A viable catalyst is needed for cleaner and more sustainable production of molecular hydrogen in the current industry and to allow for the possibility of a hydrogen fuel economy in the future. Worldwide interest has taken inspiration from biological diiron-hydrogenase enzymes, and many mimics of the [2Fe-2S] active site of the enzyme have been studied as possible catalysts for the efficient reduction of protons to molecular hydrogen. Once thought to be necessary for the catalyst stability and function, the majority of these mimics display a linker between sulfur atoms of the [2Fe-2S] cluster. Deviating from the structure of the hydrogenase active site, we have found that a class of [2Fe-2S] cluster-based catalysts notable for the lack of a bridging group between the sulfur atoms exhibit impressively high rates for the electrocatalytic production of hydrogen at reasonable overpotential. One such catalyst, [(μ–methylthiolato)(μ–2-thiophenethiolato)Fe2(CO)6], gives an observed rate constant for the electrocatalytic production of molecular hydrogen greater than 106 mol-1 s-1.

Butterfly [2Fe-2S] cluster-based electrocatalysts with fast rates for hydrogen production

253rd National Meeting (2017)

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