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基于线性聚二甲基硅氧烷链、以介晶基团作为物理交联剂进行α,ω-封端的低温可熔弹性体：一种具有粘弹性耦合潜力的被动智能材料。第二部分——粘弹性和流变特性

Low-Temperature-Meltable Elastomers Based on Linear Polydimethylsiloxane Chains Alpha, Omega-Terminated with Mesogenic Groups as Physical Crosslinker: A Passive Smart Material with Potential as Viscoelastic Coupling. Part II-Viscoelastic and Rheological Properties.

作者信息

Horodecka Sabina, Strachota Adam, Mossety-Leszczak Beata, Kisiel Maciej, Strachota Beata, Šlouf Miroslav

机构信息

Institute of Macromolecular Chemistry, Czech Academy of Sciences, Heyrovskeho nam. 2, CZ-162 06 Praha, Czech Republic.

Faculty of Science, Charles University, Albertov 6, CZ-128 00 Praha, Czech Republic.

出版信息

Polymers (Basel). 2020 Nov 29;12(12):2840. doi: 10.3390/polym12122840.

DOI:10.3390/polym12122840
PMID:33260294
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC7760245/
Abstract

Rheological and viscoelastic properties of physically crosslinked low-temperature elastomers were studied. The supramolecularly assembling copolymers consist of linear polydimethylsiloxane (PDMS) elastic chains terminated on both ends with mesogenic building blocks (LC) of azobenzene type. They are generally and also structurally highly different from the well-studied LC polymer networks or LC elastomers: The LC units make up only a small volume fraction in our materials and act as fairly efficient physical crosslinkers with thermotropic properties. The aggregation (nano-phase separation) of the relatively rare, small and spatially separated terminal LC units generates temperature-switched viscoelasticity in the molten copolymers. Their rheological behavior was found to be controlled by an interplay of nano-phase separation of the LC units (growth and splitting of their aggregates) and of the thermotropic transitions in these aggregates (which change their stiffness). As a consequence, multiple gel points (up to three) are observed in temperature scans of the copolymers. The physical crosslinks also can be reversibly disconnected by large mechanical strain in the 'warm' rubbery state, as well as in melt (thixotropy). The kinetics of crosslink formation was found to be fast if induced by temperature and extremely fast in case of internal self-healing after strain damage. Thixotropic loop tests hence display only very small hysteresis in the LC-melt-state, although the melts show very distinct shear thinning. Our study evaluates structure-property relationships in three homologous systems with elastic PDMS segments of different length (8.6, 16.3 and 64.4 repeat units). The studied copolymers might be of interest as passive smart materials, especially as temperature-controlled elastic/viscoelastic mechanical coupling.

摘要

研究了物理交联低温弹性体的流变学和粘弹性特性。超分子组装共聚物由线性聚二甲基硅氧烷（PDMS）弹性链组成，其两端由偶氮苯型介晶结构单元（LC）封端。它们在总体上以及结构上与经过充分研究的LC聚合物网络或LC弹性体有很大不同：LC单元在我们的材料中仅占很小的体积分数，并作为具有热致性的相当有效的物理交联剂。相对稀少、微小且在空间上分离的末端LC单元的聚集（纳米相分离）在熔融共聚物中产生温度切换的粘弹性。发现它们的流变行为受LC单元的纳米相分离（其聚集体的生长和分裂）以及这些聚集体中的热致转变（这会改变它们的刚度）之间的相互作用控制。因此，在共聚物的温度扫描中观察到多个凝胶点（多达三个）。物理交联在“温暖”的橡胶态以及熔体中（触变性）也可以通过大的机械应变可逆地断开。如果由温度诱导，交联形成的动力学很快，而在应变损伤后的内部自修复情况下则极快。因此，触变循环测试在LC熔体状态下仅显示非常小的滞后现象，尽管熔体表现出非常明显的剪切变稀。我们的研究评估了具有不同长度（8.6、16.3和64.4个重复单元）的弹性PDMS链段的三个同源体系中的结构 - 性能关系。所研究的共聚物作为被动智能材料可能会受到关注，特别是作为温度控制的弹性/粘弹性机械耦合材料。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/f00417273d0d/polymers-12-02840-sch011.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/c9dafa8223b0/polymers-12-02840-sch001a.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/f7f7ededb7a2/polymers-12-02840-sch002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/7c045f782626/polymers-12-02840-sch003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/a3cbaab662a0/polymers-12-02840-sch004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/0dbac870f4c6/polymers-12-02840-sch005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/9f5f71e3fcc9/polymers-12-02840-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/a7579f9fb253/polymers-12-02840-sch006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/d13949114c1f/polymers-12-02840-sch007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/b0d21b2a07bb/polymers-12-02840-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/53c2163e600d/polymers-12-02840-sch008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/09a1ba7be62e/polymers-12-02840-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/c4e2c7dfdad6/polymers-12-02840-sch009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/de82b7964707/polymers-12-02840-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/e2ed6397d5e7/polymers-12-02840-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/cda040af35c2/polymers-12-02840-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/f7dd6ca4fff9/polymers-12-02840-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/5d2eaced4552/polymers-12-02840-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/42fd/7760245/20f33d2734a7/polymers-12-02840-g009.jpg
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