Event

Molecular Electrocatalysis for Fuel Production with Surface-Immobilized Metal Complexes

Abstract

Assembling systems for the conversion and storage of solar photons as chemical fuels (i.e., artificial photosynthesis) requires the development of strategies for the functionalization of electrode surfaces with catalysts. However, studying molecular reactivity on electrode surfaces remains challenging since immobilization methods are often not general; many methods are harsh and reduce the lifetime of molecular catalysts.

Our work has focused on immobilization of molecular catalysts for fuel-forming reactions on carbon electrode surfaces via noncovalent interactions. The general approach relies on a pyrene-appended bipyridine ligand (P) that serves as the linker between the catalysts and the surface. In our initial work, we have immobilized and compared the activity of a rhodium proton-reduction catalyst, [Cp*Rh(P)Cl]Cl (Cp* is pentamethylcyclopentadienyl), and a rhenium CO2-reduction catalyst, Re(P)(CO)3Cl.

Results on these immobilized molecular catalysts will be discussed, as well as more recent work examining the activity of related systems with earth-abundant first-row transition metals.