NiS2 is a promising cocatalyst to improve the photocatalytic performance of g-C3N4 for the production of H2.However,the synthesis of the NiS2 cocatalyst usually requires harsh conditions,which risks destroying the mic...NiS2 is a promising cocatalyst to improve the photocatalytic performance of g-C3N4 for the production of H2.However,the synthesis of the NiS2 cocatalyst usually requires harsh conditions,which risks destroying the microstructures of the g-C3N4 photocatalysts.In this study,a facile and low-temperature(80 ℃) impregnation method was developed to prepare NiS2/g-C3N4 photocatalysts.First,the g-C3N4 powders were processed by the hydrothermal method in order to introduce oxygen-containing functional groups(such as-OH and-C0NH-) to the surface of g-C3N4.Then,the Ni^2+ ions could be adsorbed near the g-C3N4 via strong electrostatic interaction between g-C3N4 and Ni^2+ ions upon the addition of Ni(NO3)2 solution.Finally,NiS2 nanoparticles were formed on the surface of g-C3N4 upon the addition of TAA.It was found that the NiS2 nanoparticles were solidly and homogeneously grafted on the surface of g-C3N4,resulting in greatly improved photocatalytic H2production.When the amount of NiS2 was 3 wt%,the resultant NiS2/g-C3N4 photocatalyst showed the highest H2 evolution rate(116.343 μmol h^-1 g^-1),which is significantly higher than that of the pure g-C3N4(3 μmol h^-1 g^-1).Moreover,the results of a recycling test for the NiS2/g-C3N4(3 wt%)sample showed that this sample could maintain a stable and effective photocatalytic H2-evolution performance under visible-light irradiation.Based on the above results,a possible mechanism of the improved photocatalytic performance was proposed for the presented NiS2/g-C3N4 photocatalysts,in which the photogenerated electrons of g-C3N4 can be rapidly transferred to the NiS2 nanoparticles via the close and continuous contact between them;then,the photogenerated electrons rapidly react with H2O adsorbed on the surface of NiS2,which has a surficial metallic character and high catalytic activity,to produce H2.Considering the mild and facile synthesis method,the presented low-cost and highly efficient NiS2-modified g-C3N4 photocatalysts would have great potential for practical use in photocatalytic H2 production.展开更多
Photocatalytic H2 evolution reactions on pristine graphitic carbon nitrides(g-C3N4),as a promising approach for converting solar energy to fuel,are attractive for tackling global energy concerns but still suffer from ...Photocatalytic H2 evolution reactions on pristine graphitic carbon nitrides(g-C3N4),as a promising approach for converting solar energy to fuel,are attractive for tackling global energy concerns but still suffer from low efficiencies.In this article,we report a tractable approach to modifying g-C3N4 with vanadyl phthalocyanine(VOPc/CN)for efficient visible-light-driven hydrogen production.A non-covalent VOPc/CN hybrid photocatalyst formed viaπ-πstacking interactions between the two components,as confirmed by analysis of UV-vis absorption spectra.The VOPc/CN hybrid photocatalyst shows excellent visible-light-driven photocatalytic performance and good stability.Under optimal conditions,the corresponding H2 evolution rate is nearly 6 times higher than that of pure g-C3N4.The role of VOPc in promoting hydrogen evolution activity was to extend the visible light absorption range and prevent the recombination of photoexcited electron-hole pairs effectively.It is expected that this facile modification method could be a new inspiration for the rational design and exploration of g-C3N4-based hybrid systems with strong light absorption and high-efficiency carrier separation.展开更多
Photocatalytic hydrogen production based on semiconductor photocatalysts has been considered as one of the most promising strategies to resolve the global energy shortage.Graphitic carbon nitride(g‐C3N4)has been a st...Photocatalytic hydrogen production based on semiconductor photocatalysts has been considered as one of the most promising strategies to resolve the global energy shortage.Graphitic carbon nitride(g‐C3N4)has been a star visible‐light photocatalyst in this field due to its various advantages.However,pristine g‐C3N4usually exhibits limited activity.Herein,to enhance the performance of g‐C3N4,alkali metal ion(Li+,Na+,or K+)‐doped g‐C3N4are prepared via facile high‐temperature treatment.The prepared samples are characterized and analyzed using the technique of XRD,ICP‐AES,SEM,UV‐vis DRS,BET,XPS,PL,TRPL,photoelectrochemical measurements,photocatalytic tests,etc.The resultant doped photocatalysts show enhanced visible‐light photocatalytic activities for hydrogen production,benefiting from the increased specific surface areas(which provide more active sites),decreased band gaps for extended visible‐light absorption,and improved electronic structures for efficient charge transfer.In particular,because of the optimal tuning of both microstructure and electronic structure,the Na‐doped g‐C3N4shows the most effective utilization of photogenerated electrons during the water reduction process.As a result,the highest photocatalytic performance is achieved over the Na‐doped g‐C3N4photocatalyst(18.7?mol/h),3.7times that of pristine g‐C3N4(5.0?mol/h).This work gives a systematic study for the understanding of doping effect of alkali metals in semiconductor photocatalysis.展开更多
Cadmium sulfide(Cd S)-based photocatalysts have attracted extensive attention owing to their strong visible light absorption,suitable band energy levels,and excellent electronic charge transportation properties.This r...Cadmium sulfide(Cd S)-based photocatalysts have attracted extensive attention owing to their strong visible light absorption,suitable band energy levels,and excellent electronic charge transportation properties.This review focuses on the recent progress related to the design,modification,and construction of Cd S-based photocatalysts with excellent photocatalytic H2 evolution performances.First,the basic concepts and mechanisms of photocatalytic H2 evolution are briefly introduced.Thereafter,the fundamental properties,important advancements,and bottlenecks of Cd S in photocatalytic H2 generation are presented in detail to provide an overview of the potential of this material.Subsequently,various modification strategies adopted for Cd S-based photocatalysts to yield solar H2 are discussed,among which the effective approaches aim at generating more charge carriers,promoting efficient charge separation,boosting interfacial charge transfer,accelerating charge utilization,and suppressing charge-induced self-photocorrosion.The critical factors governing the performance of the photocatalyst and the feasibility of each modification strategy toward shaping future research directions are comprehensively discussed with examples.Finally,the prospects and challenges encountered in developing nanostructured Cd S and Cd S-based nanocomposites in photocatalytic H2 evolution are presented.展开更多
基金supported by the National Natural Science Foundation of China (21277107, 21477094, 51672203, 51472192)the Program for New Century Excellent Talents in University (NCET-13-0944)the Fundamental Research Funds for the Central Universities (WUT 2015IB002)~~
文摘NiS2 is a promising cocatalyst to improve the photocatalytic performance of g-C3N4 for the production of H2.However,the synthesis of the NiS2 cocatalyst usually requires harsh conditions,which risks destroying the microstructures of the g-C3N4 photocatalysts.In this study,a facile and low-temperature(80 ℃) impregnation method was developed to prepare NiS2/g-C3N4 photocatalysts.First,the g-C3N4 powders were processed by the hydrothermal method in order to introduce oxygen-containing functional groups(such as-OH and-C0NH-) to the surface of g-C3N4.Then,the Ni^2+ ions could be adsorbed near the g-C3N4 via strong electrostatic interaction between g-C3N4 and Ni^2+ ions upon the addition of Ni(NO3)2 solution.Finally,NiS2 nanoparticles were formed on the surface of g-C3N4 upon the addition of TAA.It was found that the NiS2 nanoparticles were solidly and homogeneously grafted on the surface of g-C3N4,resulting in greatly improved photocatalytic H2production.When the amount of NiS2 was 3 wt%,the resultant NiS2/g-C3N4 photocatalyst showed the highest H2 evolution rate(116.343 μmol h^-1 g^-1),which is significantly higher than that of the pure g-C3N4(3 μmol h^-1 g^-1).Moreover,the results of a recycling test for the NiS2/g-C3N4(3 wt%)sample showed that this sample could maintain a stable and effective photocatalytic H2-evolution performance under visible-light irradiation.Based on the above results,a possible mechanism of the improved photocatalytic performance was proposed for the presented NiS2/g-C3N4 photocatalysts,in which the photogenerated electrons of g-C3N4 can be rapidly transferred to the NiS2 nanoparticles via the close and continuous contact between them;then,the photogenerated electrons rapidly react with H2O adsorbed on the surface of NiS2,which has a surficial metallic character and high catalytic activity,to produce H2.Considering the mild and facile synthesis method,the presented low-cost and highly efficient NiS2-modified g-C3N4 photocatalysts would have great potential for practical use in photocatalytic H2 production.
基金supported by the National Natural Science Foundation of China(51572253,21771171)Scientific Research Grant of Hefei National Synchrotron Radiation Laboratory(UN2017LHJJ)+1 种基金the Fundamental Research Funds for the Central Universitiescooperation between NSFC and Netherlands Organization for Scientific Research(51561135011)~~
文摘Photocatalytic H2 evolution reactions on pristine graphitic carbon nitrides(g-C3N4),as a promising approach for converting solar energy to fuel,are attractive for tackling global energy concerns but still suffer from low efficiencies.In this article,we report a tractable approach to modifying g-C3N4 with vanadyl phthalocyanine(VOPc/CN)for efficient visible-light-driven hydrogen production.A non-covalent VOPc/CN hybrid photocatalyst formed viaπ-πstacking interactions between the two components,as confirmed by analysis of UV-vis absorption spectra.The VOPc/CN hybrid photocatalyst shows excellent visible-light-driven photocatalytic performance and good stability.Under optimal conditions,the corresponding H2 evolution rate is nearly 6 times higher than that of pure g-C3N4.The role of VOPc in promoting hydrogen evolution activity was to extend the visible light absorption range and prevent the recombination of photoexcited electron-hole pairs effectively.It is expected that this facile modification method could be a new inspiration for the rational design and exploration of g-C3N4-based hybrid systems with strong light absorption and high-efficiency carrier separation.
基金supported by the National Natural Science Foundation of of China(51472191,21407115,21773179)the Natural Science Foundation of Hubei Province of China(2017CFA031)the Opening Project of Key Laboratory of Optoelectronic Chemical Materials and Devices,Ministry of Education(JDGD-201509)~~
文摘Photocatalytic hydrogen production based on semiconductor photocatalysts has been considered as one of the most promising strategies to resolve the global energy shortage.Graphitic carbon nitride(g‐C3N4)has been a star visible‐light photocatalyst in this field due to its various advantages.However,pristine g‐C3N4usually exhibits limited activity.Herein,to enhance the performance of g‐C3N4,alkali metal ion(Li+,Na+,or K+)‐doped g‐C3N4are prepared via facile high‐temperature treatment.The prepared samples are characterized and analyzed using the technique of XRD,ICP‐AES,SEM,UV‐vis DRS,BET,XPS,PL,TRPL,photoelectrochemical measurements,photocatalytic tests,etc.The resultant doped photocatalysts show enhanced visible‐light photocatalytic activities for hydrogen production,benefiting from the increased specific surface areas(which provide more active sites),decreased band gaps for extended visible‐light absorption,and improved electronic structures for efficient charge transfer.In particular,because of the optimal tuning of both microstructure and electronic structure,the Na‐doped g‐C3N4shows the most effective utilization of photogenerated electrons during the water reduction process.As a result,the highest photocatalytic performance is achieved over the Na‐doped g‐C3N4photocatalyst(18.7?mol/h),3.7times that of pristine g‐C3N4(5.0?mol/h).This work gives a systematic study for the understanding of doping effect of alkali metals in semiconductor photocatalysis.
基金the National Natural Science Foundation of China(21975084 and 51672089)the Ding Ying Talent Project of South China Agricultural University for their support+1 种基金the Hong Kong Research Grant Council(RGC)General Research Fund GRF1305419 for financial supportthe National Natural Science Foundation of China(51972287 and 51502269)。
文摘Cadmium sulfide(Cd S)-based photocatalysts have attracted extensive attention owing to their strong visible light absorption,suitable band energy levels,and excellent electronic charge transportation properties.This review focuses on the recent progress related to the design,modification,and construction of Cd S-based photocatalysts with excellent photocatalytic H2 evolution performances.First,the basic concepts and mechanisms of photocatalytic H2 evolution are briefly introduced.Thereafter,the fundamental properties,important advancements,and bottlenecks of Cd S in photocatalytic H2 generation are presented in detail to provide an overview of the potential of this material.Subsequently,various modification strategies adopted for Cd S-based photocatalysts to yield solar H2 are discussed,among which the effective approaches aim at generating more charge carriers,promoting efficient charge separation,boosting interfacial charge transfer,accelerating charge utilization,and suppressing charge-induced self-photocorrosion.The critical factors governing the performance of the photocatalyst and the feasibility of each modification strategy toward shaping future research directions are comprehensively discussed with examples.Finally,the prospects and challenges encountered in developing nanostructured Cd S and Cd S-based nanocomposites in photocatalytic H2 evolution are presented.