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- Title
Electrode-assisted catalytic water oxidation by a flavin derivative.
- Authors
Mirzakulova, Ekaterina; Khatmullin, Renat; Walpita, Janitha; Corrigan, Thomas; Vargas-Barbosa, Nella M.; Vyas, Shubham; Oottikkal, Shameema; Manzer, Samuel F.; Hadad, Christopher M.; Glusac, Ksenija D.
- Abstract
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 +1.9 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.
- Subjects
OXIDATION; FLAVINS; ELECTROLYSIS; ELECTRODES; CATALYSIS; DENSITY functionals
- Publication
Nature Chemistry, 2012, Vol 4, Issue 10, p794
- ISSN
1755-4330
- Publication type
Article
- DOI
10.1038/nchem.1439