Interplay of chain dynamics and ion transport on mechanical behavior and conductivity in ionogels†

IF 2.9 3区 化学 Q3 CHEMISTRY, PHYSICAL
Soft Matter Pub Date : 2024-12-12 DOI:10.1039/D4SM01251H
Mengze Lu, Wei Zhen Lian, Zhenhua Xiao, Lu Liu, Zhiwei Fan, Xiaolin Jin, Chuanxia Jiang, Qian Chen, Zheng-Hai Tang, Panchao Yin and Taolin Sun
{"title":"Interplay of chain dynamics and ion transport on mechanical behavior and conductivity in ionogels†","authors":"Mengze Lu, Wei Zhen Lian, Zhenhua Xiao, Lu Liu, Zhiwei Fan, Xiaolin Jin, Chuanxia Jiang, Qian Chen, Zheng-Hai Tang, Panchao Yin and Taolin Sun","doi":"10.1039/D4SM01251H","DOIUrl":null,"url":null,"abstract":"<p >Understanding the interplay among the mechanical behavior, ionic conductivity and chain dynamics of ionogels is essential for designing flexible conductors that exhibit both high conductivity and excellent mechanical properties. In this study, ionogels were synthesized <em>via</em> the radical polymerization of <em>N</em>,<em>N</em>′-dimethylacrylamide (DMAA) and methacrylic acid (MAAc) monomers in the presence of ionic liquid 1-ethyl-3-methylimidazolium trifluoromethane sulfonate ([EMIM][OTf]). By varying the mass content of ionic liquid within ionogels, we investigated the mechanical behavior and ionic conductivity at the macroscopic scale using tensile, rheological testing and electrochemical impedance spectroscopy, as well as the dynamic behavior of chain segments and ions within the network at the microscopic scale using broadband dielectric relaxation spectroscopy (BDS) over a broad temperature range. Our findings revealed that variations in ionic liquid concentration significantly affect mechanical performance, ionic conductivity, complex conductivity spectra, and complex permittivity spectra. These ionogels exhibited remarkable stretchability, adhesion, and strain-sensing capabilities. Analysis of BDS indicated that the temperature dependence of the hopping frequency (<em>ω</em><small><sub>H</sub></small>), the conductivity of free ions (<em>σ</em><small><sub>dc</sub></small>), and the relaxation time (<em>τ</em><small><sub>s</sub></small>) of chain segments conforms to the Vogel–Tammann–Fulcher (VTF) equation for ionogels with varying ionic liquid content. By correlating <em>τ</em><small><sub>s</sub></small> measured through rheological tests and BDS, we observed a transition from Arrhenius to VTF behavior, which shifts towards lower temperatures with increasing ionic liquid content. This study highlighted a strong coupling between <em>σ</em><small><sub>dc</sub></small> and <em>ω</em><small><sub>H</sub></small>, as well as between 1/<em>τ</em><small><sub>s</sub></small> and <em>ω</em><small><sub>H</sub></small>, at low ionic concentrations, facilitating high mechanical performance of the ionogels due to viscoelastic energy dissipation. However, as the ionic concentration increased, a slight decoupling of <em>σ</em><small><sub>dc</sub></small> and <em>ω</em><small><sub>H</sub></small> was noted, leading to a substantial reduction in the mechanical properties of the ionogels. Ultimately, these ionogels demonstrate potential as polymer electrolytes for applications in flexible wearable devices.</p>","PeriodicalId":103,"journal":{"name":"Soft Matter","volume":" 3","pages":" 435-447"},"PeriodicalIF":2.9000,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Soft Matter","FirstCategoryId":"92","ListUrlMain":"https://pubs.rsc.org/en/content/articlelanding/2025/sm/d4sm01251h","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

Abstract

Understanding the interplay among the mechanical behavior, ionic conductivity and chain dynamics of ionogels is essential for designing flexible conductors that exhibit both high conductivity and excellent mechanical properties. In this study, ionogels were synthesized via the radical polymerization of N,N′-dimethylacrylamide (DMAA) and methacrylic acid (MAAc) monomers in the presence of ionic liquid 1-ethyl-3-methylimidazolium trifluoromethane sulfonate ([EMIM][OTf]). By varying the mass content of ionic liquid within ionogels, we investigated the mechanical behavior and ionic conductivity at the macroscopic scale using tensile, rheological testing and electrochemical impedance spectroscopy, as well as the dynamic behavior of chain segments and ions within the network at the microscopic scale using broadband dielectric relaxation spectroscopy (BDS) over a broad temperature range. Our findings revealed that variations in ionic liquid concentration significantly affect mechanical performance, ionic conductivity, complex conductivity spectra, and complex permittivity spectra. These ionogels exhibited remarkable stretchability, adhesion, and strain-sensing capabilities. Analysis of BDS indicated that the temperature dependence of the hopping frequency (ωH), the conductivity of free ions (σdc), and the relaxation time (τs) of chain segments conforms to the Vogel–Tammann–Fulcher (VTF) equation for ionogels with varying ionic liquid content. By correlating τs measured through rheological tests and BDS, we observed a transition from Arrhenius to VTF behavior, which shifts towards lower temperatures with increasing ionic liquid content. This study highlighted a strong coupling between σdc and ωH, as well as between 1/τs and ωH, at low ionic concentrations, facilitating high mechanical performance of the ionogels due to viscoelastic energy dissipation. However, as the ionic concentration increased, a slight decoupling of σdc and ωH was noted, leading to a substantial reduction in the mechanical properties of the ionogels. Ultimately, these ionogels demonstrate potential as polymer electrolytes for applications in flexible wearable devices.

Abstract Image

离子凝胶中链动力学和离子输运对力学行为和电导率的影响。
了解电离胶的力学行为、离子电导率和链动力学之间的相互作用,对于设计既具有高电导率又具有优异力学性能的柔性导体至关重要。本研究在离子液体1-乙基-3-甲基咪唑三氟甲烷磺酸盐([EMIM][OTf])存在下,通过N,N'-二甲基丙烯酰胺(DMAA)和甲基丙烯酸(MAAc)单体自由基聚合合成了离子凝胶。通过改变离子液体在离子凝胶中的质量含量,我们在宏观尺度上使用拉伸、流变学测试和电化学阻抗谱研究了离子的力学行为和电导率,在微观尺度上使用宽带介电弛豫光谱(BDS)在宽温度范围内研究了链段和离子在网络中的动态行为。研究结果表明,离子液体浓度的变化会显著影响材料的力学性能、离子电导率、复电导率谱和复介电常数谱。这些离子凝胶表现出显著的拉伸性、粘附性和应变传感能力。BDS分析表明,对于不同离子液体含量的离子凝胶,跳变频率(ωH)、自由离子电导率(σdc)和链段弛豫时间(τs)与温度的关系符合Vogel-Tammann-Fulcher (VTF)方程。通过对比流变试验和BDS测量的τs,我们观察到离子液体从Arrhenius行为到VTF行为的转变,随着离子液体含量的增加,这种转变向更低的温度转变。在低离子浓度下,σdc和ωH之间、1/τs和ωH之间存在较强的耦合,这使得离子凝胶具有较高的粘弹性耗散性能。然而,随着离子浓度的增加,σdc和ωH出现了轻微的解耦,导致离子凝胶的力学性能大幅下降。最终,这些离子凝胶展示了在柔性可穿戴设备中作为聚合物电解质应用的潜力。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
求助全文
约1分钟内获得全文 求助全文
来源期刊
Soft Matter
Soft Matter 工程技术-材料科学:综合
CiteScore
6.00
自引率
5.90%
发文量
891
审稿时长
1.9 months
期刊介绍: Soft Matter is an international journal published by the Royal Society of Chemistry using Engineering-Materials Science: A Synthesis as its research focus. It publishes original research articles, review articles, and synthesis articles related to this field, reporting the latest discoveries in the relevant theoretical, practical, and applied disciplines in a timely manner, and aims to promote the rapid exchange of scientific information in this subject area. The journal is an open access journal. The journal is an open access journal and has not been placed on the alert list in the last three years.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:481959085
Book学术官方微信