Structural Investigation of Chloride Ion-Containing Acrylate-Based Imidazolium Poly(Ionic Liquid) Homopolymers and Crosslinked Networks: Effect of Alkyl Spacer and N-Alkyl Substituents.

IF 4.4 3区 材料科学 Q2 CHEMISTRY, MULTIDISCIPLINARY Nanomaterials Pub Date : 2024-12-29 DOI:10.3390/nano15010040
Mahmoud Al-Hussein, Lisa Ehrlich, Doris Pospiech, Petra Uhlmann
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Abstract

Understanding the interplay between the molecular structure of the ionic liquid (IL) subunit, the resulting nanostructure and ion transport in polymerized ionic liquids (PILs) is necessary for the realization of high-performance solid-state electrolytes required in various advanced applications. Herein, we present a detailed structural characterization of a recently synthesized series of acrylate-based PIL homopolymers and networks with imidazolium cations and chloride anions with varying alkyl spacer and terminal group lengths designed for organic solid-state batteries based on X-ray scattering. The impact of the concentrations of both the crosslinker and added tetrabutylammonium chloride (TBACl) conducting salt on the structural characteristics is also investigated. The results reveal that the length of both the spacer and terminal group influence the chain packing and, in turn, the nanophase segregation of the polar domains. Long spacers and terminal groups seem to induce denser polar aggregates sandwiched between more compact alkyl spacer and terminal group domains. However, the large inter-backbone spacing achieved seems to limit the ionic conductivity of these PILs. More importantly, our findings show that the previously reported general relationships between the ionic conductivity and the structural parameters of the nanostructure of PILs are not always attainable for different molecular structures of the IL side group.

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含氯离子丙烯酸酯基咪唑聚(离子液体)均聚物及交联网络的结构研究:烷基间隔剂和n-烷基取代基的影响。
了解离子液体(IL)亚基的分子结构、所产生的纳米结构和聚合离子液体(pil)中离子传输之间的相互作用,对于实现各种先进应用所需的高性能固态电解质是必要的。本文中,我们基于x射线散射,对最近合成的一系列基于丙烯酸酯的PIL均聚物和咪唑阳离子和氯离子的网络进行了详细的结构表征,这些网络具有不同的烷基间隔和末端基团长度,设计用于有机固态电池。研究了交联剂浓度和添加四丁基氯化铵(TBACl)导电盐浓度对结构特性的影响。结果表明,间隔基团和末端基团的长度都会影响链的排列,进而影响极性畴的纳米相偏析。长间隔基团和末端基团似乎在更紧凑的烷基间隔基团和末端基团之间形成了更密集的极性聚集体。然而,大的骨干间距似乎限制了这些pil的离子电导率。更重要的是,我们的研究结果表明,对于IL侧基的不同分子结构,先前报道的离子电导率与pil纳米结构参数之间的一般关系并不总是可以实现的。
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来源期刊
Nanomaterials
Nanomaterials NANOSCIENCE & NANOTECHNOLOGY-MATERIALS SCIENCE, MULTIDISCIPLINARY
CiteScore
8.50
自引率
9.40%
发文量
3841
审稿时长
14.22 days
期刊介绍: Nanomaterials (ISSN 2076-4991) is an international and interdisciplinary scholarly open access journal. It publishes reviews, regular research papers, communications, and short notes that are relevant to any field of study that involves nanomaterials, with respect to their science and application. Thus, theoretical and experimental articles will be accepted, along with articles that deal with the synthesis and use of nanomaterials. Articles that synthesize information from multiple fields, and which place discoveries within a broader context, will be preferred. There is no restriction on the length of the papers. Our aim is to encourage scientists to publish their experimental and theoretical research in as much detail as possible. Full experimental or methodical details, or both, must be provided for research articles. Computed data or files regarding the full details of the experimental procedure, if unable to be published in a normal way, can be deposited as supplementary material. Nanomaterials is dedicated to a high scientific standard. All manuscripts undergo a rigorous reviewing process and decisions are based on the recommendations of independent reviewers.
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