Ammonia Electrosynthesis with High Selectivity under Ambient Conditions via a Li+ Incorporation Strategy

作者:Chen, Gao-Feng; Cao, Xinrui; Wu, Shunqing; Zeng, Xingye; Ding, Liang-Xin*; Zhu, Min; Wang, Haihui*
来源:Journal of the American Chemical Society, 2017, 139(29): 9771-9774.
DOI:10.1021/jacs.7b04393

摘要

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.