Kinetic and thermodynamic aspects of the electrocatalysis of acid reduction in organic solvent using molecular diiron-dithiolate compounds
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- 作者：Fran莽ois Quentel ; Frederic Gloaguen
- 关键词：Hydrogen production ; Hydrogenase model ; Molecular electrocatalyst ; Overpotential ; Turnover frequency
- 刊名：Electrochimica Acta
- 出版年：1 November, 2013
- 年：2013
- 卷：110
- 期：Complete
- 页码：641-645
- 全文大小：994 K
文摘
In an attempt to obtain molecular H2 production electrocatalysts achieving balanced basicity and reduction potential, we focused on the mono-substituted diiron-dithiolate derivative [Fe2(渭-bdt)(CO)5(P(OMe)3)] (bdt = benzenedithiolate). The electrocatalytic efficiency of this iron-iron hydrogenase model was determined by cyclic voltammetry in acetonitrile using p-toluenesulfonic acid as a proton source. Detailed analysis of the current - potential responses and comparison with the all-CO diiron-dithiolate parent compound clearly show that the effect of the chemical properties on the electrocatalytic efficiency is not fully determined by the turnover frequency under pseudo-first-order approximation and the overpotential defined as the difference between the reduction potential of the electrocatalysts in the absence of acid and the reversible potential of the couple H2/acid.