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The slow Zn2+ intercalation/deintercalation kinetics in cathodes severely limits the electrochemical performance of aqueous zinc-ion batteries (ZIBs). Herein, we demonstrate a new kind of coordinately unsaturated manganese-based metal–organic framework (MOF) as an advanced cathode for ZIBs. Coordination unsaturation of Mn is performed with oxygen atoms of two adjacent −COO–. Its proper unsaturated coordination degree guarantees the high-efficiency Zn2+ transport and electron exchange, thereby ensuring high intrinsic activity and fast electrochemical reaction kinetics during repeated charging/discharging processes. Consequently, this MOF-based electrode possesses a high capacity of 138 mAh g–1 at 100 mA g–1 and a long life span (93.5% capacity retention after 1000 cycles at 3000 mA g–1) due to the above advantages. Such distinct Zn2+ ion storage performance surpasses those of most of the recently reported MOF cathodes. This concept of adjusting the coordination degree to tune the energy storage capability provides new avenues for exploring high-performance MOF cathodes in aqueous ZIBs.

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