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It is shown that producing PrBaCo 2 O 5+δ  and Ba 0.5 Sr 0.5 Co 0.8 Fe 0.2 O 2+δ  nanoparticle by a scalable synthesis method leads to high mass activities for the oxygen evolution reaction (OER) with outstanding improvements by 10× and 50×, respectively, compared to those prepared via the state‐of‐the‐art synthesis method. Here, detailed comparisons at both laboratory and industrial scales show that Ba 0.5 Sr 0.5 Co 0.8 Fe 0.2 O 2+δ  appears to be the most active and stable perovskite catalyst under alkaline conditions, while PrBaCo 2 O 5+δ  reveals thermodynamic instability described by the density‐functional theory based Pourbaix diagrams highlighting cation dissolution under OER conditions.  Operando  X‐ray absorption spectroscopy is used in parallel to monitor electronic and structural changes of the catalysts during OER. The exceptional BSCF functional stability can be correlated to its thermodynamic meta‐stability under OER conditions as highlighted by Pourbaix diagram analysis. BSCF is able to dynamically self‐reconstruct its surface, leading to formation of Co‐based oxy(hydroxide) layers while retaining its structural stability. Differently, PBCO demonstrates a high initial OER activity while it undergoes a degradation process considering its thermodynamic instability under OER conditions as anticipated by its Pourbaix diagram. Overall, this work demonstrates a synergetic approach of using both experimental and theoretical studies to understand the behavior of perovskite catalysts.

advanced functional materials

Highly Active Nanoperovskite Catalysts for Oxygen Evolution Reaction: Insights into Activity and Stability of Ba 0.5 Sr 0.5 Co 0.8 Fe 0.2 O 2+δ  and PrBaCo 2 O 5+δ