MnO₂ is one of the most studied cathodes for aqueous neutral zinc‐ion batteries. However, the diverse reported crystal structures of MnO₂ compared to δ‐MnO₂ inevitably suffer a structural phase transition from tunneled to layered Zn‐buserite during the initial cycles, which is not as kinetically direct as the conventional intercalation electrochemistry in layered materials and thus poses great challenges to the performance and multifunctionality of devices. Here, a binder‐free δ‐MnO₂ cathode is designed and a favorable “layered to layered” Zn²⁺ storage mechanism is revealed systematically using such a “noninterferencing” electrode platform in combination with ab initio calculation. A flexible quasi‐solid‐state Zn–Mn battery with an electrodeposited flexible Zn anode is further assembled, exhibiting high energy density (35.11 mWh cm⁻³; 432.05 Wh kg⁻¹), high power density (676.92 mW cm⁻³; 8.33 kW kg⁻¹), extremely low self‐discharge rate, and ultralong stability up to 10 000 cycles. Even with a relatively high δ‐MnO₂ mass loading of 5 mg cm⁻², significant energy and power densities are still achieved. The device also works well over a broad temperature range (0–40 °C) and can efficiently power different types of small electronics. This work provides an opportunity to develop high‐performance multivalent‐ion batteries via the design of a kinetically favorable host structure.

中文翻译：

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揭示δ-MnO2“层对层”储锌机制对性能优越的中性锌锰电池的无干扰作用

MnO ₂是水性中性锌离子电池研究最多的阴极之一。然而，与δ-MnO _{2相比，报道的MnO 2}晶体结构多种多样，在初始循环过程中不可避免地会经历从隧道状到层状Zn-布塞尔矿的结构相变，这在动力学上不像层状材料中的传统插层电化学那么直接，因此对设备的性能和多功能性提出了巨大的挑战。在此，设计了一种无粘合剂的δ-MnO ₂阴极，并利用这种“非干扰”电极平台结合从头计算，系统地揭示了有利的“层状到层状”Zn ^{2+存储机制。}进一步组装了具有电沉积柔性锌阳极的柔性准固态锌锰电池，表现出高能量密度（35.11 mWh cm ^-3；432.05 Wh kg ^-1）、高功率密度（676.92 mW cm ^-3；8.33 kW kg ⁻¹ )、极低的自放电率以及高达 10 000 次循环的超长稳定性。即使具有相对较高的 δ-MnO ₂质量负载（5 mg cm ^{-2 ）}，仍然可以获得显着的能量和功率密度。该器件还可以在较宽的温度范围（0–40 °C）下正常工作，并且可以高效地为不同类型的小型电子产品供电。这项工作提供了通过设计动力学有利的主体结构来开发高性能多价离子电池的机会。