Unveiling the Interface Structure of the Exsolved Co–Fe Alloy Nanoparticles from Double Perovskite and Its Application in Solid Oxide Fuel Cells

Exsolution of catalytic nanoparticles (NPs) from perovskites has arisen as a flexible method to develop high-performance functional materials with enhanced durability for energy conversion and catalytic synthesis applications. Here, we unravel the interface structure of the <i>in situ</i> exsolved alloy nanoparticles from the double perovskite substrate on the atomic scale. The results show that the Co-Fe alloy NPs exsolved topologically from the {100} facets terminations of the Sr₂FeMo_0.65Co_0.35O_6-δ (SFMC) double perovskite along ⟨100⟩ directions exhibiting the same orientation and identical crystal structure. The lattice planes of these two phases align and insert into each other at the interface, forming a smooth and continuous coherent connection. The presence of moiré patterns at the interface confirms the topological exsolution mechanism. The coherent interface can significantly reduce the interfacial energy and therefore stabilize the exsolved nanoparticles. Therefore, excellent and stable electrochemical performance of the NP-decorated SFMC perovskite is observed as the anode for solid oxide fuel cells. Our contribution promotes a fundamental understanding of the interface structure of the <i>in situ</i> exsolved alloy nanoparticles from perovskite substrate.