Ion Transport in Glyme‐ and Sulfolane‐Based Highly Concentrated Electrolytes
Ion Transport in Glyme‐ and Sulfolane‐Based Highly Concentrated Electrolytes
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DOI：
10.1002/tcr.202200301
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发表时间：
2023-02
期刊：
影响因子：
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通讯作者：
Keisuke Shigenobu;Taku Sudoh;J. Murai;Kaoru Dokko;M. Watanabe;K. Ueno
中科院分区：
文献类型：
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作者：
Keisuke Shigenobu;Taku Sudoh;J. Murai;Kaoru Dokko;M. Watanabe;K. Ueno
高浓度电解质(HCE)在高离子性质上与离子液体(ILS)有相似之处，确实有一些HECS的行为类似于ILS。氢化物作为未来锂二次电池电解液材料的潜在候选者，由于其良好的体相和电化学界面上的性能，引起了人们极大的关注。在这项研究中，我们重点讨论了溶剂、反阴离子和稀释剂对锂离子配位结构和输运性质的影响(例如，在阴离子封闭条件下测得的离子电导率和表观锂离子迁移数tLiabc${{t}{{rm L}{\rm i}}^{{rm a}{\rm b}{\rm c})。我们对动态离子关联的研究揭示了HCE中离子传导机制的不同及其与tLiabc${{t}{{\rM L}{\rM i}}{{\rMa}{\rmb}{\rmc}$值的密切关系。我们对高价锂离子输运性质的系统分析还表明，需要在同时获得高离子电导率和高tLiabc${{t}{{\rM L}{\rMi}}{{\rMa}{\rmb}{\rmc}}$值之间进行折衷。
Highly concentrated electrolytes (HCEs) have a similarity to ionic liquids (ILs) in high ionic nature, and indeed some of HECs are found to behave like an IL. HCEs have attracted considerable attention as prospective candidates for electrolyte materials in future lithium secondary batteries owing to their favorable properties both in the bulk and at the electrochemical interface. In this study, we highlight the effects of the solvent, counter anion, and diluent of HCEs on the Li+ ion coordination structure and transport properties (e. g., ionic conductivity and apparent Li+ ion transference number measured under anion‐blocking conditions, tLiabc ${{t}_{{\rm L}{\rm i}}^{{\rm a}{\rm b}{\rm c}}}$ ). Our studies on dynamic ion correlations unveiled the difference in the ion conduction mechanisms in HCEs and their intimate relevance to tLiabc ${{t}_{{\rm L}{\rm i}}^{{\rm a}{\rm b}{\rm c}}}$ values. Our systematic analysis of the transport properties of HCEs also suggests the need for a compromise to simultaneously achieve high ionic conductivity and high tLiabc ${{t}_{{\rm L}{\rm i}}^{{\rm a}{\rm b}{\rm c}}}$ values.