Multi-component chalcogenidometalates have garnered significant attention due to their promising applications in solar energy conversion devices,including photodetectors,solar cells,and photocatalysts.Photocurrent res...Multi-component chalcogenidometalates have garnered significant attention due to their promising applications in solar energy conversion devices,including photodetectors,solar cells,and photocatalysts.Photocurrent response is not only a fundamental property of photodetectors but also serves as a key indicator of the solar energy conversion efficiency in potential semiconductor devices.Despite the growing interest,a clear and universal guideline for designing chalcogenide materials with excellent photocurrent response remains elusive,primarily due to the substantial variations in their chemical compositions and crystal structures.In this review,we present a comprehensive compilation of reported multi-component chalcogenidometalates,including main group chalcogenides with binary and ternary anionic frameworks,and discuss their photocurrent response performance.Additionally,we also highlight other special chalcogenide systems,focusing on their photocurrent response characteristics.For the first time,we systematically summarize the intricate relationships between chemical composition,crystal structure,electronic band structure,and photocurrent response in these materials.Finally,we believe that this review provides a valuable structural perspective on the photocurrent response of multi-component chalcogenidometalates,offering useful insights for the design and application of advanced solar energy conversion materials.展开更多
Solid-state oxide ion and proton conductors are garnering significant attention due to their high ionic conductivity and potential applications in a range of electrochemical devices,including solid oxide fuel cells an...Solid-state oxide ion and proton conductors are garnering significant attention due to their high ionic conductivity and potential applications in a range of electrochemical devices,including solid oxide fuel cells and gas sensors.In this study,we report the influence of partial substitution of La^(3+)in isolated tetrahedral LaVO_(4)ceramics with 0.01 mol of alkaline-earth metals Ca^(2+),Sr^(2+)and Ba^(2+)on the phase stability and electrical properties.It was found that acceptor doping effectively enhances mixed oxide ion and proton conductivities,with Sr^(2+)substitution yielding the highest conductivity,achieving∼10^(−3)S cm^(−1)at 900℃under a wet O_(2)atmosphere.DFT calculations and ab initio molecular dynamics simulations revealed that protons preferentially form hydrogen bonds with the lattice oxygen near the dopants and migrate through a continuous process of hopping and rotation between inter-and intra-tetrahedral VO_(4)groups.Additionally,the existence of oxygen vacancies facilitates the formation of V_(2)O_(7)dimers through sharing corners with adjacent isolated VO4 tetrahedra,enabling ion exchange through a synergistic mechanism involving V2O7 dimer breaking and reforming.This research highlights the critical role of the deformation and rotational flexibility of isolated tetrahedral units in facilitating oxide ion and proton transport,underscoring the potential for developing mixed oxide ion and proton conductors in oxygen vacancy-deficient oxides with tetrahedral-based structures.展开更多
The rapid advancement of organic semiconductors has fueled the remarkable growth of organic electronic devices,including organic light-emitting diodes(OLEDs),organic field-effect transistors(OFETs),and organic photovo...The rapid advancement of organic semiconductors has fueled the remarkable growth of organic electronic devices,including organic light-emitting diodes(OLEDs),organic field-effect transistors(OFETs),and organic photovoltaics(OPV).Looking ahead,the evolution of organic optoelectronic devices is moving toward cost-effective,highly integrated,and flexible solutions with multifunctional capabilities,further expanding the range of potential applications.展开更多
The oxygen reduction reaction(ORR)is a fundamental electrochemical process that occurs in various energy conversion and storage devices,including fuel cells and metal-air batteries[1].ORR can be classified as 2-electr...The oxygen reduction reaction(ORR)is a fundamental electrochemical process that occurs in various energy conversion and storage devices,including fuel cells and metal-air batteries[1].ORR can be classified as 2-electron(yielding H_(2)O_(2) or HO_(2)−)or 4-electron(yielding H_(2)O or OH−depending on the pH),with 4-electron ORR being more important for energy-storage and conversion.The ORR proceeds through a series of complex multistep reactions involving several oxygen intermediate species and multiple electron transfer processes.The complexity of the 4-electon ORR arises from the necessity to consider spin selection rules:the ground state of molecular oxygen is a triplet state(3 Rg−,with two unpaired electrons in p*orbitals with parallel spins),while the reaction products(e.g.,H_(2)O or OH−)all exist in a singlet state without unpaired electrons.This process,which involves a change in the spin state through spin-electron evolution,is spin-forbidden by traditional quantum mechanics,making it inherently slow and requiring the input of extra energy to drive a spin flip.展开更多
基金supported by the National Natural Science Foundation of China(Grants No.52202142,52171277,and 22175175)the Science and Technology Serving Enterprise Project in University and Colleges of Xi’an Science and Technology Bureau(Grant No.24GXFW0002)+1 种基金the Doctoral Scientific Research Startup Foundation of Shaanxi University of Science and Technology(2018BJ-07)Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZR118).
文摘Multi-component chalcogenidometalates have garnered significant attention due to their promising applications in solar energy conversion devices,including photodetectors,solar cells,and photocatalysts.Photocurrent response is not only a fundamental property of photodetectors but also serves as a key indicator of the solar energy conversion efficiency in potential semiconductor devices.Despite the growing interest,a clear and universal guideline for designing chalcogenide materials with excellent photocurrent response remains elusive,primarily due to the substantial variations in their chemical compositions and crystal structures.In this review,we present a comprehensive compilation of reported multi-component chalcogenidometalates,including main group chalcogenides with binary and ternary anionic frameworks,and discuss their photocurrent response performance.Additionally,we also highlight other special chalcogenide systems,focusing on their photocurrent response characteristics.For the first time,we systematically summarize the intricate relationships between chemical composition,crystal structure,electronic band structure,and photocurrent response in these materials.Finally,we believe that this review provides a valuable structural perspective on the photocurrent response of multi-component chalcogenidometalates,offering useful insights for the design and application of advanced solar energy conversion materials.
基金The National Natural Science Foundation of China(no.22365011,22005073,and 22090043)the Guangxi Natural Science Foundation(no.2020GXNSFAA297050 and 2019GXNSFBA245010)+2 种基金the EMERGIA program from Junta de Andalucía of Spain(2022/00001043)the Open Foundation of Key Laboratory of New Processing Technology for Nonferrous Metal&Materials,Ministry of Education/Guangxi Key Laboratory of Optical and Electronic Materials and Devices(22KF-1,20AA-1)the Scientific Research Start-up Fund of GLUT(GUTQDJJ 2017011)are acknowledged for the financial support.
文摘Solid-state oxide ion and proton conductors are garnering significant attention due to their high ionic conductivity and potential applications in a range of electrochemical devices,including solid oxide fuel cells and gas sensors.In this study,we report the influence of partial substitution of La^(3+)in isolated tetrahedral LaVO_(4)ceramics with 0.01 mol of alkaline-earth metals Ca^(2+),Sr^(2+)and Ba^(2+)on the phase stability and electrical properties.It was found that acceptor doping effectively enhances mixed oxide ion and proton conductivities,with Sr^(2+)substitution yielding the highest conductivity,achieving∼10^(−3)S cm^(−1)at 900℃under a wet O_(2)atmosphere.DFT calculations and ab initio molecular dynamics simulations revealed that protons preferentially form hydrogen bonds with the lattice oxygen near the dopants and migrate through a continuous process of hopping and rotation between inter-and intra-tetrahedral VO_(4)groups.Additionally,the existence of oxygen vacancies facilitates the formation of V_(2)O_(7)dimers through sharing corners with adjacent isolated VO4 tetrahedra,enabling ion exchange through a synergistic mechanism involving V2O7 dimer breaking and reforming.This research highlights the critical role of the deformation and rotational flexibility of isolated tetrahedral units in facilitating oxide ion and proton transport,underscoring the potential for developing mixed oxide ion and proton conductors in oxygen vacancy-deficient oxides with tetrahedral-based structures.
文摘The rapid advancement of organic semiconductors has fueled the remarkable growth of organic electronic devices,including organic light-emitting diodes(OLEDs),organic field-effect transistors(OFETs),and organic photovoltaics(OPV).Looking ahead,the evolution of organic optoelectronic devices is moving toward cost-effective,highly integrated,and flexible solutions with multifunctional capabilities,further expanding the range of potential applications.
基金supported by the National Natural Science Foundation of China(22209186 and 22479149)the Selfdeployed Projects of Ganjiang Innovation Academy,Chinese Academy of Sciences(E355F006)+3 种基金the Natural Science Foundation of Jiangxi Province(310306484080)the Key Research and Development Program of Jiangxi Province(20223BBG74004 and 20232BBG70003)the Youth Innovation Promotion Association,Chinese Academy of Sciences(2023343)funding support from the Mac Diarmid Institute for Advanced Materials and Nanotechnology。
文摘The oxygen reduction reaction(ORR)is a fundamental electrochemical process that occurs in various energy conversion and storage devices,including fuel cells and metal-air batteries[1].ORR can be classified as 2-electron(yielding H_(2)O_(2) or HO_(2)−)or 4-electron(yielding H_(2)O or OH−depending on the pH),with 4-electron ORR being more important for energy-storage and conversion.The ORR proceeds through a series of complex multistep reactions involving several oxygen intermediate species and multiple electron transfer processes.The complexity of the 4-electon ORR arises from the necessity to consider spin selection rules:the ground state of molecular oxygen is a triplet state(3 Rg−,with two unpaired electrons in p*orbitals with parallel spins),while the reaction products(e.g.,H_(2)O or OH−)all exist in a singlet state without unpaired electrons.This process,which involves a change in the spin state through spin-electron evolution,is spin-forbidden by traditional quantum mechanics,making it inherently slow and requiring the input of extra energy to drive a spin flip.
