Asymmetric B-coordination stimulated high-spin cobalt boosts ORR  

作　　者：Yugang Qi Kexin Song Qing Liang Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Qinhua Gu Zhongjun Chen Bingsen Zhang Wei Zhang 

机构地区：[1]Key Laboratory of Automobile Materials MOE,School of Materials Science&Engineering,Electron Microscopy Center,and International Center of Future Science,Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials,Jilin University,Changchun 130012,China [2]Shenyang National Laboratory for Materials Science,Institute of Metal Research,Chinese Academy of Sciences,Shenyang 110016,China [3]Institute of High Energy Physics,Chinese Academy of Sciences,Beijing 100049,China

出　　处：《Nano Research》2025年第4期61-69,共9页纳米研究(英文版)

基　　金：supported by the National Natural Science Foundation of China(Nos.12234018 and 51872115);Beijing Synchrotron Radiation Facility(BSRF)4B9A.

摘　　要：As affordable electrocatalysts for oxygen reduction reactions(ORR)in metal-air batteries,nitrogen-carbon supported atomically dispersed single-atom transition-metal electrocatalysts are emerging.Accurately modulating the first-shell coordination of single-atom metal sites remains challenging,which impedes the elucidation of geometric/electronic structures for optimizing ORR catalysts.Aiming to tackle this challenge by rational design and constructing an asymmetric coordination model catalyst Co-B/N-C,herein we unravel that asymmetric B-coordination stimulates the generation of Co high spin state(t_(2g)5e_(g)2).By using X-ray absorption spectroscopy(XAS),we confirm Co active sites are atomically dispersed with a first-shell coordination of boron and nitrogen atom(Co-B_(1)N_(3)).Thus,the adsorption strength and electron transfer between the cobalt centers and the reactants/intermediates were boosted for optimal ORR capacity(E_(1/2)=0.87 V).Our work will provide valuable new perspectives on the strategic development of high-performance magnetic metal catalysts for ORR.

关 键 词：ELECTROCATALYSIS oxygen reduction reaction single atom catalyst spin state 

分 类 号：O643.36[理学—物理化学]