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

Gao-Feng Chen; Xinrui Cao; Shunqing Wu; Xingye Zeng; Liang-Xin Ding; Min Zhu; Haihui Wang

doi:10.1021/jacs.7b04393

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

J Am Chem Soc. 2017 Jul 26;139(29):9771-9774. doi: 10.1021/jacs.7b04393. Epub 2017 Jul 13.

Authors

Gao-Feng Chen¹, Xinrui Cao², Shunqing Wu², Xingye Zeng¹, Liang-Xin Ding¹, Min Zhu³, Haihui Wang¹

Affiliations

¹ School of Chemistry and Chemical Engineering, South China University of Technology , Guangzhou 510640, China.
² Collaborative Innovation Center for Optoelectronic Semiconductors and Efficient Devices, Department of Physics, Xiamen University , Xiamen 361005, China.
³ School of Materials Science and Engineering, South China University of Technology , Guangzhou 510640, China.

PMID: 28693318
DOI: 10.1021/jacs.7b04393

Abstract

We 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-H_x" alternating hydrogenation mode. This atomic-scale incorporation strategy provides new insight into the rational design of NRR catalysts with higher selectivity.

Publication types

Research Support, Non-U.S. Gov't