The development of new molecular abiotic catalysts is often inspired by highly active biological systems. Mimicry of these catalysts is most commonly achieved by the choice of metal center and ligand type, which can enable the enforcement of specific structural geometries in the primary coordination sphere. Another contributing factor to the efficiency of these processes in natural systems, however, is the ability of biologically based macromolecular structures to exclude solvent from the active site and direct the flow of reactants and products. For this reason, there is interest in studying how the incorporation of molecular catalysts into supramolecular structures can be used to optimize a reaction. By incorporating bioinspired functional groups in the secondary sphere of molecular electrocatalysts for the reduction of CO<sub>2</sub> it is possible to interrogate the effects of non-covalent supramolecular assembly on well-defined molecular species. Electrochemical and spectroelectrochemical measurements can be utilized to extract information on the kinetic and thermodynamic parameters of these reactions, elucidating important mechanistic details. The use of hydrogen bonding and other driving forces for molecular assembly of abiotic catalysts promises to be a powerful way to alter catalytic mechanisms and potentially enhance catalyst properties, independent of more typical approaches that rely on unimolecular steric and electronic effects.

Improving the efficiency of electrocatalysts for the reduction of CO<sub>2</sub> through supramolecular assembly with amino acid-modified ligands

251st National Meeting (2016)

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Improving the efficiency of electrocatalysts for the reduction of CO2 through supramolecular assembly with amino acid-modified ligands

Improving the efficiency of electrocatalysts for the reduction of CO₂ through supramolecular assembly with amino acid-modified ligands