Enhanced Li+ Conduction within Single-Ion Conducting Polymer Gel Electrolytes via Reduced Cation–Polymer Interaction,ACS Materials Letters

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Enhanced Li+ Conduction within Single-Ion Conducting Polymer Gel Electrolytes via Reduced Cation–Polymer Interaction
ACS Materials Letters ( IF 9.6 ) Pub Date : 2020-02-17 , DOI: 10.1021/acsmaterialslett.9b00510
Hunter O. Ford ₁ , Bumjun Park ₁ , Jizhou Jiang ₁ , Morgan E. Seidler ₁ , Jennifer L. Schaefer ₁

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The development of advanced electrolytes compatible with lithium metal and lithium-ion batteries is crucial for meeting ever growing energy storage demands. One such class of materials, single-ion conducting polymer electrolytes (SIPEs), prevents the formation of ion concentration gradients and buildup of anions at the electrode surface, improving performance. One of the ongoing challenges for SIPEs is the development of materials that are conductive enough to compete with liquid electrolytes. Presented herein is a class of gel SIPEs based on crosslinked poly(tetrahydrofuran) diacrylate that present enhanced room temperature conductivities of 3.5 × 10^–5 S/cm when gelled with lithium metal relevant 1,3-dioxolane/dimethoxyethane, 2.5 × 10^–4 S/cm with carbonate solutions, and approaching 10^–3 S/cm with dimethyl sulfoxide. Remarkably, these materials also demonstrate high ionic conductivity at low temperatures, 1.8 × 10^–5 S/cm at −20 °C in certain solvents. Most importantly, however, when contrasted with identical SIPEs formulated with poly(ethylene glycol) diacrylate, the mechanisms responsible for the enhanced conductivity are elucidated: decreasing Li⁺–polymer interactions and gel solvent–polymer interactions leads to an increase in Li⁺ mobility. These findings are generalizable to various SIPE chemistries and can therefore be seen as an additional set of design parameters for developing future high conductivity SIPEs.

中文翻译：

通过减少阳离子-聚合物相互作用，增强单离子导电聚合物凝胶电解质中的Li ⁺导电性

与锂金属和锂离子电池兼容的先进电解质的开发对于满足不断增长的储能需求至关重要。一种这样的材料，单离子导电聚合物电解质（SIPE），可以防止离子浓度梯度的形成和阴离子在电极表面的堆积，从而提高性能。SIPE的持续挑战之一是开发具有足够导电性以与液体电解质竞争的材料。本文介绍的是一类基于交联聚四氢呋喃二丙烯酸酯的凝胶SIPE，当与锂金属相关的1,3-二氧戊环/二甲氧基乙烷，2.5×10 ^-4凝胶化时，其室温电导率提高到3.5×10 ^–5 S / cm。碳酸盐溶液的S / cm，二甲亚砜接近10 ^–3 S / cm。值得注意的是，这些材料在低温下还表现出高离子电导率，在某些溶剂中，在-20°C下为1.8×10 ^–5 S / cm。然而，最重要的是，当与用聚乙二醇二丙烯酸酯配制的相同SIPE进行对比时，阐明了导致电导率提高的机理：降低Li ⁺ -聚合物相互作用和凝胶溶剂-聚合物相互作用导致Li ⁺迁移率增加。这些发现可推广到各种SIPE化学领域，因此可以看作是开发未来高电导率SIPE的另一组设计参数。

更新日期：2020-02-18

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