期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 13, 页码 5350-5354出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201915992
关键词
N-15 isotope labeling; ammonia; electrocatalysis; in situ reconstruction; nitrate electroreduction
资金
- National Natural Science Foundation of China [21701122, 21871206]
Unveiling the active phase of catalytic materials under reaction conditions is important for the construction of efficient electrocatalysts for selective nitrate reduction to ammonia. The origin of the prominent activity enhancement for CuO (Faradaic efficiency: 95.8 %, Selectivity: 81.2 %) toward selective nitrate electroreduction to ammonia was probed. N-15 isotope labeling experiments showed that ammonia originated from nitrate reduction. H-1 NMR spectroscopy and colorimetric methods were performed to quantify ammonia. In situ Raman and ex situ experiments revealed that CuO was electrochemically converted into Cu/Cu2O, which serves as an active phase. The combined results of online differential electrochemical mass spectrometry (DEMS) and DFT calculations demonstrated that the electron transfer from Cu2O to Cu at the interface could facilitate the formation of *NOH intermediate and suppress the hydrogen evolution reaction, leading to high selectivity and Faradaic efficiency.
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