Biologically Inspired Catalytic Systems for Solar-to-Fuel Technologies

Research in the Marinescu group focuses on the development of novel catalytic systems for efficient solar-to-fuel technologies. Inspired by biological systems, we design molecular catalysts that involve hydrogen bonding networks capable of small molecule activation through multiple proton and electron transfers. We have shown that cobalt complexes with pendant secondary amine (NH) moieties act as highly efficient electrocatalysts for the reduction of CO2 to CO, and the proposed mechanism involves the formation of a hydrogen-bonding network intermediate that enables direct proton transfer from acid to the activated CO2 substrate. In addition to CO2 reduction, we also developed catalytic systems for the conversion of water into H2, such as the dithiolene-based coordination complexes and polymers that display remarkable electrocatalytic activity for the hydrogen evolution reaction (HER). We have also shown that cobalt phosphinothiolate complexes catalyze the electrochemical reduction of CO2 to formate with excellent selectivity. Additionally, we have also explored the immobilization of well-known CO2-reduction catalysts, such as metal porphyrins or rhenium bipyridine tricarbonyl moieties, via incorporation into covalent-organic frameworks or via covalent attachment through robust diazonium reductive coupling. We expect the design principles discovered in these studies to have a profound impact towards the development of advanced materials and sustainable technologies. 

Biography