Drug release behavior of electrical responsive poly(vinyl alcohol)/poly(acrylic acid) IPN hydrogels under an electric stimulus

The electrically modulated properties of interpenetrating polymer networks (IPN) composed of poly(vinyl alcohol) (PVA) and poly(acrylic acid) (PAAc) under electric field were investigated for drug delivery systems. PVA/PAAc IPNs with various compositions were synthesized by a sequential method, that is, ultraviolet polymerization of AAc in the mixture of PVA and aqueous AAc monomer solution, followed by a freeze‐thawing process to prepare elastic hydrogels. The amount of loaded drug significantly increased with the content of PAAc containing ionizable groups in IPN. The amount of introduced ionic drug (cefazoline) was greater than that of the nonionic drug (theophylline). Release behaviors of drug molecules from negatively charged PVA/PAAc IPN were switched on and off in a pulsatile pattern depending on the applied electric stimulus. The released amount and the release rate of drug were influenced significantly by the applied voltage, ionic group contents in IPN, ionic properties of drug solute, and the ionic strength of release medium. In addition, the ionic properties of drug molecules dramatically affected release behaviors, thus the release of ionic drug was much more enhanced than that of the nonionic drug. © 1999 John Wiley & Sons, Inc. J Appl Polym Sci 74: 1752–1761, 1999     

Electric stimuli responses to poly(vinyl alcohol)/chitosan interpenetrating polymer network hydrogel in NaCl solutions

An interpenetrating polymer network (IPN) hydrogel composed of poly(vinyl alcohol) (PVA) and chitosan exhibited electric‐sensitive behavior. The PVA/chitosan IPN hydrogel was synthesized by an ultraviolet (UV) irradiation method that is used in several biomedical and industrial fields. The swelling behavior of the PVA/chitosan IPN hydrogel was studied by immersion of the gel in NaCl aqueous solutions at various concentrations. The swelling ratio decreased with increasing concentration of NaCl solution. The stimuli response of the IPN hydrogel in electric fields was also investigated. When a swollen PVA/chitosan IPN was placed between a pair of electrodes, the IPN exhibited bending behavior in response to the applied electric field. The bending angle and the bending speed of the PVA/chitosan IPN increased with increasing applied voltage and concentration of NaCl aqueous solution. The PVA/chitosan IPN also showed stepwise bending behavior depending on the electric stimulus. In addition, thermal properties of PVA/chitosan IPN were investigated by differential scanning calorimetry (DSC) and dielectric analysis (DEA). © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 2285–2289, 2002     

Electrical sensitivity behavior of a hydrogel composed of polymethacrylic acid/poly(vinyl alcohol)

An interpenetrating polymer network (IPN) composed of polymethacrylic acid (PMAA) and poly(vinyl alcohol) (PVA) was prepared and exhibited electrical sensitivity behavior. The swelling behavior of the PMAA/PVA IPN hydrogel was studied by immersion of the gel in aqueous NaCl solutions at various concentrations and pH values. The stimuli response of the PMAA/PVA IPN hydrogel in electric fields was also investigated. When swollen IPN hydrogel was placed between a pair of electrodes, the PMAA/PVA IPN hydrogel exhibited bending behavior upon the application of an electric field. The PMAA/PVA IPN hydrogel also showed stepwise bending behavior depending on the electric stimulus. Also, for biomedical applications, the bending behavior of PMAA/PVA IPN hydrogel in Hank's solution at pH 7.4 was studied. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 91:3613–3617, 2004     

Synthesis and swelling characteristics of pH and thermoresponsive interpenetrating polymer network hydrogel composed of poly(vinyl alcohol) and poly(acrylic acid)

The swelling behavior of novel pH- and temperature-sensitive interpenetrating polymer networks (IPNs) composed of poly(vinyl alcohol) (PVA) and poly(acrylic acid) (PAAc) in water was investigated. The PVA/PAAc IPN hydrogels were synthesized by UV irradiation, followed by a repetitive freezing and thawing process by which PVA hydrogel networks were formed inside of cross-linked PAAc chains. The swelling behaviors of these IPNs were analyzed in buffer solution at various pH and temperature ranges. Swelling ratios of all IPNs were relatively high, and they showed reasonable sensitivity to both pH and temperature. Hydrogels showed both the positive and negative swelling behaviors depending on PAAc content. IPN46 showed the positive temperature-sensitive swelling behaviors and its stepwise changes in swelling ratio was about 1.8 and 2.0 obtained between 25 and 45°C at pH 7, and between pH 4 and 7 at 35°C, respectively. The positive temperature dependence is attributed to the formation and dissociation of hydrogen bonding complexes between PVA and PAAc. These IPNs are expected to show a pH- and temperature-sensitive drug release according to the stepwise behavior at this temperature region. © 1996 John Wiley & Sons, Inc.     

Electroactive characteristics of interpenetrating polymer network hydrogels composed of poly(vinyl alcohol) and poly(N‐isopropylacrylamide)

An interpenetrating polymer network (IPN) composed of poly(vinyl alcohol) (PVA) and poly(N‐isopropylacrylamide) (PNIPAAm) was prepared by the sequential IPN method. The equilibrium swelling ratio and bending behavior under electric fields of the IPN hydrogel were measured in an aqueous NaCl solution. The IPN exhibited a high equilibrium swelling ratio, in the range 280–380%. When the IPN in aqueous NaCl solution was subjected to an electric field, the IPN showed significant and quick bending toward the cathode. The IPN hydrogel also showed stepwise bending behavior, depending on the electric stimulus. In addition, the ionic conductivity of the IPN hydrogel was measured using dielectric analysis, and its conductive behavior followed the Arrhenius equation. The conductivity of the IPN hydrogel and the activation energy for the form of the IPN were 1.68 × 10^?5 S/cm at 36°C and 61.0 kJ/mol, respectively. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 89: 890–894, 2003     

Electrochemical behavior of an interpenetrating polymer network hydrogel composed of poly(propylene glycol) and poly(acrylic acid)

An interpenetrating polymer network (IPN) hydrogel based on poly(propylene glycol) and poly(acrylic acid) was prepared by UV irradiation. The swelling behavior of the IPN hydrogel was studied by the immersion of the gel in aqueous NaCl solutions of various concentrations. The swelling ratio decreased with an increase in the NaCl concentration. The electrically sensitive behavior of the IPN hydrogel in electric fields was also investigated. The IPN hydrogel also showed a stepwise bending behavior that depended on the electric stimulus. The bending angle and bending speed of the IPN hydrogel were greatest in 0.6 wt % aqueous NaCl and increased with an increase in the applied voltage. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 89: 2301–2305, 2003     

Permeation of solutes through interpenetrating polymer network hydrogels composed of poly(vinyl alcohol) and poly(acrylic acid)

The swelling behaviors of poly(vinyl alcohol)–poly(acrylic acid) (PVA–PAAc) interpenetrating networks (IPN) hydrogels in the presence of electrolytes were studied. The ionized carboxylic group within IPN hydrogels at pH 7 strongly interacted with electrolytes in the medium and caused anomalous swelling pattern. The permeabilities of 5 representative solutes were regulated as a function of temperature, pH, ionic strength, solute size, and ionic properties of solutes. The permeation of nonionic solutes followed the swelling behaviors dependent on external stimuli, including the above factors. However, the ionic solutes showed different trends in their permeation through IPN hydrogels. © 1998 John Wiley & Sons, Inc. J Appl Polm Sci 69: 479–486, 1998     

Synthesis and characteristics of interpenetrating polymer network hydrogel composed of chitosan and poly(acrylic acid)

Interpenetrating polymer network (IPN) hydrogels composed of chitosan and poly(acrylic acid) (PAAc) were synthesized by UV irradiation method, and their structure, crystallinity, swelling behavior, thermal property, and mechanical property were investigated. Chitosan/PAAc IPNs exhibited relatively high equilibrium water content and also showed reasonable sensitivity to pH. From the swelling behaviors at various pH's, Fourier transform infrared spectra at high temperature and thermal analysis confirmed the formation of polyelectrolyte complex due to the reaction between amino groups in chitosan and carboxyl groups in PAAc. For this reason, even at a swollen state, the present chitosan/PAAc IPNs possess good mechanical properties. Particularly, the CA‐2 sample (with a weight ratio of chitosan/PAAc = 50/50, molar ratio [NH₂]/[COOH] = 25/75) showed the lowest equilibrium water content and free water content, attributed to the more compact structure of the polyelectrolyte than CA‐1 or CA‐3 due to the high amount of interchain bond within the IPN. © 1999 John Wiley & Sons, Inc. J Appl Polym Sci 73: 113–120, 1999     

Bending of poly(vinyl alcohol)–poly(sodium acrylate) composite hydrogel in electric fields

Bending of poly(vinyl alcohol) hydrogel mixed with poly(sodium acrylate) chains, PVA–PAA gel, under the influence of dc electric fields was studied. The PVA–PAA gel was prepared by repeatedly freezing and thawing a mixture of PVA and polyacrylic acid aqueous solutions. The PVA–PAA gel was a hydrogel with the PAA chains, which were entangled with the PVA polymer network and were fixed in the gel. The PVA–PAA gel bent toward the negative electrode in electrolyte solutions under dc electric fields as did the polyelectrolyte gel with negatively charged polyions. The PVA gel, free of PAA, was insensitive to dc electric fields. The deflection of the bending and the bending speed were influenced by the filed intensity, the concentration of the polyion in the gel, and the thickness of the gel. The bending of the PVA–PAA gel was qualitatively explained by a bending theory of polyelectrolyte gel, based upon the change of the osmotic pressure due to the ion concentration difference between the inside and the outside of the gel.     

Indomethacin release behaviors from pH and thermoresponsive poly(vinyl alcohol) and poly(acrylic acid) IPN hydrogels for site-specific drug delivery

A temperature- and pH-responsive drug delivery system was studied by using interpenetrating polymer network (IPN) hydrogels constructed with poly(acrylic acid) (PAAc) and poly(vinyl alcohol) (PVA). The release of indomethacin incorporated into these hydrogels showed pulsatile patterns in response to both pH and temperature. Indomethacin diffused from the polymer matrices through the swelling and deswelling mechanism. The release amount increased at higher temperature because of the swelling caused by the dissociation of hydrogen bonding. The drastic change of drug release was achieved by alternating pH of the buffer solution and was attributed to the change of states of ionic groups within IPN hydrogels. The free water contents were calculated by using differential scanning calorimetry (DSC), and were proved to be the main factor in the swelling. These results demonstrated that the drug release could be controlled by the swelling/deswelling degree of IPN hydrogels as functions of pH and/or temperature. © 1997 John Wiley & Sons, Inc. J Appl Polm Sci 65: 685–693     

Bending behavior of hydrogels composed of poly(methacrylic acid) and alginate by electrical stimulus

Interpenetrating polymer networks (IPNs) prepared from poly(methacrylic acid) (PMAAc) and sodium alginate (SA) exhibited electrical sensitive behavior. The swelling behavior of the PMAAc/SA IPN hydrogel was studied by immersion of the gel into aqueous HCl solutions at various concentrations and into various pH buffer solutions, and their responses to electric fields were also investigated. When swollen IPN hydrogel was placed between a pair of electrodes it exhibited bending behavior on application of an electric field, and showed stepwise bending behavior depending on the magnitude of the electrical stimulus. Copyright © 2004 Society of Chemical Industry     

Preparation and characterization of polyacrylic acid‐poly(vinyl alcohol)‐based interpenetrating hydrogels

Some structural features of hydrogels from poly(acrylic acid) (PAAc) of various crosslinking degrees have been investigated through mechanical and swelling measurements. Interpenetrating polymer hydrogels (IPHs) of poly(vinyl alcohol) (PVA) and PAAc have been prepared by a sequential method: crosslinked PAAc chains were formed in aqueous solution by crosslinking copolymerization of acrylic acid and N,N‐methylenebisacrylamide in the presence of PVA. The application of freeze–thaw (F–T) cycles leads to the formation of a PVA hydrogel within the synthesized PAAc hydrogel. The swelling and viscoelastic properties of the IPHs were evaluated as a function of the content of crosslinker and the application of one F–T cycle. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 102: 5789–5794, 2006     

Swelling behavior of semi‐interpenetrating polymer network hydrogels composed of poly(vinyl alcohol) and poly(acrylamide‐co‐sodium methacrylate)

Interpenetrating polymer network (IPN) hydrogels based on poly(vinyl alcohol) (PVA) and poly(acrylamide‐co‐sodium methacrylate) poly(AAm‐co‐SMA) were prepared by the semi IPN method. These IPN hydrogels were prepared by polymerizing aqueous solution of acrylamide and sodium methacrylate, using ammonium persulphate/N,N,N¹,N¹‐tetramethylethylenediamine (APS/TMEDA) initiating system and N,N¹‐methylene‐bisacrylamide (MBA) as a crosslinker in the presence of a host polymer, poly(vinyl alcohol). The influence of reaction conditions, such as the concentration of PVA, sodium methacrylate, crosslinker, initiator, and reaction temperature, on the swelling behavior of these IPNs was investigated in detail. The results showed that the IPN hydrogels exhibited different swelling behavior as the reaction conditions varied. To verify the structural difference in the IPN hydrogels, scanning electron microscopy (SEM) was used to identify the morphological changes in the IPN as the concentration of crosslinker varied. In addition to MBA, two other crosslinkers were also employed in the preparation of IPNs to illustrate the difference in their swelling phenomena. The swelling kinetics, equilibrium water content, and water transport mechanism of all the IPN hydrogels were investigated. IPN hydrogels being ionic in nature, the swelling behavior was significantly affected by environmental conditions, such as temperature, ionic strength, and pH of the swelling medium. Further, their swelling behavior was also examined in different physiological bio‐fluids. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 98: 302–314, 2005     

Preparation of poly(vinyl alcohol)/poly(acrylic acid)/TiO2/carbon nanotube composite nanofibers and their photobleaching properties

The composite nanofibers of poly(vinyl alcohol) (PVA)/poly(acrylic acid) (PAAc)/titanium(IV) oxide (TiO₂) were prepared by electrospinning for a novel photocatalytic treatment of waste water. To improve the photoelectronic properties of PVA/PAAc/TiO₂ composite nanofibers, carbon nanotubes (CNTs) were used as an additive. The TiO₂ and CNTs were immobilized in the PVA/PAAc hydrogels as electrospun nanofibers for an easier recovery after the wastewater treatment. The improved efficiency of pollutant dye removal was observed at pH 10 due to the pH-sensitive swelling behavior of the PVA/PAAc/TiO₂/CNTs composite nanofibers. The photocatalytic activity of TiO₂ was improved noticeably by applying electric field to the CNTs-embedded composite nanofibers.     

Thermal characteristics of IPNs composed of poly(propylene glycol) and poly(acrylic acid)

Interpenetrating polymer networks (IPNs) based on poly(propylene glycol) (PPG) and poly(acrylic acid) (PAAc) were prepared by UV irradiation and characterized using fourier transform infrared (FTIR), differential scanning calorimetry (DSC), dielectric analysis (DEA), and thermogaravimetry (TGA). The glass transition temperatures (T_gs) of these IPNs exhibited a relatively higher temperature with an increased PAAc content. The decomposition temperature of PAAc is lower than that of PPG. PAAc affects the thermal stability of IPN more than PPG. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 88: 2570–2574, 2003     

Characteristics of electrical responsive chitosan/polyallylamine interpenetrating polymer network hydrogel

An interpenetrating polymer network (IPN) hydrogel composed of chitosan and polyallylamine exhibited electric‐sensitive behavior. The chitosan/polyallylamine IPN hydrogel was synthesized by radical polymerization using 2,2‐dimethoxy‐2‐phenylacetophenone (DMPAP) and methylene bisacrylicamide (MBAAm) as initiator and crosslinker, respectively. The swelling behavior of the IPN was studied by immersion of the gel samples in aqueous NaCl solutions at various concentrations and pHs. The swelling ratio decreased with increasing concentration and pH of electrolyte solution. The stimuli response of the IPN hydrogel in electric fields was also investigated. When a swollen the IPN was placed between a pair of electrodes, the IPN exhibited bending behavior in response to the applied electric field. The IPN also showed stepwise bending behavior depending on the electric stimulus. In addition, thermal properties of the IPN were investigated by differential scanning calorimetry (DSC) and dielectric analysis (DEA). © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 2290–2295, 2002     

Characterization of hydrogels based on chitosan and copolymer of poly(dimethylsiloxane) and poly(vinyl alcohol)

Copolymers composed of poly(vinyl alcohol) (PVA) and poly(dimethylsiloxane) (PDMS) were crosslinked with chitosan to prepare semi‐interpenetrating polymer network (IPN) hydrogels by an ultraviolet (UV) irradiation method for application as potential biomedical materials. PVA/PDMS copolymer and chitosan was cast to prepare hydrogel films, followed by a subsequent crosslinking with 2,2‐dimethoxy‐2‐phenylacetophenone as a nontoxic photoinitiator by UV irradiation. Various semi‐interpenetrating polymer networks (semi‐IPNs) were prepared from different weight ratios of chitosan and the copolymer of PVA/PDMS. Photocrosslinked hydrogels exhibited an equilibrium water content (EWC) in the range of 65–95%. Swelling behaviors of these hydrogels were studied by immersion of the gels in various buffer solutions. Particularly, the PCN13 as the highest chitosan weight ratio in semi‐IPN hydrogels showed the highest EWC in time‐dependent and pH‐dependent swelling. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 84: 2591–2596, 2002     

Electrical behavior of chitosan and poly(hydroxyethyl methacrylate) hydrogel in the contact system

Semi‐interpenetrating polymer networks (semi‐IPNs), as polymer hydrogels composed of chitosan and poly(hydroxyethyl methacrylate) (PHEMA), exhibiting electrical‐sensitive behavior, were prepared. The swelling behavior of the chitosan/PHEMA hydrogels was studied by immersing the gels in various concentrations of aqueous NaCl solution. The electrical responses of the semi‐IPN hydrogel, in applied electric fields, were also investigated. When the semi‐IPN hydrogels were swollen, where one electrode was placed in contact with the gel and the other fixed 30 mm apart from one, they exhibited bending behavior on the application of an electric field on a contact system. The electroresponsive behavior of the present semi‐IPN was also affected by the electrolyte concentration of the external solution. The semi‐IPN also showed various degrees of increased bending behavior depending on the electric stimulus. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 92: 915–919, 2004     

Synthesis and characterization of an interpenetrating polymer network composed of poly(methacrylic acid) and poly(vinyl alcohol)

Temperature and pH‐responsive interpenetrating polymer network (IPN) hydrogels, constructed with poly(methacrylic acid) (PMAA) and poly(vinyl alcohol) (PVA), by a sequential IPN method, were studied. The characterization of IPN hydrogels was investigated by Fourier‐transform infrared spectroscopy, differential scanning calorimetry (DSC) and swelling under various conditions. The IPN hydrogels exhibited relatively high swelling ratios, in the range 230–380 %, at 25 °C. The swelling ratios of the PMAA/PVA IPN hydrogels were pH and temperature dependent. DSC was used for the quantitative determination of the amounts of freezing and non‐freezing water. The amount of free water increased with increasing PMAA content in the IPN hydrogels. Copyright © 2004 Society of Chemical Industry     

Rapid swelling and deswelling of semi‐interpenetrating network poly(acrylic acid)/poly(aspartic acid) hydrogels prepared by freezing polymerization

Hydrogels with semi‐interpenetrating networks composed of poly(acrylic acid) (PAAc) and poly(aspartic acid) (PASP) have great potential for pharmaceutical and biomedical applications. In this study, we aimed to synthesize semi‐interpenetrating PAAc/PASP hydrogels with improved swelling–deswelling properties via two‐step polymerization, in which the first step of polymerization was performed at 37 °C for 15 min and the second step, the freezing polymerization, was performed at ?20 °C for 24 h. The synthesized hydrogels were characterized with field emission scanning electron microscopy, Fourier transform infrared spectroscopy, and thermogravimetric analysis. The swelling and deswelling behaviors of the hydrogels in response to the ionic strength of the buffer solution were investigated. The Schott's swelling kinetic model was used to elucidate the swelling behavior of the hydrogels. The swelling and deswelling rates of the hydrogels prepared via freezing polymerization were faster than those of the hydrogels prepared via conventional polymerization. This was attributed to the large mean pore size of the freeze‐polymerized hydrogels. The PAAc/PASP hydrogels that underwent freezing polymerization had better swelling–deswelling characteristics than the PAAc hydrogels. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43515.