Abstract Interfacial regions formed by incorporating a certain percentage of nanofillers into a polymer matrix can impact on the motion of molecular groups, chain units or chain segments, and alter molecular chain network dynamics, which is regarded as a key factor to achieve a finer degree control of dielectric properties of polymer nanocomposites. It is of interest to investigate the molecular chain motion behavior at interfacial regions with the incorporation of nanofillers. Epoxy resin/polyhedral oligomeric silsesquioxane (EP/POSS) nanocomposites are fabricated and the observations of morphology structure and chemical elements indicate that POSS nanofillers are well dispersed in the matrix. Differential scanning calorimeter, dynamic thermomechanical analysis, and dielectric relaxation spectroscopy are measured to analyze the effect of nanodoping on the motion properties of molecular chain units and chain segments that satisfy the Arrhenius and Vogel-Fulcher-Tammann equations respectively. The thicknesses of interfacial regions between POSS nanofillers and EP matrix are estimated from dielectric spectra and effective relative permittivity simulations, which are around several nanometers and decrease with the increment in the nanofiller content. In addition, the dielectric spectra scaling analysis indicates that the motion of small chain units can be hindered in interfacial regions and be tuned simultaneously by the variations of molecular chain network structure and dynamics. Nevertheless, the thin interfacial regions cannot effectively restrict the orientation of long molecular chain segments during the glass transition process. The variation of chain segment orientation behavior is ascribed to the interactions among molecular chains tuned by the binding effect of POSS nanofillers.

中文翻译：

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环氧树脂/POSS纳米复合材料中的界面区域和网络动力学通过它们对分子链运动的影响而解开

摘要 在聚合物基体中掺入一定比例的纳米填料形成的界面区域会影响分子基团、链单元或链段的运动，改变分子链网络动力学，这是实现更精细程度控制的关键因素。聚合物纳米复合材料的介电性能。研究结合纳米填料的界面区域的分子链运动行为是很有趣的。制备了环氧树脂/多面体低聚倍半硅氧烷 (EP/POSS) 纳米复合材料，形态结构和化学元素的观察表明 POSS 纳米填料很好地分散在基质中。差示扫描量热仪，动态热机械分析，测量和介电弛豫光谱，以分析纳米掺杂对分别满足 Arrhenius 和 Vogel-Fulcher-Tammann 方程的分子链单元和链段运动特性的影响。POSS 纳米填料和 EP 基质之间的界面区域的厚度是根据介电光谱和有效的相对介电常数模拟估算的，其大约为几个纳米，并随着纳米填料含量的增加而减小。此外，介电谱标度分析表明，小链单元的运动可以在界面区域受到阻碍，并且可以通过分子链网络结构和动力学的变化进行同步调整。尽管如此，在玻璃化转变过程中，薄的界面区域不能有效地限制长分子链段的取向。链段取向行为的变化归因于由 POSS 纳米填料的结合效应调节的分子链之间的相互作用。