(465f) First Principles Quantum Chemistry Calculations to Model CO2 Electroreduction on SnO2 Particles

Electrochemical conversion of CO₂ has drawn much attention due to the urgent need to address rising CO₂ levels in the atmosphere. Electrochemical CO₂ reduction is known on Sn electrodes, but a recent study by Bocarsly and coworkers has implicated a Sn-oxide overlayer as being the active catalysis. We have investigated this system using quantum chemistry methods to understand the adsorption mechanism of CO₂ on the most stable SnO₂ surface (110). To determine the effect of oxygen concentration on the adsorption process; stoichiometric, reduced and oxidized surfaces are also investigated. We plot Pourbaix diagrams to identify relevant thermodynamic states that catalyzes the CO₂ reduction by identifying the most stable and energetically efficient electrochemical reaction conditions. We hypothesize the structures identified by using Pourbaix diagrams will be experimentally relevant structures for the CO₂ catalysis.