文献类型：期刊文献

中文题名：Tracking structural evolution: operando regenerative CeO_(x)/Bi interface structure for high-performance CO_(2) electroreduction

作者：Ruichao Pang[1,2];Pengfei Tian[1];Hongliang Jiang[1];Minghui Zhu[1];Xiaozhi Su[3];Yu Wang[3];Xiaoling Yang[2];Yihua Zhu[2];Li Song[4];Chunzhong Li[1,2]

机构：[1]Key Laboratory for Ultrafine Materials of Ministry of Education,School of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China;[2]Shanghai Engineering Research Center of Hierarchical Nanomaterials,School of Materials Science and Engineering,East China University of Science and Technology,Shanghai 200237,China;[3]Shanghai Institute of Applied Physics,Chinese Academy of Sciences,Shanghai 201204,China;[4]National Synchrotron Radiation Laboratory,University of Science and Technology of China,Hefei 230029,China

年份：2021

卷号：8

期号：7

起止页码：153

中文期刊名：National Science Review

外文期刊名：国家科学评论（英文版）

收录：CSTPCD;;Scopus;CSCD:【CSCD2021_2022】；PubMed;

基金：by the National Natural Science Foundation of China(21838003,91834301 and 21978278);the Shanghai Scientific and Technological Innovation Project(18JC1410500 and 19JC1410400);the Fundamental Research Funds for the Central Universities(222201718002).

语种：英文

中文关键词：CO_(2)electroreduction;electrocatalyst;nanosheet;structural evolution;interface

摘要：Unveiling the structural evolution and working mechanism of catalysts under realistic operating conditions is crucial for the design of efficient electrocatalysts for CO_(2) electroreduction,yet remains highly challenging.Here,by virtue of operando structural measurements at multiscale levels,it is identified under CO_(2) electroreduction conditions that an as-prepared CeO_(2)/BiOCl precatalyst gradually evolves into CeO_(x)/Bi interface structure with enriched Ce^(3+) species,which serves as the real catalytically active phase.The derived CeO_(x)/Bi interface structure compared to pure Bi counterpart delivers substantially enhanced performance with a formate Faradaic efficiency approaching 90%for 24 hours in a wide potential window.The formate Faradaic efficiency can be further increased by using isotope D_(2)O instead of H_(2)O.Density functional theory calculations suggest that the regenerative CeO_(x)/Bi interfacial sites can not only promote water activation to increase local ?H species for CO_(2) protonation appropriately,but also stabilize the key intermediate ?OCHO in formate pathway.