材料科学
法拉第效率
石墨烯
可逆氢电极
催化作用
一氧化碳
电化学
电催化剂
碳纤维
共价键
密度泛函理论
化学工程
二氧化碳电化学还原
纳米技术
无机化学
电极
物理化学
计算化学
化学
工作电极
有机化学
复合数
工程类
复合材料
作者
Shan Chen,Jialei Chen,Youzeng Li,Sha Tan,Xuelong Liao,Tete Zhao,Kai Zhang,Enyuan Hu,Fangyi Cheng,Huan Wang
标识
DOI:10.1002/adfm.202300801
摘要
Abstract Electrochemical carbon dioxide (CO 2 ) reduction into value‐added products holds great promise in moving toward carbon neutrality but remains a grand challenge due to lack of efficient electrocatalysts. Herein, the nucleophilic substitution reaction is elaborately harnessed to synthesize carbon nanoplates with a FeN 4 O configuration anchored onto graphene substrate (FeN 4 OC/Gr) through covalent linkages. Density functional theory calculations demonstrate the unique configuration of FeN 4 O with one oxygen (O) atom in the axial direction not only suppresses the competing hydrogen evolution reaction, but also facilitates the desorption of *CO intermediate compared with the commonly planar single‐atomic Fe sites. The FeN 4 OC/Gr shows excellent performance in the electroreduction of CO 2 into carbon monoxide (CO) with an impressive Faradaic efficiency of 98.3% at −0.7 V versus reversible hydrogen electrode (RHE) and a high turnover frequency of 3511 h −1 . Furthermore, as a cathode catalyst in an aqueous zinc (Zn)‐CO 2 battery, the FeN 4 OC/Gr achieves a high CO Faradaic efficiency (≈91%) at a discharge current density of 3 mA cm −2 and long‐term stability over 74 h. This work opens up a new route to simultaneously modulate the geometric and electronic structure of single‐atomic catalysts toward efficient CO 2 conversion.
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