Active Poly(o-phenylenediamine)-Intercalated Layered δ-MnO2 Cathode for High-Performance Aqueous Zinc-Ion Batteries

Aqueous zinc-ion batteries (ZIBs) represent an emerging energy storage solution that offers significant advantages in terms of safety, cost-effectiveness, and longevity in cycling. Among the various materials available, manganese-based oxides stand out as the most promising options for cathodes due to their impressive theoretical specific capacity, suitable operating voltage, and abundant natural availability. In published reports, pre-embedding is frequently used to modify the layered cathode; however, non-electrochemically active molecular embedding often results in a decrease in battery capacity. In this paper, a hydrothermal method is employed to intercalate poly(o-phenylenediamine) (PoPD) into δ-MnO₂ (MO) to produce PoPD-MO cathode materials. Here, PoPD serves a dual role in the cathode: (1) PoPD is inserted into the interlayer of MO, providing support within the intercalation layer, enhancing material stability, increasing ionic storage sites, and creating space for more Zn²⁺ to be embedded, and (2) inserting PoPD into the interlayer structure of MO effectively expands the space between layers, thus allowing for greater ion storage, which in turn enhances the rate and efficiency of electrochemical reactions. Consequently, PoPD-MO shows remarkable cycling durability and adaptability in ZIBs, achieving a specific capacity of 359 mAh g^-1 at a current density of 0.1 A g^-1, and even under the strain of a high current density of 3 A g^-1, it maintains a respectable capacity of 107 mAh g^-1. Based on this, PoPD-MO may emerge as a new cathode material with promising applications in the future.