New Thermo-responsive Hydrogels Based on Poly (N-isopropylacrylamide)/ Hyaluronic Acid Semi-interpenetrated Polymer Networks: Swelling Properties and Drug Release Studies
Restricted accessResearch articleFirst published online March, 2010
New Thermo-responsive Hydrogels Based on Poly (N-isopropylacrylamide)/ Hyaluronic Acid Semi-interpenetrated Polymer Networks: Swelling Properties and Drug Release Studies
New pH and temperature sensitive semi-interpenetrated polymer networks (semi-IPNs) were developed by combining cross-linked PNIPAAm with hyaluronic acid (HA). At pH 7.4, the PNIPAAm/HA semi-IPN hydrogels had significantly greater and faster swelling at 25°C and a more complete deswelling at 37°C than PNIPAAm hydrogels. The temperature-dependent reversibility behavior was analyzed for biomaterial applications. Gentamicin was incorporated as a model drug, and the release profile from the hydrogels was followed under physiological conditions. The presence of HA, even in small quantities, allowed a more complete release of the gentamicin from the hydrogel. The PNIPAAm/HA semi-IPN hydrogels respond to both changes in temperature and pH making it suitable as a delivery system for therapeutics.
Mano, J.F. ( 2008). Stimuli-responsive Polymeric Systems for Biomedical Applications , Adv. Eng. Mater., 10: 515-527.
2.
Gupta, P., Vermani, K. and Garg, S. ( 2002). Hydrogels: From Controlled Release to pH-responsive Drug Delivery, Research focus, 7: 569-579.
3.
Schmaljohann, D. (2006). Thermo- and pH-responsive Polymers in Drug Delivery, Adv. Drug Deliv. Rev., 58: 1655-1670.
4.
Kulkarni, R.V. and Sa, B. (2009). Electroresponsive Polyacrylamide-Grafted-Xanthan Hydrogels for Drug Delivery, J. Bioact. Compat. Polym., 24: 368-384.
5.
Qiu, Y. and Park, K. ( 2001). Environmental-sensitive Hydrogels for Drug Delivery , Adv. Drug Deliv. Rev., 53: 321-339.
6.
Galaev, I.Y. and Mattiasson, B. (1999). ‘Smart’ Polymers and What They Could Do in Biotechnology and Medicine, Trends Biotechnol., 17: 335-340.
7.
Peppas, N.A. , Hilt, J.Z., Khademhosseini , A. and Langer, R. ( 2006). Hydrogels in Biology and Medicine: From Molecular Principles to Bionanotechnology , Adv. Mater., 18: 1345-1360.
8.
Jeong, B. and Gutowska, A. ( 2002). Lessons from Nature: Stimuli-responsive Polymers and their Biomedical Applications, Trends Biotechnol., 20: 305-311.
9.
Alarcón, C.H., Pennadam, S. and Alexander, C. (2005). Stimuli Responsive Polymers for Biomedical Applications, Chem. Society Rev., 34: 276-285.
10.
Ahn, S.-K. , Kasi, R.M., Kim , S.-C., Sharma, N. and Zhou, Y. (2008). Stimuli-responsive Polymer Gels, Soft Matter, 4: 1151-1157.
11.
Ruel-Gariépy, E. and Leroux, J.C. (2004). In Situ-forming Hydrogels-review of Temperature-sensitive Systems, Eur. J. Pharm. Biopharm. , 58: 409-426.
12.
Hsiue, G.H. , Hsu, S.H., Yang, C.C., Lee , S.H. and Yang, I.K. (2002). Preparation of Controlled Release Ophthalmic Drops, for Glaucoma Therapy Using Thermosensitive Poly-N-isopropylacrylamide , Biomaterials , 23: 457-462.
13.
Cho, J.H. , Kim, S.H., Park, K.D., Jung, M.C., Yang, W.I., Han , S.W. et al. (2004). Chondrogenic Differentiation of Human Mesenchymal Stem Cells Using a Thermosensitive Poly(N-isopropylacrylamide) and Water-soluble Chitosan Copolymer, Biomaterials, 25: 5743-5751.
14.
Reddy, T.T. , Kano, A., Maruyama , A., Hadano, M. and Takahara, A. (2008). Thermosensitive Transparent Semi-interpenetrating Polymer Networks for Wound Dressing and Cell Adhesion Control, Biomacromolecules, 9: 1313-1321.
15.
Rzaev, Z.M.O. , Dincer, S. and Piskin, E. (2007). Functional Copolymers of N-isopropylacrylamide for Bioengineering Applications, Prog. Polym. Sci., 32: 534-595.
16.
Shi, J. , Alves, N.M. and Mano, J.F. ( 2006). Drug Release of pH/ Temperature-responsive Calcium Alginate/Poly (N-isopropylacrylamide) Semi-IPN Beads, Macromol. Biosci. , 6: 358-363.
17.
Coughlan, D.C. , Quilty, F.P. and Corrigan, O.I. (2004). Effect of Drug Physicochemical Properties on Swelling/Deswelling Kinetics and Pulsatile Drug Release from Thermoresponsive Poly(N-Isopropylacrylamide) Hydrogels, J. Control. Release, 98: 97-114.
18.
Wu, J.Y. , Yang, Y.Y., Heng, P.W.S. and Moochala , S. ( 2003). Evaluating Protein Release and Interactions with Thermosensitive Hydrogels, Proc. Int. Symp. Control Release Bioact. Mater. , 30: 696-697.
19.
Zhang, X.-Z. , Zhuo, R.-X., Cui , C.-Z. and Zhang, J.-T. (2002). A Novel Thermo-responsive Drug Delivery System with Positive Controlled Release , Int. J. Pharm., 235: 43-50.
20.
Yoshida, R. , Uchida, K., Kaneko , Y., Sakai, K., Kikuchi, A., Sakurai, Y. et al. (1995 ). Comb-type Grafted Hydrogels with Rapid De-swelling Response to Temperature Changes, Nature, 374: 240-242.
21.
Gil, E.S. and Hudson, S.M. (2007). Effect of Silk Fibroin Interpenetrating Networks on Swelling/Deswelling Kinetics and Rheological Properties of Poly(N-Isopropylacrylamide) Hydrogels, Biomacromolecules , 8: 258.
22.
Yoshida, R. , Kaneko, Y., Sakai , K., Okano, T., Sakuri, Y., Bae , Y.H. et al. (1994). Positive Thermosensitive Pulsatile Drug Release Using Negative Thermosensitive Hydrogels, J. Control. Release, 32: 97-102.
23.
Yoshida, R. , Sakai, K., Okano , T. and Sakuri, Y. (1994). Modulating the Phase Transition Temperature and Thermosensitivity in N-Isopropylacrylamide Copolymers Gels, J. Biomater. Sci., Polym. Ed., 6: 585-598.
24.
Kikuchi, A. and Okano, T. (2002). Pulsatile Drug Release Control Using Hydrogels, Adv. Drug. Deliv. Rev. , 54: 53-77.
25.
Asoh, T., Kaneko, T., Matsusaki, M. and Akashi, M. ( 2006). Rapid Deswelling of Semi-IPNs with Nanosized Tracts in Response to pH and Temperature, J. Control. Release, 110: 387-394.
26.
Chaterji, S. , Kwon, K. and Park, K. (2007). Smart Polymeric Gels: Redefining the Limits of Biomedical Devices, Prog. Polym. Sci., 32: 1083-1122.
27.
Alvarez-Lorenzo, C., Concheiro, A., Dubovik , A.S., Grinberg, N.V., Burova, T.V. et al. (2005 ). Temperature-sensitive Chitosan-Poly(N-Isopropylacrylamide) Interpenetrated Networks with Enhanced Loading Capacity and Controlled Release Properties, J. Control. Release, 102: 629-641.
28.
Zhang, J.T. and Jandt, K.D. ( 2008). A Novel Approach to Prepare Porous Poly(N-Isopropylacrylamide) Hydrogel with Superfast Shrinking Kinetics, Macromol. Rap. Commun., 29: 593-597.
29.
Asoh, T., Kaneko, T., Matsusaki, M. and Akashi, M. ( 2006). Rapid Deswelling of Semi-IPNs with Nanosized Tracts in Response to pH and Temperature, J. Control. Release, 110: 387-394.
30.
Klumb, L.A. and Horbett, T.A. ( 1992). Design of Insulin Delivery Devices Based on Glucose Sensitive Membranes, J. Control. Release, 18: 59-80.
31.
Mano, J.F., Silva, G.A., Azevedo, H.S., Malafaya, P.B., Sousa, R.A., Silva, S.S. et al. (2007). Natural Biodegradable Systems in Tissue Engineering and Regenerative Medicine: Present Status and Some Moving Trends, J. Royal Soc. Interfaces, 4: 999-1030.
32.
Allison, D.D. and Grande-Allen , K.J. (2006). Hyaluronan: A Powerful Tissue Engineering Tool, Rev. Tissue Eng., 12: 2131-2140.
33.
Wei, Z. and Cuie, Y. (2006). Hyaluronic Acid and its Derivatives as Drug Carriers, Prog. Chem., 18: 1684-1690.
34.
Prestwich, G.D. (2008). Engineering a Clinically-useful Matrix for Cell Therapy, Organogenesis, 4: 42-47.
35.
Slevin, M., Krupinski, J., Gaffney, J., Matou, S., Delisser, H.Savini, R.C. et al. (2007). Hyaluronan-mediated Angiogenesis in Vascular Disease: Uncovering RHAM and CD44 Receptor Signaling Pathways, Matrix Biology, 26: 58-68.
36.
Ibrahim, S. and Ramamurthi, A. (2008). Hyaluronic Acid Cues for Functional Endothelialization of Vascular Constructs, J. Tissue Eng. Regen. Med., 2: 22-32.
37.
Collier, J.H. , Camp, J.P., Hudson, T.W. and Schmidt, C.E. (2000). Synthesis and Characterization of Polypyrrole-Hyaluronic Acid Composite Biomaterials for Tissue Engineering Applications, J. Biomed. Mater. Res. , 50: 574-584.
38.
Cao, G.Y. , Savani, R.C., Fehrenbach, M., Lyons, C., Zhang, L., Coukos, G. et al. (2006 ). Involvement of Endothelial CD44 during In Vivo Angiogenesis , Am. J. Pathol. , 169: 325-336.
39.
Peattie, R.A. , Rieke, E.R., Hewet, E.M., Fisher, R.J., Shu , X.Z. and Prestwich , G.D. (2006). Dual Growth Factor-induced Angiogenesis In Vivo Using Hyaluronan Hydrogel Implants, Biomaterials, 27: 1868-1875.
40.
Cabanillas, P.F., Pena, E.D., Barrales-Rienda , J.M. and Frutos, G. ( 2000). Validation and In Vitro Characterization of Antibiotic-loaded Bone Cement Release, Int. J. Pharm., 209: 15-26.
41.
Temtem, M., Casimiro, T., Mano, J.F. and Aguiar-Ricardo, A. ( 2007). Green Synthesis of a Temperature Sensitive Hydrogel , Green Chem., 9: 75-79.
42.
Shi, J. , Alves, N.M. and Mano, J.F. (2008). Chitosan Coated Alginate Beads Containing Poly(N-Isoprpylacrylamide) for Dual-Stimuli-Responsive Drug Release, J. Biomed. Mater. Res. Part B - Appl. Biomater. , 84B: 595-603.
43.
Shi, J. , Liu, L., Sun, X., Cao, S. and Mano, J.F. ( 2008). Biomineralized Polysaccharide Beads for Dual-Stimuli-Responsive Drug Delivery, J. Macromol. Biosci., 8: 260-267.
44.
Zhang, J., Guo, R., Yang, M., Jiang, X. and Liu, B. ( 2007). Thermo And Ph Dual-Responsive Nanoparticles For Anti-Cancer Drug Delivery, Adv. Mater., 19: 2988-2992.
45.
Guo, B.-L. and Gao, Q.-Y. (2007). Preparation and Properties of a pHTemperature-Responsive Carboxymethyl Chitosan/Poly(N-Isopropylacrylamide) Semi-IPN Hydrogel for Oral Delivery of Drugs, Carbohydrate Res., 342: 2416- 2422.
46.
Zhang, J.-T. , Bhat, R. and Jandt, K.D. ( 2009). Temperature-sensitive PVA/ PNIPAAm Semi-IPN Hydrogels with Enhanced Responsive Properties, Acta Biomaterialia, 5: 488-497.
