基于室温离子液体和深共晶溶剂的超高分子量 PEO 凝胶电解质的离子电导率增强,ACS Applied Polymer Materials

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基于室温离子液体和深共晶溶剂的超高分子量 PEO 凝胶电解质的离子电导率增强
ACS Applied Polymer Materials ( IF 4.4 ) Pub Date : 2022-03-25 , DOI: 10.1021/acsapm.2c00104
Víctor Gregorio ₁ , Nuria García ₁ , Pilar Tiemblo ₁

Affiliation

由聚（环氧乙烷）（PEO）和低共熔溶剂脲-锂双（三氟甲磺酰）亚胺（TFSI）和乙二醇/LiTFSI或吡咯烷离子液体溶液PYR13TFSI-LiTFSI和PYR14TFSI-LiTFSI制成的物理凝胶是通过以下方法制备的快速、单步工艺，不涉及辅助溶剂或中间体，具有可重复性和可扩展性。这些凝胶的性质作为 PEO 含量及其分子量和液体电解质性质的函数进行了研究。用低浓度（1-5 wt%）的超高分子量（UHMW）PEO 制备的凝胶是坚韧、可拉伸的材料，类似于柔软的弹性体，并且具有自愈性和透明性。它们的流变学表现出物理聚合物凝胶的常规行为，因此 PEO 的分子量越高，生产凝胶所需的聚合物浓度越低。然而，凝胶的离子电导率和扩散率是惊人的，在许多情况下等于或显着高于纯液体电解质。这种离子电导率增强对于具有最高分子量的最低 PEO 浓度是最高的。这种前所未有的分子量对电导率和扩散率的依赖性是两个综合效应的结果：添加 PEO 导致的液体电解质化学结构改变和弹性网络的发展，其中当添加 PEO 时离子迁移率和流变学不耦合超高分子量的。在许多情况下等于或显着高于纯液体电解质。这种离子电导率增强对于具有最高分子量的最低 PEO 浓度是最高的。这种前所未有的分子量对电导率和扩散率的依赖性是两个综合效应的结果：添加 PEO 导致的液体电解质化学结构改变和弹性网络的发展，其中当添加 PEO 时离子迁移率和流变学不耦合超高分子量的。在许多情况下等于或显着高于纯液体电解质。这种离子电导率增强对于具有最高分子量的最低 PEO 浓度是最高的。这种前所未有的分子量对电导率和扩散率的依赖性是两个综合效应的结果：添加 PEO 导致的液体电解质化学结构改变和弹性网络的发展，其中当添加 PEO 时离子迁移率和流变学不耦合超高分子量的。

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Ionic Conductivity Enhancement in UHMW PEO Gel Electrolytes Based on Room-Temperature Ionic Liquids and Deep Eutectic Solvents

Physical gels made of poly(ethylene oxide) (PEO) and deep eutectic solvents urea-Li bis(trifluoromethanesulfonyl)imide (TFSI) and ethylene glycol/LiTFSI, or pyrrolidinium ionic liquid solutions PYR13TFSI-LiTFSI and PYR14TFSI-LiTFSI, are prepared by a fast, single-step process, which involves no auxiliary solvents or intermediates and is reproducible and scalable. The properties of these gels are studied as a function of the PEO content and its molecular weight and the nature of the liquid electrolyte. The gels prepared with a low concentration (1–5 wt %) of ultrahigh molecular weight (UHMW) PEO are tough, stretchable materials which resemble soft elastomers and are also self-healing and transparent. Their rheology shows the conventional behavior of physical polymer gels, so that the higher the molecular weight of PEO, the lower the polymer concentration needed to produce the gel. However, the ion conductivities and diffusivities of the gels are striking, in many cases being equal to or significantly higher than those of pure liquid electrolytes. This ion conductivity enhancement is the highest for the lowest PEO concentration with the highest molecular weight. This unprecedented molecular weight dependence of conductivity and diffusivity is the result of two combined effects: the liquid electrolyte chemical structure modification as a consequence of the addition of PEO and the development of elastic networks, where ion mobility and rheology are uncoupled when the PEO added is of UHMW.

更新日期：2022-03-25

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