Decoupling of ion pairing and ion conduction in ultrahigh-concentration electrolytes enables wide-temperature solid-state batteries,Energy & Environmental Science

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Decoupling of ion pairing and ion conduction in ultrahigh-concentration electrolytes enables wide-temperature solid-state batteries
Energy & Environmental Science ( IF 32.4 ) Pub Date : 2022-06-23 , DOI: 10.1039/d2ee01053d
Shengjun Xu _{1,

2} , Ruogu Xu _{1,

2} , Tong Yu ₁ , Ke Chen _{1,

3} , Chengguo Sun _{1,

4} , Guangjian Hu ₁ , Shuo Bai _{1,

2} , Hui-Ming Cheng _{1,

5} , Zhenhua Sun _{1,

2} , Feng Li _{1,

2}

Affiliation

Fast ion conduction and stable interfaces are predicted to be important in the development of new electrolytes. However, many unconventional solvents for electrolytes remain challenging, although they are fast ion carriers, because of the narrow voltage window of solvent oxidation and reduction. Here, we report a general solidified localized high-concentration electrolyte (S-LHCE) strategy with the decoupling of ion pairing and ion conduction to achieve the application of unstable solvents (dimethyl sulfoxide, DMSO) in high-voltage lithium-metal batteries. By decoupling electrolytes with a non-solvating solid framework, the interfacial compatibility was further improved with lithium anodes and high-voltage cathodes. The anion migration was limited with a high Li⁺ transference number of 0.72, and the lithium-ion conduction was enhanced (0.27 mS cm⁻¹ at 20 °C) by the regulated solvation structure in an ultrahigh salt concentration regime. The S-LHCE strategy enabled solid-state lithium-metal batteries with excellent electrochemical performance over a wide temperature range from −10 to 100 °C and with 83.3% and 60.1% capacity retention of the theoretical capacity when cycled at a 30C rate and a 50C rate at an evaluated temperature. The results in this work provide new insight for the application of potential but unconventional active components to high-performance electrolytes.

中文翻译：

超高浓度电解质中离子对和离子传导的去耦可实现宽温固态电池

预计快速离子传导和稳定的界面在新电解质的开发中很重要。然而，许多用于电解质的非常规溶剂仍然具有挑战性，尽管它们是快离子载体，因为溶剂氧化和还原的电压窗口很窄。在这里，我们报告了一种通用的固化局部高浓度电解质（S-LHCE）策略，通过离子对和离子传导的去耦来实现不稳定溶剂（二甲基亚砜，DMSO）在高压锂金属电池中的应用。通过将电解质与非溶剂化固体框架解耦，进一步提高了锂负极和高压正极的界面相容性。阴离子迁移受限于高 Li ⁺转移数为 0.72，并且在超高盐浓度范围内通过调节的溶剂化结构增强了锂离子传导（在 20 °C 时为 0.27 mS cm ^{-1 ）。}S-LHCE 策略使固态锂金属电池在 -10 至 100 °C 的宽温度范围内具有出色的电化学性能，并且在以 30C 速率循环和在评估温度下的 50C 速率。这项工作的结果为将潜在但非常规的活性成分应用于高性能电解质提供了新的见解。

更新日期：2022-06-23

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