Ammonia Electrosynthesis with High Selectivity under Ambient Conditions via a Li+ Incorporation Strategy
Top Cited Papers
- 13 July 2017
- journal article
- research article
- Published by American Chemical Society (ACS) in Journal of the American Chemical Society
- Vol. 139 (29), 9771-9774
- https://doi.org/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—Hx” alternating hydrogenation mode. This atomic-scale incorporation strategy provides new insight into the rational design of NRR catalysts with higher selectivity.Funding Information
- Ministry of Science and Technology of the People's Republic of China (2016YFA0202601)
- National Natural Science Foundation of China (21406078, 51621001)
- Guangzhou Science, Technology and Innovation Commission (201610010076)
This publication has 32 references indexed in Scilit:
- Light-driven dinitrogen reduction catalyzed by a CdS:nitrogenase MoFe protein biohybridScience, 2016
- New recipe produces ammonia from air, water, and sunlightScience, 2014
- Challenges in reduction of dinitrogen by proton and electron transferChemical Society Reviews, 2014
- Evidence for Interstitial Carbon in Nitrogenase FeMo CofactorScience, 2011
- One electron at a timeNature Chemistry, 2009
- Nitrogen Cycle ElectrocatalysisChemical Reviews, 2009
- Reactions at Surfaces: From Atoms to Complexity (Nobel Lecture)Angewandte Chemie, 2008
- Towards an ammonia-mediated hydrogen economy?Catalysis Today, 2006
- Ammonia Synthesis from First-Principles CalculationsScience, 2005
- Electrosynthesis of ammoniaNature, 1985