Catalyst modified metal organic frameworks (MOFs) have been shown to carry out a wide variety of catalytic transformations. In this paper, we present a detailed study of a ruthenium terpyridine bipyridine aquo catalyst modified UiO-67-type MOF for the electrochemical oxidation of water. The inherently insulating framework was found to transmit charge via a redox hopping process. The concentration of electrochemically addressable catalysts was dependent on catalyst loading, while the rate of hopping remained constant at ~10-9 cm2/s. The MOF was competent at water oxidation with a rate constant on par with the homogeneous catalyst. Additionally, the stability of the catalyst was greatly enhanced, and the MOF could be recycled at least 3 times without loss in activity. Follow-up experiments indicate that the catalysis occurs throughout the MOF particles and is not confined to the surface. Ultimately, the catalyst operated at a rate 100 times that of a monolayer of the same catalysts on an electrochemical support. Design parameters for next-generation MOF water oxidation catalysts will be presented.

Metal organic frameworks for electrocatalytic water oxidation

2019 Spring National Meeting

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