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A Binuclear Iron–Thiolate Catalyst for Electrochemical Hydrogen Production in Aqueous Micellar Solution
Author(s) -
Quentel François,
Passard Guillaume,
Gloaguen Frederic
Publication year - 2012
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201201884
Subject(s) - chemistry , catalysis , inorganic chemistry , electrochemistry , aqueous solution , electrolysis , hydrogen production , protonation , acetic acid , hydrogen , reaction rate constant , faraday efficiency , electrocatalyst , electrode , kinetics , organic chemistry , electrolyte , ion , physics , quantum mechanics
The substituted iron–thiolate complex [Fe 2 (μ‐bdt)(CO) 4 {P(OMe) 3 } 2 ] (bdt=benzenedithiolate) is an active catalyst for electrochemical hydrogen production in aqueous sodium dodecyl sulfate solution, with a high apparent rate constant of 4×10 6 M −1 s −1 . The half‐peak potential for catalysis of proton reduction is less negative than −0.6 V versus the standard hydrogen electrode at pH 3. Voltammetric data are consistent with the rate of electrode reaction controlled by diffusion. A mechanism that begins with the rapid protonation of the iron–thiolate catalyst is proposed. The Faradaic efficiency in diluted HCl solutions is close to 100 %, but the catalytic activity decayed after about twelve turnovers when electrolysis was carried out in the presence of acetic acid.