Regulating single-atom Mn sites by precisely axial pyridinic-nitrogen coordination to stabilize the oxygen reduction  

作　　者：Yuan Qin Chaozhong Guo Zihao Ou Chuanlan Xu Qi Lan Rong Jin Yao Liu Yingchun Niu Quan Xu Yujun Si Honglin Li 

机构地区：[1]Chongqing Key Laboratory of Materials Surface&Interface Science,Chongqing University of Arts and Sciences,Chongqing 402160,China [2]School of Chemistry and Chemical Engineering,Chongqing University of Technology,Chongqing 400054,China [3]College of Chemistry and Chemical Engineering,Chongqing University,Chongqing 401331,China [4]State Key Laboratory of Heavy Oil Processing,Beijing Key Laboratory of Biogas Upgrading Utilization,China University of Petroleum-Beijing,Beijing 102249,China [5]College of Chemistry and Environmental Engineering,Sichuan University of Science and Engineering,Zigong 643000,Sichuan,China [6]School of Physics and Electronic Engineering,Chongqing Normal University,Chongqing 401331,China

出　　处：《Journal of Energy Chemistry》2023年第5期542-552,I0012,共12页能源化学（英文版）

基　　金：supported by the National Natural Science Foundation of China(22275026 and 21805024);the Natural Science Foundation of Chongqing,China(cstc2021jcyj-msxm X0783,cstc2019jscx-msxm X0393 and cstc2018jcyj AX0461);the Scientific and Technological Research Program of Chongqing Municipal Education Commission(KJZD-K202101303,KJQN201901335 and KJQN202001322);the Scientific Research Program of Chongqing Urban Administration(CGKZ2020-26)。

摘　　要：Designing single-atom catalysts for oxygen reduction reaction(ORR)are fashionable but challenging to boost the zinc-air battery performance.Significantly enhanced ORR activity by manganese(Mn)singleatom catalysts can be achieved by accurately regulating the coordination number of isolated Mn atoms.Theoretical calculations indicate that the single Mn-N5sites possess lower free energy barrier and higher oxygen adsorption performance than single Mn-N4sites to accelerate the ORR kinetics.Target to it,here we synthesize an atomically dispersed Mn-N5catalyst by precisely axial coordination of pyridinic-N doped into two-dimensional(2D)porous nanocarbon sheets(~3.56 nm thickness),which reveals outstanding catalytic activity and ultrahigh stability for the ORR in zinc-air battery owing to the inhomogeneous charge distribution of Mn-N5sites compared to the conventional single-site Mn-N4catalyst and Pt/C.This work gives a new strategy for in situ regulating the electronic structure of metal single-atoms and further promoting the overall ORR performance in energy systems.

关 键 词：Single-atom manganese catalyst Mn-N5 active moiety Oxygen reduction reaction Coordination number Axial pyridinic-nitrogen coordination 

分 类 号：TM911.41[电气工程—电力电子与电力传动] O643.36[理学—物理化学]