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Preparation of poly(N-isopropylacrylamide) hydrogel beads by sedimentation polymerization combined with electrostatic atomization

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Abstract

The preparation of monodisperse, millimeter- or submillimeter-sized polymeric hydrogel beads by a novel production method combining sedimentation polymerization and electrostatic atomization is presented herein. The beads were prepared by drop-wise addition or spray of a pre-gel aqueous solution into silicone oil through a nozzle with application of high voltage, and subsequent free-radical polymerization of the pre-gel droplets during their descent. The thermosensitive poly(N-isopropylacrylamide) hydrogel that was used as the model hydrogel has attracted much attention for application in reaction and separation processes. The size of the pre-gel droplets dispensed from the tip of the nozzle corresponded to the size of the resultant hydrogel beads and was controlled by adjusting the applied voltage. The diameter of the pre-gel droplet was estimated from the equilibrium of forces caused by gravity, the electrostatic force, and the liquid–gas surface tension.

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References

  1. Ruckenstein E, Hong L (1995) Sedimentation polymerization. Polymer 36:2857–2860. doi:10.1016/0032-3861(95)93669-D

    Article  CAS  Google Scholar 

  2. Iizawa T, Ninomiya T, Gotoh T, Sakohara S (2004) Synthesis of porous poly(N-isopropylacrylamide) gel beads by sedimentation polymerization. Polym J 36:356–360. doi:10.1295/polymj.36.356

    Article  CAS  Google Scholar 

  3. Iizawa T, Taketa H, Maruta M, Ishido T, Gotoh T, Sakohara S (2007) Synthesis of porous poly(N-isopropylacrylamide) gel beads by sedimentation polymerization and their morphology. J Appl Polym Sci 104:104–842. doi:10.1002/app.25605

    Article  Google Scholar 

  4. Iizawa T, Ishido T, Gotoh T, Sakohara S (2007) Synthesis of nonporous poly(N-alkylacrylamide) gel beads by nonaqueous sedimentation polymerization. Polym J 39:18–20. doi:10.1295/polymj.PJ2006097

    Article  CAS  Google Scholar 

  5. Tokuyama H, Yazaki N (2010) Preparation of poly(N-isopropylacrylamide) hydrogel beads by circulation polymerization. React Funct Polym 70:967–971. doi:10.1016/j.reactfunctpolym.2010.10.004

    Article  CAS  Google Scholar 

  6. Tokuyama H, Yoshida T (2013) Emulsion gel beads prepared by sedimentation polymerization using two-fluid atomization and their Pd(II) ion adsorption properties. React Funct Polym 73:550–554. doi:10.1016/j.reactfunctpolym.2012.12.006

    Article  CAS  Google Scholar 

  7. Lenggoro IW, Okuyama K, Fernández Juan, de la Mora Tohge N (2000) Preparation of ZnS nanoparticles by electrospray pyrolysis. J Aerosol Sci 31:121–136. doi:10.1016/S0021-8502(99)00534-0

    Article  CAS  Google Scholar 

  8. Bugarski B, Amsden B, Goosen MFA, Neufeld RJ, Poncelet D (1994) Effect of electrode geometry and charge on the production of polymer microbeads by electrostatics. Can J Chem Eng 72:517–521. doi:10.1002/cjce.5450720318

    Article  CAS  Google Scholar 

  9. Fukui Y, Maruyama T, Iwamatsu Y, Fujii A, Tanaka T, Ohmukai Y, Matsuyama H (2010) Preparation of monodispersed polyelectrolyte microcapsules with high encapsulation efficiency by an electrospray technique. Colloids Surf A 370:28–34. doi:10.1016/j.colsurfa.2010.08.039

    Article  CAS  Google Scholar 

  10. Xie J, Wang CH (2007) Electrospray in the dripping mode for cell microencapsulation. J Colloid Interface Sci 312:247–255. doi:10.1016/j.jcis.2007.04.023

    Article  CAS  Google Scholar 

  11. Watanabe H, Matsuyama T, Yamamoto H (2001) Preparation of immobilized enzyme gel particles using an electrostatic atomization technique. Biochem Eng J 8:171–174. doi:10.1016/S1369-703X(01)00121-8

    Article  CAS  Google Scholar 

  12. Hogan CJ, Yun KM, Chen DR, Lenggoro IW, Biswas P, Okuyama K (2007) Controlled size polymer particle production via electrohydrodynamic atomization. Colloids Surf A 311:67–76. doi:10.1016/j.colsurfa.2007.05.072

    Article  CAS  Google Scholar 

  13. Zhou Y, Sun T, Chan M, Zhang J, Han Z, Wang X, Toh Y, Chen JP, Yu H (2005) Scalable encapsulation of hepatocytes by electrostatic spraying. J Biotechnol 117:99–109. doi:10.1016/j.jbiotec.2004.11.004

    Article  CAS  Google Scholar 

  14. Nyström M, Murtomaa M, Salonen J (2010) Fabrication and characterization of drug particles produced by electrospraying into reduced pressure. J Electrostat 68:42–48. doi:10.1016/j.elstat.2009.09.002

    Article  Google Scholar 

  15. Pan G, Kurumada K (2008) Hybrid gel reinforced with coating layer for removal of phenol from aqueous solution. Chem Eng J 138:94–199. doi:10.1016/j.cej.2007.06.025

    Article  Google Scholar 

  16. Morisada S, Namazuda K, Kanda H, Hirokawa Y, Nakano Y (2010) Temperature-swing adsorption of proteins in water using N-isopropylacrylamide copolymer gel particles. Adv Powder Technol 21:28–33. doi:10.1016/j.apt.2009.10.001

    Article  CAS  Google Scholar 

  17. Chen Z, Hua Z, Xu L, Huang Y, Zhao M, Li Y (2008) Protein-responsive imprinted polymers with specific shrinking and rebinding. J Mol Recognit 21:71–77. doi:10.1002/jmr.870

    Article  Google Scholar 

  18. Tokuyama H, Kanehara A (2007) Temperature swing adsorption of gold(III) ions on poly(N-isopropylacrylamide) gel. React Funct Polym 67:136–143. doi:10.1016/j.reactfunctpolym.2006.10.006

    Article  CAS  Google Scholar 

  19. Tokuyama H, Kanazawa R, Sakohara S (2005) Equilibrium and kinetics for temperature swing adsorption of a target metal on molecular imprinted thermosensitive gel adsorbents. Sep Purif Technol 44:152–159. doi:10.1016/j.seppur.2005.01.004

    Article  CAS  Google Scholar 

  20. Tokuyama H, Yanagawa K, Sakohara S (2006) Temperature swing adsorption of heavy metals on novel phosphate-type adsorbents using thermosensitive gels and/or polymers. Sep Purif Technol 50:8–14. doi:10.1016/j.seppur.2005.11.001

    Article  CAS  Google Scholar 

  21. Tokuyama H, Iwama T (2007) Temperature-swing solid-phase extraction of heavy metals on a poly(N-isopropylacrylamide) hydrogel. Langmuir 23:13104–13108. doi:10.1021/la701728n

    Article  CAS  Google Scholar 

  22. Kanazawa R, Sasaki A, Tokuyama H (2012) Preparation of dual temperature/pH-sensitive polyampholyte gels and investigation of their protein adsorption behaviors. Sep Purif Technol 96:26–32. doi:10.1016/j.seppur.2012.05.016

    Article  CAS  Google Scholar 

  23. Schachschal S, Adler HJ, Pich A, Wetzel S, Matura A, van Pee KH (2011) Encapsulation of enzymes in microgels by polymerization/cross-linking in aqueous droplets. Colloid Polym Sci 289:693–698. doi:10.1007/s00396-011-2392-1

    Article  CAS  Google Scholar 

  24. Chen JP, Chiu SH (2000) A poly(N-isopropylacrylamide-co-N-acryloxysuccinimide-co-2-hydroxyethyl methacrylate) composite hydrogel membrane for urease immobilization to enhance urea hydrolysis rate by temperature swing. Enzyme Microb Technol 26:359–367. doi:10.1016/S0141-0229(99)00181-7

    Article  CAS  Google Scholar 

  25. Tümtürk H, Karaca N, Demirel G, Şahin F (2007) Preparation and application of poly(N, N-dimethylacrylamide-co-acrylamide) and poly(N-isopropylacrylamide-co-acrylamide)/κ-Carrageenan hydrogels for immobilization of lipase. Int J Biol Macromol 40:281–285. doi:10.1016/j.ijbiomac.2006.07.004

    Article  Google Scholar 

  26. Kato N, Oishi A, Takahashi F (2000) Peptide synthesis catalyzed by α-chymotrypsin immobilized in the poly(N-isopropylacrylamide/acrylamide) gel. Mater Sci Eng C 13:109–116. doi:10.1016/S0928-4931(00)00184-3

    Article  Google Scholar 

  27. Milašinović N, Milosavljević N, Filipović J, Knežević-Jugović Z, Krušić MK (2010) Synthesis, characterization and application of poly(N-isopropylacrylamide-co-itaconic acid) hydrogels as supports for lipase immobilization. React Funct Polym 70:807–814. doi:10.1016/j.reactfunctpolym.2010.07.017

    Article  Google Scholar 

  28. DeShon WE, Carson RS (1968) Electric field investigations and a model for electrical liquid spraying. J Colloid Interface Sci 28:161–166. doi:10.1016/0021-9797(68)90218-X

    Article  Google Scholar 

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Acknowledgments

The authors wish to acknowledge the support of The Ogasawara Foundation for the Promotion of Science & Engineering.

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Correspondence to Hideaki Tokuyama.

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Tokuyama, H., Katsuno, A., Lenggoro, I.W. et al. Preparation of poly(N-isopropylacrylamide) hydrogel beads by sedimentation polymerization combined with electrostatic atomization. Polym. Bull. 72, 1603–1610 (2015). https://doi.org/10.1007/s00289-015-1359-7

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  • DOI: https://doi.org/10.1007/s00289-015-1359-7

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