期刊
CHEM
卷 6, 期 10, 页码 2690-2702出版社
CELL PRESS
DOI: 10.1016/j.chempr.2020.07.006
关键词
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资金
- SingaporeMOE AcRF Tier 1 grant [RG113/15, 2016-T1-002-065]
- SingaporeMOE AcRF Tier 2 grant [2017-T2-2-069, 2018-T201-010]
- Welch Foundation [F-1861]
Electrocatalytic dinitrogen reduction reaction (N2RR) is an emerging route for ammonia synthesis at ambient conditions. Albeit the pi back-donation process enables N2RR activity on transition metals with empty d-orbitals, given its dilemma in overcoming hydrogen evolution reaction (HER) competition, exploring p-block-element. based catalysts with relatively inferior HER activity is achievable for high selectivity. The challenge lies in designing rational structure to improve N2RR activity. Here, we synergistically integrate oxygen vacancy (V-O) with hydroxyl on Bi4O5I2 (V-O-Bi4O5I2 -OH), which render this p-block-element-based material active to mimic Tr back-donation behavior because of sufficient vacant orbitals. In neutral media, the electrocatalytic N2RR performance of V-O-Bi4O5I2 -OH in terms of splendid faradic efficiency (32.4%) is superior to most of the prior reports using p-block-element-based catalysts. Our findings show a new strategy toward standout N2RR activity, which holds great potential in exploiting other p-block-element-based electrocatalysts.
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