Tailoring the proximity of iron and manganese atomic sites for efficient CO_(2)electroreduction reaction  

作　　者：Xiaohui Sun Bangyan Zhang Qing Lu Jingjing Jiang Chenliang Ye Guoqing Cui Zechao Zhuang Jun Zhang Johannes HBitter Guanna Li Chunming Xu 

机构地区：[1]State Key Laboratory of Heavy Oil Processing,China University of Petroleum(Beijing),Beijing 102249,China [2]Department of Chemistry,Tsinghua University,Beijing 100084,China [3]Biobased Chemistry and Technology,Wageningen University&Research,Wageningen,6708WG,The Netherlands [4]Department of Materials Science and Engineering,China University of Petroleum(East China),Qingdao 266580,China [5]Institute of Analysis and Testing,Institute of Analysis and Testing,Beijing Academy of Science and Technology(Beijing Center for Physical and Chemical Analysis),Beijing 100094,China

出　　处：《Nano Research》2025年第3期73-81,共9页纳米研究(英文版)

基　　金：supported by National Natural Science Foundation of China(Nos.22478419,22102080,and 221011150);Key Project of National Natural Science Foundation of China(No.U22B20149);Science Foundation of China University of Petroleum(Beijing)(No.ZX20230067);The authors acknowledge the Dutch Organization for Scientific Research(NWO)for access to the Dutch national e-infrastructure(Nos.EINF-4693 and EINF-6899);The authors thank the BL14W1 station in Shanghai Synchrotron Radiation Facility(SSRF)and the 1W1B station in Beijing Synchrotron Radiation Facility(BSRF)for XAFS test.

摘　　要：Electrochemical carbon dioxide reduction reaction(CO_(2)RR)into high-value added chemicals and fuels has aroused wide attention,but suffers from high overpotential and poor selectivity.Herein,nitrogen-doped carbon supported Fe and Mn heteronuclear single atom catalysts with different Fe and Mn inter-site distance were fabricated via a templating isolation approach and tested for CO_(2)RR to CO in an aqueous solution.The catalyst with atomically dispersed Fe and Mn sites in close proximity exhibited the highest CO_(2)RR performance,with a CO Faradaic efficiency of 96%at a low overpotential of 320 mV,and a Tafel slope of only 62 mV·dec^(−1),comparable to state-of-the-art gold catalysts.Experimental analysis combined with theory highlighted that single Mn atom at the neighboring site of Fe enhanced the electronic localization of Fe center,which facilitated the generation of key^(*)COOH intermediate as well as CO^(*) desorption on Fe,leading to superior CO_(2)RR performance at low overpotentials.This work offers atomic-level insights into the correlation between the inter-site distance of atomic sites and CO_(2)RR performance,and paves a new avenue for precise control of single-atom sites on carbon surface for highly active and selective electrocatalysts.

关 键 词：CO_(2)electroreduction heteronuclear single-atom catalyst inter-site distance electron localization scaling relationships low overpotentials 

分 类 号：O64[理学—物理化学]