Chain structure and mechanical properties of polyethylene/polypropylene/poly(ethylene‐co‐propylene)in‐reactor alloys synthesized with a spherical Ziegler–Natta catalyst by gas‐phase polymerization

Two polyethylene/polypropylene/poly(ethylene‐co‐propylene) in‐reactor alloy samples with a good polymer particle morphology were synthesized by sequential multistage gas‐phase polymerization with a spherical Ziegler–Natta catalyst. The alloys showed excellent mechanical properties, including both toughness and stiffness. With temperature‐gradient extraction fractionation, both alloys were fractionated into five fractions. The chain structures of the fractions were studied with Fourier transform infrared, ¹³C‐NMR, and thermal analysis. The alloys were mainly composed of polyethylene, polyethylene‐b‐polypropylene block copolymer, and polypropylene. There also were minor amounts of an ethylene–propylene segmented copolymer with very low crystallinity and an ethylene–propylene random copolymer. The block copolymer fraction accounted for more than 44 wt % of the alloys. The coexistence of these components with different structures was apparently the key factor resulting in the excellent toughness–stiffness balance of the materials. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 97: 640–647, 2005     

Structure and morphology of polyethylene/polypropylene in‐reactor alloys synthesized by spherical high‐yield Ziegler–Natta catalyst

A series of spherical polyethylene/polypropylene (PE/PP) in‐reactor alloys were synthesized with spherical high‐yield Ziegler–Natta catalyst by sequential multistage polymerization in slurry. The morphology of PE/PP alloy granule was evaluated by optical microscopy, scanning electron microscopy, and transmission electron microscopy. The results show PE/PP in‐reactor alloy with excellent morphology, high porosity, and narrow distribution of the particle size. The PE/PP in‐reactor alloys show excellent mechanical properties with good balance between toughness and rigidity. It was fractionated into five fractions by temperature‐gradient extraction fractionation, and every fractionation was analyzed by FTIR, ¹³C‐NMR, DSC, and WAXD. The PE/PP in‐reactor alloy was found to contain mainly five portions: PP, PE, segmented copolymer with PP and PE segment of different length, ethylene‐b‐propylene copolymer, and an ethylene–propylene random copolymer. The characteristic chain structure leads to good compatibility between the fractions of the alloy that shows a multiphase structure. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 103: 2075–2085, 2007     

Influence of copolymerization conditions on the structure and properties of polyethylene/polypropylene/poly(ethylene‐co‐propylene) in‐reactor alloys synthesized in gas‐phase with spherical ziegler‐natta catalyst

A spherical TiCl₄/MgCl₂‐based catalyst was used in the synthesis of polyethylene/polypropylene/poly (ethylene‐co‐propylene) in‐reactor alloys by sequential homopolymerization of ethylene, homopolymerization of propylene, and copolymerization of ethylene and propylene in gas‐phase. Different conditions in the third stage, such as the pressure of ethylene–propylene mixture and the feed ratio of ethylene, were investigated, and their influences on the compositions, structural distribution and properties of the in‐reactor alloys were studied. Increasing the feed ratio of ethylene is favorable for forming random ethylene–propylene copolymer and segmented ethylene–propylene copolymer, however, slightly influences the formation of ethylene‐b‐propylene block copolymer and homopolyethylene. Raising the pressure of ethylene–propylene mixture results in the increment of segmented ethylene–propylene copolymer, ethylene‐b‐propylene block copolymer, and PE fractions, but exerts a slight influence on both the random copolymer and PP fractions. The impact strength of PE/PP/EPR in‐reactor alloys can be markedly improved by increasing the feed ratio of ethylene in the ethylene–propylene mixture or increasing the pressure of ethylene–propylene mixture. However, the flexural modulus decreases as the feed ratio of ethylene in the ethylene–propylene mixture or the pressure of ethylene–propylene mixture increases. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 102: 2481–2487, 2006     

Influence of polymerization conditions on the structure and properties of polyethylene/polypropylene in‐reactor alloy synthesized in the gas phase with a spherical Ziegler–Natta catalyst

A spherical TiCl₄/MgCl₂‐based catalyst was used in the synthesis of in‐reactor polyethylene/polypropylene alloys by polyethylene homopolymerization and subsequent homopolymerization of propylene in the gas phase. Different conditions in the ethylene homopolymerization stage, such as monomer pressure and polymerization temperature, were investigated, and their influences on the structure and properties of in‐reactor alloys were studied. Raising the polymerization temperature is the most effective way of speeding up polymerization and regulating the ethylene content of polyethylene (PE)/polypropylene (PP) alloys, but it will cause a greater increase in the PE‐b‐PP block copolymer fraction (named fraction D) than in the fraction of PP‐block‐PE in which the PP segments have low or medium isotacticity (named fraction A). Although changing ethylene monomer pressure could influence the ethylene content of PE/PP alloys slightly, it is an effective way of regulating the structural distribution. Reducing the monomer pressure will evidently increase fractions A and D. The mechanical properties of the alloys, including impact strength and flexural modulus, can be regulated in a broad range with changes in polymerization conditions. These properties are highly dependent on the amount, distribution, and chain structure of fractions A and D. The impact strength is affected by both fraction A and fraction D in a complicated way, whereas the flexural modulus is mainly determined by the amount of fraction A. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 101: 2136–2143, 2006     

The functions of crystallizable ethylene‐propylene copolymers in the formation of multiple phase morphology of high impact polypropylene

The functions of crystallizable ethylene‐propylene copolymers in the formation of multiple phase morphology of high impact polypropylene (hiPP) were studied by solvent extraction fractionation, transmission electron microscopy (TEM), selected area electron diffraction (SAED), nuclear magnetic resonance (¹³C‐NMR), and selected reblending of different fractions of hiPP. The results indicate that hiPP contains, in addition to polypropylene (PP) and amorphous ethylene‐propylene random copolymer (EPR) as well as a small amount of polyethylene (PE), a series of crystallizable ethylene‐propylene copolymers. The crystallizable ethylene‐propylene copolymers can be further divided into ethylene‐propylene segmented copolymer (PE‐s‐PP) with a short sequence length of PE and PP segments, and ethylene‐propylene block copolymer (PE‐b‐PP) with a long sequence length of PE and PP blocks. PE‐s‐PP and PE‐b‐PP participate differently in the formation of multilayered core‐shell structure of the dispersed phase in hiPP. PE‐s‐PP (like PE) constructs inner core, PE‐b‐PP forms outer shell, while intermediate layer is resulted from EPR. The main reason of the different functions of the crystallizable ethylene‐propylene copolymers is due to their different compatibility with the PP matrix. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Preparation and characterization of high MFR polypropylene and polypropylene/poly(ethylene‐co‐propylene) in‐reactor alloys

In this work, high melt flow rate (MFR) polypropylene (HF‐PP) and polypropylene/poly(ethylene‐co‐propylene) in‐reactor alloys (HF‐PP/EPR) with MFR ≈ 30 g/10 min were synthesized by spherical MgCl₂‐supported Ziegler–Natta catalyst with cyclohexylmethyldimethoxysilane (CHMDMS) or dicyclopentyldimethoxysilane (DCPDMS) as external donor (De). The effects of De on polymerization activity, chain structure, mechanical properties, and phase morphology of HF‐PP and HF‐PP/EPR were studied. Adding CHMDMS caused more sensitive change of the polymers MFR with H₂ than DCPDMS, and produced PP/EPR alloys containing more random ethylene‐propylene copolymer (r‐EP) and segmented ethylene‐propylene copolymer (s‐EP). CHMDMS also caused formation of s‐EP with higher level of blockiness than DCPDMS. HF‐PP/EPR alloy prepared in the presence of DCPDMS exhibited higher flexural properties but lower impact strength than that prepared with CHMDMS. Toughening efficiency of the rubber phase was nearly the same in the alloys prepared using CHMDMS or DCPDMS as De, but stiffness of the alloy can be improved by using DCPDMS. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 42984.     

Study of crystallization and melting behavior of polypropylene‐block‐polyethylenes copolymers fractionated from polypropylene and polyethylene mixtures

A series of ethylene–propylene block copolymer fractions of differing compositions, while still retaining broad molecular weight distributions, were obtained by fractionation of polypropylene (PP) and polyethylene (PE) copolymers prepared by sequential polymerization of ethylene and propylene. The crystallization and melting behavior of the polypropylene‐block‐polyethylene fractions were studied. It was observed that the major component could suppress crystallization of the minor component, leading to a decrease in crystallinity and melting temperature. Non‐isothermal crystallization showed that crystallization of the ethylene block was less influenced by composition and cooling rate than the propylene block. At fast cooling rates, the ethylene block could crystallize prior to the propylene block. Isothermal crystallization kinetics experiments were also conducted. We found that the block copolymers with minor ethylene components had smaller Avrami exponents (n ≈ 1.0), hence indicating a reduced growth dimension of the PE crystals by the pre‐existing PP crystals. On the other hand, the ethylene block exhibited much larger Avrami exponents in those block copolymers with major ethylene contents. Copyright © 2004 Society of Chemical Industry     

Compositional differences of propylene–ethylene block copolymers manufactured by degradation and hydrogenation techniques

The purpose of the present work is to investigate the compositional difference of polypropylene–polyethylene block copolymers (PP‐b‐PE) manufactured industrially by the process of degradation and hydrogenation, respectively. Each of the PP‐b‐PE copolymers was fractionated into three fractions with heptane and chloroform. The compositions of the three fractions were characterized by ¹³C nuclear magnetic resonance (NMR) and Fourier transform infrared (FTIR) spectroscopy, as well as differential scanning calorimetry (DSC) and thermal fractionation. The results showed that the Chloroform‐soluble fraction was amorphous ethylene‐propylene rubber, and the content of the rubber in PP‐b‐PE manufactured by hydrogenation was less than that by degradation. The degree of crystallinity of the chloroform‐insoluble fraction of the PP‐b‐PE manufactured by hydrogenation is higher than that of by degradation. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 101: 3301–3306, 2006     

单体组成切换法调控聚丙烯/丁烯合金的结构与性能

为解决聚丙烯材料抗冲击强度低的问题,同时利用国内大量廉价的1-丁烯资源,采用单体组成切换法在反应器内进行丙烯本体均聚和丙烯/丁烯本体共聚,原位制备聚丙烯合金。该合金主要由丙丁无规共聚物、长丙烯链段的丙丁嵌段共聚物和高等规度的聚丙烯组成。共聚物作为橡胶相分散在聚丙烯基体中,形成海岛结构,充当应力集中点,起到诱发及终止银纹、吸收能量的作用。长丙烯链段的嵌段共聚物增加了橡胶相与基体的相容性,使合金材料具有优异的刚性和韧性平衡,材料的抗冲击强度最高达48.91 kJ/m²。本文探究了聚合工艺对合金组成结构的影响,并揭示了合金组成结构和相形态、力学性能的关系。     

Improving the antifouling properties of polypropylene surfaces by melt blending with polyethylene glycol diblock copolymers

Protein‐resistant polyethylene‐block‐poly(ethylene glycol) (PE‐b‐PEG) copolymers of different molecular weights at various concentrations were compounded by melt blending with polypropylene (PP) polymers in order to enhance their antifouling properties. Phase separation of the PE‐b‐PEG copolymer and its migration to the surface of the PP blend, was confirmed by attenuated total reflectance–Fourier transform infrared, X‐ray photoelectron spectroscopy, and static water contact angle measurements. Enrichment of PEG chains at the surface of the blends increased with increasing PE‐b‐PEG copolymer concentration and molecular weight. The PP blends compounded with PE‐b‐PEG copolymer having the lowest molecular weight (875 g mol^?1), at the lowest concentration (1 wt %), gave the lowest bovine serum protein adsorption (30% less) compared to that of neat PP. At higher concentrations (5 and 10 wt %), and higher molecular weights (920, 1400, and 2250 g mol^?1), the PE‐b‐PEG copolymers leached‐out resulting in protein adsorption comparable to that of neat PP. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46122.     

Structure and properties of polypropylene alloy in situ blends

A series of polypropylene (PP) alloys containing different ethylene contents have been prepared by the in situ sequential polymerization technique, using Ziegler–Natta catalyst (MgCl₂/TiCl₄/BMF; BMF is 9,9‐bis(methoxymethyl)fluorine, as an internal donor) without any external donor. The structure and properties of PP alloys obtained have been investigated by nuclear magnetic resonance, Fourier transform infrared spectroscopy, dynamic mechanical analysis, differential scanning calorimetry, and scanning electron microscopy (SEM). The results have suggested that PP alloys are the complex mixtures containing PP, the copolymer with long sequence ethylene chain, ethylene‐propylene rubber (EPR), and block copolymer etc. In the alloys, PP, EPR, and the copolymer with long sequence ethylene chain are partially compatible. The investigation of the mechanical properties indicates that notched Izod impact strength of PP alloy greatly increases at 16°C/?20°C in comparison with that of pure PP. The noticeable plastic deformation is observed in SEM photograph. The increase in the toughness, the mechanical strength of PP alloy decreases to a certain extent. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 100: 4804–4810, 2006     

New synthesis methods for polypropylene‐co‐ethylene‐propylene rubber

In this research, the reinforcement of polypropylene (PP) was studied using a new method that is more practical for synthesizing polypropylene‐block‐poly(ethylene‐propylene) copolymer (PP‐co‐EP), which can be used as a rubber toughening agent. This copolymer (PP‐co‐EP) could be synthesized by varying the feed condition and changing the feed gas in the batch reactor system using Ziegler–Natta catalysts system at a copolymerization temperature of 10°C. The ¹³C‐NMR tested by a 21.61‐ppm resonance peak indicated the incorporation of ethylene to propylene chains that could build up the microstructure of the block copolymer chain. Differential scanning calorimetry (DSC), scanning electron microscopy (SEM), and dynamic mechanical analysis (DMA) results also confirmed these conclusions. Under these conditions, the morphology of copolymer trapped in PP matrix could be observed and the copolymer T_g would decrease when the amount of PP‐co‐EP was increased. DMA study also showed that PP‐co‐EP is good for the polypropylene reinforcement at low temperature. Moreover, the PP‐co‐EP content has an effect on the crystallinity and morphology of polymer blend, i.e., the crystallinity of polymer decreased when the PP‐co‐EP content increased, but tougher mechanical properties at low temperature were observed. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 103: 3609–3616, 2007     

Preparation of toughened polypropylene‐g‐poly(butyl acrylate‐co‐acrylated castor oil) by suspension grafting polymerization

Butyl acrylate (BA) with acrylated castor oil (ACO) was grafted onto porous polypropylene (PP) granules by grafting polymerization. Crosslinked copolymer microdomains which functioned as rubber phase to improve the toughness of PP were filled into the pores of PP granules. The sizes of crosslinked copolymer microdomains were controlled in the range of 0.1–1 μm in PP matrix. The results of fourier transform infrared spectroscopy and scanning electron microscope of PP‐g‐(BA‐co‐ACO) after extracted by acetone confirmed that BA and ACO were grafted onto PP successfully. The effects of comonomer ratio, initiator content and comonomer content on grafting percentage (GP) and grafting efficiency (GE) were investigated. The GP of PP‐g‐(BA‐co‐ACO) could be up to 21.3% with the comonomer content increasing to 25%. The crosslinked copolymer decreased the melting flow index and the relative crystallinity of PP. Dynamic mechanical thermal analysis showed that the glass transition temperature of PP decreased slightly from 22°C to 15°C. The addition of 5% comonomer content led to an increase of notched impact strength from 1.96 to 3.81 kJ/m² (nearly doubled) and a marginal decrease in the tensile strength of PP. Then with further addition of comonomer, the notched impact strength increased to 8.98 kJ/m² while the tensile strength was 29.37 MPa. POLYM. ENG. SCI., 58:86–93, 2018. © 2017 Society of Plastics Engineers     

Multilayered core–shell structure of the dispersed phase in high‐impact polypropylene

The multiphase morphology of high impact polypropylene (hiPP), which is a reactor blend of polypropylene (PP) with ethylene–propylene copolymer, was investigated by transmission electron microscopy, selected area electron diffraction, atomic force microscopy, and field‐emission scanning electron microscopy techniques in conjunction with an analysis of the hiPP composition and chain structure based on solvent fractionation, ¹³C‐NMR, and differential scanning calorimetry measurements. A multilayered core–shell structure of the dispersed phase of hiPP in solution‐cast films and the bulk was observed. The inner core was mainly composed of polyethylene (including its long blocks) together with part of PP, the intermediate layer was ethylene–propylene random copolymer, and the outer shell consisted of ethylene–propylene multiblock copolymers. The formation process and controlling factors of the multilayered core–shell structure are discussed. This kind of multiphase morphology of hiPP caused the material to possess both a high rigidity and high toughness. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Fabrication of polypropylene blends with excellent low‐temperature toughness and balanced toughness‐rigidity by a combination of EPR and SEEPS

To overcome serious rigidity depression of rubber‐toughened plastics and fabricate a rigidity‐toughness balanced thermoplastic, a combination of styrene‐[ethylene‐(ethylene‐propylene)]‐styrene block copolymer (SEEPS) and ethylene‐propylene rubber (EPR) was used to toughen polypropylene. The dynamic mechanical properties, crystallization and melting behavior, and mechanical properties of polypropylene (PP)/EPR/SEEPS blends were studied in detail. The results show that the combination of SEEPS and EPR can achieve the tremendous improvement of low‐temperature toughness without significant strength and rigidity loss. Dynamic mechanical properties and phase morphology results demonstrate that there is a good interfacial strength and increased loss of compound rubber phase comprised of EPR component and EP domain of SEEPS. Compared with PP/EPR binary blends, although neither glass transition temperature (T_g) of the rubber phase nor T_g of PP matrix in PP/EPR/SEEPS blends decreases, the brittle‐tough transition temperature (T_bd) of PP/EPR/SEEPS blends decreases, indicating that the increased interfacial interaction between PP matrix and compound rubber phase is also an effective approach to decrease T_bd of the blends so as to improve low‐temperature toughness. The balance between rigidity and toughness of PP/EPR/SEEPS blends is ascribed to the synergistic effect of EPR and SEEPS on toughening PP. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 45714.     

Compatibilized blends of PVC/PA12 and PVC/PP containing poly(lauryl lactam‐block‐caprolactone)

Specially designed block copolymers have played a role as compatibilizing agents in the system of immiscible polymer blends. We applied lauryl lactam (LA)–caprolactone (CL) block copolymer [P(LA‐b‐CL)] as a compatibilizing agent for immiscible poly(vinyl chloride) (PVC) blends with various polymers. These blends possess high thermal performance and toughness. We investigated the effect of P(LA‐b‐CL) as a compatibilizing agent for immiscible PVC blends with poly(ω‐lauryl lactam) [polyamide 12 (PA12)]. We also described the invention of a new compatibilizing agent system involving P(LA‐b‐CL) for PVC/polypropylene (PP) blends. The mechanical and thermal properties of (1) PVC/PA12 blend compatibilized with P(LA‐b‐CL) and (2) PVC/PP blend compatibilized with P(LA‐b‐CL)/PA12/maleic anhydride–modified PP were both enhanced. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 91: 1983‐1992, 2004     

Waste‐reducing preparation of PE‐g‐MAH and PE‐g‐DBM via solid phase grafting reaction and their application as compatibilizers

Kinetics for grafting two reactive monomers (dibutyl maleate (DBM) and maleic anhydride (MAH)) on polyethylene (PE) was investigated for the modified PE (PE‐g‐MAH and PE‐g‐DBM) using solid phase grafting process. This process avoided solvent waste produced in solution process and high operation temperature in melt process. In the presence of the radical initiator, coupling reactions, between the PE and product, and macromolecular radicals, routinely form gels and/or increase molecular weight, resulting in a worse rheological behavior for the grafting products. By adding small amount of interface agents, using combined initiators and optimizing reactor design, graft copolymers with controlled grafting degrees and good rheological properties were prepared. The grafting degrees of copolymers were determined by chemical analysis. FTIR, DSC, and pure water contact angle characterized the chemical structure, the thermal property, and the hydrophilic property of the grafting copolymers, respectively. The peel strength of the graft copolymer as powder coating on the stainless steel surface was measured as high as 12–24 kgf/cm. Mechanical strength and toughness of PE/kaolin clay, PVC/CPE, and PVC/CPE/CaCO₃ alloys with small amount of the graft copolymer (～5 wt %) added were improved significantly. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 101: 3781–3790, 2006     

Comparison of olefin copolymers as compatibilizers for polypropylene and high‐density polyethylene

Some polyolefin elastomers were compared as compatibilizers for blends of polypropylene (PP) with 30 wt % high‐density polyethylene (HDPE). The compatibilizers included a multiblock ethylene–octene copolymer (OBC), two statistical ethylene–octene copolymers (EO), two propylene–ethylene copolymers (P/E), and a styrenic block copolymer (SBC). Examination of the blend morphology by AFM showed that the compatibilizer was preferentially located at the interface between the PP matrix and the dispersed HDPE particles. The brittle‐to‐ductile (BD) transition was determined from the temperature dependence of the blend toughness, which was taken as the area under the stress–strain curve. All the compatibilized blends had lower BD temperature than PP. However, the blend compatibilized with OBC had the best combination of low BD temperature and high toughness. Examination of the deformed blends by scanning electron microscopy revealed that in the best blends, the compatibilizer provided sufficient interfacial adhesion so that the HDPE domains were able to yield and draw along with the PP matrix. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Characterization of the fracture behavior of glass fiber reinforced thermoplastics based on PP,PE‐HD,and PB‐1

This article deals with the influence of the polymeric matrix, such as isotactic polypropylene (iPP), polyethylene (PE‐HD), and isotactic polybutene‐1 (iPB‐1), and the glass fiber content on the material behavior of short glass fiber reinforced thermoplastics. The glass fiber content of all materials ranged between 0 and 50 wt %, which corresponds to a volume content between 0 and approx. 0.264. To describe the mechanical properties of all materials, the stiffness, strength, hardness, and toughness behavior were determined. The crack toughness behavior regarding unstable crack propagation was also assessed by applying fracture mechanics concepts. It was found that the energy‐determined J‐values for the PP material system reach their maximum at a glass fiber content of 0.135. In contrast, the crack toughness of the PE‐HD materials increases continuously with increasing glass fiber content due to the unchanged deformation ability at simultaneously increasing strength. The toughness level of the PB‐1 materials is nearly the same independent of the glass fiber content due to the opposite trend of the load and the deformation ability. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2010     

Effect of the structure on the morphology and spherulitic growth kinetics of polyolefin in‐reactor alloys

Four polyolefin in‐reactor alloys with different compositions and structures were prepared by sequential polymerization. All the alloys were fractionated into five fractions: a random copolymer of ethylene and propylene (25°C fraction), an ethylene–propylene segmented copolymer (90°C fraction), an ethylene homopolymer (110°C fraction), an ethylene–propylene block copolymer (120°C fraction), and a propylene homopolymer plus a minor ethylene homopolymer of high molecular weight (>120°C fraction). The effect of the structure on the morphology and spherulitic growth kinetics of the polypropylene (PP) component in the alloys was investigated. The polyolefin alloys containing a suitable block copolymer fraction and a larger amount of PP had a more homogeneous morphology, and the crystalline particles were smaller. Quenching the polyolefin alloys led to smaller crystallites and a more homogeneous morphology as well. Isothermal crystallization was carried out above the melting temperature of polyethylene, and the growth of PP spherulites was monitored with polarized optical microscopy with a hot stage. The alloys with higher propylene contents exhibited a faster spherulitic growth rate. The fold surface free energy was derived, and it was found that a large amount of block copolymer fractions and random copolymer fractions could reduce the fold surface free energy. The structure of the alloys also affected the crystallization regime of PP. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 98: 632–638, 2005