There is great interest in the development of cheaper alternatives to platinum catalyst for the production of hydrogen, a clean alternative to fossil fuels. Current focus is on iron-based organometallic catalysts designed to mimic the structure and function of the active site of the efficient hydrogen producing [Fe-Fe] hydrogenase enzyme. Hundreds of these models, with varying catalytic efficiency and stability, have been reported in the literature. The hydrogenase models are known to decompose upon reduction following breakage of the Fe-S bond. To explore the effect of structural features on the electrochemical stability of these models, we have prepared and characterized a series of diiron-carbonyl compounds coupled to polyaromatic thiolate ligands. The structures of the compounds have been examined using X-ray crystallography and spectroscopy (IR, UV-visible and NMR). The stability and catalytic activity of the compounds have been explored using cyclic voltammetry and the results will be presented. Global reactivity indices of the models have been determined using density functional theory and used to predict the relative stability of the catalysts.

[Fe-Fe] hydrogenase models: Computational and electrocatalytic studies

247th National Meeting (2014)

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