Chen, G.-F.Cao, X.Wu, S.Zeng, X.Ding, L.-X.Zhu, M.Wang, H.2018-12-032018-12-032017Journal of the American Chemical Society, 2017; 139(29):9771-97740002-78631520-5126http://hdl.handle.net/2440/116514We report the discovery of a dramatically enhanced N2 electroreduction reaction (NRR) selectivity under ambient conditions via the Li+ 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 N2 to afford a high potential scope for the NRR process to proceed in the "[O-Li+]·N2-Hx" alternating hydrogenation mode. This atomic-scale incorporation strategy provides new insight into the rational design of NRR catalysts with higher selectivity.en© 2017 American Chemical SocietyJournal article003008281010.1021/jacs.7b043932-s2.0-85026312662362288