It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced ...It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.展开更多
Nano-black carbon(BC)is one of the most active fractions in the pyrogenic carbonaceous matter continuum.The majority of recent studies mainly focus on the role of nano-BC in the global carbon cycle.However,based on li...Nano-black carbon(BC)is one of the most active fractions in the pyrogenic carbonaceous matter continuum.The majority of recent studies mainly focus on the role of nano-BC in the global carbon cycle.However,based on literature and our recent studies,we suggest that nano-BC may also serve as a super suspending agent,carrier,and redox mediator for sorbates during its migration from terrestrial to water bodies due to its unique properties such as high colloidal stability,strong sorption capacity,and high surface reactivity.The full implications of nano-BC in water/soil environments are far more than we expected.Thus,we call for more detailed investigations on the activity and reactivity of nano-BC in water/soil environments.展开更多
基金the National Natural Science Foundation of China (22209091)the Natural Science Foundation of Shandong Province (ZR2020QB057)+1 种基金the Key Program of National Natural Science Foundation of China (22133006)the Yankuang Group 2019 Science and Technology Program (YKKJ2019AJ05JG-R60)。
文摘It is a challenge to coordinate carrier-kinetics performance and the redox capacity of photogenerated charges synchronously at the atomic level for boosting photocatalytic activity.Herein,the atomic Ni was introduced into the lattice of hexagonal ZnIn_(2)S_(4) nanosheets(Ni/ZnIn_(2)S_(4))via directionalsubstituting Zn atom with the facile hydrothermal method.The electronic structure calculations indicate that the introduction of Ni atom effectively extracts more electrons and acts as active site for subsequent reduction reaction.Besides the optimized light absorption range,the elevation of Efand ECBendows Ni/ZnIn_(2)S_(4) photocatalyst with the increased electron concentration and the enhanced reduction ability for surface reaction.Moreover,ultrafast transient absorption spectroscopy,as well as a series of electrochemical tests,demonstrates that Ni/ZnIn_(2)S_(4) possesses 2.15 times longer lifetime of the excited charge carriers and an order of magnitude increase for carrier mobility and separation efficiency compared with pristine ZnIn_(2)S_(4).These efficient kinetics performances of charge carriers and enhanced redox capacity synergistically boost photocatalytic activity,in which a 3-times higher conversion efficiency of nitrobenzene reduction was achieved upon Ni/ZnIn_(2)S_(4).Our study not only provides in-depth insights into the effect of atomic directional-substitution on the kinetic behavior of photogenerated charges,but also opens an avenue to the synchronous optimization of redox capacity and carrier-kinetics performance for efficient solar energy conversion.
基金The work was supported by the National Natural Science Foundation of China(41977278 and 41573127)the Fundamental Research Funds for the Central Universities(JUSRP22015).BX acknowledges the UMass Amherst Conti Faculty Fellowship.
文摘Nano-black carbon(BC)is one of the most active fractions in the pyrogenic carbonaceous matter continuum.The majority of recent studies mainly focus on the role of nano-BC in the global carbon cycle.However,based on literature and our recent studies,we suggest that nano-BC may also serve as a super suspending agent,carrier,and redox mediator for sorbates during its migration from terrestrial to water bodies due to its unique properties such as high colloidal stability,strong sorption capacity,and high surface reactivity.The full implications of nano-BC in water/soil environments are far more than we expected.Thus,we call for more detailed investigations on the activity and reactivity of nano-BC in water/soil environments.