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1.
Intra‐articular drug delivery is the preferred approach for targeting pharmacologic treatment directly at the joints to reduce undesirable side effects associated with systemic drug delivery. In this study, a controlled delivery system of methotrexate (MTX) based on injectable thermosensitive poly(ε‐caprolactone)‐poly(ethylene glycol)‐poly(ε‐caprolactone) (PCL‐PEG‐PCL, PEP) hydrogels was developed for the intra‐articular drug delivery. The thermosensitive PEP copolymers were prepared by ring‐opening polymerization. The synthesized PEP copolymers were characterized for their structure, composition, and the sol‐to‐gel transition. The in vitro MTX release from the PEP hydrogels was studied. MTX plasma concentration following intra‐articular injection into healthy rats was determined by HPLC. Biocompatibility was confirmed by histology analysis after the intra‐articular injection. The synthesized PEP copolymers aqueous solutions formed in situ gel rapidly after the injection. PEP hydrogels showed the ability to control the release of incorporated MTX. Following intra‐articular injection, the PEP hydrogels decreased the clearance rate of MTX in the joint cavity. The maximum plasma concentrations of MTX in rats injected with free MTX were threefold higher than that of the groups injected with MTX hydrogels. These results suggest that the intra‐articular delivery of the PEP hydrogels may be a viable strategy for the controlled release of drugs for treating arthritis diseases. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011  相似文献   

2.
To design efficient polymeric supports for lipase immobilization, two series of hydrogels based on acrylamide and three methacrylates were prepared via crosslinking with ethylene glycol methacrylate and N,N‐methylenebisacrylamide. The three methacrylates used to prepare these hydrogels had different alkyl chain lengths: C1 (methyl methacrylate), C12 (dodecyl methacrylate), and C18 (octadecyl methacrylate). In the reaction scheme, only the feed concentration of the hydrophobic component (methacrylate) was varied. The characterization of the hydrogels was carried out with Fourier transform infrared, scanning electron microscopy, and nitrogen analysis to establish their structural aspects and to obtain evidence for network formation; the swelling and water uptake of the hydrogels were studied as functions of the time, temperature, and pH. Lipase immobilization on selected hydrogels was studied as a function of the concentration of the methacrylate used in the feed and the nature of the crosslinker. The activity of the hydrogel series that showed the highest activity of the immobilized lipase was investigated further as a function of the methacrylate feed concentration, pH, and temperature. Some organic solvents were studied to investigate the effect of the nature of the solvent on the activity of the immobilized lipase. The activity of the immobilized lipase was more than that of the free lipase and was affected by the structural attributes of the polymeric supports and by the nature of the solvent. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci 2007  相似文献   

3.
ABSTRACT

Hydrogels based on acrylamide (AAM) and potassium methacrylate (KMA) were synthesized by simultaneous free radical polymerization in aqueous solution using the redox initiator ammonium persulfate (APS) and N,N,N′N′-tetramethylethylenediamine (TMEDA) at room temperature. Eight different compositions of KMA hydrogels were prepared at a fixed concentration of N,N′,-methylenebisacrylamide (MBA) or diallyl phthalate (DP) as crosslinking agents. For all the AAM-KMA hydrogels, the percentage of swelling, swelling kinetics, and diffusion characteristics were investigated. It was found that higher swelling percentage values were obtained for hydrogels crosslinked with DP than for the conventional crosslinker MBA. The de-swelling characteristics of hydrogels were also studied in detail. The power law relationship of hydrogels was evaluated in saline solutions. Hydrogels formation was confirmed by IR spectroscopy. The thermal characteristics of these hydrogels were studied by using differential scanning calorimeter (DSC) and thermogravimetric analyzer (TGA) and revealed that MBA crosslinked AAM-KMA hydrogels show higher glass transition temperature (Tg) as well as higher decomposition temperatures (Td) than DP crosslinked AAM-KMA hydrogels. It is further confirmed from the studies that the DP crosslinked hydrogels have good swelling as well as de-swelling and salinity characteristics.  相似文献   

4.
Different from the conventional method of developing stimuli‐sensitive textiles by graft copolymerization of environmental responsive polymers onto the fabric, the coating technique was applied to bond temperature‐sensitive hydrogels with cotton fabric through chemical covalent in our work. A temperature‐sensitive linear copolymer of Ntert‐butylacrylamide (NTBA) and acrylamide (AAm) was prepared in methanol. Then, the cotton fabrics were coated using an aqueous solution of this copolymer containing 1,2,3,4‐butanetertracarboxylic acid as a crosslinker and sodium hypophosphite (SHP) as a catalyst, followed by drying and curing. The surface of the cotton fabrics was bonded on more or less coatings of poly (NTBA‐co‐AAm) hydrogels, as verified by Fourier transform infrared spectroscopy and scanning electron microscopy images. The poly(NTBA‐co‐AAm) hydrogels‐coated fabrics exhibited temperature sensitive, and the temperature interval of the deswelling transition was higher than lower critical solution temperature of linear copolymer solution. The coated fabrics presented good water‐impermeable ability because of the swelling of hydrogels bonded, especially when the add‐on was as high as 14.14%. Environmental scanning electron microscopy images revealed that coating hydrogels swelled and covered on the surface as a barrier to prevent water from penetrating once the coated fabric came into contact with water. The findings demonstrate that the temperature‐sensitive hydrogels can be covalently bonded on the cotton fabrics by coating technique and the coated fabrics have potential on immersion fabrics. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009  相似文献   

5.
Thermosensitive hydrogels were prepared by free radical polymerization in aqueous solution from N‐isopropylacrylamide (NIPA) monomer and N,N‐methylenebis(acrylamide) (MBAAm) crosslinker. The swelling equilibrium of the hydrogels in deionized water was investigated as a function of temperature and MBAAm content. The results indicated that the swelling behavior and temperature sensitivity of the hydrogels were affected by the amount of MBAAm content. The average molecular mass between crosslinks and polymer–solvent interaction parameter (χ) of the hydrogels were determined from equilibrium swelling values. The swelling variations were explained according to swelling theory based on the hydrogel chemical structure. The swelling equilibrium of the hydrogels was also investigated as a function of temperature in aqueous solutions of the anionic surfactant sodium dodecyl sulfate (SDS) and the cationic surfactant dodecyltrimethylammonium bromide (DTAB). In deionized water, the hydrogels showed a discontinuous volume phase transition at 32°C. In SDS and DTAB solutions, the equilibrium swelling ratio and the volume phase transition temperature (lower critical solution temperature) of the hydrogels increased, which is ascribed to the conversion of nonionic PNIPA hydrogel into polyelectrolyte hydrogels because of binding of surfactant molecules through the hydrophobic interaction. Additionally, the amount of free SDS and DTAB ions was measured at different temperatures by a conductometric method; it was found that the electric conductivity of the PNIPA–surfactant systems depended strongly on both the type and concentration of surfactant solutions. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 101: 1756–1762, 2006  相似文献   

6.
The effect of annealing on the impact strength of PP/poly(ethylene-co-propylene) (PEP) and PP/PEP/PE blends was studied with regard to the structure of PEP and the polyethylene crystallinity. The tensile impact strength of annealed blends was remarkably affected by the PEP structure such as molecular weight and comonomer composition and the annealing temperature, while the brittle temperature was scarcely affected. For the PP/PEP/PE blends, annealing at temperatures above the melting point of PE lowers the tensile impact strength in a similar manner as the PP/crystalline PEP blend. These phenomena were explained on the basis of the deformation mechanism presented in the previous article, that is, a thicker interfacial layer of PP and PEP forms by means of annealing to increase the energy needed to deform the interface. By using a scanning electron microscope, the transition layer was observed at the interface between amorphous PEP and PE in the PP/amorphous PEP/PE blend after etching with nitric acid. The formation of a thicker transition layer between amorphous PEP and PE and a sizeable increase in PE particle size by annealing was observed. The phenomena should be correlated with the impact sensitivity, especially tensile impact strength, in the PP/crystalline PEP and PP/amorphous PEP/PE blends. A reasonable explanation of the microstructure in PP/PEP blends has been developed in terms of comonomer composition and melting property of PEP.  相似文献   

7.
Polylactic acid (PLA)/pearlescent pigments (PEPs) composites were fabricated by melt blending method and their properties were studied using a rotational rheometry, field emission scanning electron microscopy (FESEM), differential scanning calorimetry (DSC) and X-ray diffractometry (XRD). Because PEP could disperse uniformly in PLA matrix and would form PEP networks, there were improvements made in the flexural strength, tensile strength and impact strength of PLA composites. Interestingly, the viscosity of PLA composites reduced significantly as compared with neat PLA, indicating an improvement in processing properties. The rheological tests confirmed that the storage modulus of PLA composites decreased as PEP content increased at a given frequency. Also, there was a plateau at low frequency range, which was a sign of PEP networks formation. The DMA tests showed that the storage modulus of PLA composite increased with PEP content, suggesting the enhancement of rigidity. According to the XRD results, no change was observed in the crystal structure of PLA in the presence of PEP. The addition of PEP did not change melting temperature, but the glass transition temperature increased a little, and the cold crystallization temperature of PLA decreased largely. The DSC results also showed that nucleation ability of PLA was enhanced by addition of PEP at low cooling rates, but the whole crystallization process of PLA in composite was inhibited at higher cooling rates. This conclusion was also confirmed by the results of crystallization kinetics.  相似文献   

8.
This paper comprises the characterization of superabsorbent hydrogels based on methacrylated cashew gum (CGMA) co-polymerized with acrylamide (AAm) by measuring of the water uptake, water retention capacity in dependence of time, morphological and mechanical properties. The morphological features of hydrogels were evidenced by SEM images. Stress measurements of hydrogels as a function of temperature were considered as being the necessary force for compressing the hydrogels at 1 mm deformation. Stress-strain modeling was used to obtain the compressive elastic modulus and apparent cross-linking density of superabsorbent hydrogels. Hydrolyzed CGMA-co-AAm hydrogels showed highly water absorbing. Another remarkably feature of these hydrogels is the efficiency in the water retaining that was caused by increasing in CGMA content. Higher temperature leads to an enhancement in the stress values of superabsorbent hydrogels because the large content of water that penetrates into superabsorbent hydrogels and expands their polymer network. The increase in the amount of CGMA and AAm were accompanied by an increasing on the apparent cross-linking density of hydrogels. This contributed to increase their elastic modulus, which is inherent to a more rigid structure.  相似文献   

9.
Novel intelligent hydrogels composed of biodegradable and pH-sensitive poly(l-glutamic acid) (PGA) and temperature sensitive poly(N-isopropylacrylamide-co-2-hydroxyethyl methacrylate) (PNH) were synthesized and characterized for controlled release of hydrophilic drug. The influence of pH on the equilibrium swelling ratios of the hydrogels was investigated. A higher PNH content resulted in lower equilibrium swelling ratios. Although temperature had little influence on the swelling behaviors of the hydrogels, the changes of optical transmittance of hydrogels as a function of temperature were marked, which showed that the PNH part of hydrogel exhibited hydrophobic property at temperature above the lower critical solution temperature (LCST). The biodegradation rate of the stimuli-sensitive hydrogels in the presence of enzyme was directly proportional to the PGA content. Lysozyme was chosen as a model drug and loaded into the hydrogels. The in vitro drug release experiment was carried out at different pH values and the release data suggested that both the pH and PNH content played important roles in the drug release behaviors of the hydrogels.  相似文献   

10.
Using N, N′‐methylene bisacrylamide as crosslinking agent and potassium peroxydisulfate as initiator, the temperature‐sensitive hydrogels were prepared with organic monomer N‐isopropylacrylamide (NIPAAm) and acrylic amide and inorganic material ethyl orthosilicate (TEOS). The structure of hybrid hydrogels was represented by scanning electron microscopy and Fourier transform infrared spectroscopy. The volume phase transition temperature (VPTT) of hybrid hydrogels was determined by differential scanning calorimetry thermograms of the swollen hydrogel. The results showed that the VPTT of the hydrogels increased with the increasing of TEOS dosage. When the temperature was lower than VPTT, the hydrogels exhibited excellent temperature sensitivity and kept at a swelling state, but when the temperature was higher than VPTT, the hydrogels deswelled significantly. In addition, the compressive strength of hydrogels was studied, the results showed that hybrid hydrogels had more ideal mechanical properties than organic hydrogels. © 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013  相似文献   

11.
pH‐ and temperature‐responsive semi‐interpenetrating nanocomposite hydrogels (NC hydrogels) were prepared with surface‐functionalized graphene oxide (GO) as the crosslinker, N‐isopropylacrylamide (NIPAM) as the monomer, and chitosan (CS) as an additive. The effects of 3‐(trimethoxysilyl)propylmethacrylate‐modified GO sheets and CS content on various physical properties were investigated. Results show that PNIPAM/CS/GO hydrogels undergo a large volumetric change in response to temperature. Swelling ratios of PNIPAM/CS/GO hydrogels are much larger than those of the conventional organically crosslinked PNIPAM hydrogels. The deswelling test indicates that the deswelling rate was greatly enhanced by incorporating CS into the hydrogel network and using the surface‐functionalized GO as the crosslinker. The pH‐sensitivity of PNIPAM/CS/GO hydrogels is evident below their volume phase transition temperature. Moreover, the PNIPAM/CS/GO hydrogels have a much better mechanical property compared with traditional hydrogels even in a high water content of 90%. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41530.  相似文献   

12.
Hydrophobic poly(N‐[3‐(dimethylaminopropyl)]methacrylamide‐co‐lauryl acrylate) [P(DMAPMA‐co‐LA)] hydrogels with different LA content were synthesized by free‐radical crosslinking copolymerization of corresponding monomers in water by using N,N‐methylenebis(acrylamide) as the crosslinker, ammonium persulfate as the initiator, and N,N,N′,N′‐tetramethylethylenediamine as the activator. The swelling equilibrium of the hydrogels was investigated as a function of temperature and hydrophobic comonomer content in pure water. An interesting feature of the swelling behavior of the P(DMAPMA‐co‐LA) hydrogels with low LA content was the reshrinking phase transition where the hydrogels swell once and collapse as temperature was varied in the range of 30–40°C. The average molecular mass between crosslinks (M?c) and polymer–solvent interaction parameter (χ) of the hydrogels were calculated from equilibrium swelling values. The enthalpy (ΔH) and entropy (ΔS) changes appearing in the χ parameter for the hydrogels were determined by using the Flory–Rehner theory based on the phantom network model of swelling equilibrium. The positive values for ΔH and ΔS indicated that the hydrogels had a positive temperature‐sensitive property in water, that is, swelling at a higher temperature and shrinking at a lower temperature. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 101: 4159–4166, 2006  相似文献   

13.
A series of copolymeric hydrogels comprising of acrylic acid and acrylamide and crosslinked with trimethylolpropane triacrylate (TMPTA) were prepared using ammonium persulfate (APS) as initiator. The hydrogels were functionalized further by partial hydrolysis and were characterized by SEM, FTIR, nitrogen analysis, and also by water uptake studies as a function of time, temperature, pH, NaCl, and concentration of sodium dodecyl sulfate (SDS). These hydrogels were used as sorbents for the uranyl ions uptake in the presence of 5% NaCl, which was studied as function of time, temperature, pH, and ion strength. The uranyl uptake was found to be affected both by the structural aspects of the hydrogels as well as by the external environmental factors. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008  相似文献   

14.
Thermosensitive hydrogels were prepared by free radical polymerization starting from a methacrylated pullulan derivative (acting as the cross-linker) and using N-isopropylacrylamide (NIPAAM) as the monomer. Several hydrogels were obtained by changing the monomer to cross-linker ratio. A significant thermosensitivity was observed only when the molar amount of NIPAAM incorporated in the network was at least eight times higher that of methacrylate groups on pullulan. The hydrogel with high amount of NIPAAM deswells more than 80% after the T-jump. The lower critical solution temperature of thermosensitive hydrogels decreases with increasing amount of NIPAAM. The mechanical properties of the hydrogels are strongly affected by the percentage of incorporated NIPAAM and by the temperature.  相似文献   

15.
In this study, pH‐ and temperature‐responsive hydrogels based on linear sodium alginate (SA) and crosslinked poly(N‐isopropylacrylamide) (PNIPAAm) were prepared by semi‐interpenetrating network (semi‐IPN) technique. The dually responsive hydrogels were characterized by FTIR, DSC, and SEM, and their temperature‐ and pH‐responsive behaviors were investigated by measuring equilibrium swelling ratios and pulsatile swelling experiments. The results showed that these hydrogels underwent volume phase transition at around 33°C irrespective of the pH value of the medium, but their pH sensitivity was evident only below their volume phase transition temperature. Under basic conditions, the swelling ratios of SA/PNIPAAm semi‐IPN hydrogels were greater than that of pure PNIPAAm hydrogel and increased with increasing SA content incorporated into the hydrogels, but the case was inverse under acidic conditions. The pulsatile swelling experiments indicated that the higher the SA content in SA/PNIPAAm semi‐IPN hydrogels, the faster the response rate to both pH and temperature change. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 97: 1931–1940, 2005  相似文献   

16.
Poly(vinyl alcohol)/poly(N‐vinyl pyrrolidone) (PVP)/chitosan hydrogels were prepared by a low‐temperature treatment and subsequent 60Co γ‐ray irradiation and then were medicated with ciprofloxacin lactate (an antibiotic) and chitosan oligomer (molecular weight = 3000 g/mol). The gel content, swelling ratio, tensile strength, and crystallinity of the hydrogels were determined. The effects of the chitosan molecular weight, the low‐temperature treatment procedure, and the radiation dosage on the hydrogel properties were examined. The molecular weight of chitosan was lowered by the irradiation, but its basic polysaccharide structure was not destroyed. Repeating the low‐temperature treatment and γ‐ray irradiation caused effective physical crosslinking and chemical crosslinking, respectively, and contributed to the mechanical strength of the final hydrogels. The incorporation of PVP and chitosan resulted in a significant improvement in the equilibrium swelling ratio and elongation ratio of the prepared hydrogels. The ciprofloxacin lactate and chitosan oligomer were soaked into the hydrogels. Their in vitro release behaviors were examined, and they were found to follow diffusion‐controlled kinetics. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 101: 2453–2463, 2006  相似文献   

17.
A new strategy was developed to prepare thermo‐ and pH‐sensitive hydrogels by the crosslinking of poly(N‐isopropylacrylamide) with a biodegradable crosslinker derived from poly(L ‐glutamic acid). Hydrogels were fabricated by exposing aqueous solutions of precursor containing photoinitiator to UV light irradiation. The swelling behaviors of hydrogels at different temperatures, pHs, and ionic strengths were examined. The hydrogels shrank under acidic condition or at temperature above their collapse temperature and would swell in neutral or basic media or at lower temperature. These processes were reversible as the pH or temperature changed. All hydrogels exhibited no weight loss in the simulated gastric fluid but degraded rapidly in the simulated intestinal condition. Bovine serum albumin were used as a model protein drug and loaded into the hydrogels. The in vitro drug release experiment was carried out at different pH values and temperatures. The pH and temperature dependent release behaviors indicated the promising application of these materials as stimuli‐responsive drug delivery vehicles. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012  相似文献   

18.
pH‐ and temperature‐responsive interpenetrating polymer network (IPN) hydrogels based on soy protein and poly(N‐isopropylacrylamide‐co‐sodium acrylate) were successfully prepared. The structure and properties of the hydrogels were characterized by Fourier transform infrared spectroscopy, scanning electron microscopy, differential scanning calorimetry, and thermogravimetric analyzer. The equilibrium and dynamic swelling/deswelling behaviors and the drug release properties of the hydrogels responding to pH and/or temperature were also studied in detail. The hydrogels have the porous honeycomb structures, good miscibility and thermal stability, and good pH‐ and temperature‐responsivity. The volume phase transition temperature of the hydrogels is ca. 40°C. Changing the soy protein or crosslinker content could be used to control the swelling behavior and water retention, and the hydrogels have the fastest deswelling rate in pH 1.2 buffer solutions at 45°C. Bovine serum albumin release from the hydrogels has the good pH and temperature dependence. The results show that the proposed IPN hydrogels may have potential applications in the field of biomedical materials such as in drug delivery systems. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 39781.  相似文献   

19.
BACKGROUND: This paper focuses on the development of temperature induced phase transition hydrogels based on poly(N‐isopropylocrylamide (PNIPA) copolymers and their application as an immobilization matrix for biocatalysts. RESULTS: PNIPA‐co‐AAc and PNIPA‐co‐MAAc hydrogels were synthesized with different comonomer concentrations and analysed. In order to evaluate the capacity of hydrogels to take up or to release liquids the mass exchange capacity is introduced. In the presented work mass exchange capacities up to 22.4 were realized. To enhance the mechanical stability, composites of hydrogels and cellulosic fleeces were prepared. The enzyme Lipozyme ® TL 100 L (Thermomyces languniosa Lipase) was successfully inserted into the hydrogels and into the hydrogel composites. Lipase‐catalysed transesterification of rapeseed oil with ethanol to the corresponding ethyl ester was investigated to prove the activity of immobilized enzyme and thus, the concept. The activity was found to be similar to that of free enzyme. CONCLUSION: Smart hydrogel composites were used for the transesterification of oil. Based on the results obtained, reversible loadable and mechanical stable hydrogel composites could be developed for continuous working reactor concepts. Copyright © 2010 Society of Chemical Industry  相似文献   

20.
pH‐ and temperature‐responsive double network hydrogels (DN hydrogels) were prepared by using poly (N‐isopropylacrylamide) (PNIPAM) as a tightly crosslinked network (1st network), polyacrylic acid (PAA) as a loosely crosslinked network (2nd network), with clay and graphene oxide as effective crosslinkers and reinforcing fillers. The structure and morphology of the hydrogels were characterized by SEM, FTIR, DSC, and TGA. The synergetic effects of clay, GO and DN structure on various physical properties were investigated. With the increasing of crosslinking densities, the swelling ratios of DN hydrogels gradually decreased by increasing the contents of graphene oxide and PAA. While the DN hydrogels had much better mechanical properties than that of the conventional chemically cross‐linked PNIPAM hydrogels. POLYM. ENG. SCI., 55:1361–1366, 2015. © 2015 Society of Plastics Engineers  相似文献   

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