A promising solution to the challenge of storing intermittently produced energy from renewable sources is its conversion to chemical energy in the form of molecular hydrogen, generating a clean-burning, carbon-neutral fuel. However, finding affordable and efficient electrocatalysts for hydrogen production using inexpensive electrodes such as carbon-based ones remains a challenge. Nature accomplishes the reduction of protons to H<sub>2</sub> in anaerobic bacteria with a class of hydrogenase enzymes, the most active of which feature active sites with earth-abundant, inexpensive elements forming [2Fe-2S] clusters. Small molecule mimetics of these hydrogenase active sites have yielded impressive catalytic rates for hydrogen production but are typically not water-soluble and often have short catalyst lifetimes due to deactivation pathways and oxygen sensitivity. Using rational design derived from the mechanistic pitfalls of small molecule mimetics, we have integrated [2Fe-2S] cores into polymer systems to get polymer-supported single site electrocatalysts (metallopolymers) which we have shown to inhibit deactivation processes and increase oxygen stability. By varying the monomers used in the polymer composition, these novel metallopolymer catalysts can be tuned to have a variety of attributes such as water solubility and built-in sites for proton transport, which can grant the catalysts exceptional catalytic rates with low energy requirement.

Synthetic [2Fe2S] biomimietics in metallopolymers as hydrogen evolution electrocatalysts

2019 Fall National Meeting

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