Catalytic CO2/CO Reduction: Gas, Aqueous, and Aprotic Phases

The catalytic reduction of CO2/CO is key to reducing the carbon footprint and producing the chemical building blocks needed for society. In this work, we performed a theoretical investigation of the differences and similarities of the CO2/CO catalytic reduction reactions in gas, aqueous solution, and aprotic solution. We demonstrate that the binding energy serves as a good descriptor for the gaseous and aqueous phases and allows catalysts to be categorized by reduction products. The CO* vs O* and CO* vs H* binding energies for these phases give a convenient mapping of catalysts regarding their main product for the CO2/CO reduction reactions. However, for the aprotic phase, descriptors alone are insufficient for the mapping. We show that a microkinetic model (including the CO* and H* binding energies) allows spanning and interpreting the reaction space for the aprotic phase.

Automated summary

This work investigates the theoretical differences and similarities of CO2/CO catalytic reduction reactions in gas, aqueous solution, and aprotic solution. The binding energy serves as a good descriptor for the gaseous and aqueous phases and allows catalysts to be categorized by reduction products. However, descriptors alone are insufficient for mapping in the aprotic phase, requiring the use of a microkinetic model.