The growing interest in renewable energy has focused considerable attention on artificial photosynthesis for the conversion of solar energy into value-added products. However, challenges remain in identifying effective catalysts for the CO2 reduction reaction. Current homogeneous electrocatalysts require very high overpotentials, and exhibit low current densities while being susceptible to poisoning by the intermediates and/or products. Here, we employ density functional theory calculations to study the mechanism for the selective conversion of CO2 to CO using {Re[bpyMe(ImMe)](CO)3Cl}+ in the presence of H2O as a proton source. Our results suggest that the imidazolium group in the secondary coordination sphere stabilizes the Re-CO2 adduct through hydrogen bond interactions, as well as facilitates a hydrogen-bonding network that enables proton transfer from H2O to CO2.

Computational modeling of rhenium electrocatalysts featuring charged functional groups in the secondary coordination sphere for CO2 reduction

256th National Meeting (2018)

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