Synthesis of nanotubular oxide on Ti–24Zr–10Nb–2Sn as a drug-releasing system to prevent the growth of Staphylococcus aureus

Chemical Papers (2021)Cite this article

Abstract

The aim in the present study was to explore the potential application of titanium nanotubes developed in the Ti–24Zr–10Nb–2Sn alloy, as drug delivery systems to prevent bacterial infections in medical devices. A nanotubular oxide layer was synthesized by electrochemical anodizing on the Ti–24Zr–10Nb–2Sn superelastic alloy and the electrical variables that control the growth at constant potential were determined. Scanning electron microscopy (SEM) showed that the nanostructures show a positive linear growth as a function of the applied potential, the superficial analysis carried out by X-ray photoelectron spectroscopy (XPS) showed different states of valence evidencing the presence of TiO2, Nb2O5, SnO2, and ZrO2. FTIR spectra confirm the presence of the antibiotic gentamicin in the Ti–24Zr–10Nb–2Sn nanotubes. The developed nanostructures were evaluated in a phosphate buffer solution (PBS) as a controlled release system of antibiotics. It was observed by bacteriological tests that the nanostructured morphology in combination with the chemical composition has bacteriostatic properties; while the release of the antibiotic-loaded inside the nanotubes had a bactericidal effect. The results showed that it is possible to grow and control the morphology of the developed nanostructures on Ti–24Zr–10Nb–2Sn, which can be used for orthopedic purposes to transport and control the local release of molecules like antibiotics at the site of interest and thus prevent postoperative infections.

Graphic abstract

This is a preview of subscription content, access via your institution.

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

References

  1. Abdul-Khodir WKW, Abdul-Razak AH, Ng MH, Guarino V, Susanti D (2018) Encapsulation and characterization of gentamicin sulfate in the collagen added electrospun nanofibers for skin regeneration. J Funct Biomater 9:36. https://doi.org/10.3390/jfb9020036

    CAS  Article  PubMed Central  Google Scholar 

  2. Aguilera-Correa JJ, Doadrio AL, Conde A, Arenas MA, de-Damborenea JJ, Vallet-Regi M, Esteban J (2018) Antibiotic release from F-doped nanotubular oxide layer on TI6AL4V alloy to decrease bacterial viability. J Mater Sci Mater Med 29:118. https://doi.org/10.1007/s10856-018-6119-4

    CAS  Article  PubMed  Google Scholar 

  3. Allam NK, Alamgir F, El-Sayed MA (2010) Enhanced photoassisted water electrolysis using vertically oriented anodically fabricated Ti–Nb–Zr–O mixed oxide nanotube arrays. ACS Nano 4:5819–5826. https://doi.org/10.1021/nn101678n

    CAS  Article  PubMed  Google Scholar 

  4. Barth E, Myrvik QM, Wagner W, Gristina AG (1989) vitro and in vivo comparative colonization of Staphylococcus aureus and Staphylococcus epidermidis on orthopaedic implant materials. Biomaterials 10:325–328. https://doi.org/10.1016/0142-9612(89)90073-2

    CAS  Article  PubMed  Google Scholar 

  5. Berger S, Tsuchiya H, Schmuki P (2008) Transition from nanopores to nanotubes: self-ordered anodic oxide structures on titanium−aluminides. Chem Mater 20:3245–3247. https://doi.org/10.1021/cm8004024

    CAS  Article  Google Scholar 

  6. Bint AJ, George RH, Healing DE, Wise R, Davies M (1977) An outbreak of infection caused by a gentamicin-resistant Staphylococcus aureus. J Clin Pathol 30:165–167. https://doi.org/10.1136/jcp.30.2.165

    CAS  Article  PubMed  PubMed Central  Google Scholar 

  7. Feng XJ, Macak JM, Albu SP, Schmuki P (2008) Electrochemical formation of self-organized anodic nanotube coating on Ti–28Zr–8Nb biomedical alloy surface. Acta Biomater 4:318–323. https://doi.org/10.1016/j.actbio.2007.08.005

    CAS  Article  PubMed  Google Scholar 

  8. Filova E, Fojt J, Kryslova M, Moravec H, Joska L, Bacakova L (2015) The diameter of nanotubes formed on Ti–6Al–4V alloy controls the adhesion and differentiation of Saos-2 cells. Int J Nanomed 10:7145–7163. https://doi.org/10.2147/IJN.S87474

    CAS  Article  Google Scholar 

  9. Fornell J, Oliveira NTC, Pellicer E, Van Steenberge N, Baró MD, Bolfarini C, Sort J (2013) Anodic formation of self-organized Ti(Nb, Sn) oxide nanotube arrays with tuneable aspect ratio and size distribution. Electrochem Commun 33:84–87. https://doi.org/10.1016/j.elecom.2013.04.023

    CAS  Article  Google Scholar 

  10. Ghicov A, Schmuki P (2009) Self-ordering electrochemistry: a review on growth and functionality of TiO2 nanotubes and other self-aligned MO(x) structures. Chem Commun (Camb). https://doi.org/10.1039/b822726h

    Article  Google Scholar 

  11. Gulati K, Aw MS, Losic D (2011) Drug-eluting Ti wires with titania nanotube arrays for bone fixation and reduced bone infection. Nanoscale Res Lett 6:571. https://doi.org/10.1186/1556-276X-6-571

    Article  PubMed  PubMed Central  Google Scholar 

  12. Gulati K, Ramakrishnan S, Aw MS, Atkins GJ, Findlay DM, Losic D (2012) Biocompatible polymer coating of titania nanotube arrays for improved drug elution and osteoblast adhesion. Acta Biomater 8:449–456. https://doi.org/10.1016/j.actbio.2011.09.004

    CAS  Article  PubMed  Google Scholar 

  13. Gulati K, Kogawa M, Prideaux M, Findlay DM, Atkins GJ, Losic D (2016) Drug-releasing nano-engineered titanium implants: therapeutic efficacy in 3D cell culture model, controlled release and stability. Mater Sci Eng C Mater Biol Appl 69:831–840. https://doi.org/10.1016/j.msec.2016.07.047

    CAS  Article  PubMed  Google Scholar 

  14. Hang R, Liu Y, Zhao L, Gao A, Bai L, Huang X, Zhang B, Tang B, Chu PK (2014) Fabrication of Ni–Ti–O nanotube arrays by anodization of NiTi alloy and their potential applications. Sci Rep 4:7547. https://doi.org/10.1038/srep07547

    CAS  Article  PubMed  PubMed Central  Google Scholar 

  15. Jeong Y-H, Kim E-J, Brantley WA, Choe H-C (2014) Morphology of hydroxyapatite nanoparticles in coatings on nanotube-formed Ti–Nb–Zr alloys for dental implants. Vacuum 107:297–303. https://doi.org/10.1016/j.vacuum.2014.03.004

    CAS  Article  Google Scholar 

  16. Ji Y, Zhang M, Cui J, Lin K-C, Zheng H, Zhu J-J, Samia ACS (2012) Highly-ordered TiO2 nanotube arrays with double-walled and bamboo-type structures in dye-sensitized solar cells. Nano Energy 1:796–804. https://doi.org/10.1016/j.nanoen.2012.08.006

    CAS  Article  Google Scholar 

  17. Li G-Z, Tang H-P, Zhang W-Y, Li G, Yu L-L, Li Y-N (2013) Fabrication of multilayer Nb2O5 nanoporous film by anodization of niobium foils. Rare Met 34:77–80. https://doi.org/10.1007/s12598-013-0140-z

    CAS  Article  Google Scholar 

  18. Liang YQ, Cui ZD, Zhu SL, Yang XJ (2011) Characterization of self-organized TiO2 nanotubes on Ti–4Zr–22Nb–2Sn alloys and the application in drug delivery system. J Mater Sci Mater Med 22:461–467. https://doi.org/10.1007/s10856-011-4234-6

    CAS  Article  PubMed  Google Scholar 

  19. Liu H, Ding D, Ning C, Li Z (2012) Wide-range hydrogen sensing with Nb-doped TiO2 nanotubes. Nanotechnology 23:015502. https://doi.org/10.1088/0957-4484/23/1/015502

    CAS  Article  PubMed  Google Scholar 

  20. Liu Q, Ding D, Ning C (2014) Anodic fabrication of Ti–Nb–Zr–O nanotube arrays. J Nanomater 2014:1–7. https://doi.org/10.1155/2014/240346

    CAS  Article  Google Scholar 

  21. Losic D, Aw MS, Santos A, Gulati K, Bariana M (2015) Titania nanotube arrays for local drug delivery: recent advances and perspectives. Expert Opin Drug Deliv 12:103–127. https://doi.org/10.1517/17425247.2014.945418

    CAS  Article  PubMed  Google Scholar 

  22. Macak JM, Tsuchiya H, Schmuki P (2005) High-aspect-ratio TiO2 nanotubes by anodization of titanium. Angew Chem Int Ed Engl 44:2100–2102. https://doi.org/10.1002/anie.200462459

    CAS  Article  PubMed  Google Scholar 

  23. Nampi PP, Mohan VS, Sinha AK, Varma H (2012) High surface area sol–gel nano silica as a novel drug carrier substrate for sustained drug release. Mater Res Bull 47:1379–1384. https://doi.org/10.1016/j.materresbull.2012.03.003

    CAS  Article  Google Scholar 

  24. Nemati SH, Hadjizadeh A (2017) Gentamicin-eluting titanium dioxide nanotubes grown on the ultrafine-grained titanium. AAPS PharmSciTech 18:2180–2187. https://doi.org/10.1208/s12249-016-0679-8

    CAS  Article  PubMed  Google Scholar 

  25. O’Neil MJ, Smith A, Heckelman PE (2006) The merck index: an encyclopedia of chemicals drugs, and biologicals. Merck & Co. Inc., Whitehouse Station, NJ

    Google Scholar 

  26. Pavón LL, Kim HY, Hosoda H, Miyazaki S (2015) Effect of Nb content and heat treatment temperature on superelastic properties of Ti–24Zr–(8–12)Nb–2Sn alloys. Scripta Mater 95:46–49. https://doi.org/10.1016/j.scriptamat.2014.09.029

    CAS  Article  Google Scholar 

  27. Pavón LL, Dagnino D, Moreno IE, Lopez E, Zarate D, Kim HY, Miyazaki S (2017) A novel method for fabrication of Ti24Zr10Nb2Sn alloy oxide nanotubes-chitosan nanocomposite films. Mater Lett 205:134–137. https://doi.org/10.1016/j.matlet.2017.06.078

    CAS  Article  Google Scholar 

  28. Pavón LL, Cuellar EL, Hernandez SV, Moreno-Cortez IE, Kim HY, Miyazaki S (2019) Effect of heat treatment condition on microstructure and superelastic properties of Ti24Zr10Nb2Sn. J Alloys Compd 782:893–898. https://doi.org/10.1016/j.jallcom.2018.12.266

    CAS  Article  Google Scholar 

  29. Pawlik A, Jarosz M, Syrek K, Sulka GD (2017) Co-delivery of ibuprofen and gentamicin from nanoporous anodic titanium dioxide layers. Colloids Surf B Biointerfaces 152:95–102. https://doi.org/10.1016/j.colsurfb.2017.01.011

    CAS  Article  PubMed  Google Scholar 

  30. Popat KC, Eltgroth M, Latempa TJ, Grimes CA, Desai TA (2007) Decreased Staphylococcus epidermis adhesion and increased osteoblast functionality on antibiotic-loaded titania nanotubes. Biomaterials 28:4880–4888. https://doi.org/10.1016/j.biomaterials.2007.07.037

    CAS  Article  PubMed  Google Scholar 

  31. Raphel J, Holodniy M, Goodman SB, Heilshorn SC (2016) Multifunctional coatings to simultaneously promote osseointegration and prevent infection of orthopaedic implants. Biomaterials 84:301–314. https://doi.org/10.1016/j.biomaterials.2016.01.016

    CAS  Article  PubMed  PubMed Central  Google Scholar 

  32. Ruiquan Y, Longfei J, Xufei Z, Ye S, Dongliang Y, Aijun H (2012) Theoretical derivation of ionic current and electronic current and comparison between fitting curves and measured curves. RSC Adv 2:12474–12481. https://doi.org/10.1039/C2RA22124A

    Article  Google Scholar 

  33. Sul YT (2010) Electrochemical growth behavior, surface properties, and enhanced in vivo bone response of TiO2 nanotubes on microstructured surfaces of blasted, screw-shaped titanium implants. Int J Nanomed 5:87–100. https://doi.org/10.2147/ijn.s8012

    CAS  Article  Google Scholar 

  34. Verissimo NC, Cremasco A, Rodrigues CA, Bertazzoli R, Caram R (2014) In situ characterization of the effects of Nb and Sn on the anatase–rutile transition in TiO2 nanotubes using high-temperature X-ray diffraction. Appl Surf Sci 307:372–381. https://doi.org/10.1016/j.apsusc.2014.04.040

    CAS  Article  Google Scholar 

  35. Wong JY, Leach JB, Brown XQ (2004) Balance of chemistry, topography, and mechanics at the cell–biomaterial interface: issues and challenges for assessing the role of substrate mechanics on cell response. Surf Sci 570:119–133. https://doi.org/10.1016/j.susc.2004.06.186

    CAS  Article  Google Scholar 

  36. Yasuda K, Schmuki P (2007a) Control of morphology and composition of self-organized zirconium titanate nanotubes formed in (NH4)2SO4/NH4F electrolytes. Electrochim Acta 52:4053–4061. https://doi.org/10.1016/j.electacta.2006.11.023

    CAS  Article  Google Scholar 

  37. Yasuda K, Schmuki P (2007b) Electrochemical formation of self-organized zirconium titanate nanotube multilayers. Electrochem Commun 9:615–619. https://doi.org/10.1016/j.elecom.2006.10.043

    CAS  Article  Google Scholar 

  38. Zhang Y, Ni M, Zhang M, Ratner B (2003) Calcium phosphate-chitosan composite scaffolds for bone tissue engineering. Tissue Eng 9:337–345. https://doi.org/10.1089/107632703764664800

    CAS  Article  PubMed  Google Scholar 

  39. Zhao X, Dai M, Li S, Hao Y, Yang R, Wang L, Liu Y (2016) Mixture of oxides with different valence states in nanotubes. J Mater Sci Technol 32:142–146. https://doi.org/10.1016/j.jmst.2015.10.017

    CAS  Article  Google Scholar 

Download references

Acknowledgements

The authors thank Consejo Nacional de Ciencia y Tecnología (CONACYT) for the support of the project 219535.

Author information

Affiliations

  1. Facultad de Ingeniería Mecánica y Eléctrica, Universidad Autónoma de Nuevo León, Avenida Universidad s/n, Ciudad Universitaria, C.P. 66451, San Nicolás de los Garza, NL, México

    Luis López-Pavón, Daniel Dagnino-Acosta, Enrique López-Cuéllar, Frank Meléndez-Anzures & Iván Moreno-Cortez

  2. Facultad de Ciencias Biológicas, Universidad Autónoma de Nuevo León, Universidad s/n, Ciudad Universitaria, C.P. 66451, San Nicolás de los Garza, NL, México

    Diana Zárate-Triviño & María Barrón-González

  3. Division of Materials Science, University of Tsukuba, Tsukuba, Ibaraki, 305-8573, Japan

    Hee Young Kim & Shuichi Miyazaki

Authors
  1. Luis López-Pavón
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Daniel Dagnino-Acosta
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Enrique López-Cuéllar
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Frank Meléndez-Anzures
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Diana Zárate-Triviño
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. María Barrón-González
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Iván Moreno-Cortez
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Hee Young Kim
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Shuichi Miyazaki
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Enrique López-Cuéllar.

Ethics declarations

Conflict of interest

On behalf of all authors, the corresponding author states that there is no conflict of interest.

Additional information

Publisher's Note

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

Rights and permissions

Reprints and Permissions

About this article

Verify currency and authenticity via CrossMark

Cite this article

López-Pavón, L., Dagnino-Acosta, D., López-Cuéllar, E. et al. Synthesis of nanotubular oxide on Ti–24Zr–10Nb–2Sn as a drug-releasing system to prevent the growth of Staphylococcus aureus. Chem. Pap. (2021). https://doi.org/10.1007/s11696-020-01495-6

Download citation

Keywords

  • Anodization
  • Titanium nanotubes
  • Antibacterial