Jahn–Teller Distortion Induced Mn(2+)‐Rich Cathode Enables Optimal Flexible Aqueous High‐Voltage Zn‐Mn Batteries

Although one of the most promising aqueous batteries, all Zn‐Mn systems suffer from Zn dendrites and the low‐capacity Mn(4+)/Mn(3+) process (readily leading to the occurrence of Jahn–Teller distortion, which in turn causes structural collapse and voltage/capacity fading). Here, the Mn(3+) reconstruction and disproportionation are exploited to prepare the stable, Mn(2+)‐rich manganese oxides on carbon‐cloth (CMOs) in a discharged state through an inverted design, which promotes reversible Mn(2+)/Mn(4+) kinetics and mitigates oxygen‐related redox activity. Such a 1.65 V Mn(2+)‐rich cathode enable constructing a 2.2 V Zn‐Mn battery, providing a high area capacity of 4.16 mA h cm(–2) (25 mA h cm(–2) for 10 mL electrolyte) and superior 4000‐cycle stability. Moreover, a flexible hybrid 2.7 V Zn‐Mn battery is constructed using 2‐pH hydrogel electrolytes to demonstrate excellent practicality and stability. A further insight has been gained to the commercial application of aqueous energy storage devices toward low‐cost, high safety, and excellent energy density.