The marriage of renewable electricity with the reductive conversion of carbon dioxide is an attractive strategy for energy storage and liquid fuel production. An intriguing strategy in this regard is the reduction of CO2 to CO, which generates an energy rich commodity chemical for the production of synthetic petroleum. A number of heterogeneous cathode materials can facilitate the electrocatalytic conversion of CO2 to CO, however historically, only noble metals such as Ag and Au had been shown to catalyze this reaction with Faradaic Efficiencies (FEs) in excess of 80% at ambient pressures.Although these precious metal cathodes can be efficient platforms for electrolytic production of CO, the exorbitant cost of these materials has precluded their use on the scale required for alternative fuel synthesis. Against this backdrop, we developed a bismuth-based Carbon Monoxide Evolving Catalyst (Bi-CMEC) that can be formed upon cathodic polarization of an inexpensive carbon or metallic electrode in acidic solutions containing Bi3+ ions. This catalyst drives the electrolytic conversion of CO2 to CO with a FE over 90% and with high current density at low overpotential. The ability of Bi-CMEC to drive production of CO from carbon dioxide is on par with that which has historically only been observed using expensive silver and gold cathodes. In addition to developing new inexpensive platforms for CO2 reduction, we have also worked to elucidate the molecular design principles that enable efficient CO2 activation at low overpotentials. Interrogation of the pathway by which Bi-CMEC and other catalysts activate CO2 has revealed the primary factors that drive fuel generation. Implications for the future development of efficient cost-effective architectures that can promote CO2 reduction with high selectivity and efficiency will be discussed.

Poor metal cathode materials for the efficient conversion of carbon dioxide to fuels

248th National Meeting (2014)

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