Journal
ENERGY & ENVIRONMENTAL SCIENCE
Volume 5, Issue 7, Pages 7757-7761Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c2ee21531d
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Funding
- Agence Nationale de la Recherche (ANR)
- Centre Nationale de la Recherche Scientifique (CNRS)
- Universite de Bretagne Occidentale
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The diiron hydrogenase model Fe-2(bdt)(CO)(6) (1, bdt = benzenedithiolate) was dispersed in an aqueous micellar solution prepared from sodium dodecyl sulfate (SDS). The aqueous solution of 1 showed no sign of decomposition when left in contact with air over a period of several days. Current-potential responses recorded at a dropping mercury electrode over pH 7-3 were consistent with reduction of freely diffusing species. Catalysis of proton reduction was observed at pH < 6 with current densities exceeding 0.5 mA cm(-2) at an acid-to-catalyst ratio of 17. Bulk electrolysis at -0.66 V vs. SHE of a solution of 1 at pH 3 confirmed the production of hydrogen with Faradaic efficiency close to 100%. A mechanism involving initial reduction of 1 and subsequent proton-coupled electron transfer is proposed.
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