The
solar-driven conversion of CO2 to value-added products
provides a promising route for solar energy storage and atmospheric
CO2 remediation. In this report, a variety of supporting
electrode materials were successfully modified with a [2,2′-bipyridine]-5,5′-bis(diazonium)
rhenium complex through a surface-localized electropolymerization
method. Physical characterization of the resulting multilayer films
confirms that the coordination environments of the rhenium bipyridine
tricarbonyl sites are preserved upon immobilization and that the polymerized
catalyst moieties exhibit long-range structural order with uniform
film growth. UV–vis studies reveal additional absorption bands
in the visible region for the polymeric films that are not present
in the analogous rhenium bipyridine complexes. Electrochemical studies
with modified graphite rod electrodes show that the electrocatalytic
activity of these films increases with catalyst loading up to an optimal
value, beyond which electron and mass transport through the material
become rate-limiting. Electrocatalytic studies performed at −2.25
V vs Fc/Fc+ for 2 h reveal CO production with faradaic
efficiencies and turnover numbers up to 99% and 3606, respectively.
Photocatalytic studies of the modified TiO2 devices demonstrate
enhanced activity at low catalyst loadings, with turnover numbers
up to 70 during 5 h of irradiation.
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