Hydrogen gas is in high demand, primarily due to its role in the production of ammonia. Current means of hydrogen production involve carbon-rich sources which generate ten times the amount of carbon dioxide for hydrogen that is produced. Due to environmental concerns, alternative means of hydrogen production must be developed. The butterfly [2Fe-2S] active sites of diiron-hydrogenase enzymes efficiently reduce protons to hydrogen gas, prompting research into biologically inspired catalysts designed for hydrogen production. A series of bridging [2Fe-2S] catalysts were synthesized and characterized. Using weak acid as the proton source in an organic solvent, observed rate constants were measured to be greater than 1 x 106 s-1. Density functional theory was employed to compute reduction potentials, pKa values, and Gibbs free energies leading to the proposed catalytic mechanisms. Kinetic analysis comparisons were conducted between this series and the μ-1,2-benzenedithiolate system. Electrochemical simulations are consistent with the conclusions drawn.

Electrocatalytic hydrogen production by bridged butterfly [2Fe-2S] catalysts

255th National Meeting (2018)

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