Semi-interpenetrating Polymer Network Superporous Hydrogels Based on Poly(3-Sulfopropyl Acrylate,Potassium Salt) and Poly(Vinyl Alcohol): Synthesis and Characterization

Abstract

Semi-interpenetrating polymer network (semi-IPN) superporous hydrogels (SPHs) based on poly(3-sulfopropyl acrylate, potassium salt) (PSPA) and linear polymers were synthesized using poly(ethylene glycol) diacrylate (PEGDA) or N,N′-methylenebisacrylamide (BIS) as a crosslinker. The swelling ratio of SPHs was determined by measuring the weight of absorbed water; and the mechanical strength of swollen SPHs was evaluated using texture analyzer. Taguchi orthogonal experimental design [L9(3⁴)] was used to evaluate the influence of four factors, consisting of the ratios of 3-sulfopropyl acrylate (SPA) to PEGDA, to initiator, and to acrylic acid (AAc), and acidification of PSPASPHs, with each containing three levels on the swelling ratio and mechanical strength of semi-IPN PSPA-SPHs. Analysis of variance (ANOVA) of the experimental design results was carried out using a SAS program. The structure of SPHs was examined using a scanning electron microscope (SEM). Among the polymers evaluated, poly(vinyl alcohol) (PVA) was the best linear polymer to improve the mechanical strength of swollen SPHs. ANOVA indicated that the ratio of SPA to PEGDA and to an initiator, as well as acidification had significant effects on the swelling ratios of PSPA-SPHs. The ratio of SPA to AAc and acidification had significant effects on the mechanical strength, which deceased with increased swelling ratio and time. The optimized semi-IPN PSPA-SPH containing 5% w/w PVA had a swelling ratio 20 times greater within minutes and then up to 40 times. The mechanical strength was over 200 g/cm² for a fully swollen gel in a pH 1.2HCl medium. The optimal PSPA-SPH has swelling and mechanical properties suitable for development of gastro retentive drug delivery systems.

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References

1. Chen, J., Park, H. and Park, K. (1999). Synthesis of Superporous Hydrogels. Hydrogels with Fast Swelling and Superabsorbent Properties , J. Biomed. Mater. Res., 44(1): 53–62 .

2. Gutierrez-Rocca, J., Dunne, J. and Lally, M. (2002). A Release Pharmaceutical Construct Containing Acrylic Polymers for Gastric Retention, WO Patent 0,285,112.

3. Park, K., Chen, J. and Park, H. (2001). Superporous Hydrogel Composites: A New Generation of Hydrogels with Fast Swelling Kinetics, High Swelling Ratio and High Mechanical Strength, In: Ottenbrite, R.M. and Kim, S.W. (eds), Polymeric Drugs & Drug Delivery Systems, pp. 145–156, Technomic Publishing Co., Lancaster, PA .

4. Park, K., Chen, J. and Park, H. (2001). Hydrogel Composites and Superporous Hydrogel Composites having Fast Swelling, High Mechanical Strength, and Superabsorbent Properties, U.S. Patent 6,271,278.

5. Chen, J. and Park, K. (2000). Synthesis and Characterization of Superporous Hydrogel Composites , J. Controlled Rel., 65(1–2): 73–82 .

6. Langer, R.S., Elisseeff, J.H., Anseth, K. and Sims, D. (2001). Semiinterpenetrating or Interpenetrating Polymer Networks for Drug Delivery and Tissue Engineering, U.S. Patent 6,224,893.

7. Sperling, L.H. and Mishra, V. (1996). The Current Status of Interpenetrating Polymer Networks , Polym. Adv. Technol., 7(4): 197–208 .

8. Barrett, L.W., Sperling, L.H., Gilmer, J.W. and Mylonakis, S.G. (1994). Semi-interpenetrating Polymer Networks Composed of Poly(Ethylene Terephthalate) and Castor Oil. Synthesis, Structure, Physical Properties, and Crystallization , Adv. Chem. Ser., 239 (Interpenetrating Polymer Networks): 489–516 .

9. Khalid, M.N., Agnely, F., Yagoubi, N., Grossiord, J.L. and Couarraze, G. (2002). Water State Characterization, Swelling Behavior, Thermal and Mechanical Properties of Chitosan Based Networks , Eur. J. Pharm. Sci., 15(5): 425–432 .

10.

10. Amiji, M., Tailor, R., Ly, M.-K. and Goreham, J. (1997). Gelatin-Polyethylene Oxide Semi-interpenetrating Polymer Network with pH-Sensitive Swelling and Enzyme-degradable Properties for Oral Drug Delivery , Drug Dev. Ind. Pharm., 23(6): 575–582 .

11.

11. Burugapalli, K., Bhatia, D., Koul, V. and Choudhary, V. (2001). Interpenetrating Polymer Networks Based on Poly(Acrylic Acid) and Gelatin. I: Swelling and Thermal Behavior , J. Appl. Polym. Sci., 82(1): 217–227 .

12.

12. Dhara, D., Nisha, C.K. and Chatterji, P.R. (1999). Super Absorbent Hydrogels: Interpenetrating Networks of Poly(Acrylamide-co-Acrylic Acid) and Poly (Vinyl Alcohol): Swelling Behavior and Structural Parameters , J. Macromol. Sci. Pure Appl. Chem., A36(2): 197–210 .

13.

13. Zlatanic, A. and Petrovic, Z.S. (2001). Effect of Crosslinking on Swelling, Transitions and Mechanical Properties of Poly(N-Isopropylacrylamide) Responsive Hydrogels , Annual Technical Conference – Society of Plastics Engineers, 59(3): 3319–3323 .

14.

14. Buonguidi, M., Carelli, V., Di Colo, G., Nannipieri, E. and Serafini, M.F. (1997). Evaluation of a pH-Sensitive Semi-interpenetrating Polymer Network of Control of GI Drug Delivery , Int. J. Pharm., 147(1): 1–10 .

15.

15. Montgomery, D.C. (1997). Design and Analysis of Experiments, John Wiley & Sons, Inc., New York .

16.

16. Li, H., Zhang, W., Xu, W. and Zhang, X. (2000). Hydrogen Bonding Governs the Elastic Properties of Poly(Vinyl Alcohol) in Water: Singlemolecule Force Spectroscopic Studies of PVA by AFM Macromolecules, 33(2): 465–469 .

17.

17. Kibbe, A.H. (2000). Handbook of Pharmaceutical Excipients, 3rd edn, American Pharmaceutical Association and Pharmaceutical Press. Washington .

18.

18. Peppas, N.A., Bures, P., Leobandung, W. and Ichikawa, H. (2000). Hydrogels in Pharmaceutical Formulations , Eur. J. Pharm. Biopharm., 50(1): 27–46 .

19.

19. Lee, Y.M., Kim, S.H. and Cho, C.S. (1996). Synthesis and Swelling Characteristics of pH and Thermoresponsive Interpenetrating Polymer Network Hydrogel Composed of Poly(Vinyl Alcohol) and Poly(Acrylic Acid) , J. Appl. Polym. Sci., 62(2): 301–311 .

20.

20. Kim, S.Y. and Lee, Y.M. (1999). Drug Release Behavior of Electrical Responsive Poly(Vinyl Alcohol)/Poly(Acrylic Acid) IPN Hydrogels under an Electric Stimulus , J. Appl. Polym. Sci., 74(7): 1752–1761 .

21.

21. Byun, J., Lee, Y.M. and Cho, C.-S. (1996). Swelling of Thermosensitive Interpenetrating Polymer Networks Composed of Poly(Vinyl Alcohol) and Poly(Acrylic Acid) , J. Appl. Polym. Sci., 61(4): 697–702 .

22.

22. Kim, S.Y., Shin, H.S., Lee, Y.M. and Jeong, C.N. (1999). Properties of Electroresponsive Poly(Vinyl Alcohol)/Poly(Acrylic Acid) IPN Hydrogels Under an Electric Stimulus , J. Appl. Polym. Sci., 73(9): 1675–1683 .

23.

23. Hougton, L.A., Read, N.W., Heddle, R., Maddern, G.J., Downtown, J., Toouli, J. and Dent, J. (1988). Motor Activity of the Gastric Antrum, Pylorus, and Duodenum under Fasted Conditions and After Liquid Meal , Gastroenterology, 94(6): 1276–1284 .

24.

24. Hougton, L.A., Read, N.W., Heddle, R., Horowitz, M., Collins, P.J., Chatterton, B.B. and Dent, J. (1988). Relationship of the Motor Activity of the Antrum, Pylorus, and Duodenum to Gastric Emptying of a Solid–Liquid Mixed Meal , Gastroenterology, 94(6): 1285–1291 .

25.

25. Liaw, D.-J. and Huang, C.-C. (1996). Dilute Solution Properties of Anionic Poly(Potassium 3-Sulfopropylacrylate) , Polym. Int., 41(3): 267–276 .

26.

26. Zhou, Q.-Y., Zuo, J., Song, M.-D., Zhang, B.-H. and He, B.-L. (1998). Mechanical Property and Swelling Behavior of Semi-interpenetration Polymer Networks Based on Poly(Vinyl Alcohol) and Polyurethane , J. Appl. Polym. Sci., 67(3): 473–479 .

27.

27. Chen, J., Blevins, W.E., Park, H. and Park, K. (2000). Gastric Retention Properties of Superporous Hydrogel Composites , J. Controlled Rel., 64(1–3): 39–51 .

28.

28. Gemeinhart, R.A., Park, H. and Park, K. (2000). Effect of Compression on Fast Swelling of Poly(Acrylamide-co-Acrylic Acid) Superporous Hydrogels , J. Biomed. Mater. Res., 55(1): 54–62 .