Tertiary Amine-Assisted Electroreduction of Carbon Dioxide to Formate Catalyzed by Iron Tetraphenylporphyrin

被引:64
作者
Margarit, Charles G. [1 ]
Asimow, Naomi G. [1 ]
Costentin, Cyrille [1 ,2 ,3 ]
Nocera, Daniel G. [1 ]
机构
[1] Harvard Univ, Dept Chem & Chem Biol, Cambridge, MA 02138 USA
[2] Univ Paris Diderot, Sorbonne Paris Cite, F-75205 Paris 13, France
[3] Univ Grenoble Alpes, CNRS, UMR 5250, Dept Chim Mol, F-3800 Grenoble, France
关键词
ELECTROCHEMICAL REDUCTION; MOLECULAR CATALYSIS; ELECTROCATALYTIC REDUCTION; CO2; BOND; PORPHYRINS; CONVERSION; EVOLUTION; INSERTION;
D O I
10.1021/acsenergylett.9b02093
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The reduction of CO, by electrogenerated Fe(0)TPP can be directed toward formate with a good selectivity (ca. 70%) upon addition of a tertiary amine in the presence of a weak proton donor. Whereas most systems generating formate from CO2 involve the initial formation of a hydride, we demonstrate herein that the hydride pathway is avoided by preferential binding of CO2 that may then be protonated by weak acids. The net result is that hydrogen production via the hydride is disfavored, thus leading to high yields of formate. These results demonstrate an alternative route for the activation of CO2 to formate.
引用
收藏
页码:72 / +
页数:13
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