Abstract
Electrochemical reduction of carbon dioxide can yield valuable chemicals, energy carriers, and renewable fuels that serve as storage forms of renewable energy. This transformation can be achieved using molecular catalysts immobilized on conductive (or semi-conductive) surfaces. A prerequisite for achieving control over CO2 reduction is a detailed understanding of proton-coupled electron transfer (PCET) mechanisms in such adsorbed systems. Using Fe and Co complexes, we have demonstrated that CO2 can undergo 2-, 4-, or 6-electron reductions to afford CO, formaldehyde, and methanol, respectively, and we have elucidated the underlying mechanisms. Building on these insights, polyoxygenated compounds such as sugars can be synthesized via a one-pot, two-step electro-organocatalytic strategy. Our latest investigations will be presented.
