Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 29, Pages 9771-9774Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b04393
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Funding
- National Natural Science Foundation of China [21406078, 51621001]
- National Key RD Program [2016YFA0202601]
- Pearl River and S&T Nova Program of Guangzhou [201610010076]
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We report the discovery of a dramatically enhanced N-2 electroreduction reaction (NRR) selectivity under ambient conditions via the Lit incorporation into poly(N-ethyl-benzene-1,2,4,5-tetracarboxylic diimide) (PEBCD) as a catalyst. The detailed electrochemical evaluation and density functional theory calculations showed that Li+ association with the O atoms in the PEBCD matrix can retard the HER process and can facilitate the adsorption of N-2 to afford a high potential scope for the NRR process to proceed in the [O-Li+]center dot N-2-H-x alternating hydrogenation mode. This atomic scale incorporation strategy provides new insight into the rational design of NRR catalysts with higher selectivity.
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