Polyester biocomposites from recycled natural fibers: Characterization and biodegradability

The structure, biodegradability, and morphological properties of composite materials composed of poly(butylene succinate adipate) (PBSA) and bamboo fiber (BF) were evaluated. Composites containing acrylic acid‐grafted PBSA (PBSA‐g‐AA/BF) exhibited noticeably enhanced compatibility between the two components. The dispersion of BF in the PBSA‐g‐AA matrix was highly homogeneous as a result of ester formation and the consequent creation of branched and crosslinked macromolecules between the carboxyl groups of PBSA‐g‐AA and hydroxyl groups in BF. In addition, the PBSA‐g‐AA/BF composite was more easily processed due to a lower melt viscosity. Each composite was subjected to biodegradation tests in an Acinetobacter baumannii compost. Morphological observations indicated severe disruption of film structure after 10–20 days of incubation, and both the PBSA and the PBSA‐g‐AA/BF composite films were eventually completely degraded. The PBSA‐g‐AA/BF films were more biodegradable than those made of PBSA and exhibited a lower molecular weight and intrinsic viscosity, implying a strong connection between these characteristics and biodegradability. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Polyester/natural fiber biocomposites: preparation,characterization, and biodegradability

In this study, the biodegradability, morphology, mechanical, and thermal properties of composite materials composed of polybutyleneterephthalate (PBT), acrylic acid-grafted PBT (PBT-g-AA), and sisal fibers (SFs) were evaluated. Composites containing acrylic acid-grafted PBT (PBT-g-AA/SF) exhibited superior mechanical properties because of their greater compatibility with SF than PBT/SF. The dispersion of SF in the PBT-g-AA matrix was highly homogeneous due to ester formation and the creation of branched and cross-linked macromolecules between the carboxyl groups of PBT-g-AA and the hydroxyl groups of SF. Furthermore, due to its lower melting temperature (T _m), the PBT-g-AA/SF composite was more readily synthesized. Each composite was subjected to biodegradation tests in a soil environment. Both the PBT and PBT-g-AA/SF composite films were completely degraded, with severe disruption of the film structures observed after 60–100 days of incubation. Although the degree of weight loss following burial indicated that both materials were biodegradable, even with high levels of SF loading, the higher water resistance of PBT-g-AA/SF films indicated their higher biodegradability than the PBT films.     

Performance and biodegradability of a maleated polyester bioplastic/recycled sugarcane bagasse system

The biodegradability, morphology, and mechanical properties of composite materials made of poly(butylene succinate adipate) (PBSA) and sugarcane bagasse (SCB) were evaluated. Composites containing maleic anhydride (MA)‐grafted PBSA (PBSA‐g‐MA/SCB) exhibited noticeably superior mechanical properties because of greater compatibility between the two components. The dispersion of SCB in the PBSA‐g‐MA matrix was highly homogeneous as a result of ester formation between the carboxyl groups of PBSA‐g‐MA and hydroxyl groups in SCB and the consequent creation of branched and crosslinked macromolecules. Each composite was subjected to biodegradation tests in a Rhizopus oryzae compost. Morphological observations indicated severe disruption of film structure after 60 days of incubation, and both the PBSA and the PBSA‐g‐MA/SCB composite films were eventually completely degraded. The PBSA‐g‐MA/SCB films were more biodegradable than those made of PBSA and exhibited a higher intrinsic viscosity, implying a strong connection between these characteristics and biodegradability. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Preparation and properties of L‐lactide‐grafted sisal fiber–reinforced poly(lactic acid) composites

Pretreatment of the sisal fiber (SF) grafting with L‐lactide (LA) monomer via a ring‐opening polymerization catalyzed by a Sn(II)‐based catalyst was performed to improve the interfacial adhesion between SF and poly (lactic acid) (PLA). Biocomposites from LA‐grafted SF (SF‐g‐LA) and PLA were prepared by compression molding with fiber weight fraction of 10, 20, 30, and 40%, and then were investigated in contrast with alkali‐treated sisal fiber (ASF) reinforced PLA composites and untreated SF reinforced PLA composites. PLA composites reinforced by half‐and‐half SF‐g‐LA/untreated SF (half SF‐g‐LA) were prepared and studied as well, considering the disadvantages of SF‐g‐LA. The results showed that both the tensile properties and flexural properties of the SF‐g‐LA reinforced PLA composites were improved noticeably as the introduction of SF‐g‐LA, compared with pure PLA, untreated SF reinforced PLA composites and ASF reinforced PLA composites. The mechanical properties of the half SF‐g‐LA reinforced PLA composites were not worse, even better in some aspects, than the SF‐g‐LA reinforced PLA composites. Fourier transform infrared analysis and differential scanning calorimetry analysis exhibited that both the chemical composition and crystal structure of the SFs changed after LA grafting. In addition, the fracture surface morphology of the composites was studied by scanning electron microscopy. The morphological studies demonstrated that a better adhesion between LA‐grafted SF and PLA matrix was achieved. POLYM. COMPOS., 37:802–809, 2016. © 2014 Society of Plastics Engineers     

Assessing biodegradability and mechanical,thermal, and morphological properties of an acrylic acid‐modified poly(3‐hydroxybutyric acid)/wood flours biocomposite

A poly(3‐hydroxybutyric acid) and wood flours (PHB/wood flours) composite and an acrylic acid‐grafted PHB/wood flours composite were characterized and their properties were examined and compared. Mechanical properties of PHB became significantly worse when it was blended with wood flours, due to the poor compatibility between the two phases. Much better dispersion and homogeneity of wood flours in the polymer matrix was obtained when PHB‐g‐acrylic acid (AA) was used in place of PHB in the composite. Improved mechanical and thermal properties of the PHB‐g‐AA/wood flours composite, notably an increase in tensile strength at breakpoint, evidenced its superiority to the PHB/wood flours composite. Furthermore, PHB‐g‐AA/wood flours composites were more easily processed because of their lower melt viscosity. Under soil and enzymatic environments, weight loss data indicated that both composites were more biodegradable with higher wood flours content. A reduction in tensile strength at break after exposure to soil and enzymatic environments was also observed in both blends, especially at high wood flours content. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 102: 3565–3574, 2006     

Characterization and biocompatibility of chestnut shell fiber–based composites with polyester

The structural, mechanical, biocompatibility, and biodegradability properties of composite materials formed of poly(butylene succinate) (PBS) and natural fiber (chestnut shell fiber; CSF) were evaluated. Maleic anhydride‐grafted poly(butylene succinate) (PBS‐g‐MA) and treated (crosslinked) CSF (TCSF) were used to improve the mechanical properties of PBS/CSF composites. The results show that PBS‐g‐MA/TCSF composites have superior mechanical properties compared with both pure PBS and PBS/CSF composites, which is attributed to better compatibility between the polymer and TCSF. Normal human foreskin fibroblasts (FBs) were seeded onto these two series of composites to characterize the biocompatibility. FB proliferation, collagen production, and cytotoxicity assays on the PBS/CSF series of composites exhibited superior results compared with those on the PBS‐g‐MA/TCSF composites. PBS‐g‐MA/TCSF was found to be more water resistant than PBS/CSF, and the weight loss of both the composites buried in soil compost indicated that both were biodegradable, especially at high levels of CSF substitution. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 40730.     

Mechanical,thermal, and biodegradability properties of PLA/modified starch blends

Three different kinds of modified starch (MS) were prepared as fillers to assess the compatibility between them and poly(lactic acid) (PLA) resin. The blends were prepared by incorporating 15 wt% of the MS into PLA using a twin‐screw extruder. Through morphology analysis, it can be seen that the dispersion state of MS granules was greatly different. Investigations of thermal behavior indicated that the addition of MS decreased thermal properties which found expression in the decrease of melting temperature and vicat softening temperature (VST). But thermal stability of PLA/maleic anhydride grafted starch (MA‐g‐ST) was slightly higher than those of other blends. PLA/MA‐g‐ST blend exhibited the highest notched impact strength, elongation at break, and tensile strength, which means MA‐g‐ST was suitable as a filler improving the toughness of PLA. It was also proved that biodegradability rate of blends increased dramatically and reached up to 1.80, 1.89, 1.44 g day⁻¹ after 60 days, respectively. POLYM. COMPOS., 2011. © 2011 Society of Plastics Engineers     

Effect of fiber surface treatments on the properties of short sisal fiber/poly(lactic acid) biocomposites

Sisal fiber (SF)‐reinforced poly(lactic acid) (PLA) biocomposites were prepared from biodegradable PLA and surface‐untreated or ‐treated short SF by melt mixing and subsequent compression molding. It is found that the surface treatments facilitate good adhesion between SFs and PLA matrix, which is consistent with the higher mechanical properties of the treated‐SF/PLA biocomposites. Moreover, the surface treatments have similar effects on the biodegradability and water absorption of the biocomposites with the order as following: neat PLA < acetylated SF (A‐SF)/PLA biocomposite ≈ silane‐treated SF (S‐SF)/PLA biocomposite < permanganate‐treated SF (P‐SF)/PLA biocomposite < mercerized SF (M‐SF)/PLA biocomposite < untreated fiber (U‐SF)/PLA biocomposite. In terms of overall consideration of the properties, acetylation treatment seems to be the most desirable surface method owing to the maximum tensile strength and water resistance, medium impact strength, and minimum degradability of the A‐SF/PLA biocomposite. POLYM. COMPOS., 2012. © 2012 Society of Plastics Engineers     

Valorization of bio-calcium carbonate based Chamelea gallina shell waste fillers in shape memory polymer composites

In recent years, the focus has been on the use of calcium carbonate-based seashell wastes in the production of new thermoplastic and thermoset polymer materials, paving the way for their use as biofillers in polymeric composites. In this study, it is aimed to obtain a new polymeric composite material by doping Chamelea gallina shells, on polylactic acid (PLA)/polyethylene glycol (PEG) blend. Structural characterization of the obtained PLA/PEG blend/C. gallina composite films was performed with attenuated total reflection infrared spectroscopy (ATR-IR). When the thermal properties of composite materials were examined by thermogravimetric analysis (TGA), it was determined that the thermal stability of polymeric composites increased with the addition of C. gallina. SEM images showed that the polymer blend films, which appeared to have a porous structure, filled the pores with increasing C. gallina ratio. It was observed that the biodegradability of PLA/PEG blend composite films decreased with increasing C. gallina shells addition. However, C. gallina had a positive effect on the swelling and water absorption capacities of polymeric composites. The increase in tensile strength and elongation at break values of PLA/PEG blend/C. gallina composite films with increasing C. gallina means that the mechanical properties of the polymer are improved.     

Mechanical and thermal properties,morphology and relaxation characteristics of poly(lactic acid) and soy flour/wood flour blends

Poly(lactic acid) (PLA) is a biodegradable polymer derived from sugar‐based materials, and its applications are varied. PLA blends are commonly employed to overcome certain disadvantages such as poor impact strength, low heat distortion temperature, poor processability and relatively high cost. In this study, blending PLA with soy flour (SF), wood flour (WF) and sodium bisulfite‐modified SF was used to improve the adhesion to PLA. In all cases, 0.5 wt% methylenediphenyl diisocyanate (MDI) was used as a coupling agent. Mechanical and thermal properties, morphology and relaxation characteristics of the blends were investigated. The results showed that MDI was an effective coupling agent for the WF/PLA system in improving tensile strength and elongation. Differential scanning calorimetry results indicated that SF and modified SF act as nucleation agents and facilitate the crystallization behavior of PLA by increasing the percentage crystallinity. From mechanical relaxation of the temperature‐variant system, we determined how the mechanical relaxation time evolves during the course of heating and obtained the Kohlrausch–Williams–Watts parameter and activation energy (ΔE). PLA and its blends exhibited highly homogeneous relaxational dynamics in their transition from glass to liquid, and ΔE of PLA and its blends is mainly affected by their densities and compositions. Copyright © 2010 Society of Chemical Industry     

Chemomechanical,morphological, and rheological studies of chitosan‐graft‐lactic acid oligomer reinforced poly(lactic acid) bionanocomposite films

Various compositions of nontoxic biodegradable poly(lactic acid) (PLA)/chitosan‐graft‐lactic acid oligomer (CH‐g‐OLLA) bionanocomposite films were fabricated with a solution casting technique by the dispersal of CH‐g‐OLLA copolymer at different amounts (1, 3, and 5 wt %) into the PLA matrix. The filler (CH‐g‐OLLA) was synthesized by an in situ condensation polymerization reaction in a microwave, and the grafting of lactic acid oligomer chains at the C2 position of the chitosan backbone was confirmed by the presence of new peaks at 179.08 and 174.41 ppm in ¹³C‐NMR analysis. The transparency results show the synergic effect of CH‐g‐OLLA in the form of reduced transparency and excellent blocking capability of UV light. Dynamic mechanical analysis confirmed a reduction in the glass‐transition temperature (up to ～13 °C) with increasing filler concentration; this signified the improvement in the elongation of bionanocomposite films. The rheological studies showed the viscous behavior of the PLA and PLA–CH‐g‐OLLA bionanocomposite films as the storage modulus values were found to be lower than the loss modulus values over the entire range of angular frequency at 180 °C. Furthermore, a Cole–Cole plot and Han plot described the uniform dispersion of the filler in the PLA matrix, its agglomeration at higher loading, and the structural change between the PLA and PLA–CH‐g‐OLLA bionanocomposite films. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 45546.     

Effect of silk fiber to the mechanical and thermal properties of its biodegradable composites

In recent years, natural fiber‐reinforced biodegradable thermoplastics are being recognized as an emerging new environmentally friendly material for industrial, commercial, and biomedical applications. Among different types of natural fibers, silk fiber is a common type of animal‐based fiber, has been used for biomedical engineering and surgical operation applications for many years because of its biocompatible and bioresorbable properties. On the basis of our previous study, a novel biodegradable biocomposite for biomedical applications was developed by mixing chopped silk fiber and polylactic acid (PLA) through the injection molding process. This article is aimed at studying the dynamic mechanical and thermal properties of the composite in relation to its biodegradation effect. At the beginning, it was found that the initial storage modulus of a silk fiber/PLA composite increased while its glass transition temperature decreased as compared with a pristine PLA sample. Besides, the coefficient of linear thermal expansions (CLTE) of the composite was reduced by 28%. This phenomenon was attributed to the fiber–matrix interaction that restricted the mobility of polymer chains adhered to the fiber surface, and consequently reduced the T_g and CLTE. It was found that the degraded composite exhibited lower initial storage modulus, loss modulus and tan delta (tan δ) but the T_g was higher than the silk fiber/PLA composite. This result was mainly due to the increase of crystallinity of the composite during its degradation process. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

Toughening of polylactic acid using styrene ethylene butylene styrene: Mechanical,thermal, and morphological studies

Polylactic acid, PLA, derived from renewable resources has gained great attention nowadays owing to their sustainability, biodegradability, superior property, and transparency. However, intrinsic brittleness and low toughness severely limits its variety of applications. Blending of PLA with other polymers is more economical and more flexible technique for the property improvement of PLA. In this study, Styrene Ethylene Butylene Styrene (SEBS) and Maleic Anhydride grafted SEBS (MA‐g‐SEBS) are used as toughening agents to study their effect for its toughness, high strength and heat resistance on PLA. PLA/SEBS and PLA/Maleic Anhydride grafted SEBS blends were prepared under four different compositions by melt mixing technique using a corotating twin–screw extruder after optimizing the mixing conditions. The mechanical properties of the blends such as tensile, flexural, and impact strengths were investigated using specimens prepared by injection molding process. The percentage elongation and impact strength of PLA/MA‐g‐SEBS blends were found to be increased significantly by 540 and 135%, respectively in comparison with virgin PLA and PLA/SEBS blends. However, tensile strength and modulus of PLA/SEBS and PLA/MA‐g‐SEBS blends decreased compared with pristine PLA. SEM behaviour supported the higher impact property of PLA with the incorporation of modified SEBS via multiple crazing and cavitation mechanisms. DSC study also supported greater compatibility between maleated SEBS and PLA. POLYM. ENG. SCI., 56:669–675, 2016. © 2016 Society of Plastics Engineers     

Micromorphology,mechanical, crystallization and permeability properties analysis of HA/PBAT/PLA (HA,hydroxyapatite; PBAT,poly(butylene adipate‐co‐butylene terephthalate); PLA,polylactide) degradability packaging films

In this study, the self‐made nano‐hydroxyapatite (HA) and poly(butylene adipate‐co‐butylene terephthalate) copolyesters (PBAT) were used as fillers, and composite films of HA/PLA (PLA, polylactide) and HA/PBAT/PLA systems were prepared. The micromorphology, mechanical properties, thermal properties, crystallinity, water vapor permeability and oxygen permeability of the composite films were studied. The results show that the self‐made HA has a porous rod‐like structure with a size of 30–50 nm. PBAT was dispersed uniformly in the HA/PLA matrix in the form of spherical particles and formed many pores and holes. The tensile strength, elongation at break and modulus of elasticity of HA/PLA composite films were increased by adding 10 wt% PBAT. The addition of HA and PBAT played a synergistic function in improving the crystallinity of the composite films. The water vapor and oxygen permeabilities of HA/PLA and HA/10%PBAT/PLA composite films can be regulated by adjusting the amount of HA. The results of this study indicate that composite films with higher water vapor and oxygen permeabilities exhibit great potential for applications in green packaging and fresh‐keeping packaging. © 2019 Society of Chemical Industry     

Effect of Al2O3 fibers on the thermal conductivity and mechanical properties of high density polyethylene with the absence and presence of compatibilizer

Alumina (Al₂O₃) fiber/high density polyethylene (HDPE) composites were prepared by molding injection with or without compatibilizer, in which, maleic anhydride‐grafted polyethylene (PE‐g‐MA) and acrylic acid‐grafted polyethylene (PE‐g‐AA) were used as the compatibilizers. The thermal conductivities of the composites were anisotropic and the conductivities in the injection direction of the samples were higher than those in perpendicular direction of the injection. The anisotropic thermal conductivity for Al₂O₃/PE‐g‐AA/HDPE was the most obvious and this composite also gave the best mechanical performance. The SEM and DMA test revealed that PE‐g‐AA was more effective than PE‐g‐MA in improving the matrix–filler interaction. The high interfacial interaction was more favorable for the viscous flow‐induced fiber orientation, which resulted in the largest anisotropic degree of thermal conductivity of the Al₂O₃/PE‐g‐AA/HDPE among the studied composite. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Surface modification of spruce wood flour and effects on the dynamic fragility of PLA/wood composites

Poly (lactic acid) (PLA), a biodegradable aliphatic semicrystalline polyester was filled with 40 wt% spruce wood flour (WF), to produce composite materials. Hydrothermal treatment, as well as maleic anhydride, vinyltrimethoxysilane, and stearic acid surface treatments were applied. The influence of surface modifications for WF was tested in terms of thermal, mechanical, and viscoelastic properties. The recorded results show that in both, the untreated and treated PLA/WF composites, the rigid amorphous phase content has been enhanced. The presence of WF causes a stiffness increase of the PLA/WF composites, while damping factor was decreased. The effect of wood surface modifications on interfacial compatibility with PLA was estimated by dynamic fragility parameter m calculated according the Williams‐Landel‐Ferry equation. The incorporation of untreated WF increased dynamic fragility of PLA/WF composites markedly, whereas used silane, maleic anhydride and hydrothermal treatments lead to lower values of parameter m. POLYM. ENG. SCI., 2011. © 2010 Society of Plastics Engineers     

Mechanical,thermal, and morphological properties of injection molded poly(lactic acid)/SEBS‐g‐MAH/organo‐montmorillonite nanocomposites

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     

Tri‐(butanediol‐monobutyrate) citrate plasticizing poly(lactic acid): Synthesis,crystallization, thermal,and mechanical properties

Tri‐(butanediol‐monobutyrate) citrate (TBBC) as a new plasticizer for poly(lactic acid) (PLA) was synthesized via a two‐step esterification. The chemical structure of TBBC was characterized by ¹H‐nuclear magnetic resonance. The studies on solubility parameters, transparence, and storage stability indicated the good miscibility between PLA and TBBC. The glass transition, crystallization, thermal, and mechanical properties of PLA plasticized by TBBC were evaluated. With an increase in TBBC content, the glass transition temperature (T_g), melting point (T_m), and the cold crystallization temperature (T_cc) of plasticized PLA gradually shifted to a lower temperature. The elongation at break and flexibility were greatly improved by the addition of TBBC. After 30 days of storage, PLA plasticized with up to 20 wt% of TBBC exhibited good storage stability and remained the original transparence and mechanical properties. The flexibility of PLA/TBBC films can be tuned by changing TBBC content. The corresponding crystalline morphology and structure were investigated by Polarizing optical microscope and X‐ray diffraction as well. This study revealed that TBBC was miscible with PLA and may therefore be a promising plasticizer for PLA‐based packaging materials. POLYM. ENG. SCI., 55:205–213, 2015. © 2014 Society of Plastics Engineers     

Porous biodegradable polyester blends of poly(L‐lactic acid) and poly(ε‐caprolactone): physical properties,morphology, and biodegradation

Poly(L ‐lactic acid) (PLLA), poly(ε‐caprolactone) (PCL), and their films without or blended with 50 wt% poly(ethylene glycol) (PEG) were prepared by solution casting. Porous films were obtained by water‐extraction of PEG from solution‐cast phase‐separated PLLA‐blend‐PCL‐blend‐PEG films. The effects of PLLA/PCL ratio on the morphology of the porous films and the effects of PLLA/PCL ratio and pores on the physical properties and biodegradability of the films were investigated. The pore size of the blend films decreased with increasing PLLA/PCL ratio. Polymer blending and pore formation gave biodegradable PLLA‐blend‐PCL materials with a wide variety of tensile properties with Young's modulus in the range of 0.07–1.4 GPa and elongation at break in the range 3–380%. Pore formation markedly increased the PLLA crystallinity of porous films, except for low PLLA/PCL ratio. Polymer blending as well as pore formation enhanced the enzymatic degradation of biodegradable polyester blends. Copyright © 2006 Society of Chemical Industry     

Polyester and multiwalled carbon nanotube composites: characterization,electrical conductivity and antibacterial activity

Poly(butylene terephthalate) (PBT) composites containing multiwalled carbon nanotubes (MWCNTs) were prepared using a melt‐blending process and used to examine the effects on the composite structure and properties of replacing PBT with acrylic acid‐grafted PBT (PBT‐g‐AA). PBT‐g‐AA and multihydroxyl‐functionalized MWCNTs (MWCNTs‐OH) were used to improve the compatibility and dispersibility of the MWCNTs within the PBT matrix. The composites were characterized morphologically using transmission electron microscopy, and chemically using Fourier transform infrared, solid‐state ¹³C NMR and UV‐visible absorption spectroscopy. The antibacterial and electrical conductivity properties of the composites were also evaluated. MWCNTs or MWCNTs‐OH enhanced the antibacterial activity and electrical conductivity of the PBT/MWCNT or PBT‐g‐AA/MWCNTs‐OH composites. The functionalized PBT‐g‐AA/MWCNTs‐OH composites showed markedly enhanced antibacterial properties and electrical conductivity due to the formation of ester bonds from the condensation of the carboxylic acid groups of PBT‐g‐AA with the hydroxyl groups of MWCNTs‐OH. The optimal proportion of MWCNTs‐OH in the composites was 1 wt%; in excess of this amount, the compatibility between the organic and inorganic phases was compromised. Copyright © 2011 Society of Chemical Industry