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The synthesis, structure, photophysics, and spectroscopic characterization of an organometallic rhenium multichromophore compound carrying a central 2,2′-bipyridyl acceptor moiety with additional phenylethynyl substituents conjugated at the 4,4′-positions of the acceptor ligands and its effect on the electron density of the central rhenium atom as metal center for CO reduction is reported. The results were compared to -(2,2′-bipyridyl)Re(CO)Cl and -(5,5′-bisphenylethynyl-2,2′-bipyridyl)Re(CO)Cl. Cyclovoltammetric studies and rotating disk electrochemistry were performed for electrochemical characterization. Ultraviolet and visible (UV-vis) absorption, Fourier transform infrared (FTIR), and luminescence measurements were carried out for a spectroscopic characterization and compared to theoretical calculations at the density functional theory (DFT) level. In addition, the rhenium complex -(4,4′-bisphenyl-ethynyl-2,2′-bipyridyl)-Re(CO)Cl was used as a novel catalyst for the electrochemical reduction of CO in homogeneous solution. Results showed an 11-fold increase in the current density under CO saturation and a catalytic second-order rate constant for CO formation of about 560 M s on a Pt working electrode. For further characterization of the CO reduction capabilities, bulk controlled potential electrolysis experiments were performed using a CO-saturated acetonitrile electrolyte solution. The headspace product gas analysis yields CO as main reduction product with faradaic efficiencies of about 12 % over 5-h electrolysis time.

electrocatalysis

Using the Alkynyl-Substituted Rhenium(I) Complex (4,4′-Bisphenyl-Ethynyl-2,2′-Bipyridyl)Re(CO)3Cl as Catalyst for CO2 Reduction—Synthesis, Characterization, and Application