Synergistic Vertical Graphene‐Exsolved Perovskite to Boost Reaction Kinetics for Flexible Zinc–Air Batteries

Abstract Zinc–air batteries (ZABs) hold significant promise for flexible electronics due to their high energy density and low cost. However, their practical application is hindered by the sluggish kinetics of the oxygen evolution and oxygen reduction reactions (OER/ORR). This study highlights a novel design of vertical graphene arrays (VGs) anchored on PrBa_0.5Sr_0.5Co_1.8Ru_0.2O_5+δ (PBSCRu) perovskite nanofibers, fabricated via plasma‐enhanced chemical vapor deposition. Notably, the VG growth induces the exsolution of Co nanoparticles from the PBSCRu perovskite, resulting in a unique PBSCRu‐Co‐VG heterostructure. Theoretical calculations demonstrate that constructing PBSCRu‐Co‐VG heterojunction regulates interfacial electronic redistribution, thereby lowering energy barriers for both OER and ORR. As a result, the PBSCRu@VG‐5 electrocatalyst exhibits superior stability and higher peak power density in both liquid and flexible solid‐state ZABs compared to the pristine PBSCRu electrocatalyst. This protocol advances the integration of synergetic perovskite/metal/graphene composites, offering considerable potential for next‐generation energy conversion technologies.