Hydrogen gas production, already more than a 250 billion dollar industry, is only predicted to grow as hydrogen fuel takes more of a center stage in the shift towards renewable energy resources. Electrocatalysts with the ability to produce H2 at low cost using renewable resources are desirable. A series of aromatically bridged synthetic analogues of the enzymatic active site of [FeFe]-hydrogenase have been synthesized and characterized. In the present work, (2,3-thiophenedithiolato)Fe2(CO)6 and (3,4-thiophenedithiolato)Fe2(CO)6 are compared with the well-known complex (1,2-benzenedithiolato)Fe2(CO)6. Each analogue shows catalytic activity several orders of magnitude above the enzyme. Additionally, these isomers of the thiophene system show potential in tuning the overpotential and significantly increase the rate of catalysis. Density functional theory was used to investigate the catalytic mechanism and define the key relationship between these results with the aromaticity and asymmetric nature of the bridging ligands.

Electrocatalytic hydrogen production via aromatically bridged butterfly [2Fe-2S] clusters

2019 Spring National Meeting

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