期刊
CHEM CATALYSIS
卷 1, 期 5, 页码 1088-1103出版社
CELL PRESS
DOI: 10.1016/j.checat.2021.08.014
关键词
-
资金
- Natural Science Foundation of China [22022605, 21936005]
- China Postdoctoral Science Foundation [2020TQ0166, 2021M691771]
PdCu/Cu2O hybrids with mesoporous hollow sphere structure exhibit high selectivity and Faradaic efficiency for NH3 synthesis from NO3(-) due to the electron transfer between Pd and Cu, as well as the blockage of intermediate generation by PdCu alloys.
Electrocatalytic conversion of nitrate (NO3-) to ammonia (NH3) holds significant potential in the control of nitrogen oxide (NOx) from stationary sources. However, previous studies on reaction intermediates remain unclear. Here we report that PdCu/Cu2O hybrids with mesoporous hollow sphere structure show high selectivity (96.70%) and Faradaic efficiency (94.32%) for NH3 synthesis from NO3 (-) , Detailed characterizations demonstrate that (1) Pd enables electron transfer (Pd 3d/ Cu 3d) and causes the polarization of Cu 3d orbitals by forming partial PdCu alloys, which makes Pd electron deficient but offers empty orbits to adsorb NO3-, and (2) electron-rich Cu ismore conducive to the occurrence of NO3- reduction. The mutual confirmation of online differential electrochemical mass spectrometry and density functional theory calculations demonstrates that PdCu alloys block the generation of *NOH intermediate and facilitate the formation of * N, providing a new mechanism for NH3 synthesis from NO3- reduction reactions.
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