Effect of Mixed Ionic Liquids on Chain Entanglement and Relaxation of Poly(methyl methacrylate)

Xi He; Huan Luo; Yan-hua Niu; Guang-xian Li

doi:10.11777/j.issn1000-3304.2020.20116

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Effect of Mixed Ionic Liquids on Chain Entanglement and Relaxation of Poly(methyl methacrylate)

Research Article | 更新时间：2021-05-15

- Effect of Mixed Ionic Liquids on Chain Entanglement and Relaxation of Poly(methyl methacrylate)
- Acta Polymerica Sinica Vol. 52, Issue 1, Pages: 84-93(2021)
- 作者机构：
  
  四川大学高分子科学与工程学院高分子材料工程国家重点实验室　成都 610065
- 作者简介：
- 基金信息：
- DOI：10.11777/j.issn1000-3304.2020.20116
  CLC：
- Published：3 January 2021，
  
  Published Online：31 July 2020，
  
  Received：8 May 2020，
  
  Revised：5 June 2020，
扫描看全文
Xi He, Huan Luo, Yan-hua Niu, Guang-xian Li. Effect of Mixed Ionic Liquids on Chain Entanglement and Relaxation of Poly(methyl methacrylate). [J]. Acta Polymerica Sinica 52(1):84-93(2021)
DOI：

Xi He, Huan Luo, Yan-hua Niu, Guang-xian Li. Effect of Mixed Ionic Liquids on Chain Entanglement and Relaxation of Poly(methyl methacrylate). [J]. Acta Polymerica Sinica 52(1):84-93(2021) DOI： 10.11777/j.issn1000-3304.2020.20116.

摘要

首先通过两步法合成了具有双咪唑环阳离子结构的离子液体(DIL)，并将其与单咪唑环离子液体(MIL)进行混合以调控黏度变化，混合离子液体(ILs)的黏度符合对数混合规则且随温度变化呈现Arrhenius型流体行为. 进一步通过动态流变、示差扫描量热(DSC)、电化学测试等方法研究了混合离子液体中DIL比例对聚甲基丙烯酸甲酯(PMMA)链缠结和松弛行为的影响，并讨论了PMMA/ILs体系热稳定性、玻璃化转变及离子电导率等的变化. 结果表明，DIL独特的双咪唑环结构可与PMMA分子形成更多相互作用位点，从而导致凝聚缠结的形成，很大程度上限制了PMMA分子链的运动和松弛. 随DIL含量增加，PMMA/ILs体系的松弛时间、热分解温度、玻璃化转变温度等参数均呈增大趋势，但其离子电导率有所损失，这与DIL较大的分子尺寸和运动能力有关.

Abstract

A kind of dicationic ionic liquid (DIL) [C

(MIM)

][TFSI]

with double charged imidazole rings was successfully synthesized and mixed with a monocationic ionic liquids (MIL) [C

(MIM)][TFSI]

. Compared with MIL

the double imidazolium rings on the DIL cation greatly limits the vibration ability of the alkyl chain

which shows a much higher wavenumber in infrared spectrum. The DIL/MIL mixtures show Arrhenius fluid behaviour

and their viscosities follow the logarithmic mixing rule. With the increase of DIL content in the ILs mixtures

the viscosity and flow activation energy gradually increase

which is closely related to the molecular size and intermolecular interaction of DIL. Then

the effect of mixed ILs on the entanglement and relaxation of poly(methyl methacrylate) (PMMA) was extensively investigated by rheological tests. The master curves obtained by time-temperature superposition principle show that DIL could significantly change the relaxation behaviour and entanglement state of PMMA chains in mixed ILs. With increasing DIL content in the mixed ILs

both the terminal relaxation

and entanglement relaxation

of PMMA chains were retarded

and the entanglement network of the PMMA/ILs becomes more compact

showing higher plateau modulus and greater viscosity. More interaction sites could be formed between PMMA chains and DIL molecules due to its unique double imidazolium rings structure

which results in more cohesive entanglements among PMMA chains and thus restrict their relaxation. Moreover

there is a mathematical relationship between the rheological parameters (such as

and

) of PMMA/ILs and the viscosity of ILs mixtures

so the rheological behaviour of the system could be approximately predicted. On the other hand

thermal stability

glass transition and ion conductivity of PMMA/ILs were also discussed. The thermal decomposition temperature and glass transition temperature of PMMA/ILs increased with the DIL content

while the ionic conductivity decreased slightly.

关键词

混合离子液体聚甲基丙烯酸甲酯缠结松弛

Keywords

Mixed ionic liquidsPoly(methyl methacrylate)EntanglementRelaxation

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Beijing National Laboratory for Molecular Sciences, Key Laboratory of Polymer Chemistry and Physics of Ministry of Education, Center for Soft Mater Science and Engineering, College of Chemistry and Molecular Engineering, Peking University

Center for Advanced Low-dimension Materials, State Key Laboratory for Modification of Chemcial Fibers and Polymer Materials, College of Materials Science and Engineering, Donghua University

College of materials science and engineering, Zhejiang University of Technology

Department of Polymer Science and Engineering, Zhejiang University

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