Towards advanced aqueous zinc battery by exploiting synergistic effects between crystalline phosphide and amorphous...

High-performance aqueous zinc batteries are expected to be realized, rooting from component synergistic effects of the hierarchical composite electrode materials. Herein, hierarchical crystalline Ni-Co phosphide coated with amorphous phosphate nanoarrays (C-NiCoP@A-NiCoPO₄) self-supporting on the Ni foam are constructed as cathode material of an aqueous zinc battery. In this unique core-shell structure, the hexagonal phosphide with high conductivity offers ultra-fast electronic transmission and amorphous phosphate with high stability, and open-framework provides more favorable ion diffusivity and a stable protective barrier. The synergistic effects of this intriguing core-shell structure endow the electrode material with outstanding reaction kinetics and structural stability, which is theoretically confirmed by density functional theory (DFT) calculations. As a result, the C-NiCoP@A-NiCoPO₄ electrode exhibits a higher specific capacity of 350.6 mA h g^-1 and excellent cyclic stability with 92.6% retention after 10 000 cycles. Moreover, the C-NiCoP@A-NiCoPO₄ is coupled with Zn anode to assemble an aqueous pouch battery that delivers ultra-high energy density (626.33 W h kg^-1 at 1.72 kW kg^-1) with extraordinary rate performance (452.05 W h kg^-1 at 33.56 kW kg^-1). Moreover, the corresponding quasi-solid flexible battery with polyacrylamide hydrogel electrolyte exhibits favorable durability under frequent mechanical strains, which indicates the great promise of crystalline/amorphous hierarchical electrodes in the field of energy storage.