Ammonia Electrosynthesis with High Selectivity under Ambient Conditions via a Li+ Incorporation Strategy
Ammonia Electrosynthesis with High Selectivity under Ambient Conditions via a Li+ Incorporation Strategy
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DOI：
10.1021/jacs.7b04393
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发表时间：
2017-07-26
影响因子：
15
通讯作者：
Wang, Haihui
中科院分区：
文献类型：
--
作者：
Chen, Gao-Feng;Cao, Xinrui;Wang, Haihui
我们报告了一个显着增强的N-2电还原反应（NRR）的选择性，在环境条件下，通过Lit纳入聚（N-乙基-苯-1，2，4，5-四羧酸二酰亚胺）（PEBCD）作为催化剂的发现。详细的电化学评价和密度泛函理论计算表明，Li+与PEBCD基体中O原子的缔合可以延缓HER过程的进行，并促进N2的吸附，为NRR过程提供了一个高电位范围，使其以“[O-Li+]中心点N2-H-x”交替加氢模式进行。这种原子尺度的掺入策略为具有更高选择性的NRR催化剂的合理设计提供了新的见解。
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.