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Electrochemical hydrogen production in aqueous micellar solution by a diiron benzenedithiolate complex relevant to [FeFe] hydrogenases

Abstract : The diiron hydrogenase model Fe2(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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https://hal.univ-brest.fr/hal-01559120
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Submitted on : Monday, July 10, 2017 - 2:09:08 PM
Last modification on : Wednesday, September 11, 2019 - 2:14:07 PM

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François Quentel, Guillaume Passard, Frederic Gloaguen. Electrochemical hydrogen production in aqueous micellar solution by a diiron benzenedithiolate complex relevant to [FeFe] hydrogenases. Energy & Environmental Science, Royal Society of Chemistry, 2012, 5 (7), ⟨10.1039/C2EE21531D⟩. ⟨hal-01559120⟩

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