CONSPECTUS:Single-atomic catalyst(SAC)incorporated in graphene plays an increasingly significant role in many applications,including sustainable energy conversion/storage and environmental systems.Such a synergistic s...CONSPECTUS:Single-atomic catalyst(SAC)incorporated in graphene plays an increasingly significant role in many applications,including sustainable energy conversion/storage and environmental systems.Such a synergistic structure commonly consisting of atomic metal active sites stabilized on a robust graphene support,is breaking through the intrinsic limitations of precious-metalbased catalysts and broadening a spectrum of applications,while attaining high atom utilization,remarkable novel catalytic activity,and conformational flexibility.Motivated from the unprecedented attractive features of SAC in graphene,enormous research efforts have been devoted to the development of this ultimate catalytic system.For the further advance and eventual success in this field,a general rule for the rational design of SAC is the first prerequisite.Unfortunately,the research effort for the exploration of the fundamental reaction mechanism and rational design principle has been frequently overlooked in spite of the significantly accumulated research efforts thus far.In this Account,we highlight a new perspective for the rational design of SAC in graphene,conceptually centered on the atomistic level heteroelement dopants of graphene.To provide the intuitive viewpoint on the SAC from the scientific perspective,we suggest a new classification scheme for versatile SACs reported thus far into“dopant catalyst”and“dopant-assisted catalyst”,based on the detailed role of dopant in the catalyst system.Thereafter,we highlight the crucial influencing factors on the catalytic activity of the dopant-induced-catalyst system and toward rational designing rule for high performance catalysts.The recent progress in the dopantinduced-catalyst system for a wide spectrum of catalytic applications,including oxygen reduction,oxygen evolution,hydrogen evolution,and CO_(2)reduction is summarized.Finally,we briefly discuss the challenges and opportunities for the future research direction.The exciting expectation for the well-defined,specifically tailored,high performance dopant-induced-catalyst system is anticipated to address global challenges,including climate change,energy crisis and worldwide pandemics.展开更多
基金supported by the National Creative Research Initiative(CRI)Center for Multi-Dimensional Directed Nanoscale Assembly(2015R1A3A2033061)through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT and Future Planning.
文摘CONSPECTUS:Single-atomic catalyst(SAC)incorporated in graphene plays an increasingly significant role in many applications,including sustainable energy conversion/storage and environmental systems.Such a synergistic structure commonly consisting of atomic metal active sites stabilized on a robust graphene support,is breaking through the intrinsic limitations of precious-metalbased catalysts and broadening a spectrum of applications,while attaining high atom utilization,remarkable novel catalytic activity,and conformational flexibility.Motivated from the unprecedented attractive features of SAC in graphene,enormous research efforts have been devoted to the development of this ultimate catalytic system.For the further advance and eventual success in this field,a general rule for the rational design of SAC is the first prerequisite.Unfortunately,the research effort for the exploration of the fundamental reaction mechanism and rational design principle has been frequently overlooked in spite of the significantly accumulated research efforts thus far.In this Account,we highlight a new perspective for the rational design of SAC in graphene,conceptually centered on the atomistic level heteroelement dopants of graphene.To provide the intuitive viewpoint on the SAC from the scientific perspective,we suggest a new classification scheme for versatile SACs reported thus far into“dopant catalyst”and“dopant-assisted catalyst”,based on the detailed role of dopant in the catalyst system.Thereafter,we highlight the crucial influencing factors on the catalytic activity of the dopant-induced-catalyst system and toward rational designing rule for high performance catalysts.The recent progress in the dopantinduced-catalyst system for a wide spectrum of catalytic applications,including oxygen reduction,oxygen evolution,hydrogen evolution,and CO_(2)reduction is summarized.Finally,we briefly discuss the challenges and opportunities for the future research direction.The exciting expectation for the well-defined,specifically tailored,high performance dopant-induced-catalyst system is anticipated to address global challenges,including climate change,energy crisis and worldwide pandemics.
