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

• 作者: Ruichao Pang Pengfei Tian Hongliang Jiang Minghui Zhu Xiaozhi Su Yu Wang Xiaoling Yang Yihua Zhu Li Song Chunzhong Li
• 来源期刊: 国家科学评论（英文版）
• 年，卷（期）: 2021,（7）
• 所属期刊栏目: RESEARCH ARTICLES
• 页码范围: 153-161
• 页数: 9页
• 语种: 英文

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 in formate pathway.