Mechanical Behavior and Fracture Toughness of Poly(L‐lactic acid)‐Natural Fiber Composites Modified with Hyperbranched Polymers

Summary: The use of hyperbranched polymers (HBP) with hydroxy functionality as modifiers for poly(L ‐lactic acid) (PLLA)‐flax fiber composites is presented. HBP concentrations were varied from 0 to 50% v/v and the static and dynamic tensile properties were investigated along with interlaminar fracture toughness. Upon addition of HBP, the tensile modulus and dynamic storage modulus (E′) both diminished, although a greater decline was noticed in the static modulus. The elongation of the composites with HBP showed a pronounced increase as large as 314% at 50% v/v HBP. The loss factor (tan δ) indicated a lowering of the glass transition temperature (T_g) due to a change in crystal morphology from large, mixed perfection spherulites to finer, smaller spherulites. The change in T_g could have also resulted from some of the HBP being miscible in the amorphous phase, which caused a plasticizing effect of the PLLA. The interlaminar fracture toughness measured as the critical strain energy release rate (G_IC) was significantly influenced by HBP. At 10% v/v HBP, G_IC was at least double that of the unmodified composite and a rise as great as 250% was achieved with 50% v/v. The main factor contributing to high fracture toughness in this study was better wetting of the fibers by the matrix when the HBP was present. With improved ductility of the matrix, it caused ductile tearing along the fiber‐matrix interface during crack propagation.

ESEM photograph of propagation region of the interlaminar fracture toughness specimens with 30% v/v of HBP.     

Poly(3‐hydroxybutyrate)–thermoplastic starch–organoclay bionanocomposites: Surface properties

Bionanocomposites based on poly(3‐hydroxybutyrate) (PHB) and starch plasticized with glycerol and water [thermoplastic starch (TPS)] with organically modified montmorillonite clay as a nanofiller were obtained by melt‐blending. The influence of the clay and TPS on the thermal and mechanical properties of the resultant bionanocomposite was investigated by various techniques, such as X‐ray diffraction (XRD), scanning electron microscopy, transmission electron microscopy (TEM), atomic force microscopy (AFM), thermogravimetric analysis, differential scanning calorimetry, and nanoindentation. The results obtained by AFM showed that bionanocomposites have a surface roughness of 30.88 nm, compared to 14.53 nm for processed PHB. This result is obtained due to the migration of clay layers to the surface. From XRD and TEM it was determined that the clay layers of the bionanocomposites are completely separated. The hardness and elastic moduli of bionanocomposites have values similar to those of PHB, improving the drawbacks of the PHB–TPS blends (65:35 weight ratio). The thermal properties do not present significant changes, and only the degree of crystallinity decreased with increasing clay content. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45217.     

Poly(L‐lactic acid) nanocomposites with layered double hydroxides functionalized with ibuprofen

The detrimental effect of cell adhesion on polymer surfaces has been a limiting factor in the medical deployment of many implants. We examined the potential to decrease cell proliferation while simultaneously increasing mechanical performance through Zn–Al layered double hydroxide (LDH) organically modified with ibuprofen dispersed in poly(L ‐lactic acid) (PLLA). These composites are commonly referred to as nanocomposites. The thermophysical and mechanical properties of the hybrids were studied with wide‐angle X‐ray diffraction (WAXD), transmission electron microscopy (TEM), differential scanning calorimetry, thermogravimetric analysis, dynamic mechanical analysis, and tensile testing. The WAXD and TEM results indicated that intercalated and exfoliated nanocomposites were obtained. The storage modulus, tensile modulus, and ultimate tensile strength were improved. The LDH affected the cold crystallization and reduced the thermal stability of the neat PLLA. Smooth muscle cells were used for in vitro studies of the nanocomposites. It was found that the hybrids reduced cell proliferation, and the amount of cell reduction was related to ibuprofen release. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Morphology,Thermal and Mechanical Properties of Poly(propylene) Fibre‐Matrix Composites

Preparation and properties of poly(propylene)‐poly(propylene) composites have been investigated. Poly(propylene) fibres of varying diameter have been incorporated in a random ethylene co‐poly(propylene). The composites prepared from the same semi‐crystalline polymer in the matrix and reinforcement have lead to inherently strong interfacial bonding between the two phases of the same polymer. The composites demonstrated enhanced stiffness, which increased with fibre diameter. The structure, thermal, static and mechanical properties of poly(propylene) long fibre reinforced random co‐poly(propylene) composites have been studied with reference to the fibre diameter. The matrix and fibre components retained their separate melting temperatures. After melting, the two phases remained separate and showed their individual crystallization temperatures on cooling, and melting temperatures on a second heating. The melting temperature of the poly(propylene) fibres increased after formation of the composites. The compression molding of the composites at a temperature below the melting temperature of the fibres caused annealing of the fibre crystals. By incorporation of long poly(propylene) fibre into random co‐poly(propylene), the glass transition, storage and static modulus have been found to be increasing and composite with the largest fibre diameter shows better properties. Transcrystallization of the matrix poly(propylene) was observed.

Optical microscopy of composites with fibre diameter 68 μm.     

Wood‐fiber‐reinforced poly(lactic acid) composites: Evaluation of the physicomechanical and morphological properties

This article presents the results of a study of the processing and physicomechanical properties of environmentally friendly wood‐fiber‐reinforced poly(lactic acid) composites that were produced with a microcompounding molding system. Wood‐fiber‐reinforced polypropylene composites were also processed under similar conditions and were compared to wood‐fiber‐reinforced poly(lactic acid) composites. The mechanical, thermomechanical, and morphological properties of these composites were studied. In terms of the mechanical properties, the wood‐fiber‐reinforced poly(lactic acid) composites were comparable to conventional polypropylene‐based thermoplastic composites. The mechanical properties of the wood‐fiber‐reinforced poly(lactic acid) composites were significantly higher than those of the virgin resin. The flexural modulus (8.9 GPa) of the wood‐fiber‐reinforced poly(lactic acid) composite (30 wt % fiber) was comparable to that of traditional (i.e., wood‐fiber‐reinforced polypropylene) composites (3.4 GPa). The incorporation of the wood fibers into poly(lactic acid) resulted in a considerable increase in the storage modulus (stiffness) of the resin. The addition of the maleated polypropylene coupling agent improved the mechanical properties of the composites. Microstructure studies using scanning electron microscopy indicated significant interfacial bonding between the matrix and the wood fibers. The specific performance evidenced by the wood‐fiber‐reinforced poly(lactic acid) composites may hint at potential applications in, for example, the automotive and packaging industries. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 102: 4856–4869, 2006     

Plasticized poly(3‐hydroxybutyrate) with improved melt processing and balanced properties

The widespread application of poly(3‐hydroxybutyrate) (PHB) in the food packaging and biomedical fields has been hindered by its high brittleness, slow crystallization, poor thermal stability, and narrow processing window. To overcome these limitations, a mixture of biodegradable and biocompatible plasticizers was used to modify PHB. Epoxidized soybean oil (ESO), acetyl tributyl citrate, poly(ethylene glycol) 4000 (PEG4000), and poly(ethylene glycol) 6000 (PEG6000) were tested to improve PHB melt processing and to achieve balanced thermal and mechanical properties. These plasticizers increased the flexibility and decreased the melt viscosity, improving the processability. The tensile strength was maintained within the limit of experimental error for ESO and decreased slightly (6–7%) for the other plasticizers. PEG6000 and ESO delayed the decomposition process of PHB. The plasticizers did not hinder the crystallization, and poly(ethylene glycol)s increased the crystallinity. The change in the interplanar distance and crystallite size, correlated with lamellar stack dimensions, gave more information on the plasticizers' effects in PHB. The blend with 5 wt % ESO was considered suitable for the fabrication of marketable PHB films. This study showed that it is possible to tailor the rheological, thermal, and mechanical behavior of a commercial PHB through the addition of a second plasticizer. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 44810.     

Mechanical and thermal properties of poly(butylene succinate)/poly(3‐hydroxybutyrate‐co‐3‐hydroxyvalerate) biodegradable blends

Biodegradable polymer blends of poly(butylene succinate) (PBS) and poly(3‐hydroxybutyrate‐co‐3‐hydroxyvalerate) (PHBV) were prepared with different compositions. The mechanical properties of the blends were studied through tensile testing and dynamic mechanical thermal analysis. The dependence of the elastic modulus and strength data on the blend composition was modeled on the basis of the equivalent box model. The fitting parameters indicated complete immiscibility between PBS and PHBV and a moderate adhesion level between them. The immiscibility of the parent phases was also evidenced by scanning electron observation of the prepared blends. The thermal properties of the blends were studied through differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA). The DSC results showed an enhancement of the crystallization behavior of PBS after it was blended with PHBV, whereas the thermal stability of PBS was reduced in the blends, as shown by the TGA thermograms. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42815.     

Mechanical properties of poly(ε‐caprolactone) and poly(lactic acid) blends

The aim of this work was to better understand the performance of binary blends of biodegradable aliphatic polyesters to overcome some limitations of the pure polymers (e.g., brittleness, low stiffness, and low toughness). Binary blends of poly(ε‐caprolactone) (PCL) and poly(lactic acid) (PLA) were prepared by melt blending (in a twin‐screw extruder) followed by injection molding. The compositions ranged from pure biodegradable polymers to 25 wt % increments. Morphological characterization was performed with scanning electron microscopy and differential scanning calorimetry. The initial modulus, stress and strain at yield, strain at break, and impact toughness of the biodegradable polymer blends were investigated. The properties were described by models assuming different interfacial behaviors (e.g., good adhesion and no adhesion between the dissimilar materials). The results indicated that PCL behaved as a polymeric plasticizer to PLA and improved the flexibility and ductility of the blends, giving the blends higher impact toughness. The strain at break was effectively improved by the addition of PCL to PLA, and this was followed by a decrease in the stress at break. The two biodegradable polymers were proved to be immiscible but nevertheless showed some degree of adhesion between the two phases. This was also quantified by the mechanical property prediction models, which, in conjunction with material property characterization, allowed unambiguous detection of the interfacial behavior of the polymer blends. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Green composites of poly(3‐hydroxybutyrate) and curaua fibers: Morphology and physical,thermal, and mechanical properties

In this article, we report the morphology and thermal, mechanical and physical properties of poly(3‐hydroxybutyrate) (PHB)/curaua composites containing triethyl citrate (TEC) as the plasticizer. The composites were prepared by mechanical mixing using pristine and chemically treated fibers (10 wt %) and TEC (30 wt %) and characterized by differential scanning calorimetry, dynamic mechanical analysis, X‐ray diffraction, small angle X‐ray scattering, polarized optical microscopy, scanning electron microscopy, tensile tests, impact resistance test, thermodilatometry, and thermal conductivity measurements. The curaua fibers acted as nucleating agent and strongly influenced the morphology of the crystalline phase of PHB, increasing the lamella thickness, decreasing the crystal size and inducing spherulite–axialite transition. These characteristics of the PHB crystalline phase determined all the properties of the composites. The tensile properties of the composites were comparable with those of neat PHB, while the impact resistance of composites was comparable with that of plasticized PHB. The higher heat capacity and thermal expansion coefficient and the lower thermal conductivity of the composites compared with neat PHB reflect the morphological changes in the PHB crystalline phase. The strategy of developing a green polymeric material from ecofriendly components exhibiting a good balance of properties by combining curaua fibers, TEC, and PHB was successful. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 44676.     

Poly(lactic acid) and zeolite composites prepared by melt processing: Morphological and physical–mechanical properties

Poly(lactic acid), PLA, composites containing 0, 1, 3, and 5 wt % zeolite type 4A were prepared using extrusion/injection compounding techniques. Morphological characterizations were carried out by scanning electron microscopy (SEM) and transmission electron microscopy (TEM). Physical properties were evaluated by differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA) and mechanical properties by standard tensile testing. The morphological studies showed a homogenous dispersion of zeolite particles within the PLA matrix. As the fracture stress propagated, zeolite particles remained embedded into the matrix, indicating the existence of good interfacial adhesion between zeolite particles and the PLA matrix. The improvement in the interfacial adhesion was also confirmed by applying Nicolais‐Narkis and Pukanszky models. The percent crystallinity of the PLA and the temperature‐ dependant elastic and viscous modulus of the composite increased with the proportion of zeolites. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2010     

Production and properties of solvent‐cast poly(ε‐caprolactone) composites with carbon nanostructures

Composites based on carbon nanostructures (CNS) and poly(ε‐caprolactone) (PCL) were produced by solvent casting technique. Single‐walled carbon nanotubes (SWCNTs) and carbon nanofibers (CNFs) were selected, to produce composite films with enhanced properties. The role of CNS type and percentage were investigated in terms of morphological, thermal, mechanical, and dielectrical properties. Composite morphological analysis reveals a good dispersion of CNS, at low and high content. Thermal properties underline the nucleation effect of CNS on PCL polymer matrix. Reinforcing effects in terms of increased tensile modulus were obtained with both nanofillers, but a higher reduction of the ductility was shown in PCL/CNF materials. A higher efficiency to form a conductive network, assessed by AC conductivity, was observed for SWCNTs at concentration lower than 1 wt. % © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Properties of soy protein isolate/poly(ethylene‐co‐ethyl acrylate‐co‐maleic anhydride) blends

Blends of soy protein isolate (SPI) with 10, 20, 30, 40, and 50% poly(ethylene‐co‐ethyl acrylate‐co‐maleic anhydride) (PEEAMA), with or without addition of 2.0 wt % methylene diphenyl diisocyanate (MDI), were prepared by mixing with an intensive mixer at 150°C for 5 min, and then milling through a 1‐mm sieve. Blends were then compression‐molded into a tensile bar at 140°C. Thermal and mechanical properties and water absorption of the blends were studied by differential scanning calorimetry (DSC), dynamical mechanic analysis (DMA), a test of modulus and tensile strength (with an Instron tensile tester), a water absorption test, and scanning electron microscopy (SEM). The blends showed two composition‐dependent glass transition temperatures. Furthermore, as the SPI content increased, the melting temperature of PEEAMA remained constant but the heat of fusion decreased. These results indicate that SPI and PEEAMA were partially miscible. Morphology observations support these results. Increasing the PEEAMA content resulted in decreases in the modulus and tensile strengths and increases in the elongation and toughness of the blends. Water absorption of the blends also decreased with increased PEEAMA content. Incorporating MDI further decreased the water absorption of the blends. The mechanism of water sorption of SPI was relaxation controlled, and that of the blends was diffusion controlled. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 88: 407–413, 2003     

Peroxide induced cross‐linking by reactive melt processing of two biopolyesters: Poly(3‐hydroxybutyrate) and poly(l‐lactic acid) to improve their melting processability

Poly(3‐hydroxybutyrate) (PHB) and poly(l ‐lactic acid) (PLLA) were individually cross‐linked with dicumyl peroxide (DCP) (0.25–1 wt %) by reactive melt processing. The cross‐linked structures of the polymer gel were investigated by nuclear magnetic resonance (NMR) and Fourier transform infrared (FTIR) spectroscopies. The size of the polymer crystal spherulites, glass transition temperature (T_g), melting transition temperature (T_m), and crystallinity were all decreased as a result of cross‐linking. Cross‐linking density (ν_e) was shown to increase with DCP concentration. Based on parallel plate rheological study (dynamic and steady shear), elastic and viscous modulus (G″ and G′), complex viscosity (η^*) and steady shear viscosity (η) were all shown to increase with cross‐linking. Cross‐linked PHB and PLLA showed broader molar mass distribution and formation of long chain branching (LCB) as estimated by RheoMWD. Improvements in melt strength offer bioplastic processors improved material properties and processing options, such as foaming and thermoforming, for new applications. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41724.     

Miscibility and Physical Properties of Poly(3‐hydroxybutyrate‐co‐3‐hydroxyhexanoate)/Poly(ethylene oxide) Binary Blends

In order to improve some inferior physical properties of bacterial poly(3‐hydroxybutyrate‐co‐3‐hydroxyhexanoate) [P(3HB‐co‐3HHx)] by blending with PEO, the miscibility, spherulite morphology, crystallization behavior and mechanical properties of P(3HB‐co‐3HHx)/PEO binary biodegradable polymer blends were investigated. A good miscibility between P(3HB‐co‐3HHx) with a 3HHx unit content of 11 mol‐% and PEO in the amorphous state was found when the PEO weight fraction was 10 wt.‐%, while the miscibility decreased dramatically when the PEO weight fraction exceeded 20 wt.‐%. Strongly depending on the blend composition, the mechanical properties of P(3HB‐co‐3HHx) was found to be significantly improved by blending with PEO with a weight fraction of ≈5–17.5 wt.‐%.

     

Design of highly tough poly(l‐lactide)‐based ternary blends for automotive applications

Technical renewable poly(l ‐lactide) (PLA)‐based blends represent an elegant way to achieve attractive properties for engineering applications. Recently, the miscibility between PLA and poly(methyl methacrylate) (PMMA) gave rise to new formulations with enhanced thermo‐mechanical properties but their high brittleness still remains a challenge to be overcome. This work here focuses on rubber‐toughened PLA/PMMA formulations for injection‐molding processes upon the addition of a commercially available ethylene‐acrylate impact modifier (BS). The miscibility between PLA and PMMA is not altered by the presence of BS but the incorporation of BS (17% by weight) into a PLA/PMMA matrix could enhance both ductility and toughness of PLA/PMMA blends for PMMA content up to 50 wt %. An optimum range of particle sizes (d_n ～0.5 µm) of the dispersed domains for high impact toughness is identified. These bio‐based ternary blends appear as promising alternatives to petro‐sourced blends such as ABS‐based blends in engineering injection‐molding parts. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43402.     

Properties of poly(butylene adipate‐co‐terephthalate) and sunflower head residue biocomposites

Utilization of low‐value agricultural waste for polymer composite materials has great environmental and economical benefits. Sunflower head residue (SHR) as an agricultural waste may be used as a reinforcement in polymeric materials because of its fiber characteristics. In this work, composites of biodegradable poly(butylene adipate‐co‐terephthalate) (PBAT) and SHR were prepared via melt‐extrusion compounding. To improve interfacial compatibility, maleic anhydride (MA) grafted PBAT (PBAT‐g‐MA) was prepared and used as a compatibilizer for the PBAT/SHR composites. The effects of the concentrations of SHR and PBAT‐g‐MA on the morphology, mechanical properties, melt rheology, and water resistance of the composites were examined. Interfacial adhesion between phases in the PBAT/SHR composites was enhanced by the introduction PBAT‐g‐MA as interface‐strengthening agent, resulting in improved mechanical properties and moisture resistance of the composite. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 44644.     

All‐wood biocomposites by partial dissolution of wood flour in 1‐butyl‐3‐methylimidazolium chloride

After cedar‐derived wood flour (WF) and bark flour (BF) were mixed with 1‐butyl‐3‐methylimidazolium chloride (BMIC) at 100°C, the obtained compounds with BMIC content 40 wt % were compression‐molded at 210°C to give WF/BMIC and BF/BMIC composites, respectively. The BMIC contained in the composites was twice extracted with ethanol at 60°C to afford WF/BMIC‐E and BF/BMIC‐E biocomposites, which were subsequently annealed at 200°C for 24 h to produce WF/BMIC‐A and BF/BMIC‐A biocomposites. The Fourier transform infrared spectroscopic analysis revealed that WF has a higher content of cellulose and a lower content of lignin than BF does, and that the BMIC content diminished by the extraction process. The scanning electron microscopy analysis showed that woody particles joined together by the compression molding of WF/BMIC and BF/BMIC compounds, and that the extraction of BMIC roughened the surface and the annealing again smoothed the surface due to the fusion of the residual BMIC and woody particles. The XRD measurements indicated that the annealing enhanced the crystallinity of cellulose component. The tensile properties and 5% weight loss temperature of the biocomposites were considerably improved by the extraction of BMIC and further by the annealing. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

Nanocomposites based on poly(ϵ‐caprolactone) and the montmorillonite treated with dibutylamine‐terminated ϵ‐caprolactone oligomer

Dibutylamine‐terminated ε‐caprolactone oligomers (CLOs: CLOL, CLOM, and CLOH) with number–averaged molecular weight (M_n), 500, 1300, and 2200, respectively, were synthesized by the ring‐opening polymerization of ε‐caprolactone initiated by 2‐(dibutylamino)ethanol in the presence of tin(II) 2‐ethylhexanoate. Nanocomposites based on poly(ε‐caploractone) (PCL) and the caprolactone oligomer‐treated montmorillonites (CLO‐Ms: CLOL‐M, CLOM‐M, and CLOH‐M) were prepared by melt intercalation method. The XRD and TEM analyses of the PCL composites revealed that the extent of exfoliation of the clay platelets increased with increasing molecular weight of the used CLOs. Tensile strength and modulus of the PCL/CLO‐M composites increased with increasing molecular weight of the CLO and increasing inorganic content. The tensile modulus of the PCL/CLOH‐M nanocomposite with inorganic content 5.0 wt % was three times higher than that of control PCL. Among the PCL/CLO‐M composites, the PCL/CLOM‐M composite had the highest crystallization temperature and melting temperature. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci 2007     

Study on the poly(3‐hydroxybutyrate‐co−4‐hydroxybutyrate)‐based composites toughened by synthesized polyester polyurethane elastomer

In this study, polycaprolactone(PCL)‐based polyurethane (PU) elastomer containing 45 wt % hard segment component was synthesized and characterized by fourier transform infrared spectroscopy, gel permeation chromatography, and X‐ray diffraction. As a toughening agent, the as‐synthesized PU was incorporated into biodegradable poly(3‐hydroxybutyrate‐co‐4‐hydroxybutyrate) [P(3,4)HB] by solution casting to prepare P(3,4)HB/PU composites. The microstructure and properties of P(3,4)HB/PU composites were investigated using transmission electron microscopy, X‐ray diffraction, tensile testing, scanning electron microscopy, differential scanning calorimetry, thermogravimetric analysis, and activated sludge degradation testing. The results show that PU can disperse well in a P(3,4)HB matrix. The elongation at break of P(3,4)HB/PU composites is remarkably increased while the yield strength and elastic modulus are decreased with an increase in PU content. At the same time, it is found that the fracture characteristic of P(3,4)HB is obviously transformed from brittleness into ductility with a gradual increase in PU loading. Moreover, the thermal stability of P(3,4)HB/PU composites is significantly improved compared with that of pure P(3,4)HB. In addition, the biodegradation rate of P(3,4)HB/PU composites is evidently reduced with the increase of PU content in the activated sludge degradation testing. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42740.     

Poly(methyl methacrylate)–epoxy vitrimer composites

In this study, we synthesized poly(methyl methacrylate) (PMMA) epoxy vitrimer composites by doping methyl methacrylate (MMA) and benzoyl peroxide into a curing system of epoxy resin and citric acid. The vitrimer composites were characterized with dynamic mechanical thermal analysis, scanning electron microscopy, and stress‐relaxation and lap‐shear testing. The test results show that with increasing amount of MMA, the existence of PMMA in the epoxy vitrimer matrix in the form of intermiscible, slightly soluble, and phase separation became more evident. When the doping amount of PMMA reached 10–25 wt %, the bonding strength of the PMMA–epoxy vitrimer composites was about two times that of the epoxy vitrimer (from 2.3 to 4.3 MPa). This showed that the self‐healing strength of the vitrimer composites was better than that of the pure vitrimer. When the PMMA in the epoxy matrix was in a slightly soluble form, the linear PMMA improved the mechanical properties of the epoxy vitrimer by physical winding. At the same time, the doping of PMMA promoted the transesterification rate of the epoxy vitrimer and enhanced the bonding strength of the composites without lowering the epoxy vitrimer glass‐transition temperature. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46307.