Despite the promising previous reports on the development of electrocatalytic dithiolene-based metal-organic frameworks (MOFs) for the hydrogen evolution reaction (HER), these materials often display poor reproducibility of the HER performance, owing to their poor bulk properties upon integration with electrode materials. We demonstrate here an in-depth investigation of the electrocatalytic HER activity of a cobalt 2,3,6,7,10,11-triphenylenehexathiolate (CoTHT) MOF. To enhance the durability and charge transport properties of the constructed CoTHT/electrode architecture, two properties that hinder the understanding of the intrinsic HER activity of MOF-based electrocatalysts, CoTHT is deposited as an ink composite (1). We leverage here the well-established use of catalyst inks in the literature to increase adhesion of the catalyst to the electrode surface and to improve the overall electronic conductivity of the integrated catalyst/electrode. The utilization of the composite 1 leads to a huge improvement in the HER activity. Density functional theory (DFT) calculations were also applied to understand the mechanistic pathways of the HER for CoTHT for the first time.

Improving and understanding the hydrogen evolving activity of a cobalt dithiolene metal-organic framework

2019 Fall National Meeting

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