Competing effects of low salt ratio on electrochemical performance and compressive modulus of PEO-LiTFSI/LLZTO composite electrolytes†

IF 3.2 Q2 CHEMISTRY, PHYSICAL
Energy advances Pub Date : 2024-10-03 DOI:10.1039/D4YA00467A
Jiaxin Zhang, Valeria Perez, ThomasJae Garcia, Dan-il Yoon, David Wagner, Yanika Schneider, Min Hwan Lee, Sang-Joon John Lee and Dahyun Oh
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Abstract

Polyethylene oxide (PEO)-based solid composite electrolytes (SCEs), with inorganic fillers, are studied extensively due to their effective balance between mechanical and electrochemical properties. The correlation between the composition of SCEs and their electrochemical behavior has been studied extensively, primarily focusing on the type of polymer matrix with a bias towards high lithium (Li) salt. In this study, we examine the changes in the properties of SCEs at two low EO : Li ratios, 43 : 1 and 18 : 1, in the PEO-LiTFSI matrix (with and without 10 wt% of 5 μm LLZTO) and evaluate their impact on Li stripping and plating reactions. Although higher salt concentration (18 : 1) results in substantially higher ionic conductivity (by approximately an order of magnitude), interestingly we observe that lower salt concentration (43 : 1) exhibits up to 3 times longer Li cycling life. Notably, electrolytes with low salt concentration (43 : 1) are much stiffer, with compressive modulus more than twice as high as the 18 : 1 counterpart. Although the ionic conductivity of the electrolyte is often the most immediate concern in the electrolyte design process, these findings accentuate the equal importance of mechanical properties in order to ensure successful electrolyte performance throughout prolonged Li cycling.

Abstract Image

低盐比对 PEO-LiTFSI/LLZTO 复合电解质电化学性能和压缩模量的竞争效应†。
含有无机填料的聚环氧乙烷(PEO)基固体复合电解质(SCE)因其机械性能和电化学性能之间的有效平衡而被广泛研究。人们对 SCE 的成分与其电化学行为之间的相关性进行了广泛的研究,主要集中在聚合物基体的类型上,并偏向于高锂(Li)盐。在本研究中,我们考察了两种低 EO :锂比率(43 :1 和 18 :1 的 PEO-LiTFSI 基体中 SCE 特性的变化(含 10 wt% 的 5 μm LLZTO 和不含 10 wt% 的 5 μm LLZTO),并评估其对锂剥离和电镀反应的影响。虽然较高的盐浓度(18:1)会大大提高离子导电率(大约一个数量级),但有趣的是,我们观察到较低的盐浓度(43:1)可将锂循环寿命延长 3 倍。值得注意的是,低盐浓度(43 : 1)电解质的硬度更高,压缩模量是 18 :1 的两倍多。虽然电解质的离子传导性通常是电解质设计过程中最直接的关注点,但这些发现突出表明,为了确保电解质在长时间锂循环过程中的性能,机械性能同样重要。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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