Skip to main content
Log in

Corrosion resistance of Ca-P coating induced by layer-by-layer assembled polyvinylpyrrolidone/DNA multilayer on magnesium AZ31 alloy

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

Abstract

A hydrothermal deposition method was utilized to fabricate Ca-P composite coating induced by the layer-by-layer (LbL) assembled polyvinylpyrrolidone/deoxyribonucleic acid (PVP/DNA)20 multilayer on AZ31 alloy. The surface morphology and compositions were characterized by SEM, EDS, FTIR and XRD. Besides, the corrosion resistance and degradation behavior of the coating were tested via electrochemical polarization, impedance spectroscopy and immersion measurements. Results show that the main components of Ca-P coatings are hydroxyapatite, Ca3(PO4)2 and Mg3(PO4)2·nH2O. The LbL-assembled DNA and PVP promote the adsorption of Ca-P deposits on the sample surface, and structures and functional groups of the polyelectrolyte in the outermost layer are the primary influencing factor for the induction of the Ca-P coating. Carboxyl groups have the best biomineralization effect among all related functional groups. The enhanced corrosion resistance and adhesion highlight a promising use of (PVP/DNA)20-induced Ca-P coatings in the field of biomedical magnesium alloys.

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.

Similar content being viewed by others

References

  1. Zhang C, Lin J, Nguyen N T, et al. Antimicrobial bioresorbable Mg-Zn-Ca alloy for bone repair in a comparison study with Mg-Zn-Sr alloy and pure Mg. ACS Biomaterials Science & Engineering, 2020, 6(1): 517–538

    Article  CAS  Google Scholar 

  2. Zhang J, Tang L, Qi H, et al. Dual function of magnesium in bone biomineralization. Advanced Healthcare Materials, 2019, 8(21): 1901030

    Article  CAS  Google Scholar 

  3. Zhang Z Q, Wang L, Zeng M Q, et al. Biodegradation behavior of micro-arc oxidation coating on magnesium alloy — From a protein perspective. Bioactive Materials, 2020, 5(2): 398–409

    Article  Google Scholar 

  4. Chandra G, Pandey A. Preparation strategies for Mg-alloys for biodegradable orthopaedic implants and other biomedical applications: A review. IRBM, 2020 (in press)

  5. Li C Y, Yu C, Zeng R C, et al. In vitro corrosion resistance of a Ta2O5 nanofilm on MAO coated magnesium alloy AZ31 by atomic layer deposition. Bioactive Materials, 2020, 5(1): 34–43

    Article  Google Scholar 

  6. Cui L Y, Qin P H, Huang X L, et al. Electrodeposition of TiO2 layer-by-layer assembled composite coating and silane treatment on Mg alloy for corrosion resistance. Surface and Coatings Technology, 2017, 324: 560–568

    Article  CAS  Google Scholar 

  7. Cui L Y, Liu H P, Xue K, et al. In vitro corrosion and antibacterial performance of micro-arc oxidation coating on AZ31 magnesium alloy: Effects of tannic acid. Journal of the Electrochemical Society, 2018, 165(11): C821–C829

    Article  CAS  Google Scholar 

  8. Cui L Y, Wei G B, Han Z Z, et al. In vitro corrosion resistance and antibacterial performance of novel tin dioxide-doped calcium phosphate coating on degradable Mg-1Li-1Ca alloy. Journal of Materials Science and Technology, 2019, 35(3): 254–265

    Article  Google Scholar 

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

    Article  CAS  Google Scholar 

  10. Chen L, Sheng Y, Zhou H, et al. Influence of a MAO + PLGA coating on biocorrosion and stress corrosion cracking behavior of a magnesium alloy in a physiological environment. Corrosion Science, 2019, 148: 134–143

    Article  CAS  Google Scholar 

  11. Chen Y Q, Zhao S, Chen M Y, et al. Sandwiched polydopamine (PDA) layer for titanium dioxide (TiO2) coating on magnesium to enhance corrosion protection. Corrosion Science, 2015, 96: 67–73

    Article  CAS  Google Scholar 

  12. Kunjukunju S, Roy A, Ramanathan M, et al. A layer-by-layer approach to natural polymer-derived bioactive coatings on magnesium alloys. Acta Biomaterialia, 2013, 9(10): 8690–8703

    Article  CAS  Google Scholar 

  13. 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  CAS  Google Scholar 

  14. Wu F, Li T Y, Su S C, et al. STC2 as a novel mediator for Mus81-dependent proliferation and survival in hepatocellular carcinoma. Cancer Science, 2018, 109(S1): 1121

    Google Scholar 

  15. Ali A, Iqbal F, Ahmad A, et al. Hydrothermal deposition of high strength calcium phosphate coatings on magnesium alloy for biomedical applications. Surface and Coatings Technology, 2019, 357: 716–727

    Article  CAS  Google Scholar 

  16. Kavitha R J, Ravichandran K, Narayanan T S N S. Deposition of strontium phosphate coatings on magnesium by hydrothermal treatment: Characteristics, corrosion resistance and bioactivity. Journal of Alloys and Compounds, 2018, 745: 725–743

    Article  CAS  Google Scholar 

  17. Zeng R C, Sun X X, Song Y W, et al. Influence of solution temperature on corrosion resistance of Zn-Ca phosphate conversion coating on biomedical Mg-Li-Ca alloys. Transactions of Nonferrous Metals Society of China, 2013, 23(11): 3293–3299

    Article  CAS  Google Scholar 

  18. Yeganeh M, Mohammadi N. Superhydrophobic surface of Mg alloys: A review. Journal of Magnesium and Alloys, 2018, 6(1): 59–70

    Article  CAS  Google Scholar 

  19. Li Q, Zhang Q, An M. Enhanced corrosion and wear resistance of AZ31 magnesium alloy in simulated body fluid via electrodeposition of nanocrystalline zinc. Materialia, 2018, 4: 282–286

    Article  Google Scholar 

  20. Wen C, Zhan X, Huang X, et al. Characterization and corrosion properties of hydroxyapatite/graphene oxide bio-composite coating on magnesium alloy by one-step micro-arc oxidation method. Surface and Coatings Technology, 2017, 317: 125–133

    Article  CAS  Google Scholar 

  21. Li C Y, Fan X L, Cui L Y, et al. Corrosion resistance and electrical conductivity of a nano ATO-doped MAO/methyltrimethoxysilane composite coating on magnesium alloy AZ31. Corrosion Science, 2020, 168: 108570

    Article  CAS  Google Scholar 

  22. Zhang Z Q, Zeng R C, Lin C G, et al. Corrosion resistance of self-cleaning silane/polypropylene composite coatings on magnesium alloy AZ31. Journal of Materials Science and Technology, 2020, 41: 43–55

    Article  Google Scholar 

  23. Su Y, Li K, Zhang L, et al. Ca-P bioactive coating prepared by combining microwave-hydrothermal and supersonic atmospheric plasma spraying methods. Materials Science and Engineering C: Materials for Biological Applications, 2017, 72: 371–377

    Article  CAS  Google Scholar 

  24. He D H, Liu P, Liu X K, et al. Hydroxyapatite bioceramic coatings prepared by hydrothermal-electrochemical deposition method. Journal of Wuhan University of Technology: Materials Science Edition, 2014, 29(2): 398–400

    Article  CAS  Google Scholar 

  25. Li L Y, Cui L Y, Liu B, et al. Corrosion resistance of glucose-induced hydrothermal calcium phosphate coating on pure magnesium. Applied Surface Science, 2019, 465: 1066–1077

    Article  CAS  Google Scholar 

  26. Cui L Y, Cheng S C, Liang L X, et al. In vitro corrosion resistance of layer-by-layer assembled polyacrylic acid multilayers induced Ca-P coating on magnesium alloy AZ31. Bioactive Materials, 2020, 5(1): 153–163

    Article  Google Scholar 

  27. van den Beucken J J, Vos M R, Thüne P C, et al. Fabrication, characterization, and biological assessment of multilayered DNA-coatings for biomaterial purposes. Biomaterials, 2006, 27(5): 691–701

    Article  CAS  Google Scholar 

  28. Duffy E, Florek J, Colon S, et al. Selected DNA aptamers as hydroxyapatite affinity reagents. Analytica Chimica Acta, 2020, 1110: 115–121

    Article  CAS  Google Scholar 

  29. van den Beucken J J J P, Walboomers X F, Leeuwenburgh S C G, et al. Multilayered DNA coatings: In vitro bioactivity studies and effects on osteoblast-like cell behavior. Acta Biomaterialia, 2007, 3(4): 587–596

    Article  CAS  Google Scholar 

  30. Gao W L, Feng B, Ni Y X, et al. Protein adsorption and biomimetic mineralization behaviors of PLL-DNA multilayered films assembled onto titanium. Applied Surface Science, 2010, 257(2): 538–546

    Article  CAS  Google Scholar 

  31. Sakurai T, Yoshinari M, Toyama T, et al. Effects of a multilayered DNA/protamine coating on titanium implants on bone responses. Journal of Biomedical Materials Research Part A, 2016, 104(6): 1500–1509

    Article  CAS  Google Scholar 

  32. Zuo G, Wan Y, Meng X, et al. Synthesis and characterization of a lamellar hydroxyapatite/DNA nanohybrid. Materials Chemistry and Physics, 2011, 126(3): 470–475

    Article  CAS  Google Scholar 

  33. Hu K, Zhuang J, Ding J, et al. Influence of biomacromolecule DNA corrosion inhibitor on carbon steel. Corrosion Science, 2017, 125: 68–76

    Article  CAS  Google Scholar 

  34. Ngourn S C, Butts H A, Petty A R, et al. Quartz crystal microbalance analysis of DNA-templated calcium phosphate mineralization. Langmuir, 2012, 28(33): 12151–12158

    Article  CAS  Google Scholar 

  35. Cui L Y, Zeng R C, Li S Q, et al. Corrosion resistance of layer-by-layer assembled polyvinylpyrrolidone/polyacrylic acid and amorphous silica films on AZ31 magnesium alloys. RSC Advances, 2016, 6(68): 63107–63116

    Article  CAS  Google Scholar 

  36. Saravanan S, Leena R S, Selvamurugan N. Chitosan based biocomposite scaffolds for bone tissue engineering. International Journal of Biological Macromolecules, 2016, 93(Pt B): 1354–1365

    Article  CAS  Google Scholar 

  37. Sruthi R, Balagangadharan K, Selvamurugan N. Polycaprolactone/polyvinylpyrrolidone coaxial electrospun fibers containing veratric acid-loaded chitosan nanoparticles for bone regeneration. Colloids and Surfaces B: Biointerfaces, 2020, 193: 111110

    Article  CAS  Google Scholar 

  38. Yao Q, Li W, Yu S, et al. Multifunctional chitosan/polyvinyl pyrrolidone/45S5 Bioglass®scaffolds for MC3T3-E1 cell stimulation and drug release. Materials Science and Engineering C: Materials for Biological Applications, 2015, 56: 473–480

    Article  CAS  Google Scholar 

  39. Fan F, Zhou C, Wang X, et al. Layer-by-layer assembly of a self-healing anticorrosion coating on magnesium alloys. ACS Applied Materials & Interfaces, 2015, 7(49): 27271–27278

    Article  CAS  Google Scholar 

  40. 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  CAS  Google Scholar 

  41. Yavari S A, Croes M, Akhavan B, et al. Layer by layer coating for bio-functionalization of additively manufactured meta-biomaterials. Additive Manufacturing, 2020, 32: 100991

    Article  CAS  Google Scholar 

  42. Abdelkebir K, Morin-Grognet S, Gaudière F, et al. Biomimetic layer-by-layer templates for calcium phosphate biomineralization. Acta Biomaterialia, 2012, 8(9): 3419–3428

    Article  CAS  Google Scholar 

  43. Liu P, Wang J M, Yu X T, et al. Corrosion resistance of bioinspired DNA-induced Ca-P coating on biodegradable magnesium alloy. Journal of Magnesium and Alloys, 2019, 7(1): 144–154

    Article  CAS  Google Scholar 

  44. Li C Y, Fan X L, Zeng R C, et al. Corrosion resistance of in-situ growth of nano-sized Mg(OH)2 on micro-arc oxidized magnesium alloy AZ31 — Influence of EDTA. Journal of Materials Science and Technology, 2019, 35(6): 1088–1098

    Article  Google Scholar 

  45. Jia Z J, Li M, Liu Q, et al. Micro-arc oxidization of a novel Mg-1Ca alloy in three alkaline KF electrolytes: Corrosion resistance and cytotoxicity. Applied Surface Science, 2014, 292: 1030–1039

    Article  CAS  Google Scholar 

  46. Cui W, Beniash E, Gawalt E, et al. Biomimetic coating of magnesium alloy for enhanced corrosion resistance and calcium phosphate deposition. Acta Biomaterialia, 2013, 9(10): 8650–8659

    Article  CAS  Google Scholar 

  47. Isakhani-Zakaria M, Allahkaram S R, Ramezani-Varzaneh H A. Evaluation of corrosion behaviour of Pb-Co3O4 electrodeposited coating using EIS method. Corrosion Science, 2019, 157: 472–480

    Article  CAS  Google Scholar 

  48. Ramezani-Varzaneh H A, Allahkaram S R, Isakhani-Zakaria M. Effects of phosphorus content on corrosion behavior of trivalent chromium coatings in 3.5 wt.% NaCl solution. Surface and Coatings Technology, 2014, 244: 158–165

    Article  CAS  Google Scholar 

  49. Jorcin J B, Orazem M E, Pébère N, et al. CPE analysis by local electrochemical impedance spectroscopy. Electrochimica Acta, 2006, 51(8–9): 1473–1479

    Article  CAS  Google Scholar 

  50. Gao G J, Zeng M Q, Zhang E L, et al. Dealloying corrosion of anodic and nanometric Mg41Nd5 in solid solution-treated Mg-3Nd-1Li-0.2Zn alloy. Journal of Materials Science and Technology, 2021, 83: 161–178

    Article  Google Scholar 

  51. Li C Y, Fan X L, Cui L Y, et al. Corrosion resistance and electrical conductivity of a nano ATO-doped MAO/methyltrimethoxysilane composite coating on magnesium alloy AZ31. Corrosion Science, 2020, 168: 108570

    Article  CAS  Google Scholar 

  52. Huang Y, Hao M, Nian X F, et al. Strontium and copper co-substituted hydroxyapatite-based coatings with improved antibacterial activity and cytocompatibility fabricated by electrode-position. Ceramics International, 2016, 42(10): 11876–11888

    Article  CAS  Google Scholar 

  53. 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: Materials for Biological Applications, 2018, 91: 218–227

    Article  CAS  Google Scholar 

  54. Lin B P, Zhong M, Zheng C D, et al. Preparation and characterization of dopamine-induced biomimetic hydroxyapatite coatings on the AZ31 magnesium alloy. Surface and Coatings Technology, 2015, 281: 82–88

    Article  CAS  Google Scholar 

  55. Ji X J, Gao L, Liu J C, et al. Corrosion resistance and antibacterial properties of hydroxyapatite coating induced by gentamicin-loaded polymeric multilayers on magnesium alloys. Colloids and Surfaces B: Biointerfaces, 2019, 179: 429–436

    Article  CAS  Google Scholar 

  56. Ji X J, Gao L, Liu J C, et al. Corrosion resistance and antibacterial activity of hydroxyapatite coating induced by ciprofloxacin-loaded polymeric multilayers on magnesium alloy. Progress in Organic Coatings, 2019, 135: 465–474

    Article  CAS  Google Scholar 

  57. 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  CAS  Google Scholar 

  58. Ma J, Wang J, Ai X, et al. Biomimetic self-assembly of apatite hybrid materials: from a single molecular template to bi-/multimolecular templates. Biotechnology Advances, 2014, 32(4): 744–760

    Article  CAS  Google Scholar 

  59. 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: 452–459

    Article  CAS  Google Scholar 

  60. Zeng R C, Lan Z D, Kong L H, et al. Characterization of calcium-modified zinc phosphate conversion coatings and their influences on corrosion resistance of AZ31 alloy. Surface and Coatings Technology, 2011, 205(11): 3347–3355

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Grant No. 52071191), the Natural Science Foundation of Shandong Province (ZR2020QE009), the Research Start-up Fund of Shandong University of Science and Technology (01040125219), and the “Elite Plan” Foundation of Shandong University of Science and Technology (0104060541112).

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Lan-Yue Cui.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, ZY., Wang, D., Liang, LX. et al. Corrosion resistance of Ca-P coating induced by layer-by-layer assembled polyvinylpyrrolidone/DNA multilayer on magnesium AZ31 alloy. Front. Mater. Sci. 15, 391–405 (2021). https://doi.org/10.1007/s11706-021-0560-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11706-021-0560-x

Keywords

Navigation