Extruder‐made TPO nanocomposites. I. Effect of maleated polypropylene and organoclay ratio on the morphology and mechanical properties

PP/PP‐g‐MA/MMT/EOR blend nanocomposites were prepared in a twin‐screw extruder at fixed 30 wt % elastomer and 0 to 7 wt % MMT content. Elastomer particle size and shape in the presence of MMT were evaluated at various PP‐g‐MA/organoclay masterbatch ratios of 0, 0.5, 1.0, and 1.5. The organoclay dispersion facilitated by maleated polypropylene serves to reduce the size of the elastomer dispersed phase particles and facilitates toughening of these blend nanocomposites. The rheological data analysis using modified Carreau‐Yasuda model showed maximum yield stress in extruder‐made nanocomposites compared with nanocomposites of reactor‐made TPO. Increasing either MMT content or the PP‐g‐MA/organoclay ratio can drive the elastomer particle size below the critical particle size below which toughness is dramatically increased. The ductile‐brittle transition shift toward lower MMT content as the PP‐g‐MA/organoclay ratio is increased. The D‐B transition temperature also decreased with increased MMT content and masterbatch ratio. Elastomer particle sizes below ～1.0 μm did not lead to further decrease in the D‐B transition temperature. The tensile modulus, yield strength, and elongation at yield improved with increasing MMT content and masterbatch ratio while elongation at break was reduced. The modified Mori‐Tanaka model showed better fit to experimental modulus when the effect of MMT and elastomer are considered individually. Overall, extruder‐made nanocomposites showed balanced properties of PP/PP‐g‐MA/MMT/EOR blend nanocomposites compared with nanocomposites of reactor‐made TPO. © 2012 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2012     

Preparation of poly(ethylene terephthalate)/organoclay nanocomposites using a polyester ionomer as a compatibilizer

In this work, poly(ethylene terephthalate)/organically modified montmorillonite (PET/o‐MMT) nanocomposites were prepared via direct melt compounding in a twin‐screw extruder. The main objective was to study the effects of using a polyester ionomer (PETi) as a compatibilizer to promote the intercalation and/or exfoliation of the o‐MMT in the PET. The o‐MMT content was 0, 1, 3, or 5 wt % and the PETi/o‐MMT mass ratio was 0/1, 1/1, or 3/1. The PETi was efficient to promote the intercalation/exfoliation of the o‐MMT in the PET matrix, as revealed by wide angle X‐ray scattering and transmission electron microscopy. Rheological characterization showed that the PET/o‐MMT nanocomposites exhibited a higher complex viscosity at low frequencies than PET, which is characteristic of materials presenting yield strength. Moreover, the higher the content and/or the degree of intercalation/exfoliation of the o‐MMT, the more the nanocomposite behaved like a solid because of a percolated structure formed by the o‐MMT layers, and the more the storage and loss modulus, G′ and G″, became independent of the frequency at low frequencies. © 2007 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 45: 3084–3091, 2007     

Preparation and characterization of PP/clay nanocomposites based on modified polypropylene and clay

X‐ray diffraction and differential scanning calorimeter (DSC) methods have been used to investigate the crystallization behavior and crystalline structure of hexamethylenediamine (HMDA)‐modified maleic‐anhydride‐grafted polypropylene/clay (PP‐g‐MA/clay) nanocomposites. These nanocomposites have been prepared by using HMDA to graft the PP‐g‐MA (designated as PP‐g‐HMA) and then mixing the PP‐g‐HMA polymer in hot xylene solution, with the organically modified montmorillonite. Both X‐ray diffraction data and transmission electron microscopy images of PP‐g‐HMA/clay nanocomposites indicate that most of the swellable silicate layers are exfoliated and randomly dispersed into PP‐g‐HMA matrix. DSC isothermal results revealed that introducing 5 wt % of clay into the PP‐g‐HMA structure causes strongly heterogeneous nucleation, which induced a change of the crystal growth process from a three‐dimensional crystal growth to a two‐dimensional spherulitic growth. Mechanical properties of PP‐g‐HMA/clay nanocomposites performed by dynamic mechanical analysis show significant improvements in the storage modulus when compared to neat PP‐g‐HMA. © 2005 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 43: 3242–3254, 2005     

Exploitation of introducing of catalytic centers into layer galleries of layered silicates and related epoxy nanocomposites. I. Epoxy nanocomposites derived from montmorillonite modified with catalytic surfactant‐bearing carboxyl groups

Montmorillonite (MMT) was modified with the acidified cocamidopropyl betaine (CAB) and the resulting organo‐montmorillonite (O‐MMT) was dispersed in an epoxy/methyl tetrahydrophthalic anhydride system to form epoxy nanocomposites. The intercalation and exfoliation behavior of the epoxy nanocomposites were examined by X‐ray diffraction and transmission electron microscopy. The curing behavior and thermal property were investigated by in situ Fourier transform infrared spectroscopy and DSC, respectively. The results showed that MMT could be highly intercalated by acidified CAB, and O‐MMT could be easily dispersed in epoxy resin to form intercalated/exfoliated epoxy nanocomposites. When the O‐MMT loading was lower than 8 phr (relative to 100 phr resin), exfoliated nanocomposites were achieved. The glass‐transition temperatures (T_g's) of the exfoliated nanocomposite were 20 °C higher than that of the neat resin. At higher O‐MMT loading, partial exfoliation was achieved, and those samples possessed moderately higher T_g's as compared with the neat resin. O‐MMT showed an obviously catalytic nature toward the curing of epoxy resin. The curing rate of the epoxy compound increased with O‐MMT loading. © 2004 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 42: 1192–1198, 2004     

Impact‐modified polypropylene/vermiculite nanocomposites

Impact‐modified polypropylene (PP)/vermiculite (VMT) nanocomposites toughened with maleated styrene–ethylene butylene–styrene (SEBS‐g‐MA) were compounded in a twin‐screw extruder and injection‐molded. VMT was treated with maleic anhydride, which acted both as a compatibilizer for the polymeric matrices and as a swelling agent for VMT in the nanocomposites. The effects of the impact modifier on the morphology and the impact, static, and dynamic mechanical properties of the PP/VMT nanocomposites were investigated. Transmission electron microscopy revealed that an exfoliated VMT silicate layer structure was formed in ternary (PP–SEBS‐g‐MA)/VMT nanocomposites. Tensile tests showed that the styrene–ethylene butylene–styrene additions improved the tensile ductility of the (PP–SEBS‐g‐MA)/VMT ternary nanocomposites at the expense of their tensile stiffness and strength. Moreover, Izod impact measurements indicated that the SEBS‐g‐MA addition led to a significant improvement in the impact strength of the nanocomposites. The SEBS‐g‐MA elastomer was found to be very effective at converting brittle PP/VMT organoclay composites into tough nanocomposites. © 2003 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 41: 2332–2341, 2003     

Atomic force microscopy study on blend morphology and clay dispersion in polyamide‐6/polypropylene/organoclay systems

The phase structure and clay dispersion in polyamide‐6(PA6)/polypropylene(PP)/organoclay (70/30/4) systems with and without an additional 5 parts of maleated polypropylene (MAH‐g‐PP) as a compatibilizer were studied with atomic force microscopy (AFM). AFM scans were taken from the polished surface of specimens that were chemically and physically etched with formic acid and argon ion bombardment, respectively. The latter technique proved to be very sensitive to the blend morphology, as PP was far more resistant to ion bombardment than PA6. In the absence of the MAH‐g‐PP compatibilizer, the organoclay is located in the PA6 phase; this finding is in line with transmission electron microscopic results. Further, the PP is coarsely dispersed in PA6 and the adhesion between PA6 and PP is poor. The addition of MAH‐g‐PP resulted in a markedly finer PP dispersion and good interfacial bonding between PA6 and PP. In this blend, the organoclay was likely dispersed in the PA6‐grafted PP phase. © 2005 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 43:1198–1204, 2005     

Shear‐induced change of exfoliation and orientation in polypropylene/montmorillonite nanocomposites

For the improved dispersion of montmorillonite (MMT) in a polypropylene (PP) matrix, PP/MMT nanocomposites prepared via direct melt intercalation were further subjected to oscillating stress achieved by dynamic packing injection molding. The shear‐induced morphological changes were investigated with an Instron machine, wide‐angle X‐ray diffraction, scanning electron microscopy, and transmission electron microscopy. The original nanocomposites possessed a partly intercalated and partly exfoliated morphology. A transformation of the intercalated structure into an exfoliated structure occurred after shearing, and a more homogeneous dispersion of MMT in the PP matrix was obtained. However, the increase of the exfoliated structure was accompanied by the scarifying of the orientation of MMT layers along the shear direction. Some bended or curved MMT layers were found for the first time by TEM after shearing. However, the orientation of PP chains in the PP/MMT nanocomposites became very difficult under an external shear force; this indicated that the molecular motion of PP chains intercalated between MMT layers was highly confined. © 2002 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 41: 1–10, 2003     

Morphologies, crystallinity and dynamic mechanical characterizations of polypropylene/polystyrene blends compatibilized with PP-g-PS copolymer: Effect of the side chain length

PP-g-PS copolymers were synthesized with the same polypropylene (PP) backbones and various side chain lengths of PS sequences via reactive comonomer p-allyltoluene (p-AT) by Ziegler–Natta copolymerization and the subsequent living anionic graft-polymerization. ¹H NMR characterized that the PP-g-PS copolymer had grafted 3.15 side chains per 1000 carbons in the PP backbones and the length of PS sequences varied in the range of 25.8–309.9 units. PP/PS blends with the PP-g-PS copolymer as compatibilizer (wt. 75/25/5) were prepared and characterized by SEM, WAXD and DMA to investigate the morphologies, crystallinity and glass transition temperatures of the PP/PS blends. All the results pointed out that the average side chain length (GL) of the graft copolymer (GL is from 25.8 to 309.9) made great effects of the PP/PS blends, such as the PS dispersed phase, the crystallinity of the PP component and the two glass transition temperatures of the blends, which showed the same trend with the increase of the GL. Overall, only with a suitable average side chain length, the PP-g-PS copolymer could achieve optimal compatibilizing efficiency of the PP/PS blends.     

Dispersibility of clay and crystallization kinetics for in situ polymerized PET/pristine and modified montmorillonite nanocomposites

Nanocomposite materials composed of poly (ethylene terephthalate) (PET) and montmorillonite (MMT) clays were prepared by in situ polymerization. Samples consisted of PET blended with various quantities of either pristine (Na⁺‐MMT) or organically modified MMT (A10‐MMT). The morphology and thermal and mechanical properties were evaluated for each sample. TEM micrographs, acquired at a 20 nm resolution, provide direct evidence of exfoliation of the clay particles into the PET matrix and show the effect of the alkyl‐modifier on clay dispersibility. The dispersion of PET/A10‐MMT was greater than that observed for the PET/Na⁺‐MMT nanocomposites. The greatest degree of exfoliation occurred for PET/A10‐MMT 0.5 wt %. However, PET/Na⁺‐MMT exhibited higher crystallization temperatures and rates suggesting that Na⁺‐MMT is a more efficient nucleating agent. Both mechanically and thermally, PET/A10‐MMT nanocomposites exhibited superior properties over pure PET. © 2008 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 46: 1022–1035, 2008     

Concurrent crystallization in polypropylene/nylon-6 blends using maleic anhydride grafted polypropylene as a compatibilizing agent

This paper describes the nonisothermal crystallization of molten blends of two semicrystalline polymers, polypropylene (PP) and Nylon-6 (N6). A discussion details the effect of the concentration of the compatibilizing agent, maleic anhydride grafted polypropylene (MAH-g-PP), on the crystallization behavior. The crystallization thermograms showed one crystallization peak or two crystallization peaks, which were significantly affected by the presence of MAH-g-PP. The crystallization temperature of N6 levels off down as the concentration of MAH-g-PP increases, whereas that of PP stays at a roughly constant temperature. These blends containing the compatibilizing agent exhibited concurrent crystallization at the crystallization temperature of PP. The crystallization behavior are also studied by optical microscopy under crossed polarizers. © 1994 John Wiley & Sons, Inc.     

Synthesis of polypropylene graft copolymers by the combination of a polypropylene copolymer containing pendant vinylbenzene groups and atom transfer radical polymerization

This article discusses a facile and inexpensive reaction process for preparing polypropylene‐based graft copolymers containing an isotactic polypropylene (i‐PP) main chain and several functional polymer side chains. The chemistry involves an i‐PP polymer precursor containing several pendant vinylbenzene groups, which is prepared through the Ziegler–Natta copolymerization of propylene and 1,4‐divinylbenzene mediated by an isospecific MgCl₂‐supported TiCl₄ catalyst. The selective monoenchainment of 1,4‐divinylbenzene comonomers results in pendant vinylbenzene groups quantitatively transformed into benzyl halides by hydrochlorination. In the presence of CuCl/pentamethyldiethylenetriamine, the in situ formed, multifunctional, polymeric atom transfer radical polymerization initiators carry out graft‐from polymerization through controlled radical polymerization. Some i‐PP‐based graft copolymers, including poly(propylene‐g‐methyl methacrylate) and poly(propylene‐g‐styrene), have been prepared with controlled compositions. © 2004 Wiley Periodicals, Inc. J Polym Sci Part A: Polym Chem 43: 429–437, 2005     

Extruder‐made TPO nanocomposites. II. Effect of maleated poly(propylene)/organoclay ratio on morphology and thermal expansion behavior

Coefficients of linear thermal expansion (CTE) for poly(propylene)/ poly(propylene)‐grafted‐maleic anhydride/montmorillonite ethylene‐co‐octene elastomer (PP/PP‐g‐MA/MMT/EOR) blend nanocomposites were determined as a function of MMT content and various PP‐g‐MA/organoclay masterbatch ratios. The nanocomposites were prepared in a twin‐screw extruder at a fixed 30 wt % elastomer, 0–7 wt % MMT content, and various PP‐g‐MA/organoclay ratio of 0, 0.5, 1.0, and 1.5. The organoclay dispersion facilitated by the maleated PP helps to reduce the size of the dispersed phase elastomer particles in the PP matrix. The elastomer particle size decreased significantly as the PP‐g‐MA/organoclay ratio and MMT content increased; the elastomer particles viewed // to flow direction (FD) are smaller and less deformed compared to those viewed // to transverse direction (TD). The elastomer particle shape based on the view along the three orthogonal directions of the injection molded sample is similar to a prolate ellipsoid. The CTE decreased significantly in the FD and TD, whereas a slight increase is observed in the normal direction in the presence of MMT and PP‐g‐MA. The Chow model based on a two population approach showed better fit to experimental CTE when the effect of MMT and elastomer are considered individually. © 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part B Polym. Phys. 2013 , 51, 952–965     

Polyolefin-based nanocomposite: The effect of organoclay modifier

Polypropylene (PP) nanocomposites were prepared using montmorillonite with different organic modifiers, and the effect of processing aid (EMCA and PPG) on the dispersion of the nanofillers in the PP matrix was evaluated by WAXD, TEM, DSC, TGA, DMA, and mechanical tests. The present study helps to clarify the effects of the organic modifiers of clays on the intercalation and exfoliation processes. Nanocomposites of intercalated and partially exfoliated morphology were obtained, mainly when a low amount (1:1) of PP-g-MA/MMT was used. The results of the tests on mechanical properties showed that the clays with larger d₀₀₁ (C-15A and Nanofil 5) using PPG presented a more considerable gain in impact strength. The nanocomposites using clays with smaller d₀₀₁(C-20A) presented larger modulus when compared with those of pristine PP. The heat deflection temperature, crystallization temperature, and thermal stability of the nanocomposites were improved compared to neat PP. The DMA results showed that the organoclay improved the modulus of PP, but decreased the T_g. © 2008 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 46: 2519–2531, 2008     

Nanocomposites of poly(ethylene terephthalate‐co‐ethylene naphthalate) with organoclay

Poly(ethylene terephthalate‐co‐ethylene naphthalate) (PETN)/organoclay was synthesized with the solution intercalation method. Hexadecylamine was used as an organophilic alkylamine in organoclay. Our aim was to clarify the intercalation of PETN chains to hexadecylamine–montmorillonite (C₁₆–MMT) and to improve both the thermal stability and tensile property. We found that the addition of only a small amount of organoclay was enough to improve the thermal stabilities and mechanical properties of PETN/C₁₆–MMT hybrid films. Maximum enhancement in both the ultimate tensile strength and initial modulus for the hybrids was observed in blends containing 4 wt % C₁₆–MMT. Below a 4 wt % clay loading, the clay particles could be highly dispersed in the polymer matrix without a large agglomeration of particles. However, an agglomerated structure did form in the polymer matrix at a 6 wt % clay content. © 2001 John Wiley & Sons, Inc. J Polym Sci Part B: Polym Phys 39: 2581–2588, 2001     

Polypropylene/polystyrene/clay blends prepared by an innovative eccentric rotor extruder based on continuous elongational flow: Analysis of morphology,rheology property,and crystallization behavior

The polypropylene (PP)/polystyrene (PS)/montmorillonite (MMT) blends were prepared by an innovative eccentric rotor extruder based on continuous elongational flow. Addition of MMT nanoparticles was found to reduce the PS droplet size and improve the compatibility of PP/PS. The MMT nanoparticles had clear intercalation and/or exfoliation structures and were located mostly at the interface of PP/PS. It was found that the intercalation and exfoliation of MMT was finished under the synergy of interfacial interaction and tensile deformation so that we called the mechanism as “MMT exfoliation mechanism induced by synergy of interface and tensile deformation”. The rheological analysis showed that incorporation of MMT led to an increase in complex viscosity to an optimum level (5 wt%), after which any further increase in MMT concentration decreased the complex viscosity. Moreover, the degree of crystallinity of blends was controlled by the heterogeneous nucleation effect of MMT and the inhibition effect of PS.     

Synergistic flammability and thermal stability of polypropylene/aluminum trihydroxide/Fe‐montmorillonite nanocomposites

In the present study, polypropylene/aluminium trihydroxide/Fe‐montmorillonite (PP/ATH/Fe‐MMT) nanocomposites were prepared by melt‐intercalation method. This was been designed to determine whether the presence of structural iron in the matrix could enhance the thermal stability and flammability of nanocomposites. In order to prove the effect of Fe³⁺ in the structural silicate layers, samples of PP/ATH and PP/ATH/Na‐MMT (no Fe³⁺ in structural silicate layers) were prepared under the same conditions. Fe‐MMT and Na‐MMT were modified by cetyltrimethyl ammonium bromide (CTAB). The nanocomposite structures were characterized by X‐ray diffraction (XRD), transmission electron microscopy (TEM), and thermogravimetric analysis (TGA) was applied to test the thermal properties of nanocomposites. In addition, the limiting oxygen index (LOI) of PP/ATH/Fe‐MMT nanocomposites was increased, and no dripping phenomenon was found through the UL‐94 vertical burning test. Copyright © 2009 John Wiley & Sons, Ltd.     

Preparation of thermosetting polyurethane nanocomposites by montmorillonite modified with a novel intercalation agent

A novel thermosetting polyurethane (TSPU)/organic montmorillonite (OMMT) nanocomposite has been synthesized. N‐diamino octadecyl trimethyl ammonium chloride (DODTMAC) was used as an intercalation agent to treat Na⁺‐montmorillonite (MMT) and form a novel kind of OMMT. Fourier transform infrared spectroscopy (FT‐IR), wide angle X‐ray diffraction (WAXD), and thermogravimetric analysis (TGA) data indicated that the MMT was successfully intercalated by this intercalation agent, as evidenced by the fact that the basal spacing of MMT galleries was expanded from 1.5 to 3.2 nm. This OMMT was used to prepare the TSPU nanocomposites. Both the reinforcing and compatibilizing performance of the filler were investigated. Tensile tests showed that the tensile strength of TSPU/OMMT‐4 was the highest, and was about 3.62 times higher than that of the pure TSPU, and also the elongation at break showed an enhancement. Differential scanning calorimetry (DSC) and dynamic mechanical analysis (DMA) measurements illustrated that the glass transition temperature of the TSPU/OMMT‐4 nanocomposite was improved from 0.5 to 6.5 °C, which corresponded to the restriction of the soft segments of TSPU. The highest initial and center temperatures of TSPU/OMMT‐4 obtained from TGA were due to the highest retard effect of the TSPU molecular chains. WAXD studies showed that the formation of the nanocomposites in all the cases with the almost disappearance of the peaks corresponding to the basal spacing of MMT. SEM and TEM were used to investigate the morphologies of the TSPU/OMMT‐4 nanocomposite, and demonstrated that the nanocomposite was comprised of a well dispersion of a mixture of intercalated and exfoliated silicate layers throughout the matrix. It was proposed that the nano‐reinforcing effect caused by the well‐dispersed silicate layers might reduce the amount and size of voids and increase the length of the crack‐spreading path during tensile drawing. © 2007 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 45: 519–531, 2007.     

Polypropylene/montmorillonite nanocomposites toughened with SEBS‐g‐MA: Structure–property relationship

Polypropylene (PP)/organo‐montmorillonite (Org‐MMT) nanocomposites toughened with maleated styrene‐ethylene‐butylene‐styrene (SEBS‐g‐MA) were prepared via melt compounding. The structure, mechanical properties, and dynamic mechanical properties of PP/SEBS‐g‐MA blends and their nanocomposites were investigated by X‐ray diffraction (XRD), polarizing optical microscopy (POM), tensile, and impact tests. XRD traces showed that Org‐MMT promoted the formation of β‐phase PP. The degree of crystallinity of PP/SEBS‐g‐MA blends and their nanocomposites were determined from the wide angle X‐ray diffraction via profile fitting method. POM experiments revealed that Org‐MMT particles served as nucleating sites, resulting in a decrease of the spherulite size. The essential work of fracture approach was used to evaluate the tensile fracture toughness of the nanocomposites toughened with elastomer. © 2005 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 43: 3112–3126, 2005     

Isothermal crystallization behavior of exfoliated‐PP/IMMT nanocomposites via in situ polymerization

Highly exfoliated isotactic‐polypropylene/alkyl‐imidazolium modified montmorillonite (PP/IMMT) nanocomposites have been prepared via in situ intercalative polymerization. TEM and XRD results indicated that the obtained composites were highly exfoliated PP/IMMT nanocomposites and the average thickness of IMMT in PP matrix was less than 10 nm, and the distance between adjacent IMMT particles was in the range of 20–200 nm. The isothermal crystallization kinetics of highly exfoliated PP/IMMT nanocomposites were investigated by using differential scanning calorimeter(DSC) and polarized optical microscope (POM). The crystallization half‐time t_1/2, crystallization peak time t_max, and the Avrami crystallization rate constant K_n showed that the nanosilicate layers accelerate the overall crystallization rate greatly due to the nucleation effect, and the crystallization rate was increased with the increase in MMT content. Meanwhile, the crystallinity of PP in nanocomposites decreased with the increase in clay content which indicated the PP chains were confined by the nanosilicate layers during the crystallization process. Although the well‐dispersed silicate layers did not have much influence on spherulites growth rate, the nucleation rate and the nuclei density increased significantly. Accordingly, the spherulite size decreased with the increase in MMT content. © 2009 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 47: 2215–2225, 2009     

Effects of functionalized multiwalled carbon nanotubes on the morphologies and mechanical properties of PP/EVA blend

The maleic anhydride‐grafted multiwalled carbon nanotubes (MWCNTs‐g‐MA) have been introduced into polypropylene/ethylene‐co‐vinyl acetate (PP/EVA) blend. To clearly describe the effects of MWCNTs‐g‐MA on the morphology and mechanical properties of PP/EVA blends, the selective distribution of MWCNTs‐g‐MA in the blends is realized through different sample preparation methods, namely, MWCNTs‐g‐MA disperse in EVA phase and MWCNTs‐g‐MA disperse in PP matrix. The results show that the distribution of MWCNTs‐g‐MA has an important effect on the final morphology of EVA and the crystallization structure of PP matrix. Compared with PP/EVA binary blend, distribution of MWCNTs‐g‐MA in PP matrix induces the aggregation of EVA phase at high EVA content and the decrease of spherulite diameters of PP matrix simultaneously. However, when MWCNTs‐g‐MA are dispersed in the EVA phase, they induce more homogeneous distribution of EVA, and the crystallization behavior of PP is slightly affected by MWCNTs‐g‐MA. The corresponding mechanical properties including impact strength and tensile strength are tested and analyzed in the work. © 2009 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys 47: 1481–1491, 2009