Journal
NATURE COMMUNICATIONS
Volume 6, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms9177
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Funding
- Chinese Scholarship Council
- NanoNextNL
- micro and nanotechnology consortium of the Government of the Netherlands
- BioSolar Cells open innovation consortium
- Dutch Ministry of Economic Affairs, Agriculture and Innovation
- Netherlands Organization for Scientific Research (NWO)
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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 Bronsted 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.
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