期刊
SCIENCE CHINA-CHEMISTRY
卷 63, 期 10, 页码 1469-1476出版社
SCIENCE PRESS
DOI: 10.1007/s11426-020-9795-x
关键词
ammonia synthesis; nitrate reduction; electron deficient Co; Schottky rectifying effect; high selectivity
资金
- National Natural Science Foundation of China [21871206, 21701122]
Developing efficient electrocatalysts for selective nitrate contamination reduction into value-added ammonia is significant. Here, heterostructured Co/CoO nanosheet arrays (Co/CoO NSAs) exhibited excellent Faradaic efficiency (93.8%) and selectivity (91.2%) for nitrate electroreduction to ammonia, greatly outperforming Co NSAs.N-15 isotope labeling experiments and(1)H nuclear magnetic resonance (NMR) quantitative testing methods confirmed the origin of the produced ammonia. Electrochemicalin situFourier transform infrared (FTIR) spectroscopy, online differential electrochemical mass spectrometry (DEMS) data and density functional theory (DFT) results revealed that the superior performances arose from the electron deficiency of Co induced by the rectifying Schottky contact in the Co/CoO heterostructures. The electron transfer from Co to CoO at the interface could not only suppress the competitive hydrogen evolution reaction, but also increase energy barriers for by-products, thus leading to high Faradaic efficiency and selectivity of ammonia.
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