Detrimental MnPO4F and MnF2 formation on LiMn2O4 in the 3 V region,Journal of Materials Chemistry A

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Detrimental MnPO4F and MnF2 formation on LiMn2O4 in the 3 V region
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2021-10-02 , DOI: 10.1039/d1ta06227a
Louis L. De Taeye _{1,

2} , Philippe M. Vereecken _{1,

2}

Affiliation

In this work, we studied the electrochemistry of LMO using thin-film electrodes in LiClO₄ and LiPF₆ based electrolyte solutions. The thin-film system allows the removal of all passive components, leaving only the LMO with a single well-defined electrode/electrolyte interface, making it an ideal system to study interactions at this interface. We observed a peculiar decomposition reaction when using a LiPF₆ salt based electrolyte solution, as soon as the LMO electrode was discharged below 3 V. This decomposition reaction led to the formation of a highly ionically resistive interphase layer, greatly affecting the insertion kinetics into the active material. This was in stark contrast to the LiClO₄ based electrolyte solutions, which showed ideal insertion behaviour. Through the combination of elastic recoil detection analysis (ERDA) and X-ray photoelectron spectroscopy (XPS) we determined that the reaction stems from a direct interaction between the LiPF₆ salt and tetragonal Li₂Mn₂O₄.

中文翻译：

在 3 V 区域的 LiMn2O4 上形成有害的 MnPO4F 和 MnF2

在这项工作中，我们在基于LiClO ₄和 LiPF ₆的电解质溶液中使用薄膜电极研究了 LMO 的电化学。薄膜系统允许去除所有无源元件，只留下 LMO 具有单个明确定义的电极/电解质界面，使其成为研究该界面相互作用的理想系统。当使用 LiPF ₆盐基电解质溶液时，我们观察到一种特殊的分解反应，一旦 LMO 电极放电至低于 3 V。这种分解反应导致形成高离子电阻界面层，极大地影响插入动力学活性物质。这与 LiClO ₄形成鲜明对比基于电解质溶液，表现出理想的插入行为。通过弹性反冲检测分析 (ERDA) 和 X 射线光电子能谱 (XPS) 的组合，我们确定反应源于 LiPF ₆盐和四方 Li ₂ Mn ₂ O ₄之间的直接相互作用。

更新日期：2021-10-12

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