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Membrane-Modified Metal Triazole Complexes for the Electrocatalytic Reduction of Oxygen and Carbon Dioxide
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In this manuscript, an electrochemical architecture is designed that controls the kinetics of proton transfer to metal triazole complexes for electrocatalytic O-2 and CO2 reduction. Self-assembled monolayers of these catalysts are attached to a glassy carbon electrode and covered with a lipid monolayer containing proton carriers, which acts as a proton-permeable membrane. The O-2 reduction voltammograms on carbon are similar to those obtained on membrane-modified Au electrodes, which through the control of proton transfer rates, can be used to improve the selectivity of O-2 reduction. The improved voltage stability of the carbon platforms allows for the investigation of a CO2 reduction catalyst inside a membrane. By controlling proton transfer kinetics across the lipid membrane, it is found that the relative rates of H-2, CO, and HCOOH production can be modulated. It is envisioned that the use of these membrane-modified carbon electrodes will aid in understanding catalytic reactions involving the transfer of multiple protons and electrons.