Self-organization of nano catalysts, particularly nanoparticle exsolution under operational conditions, has significantly enhanced energy conversion, including catalytic reactions, electrolyzers, fuel cells, and SOERs. Exsolved metal or alloy nanoparticles (e.g., Ni, Fe, Pd, Pt, and Co) primarily form under reducing conditions characterized by limited oxygen availability from solid and gas phases. However, this presents challenges for olefin synthesis because oxygen species are crucial for oxidizing alkanes into olefins while minimizing carbon deposition at the anode. The self-organization of core-shell catalysts has been explored in SOERs for water splitting 5 and CO2 reduction 29 (Table ), owing to their easy access to oxygen species and the unique electronic structure resulting from the synergy between the core and shell. However, their application in the oxidative dehydrogenation of propane remains unexamined. Furthermore, the lack of information regarding reaction intermediates and insufficient understanding of defect evolution from surface to bulk in heterostructure catalysts hinders the development of more efficient and stable catalytic systems.