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1.
In this article, high density polyethylene/styrene‐ethylene‐butylene‐styrene block copolymer blends (HDPE/SEBS) grafted by maleic anhydride (HDPE/SEBS‐g‐MAH), which is an effective compatibilizer for HDPE/wood flour composites was prepared by means of torque rheometer with different contents of maleic anhydride (MAH). The experimental results indicated that MAH indeed grafted on HDPE/SEBS by FTIR analysis and the torque increased with increasing the content of maleic anhydride and dicumyl peroxide (DCP). Styrene may increase the graft reaction rate of MAH and HDPE/SEBS. When HDPE/SEBS MAH was added to HDPE/wood flour composites, tensile strength and flexural strength of composites can reach 25.9 and 34.8 MPa in comparison of 16.5 and 23.8 MPa (without HDPE/SEBS‐g‐MAH), increasing by 157 and 146%, respectively. Due to incorporation of thermoplastic elastomer in HDPE/SEBS‐g‐MAH, the Notched Izod impact strength reached 5.08 kJ m?2, increasing by 145% in comparison of system without compatibilizer. That HDPE/SEBS‐g‐MAH improved the compatibility was also conformed by dynamic mechanical measurement. Scanning electron micrographs provided evidence for strong adhesion between wood flour and HDPE matrix with addition of HDPE/SEBS‐g‐MAH. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci 2007  相似文献   

2.
A new and effective route to synthesize conducting polyaniline‐multiwalled carbon nanotube (PANI ‐f‐MWNT) nanocomposites (where ‘f’ denotes that the MWNTs have been functionalized) starting with amine‐protected 4‐aminophenol is reported. Aminophenol‐functionalized MWNTs were initially synthesized by functionalizing acyl chloride‐terminated nanotubes with N‐(tert‐butoxycarbonyl)‐4‐aminophenol followed by the in situ chemical oxidative grafting of aniline in the presence of ammonium persulfate as an oxidizing agent. Control of the morphology and thickness of the polymer–MWNT nanocomposites was achieved by varying the weight ratios of aniline monomers and MWNTs in the polymerization process. Fourier transform infrared spectroscopy was employed to characterize the initial changes in surface functionalities which also confirmed that PANI was covalently grafted to the MWNTs. Electron microscopy and UV‐visible absorption spectroscopy were employed to characterize the morphology and chemical structure of the resulting hybrids. The results obtained indicate that the structure of the MWNTs was not perturbed by the incorporation of PANI. The content of the polymer in the nanocomposites was determined thermogravimetrically, while the electrical conductivity was obtained using four‐probe measurements. The PANI ‐f‐MWNT nanocomposites were adopted as templates for further decoration with gold nanoparticles in solution, thus opening new possibilities for their prospective technological applications. Copyright © 2010 Society of Chemical Industry  相似文献   

3.
Poly(butylene terephthalate)/high density polyethylene (PBT/HDPE) blends and PBT/HDPE‐grafted maleic anhydride (PBT/HDPE‐g‐MAH) blends were prepared by the reactive extrusion approach, and the effect of blend compositions on the morphologies and properties of PBT/HDPE blends and PBT/HDPE‐g‐MAH blends was studied in detail. The results showed that flexural strength, tensile strength, and notched impact strength of PBT/HDPE blends decreased with the addition of HDPE, and flexural strength and tensile strength of PBT/HDPE‐g‐MAH blends decreased, while the notched impact strength of PBT/HDPE‐g‐MAH increased with the addition of HDPE‐g‐MAH. Compared with PBT/HDPE blends, the dimension of the dispersed phase particles in PBT/HDPE‐g‐MAH blends was decreased and the interfacial adhesion was increased. On the other hand, the effects of HDPE and HDPE‐g‐MAH contents on the crystalline and the rheological properties of the blends were also investigated. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 102: 6081–6087, 2006  相似文献   

4.
Multiwalled carbon nanotubes‐graft‐polystyrene (MWNTs‐g‐PS) was synthesized by atom transfer nitroxide radical coupling chemistry. MWNTs with 2,2,6,6‐tetramethylpiperidine‐1‐oxy (MWNTs‐TEMPO) groups was prepared first by esterification of 4‐hydroxy (HO)‐TEMPO and carboxylic acid group on the surface of MWNTs (MWNTs‐COOH); PS with bromide end group (PS‐Br) were then obtained by atom transfer radical polymerization using ethyl 2‐bromoisobutyrate as initiator and CuBr/N,N,N′,N″,N″‐pentamethyldiethylenetriamine as catalyst. The MWNTs‐TEMPO was mixed with PS‐Br and heated to 90°C in the presence of CuBr/PMDETA to form MWNTs‐g‐PS. The product was characterized by FTIR, NMR, TGA, and TEM. TEM indicates that the MWNTs are enveloped by the polymer molecules. The content of grafted polymers is 46.7% by TGA measurements when the number‐average molecular weight (Mn) of PS‐Br is 10,200 g/mol. The as‐prepared nanocomposites exhibit relatively good dispersibility in solvents such as CH2Cl2, THF, and toluene. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009  相似文献   

5.
Raw multiwall carbon nanotubes (MWNTs) were first treated with strongly oxidated acid to form MWNTs–COOH and driven to a high dispersion quality in the dispersing medium via ultrasonic method. Then the MWNTs/poly (p‐phenylene benzobisoxazole)(MWNTs–COOH/PBO) nanocomposites were prepared by an in situ polymerization technique. In this process, the morphological structure of MWNTs and MWNTs–COOH were investigated by XPS, FTIR, and TEM. The experimental results showed that the carboxyl group was introduced into the surface of nanotubes and the length of nanotubes was shortened. The images of SEM and AFM illustrated that the MWNTs–COOH was homogeneously dispersed in PBO matrix, and the DTA analysis indicated that the molecular weight of MWNTs–COOH/PBO was almost equal to that of PBO. Furthermore, the thermogravimetry results proved that the thermal property of MWNTs–COOH/PBO was more stable than that of PBO. Also, the knot strength and the tensile strength of MWNTs–COOH/PBO were 30% higher than that of PBO. In addition, the reaction route of the MWNTs–COOH and PBO oligomer was given according to the ATR–FTIR spectra of PBO polymer and MWNTs–COOH/PBO. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 102: 2500–2508, 2006  相似文献   

6.
In this study, poly(ethylene terephthalate)/organo‐montmorillonite (PET/OMMT) nanocomposites were melt‐compounded using twin screw extruder followed by injection molding. Maleic anhydride grafted styrene‐ethylene/butylene‐styrene (SEBS‐g‐MAH) was used to improve the impact properties of the PET/OMMT nanocomposites. The notched and un‐notched impact strength of PET/OMMT nanocomposites increased at about 2.5 times and 5.5 times by the addition of 5 wt % of SEBS‐g‐MAH. Atomic force microscopy (AFM) scans were taken from the polished surface of both PET/OMMT and SEBS‐g‐MAH toughened PET/OMMT nanocomposites. The addition of SEBS‐g‐MAH altered the phase structure and clay dispersion in PET matrix. It was found that some of the OMMT silicate layers were encapsulated by SEBS‐g‐MAH. Further, the addition of SEBS‐g‐MAH decreased the degree of crystallinity of the PET/OMMT nanocomposites. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012  相似文献   

7.
High‐density polyethylene grafted isotactic polypropylene (PP‐g‐HDPE) was prepared by the imidization reaction between maleic anhydride grafted polyethylene and amine‐grafted polypropylene in a xylene solution. The branch density was adjusted by changes in the molar ratio between maleic anhydride and primary amine groups. Dynamic rheology tests were conducted to compare the rheological properties of linear polyolefins and long‐chain‐branched polyolefins. The effects of the density of long‐chain branches on the rheological properties were also investigated. It was found that long‐chain‐branched hybrid polyolefins had a higher storage modulus at a low frequency, a higher zero shear viscosity, a reduced phase angle, enhanced shear sensitivities, and a longer relaxation time. As the branch density was increased, the characteristics of the long‐chain‐branched structure became profounder. The flow activation energy of PP‐g‐HDPE was lower than that of neat maleic anhydride grafted polypropylene (PP‐g‐MAH) because of the lower flow activation energy of maleic anhydride grafted high‐density polyethylene (HDPE‐g‐MAH). However, the flow activation energy of PP‐g‐HDPE was higher than that of PP‐g‐MAH/HDPE‐g‐MAH blends because of the presence of long‐chain branches. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2009  相似文献   

8.
A functionalized high‐density polyethylene (HDPE) with maleic anhydride (MAH) was prepared using a reactive extruding method. This copolymer was used as a compatibilizer of blends of polyamide 6 (PA6) and ultrahigh molecular weight polyethylene (UHMWPE). Morphologies were examined by a scanning electron microscope. It was found that the dimension of UHMWPE and HDPE domains in the PA6 matrix decreased dramatically, compared with that of the uncompatibilized blending system. The size of the UHMWPE domains was reduced from 35 μm (PA6/UHMWPE, 80/20) to less than 4 μm (PA6/UHMWPE/HDPE‐g‐MAH, 80/20/20). The tensile strength and Izod impact strength of PA6/UHMWPE/HDPE‐g‐MAH (80/20/20) were 1.5 and 1.6 times as high as those of PA6/UHMWPE (80/20), respectively. This behavior could be attributed to chemical reactions between the anhydride groups of HDPE‐g‐MAH and the terminal amino groups of PA6 in PA6/UHMWPE/HDPE‐g‐MAH blends. Thermal analysis was performed to confirm that the above chemical reactions took place during the blending process. © 2000 John Wiley & Sons, Inc. J Appl Polym Sci 75: 232–238, 2000  相似文献   

9.
A series of novel nanocomposite hydrogels were prepared by a cross‐linking copolymerization method. Structural and morphological characterizations of the nanocomposite hydrogels revealed that a good compatibility exists between poly(acrylamide‐co‐sodium methacrylate) [P(AM‐co‐SMA)] and carboxyl‐functionalized carbon nanotubes (MWNTs–COOH). The P(AM‐co‐SMA)/MWNTs–COOH nanocomposite hydrogels with a suitable MWNTs–COOH loading exhibited better swelling capability, higher pH sensitivity, good reversibility, and repeatability, and rapid response to external pH stimuli, compared with the P(AM‐co‐SMA). The compression mechanical tests revealed that the nanocomposite hydrogel displayed excellent compressive strengths and elastic mechanical properties, with higher ultimate compressive stress, and meanwhile still retain a good recoverable strain in the presence of MWNTs–COOH. These excellent properties may primarily be attributed to effectively dispersing of a suitable MWNTs–COOH loading into the matrix of the polymers and formation of additional hydrogen bonds. The nanocomposite hydrogels were expected to find applications in drug controlled release and issue engineering. POLYM. COMPOS., 2012. © 2012 Society of Plastics Engineers  相似文献   

10.
Multiwalled carbon nanotubes (MWNTs) with acyl chloride functional groups and a metallocene polyethylene–octene elastomer (POE) or an acrylic acid‐grafted metallocene polyethylene–octene elastomer (POE‐g‐AA) were used to prepare hybrids (POE/MWNTs or POE‐g‐AA/MWNTs) using a melting method, with a view to identify a hybrid with improved thermal properties. Hybrids were characterized using Fourier transform infrared spectroscopy, 13C solid‐state nuclear magnetic resonance, X‐ray diffraction, thermogravimetry analysis, and scanning electron microscopy. MWNTs were purified using acid treatment, and results showed that ? COOH of MWNTs increased with acid treatment time and leveled off after 24‐h treatment. Much better dispersion and homogeneity of MWNTs was obtained with POE‐g‐AA in place of POE as the matrix. As a result, tensile strength at break of POE‐g‐AA/MWNTs was significantly improved even at 5 wt % MWNT content. Moreover, temperature of thermal decomposition for POE‐g‐AA/MWNTs was about 40–50°C higher than that for POE‐g‐AA, indicating higher thermal stability. This was because the carboxylic acid groups in POE‐g‐AA and the acyl chloride functional sites in MWNTs allow the formation of stronger chemical bonds. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci 104: 1328–1337, 2007  相似文献   

11.
The formation of core‐shell morphology within the dispersed phase was studied for composite droplet polymer‐blend systems comprising a polyamide‐6 matrix, ethylene‐propylene‐diene terpolymer (EPDM) shell and high density polyethylene (HDPE) core. In this article, the effect of EPDM with different molecular weights on the morphology and properties of the blends were studied. To improve the compatibility of the ternary blends, EPDM was modified by grafting with maleic anhydride (EPDM‐g‐MAH). It was found that core‐shell morphology with EPDM‐g‐MAH as shell and HDPE as core and separated dispersion morphology of EPDM‐g‐MAH and HDPE phase were obtained separately in PA6 matrix with different molecular weights of EPDM‐g‐MAH in the blends. DSC measurement indicated that there may be some co‐crystals in the blends due to the formation of core‐shell structure. Mechanical tests showed that PA6/EPDM‐g‐MAH/HDPE ternary blends with the core‐shell morphology exhibited a remarkable rise in the elongation at break. With more perfect core‐shell composite droplets and co‐crystals, the impact strength of the ternary blends could be greatly increased to 51.38 kJ m?2, almost 10 times higher than that of pure PA6 (5.50 kJ m?2). POLYM. ENG. SCI., 2013. © 2012 Society of Plastics Engineers  相似文献   

12.
Ternary nanocomposites based on poly(butylene terephthalate) (PBT), maleic anhydride grafted poly(ethylene‐co‐vinyl acetate) (EVA‐g‐MAH), and organically modified montmorllonite (organoclays) were prepared through four different blending sequences in a Haake rheocord mixer: (1) To blend PBT, EVA‐g‐MAH and organoclays in one step; (2) First to prepare EVA‐g‐MAH/organoclay nanocomposite, then mix it with PBT to get the final nanocomposite; (3) To mix PBT with organoclays first, then the PBT/organoclay nanocomposite with EVA‐g‐MAH. (4) To mix organoclays with the PBT/EVA‐g‐MAH blend. The microstructure of the PBT/EVA‐g‐MAH/organoclay ternary hybrids was characterized by X‐ray diffraction (XRD) and transmission electron microscopy (TEM). It was found that the blending sequence significantly influences the microstructure of PBT/EVA‐g‐MAH/organoclay ternary hybrids and the dispersion behavior of the organoclays in the polymer matrix. Tensile and impact properties of the hybrids were also studied. The results showed that the mixing sequence (2) gives the best tensile and impact strength due to its fine “sea‐island” morphology of PBT/EVA‐g‐MAH blend and good dispersion of the organoclays in the continuous PBT matrix.  相似文献   

13.
A high‐density polyethylene (HDPE) masterbatch containing 20.2 wt% multiwalled carbon nanotubes (MWNTs) was melt diluted with neat HDPE using two different methods: a twin screw microcompounder and a single‐screw extruder. The electrical properties of these composites were assessed using bulk electrical conductivity measurements, their mechanical properties were evaluated using tensile tests and dynamic mechanical analysis (DMA), and percent crystallinity was determined by wide angle x‐ray diffraction (WAXD) and differential scanning calorimetry (DSC). A percolation threshold (pc) of 4.5 wt% MWNTs was found in compression‐molded samples. Extruded samples were prepared with nanotube concentrations below and above the compression‐molded percolation threshold (2 and 7 wt% MWNTs) and passed through the extruder twice before entering a low‐shear melt annealing zone. Different melt annealing times were used and their effects on the electrical and mechanical properties of the resulting quench‐cooled composites were evaluated. Results showed that extruded composites were nonconductive, indicating that a conductive nanotube network did not form on the time scale of these experiments. Annealing time also did not affect significantly the mechanical properties of the resulting solid composites. POLYM. ENG. SCI., 2012. © 2012 Society of Plastics Engineers  相似文献   

14.
The nonisothermal crystallization kinetics of high‐density polyethylene (HDPE) and polyethylene (PE)/PE‐grafted maleic anhydride (PE‐g‐MAH)/organic‐montmorillonite (Org‐MMT) nanocomposite were investigated by differential scanning calorimetry (DSC) at various cooling rates. Avrami analysis modified by Jeziorny, Ozawa analysis, and a method developed by Liu well described the nonisothermal crystallization process of these samples. The difference in the exponent n, m, and a between HDPE and the nanocomposite indicated that nucleation mechanism and dimension of spherulite growth of the nanocomposite were different from that of HDPE to some extent. The values of half‐time (t1/2), K(T), and F(T) showed that the crystallization rate increased with the increase of cooling rates for HDPE and composite, but the crystallization rate of composite was faster than that of HDPE at a given cooling rate. Moreover, the method proposed by Kissinger was used to evaluate the activation energy of the mentioned samples. It was 223.7 kJ/mol for composite, which was much smaller than that for HDPE (304.6 kJ/mol). Overall, the results indicated that the addition of Org‐MMT and PE‐g‐MAH could accelerate the overall nonisothermal crystallization process of PE. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 91: 3054–3059, 2004  相似文献   

15.
Organically modified montmorillonite (org‐MMT) and high‐density polyethylene (HDPE) grafted with silane groups (HDPE‐g‐silane) were melt compounded to give HDPE‐g‐silane‐blend‐org‐MMT nanocomposites. X‐ray diffractometry was performed to investigate the intercalation effect. Transmission electron microscopy was applied to observe the dispersion of org‐MMT layers in HDPE matrices. The results indicate that an intercalated structure can be easily obtained in HDPE‐g‐silane‐blend‐org‐MMT nanocomposites. Furthermore, positron annihilation lifetime spectroscopy was used to characterize the microstructure of the composites. It is found that the ortho‐positron (o‐Ps) intensity for HDPE‐g‐silane is decreased by approximately 10% with a narrower lifetime distribution than that for HDPE. With increasing org‐MMT concentration, the o‐Ps intensity I3 increases for HDPE‐g‐silane‐blend‐org‐MMT nanocomposites; however, for HDPE‐blend‐org‐MMT composites I3 decreases. It is found that HDPE composites with good dispersion can be obtained following appropriate modification of the HDPE. And silane grafting has an effect on the free volume of the HDPE nanocomposites. Copyright © 2007 Society of Chemical Industry  相似文献   

16.
Poly(lactic acid)/organo‐montmorillonite (PLA/OMMT) nanocomposites toughened with maleated styrene‐ethylene/butylene‐styrene (SEBS‐g‐MAH) were prepared by melt‐compounding using co‐rotating twin‐screw extruder followed by injection molding. The dispersibility and intercalation/exfoliation of OMMT in PLA was characterized using X‐ray diffraction and transmission electron microscopy (TEM). The mechanical properties of the PLA nanocomposites was investigated by tensile and Izod impact tests. Thermogravimetric analyzer and differential scanning calorimeter were used to study the thermal behaviors of the nanocomposite. The homogenous dispersion of the OMMT silicate layers and SEBS‐g‐MAH encapsulated OMMT layered silicate can be observed from TEM. Impact strength and elongation at break of the PLA nanocomposites was enhanced significantly by the addition of SEBS‐g‐MAH. Thermal stability of the PLA/OMMT nanocomposites was improved in the presence of SEBS‐g‐MAH. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012  相似文献   

17.
The reactive extrusion of maleic anhydride grafted polypropylene (PP‐g‐MAH) with ethylenediamine (EDA) as coupling agent is carried out in a corotating twin‐screw extruder to produce long chain branched polypropylene (LCBPP). Part of PP‐g‐MAH is replaced by maleic anhydride grafted high‐density polyethylene (HDPE‐g‐MAH) or linear low‐density polyethylene (LLDPE‐g‐MAH) to obtain hybrid long chain branched (LCB) polyolefins. Compared with the PP‐g‐MAH, PE‐g‐MAH, and their blends, the LCB polyolefins exhibit excellent dynamic shear and transient extensional rheological characteristics such as increased dynamic modulus, higher low‐frequency complex viscosity, broader relaxation spectra, significantly enhanced melt strength and strain‐hardening behaviors. The LCB polyolefins also have higher tensile strength, tensile modulus, impact strength and lower elongation at break than their blends. Furthermore, supercritical carbon dioxide (scCO2) is constructively introduced in the reactive extrusion process. In the presence of scCO2, the motor current of the twin extruder is decreased and LCB polyolefins with lower melt flow rate (MFR), higher complex viscosity and increased tensile strength and modulus can be obtained. This indicates that the application of scCO2 can reduce the viscosity of melt in extruder, enhance the diffusion of reactive species, and then facilitate the long chain branching reaction between anhydride group and primary amine group. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011  相似文献   

18.
Supermacroporous poly(2‐hydroxyethyl methacrylate) [poly(HEMA)]‐based monolithic cryogel column was prepared by radical cryocopolymerization of HEMA with N‐methacryloyl‐L ‐histidine methyl ester (MAH) as functional comonomer and N,N′‐methylene‐bisacrylamide (MBAAm) as crosslinker directly in a plastic syringe for affinity purification of lysozyme from chicken egg white. The monolithic cryogel containing a continuous polymeric matrix having interconnected pores of 10–50 μm size was loaded with Zn2+ ions to form the metal chelate with poly(HEMA‐MAH) cryogel. Poly(HEMA‐MAH) cryogel was characterized by swelling studies, FTIR, scanning electron microscopy, and elemental analysis. The equilibrium swelling degree of the poly(HEMA‐MAH) monolithic cryogel was 5.62 g H2O/g cryogel. Poly(HEMA‐MAH) cryogel containing 45.8 μmol MAH/g was used in the adsorption/desorption of lysozyme from aqueous solutions. The nonspecific adsorption of lysozyme was very low (7.5 mg/g). The maximum amount of lysozyme adsorption from aqueous solution in phosphate buffer was 209 mg/g at pH 7.0. It was observed that lysozyme could be repeatedly adsorbed and desorbed with the poly(HEMA‐MAH) cyogel without significant loss of adsorption capacity. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008  相似文献   

19.
Summary: The new nanocomposites consisting of metallocene poly(ethylene‐octene) (POE), silicate clay and wood flour (WF) were prepared by means of a melt blending method. In addition, maleic anhydride grafted poly(ethylene‐octene) (POE‐g‐MAH) was studied as an alternative to POE. The samples were characterized by XRD, FT‐IR spectroscopy, DSC, TGA, SEM, and mechanical testing. Based on the consideration of thermal and mechanical properties, it was found that the clay content of 11 wt.‐% was optimal for the preparation of POE‐g‐MAH/clay nanocomposites. The POE‐g‐MAH/clay/WF hybrid could obviously improve the mechanical properties of POE‐g‐MAH/WF hybrid since the former had the smaller WF phase size (being always less than 1.5 µm), the Si? O? C bond and the nanoscale dispersion of silicate layers in the polymer matrix. The biodegradation studies showed that the mass of hybrids reduced by about the content of WF. The new POE‐g‐MAH/clay/WF nanocomposites produced from our laboratory can provide a plateau tensile strength at break when the WF content was up to 50 wt.‐%.

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20.
Polypropylene (PP)/layered double hydroxide (LDH) nanocomposites were prepared by the direct melt intercalation method using maleic anhydride grafted polypropylene (PP‐g‐MAH) as a reactive compatibilizer. The compatibilization effects provided by PP‐g‐MAH in different weight fractions and their influence on the structure and properties of the final nanocomposites were investigated. The interactions and structural morphology of the nanocomposites were examined by Fourier transform infrared spectroscopy, X‐ray diffraction and transmission electron microscopy. Thermal, mechanical and rheological properties of these nanocomposites were investigated as a function of compatibilizer concentration. The detailed morphological and X‐ray diffraction results revealed that the degree of LDH dispersion increases as the amount of PP‐g‐MAH increases. Study of the linear viscoelastic properties showed that the storage modulus G′ is very sensitive to the microstructure of the nanocomposite. The thermal properties of the nanocomposites were significantly influenced by the weight fraction of PP‐g‐MAH due to the shielding and nucleating effect of exfoliated layers. Both the tensile strength and modulus showed substantial improvements with increasing PP‐g‐MAH content, while the elongation at break substantially decreased, although the presence of PP‐g‐MAH somewhat improves these values. The overall results showed that 10 wt% of compatibilizer is optimum to achieve nanocomposites with better performance. Copyright © 2011 Society of Chemical Industry  相似文献   

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