Metal silicate hydroxides have been recognized as efficient oxygen evolution reaction(OER)electrocatalysts,yet tailoring of their intrinsic activity remains confused.Herein,Fe had been incorporated into cobalt silicate hydroxide nanosheets and the resulted material achieves a competitive OER catalytic activity.It is found that the doping state obviously affects the electrical transport property.Specifically,highly dispersed Fe atoms(low-concentration Fe doping)trigger slight electron transfer to Co atoms while serried Fe(high-concentration Fe doping)attract vast electrons.By introducing 6 at.％Fe doping,partial relatively inert Co sites are activated by atomically dispersed Fe,bearing an optimal metal 3d electronic occupation and adsorption capacity to oxygen intermediate.The introduced Co-O-Fe unit trigger theπ-donation effect and decrease the number of electrons in π*-antibonding orbitals,which enhance the Fe-O covalency and the structural stability.As a result,the sample delivers a low overpotential of 293 mV to achieve a current density of 10 mA cm-2.This work clarifies the superiority of atomically dispersed doping state,which is of fundamental interest to the design of doped catalyst.

Jiexin Zhu;Lixue Xia;Wenxuan Yang;Ruohan Yu;Wei Zhang;Wen Luo;Yuhang Dai;Wei Wei;Liang Zhou;Yan Zhao;Liqiang Mai

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing,Wuhan University of Technology,Wuhan 430070,China;International School of Materials Science and Engineering,Wuhan University of Technology,Wuhan 430070,China;Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory,Xianhu Hydrogen Valley,Foshan 528200,China

能源与环境材料（英文）

[1]Jiexin Zhu;Lixue Xia;Wenxuan Yang;Ruohan Yu;Wei Zhang;Wen Luo;Yuhang Dai;Wei Wei;Liang Zhou;Yan Zhao;Liqiang Mai-.Activating Inert Sites in Cobalt Silicate Hydroxides for Oxygen Evolution through Atomically Doping)[J].能源与环境材料（英文）,2022(02):655-661

serried,antibonding,covalency

Activating,Inert,Sites,Cobalt,Silicate,Hydroxides,Oxygen,Evolution,through,Atomically,Doping,Metal,silicate,hydroxides,have,been,recognized,efficient,oxygen,evolution,reaction,OER,electrocatalysts,yet,tailoring,their,intrinsic,activity,remains,confused,Herein,had,incorporated,into,cobalt,nanosheets,resulted,material,achieves,competitive,catalytic,It,found,that,doping,state,obviously,affects,electrical,transport,property,Specifically,highly,dispersed,atoms,low,concentration,trigger,slight,transfer,while,attract,vast,electrons,By,introducing,partial,relatively,inert,sites,are,activated,by,atomically,bearing,optimal,metal,3d,electronic,occupation,adsorption,capacity,intermediate,introduced,unit,donation,effect,decrease,number,orbitals,which,enhance,structural,stability,sample,delivers,overpotential,mV,current,density,mA,This,work,clarifies,superiority,fundamental,interest,design,doped

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