Storing solar energy in battery systems is crucial to achieving a green and sustainable society.However,the efficient development of photo-enhanced zinc-air batteries(ZABs)is limited by the rapid recombination of phot...Storing solar energy in battery systems is crucial to achieving a green and sustainable society.However,the efficient development of photo-enhanced zinc-air batteries(ZABs)is limited by the rapid recombination of photogenerated carriers on the photocathode.In this work,the visible-light-driven CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst with unique petal-like layer structure was designed and developed,which can be used as air electrode for visible-light-driven ZABs.The superior performance of ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)was mainly attributed to the successful construction of Schottky heterojunction between g-C_(3)N_(4)and carbon nanotubes(CNTs),which accelerates the transfer of electrons from g-C_(3)N_(4)to CoS_(2)/CuS cocatalysts,improves the carrier separation ability,and extends the carrier lifetime.Thereinto,the visible-driven ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst has a power density of 588.90 mW cm-2 and a charge-discharge cycle of 643 h under visible light irradiation,which is the highest performance ever reported for photo-enhanced ZABs.More importantly,the charge-discharge voltage drop of ZABs was only 0.54 V under visible light irradiation,which is significantly lower than the voltage drop(0.94 V)in the dark.This study provides a new idea for designing efficient and stable visible-light-driven ZABs cathode catalysts.展开更多
The stereochemically active lone pairs around post-transition metal atoms play an important role in determining distorted lattice structure and optical response.The lone pair electrons are characterized by crystal orb...The stereochemically active lone pairs around post-transition metal atoms play an important role in determining distorted lattice structure and optical response.The lone pair electrons are characterized by crystal orbitals,electron localization function(ELF)and partial density of states(PDOS).Birefringence is evaluated by means of a Born effective charge approach based on modern polarization theory.The origin of the different responses of birefringence and second-harmonic generation(SHG)is explored,as well as the effect of spin-orbit coupling(SOC)on the band structure and optical properties is explored.The study of this paper can help to deeply understand the lone pairs and their contribution to optical property.展开更多
文摘Storing solar energy in battery systems is crucial to achieving a green and sustainable society.However,the efficient development of photo-enhanced zinc-air batteries(ZABs)is limited by the rapid recombination of photogenerated carriers on the photocathode.In this work,the visible-light-driven CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst with unique petal-like layer structure was designed and developed,which can be used as air electrode for visible-light-driven ZABs.The superior performance of ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)was mainly attributed to the successful construction of Schottky heterojunction between g-C_(3)N_(4)and carbon nanotubes(CNTs),which accelerates the transfer of electrons from g-C_(3)N_(4)to CoS_(2)/CuS cocatalysts,improves the carrier separation ability,and extends the carrier lifetime.Thereinto,the visible-driven ZABs assembled by CoS_(2)/CuS@CNT-C_(3)N_(4)photocatalyst has a power density of 588.90 mW cm-2 and a charge-discharge cycle of 643 h under visible light irradiation,which is the highest performance ever reported for photo-enhanced ZABs.More importantly,the charge-discharge voltage drop of ZABs was only 0.54 V under visible light irradiation,which is significantly lower than the voltage drop(0.94 V)in the dark.This study provides a new idea for designing efficient and stable visible-light-driven ZABs cathode catalysts.
基金supported by the National Natural Science Foundation of the People's Republic of China“Mechanistic study of the influence of ns^(2) cation intrinsic properties and coordination environment on birefringence and frequency doubling effects”(12264047),“The study of the mechanism of the influence of lead-oxygen polyhedra and their coordination environments on the gain of the frequency doubling effect”(11864040)Tianshan Talent Project of Xinjiang Uygur Autonomous Region of China“Design,synthesis and photofunctional study of novel rare earth phosphate materials”(2022TSYCJU0004)。
文摘The stereochemically active lone pairs around post-transition metal atoms play an important role in determining distorted lattice structure and optical response.The lone pair electrons are characterized by crystal orbitals,electron localization function(ELF)and partial density of states(PDOS).Birefringence is evaluated by means of a Born effective charge approach based on modern polarization theory.The origin of the different responses of birefringence and second-harmonic generation(SHG)is explored,as well as the effect of spin-orbit coupling(SOC)on the band structure and optical properties is explored.The study of this paper can help to deeply understand the lone pairs and their contribution to optical property.