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1.
Physical blends of poly(ethylene terephthalate) (PET) and poly(ethylene isophthalate) (PEI), abbreviated PET/PEI (80/20) blends, and of PET and a random poly(ethylene terephthalate‐co‐isophthalate) copolymer containing 40% ethylene isophthalate (PET60I40), abbreviated PET/PET60I40 (50/50) blends, were melt‐mixed at 270°C for different reactive blending times to give a series of copolymers containing 20 mol % of ethylene isophthalic units with different degrees of randomness. 13C‐NMR spectroscopy precisely determined the microstructure of the blends. The thermal and mechanical properties of the blends were evaluated by DSC and tensile assays, and the obtained results were compared with those obtained for PET and a statistically random PETI copolymer with the same composition. The microstructure of the blends gradually changed from a physical blend into a block copolymer, and finally into a random copolymer with the advance of transreaction time. The melting temperature and enthalpy of the blends decreased with the progress of melt‐mixing. Isothermal crystallization studies carried out on molten samples revealed the same trend for the crystallization rate. The effect of reaction time on crystallizability was more pronounced in the case of the PET/PET60I40 (50/50) blends. The Young's modulus of the melt‐mixed blends was comparable to that of PET, whereas the maximum tensile stress decreased with respect to that of PET. All blend samples showed a noticeable brittleness. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 90: 3076–3086, 2003  相似文献   

2.
Blends of poly(ethylene terephthalate) (PET) and poly(ethylene octene) (POE) were prepared by melt blending with various amounts of trimethylolpropane triacylate (TMPTA). The mechanical properties, phase morphologies, and gel fractions at various absorbed doses of γ‐irradiation have been investigated. It was found that the toughness of blends was enhanced effectively after irradiation as well as the tensile properties. The elongation at break for all studied PET/POE blends (POE being up to 15 wt %) with 2 wt % TMPTA reached 250–400% at most absorbed doses of γ‐irradiation, approximately 50–80 times of those of untreated PET/POE blends. The impact strength of PET/POE (85/15 wt/wt) blends with 2 wt % TMPTA irradiated with as little as 30 kGy absorbed dose exceeded 17 kJ/m2, being approximately 3.4 times of those of untreated blends. The improvement of the mechanical properties was supported by the morphology changes. Scanning electron microscope images of fracture surfaces showed a smaller dispersed phase and more indistinct inter‐phase boundaries in the irradiated blends. This indicates increased compatibility of PET and POE in the PET/POE blends. The changes of the morphologies and the enhancement of the mechanical properties were ascribed to the enhanced inter‐phase boundaries by the formation of complex graft structures confirmed by the results of the gelation extraction and Fourier Transform Infrared analyses. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013  相似文献   

3.
Biosourced poly(lactic acid) (PLA) blends with different content of poly(ethylene oxide‐b‐amide‐12) (PEBA) were prepared by melt compounding. The miscibility, phase structure, crystallization behavior, mechanical properties, and toughening mechanism were investigated. The blend was an immiscible system with the PEBA domains evenly dispersed in the PLA matrix. The PEBA component suppressed the nonisothermal melt crystallization of PLA. With the addition of PEBA, marked improvement in toughness of PLA was achieved. The maximum for elongation at break and impact strength of the blend reached the level of 346% and 60.5 kJ/m2, respectively. The phase morphology evolution in the PLA/PEBA blends after tensile and impact tests was investigated, and the corresponding toughening mechanism was discussed. It was found that the PLA matrix demonstrates obvious shear yielding in the blend during the tensile and impact tests, which induced energy dissipation and therefore lead to improvement in toughness of the PLA/PEBA blends. POLYM. COMPOS., 2013. © 2012 Society of Plastics Engineers  相似文献   

4.
Binary blends of poly(vinyl chloride) (PVC) with α‐methylstyrene‐acrylonitrile‐butadiene‐styrene copolymer (AMS‐ABS) were prepared via melt blending. A single glass transition temperature (Tg) was observed by differential scanning calorimetry, thus indicating that PVC is miscible with the α‐methylstyrene‐acrylonitrile‐styrene in AMS‐ABS. The results from attenuated total reflection Fourier transform infrared spectra indicated that specific strong interactions were not available in the blends. With increasing amounts of AMS‐ABS, both heat distortion temperature and thermal stability were increased considerably. With regard to mechanical properties, flexural and tensile properties decreased with increasing AMS‐ABS content. A synergism was observed in impact strength. The morphology of both impact‐fractured and tensile‐fractured surfaces, observed by scanning electron microscopy, correlated well with the mechanical properties. It is suggested that there was a transition of fracture mechanisms with the changing composition of the binary blends—from shear yielding for blends rich in PVC to cavitation for blends rich in AMS‐ABS. J. VINYL ADDIT. TECHNOL., 19:1–10, 2013. © 2013 Society of Plastics Engineers  相似文献   

5.
One of the most significant limitations to widespread industrial implementation of emerging bioplastics such as poly(lactic acid) and poly(hydroxyalkanoate) (PHA) is that they do not match the flexibility and impact resistance of petroleum‐based plastics like poly(propylene) or high‐density poly(ethylene). The basic goal of this research is to identify alternative, affordable, sustainable, biodegradable materials that can replace petroleum‐based polymers in a wide range of industrial applications, with an emphasis on providing a solution for increasing the flexibility of PHA to a level that makes it a superior material for bioplastic nursery‐crop containers. A series of bio‐based PHA/poly(amide) (PA) blends with different concentrations were mechanically melt processed using a twin‐screw extruder and evaluated for physical characteristics. The effects of blending on viscoelastic properties were investigated using small‐amplitude oscillatory shear flow experiments to model the physical character as a function of blend composition and angular frequency. The mechanical, thermal, and morphological properties of the blends were investigated using dynamic mechanical analysis, differential scanning calorimetry, thermogravimetric analysis, scanning electron microscopy, and tensile tests. The complex viscosity of the blends increased significantly with increasing concentration of PHA and reached a maximum value for 80 wt % PHA blend. In addition, the tensile strength of the blends increased markedly as the content of PHA increased. For blends containing PA at >50 wt %, samples failed only after a very large elongation (up to 465%) without significant decrease in tensile strength. The particle size significantly increased and the blends became more brittle with increasing concentration of PHA. In addition, the concentration of the PA had a substantial effect on the glass relaxation temperature of the resulting blends. Our results demonstrate that the thermomechanical and rheological properties of PHA/PA blends can be tailored for specific applications, and that blends of PHA/PA can fulfill the mechanical properties required for flexible, impact‐resistant bio‐based nursery‐crop containers. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42209.  相似文献   

6.
A series of blends of furan‐based green polyesters, for eco‐friendly packaging materials, are synthesized. Poly(ethylene 2,5‐furandicarboxylate) (PEF), poly(propylene 2,5‐furandicarboxylate) (PPF), and poly(butylene 2,5‐furandicarboxylate) (PBF) are synthesized by applying melt polycondensation. Blends of the above polyesters with 50/50 w/w composition as well as blends of furanoate/terephthalate (PPF/PPT) are also prepared. The glass temperature along with the crystallization and melting behaviors of melt quenched blends are studied aiming at understanding their dynamic state and miscibility. Based on their Tg and crystallization behavior, PEF/PPF shows dynamic homogeneity and miscibility whereas PPF/PBF and PEF/PBF exhibit partial miscibility and immiscibility, respectively. In an effort to dynamically homogenize the compounds, reactive blending is applied and the behavior of the resulting blends is monitored following quenching. A profound improvement in blend homogenization is observed with increasing melt mixing time for the PPF/PPT sample, evidenced by the single glass temperature and by the narrowing in liquid‐to‐glass regime. The obtained single glass temperature together with the suppressed tendency for crystallization with increasing mixing time are taken as evidences of dynamic and thermodynamic homogeneity.  相似文献   

7.
Polylactide (PLA) was melt blended with poly(1,2‐propylene glycol adipate) (PPA) in a Thermo‐Haake mixer. Thermal, mechanical, and rheological properties of the blends were investigated by means of differential scanning calorimetry, dynamic mechanical analysis, tensile test, and small amplitude oscillatory shear rheometry. PPA lowered the glass transition temperature and increased the ability of PLA to cold crystallization. With the increase in PPA content (5–25 wt%), the blends showed decreased tensile strength and Young's modulus; however, impact strength and elongation‐at‐break along were dramatically increased due to the plastic deformation. Morphological results of PLA/PPA blends showed that PPA was good compatible with PLA. The plasticization effect of PPA was also manifested by the lowering of dynamic storage modulus and viscosity in the melt state of the blends compared with neat PLA. POLYM. ENG. SCI., 2013. © 2012 Society of Plastics Engineers  相似文献   

8.
Poly(lactic acid)/poly(ethylene‐co‐vinyl acetate)/starch (PLA/EVA/starch) ternary blends were prepared by multi‐step melt processing (reactive extrusion) in the presence of maleic anhydride (MA), benzoyl peroxide and glycerol. The effects of MA and glycerol concentration on the morphology and properties of the PLA/EVA/starch blends were studied using scanning electron microscopy, transmission electron microscopy, atomic force microscopy, the Molau experiment, dynamic mechanical thermal analysis and differential scanning calorimetry etc. The plasticization and compatibilization provided a synergistic effect to these blends accompanied by a significant reduction in starch particle size and an increase in interfacial adhesion. Starch was finely dispersed in the ternary blends with a dimension of 0.5 ? 2 µm. Furthermore, EVA‐coated starch or a starch‐in‐EVA type of morphology was observed for the reactively compatibilized PLA/EVA/starch blends. The EVA with starch gradually changed into a co‐continuous phase with increasing MA concentration. Consequently, the toughness of the blends was improved. Since property stability of starch is an issue, the tensile properties of these blends were measured after different storage times and the blends showed good property stability. Copyright © 2012 Society of Chemical Industry  相似文献   

9.
Recycled poly(ethylene terephthalate) (rPET), obtained mainly from postconsumer bottles, was melt‐mixed with either poly(butylene adipate‐co‐terephthalate) (PBAT) or PBAT plus ultrafine wollastonite (~5 μm) at different weight ratios on a twin‐screw extruder and then injection‐molded. Among the five rPET/PBAT blends (10–50 wt% PBAT) evaluated, the 80/20 wt% rPET/PBAT blend exhibited the highest tensile strength and degree of crystallinity, a slight increase in the tensile strain, and a remarkable increase in the melt flow index, but a lower tensile modulus and thermal stability with respect to the neat rPET. This blend was subsequently filled with four loading levels of wollastonite (10–40 wt%), where the tensile properties (modulus, strain at break, and strength) and thermal stability of the blend were all improved by the addition of wollastonite in a dose‐dependent manner. Based on differential scanning calorimetry analysis, the crystallinity of rPET in the rPET/PBAT/wollastonite composites decreased in the presence of wollastonite, accompanied with a noticeable increase in the glass transition, cold crystallization, and crystallization temperatures, but only a slight change in the melting temperature was noted compared with those of the neat 80/20 wt% blend. Moreover, the addition of wollastonite at 30 wt% or higher showed a strong reduction in the melt dripping of the composites during combustion. J. VINYL ADDIT. TECHNOL., 23:106–116, 2017. © 2015 Society of Plastics Engineers  相似文献   

10.
In a blend of two immiscible polymers a controlled morphology can be obtained by adding a block or graft copolymer as compatibilizer. In the present work blends of low‐density polyethylene (PE) and polyamide‐6 (PA‐6) were prepared by melt mixing the polymers in a co‐rotating, intermeshing twin‐screw extruder. Poly(ethylene‐graft‐polyethylene oxide) (PE‐PEO), synthesized from poly(ethylene‐co‐acrylic acid) (PEAA) (backbone) and poly(ethylene oxide) monomethyl ether (MPEO) (grafts), was added as compatibilizer. As a comparison, the unmodified backbone polymer, PEAA, was used. The morphology of the blends was studied by scanning electron microscopy (SEM). Melting and crystallization behavior of the blends was investigated by differential scanning calorimetry (DSC) and mechanical properties by tensile testing. The compatibilizing mechanisms were different for the two copolymers, and generated two different blend morphologies. Addition of PE‐PEO gave a material with small, well‐dispersed PA‐spheres having good adhesion to the PE matrix, whereas PEAA generated a morphology characterized by small PA‐spheres agglomerated to larger structures. Both compatibilized PE/PA blends had much improved mechanical properties compared with the uncompatibilized blend, with elongation at break b) increasing up to 200%. Addition of compatibilizer to the PE/PA blends stabilized the morphology towards coalescence and significantly reduced the size of the dispersed phase domains, from an average diameter of 20 μm in the unmodified PE/PA blend to approximately 1 μm in the compatibilized blends. © 2000 John Wiley & Sons, Inc. J Appl Polym Sci 78: 2416–2424, 2000  相似文献   

11.
Hydroxyl‐terminated poly(lactic acid) prepolymer (LA prepolymer) were prepared via L ‐lactic acid as monomer, 1,4‐butanediol as blocking agent and Sn(II) octoate as catalyst by direct melt polymerization. Then the LA prepolymer was blended with starch followed by in situ chain extending reaction using different content of TDI as chain extender, producing the high molecular weight of poly(ester urethane) in the blends. The LA prepolymer/starch‐TDI blends were characterized by GPC, 1H‐NMR, SEM, DSC, tensile strength testing, and water resistance. The SEM results of cross‐section show that, compared with the simple PLA/starch blends, almost the starch granules were completely covered by ploy(ester urethane) in the LA prepolymer/starch‐TDI blends system. In comparison to the simple PLA/starch blends, the mechanical properties of LA prepolymer/starch‐TDI blends were increased, such as tensile strength increasing from 18.6 ± 3.8 to 44.2 ± 6.2 Mpa, tensile modulus increasing from 510 ± 62 to 1,850 ± 125 Mpa and elongation at break increasing from 1.8 ± 0.4 to 4.0 ± 0.5 %, respectively. This is attributed to high weight of poly (ester urethane) was formed via in situ reaction of the end of hydroxyl (LA prepolymer) and isocyanate groups and the starch granules were easily covered by ploy(ether urethane) via in situ polymerization in the blends. Moreover, covalent linkage was formed between the two phases interfaces. As a result, the interfacial adhesion was enhance and improved the mechanical property. In addition, the water resistance of LA prepolymer/starch‐TDI blends was much better that of the simple PLA/starch blends. POLYM. COMPOS., 2013 © 2013 Society of Plastics Engineers  相似文献   

12.
Films of LDPE containing 1–10 wt % of various polymeric additives were prepared by different techniques. Three poly(ethylene‐graft‐ethylene oxide)s synthesized by grafting poly(ethylene‐co‐acrylic acid) with poly(ethylene oxide) monomethyl ether (MPEO), and two pure MPEOs having molecular weights 750 and 2000 were used as additives. The additives were mixed with LDPE both by blending in a common solvent and by melt mixing. The blends were then solvent cast from xylene onto glass Petri dishes or compression molded between glass plates. The film surfaces were studied by water contact angle measurements and by X‐ray photoelectron spectroscopy (XPS), and melting points and heats of melting were recorded by differential scanning calorimetry (DSC). The blends had a two‐phase morphology, with enrichment of the graft copolymers at the glass–polymer interface, as shown by contact angle values and XPS spectra. Large differences in the interface accumulation between the different film samples were observed. Films prepared by compression molding of solution‐mixed blends exhibited much lower surface accumulation of graft copolymer at the glass–polymer interface than did the solvent cast or melt‐mixed/compression‐molded samples. © 2000 John Wiley & Sons, Inc. J Appl Polym Sci 75: 316–326, 2000  相似文献   

13.
The blends of poly(ether sulfone) and poly(aryl ether ketone) containing 1,4‐naphthalene were prepared by melt mixing in a Brabender‐like apparatus. The specimens for measurements were made by compression molding under pressure and then were water‐quenched at room temperature. The tensile strength, tensile modulus, elongation at break, thermal analysis, and scanning electron microscopy were each measured. The dependence of tensile strength, tensile modulus, and elongation at break on blend systems was obtained. The effects of composition and miscibility on the mechanical properties are discussed. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 99: 472–476, 2006  相似文献   

14.
Crushed tire rubber particles (CR) have been dispersed into a recycled poly(carbonate) matrix (rPC) to obtain an eco‐friendly plastic (EFP). A positive synergy was expected from the association of an elastomeric phase to a tough thermoplastic matrix, helping on the other hand to develop a plastic with low impact on the environment. Mechanical melt‐mixing alone cannot provide a suitable interface, and led to blends with poor mechanical properties. Consequently, we have investigated different strategies to improve the EFP properties: First, the rubber surface has been treated by flaming or washing with dichloromethane and second, two copolymers, poly(ethylene‐co‐ethyl acrylate‐tert‐hydroxyl methacrylate) (E‐EA‐MAH) and poly(ethylene‐co‐methyl acrylate‐ter‐glycidyl methacrylate) (E‐MA‐GMA), were used to compatibilize CR particles with rPC matrix by reactive melt‐mixing in an internal mixer. The resulting blends mechanical properties were studied through static tension experiments and interpreted to the light of electronic microscopy fractography analysis and nanoindentation experiments. Significant gain of mechanical properties can be obtained by decreasing CR size under 140 μm (especially for CR contents between 5 and 20% m/m). To reach similar properties with rubber particles of diameter over 140 μm (but under 350 μm), it is necessary to activate their surface by either dichloromethane washing or flaming. Additional use of a compatibilizer extends the plastic behaviour domain of the EFP. rPC‐20% w/w CR is the best alternative material of our study. POLYM. ENG. SCI., 47:1768–1776, 2007. © 2007 Society of Plastics Engineers  相似文献   

15.
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  相似文献   

16.
Biodegradable blends of poly(propylene carbonate) (PPC) and poly(ethylene‐co‐vinyl alcohol) (EVOH) were melt compounded in a batch mixer followed by compression molding. The processability, mechanical properties, thermal behavior, and morphologies of the blends were investigated with torque rheometer, Fourier transform infrared spectroscopy, tensile tests, dynamic mechanical analysis, thermogravimetric analysis, differential scanning calorimetry, and scanning electron microscopy. Torque rheometry indicated good interfacial miscibility between PPC and EVOH phases, and then fourier transform infrared spectroscopy spectra demonstrated that a certain extent of hydrogen‐bonding interactions between PPC and EVOH matrix in the blends. A study of the mechanical properties and thermal behavior showed that the EVOH incorporation can significantly enhance the tensile strength, thermal stability, and crystallinity of the blends. Moreover, dynamic mechanical analysis and differential scanning calorimetry both revealed that PPC and EVOH were compatible to some extent. Further, scanning electron microscopic examination also revealed the good interfacial adhesion between EVOH and PPC phases. POLYM. ENG. SCI., 47:174–180, 2007. © 2007 Society of Plastics Engineers  相似文献   

17.
The transesterification reaction of poly(ethylene terephthalate)/poly(ethylene 2,6‐naphthalate) blends during melt‐mixing was studied as a function of blending temperature, blending time, blend composition, processing equipment, and different grades of poly(ethylene terephthalate) and poly(ethylene 2,6‐naphthalate). Results show that the major factors controlling the reaction are the temperature and time of blending. Efficiency of mixing also plays an important role in transesterification. The reaction kinetics can be modeled using a second‐order direct ester–ester interchange reaction. The rate constant (k) was found to have a minimum value at an intermediate PEN content and the activation energy of the rate constant was calculated to be 140 kJ/mol. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 80: 2422–2436, 2001  相似文献   

18.
The compatibility of low‐density polyethylene and poly(ethylene‐co‐vinyl acetate) containing 18 wt % vinyl acetate units (EVA‐18) was studied. For this purpose, a series of different blends containing 25, 50, or 75 wt % EVA‐18 were prepared by melt mixing with a single‐screw extruder. For each composition, three different sets of blends were prepared, which corresponded to the three different temperatures used in the metering section and the die of the extruder (140, 160, and 180°C), at a screw rotation speed of 42 rpm. Blends that contained 25 wt % EVA‐18 were also prepared through mixing at 140, 160, or 180°C but at a screw speed of 69 rpm. A study of the blends by differential scanning calorimetry showed that all the prepared blends were heterogeneous, except that containing 75 wt % EVA‐18 and prepared at 180°C. However, because of the high interfacial adhesion, a fine dispersion of the minor component in the polymer matrix was observed for all the studied blends with scanning electron microscopy. The tensile strengths and elongations at break of the blends lay between the corresponding values of the two polymers. The absence of any minimum in the mechanical properties was strong evidence that the two polymers were compatible over the whole range of composition. The thermal shrinkage of the blends at various temperatures depended mainly on the temperature and EVA‐18 content. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 90: 841–852, 2003  相似文献   

19.
In this work, ethylene‐co‐vinyl acetate (EVA), poly(ethylene‐co‐octene) (POE), and poly(vinyl chloride) (PVC) blends were processed in a molten state process using a corotating twin‐screw extruder to assess both the balance of mechanical properties and physical interactions in the melt state. Tensile measurements, scanning electron microscopy, and oscillatory rheometry were performed. By means of flow curves, the parameters of the power law as well as the distribution of relaxation times were assessed with the aid of a nonlinear regularization method. The mechanical properties for the EVA‐POE blend approximated the values for POE, while inclusion of PVC shifted the modulus values to those of neat EVA. The rise in modulus was corroborated by the PVC phase dispersion as solid particles that act as a reinforcement for the ternary blend. The rheological properties in the molten state show that the POE does not present molecular entanglement effects and so tends both to diminish the EVA mechanical properties and increase the fluidity of the blend. However, the addition of PVC both restored the EVA typical pseudoplastic feature and promoted the increase in the viscosity and the mechanical properties of the ternary blend. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013  相似文献   

20.
Biobased non‐fossil polyester poly(3‐hydroxybutyrate‐co‐4‐hydroxybutyrate) (P3/4HB) containing 4.0 mol % 4‐hydroxybutyrate (4HB) was melt‐mixed with short glass fibers (SGF) via a co‐rotating twin‐screw extruder. The compositing conditions, average glass fiber length and distribution, thermal, crystallization, and mechanical properties of the P3/4HB/SGF composites were investigated. Calcium stearate, two kinds of paraffin wax and modified ethylene bis‐stearamide (TAF) were investigated as lubricants for the P3/4HB/SGF composites. It revealed that TAF is the most efficient lubricant of the P3/4HB/SGF composites. Coupling agents 2,2′‐(1,3‐phenylene)bis‐2‐oxazoline (1,3‐PBO) and pyromellitic dianhydride (PMDA) were used as end‐group crosslinkers to reduce the degradation of P3/4HB and increase the mechanical properties of the P3/4HB/SGF composites. It showed that 1,3‐PBO is the efficient coupling agent. The optimum condition of the P3/4HB/SGF composites is 1.5 phr TAF, 1.0 phr 1,3‐PBO, and 30 wt % glass fiber content. And the maximum of tensile strength, tensile modulus, and impact strength of the composites is 3.7, 6.6, 1.8 times of the neat P3/4HB polymer, respectively. © 2012 Wiley Periodicals, Inc. J Appl Polym Sci, 2012  相似文献   

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