This review provides a detailed overview on the latest developments in the design and control of the interface in polymer based composite dielectrics for energy storage applications. The methods employed for interface design in composite systems are described for a variety of filler types and morphologies, along with novel approaches employed to build hierarchical interfaces for multi-scale control of properties. Efforts to achieve a close control of interfacial properties and geometry are then described, which includes the creation of either flexible or rigid polymer interfaces, the use of liquid crystals and developing ceramic and carbon-based interfaces with tailored electrical properties. The impact of the variety of interface structures on composite polarization and energy storage capability are described, along with an overview of existing models to understand the polarization mechanisms and quantitatively assess the potential benefits of different structures for energy storage. The applications and properties of such interface-controlled materials are then explored, along with an overview of existing challenges and practical limitations. Finally, a summary and future perspectives are provided to highlight future directions of research in this growing and important area.

/pdf/interface-design-for-high-energy-density-polymer-461ds0csrx.pdf

Interface design for high energy density polymer nanocomposites

With the development of flexible electronic devices and large-scale energy storage technologies, functional polymer-matrix nanocomposites with high permittivity (high-k) are attracting more attention due to their ease of processing, flexibility, and low cost. The percolation effect is often used to explain the high-k characteristic of polymer composites when the conducting functional fillers are dispersed into polymers, which gives the polymer composite excellent flexibility due to the very low loading of fillers. Carbon nanotubes (CNTs) and graphene nanosheets (GNs), as one-dimensional (1D) and two-dimensional (2D) carbon nanomaterials respectively, have great potential for realizing flexible high-k dielectric nanocomposites. They are becoming more attractive for many fields, owing to their unique and excellent advantages. The progress in dielectric fields by using 1D/2D carbon nanomaterials as functional fillers in polymer composites is introduced, and the methods and mechanisms for improving dielectric properties, breakdown strength and energy storage density of their dielectric nanocomposites are examined. Achieving a uniform dispersion state of carbon nanomaterials and preventing the development of conductive networks in their polymer composites are the two main issues that still need to be solved in dielectric fields for power energy storage. Recent findings, current problems, and future perspectives are summarized.

1D/2D Carbon Nanomaterial‐Polymer Dielectric Composites with High Permittivity for Power Energy Storage Applications

Interaction with electron donor and acceptor molecules such as aniline and nitrobenzene brings about marked changes in the Raman spectrum and the electronic structure of graphene, prepared by the exfoliation of graphitic oxide.

Changes in the electronic structure and properties of graphene induced by molecular charge-transfer

Graphene nanosheet- and flake carbonyl iron particle-filled epoxy–silicone composites as thin–thickness and wide-bandwidth microwave absorber

Nano Ag-deposited BaTiO3 (BT-Ag) hybrid particles usable as fillers for flexible polymeric composites to obtain high dielectric constant, low conductivity, and low dielectric loss were developed. BT-Ag hybrid particles were synthesized via a seed-mediated growing process by a redox reaction between silver nitrate and ethylene glycol. Nano Ag particles with a size less than 20 nm were discretely grown on the surface of the 100 nm BaTiO3. The similar lattice spacing of the (1 1 1) planes of BT and Ag led to the hetero-epitaxial growth of Ag on the BT surface. The thickness of the coherent interface was about 3 nm. The adhesion of Ag to BT efficiently prevented the continuous contact between Ag particles in the polyvinylidene fluoride (PVDF) matrix and suppressed the formation of the conducting path in the composite. As a result, with a filler loading of 43.4 vol %, the composite exhibited a dielectric constant (Dk) value of 94.3 and dielectric loss (tan δ) of 0.06 at 1 kHz. An even higher Dk value of 160 at...

Nano Ag-Deposited BaTiO3 Hybrid Particles as Fillers for Polymeric Dielectric Composites: Toward High Dielectric Constant and Suppressed Loss

In this work, two series of nanocomposites of poly(vinylidene fluoride) (PVDF) incorporated with reduced graphene oxide (rGO) and poly(vinyl alcohol)-modified rGO (rGO-PVA) were fabricated using solution-cast method and their dielectric properties were carefully characterized. Infrared spectroscopy and atom force microscope analysis indicated that PVA chains were successfully grafted onto graphene through ester linkage. The PVA functionalization of graphene surface can not only prevent the agglomeration of original rGO but also enhance the interaction between PVDF and rGO-PVA. Strong hydrogen bonds and charge transfer effect between rGO-PVA and PVDF were determined by infrared and Raman spectroscopies. The dielectric properties of rGO-PVA/PVDF and rGO/PVDF nanocomposites were investigated in a frequency range from 10² Hz to 10⁷ Hz. Both composite systems exhibited an insulator-to-conductor percolating transition as the increase of the filler content. The percolation thresholds were estimated to be 2.24 vol % for rGO-PVA/PVDF composites and 0.61 vol % for rGO/PVDF composites, respectively. Near the percolation threshold, the dielectric permittivity of the nanocomposites was significantly promoted, which can be well explained by interfacial polarization effect and microcapacitor model. Compared to rGO/PVDF composites, higher dielectric constant and lower loss factor were simultaneously achieved in rGO-PVA/PVDF nanocomposites at a frequency range lower than 1 × 10³ Hz. This work provides a potential design strategy based on graphene interface engineering, which would lead to higher-performance flexible dielectric materials.

Yaru Bao

Papers

Improved dielectric properties of nanocomposites based on poly(vinylidene fluoride) and poly(vinyl alcohol)-functionalized graphene.