Molecular hydrogen (H2) is an energy-dense alternative to fossil fuels. When generated by the reduction of aqueous protons, the production and combustion of hydrogen are carbon-free. Biomolecules are attractive scaffolds for the engineering of water-soluble catalysts for aqueous proton reduction. One example is cobalt-substituted microperoxidase-11 (CoMP11-Ac), with a turnover number > 20,000 in neutral water in the presence of air [Kleingardner et al., J. Am. Chem. Soc., 2014  , 136, 4-7]. CoMP11-Ac, however, suffers from poor stability during electrocatalysis, sensitivity to impurities in solution, and a high overpotential. To prepare a more robust version of this catalyst, variants with a protected active site have been engineered. This approach also allows second-sphere interactions with the active site to be introduced to lower overpotential. Progress on these efforts as well as the development of novel metallopeptide catalysts will be described.

Metalloprotein and metallopeptide catalysts for hydrogen evolution from neutral water

248th National Meeting (2014)

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