Corrosion resistance of biodegradable polymeric layer-by-layer coatings on magnesium alloy AZ31

Abstract

Biocompatible polyelectrolyte multilayers (PEMs) and polysiloxane hybrid coatings were prepared to improve the corrosion resistance of biodegradable Mg alloy AZ31. The PEMs, which contained alternating poly(sodium 4-styrenesulfonate) (PSS) and poly(allylamine hydrochloride) (PAH), were first self-assembled on the surface of the AZ31 alloy substrate via electrostatic interactions, designated as (PAH/PSS)₅/AZ31. Then, the (PAH/PSS)₅/AZ31 samples were dipped into a methyltrimethoxysilane (MTMS) solution to fabricate the PMTMS films, designated as PMTMS/(PAH/PSS)₅/AZ31. The surface morphologies, microstructures and chemical compositions of the films were investigated by FE-SEM, FTIR, XRD and XPS. Potentiodynamic polarization, electrochemical impedance spectroscopy and hydrogen evolution measurements demonstrated that the PMTMS/(PAH/PSS)₅/AZ31 composite film significantly enhanced the corrosion resistance of the AZ31 alloy in Hank’s balanced salt solution (HBSS). The PAH and PSS films effectively improved the deposition of Ca–P compounds including Ca₃(PO₄)₂ and hydroxyapatite (HA). Moreover, the corrosion mechanism of the composite coating was discussed. These coatings could be an alternative candidate coating for biodegradable Mg alloys.

Keywords

magnesium alloy / polyelectrolyte / polysiloxane / corrosion / layer-by-layer

References

[1] Zheng Y F, Gu X N, Witte F. Biodegradable metals. Materials Science and Engineering R: Reports, 2014, 77(2): 1–34

[2] Wang J, Smith C E, Sankar J, . Absorbable magnesium-based stent: physiological factors to consider for in vitro degradation assessments. Regenerative Biomaterials, 2015, 2(1): 59–69

[3] Moravej M, Mantovani D. Biodegradable metals for cardiovascular stent application: interests and new opportunities. International Journal of Molecular Sciences, 2011, 12(7): 4250–4270

[4] Chen Y, Xu Z, Smith C, . Recent advances on the development of magnesium alloys for biodegradable implants. Acta Biomaterialia, 2014, 10(11): 4561–4573

[5] Ishizaki T, Saito N. Rapid formation of a superhydrophobic surface on a magnesium alloy coated with a cerium oxide film by a simple immersion process at room temperature and its chemical stability. Langmuir, 2010, 26(12): 9749–9755

[6] Zeng R C, Qi W C, Cui H Z, . In vitro corrosion of as-extruded Mg–Ca alloys — The influence of Ca concentration. Corrosion Science, 2015, 96: 23–31

[7] Zhang C Y, Zeng R C, Liu C L, . Comparison of calcium phosphate coatings on Mg–Al and Mg–Ca alloys and their corrosion behavior in Hank’s solution. Surface and Coatings Technology, 2010, 204(21–22): 3636–3640

[8] Zeng R C, Sun L, Zheng Y F, . Corrosion and characterisation of dual phase Mg–Li–Ca alloy in Hank’s solution: The influence of microstructural features. Corrosion Science, 2014, 79(79): 69–82

[9] Ishizaki T, Masuda Y, Sakamoto M. Corrosion resistance and durability of superhydrophobic surface formed on magnesium alloy coated with nanostructured cerium oxide film and fluoroalkylsilane molecules in corrosive NaCl aqueous solution. Langmuir, 2011, 27(8): 4780–4788

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

[11] Zeng R C, Lan Z D, Kong L, . 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

[12] Zeng R C, Liu Z G, Zhang F, . Corrosion of molybdate intercalated hydrotalcite coating on AZ31 Mg alloy. Journal of Materials Chemistry A: Materials for Energy and Sustainability, 2014, 2(32): 13049–13057

[13] Zhang F, Liu Z G, Zeng R C, . Corrosion resistance of Mg–Al–LDH coating on magnesium alloy AZ31. Surface and Coatings Technology, 2014, 258: 1152–1158

[14] Li M, Cheng Y, Zheng Y F, . Plasma enhanced chemical vapor deposited silicon coatings on Mg alloy for biomedical application. Surface and Coatings Technology, 2013, 228(9): S262–S265

[15] Lu Y, Wan P, Tan L, . Preliminary study on a bioactive Sr containing Ca–P coating on pure magnesium by a two-step procedure. Surface and Coatings Technology, 2014, 252(9): 79–86

[16] Ishizaki T, Okido M, Masuda Y, . Corrosion resistant performances of alkanoic and phosphonic acids derived self-assembled monolayers on magnesium alloy AZ31 by vapor-phase method. Langmuir, 2011, 27(10): 6009–6017

[17] Guan X, Xiong M, Zeng F, . Enhancement of osteogenesis and biodegradation control by brushite coating on Mg–Nd–Zn–Zr alloy for mandibular bone repair. ACS Applied Materials & Interfaces, 2014, 6(23): 21525–21533

[18] Zeng R C, Qi W C, Song Y W, . In vitro degradation of MAO/PLA coating on Mg–1.21Li–1.12Ca–1.0Y alloy. Frontiers of Materials Science, 2014, 8(4): 343–353

[19] Sankara Narayanan T S N, Park I S, Lee M H. Strategies to improve the corrosion resistance of microarc oxidation (MAO) coated magnesium alloys for degradable implants: Prospects and challenges. Progress in Materials Science, 2014, 60(3): 1–71

[20] Liu P, Pan X, Yang W, . Improved anticorrosion of magnesium alloy via layer-by-layer self-assembly technique combined with micro-arc oxidation. Materials Letters, 2012, 75(1): 118–121

[21] Song L, Song Y, Shan D, . Product/metal ratio (PMR): A novel criterion for the evaluation of electrolytes on micro-arc oxidation (MAO) of Mg and its alloys. Science China Technological Sciences, 2011, 54(10): 2795–2801

[22] Mao L, Shen L, Chen J, . Enhanced bioactivity of Mg–Nd–Zn–Zr alloy achieved with nanoscale MgF₂ surface for vascular stent application. ACS Applied Materials & Interfaces, 2015, 7(9): 5320–5330

[23] Ostrowski N, Lee B, Enick N, . Corrosion protection and improved cytocompatibility of biodegradable polymeric layer-by-layer coatings on AZ31 magnesium alloys. Acta Biomaterialia, 2013, 9(10): 8704–8713

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

[25] Wang B L, Ren K F, Chang H, . Construction of degradable multilayer films for enhanced antibacterial properties. ACS Applied Materials & Interfaces, 2013, 5(10): 4136–4143

[26] Liang J, Hu Y, Wu Y, . Fabrication and corrosion resistance of superhydrophobic hydroxide zinc carbonate film on aluminum substrates. Journal of Nanomaterials, 2013, (1): 1–6

[27] Liu X, Yue Z, Romeo T, . Biofunctionalized anti-corrosive silane coatings for magnesium alloys. Acta Biomaterialia, 2013, 9(10): 8671–8677

[28] Zeng R C, Chen J, Kuang J, . Influence of silane on corrosion resistance of magnesium alloy AZ31 with thermally sprayed aluminum coatings. Rare Metals, 2010, 29(2): 193–197

[29] Zeng R C, Liu L J, Pang T T, . Corrosion resistance of silane-modified hydroxide zinc carbonate film on AZ31 magnesium alloy. Acta Metallurgica Sinica, English Letters, 2015, 28(3): 373–380

[30] Ishizaki T, Sakamoto M. Facile formation of biomimetic color-tuned superhydrophobic magnesium alloy with corrosion resistance. Langmuir, 2011, 27(6): 2375–2381

[31] Zeng R C, Sun X X, Song Y W, . 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

[32] Xu R, Sun G, Li Q, . A dual-responsive superparamagnetic Fe₃O₄/Silica/PAH/PSS material used for controlled release of chemotherapeutic agent, keggin polyoxotungstate, PM-19. Solid State Sciences, 2010, 12(10): 1720–1725

[33] Shaikh J S, Pawar R C, Moholkar A V, . CuO–PAA hybrid films: Chemical synthesis and supercapacitor behavior. Applied Surface Science, 2011, 257(9): 4389–4397

[34] Sun J, Liu X, Meng L, . One-step electrodeposition of self-assembled colloidal particles: a novel strategy for biomedical coating. Langmuir, 2014, 30(37): 11002–11010

[35] Tang Z, Wang Y, Podsiadlo P, . Biomedical applications of layer-by-layer assembly: from biomimetics to tissue engineering. Advanced Materials, 2006, 18(24): 3203–3224

[36] Rusling J F, Hvastkovs E G, Hull D O, . Biochemical applications of ultrathin films of enzymes, polyions and DNA. Chemical Communications, 2008, 39(2): 141–154

[37] Sakr O S, Borchard G. Encapsulation of enzymes in Layer-by-Layer (LbL) structures: latest advances and applications. Biomacromolecules, 2013, 14(7): 2117–2135

[38] Sato K, Anzai J. Dendrimers in layer-by-layer assemblies: synthesis and applications. Molecules, 2013, 18(7): 8440–8460

[39] Xu W, Ledin P A, Shevchenko V V, . Architecture, assembly, and emerging applications of branched functional polyelectrolytes and poly(ionic liquid)s. ACS Applied Materials & Interfaces, 2015, 7(23): 12570–12596

[40] Jang H, Kim D E, Min D H. Self-assembled monolayer mediated surface environment modification of poly(vinylpyrrolidone)-coated hollow Au–Ag nanoshells for enhanced loading of hydrophobic drug and efficient multimodal therapy. ACS Applied Materials & Interfaces, 2015, 7(23): 12789–12796

[41] Pérez-Anes A, Gargouri M, Laure W, . Bioinspired titanium drug eluting platforms based on a poly-β-cyclodextrin-chitosan layer-by-layer self-assembly targeting infections. ACS Applied Materials & Interfaces, 2015, 7(23): 12882–12893

[42] Gentile P, Frongia M E, Cardellach M, . Functionalised nanoscale coatings using layer-by-layer assembly for imparting antibacterial properties to polylactide-co-glycolide surfaces. Acta Biomaterialia, 2015, 21: 35–43

[43] Zeng R C, Dietzel W, Witte F, . Progress and challenge for magnesium alloys as biomaterials. Advanced Engineering Materials, 2008, 10(8): B3–B14

[44] Zomorodian A, Garcia M P, Moura e Silva T, . Corrosion resistance of a composite polymeric coating applied on biodegradable AZ31 magnesium alloy. Acta Biomaterialia, 2013, 9(10): 8660–8670

[45] Cai K, Sui X, Hu Y, . Fabrication of anticorrosive multilayer onto magnesium alloy substrates via spin-assisted layer-by-layer technique. Materials Science and Engineering C, 2011, 31(8): 1800–1808

[46] Caruso F, Furlong D N, Ariga K, . Characterization of polyelectrolyte-protein multilayer films by atomic force microscopy, scanning electron microscopy, and Fourier transform infrared reflection-absorption spectroscopy. Langmuir, 1998, 14(16): 4559–4565

[47] Ibarz G, Dähne L, Donath E, . Smart micro- and nanocontainers for storage, transport, and release. Advanced Materials, 2001, 13(17): 1324–1327

[48] Mark J E. Some interesting things about polysiloxanes. Accounts of Chemical Research, 2004, 37(12): 946–953

[49] Abe Y, Gunji T. Oligo- and polysiloxanes. Progress in Polymer Science, 2004, 29(3): 149–182

[50] Waizy H, Weizbauer A, Modrejewski C, . In vitro corrosion of ZEK100 plates in Hank’s Balanced Salt Solution. Biomedical Engineering Online, 2012, 11(1): 12

[51] Jalota S, Bhaduri S B, Tas A C, . Using a synthetic body fluid (SBF) solution of 27 mM HCO₃^- to make bone substitutes more osteointegrative. Materials Science and Engineering C, 2008, 28(1): 129–140

[52] Zha J, Lu X, Xin Z. A rational design of double layer mesoporous polysiloxane coatings for broadband antireflection. Journal of Sol-Gel Science and Technology, 2015, 74(3): 677–684

[53] Dai T Y, Wang H J, Cao Y, . Preparation, characterization and application of polyaniline/epoxide polysiloxane composite films. Chinese Journal of Polymer Science, 2015, 33(5): 732–742

[54] Hammer P, Schiavetto M G, Dos Santos F C, . Improvement of the corrosion resistance of polysiloxane hybrid coatings by cerium doping. Journal of Non-Crystalline Solids, 2010, 356(44–49): 2606–2612

[55] Jamesh M I, Wu G, Zhao Y, . Electrochemical corrosion behavior of biodegradable Mg–Y–RE and Mg–Zn–Zr alloys in Ringer’s solution and simulated body fluid. Corrosion Science, 2015, 91: 160–184

[56] Cui X J, Lin X Z, Liu C H, . Fabrication and corrosion resistance of a hydrophobic micro-arc oxidation coating on AZ31 Mg alloy. Corrosion Science, 2015, 90: 402–412

[57] Zoltowski P. On the electrical capacitance of interfaces exhibiting constant phase element behaviour. Journal of Electroanalytical Chemistry, 1998, 443(1): 149–154

[58] Zomorodian A, Garcia M P, Moura e Silva T, . Corrosion resistance of a composite polymeric coating applied on biodegradable AZ31 magnesium alloy. Acta Biomaterialia, 2013, 9(10): 8660–8670

[59] Lim T S, Ryu H S, Hong S H. Electrochemical corrosion properties of CeO₂-containing coatings on AZ31 magnesium alloys prepared by plasma electrolytic oxidation. Corrosion Science, 2012, 62: 104–111

[60] Arrabal R, Mota J M, Criado A, . Assessment of duplex coating combining plasma electrolytic oxidation and polymer layer on AZ31 magnesium alloy. Surface and Coatings Techno-logy, 2012, 206(22): 4692–4703

[61] Ander P, Kardan M. Interactions of sodium ions with polyelectrolytes of constant charge density. Macromolecules, 2002, 17(11): 2436–2441

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

Acknowledgments

This work was supported by the National Natural Science Foundation of China (Grant No. 51571134), Scientific Research Foundation of Shandong University of Science and Technology (SDUST) for Recruited Talents (2013RCJJ006), SDUST Research Fund (2014TDJH 104) and Science and Technology Innovation Fund of SDUST for graduate students (YC150358).

RIGHTS & PERMISSIONS

2014 Higher Education Press and Springer-Verlag Berlin Heidelberg