Skip to main content

Advertisement

Log in

Hydroxyapatite−loaded starch/polyvinyl alcohol scaffold for bone regeneration application: preparation and characterization

  • Original Paper: Sol-gel and hybrid materials for biological and health (medical) applications
  • Published:
Journal of Sol-Gel Science and Technology Aims and scope Submit manuscript

Abstract

Hydroxyapatite (HA) embedded in polymer-based bone scaffold exhibits excellent medical properties for bone healing. Indeed, limited studies have reported on the addition of HA into starch/polyvinyl alcohol (PVA) scaffold system, especially HA role as bio-additive releasing Ca2+ ion promoting biomineralization. Herein, HA derived from chicken bone with the particles size ranging from 100 to 600 nm loaded starch/PVA composite scaffold with different amount was fabricated using a salt-leaching method. XRD and SEM-EDS analysis indicated the presence of HA in starch/PVA composite. FTIR results showed that the chemical bondings in starch/PVA matrices were not affected by the introduction of HA. Morphology and architecture of scaffolds characterized by SEM demonstrated pore size and their structure satisfying the needs of bone scaffolds. Young modulus of composite scaffold increased with the increase of HA loading content. The Ca2+ release analyzed by ion chromatography system showed the increasing trend with amount of HA addition into scaffold, which improved mineralization of composite scaffold in in-vitro observed by SEM-EDS. HA-loaded starch/PVA scaffold demonstrated a similar biodegradation rate and amount to the starch/ PVA scaffold. According to the result, loading starch/PVA with HA can be proposed a potential candidate for bone regeneration.

Graphical Abstract

Highlights

  • HA-loaded starch/PVA scaffolds prepared by salt leaching method showed high porous structure with porosity ranging from 85.2 to 90.3%, interconnected pores and wide range of pore size (up to 500 µm for large pore).

  • Calcium ion release from HA increased with the HA content in composite scaffolds.

  • HA acted as a bio-additive accelerating the formation of hydroxyapatite precursor in the surface during the incubation in the SBF solution.

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

Access this article

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

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Similar content being viewed by others

References

  1. Amini AR, Laurencin CT, Nukavarapu SP (2012) Bone tissue engineering: recent advances and challenges. Crit Rev Biomed Eng 40(5):363–408

    Article  Google Scholar 

  2. Roseti L, Parisi V, Petretta M, Cavallo C, Desando G, Bartolotti I, Grigolo B (2017) Scaffolds for bone tissue engineering: State of the art and new perspectives. Mater Sci Eng C 78:1246–1262

    Article  CAS  Google Scholar 

  3. Le TDH, Liaudanskaya V, Bonani W, Migliares C, Motta A (2020) Diatom Particles: A Promising Osteoinductive Agent of Silk Fibroin-Based Scaffold for Bone Regeneration. IFMBE Proceedings 69. Springer, Singapore, p 147–151

    Google Scholar 

  4. Pati F, Song TH, Rijal G, Jang J, Kim WS, Cho DW (2015) Ornamenting 3D printed scaffolds with cell-laid extracellular matrix for bone tissue regeneration. Biomaterials 37:230–241

    Article  CAS  Google Scholar 

  5. Blaker JJ, Maquet V, Jérôme R, Boccaccini AR, Nazhat SN (2005) Mechanical properties of highly porous PDLLA/Bioglass composite foams as scaffolds for bone tissue engineering. Acta Biomater 1(6):643–652

    Article  CAS  Google Scholar 

  6. Olszta MJ, Cheng X, Jee SS, Kumar R, Kim YY, Kaufman MJ, Douglas EP, Gower LB (2007) Bone structure and formation: A new perspective. Mater Sci Eng R Rep. 58(3–5):77–116

    Article  Google Scholar 

  7. Thorwarth M, Schultze-Mosgau S, Kessler P, Wiltfang J, Schlegel KA (2005) Bone regeneration in osseous defects using a resorbable nanoparticular hydroxyapatite. J Oral Maxillofac Surg 63(11):1626–1633

    Article  Google Scholar 

  8. Fang J, Li P, Lu X, Fang L, Lü X, Ren F (2019) A strong, tough, and osteoconductive hydroxyapatite mineralized polyacrylamide/dextran hydrogel for bone tissue regeneration. Acta Biomater 88:503–513

    Article  CAS  Google Scholar 

  9. Lew D, Farrell B, Bardach J, Keller J (1997) Repair of craniofacial defects with hydroxyapatite cement. J Oral Maxillofac Surg 55(12):1441–1449

    Article  CAS  Google Scholar 

  10. Ratnayake JTB, Mucalo M, Dias GJ (2017) Substituted hydroxyapatites for bone regeneration: A review of current trends. J Biomed Mater Res - Part B Appl Biomater 105(5):1285–1299

    Article  CAS  Google Scholar 

  11. Darimont GL, Cloots R, Heinen E, Seidel L, Legrand R (2002) In vivo behaviour of hydroxyapatite coatings on titanium implants: A quantitative study in the rabbit. Biomaterials 23(12):2569–2575

    Article  CAS  Google Scholar 

  12. Kattimani VS, Kondaka S, Lingamaneni KP (2016) Hydroxyapatite–Past, Present, and Future in Bone Regeneration. Bone Tissue Regen Insights 7:9–18

    Google Scholar 

  13. Caria PHF, Kawachi EY, Bertran CA, Camilli JA (2007) Biological assessment of porous-implant hydroxyapatite combined with periosteal grafting in maxillary defects. J Oral Maxillofac Surg 65(5):847–854

    Article  Google Scholar 

  14. Huang X, Bai S, Lu Q, Liu X, Liu S, Zhu H (2015) Osteoinductive-nanoscaled silk/HA composite scaffolds for bone tissue engineering application. J Biomed Mater Res - Part B Appl Biomater 103(7):1402–1414

    Article  CAS  Google Scholar 

  15. Hallman M, Driscoll JA, Lubbe R, Jeon S, Chang K, Haleem M, Jakus A, Pahapill R, Yun C, Shah R, Hsu WK, Stock SR, Hsu EL (2021) Influence of geometry and architecture on the in vivo success of 3D-printed scaffolds for spinal. Fusion Tissue Eng - Part A 27(1–2):26–36

    Article  CAS  Google Scholar 

  16. Jin P, Liu L, Cheng L, Chen X, Xi S, Jiang T (2023) Calcium-to-phosphorus releasing ratio affects osteoinductivity and osteoconductivity of calcium phosphate bioceramics in bone tissue engineering. Biomed Eng Online 22(1):1–16

    Article  Google Scholar 

  17. Meagher MJ, Weiss-Bilka HE, Best ME, Boerckel JD, Wagner DR, Roeder RK (2016) Acellular hydroxyapatite-collagen scaffolds support angiogenesis and osteogenic gene expression in an ectopic murine model: Effects of hydroxyapatite volume fraction. J Biomed Mater Res—Part A 104(9):2178–2188

    Article  CAS  Google Scholar 

  18. Ielo I, Calabrese G, De Luca G, Conoci S (2022) Recent advances in hydroxyapatite-based biocomposites for bone tissue regeneration in orthopedics. Int J Mol Sci 23:17

    Article  Google Scholar 

  19. Hasegawa S, Tamura J, Neo M, Shikinami Y, Saito M, Kita M, Nakamura T (2005) In vivo evaluation of a porous hydroxyapatite/poly-DL-lactide composite for use as a bone substitute. J Biomed Mater Res—Part A 75(3):567–579

    Article  Google Scholar 

  20. Martin V, Ribeiro IA, Alves MM, Gonçalves L, Claudio RA, Grenho L, Fernandes MH, Gomes P, Santos CF, Bettencourt AF (2019) Engineering a multifunctional 3D-printed PLA-collagen-minocycline-nanoHydroxyapatite scaffold with combined antimicrobial and osteogenic effects for bone regeneration. Mater Sci Eng C 101:15–26

    Article  CAS  Google Scholar 

  21. Wang Y, Guo Y, Wei Q, Li X, Ji K, Zhang K (2021) Current researches on design and manufacture of biopolymer-based osteochondral biomimetic scaffolds. Bio-Des Manuf 4(3):541–567

    Article  Google Scholar 

  22. Gao X, Xu Z, Li S, Cheng L, Xu D, Li L, Chen L, Xu Y, Liu Z, Liu Y, Sun J (2023) Chitosan-vancomycin hydrogel incorporated bone repair scaffold based on staggered orthogonal structure: a viable dually controlled drug delivery system. RSC Adv 13(6):3759–3765

    Article  Google Scholar 

  23. Saboktakin MR, Akhyari S, Nasirov FA (2014) Synthesis and characterization of modified starch/polybutadiene as novel transdermal drug delivery system. Int J Biol Macromol 69:442–446

    Article  CAS  Google Scholar 

  24. Marto J, Ribeiro H M, Almeida A J(2020) Starch-based nanocapsules as drug carriers for topical drug delivery Smart Nanocontainers: Micro Nano Technol 1:287–294

    Article  Google Scholar 

  25. Marto JM, Gouveia LF, Gonçalves LMD, Ribeiro HM, Almeida AJ (2018) Design of minocycline-containing starch nanocapsules for topical delivery. J Microencapsul 35(4):344–356

    Article  CAS  Google Scholar 

  26. Santander-Ortega MJ, Stauner T, Loretz B, Ortega-Vinuesa JL, Bastos-González D, Wenz G, Schaefer UF, Lehr CM (2010) Nanoparticles made from novel starch derivatives for transdermal drug delivery. J Control Release 141(1):85–92

    Article  CAS  Google Scholar 

  27. Mohammad DM, Stiharu I (2022) Preparing and characterizing novel biodegradable starch/PVA-based films with nano-sized zinc-oxide particles for wound-dressing applications. Appl Sci 12:4001

    Article  Google Scholar 

  28. Rodrigues AI, Gomes ME, Leonor IB, Reis RL (2012) Bioactive starch-based scaffolds and human adipose stem cells are a good combination for bone tissue engineering. Acta Biomater 8(10):3765–3776

    Article  CAS  Google Scholar 

  29. Shahriarpanah S, Nourmohammadi J, Amoabediny G (2016) Fabrication and characterization of carboxylated starch-chitosan bioactive scaffold for bone regeneration. Int J Biol Macromol 93:1069–1078

    Article  CAS  Google Scholar 

  30. Manavitehrani I, Fathi A, Wang Y, Maitz PK, Mirmohseni F, Cheng TL, Peacock L, Little DG, Schindeler A, Dehghani F (2017) Fabrication of a biodegradable implant with tunable characteristics for bone implant applications. Biomacromolecules 18(6):1736–1746

    Article  CAS  Google Scholar 

  31. Taherimehr M, Bagheri R, Taherimehr M (2021) In-vitro evaluation of thermoplastic starch/beta-tricalcium phosphate nano-biocomposite in bone tissue engineering. Ceram Int 47(11):15458–15463

    Article  CAS  Google Scholar 

  32. Lu DR, Xiao CM, Xu SJ (2009) Starch-based completely biodegradable polymer materials. Express Polym Lett 3(6):366–375

    Article  CAS  Google Scholar 

  33. Hsieh W, Liau J (2013) Cell culture and characterization of cross-linked poly (vinyl alcohol) -g-starch 3D scaffold for tissue engineering. Carbohydr Polym 98(1):574–580

    Article  CAS  Google Scholar 

  34. Mirab F, Eslamian M, Bagheri R (2018) Fabrication and characterization of a starch-based nanocomposite scaffold with highly porous and gradient structure for bone tissue engineering. Biomed Phys Eng Express 4:055021

    Article  Google Scholar 

  35. Ramesh S, Loo ZZ, Tan CY, Chew WJ, Ching YC, Tarlochan F, Chandran H, Krishnasamy S, Bang LT, Sarhan AAD (2018) Characterization of biogenic hydroxyapatite derived from animal bones for biomedical applications. Ceram Int 44(9):10525–10530

    Article  CAS  Google Scholar 

  36. Trinh KS, Dang TB (2019) Structural, physicochemical, and functional properties of electrolyzed cassava starch. Int J Food Sci 2019:1–8

    Article  Google Scholar 

  37. Kokubo T, Takadama H (2006) How useful is SBF in predicting in vivo bone bioactivity? Biomaterials 27(15):2907–2915

    Article  CAS  Google Scholar 

  38. Bee SL, Hamid ZAA (2019) Characterization of chicken bone waste-derived hydroxyapatite and its functionality on chitosan membrane for guided bone regeneration. Compos Part B Eng 163:562–573

    Article  CAS  Google Scholar 

  39. Pramanik S, Agarwala P, Vasudevan K, Sarkar K (2020) Human-lymphocyte cell friendly starch–hydroxyapatite biodegradable composites: Hydrophilic mechanism, mechanical, and structural impact. J Appl Polym Sci 137(30):1–11

    Article  Google Scholar 

  40. Gomaa MM, Hugenschmidt C, Dickmann M, Abdel-Hady EE, Mohamed HFM, Abdel-Hamed MO (2018) Crosslinked PVA/SSA proton exchange membranes: Correlation between physiochemical properties and free volume determined by positron annihilation spectroscopy. Phys Chem Chem Phys 20(44):28287–28299

    Article  CAS  Google Scholar 

  41. Abdullah AHD, Chalimah S, Primadona I, Hanantyo MHG (2018) Physical and chemical properties of corn, cassava, and potato starchs. IOP Conf Ser Earth Environ Sci 160(1):2003

    Google Scholar 

  42. Salgado AJ, Coutinho OP, Reis RL (2004) Bone tissue engineering: State of the art and future trends. Macromol Biosci 4(8):743–765

    Article  CAS  Google Scholar 

  43. Karageorgiou V, Kaplan D (2005) Porosity of 3D biomaterial scaffolds and osteogenesis. Biomaterials 26:5474–5491

    Article  CAS  Google Scholar 

  44. Chao H, Riggleman RA (2013) Effect of particle size and grafting density on the mechanical properties of polymer nanocomposites. Polymer 54(19):5222–5229

    Article  CAS  Google Scholar 

  45. Liu H, Webster TJ (2010) Mechanical properties of dispersed ceramic nanoparticles in polymer composites for orthopedic applications. Int J Nanomed 5(1):299–313

    CAS  Google Scholar 

  46. Zhang H, Li S, Yan Y (2001) Dissolution behavior of hydroxyapatite powder in hydrothermal solution. Ceram Int 27(4):451–454

    Article  Google Scholar 

  47. Seol YJ, Park JY, Jung JW, Jang J, Girdhari R, Kim SW, Cho DW (2014) Improvement of bone regeneration capability of ceramic scaffolds by accelerated release of their calcium ions. Tissue Eng - Part A 20(21–22):2840–2849

    Article  CAS  Google Scholar 

  48. Cattalini JP, Hoppe A, Pishbin F, Roether J, Boccaccini AR, Lucangioli S, Mouriño V (2015) Novel nanocomposite biomaterials with controlled copper/calcium release capability for bone tissue engineering multifunctional scaffolds. J R Soc Interface 12(110):1–13

    Article  Google Scholar 

  49. Matthews JL, Martin JH (1971) Intracellular transport of calcium and its relationship to homeostasis and mineralization. An electron microscope study. Am J Med 50(5):589–597

    Article  CAS  Google Scholar 

  50. Kong L, Gao Y, Lu G, Gong Y, Zhao N, Zhang X (2006) A study on the bioactivity of chitosan/nano-hydroxyapatite composite scaffolds for bone tissue engineering. Eur Polym J 42(12):3171–3179

    Article  CAS  Google Scholar 

  51. Niu X, Fan R, Tian F, Guo X, Li P, Feng Q, Fan Y (2017) Calcium concentration dependent collagen mineralization. Mater Sci Eng C 73:137–143

    Article  CAS  Google Scholar 

  52. Yu S, Hariram KP, Kumar R, Cheang P, Aik KK (2005) In vitro apatite formation and its growth kinetics on hydroxyapatite/polyetheretherketone biocomposites. Biomaterials 26(15):2343–2352

    Article  CAS  Google Scholar 

  53. Cowles EA, DeRome ME, Pastizzo G, Brailey LL, Gronowicz GA (1998) Mineralization and the expression of matrix proteins during in vivo bone development. Calcif Tissue Int 62(1):74–82

    Article  CAS  Google Scholar 

  54. Prins HJ, Braat AK, Gawlitta D, Dhert WJA, Egan DA, Tijssen-Slump E, Yuan H, Coffer PJ, Rozemuller H, Martens AC (2014) In vitro induction of alkaline phosphatase levels predicts in vivo bone forming capacity of human bone marrow stromal cells. Stem Cell Res 12(2):428–40

    Article  CAS  Google Scholar 

  55. He C, Jin X, Ma PX (2014) Calcium phosphate deposition rate, structure and osteoconductivity on electrospun poly(l-lactic acid) matrix using electrodeposition or simulated body fluid incubation. Acta Biomater 10(1):419–427

    Article  CAS  Google Scholar 

  56. Le TDH, Liaudanskaya V, Bonani W, Migliaresi C, Motta A (2018) Enhancing bioactive properties of silk fibroin with diatom particles for bone tissue engineering applications. J Tissue Eng Regen Med 12(1):89–97

    Article  CAS  Google Scholar 

  57. Chiralt A, Gonz C, Cano AI (2016) Biodegradation behavior of starch-PVA films as affected by the incorporation of different antimicrobials. Polym Degrad Stab 132:11–20

    Article  Google Scholar 

Download references

Acknowledgements

We would like to thank Ho Chi Minh City University of Technology and Education for providing financial assistance for the study (T2022-123). We acknowledge the support of time and facilities from Ho Chi Minh City University of Technology and Education (HCMUTE) for supporting this study. We are really grateful to prof. Claudio Migliaresi of University of Trento (Italy) for discussing the use of glutaraldehyde at survey experiment and Mr. Long Nhat Tran (HCMUTE, Vietnam) for materials preparation support of this work.

Author information

Authors and Affiliations

Authors

Corresponding authors

Correspondence to Thi Duy Hanh Le or Huynh Nguyen Anh Tuan.

Ethics declarations

Conflict of interest

The authors declare no competing interests.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Le, T.D.H., Tuan, H.N.A., Nguyen, V.T. et al. Hydroxyapatite−loaded starch/polyvinyl alcohol scaffold for bone regeneration application: preparation and characterization. J Sol-Gel Sci Technol 107, 441–451 (2023). https://doi.org/10.1007/s10971-023-06137-3

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10971-023-06137-3

Keywords

Navigation