Journal
NATURE CHEMISTRY
Volume 4, Issue 10, Pages 794-801Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.1439
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Funding
- Bowling Green State University [CHE-1055397, CHE-0743258]
- National Science Foundation [CHE-1055397, CHE-0743258]
- Ohio Supercomputer Center
- Ohio State University
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The success of solar fuel technology relies on the development of efficient catalysts that can oxidize or reduce water. All molecular water-oxidation catalysts reported thus far are transition-metal complexes, however, here we report catalytic water oxidation to give oxygen by a fully organic compound, the N(5)-ethylflavinium ion, Et-Fl(+). Evolution of oxygen was detected during bulk electrolysis of aqueous Et-Fl(+) solutions at several potentials above +11.9 V versus normal hydrogen electrode. The catalysis was found to occur on glassy carbon and platinum working electrodes, but no catalysis was observed on fluoride-doped tin-oxide electrodes. Based on spectroelectrochemical results and preliminary calculations with density functional theory, one possible mechanistic route is proposed in which the oxygen evolution occurs from a peroxide intermediate formed between the oxidized flavin pseudobase and the oxidized carbon electrode. These findings offer an organic alternative to the traditional water-oxidation catalysts based on transition metals.
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