Regulating the orbital spin-electron filling of metal centers via interatomic electron transfer in transition metal oxides is one promising approach to enhancing their electrocatalytic oxygen evolution reaction(OER)pe...Regulating the orbital spin-electron filling of metal centers via interatomic electron transfer in transition metal oxides is one promising approach to enhancing their electrocatalytic oxygen evolution reaction(OER)performances,while it is still a challenge due to lacking of efficient strategy and deep understanding.In this work,a facile strategy containing electrochemical deposition and annealing in air atmosphere has been proposed to introduce monodispersed neodymium(Nd)atoms into spinel Co_(3)O_(4)nanosheets to trigger the electron transfer.Accordingly,the as-prepared Nd doped Co_(3)O_(4)nanosheets(Nd/Co_(3)O_(4))on nickel foam or carbon cloth showed greatly enhanced OER performances,with low overpotential of 284 and 396 mV at 10 m A cm^(-2),small Tafel slope of 95 and 119 mV dec^(-1)in 1.0 M KOH and 0.5 M H_(2)SO_(4),respectively.The experimental and density function theory results coherently indicate that the charge transfer in the Nd-O-Co asymmetric configuration not only enhances the conductivity of Co_(3)O_(4),but also regulates the filling degree of egorbitals of Co,leading to higher spin states,optimized adsorption ability,and accelerated H_(2)O dissociation process,thus achieving boosted OER activity.展开更多
基金support from the Natural Science Foundation and Overseas Talent Projects of Jiangxi Province(20242BAB25217,20232BAB214025,20232BCJ25044)the Jiangxi Provincial Natural Science Foundation(20232BAB204088)the National Natural Science Foundation of China(52402132)。
文摘Regulating the orbital spin-electron filling of metal centers via interatomic electron transfer in transition metal oxides is one promising approach to enhancing their electrocatalytic oxygen evolution reaction(OER)performances,while it is still a challenge due to lacking of efficient strategy and deep understanding.In this work,a facile strategy containing electrochemical deposition and annealing in air atmosphere has been proposed to introduce monodispersed neodymium(Nd)atoms into spinel Co_(3)O_(4)nanosheets to trigger the electron transfer.Accordingly,the as-prepared Nd doped Co_(3)O_(4)nanosheets(Nd/Co_(3)O_(4))on nickel foam or carbon cloth showed greatly enhanced OER performances,with low overpotential of 284 and 396 mV at 10 m A cm^(-2),small Tafel slope of 95 and 119 mV dec^(-1)in 1.0 M KOH and 0.5 M H_(2)SO_(4),respectively.The experimental and density function theory results coherently indicate that the charge transfer in the Nd-O-Co asymmetric configuration not only enhances the conductivity of Co_(3)O_(4),but also regulates the filling degree of egorbitals of Co,leading to higher spin states,optimized adsorption ability,and accelerated H_(2)O dissociation process,thus achieving boosted OER activity.
