Pt3Ni Alloy Nanoparticle Electro‐Catalysts with Unique Core‐Shell Structure on Oxygen‐Deficient Layered Perovskite for Solid Oxide Cells

Abstract Solid oxide cells (SOCs) are pivotal in electrochemical energy conversion technologies, but their operation at high temperatures necessitates the development of efficient and durable electro‐catalysts. Herein, a novel electro‐catalyst composed of Pt 3 Ni alloy nanoparticles exsolved on oxygen‐deficient PrBaMn 1.8 Pt 0.15 Ni 0.05 O 5+δ layered perovskite oxides is presented. This design addresses the critical problem of nanoparticle agglomeration at high temperatures, a major hurdle for SOCs. The atomic‐scale mechanisms of oxygen vacancy formation and hydrogen evolution reaction kinetics in the material are unraveled through density functional theory calculations. A unique finding of this work is the formation of a core‐shell structure during water electrolysis, simultaneously enhancing the electrochemical performance and operational durability in both fuel cell and electrolysis cell modes. This study not only strengthens the potential of Pt‐Ni alloy nanoparticles as efficient electro‐catalysts for SOCs, but also opens up avenues for future exploration in energy‐related fields.