期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 59, 期 31, 页码 13021-13027出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202004213
关键词
2D carbon allotropes; ammonia synthesis; graphdiyne; heterostructures; self-supporting electrocatalysts
资金
- National Nature Science Foundation of China [21790050, 21790051, 21771156]
- National Key Research and Development Project of China [2016YFA0200104, 2018YFA0703501]
- Key Program of the Chinese Academy of Sciences [QYZDY-SSW-SLH015]
- Early Career Scheme (ECS) fund from the Research Grant Council (RGC) in Hong Kong [PolyU 253026/16P]
A freestanding 3D graphdiyne-cobalt nitride (GDY/Co2N) with a highly active and selective interface is fabricated for the electrochemical nitrogen reduction reaction (ECNRR). Density function theory calculations reveal that the interface-bonded GDY contributes an unique p-electronic character to optimally modify the Co-N compound surface bonding, which generates as-observed superior electronic activity for NRR catalysis at the interface region. Experimentally, at atmospheric pressure and room temperature, the electrocatalyst creates a new record of ammonia yield rate (YNH3 ) and Faradaic efficiency (FE) of 219.72 mu g h(-1) mg(cat.)(-1) and 58.60 %, respectively, in acidic conditions, higher than reported electrocatalysts. Such a catalyst is promising to generate new concepts, new knowledge, and new phenomena in electrocatalytic research, driving rapid development in the field of electrocatalysis.
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