Atomically Thin Mesoporous Co3O4 Layers Strongly Coupled with N‐rGO Nanosheets as High‐Performance Bifunctional Catalysts for 1D Knittable Zinc–Air Batteries

Abstract Under development for next‐generation wearable electronics are flexible, knittable, and wearable energy‐storage devices with high energy density that can be integrated into textiles. Herein, knittable fiber‐shaped zinc–air batteries with high volumetric energy density (36.1 mWh cm −3 ) are fabricated via a facile and continuous method with low‐cost materials. Furthermore, a high‐yield method is developed to prepare the key component of the fiber‐shaped zinc–air battery, i.e., a bifunctional catalyst composed of atomically thin layer‐by‐layer mesoporous Co 3 O 4 /nitrogen‐doped reduced graphene oxide (N‐rGO) nanosheets. Benefiting from the high surface area, mesoporous structure, and strong synergetic effect between the Co 3 O 4 and N‐rGO nanosheets, the bifunctional catalyst exhibits high activity and superior durability for oxygen reduction and evolution reactions. Compared to a fiber‐shaped zinc–air battery using state‐of‐the‐art Pt/C + RuO 2 catalysts, the battery based on these Co 3 O 4 /N‐rGO nanosheets demonstrates enhanced and stable electrochemical performance, even under severe deformation. Such batteries, for the first time, can be successfully knitted into clothes without short circuits under external forces and can power various electronic devices and even charge a cellphone.