期刊
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 21, 期 3, 页码 1546-1551出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8cp06978f
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资金
- Australian Government
- Government of Western Australia
- Australian Research Council [DP170103598]
Electrochemical reduction of dinitrogen molecules (N-2) to value-added ammonia by using renewable electricity under mild conditions is regarded as a sustainable and promising strategy for N-2 fixation. However, the lack of efficient, robust and inexpensive electrocatalysts for such electrochemical reduction has prevented its wide application. Herein, we report a novel single-atom catalyst, i.e., a single tungsten (W) atom anchored on N-doped graphyne (W@N-doped graphyne) as a highly efficient and low-cost electrocatalyst for the N-2 reduction reaction. The inert N?N triple bond can be sufficiently activated when an N-2 molecule is adsorbed on the W atom. A single atom of W coordinated with one N atom (doping into an sp-hybridized carbon atom) exhibits the highest catalytic performance with ultra-low onset potential of 0.29 V for N-2 reduction reactions. The distal mechanism' is identified as the most favourable catalytic pathway. Moreover, the improved electrical conductivity of W@N-doped graphyne compared to that of pristine graphyne can ensure better electron transfer efficiency during the reduction processes. Our study provides a novel electrocatalyst with excellent catalytic performance for electrochemical reduction of N-2 to NH3 under ambient conditions.
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