期刊
SCIENCE CHINA-CHEMISTRY
卷 64, 期 9, 页码 1493-1497出版社
SCIENCE PRESS
DOI: 10.1007/s11426-021-1073-5
关键词
Electrocatalysis; NO; ammonia synthesis; in situ characterizations; Ru-doped Cu
资金
- National Natural Science Foundation of China [22071173]
- Natural Science Foundation of Tianjin City [20JCJQJC00050, 17JCJQJC44700]
The electrochemical reduction of nitric oxide to produce ammonia using Ru-doped Cu materials shows superior performance compared to pure Cu catalysts, with increased Faradaic efficiency and yield rates. The Ru doping induces changes in the Cu d-band center, facilitating the hydrogenation step and reducing the desorption energy of ammonia for enhanced catalytic activity.
Electrocatalytic nitric oxide (NO) reduction is a promising strategy to produce ammonia. Developing a facile approach to synthesize efficient catalysts with enhanced NO electroreduction performance is highly desirable. Here, a series of Ru-doped Cu materials are constructed through in situ electroreduction of corresponding metal hydroxides. The optimized Ru0.05Cu0.95 exhibits superior electrocatalytic performance for ammonia synthesis by using NO/Ar (1/4, n/n) as the feedstocks (Faradaic efficiency: 64.9%, yield rate: 17.68 mu mol cm(-2) h(-1)), obviously outperforming Cu counterpart (Faradaic efficiency: 33.0%, yield rate: 5.73 mu mol cm(-2) h(-1)). Electrochemical in situ Fourier transform infrared (FTIR) spectroscopy and online differential electrochemical mass spectrometry (DEMS) are adopted to detect intermediates and unveil the possible reaction pathway. The downshift of the Cu d-band center induced by Ru doping facilitates the rate-limiting hydrogenation step and decreases the desorption energy of NH3, leading to high Faradaic efficiency and yield of ammonia.
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