Electrocatalytic reduction of carbon dioxide to carbon monoxide and methane at an immobilized cobalt protoporphyrin

Nature Communications
Jing ShenMarc T M Koper

Abstract

The electrochemical conversion of carbon dioxide and water into useful products is a major challenge in facilitating a closed carbon cycle. Here we report a cobalt protoporphyrin immobilized on a pyrolytic graphite electrode that reduces carbon dioxide in an aqueous acidic solution at relatively low overpotential (0.5 V), with an efficiency and selectivity comparable to the best porphyrin-based electrocatalyst in the literature. While carbon monoxide is the main reduction product, we also observe methane as by-product. The results of our detailed pH-dependent studies are explained consistently by a mechanism in which carbon dioxide is activated by the cobalt protoporphyrin through the stabilization of a radical intermediate, which acts as Brønsted base. The basic character of this intermediate explains how the carbon dioxide reduction circumvents a concerted proton-electron transfer mechanism, in contrast to hydrogen evolution. Our results and their mechanistic interpretations suggest strategies for designing improved catalysts.

References

May 19, 2005·Journal of the American Chemical Society·Matheus T de GrootMarc T M Koper
Feb 9, 2008·Physical Chemistry Chemical Physics : PCCP·Matheus T de Groot, Marc T M Koper
Jul 16, 2008·Chemical Reviews·Jean-Michel Savéant
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Citations

Jan 2, 2016·The Journal of Physical Chemistry Letters·Ruud KortleverMarc T M Koper
Jun 17, 2016·Journal of the American Chemical Society·Zhe WengHailiang Wang
Jan 19, 2017·Journal of the American Chemical Society·Yuvraj Y Birdja, Marc T M Koper
Mar 18, 2017·Chemical Reviews·Chaoliang TanHua Zhang
May 4, 2017·Journal of the American Chemical Society·Moritz F KuehnelErwin Reisner
Jun 1, 2017·Physical Chemistry Chemical Physics : PCCP·Cang Lang YaoQing Jiang
Jan 24, 2018·Angewandte Chemie·Sabine MöhleSiegfried R Waldvogel
Oct 19, 2017·Anais Da Academia Brasileira De Ciências·Caterina G C MarquesHenrique E Toma
Jun 1, 2018·Chemical Communications : Chem Comm·Sze Koon LeeShigeyuki Masaoka
Aug 22, 2018·Advanced Materials·Tingting ZhengHaotian Wang
Jan 5, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Pritha SenAbhishek Dey
Jan 5, 2019·Chembiochem : a European Journal of Chemical Biology·Hathaichanok SeelajaroenNiyazi Serdar Sariciftci
Apr 13, 2019·Physical Chemistry Chemical Physics : PCCP·Xiaoli WangFang Huang
Apr 26, 2019·Dalton Transactions : an International Journal of Inorganic Chemistry·Changcheng JiangCharles W Machan
Jul 16, 2019·Angewandte Chemie·Jianyu HanZhiyong Tang
Aug 29, 2019·Nature Communications·Sabrina GonglachSoumyajit Roy
Nov 7, 2018·Nature Communications·Jun LiDavid Sinton
Feb 27, 2020·Nature Materials·Dae-Hyun NamEdward H Sargent

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Methods Mentioned

BETA
scanning
atomic force microscopy
X-ray
nuclear magnetic resonance

Software Mentioned

IviumStat

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