Supported single-atom catalysts(SACs)possess high catalytic activity,selectivity,and atom utilizations.However,the atom coordination environments of SACs are difficult to accurately regulate due to the high complexity...Supported single-atom catalysts(SACs)possess high catalytic activity,selectivity,and atom utilizations.However,the atom coordination environments of SACs are difficult to accurately regulate due to the high complexity of coordination site and local environment of support.Herein,we develop an in-situ electrochemical cation-exchange method to fill the cation vacancies in MnO_(2)with Ru single atoms(SAs).This obtained catalyst exhibits high mass activity,which is~44 times higher than commercial RuO2 catalyst and excellent stability,superior to the most state-of-the-art oxygen evolution reaction(OER)catalysts.The experimental and theoretical results confirm that the doped Ru can induce charge density redistribution,resulting in the optimized binding of oxygen species,and the strong covalent interaction between Ru and MnO2 for resisting oxidation and corrosion.This work will provide a new concept in the synthesis of well-defined local environments of supported SAs.展开更多
基金supported by the National Natural Science Foundation of China(Nos.21805051 and 21875048)Outstanding Youth Project of Guangdong Natural Science Foundation(No.2020B1515020028)+4 种基金Science and Technology Research Project of Guangzhou(No.202002010007)the Research Fund Program of Key Laboratory of Fuel Cell Technology of Guangdong Province,Australian Research Council(ARC)Future Fellowship(No.FT210100298)Discovery Project(No.DP220100603)CSIRO Energy Centre and Kick-Start ProjectThe Study Melbourne Research Partnerships program has been made possible by funding from the Victorian Government through Study Melbourne.
文摘Supported single-atom catalysts(SACs)possess high catalytic activity,selectivity,and atom utilizations.However,the atom coordination environments of SACs are difficult to accurately regulate due to the high complexity of coordination site and local environment of support.Herein,we develop an in-situ electrochemical cation-exchange method to fill the cation vacancies in MnO_(2)with Ru single atoms(SAs).This obtained catalyst exhibits high mass activity,which is~44 times higher than commercial RuO2 catalyst and excellent stability,superior to the most state-of-the-art oxygen evolution reaction(OER)catalysts.The experimental and theoretical results confirm that the doped Ru can induce charge density redistribution,resulting in the optimized binding of oxygen species,and the strong covalent interaction between Ru and MnO2 for resisting oxidation and corrosion.This work will provide a new concept in the synthesis of well-defined local environments of supported SAs.
