Aqueous rechargeable Zn/birnessite batteries have recently attracted extensive attention for energy storage system because of their low cost and high safety. However, the reaction mechanism of the birnessite cathode in aqueous electrolytes and the cathode structure degradation mechanics still remain elusive and controversial. In this work, it is found that solvation water molecules coordinated to Zn²⁺ are coinserted into birnessite lattice structure contributing to Zn²⁺ diffusion. However, the birnessite will suffer from hydroxylation and Mn dissolution with too much solvated water coinsertion. Through engineering Zn²⁺ primary solvation sheath with strong‐field ligand in aqueous electrolyte, highly reversible [Zn(H₂O)₂]²⁺ complex intercalation/extraction into/from birnessite cathode is obtained. Cathode–electrolyte interface suppressing the Mn dissolution also forms. The Zn metal anode also shows high reversibility without formation of “death‐zinc” and detrimental dendrite. A full cell coupled with birnessite cathode and Zn metal anode delivers a discharge capacity of 270 mAh g⁻¹, a high energy density of 280 Wh kg⁻¹ (based on total mass of cathode and anode active materials), and capacity retention of 90% over 5000 cycles.

中文翻译：

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通过可逆水和Zn2 +共插入的高能量，长寿命的Zn /水钠锰矿水电池。

水性可再充电锌/水钠锰矿电池由于其低成本和高安全性而近来已引起能量存储系统的广泛关注。但是，钠水钠锰矿阴极在水性电解质中的反应机理和阴极结构的降解机理仍然难以捉摸和存在争议。在这项工作中，发现与Zn ²⁺配位的溶剂化水分子共聚成水钠锰矿晶格结构，这有助于Zn ²⁺扩散。但是，水钠锰矿过多的溶剂化水会使水钠锰矿遭受羟基化和锰溶解。通过在水电解质中工程化具有强场配体的Zn ²⁺初级溶剂化鞘，可高度逆转的[Zn（H ₂ O）₂得到²⁺络合物插层/从水钠锰矿阴极中萃取/萃取。也可以形成抑制Mn溶解的阴极-电解质界面。锌金属阳极还显示出高可逆性，而不会形成“死亡锌”和有害枝晶。结合水钠锰矿阴极和Zn金属阳极的全电池可提供270 mAh g ^-1的放电容量，280 Wh kg ^-1的高能量密度（基于阴极和阳极活性材料的总质量）以及90的容量保持率5000次循环中的％。