Interfacial Designing of MnO2 Half‐Wrapped by Aromatic Polymers for High‐Performance Aqueous Zinc‐Ion Batteries

Abstract Due to the excellent specific capacity and high working voltage, manganese oxide (MnO 2 ) has attracted considerable attention for aqueous zinc‐ion batteries (AZIBs). However, the irreversible structural collapse and sluggish ionic diffusion lead to poor rate capability and inferior lifespan. Herein, we proposed a novel organic/inorganic hybrid cathode of carbon‐based poly(4,4′‐oxybisbenzenamine)/MnO 2 (denoted as C@PODA/MnO 2 ) for AZIBs. Various in/ex situ analyses and theoretical calculations prove that PODA chains with C=N groups can provide a more active surface/interface for ion/electron mobility and zinc ion storage in the hybrid cathode. More importantly, newly formed Mn−N interfacial bonds can effectively promote ion diffusion and prevent Mn atoms dissolution, enhancing redox kinetics and structural integrity of MnO 2 . Accordingly, C@PODA/MnO 2 cathode exhibits high capacity (321 mAh g −1 or 1.7 mAh cm −2 at 0.1 A g −1 ), superior rate performance (88 mAh g −1 at 10 A g −1 ) and excellent cycling stability over 2000 cycles. Hence, rational interfacial designs shed light on the development of organic/inorganic cathodes for advanced AZIBs.