期刊
NATIONAL SCIENCE REVIEW
卷 8, 期 7, 页码 -出版社
OXFORD UNIV PRESS
DOI: 10.1093/nsr/nwaa187
关键词
CO2 electroreduction; electrocatalyst; nanosheet; structural evolution; interface
资金
- National Natural Science Foundation of China [21838003, 91834301, 21978278]
- Shanghai Scientific and Technological Innovation Project [18JC1410500, 19JC1410400]
- Fundamental Research Funds for the Central Universities [222201718002]
The study reveals that under CO2 electroreduction conditions, the CeOx/Bi interface structure evolved from CeO2/BiOCl precatalyst plays a crucial role in promoting formate production, with substantially enhanced performance and high Faradaic efficiency approaching 90% for 24 hours.
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.
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