energy faces challenges as a result of its diffusive （hence low energy density） and intermittent nature. How to effectively harvest, concentrate, store and redistribute solar energy constitutes a fundamental challenge that the scientific community needs to address. Photoelectrochemical （PEC） water splitting is a process that can directly convert solar energy into chemical energy and store it in chemical bonds, by producing hydrogen as a clean fuel source. It has received significant research attention lately. Here we provide a concise review of the key issues encountered in carrying out PEC water splitting. Our focus is on the balance of considerations such as stability, earth abundance, and efficiency. Particular attention is paid to the combination of photoelectrodes with electrocatalysts, especially on the interfaces between different components.展开更多
To drive photoelectrochemical water splitting on porous BiVO4 photoanode,we herein prepared a carnationlike CuS powder by hydrothermal method and then loaded it onto BiVO4 photoelectrode.Expectedly,the CuS/BiVO4 compo...To drive photoelectrochemical water splitting on porous BiVO4 photoanode,we herein prepared a carnationlike CuS powder by hydrothermal method and then loaded it onto BiVO4 photoelectrode.Expectedly,the CuS/BiVO4 composite not only presents a higher photocurrent response value at 1.23 V versus RHE(reversible hydrogen electrode)than pure BiVO4 electrode under visible light irradiation,but also exhibits an excellent photoelectrochemical hydrogen production activity in comparison with either the BiVO4 or the CuS.The high ameliorated performance of CuS/BiVO4 composite may be due to the strong absorption of visible light and an effective abatement in combination of carriers.These results demonstrate an effective potential approach to design and construct efficient photoelectrochemical(PEC)systems.展开更多
Transition-metal dichalcogenide(TMD) semiconductors have attracted interest as photoelectrochemical(PEC) electrodes due to their novel band-gap structures,optoelectronic properties, and photocatalytic activities.Howev...Transition-metal dichalcogenide(TMD) semiconductors have attracted interest as photoelectrochemical(PEC) electrodes due to their novel band-gap structures,optoelectronic properties, and photocatalytic activities.However, the photo-harvesting efficiency still requires improvement. In this study, A TMD stacked heterojunction structure was adopted to further enhance the performance of the PEC cathode. A P-type WSe_2 and an N-type Mo S_2 monolayer were stacked layer-by-layer to build a ultrathin vertical heterojunction using a micro-fabrication method.In situ measurement was employed to characterize the intrinsic PEC performance on a single-sheet heterostructure.Benefitting from its built-in electric field and type II band alignment, the MoS_2/WSe_2 bilayer heterojunction exhibited exceptional photocatalytic activity and a high incident photo-to-current conversion efficiency(IPCE). Comparing with the monolayer WSe_2 cathode, the PEC current and the IPCE of the bilayer heterojunction increased by a factor of 5.6 and enhanced 50%, respectively. The intriguing performance renders the MoS_2/WSe_2 heterojunction attractive for application in high-performance PEC water splitting.展开更多
Photoanodes, which are used in photoelectrochemical （PEC） water splitting, have been shown to be applicable in the construction of a PEC biosensing platform. This was realized by replacing water oxidization with oxi...Photoanodes, which are used in photoelectrochemical （PEC） water splitting, have been shown to be applicable in the construction of a PEC biosensing platform. This was realized by replacing water oxidization with oxidation of an appropriate test molecule. Here, we have demonstrated the feasibility of adopting photoanodes consisting of zinc oxide nanorods arrays decorated with plasmonic gold nanoparticles （Au NPs@ZnO NRs） for the self-powered PEC bioanalysis of glutathione （GSH） in phosphate-buffered saline （PBS） at an applied bias potential of 0 V vs. Ag/AgCl. This heterostructure exhibited enhanced PEC properties because of the introduction of the Au/ZnO interface. Under visible light illumination, hot electrons from surface-plasmon resonance （SPR） at the Au NP surface were injected into the adjacent ZnO and subsequently driven to the photocathode. Under ultraviolet （UV） light illumination, the photogenerated electrons in ZnO tended to transfer to the fluorine-doped tin oxide due to the step-wise energy band structure and the upward energy band bending at the ZnO/ electrolyte interface. These results indicate that plasmonic metal/semiconductor heterostructure photoanodes have great potential for self-powered PEC bioanalysis applications and extended field of other photovoltaic beacons.展开更多
Well-ordered TiO_2 nanotube arrays(TNTAs)decorated with graphitic carbon nitride(g-C_3N_4) were fabricated by anodic oxidization and calcination process.First, TNTAs were prepared via the anodic oxidation of Ti foil i...Well-ordered TiO_2 nanotube arrays(TNTAs)decorated with graphitic carbon nitride(g-C_3N_4) were fabricated by anodic oxidization and calcination process.First, TNTAs were prepared via the anodic oxidation of Ti foil in glycerol solution containing fluorinion and 20%deionized water. Subsequently, g-C_3N_4 film was hydrothermally grown on TNTAs via the hydrogen-bonded cyanuric acid melamine supramolecular complex. The results showed that g-C_3N_4 was successfully decorated on the TNTAs and the g-C_3N_4/TNTAs served as an efficient and stable photoanode for photoelectrochemical water splitting. The facile deposition method enables the fabrication of efficient and low-cost photoanodes for renewable energy applications.展开更多
Nanostructures have drawn great attentions for functional device applications. Among the various techniques developed for fabricating arrayed nanostructures of functional materials, nanostructuring technique with poro...Nanostructures have drawn great attentions for functional device applications. Among the various techniques developed for fabricating arrayed nanostructures of functional materials, nanostructuring technique with porous anodic aluminum oxide （AAO） membrane as templates becomes more attractive owing to the superior geometrical characteristics and low-cost preparation process. In this mini review, progress about functional we summarize our recent nanostructuring based on perfectly-ordered AAO membrane to prepare perfectly- ordered nanostructure arrays of functional materials toward constructing high-performance energy conversion and storage devices. By employing the perfectly-ordered AAO membrane as templates, arrayed nanostructures in the form ofnanodot, nanorod, nanotube and nanopore have been synthesized over a large area. These as-obtained nanostructure arrays have large specific surface area, high regularity, large-scale implementation, and tunable nanos- cale features. All these advanced features enable them to be of great advantage for the performance improvement of energy conversion and storage devices, including photo- electrochemical water splitting cells, supercapacitors, and batteries, etc.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
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
Yolk-shell architectures have attracted extensive attention owing to their unique structure and infusive applications. MoS2 is regarded as one of the most promising catalytic materials for hydrogen evolution by the sp...Yolk-shell architectures have attracted extensive attention owing to their unique structure and infusive applications. MoS2 is regarded as one of the most promising catalytic materials for hydrogen evolution by the splitting of water. In this work, a simple self-template solvothermal approach is developed for the synthesis of novel MoS2 yolk-shell microspheres with a hierarchical porous structure by reacting MoO2 microspheres with L-cysteine. A dissolution- recrystallization formation mechanism is proposed for the MoS2 yolk-shell microspheres. Owing to structural superiority, the new material architecture exhibits improved photoelectrochemical properties, including efficient hydrogen evolution reaction catalytic activities, a high photocurrent density, a small overpotential, and a low charge-transfer resistance.展开更多
Bismuth vanadate(BiVO4)is a promising photoanode material owing to the narrow bandgap,appropriate band position,and excellent resistance against photocorrosion,however,the performance of photoelectrochemical(PEC)water...Bismuth vanadate(BiVO4)is a promising photoanode material owing to the narrow bandgap,appropriate band position,and excellent resistance against photocorrosion,however,the performance of photoelectrochemical(PEC)water splitting is largely limited by the poor carrier separation and transport ability.To address these issues,for the first time,we fabricate BiVO4 film/CuO nanocone p-n junctions as photoanodes by combing a facile spin-coating process and water bath reaction.This structure strengthens the light harvesting and promotes the charge separation and transport ability.The surface defects states are passivated by coating conformally ultrathin TiO2 onto CuO surface through atomic layer deposition(ALD)technique.Benefiting from the favorable morphology,energy band,and surface treatment,the BiVO4/CuO/TiO2 heterojunction generates an improved photocurrent that is much higher than pure BiVO4.The detailed mechanism investigations indicate that the synergetic optimization of charge separation and injection efficiency in the bulk and surface of photoelectrodes can significantly improve the performance of PEC cells.展开更多
Surface treatment is an effective method to improve the photoelectrochemical(PEC) performance of photoelectrodes. Herein, we introduced a novel strategy of surface sulfurization to modify hematite(a-Fe2 O3)nanorods gr...Surface treatment is an effective method to improve the photoelectrochemical(PEC) performance of photoelectrodes. Herein, we introduced a novel strategy of surface sulfurization to modify hematite(a-Fe2 O3)nanorods grown in an aqueous solution, which triggered encouraging improvement in PEC performances.In comparison to the solution-grown pristine a-Fe2 O3 nanorod photoanode that is PEC inefficient and always needs high temperature(>600 °C) activation, the surface sulfurized a-Fe2 O3 nanorods show photocurrent density increased by orders of magnitude, reaching 0.46 mA cmà2 at 1.23 V vs. RHE(reversible hydrogen electrode) under simulated solar illumination. This improvement in PEC performances should be attributed to the synergy of the increased carrier density, the reduced surface charge carrier recombination and the accelerated water oxidation kinetics at the a-Fe2 O3/electrolyte interface, as induced by the incorporation of S ions and the formation of multi-state S species(Fe-Sx-Oy) at the surface of a-Fe2 O3 nanorods. This study paves a new and facile approach to activate a-Fe2 O3 and even other metal oxides as photoelectrodes for improved PEC water splitting performances, by engineering the surface structure to relieve the bottlenecks of charge transfer dynamics and redox reaction kinetics at the electrode/electrolyte interface.展开更多
Photoelectrochemical （PEC） water splitting is a promising approach to harvest and store solar energy [1]. Silicon has been widely investigated for PEC photoelectrodes due to its suitable band gap （1.12 eV） matchin...Photoelectrochemical （PEC） water splitting is a promising approach to harvest and store solar energy [1]. Silicon has been widely investigated for PEC photoelectrodes due to its suitable band gap （1.12 eV） matching the solar spectrum [2]. Here we investigate employing nickel both as a catalyst and protecting layer of a p-type silicon photocathode for photoelectrochemical hydrogen evolution in basic electrolytes for the first time. The silicon photocathode was made by depositing 15 nm Ti on a p-type silicon wafer followed by 5 nm Ni. The photocathode afforded an onset potential of -0.3 V vs. the reversible hydrogen electrode （RHE） in alkaline solution （1 M KOH）. The stability of the Ni/Ti/p-Si photocathode showed a 100 mV decay over 12 h in KOH, but the stability was significantly improved when the photocathode was operated in potassium borate buffer solution （pH ≈ 9.5）. The electrode surface was found to remain intact after 12 h of continuous operation at a constant current density of 10 mA/cm^2 in potassium borate buffer, suggesting that Ni affords good protection of Si based photocathodes in borate buffers.展开更多
基金supported by National Natural Science Foundation of China(Grant no.41506093)
文摘Photoelectrochemical(PEC) cathodic protection is considered as an environment friendly method for metals anticorrosion. In this technology, a n-type semiconductor photoanode provides the photogenerated electrons for metal to achieve cathodic protection. Comparing with traditional PEC photoanode for water splitting, it requires the photoanode providing a suitable cathodic potential for the metal, instead of pursuit ultimate photon to electric conversion efficiency, thus it is a more possible PEC technology for engineering application. To date, great efforts have been devoted to developing novel n-type semiconductors and advanced modification method to improve the performance on PEC cathodic protection metals. Herein, recent progresses in this field are summarized. We highlight the fabrication process of PEC cathodic protection thin film, various nanostructure controlling, doping, compositing methods and their operation mechanism. Finally, the current challenges and future potential works on improving the PEC cathodic protection performance are discussed.
基金This study was supported by Developed and Applied Funding of Tianjin Normal University(135202XK1702)Program for Innovative Research in the University of Tianjin(TD13-5077)+1 种基金National Natural Science Foundation of China(Number 21905202)Australian Research Council(ARC)through Discovery Early Career Researcher Awards(DECRA,DE170100871).
文摘Photoelectrochemical(PEC)water splitting is recognized as a sustainable strategy for hydrogen generation due to its abundant hydrogen source,utilization of inexhaustible solar energy,high-purity product,and environment-friendly process.To actualize a practical PEC water splitting,it is paramount to develop efficient,stable,safe,and low-cost photoelectrode materials.Recently,graphitic carbon nitride(g-C3N4)has aroused a great interest in the new generation photoelectrode materials because of its unique features,such as suitable band structure for water splitting,a certain range of visible light absorption,nontoxicity,and good stability.Some inherent defects of g-C3N4,however,seriously impair further improvement on PEC performance,including low electronic conductivity,high recombination rate of photogenerated charges,and limited visible light absorption at long wavelength range.Construction of g-C3N4-based nanosized heteroarrays as photoelectrodes has been regarded as a promising strategy to circumvent these inherent limitations and achieve the high-performance PEC water splitting due to the accelerated exciton separation and the reduced combination of photogenerated electrons/holes.Herein,we summarize in detail the latest progress of g-C3N4-based nanosized heteroarrays in PEC water-splitting photoelectrodes.Firstly,the unique advantages of this type of photoelectrodes,including the highly ordered nanoarray architectures and the heterojunctions,are highlighted.Then,different g-C3N4-based nanosized heteroarrays are comprehensively discussed,in terms of their fabrication methods,PEC capacities,and mechanisms,etc.To conclude,the key challenges and possible solutions for future development on g-C3N4-based nanosized heteroarray photoelectrodes are discussed.
基金supported by the National Key Research and Development Program of China (2018YFA0209600)Shenzhen Peacock Plan (KQTD2016053015544057)Nanshan Pilot Plan (LHTD20170001)
文摘Solar energy driven photoelectrochemical(PEC) water splitting is a clean and powerful approach for renewable hydrogen production. The design and construction of metal oxide based nanoarray photoanodes is one of the promising strategies to make the continuous breakthroughs in solar to hydrogen conversion efficiency of PEC cells owing to their owned several advantages including enhanced reactive surface at the electrode/electrolyte interface, improved light absorption capability, increased charge separation efficiency and direct electron transport pathways. In this Review, we first introduce the structure,work principle and their relevant efficiency calculations of a PEC cell. We then give a summary of the state-of the-art research in the preparation strategies and growth mechanism for the metal oxide based nanoarrays, and some details about the performances of metal oxide based nanoarray photoanodes for PEC water splitting. Finally, we discuss key aspects which should be addressed in continued work on realizing high-efficiency metal oxide based nanoarray photoanodes for PEC solar water splitting systems.
基金This work was financially supported by the National Natural Science Foundation of China （Nos. 51372173, 21673160, and 51420105002）, Natural Science Foundation of Zhejiang for Distinguished Young Scholars （No. LR16B010002）, Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure （No. SKL201409SIC）, and startup funds of Syracuse University.
文摘Nanomaterial shapes can have profound effects on material properties, and therefore offer an efficient way to improve the performances of designed materials and devices. The rational fabrication of multidimensional architectures such as one dimensional （1D）-two dimensional （2D） hybrid nanomaterials can integrate the merits of individual components and provide enhanced functionality. However, it is still very challenging to fabricate 1D/2D architectures because of the different growth mechanisms of the nanostructures. Here, we present a new solvent- mediated, surface reaction-driven growth route for synthesis of CdS nanowire （NW）/CdIn2S4 nanosheet （NS） 1D/2D architectures. The as-obtained CdS NW/ CdIn2S4 NS structures exhibit much higher visible-light-responsive photocatalytic activities for water splitting than the individual components. The CdS NW/CdIn2S4 NS heterostructure was further fabricated into photoelectrodes, which achieved a considerable photocurrent density of 2.85 mA·cm^-2 at 0 V vs. the reversible hydrogen electrode （RHE） without use of any co-catalysts. This represents one of the best results from a CdS-based photoelectrochemical （PEC） cell. Both the multidimensional nature and type II band alignment of the 1D/2D CdS/CdIn2S4 heterostructure contribute to the enhanced photocatalyfic and photoelectrochemical activity. The present work not only provides a new strategy for designing multidimensional 1D/2D heterostructures, but also documents the development of highly efficient energy conversion catalysts.
文摘Electrochemical water splitting is an efficient and clean strategy to produce sustainable energy produc- tions （especially hydrogen） from earth-abundant water. Recently, layered double hydroxide （LDH）-based materi- als have gained increasing attentions as promising electrocatalysts for water splitting. Designing LDHs into hierarchical architectures （e.g., core-shell nanoarrays） is one of the most promising strategies to improve their electrocatalytic performances, owing to the abundant exposure of active sites. This review mainly focuses on recent progress on the synthesis of hierarchical LDH-based core-shell nanoarrays as high performance electrocatalysts for electrochemical water splitting. By classifying different nanostructured materials combined with LDHs, a number of LDH-based core-shell nanoarrays have been developed and their synthesis strategies, structural characters and electrochemical performances are rationally described. Moreover, further developments and challenges in devel- oping promising electrocatalysts based on hierarchical nanostructured LDHs are covered from the viewpoint of fundamental research and practical applications.
文摘Sustainable development and continued prosperity of humanity hinge on the availability of renewable energy sources on a terawatts scale. In the long run, solar energy is the only source that can meet this daunting demand. Widespread utilization of solar energy faces challenges as a result of its diffusive （hence low energy density） and intermittent nature. How to effectively harvest, concentrate, store and redistribute solar energy constitutes a fundamental challenge that the scientific community needs to address. Photoelectrochemical （PEC） water splitting is a process that can directly convert solar energy into chemical energy and store it in chemical bonds, by producing hydrogen as a clean fuel source. It has received significant research attention lately. Here we provide a concise review of the key issues encountered in carrying out PEC water splitting. Our focus is on the balance of considerations such as stability, earth abundance, and efficiency. Particular attention is paid to the combination of photoelectrodes with electrocatalysts, especially on the interfaces between different components.
基金financially supported by the National Natural Science Foundation of China (Nos. 21663027 and 21808189)the Natural Science Foundation of Gansu Province (No. 18JR3RA090)the Opening Project of Key Laboratory of Green Catalysis of Sichuan Institutes of High Education (No. LYJ18205)
文摘To drive photoelectrochemical water splitting on porous BiVO4 photoanode,we herein prepared a carnationlike CuS powder by hydrothermal method and then loaded it onto BiVO4 photoelectrode.Expectedly,the CuS/BiVO4 composite not only presents a higher photocurrent response value at 1.23 V versus RHE(reversible hydrogen electrode)than pure BiVO4 electrode under visible light irradiation,but also exhibits an excellent photoelectrochemical hydrogen production activity in comparison with either the BiVO4 or the CuS.The high ameliorated performance of CuS/BiVO4 composite may be due to the strong absorption of visible light and an effective abatement in combination of carriers.These results demonstrate an effective potential approach to design and construct efficient photoelectrochemical(PEC)systems.
基金supported by the National Natural Science Foundation of China (Grant Nos.51290271,51672314)the Guangdong Natural Science Foundation (Grant No.2016A030313359)+2 种基金the Science and Technology Program of Guangzhou (Grant No.201707010224)the Science and Technology Department of Guangdong Provincethe Fundamental Research Funds for the Central Universities
文摘Transition-metal dichalcogenide(TMD) semiconductors have attracted interest as photoelectrochemical(PEC) electrodes due to their novel band-gap structures,optoelectronic properties, and photocatalytic activities.However, the photo-harvesting efficiency still requires improvement. In this study, A TMD stacked heterojunction structure was adopted to further enhance the performance of the PEC cathode. A P-type WSe_2 and an N-type Mo S_2 monolayer were stacked layer-by-layer to build a ultrathin vertical heterojunction using a micro-fabrication method.In situ measurement was employed to characterize the intrinsic PEC performance on a single-sheet heterostructure.Benefitting from its built-in electric field and type II band alignment, the MoS_2/WSe_2 bilayer heterojunction exhibited exceptional photocatalytic activity and a high incident photo-to-current conversion efficiency(IPCE). Comparing with the monolayer WSe_2 cathode, the PEC current and the IPCE of the bilayer heterojunction increased by a factor of 5.6 and enhanced 50%, respectively. The intriguing performance renders the MoS_2/WSe_2 heterojunction attractive for application in high-performance PEC water splitting.
基金This work was supported by the National Major Research Program of China （No. 2013CB932602）, the Program of Introducing Talents of Discipline to Universities （No. B14003）, the National Natural Science Foundation of China （No. 51232001 and 51527802）, Beijing Municipal Science ＆ Technology Commission, the Fundamental Research Funds for the Central Universities.
文摘Photoanodes, which are used in photoelectrochemical （PEC） water splitting, have been shown to be applicable in the construction of a PEC biosensing platform. This was realized by replacing water oxidization with oxidation of an appropriate test molecule. Here, we have demonstrated the feasibility of adopting photoanodes consisting of zinc oxide nanorods arrays decorated with plasmonic gold nanoparticles （Au NPs@ZnO NRs） for the self-powered PEC bioanalysis of glutathione （GSH） in phosphate-buffered saline （PBS） at an applied bias potential of 0 V vs. Ag/AgCl. This heterostructure exhibited enhanced PEC properties because of the introduction of the Au/ZnO interface. Under visible light illumination, hot electrons from surface-plasmon resonance （SPR） at the Au NP surface were injected into the adjacent ZnO and subsequently driven to the photocathode. Under ultraviolet （UV） light illumination, the photogenerated electrons in ZnO tended to transfer to the fluorine-doped tin oxide due to the step-wise energy band structure and the upward energy band bending at the ZnO/ electrolyte interface. These results indicate that plasmonic metal/semiconductor heterostructure photoanodes have great potential for self-powered PEC bioanalysis applications and extended field of other photovoltaic beacons.
基金financial support from the National Natural Science Foundation of China (Nos. 51702025, 51574047)Natural Science Foundation of Jiangsu Province (Nos. BK20160277, BK20150259)
文摘Well-ordered TiO_2 nanotube arrays(TNTAs)decorated with graphitic carbon nitride(g-C_3N_4) were fabricated by anodic oxidization and calcination process.First, TNTAs were prepared via the anodic oxidation of Ti foil in glycerol solution containing fluorinion and 20%deionized water. Subsequently, g-C_3N_4 film was hydrothermally grown on TNTAs via the hydrogen-bonded cyanuric acid melamine supramolecular complex. The results showed that g-C_3N_4 was successfully decorated on the TNTAs and the g-C_3N_4/TNTAs served as an efficient and stable photoanode for photoelectrochemical water splitting. The facile deposition method enables the fabrication of efficient and low-cost photoanodes for renewable energy applications.
文摘Nanostructures have drawn great attentions for functional device applications. Among the various techniques developed for fabricating arrayed nanostructures of functional materials, nanostructuring technique with porous anodic aluminum oxide （AAO） membrane as templates becomes more attractive owing to the superior geometrical characteristics and low-cost preparation process. In this mini review, progress about functional we summarize our recent nanostructuring based on perfectly-ordered AAO membrane to prepare perfectly- ordered nanostructure arrays of functional materials toward constructing high-performance energy conversion and storage devices. By employing the perfectly-ordered AAO membrane as templates, arrayed nanostructures in the form ofnanodot, nanorod, nanotube and nanopore have been synthesized over a large area. These as-obtained nanostructure arrays have large specific surface area, high regularity, large-scale implementation, and tunable nanos- cale features. All these advanced features enable them to be of great advantage for the performance improvement of energy conversion and storage devices, including photo- electrochemical water splitting cells, supercapacitors, and batteries, etc.
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This work received financial support from the Dean Fund of Chinese Academy of Inspection and Quaran- tine （No. 2016JK025）, the Science Foundation of Administration of Quality Supervision, Inspection and Quarantine （AQSIQ） （No. 2015IK308）, and the National Natural Science Foundation of China （No. 51472226）.
文摘Yolk-shell architectures have attracted extensive attention owing to their unique structure and infusive applications. MoS2 is regarded as one of the most promising catalytic materials for hydrogen evolution by the splitting of water. In this work, a simple self-template solvothermal approach is developed for the synthesis of novel MoS2 yolk-shell microspheres with a hierarchical porous structure by reacting MoO2 microspheres with L-cysteine. A dissolution- recrystallization formation mechanism is proposed for the MoS2 yolk-shell microspheres. Owing to structural superiority, the new material architecture exhibits improved photoelectrochemical properties, including efficient hydrogen evolution reaction catalytic activities, a high photocurrent density, a small overpotential, and a low charge-transfer resistance.
基金the National Natural Science Foundation of China(22127803,22222408,22174110 and 22001193)the Industrial Support Plan of Gansu Provincial Department of Education(2021cyzc-01)+1 种基金the Special Fund Project for Guiding Local Scientific and Technological Development by the Central Government(2020-2060503-17)the Qin Chuangyuan Innovation and Entrepreneurship Talent Project(QCYRCXM-2022-338)。
基金supported by the National Natural Science Foundation of China (51772197, 51422206, 51372159)1000 Youth Talents Plan+3 种基金Key University Science Research Project of Jiangsu Province (17KJA430013)333 High-level Talents Cultivation Project of Jiangsu ProvinceSix Talents Peak Project of Jiangsu ProvinceFunded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)
文摘Bismuth vanadate(BiVO4)is a promising photoanode material owing to the narrow bandgap,appropriate band position,and excellent resistance against photocorrosion,however,the performance of photoelectrochemical(PEC)water splitting is largely limited by the poor carrier separation and transport ability.To address these issues,for the first time,we fabricate BiVO4 film/CuO nanocone p-n junctions as photoanodes by combing a facile spin-coating process and water bath reaction.This structure strengthens the light harvesting and promotes the charge separation and transport ability.The surface defects states are passivated by coating conformally ultrathin TiO2 onto CuO surface through atomic layer deposition(ALD)technique.Benefiting from the favorable morphology,energy band,and surface treatment,the BiVO4/CuO/TiO2 heterojunction generates an improved photocurrent that is much higher than pure BiVO4.The detailed mechanism investigations indicate that the synergetic optimization of charge separation and injection efficiency in the bulk and surface of photoelectrodes can significantly improve the performance of PEC cells.
基金financially supported by the National Natural Science Foundation of China (21875183, 51672210 and 51888103)the National Program for Support of Top-notch Young Professionalsthe ‘‘Fundamental Research Funds for the Central Universities”
文摘Surface treatment is an effective method to improve the photoelectrochemical(PEC) performance of photoelectrodes. Herein, we introduced a novel strategy of surface sulfurization to modify hematite(a-Fe2 O3)nanorods grown in an aqueous solution, which triggered encouraging improvement in PEC performances.In comparison to the solution-grown pristine a-Fe2 O3 nanorod photoanode that is PEC inefficient and always needs high temperature(>600 °C) activation, the surface sulfurized a-Fe2 O3 nanorods show photocurrent density increased by orders of magnitude, reaching 0.46 mA cmà2 at 1.23 V vs. RHE(reversible hydrogen electrode) under simulated solar illumination. This improvement in PEC performances should be attributed to the synergy of the increased carrier density, the reduced surface charge carrier recombination and the accelerated water oxidation kinetics at the a-Fe2 O3/electrolyte interface, as induced by the incorporation of S ions and the formation of multi-state S species(Fe-Sx-Oy) at the surface of a-Fe2 O3 nanorods. This study paves a new and facile approach to activate a-Fe2 O3 and even other metal oxides as photoelectrodes for improved PEC water splitting performances, by engineering the surface structure to relieve the bottlenecks of charge transfer dynamics and redox reaction kinetics at the electrode/electrolyte interface.
文摘Photoelectrochemical （PEC） water splitting is a promising approach to harvest and store solar energy [1]. Silicon has been widely investigated for PEC photoelectrodes due to its suitable band gap （1.12 eV） matching the solar spectrum [2]. Here we investigate employing nickel both as a catalyst and protecting layer of a p-type silicon photocathode for photoelectrochemical hydrogen evolution in basic electrolytes for the first time. The silicon photocathode was made by depositing 15 nm Ti on a p-type silicon wafer followed by 5 nm Ni. The photocathode afforded an onset potential of -0.3 V vs. the reversible hydrogen electrode （RHE） in alkaline solution （1 M KOH）. The stability of the Ni/Ti/p-Si photocathode showed a 100 mV decay over 12 h in KOH, but the stability was significantly improved when the photocathode was operated in potassium borate buffer solution （pH ≈ 9.5）. The electrode surface was found to remain intact after 12 h of continuous operation at a constant current density of 10 mA/cm^2 in potassium borate buffer, suggesting that Ni affords good protection of Si based photocathodes in borate buffers.
