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1.
Polymer nanocomposites containing several percent of exfoliated layered silicates are materials with a unique weight/performance ratio. The only parameter that is not enhanced, but even decreased, is toughness. This work focused on the toughness enhancement of these advanced systems with polyamide matrix prepared via melt‐mixing (i.e., by a conventional method of polymer processing having an advantage of easy simultaneous addition of other components). Analogously to ternary polyamide blends with improved mechanical behavior, containing finely and separately dispersed elastomer and rigid polymer, elastomer particles with an average size of 60 nm were incorporated in the nanocomposite. The very low particle size was achieved by in situ reactive compatibilization by using suitably functionalized elastomers. The simultaneously increasing viscosity of the system enhanced exfoliation of the silicate. Melt exfoliated nanocomposites containing 3 wt % of clay and 5 wt % of elastomer particles exhibit increased toughness without significant loss of other properties. Elastomer particles increase toughness by both acting as stress concentrators (by initiating energy absorbing microdeformations) and influencing the clay‐induced matrix crystalline structure. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 96: 288–293, 2005  相似文献   

2.
The effects of ethylene-methyl acrylate-glycidyl methacrylate (E-MA-GMA) terpolymer and three types of organoclays (Cloisite® 15A, 25A, and 30B) on mechanical and rheological properties, and morphology of impact modified polyamide-6/montmorillonite ternary nanocomposites were investigated by X-ray diffraction (XRD), transmission electron microscopy (TEM), scanning electron microscopy (SEM), parallel disk rheometry, melt flow index measurements, and tensile and impact tests. The materials were prepared by melt blending using a co-rotating twin-screw extruder. XRD and TEM analyses showed that exfoliated-intercalated nanocomposites were formed in both polyamide-6/Cloisite® 25A and Cloisite® 30B binary nanocomposites and in ternary systems. SEM micrographs showed that rubber domain sizes were larger in the nanocomposites than in their corresponding polyamide-6/elastomer blends. Generally, tensile strength, Young's modulus, and elongation at break decreased with the addition of elastomer to polyamide-6/organoclay binary nanocomposites. In the melt state, liquid-like behavior of polyamide-6 slightly turned to pseudo solid-like in the binary and ternary nanocomposites. © 2012 Wiley Periodicals, Inc. J Appl Polym Sci, 2012  相似文献   

3.
The effects of melt state compounding of ethylene‐butyl acrylate‐maleic anhydride (E‐BA‐MAH) terpolymer and/or three types of organoclays (Cloisite® 15A, 25A, and 30B) on thermal and mechanical properties and morphology of polyamide‐6 are investigated. E‐BA‐MAH formed spherical domains in the materials to which it is added, and increased the impact strength, whereas the organoclays decreased the impact strength. In general, the organoclays increased the tensile strength (except for Cloisite 15A), Young's modulus and elongation at break, but the addition of E‐BA‐MAH had the opposite effect. XRD patterns showed that the interlayer spacing for the organoclays Cloisite 25A and Cloisite 30B increased in both polyamide‐6/organoclay binary nanocomposites and in polyamide‐6/organoclay/impact modifier ternary systems. TEM analysis showed that exfoliated‐intercalated nanocomposites were formed. The crystallinities of polyamide‐6/organoclay nanocomposites were in general lower than that of polyamide‐6 (except for Cloisite 15A). In ternary nanocomposites, crystallinities generally were lower than those of polyamide‐6/organoclay nanocomposites. Cloisite 15A containing ternary nanocomposites had higher tensile and impact strengths and Young's modulus than the ternary nanocomposites prepared with Cloisite 25A and Cloisite 30B, owing to its surface hydrophobicity and compatibility with the impact modifier. POLYM. COMPOS., 2008. © 2007 Society of Plastics Engineers  相似文献   

4.
The objective of the study is to investigate the effect of inclusion of nanotalc on the strength properties of polyamide 6 (PA6)‐based binary and ternary nanocomposites. Binary nanocomposites were prepared by melt compounding of PA6 with varying content of nanotalc (1, 2, and 4 wt%). Ternary nanocomposites were prepared by melt compounding of compatibilized blend of PA 6 and ethylene‐co‐butyl acrylate (EBA elastomer) with varying content of nanotalc (1, 2, and 4 wt%). Both the binary and ternary nanocomposites registered a very high improvement in the strength/stiffness‐related properties at lower filler loading of 1 wt%. Phase morphology of the composites studied by SEM, TEM, and XRD revealed the formation of extended brane‐like structures and delaminated talc layers in the binary nanocomposites. The modulus predicted by Halpin‐Tsai and Mooney equation suggests that the composites retained a very good aspect ratio after melt mixing. Orientation effects of nanotalc enhanced the melt flow behavior in the composites. POLYM. ENG. SCI., 50:1978–1993, 2010. © 2010 Society of Plastics Engineers  相似文献   

5.
Thermoplastic elastomer (TPE) nanocomposites based on polyamide‐6 (PA6)/poly(epichlorohydrin‐co‐ethylene oxide) (ECO)/multiwall carbon nanotube (MWCNTs) were prepared by melt compounding process. Different weight ratios of ECO (20, 40, and 60 wt %) and two kinds of functionalized and non‐functionalized MWCNTs were employed to fabricate the nanocomposites. The morphological, rheological, and mechanical properties of MWCNTs‐filled PA6/ECO blends were studied. The scanning electron microscopy of PA6/ECO blends showed that the elastomer particles, ECO, are well‐dispersed within the PA6 matrix. The significant improvement in the dispersibility of the carboxylated carbon nanotubes (COOH‐MWCNTs) compared to that of non‐functionalized MWCNTs (non‐MWCNTs) was confirmed by transmission electron microscopy images. The tensile modulus of samples improved with the addition of both types of MWCNTs. However, the effect of COOH‐MWCNTs was much more pronounced in improving mechanical properties of PA6/ECO TPE nanocomposites. Crystallization results demonstrated that the MWCNTs act as a nucleation agent of the crystallization process resulted in increased crystallization temperature (Tc) in nanocomposites. Rheological characterization in the linear viscoelastic region showed that complex viscosity and a non‐terminal storage modulus significantly increased with incorporation of both types of MWCNTs particularly at low frequency region. The increase of rheological properties was more pronounced in the presence of carboxylic (COOH) functional groups, in the other words by addition of COOH‐MWCNTs. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 45977.  相似文献   

6.
The effect of addition of organoclay and the reactive ABS‐g‐MA core‐shell particles on the mechanical properties and morphology of blends of polyamide (PA6) were reported. The reactive rubber particles with core‐shell structure were selected as modifier instead of conventional reactive bulk rubber. The microstructure of the ternary nanocomposites was characterized by X‐ray diffraction (XRD), transmission electron microscopy (TEM), and scanning electron microscopy (SEM). Impact strength and stress–strain behavior of blends were measured as a function of organoclay content and core/shell ratio of ABS‐g‐MA. The organoclay plates affected the interfacial adhesion between polyamide and the core‐shell particles because of a shielding effect of organclay on the interacting of amine end groups of PA6 with the MA groups of ABS‐g‐MA. The poor dispersion behavior of ternary nanocomposites was observed when the core/shell ratio is 80/20, and with an increase of organoclay content, the core/shell dispersed phase size increased. Blends based on the maleated elastomer with the core/shell ratio 60/40 gave a more beneficial balance of toughness versus stiffness. POLYM. COMPOS., 35:864–871, 2014. © 2013 Society of Plastics Engineers  相似文献   

7.
The microstructure and mechanical properties of polypropylene (PP)/OMMT binary nanocomposites and PP/styrene‐6‐(ethylene‐co‐butylenes)‐6‐styrene triblock copolymer (SEBS)/OMMT ternary nanocomposites were investigated using X‐ray diffraction (XRD), transmission electron microscopy (TEM), and rheology and electromechanical testing machine. The results show that the organoclay layers are mainly intercalated and partially exfoliated in the PP‐based nanocomposites. The additions of SEBS and OMMT have no significant effect on the crystallization behavior of PP. At the same time, it can be concluded that the polymer chains of PP and SEBS have intercalated into the organoclay layers and increase the gallery distance after blending process based on the analytical results from TEM, XRD, and rheology, which result in the form of a percolated nanostructure in the PP‐based nanocomposites. The results of mechanical properties show that SEBS filler greatly improve the notched impact strength of PP, but with the sacrifice of strength and stiffness. OMMT can improve the strength and stiffness of PP and slightly enhance the notched impact strength of PP/PP‐g‐MA. In comparison with neat PP, PP/OMMT, and PP/SEBS binary composites, notched impact toughness of the PP/SEBS/OMMT ternary composites significantly increase. Moreover, the stiffness and strength of PP/SEBS/OMMT ternary nanocomposites are slightly enhanced when compared with neat PP. It is believed that the synergistic effect of both SEBS elastomer and OMMT nanoparticles account for the balanced mechanical performance of the ternary nanocomposites. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009  相似文献   

8.
Polyamide‐6/clay nanocomposites were prepared employing melt bending or compounding technique followed by injection molding using different organically modified clays. X‐ray diffraction and transmission electron microscopy were used to determine the molecular dispersion of the modified clays within the matrix polymer. Mechanical tests revealed an increase in tensile and flexural properties of the matrix polymer with the increase in clay loading from 0 to 5%. C30B/polyamide‐6 nanocomposites exhibited optimum mechanical performance at 5% clay loading. Storage modulus of polyamide‐6 also increased in the nanocomposites, indicating an increase in the stiffness of the matrix polymer with the addition of nanoclays. Furthermore, water absorption studies confirmed comparatively lesser tendency of water uptake in these nanocomposites. HDT of the virgin matrix increased substantially with the addition of organically modified clays. DSC measurements revealed both γ and α transitions in the matrix polymer as well as in the nanocomposites. The crystallization temperature (Tc) exhibited an increase in case of C30B/polyamide‐6 nanocomposites. Thermal stability of virgin polyamide‐6 and the nanocomposites has been investigated employing thermogravimetric analysis. POLYM. COMPOS., 28:153–162, 2007. © 2007 Society of Plastics Engineers  相似文献   

9.
In this study, elastomer toughening is explored as a means of recovering ductility of polyamide 6/intumescent flame-retardant composite systems. This was achieved using a maleic anhydride modified SEBS elastomer incorporated into the system by twin-screw melt extrusion. TEM micrographs show an even distribution of both flame retardant and elastomer particles. The effects of elastomer content on mechanical properties, Izod impact behavior, and flammability of the polymer system were investigated. The incorporation of flame retardant significantly degraded the elongation and ductility of the polymer system. The addition of the elastomer succeeded in significantly enhancing the Izod impact strength and partially recovering the elongation at break without compromising the flame-retardant performance. Micro-scale Combustion Calorimeter (MCC) tests show that samples containing both elastomer and FR additives exhibit slightly improved combustion properties compared to the original polyamide 6/intumescent flame-retardant system. Rubber loadings of up to 15?wt% were possible while still achieving the highest UL-94 V0 flame exposure rating indicating a self-extinguishing and non-drip behavior.  相似文献   

10.
Thermoplastic elastomer nanocomposites based on acrylonitrile butadiene rubber (NBR) and polyamide 6 (PA6), with acid functionalized single‐wall carbon nanotubes (SWNT), were prepared via a direct melt‐mixing process in an internal mixer. The influence of SWNT content (0, 0.5, 1, 1.5) on morphological properties of PA6/NBR with different ratios (80/20, 70/30, 60/40) were then investigated. Characterization of nanocomposites was conducted by using transmission electron microscopy, scanning electron microscopy, differential scanning calorimetry, and mechanical properties. Scanning electron microscopy micrographs proved the droplet‐matrix blend morphology in which the size of NBR droplets decreased as the SWNT loading increased, suggesting dispersion of SWNT in the PA6 phase. It was further proved by transmission electron microscopy images, showing homogenous dispersion of SWNT in the PA6 phase. Differential scanning calorimetry results showed a slightly reduced percentage of crystallinity in samples containing SWNT. The mechanical properties of nanocomposites indicated an enhancement in tensile strength, modulus, and hardness on increasing SWNT content. J. VINYL ADDIT. TECHNOL., 22:336–341, 2016. © 2014 Society of Plastics Engineers  相似文献   

11.
Addition of carbon nanotubes to immiscible polymer blends with co‐continuous morphology features to improve the electrical conductivity has attracted much attention in recent years; however, less attention has been paid to the effect of carbon nanotubes on the morphology and corresponding physical properties of immiscible polymer blends with typical sea‐island morphology. In this work, therefore, functionalized multiwalled carbon nanotubes (FMWCNTs) were introduced into an immiscible high density polyethylene/polyamide 6 (HDPE/PA6) blend which was compatibilized by maleic anhydride grafted HDPE (HDPE‐MA). The distribution of FMWCNTs and the phase morphologies of the nanocomposites were characterized using scanning electron microscopy and transmission electron microscopy. The crystallization and melting behaviors of the components were analyzed by differential scanning calorimetry, which is thought to be favorable for an understanding of the distribution of FMWCNTs. It is interesting to observe that the morphology of PA6 particles is very dependent on the method of preparation of the nanocomposites. Correspondingly, FMWCNTs exhibit an apparent reinforcement effect and/or an excellent toughening effect for the compatibilized HDPE/PA6 blend, depending upon their distribution state and the variation of PA6 morphology. This work proves that FMWCNTs have a potential application in further improving the mechanical properties of compatibilized immiscible polymer blends. Copyright © 2012 Society of Chemical Industry  相似文献   

12.
Superior impact properties were obtained when maleic anhydride grafted styrene ethylene/butylene styrene block copolymer (SEBS-g-MAH) was used as a compatibilizer in blends of polyamide 6 (PA 6) and isotactic polypropylene (PP), where polyamide was the majority phase and polypropylene the minority phase. The optimum impact properties were achieved when the weight relation PA:PP was 80:20 and 10 wt% SEBS-g-MAH was added. The blend morphology was systematically investigated. Transmission electron microscopy (TEM) indicated that the compatibilizer forms a cellular structure in the PA phase in addition to acting as an interfacial agent between the two polymer phases. In this cellular-like morphology the compatibilizer appears to form the continuous phase, while polyamide and polypropylene form separate dispersions. In microscopy, PA appeared as a fine dispersion and PP as a coarse dispersion. The mechanical properties indicated that in fact PA, too, is continuous, and the blend can be interpreted as possessing a modified semi-interpenetrating network (IPN) structure with separate secondary dispersion of PP. The coarser PP dispersion plays an essential role in impact modification. Binary blends of the compatibilizer and one blend component were also investigated separately. The same cellular structure was observed in the binary PA/SEBS-g-MAH blends, and SEBS-g-MAH again appeared to form the continuous phase when the elastomer concentration was at least 10 to 20 wt%. By contrast, in PP/SEBS-g-MAH only conventional dispersion of elastomeric SEBS-g-MAH was observed up to 40 wt% elastomer. Impact strength was improved and the elastic modulus was lowered in both PA/SEBS-g-MAH and PP/SEBS-g-MAH blends when the elastomer content was increased. The changes in modulus indicate that the semi-IPN-like structure is formed in the binary PA/SEBS-g-MAH blends as well as in the ternary structure.  相似文献   

13.
In this paper, polyamide‐6 and polyamide‐6 nanocomposites were prepared by direct melt intercalation technique. The thermal degradation behavior of both polyamide‐6 and polyamide‐6 clay nanocomposites has been studied. The apparent activation energy of the nanocomposites is almost the same with that of pure polymer under nitrogen, but the apparent activation energy of the nanocomposites is greatly enhanced in air atmosphere. This increasing trend coincides with the thermal analysis and the cone calorimeter results, which may suggest that the polymer/clay nanocomposites have a higher thermal stability and lower flammability. The kinetic analysis also indicates that the pyrolytic degradation and the thermal oxidative degradation of PA6 and PA6/OMT nanocomposites are two kinds of different reaction models. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci 104: 2297–2303, 2007  相似文献   

14.
Addition of small amounts (0.5-10 vol%) of multiwall carbon nanotubes (CNT) to thermoplastic elastomer Morthane produced polymer nanocomposites with high electrical conductivity (σ∼1-10 S/cm), low electrical percolation (?∼0.005) and enhancement of mechanical properties including increased modulus and yield stress without loss of the ability to stretch the elastomer above 1000% before rupture. In situ X-ray scattering during deformation indicated that these mechanical enhancements arise not only from the CNTs, but also from their impact on soft-segment crystallization. The deformation behavior after yielding of the nanocomposites, irrespective of CNT concentration, is similar to the unfilled elastomer, implying that the mechanistics of large deformation is mainly governed by the matrix. The relative enhancement of the Young's modulus of the nanocomposites is comparable to other elastomeric nanocomposites, implying that to the first order specific chemical details of the elastomeric system is unimportant.  相似文献   

15.
Elastomer nanocomposites reinforced with carbon nanofiber (CNF) decorated with metal nanoparticles exhibit excellent thermal, mechanical, and magnetic properties with low volume fraction of the reinforcement. Generally, metal nanoparticles are used to modify the surface of CNF, to improve their dispersion and contact resistance in the polymer matrix. In this study, Fe2O3 metal nanoparticles were decorated on CNF by electrostatic attraction via a green and facile solution‐based method. Interestingly, the CNF decorated with Fe2O3 (CNF‐Fe2O3)/elastomer improved both the tensile strength and the fatigue property of plain CNF/elastomer by as much as 57.2% and 27.2%, respectively. Moreover, the CNF‐Fe2O3/elastomer exhibited superior thermal conductivity, a twofold enhancement compared with carbon fibers. The elastomer nanocomposites consisting of CNF‐Fe2O3 also exhibited enhanced magnetic properties due to synergies between the Fe2O3 nanoparticles and the CNF. The elastomer nanocomposites prepared with CNF‐Fe2O3 will open significant new opportunities for preparing advanced elastomer nanocomposites for future engineering applications. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45376.  相似文献   

16.
Binary polyamide 66 nanocomposites containing 2 wt % organoclay, polyamide 66 blend containing 5 wt % impact modifier, and ternary polyamide 66 nanocomposites containing 2 wt % organoclay and 5 wt % impact modifier were prepared by melt compounding method. The effects of E-GMA and the types of the organoclays on the interaction between the organoclay and the polymer, dispersion of the organoclay, morphology, mechanical, flow, and thermal properties of the nanocomposites were investigated. Partial exfoliation and improved mechanical properties are observed for Cloisite® 15A and Cloisite® 25A nanocomposites. On the other hand, the organoclay was intercalated or in the form of tactoids in Cloisite® 30B nanocomposites. Components of the nanocomposites containing Cloisite® 15A and Cloisite® 25A were compounded in different addition orders. Mixing sequence of the components affected both the dispersion of the organoclay and the mechanical properties drastically. SEM analyses revealed that homogeneous dispersion of the organoclay results in a decrease in the domain sizes and promotes the improvements in the toughness of the materials. Melt viscosity was also found to have a profound effect on the dispersion of the organoclay according to MFI and XRD results. Crystallinity of the nanocomposites did not change significantly. It is only the type of the constituents and their addition order what dramatically influence the nanocomposite properties. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci 2008  相似文献   

17.
Reactive bulk rubber (EOR-g-MA) and reactive core-shell rubber (ABS-g-MA) are selected as toughening agents to toughen PA6 nanocomposites. The two blends are designed with 20?wt-% rubber phase and 3?wt-% organoclay. X-ray diffraction, transmission electron microscopy and scanning electron microscopy were used to evaluate the degree of exfoliation of organoclays and morphology of the nanocomposites. The organoclay platelets are well exfoliated in the nanocomposites. At the same time, the size of the elastomer particles and interfacial adhesion between polyamide 6 and elastomers are dramatically affected by the existence of organoclay. ABS-g-MA is found to promote the toughness efficiency of PA6 than does EOR-g-MA, which reveals higher impact strength and elongation at break. However, tensile strength and Young's modulus of PA6 blends based on EOR-g-MA elastomer are higher than those based on ABS-g-MA elastomer.  相似文献   

18.
This work is aimed at determining the effect of nanoclay and polyepichlorohydrin‐co‐ethylene oxide (ECO) content on the microstructure and mechanical properties of PA6/ECO thermoplastic elastomers (TPEs). TPE nanocomposites were prepared in a laboratory mixer using polyamide 6 (PA6), ECO, and an organoclay by a two‐step melt mixing process. First, the PA6 was melt blended with Cloisite 30B and then mixed by ECO rubber. X‐ray diffraction results and transmission electron microscopy image showed that the nanoclay platelets were nearly exfoliated in both the phases. The SEM photomicrograph of PA6 with ECO showed that the elastomer particles are dispersed throughout the polyamide matrix and the size of rubber particles is less than 3 μm. Introduction of organoclay in the PA6 matrix increased the size of dispersed rubber particles in comparison with the unfilled but otherwise similar blends. The nanoscale dimension of the dispersed clay results in an improvement of the tensile modulus of the nanocomposites. POLYM. ENG. SCI., 2011. © 2010 Society of Plastics Engineers  相似文献   

19.
Titanium dioxide nanoparticles were functionalized with toluene-2,4-diisocyanate and then polypropylene/polyamide 6 blends containing functionalized titanium dioxide were prepared using a twin-screw extruder. The nonisothermal crystallization and melting behaviors of the as-prepared nanocomposites were investigated using differential scanning calorimetry. The nonisothermal crystallization differential scanning calorimetry data were analyzed by the modified-Avrami (Jeziorny) and combination of Ozawa and Avrami (Mo) methods. It can be found that the Jeziorny method can be used to describe the main crystallization process, and the Mo method can better deal with nonisothermal crystallization kinetics of the polypropylene and polyamide 6 phase in polypropylene/polyamide 6-based nanocomposites. The nonisothermal crystallization analysis shows that the titanium dioxide nanoparticles have two effects on polypropylene/polyamide 6 blends, i.e., it can favor the improvement of crystallization ability and decrease the crystallization rate of the polypropylene and polyamide 6 phase in polypropylene/polyamide 6-based nanocomposites. For one thing, the functionalized titanium dioxide nanoparticles in the polypropylene/polyamide 6-based nanocomposites act as effective nucleation agents and result in higher crystallization temperature (T0) than that of the polypropylene and polyamide 6 in pure polypropylene/polyamide 6 blends, which indicated titanium dioxide nanoparticles favor the improvement of crystallization ability of the polypropylene and polyamide 6 phase. For another, the existence of functionalized titanium dioxide nanoparticles hinders the free movement of polymer chains and results in lower crystallinity than that of the polypropylene and polyamide 6 in pure polypropylene/polyamide 6 blends, which indicated titanium dioxide nanoparticles decrease the crystallization rate of the polypropylene and polyamide 6 phase in polypropylene/polyamide 6-based nanocomposites. The nonisothermal crystallization melting behaviors show that there is single or double melting peak, which varies with different cooling rates for the polyamide 6 phase in polypropylene/polyamide 6-based nanocomposites. Multiple melting peak is mainly caused by the different crystalline structure of the polyamide 6 phase, the melting peak I is mainly caused by γ crystal of the polyamide 6 phase, while the melting peak II corresponds to the thermodynamic stability of α crystal. Besides, the recrystallization of the polyamide 6 phase in the heating process, and the effect of the incorporation of the titanium dioxide nanoparticles may have some contributions to the appeared multiple melting peak of the polyamide 6 phase in the polypropylene/polyamide 6-based nanocomposites.  相似文献   

20.
A ternary blend of the PA6 matrix with a finely dispersed rigid polymer and elastomer is a system with well‐balanced mechanical properties. Its micromechanical behavior, especially that of the elastomer phase, apparently differs from corresponding binary mixtures. This study shows the influence of the elastomer type, modulus, and reactivity on the behavior of ternary blends in comparison with analogous binary PA6/elastomer combinations. The presence of rigid reactive poly(styrene‐co‐maleic anhydride) (SMA) enhanced the properties of all the systems studied. For nonreactive elastomers, the dominant effect was refinement of their size due to enhanced viscosity, whereas for functionalized low‐modulus elastomers, the very good balance of properties was due to synergistic influences of both finely dispersed phases. Of interest is the enhanced toughness of ternary blends also for more rigid elastomers having a low toughening efficiency in binary blends. An appropriate addition of rigid SMA together with an elastomer enhances the energy absorption of the matrix, probably without cavitation of very small elastomer particles. Of importance also is the simultaneous strain‐hardening effect of deformed rigid particles. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 89: 3647–3651, 2003  相似文献   

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