Biodegradation of montmorillonite filled oxo‐biodegradable polyethylene

Oxo‐biodegradation of polyethylene has been well studied with different pro‐oxidants and it has been shown that pro‐oxidants have limited role in the oxidation of polyethylene and do not have any role in microbial growth. However, in few recent studies, montmorillonite clay has been reported to promote the growth of microbes by keeping the pH of the environment at levels conducive to growth. In an attempt to improve the overall oxo‐biodegradation of polyethylene, montmorillonite nanoclay has been used in this study along with a pro‐oxidant. Film samples of oxo‐biodegradable polyethylene (OPE) and oxo‐biodegradable polyethylene nanocomposite (OPENac) were subjected to abiotic oxidation followed by microbial degradation using microorganism Pseudomonas aeruginosa. The progress of degradation was followed by monitoring the chemical changes of the samples using high‐temperature gel permeation chromatography (GPC) and infrared spectroscopy (FTIR). The growth of bacteria on the surface of the polymer was monitored using environmental scanning electron microscopy. GPC data and FTIR results have shown that the abiotic oxidation of polyethylene is influenced significantly by the pro‐oxidant but not by nanoclay. But, the changes in molecular weight distribution and FTIR spectra for the biodegraded samples indicate that the growth rate of P. aeruginosa on OPENac is significantly greater than that on OPE. It indicates that nanoclay, by providing a favourable environment, helps in the growth of the microorganism and its utilisation of the polymer surface and the bulk of the polymer volume. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Effect of pro‐oxidants on biodegradation of polyethylene (LDPE) by indigenous fungal isolate,Aspergillus oryzae

Proxidant additives represent a promising solution to the problem of the environment contamination with polyethylene film litter. Pro‐oxidants accelerate photo‐ and thermo‐oxidation and consequent polymer chain cleavage rendering the product apparently more susceptible to biodegradation. In the present study, fungal strain, Aspergillus oryzae isolated from HDPE film (buried in soil for 3 months) utilized abiotically treated polyethylene (LDPE) as a sole carbon source and degraded it. Treatment with pro‐oxidant, manganese stearate followed by UV irradiation and incubation with A. oryzae resulted in maximum decrease in percentage of elongation and tensile strength by 62 and 51%, respectively, compared with other pro‐oxidant treated LDPE films which showed 45% (titanium stearate), 40% (iron stearate), and 39% (cobalt stearate) decrease in tensile strength. Fourier transform infrared (FTIR) analysis of proxidant treated LDPE films revealed generation of more number of carbonyl and carboxylic groups (1630–1840 cm⁻¹ and 1220–1340 cm⁻¹) compared with UV treated film. When these films were incubated with A. oryzae for 3 months complete degradation of carbonyl and carboxylic groups was achieved. Scanning electron microscopy of untreated and treated LDPE films also revealed that polymer has undergone degradation after abiotic and biotic treatments. This concludes proxidant treatment before UV irradiation accelerated photo‐oxidation of LDPE, caused functional groups to be generated in the polyethylene film and this resulted in biodegradation due to the consumption of carbonyl and carboxylic groups by A. oryzae which was evident by reduction in carbonyl peaks. Among the pro‐oxidants, manganese stearate treatment caused maximum degradation of polyethylene. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Stress relaxation in low‐shrink‐force polyolefin films

The morphology and stress relaxation of coextruded five‐layer LLDPE (linear low‐density polyethylene)/EVA (ethylene‐vinyl‐acetate) copolymer films were studied. Increasing VA (vinyl acetate) content in EVA causes a decrease of shrink tension in the films, which can be explained by a decrease in amount of crystallinity. The relaxation time spectrum of the coextruded crosslinked LLDPE/EVA films is similar to the relaxation time spectrum of crosslinked LLDPE film at room temperature. However, at elevated temperatures, an additional peak appears on the spectrum of coextruded film. The cause of this peak is temperature‐ and stress‐induced recrystallization of EVA during the relaxation test. This recrystallization was confirmed with DSC and wide angle X‐ray analysis. Polym. Eng. Sci. 44:1716–1720, 2004. © 2004 Society of Plastics Engineers.     

Biodegradation of oxo‐biodegradable polyethylene

Biodegradation of polyethylene and oxo‐biodegradable polyethylene films was studied in this work. Abiotic oxidation, which is the first stage of oxo‐biodegradation, was carried out for a period corresponding to 4 years of thermo‐oxidation at composting temperatures. The oxidation was followed by biodegradation, which was achieved by inoculating the microorganism Pseudomonas aeruginosa on polyethylene film in mineral medium and monitoring its degradation. The changes in the molecular weight of polyethylene and the concentration of oxidation products were monitored by size exclusion chromatography and Fourier transform infrared (FTIR) spectroscopy, respectively. It has been found that the initial abiotic oxidation helps to reduce the molecular weight of oxo‐biodegradable polyethylene and form easily biodegradable product fractions. In the microbial degradation stage, P. aeruginosa is found to form biofilm on polymer film indicating its growth. Molecular weight distribution data for biodegraded oxo‐biodegradable polyethylene have shown that P. aeruginosa is able to utilize the low‐molecular weight fractions produced during oxidation. However, it is not able to perturb the whole of the polymer volume as indicated by the narrowing of the polymer molecular weight distribution curve toward higher molecular fractions. The decrease in the carbonyl index, which indicates the concentration of carbonyl compounds, with time also indicates the progress of biodegradation. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Photobiodegradation of low‐density polyethylene/banana starch films

The effects of the starch content, photosensitizer content, and compatibilizer on the photobiodegradability of low‐density polyethylene (LDPE) and banana starch polymer blend films were investigated. The compatibilizer and photosensitizer used in the films were PE‐graft‐maleic anhydride (PE‐g‐MA) and benzophenone, respectively. Dried banana starch at 0–20% (w/w) of LDPE, benzophenone at 0–1% (w/w) of LDPE, and PE‐g‐MA at 10% (w/w) of banana starch were added to LDPE. The photodegradation of the blend films was performed with outdoor exposure. The progress of the photodegradation was followed by determining the carbonyl index derived from Fourier transform IR measurements and the changes in tensile properties. Biodegradation of the blend films was investigated by a soil burial test. The biodegradation process was followed by measuring the changes in the physical appearance, weight loss, and tensile properties of the films. The results showed that both photo‐ and biodegradation rates increased with increasing amounts of banana starch, whereas the tensile properties of the films decreased. The blends with higher amounts of benzophenone showed higher rates of photodegradation, although their biodegradation rates were reduced with an increase in benzophenone content. The addition of PE‐g‐MA into polymer blends led to an increase in the tensile properties whereas the photobiodegradation was slightly decreased compared to the films without PE‐g‐MA. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 100: 2725–2736, 2006     

Effect of damp‐heat aging on the structures and properties of ethylene‐vinyl acetate copolymers with different vinyl acetate contents

We reported herein the damp‐heat aging of ethylene‐vinyl acetate copolymers (EVA) with different vinyl acetate (VAc) contents simultaneously for weeks. The aging was carried out under temperature of 40°C and relative humidity of 93% in air atmosphere. The changes of copolymers' structures and properties were investigated by means of FTIR, wide angle X‐ray diffraction (WAXD) and differential scanning calorimetry (DSC) and mechanical tests. CI values derived from ATR‐FTIR spectra have a decrease when aging time is 1 week and then increase during damp‐heat aging process which suggests the first loss then incorporation of O?C group. WAXD infer that the narrowing trend of FWHM and increase of crystal sizes may attribute to the melting and re‐crystallization of secondary crystallization, which is also confirmed by DSC results. Mechanical tests including Shore A and Shore D hardness, modulus at 100%, tensile strength and elongation at break, are all depending on the primary crystallization and influenced little by damp‐heat aging. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Preparation and properties of dynamically cured PP/MAH‐g‐EVA/epoxy blends

A method concerning with the simultaneous reinforcing and toughening of polypropylene (PP) was reported. Dynamical cure of the epoxy resin with 2‐ethylene‐4‐methane‐imidazole (EMI‐2,4) was successfully applied in the PP/maleic anhydride‐grafted ethylene‐vinyl acetate copolymer (MAH‐g‐EVA), and the obtained blends named as dynamically cured PP/MAH‐g‐EVA/epoxy blends. The stiffness and toughness of the blends are in a good balance, and the smaller size of epoxy particle in the PP/MAH‐g‐EVA/epoxy blends shows that MAH‐g‐EVA was also used as a compatibilizer. The structure of the dynamically cured PP/MAH‐g‐EVA/epoxy blends is the embedding of the epoxy particles by the MAH‐g‐EVA. The cured epoxy particles as organic filler increases the stiffness of the PP/MAH‐g‐EVA blends, and the improvement in the toughness is attributed to the embedded structure. The tensile strength and flexural modulus of the blends increase with increasing the epoxy resin content, and the impact strength reaches a maximum of 258 J/m at the epoxy resin content of 10 wt %. DSC analysis shows that the epoxy particles in the dynamically cured PP/MAH‐g‐EVA/epoxy blends could have contained embedded MAH‐g‐EVA, decreasing the nucleating effect of the epoxy resin. Thermogravimetric results show the addition of epoxy resin could improve the thermal stability of PP, the dynamically cured PP/MAH‐g‐EVA/epoxy stability compared with the pure PP. Wide‐angle x‐ray diffraction analysis shows that the dynamical cure and compatibilization do not disturb the crystalline structure of PP in the blends. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Poly(ethylene‐co‐vinyl acetate) blends with phenoxy

EVA was blended with phenoxy over the whole range of composition using a twin‐screw Brabender. Two‐phase separation caused by EVA crystallization was observed in the EVA‐rich blends and the dispersed domain of EVA was not clearly shown in the phenoxy‐rich blends. Differential scanning calorimetry (DSC) showed that the glass transition temperature (T_g) of EVA was increased by 5–10°C in the EVA‐rich blends but the T_g of phenoxy was superposed over the melting behavior of EVA. X‐ray diffraction measurement indicated that EVA crystallization was restricted in the phenoxy‐rich blends and the EVA crystal structure was influenced by incorporation of phenoxy into the EVA‐rich blends. © 1999 John Wiley & Sons, Inc. J Appl Polym Sci 73: 227–236, 1999     

Free‐radical grafting of trans‐ethylene‐1,2‐dicarboxylic acid onto molten ethylene‐vinyl acetate copolymer

Distinctive features of free‐radical grafting of trans‐ethylene‐1,2‐dicarboxylic acid (TEDA) onto macromolecules of molten ethylene‐vinyl acetate copolymer (EVA) in the course of reactive extrusion have been investigated along with structure, mechanical characteristics, and high‐elastic properties of molten functionalized products (EVA‐g‐TEDA). It is shown that EVA‐g‐TEDA yield depends on both the peroxide initiator concentration and content of vinyl acetate units in the copolymer molecular structure. At functionalization, acid grafting is accompanied by secondary reactions of macromolecular degradation and crosslinking. With a low‐peroxide initiator concentration (0.1 wt %), degradation prevails; with a higher (0.3 wt %) concentration, crosslinking of macromolecules prevails. It is reported that monomers being grafted attach mostly over secondary carbon atoms in the polymer chain. EVA‐g‐TEDA appears to have a less perfect crystal structure with a lower‐melting temperature and crystallinity as against the starting polymer. The functionalized products display enhanced rigidity and lower deformability in comparison with the initial copolymer. Variations in the swelling ratio and melt strength of EVA‐g‐TEDA depend on the course of competing secondary processes of macromolecular degradation and crosslinking. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

Thermal and physicomechanical properties of ethylene-vinyl acetate copolymer and layered double hydroxide composites

A series of ethylene-vinyl acetate (EVA) copolymer films have been prepared with different compositions viz. 2, 4, 6, and 8 wt % layered double hydroxide (LDH) nanoparticles by solution intercalation method. These solution-casted EVA/LDH nanocomposite films were dried and characterized by differential scanning calorimetry (DSC) and Fourier transform infrared (FTIR) spectroscopy. EVA/LDH films were further tested for tensile strength, density, moisture content, solubility resistance, flammability, and electrical properties. The DSC and FTIR analysis indicate strong interactions between the LDH layers and vinyl acetate groups in EVA. Further, EVA nanocomposite films show enhanced tensile strength, limiting oxygen index (LOI), and flammability rating for the addition of LDH without sacrificing the electrical properties. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci 2008     

Study on the nonisothermal crystallization process of mLLDPE/EVA blends using FTIR micro‐spectroscopy

The nonisothermal crystallization process has been investigated by Fourier transform infrared (FTIR) micro‐spectroscopy for the 40/60 wt % blends of metallocene linear low density polyethylene (m‐LLDPE) and ethylene/vinyl acetate copolymer (EVA) at the molecular level. In the cooling process, thermal spectra of mLLDPE/EVA blends were collected between 150°C and 67°C at 1°C interval. According to the van't Hoff equation at constant pressure, the changes of absorbance ratio corresponding to high and low vibrational states were calculated; hereby, apparent enthalpy differences of vibration energy states transformation (?H_v) of characteristic groups could be obtained. Combining with DSC analysis, two exothermal peaks were examined in the crystallization process, corresponding to mLLDPE‐rich and EVA‐rich domains, respectively; while in comparison of the ?H_v values of various characteristic groups corresponding to the two exothermal peaks, the bending vibrational mode of methylene groups has been found to make a prominent contribution to the movement and regular arrangement of mLLDPE and EVA chain segments towards each rich domain in the crystallizing process. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 96: 261–267, 2005     

Influence of processing condition and HA content on the crystallization behavior of HA‐filled EVA biocomposite

Hydroxyapatite/ethylene‐vinyl acetate (HA/EVA) composites with a HA content of 30 and 50 wt% were prepared by injection molding. The crystallization behaviors of EVA under different injection pressure, annealing temperature, and HA content were investigated. Fourier transform infrared spectroscopy (FTIR), X‐ray diffraction (XRD), differential scanning calorimetry (DSC), and scanning electron microscope were used to evaluate the composites. The result of FTIR analysis infers the occurrence of hydrogen bonding between HA and EVA. XRD and DSC analyses show that the increasing injection pressure can accelerate the crystallization rate of EVA but it tends to decrease the crystallization degree slightly, which may be caused by the increase of EVA segmental activity and the loss of EVA crystallization order with the increase of pressure. The EVA crystallization degree can be improved by the annealing process. It is found that HA can induce more nucleation sites of EVA, but the crystallization degree of EVA decreases with the increase of HA content. The large content of HA acts to reduce the mobility of EVA crystallizable chain segments and inhibits the crystal growth of EVA. POLYM. ENG. SCI., 2011. © 2010 Society of Plastics Engineers     

Biodegradation behavior of acid‐containing cellulose acetate film in soil

The biodegradation behavior of various cellulose acetate (CA; degree of substitution = 2.5) films that contain acids was examined by a laboratory soil burial test to clarify the effects of additives on the biodegradability of CA. The biodegradation rate of the CA films containing polyphosphoric acid, phosphoric acid, and p‐toluenesulfonic acid increased compared to that of the nonadditive CA film. CA films containing mandelic acid and maleic acid showed a small tendency to increase. Conversely, CA films containing adipic acid did not affect the biodegradability of CA. A similar experiment was carried out with a sterilization system. The acid‐containing CA film, which showed an accelerated biodegradation rate, was chemically deacetylated by contact with water in the environment and was consequently converted to a lower degree of acetyl group substitution matter that had higher biodegradability. An IR analysis suggested that this deacetylating ability of acids is correlated with the intensity of their interaction with the acetyl group of CA. In the biodegradation process, the contact efficiency of acids to CA was considerably lowered by the elution of internal acids with time. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 98: 466–473, 2005     

Triple‐shape‐memory polymer films created by forced‐assembly multilayer coextrusion

Triple‐shape‐memory polymers are capable of memorizing two temporary shapes and sequentially recovering from the first temporary shape to the second temporary shape and eventually to the permanent shape upon exposure to a stimulus. In this study, unique three‐component, multilayered films with an ATBTA configuration [where A is polyurethane (PU), B is ethylene vinyl acetate (EVA), and T is poly(vinyl acetate) (PVAc)] were produced as a triple‐shape‐memory material via a forced‐assembly multilayer film coextrusion process from PU, EVA, and PVAc. The two well‐separated thermal transitions of the PU–EVA–PVAc film, the melting temperature of EVA and the glass‐transition temperature of PVAc, allow for the fixing of the two temporary shapes. The cyclic thermomechanical testing results confirm that the 257‐layered PU–EVA–PVAc films possessed outstanding triple‐shape‐memory performance in terms of the shape fixity and shape‐recovery ratios. This approach allowed greater design flexibility and simultaneous adjustment of the mechanical and shape‐memory properties. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 44405.     

Development of new thermoplastic elastomers from blends of polyethylene and ethylene–vinyl acetate copolymer by electron‐beam technology

Electron beam‐initiated crosslinking of films prepared from a blend of low‐density polyethylene (LDPE) and ethylene–vinyl acetate (EVA) containing 45% vinyl acetate, with ditrimethylol propane tetraacrylate (DTMPTA), was carried out over a range of radiation doses (20–500 kGy), concentration of DTMPTA (1–5 parts by weight), and blend compositions. The gel fraction of the films increases with increase in the irradiation dose, DTMPTA level, and EVA content of the blends. The mechanical and dynamic mechanical properties of the films are also changed with the above variables. Reprocessibility studies revealed that the blends irradiated at 50 kGy and below are thermoplastic elastomers with a low permanent set. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 79: 1877–1889, 2001     

Effect of hot air aging on the properties of ethylene‐vinyl acetate copolymer and ethylene‐acrylic acid copolymer blends

The aim of this investigation is to evaluate the effect of hot air aging on properties of ethylene‐vinyl acetate copolymer (EVA, 14 wt % vinyl acetate units), ethylene‐acrylic acid copolymer (EAA, 8 wt % acrylic acid units), and their blends. Attenuated total reflection‐Fourier transform infrared spectroscopy, differential scanning calorimeter (DSC), wide angle X‐ray diffraction, and mechanical tests are employed to investigate the changes of copolymer blends' structures and properties. Increase of carbonyl index derived from ATR measurements with aging time suggests the incorporation of oxygen into the polymeric chain. By DSC measurements, the enthalpy at low temperature endothermic peak (T_m2) of EAA becomes less and disappears after 8 weeks aging, but enthalpy at T_m2 of EVA is not influenced by the hot air aging and remains stable despite of the aging time. For various proportions of EAA and EVA blends, enthalpy at T_m2 decreases as the EAA proportion increases when aging time is 8 weeks; after several weeks of hot air aging, the various blends appear a same new peak just over the aging temperature 70°C which is due to the completion of crystals which are not of thermodynamic equilibrium state. Mechanical tests show that increase of crystallinity and hot air aging deterioration both have influence on the hardness, tensile strength, and elongation at break. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Poly(vinyl alcohol)‐g‐lactic acid copolymers and films with silver nanoparticles

Poly(vinyl alcohol) (PVA), a well‐known synthetic biodegradable, biocompatible, and hydrophilic polymer is susceptible to several structural modifications, due to the presence of hydroxyl groups in its backbone. PVA was grafted with L (+)‐lactic acid (LA) in molar ratios VA/LA (1/1, 1.5/1, and 2.2/1), manganese acetate as catalyst, by solution polycondensation procedure, resulting the poly(vinyl alcohol)‐g‐lactic acid copolymers. Aqueous solutions of copolymers with glycerol as plasticizer, silver nanoparticles (Ag^o), and sodium tetraborate as crosslinking agent were used for films casting. The copolymers were characterized by FTIR and ¹H RMN spectroscopy, gel permeation chromatography, thermal analyses (DTG and DSC), silver particles size, while films were characterized by mechanical properties and mechanodynamic analyses. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Synthesis of novel phosphorous‐containing biphenol, 2‐(5, 5‐dimethyl‐4‐phenyl‐2‐oxy‐1,3,2‐dioxaphosphorin‐6‐yl)‐1,4‐benzenediol and its application as flame‐retardant in epoxy resin

A novel phosphorous‐containing biphenol, 2‐(5,5‐dimethyl‐4‐phenyl‐2‐oxy‐1,3,2‐dioxaphosphorin‐6‐yl)‐ 1,4‐benzenediol (DPODB), was prepared by the addition reaction between 5,5‐dimethyl‐4‐phenyl‐2‐oxy‐1,3,2‐dioxaphosphorinane phosphonate (DPODP) and p‐benzoquinone (BQ). The compound (DPODB) was used as a reactive flame retardant in o‐cresol formaldehyde novolac epoxy resin (CNE) for electronic application. The structure of DPODB was confirmed by FTIR and NMR spectra. Thermal properties of cured epoxy resin were studied using differential scanning calorimetry (DSC) and thermal gravimetric analysis (TGA). The flame retardancy of cured epoxy resins was tested by UL‐94 vertical test and achieved UL‐94 vertical tests of V‐0 grade (nonflammable). © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 102: 3842–3847, 2006     

Oxygen permeability and the mechanical and thermal properties of (low‐density polyethylene)/poly (ethylene‐co‐vinyl acetate)/organoclay blown film nanocomposites

Various (low‐density polyethylene)/poly(ethylene‐co‐vinyl acetate) (LDPE/EVA) nanocomposites containing organoclay were prepared by one‐ and two‐step procedures through melt blending. The resultant nanocomposites were then processed via the film blowing method. From the morphological point of view, X‐ray diffraction and optical microscopy studies revealed that although a prevalent intercalated morphology was evident in the absence of EVA, a remarkable increase of organoclay interlayer spacing occurred in the EVA‐containing systems. The advantages of the addition of EVA to the LDPE/organoclay nanocomposites were confirmed in terms of oxygen barrier properties. In other words, the oxygen transmission rates of the LDPE/EVA/organoclay systems were significantly lower than that of the LDPE/organoclay sample. The LDPE/EVA/organoclay films had better mechanical properties than their counterparts lacking the EVA, a result which could be attributed to the improvement of the organoclay reinforcement efficiency in the presence of EVA. Differential scanning calorimetry and thermogravimetric analysis experiments were performed to follow the effects of the EVA and/or organoclay on the thermal properties of LDPE. Finally, the films produced from the two‐step‐procedure compound showed enhanced oxygen barrier properties and mechanical behavior as compared to the properties of the films produced via the one‐step procedure. J. VINYL ADDIT. TECHNOL., 19:132–139, 2013. © 2013 Society of Plastics Engineers     

Degradation in soil behavior of artificially aged polyethylene films with pro‐oxidants

Bio‐based, biodegradable in soil, as well as degradable polyethylene mulching films with pro‐oxidants, have been introduced in the market in an effort to deal with the serious problem of managing plastic waste streams generated from conventional mulching films. In a previous experimental investigation, a series of naturally degraded under water melon cultivation conditions linear low density polyethylene (LLDPE) mulching films with pro‐oxidants, buried in the field for 8.5 years, were recovered intact even though undergoing a continuous slow abiotic degradation in soil. The aim of the present article was to simulate the behavior of the LLDPE mulching films with pro‐oxidants under a much longer time‐scale (e.g. some decades). Toward this purpose, samples of LLDPE with pro‐oxidants film were artificially degraded to simulate severe degradation/fragmentation of these films while been buried in the soil for many years, following the end of the cultivation season. Further degradation of these severely degraded samples was investigated by burying them in the soil over a period of seven years. During this burial period, all degradation parameters and their evolution with time were measured. The artificially degraded LLDPE film samples with pro‐oxidants, in contrast to the naturally degraded film that remained intact for 8.5 years, were gradually transformed into tiny micro‐fragments in the soil. These fragments, through a continuing abiotic degradation process under natural soil conditions are eventually transformed into invisible micro‐fragments. The fate of these micro‐fragments and their long‐term impact to the environment and human health is unpredictable. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42289.