The integration of multi-scale active sites has emerged as a promising strategy to overcome the intrinsic limitations of each individual component in electrocatalysis.While single-atom catalysts(SACs)enable maximum at...The integration of multi-scale active sites has emerged as a promising strategy to overcome the intrinsic limitations of each individual component in electrocatalysis.While single-atom catalysts(SACs)enable maximum atomic utilization and well-defined coordination environments,nanoparticles/clusters(NPs/CLs)deliver superior electronic adaptability.However,the synergistic combination introduces complex interfacial interactions that significantly influence reaction pathways,intermediate transport,and microenvironment modulation,yet these effects remain insufficiently understood.This review systematically analyzes recent advances of NPs/CLs-SACs in electrocatalysis,mainly including the local reaction environment and coordinating reaction pathways.NPs/CLs-SACs systems enable unique optimization of electronic structures,stabilization/transport of key intermediates,and decoupling of multi-step reaction pathways.We classify and analyze three major synergistic catalytic modes,including co-adsorption catalysis,tandem catalysis,and parallel adsorption for coupling reactions.Finally,we identify key challenges in synthesis,stability,and mechanism understanding,while outlining future directions for the rational design of sustainable catalytic technologies.展开更多
基金the National Key R&D Program of China(2021YFA1500900)the National Natural Science Foundation of China(22425021,22102053,22372104,22472050,22172047)+4 种基金the Provincial Natural Science Foundation of Hunan(2024JJ2012,2024JJ1003,2021JJ30089)the Science and Technology Innovation Program of Hunan Province(2022RC1036)the Guangdong Basic and Applied Basic Research Foundation(2024A1515012889)the Shenzhen Science and Technology Program(JCYJ20220531102408019,JCYJ20210324122209025,KQTD20190929173914967)the China Postdoctoral Science Foundation(GZC20231710 and 2024M752100)。
文摘The integration of multi-scale active sites has emerged as a promising strategy to overcome the intrinsic limitations of each individual component in electrocatalysis.While single-atom catalysts(SACs)enable maximum atomic utilization and well-defined coordination environments,nanoparticles/clusters(NPs/CLs)deliver superior electronic adaptability.However,the synergistic combination introduces complex interfacial interactions that significantly influence reaction pathways,intermediate transport,and microenvironment modulation,yet these effects remain insufficiently understood.This review systematically analyzes recent advances of NPs/CLs-SACs in electrocatalysis,mainly including the local reaction environment and coordinating reaction pathways.NPs/CLs-SACs systems enable unique optimization of electronic structures,stabilization/transport of key intermediates,and decoupling of multi-step reaction pathways.We classify and analyze three major synergistic catalytic modes,including co-adsorption catalysis,tandem catalysis,and parallel adsorption for coupling reactions.Finally,we identify key challenges in synthesis,stability,and mechanism understanding,while outlining future directions for the rational design of sustainable catalytic technologies.