Noncovalent Immobilization of Electrocatalysts on Carbon Electrodes for Fuel Production

作者:Blakemore James D; Gupta Ayush; Warren Jeffrey J; Brunschwig Bruce S*; Gray Harry B
来源:Journal of the American Chemical Society, 2013, 135(49): 18288-18291.
DOI:10.1021/ja4099609

摘要

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 CO2-reduction catalyst, Re(P)(CO)(3)Cl (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 CO2 results in catalytic CO production.

  • 出版日期2013-12-11

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