(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.