Tailoring the nonlinear conducting behavior of silicone composites by ZnO microvaristor fillers

Silicone composite filled with zinc oxide microvaristors possesses excellent nonlinear conducting behavior as ZnO varistor does. For better adjusting the composite's electrical behavior to satisfy the practical field‐grading requirement, this article studied the influence of ZnO filler's property on the nonlinearity of the composite. Several groups of ZnO‐silicone composite samples in different filler volume fraction and filler diameter were prepared, the measured J‐E characteristics show that the percolation threshold of ZnO‐silicone composite is around 35%, above which the composites present reliable nonlinear behavior. The switching voltage of the composite exhibits a considerable decrease as filler's diameter increases or filler's volume fraction increases, while the nonlinear coefficient remains stable. Moreover, filler's size also has a little influence on composite's percolation limit. The conclusion above fits very well with the theory of the conducting composites and percolation process. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42645.     

Preparation,Characterization, and Dielectric Properties of PP/CaTiO3 Composites for Microwave Substrate Applications

Calcium titanate (CaTiO₃) filled polypropylene (PP) composites have been fabricated through compression molding method. The phase purity of the PP/CaTiO₃ composites was studied using X‐ray diffraction studies. Scanning electron microscopy technique has been employed to study the dispersion of the particulate filler in the PP matrix. The dielectric constant and loss tangent of the composites were measured at X‐band frequency region using waveguide cavity perturbation technique. PP/CaTiO₃ composite has an effective dielectric constant of 11.74 and loss tangent 0.007 at optimum filler loading. The experimental dielectric constant of filled composites was compared with theoretically predicted dielectric constant values obtained using different modeling approaches. The linear coefficient of thermal expansion of PP/CaTiO₃ composites was studied using thermomechanical analyzer.     

Dielectric,Mechanical, and Thermal Properties of Low-Permittivity Polymer–Ceramic Composites for Microelectronic Applications

A new low-permittivity polymer–ceramic composite for packaging applications has been developed. The ceramic-reinforced polyethylene and polystyrene composites were prepared by melt mixing and hot molding techniques. Low-loss, low-permittivity Li₂MgSiO₄ (LMS) ceramics prepared by the solid-state ceramic route were used as the filler to improve the dielectric properties of the composites. The relative permittivity and dielectric loss were increased with the increase in the ceramic loading at radio and microwave frequencies. The mechanical properties and thermal conductivity of the Li₂MgSiO₄-reinforced polymer–ceramic composite were also investigated. The stability of the relative permittivity of polymer–ceramic composites with temperature and frequency was investigated. The experimentally observed relative permittivity, thermal expansion, and thermal conductivity were compared with theoretical models.     

Preparation,characterization, electrical and antibacterial properties of sericin/poly(vinyl alcohol)/poly(vinyl pyrrolidone) composites

In this study, we focused on the fabrication of poly(vinyl alcohol) (PVA)/poly(vinyl pyrrolidone) (PVP)/sericin composites via a simple solution‐blending method. The composites were characterized by Fourier transform infrared (FTIR) spectroscopy, UV spectroscopy, X‐ray diffraction (XRD), scanning electron microscopy (SEM), differential scanning calorimetry, thermogravimetric analysis (TGA), and measurements of the conductivity, tensile strength, and antibacterial activity against Staphylococcus aureus. The results of FTIR and UV spectroscopy implied the occurrence of hydrogen bonding between sericin and the PVA/PVP blend. The structure and morphology, studied by XRD and SEM, revealed that the sericin particles were well dispersed and arranged in an orderly fashion in the blend. The glass‐transition temperature (T_g) of the composite was higher than that of the pure blend, and the T_g value shifted toward higher temperatures when the volume fraction of sericin increased. TGA indicated that sericin retarded the thermal degradation; this depended on the filler concentration. The mechanical and electrical properties, such as the tensile strength, alternating‐current electrical conductivity, dielectric constant, and dielectric loss of the composites, were higher than those of the pure blend, and these properties were enhanced when the concentration of sericin was increased up to 10 wt % filler content, whereas the elongation at break of the composite decreased with the addition of sericin particles. The antibacterial properties of the composite showed that sericin had a significant inhibitory effect against S. aureus. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43535.     

Influence of Ca[(Li1/3Nb2/3)0.8Ti0.2]O3‐δ filler on the microwave dielectric properties of polyethylene and polystyrene for microelectronic applications

Ceramic reinforced polyethylene and polystyrene composites were prepared by melt mixing and hot molding techniques. Temperature stable low‐loss Ca[(Li_1/3Nb_2/3)_0.8Ti_0.2]O_3‐δ (CLNT) ceramic was used as the filler to improve the dielectric properties of the polymers. The relative permittivity and dielectric loss in the microwave frequency range were increased with increase in the ceramic loading. As the filler content increased from 0 to 0.50 volume fraction, the relative permittivity increased from 2.3 to 9 and dielectric loss tangent from 0.0006 to 0.005 for polyethylene‐CLNT composite. In the case of polystyrene‐CLNT composite, the relative permittivity and dielectric loss tangent increased from 2.1 to 10.5 and 0.0005 to 0.0032 respectively with increase in filler content from 0 to 0.50 volume fractions. The thermal stability of the relative permittivity of polymer ceramic composites was also investigated. The experimentally observed relative permittivity was compared with theoretical models. POLYM. ENG. SCI., 2010. © 2009 Society of Plastics Engineers     

Dielectric,magnetic, and mechanical properties of composites consisting of biopolymer chitosan matrix and hybrid spinel/cellulose filler

The composites consisting of a biopolymer chitosan matrix and hybrid spinel/cellulose filler were prepared by solvent casting method whereas the spinel CoFe₂O₄ was obtained by mechanical synthesis followed by thermal annealing. Incorporation of cellulose to the spinel – chitosan composite significantly modified dielectric, magnetic and mechanical properties of a composite consisting of the biopolymer with hybrid filler. In dielectric response the presence of the filler in the chitosan matrix hindered the molecular motion. The lowering of the activation energy and the cooperativity of the motion was observed. According to the magnetic properties, addition of cellulose to the filler enhanced coercivity field H_c in comparison to the pure spinel powder from value 0.1453 to 0.2033?T. In mechanical properties incorporation of the filler resulted in improvement of Young's modulus and tensile strength in comparison to unfilled chitosan. For composites with nanocellulose filler tensile strength was over two times higher than for chitosan.     

Study on the properties of crosslinking of poly(ethylene oxide) and hydroxyapatite–poly(ethylene oxide) composite

This study covers the crosslinking of poly(ethylene oxide) (PEO) and its composite with calcium hydroxyapatite (HA), their mechanical and swelling properties, and morphology. Sheets of the composites of PEO (two different grades with M_v: 5 × 10⁶ and 2 × 10⁵) and HA and neat PEO were prepared by compression molding. The prepared composite and PEO (0.1‐mm‐thick) sheets were crosslinked with exposure of UV‐irradiation in the presence of a photoinitiator, acetophenone (AP). This simple method for crosslinking, induced by UV‐irradiation in the presence of AP, yielded PEO with gel content up to 90%. Gel content, equilibrium swelling ratio, and mechanical and morphological properties of the low molecular weight polyethylene oxide (LMPEO)–HA crosslinked and uncrosslinked composites were evaluated. Although the inclusion of HA into LMPEO inhibits the extent of crosslinking, the LMPEO–HA composite with 20% HA by weight shows the highest gel content, with appreciable equilibrium swelling and mechanical strength. The growth of HA in simulated body fluid solutions on fractured surfaces of LMPEO and also LMPEO–HA was found to be very favorable within short times. The dimensional stability of these samples was found to be satisfactory after swelling and deposition experiments. The good compatibility between the filler hydroxyapatite and poly(ethylene oxide) makes this composite a useful tissue‐adhesive material. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 90: 488–496, 2003     

Electrical and thermal properties of γ‐irradiated nitrile rubber/rice husk ash composites

The effects of both the rice husk ash (RHA) loading and fumed silica (FS) loading on the structure, thermal stability, and electrical properties of acrylonitrile–butadiene rubber (NBR) composites were studied. The filler loading were chosen to be 5 and 20 phr for RHA and 5 and 30 phr for silica. Also, the effect of the γ‐irradiation dose (25 kGy) on these parameters was investigated. The structure and thermal stability were studied with X‐ray diffraction and thermogravimetric analysis techniques. Furthermore, some electrical parameters, such as the direct‐current electrical conductivity (σ_dc), activation energy (E_a), dielectric constant (?′), and dielectric loss (?″), were determined. The incorporation of both RHA and FS resulted in improved thermal stability after γ irradiation at 25 kGy. The loading of FS on NBR was shown to decrease σ_dc, ?′, and ?″ and increase E_a. On the other hand, the loading of RHA showed the opposite trend. Finally, γ irradiation of NBR composites filled with both fillers decreased the values of σ_dc, ?′, and ?″ for all the samples, which followed the trend for the unirradiated composites. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2010     

The mechanism for inorganic fillers accelerating and inhibiting the UV irradiation aging behaviors of rigid poly(vinyl chloride)

The UV irradiation aging behaviors of PVC composites with several inorganic fillers were studied through Fourier transform spectroscopy (FTIR), ultraviolet spectroscopy (UV‐Vis), differential scanning calorimeter (DSC), scanning electron microscopy (SEM), and mechanical property test. It was found that incorporation of a small amount of the inorganic fillers such as CaCO₃, talc and SiO₂ could hold up the UV aging behaviors of PVC. Those filler‐filled PVC composites sheets after 20 days UV irradiation maintain lower carbonyl index (CI) and good appearance of surfaces, as compared with the corresponding neat PVC sheets, ascribed to high reflection of those fillers to UV light. While montmorillonite (MMT) and pyrophyllite fillers could accelerate the UV aging behaviors of PVC, which could be concluded from both the sharp increase of the CI and lower T_g due to the chain scission reactions because of their high absorbance of these fillers to UV light in 290–400 nm. In these two PVC composites, UV irradiation caused the deterioration of their mechanical properties and the appearance of rough, cracked and chalked surfaces after 20 days UV irradiation. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Microwave dielectric properties of flexible butyl rubber–strontium cerium titanate composites

Butyl rubber–strontium cerium titanate (BS) composites have been prepared by hot pressing. The tensile tests show that the BS composites are flexible. The dielectric properties of the composites have been investigated at 1 MHz and 5 GHz as a function of ceramic contents. The composite with volume fraction 0.43 of ceramic filler has a dielectric constant (ε_r) of 11.9 and dielectric loss (tan δ) 1.8 × 10^?3 at 5 GHz. The measured values of ε_r are compared with the effective values calculated using different theoretical models. The thermal conductivity of the composites is found to increase with ceramic contents and reaches a value of 4.5 Wm^?1 K^?1 for maximum filler loading 0.43 volume fraction. The coefficient of thermal expansion of the composites decreases gradually with filler loading and reaches a minimum value of 30.2 ppm °C^?1 at a volume fraction 0.43. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Thermal properties and processability of talc‐ and calcium carbonate‐filled poly(vinyl chloride) hybrid composites

The main objective of this investigation was to study and compare the thermal rigidity, thermal stability, and processability of poly(vinyl chloride) (PVC) composites filled with single fillers of talc and uncoated ground CaCO₃ (SM 90) or a hybrid filler consisting of talc/SM 90. To produce the composites, the PVC resin, fillers, and other additives were dry‐blended in a laboratory mixer before being milled into sheets by using a two‐roll mill. Test specimens were prepared by compression molding, after which the thermal properties and processability of the composites were determined. Single and hybrid filler loadings used were fixed at 30 phr (parts per hundred parts of resin). Talc‐filled PVC composite showed slightly better thermal stability and rigidity than the composite filled with SM 90, and its thermal stability and rigidity slightly decreased with SM 90 content increasing from 5 to 25 phr in order to replace talc filler in the hybrid composites. The fusion time of talc‐filled PVC composite was shorter than that of SM 90‐filled PVC composite; thus, the fusion time of hybrid composites increased with increasing SM 90. The fusion torque showed an opposite behavior. J. VINYL ADDIT. TECHNOL., 2012. © 2012 Society of Plastics Engineers     

Changes in morphology and properties by grafting reaction in PP/EOR/CaCO3 ternary composites

The phase morphology and mechanical properties of polypropylene (PP) composites containing ethylene–octene elastomer (EOR) and calcium carbonate (CaCO₃) filler were investigated by comparing the toughening effect of unmodified EOR with EOR grafted with maleic anhydride (EOR–MA). EORs of various MA contents were prepared by free‐radical grafting of MA onto the EOR backbone using a reactive extrusion process. The composite morphology was directly explored by scanning electron microscopy technique and indirectly explored by differential scanning calorimetry and dynamic mechanical analysis. Separate dispersion of the elastomer and filler particles was achieved by using unmodified EOR. Modification of EOR by maleic anhydride grafting resulted in encapsulation of the filler particles. The mechanical properties of the composites were found to depend mainly on composite morphology and composition and, to a lesser degree, on maleic anhydride concentration. The results of this study showed that when composites contained an equal or higher amount of elastomer relative to filler, a composite with a separate dispersion structure was preferred. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 89: 3557–3562, 2003     

Electrical and thermal studies of the distribution of carbon black in a polyester matrix in the presence of aluminum oxide

The distribution of a filler in a polymeric matrix is one of the most important factors affecting the physical properties of the final product. For this reason, the main objective of this study was to introduce aluminum oxide (Al₂O₃), acting as a dispersing agent, to reduce the filler–filler interaction and enhance the filler–polymer interaction. To achieve this aim, the electrical behavior of a styrenated polyester resin filled with different amounts of high‐abrasion furnace black in the presence of 5% Al₂O₃ was studied in the vicinity of the percolation threshold to evaluate the effect of the addition of Al₂O₃ in an attempt to reduce the filler–filler interaction through the polyester matrix. At a certain concentration of carbon black, an abrupt increase was noticed through electrical conductivity, permittivity, and dielectric loss investigations. With this increase, the tendency of conductive chain formation increased through the aggregation of a carbon black particle network. The addition of 5% Al₂O₃ improved the filler distribution by lowering the aggregate size and consequently enhanced the formation of the network. From the Arrhenius temperature dependence of the electrical conductivity, the activation energy and pre‐exponential factor were obtained, and they confirmed the validity of the compensation law for the semiconducting composite systems. The composites were also analyzed by thermogravimetric analysis. Al₂O₃ improved the thermal stability of the composites in comparison with that of a sample free of Al₂O₃. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Improving mechanical properties of poly(vinyl chloride) by doping with organically functionalized reactive nanosilica

Nanosilica particles are functionalized by in situ surface‐modification with trimethyl silane and vinyl silane. Resultant reactive nanosilica (coded as RNS) contains double bonds and possesses good compatibility with vinyl chloride (VC) and polyvinyl chloride (PVC). This makes it feasible for RNS to copolymerize with VC generating RNS/PVC composites via in situ suspension polymerization. As‐prepared RNS/PVC composite resins are analyzed by means of FTIR. The tensile strength and impact strength of compression‐molded RNS/PVC composites are measured and compared with that of compression‐molded PVC composites doped with dispersible nano‐SiO₂ particles (abridged as DNS) surface‐modified with trimethyl silane alone. Moreover, the thermal stability of compression‐molded RNS/PVC and DNS/PVC composites is evaluated by thermogravimetric analysis. It has been found that RNS/PVC composites possess greatly increased impact strength and tensile strength than PVC matrix, while DNS/PVC composites possess higher impact strength than PVC matrix but almost the same tensile strength as the PVC matrix. This implies that DNS is less effective than RNS in improving the mechanical strength of PVC matrix. Particularly, RNS/PVC composites prepared by in situ suspension polymerization have much higher mechanical strength than RNS/PVC composites prepared by melt‐blending, even when their nanosilica content is only 1/10 of that of the melt‐blended ones. Besides, in situ polymerized RNS/PVC and DNS/PVC composites have better thermal stability than melt‐blended nanosilica/PVC composites. Hopefully, this strategy, may be extended to fabricating various novel high‐performance polymer‐matrix composites doped with organically functionalized nanoparticles like RNS. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

Thermal,mechanical, and dielectric properties of aluminum silicate fiber reinforced aluminum phosphate–poly(ether sulfone) layered composites

In this study, a novel aluminum phosphate (AlPO₄) heat‐resistant layer reinforced with aluminum silicate fiber (ASF) was successfully compounded on a poly(ether sulfone) (PES) matrix via the preparation process of high‐temperature heat treatment and vacuum hot‐pressing sintering technique. The influence of the ASF content on the morphology, thermal, mechanical, and dielectric properties of the as‐fabricated aluminum silicate fiber reinforced aluminum phosphate–poly(ether sulfone) (ASF/AlPO₄–PES) layered composite was investigated. The results reveal that the incorporation of aluminum silicate fiber/aluminum phosphate (ASF/AlPO₄) heat‐resistant layer can significantly improve the thermal stability and mechanical performances of the PES matrix composites. Compared with the pristine PES, the ASF/AlPO₄–PES layered composite containing 8.0 wt % ASF exhibited better high‐temperature resistance properties (300 °C) and a lower thermal conductivity (0.16 W m^?1 K^?1). Furthermore, the dielectric constant and dielectric loss tangent of this PES matrix composite decreased to 2.16 and 0.007, respectively. Meanwhile, the frequency stability of the dielectric properties for the ASF/AlPO₄–PES layered composites was remarkably enhanced with increasing ASF addition at frequencies ranging from 10² Hz to 5 MHz. This was attributed to the existence of microscopic pores within the ASF/AlPO₄ layer and the strong interfacial bonding between the ASF/AlPO₄ layer and the PES matrix. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134 , 45542.     

Low dielectric loss BST/PTFE composites for microwave applications

Ba_0.3Sr_0.475Ce_0.03La_0.12Ti_0.997Mn_0.003O₃/Polytetrafluoroethylene (PTFE) composites were prepared using powder processing technique. The effects of the ceramic filler volume fraction and the coupling agent on the phase composition, microstructure, dielectric and thermal properties of the composites were investigated in this paper. The ceramic filler dispersion in the PTFE matrix, thus the dielectric loss, permittivity, and dimensional thermal stability of the composite was considerably improved by the modification of BST filler surface using phenyl trimethoxy silane (PTMS) coupling agent. Variation of the dielectric permittivity of the composite with composition was well fitted by the effective medium theory (EMT) model in the experimental compositional range. The obtained silane-treated composite with 0.5 V_f BST exhibits extremely low dielectric loss: ε_r = 16, tan δ = 5.4 × 10⁻⁴ @1 MHz and 5.16 ± 0.6 × 10⁻³ @ 10 GHz. The CTE of the composites was reduced to 43 ppm/°C.     

Effects of acrylic‐based processing aids on processibility,rheology, thermal and structural stability,and mechanical properties of PVC/wood–sawdust composites

Methyl methacrylate and ethylacrylate (MMA‐co‐EA) and methyl methacrylate and butylacrylate (MMA‐co‐BA) copolymeric processing aids were introduced into poly(vinyl chloride) (PVC)/33.3 wt % wood–sawdust composites containing 0.6 and 2.4 phr of calcium stearate lubricant. The properties of the composites were monitored in terms of processibility, rheology, thermal and structural stability, and mechanical properties. It was found that the mixing torque, wall shear stress, and extrudate swell ratio increased with increasing processing aid content because of increased PVC entanglement. MMA‐co‐BA (PA20) was found to be more effective than MMA‐co‐EA (K120 and K130), this being associated with the flexibility of the processing aids, and the dipole–dipole interactions between sawdust particles and polymeric processing aids. The sharkskin characteristic of the composite extrudate at high extrusion rate was moderated by the presence of processing aids. Adding the acrylic‐based processing aids and lubricant into PVC/sawdust composites improved the thermal and structural stability of the composites, which were evidenced by an increase in glass transition and decomposition temperatures and a decrease in polyene sequences, respectively. The changes in the mechanical properties of the composites involved a composite homogeneity, which was varied by degree of entanglement and the presence of wood sawdust, and un‐reacted processing aids left in the composites. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 92: 782–790, 2004     

Percolation phenomena in polymers containing dispersed iron

Metal‐polymer composites based on polyethylene (PE), polyoxymethylene (POM), polyamide (PA) and a PE/POM blend as matrix and dispersed iron (Fe) as filler have been prepared by extrusion of the appropriate mechanical mixtures, and their electrical conductivity, dielectric properties and thermal conductivity have been investigated. The filler spatial distribution is random in the PE‐Fe, POM‐Fe and PA‐Fe composites. In the PE/POM‐Fe composite the polymer matrix is two‐phase and the filler is contained only in the POM phase, resulting in an ordered distribution of dispersed Fe in the volume of polymer blend. The transition through the percolation threshold ?_c is accompanied by a sharp increase of the values of conductivity σ, dielectric constant ε′ and dielectric loss tangent tan δ. The critical indexes of the equations of the percolation theory are close to the theoretical ones in the PE‐Fe and POM‐Fe composites, whereas they take unusually high values in the PE/POMFe composite. Thus, t in the equation σ ～ (φ – φ_c)^t is 2.9–3.0 in the systems characterized by random distribution of dispersed filler and 8.0 in the PE/POM‐Fe system. The percolation threshold φ_c depends on the kind of polymer matrix, becoming 0.21, 0.24, 0.29 and 0.09 for the composites based on PE, POM, PA and PE/POM, respectively. Also the thermal parameters of the PE/POM‐Fe composite are different from those of all other composites. A model explaining the unusual electrical characteristics of the composite based on the polymer blend (PE/POM‐Fe) is proposed, in agreement with the results of optical microscopy.     

Preparation and dielectric properties of (Ba0.5Sr0.4Ca0.1)TiO3/polystyrene composites

Polymer composites with polystyrene (PS) as matrix and (Ba_0.5Sr_0.4Ca_0.1)TiO₃ (BSCT) as fillers are prepared by solution casting method. It is found that the dielectric constant of the prepared BSCT/PS composites increases with increasing filler content over the frequency range from 100 Hz to 500 MHz. And the dielectric properties of the composites show a good temperature independency over the range of ?30°C to 80°C. For the composite with 50 vol % filler content, the dielectric constant and dielectric loss are comparable with the literature values reported for other PS composites used for microwave substrate. Several theoretical models are used to compare with the experimental data of the dielectric constant of the composites. The microstructure and thermal properties of the composites were also studied. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41398.     

Investigation of conductivity characteristics of nitrile butadiene rubber vulcanizates filled with semiconducting carbide ceramic

SiC‐ and B₄C‐filled NBR rubber composites were prepared with various volume fractions of filler by a conventional roll‐mill method. The morphological structures of the NBR–SiC and NBR–B₄C composites were analyzed by scanning electron microscopy. The dependence of room‐temperature volume resistivity (ρ_v) on the concentration of filler in the two systems was studied. In addition, variation in the number of current carriers (n), mobility carriers (μ), dielectric constant (ε), and dielectric loss factor (tan δ) on filler concentration in the two systems were investigated in detail. The applicability of composites as negative temperature coefficient (NTCR) linear thermistors was studied by the dependence of volume resistivity on temperature. The resistivity showed negative temperature dependence and changed linearly with temperature parallel. The conduction mechanism of the conductivity of the two composites was analyzed in terms of the computed activation energy and hopping energy. Change in volume resistivity as a function of frequency for the two systems was also investigated. Finally, the dependence of volume resistivity on applied pressure and possible real applications of these composites as transducers in pressure sensors were also studied. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 103: 2158–2165, 2007