Siloxane-poly(lactic acid)-vaterite composites with 3D cotton-like structure

  • Toshihiro Kasuga
  • Akiko Obata
  • Hirotaka Maeda
  • Yoshio Ota
  • Xianfeng Yao
  • Kazuya Oribe


Trace amounts of ionic calcium and silicon species have been reported to stimulate the proliferation, differentiation, and mineralization of bone-forming cells. Composite materials comprising siloxane-doped calcium carbonate (vaterite) particles and poly(l-lactic acid) have been developed [siloxane-poly(lactic acid)-vaterite hybrid-composite, SiPVH] so far; they were designed such that calcium and silicate ions are gradually released from SiPVH and they show the chronic effects of ions on cellular activities. In the present work, SiPVH with a 3D cotton-like structure was prepared by electrospinning to obtain the major advantages of excellent bioactivity and ease of handling for bone filling surgery. The diameter of the fibrous skeletons that form structure of the cotton-like SiPVH was controlled to ~10 μm to achieve cellular migration into the spaces between fibers. The resulting cotton-like SiPVH showed good flexibility. The fiber surface was coated rapidly with numerous particles of several hundred nanometers in size by alternate soaking in CaCl2 and Na2HPO4. The treated cotton-like material, which released calcium and silicate ions gradually, showed good cellular migration behavior into the 3D structure in cell culture tests using murine osteoblast-like MC3T3-E1 cells.


PLLA Vaterite Amorphous Calcium Phosphate Electrospinning Method Sodium Hydrogen Phosphate 
These keywords were added by machine and not by the authors. This process is experimental and the keywords may be updated as the learning algorithm improves.



The present work was supported in part by Grants-in-Aid for Scientific Research from the Japan Society for the Promotion of Science (Nos. 20390497 and 21700487) and a grant from Institute of Ceramics Research and Education, NITech.


  1. 1.
    Hench LL, Polak JM. Third generation biomedical materials. Science. 2002;295:1014–7.CrossRefGoogle Scholar
  2. 2.
    Kenny SM, Buggy M. Bone cements and fillers: a review. J Mater Sci Mater Med. 2003;14:923–38.CrossRefGoogle Scholar
  3. 3.
    Rezwan K, Chen QZ, Blaker JJ, Boccaccini AR. Biodegradable and bioactive porous polymer/inorganic composite scaffolds for bone tissue engineering. Biomater. 2006;27:3413–31.CrossRefGoogle Scholar
  4. 4.
    Pietrzak WS, Ronk R. Calcium sulfate bone void filler: a review and a look ahead. J Craniofacial Surg. 2000;11:327–33.CrossRefGoogle Scholar
  5. 5.
    Jones JR, Ehrenfried LM, Hench LL. Optimising bioactive glass scaffolds for bone tissue engineering. Biomater. 2006;27:964–73.CrossRefGoogle Scholar
  6. 6.
    Xynos ID, Edgar AJ, Buttery LDK, Hench LL, Polak JM. Ionic products of bioactive glass dissolution increase proliferation of human osteoblasts and induce insulin-like growth factor II mRNA expression and protein synthesis. Biochem Biophys Res Comm. 2000;276:461–5.CrossRefGoogle Scholar
  7. 7.
    Gough JE, Jones JR, Hench LL. Nodule formation and mineralization of human primary osteoblasts cultured on a porous bioactive glass scaffold. Biomater. 2004;25:2039–46.CrossRefGoogle Scholar
  8. 8.
    Jones JR, Tsigkou O, Coates EE, Stevens MM, Polak JM, Hench LL. Extracellular matrix formation and mineralization on a phosphate-free porous bioactive glass scaffold using primary human osteoblast (HOB) cells. Biomater. 2007;28:1653–63.CrossRefGoogle Scholar
  9. 9.
    Maeda H, Kasuga T, Hench LL. Preparation of poly(l-lactic acid)-polysiloxane-calcium carbonate hybrid membranes for guided bone regeneration. Biomater. 2006;27:1216–22.CrossRefGoogle Scholar
  10. 10.
    Maeda H, Kasuga T. Control of silicon species released from poly(lactic acid)-polysiloxane hybrid membranes. J Biomed Mater Res. 2008;85A:742–6.CrossRefGoogle Scholar
  11. 11.
    Maeda H, Kasuga T. Preparation of poly(lactic acid) composite hollow spheres containing calcium carbonates. Acta Biomater. 2006;2:403–8.CrossRefGoogle Scholar
  12. 12.
    Obata A, Kasuga T. Cellular compatibility of bone-like apatite containing silicon species. J Biomed Mater Res. 2008;85A:140–4.CrossRefGoogle Scholar
  13. 13.
    Obata A, Kasuga T. Stimulation of human mesenchymal stem cells and osteoblasts activities in vitro on silicon-releasable scaffolds. J Biomed Mater Res. 2009;91A:11–7.CrossRefGoogle Scholar
  14. 14.
    Obata A, Tokuda S, Kasuga T. Enhanced in vitro cell activity on silicon-doped vaterite/poly(lactic acid) composites. Acta Biomater. 2009;5:57–62.CrossRefGoogle Scholar
  15. 15.
    Obata A, Hotta T, Wakita T, Ota Y, Kasuga T. Electrospun microfiber meshes of silicon-doped vaterite/poly(lactic acid) hybrid for guided bone regeneration. Acta Biomater. 2010;6:1248–57.CrossRefGoogle Scholar
  16. 16.
    Wakita T, Obata A, Poologasundarampillai G, Jones JR, Kasuga T. Preparation of electrospun siloxane-poly(lactic acid)-vaterite hybrid fibrous membranes for guided bone regeneration. Compos Sci Technol. 2010;70:1889–93.CrossRefGoogle Scholar
  17. 17.
    Nakamura J, Maeda H, Obata A, Kasuga T. Private Communication, Structure of siloxane-containing vaterite particles and their dissolution behavior. In: Preprints of 24th Fall Meeting of The Ceramic Society of Japan. Tokyo: The Ceramic Society of Japan: 2011. p. 10 (1A27).Google Scholar
  18. 18.
    Wakita T, Nakamura J, Ota Y, Obata A, Kasuga T, Ban S. Effect of preparation route on the degradation behavior and ion releasability of siloxane-poly(lactic acid)-vaterite hybrid nonwoven fabrics for guided bone regeneration. Dental Mater J. 2011;30:232–8.CrossRefGoogle Scholar
  19. 19.
    Wakita T, Obata A, Kasuga T. New fabrication process of layered membranes based on poly(lactic acid) fibers for guided bone regeneration. Mater Trans. 2009;50:1737–41.CrossRefGoogle Scholar
  20. 20.
    Takeuchi N, Machigashira M, Yamashita D, Shirakata Y, Kasuga T, Noguchi K, Ban S. Cellular compatibility of a gamma-irradiated modified siloxane-poly(lactic acid)-calcium carbonate hybrid membrane for guided bone regeneration. Dental Mater J. in press.Google Scholar
  21. 21.
    Juhasz JA, Best SM, Brooks R, Kawashita M, Miyata N, Kokubo T, Nakamura T, Bonfield W. Mechanical properties of glass-ceramic A-W-polyethylene composites: effect of filler content and particle. Biomater. 2004;25:949–55.CrossRefGoogle Scholar
  22. 22.
    Zeng C, Zhang J, Zeng Y, Chen X, Yan Y. A new technique for preparation of porous bioceramics with controllable macrostructures. Clay Miner. 2009;44:411–6.CrossRefGoogle Scholar
  23. 23.
    Ogomi D, Serizawa T, Akashi M. Bioinspired organic–inorganic composite materials prepared by an alternate soaking process as a tissue reconstitution matrix. J Biomed Mater Res. 2003;67A:1360–6.CrossRefGoogle Scholar
  24. 24.
    Liang D, Hsiao BS, Chu B. Functional electrospun nanofibrous scaffolds for biomedical applications. Adv Drug Delivery Rev. 2007;59:1392–412.CrossRefGoogle Scholar
  25. 25.
    Li WJ, Laurencin CT, Caterson EJ, Tuan RS, Ko FK. Electrospun nanofibrous structure: a novel scaffold for tissue engineering. J Biomed Mater Res. 2002;60:613–21.CrossRefGoogle Scholar
  26. 26.
    Zhang YZ, Su B, Venugopal J, Ramakrishna S, Lim CT. Biomimetic and bioactive nanofibrous scaffolds from electrospun composite nanofibers. Int J Nanomedicine. 2007;2:623–38.Google Scholar
  27. 27.
    Fujikura K, Obata A, Lin S, Jones JR, Law RV, Kasuga T. Preparation of electrospun poly(lactic acid)-based hybrids containing siloxane-doped vaterite particles for bone regeneration, J Biomater Sci. in press (doi: 10.1163/092050611X582867).
  28. 28.
    Schneider OD, Loher S, Brunner TJ, Uebersax L, Simonet M, Grass RN, Merkle HP, Stark WJ. Cotton wool-like nanocomposite biomaterials prepared by electrospinning: in vitro bioactivity and osteogenic differentiation of human mesenchymal stem cells. J Biomed Mater Res B Appl Biomater. 2008;84B:350–62.CrossRefGoogle Scholar
  29. 29.
    Fujikura K, Obata A, Kasuga T. Cellular migration to electrospun poly(lactic acid) fibermats. J Biomater Sci. in press (doi: 10.1163/092050611X599328).
  30. 30.
    Huang ZM, Zhang YZ, Kotakic M, Ramakrishna S. A review on polymer nanofibers by electrospinning and their applications in nanocomposites. Compos Sci Technol. 2003;63:2223–53.CrossRefGoogle Scholar
  31. 31.
    Kim GT, Lee JS, Shin JH, Ahn YC, Hwang YJ, Shin HS, Lee JK, Sung CM. Investigation of pore formation for polystyrene electrospun fiber: effect of relative humidity. Korean J Chem Eng. 2005;22:783–8.CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media, LLC 2012

Authors and Affiliations

  • Toshihiro Kasuga
    • 1
  • Akiko Obata
    • 1
  • Hirotaka Maeda
    • 2
  • Yoshio Ota
    • 3
  • Xianfeng Yao
    • 3
  • Kazuya Oribe
    • 3
  1. 1.Department of Frontier MaterialsNagoya Institute of TechnologyNagoyaJapan
  2. 2.Center for Fostering Young and Innovative ResearchersNagoya Institute of TechnologyNagoyaJapan
  3. 3.Orthorebirth Co., LtdYokohamaJapan

Personalised recommendations