卟啉
催化作用
铜
法拉第效率
电催化剂
接受者
密度泛函理论
选择性
材料科学
光化学
无机化学
电化学
组合化学
化学
电极
计算化学
有机化学
物理化学
物理
凝聚态物理
作者
Pinger Yu,Ximeng Lv,Qihao Wang,Haoliang Huang,Weijun Weng,Peng Chen,Linjuan Zhang,Gengfeng Zheng
出处
期刊:Small
[Wiley]
日期:2022-11-24
卷期号:19 (4)
被引量:30
标识
DOI:10.1002/smll.202205730
摘要
Molecular catalysts have been receiving increasingly attention in the electrochemical CO2 reduction reaction (CO2 RR) with attractive features such as precise catalytic sites and tunable ligands. However, the insufficient activity and low selectivity of deep reduction products restrain the utilization of molecular catalysts in CO2 RR. Herein, a donor-acceptor modified Cu porphyrin (CuTAPP) is developed, in which amino groups are linked to donate electrons toward the central CuN4 site to enhance the CO2 RR activity. The CuTAPP catalyst exhibited an excellent CO2 -to-CH4 electroreduction performance, including a high CH4 partial current density of 290.5 mA cm-2 and a corresponding Faradaic efficiency of 54.8% at -1.63 V versus reversible hydrogen electrode in flow cells. Density functional theory calculations indicated that CuTAPP presented a much lower energy gap in the pathway of producing *CHO than Cu porphyrin without amino group modification. This work suggests a useful strategy of introducing designed donor-acceptor structures into molecular catalysts for enhancing electrochemical CO2 conversion toward deep reduction products.
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