The demand for clean and sustainable energy has encouraged the production of hydrogen from water electrolyzers.To overcome the obstacle to improving the efficiency of water electrolyzers,it is highly desired to fabric...The demand for clean and sustainable energy has encouraged the production of hydrogen from water electrolyzers.To overcome the obstacle to improving the efficiency of water electrolyzers,it is highly desired to fabricate active electrocatalysts for the sluggish oxygen evolution process.However,there is generally an intrinsic gap between the as-prepared and real electrocatalysts due to structure evolution under the oxidative reaction conditions.Here,we combine in-situ anionic leaching and atomic deposition to realize single-atom catalysts with self-optimized structures.The introduced F ions facilitate structural transformation from Co(OH)xF into CoOOH(F),which generates an amorphous edge surface to provide more anchoring sites for Ir single atoms.Meanwhile,the in-situ anionic leaching of F ions elevates the Co valence state of Ir_(1)/CoOOH(F)more significantly than the counterpart without F ions(Ir_(1)/CoOOH),leading to stronger adsorption of oxygenated intermediates.As revealed by electrochemical measurements,the increased Ir loading together with the favored adsorption of*OH intermediates improve the catalytic activity of Ir_(1)/CoOOH(F).Specifically,Ir_(1)/CoOOH(F)delivered a current density of 10 mA cm-2at an overpotential of 238 mV,being lower than 314 mV for Ir_(1)/CoOOH.The results demonstrated the facility of the in-situ optimization process to optimize catalyst structure for improved performance.展开更多
基金supported by National Key Research and Development Program of China(2021YFA1500500,2019YFA0405600,2017YFA0204904,2019YFA0405602,and 2017YFA0403402)the National Science Fund for Distinguished Young Scholars(21925204)+8 种基金the National Natural Science Foundation of China(21972132,U1732149,U19A2015,U1732272,21673214,92045301,and 21902149)the Fundamental Research Funds for the Central Universities(20720220010)the Provincial Key Research and Development Program of Anhui(202004a05020074)the Anhui Natural Science Foundation for Young Scholars(2208085QB52)K.C.Wong Education(GJTD2020-15)the Hefei Municipal Natural Science Foundation(2021018)the DNL Cooperation Fund,CAS(DNL202003)Users with Excellence Program of Hefei Science Center CAS(2020HSCUE001)USTC Research Funds of the Double First-Class Initiative(YD2340002002)。
文摘The demand for clean and sustainable energy has encouraged the production of hydrogen from water electrolyzers.To overcome the obstacle to improving the efficiency of water electrolyzers,it is highly desired to fabricate active electrocatalysts for the sluggish oxygen evolution process.However,there is generally an intrinsic gap between the as-prepared and real electrocatalysts due to structure evolution under the oxidative reaction conditions.Here,we combine in-situ anionic leaching and atomic deposition to realize single-atom catalysts with self-optimized structures.The introduced F ions facilitate structural transformation from Co(OH)xF into CoOOH(F),which generates an amorphous edge surface to provide more anchoring sites for Ir single atoms.Meanwhile,the in-situ anionic leaching of F ions elevates the Co valence state of Ir_(1)/CoOOH(F)more significantly than the counterpart without F ions(Ir_(1)/CoOOH),leading to stronger adsorption of oxygenated intermediates.As revealed by electrochemical measurements,the increased Ir loading together with the favored adsorption of*OH intermediates improve the catalytic activity of Ir_(1)/CoOOH(F).Specifically,Ir_(1)/CoOOH(F)delivered a current density of 10 mA cm-2at an overpotential of 238 mV,being lower than 314 mV for Ir_(1)/CoOOH.The results demonstrated the facility of the in-situ optimization process to optimize catalyst structure for improved performance.
