(15f) Mechanistic Insight into Water Oxidation to Ozone on Rutile Sno2 (110) with Computational Chemistry

Ozone is a powerful oxidant that has promise as a sustainable sanitizing agent. Electrochemical ozone production (EOP) processes are schematically simple, but existing EOP catalysts are also generally very inefficient by having high anodic overpotentials of 1 V or more above the standard oxidation potential. The present work shows our progress in computationally modeling the atomic scale EOP reaction mechanism on the rutile SnO₂(110) surface. A complicating factor is that elementary steps for EOP are believed to take place both on electrode surfaces as well as in solution phase within the double layer as homogeneous reactions. To understand the thermodynamic and kinetic feasibility of (electro-)chemical reaction steps on and off of the electrode surface, we use Kohn-Sham density functional theory (DFT) in combination with solvation modeling. Adsorbate binding energies and reaction pathways with transition states will be discussed in the context of understanding how to engineer higher efficiencies with these reactions via doping. Results obtained from computational modeling will be critically presented alongside experimental data to validate and assess latest progress toward improved EOP catalysts.