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The development of a high specific capacity and stable manganese (Mn)-based cathode material is very attractive for aqueous zinc-ion (Zn2+) batteries (ZIBs). However, the inherent low electrical conductivity and volume expansion challenges limit its stability improvement. Here, a mesoporous ZnMn2O4 (ZMO) nanocage (N-ZMO) coupled with nitrogen doping and oxygen vacancies is prepared by defect engineering and rational structural design as a high-performance cathode material for rechargeable ZIBs. The oxygen vacancies enhance the electrical conductivity of the material and the nitrogen doping releases the strong electrostatic force of the material to maintain a higher structural stability. Interestingly, N-ZMO exhibits excellent ability of Zn2+ storage (225.4 mAh·g−1 at 0.3 A·g−1), good rate, and stable cycling performance (88.4 mAh·g−1 after 1,000 cycles at 3 A·g−1). Furthermore, a flexible quasi-solid-state device with high energy density (261.6 Wh·kg−1) is assembled, demonstrating long-lasting durability. We believe that the strategy in this study can provide a new approach for developing aqueous ZIBs.
We gratefully acknowledge the financial support of the National Natural Science Foundation of China (Nos. 51702369 and 51873233), Innovation group of National Ethanic Affairs Commission of China (No. MZR20006), Key R&D Plan of Hubei Province (No. 2020BAB077), and the Fundamental Research Funds for the Central Universities (Nos. CZZ21009 and CZP20006).