Skip to main content
SpringerLink
Log in

Corrosion resistance and antibacterial effects of hydroxyapatite coating induced by polyacrylic acid and gentamicin sulfate on magnesium alloy

  • Research Article
  • Published:
Frontiers of Materials Science Aims and scope Submit manuscript

Abstract

Magnesium (Mg) alloys have attracted considerable research attention as potential biocompatible implant materials. However, the major barriers to the extended use of such medical devices are the possibility of high corrosion rate and implant-associated infections. To solve them, a novel polyacrylic acid (PAA)/gentamicin sulfate (GS)-hydroxyapatite (HAp) coating was synthesized by a one-step hydrothermal deposition method. Characteristics of functional coatings were investigated by SEM, FTIR and XRD. Corrosion properties of samples were evaluated by electrochemical and hydrogen evolution tests. Antibacterial activities of the coatings against Staphylococcus aureus (S. aureus) were measured by the plate-counting method. Results showed that the as-prepared HAp coating with dense and flawless morphologies could not only enhance the corrosion resistance of Mg alloys, but also improve the adhesion strength between the HAp coating and the substrate. In addition, the induction of the apatite coating during immersion confirmed the excellent mineralization ability of the HAp coating. Moreover, the obtained HAp coating possessed antibacterial properties and could prolong the release of GS. Thus, the PAA/GS-HAp coated Mg alloy could serve as a better candidate for biomedical applications with good anti-corrosion and antibacterial properties.

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

Similar content being viewed by others

References

  1. Zhu D, Su Y, Young M L, et al. Biological responses and mechanisms of human bone marrow mesenchymal stem cells to Zn and Mg biomaterials. ACS Applied Materials & Interfaces, 2017, 9(33): 27453–27461

    Article  Google Scholar 

  2. Zhang X, Li X W, Li J G, et al. Preparation and mechanical property of a novel 3D porous magnesium scaffold for bone tissue engineering. Materials Science and Engineering C, 2014, 42: 362–367

    Article  Google Scholar 

  3. Witte F, Kaese V, Haferkamp H, et al. In vivo corrosion of four magnesium alloys and the associated bone response. Biomaterials, 2005, 26(17): 3557–3563

    Article  Google Scholar 

  4. Razavi M, Fathi M, Savabi O, et al. Nanostructured merwinite bioceramic coating on Mg alloy deposited by electrophoretic deposition. Ceramics International, 2014, 40(7): 9473–9484

    Article  Google Scholar 

  5. Zhao Y B, Shi L Q, Cui L Y, et al. Corrosion resistance of silane-modified hydroxyapatite films on degradable magnesium alloys. Acta Metallurgica Sinica (English Letters), 2018, 31(2): 180–188

    Article  Google Scholar 

  6. Cui L Y, Wei G B, Zeng R C, et al. Corrosion resistance of a novel SnO2-doped dicalcium phosphate coating on AZ31 magnesium alloy. Bioactive Materials, 2018, 3(3): 245–249

    Article  Google Scholar 

  7. Liu Y, Huang J, Li H. Synthesis of hydroxyapatite-reduced graphite oxide nanocomposites for biomedical applications: oriented nucleation and epitaxial growth of hydroxyapatite. Journal of Materials Chemistry B: Materials for Biology and Medicine, 2013, 1(13): 1826–1834

    Article  Google Scholar 

  8. Liu Y, Dang Z, Wang Y, et al. Hydroxyapatite/graphenenanosheet composite coatings deposited by vacuum cold spraying for biomedical applications: Inherited nanostructures and enhanced properties. Carbon, 2014, 67(2): 250–259

    Article  Google Scholar 

  9. Zhao Y B, Liu H P, Li C Y, et al. Corrosion resistance and adhesion strength of a spin-assisted layer-by-layer assembled coating on AZ31 magnesium alloy. Applied Surface Science, 2018, 434: 787–795

    Article  Google Scholar 

  10. Cui L Y, Zeng R C, Guan S K, et al. Degradation mechanism of micro-arc oxidation coatings on biodegradable Mg–Ca alloys: The influence of porosity. Journal of Alloys and Compounds, 2017, 695: 2464–2476

    Article  Google Scholar 

  11. Hutchens S A, Benson R S, Evans B R, et al. Biomimetic synthesis of calcium-deficient hydroxyapatite in a natural hydrogel. Biomaterials, 2006, 27(26): 4661–4670

    Article  Google Scholar 

  12. Cho J S, Kang Y C. Nano-sized hydroxyapatite powders prepared by flame spray pyrolysis. Journal of Alloys and Compounds, 2008, 464(1–2): 282–287

    Article  Google Scholar 

  13. Yu M, Zhou K, Zhang F, et al. Porous HA microspheres as drug delivery: Effects of porosity and pore structure on drug loading and in vitro release. Ceramics International, 2014, 40(8): 12617–12621

    Article  Google Scholar 

  14. Takai C, Hotta T, Shiozaki S, et al. Unique porous microspheres with dense core and a porous layer prepared by a novel S/O/W emulsion technique. Chemical Communications, 2009, 37(37): 5533–5535

    Article  Google Scholar 

  15. Kang Z, Zhang J, Niu L. A one-step hydrothermal process to fabricate superhydrophobic hydroxyapatite coatings and determination of their properties. Surface and Coatings Technology, 2018, 334: 84–89

    Article  Google Scholar 

  16. Song Y, Zhang S, Li J, et al. Electrodeposition of Ca–P coatings on biodegradable Mg alloy: in vitro biomineralization behavior. Acta Biomaterialia, 2010, 6(5): 1736–1742

    Article  Google Scholar 

  17. Tan C, Zhang X, Li Q. Fabrication of multifunctional CaP–TC composite coatings and the corrosion protection they provide for magnesium alloys. Biomedical Engineering, 2017, 62(4): 375–381

    Article  Google Scholar 

  18. Zeng R C, Zhang F, Lan Z D, et al. Corrosion resistance of calcium-modified zinc phosphate conversion coatings on magnesium–aluminium alloys. Corrosion Science, 2014, 88(6): 452–459

    Article  Google Scholar 

  19. Li F, Xing Q, Han Y, et al. Ultrasonically assisted preparation of poly(acrylic acid)/calcium phosphate hybrid nanogels as pHresponsive drug carriers. Materials Science and Engineering C, 2017, 80: 688–697

    Article  Google Scholar 

  20. Bigi A, Boanini E, Cojazzi G, et al. Morphological and structural investigation of octacalcium phosphate hydrolysis in the presence of polyacrylic acids: effect of relative molecular weights. Crystal Growth & Design, 2001, 1(3): 239–244

    Article  Google Scholar 

  21. Kazemzadeh-Narbat M, Lai B F, Ding C, et al. Multilayered coating on titanium for controlled release of antimicrobial peptides for the prevention of implant-associated infections. Biomaterials, 2013, 34(24): 5969–5977

    Article  Google Scholar 

  22. Guo Y J, Long T, Chen W, et al. Bactericidal property and biocompatibility of gentamicin-loaded mesoporous carbonated hydroxyapatite microspheres. Materials Science and Engineering C, 2013, 33(7): 3583–3591

    Article  Google Scholar 

  23. Min J, Braatz R D, Hammond P T. Tunable staged release of therapeutics from layer-by-layer coatings with clay interlayer barrier. Biomaterials, 2014, 35(8): 2507–2517

    Article  Google Scholar 

  24. Com E, Boitier E, Marchandeau J P, et al. Integrated transcriptomic and proteomic evaluation of gentamicin nephrotoxicity in rats. Toxicology and Applied Pharmacology, 2012, 258(1): 124–133

    Article  Google Scholar 

  25. Gamazo C, Prior S, Concepción Lecároz M, et al. Biodegradable gentamicin delivery systems for parenteral use for the treatment of intracellular bacterial infections. Expert Opinion on Drug Delivery, 2007, 4(6): 677–688

    Article  Google Scholar 

  26. Ding Z Y, Cui L Y, Zeng R C, et al. Exfoliation corrosion of extruded Mg–Li–Ca alloy. Journal of Materials Science and Technology, 2018, 34(9): 1550–1557

    Article  Google Scholar 

  27. Zeng R C, Cui L Y, Jiang K, et al. In vitro corrosion and cytocompatibility of a microarc oxidation coating and poly(Llactic acid) composite coating on Mg–1Li–1Ca alloy for orthopedic implants. ACS Applied Materials & Interfaces, 2016, 8 (15): 10014–10028

    Article  Google Scholar 

  28. Yao Q S, Zhang F, Song L, et al. Corrosion resistance of a ceria/ polymethyltrimethoxysilane modified Mg–Al-layered double hydroxide on AZ31 magnesium alloy. Journal of Alloys and Compounds, 2018, 764: 913–928

    Article  Google Scholar 

  29. Ren Y, Zhou H, Nabiyouni M, et al. Rapid coating of AZ31 magnesium alloy with calcium deficient hydroxyapatite using microwave energy. Materials Science and Engineering C, 2015, 49: 364–372

    Article  Google Scholar 

  30. Zhou K, Zhang Y, Zhang D, et al. Porous hydroxyapatite ceramics fabricated by an ice-templating method. Scripta Materialia, 2011, 64(5): 426–429

    Article  Google Scholar 

  31. Cui L Y, Fang X H, Cao W, et al. In vitro corrosion resistance of a layer-by-layer assembled DNA coating on magnesium alloy. Applied Surface Science, 2018, 457: 49–58

    Article  Google Scholar 

  32. Mantilaka M M M G P G, Pitawala H M T G A, Karunaratne D G G P, et al. Nanocrystalline magnesium oxide from dolomite via poly(acrylate) stabilized magnesium hydroxide colloids. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2014, 443(4): 201–208

    Article  Google Scholar 

  33. Guo L, Zhang F, Song L, et al. Corrosion resistance of ceria/polymethyltrimethoxysilane modified magnesium hydroxide coating on AZ31 magnesium alloy. Surface and Coatings Technology, 2017, 328: 121–133

    Article  Google Scholar 

  34. Moore R C, Rigali M J, Brady P. Selenite sorption by carbonate substituted apatite. Environmental Pollution, 2016, 218: 1102–1107

    Article  Google Scholar 

  35. Liu L, Li P, Zou Y, et al. In vitro corrosion and antibacterial performance of polysiloxane and poly(acrylic acid)/gentamicin sulfate composite coatings on AZ31 alloy. Surface and Coatings Technology, 2016, 291: 7–14

    Article  Google Scholar 

  36. Zhang Y, Gao P, Zhao L, et al. Preparation and swelling properties of a starch-g-poly(acrylic acid)/organo-mordenite hydrogel composite. Frontiers of Chemical Science and Engineering, 2016, 10 (1): 147–161

    Article  Google Scholar 

  37. Liao S, Watari F, Xu G, et al. Morphological effects of variant carbonates in biomimetic hydroxyapatite. Materials Letters, 2007, 61(17): 3624–3628

    Article  Google Scholar 

  38. Walsh D, Furuzono T, Tanaka J. Preparation of porous composite implant materials by in situ polymerization of porous apatite containing ε-caprolactone or methyl methacrylate. Biomaterials, 2001, 22(11): 1205–1212

    Article  Google Scholar 

  39. Fathi M H, Hanifi A, Mortazavi V. Preparation and bioactivity evaluation of bone-like hydroxyapatite nanopowder. Journal of Materials Processing Technology, 2008, 202(1–3): 536–542

    Article  Google Scholar 

  40. Geuli O, Metoki N, Zada T, et al. Synthesis, coating and drugrelease of hydroxyapatite nanoparticles loaded with antibiotics. Journal of Materials Chemistry B: Materials for Biology and Medicine, 2017, 5(38): 7819–7830

    Article  Google Scholar 

  41. Venkatesan P, Puvvada N, Dash R, et al. The potential of celecoxib-loaded hydroxyapatite–chitosan nanocomposite for the treatment of colon cancer. Biomaterials, 2011, 32(15): 3794–3806

    Article  Google Scholar 

  42. Zhao Y, Shi L, Ji X, et al. Corrosion resistance and antibacterial properties of polysiloxane modified layer-by-layer assembled selfhealing coating on magnesium alloy. Journal of Colloid and Interface Science, 2018, 526: 43–50

    Article  Google Scholar 

  43. Cui L Y, Gao S D, Li P P, et al. Corrosion resistance of a selfhealing micro-arc oxidation/polymethyltrimethoxysilane composite coating on magnesium alloy AZ31. Corrosion Science, 2017, 118: 84–95

    Article  Google Scholar 

  44. Ding Z Y, Cui L Y, Chen X B, et al. In vitro corrosion of micro-arc oxidation coating on Mg–1Li–1Ca alloy — The influence of intermetallic compound Mg2Ca. Journal of Alloys and Compounds, 2018, 764: 250–260

    Article  Google Scholar 

  45. Ostrowski N, Lee B, Hong D, et al. Synthesis, osteoblast, and osteoclast viability of amorphous and crystalline tri-magnesium phosphate. ACS Biomaterials Science & Engineering, 2015, 1(1): 52–63

    Article  Google Scholar 

  46. Jiang S, Cai S, Zhang F, et al. Synthesis and characterization of magnesium phytic acid/apatite composite coating on AZ31 Mg alloy by microwave assisted treatment. Materials Science and Engineering C, 2018, 91: 218–227

    Article  Google Scholar 

  47. Guo Y, Zhou Y, Jia D. Fabrication of hydroxycarbonate apatite coatings with hierarchically porous structures. Acta Biomaterialia, 2008, 4(2): 334–342

    Article  Google Scholar 

  48. Robinson D A, Griffith R W, Shechtman D, et al. In vitro antibacterial properties of magnesium metal against Escherichia coli, Pseudomonas aeruginosa and Staphylococcus aureus. Acta Biomaterialia, 2010, 6(5): 1869–1877

    Article  Google Scholar 

  49. Nazaruk E, Górecka E, Osornio Y M, et al. Charged additives modify drug release rates from lipidic cubic phase carriers by modulating electrostatic interactions. Journal of Electroanalytical Chemistry, 2018, 819: 269–274

    Article  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant No. 51571134), the Shandong University of Science and Technology (SDUST) Research Fund (2014TDJH104), the Shandong Provincial Natural Science Foundation (ZR2017BEM002), and the Science and Technology Innovation Fund of SDUST for graduate students (SDKDYC180371).

Author information

Authors and Affiliations

  1. College of Materials Science and Engineering, Shandong University of Science and Technology, Qingdao, 266590, China

    Xiao-Jing Ji, Qiang Cheng, Jing Wang, Yan-Bin Zhao, Zhuang-Zhuang Han, Fen Zhang, Shuo-Qi Li & Rong-Chang Zeng

  2. College of Materials Science and Engineering, Chongqing University of Technology, Chongqing, 400065, China

    Zhen-Lin Wang

Authors
  1. Xiao-Jing Ji
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Qiang Cheng
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Jing Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Yan-Bin Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Zhuang-Zhuang Han
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Fen Zhang
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Shuo-Qi Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Rong-Chang Zeng
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Zhen-Lin Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding authors

Correspondence to Shuo-Qi Li or Rong-Chang Zeng.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Ji, XJ., Cheng, Q., Wang, J. et al. Corrosion resistance and antibacterial effects of hydroxyapatite coating induced by polyacrylic acid and gentamicin sulfate on magnesium alloy. Front. Mater. Sci. 13, 87–98 (2019). https://doi.org/10.1007/s11706-019-0448-1

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11706-019-0448-1

Keywords

Search

Navigation