Unveiling the Intricate Intercalation Mechanism in Manganese Sesquioxide as Positive Electrode in Aqueous Zn-Metal Battery,Advanced Energy Materials

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Unveiling the Intricate Intercalation Mechanism in Manganese Sesquioxide as Positive Electrode in Aqueous Zn-Metal Battery
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2021-07-28 , DOI: 10.1002/aenm.202100962
Yuan Ma _{1,

2} , Yanjiao Ma _{1,

2} , Thomas Diemant ₃ , Kecheng Cao ₄ , Xu Liu _{1,

2} , Ute Kaiser ₄ , R. Jürgen Behm _{1,

3} , Alberto Varzi _{1,

2} , Stefano Passerini _{1,

2}

Affiliation

In the family of Zn/manganese oxide batteries with mild aqueous electrolytes, cubic α-Mn₂O₃ with bixbyite structure is rarely considered, because of the lack of the tunnel and/or layered structure that are usually believed to be indispensable for the incorporation of Zn ions. In this work, the charge storage mechanism of α-Mn₂O₃ is systematically and comprehensively investigated. It is demonstrated that the electrochemically induced irreversible phase transition from α-Mn₂O₃ to layered-typed L-Zn_xMnO₂, coupled with the dissolution of Mn²⁺ and OH⁻ into the electrolyte, allows for the subsequent reversible de-/intercalation of Zn²⁺. Moreover, it is proven that α-Mn₂O₃ is not a host for H⁺. Instead, the MnO₂ formed from L-Zn_xMnO₂ and the Mn²⁺ in the electrolyte upon the initial charge is the host for H⁺. Based on this electrode mechanism, combined with fabricating hierarchically structured mesoporous α-Mn₂O₃ microrod array material, an unprecedented rate capability with 103 mAh g⁻¹ at 5.0 A g⁻¹ as well as an appealing stability of 2000 cycles (at 2.0 A g⁻¹) with a capacity decay of only ≈0.009% per-cycle are obtained.

中文翻译：

揭示三氧化二锰作为水系锌金属电池正极的复杂插层机制

在具有温和水性电解质的锌/锰氧化物电池系列中，很少考虑具有方铁锰矿结构的立方 α-Mn ₂ O ₃，因为缺乏通常被认为是掺入必不可少的隧道和/或层状结构锌离子。在这项工作中，系统全面地研究了α-Mn ₂ O ₃的电荷存储机制。结果表明，电化学诱导的从α-Mn ₂ O ₃到层状L-Zn _x MnO _{2 的}不可逆相变，以及Mn ²⁺和OH ^-的溶解。进入电解质，允许随后可逆的 Zn ²⁺脱/嵌入。此外，已证明α-Mn ₂ O ₃不是H ⁺的主体。相反，在初始充电时由 L-Zn _x MnO ₂和电解液中的 Mn ²⁺形成的 MnO ₂是 H ⁺的主体。基于这种电极机制，结合制备分层结构的介孔 α-Mn ₂ O _{3 微}棒阵列材料，在 5.0 A g ^{-1 下}具有 103 mAh g ^-1的前所未有的倍率能力以及 2000 次循环（在 2.0 A g ^{-1 下}）的吸引人的稳定性，每个循环的容量衰减仅为 ≈0.009%。

更新日期：2021-09-16

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