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.
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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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
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
Zhou K, Zhang Y, Zhang D, et al. Porous hydroxyapatite ceramics fabricated by an ice-templating method. Scripta Materialia, 2011, 64(5): 426–429
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
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
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
Moore R C, Rigali M J, Brady P. Selenite sorption by carbonate substituted apatite. Environmental Pollution, 2016, 218: 1102–1107
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
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
Liao S, Watari F, Xu G, et al. Morphological effects of variant carbonates in biomimetic hydroxyapatite. Materials Letters, 2007, 61(17): 3624–3628
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
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
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
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
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
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
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
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
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
Guo Y, Zhou Y, Jia D. Fabrication of hydroxycarbonate apatite coatings with hierarchically porous structures. Acta Biomaterialia, 2008, 4(2): 334–342
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
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
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).
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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
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DOI: https://doi.org/10.1007/s11706-019-0448-1