Skip to main content

Advertisement

SpringerLink
Log in

Biomimetic remineralization of demineralized enamel with nano-complexes of phosphorylated chitosan and amorphous calcium phosphate

  • Published:
Journal of Materials Science: Materials in Medicine Aims and scope Submit manuscript

Abstract

Remineralization of enamel plays a crucial role in the progression of carious process and the management of early caries lesion. Based on the influence of phosphorylated proteins in biomineralization, the objective of this study was to synthesize nano-complexes of phosphorylated chitosan and amorphous calcium phosphate (Pchi–ACP), and evaluate their ability to remineralize enamel subsurface lesions in vitro. Pchi was synthesized using a previously established chemical method. The biomimetic remineralizing solution containing nano-complexes of Pchi–ACP was prepared by adding CaCl2 and K2HPO4 into Pchi–ACP solution (0.5 % w/v) in sequence. The final concentrations of calcium and phosphate ions were 10 and 6 mM, respectively. The nano-complexes of Pchi–ACP were characterized by Fourier-transform infrared (FTIR), X-ray diffraction (XRD), transmission electron microscopy (TEM), and selected area electron diffraction (SAED). During testing the enamel lesions were treated with Pchi–ACP and fluoridated remineralizing solutions, respectively. The remineralizing of enamel lesions was examined with field emission electron microscope (FE-SEM) and Micro-CT. ACP was stabilized by Pchi to form nano-complexes that were soluble in water. The size of Pchi–ACP nano-complexes particles was determined to be less than 50 nm. XRD and SAED results confirmed their amorphous phases. FE-SEM and Micro-CT results showed that the remineralizing effect of Pchi–ACP on enamel lesions was similar to that of fluoride. However, the remineralizing rate of Pchi–ACP treatment was significantly higher than that of fluoride treatment (P < 0.05). This study highlighted the potential of nanoparticles functionalized with a natural analogue involved in biomineralization, to remineralize early enamel caries.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10

Similar content being viewed by others

References

  1. Featherstone JDB. The science and practice of caries prevention. J Am Dent Assoc. 2000;131:887–99.

    Article  Google Scholar 

  2. Mount GJ, Ngo H. Minimal intervention: a new concept for operative dentistry. Quintessence Int. 2000;31:527–33.

    Google Scholar 

  3. Featherstone JDB. Fluoride, remineralization and root caries. Am J Dent. 1994;7:271–4.

    Google Scholar 

  4. ten Cate JM. Remineralization of deep enamel dentine caries lesions. Aust Dent J. 2008;53:281–5.

    Article  Google Scholar 

  5. ten Cate JM. Remineralization of caries lesions extend into dentine. J Dent Res. 2001;80:1407–11.

    Article  Google Scholar 

  6. Fomon SJ, Ekstrand J, Ziegler EE. Fluoride intake and prevalence of dental fluorosis: trends in fluoride intake with special attention to infants. J Public Health Dent. 2000;60(3):131–9.

    Article  Google Scholar 

  7. Arthur V. A window on biomineralization. Science. 2005;37:1419–20.

    Google Scholar 

  8. George A, Sabsay B, Simonian PA, Veis A. Characterization of a novel dentine matrix acidic phosphoprotein. Implications for induction of biomineralization. J Biol Chem. 1993;268:12624–30.

    Google Scholar 

  9. He G, Gajjeraman S, Schultz D, Cookson D, Qin C, Butler WT, Hao J, George A. Spatially and temporally controlled biomineralization is facilitated by interaction between self-assembled dentin matrix protein 1 and calcium phosphate nuclei in solution. Biochemistry. 2005;44:16140–8.

    Article  Google Scholar 

  10. George A, Arthur V. Phosphorylated proteins and control over apatite nucleation, crystal growth and inhibition. Chem Rev. 2008;108(11):4670–93.

    Article  Google Scholar 

  11. Gebauer D, Cölfen H. Prenucleation clusters and non-classical nucleation. Nano Today. 2011;6(6):564–84.

    Article  Google Scholar 

  12. Cross KJ, Huq NL, Reynolds EC. Casein phosphopeptides in oral health—chemistry and clinical applications. Curr Pharm Des. 2007;13:793–800.

    Article  Google Scholar 

  13. Reynolds EC. Remineralization of enamel subsurface lesions by casein phosphopeptide-stabilized calcium phosphate solutions. J Dent Res. 1997;76:1587–95.

    Article  Google Scholar 

  14. Burwell AK, Thula-Mata T, Gower LB, Habeliz S, Kurylo M, Ho SP, Chien YC, Cheng J, Cheng NF, Gransky SA, Marshall SJ, Marshall GW. Functional remineralization of dentin lesions using polymer-induced liquid-precursor process. PLoS ONE. 2012;7(6):e38852.

    Article  Google Scholar 

  15. Kim SK, Park PJ, Jung WK, Byun HG, Mendis E, Cho YI. Inhibitory activity of phosphorylated chitooligosaccharides on the formation of calcium phosphate. Carbohydr Polym. 2005;60(4):483–7.

    Article  Google Scholar 

  16. Wan Andrew CA, Khor E, Hastings GW. The influence of anionic chitin derivatives on calcium phosphate crystallization. Biomaterials. 1998;19(14):1309–16.

    Article  Google Scholar 

  17. Walsh LJ. Contemporary technologies for remineralization therapies: a review. Int Dent SA. 2009;4:34–46.

    Google Scholar 

  18. Rinaudo M. Chitin and chitosan: properties and applications. Prog Polym Sci. 2006;31:603–32.

    Article  Google Scholar 

  19. Hiroshi S, Shibasaki KI, Takashi M, Yoshinori T. Comparison of the activity of four chitosan derivatives in reducing initial adherence of oral bacterial onto tooth surface. Bull Tokyo Dent Coll. 2001;42(4):243–9.

    Article  Google Scholar 

  20. Hiroshi S, Shibasaki KI, Takashi M, Yoshinori T. Effect of rinsing with phosphorylated chitosan on four-day plaque regrowth. Bull Tokyo Dent Coll. 2001;42(4):251–6.

    Article  Google Scholar 

  21. Wang X, Ma J, Feng QL, Cui FZ. Skeletal repair in rabbits with calcium phosphate cements incorporated phosphorylated chitin. Biomaterials. 2002;23:4591–600.

    Article  Google Scholar 

  22. Jayakumar R, Rajkumar M, Fretias H, Selvamurgan N, Nair SV, Furuike T, Tamura H. Preparation of alginate/phosphorylated chitin blend films for tissue engineering and environmental applications. Int J Biol Macromol. 2009;44(1):107–11.

    Article  Google Scholar 

  23. Jayakumar R, Egawa T, Furuike T, Nair SV, Tamura H. Synthesis, characterization and thermal properties of phosphorylated chitin for biomedical applications. Polym Eng Sci. 2009;49(5):844–9.

    Article  Google Scholar 

  24. Jayakumar R, Nwe N, Tokura S, Tamura H. Sulfated chitin and chitosan as novel biomaterials. Int J Biol Macromol. 2007;40:175–81.

    Article  Google Scholar 

  25. Zhang X, Yang P, Yang WT, Chen JC. The bio-inspired approach to controllable biomimetic synthesis of silver nanoparticles in organic matrix of chitosan and silver-binding peptide (NPSSLFRYLPSD). Mater Sci Eng C. 2008;28:237–42.

    Article  Google Scholar 

  26. Zhang X, Neoh KG, Lin CC, Kishen A. Biomimetic deposition of calcium phosphate minerals on the surface of partially demineralized dentine modified with phosphorylated chitosan. J Biomed Mater Res B. 2011;98(1):150–9.

    Google Scholar 

  27. Sakairi N, Shirai A, Miyazaki S, Tashiro H, Tsuji Y, Kawahara H, Yoshida T, Tokura S. Synthesis and properties of chitin phosphate. Jpn J Polym Sci Technol. 1998;55:212–6.

    Google Scholar 

  28. Nishi N, Ebina A, Nishimura S, Tsutsumi A, Hasegawa O, Tokura S. Highly phosphorylated derivatives of chitin, partially deacetylated chitin and chitosan as new functional polymers: preparation and characterization. Int J Biol Macromol. 1986;8:311–7.

    Article  Google Scholar 

  29. Zhou H, Bhaduri S. Novel microwave synthesis of amorphous calcium phosphate nanospheres. J Biomed Mater Res B. 2012;100(4):1142–50.

    Article  Google Scholar 

  30. Liu Y, Li N, Qi Y, Niu LN, Elshafiy S, Mao J, Breschi L, Pashley DH, Tay FR. The use of sodium trimetaphosphate as a biomimetic analog of matrix phosphoproteins for remineralization of artificial caries-like dentin. Dent Mater. 2011;27(5):465–77.

    Article  Google Scholar 

  31. Amaral IF, Granja PL, Barbosa MA. Chemical modification of chitosan by phosphorylation: an XPS, FT-IR and SEM study. J Biomater Sci Polym Ed. 2005;12:1575–93.

    Article  Google Scholar 

  32. Jayakumar R, Nagahama H, Furuike T, Tamura H. Synthesis of phosphorylated chitosan by novel method and its characterization. Int J Biol Macromol. 2008;42(4):335–9.

    Article  Google Scholar 

  33. LeGeros RZ. Calcium phosphates in oral biology and medicine. In: Myers HM, editor. Monographs in oral science. Basel: Karger; 1991. p. 84.

    Google Scholar 

  34. Combes C, Rey C. Amorphous calcium phosphates: synthesis, properties and uses in biomaterials. Acta Biomater. 2010;6(9):3362–78.

    Article  Google Scholar 

  35. Li L, Pan H, Tao J, Xu X, Mao C, Gu X, Tang R. Repair of enamel by using hydroxyapatite nanoparticles as the building blocks. J Mater Chem. 2008;18(34):4079–84.

    Article  Google Scholar 

  36. Bodier-Houllé P, Steuer P, Meyer JM, Bigeard L, Cuisinier FJG. High-resolution electron-microscopic study of the relationship between human enamel and dentin crystals at the dentinoenamel junction. Cell Tissue Res. 2000;301(3):389–95.

    Article  Google Scholar 

  37. Skrtic D, Antonucci JM, Eanes ED, Brunworth RT. Silica-and zirconia-hybridized amorphous calcium phosphate: effect on transformation to hydroxyapatite. J Biomed Mater Res. 2002;59(4):597–604.

    Article  Google Scholar 

  38. Yang X, Wang L, Qin Y, Sun Z, Henneman ZJ, Moradian-Oldak J, Nancollas GH. How amelogenin orchestrates the organization of hierarchical elongated microstructures of apatite. J Phys Chem B. 2010;114(6):2293–300.

    Article  Google Scholar 

  39. Muzzarelli R, Mattioli-Belmonte TCBRM, Refioli G, Brunelli MA. Stimulatory effect on bone formation exerted by a modified chitosan. Biomaterials. 1994;15:1075–81.

    Article  Google Scholar 

Download references

Acknowledgments

This work was jointly supported by Tianjin Research Program of Application Foundation and Advanced Technology (Youth Research Program) (Grant No. 12JCQNJC09200), National Natural Science Foundation of China (Grant No. 81200817), National Basic Research Program of China (Grant No. 2012CB933900), National Science and Technology Support Project Foundation (2012BAI07B00).

Author information

Authors and Affiliations

  1. School of Dentistry, Hospital of Stomatology, Tianjin Medical University, 12 Observatory Road, Tianjin, 300070, People’s Republic of China

    Xu Zhang, Yanqiu Li, Xiaoxi Sun, Changhong Cong, Yinghui Wang & Mingyao Wu

  2. Discipline of Endodontics, Faculty of Dentistry, University of Toronto, 124 Edward Street, Toronto, ON, Canada

    Anil Kishen

  3. Department of Geriatric Dentistry, Peking University School and Hospital of Stomatology, Beijing, 100081, People’s Republic of China

    Xuliang Deng

  4. The Key Laboratory of Beijing City on Preparation and Processing of Novel Polymer, Beijing University of Chemical Technology, Beijing, 100029, People’s Republic of China

    Xiaoping Yang

  5. School of Energy and Environment Engineering, Hebei University of Technology, Tianjin, 300401, People’s Republic of China

    Huajun Wang

Authors
  1. Xu Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Yanqiu Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Xiaoxi Sun
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Anil Kishen
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Xuliang Deng
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Xiaoping Yang
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Huajun Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Changhong Cong
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Yinghui Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Mingyao Wu
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Xu Zhang.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, X., Li, Y., Sun, X. et al. Biomimetic remineralization of demineralized enamel with nano-complexes of phosphorylated chitosan and amorphous calcium phosphate. J Mater Sci: Mater Med 25, 2619–2628 (2014). https://doi.org/10.1007/s10856-014-5285-2

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10856-014-5285-2

Keywords

Search

Navigation