Noncovalent Immobilization of Electrocatalysts on Carbon Electrodes for Fuel Production

Abstract

We show that molecular catalysts for fuel-forming reactions can be immobilized on graphitic carbon electrode surfaces via noncovalent interactions. A pyrene-appended bipyridine ligand (P) serves as the linker between each complex and the surface. Immobilization of a rhodium proton-reduction catalyst, [Cp*Rh(P)Cl]Cl (1), and a rhenium CO_2-reduction catalyst, Re(P)(CO)_3Cl (2), afford electrocatalytically active assemblies. X-ray photoelectron spectroscopy and electrochemistry confirm catalyst immobilization. Reduction of 1 in the presence of p-toluenesulfonic acid results in catalytic H_2 production, while reduction of 2 in the presence of CO_2 results in catalytic CO production.

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