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Composite materials and especially polymer composites are widely used in daily life and different industries due to their vastly different properties and design flexibility. It is known that the properties of the composites are strongly related to the properties of its constituents. However, it has been reported in many studies, experimentally and by simulations, that the characteristics of the composites do not follow the rule of mixing. It means that in addition to properties of the constituents, there are other parameters affecting the final physicochemical properties of composites. The interfacial interactions between fillers and host is one of the factors which can strongly affect the properties of the composite. In this review, we summarized the type of interactions between the constituents, their improvement techniques, interaction measurement methods, and the effects of interfacial interactions on thermal, mechanical, and electrical properties of composites.

Molecular level engineering of polymer or polymer blends has been recently demonstrated an effective strategy to regulate thermal conductivity. Such materials are of great interest to meet critical requirements of transparent, lightweight, flexible, and so on for thermal management in electronic applications. In this work, modulated polymer blends with poly(vinyl alcohol) (PVA) and biopolymers (lignin, gelatin) were designed and significantly enhanced thermal conductivity was achieved by tuning the intermolecular interaction among polymer components. The hydrogen bond interaction has been revealed as the major driving force that affects the polymer coil dimension in aqueous solution, the microstructure of coil−coil interaction in solid film, and thus, the thermal conduction. A solid relationship across molecular level interaction to macroscale thermal conduction is constructed via careful characterization of the coil size in liquid phase and assembled microstructure in solid phase. Appropriate integration of biopolymers and PVA is essential to achieve synergistic effect. Specifically, thermal conductivity of polymer blend with 10% lignin and 10% G90 in PVA reaches 0.71 W/m•K, which is 184% enhancement as compared to pure PVA. This work reveals the fundamental molecular origin of polymer blends in association with thermal conductivity and has great potential to guide molecular engineering for superior physicochemical properties.

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Phonon transfer is greatly scattered in traditional polymer composites due to the unpaired phonon frequency at the polymer/filler interface. A key innovation of this work is to build continuous crystal network by self-organization and utilize it as "thermal highway" that circumvents the long-existing interfacial thermal barrier issue in traditional composites. By tuning the molecular diffusion rate of dicarboxylic acids (oxalic acid, malonic acid, and succinic acid), different crystal structures including skeletal, dendrite, diffusion-limited aggregates, and spherulite were synthesized in PVA film. These continuous crystal structures benefit the efficient phonon transfer in the composites with minimized interfacial scattering and lead to a significant thermal conductivity enhancement of up to 180% compared to that of pure polymer. Moreover, the transparent feature of these composite films provides additional benefits in display applications. The post heat treatment effect on the thermal conductivity of the composite films shows a time-dependent behavior. These uniquely structured polymer/crystal composites are expected to generate significant impacts in thermal management applications.

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In this work, poly(vinyl alcohol) (PVA)/amino acid (AA) composites were prepared by a self-organized crystallization process. Five different AAs (cysteine, aspartic acid, glutamic acid, ornithine, and lysine) were selected based on their similar functional groups but different molecular structures. The different PVA-AA interactions in the five PVA/AA composites lead to two crystal patterns, i.e., continuous network (cysteine and lysine) and discrete particles (glutamic acid, ornithine, and aspartic acid). Scanning thermal microscopy is then applied to map the distribution of thermal conduction in these composites. It is found that the interface surrounding the crystals plays a dominating role in phonon transport where the polymer chains are greatly restrained by the interfacial confinement effect. Continuous crystal network builds up a continuous interface that facilitates phonon transfer while phonon scattering occurs in discrete crystalline structures. Significantly improved thermal conductivity of ∼0.7 W/m·K is observed in PVA/cysteine composite with AA loading of 8.4 wt %, which corresponds to a 170% enhancement as compared to pure PVA. The strong PVA-AA molecular interaction and self-organized crystal structure are considered the major reasons for the unique interface property and superior thermal conductivity.