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The High Performance of Crystal Water Containing Manganese Birnessite Cathodes for Magnesium Batteries

机译：镁电池用锰水钠锰矿型结晶水的高性能

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Rechargeable magnesium batteries have lately received great attention for large-scale energy storage systems due to their high volumetric capacities, low materials cost, and safe characteristic. However, the bivalency of Mg2+ ions has made it challenging to find cathode materials operating at high voltages with decent (de)intercalation kinetics. In an effort to overcome this challenge, we adopt an unconventional approach of engaging crystal water in the layered structure of Birnessite MnO2 because the crystal water can effectively screen electrostatic interactions between Mg2+ ions and the host anions. The crucial role of the crystal water was revealed by directly visualizing its presence and dynamic rearrangement using scanning transmission electron microscopy (STEM). Moreover, the importance of lowering desolvation energy penalty at the cathodeelectrolyte interface was elucidated by working with water containing nonaqueous electrolytes. In aqueous electrolytes, the decreased interfacial energy penalty by hydration of Mg2+ allows Birnessite MnO2 to achieve a large reversible capacity (231.1 mAh g(-1)) at high operating voltage (2.8 V vs Mg/Mg2+) with excellent cycle life (62.5% retention after 10000 cycles), unveiling the importance of effective charge shielding in the host and facile Mg2+ ions transfer through the cathodes interface.
机译：可充电镁电池由于其高容量，低材料成本和安全特性，最近在大型储能系统中引起了广泛关注。但是，Mg2 +离子的双价性使寻找具有良好（de）嵌入动力学的高压材料成为挑战。为了克服这一挑战，我们采用一种非常规方法将结晶水结合到Birnessite MnO2的层状结构中，因为结晶水可以有效地筛选Mg2 +离子与主体阴离子之间的静电相互作用。通过使用扫描透射电子显微镜（STEM）直接可视化结晶水的存在和动态重排，揭示了结晶水的关键作用。此外，通过使用含有非水电解质的水可以阐明降低阴极电解质界面上的脱溶剂能损失的重要性。在水性电解质中，因水合Mg2 +而降低的界面能损失使Birnessite MnO2在高工作电压（2.8 V vs Mg / Mg2 +）下具有出色的循环寿命（62.5％），可实现大的可逆容量（231.1 mAh g（-1））。 10000次循环后的保留时间），揭示了有效的电荷屏蔽在主体中以及通过阴极界面进行便捷的Mg2 +离子转移的重要性。

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