Assembling systems for the conversion of solar light energy into chemical fuels (i.e., artificial photosynthesis) requires the development of strategies for functionalization of electrode surfaces with catalysts. We have demonstrated that molecular catalysts for fuel-forming reactions can be immobilized on graphitic carbon electrode surfaces via noncovalent interactions. Our general approach relies on a pyrene-appended bipyridine ligand that serves as the linker between the catalysts and the surface. Immobilization of a rhodium proton-reduction catalyst and a rhenium CO2-reduction catalyst afford electrocatalytically active assemblies. X-ray photoelectron spectroscopy and electrochemical studies confirm catalyst immobilization. Reduction of the rhodium system in the presence of p-toluenesulfonic acid results in catalytic H2 production, while reduction of the rhenium system in the presence of CO2 results in catalytic CO production.

Noncovalent immobilization of electrocatalysts for fuel production on carbon electrodes

248th National Meeting (2014)

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