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

作者机构：Chongqing Key Laboratory of Materials Surface&Interface ScienceChongqing University of Arts and SciencesChongqing 402160China School of Chemistry and Chemical EngineeringChongqing University of TechnologyChongqing 400054China College of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China State Key Laboratory of Heavy Oil ProcessingBeijing Key Laboratory of Biogas Upgrading UtilizationChina University of Petroleum-BeijingBeijing 102249China College of Chemistry and Environmental EngineeringSichuan University of Science and EngineeringZigong 643000SichuanChina School of Physics and Electronic EngineeringChongqing Normal UniversityChongqing 401331China 

出 版 物：《Journal of Energy Chemistry》 (能源化学（英文版）)

年 卷 期：2023年第80卷第5期

页      面：542-552,I0012页

核心收录：

学科分类：0808[工学-电气工程] 081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 0703[理学-化学] 0702[理学-物理学] 

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) 

主　　题：Single-atom manganese catalyst Mn-N5 active moiety Oxygen reduction reaction,Coordination number Axial pyridinic-nitrogen coordination 

摘      要：Designing single-atom catalysts for oxygen reduction reaction(ORR)are fashionable but challenging to boost the zinc-air battery *** enhanced ORR activity by manganese(Mn)singleatom catalysts can be achieved by accurately regulating the coordination number of isolated Mn *** 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 *** 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/*** 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.