Rheological Percolation Threshold Research Articles

Rheological and electrical percolation of reinforced soft polyvinyl chloride composites with different morphological carbon fillers

The study analyzed the electrical properties, mechanical performance, and rheological behavior of three kinds of high plasticizer-content polyvinyl chloride (PVC) composites, herein referred as SCBC, EGC and MCNTC, respectively filled with porous superconductive carbon black (SCB), flake-like expanded graphite (EG), and tubular multi-walled carbon nanotubes (MCNT). The impact of the conductive fillers' morphology on the electrical percolation and viscoelastic percolation performance of the composites were investigated to understand the conductive mechanisms. It revealed that the incorporation of SCB and MCNT can induce both viscoelastic and electrical percolation in the composites. The thresholds for viscoelastic percolation for SCBC and MCNTC are between 2.35-3.11 vol% and 2.72–3.59 vol%, respectively, which are lower than their electrical percolation thresholds of 3.85 vol% for SCBC and 3.65 vol% for MCNTC. The nature of PVC chains, which can transmit force but not electrons, results in a higher electrical percolation threshold than the rheological percolation threshold. Despite MCNT's poorer dispersion, its high aspect ratio and one-dimensional tubular shape enabled it to achieve electrical percolation at a lower loading level. Due to the poor dispersion, EG did not cause either viscoelastic or electrical percolation in the composites within the 0–9 vol% range.

Matching Low Viscosity with Enhanced Conductivity in Vat Photopolymerization 3D Printing: Disparity in the Electric and Rheological Percolation Thresholds of Carbon-Based Nanofillers Is Controlled by the Matrix Type and Filler Dispersion

Matching Low Viscosity with Enhanced Conductivity in Vat Photopolymerization 3D Printing: Disparity in the Electric and Rheological Percolation Thresholds of Carbon-Based Nanofillers Is Controlled by the Matrix Type and Filler Dispersion

Rheological percolation, gel‐like behavior and electrical conductivity of multi‐walled carbon nanotubes filled ethylene‐vinyl acetate copolymer/acrylonitrile‐butadiene rubber nanocomposites

AbstractReasonable studies on the composite systems containing conductive nanoparticles are very important to manufacture the materials with physico‐mechanical tailor‐made properties. In this work, rheological percolation, gel‐like behavior and electrical properties of multi‐walled carbon nanotubes (MWCNTs) filled ethylene‐co‐vinyl acetate/acrylonitrile‐butadiene copolymer blends containing 0–7 wt% MWCNTs were studied. The Winter‐Chambon criterion validity was evaluated for physical gelation of the system. The rheological and electrical percolation threshold, gel point (Pg), relaxation exponent (n), gel strength (Sg), and the fractal dimension (df) at the gel point were calculated. The formation of physical gel and rheological percolation threshold were both found to occur at 1 wt% MWCNTs concentration. Based on the df value determined, it was revealed that the system behaved similar to the one in which the excluded volume interactions were nearly screened. It was also found that the storage modulus (G′) near the Pg followed a power‐law scaling relationship in the form where is the distance from Pg. The electrical conductivity of the nanocomposites increased with the increase in MWCNTs loading after the nanofillers content surpassed a certain value. A schematic model was proposed to demonstrate the variation of electrical conduction with the increase in MWCNTs concentration. The excluded volume and hard‐core models were also employed to estimate the average aspect ratio of the nanofillers embedded in the system.Highlights Morphology and gel‐like behavior of EVA/NBR/MWCNTs system were studied Winter‐Chambon criterion was found to be valid for the gelation of the system Rheological percolation and gel point were occurred at the same MWCNTs loading It was found excluded volume interactions were nearly screened at gel point A schematic model for microstructure development was suggested for the system

Preparation and properties of double percolated co-continuous PC/PET/MWCNT/GNP engineering polymer blend nanocomposites

This study reports on the preparation and characterization of nanocomposites based on polycarbonate (PC)/poly ethylene terephthalate (PET) blend containing low amounts of hybrid of multiwalled carbon nanotube (MWCNTs) and graphene nanoplates (GNPs) by melt mixing. To use double percolation mechanism, at first a co-continuous polymer blend was prepared and the influence of nanofiller content on morphology, electrical conductivity, rheological and mechanical properties of co-continuous PC/PET blend was investigated. Blend containing 60 wt. % PET showed co-continuous morphology as observed by scanning electron microscopy and it was found that co-continuity remained unchanged by the addition of nanofillers. The direct current (DC) electrical conductivity results showed a low electrical percolation threshold around 0.5 phr. The results obtained from differential scanning calorimetry (DSC) and thermal gravimetric analysis (TGA) showed an increase in thermal stability and crystallinity of nanocomposites. By increasing nanofiller amount, the storage modulus, loss modulus, and complex viscosity of samples increased as an indication of the strong network formation between nanofillers and polymer chains. The rheological percolation threshold was also found in the range of 2.5–3.5 phr of nanofillers. The tensile measurements results showed that the addition PC to PET increases the tensile strength of PET.

Toward understanding the crystallization behavior of polypropylene‐based nanocomposites: Effect of ethylene–octene copolymer and nanoclay localization

AbstractThe crystallization properties of polypropylene (PP), a widely used polymer in industry, can be modified to overcome its mechanical limitations. In the current work, we investigated the effect of ethylene octene copolymer (EOC), blend morphology, nanoclay loading, nano‐localization, and component ratios on PP/EOC crystallization behavior in various aspects, including crystallization rate, degree of crystallinity, nucleation state, and crystalline phases. The results revealed that adding EOC with varying ratios can decrease PP crystallinity both in degree and rate due to the partial miscibility of components through grafting. Furthermore, it was found that the effect of the nanoclay on the crystallization behavior of PP is dependent on the nanoclay loading and its localization in the blend. The nanoclay, therefore, served as a nucleation agent at low nanoparticle contents, accelerating the crystallization rate regardless of the blend's microstructure. However, the crystallization rate of the blend samples at high nanoclay contents (above the rheological percolation threshold) was strongly influenced by the type of morphology. Accordingly, high nanoclay concentrations in blends with matrix‐dispersed morphologies reduced crystallization rates (increasing half‐time from 164 to 216 and 186 s), primarily because PP chains slowed down due to their interactions with nanoparticles and nanoclay hindrance. In contrast, in a blend with a co‐continues‐type morphology, the crystallization rates increased (decreasing half‐time from 624 to 270 and 236 s) due to nano‐localization at the interface and morphology transformation to the matrix‐dispersed one. The blends and nanocomposites based on PP/EOC were also investigated to determine the relationship between the crystallization behavior and mechanical properties.

Effect of specific surface area on the rheological properties of graphene nanoplatelet/poly(ethylene oxide) composites

The rheological properties of poly(ethylene oxide) containing graphene nanoplatelets (GNPs) having different specific surface areas (SSAs) are studied using steady shear and small amplitude oscillatory shear experiments. A series of GNPs having SSAs ranging from 175 ± 5 to 430 ± 13 m2/g was prepared using a thermomechanical exfoliation process. The complex viscosity, moduli, and yield stress of the composites increase with SSA, whereas electrical and rheological percolation threshold concentrations decrease, suggesting that higher SSAs promote filler network formation. Modeling of small amplitude oscillatory shear data using a two-phase model confirms that hydrodynamic effects dominate at low concentrations below 8 wt. %, where the particles are noninteracting. At higher concentrations, the response is dominated by filler-phase contributions. We demonstrate that the two-phase model parameters can be used to track the exfoliation of graphite into GNPs. Fitting of rheological percolation curves using Utracki and Lyngaae–Jørgensen models at low concentrations (noninteracting regime) resulted in aspect ratios between 19 and 76. At high concentrations (interacting particles), the aspect ratios determined by the Krieger–Daugherty model ranged between 5 and 24 due to aggregation. The highest aspect ratios (defined as the ratio of major dimension to minor dimension) were associated with GNPs that had the highest SSA of 430 m2/g. Strain sweeps revealed that the critical strain for the onset of nonlinear viscoelasticity scaled with SSA above the percolation threshold. The scaling relationships of the critical strain and storage modulus with volume fraction were used to infer the fractal dimensions of filler networks.

A comparative study on nanoparticle network‐dependent electrical conductivity, electromagnetic wave shielding effectiveness and rheological properties in multiwall carbon nanotubes filled polymer nanocomposites

AbstractHerein, a comparative study for the effect of nanoparticle networks on rheological behavior, electrical conductivity, and electromagnetic wave (EMW) shielding effectiveness (SE) is carried in conductive polymer composites (CPC). Two different polymers, that is, poly(ε‐caprolactone) (PCL) and isotactic polypropylene (iPP), which have different dispersion of multiwall carbon nanotubes (MWCNT), are used as polymer matrices. A transmission electron microscope (TEM) and a scanning electron microscope (SEM) are employed to determine the dispersion of MWCNTs in different polymer matrices. A rotational rheometer and a vector network analyzer are used to evaluate the percolation thresholds of storage modulus, complex viscosity and EMW SE, respectively. The results indicate that the EMW SE percolation thresholds are much larger than the electrical and rheological percolation thresholds. Specifically, the percolation thresholds of storage modulus and complex viscosity are 0.39 and 0.33 vol% for the MWCNT/PCL samples, and 1.57 and 1.57 vol% for the MWCNT/iPP samples, respectively. The electrical and EMW SE percolation thresholds are 0.33 and 1.99 vol%, 1.24 and 5.41 vol% for the MWCNT/PCL and MWCNT/iPP nanocomposites, respectively. The electrical and rheological percolation may happen in the samples with a sparse MWCNT network, while EMW SE percolation may require a dense MWCNT network in the samples.

Estimation of rheological percolation threshold and influence of fibre length on properties of polypropylene/sisal fibre composites having near critical fibre length

In this paper, the rheological percolation threshold and the hardness of Polypropylene/Sisal fibre (PP/SF) composites were correlated. Power law fit was implemented for the estimation of rheological percolation threshold. Further, the performance properties of PP/SF composites having near-critical length fibre (NCLF) and short fibre were investigated in terms of thermomechanical, rheological, and dynamic mechanical parameters. The Shore D hardness data revealed that the rheological percolation threshold of the prepared composites remained in the range of 20–30 wt% of sisal fibre. Moreover, sisal fibre had an undeniable impact on the dynamic mechanical properties of the prepared composites. Further, the rise in the onset degradation temperature by 40 °C proved the improvement in thermal stability of the prepared composites. It was also found that PP/SF composite having 20 wt% of near critical length fibre had properties equivalent to that of PP/SF composite having 40 wt% of short fibre (fibre length less then critical fibre length). • Correlation between Rheological Percolation threshold and Shore D hardness. • PP/SF composites having near critical length fibres. • Effect of fibre length on performance properties of PP/SF composites.

Fabrication of PLA/PCL/Graphene Nanoplatelet (GNP) Electrically Conductive Circuit Using the Fused Filament Fabrication (FFF) 3D Printing Technique.

For the purpose of fabricating electrically conductive composites via the fused filament fabrication (FFF) technique whose properties were compared with injection-moulded properties, poly(lactic acid) (PLA) and polycaprolactone (PCL) were mixed with different contents of graphene nanoplatelets (GNP). The wettability, morphological, rheological, thermal, mechanical, and electrical properties of the 3D-printed samples were investigated. The microstructural images showed the selective localization of the GNPs in the PCL nodules that are dispersed in the PLA phase. The electrical resistivity results using the four-probes method revealed that the injection-moulded samples are insulators, whereas the 3D-printed samples featuring the same graphene content are semiconductors. Varying the printing raster angles also exerted an influence on the electrical conductivity results. The electrical percolation threshold was found to be lower than 15 wt.%, whereas the rheological percolation threshold was found to be lower than 10 wt.%. Furthermore, the 20 wt.% and 25 wt.% GNP composites were able to connect an electrical circuit. An increase in the Young’s modulus was shown with the percentage of graphene. As a result, this work exhibited the potential of the FFF technique to fabricate biodegradable electrically conductive PLA-PCL-GNP composites that can be applicable in the electronic domain.

Scalable production of crosslinked rubber nanofibre networks as highly efficient toughening agent for isotactic polypropylene: Toughening mechanism of Non-traditional anisotropic rubber inclusion

Incorporation of homogenous rubber microparticles is a widely adopted toughening method for extending the range of applications of polypropylene (PP). Herein, a new toughening strategy with nano-structured rubber inclusion is devised and its efficiency is evaluated against the classical counterpart. The presented methodology integrates two well-established processes, namely vulcanization and in situ fibrillation, to allow scalable fabrication of PP nanocomposites toughened with crosslinked ethylene-propylene-diene terpolymer (EPDM) nanofibrils, which is otherwise technologically challenging. Morphological observation of the PP nanocomposites, supported by the drastic change in rheological behaviour under shear flow, substantiates the self-assembly of physical EPDM network nanostructure throughout the entire composite system above their rheological percolation threshold. The distinct morphology imparts unique characteristics that are vastly different from classical PP blends produced with the equivalent material composition. Massive improvement in macroscopic fracture behaviour is observed as the tensile fracture toughness is markedly enhanced at a comparatively low EPDM loading while the yield strength and elastic modulus are only marginally decreased. In our attempt to explain the superior toughening efficiency of crosslinked EPDM nanofibrillar network, we propose a collective toughening mechanism which is possibly triggered by several micro-scale mechanisms in play. This industrially relevant process potentially opens up a new avenue in material design for high-volume/lost-cost applications in the transportation sectors where excellent strength/toughness balance is indispensable.

Rheological, electrical, and dynamic thermomechanical properties: Comparison between multiwall and double-wall carbon nanotubes in polylactide and polyamide 11

In this study, multiwall carbon nanotubes (MWCNTs) and double-wall carbon nanotubes (DWCNTs) have been dispersed in polylactide (PLA) and polyamide 11 (PA11) using an internal mixer. Rheological characterization confirmed the formation of carbon nanotube (CNT) networks in PLA and PA11 attributed to well-dispersed CNTs in the respective matrices. A lower rheological percolation threshold of PLA/MWCNT nanocomposites (less than 0.5 wt. %) compared to PA11/MWCNT nanocomposites (about 2 wt. %) confirmed the greater affinity of CNTs for PLA. The threshold for DWCNTs was below 0.5 wt. % in PLA and between 0.5 and 1 wt. % in PA11. PLA-based nanocomposites also showed higher electrical conductivity values compared to PA11-based nanocomposites. Nanocomposites containing DWCNTs exhibited higher electrical conductivities compared to those containing MWCNTs due to the higher aspect ratio of DWCNTs. Dynamic mechanical thermal analysis showed enhanced storage modulus values and reduced damping behavior with increasing content of CNTs for both polymers.

Fabrication and characterization of piezoresistive flexible pressure sensors based on poly(vinylidene fluoride)/thermoplastic polyurethane filled with carbon black‐polypyrrole

AbstractElectrically conductive composites of thermoplastic polyurethane (TPU), poly(vinylidene fluoride) (PVDF), and carbon black‐polypyrrole (CB‐PPy) were prepared by melt compounding followed by compression molding or by filament production followed by fused filament fabrication (FFF). The storage modulus (G′) and complex viscosity (η*) of the composites increased with the addition of CB‐PPy leading to a more rigid material. The electrical and rheological percolation threshold of composites were 5 and 3 wt%, respectively. In fact, composites with 5 wt% or more CB‐PPy content display G′ higher than G″ indicating a solid‐like behavior. Furthermore, the addition of CB‐PPy increased the electrical conductivity of all composites. However, the electrical conductivity values of composites containing 5 and 6 wt% of CB‐PPy produced by compression molding are one and seven order of magnitude higher than those of FFF composites with same composition. Compression molded and 3D printed composites with 6 wt% of CB‐PPy displayed high sensitivity/gauge factor, large measurement range and reproducible piezoresistive response during 100 loading‐unloading cycles for both processing methods. The results presented in this study demonstrated the potential use of FFF for producing piezoresistive flexible sensors based on PVDF/TPU/CB‐PPy composites.

Comparison of Three Interfacial Conductive Networks Formed in Carbon Black-Filled PA6/PBT Blends.

Interfacial localization of carbon fillers in cocontinuous-structured polymer blends is well-known as a high-efficiency strategy for conductive network formation. However, a comparison with interfacial localization of carbon fillers in sea-island-structured polymer blends is lacking. Here, three types of highly efficient conductive networks formed on the basis of interfacial localization of carbon black (CB) in polyamide 6 (PA6)/poly(butylene terephthalate) (PBT) blends with different blend compositions (80/20, 50/50 and 20/80 vol/vol) were investigated and compared in terms of electrical resistivity, morphology as well as rheological and mechanical properties. The order of the electrical percolation threshold of CB in the three blends is 50/50 < 20/80 < 80/20, which can be attributed to different network structures. The rheological percolation thresholds are close to the electrical ones, confirming the formation of CB networks. The formation mechanisms for the three types of CB network structures are analyzed. All the three types of PA6/PBT-6 vol% CB composites showed improved tensile strength compared with PA6/PBT blends, being in favor for practical applications.

Characterizations of Polypropylene/Single-Walled Carbon Nanotube Nanocomposites Prepared by the Novel Melt Processing Technique with a Controlled Residence Time

Melt processing is considered one of the favored techniques to produce polymer nanocomposites with various inorganic fillers such as graphene and carbon nanotubes (CNTs). Due to their superior conductivity and tensile properties, among others, CNTs have been applied in broad applications. When a low filler fraction is desired, a high degree of dispersion is required in order to benefit from the intrinsic properties of CNTs. However, due to their high cohesive energy, dispersing CNTs in polymer melts is a difficult task. This study employed the melt mixing technique with a controlled residence time of 20 min to disperse single-walled carbon nanotubes (SWNTs) into a polypropylene matrix. The composites were prepared by using a corotating twin-screw extruder equipped with a back-conveying element with varying amounts of SWNTs from 0.29 to 6.56 wt.%. Mechanical, electrical, morphological, and rheological properties were evaluated. Due to the filler effect, storage, loss modulus, and complex viscosity increased with the SWNT content. Based on the van Gurp–Palmen plot, 0.29 wt.% SWNTs was the rheological percolation threshold, and the electrical property measurement revealed a 1.4 wt.% SWNT electrical percolation threshold based on the statistical percolation theory. Relatively large agglomerates were found when the SWNT content increased more than 1.28 wt.%.

Micro-Injection Molding of Polymer Nanocomposites Composition-Process-Properties Relationship

Abstract The mechanical, electrical, thermal, and rheological properties of micro injection molded nanocomposites comprising 2% and 5% carbon nanotubes (CNTs) incorporated in polycarbonate (PC), and polyamide 66 (PA) were studied. The design of experiments method was used to investigate the composition-process – properties relationship. Results indicated that the process variables significantly affected the flow patterns and resulting morphology during the filling stage of the microinjection molding (lIM) process, using 0.45 mm diameter lIM samples. Two distinct flow regimes have been identified in lIM using the low cross-section samples. The first was a conventional “fountain flow,” which resulted in a skin/core structure and reduced volume resistivity up to 10 X cm in the case of 5% CNTs and up to 100 X cm in 2% CNTs, in both polymers, respectively. In addition, inferior mechanical properties were obtained, attributed to polymer degradation under high shear rate conditions, when practicing high injection speeds, high mold temperatures, and high screw rotation velocities. The second was a “plug flow” due to wall slippage, obtained under low injection speeds, low mold temperatures, and low rotation velocities, leading to a substantial increase in modulus of elasticity (60%) with increased electrical resistivity up to 103 X cm for 5% CNTs and 105 X cm for 2% CNTs, respectively. The rheological percolation threshold was obtained at 2% CNTs while the electrical threshold was attained at 0.4% CNTs, in both polymers. It was concluded that in lIM, the process conditions should be closely monitored. In the case of high viscous heating, degradation of mechanical properties was obtained, while skin- core morphology formation enhanced electrical conductivity.

Composites of Cysteamine Functionalised Graphene Oxide and Polypropylene

Abstract Cysteamine functionalised reduced graphene oxide (rGO) was grafted to polypropylene-graft-maleic anhydride (PP-g-MA) and subsequently melt blended with PP. The covalent bridging of rGO to PP-g-MA via the cysteamine molecule and co-crystallization are routes to promoting interfacial interactions between rGO and the PP matrix. A rheological percolation threshold was achieved for a nanofiller loading between 3 wt% and 5 wt%, but none detected for the composites prepared with un-functionalized rGO. At low loadings (0.1 wt%), functionalized rGO is well dispersed in the PP matrix, an interconnecting filler-filler, polymer-filler and polymer-polymer network is formed, resulting in increased tensile toughness (1 500%) and elongation at break (40%) relative to neat PP. Irrespective of whether the rGO was functionalised or not, it had a significant effect on the crystallization behavior of PP, inducing heterogeneous nucleation, increasing the crystallisation temperature (Tm) of PP by up to 10°C and decreasing the crystalline content (Xc) by ∼30% for the highest (5 wt%) filler loading. The growth of the monoclinic a-phase of PP is preferred on addition of functionalised rGO and b crystal growth suppressed.

Evaluation of the rheological and electrical percolation of high‐density polyethylene/carbon black composites using mathematical models

AbstractIn this work, conductive polymer composites (CPCs) of bio‐based polyethylene (BioPe) containing different concentrations of carbon black (CB) were developed. By using oscillatory rheology analysis, a Newtonian plateau was observed in BioPe, and all BioPe/CB composites had a behavior of a pseudo‐solid and that composites with volume fractions ranging from 0.24 to 0.56 presented higher viscosity, storage, and loss modulus. This suggests the formation of a percolated network and by using the power‐law models, it was observed that the electrical percolation threshold was higher than the rheological percolation threshold. The electrical conductivity was measured using the four‐point probe method and a sigmoid model was used to predict the CPCs' electrical conductivity percolation threshold. The results indicated that the four‐point probe method presented satisfactory results according to the calculated standard deviations and voltage–current characteristics for each round of measurements considering the same ranging as used in rheology analysis. The analytical model used showed a coefficient of determination (R2) higher than 95%, allowing the prediction of the electrical conductivity of the CPC and the percolation threshold as a function of the volumetric fraction of the CB.

Matching Rheology, Conductivity and Joule Effect in PU/CNT Nanocomposites.

We investigated polyurethane (PU)–carbon nanotube (CNT) nanocomposites (PU/CNT) in a range of concentrations from 1 to 8 wt% CNT as hot melt adhesives. We studied the thermal properties of the nanocomposites, which is relevant from an applied point of view. The phase angle plots versus complex modulus results revealed the existence of a maximum above a given CNT concentration. The intensity of the peak and associated relaxation time was analyzed with percolation theory, leading to a new method to determine the rheological percolation threshold. A lower threshold value was obtained from the electrical conductivity data, which was justified recalling that the hopping/tunnelling effect takes place in the nanocomposite, as stated by previous studies in the literature. Joule effect studies indicated that the heating effect was very significant, reaching temperature increases, ΔT, of 60 °C for low voltages. For the first time, the percolation equation was applied to the ΔT to obtain the corresponding threshold. Stimulus-responsive systems were conceived considering the correlation between the ΔT and the conductivity. The case of PU/CNT nanocomposites acting as hot melt adhesives that are welded/unglued by applying/removing an electrical voltage is presented.

Electrical conductivity and rheological properties of carbon black based conductive polymer composites prior to and after annealing

The effect of annealing on the electrical and rheological properties of polymer (poly (methyl methacrylate) (PMMA) and polystyrene (PS)) composites filled with carbon black (CB) was investigated. For a composite with CB content near the electrical percolation threshold, the formation of conductive pathways during annealing has a significant impact on electrical conductivity, complex viscosity, storage modulus and loss modulus. For the annealed samples, a reduction in the electrical and rheological percolation threshold was observed. Moreover, a simple model is proposed to explain these behaviors. This finding emphasizes the differences in network formation with respect to electrical or rheological properties as both properties belong to different physical origins.

Electrical, rheological, and mechanical properties copolymer/carbon black composites

AbstractThis work aims to evaluate the electrical conductivity and the rheological and mechanical properties of copolymer/carbon black (CB) conductive polymer composites (CPCs). The copolymers, containing ethylene groups in their structure, used as matrix were polyethylene grafted with maleic anhydride (PEgMA), ethylene‐methyl acrylate–glycidyl methacrylate (EMA‐GMA), and ethylene‐vinyl acetate (EVA). For comparison purposes, bio‐based polyethylene (BioPE)/CB composites were also studied. The electrical conductivity results showed that the electrical percolation threshold of BioPE/CB composite was 0.36 volume fraction of CB, whereas the rheological percolation threshold was 0.25 volume fraction of CB. The most conductive CPC was BioPE/CB. Among the copolymer/CB CPCs, PEgMA/CB showed the highest conductivity, which can be attributed to the fact that the PEgMA copolymer had higher crystallinity. It also has a higher amount of ethylene groups in its structure. Torque rheometry analysis indicated that EMA‐GMA copolymer may have reacted with CB. Rheological measurements under oscillatory shear flow indicated the formation of a percolated network in BioPE/CB and copolymer/CB composites. Morphology analysis by scanning electron microscopy (SEM) indicated the formation of a percolated network structure in BioPE/CB composite and finely dispersed CB particles within the PEgMA copolymer. Wetting of CB particles/agglomerates by the copolymer matrix was observed in EVA/CB and EMA‐GMA/CB composites. Conductive CB acted as reinforcing filler as it increased the elastic modulus and tensile strength of BioPE and the copolymers.