期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 39, 页码 16974-16981出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202005574
关键词
amines; electrochemistry; nanostructures; oxidation; surface chemistry
资金
- National Natural Science Foundation of China [21805102, 21825103, 51727809]
- Hubei Provincial Natural Science Foundation of China [2019CFA002]
- Fundamental Research Funds for the Central University [2019kfyXMBZ018]
- Analytical and Testing Center in Huazhong University of Science and Technology
Electrochemical synthesis based on electrons as reagents provides a broad prospect for commodity chemical manufacturing. A direct one-step route for the electrooxidation of amino C-N bonds to nitrile C equivalent to N bonds offers an alternative pathway for nitrile production. However, this route has not been fully explored with respect to either the chemical bond reforming process or the performance optimization. Proposed here is a model of vacancy-rich Ni(OH)(2)atomic layers for studying the performance relationship with respect to structure. Theoretical calculations show the vacancy-induced local electropositive sites chemisorb the N atom with a lone pair of electrons and then attack the corresponding N(sp(3))-H, thus accelerating amino C-N bond activation for dehydrogenation directly into the C equivalent to N bond. Vacancy-rich nanosheets exhibit up to 96.5 % propionitrile selectivity at a moderate potential of 1.38 V. These findings can lead to a new pathway for facilitating catalytic reactions in the chemicals industry.
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