Thermoresponsive hydrogels based on poly(N-isopropylacrylamide)/chondroitin sulfate

Centre for Bio-Artificial Muscle, Hanyang University, Seoul 133-791, Republic of Korea; Department of Biomedical Engineering, Hanyang University, Seoul 133-791, Republic of Korea; Department of Physiology, Seoul National University, Seoul 110-744, Republic of Korea
Sensors and Actuators B Chemical (Impact Factor: 3.84). 01/2008; DOI: 10.1016/j.snb.2008.09.001

ABSTRACT A fast, thermoresponsive hydrogel composed of poly(N-isopropylacrylamide) (PNIPAm) and chondroitin sulfate (ChS) was synthesized using precipitation polymerization. ChS was introduced to increase the water absorption of the PNIPAm hydrogel, and the precipitation polymerization method was used to induce a porous network morphology to enhance the thermal response of the hydrogel. PNIPAm/ChS hydrogels (15:7.5 wt.%) underwent a very fast deswelling, within a period of approximately 2 min, due to the presence of a large free water content (∼90–94%), which was associated with the interconnected filamentous morphology within the hydrogel. The swelling ratio was greatly enhanced by the addition of ChS. The hydrogels exhibited stable thermoactuation behavior, following a volume change of 75% while cycling the temperature between 20 and 45 °C.

  • [Show abstract] [Hide abstract]
    ABSTRACT: The poly(N,N-diethylacrylamide-co-(2-dimethylamino)ethyl methacrylate) (poly(DEA-co-DMAEMA)) macromonomers with three different chain lengths were prepared by telomerization of DEA and DMAEMA monomers with different ratios of the chain transfer agent, 2-mercaptoethanol. The number-average weight of three macromonomers determined by gel permeation chromatography of the terminal hydroxyl groups was 8355, 10,516 and 15,953, respectively. The comb-type grafted poly(DEA-co-DMAEMA) hydrogels having the different lengths of the grafted chains were synthesized in the presence of crosslinker. Equilibrium and dynamic swelling/deswelling properties of the prepared hydrogels responding to temperature and pH were investigated. Compared to normal-type hydrogel, the comb-type grafted hydrogels exhibited excellent variational values in response to an alternation of the temperature and pH. Moreover, the grafted hydrogels showed quite fast reswelling and deswelling behaviors in response to simultaneous dual temperature and pH stimuli. This is because that the introduction of side chains with freely mobile ends in the comb-type grafted hydrogels made the mobility of the networks increased. The responsive rates of the grafted hydrogels were also controlled by modifying the length of the grafted chains. The dual thermo- and pH-sensitive comb-type grafted poly(DEA-co-DMAEMA) hydrogels in this study may find various potential applications.
    Sensors and Actuators B-chemical - SENSOR ACTUATOR B-CHEM. 01/2010; 149(1):34-43.
  • Source
    [Show abstract] [Hide abstract]
    ABSTRACT: Nanostructured three-dimensional constructs combining layer-by-layer technology (LbL) and template leaching were processed and evaluated as possible support structures for cartilage tissue engineering. Multilayered constructs were formed by depositing the polyelectrolytes chitosan (CHT) and chondroitin sulphate (CS) on either bidimensional glass surfaces or 3D packet of paraffin spheres. 2D CHT/CS multi-layered constructs proved to support the attachment and proliferation of bovine chondrocytes (BCH). The technology was transposed to 3D level and CHT/CS multi-layered hierarchical scaffolds were retrieved after paraffin leaching. The obtained nanostructured 3D constructs had a high porosity and water uptake capacity of about 300%. Dynamical mechanical analysis (DMA) showed the viscoelastic nature of the scaffolds. Cellular tests were performed with the culture of BCH and multipotent bone marrow derived stromal cells (hMSCs) up to 21 days in chondrogenic differentiation media. Together with scanning electronic microscopy analysis, viability tests and DNA quantification, our results clearly showed that cells attached, proliferated and were metabolically active over the entire scaffold. Cartilaginous extracellular matrix (ECM) formation was further assessed and results showed that GAG secretion occurred indicating the maintenance of the chondrogenic phenotype and the chondrogenic differentiation of hMSCs.
    PLoS ONE 01/2013; 8(2):e55451. · 3.53 Impact Factor
  • [Show abstract] [Hide abstract]
    ABSTRACT: The goal of this work is to develop an injectable nucleus pulposus (NP) tissue engineering scaffold with the ability to form an adhesive interface with surrounding disc tissue. A family of in situ forming hydrogels based on poly(N-isopropylacrylamide)-graft-chondroitin sulfate (PNIPAAm-g-CS) were evaluated for their mechanical properties, bioadhesive strength, and cytocompatibility. It was shown experimentally and computationally with the Neo-hookean hyperelastic model that increasing the crosslink density and decreasing the CS concentration increased mechanical properties at 37 °C, generating several hydrogel formulations with unconfined compressive modulus values similar to what has been reported for the native NP. The adhesive tensile strength of PNIPAAm increased significantly with CS incorporation (p < 0.05), ranging from 0.4 to 1 kPa. Live/Dead and XTT assay results indicate that the copolymer is not cytotoxic to human embryonic kidney (HEK) 293 cells. Taken together, these data indicate the potential of PNIPAAm-g-CS to function as a scaffold for NP regeneration.
    Journal of Materials Science Materials in Medicine 01/2013; · 2.14 Impact Factor