Exploring efficient,cost-effective,and durable electrocatalysts for electrochemical oxygen evolution reaction(OER)is pivotal for the large-scale application of water electrolysis.Recent advance has demonstrated that t...Exploring efficient,cost-effective,and durable electrocatalysts for electrochemical oxygen evolution reaction(OER)is pivotal for the large-scale application of water electrolysis.Recent advance has demonstrated that the activity of electrocatalysts exhibits a strong dependence on the surface electronic structure.Herein,a series of ultrathin metal silicate hydroxide nanosheets(UMSHNs)M_(3)Si_(2)O_(5)(OH)_(4)(M=Fe,Co,and Ni)synthesized without surfactant are introduced as highly active OER electrocatalysts.Cobalt silicate hydroxide nanosheets show an optimal OER activity with overpotentials of 287 and 358 m V at 1 and 10 m A cm^(-2),respectively.Combining experimental and theoretical studies,it is found that the OER activity of UMSHNs is dominated by the metal-oxygen covalency(MOC).High OER activity can be achieved by having a moderate MOC as reflected by aσ^(*)-orbital(e_(g))filling near unity and moderate[3d]/[2p]ratio.Moreover,the UMSHNs exhibit favorable chemical stability under oxidation potential.This contribution provides a scientific guidance for further development of active metal silicate hydroxide catalysts.展开更多
To address climate change and promote environmental sustainability,electrochemical energy conversion and storage systems emerge as promising alternative to fossil fuels,catering to the escalating demand for energy.Ach...To address climate change and promote environmental sustainability,electrochemical energy conversion and storage systems emerge as promising alternative to fossil fuels,catering to the escalating demand for energy.Achieving optimal energy efficiency and cost competitiveness in these systems requires the strategic design of electrocatalysts,coupled with a thorough comprehension of the underlying mechanisms and degradation behavior occurring during the electrocatalysis processes.Scanning electrochemical microscopy(SECM),an analytical technique for studying surface electrochemically,stands out as a powerful tool offering electrochemical insights.It possesses remarkable spatiotemporal resolution,enabling the visualization of the localized electrochemical activity and surface topography.This review compiles crucial research findings and recent breakthroughs in electrocatalytic processes utilizing the SECM methodology,specifically focusing on applications in electrolysis,fuel cells,and metal–oxygen batteries within the realm of energy conversion and storage systems.Commencing with an overview of each energy system,the review introduces the fundamental principles of SECM,and aiming to provide new perspectives and broadening the scope of applied research by describing the major research categories within SECM.展开更多
Oxygen evolution reaction(OER)is crucial for hydrogen production as well as other energy storage technologies.CoFe-layered double hydroxide(CoFe-OH)has been widely considered as one of the most efficient electrocataly...Oxygen evolution reaction(OER)is crucial for hydrogen production as well as other energy storage technologies.CoFe-layered double hydroxide(CoFe-OH)has been widely considered as one of the most efficient electrocatalysts for OER in basic aqueous solution.However,it still suffers from low activity in neutral electrolyte.This paper describes partially oxidized CoFe-OH(PO-CoFe-OH)with enhanced covalency of M-O bonds and displays enhanced OER performance under mild condition.Mechanism studies reveal the suitably enhanced M-O covalency in PO-CoFe-OH shifts the OER mechanism to lattice oxygen oxidation mechanism and also promotes the rate-limiting deprotonation,providing superior OER performance.It just requires the overpotentials of 186 and 365 mV to drive the current density densities of 1 and 10 mA·cm^(-2) in 0.1 M KHCO_(3) aqueous solution(pH=8.3),respectively.It provides a new process for rational design of efficient catalysts for water oxidation in mild conditions.展开更多
基金supported by the NationallNaturallScience Foundation of China(51832004,51521001,51872218)the NationallKey Research and Development Program of China(2016YFA0202603)+3 种基金the Programme of Introducing Talents of Discipline to Universities(B17034)the Yellow Crane Talent(Science&Technology)Program of Wuhan CityFoshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory(XHT2020-003)the FundamentallResearch Funds for the CentrallUniversities(195101005)。
文摘Exploring efficient,cost-effective,and durable electrocatalysts for electrochemical oxygen evolution reaction(OER)is pivotal for the large-scale application of water electrolysis.Recent advance has demonstrated that the activity of electrocatalysts exhibits a strong dependence on the surface electronic structure.Herein,a series of ultrathin metal silicate hydroxide nanosheets(UMSHNs)M_(3)Si_(2)O_(5)(OH)_(4)(M=Fe,Co,and Ni)synthesized without surfactant are introduced as highly active OER electrocatalysts.Cobalt silicate hydroxide nanosheets show an optimal OER activity with overpotentials of 287 and 358 m V at 1 and 10 m A cm^(-2),respectively.Combining experimental and theoretical studies,it is found that the OER activity of UMSHNs is dominated by the metal-oxygen covalency(MOC).High OER activity can be achieved by having a moderate MOC as reflected by aσ^(*)-orbital(e_(g))filling near unity and moderate[3d]/[2p]ratio.Moreover,the UMSHNs exhibit favorable chemical stability under oxidation potential.This contribution provides a scientific guidance for further development of active metal silicate hydroxide catalysts.
基金supported by a characterization platform for advanced materials funded by the Korea Research Institute of Standards and Science(KRISS-2023-GP2023-0014)the KRISS(Korea Research Institute of Standards and Science)MPI Lab.program。
文摘To address climate change and promote environmental sustainability,electrochemical energy conversion and storage systems emerge as promising alternative to fossil fuels,catering to the escalating demand for energy.Achieving optimal energy efficiency and cost competitiveness in these systems requires the strategic design of electrocatalysts,coupled with a thorough comprehension of the underlying mechanisms and degradation behavior occurring during the electrocatalysis processes.Scanning electrochemical microscopy(SECM),an analytical technique for studying surface electrochemically,stands out as a powerful tool offering electrochemical insights.It possesses remarkable spatiotemporal resolution,enabling the visualization of the localized electrochemical activity and surface topography.This review compiles crucial research findings and recent breakthroughs in electrocatalytic processes utilizing the SECM methodology,specifically focusing on applications in electrolysis,fuel cells,and metal–oxygen batteries within the realm of energy conversion and storage systems.Commencing with an overview of each energy system,the review introduces the fundamental principles of SECM,and aiming to provide new perspectives and broadening the scope of applied research by describing the major research categories within SECM.
基金support from the National Natural Science Foundation of China(Nos.21878202,21975175,and U1932119)the research project supported by Shanxi Scholarship Council of China(No.2017-041)+1 种基金the Natural Science Foundation of Shanxi Province(No.201801D121052)the National Key Basic Research Program of China(No.2017YFA0403402).
文摘Oxygen evolution reaction(OER)is crucial for hydrogen production as well as other energy storage technologies.CoFe-layered double hydroxide(CoFe-OH)has been widely considered as one of the most efficient electrocatalysts for OER in basic aqueous solution.However,it still suffers from low activity in neutral electrolyte.This paper describes partially oxidized CoFe-OH(PO-CoFe-OH)with enhanced covalency of M-O bonds and displays enhanced OER performance under mild condition.Mechanism studies reveal the suitably enhanced M-O covalency in PO-CoFe-OH shifts the OER mechanism to lattice oxygen oxidation mechanism and also promotes the rate-limiting deprotonation,providing superior OER performance.It just requires the overpotentials of 186 and 365 mV to drive the current density densities of 1 and 10 mA·cm^(-2) in 0.1 M KHCO_(3) aqueous solution(pH=8.3),respectively.It provides a new process for rational design of efficient catalysts for water oxidation in mild conditions.
