(66d) Electrochemistry with Oxygen: Activity, Stability, and New Design Principles for the Next Generation of Electrocatalysis

The oxygen electrochemistry necessarily evolves around metal-oxides and their derivatives, since they are the most stable catalysts where the oxygen is both the building block and also the intermediate of a reaction. From this perspective, the activity of an electrocatalyst, i.e. its surface properties, cannot be separated from its operational/electrochemical stability, i.e its bulk properties. In my talk, I will highlight our efforts to understand this link both computationally and experimentally from the observed surface transformation in atomically flat LaNiO3 thin films for enhanced water electrolysis [1]. Next, I will discuss our efforts to control these properties via ion insertion from the electrolyte in the MnOx polymorphs for bifunctional oxygen reduction and oxygen evolution reaction. Bulk polymorphic search is increasingly important for the discovery of new types of stable and active catalysts, and I will show how an Active Machine Learning method can be applied to search a bulk-oxide prototype space [2]. Finally, I will show how newly developed design rules in metal-oxides can be applied to create a single-atom oxygen-evolution electrocatalyst with a breakthrough performance [3].

[1] Baeumer, C.; Li, J.; Lu, Q.; Liang, Bajdich, Chueh; et al. Tuning Electrochemially Driven Surface Transformation in Atomically Flat LaNiO<inf>3</Inf> Thin Films for Enhanced Water Electrolysis. Nat. Mater. 2021.

[2] Flores, R. A.; Paolucci, C.; Winther, K. T.; Nørskov, J. K.; Bajdich, M.; Bligaard, T. Active Learning Accelerated Discovery of Stable Iridium-Oxide Polymorphs for the Oxygen Evolution Reaction. Chem. Mater. 2020, acs.chemmater.0c01894.

[3] Zheng, X.; Tang, J.; Gallo, A.; Garrido Torres, Jose, A.; Bajdich, M.; Cui, Y. et.al. Origin of Enhanced Water Oxidation Activity in an Iridium Single Atom Catalyst. PNAS in review.