The intermittency of solar and wind power has prompted investigations into efficient methods for long-term energy storage in chemical fuels and for on-demand release. One promising avenue for the latter is through the use of fuel cells; however, current technologies typically utilize hydrogen as the fuel, which is challenging to store and transport and has a low volumetric energy density, even at high pressures. Carbon-based liquid fuels, such as formate and methanol, have shown significant promise as fuels as they are much easier to handle, are relatively energy dense, and can be produced from the direct hydrogenation or electrochemical reduction of CO2 using renewable energy sources. However, there is a dearth of molecular electrocatalysts for the oxidation of methanol and formate, with most examples based on precious metals and/or high energy metal-oxo species. The only known first-row transition metal catalysts capable of formate oxidation is a Ni-based system; however, its reactivity towards methanol was not reported and a closely related system was not active for methanol oxidation.1 Notably, these Ni complexes contain pendent amines on the ligand backbone, which likely participate in the mechanism of formate oxidation. In our efforts, we have synthesized and characterized a series of Co compounds featuring pendent amine ligands as electrocatalysts for the oxidation of formate and alcohols. Significantly, we find that these complexes are able to oxidize formate via a CoIII-hydride intermediate.

Exploration of cobalt catalysts for the electro-oxidation of liquid fuels

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.