期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 36, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202207807
关键词
Boron Carbon Nitride; Defects; Electrochemical; Frustrated Lewis Pairs; Nitrogen Fixation
资金
- National Key R&D Program of China [2021YFC2103704]
- National Natural Science Foundation of China [22022812, 21978259]
- Fundamental Research Funds for the Central Universities [226-2022-00055]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division
In this study, a defective boron carbon nitride catalyst was developed, which achieved high Faraday efficiency and ammonia yield, and had long-term durability.
The electrocatalytic nitrogen reduction reaction (NRR) on metal-free catalysts is an attractive alternative to the industrial Haber-Bosch process. However, the state-of-the-art metal-free electrocatalysts still suffer from low Faraday efficiencies and low ammonia yields. Herein, we present a molecular design strategy to develop a defective boron carbon nitride (BCN) catalyst with the abundant unsaturated B and N atoms as Lewis acid and base sites, which upgrades the catalyst from a single Lewis acid catalysis to frustrated Lewis pairs (FLPs) catalysis. N-14(2)/N-15(2) exchange experiments and density functional theory (DFT) calculations reveal that FLPs can adsorb an N-2 molecule to form a six-membered ring intermediate, which enables the cleavage of N-2 via a pull-pull effect, thereby significantly reducing the energy barrier to -0.28 eV. Impressively, BCN achieves a high Faraday efficiency of 18.9 %, an ammonia yield of 20.9 mu g h(-1) mg(cat.)(-1), and long-term durability.
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