Polyether-segmented nylon hemodialysis membrane. VI. Effect of polyether segment on morphology and surface structure of membrane

Amorphous nylon, poly(iminoisophthaloyliminomethylene-1,3-cyclohexylenemethylene) (NyBI) and poly(ethylene oxide) (PEO)-segmented NyBI (PEO–NyBI) membranes were prepared by a phase-inversion method using water/dimethyl sulfoxide (DMSO) mixtures as coagulants. The influence of the PEO segment and coagulant compositions on the morphology of the membranes was investigated. The cloud-point curves in the polymer/DMSO/water ternary system showed that PEO–NyBI and NyBI had the same coagulation processes, that is, instantaneous liquid–liquid phase separation occurred, resulting in a fingerlike structure in the cross section of the membranes. The membrane morphologies observed under a scanning electron microscope (SEM) agreed with the prediction. The PEO segment had little or no effect on the membrane morphologies which were prepared in the coagulants with a low DMSO concentration, and it promoted the change of the phase-separation style from the instantaneous to the delayed one in the case of the DMSO-rich coagulant. The PEO segment, however, significantly influenced the ultrafiltration rate. Additionally, the relationship between the surface composition of the PEO–NyBI membrane and the coagulation condition was also investigated by use of electron spectroscopy for chemical analysis (ESCA) and static secondary ion mass spectrometry (SSIMS). A small enrichment of the PEO segment at the top surface of the membranes was observed with the increase of the DMSO concentration in the coagulant. © 1998 John Wiley & Sons, Inc. J Appl Polym Sci 69: 1645–1659, 1998     

Surface structures of solvent‐cast films prepared from poly(ethylene oxide)‐segmented nylons

The surface structures of three kinds of poly(ethylene oxide)‐segmented nylon (PEO‐Ny) films prepared by the solvent‐cast method were investigated with electron spectroscopy for chemical analysis (ESCA). The PEO‐Ny's used were high‐crystalline PEO‐segmented poly(iminosebacoyliminohexamethylene), low‐crystalline PEO‐segmented poly(iminosebacoylimino‐m‐xylene), and amorphous PEO‐segmented poly(iminoisophthaloyliminomethylene‐1,3‐cyclohexylenemethylene), and the PEO contents in the bulk polymers were approximately 10 wt %. The ESCA results showed that the PEO segment was enriched on the top surfaces of all the films, and the degrees of enrichment were different. The mechanism of the PEO enrichment was examined. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 10–16, 2002     

Polyether-segmented nylon hemodialysis membranes. II. Morphologies and permeability characteristics of polyether-segmented nylon 610 membrane prepared by the phase inversion method

The relationships between the morphologies and the permeability characteristics as dialysis membrane of polyether-segmented nylon 610 (PE-Ny610) have been investigated. PE-Ny610 used are poly(propylene oxide) (PPO)-segmented nylon 610 containing 25 wt % PPO (PPO-Ny610) and poly(ethylene oxide) (PEO)-segmented nylon 610 containing 15 wt % PEO (PEO-Ny610). The morphologies in the cross section of the membranes exhibit the cellular porous structures due to liquid-liquid phase separation. On the other hand, the structures of the surfaces are mainly composed of the crystalline spherulite due to liquid-solid phase separation. These morphologies are little affected by the composition ratio of the coagulant, calcium chloride/methanol/water mixture. PEO-Ny610 membranes have shown superior membrane performances to the PPO-Ny610 membrane. The effect of PEO content in PEO-Ny610 on the adhesion of platelet onto the PEO-Ny610 film surface was investigated and it is concluded that PEO-Ny610 having > 10 wt % PEO shows a good nonthrombogenicity equal to PPO-Ny610. © 1997 John Wiley & Sons, Inc. J Appl Polym Sci 65:1713–1721, 1997     

Polyether-segmented nylon hemodialysis membrane. V. Evaluation of blood compatibility of polyether-segmented nylons

The biocompatibility of poly(propylene oxide)-segmented nylon610 (PPO-Ny610), poly(ethylene oxide)-segmented nylon610 (PEO-Ny610), poly(ethylene oxide)-segmented nylonM10 (PEO-NyM10), and poly(ethylene oxide)-segmented nylon69/M10 (PEO-Ny69/M10) hollow fibers were investigated in terms of the transient leukopenia by the extracorporeal circulation in a rabbit. PPO-Ny610 and PEO-Ny610 hollow fibers showed that the minimum leukocyte counts during the circulations were > 80% against the initial count of leukocyte. These results indicate that these polymers have good blood compatibility. In PEO-NyM10 and PEO-Ny69/M10, the remarkable decreases of the leukocyte count were observed and the minimum counts were in the range of 45–50%. From the evaluation results of homo nylons (Ny610 and NyM10) hollow fibers, the low blood compatibilities observed in PEO-NyM10 and PEO-Ny69/M10 are not attributed to the chemical structure of the nylon blocks. © 1998 John Wiley & Sons, Inc. J Appl Polym Sci 67:1253–1257, 1998     

A facile synthesis of mixed soft‐segmented poly(urethane‐imide)–polyhedral oligomeric silsesquioxone hybrid nanocomposites and study of their structure–transport properties

The structure–transport properties of mixed soft‐segmented poly(urethane‐imide) (MSPUI) membranes and their microstructures were investigated. Polypropylene glycol, polycaprolactone diol and bis(3‐aminopropyl)‐terminated polydimethylsiloxane were used as the soft segments in the membrane synthesis via a three‐step polymerization reaction. The chemical structures of the MSPUI membranes were characterized using attenuated total reflectance Fourier transform infrared spectroscopy. Morphology and surface properties of the membranes were studied using scanning electron and atomic force microscopy techniques. Surface energy measurements indicated the enrichment of the hydrophobic soft segment in the membranes. The amorphous nature of the polymers was analysed using wide‐angle X‐ray diffraction. The effect of morphology on the permeability and selectivity of the membranes is discussed. Finally, membrane structure–transport property relationships were correlated. © 2013 Society of Chemical Industry     

Nonfouling biomaterials based on polyethylene oxide‐containing amphiphilic triblock copolymers as surface modifying additives: Synthesis and characterization of copolymers and surface properties of copolymer–polyurethane blends

The objective of this work is to develop nonfouling biomaterials by blending polyethylene oxide (PEO)‐containing block copolymers with a polyurethane (PU) matrix; it is expected that the PEO component will migrate to the tissue‐material interface. Three amphiphilic triblock copolymers, PEO‐PU‐PEO, in which the PEO MW was 550 (copolymer 1), 2000 (copolymer 2), and 5000 (copolymer 3), respectively, were synthesized. XPS data showed that the polymer/vacuum interfaces of copolymers 2 and 3 were enriched in the PU block, whereas that of copolymer 1 was enriched in the PEO block. In contact with water, the PEO blocks for all three copolymers migrated to the surface as indicated by water contact angles. Blends of the copolymers with a segmented polyurethane were investigated. Surface enrichment of the copolymers occurred and increased over time up to a limit; the degree of enrichment was dependent on PEO block size and copolymer content. At copolymer content <10%, enrichment decreased with increasing PEO block size. For the copolymer 2 and copolymer 3 blends, enrichment increased with increasing copolymer content; at 20% copolymer the surfaces consisted essentially of pure copolymer. For the copolymer 1 blends, the surface was completely covered by copolymer at content ≥ 1%. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Structure‐property relationships of degradable polyurethane elastomers containing an amino acid‐based chain extender

A series of degradable polyurethanes of variable soft segment chemistry and content were synthesized and characterized. An amino acid‐based diester chain extender was used to confer degradability and both polycaprolactone diol (PCL) and polyethylene oxide (PEO) were used as soft segments. In addition, the diisocyanate component was a potentially nontoxic diisocyanate (2,6‐diisocyanato methyl caproate, LDI). The physicochemical properties of these unique series of polyurethanes were investigated. It was found that the PEO containing polyurethanes were generally weak, tacky amorphous materials. In contrast, the PCL polyurethanes were relatively strong, elastomeric materials which ranged from completely amorphous to semicrystalline as noted by differential scanning calorimetry. The PCL containing polyurethanes exhibited increasing tensile strength, modulus, and ultimate strain with increasing PCL molecular weight because of increasing phase separation and increasing soft segment crystallinity. Fourier transform infrared analysis showed significant hard segment urea and urethane hydrogen bonding which increased with hard segment content, although interphase bonding is believed to be significant for the PCL polyurethanes. Surface characterization carried out by contact angle analysis and X‐ray photoelectron spectroscopy indicated soft segment surface enrichment for all of the polyurethanes. The PEO‐based polymers were very hydrophilic whereas the PCL‐based polymers displayed significantly higher contact angles, indicating greater surface hydrophobicity. The observed diversity in material properties suggests that these polyurethanes may be useful for a wide range of applications. © 2000 John Wiley & Sons, Inc. J Appl Polym Sci 75: 1522–1534, 2000     

Synthesis and properties of hydrophilic segmented block copolymers based on poly(ethylene oxide)‐ran‐poly(propylene oxide)

The present article discusses the synthesis and various properties of segmented block copolymers with random copolymer segments of poly(ethylene oxide) and poly(propylene oxide) (PEO‐r‐PPO) together with monodisperse amide segments. The PEO‐r‐PPO contained 25 wt % PPO units and the segment presented a molecular weight of 2500 g/mol. The synthesized copolymers were analyzed by differential scanning calorimetry, Fourier transform infra‐red spectroscopy, atomic force microscopy and dynamic mechanical thermal analysis. In addition, the hydrophilicity and the contact angles (CAs) were studied. The PEO‐r‐PPO segments displayed a single low glass transition temperature, as well as a low PEO crystallinity and melting temperature, which gave enhanced low‐temperature properties of the copolymer. The water absorption values remained high. In comparison to mixtures of PEO/PPO segments, the random dispersion of PPO units in the PEO segments was more effective in reducing the PEO crystallinity and melting temperature, without affecting the hydrophilicity. Increasing the polyether segment length with terephthalic groups from 2500 to 10,000 g/mol increased the hydrophilicity and the room temperature elasticity. Furthermore, the CAs were found to be low 22–39° and changed with the crosslink density. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci 117:1394–1404, 2010     

Polyvinyl alcohol‐polyethylene oxide‐carboxymethyl cellulose membranes for drug delivery

The purpose of this research was to develop blends of poly(vinyl alcohol) (PVA)‐poly(ethylene oxide) (PEO) and carboxymethyl cellulose (CMC) by two approaches: solvent casting and freeze‐drying to develop membranes for various biomedical applications. The PVA/PEO/CMC blends in different compositions of 90/10/20, 80/20/20, 70/30/20, 60/40/20, and 50/50/20 were prepared and were coated on polyester (PET) nonwoven fabric and were subsequently freeze‐dried (FD). The influence of PEO concentration on the blend membranes was investigated and characterized by X‐ray diffraction (XRD), differential scanning calorimetry, and attenuated total reflectance‐fourier transform infra‐red (ATR–FTIR) techniques. The water vapor transmission rate (WVTR), swelling behavior, and surface morphology of the FD membranes was also investigated. It was observed that an increase of PEO concentration in blends makes the membranes more fragile. However, the coating of this blend on PET fabric helps in developing the stable membrane. Swelling of the membranes decreased with the increase in the PEO concentration. XRD showed decrease in crystallinity with increase in concentration of PEO. Morphological studies showed a highly porous structure with interconnected pores. The total porosity of the membranes was found to be in the range 89–92%. The FD membranes were found to have WVTR in the range 2000–3000 g/m²/day. A model drug, ciprofloxacin hydrochloride was also incorporated in the matrix and drug release was studied. The antimicrobial nature of the membranes was monitored against E. coli by zone of inhibition method. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

Polyether-segmented nylon hemodialysis membranes. IV. Membrane morphologies and permeability characteristics of dialysis membrane composed of poly(ethylene oxide)-segmented Ny69/M10

Dialysis membrane was prepared by a phase inversion method using a new polyether-segmented nylon which dissolves in common organic solvents such as dimethylsulfoxide. The polyether-segmented nylon contained poly(ethylene oxide) block and nylon block (random copolyamide: Ny69/M10) prepared by sebacic acid, azelaic acid, m-xylenediamine, and hexamethylenediamine. The morphologies and permeability characteristics of the membranes were investigated. It was shown by scanning electron microscope observation that the membrane had a fingerlike structure when dimethylsulfoxide was used as a polymer solvent, and a spongelike structure when an additive such as calcium chloride was added to the polymer solution. The high permeability for the solutes such as urea and vitamin B₁₂ were observed in comparison with the polyether-segmented Ny610 membranes prepared by a phase inversion method. © 1997 John Wiley & Sons, Inc. J Appl Polym Sci 65:1731–1737, 1997     

Evaluation of the permeability and blood‐compatibility properties of membranes formed by physical interpenetration of chitosan with PEO/PPO/PEO triblock copolymers

In order to develop blood compatible membranes with controlled porosity, we have fabricated and examined the properties of physical interpenetrating network (PIN) of chitosan and poly(ethylene oxide)/poly(propylene oxide)/poly(ethylene oxide) (PEO/PPO/PEO) triblock copolymers (Pluronics^®). Degree of equilibrium swelling, scanning electron microscopy, and electron spectroscopy for chemical analysis (ESCA) were used to characterize the bulk and surface properties. Vitamin B₁₂ and human serum albumin were used as permeability markers. Platelet adhesion and activation were used to determine the blood‐interaction properties of the PIN membranes. Unlike chitosan membranes that were nonporous, the chitosan‐Pluronic PIN membranes were highly porous with the pore size, depending on the type of incorporated Pluronic polyol. ESCA results showed a significant increase in the ? C ? O? signal of C1s spectra on the PIN membranes that correlates with the presence of PEO chains on the surface. The permeability coefficients of vitamin B₁₂ and albumin were higher in the chitosan‐Pluronic PIN membranes than in the control. The number of adherent platelets and the extent of activation were significantly reduced on the chitosan‐Pluronic PIN membranes. The decrease in platelet adhesion and activation correlated positively with the PEO chain length of the incorporated Pluronic polyols. The results of this study show that chitosan‐Pluronic PIN membranes offer a blood‐compatible alternative with a higher‐molecular‐weight cutoff for use in hemodialysis and related applications. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 80: 1274–1284, 2001     

Polyether-segmented nylon hemodialysis membranes. I. Preparation and permeability characteristics of polyether-segmented nylon 610 hemodialysis membrane

The effect of the coagulation condition in the phase inversion method on the permeability characteristics of poly(propylene oxide) or poly(tetramethylene oxide)-segmented nylon 610 (PPO-Ny610 or PTMO-Ny610) hemodialysis membranes, the stability of the membrane performance, and the mechanical strength were investigated. The polymers were dissolved in a solvent such as formic acid and methanol saturated with calcium chloride, and thus PPO-Ny610 and PTMO-Ny610 membranes were prepared using formic acid and a calcium chloride/methanol/water mixture as a polymer solvent and a coagulant, respectively. It is concluded that PPO-Ny610 membrane has better permeability characteristics than PTMO-Ny610 membrane, and possesses additional properties for hemodialysis membranes such as mechanical properties and permeability stability in the drying and sterilizing processes. Furthermore, the blood compatibilities of PPO-Ny610 and PTMO-Ny610 membranes were superior to regenerated cellulose membranes on the basis of the result of platelet adhesion test. © 1997 John Wiley & Sons, Inc. J Appl Polym Sci 65:1703–1711, 1997     

Characterization of glow‐discharge–treated cellulose acetate membrane surfaces for single‐layer enzyme electrode studies

Cellulose acetate membranes (CA) were modified by means of plasma polymerization of ethylene diamine (EDA) and n‐butylamine (n‐BA). The motivation for this work was the application of a modified membrane for the single‐layer enzyme electrode. A tubular reactor with the external radiofrequency (13.56 MHz) excitation was used. Surface modification was performed at 5, 10, and 15 W power (at 27 Pa working pressure) for 5, 10, 15 min. Modified surfaces were characterized in detail by FTIR–ATR, XPS (ESCA), contact angle, and enzyme immobilization activity. The best treatment results were obtained for EDA with 5 W and 30 min and 15 W and 10 min. These results are discussed using surface analysis data. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 81: 1341–1352, 2001     

Structural characterization and mass transfer properties of dense segmented polyurethane membrane: Influence of hard segment and soft segment crystal melting temperature

An attempt has been taken to investigate the microstructure and mass transfer properties of polycaprolactone diol (M_n = 2000 g mol^–1, PCL 2000)‐based dense segmented polyurethane (SPU) membrane as a function of hard segment (HS) content. Structure of SPUs were investigated by Fourier transform infrared analysis, wide angle X‐ray diffraction, differential scanning calorimetry, dynamic mechanical thermal analysis, and scanning electron microscopy (SEM). On the other hand, mass transfer properties were measured by equilibrium sorption, dynamic sorption, and water vapor permeability measurements. From the experimental results, it was observed that with the increasing HS content in SPU the percentage crystallinity decreases, whereas the glassy state storage modulus increases. α transition temperature of polyurethane copolymers also increases with increasing HS content. SEM micrograph shows the dense surface structure of SPU films. Mass transfer rate of dense polyurethane membranes decreases with increasing HS content. In contrast, hydrophilic segment and soft segment crystal melting could enhance the mass transfer properties. POLYM. ENG. SCI., 2008. © 2007 Society of Plastics Engineers     

Immobilization of polyethylene oxide surfactants for non-fouling biomaterial surfaces using an argon glow discharge treatment

A non-fouling (protein-resistant) polymer surface is achieved by the covalent immobilization of polyethylene oxide (PEO) surfactants using an inert gas discharge treatment. Treated surfaces have been characterized using electron spectroscopy for chemical analysis (ESCA), static secondary ion mass spectrometry (SSIMS), water contact angle measurement, fibrinogen adsorption, and platelet adhesion. This paper is intended to review our recent work in using this simple surface modification process to obtain wettable polymer surfaces in general, and non-fouling biomaterial surfaces in particular.     

Simultaneously enhanced cryogenic mechanical behaviors of cyanate ester/epoxy resins by poly(ethylene oxide)‐co‐poly(propylene oxide)‐co‐poly(ethylene oxide) (PEO‐PPO‐PEO) block copolymer and clay

Cryogenic mechanical properties are important parameters for thermosetting resins used in cryogenic engineering areas. The hybrid nanocomposites were prepared by modification of a cyanate ester/epoxy/poly(ethylene oxide)‐block‐poly(propylene oxide)‐block‐poly(ethylene oxide) (PEO‐PPO‐PEO) system with clay. It is demonstrated that the cryogenic tensile strength, Young's modulus, ductility (failure strain), and fracture resistance (impact strength) are simultaneously enhanced by the addition of PEO‐PPO‐PEO and clay. The results show that the tensile strength and Young's modulus at 77 K of the hybrid nanocomposite containing 5 wt% PEO‐PPO‐PEO and 3 wt% clay were enhanced by 31.0% and 14.6%, respectively. The ductility and impact resistance at both room temperature and 77K are all improved for the hybrid composites. The fracture surfaces of the neat BCE/EP and its nanocomposites were examined using scanning electron microscopy (SEM). Finally, the dependence of the coefficients of thermal expansion (CTE) on the clay and PEO‐PPO‐PEO contents was examined by thermal dilatometer. POLYM. COMPOS., 38:2237–2247, 2017. © 2015 Society of Plastics Engineers     

Preparation and properties of transparent thermoplastic segmented polyurethanes derived from different polyols

Various segmented polyurethanes of different soft segment structure with hard segment content of about 50 wt% were prepared from 4,4′‐diphenylmethane diisocyanate (MDI), 1,4‐butanediol and different polyols with a M_n of 2000 by a one‐shot, hand‐cast bulk polymerization method. The polyols used were a poly(tetramethylene ether)glycol, a poly(tetramethylene adipate)glycol, a polycaprolactonediol and two polycarbonatediols. The segmented polyurethanes were characterized by gel permeation chromatography (GPC), UV‐visible spectrometry, differential scanning calorimetry (DSC), dynamic mechanical analysis (DMA), X‐ray diffraction, and their tensile properties and Shore A hardness were determined. The DSC and DMA data indicate that the miscibility between the soft segments and the hard segments of the segmented polyurethanes is dependent on the type of the soft segment, and follows the order: polycarbonate segments > polyester segments > polyether segments. The miscibility between the soft segments and the hard segments plays an important role in determining the transparency of the segmented polyurethanes. As the miscibility increases, the transparency of the segmented polyurethanes increases accordingly. The segmented polyurethanes exhibit high elongation and show ductile behavior. The tensile properties are also affected by the type of the soft segment to some extent. POLYM. ENG. SCI., 47:695–701, 2007. © 2007 Society of Plastics Engineers.     

Siloxane‐based segmented poly(urethane‐urea) elastomer: Synthesis and characterization

A series of segmented poly(urethane‐urea) block copolymers were synthesized with varying proportions of polydimethylsiloxane diols in combination with polytetramethylene ether glycol (PTMG) using 4,4'‐methylenediphenyl diisocyanate followed by chain extension with a (50:50 mol %) mixture of 4,4'‐methylene‐bis(3‐chloro‐2,6‐diethylaniline) (M‐CDEA) and 1,4‐butanediol (BD). The molecular structures of polydimethylsiloxane urethane‐ureas were characterized by ATR‐FTIR and ¹H‐NMR spectroscopic techniques. Distribution of siloxane domain and its influence on surface roughness were investigated by scanning electron microscopy (SEM) and atomic forced microscopy (AFM), respectively. The mechanical and thermal properties of the elastomers were studied by thermogravimetric analysis, dynamical mechanical thermal analysis, and tensile measurement. The results showed that by incorporation of polydimethylsiloxane diol and M‐CDEA chain extender in polyurethane formulation, some improvements in thermal stability, fire resistance and surface hydrophilicity were achieved. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 1743–1751, 2013     

Crystallization behavior of dry‐brush PEO‐PS block copolymer and PEO homopolymer blend

The crystallization behavior of semicrystalline PEO homopolymer/triblock PS‐PEO‐PS copolymer blend system, which exhibited “Dry‐Brush” in the melt. A symmetric polystyrene–poly(ethylene oxide)–polystyrene triblock copolymer was blended with PEO homopolymer (h‐PEO) having the same molecular weight as that of the PEO block in the copolymer. Considering the composition of the blend (W_ps ≥ 0.8), PEO spheres were formed in the blend. Because of the dry‐brush phase behavior of this blend, h‐PEO added was localized in the PEO microdomains, which increases the domain size without changing the microdomain morphology. The crystallization of PEO block was confined within the microdomains and the crystallization temperature was about 60°C lower than normal. Self‐seeding tests were performed to clarify the nucleation mechanism of the blend. Because the droplets size varies greatly, multicrystallization peaks were witnessed in the self‐seeding process. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci 2007     

Differential scanning calorimetry analysis of silicon‐containing and phosphorus‐containing segmented polyurethane. I—Thermal behaviors and morphology

This article investigated thermal transition and morphology utilizing differential scanning calorimetry (DSC), which was performed on silicon‐containing and phosphorus‐containing segmented polyurethane (Si‐PU and P‐PU). The hard segments of those Si‐PU and P‐PU polymers investigated consisted of 4,4′‐diphenylmethane diisocyanate (MDI) and diphenylsilanediol (DSiD), MDI, and methylphosponic (MPA), respectively. The soft segment of those polymers comprised polytetramethylene ether glycol, with an average molecular weight of 1000 or 2000 (PTMG 1000 and PTMG 2000, respectively). Several thermal transitions appeared for on the Si‐PU and P‐PU polymers, reflecting both the soft‐segment and hard‐segment phases. The Si‐PU and P‐PU polymers with a lower hard‐segment content exhibited a high degree of phase separating as indicated by the constancy of both the soft‐segment glass transition temperature (T_gs) and the breadth of transition zone (ΔB). The polymers in which PTMG 2000 was used as the soft segment generally exhibited a crystalline melting endotherm about 10°C, while crystallization usually disappeared upon melt quenching. The hard segments of the Si‐PU and P‐PU polymers displayed multiple endotherms. The first endotherm was related to a short‐range ordering of the hard segment domain (Region I), and the second endotherm was ascribed to a long‐range ordering of the domain (Region II). The wide‐angle X‐ray demonstrated that the structure in Region I and Region II was almost completely amorphous. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 81: 3489–3501, 2001