Molecular Dynamics and Charge Transport in Polymeric Polyisobutylene-Based Ionic Liquids
Molecular Dynamics and Charge Transport in Polymeric Polyisobutylene-Based Ionic Liquids
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DOI：
10.1021/acs.macromol.6b00011
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发表时间：
2016-03
期刊：
影响因子：
5.5
通讯作者：
F. Frenzel;Makafui Y. Folikumah;M. Schulz;A. Anton;Wolfgang H. Binder;F. Kremer
中科院分区：
文献类型：
--
作者：
F. Frenzel;Makafui Y. Folikumah;M. Schulz;A. Anton;Wolfgang H. Binder;F. Kremer
基于带有类似离子液体 (IL) 的阳离子头基（N,N,N-三乙铵或 1-甲基吡咯烷鎓）和 Br、NTf2、OTf 或 pTOS 作为阴离子的单价和二价遥爪聚异丁烯 (PIB)，研究了 16 种同系聚合物离子液体 (PIL)。通过宽带介电谱 (BDS) 在宽频率 (10–2–107 Hz) 和温度 (200–400 K) 范围内分析介观尺度的分子动力学、电荷传输和极化；此外，还采用差示扫描量热法（DSC）。具体而言，观察到（i）三个分子弛豫过程，包括聚合物基质的动态玻璃化转变，（ii）源自类IL部分中的电荷传输的电导率弛豫，以及（iii）由移动电荷载流子在金属界面处的积累引起的弱电极极化。 PIL 的净电导率作为一个整体通过有效介质近似 (EMA) 反射定量描述...
A homologous series of 16 polymeric ionic liquids (PIL) are investigated based on monovalent and bivalent telechelic polyisobutylene (PIB) carrying the ionic liquid (IL)-like cationic headgroup (N,N,N-triethylammonium or 1-methylpyrrolidinium) and Br, NTf2, OTf, or pTOS as anions. Molecular dynamics, charge transport, and polarization at mesoscopic scales are analyzed over a wide frequency (10–2–107 Hz) and temperature (200–400 K) range by means of broadband dielectric spectroscopy (BDS); additionally, differential scanning calorimetry (DSC) is employed. In detail, (i) three molecular relaxation processes are observed including the dynamic glass transition of the polymeric matrix, (ii) a conductivity relaxation originating from charge transport in the IL-like moieties, and (iii) a weak electrode polarization caused by the accumulation of mobile charge carriers at the metal interfaces. The net conductivity of the PIL as a whole is quantitatively described by an effective-medium approximation (EMA) reflecti...