Epoxy/benzoxazinyl POSS nanocomposite resin with low dielectric constant and excellent thermal stability

Benzoxazinyl modified polyhedral oligomeric silsesquioxane (BZPOSS) is successfully synthesized and used to prepare nanocomposites with bisphenol A type epoxy resin (E51). The differential scanning calorimetry results showed the curing peak temperature of E51/BZPOSS blend decrease to 242°C, suggesting the high catalytic activity of BZPOSS to the polymerization of E51. The scanning electron microscope micrographs of poly(E51/BZPOSS)s and silicon element distribution maps given by EDS both demonstrated homogeneous dispersion of BZPOSS. Dielectric properties tests confirmed the dielectric constant can be reduced by the introduction of BZPOSS, which is attributed to the nano-pores from the cage structure of POSS. When 20 wt% BZPOSS was added, the dielectric constant decreased to 2.28 at 1 MHz. Meanwhile, DMA and TGA results indicated the thermal stability and heat resistance of poly(E51/BZPOSS)s at high temperature increased with the increase of BZPOSS, which is due to the increase of the crosslinking density and the change of crosslinking structure of copolymer.     

Optimization of properties in a rubber compound containing a ternary polymer blend using response surface methodology

In order to find the best combination of three synthetic rubbers, that is, styrene‐butadiene rubber (SBR) grade 1712, SBR grade 1721 and high‐1,4‐cis polybutadiene, that produce a compound with specific end‐use properties, a statistical experimental design is proposed in this work. The design consists of ten mixtures containing specific amounts of total styrene and BR content. A number of properties are tested in each mixture, selecting those related to requirements for the tread of a high performance tire: glass transition temperature (T_g), the ratio between the viscous modulus and the elastic modulus (tanδ@60 °C), Mooney viscosity, and the tensile properties. The values obtained for each property are fit to statistically significant models, obtaining the respective response surfaces. These are next used to define a desirable formulation with the optimal ratio of each rubber, and finally the optimized formulation is validated by comparing the experimental and predicted values for each modeled property. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46548.     

Fumed SiO2 nanoparticle reinforced biopolymer blend nanocomposites with high dielectric constant and low dielectric loss for flexible organic electronics

In the present study, fumed silica (SiO₂) nanoparticle reinforced poly(vinyl alcohol) (PVA) and poly(vinylpyrrolidone) (PVP) blend nanocomposite films were prepared via a simple solution‐blending technique. Fourier transform infrared spectroscopy (FTIR), ultraviolet–visible spectroscopy (UV–vis), X‐ray diffraction (XRD), and scanning electron microscopy (SEM) were employed to elucidate the successful incorporation of SiO₂ nanoparticles in the PVA/PVP blend matrix. A thermogravimetric analyzer was used to evaluate the thermal stability of the nanocomposites. The dielectric properties such as dielectric constant (?) and dielectric loss (tan δ) of the PVA/PVP/SiO₂ nanocomposite films were evaluated in the broadband frequency range of 10^?2 Hz to 20 MHz and for temperatures in the range 40–150 °C. The FTIR and UV–vis spectroscopy results implied the presence of hydrogen bonding interaction between SiO₂ and the PVA/PVP blend matrix. The XRD and SEM results revealed that SiO₂ nanoparticles were uniformly dispersed in the PVA/PVP blend matrix. The dielectric property analysis revealed that the dielectric constant values of the nanocomposites are higher than those of PVA/PVP blends. The maximum dielectric constant and the dielectric loss were 125 (10^?2 Hz, 150 °C) and 1.1 (10^?2 Hz, 70 °C), respectively, for PVA/PVP/SiO₂ nanocomposites with 25 wt % SiO₂ content. These results enable the preparation of dielectric nanocomposites using a facile solution‐casting method that exhibit the desirable dielectric performance for flexible organic electronics. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 44427.     

Relaxation phenomenon of poly(vinyl alcohol)/sodium carboxy methyl cellulose blend by thermally stimulated depolarization currents and thermal sample technique

The dipolar relaxation in poly(vinyl alcohol) (PVA), sodium carboxy methyl cellulose (NaCMC_s), and their blends were studied using a thermally stimulated depolarization current (TSDC) technique. The mutual effects of polarization conditions such as heating rate, poling temperature, time, and field on the properties of TSDC were investigated. Quantitative analysis of the experimental data is given in terms of dipolar and space charge polarization. A thermal sampling (TS) technique was applied to decompose the complex relaxations in individual polymers and their blend of 0.5/0.5 wt/wt into its normal distribution components. The activation energy of TS‐formed electrets was determined by fitting the experimental curve to Bucci and Fieschi equations. Peak parameters such as activation energy and preexponential factor τ₀ were obtained. A linear relationship between the activation energy and logarithm of the preexponential factor was found, thus confirming operation of the compensation law. In addition, by using the Eyring equation of the rate theory, the activation enthalpy ΔH^≠ and the activation entropy ΔS^≠ were calculated. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 95: 1342–1353, 2005     

Low dielectric loss LNT/PEEK composites with high mechanical strength and dielectric thermal stability

(3-Aminopropyl)triethoxysilane treated La_(2−x)/3Na_0.06TiO₃ (x = 0.06) (LNT) microparticles filled polyetheretherketone (PEEK) composites were prepared using hot pressing process. The effects of variation of LNT ceramic filling fraction on dielectric properties, water absorption, thermal stability and mechanical strength were investigated. All composites demonstrate low water absorption (less than 0.4%) when the ceramic filling fraction is lower than 0.6V_f. The obtained composites exhibited dielectric permittivities varying from ~4 to ~22 as the ceramic fillers increased from 0.1 to 0.8V_f and low losses (~10⁻⁴ @1 MHz, 3~5 × 10⁻³ at the frequencies of microwave (10 GHz) and millimeter wave (29-50 GHz), respectively). The mechanical strength, dimensional and dielectric thermal stability of the composite are remarkably improved by the addition of LNT ceramic fillers. A composite with near zero temperature coefficients of dielectric permittivity or resonant frequency and flexural strength of ~140 MPa could be obtained. The out-of-plane coefficient of thermal expansion (CTE) could be reduced to ~20 ppm/°C as the ceramic filler loading reached 0.7V_f.     

Development of HDPE/EPDM‐g‐TMEVS nanocomposites with enhanced electrical and flame properties

Nanoclay reinforced HDPE/silane grafted EPDM composites have been developed using an epoxy functionalized HDPE as compatibilizer.The nanoclay has been varied from 0% to 10% in the composites along with the incorporation of compatibilizer and without compatibilizer in a brabender plasticorder.The dielectric and fire retardant properties of these nanocomposites have been examined. Addition of nanoclay enhanced char formation with increased values of limiting oxygen index. Electrical properties such as volume and surface Resistivity improved with addition of nanoclay and compatibilizer. The values of tan δ increased with increase in grafted EPDM and silanated nanoclay loading. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

Composition design and properties investigation of BPDA/PDA/TFDB co-polyimide films with low dielectric permittivity

Aiming at fabricating the polyimide (PI) films with low permittivity and excellent comprehensive properties, 2,2′-bis-(trifluoromethyl)-4,4′-diaminobiphenyl was incorporated into the polyimide backbone composed of 3,3′,4,4′-biphenyltetracarboxylic dianhydride and p-phenylenediamine. The introduction of trifluoromethyl ( CF₃) groups led to a substantial reduction of the PI's permittivity (3.42–2.96). Meanwhile, as-prepared co-PI films showed excellent mechanical performance (217.13–238.20 MPa for strength and 3.49–4.90 GPa for modulus), as well as good thermal stability (high glass transition temperature over 354 °C, whereas low thermal expansion coefficient below 10 ppm/K). Structure–property relationship of the PI samples was further established through molecular simulations (MS), which suggested the crucial effects of polarizability per unit volume (α/V_vdw) and free volume on PI permittivity. The computational results were highly consistent with the experimental findings, meaning that MS technique is of guiding importance in copolymer design. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 47989.     

Thermal and dielectric properties of the aluminum particle/epoxy resin composites

Microsized aluminum/epoxy resin composites were prepared, and the thermal and dielectric properties of the composites were investigated in terms of composition, aluminum particle sizes, frequency, and temperature. The results showed that the introduction of aluminum particles to the composites hardly influenced the thermal stability behavior, and decreased T_g of the epoxy resin; moreover, the size, concentration, and surface modification of aluminum particles had an effect on their thermal conductivity and dielectric properties. The dielectric permittivity increased smoothly with a rise of aluminum particle content, as well as with a decrease in frequency at high loading with aluminum particles. While the dissipation factor value increased slightly with an increase in frequency, it still remained at a low level. The dielectric permittivity and loss increased with temperature, owing to the segmental mobility of the polymer molecules. We found that the aluminum/epoxy composite containing 48 vol % aluminum‐particle content possessed a high thermal conductivity and a high dielectric permittivity, but a low loss factor, a low electric conductivity, and a higher breakdown voltage. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2010     

Mechanical,dielectric, and thermal properties of fluorosilicone rubber composites filled with silica/multiwall carbon nanotube hybrid fillers

In this work, hybrid fillers consist of modified silica (SiO₂) and multiwalled carbon nanotube (MWCNT) were used to improve the mechanical, dielectric, and thermal properties of fluorosilicone (FSR) composites via a direct mechanical mixing method. With the increase of CNT loading in SiO₂/CNT hybrid loading ratio, the tensile properties, dielectric constant, electrical conductivity, and thermal properties all increase without a sharp sacrifice of flexibility. The dielectric constant of FSR-S15/C5 achieved 7,370 @1 kHz, which is about four orders of the FSR-S20, and the dielectric loss remains as low as 0.676 @1 kHz. Therefore, the linkage of SiO₂ and FSR chains not only enhances the interfacial interaction between the fillers and FSR matrix but also decreases the agglomeration of the fillers in matrix. What is more, modified SiO₂ and CNT were designed as the effective hybrid filler to improve the performance of the polymeric matrix through synergic effect.     

Influences of porous reduction graphene oxide/molybdenum disulfide as filler on dielectric properties,thermal stability,and mechanical properties of natural rubber

A ternary composite system consisting of natural rubber (NR), porous reduced graphene oxide (rPGO), and molybdenum disulfide (MoS₂) was introduced for applying in the dielectric field, of which rPGO and MoS₂ hybrid conductive filler (rPGM) was prepared by an effective and environmentally friendly method-microwave reduction. And the well-dispersed NR composites (NGM) were made by the latex co-precipitation method. Due to the large specific surface area of rPGM itself and the synergistic dispersion of rPGO and MoS₂, it formed many stable interface structures with the NR matrix, which not only made the blend exhibit high elasticity and withstood large deformation as NR but also greatly improved the dielectric, mechanical and thermal stability of the NR matrix. Compared with neat NR, the dielectric constant of nanocomposite increased by 11 times in the presence of rPGM conductive filler, and the leakage current generated by direct contact of fillers was reduced due to the attachment of MoS₂ to the surface of rPGO; when 2% rPGM was added, the NR exhibited the highest tensile strength (21.3 MPa), elongation at break (495%), and abrasion resistance (0.165 cm⁻³); in addition, the thermal stability of the nanocomposite was also improved. These phenomena indicate that rPGM had great potential in conductive fillers and provided a reliable way for NR applications in the field of dielectric elastomers.     

Silacyclobutane-functionalized cyclosiloxanes as photoactive precursors for high thermal stability,low dielectric constant and low dielectric loss polymers

Low dielectric photoactive materials have significant potential as components in future microelectronics. Although a number of photosensitive groups have been used to construct photopatternable materials, it remains challenging to introduce these groups into polymer chains via facile yet controlled polymerization techniques. The present work demonstrates the synthesis of a new class of photoactive cyclosiloxane monomers having hybrid siloxane-carbosilane main chains. These compounds can be cured by applying ultraviolet radiation and heat to promote the reaction of the silacyclobutene units and form hyper-cross-linked cyclosiloxanes. The cured resins show high thermal stability (with T_5% values in the range of 460–550°C), low dielectric constants (2.36–2.76 at 10 MHz) and low dielectric losses (10⁻³ at 10 MHz). Thus, these polymers could possibly be used as high-performance dielectric materials.     

Fluorinated bismaleimide resin with good processability,high toughness,and outstanding dielectric properties

In this study, novel fluorinated bismaleimide (BMI) resins were prepared by the copolymerization of 2,2′‐bis[4‐(4‐maleimidephenoxy)phenyl]hexafluoropropane (6FBMP) and diallyl hexafluorobisphenol A (6FDABPA) to enhance their dielectric properties. The dielectric properties of the resins were investigated in the frequency range 7–18 GHz through a cavity method. Through the incorporation of a hexafluoroisopropyl group with the polymer chain, the dielectric constant (ε) was effectively decreased because of the small dipole and the low polarizability of the carbon‐fluorine (C? F) bonds. The 6FBMP/6FDABPA resin possessed excellent dielectric properties, with ε being 2.88 and the dielectric loss being 0.009 at 10 GHz and 25°C. In comparison with the 4,4′‐bismaleimidodiphenylmethane (BDM)/2,2′‐diallyl bisphenol A (DABPA) resin, the glass‐transition temperature (T_g) of 6FBMP/6FDABPA decreased. The flexible ether group in the long chain of 6FBMP was considered to disrupt chain packing and cause a decreased crosslinking density and a lower T_g. 6FBMP/6FDABPA showed a similar thermal decomposition temperature and good thermal properties like the BDM/DABPA resin, whereas the impact strength of the 6FBMP/6FDABPA resin was almost 1.6 times higher than that of the BDM/DABPA resin. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42791.     

Dielectric properties of isotactic polypropylene/nitrile rubber blends: Effects of blend ratio,filler addition,and dynamic vulcanization

The dielectric properties of isotactic polypropylene/acrylonitrile–butadiene rubber blends have been investigated as a function of frequency with special reference to the effect of blend ratio. The dielectric properties measured were volume resistivity, dielectric constant (ϵ′), dissipation factor (tan δ), and loss factor (ϵ″). At high frequencies, a transition in relaxation behavior was observed whereby the dielectric constant of the blends decreased with frequency, whereas the loss tangent and loss factor increased on reaching a maximum. The variation of the dielectric properties with blend composition was correlated with blend morphology, and relationships were established with reference to blend composition. Experimental ϵ′ values were compared with theoretical predictions. The effect of the addition of fillers on the dielectric properties was also investigated for different fillers and filler loadings. It was found that silica filler increases the dissipation factor, whereas carbon black and cork gave a reverse trend. The variation in dielectric properties upon dynamic vulcanization of the rubber phase using different vulcanizing agents (such as sulfur, peroxide, and mixed systems) was also investigated. © 1999 John Wiley & Sons, Inc. J Appl Polym Sci 73: 255–270, 1999     

Studies on dielectric relaxation and ac conductivity of cellulose acetate hydrogen phthalate–poly (vinyl pyrrolidone) blend

The dielectric constant, dielectric loss, and ac conductivity of polyblends of cellulose acetate hydrogen phthalate (CAP) and poly (vinyl pyrrolidone) (PVP) of different compositions were measured in the temperature range of 300–430 K and in the frequency range of 50 Hz–100 kHz. In the blends, the dielectric constant as well as the dielectric loss as a function of the temperature display a single peak corresponding to the glass transition temperature (T_g) in the region between the T_g values of the pure polymers. The T_g values observed agree well with those values obtained from DSC. Dielectric studies show that CAP forms a miscible blend with PVP. Ac conductivity values were calculated from the dielectric data and the conduction mechanism is discussed. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 1702–1708, 2002     

X‐ray irradiated LDPE/PP blends with high mechanical and dielectric performance

In this study, the influences of polypropylene (PP) additive (varying from 20% to 80% wt) and low dose X‐ray irradiation (changing from 25 to 100 Gy) on the mechanical and dielectric properties of low‐density polyethylene (LDPE) were investigated. LDPE/PP film blends were prepared by hot press technique. While the highest Young modulus and tensile strength were observed for the 20%LDPE/80%PP blend at 25 Gy X‐ray irradiation, the same blend had the highest energy at break and percentage strain at break values for 50 Gy X‐ray exposure. These results also indicated a chain scission in the material. The differential scanning calorimetry curves also indicated a chain scission and crosslinking effects in the blends due to X‐ray irradiation. Hence, the higher concentration of PP additive and exposure of low dose X‐ray resulted in a polymer composite with high mechanical performance. On the other hand, the dielectric investigations revealed that the 25 Gy X‐ray irradiated 20%LDPE/80%PP blend may also attract attention for capacitor applications due to its increased static dielectric constant and reduced dielectric loss. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46571.     

Mechanical and dielectric properties of polymer composites containing tubules

The thermal, dynamic mechanical, and dielectric properties of copper‐coated lipid tubules incorporated into three polyurethane matrices with varying surface tensions have been examined. The tubules did not affect the glass‐transition temperature of the polymer matrices, indicating that the tubule–polymer interactions may not be strong enough to restrict the mobility of polymer chains near the filler surface. The composite's elastic modulus can also be adequately modeled using the Nielsen equation. In addition, the real part of the permittivity for the composites increased monotonically over the tubule concentration range. All samples had a small imaginary part of the permittivity, indicating the tubule concentrations were below the percolation threshold concentration. Also, the three types of matrices had comparable permittivity values at each tubule concentration, suggesting the polymer surface tension did not affect the tubule distribution in the composite. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 88: 3218–3224, 2003     

Hyperbranched-polysiloxane-based hyperbranched polyimide films with low dielectric permittivity and high mechanical and thermal properties

A series of hyperbranched polysiloxane (HBPSi)-based hyperbranched polyimide (HBPI) films with low dielectric permittivity and multiple branched structures are fabricated by copolymerizing 2,4,6-triaminopyrimidine (TAP) with 4,4′-(hexafluoroisopropylidene)diphthalic anhydride, 4,4′-diaminodiphenyl ether, and HBPSi via the two-step polymerization method. The dielectric permittivity of HBPSi hyperbranched polyimide films decreases with increasing TAP fraction, namely, from 3.28 for sample PI-1 to 2.80 for PI-4, mainly owing to the enlarged free volume created by the incorporation of multiple branched structures. Moreover, HBPSi HBPI possesses desirable solubility and good mechanical properties and thermal stability. PI-4 not only has low dielectric permittivity (2.80, 1 MHz), excellent solubility (soluble in several common organic solvents), and remarkable thermal properties (glass-transition temperature of 273 °C, 5% weight loss temperature of 498 °C in N₂ and 486 °C in O₂), but it also demonstrates admirable mechanical properties with a tensile strength of 103 MPa, elongation at break of 7.3%, and a tensile modulus of 2.16 GPa. HBPSi HBPI might have potential applications in interlayer dielectrics and other microelectronics fields. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 47771.     

Simultaneously improving thermal conductivity and dielectric properties of poly(vinylidene fluoride)/expanded graphite via melt blending with polyamide 6

Poly(vinylidene fluoride)/polyamide 6/expanded graphite (PVDF/PA6/EG) composite is prepared via one-step melt extrusion. The EG is well dispersed with the addition of PA6 and mainly distributed in the PA6 phase due to the stronger affinity between them. As a result, the PVDF/PA6/EG sample presents higher dielectric permittivity than the PVDF/EG sample and maintain a low dielectric loss due to its sea-island phase structure, which impedes the formation of conductive path in the composite. The mean interlayer spacing of the EG in the polymer matrix decreases obviously due to its improved dispersion state, which is in favor of the phonon transportation in the composite. As a result, the PVDF/PA6/EG sample exhibits a significantly improved thermal conductivity of about 0.48 W m⁻¹ K⁻¹, which is 140% higher than that of the PVDF sample and 37% higher than that of the PVDF/EG sample. Moreover, the PVDF/PA6/EG sample presents higher Young's modulus and tensile strength than the PVDF/EG sample. While the elongation at break of the PVDF/PA6/EG sample is only a little lower than that of the PVDF/EG sample. This means that the tensile properties of the composite are not destroyed obviously by melt blending with the immiscible PA6.     

Synthesis,characterization and dielectric properties of nickel-based polyoxometalate/polyurethane composites

The aim of this study was to synthesis, characterization and investigation of the influence of the polyoxometalate concentrations (1, 3, 5 and 10 wt%) on chemical, thermal, physical and morphological properties of nickel-based polyoxometalate/polyurethane composite (Ni-POM/PU) materials. Firstly, nickel-based polyoxometalate (Ni-POM) compound has been synthesized and characterized through various spectroscopic techniques. Synthesized Ni-POM compounds have been used for preparation of polyurethane composites as a reinforcement. Three different Ni-POM/PU composites containing Ni-POM were prepared by solution mixing and casting techniques. The chemical structure and morphology of prepared Ni-POM/PU composite samples were confirmed by Fourier transform infrared spectroscopy (FTIR), elemental analysis and SEM techniques. Effects of Ni-POM on thermal stability, glass transition temperature, optical transparency, hydrophilicity and physical properties of polyurethane composites were examined. Thermal stabilities and glass temperatures of the materials have been checked by differential thermal analysis (DTA), thermogravimetric analysis (TGA) and differential scanning calorimeter (DSC). The SEM results confirmed the highly porous structure and the formation of Ni-POM structures in the polymer matrix. Synthesized composites showed high chemical stability, good processability, and low Tg values. The dielectric properties of the prepared Ni-POM/polyurethane composites were also investigated at room temperature. These results displayed that the dielectric constant of the POM/polyurethane composites decreased with the increase of the Ni-POM content in polymeric matrix.     

Mechanical,thermal, and dielectric properties of SiCf/SiC composites reinforced with electrospun SiC fibers by PIP

Electrospun unidirectional SiC fibers reinforced SiC_f/SiC composites (e-SiC_f/SiC) were prepared with ∼10% volume fraction by polymer infiltration and pyrolysis (PIP) process. Pyrolysis temperature was varied to investigate the changes in microstructures, mechanical, thermal, and dielectric properties of e-SiC_f/SiC composites. The composites prepared at 1100 °C exhibit the highest flexural strength of 286.0 ± 33.9 MPa, then reduced at 1300 °C, mainly due to the degradation of electrospun SiC fibers, increased porosity, and reaction-controlled interfacial bonding. The thermal conductivity of e-SiC_f/SiC prepared at 1300 °C reached 2.663 W/(m∙K). The dielectric properties of e-SiC_f/SiC composites were also investigated and the complex permittivities increase with raising pyrolysis temperature. The e-SiC_f/SiC composites prepared at 1300 °C exhibited EMI shielding effectiveness exceeding 24 dB over the whole X band. The electrospun SiC fibers reinforced SiC_f/SiC composites can serve as a potential material for structural components and EMI shielding applications in the future.