文献类型：期刊文献

英文题名：Tracking structural evolution: operando regenerative CeOx/Bi interface structure for high-performance CO2 electroreduction

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

机构：[1]East China Univ Sci & Technol, Sch Chem Engn, Key Lab Ultrafine Mat, Minist Educ, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Hierarch Nanomat, Sch Mat Sci & Engn, Shanghai 200237, Peoples R China;[3]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201204, Peoples R China;[4]Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China

年份：2021

卷号：8

期号：7

外文期刊名：NATIONAL SCIENCE REVIEW

收录：;EI(收录号：20213310774319);WOS:【SCI-EXPANDED(收录号:WOS:000697170300006)】；

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

语种：英文

外文关键词：CO2 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 CO2 electroreduction, yet remains highly challenging. Here, by virtue of operando structural measurements at multiscale levels, it is identified under CO2 electroreduction conditions that an as-prepared CeO2/BiOCl precatalyst gradually evolves into CeOx/Bi interface structure with enriched Ce3+ species, which serves as the real catalytically active phase. The derived CeOx/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 D2O instead of H2O. Density functional theory calculations suggest that the regenerative CeOx/Bi interfacial sites can not only promote water activation to increase local H-* species for CO2 protonation appropriately, but also stabilize the key intermediate (OCHO)-O-* in formate pathway.