Polymer nanocomposites with high energy density and low dielectric loss are highly desirable in electronic and electric industry. Achieving the ability to tailor the interface between polymer and nanoparticle is the key issue to realize desirable dielectric properties and high energy density in the nanocomposites. However, the understanding of the role of interface on the dielectric properties and energy density of polymer nanocomposites is still very poor. In this work, we report a novel strategy to improve the interface between the high dielectric constant nanoparticles (i.e., BaTiO3) and ferroelectric polymer [i.e., poly(vinylidene fluoride-co-hexafluoro propylene)]. Core–shell structured BaTiO3 nanoparticles either with different shell thickness or with different molecular structure of the shell were prepared by grafting two types of fluoroalkyl acrylate monomers via surface-initiated reversible addition–fragmentation chain transfer (RAFT) polymerization. The dielectric properties and energy storage capability of the corresponding nanocomposites were investigated by broadband dielectric spectroscopy and electric displacement-electric field loop measurement, respectively. The results show that high energy density and low dielectric loss are successfully realized in the nanocomposites. Moreover, the energy storage densities of the P(VDF-HFP)-based nanocomposites could be tailored by adjusting the structure and thickness of the fluoro-polymer shell. The approach described is applicable to a wide range of nanoparticles and polymer matrix, thereby providing a new route for preparing polymer-based nanocomposites used in electronic and electric industry.

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Polymer nanocomposites with high dielectric constant have extensive applications in the electronic and electrical industry because of ease of processing and low cost. Blending and in situ polymerization are two conventional methods for the preparation of polymer nanocomposites. However, the resulting nanocomposites, particularly highly filled nanocomposites, generally have some disadvantages such as high dielectric loss and low dielectric constant and thus show low energy density and low energy efficiency. Here we developed a core@double-shell strategy to prepare barium titanate (BT)-based high performance polymer nanocomposites, in which the first shell is hyperbranched aromatic polyamide (HBP) and the second shell is poly(methyl methacrylate) (PMMA). This method utilized the advantages of both polymer shells, resulting in superior dielectric property which cannot be achieved in nanocomposites prepared by the conventional blending methods. It is found that, compared with the conventional solution blended BT/PMMA nanocomposites, the core@double-shell structured BT@HBP@PMMA nanocomposites had higher dielectric constant and lower dielectric loss. The energy densities of BT@HBP@PMMA nanocomposites were higher than that of BT/PMMA nanocomposites accordingly. The dielectric response of the nanocomposites was analyzed, and the mechanisms resulting in the higher dielectric constant and lower dielectric loss in BT@HBP@PMMA nanocomposites were proposed. This study suggests that the core@double-shell strategy shows strong potential for preparing polymer nanocomposites with desirable dielectric properties.

Polymer-based materials with a high dielectric constant show great potential for energy storage applications. Since the intrinsic dielectric constant of most polymers is very low, the integration of carbon nanotubes (CNTs) into the polymers provides an attractive and promising way to reach a high dielectric constant owing to their outstanding intrinsic physical performances. However, these CNT-based composites usually suffer from high dielectric loss, low breakdown strength and the difficulty to tailor the dielectric constant. Herein, we have designed and fabricated a new class of candidates composed of graphene oxide-encapsulated carbon nanotube (GO-e-CNT) hybrids. The obtained GO-e-CNT-polymer composites not only exhibit a high dielectric constant and low dielectric loss, but also have a highly enhanced breakdown strength and maximum energy storage density. Moreover, the dielectric constant of the composites can be tuned easily by tailoring the loading of GO-e-CNTs. It is believed that the GO shells around CNTs play an important role in realizing the high dielectric performances of the composites. GO shells can not only effectively improve the dispersion of CNTs, but also act as insulation barriers for suppressing leakage current and increasing breakdown strength. Our strategy provides a new pathway to achieve CNT-based polymer composites with high dielectric performances for energy storage applications.

Polymer nanocomposites with the dielectric constant comparable to that of percolative composites are successfully prepared by using core-shell structured hyperbranched aromatic polyamide grafted barium titanate (BT-HBP) hybrid nanofiller. Poly(vinylidene fluoride-trifluoroethylene-chlorofluoroethylene) (PVDF-TrFE-CFE) was used as the polymer matrix because of its high intrinsic dielectric constant and easy processability. The BT-HBP hybrid nanofiller were prepared by a solution polymerization of diaminobenzoic acid on the surface of amino-funcationalized BT nanoparticles. Nuclear magnetic resonance ((1)H NMR) and transmission electron microscopy (TEM) were used to verify the chemical structure of the hyperbranched aromatic polyamide and core-shell structure of the hybrid filler, respectively. It was found that the nanocomposite with 40 vol % BaTiO3-HBP had a dielectric constant of 1485.5 at 1000 Hz, whereas the corresponding nanocomposite sample with untreated BaTiO3 only showed a dielectric constant of 206.3. Compared with classic percolative composites, the advantage of the PVDF-TrFE-CFE/BaTiO3-HBP nanocomposites is that the composites show high enough breakdown strength and high dielectric constant simultaneously. An enhanced interfacial polarization mechanism between the BT-HBP and the polymer matrix was suggested for understanding the observed unusually high dielectric constant.

Ferroelectric polymer nanocomposites with silver (Ag) nanoparticles as inclusions were prepared and the dielectric properties and thermal conductivity were studied. The results showed that the nanocomposites have high dielectric constant and high thermal conductivity. When the loading level of Ag nanoparticles is 20.0 vol %, the dielectric constant and thermal conductivity of the nanocomposites were 120 at 103 Hz and 6.5 W/mK, respectively. Our results also showed that there is no percolation in the nanocomposites when Ag loading range is within 20.0%.

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Nanodielectric materials with high dielectric constant, low dielectric loss, and high energy storage capability are highly desirable in modern electric and electronics industries. It has been proved that the preparation of core-shell structured dielectric polymer nanocomposites via "grafting from" method is an effective approach to these materials. However, by using this approach, the deep understanding of the structure-dielectric property relationship of the core-shell structured nanodielectrics has been limited because of the lack of detailed information (e.g., molecular weight, grafting density) about the macromolecules grafted onto the nanoparticle surfaces. In this work, by the combination of reversible addition-fragmentation chain transfer (RAFT) polymerization and thiol-ene click reaction, two types of core-shell structured polymer@BaTiO3 (polymer@BT) nanocomposites with high dielectric constant and low dielectric loss were successfully prepared via a "grafting to" method. Compared with the "grafting from" method, this "grafting to" method has two merits: the molecular weight of the polymer chains in the shell layer can be easily controlled and the grafting density can be tailored by changing the molecular weight of the grafting polymer. Moreover, a clear insight into the relationship among the dielectric properties and energy storage capability of the core-shell structured polymer@BT nanocomposites, the molecular weight of the polymer chains, and the grafting density of the core-shell structured nanoparticles was achieved. The study provides new insights into the design and preparation of nanodielectric materials with desirable dielectric properties.