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

Jing Shen, Ruud Kortlever, Recep Kas, Yuvraj Y. Birdja, Oscar Diaz-Morales, Youngkook Kwon, Isis Ledezma-Yanez, Klaas Jan P. Schouten, Guido Mul and Marc T. M. Koper ()
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Jing Shen: Leiden Institute of Chemistry, Leiden University
Ruud Kortlever: Leiden Institute of Chemistry, Leiden University
Recep Kas: PhotoCatalytic Synthesis Group, MESA+ Institute for Nanotechnology, Faculty of Science and Technology, University of Twente
Yuvraj Y. Birdja: Leiden Institute of Chemistry, Leiden University
Oscar Diaz-Morales: Leiden Institute of Chemistry, Leiden University
Youngkook Kwon: Leiden Institute of Chemistry, Leiden University
Isis Ledezma-Yanez: Leiden Institute of Chemistry, Leiden University
Klaas Jan P. Schouten: Leiden Institute of Chemistry, Leiden University
Guido Mul: PhotoCatalytic Synthesis Group, MESA+ Institute for Nanotechnology, Faculty of Science and Technology, University of Twente
Marc T. M. Koper: Leiden Institute of Chemistry, Leiden University

Nature Communications, 2015, vol. 6, issue 1, 1-8

Abstract: 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.

Date: 2015
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DOI: 10.1038/ncomms9177

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