Abstract

Benefiting from the remarkable advantages (eco-friendly, cost-effective, and high safety) of rechargeable aqueous zinc-ion batteries (AZIBs), AZIBs are regarded as viable alternatives to traditional Lithium-ion batteries (LIBs). However, in prevailing research, the excellent electrochemical performance usually achieved by ultra-low active material loadings (e.g., <1 mg/cm²), which is far from the active material mass loading of commercial electrodes in practical (≥10 mg/cm²). Balancing superior properties with high mass loading has posed a challenge. To surmount this, an innovative method combined ultrasonic processing, freeze-drying, and 3D printing technologies is used to engineer a high MnO2 mass loading cathode for AZIBs (3D cathode). Notably, the grid structure of 3D cathode substantially augmenting the surface area for redox reactions during charge/discharge processes, which greatly enhanced the pseudo-capacitance process of cathode. Additionally, the uniform and stable microstructure exhibited the dual capability of expediting ion/electron transfer and sustaining the structural integrity throughout charge/discharge cycles. Consequently, the 3D cathode demonstrated superior comprehensive electrochemical properties at the MnO2 high mass loading of 10 mg/cm2 (138.7 mAh/g at 1 A/g, 87.4 mAh/g after 500 cycles, 82 % energy efficiency) and 15 mg/cm2 (113.3 mAh/g at 1 A/g, 56.3 mAh/g after 400 cycles, 81 % energy efficiency).

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