Thermally crosslinked anionic hydrogels composed of poly(vinyl alcohol) and poly(γ‐glutamic acid): Preparation,characterization, and drug permeation behavior

pH‐sensitive anionic hydrogels composed of poly(vinyl alcohol) (PVA) and poly(γ‐glutamic acid) (γ‐PGA) were prepared by the freeze drying method and thermally crosslinked to suppress hydrogel deformation in water. The physical properties, swelling, and drug‐diffusion behaviors were characterized for the hydrogels. In the equilibrium swelling study, PVA/γ‐PGA hydrogels shrunk in pH regions below the pK_a (2.27) of γ‐PGA, whereas they swelled above the pK_a. In the drug‐diffusion study, the drug permeation rates of the PVA/γ‐PGA hydrogels were directly proportional to their swelling behaviors. The cytocompatibility test showed no cytotoxicity of the PVA/γ‐PGA hydrogels for the 3T3 fibroblast cell lines. The results of these studies suggest that hydrogels prepared from PVA and γ‐PGA could be used as orally administrable drug‐delivery systems. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

A poly(γ‐glutamic acid)‐based hydrogel loaded with superoxide dismutase for wound healing

The purpose of this study was to develop a poly(γ‐glutamic acid) (γ‐PGA)‐based hydrogel loaded with superoxide dismutase (SOD) to accelerate wound healing. First, γ‐PGA was modified with taurine (γ‐PGAS), and then the SOD‐loaded γ‐PGAS/γ‐PGA hydrogel (SOD‐PGAS/PGA‐H) was prepared by cross‐linking of ethylene glycol diglycidyl ether. The swelling behavior and water vapor transmission rate revealed that PGAS/PGA‐H could create a moist environment for wound surface. In vitro kinetics of SOD release showed that SOD released from PGAS/PGA‐H maintained high activity and SOD‐PGAS/PGA‐H effectively scavenged the superoxide anion. The results of our fibroblast proliferation experiments showed that PGAS/PGA‐H had good cytocompatibility. The effects of SOD‐PGAS/PGA‐H on wound healing were examined in a Type I diabetic rat model with full‐thickness wounds. Twenty‐one days after grafted to wounds, SOD‐PGAS/PGA‐H exhibited a higher rate of wound healing than control group and showed increased collagen deposition and epithelialization. SOD‐PGAS/PGA‐H seems to promote better wound healing and thus might be a promising candidate for wound healing management. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42033.     

Synthesis and swelling properties of pH‐ and temperature‐sensitive interpenetrating polymer networks composed of polyacrylamide and poly(γ‐glutamic acid)

Novel hydrogels of interpenetrating polymer networks (IPNs) composed of polyacrylamide and poly(γ‐glutamic acid) were synthesized. In these systems, both polymers were crosslinked independently; this reduced the potential loss of a polymer during the washing process, as often occurs in semi‐IPN systems. Interpolymer interactions were investigated with Fourier transform infrared spectroscopy and differential scanning calorimetry. These studies suggested possible interactions between both polymers by the formation of hydrogen bonds. The swelling behavior of these hydrogels was analyzed by immersion of the hydrogel samples in deionized water at 25 and 37°C and in buffer solutions with pHs of 3, 7, and 10. The kinetics of swelling showed increases in the values of the swelling ratio with increasing immersion time in the swelling medium, molar proportion of the biopolymer in the hydrogel, temperature, and pH of the swelling medium. All of the hydrogels swelled rapidly and reached equilibrium in an average time of 40 min. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Reinforcement of pH‐responsive γ‐poly(glutamic acid)/chitosan hydrogel for orally administrable colon‐targeted drug delivery

Orally administrable hydrogel was prepared by crosslinking chitosan (CS) with γ‐poly(glutamic acid) (γ‐PGA) for an excellent pH‐responsive colon‐targeted drug delivery system. The stable crosslinked amide bond appeared in the shifted region of FTIR spectroscopy, and the tensile strength and elastic modulus were also reduced by crosslinking of CS and γ‐PGA. The surfaces of crosslinked hydrogel have a homogeneous pore array with pore size corresponding to the varied blending ratio. The swelling ratio was dramatically changed by increasing the pH from 3 to 6, and the responsiveness of swelling ratio to the reversible pH changes between 3 and 10 was reliable for 72 h. The drug diffusion rate was mainly dependent on the pH, and a water‐soluble tetrazolium (WST‐1) assay indicated that cytocompatibility of the hydrogel was in an acceptable range. © 2012 Wiley Periodicals, Inc. J Appl Polym Sci. 2013     

Crosslinking structures of gelatin hydrogels crosslinked with genipin or a water‐soluble carbodiimide

It was suggested in our previous studies that carbodiimide‐ and genipin‐crosslinked gelatin hydrogels could be used as bioadhesives to overcome the cytotoxicity problem associated with formaldehyde‐crosslinked gelatin hydrogels. In this study, we investigated the crosslinking structures of carbodiimide‐ and genipin‐crosslinked gelatin hydrogels. We found that crosslinking gelatin hydrogels with carbodiimide or genipin could produce distinct crosslinking structures because of the differences in their crosslinking types. Carbodiimide could form intramolecular crosslinks within a gelatin molecule or short‐range intermolecular crosslinks between two adjacent gelatin molecules. On the basis of gel permeation chromatography, we found that the polymerization of genipin molecules could occur under the conditions used in crosslinking gelatin hydrogels via a possible aldol condensation. Therefore, besides intramolecular and short‐range intermolecular crosslinks, additional long‐range intermolecular crosslinks could be introduced into genipin‐crosslinked gelatin hydrogels. Crosslinking a gelatin hydrogel with carbodiimide was more rapid than crosslinking with genipin. Therefore, the gelation time for the carbodiimide‐crosslinked gelatin hydrogels was significantly shorter than that of the genipin‐crosslinked gelatin hydrogels. However, the cohesive (interconnected) structure of the carbodiimide‐crosslinked gelatin hydrogels was readily broken because, unlike the genipin‐crosslinked gelatin hydrogels, there were simply intramolecular and short‐range intermolecular crosslinks present in the carbodiimide‐crosslinked hydrogel. In the cytotoxicity study, the carbodiimide‐crosslinked gelatin hydrogels were dissolved into small fragments in the cultural medium within 10 min. In contrast, the genipin‐crosslinked gelatin hydrogels remained intact in the medium throughout the entire course of the study. Again, this may be attributed to the differences in their crosslinking structures. The genipin‐crosslinked gelatin hydrogels were less cytotoxic than the carbodiimide‐crosslinked gelatin hydrogels. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 91: 4017–4026, 2004     

3D Bioprinting of Gelatin–Xanthan Gum Composite Hydrogels for Growth of Human Skin Cells

In recent years, bioprinting has attracted much attention as a potential tool for generating complex 3D biological constructs capable of mimicking the native tissue microenvironment and promoting physiologically relevant cell–cell and cell–matrix interactions. The aim of the present study was to develop a crosslinked 3D printable hydrogel based on biocompatible natural polymers, gelatin and xanthan gum at different percentages to be used both as a scaffold for cell growth and as a wound dressing. The CellInk Inkredible 3D printer was used for the 3D printing of hydrogels, and a glutaraldehyde solution was tested for the crosslinking process. We were able to obtain two kinds of printable hydrogels with different porosity, swelling and degradation time. Subsequently, the printed hydrogels were characterized from the point of view of biocompatibility. Our results showed that gelatin/xanthan-gum bioprinted hydrogels were biocompatible materials, as they allowed both human keratinocyte and fibroblast in vitro growth for 14 days. These two bioprintable hydrogels could be also used as a helpful dressing material.     

Effect of gelatin on the swelling behavior of organic hybrid gels based on N‐isopropylacrylamide and gelatin

Organic hybrid gels based on poly(N‐isopropylacrylamide) and a natural polymer, gelatin, were prepared through two‐step crosslinking with genipin or glutaraldehyde. The effects of the gelatin content on the swelling behaviors and physical properties of these hybrid gels were investigated. The results indicated that the swelling ratio decreased with an increase in the content of gelatin in these hybrid gels. The swelling ratio for the gel crosslinked by genipin was significantly smaller than that for the gel crosslinked by glutaraldehyde. The results also showed that the gel crosslinked with genipin had a higher crosslinking density and a higher gel strength. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 98: 1092–1099, 2005     

In situ injectable poly(γ‐glutamic acid) based biohydrogel formed by enzymatic crosslinking

Enzymatic crosslinking was developed to prepare in situ forming poly(γ‐glutamic acid) (γ‐PGA) based hydrogel in this study. First, the precursor of poly(γ‐glutamic acid)–tyramine (γ‐PGA–Ty) was synthesized through the reaction of carboxyl groups from a γ‐PGA backbone with tyramine. The structure of the grafted precursor was confirmed by ¹H‐NMR and Fourier transform infrared spectroscopy. After that, the crosslinking of the phenol‐containing γ‐PGA–Ty precursor was triggered by horseradish peroxidase in the presence of H₂O₂; this resulted in the formation of the γ‐PGA–Ty hydrogels. The equilibrium water content, morphology, enzymatic degradation rate, and mechanical properties of the hydrogels were characterized in detail. The data revealed that the well‐interconnected hydrogels had tunable water contents, mechanical properties, and degradability through adjustments of the composition. Furthermore, cell experiments proved the biocompatibility of the hydrogels by 3‐(4,5‐dimethylthiazol‐2‐yl)‐2,5‐diphenyltetrazolium bromide assay. These characteristics provide an opportunity for the in situ formation of injectable biohydrogels as potential candidates in cell encapsulation and drug delivery. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42301.     

Preparation and characterization of PVA/PVP/glycerin/antibacterial agent hydrogels using <Emphasis Type="Italic">γ</Emphasis>-irradiation followed by freeze-thawing

Hydrogels for wound dressings from a mixture of poly(vinyl alcohol) (PVA), poly(N-vinylpyrrolidone) (PVP), glycerin and an antibacterial agent were obtained by a γ-irradiation combined with freeze-thawing. The physical properties such as the gelation and swelling degree of the hydrogels were examined. When the PVP/PVA ratio was 6: 4 (wt%) and prepared by combined irradiation and freeze-thawing, it showed an excellent swelling capacity (>1,200%). The antibacterial effect of the hydrogels containing the antibacterial agents was observed to be effective as the concentration of antibacterial agents increased. The results demonstrated that hydrogel in a proper blending ratio could be used as a wound dressing that can accelerate wound healing with an antibacterial effect.     

Thermoreversible hydrogels. IX. Swelling behaviors of thermosensitive hydrogels copolymerized by N‐isopropylacrylamide with 1‐vinyl‐3‐(3‐sulfopropyl) imidazolium betaine

A series of thermosensitive hydrogels were prepared from the various molar ratios of N‐isopropylacrylamide, 1‐vinyl‐3‐(3‐sulfopropyl) imidazolium betaine (VSIB), and N,N′‐methylene‐bis‐acrylamide. The influence of the amount of VSIB in the copolymeric gels on the swelling behaviors in water, in various saline solutions, and at various temperatures was investigated. The results indicated that the higher the VSIB content in the hydrogel system, the higher the swelling ratio and the gel transition temperature. In the saline solution the results showed that when the concentration of salt is higher than the minimum salt concentration (MSC) of poly(VSIB), the deswelling behavior of the copolymeric gel was more effectively suppressed as more VSIB was added to the copolymeric gels. In addition, only the sample containing 12 mol % VSIB (V4) exhibited an antipolyelectrolyte's swelling behavior when the concentration of salt was higher than the MSC of poly(VSIB). This means that the swelling ratio of the hydrogel can be improved with a higher concentration salt solution. In addition, the anion effects were larger than the cation effects in the presence of a common anion (Cl⁻) with different cations and a common cation (K⁺) with different anions for the hydrogel. Finally, the more VSIB in the hydrogel, the higher the diffusion coefficient in dynamic swelling. © 2000 John Wiley & Sons, Inc. J Appl Polym Sci 77: 14–23, 2000     

Polyelectrolyte complex hydrogel composed of chitosan and poly(γ‐glutamic acid) for biological application: Preparation,physical properties,and cytocompatibility

Polyelectrolyte complex (PEC) hydrogels composed of chitosan as a cationic polyelectrolyte and poly (γ‐glutamic acid) (γ‐PGA) as an anionic polyelectrolyte were prepared from PEC dispersions based on a chitosan solution to which different amounts of γ‐PGA solutions were added to charge equivalency. The chemical structures of the PEC hydrogels were investigated by Fourier transform infrared spectroscopy. The physical properties, fixed charge concentration, crystallinity, mechanical properties, micromorphology, and swelling properties of the PEC hydrogels were also investigated. The total fixed charge concentration of the PEC hydrogels varied as a function of pH on the pK intervals between chitosan (pK = 6.5) and γ‐PGA (pK = 2.27). The isoelectric points (IEP) were shifted to a lower pH with a higher weight ratio of γ‐PGA to chitosan. The elastic modulus was decreased with the weight ratio increasing from 0 : 1 to 1 : 1 (γ‐PGA/chitosan) by ionic crosslinking between the amino groups of chitosan and the carboxyl groups of γ‐PGA. The results of the swelling study showed that the swelling properties of PEC hydrogels were more affected by the change in the elastic restoring force than by the change in the fixed charge concentration depending on the pH. Also, the cytotoxicity of the PEC hydrogels was investigated using normal human dermal fibroblast (NHDF) cell lines, and the results showed the PEC hydrogels were not toxic. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 103:386–394, 2007     

Swelling behavior and cell viability of dehydrothermally crosslinked poly(vinyl alcohol) hydrogel grafted with N‐vinyl pyrrolidone or acrylic acid using γ‐radiation

To improve equilibrium water content, dehydrothermally crosslinked poly(vinyl alcohol) (PVA) hydrogel was grafted with N‐vinyl pyrrolidone (NVP) or acrylic acid (AA) monomer using γ‐radiation. Swelling behavior of the grafted hydrogels was studied in phosphate‐buffered saline, and cell viability was evaluated using fibroblast cells from mouse connective tissue. Equilibrium water content of AA‐ and NVP‐grafted PVA hydrogel ranged between 40–60% and 60–80%, respectively, depending on radiation dose and monomer concentration. For maximum degree of swelling, the optimum monomer concentration and radiation dose were 20% by weight and 20 kGy, respectively. Fibroblast cells seeded on NVP‐grafted hydrogel had an extended oval morphology while those seeded on AA‐grafted PVA had a rounded spherical morphology. These results support the use of NVP for grafting PVA to increase swelling and improve cell viability. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 91: 2862–2868, 2004     

Preparation and drug‐release behavior of minocycline‐loaded poly[hydroxyethyl methacrylate‐co‐poly(ethylene glycol)–methacrylate] films

In this work, biocompatible hydrogel matrices for wound‐dressing materials and controlled drug‐release systems were prepared from poly[hydroxyethyl methacrylate‐co‐poly(ethylene glycol)–methacrylate] [p(HEMA‐co‐PEG–MA] films via UV‐initiated photopolymerization. The characterization of the hydrogels was conducted with swelling experiments, Fourier transform infrared spectroscopy, scanning electron microscopy, thermogravimetric analysis (differential scanning calorimetry), and contact‐angle studies. The water absorbency of the hydrogel films significantly changed with the change of the medium pH from 4.0 to 7.4. The thermal stability of the copolymer was lowered by an increase in the ratio of poly(ethylene glycol) (PEG) to methacrylate (MA) in the film structure. Contact‐angle measurements on the surface of the p(HEMA‐co‐PEG–MA) films demonstrated that the copolymer gave rise to a significant hydrophilic surface in comparison with the homopolymer of 2‐hydroxyethyl methacrylate (HEMA). The blood protein adsorption was significantly reduced on the surface of the copolymer hydrogels in comparison with the control homopolymer of HEMA. Model antibiotic (i.e., minocycline) release experiments were performed in physiological buffer saline solutions with a continuous flow release system. The amount of minocycline release was shown to be dependent on the HEMA/PEG–MA ratio. The hydrogels have good antifouling properties and therefore are suitable candidates for wound dressing and other tissue engineering applications. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Preparation,characterization and the effect of carboxymethylated chitosan–cellulose derivatives hydrogels on wound healing

Oxidized carboxymethyl cellulose (OCMC) was prepared by an oxidation reaction of carboxymethyl cellulose in the presence of sodium periodate. In situ crosslinked hydrogels were obtained through the crosslinking reaction between the active aldehyde of OCMC and the amino groups of the carboxymethyl chitosan (CMCS). The structure of the hydrogels was characterized by FTIR and scanning electron microscopy. Gelation time test showed that the hydrogel had the shortest gelation time of 24 s. The equilibrium fluid content, which represented the swelling degree, was evaluated and we found that the pH increased from 3.0 to 9.0, the equilibrium fluid content increased, and the highest equilibrium fluid content reached 312.83% as pH = 9.0. The wound healing efficacy of the hydrogel was evaluated in experimental deep second degree burns using a rat model. Results indicated that the wound covered with hydrogel was completely filled with new epithelium within 2 weeks, without any significant adverse reactions. The in situ crosslinked hydrogel fulfilled many critical elements in a wound dressing material. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

Carbon nanotube‐hybridized supramolecular hydrogel based on PEO‐b‐PPO‐b‐PEO/α‐cyclodextrin as a potential biomaterial

In virtue of the potential biomedical application of carbon nanotube (CNT), the CNT was hybridized into a supramolecular hydrogel based on the selective inclusion of α‐cyclodextrin (α‐CD) onto poly(ethylene oxide) (PEO) segments of a triblock copolymer, i.e., PEO‐block‐poly(propylene oxide)‐block‐PEO. Different from the previous report, the content of α‐CD, in contrast to that of ethylene oxide unit, was decreased to decrease the network density in hydrogel and hence improve the diffusion of encapsulated substances. As a result, the modulus of the hydrogels climbed slightly after introducing CNT. Furthermore, as the essential properties for wound dressing, the antimicrobial activity, the skin‐adhesion, and water‐retention of such supramolecular hybrid hydrogels were also verified. On the other hand, the supramolecular hybrid hydrogels inherited the shear‐thinning property and are suitable as an injectable biomaterial. The cell viability assay confirmed the equivalent cytotoxicity of the supramolecular hybrid hydrogels to that of the native hydrogels without CNT. Consequently, such CNT‐hybridized supramolecular hydrogel shows a great potential in the biomedical application. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2010     

Release of vitamin B12 from poly(N‐vinyl‐2‐pyrrolidone)‐crosslinked polyacrylamide hydrogels: A kinetic study

Hydrogels, composed of poly(N‐vinyl‐2‐pyrrolidone) and crosslinked polyacrylamide, were synthesized and the release of vitamin B₁₂ from these hydrogels was studied as a function of the degree of crosslinking and pH of the external swelling media. The three drug‐loaded hydrogel samples synthesized with different crosslinking ratios of 0.3, 0.7, and 1.2 (in mol %) follow different drug‐release mechanisms, that is, chain relaxation with zero‐order, non‐Fickian and Fickian, or diffusion‐controlled mechanisms. To establish a correlation between their swelling behavior and drug‐release mechanism, the former was studied by the weight‐gain method and, at the same time, the concentration of the drug released was studied colorimetrically. Various swelling parameters such as the swelling exponent n, gel‐characteristic constant k, penetration velocity v, and diffusion coefficient D were evaluated to reflect the quantitative aspect of the swelling behavior of these hydrogels. Finally, the drug‐release behavior of the hydrogels was explained by proposing the swelling‐dependent mechanism. © 2000 John Wiley & Sons, Inc. J Appl Polym Sci 76: 1706–1714, 2000     

Poly(vinyl alcohol)/chitosan/honey/clay responsive nanocomposite hydrogel wound dressing

Many efforts have been made to develop modern wound dressings to overcome limitations of traditional ones. Smart nanocomposite hydrogels are appropriate candidates. In this work, a novel responsive nanocomposite hydrogel based on poly(vinyl alcohol)/chitosan/honey/clay was developed and evaluated as a novel wound dressing. The morphology and properties of synthesized nanocomposite hydrogels loaded with honey as a drug model were investigated. The exfoliated morphology of nanocomposite was confirmed by X‐ray diffractometry. Swelling studies were performed at 20 and 37 °C at various pH. The results showed that swelling increased as a result of temperature rise and maximum swelling occurred at a pH of 2. In vitro release of honey was also studied at the same conditions. Corresponding results indicated faster honey release rate at higher pH values. MTT results exhibited no cytotoxicity in nanocomposite hydrogel system. Investigation of antibacterial activity revealed more than 99% antibacterial activity for proposed system. In vivo results confirmed the wound healing ability of developed system. Generally, appropriate properties of proposed system made it ideal in wound dressing applications. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46311.     

Thermosensitive elastin-derived polypeptide hydrogels crosslinked by genipin

In this paper, first, elastin-derived peptides (EPs) with low molecular weight were prepared by acid degradation. Second, elastin-derived peptide hydrogels were fabricated by crosslinking EP with genipin. EP exhibited an inverse transition temperature, and the inverse transition temperature (T_t) could be adjusted by changing the concentration and molecular weight of EP, pH, and adding salt. The freeze-dried EP hydrogels were obviously three-dimensional network structure and the property of EP hydrogel can be optimized by dosage of genipin. Differential scanning calorimetry (DSC) tests and the swelling ratio changing with temperature showed the crosslinked EP hydrogels were still thermosensitive and exhibited a negative swelling behavior. The compression modulus of EP hydrogels can even reach 39.4?kPa, surpassing many other elastin-based hydrogels. This genipin crosslinked EP hydrogel is a good biological material and has great potentiality in tissue engineering.     

Theophylline‐loaded pectin‐based hydrogels. I. Effect of medium pH and preparation conditions on drug release profile

In this study, a series of theophylline‐loaded calcium pectin gel films were prepared in three different Ca⁺² concentrations with three different methods for wound dressing applications. Drug release performance of the films were investigated in four different medium pH in order to mimic wound healing pH conditions. Hydrogel films were characterized by Fourier transform infrared spectroscopy, differential scanning calorimetry, scanning electron microscopy and atomic force microscopy. Their absorbency (fluid handling), swelling behavior, dehydration rate, dispersion characteristic, dressing pH determination, water vapor permeability, oxygen permeability, surface contact angle, flexibility, Shore A hardness, mean mass per unit area and thickness were determined. The effect of the hydrogels on wound healing was evaluated with an in vitro wound healing assay. After evaluating all data, we suggested that the hydrogel film prepared with swelling method using 7% or 10% crosslinker and dried at 26 °C is more suitable for controlled drug release process. We showed that between pH 3.25 and 7.12 the form of the hydrogel did not change, and drug release was continuous. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46731.     

Release of fluorescent markers from phase‐separated gelatin‐maltodextrin hydrogels

Genipin‐crosslinked gelatin‐maltodextrin phase‐separated hydrogels consisting of gelatin‐continuous or bicontinuous microstructures were developed to regulate swelling and release behavior of four fluorescent markers of varying molecular weights [(fluorescein (332 Da) and FITC‐dextrans (FD) (4000–250,000 Da)]. Bicontinuous hydrogels showed significantly greater swelling than gelatin‐continuous hydrogels under all conditions (at pH 1.5 and 7.4 and three genipin/gelatin crosslinking ratios) (P < 0.05). With both microstructures, fluorescein showed the largest release rate and total release followed by FD 4000 Da, FD 40,000 Da, and FD 250,000 Da (P < 0.05). Marker molecular weight, pH, and crosslink ratio all affected the rate and amount of release. The mode of transport for the solvent and all markers was Fickian or slightly anomalous, with diffusional exponent (n) values ranging from 0.35 to 0.64. These results demonstrated that with the proper combination of crosslink density, solvent pH, and microstructure, hydrogels with a specified swelling behavior may be developed. This, coupled with a marker of appropriate size, can lead to controllable levels and rates of release. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011