Dielectric breakdown strength of regenerated silk fibroin films as a function of protein conformation.

Derived from Bombyx mori cocoons, regenerated silk fibroin (RSF) exhibits excellent biocompatibility, high toughness, and tailorable biodegradability. Additionally, RSF materials are flexible, optically clear, easily patterned with nanoscale features, and may be doped with a variety bioactive species. This unique combination of properties has led to increased interest in the use of RSF in sustainable and biocompatible electronic devices. In order to explore the applicability of this biopolymer to the development of future bioelectronics, the dielectric breakdown strength (Ebd) of RSF thin films was quantified as a function of protein conformation. The application of processing conditions that increased ß-sheet content (as determined by FTIR analysis) and produced films in the silk II structure resulted in RSF materials with improved Ebd with values reaching up to 400 V/µm.

Dielectric breakdown in silica-amorphous polymer nanocomposite films: the role of the polymer matrix.

The ultimate energy storage performance of an electrostatic capacitor is determined by the dielectric characteristics of the material separating its conductive electrodes. Polymers are commonly employed due to their processability and high breakdown strength; however, demands for higher energy storage have encouraged investigations of ceramic-polymer composites. Maintaining dielectric strength, and thus minimizing flaw size and heterogeneities, has focused development toward nanocomposite (NC) films; but results lack consistency, potentially due to variations in polymer purity, nanoparticle surface treatments, nanoparticle size, and film morphology. To experimentally establish the dominant factors in broad structure-performance relationships, we compare the dielectric properties for four high-purity amorphous polymer films (polymethyl methacrylate, polystyrene, polyimide, and poly-4-vinylpyridine) incorporating uniformly dispersed silica colloids (up to 45% v/v). Factors known to contribute to premature breakdown-field exclusion and agglomeration-have been mitigated in this experiment to focus on what impact the polymer and polymer-nanoparticle interactions have on breakdown. Our findings indicate that adding colloidal silica to higher breakdown strength amorphous polymers (polymethyl methacrylate and polyimide) causes a reduction in dielectric strength as compared to the neat polymer. Alternatively, low breakdown strength amorphous polymers (poly-4-vinylpyridine and especially polystyrene) with comparable silica dispersion show similar or even improved breakdown strength for 7.5-15% v/v silica. At ∼15% v/v or greater silica content, all the polymer NC films exhibit breakdown at similar electric fields, implying that at these loadings failure becomes independent of polymer matrix and is dominated by silica.

Nanolaminates: increasing dielectric breakdown strength of composites.

Processable, low-cost, high-performance hybrid dielectrics are enablers for a vast array of green technologies, including high-temperature electrical insulation and pulsed power capacitors for all-electric transportation vehicles. Maximizing the dielectric breakdown field (E(BD)), in conjunction with minimization of leakage current, directly impacts system performance because of the field's quadratic relationship with electrostatic energy storage density. On the basis of the extreme internal interfacial area and ultrafine morphology, polymer-inorganic nanocomposites (PNCs) have demonstrated modest increases in E(BD) at very low inorganic loadings, but because of insufficient control of the hierarchal morphology of the blend, have yielded a precipitous decline in E(BD) at intermediate and high inorganic volume fractions. Here in, we demonstrate that E(BD) can be increased up to these intermediate inorganic volume fractions by creating uniform one-dimensional nanocomposites (nanolaminates) rather than blends of spherical inorganic nanoparticles and polymers. Free standing nanolaminates of highly aligned and dispersed montmorillonite in polyvinyl butyral exhibited enhancements in E(BD) up to 30 vol % inorganic (70 wt % organically modified montmorillonite). These relative enhancements extend up to five times the inorganic fraction observed for random nanoparticle dispersions, and are anywhere from two to four times greater than observed at comparable volume fraction of nanoparticles. The breakdown characteristics of this model system suggested a trade-off between increased path tortuosity and polymer-deficient structural defects. This implies that an idealized PNC morphology to retard the breakdown cascade perpendicular to the electrodes will occur at intermediate volume fractions and resemble a discotic nematic phase where highly aligned, high-aspect ratio nanometer thick plates are uniformly surrounded by nanoscopic regions of polymer.