期刊
SMALL
卷 16, 期 2, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.201905825
关键词
CO2 electroreduction; electrocatalysis; Nb4N5; nitrogen vacancies; surface engineering
类别
资金
- National Key R&D Program of China [2017YFA0700104]
- National Science Fund for Distinguished Young Scholars [51825102]
- National Natural Science Foundation of China [51971157, 21601136, 21677010, 21603161, 21501132, 51671145, 51761165012]
- National Program for Thousand Young Talents of China, Wuxi Research Institute of Applied Technologies of Tsinghua University
- Institute for Electronics and Information Technology in Tianjin, Tsinghua University
Surface vacancy engineering holds great promise for boosting the electrocatalytic activity for CO2 reduction reaction; however, the vacancies are generally unstable and may degrade into the inactive phase during electrolysis. Stabilizing the vacancy-enriched structure by heteroatoms can be an effective strategy to get a robust and active catalyst. Herein, a nitrogen-vacancy enriched Nb4N5 on N-doped carbons is constructed, which is thereafter stabilized by a self-enhanced oxygen doping process. This oxygen-doped complex is used as an effective CO2 catalyst, which exhibits a maximum CO Faradaic efficiency of 91% at -0.8 V (vs reversible hydrogen electrode, RHE) and long-term stability throughout 30 h of electrocatalysis. Density function theory calculations suggest that the incorporation of oxygen in Nb4N5 facilitates the formation of *COOH and thus promotes the CO2 reduction.
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