The morphology as well as the distribution of conductive fillers in conductive filler/polymer nanocomposites have a decisive effect on the dielectric properties of blend composites. In this study, the relationship between morphology and properties was carefully investigated and the underlying mechanism is discussed based on the microcapacitor model. Multiwalled carbon nanotubes (CNTs) were introduced into an immiscible poly(vinylidene fluoride) (PVDF)/polyamide 6 (Nylon 6) blend and the morphologies of PVDF/Nylon 6 were tailored by changing the weight ratio of PVDF to Nylon 6, varying from sea‐island morphology to co‐continuous morphology. Interestingly, the CNTs are selectively localized in the Nylon 6 phase in both sea‐island and co‐continuous morphological blends, which is due to the finer interaction between Nylon 6 and CNTs. In the sea‐island morphological blend only, a strong increase of the dielectric permittivity can be found when the content of CNTs is increased. It is surprising that no effects of CNTs on the dielectric properties can be found in the co‐continuous morphological blend. The CNT filled Nylon 6 domains in the sea‐island morphological blend act as a microcapacitor with improved charge accumulation and interfacial polarization, resulting in a marked increase in dielectric permittivity. © 2016 Society of Chemical Industry

The crystallization behaviors of miscible poly(vinylidene fluoride)/poly(butylene succinate) (PVDF/PBS) and its blend composites with carbon nanotubes (CNTs) during non-isothermal and isothermal processes were investigated. The results showed that CNTs acted as heterogeneous nucleation agents and further improved the nucleation ability of PBS and PVDF in blends. However, compared with the nucleation effects of CNTs in PBS/CNT or PVDF/CNT binary composites, the nucleation effect of CNTs in miscible PVDF/PBS was largely restricted and nucleation efficiency was lowered. A reasonable explanation about the restricted nucleation ability of CNTs was studied from the viewpoint of interfacial interactions between polymer components and CNTs, in which a preferential affinity of CNTs to PBS was found. Further combined with the preparation method, it is proposed that PVDF chains adsorbed on the CNT surface in the master batch were peeled off from the CNTs by incorporated PBS chains, due to the better interaction between PBS and CNTs. Finally, the PVDF chains at the interface were diluted by PBS, and most of theCNT surface was covered by PBS chains, giving rise to the nucleation of PBS on the CNTs. On the other hand, unremoved PVDF still adsorbed on the CNT surface and crystallized. Compared with PVDF/CNT and PBS/CNT binary composites, the nucleation density in the ternary composites was greatly lowered, resulting in restricted nucleation effects of CNTs. On the other hand, the preferable adsorption of PBS on CNTs induced an apparent phase fluctuation in the PVDF/PBS blend composites, which also reflected the selective adsorption of PBS on the CNT surface.

Tailoring the distribution of nanoparticles and further constructing effective microcapacitors in polymer blends are important issues for developing high-performance polymer dielectric nanocomposites. The common method to control the selective localization of nanoparticles in an immiscible polymer blend is relatively difficult and it easily results in the accumulation of nanoparticles in one component, which usually leads to a dramatic increase of the dielectric loss in the nanocomposites. In this work, a novel strategy based on step-by-step crystallization has been proposed to tailor the refined distribution and dispersion of carbon nanotubes (CNTs) in a melt-miscible blend poly­(butylene succinate)/poly­(vinylidene fluoride) (PBS/PVDF) through the crystallization-induced phase separation and the engineered interfacial affinity between CNTs and polymer components to acquire high dielectric constant and low dielectric loss. The results reveal that PBS is excluded along the growth front of PVDF spherulites and locates in the margin areas of PVDF spherulites during the step-by-step crystallization process. Moreover, because of the higher interfacial interaction between CNTs and PBS, CNTs are located in the PBS-rich domain, resulting in a high concentration of CNTs in the interspherulites of PVDF. Thus, the dielectric constants of the nanocomposites are greatly improved by nearly 5–24 times compared with the nanocomposites achieved by quick cooling and, simultaneously, the dielectric loss of the nanocomposites is still maintained at a low level. This work shows that the step-by-step crystallization method can be used to fabricate the nanocomposites with a synergistic increase in the dielectric performance due to the formation of a refined microcapacitor assembly. To the best of our knowledge, this is the first report to show that the dielectric constant of the nanocomposites can be greatly enhanced just through the crystallization-optimized distribution and dispersion of CNTs in immiscible polymer blends, and it possibly gives a new technical route for the fabrication of advanced dielectric composites.

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The effects of particle morphology on the structure and swelling/dissolution and rheological properties of nascent ultra-high molecular weight polyethylene (UHMWPE) in liquid paraffin (LP) were elaborately explored in this article. Nascent UHMWPE with different particle morphologies was prepared via pre-polymerization technique and direct polymerization. The melting temperature and crystallinity of UHMWPE resins with different particle morphologies were compared, and a schematic diagram was proposed to illustrate the mechanism of UHMWPE particle growth synthesized by pre-polymerization method and direct polymerization. The polymer globules in the nascent UHMWPE prepared by using pre-polymerization technique are densely packed and a positive correlation between the particle size and the viscosity-averaged molecular weight can be observed. The split phenomenon of particles and the fluctuation in the viscosity of UHMWPE/LP system prepared by direct polymerization can be observed at a low heating rate and there is no correlation between particle size and viscosity-averaged molecular weight.