We will discuss recent progress in interrogating (electro)chemical reaction mechanisms of electrochemical ozone production on doped tin oxide considering insights from computational theory and experiment. This collaborative work is motivated to elucidate fundamental atomic scale reaction mechanisms that consist of steps where ozone is generated from a) traditional water oxidation steps on the catalyst surface, b) lattice oxygen steps where surface oxygen atoms are depleted and then regenerated from water solvent, and c) steps involving solvated radicals in solution. We carried out computational modeling of tin oxide surfaces using Kohn-Sham density functional theory, the computational hydrogen electrode model, and ab initio thermodynamics approaches to show the most salient intermediate states for this six-electron oxidation process. We highlight the critical role of hydrogenated species on the surface that stabilize these structures. We also reflect on our prior work that reported energies of solvated reaction intermediates, and explain these results alongside data that assess the feasibility of hypothetical lattice oxygen mechanims. Insight from computational modeling will then be summarized alongside independent experimental work that includes results using different solvents and kinetic isotope effect studies. In sum, we will present a thorough assessment of complex electrochemical ozone pathways that can operate via multiple competitive pathways.

Computational and experimental investigations into electrochemical ozone production on doped tin oxides

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