化学
石墨氮化碳
法拉第效率
氢键
氨
离解(化学)
氢
固碳
吸附
电化学
光化学
催化作用
分子
有机化学
二氧化碳
物理化学
光催化
电极
作者
Jiayin Shang,Kai Zhang,Qiguan Wang,Siqin Jia,Sumin Wang,Zhiruo Shen,Xinhai Wang
标识
DOI:10.1016/j.cej.2022.139606
摘要
N2 electrochemical reduction (NRR) suffers from weak activity and fierce competition of hydrogen evolution reaction (HER). Herein, we propose a strengthened activating strategy for N2 fixation via hydrogen bonds. To this end, amino functionalized graphitic carbon nitride (NHx-gCN) is designed. Through the NH⋯N hydrogen bonds between amino groups and N2 as well as NRR intermediates of NxHy, NHx-gCN presents dramatically enhanced NRR performance, with NH3 yield rate of 56.38 µg mg−1cat h−1 and Faradaic efficiency of 27.00 % at −0.73 V (vs RHE). Theoretical calculations certify through hydrogen bonds the adsorption of N2 and NxHy on NHx-gCN is enhanced and the dissociation of N2 into *N2H and *N2H2 is greatly facilitated. Besides, hydrogen bonding interactions between amino groups and heptazine can suppress the HER by inhibiting adsorption of proton H. This work delivers a new hydrogen-bond strategy to optimal NRR performance with both high NH3 production and high Faradaic efficiency.
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