Cocatalysts play a vital role in accelerating the reaction kinetics and improving the charge separation of photocatalysts for solar hydrogen production.The promotion of the photocatalytic activity largely relies on th...Cocatalysts play a vital role in accelerating the reaction kinetics and improving the charge separation of photocatalysts for solar hydrogen production.The promotion of the photocatalytic activity largely relies on the loading approach of the cocatalysts.Herein,we introduce a metal-seed assistant photodeposition approach to load the hydrogen evolution cocatalyst of platinum onto the surface of Ta_(3)N_(5) photocatalyst,which exhibits about 3.6 times of higher photocatalytic proton reduction activity with respect to the corresponding impregnation or photodeposition loading.Based on our characterizations,the increscent contact area of the cocatalyst/semiconductor interface with metal-seed assistant photodeposition method is proposed to be responsible for the promoted charge separation as well as enhanced photocatalytic H2 evolution activity.It is interesting to note that this innovative deposition strategy can be easily extended to loading of platinum cocatalyst with other noble or non-noble metal seeds for promoted activities,demonstrating its good generality.Our work may provide an alternative way of depositing cocatalyst for better photocatalytic performances.展开更多
Hydrogen generation via artificial photosynthesis paves a promising way to remit the ever-increasing energy crisis and deteriorative environmental issues.Among all the materials utilized for solar hydrogen production,...Hydrogen generation via artificial photosynthesis paves a promising way to remit the ever-increasing energy crisis and deteriorative environmental issues.Among all the materials utilized for solar hydrogen production,perovskite has emerged as a rising star due to its superior optoelectronic properties.This manuscript aims to provide a comprehensive review summarizing the recent inspiring advancements on perovskite-based solar hydrogen production systems,including the particulate photocatalysis,photoelectrochemical cells,and photovoltaic-electrocatalytic cells.We start with a brief introduction of the advantages of perovskites for solar hydrogen production and the basic principles of the three most prominent solar hydrogen production systems.The representative progresses in this field are then detailed with a special emphasis on the strategies to improve the efficiency and the stability of the systems.Finally,challenges and opportunities for the further development of the PVK-based solar hydrogen production systems are presented with perspective given on outlook,performance,cost and stability.展开更多
Combining a progressive tandem junction design with a unique Si nanowire(SiNW)framework paves the way for the development of high‐onset‐potential photocathodes and enhancement of solar hydrogen production.Herein,a r...Combining a progressive tandem junction design with a unique Si nanowire(SiNW)framework paves the way for the development of high‐onset‐potential photocathodes and enhancement of solar hydrogen production.Herein,a radial tandem junction(RTJ)thin film water‐splitting photo‐cathode has been demonstrated experimentally for the first time.The photocathode is directly fab‐ricated on vapor‐liquid‐solid‐grown SiNWs and consists of two radially stacked p‐i‐n junctions,featuring hydrogenated amorphous silicon(a‐Si:H)as the outer absorber layer,which absorbs short wavelengths,and hydrogenated amorphous silicon germanium(a‐SiGe:H)as the inner layer,which absorbs long wavelengths.The randomly distributed SiNW framework enables highly efficient light‐trapping,which facilitates the use of very thin absorber layers of a‐Si:H(~50 nm)and a‐SiGe:H(~40 nm).In a neutral electrolyte(pH=7),the three‐dimensional(3D)RTJ photocathode delivers a high photocurrent onset of 1.15 V vs.the reversible hydrogen electrode(RHE),accompanied by a photocurrent of 2.98 mA/cm^(2) at 0 V vs.RHE,and an overall applied‐bias photon‐to‐current effi‐ciency of 1.72%.These results emphasize the promising role of 3D radial tandem technology in developing a new generation of durable,low‐cost,high‐onset‐potential photocathodes capable of large‐scale implementation。展开更多
The effective utilization of solar energy for hydrogen production requires an abundant supply of thermodynamically active photo-electrons;however,the photocatalysts are generally impeded by insufficient light absorpti...The effective utilization of solar energy for hydrogen production requires an abundant supply of thermodynamically active photo-electrons;however,the photocatalysts are generally impeded by insufficient light absorption and fast photocarrier recombination.Here,we report a multiple-regulated strategy to capture photons and boost photocarrier dynamics by devel-oping a broadband photocatalyst composed of defect engineered g-C_(3)N_(4)(DCN)and upconversion NaYF4:Yb^(3+),Tm^(3+)(NYF)nanocrystals.Through a precise defect engineering,the S dopants and C vacancies jointly render DCN with defect states to effectively extend the visible light absorption to 590 nm and boost photocarrier separation via a moderate electron-trapping ability,thus facilitating the subsequent re-absorption and utilization of upconverted photons/electrons.Importantly,we found a promoted interfacial charge polarization between DCN and NYF has also been achieved mainly due to Y-N interaction,which further favors the upconverted excited energy transfer from NYF onto DCN as verified both theoretically and experimentally.With a 3D architecture,the NYF@DCN catalyst exhibits a superior solar H2 evolution rate among the reported upconversion-based system,which is 19.3 and 1.5 fold higher than bulk material and DCN,respectively.This work provides an innovative strategy to boost solar utilization by using defect engineering and building up interaction between hetero-materials.展开更多
In this study, we prepared horn-like ZnO structures on carbon films(ZnO/CF) by electrodeposition and decorated the ZnO horns with different metals(Ag, Au, and Pt) via photodeposition(M-ZnO/CF). Using M-ZnO/CF as...In this study, we prepared horn-like ZnO structures on carbon films(ZnO/CF) by electrodeposition and decorated the ZnO horns with different metals(Ag, Au, and Pt) via photodeposition(M-ZnO/CF). Using M-ZnO/CF as photocatalysts, we examined ways to enhance solar hydrogen production from various points of view, such as modifying the intrinsic physical properties and thermodynamics of the materials, and varying the chemical environment during M-ZnO/CF fabrication. In particular, we focused on the effects of the carbon film and metals in M-ZnO/CF hybrid photocatalysts on solar hydrogen production. The type of metal nanoparticles is an important factor in solar hydrogen production because the deposition rate and electrical conductivity of each metal affect the proton-water reduction ability.展开更多
Photoelectrocatalytic seawater splitting is a promising low-cost method to produce green hydrogen in a large scale.The effects of Cl^(-)ions in seawater on the performance of a photoanode have been reported in previou...Photoelectrocatalytic seawater splitting is a promising low-cost method to produce green hydrogen in a large scale.The effects of Cl^(-)ions in seawater on the performance of a photoanode have been reported in previous studies.However,few researches have been done on the roles of Cl^(-)ions in a photocathode.Herein,for the first time,we find that Cl^(-)ions in the electrolyte improve the photocurrent of a Si/In_(2)S_(3) photocathode by 50% at-0.6 V_(RHE).An in-situ X-ray photoelectron spectroscopy(XPS)characterization combined with the time-of-flight secondary-ion mass spectrometry by simulating photoelectrochemical conditions was used to investigate the interface charge transfer mechanism.The results suggest that there is an In_(2)^(+3)S_(3-x)(OH)_(2x)layer on the surface of In_(2)S_(3) in the phosphate buffer solution(PBS)electrolyte,which plays a role as an interface charge transfer mediator in the Si/In_(2)S_(3) photocathode.The In_(2)^(+3)S_(3-x)(OH)_(2x)surface layer becomes In_(2)^(+3)S_(3-x)(Cl)_(2x)in the PBS electrolyte with NaCl and accelerates the charge transfer rate at the In_(2)S_(3)/electrolyte interface.These results offer a new concept of regulating interface charge transfer mediator to enhance the performance of photoelectrocatalytic seawater splitting for hydrogen production.展开更多
基金supported by the National Natural Science Foundation of China(21633009,21925206,21902156)the Dalian National Laboratory for Clean Energy(DNL)Cooperation Fund,CAS(no.DNL 201913)+2 种基金the International Partnership Program of Chinese Academy of Sciences(121421KYSB20190025)the DICP foundation of innovative research(DICP I201927)the support from Liao Ning Revitalization Talents Program(XLYC1807241)。
文摘Cocatalysts play a vital role in accelerating the reaction kinetics and improving the charge separation of photocatalysts for solar hydrogen production.The promotion of the photocatalytic activity largely relies on the loading approach of the cocatalysts.Herein,we introduce a metal-seed assistant photodeposition approach to load the hydrogen evolution cocatalyst of platinum onto the surface of Ta_(3)N_(5) photocatalyst,which exhibits about 3.6 times of higher photocatalytic proton reduction activity with respect to the corresponding impregnation or photodeposition loading.Based on our characterizations,the increscent contact area of the cocatalyst/semiconductor interface with metal-seed assistant photodeposition method is proposed to be responsible for the promoted charge separation as well as enhanced photocatalytic H2 evolution activity.It is interesting to note that this innovative deposition strategy can be easily extended to loading of platinum cocatalyst with other noble or non-noble metal seeds for promoted activities,demonstrating its good generality.Our work may provide an alternative way of depositing cocatalyst for better photocatalytic performances.
基金National Key Research Program of China(2017YFA0204800)National Natural Science Foundation of China(No.21603136)+1 种基金the National Science Basic Research Plan in Shaanxi Province of China(2017JM2007)the Fundamental Research Funds for the Central Universities(2019TS005)。
文摘Hydrogen generation via artificial photosynthesis paves a promising way to remit the ever-increasing energy crisis and deteriorative environmental issues.Among all the materials utilized for solar hydrogen production,perovskite has emerged as a rising star due to its superior optoelectronic properties.This manuscript aims to provide a comprehensive review summarizing the recent inspiring advancements on perovskite-based solar hydrogen production systems,including the particulate photocatalysis,photoelectrochemical cells,and photovoltaic-electrocatalytic cells.We start with a brief introduction of the advantages of perovskites for solar hydrogen production and the basic principles of the three most prominent solar hydrogen production systems.The representative progresses in this field are then detailed with a special emphasis on the strategies to improve the efficiency and the stability of the systems.Finally,challenges and opportunities for the further development of the PVK-based solar hydrogen production systems are presented with perspective given on outlook,performance,cost and stability.
文摘Combining a progressive tandem junction design with a unique Si nanowire(SiNW)framework paves the way for the development of high‐onset‐potential photocathodes and enhancement of solar hydrogen production.Herein,a radial tandem junction(RTJ)thin film water‐splitting photo‐cathode has been demonstrated experimentally for the first time.The photocathode is directly fab‐ricated on vapor‐liquid‐solid‐grown SiNWs and consists of two radially stacked p‐i‐n junctions,featuring hydrogenated amorphous silicon(a‐Si:H)as the outer absorber layer,which absorbs short wavelengths,and hydrogenated amorphous silicon germanium(a‐SiGe:H)as the inner layer,which absorbs long wavelengths.The randomly distributed SiNW framework enables highly efficient light‐trapping,which facilitates the use of very thin absorber layers of a‐Si:H(~50 nm)and a‐SiGe:H(~40 nm).In a neutral electrolyte(pH=7),the three‐dimensional(3D)RTJ photocathode delivers a high photocurrent onset of 1.15 V vs.the reversible hydrogen electrode(RHE),accompanied by a photocurrent of 2.98 mA/cm^(2) at 0 V vs.RHE,and an overall applied‐bias photon‐to‐current effi‐ciency of 1.72%.These results emphasize the promising role of 3D radial tandem technology in developing a new generation of durable,low‐cost,high‐onset‐potential photocathodes capable of large‐scale implementation。
基金support provided by the ARC through the ARC DP200101249 project.J.Feng would like to thank the computational resources provided by the High-Performance Computing Center of Qufu Normal University.D.Wang would like to acknowledge the National Natural Science Foundation of China(21903048,21971244,51932001,21931012,21590795)and National Key R&D Program of China(2018YFA0703504,2021YFB3802600).
文摘The effective utilization of solar energy for hydrogen production requires an abundant supply of thermodynamically active photo-electrons;however,the photocatalysts are generally impeded by insufficient light absorption and fast photocarrier recombination.Here,we report a multiple-regulated strategy to capture photons and boost photocarrier dynamics by devel-oping a broadband photocatalyst composed of defect engineered g-C_(3)N_(4)(DCN)and upconversion NaYF4:Yb^(3+),Tm^(3+)(NYF)nanocrystals.Through a precise defect engineering,the S dopants and C vacancies jointly render DCN with defect states to effectively extend the visible light absorption to 590 nm and boost photocarrier separation via a moderate electron-trapping ability,thus facilitating the subsequent re-absorption and utilization of upconverted photons/electrons.Importantly,we found a promoted interfacial charge polarization between DCN and NYF has also been achieved mainly due to Y-N interaction,which further favors the upconverted excited energy transfer from NYF onto DCN as verified both theoretically and experimentally.With a 3D architecture,the NYF@DCN catalyst exhibits a superior solar H2 evolution rate among the reported upconversion-based system,which is 19.3 and 1.5 fold higher than bulk material and DCN,respectively.This work provides an innovative strategy to boost solar utilization by using defect engineering and building up interaction between hetero-materials.
基金supported by the DGIST R&D Program of Ministry of Science,ICT and Future Planning of Korea (16-NB-03)
文摘In this study, we prepared horn-like ZnO structures on carbon films(ZnO/CF) by electrodeposition and decorated the ZnO horns with different metals(Ag, Au, and Pt) via photodeposition(M-ZnO/CF). Using M-ZnO/CF as photocatalysts, we examined ways to enhance solar hydrogen production from various points of view, such as modifying the intrinsic physical properties and thermodynamics of the materials, and varying the chemical environment during M-ZnO/CF fabrication. In particular, we focused on the effects of the carbon film and metals in M-ZnO/CF hybrid photocatalysts on solar hydrogen production. The type of metal nanoparticles is an important factor in solar hydrogen production because the deposition rate and electrical conductivity of each metal affect the proton-water reduction ability.
基金supported by the National Natural Science Foundation of China(22279052)the China Postdoctoral Science Foundation(2023M741613)。
文摘Photoelectrocatalytic seawater splitting is a promising low-cost method to produce green hydrogen in a large scale.The effects of Cl^(-)ions in seawater on the performance of a photoanode have been reported in previous studies.However,few researches have been done on the roles of Cl^(-)ions in a photocathode.Herein,for the first time,we find that Cl^(-)ions in the electrolyte improve the photocurrent of a Si/In_(2)S_(3) photocathode by 50% at-0.6 V_(RHE).An in-situ X-ray photoelectron spectroscopy(XPS)characterization combined with the time-of-flight secondary-ion mass spectrometry by simulating photoelectrochemical conditions was used to investigate the interface charge transfer mechanism.The results suggest that there is an In_(2)^(+3)S_(3-x)(OH)_(2x)layer on the surface of In_(2)S_(3) in the phosphate buffer solution(PBS)electrolyte,which plays a role as an interface charge transfer mediator in the Si/In_(2)S_(3) photocathode.The In_(2)^(+3)S_(3-x)(OH)_(2x)surface layer becomes In_(2)^(+3)S_(3-x)(Cl)_(2x)in the PBS electrolyte with NaCl and accelerates the charge transfer rate at the In_(2)S_(3)/electrolyte interface.These results offer a new concept of regulating interface charge transfer mediator to enhance the performance of photoelectrocatalytic seawater splitting for hydrogen production.