Journal
SCIENCE
Volume 338, Issue 6103, Pages 90-94Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1224581
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Funding
- Agence Nationale de la Recherche [ANR 2010 BLAN 0808]
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Electrochemical conversion of carbon dioxide (CO2) to carbon monoxide (CO) is a potentially useful step in the desirable transformation of the greenhouse gas to fuels and commodity chemicals. We have found that modification of iron tetraphenylporphyrin through the introduction of phenolic groups in all ortho and ortho' positions of the phenyl groups considerably speeds up catalysis of this reaction by the electrogenerated iron(0) complex. The catalyst, which uses one of the most earth-abundant metals, manifests a CO faradaic yield above 90% through 50 million turnovers over 4 hours of electrolysis at low overpotential (0.465 volt), with no observed degradation. The basis for the enhanced activity appears to be the high local concentration of protons associated with the phenolic hydroxyl substituents.
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