Hostname: page-component-7479d7b7d-wxhwt Total loading time: 0 Render date: 2024-07-12T02:09:31.093Z Has data issue: false hasContentIssue false

Synthesis and evaluation of protective poly(lactic acid) and fluorine-doped hydroxyapatite–based composite coatings on AZ31 magnesium alloy

Published online by Cambridge University Press:  24 October 2019

Prabaha Sikder*
Affiliation:
MIME Department, The University of Toledo, Toledo, Ohio 43606, USA
Yufu Ren
Affiliation:
MIME Department, The University of Toledo, Toledo, Ohio 43606, USA
Sarit B. Bhaduri
Affiliation:
MIME Department, The University of Toledo, Toledo, Ohio 43606, USA
*
a)Address all correspondence to these authors. e-mail: james.sikder@gmail.com, Prabaha.sikder@rockets.utoledo.edu
Get access

Abstract

Magnesium (Mg) alloys have received considerable attention as favorable orthopedic implant materials. However, their uncontrolled degradation in the physiological environment has led to premature implant failure. Thus, to address this problem, the present study was focused on developing protective monolayer coatings of fluorine-doped hydroxyapatite (FHA) and a bilayer coating of FHA and poly(lactic acid) (FHA–PLA) on AZ31 Mg. The synthesis involved microwave irradiation which helped in rapid synthesis of FHA coatings and spin coating for developing the PLA layer. Results revealed the formation of dense and defect-free FHA–PLA hybrid coatings. Importantly, they helped in significant reduction of galvanic–corrosion reactions of AZ31 in a physiological medium. The corrosion current density of FHA/PLA–coated samples was about two orders of magnitude lower than uncoated samples. Their lower weight losses further confirmed the coatings’ corrosion resistance. Combined, the as-synthesized FHA–PLA coatings can provide favorable corrosion protection to AZ31 Mg.

Type
Article
Copyright
Copyright © Materials Research Society 2019 

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

Footnotes

b)

These authors contributed equally to this work.

References

Staiger, M.P., Pietak, A.M., Huadmai, J., and Dias, G.: Magnesium and its alloys as orthopedic biomaterials: A review. Biomaterials 27, 1728 (2006).CrossRefGoogle ScholarPubMed
Witte, F.: The history of biodegradable magnesium implants: A review. Acta Biomater. 6, 1680 (2010).CrossRefGoogle ScholarPubMed
Shadanbaz, S. and Dias, G.J.: Calcium phosphate coatings on magnesium alloys for biomedical applications: A review. Acta Biomater. 8, 20 (2012).CrossRefGoogle ScholarPubMed
Nabiyouni, M., Ren, Y., and Bhaduri, S.B.: Magnesium substitution in the structure of orthopedic nanoparticles: A comparison between amorphous magnesium phosphates, calcium magnesium phosphates, and hydroxyapatites. Mater. Sci. Eng. C 52, 11 (2015).CrossRefGoogle ScholarPubMed
Sikder, P. and Bhaduri, S.B.: Microwave assisted synthesis and characterization of single-phase tabular hexagonal newberyite, an important bioceramic. J. Am. Ceram. Soc. 101, 2537 (2018).CrossRefGoogle Scholar
Tamimi, F., Le Nihouannen, D., Bassett, D.C., Ibasco, S., Gbureck, U., Knowles, J., Wright, A., Flynn, A., Komarova, S.V., and Barralet, J.E.: Biocompatibility of magnesium phosphate minerals and their stability under physiological conditions. Acta biomaterialia 7, 2678 (2011).CrossRefGoogle ScholarPubMed
Witte, F., Kaese, V., Haferkamp, H., Switzer, E., Meyer-Lindenberg, A., Wirth, C.J., and Windhagen, H.: In vivo corrosion of four magnesium alloys and the associated bone response. Biomaterials 26, 3557 (2005).CrossRefGoogle ScholarPubMed
Ren, Y., Sikder, P., Lin, B., and Bhaduri, S.B.: Microwave assisted coating of bioactive amorphous magnesium phosphate (AMP) on polyetheretherketone (PEEK). Mater. Sci. Eng. C 85, 107 (2018).CrossRefGoogle Scholar
Touny, A.H., Sikder, P., Saleh, M.M., and Bhaduri, S.B.: Facile synthesis and characterization of biphasic magnesium phosphate bioceramic nanosheets by a reflux approach. Mater. Res. Express 6 (2019).CrossRefGoogle Scholar
Sikder, P., Bhaduri, S.B., Ong, J.L., and Guda, T.: Silver (Ag) doped magnesium phosphate microplatelets as next-generation antibacterial orthopedic biomaterials. J. Biomed. Mater. Res., Part B 1 (2019).Google Scholar
Hornberger, H., Virtanen, S., and Boccaccini, A.R.: Biomedical coatings on magnesium alloys–A review. Acta Biomater. 8, 2442 (2012).CrossRefGoogle ScholarPubMed
Kraus, T., Fischerauer, S.F., Hanzi, A.C., Uggowitzer, P.J., Loffler, J.F., and Weinberg, A.M.: Magnesium alloys for temporary implants in osteosynthesis: In vivo studies of their degradation and interaction with bone. Acta Biomater. 8, 1230 (2012).CrossRefGoogle ScholarPubMed
Dorozhkin, S.V. and Epple, M.: Biological and medical significance of calcium phosphates. Angew. Chem., Int. Ed. 41, 3130 (2002).3.0.CO;2-1>CrossRefGoogle ScholarPubMed
Koju, N., Sikder, P., Gaihre, B., and B Bhaduri, S.: Smart injectable self-setting monetite based bioceramics for orthopedic applications. Materials 11, 1258 (2018).CrossRefGoogle ScholarPubMed
Sikder, P., Koju, N., Lin, B., and Bhaduri, S.B.: Conventionally sintered hydroxyapatite–barium titanate piezo-biocomposites. Trans. Indian Inst. Met. 72, 20112018 (2019).CrossRefGoogle Scholar
Dorozhkin, S.V.: Calcium orthophosphate-based bioceramics. Materials 6, 3840 (2013).CrossRefGoogle ScholarPubMed
Liu, G.Y., Hu, J., Ding, Z.K., and Wang, C.: Bioactive calcium phosphate coating formed on micro-arc oxidized magnesium by chemical deposition. Appl. Surf. Sci. 257, 2051 (2011).CrossRefGoogle Scholar
Waterman, J., Pietak, A., Birbilis, N., Woodfield, T., Dias, G., and Staiger, M.P.: Corrosion resistance of biomimetic calcium phosphate coatings on magnesium due to varying pretreatment time. Mater. Sci. Eng., B 176, 1756 (2011).CrossRefGoogle Scholar
Cui, W., Beniash, E., Gawalt, E., Xu, Z., and Sfeir, C.: Biomimetic coating of magnesium alloy for enhanced corrosion resistance and calcium phosphate deposition. Acta Biomater. 9, 8650 (2013).CrossRefGoogle ScholarPubMed
Yang, J.X., Cui, F.Z., Yin, Q.S., Zhang, Y., Zhang, T., and Wang, X.M.: Characterization and degradation study of calcium phosphate coating on magnesium alloy bone implant in vitro. IEEE Trans. Plasma Sci. 37, 1161 (2009).CrossRefGoogle Scholar
Yanovska, A., Kuznetsov, V., Stanislavov, A., Danilchenko, S., and Sukhodub, L.: Calcium–phosphate coatings obtained biomimetically on magnesium substrates under low magnetic field. Appl. Surf. Sci. 258, 8577 (2012).CrossRefGoogle Scholar
Cortes, D.A., Lopez, H.Y., and Mantovani, D.: Spontaneous and biomimetic apatite formation on pure magnesium. Thermec 2006, Vol. 539–543, Pts 1–5 (2007); p. 589.Google Scholar
Cui, F-z., Yang, J-x., Jiao, Y-p., Yin, Q-s., Zhang, Y., and Lee, I-S.: Calcium phosphate coating on magnesium alloy for modification of degradation behavior. Front. Mater. Sci. China 2, 143 (2008).CrossRefGoogle Scholar
Wang, H.X., Guan, S.K., Wang, X., Ren, C.X., and Wang, L.G.: In vitro degradation and mechanical integrity of Mg–Zn–Ca alloy coated with Ca-deficient hydroxyapatite by the pulse electrodeposition process. Acta Biomater. 6, 1743 (2010).CrossRefGoogle ScholarPubMed
Guan, R.G., Johnson, I., Cui, T., Zhao, T., Zhao, Z.Y., Li, X., and Liu, H.: Electrodeposition of hydroxyapatite coating on Mg–4.0Zn–1.0Ca–0.6Zr alloy and in vitro evaluation of degradation, hemolysis, and cytotoxicity. J. Biomed. Mater. Res., Part A 100, 999 (2012).CrossRefGoogle ScholarPubMed
Song, Y.W., Shan, D.Y., and Han, E.H.: Electrodeposition of hydroxyapatite coating on AZ91D magnesium alloy for biomaterial application. Mater. Lett. 62, 3276 (2008).CrossRefGoogle Scholar
Rojaee, R., Fathi, M., and Raeissi, K.: Controlling the degradation rate of AZ91 magnesium alloy via sol–gel derived nanostructured hydroxyapatite coating. Mater. Sci. Eng. A 33, 3817 (2013).CrossRefGoogle ScholarPubMed
Tomozawa, M. and Hiromoto, S.: Growth mechanism of hydroxyapatite-coatings formed on pure magnesium and corrosion behavior of the coated magnesium. Appl. Surf. Sci. 257, 8253 (2011).CrossRefGoogle Scholar
Tomozawa, M., Hiromoto, S., and Harada, Y.: Microstructure of hydroxyapatite-coated magnesium prepared in aqueous solution. Surf. Coat. Technol. 204, 3243 (2010).CrossRefGoogle Scholar
Sikder, P., Koju, N., Ren, Y., Goel, V.K., Phares, T., Lin, B., and Bhaduri, S.B.: Development of single-phase silver-doped antibacterial CDHA coatings on Ti6Al4V with sustained release. Surf. Coat. Technol. 342, 105 (2018).CrossRefGoogle Scholar
Dhert, W., Klein, C., Jansen, J., Van der Velde, E., Vriesde, R., Rozing, P., and De Groot, K.: A histological and histomorphometrical investigation of fluorapatite, magnesiumwhitlockite, and hydroxylapatite plasma-sprayed coatings in goats. J. Biomed. Mater. Res. 27, 127 (1993).CrossRefGoogle ScholarPubMed
Nabiyouni, M., Zhou, H., Luchini, T.J., and Bhaduri, S.B.: Formation of nanostructured fluorapatite via microwave assisted solution combustion synthesis. Mater. Sci. Eng., C 37, 363 (2014).CrossRefGoogle ScholarPubMed
Li, J., Song, Y., Zhang, S., Zhao, C., Zhang, F., Zhang, X., Cao, L., Fan, Q., and Tang, T.: In vitro responses of human bone marrow stromal cells to a fluoridated hydroxyapatite coated biodegradable Mg–Zn alloy. Biomaterials 31, 5782 (2010).CrossRefGoogle ScholarPubMed
Wang, J., Chao, Y., Wan, Q., Zhu, Z., and Yu, H.: Fluoridated hydroxyapatite coatings on titanium obtained by electrochemical deposition. Acta Biomater. 5, 1798 (2009).CrossRefGoogle ScholarPubMed
Guha-Chowdhury, N., Clark, A., and Sissons, C.: Inhibition of purified enolases from oral bacteria by fluoride. Mol. Oral Microbiol. 12, 91 (1997).Google ScholarPubMed
Koju, N., Sikder, P., Ren, Y., Zhou, H., and Bhaduri, S.B.: Biomimetic coating technology for orthopedic implants. Curr. Opin. Chem. Eng. 15, 49 (2017).CrossRefGoogle Scholar
Bhaduri, S.B., Goel, V.K., Ren, Y., and Sikder, P.: Bifunctional bioactive antibacterial coatings, and process for coating implant surfaces therewith. Google Patents, 2018.Google Scholar
Zhou, H., Nabiyouni, M., and Bhaduri, S.B.: Microwave assisted apatite coating deposition on Ti6Al4V implants. Mater. Sci. Eng., C 33, 4435 (2013).CrossRefGoogle ScholarPubMed
Ren, Y., Zhou, H., Nabiyouni, M., and Bhaduri, S.B.: Rapid coating of AZ31 magnesium alloy with calcium deficient hydroxyapatite using microwave energy. Mater. Sci. Eng., C 49, 364 (2015).CrossRefGoogle ScholarPubMed
Ren, Y., Babaie, E., Lin, B., and Bhaduri, S.B.: Microwave-assisted magnesium phosphate coating on the AZ31 magnesium alloy. Biomed. Mater. 12, 045026 (2017).CrossRefGoogle ScholarPubMed
Sikder, P., Grice, C., and Bhaduri, S.B.: Processing-structure-property correlations of crystalline antibacterial magnesium phosphate (newberyite) coatings and their in vitro effect. Surf. Coat. Technol. 374, 276 (2019).CrossRefGoogle Scholar
Sikder, P., Grice, C.R., Lin, B., Goel, V.K., and Bhaduri, S.B.: Single-phase, antibacterial trimagnesium phosphate hydrate coatings on polyetheretherketone (PEEK) implants by rapid microwave irradiation technique. ACS Biomater. Sci. Eng. 4, 2767 (2018).CrossRefGoogle Scholar
Ren, Y., Babaie, E., and Bhaduri, S.B.: Nanostructured amorphous magnesium phosphate/poly(lactic acid) composite coating for enhanced corrosion resistance and bioactivity of biodegradable AZ31 magnesium alloy. Prog. Org. Coat. 118, 1 (2018).CrossRefGoogle Scholar
Zheludkevich, M., Serra, R., Montemor, M., Salvado, I.M., and Ferreira, M.: Corrosion protective properties of nanostructured sol–gel hybrid coatings to AA2024-T3. Surf. Coat. Technol. 200, 3084 (2006).CrossRefGoogle Scholar
Xu, L. and Yamamoto, A.: Characteristics and cytocompatibility of biodegradable polymer film on magnesium by spin coating. Colloids Surf., B 93, 67 (2012).CrossRefGoogle ScholarPubMed
Ren, Y.: Microwave Assisted Synthesis of Alkaline Earth Phosphate Coating and its Applications for Biomedical Implants (University of Toledo, 2017).Google Scholar
Gadaleta, S.J., Paschalis, E.P., Betts, F., Mendelsohn, R., and Boskey, A.L.: Fourier transform infrared spectroscopy of the solution-mediated conversion of amorphous calcium phosphate to hydroxyapatite: New correlations between X-ray diffraction and infrared data. Calcif. Tissue Int. 58, 9 (1996).CrossRefGoogle ScholarPubMed
Gu, X., Zheng, W., Cheng, Y., and Zheng, Y.: A study on alkaline heat treated Mg–Ca alloy for the control of the biocorrosion rate. Acta Biomater. 5, 2790 (2009).CrossRefGoogle Scholar
Li, X., Weng, Z., Yuan, W., Luo, X., Wong, H.M., Liu, X., Wu, S., Yeung, K., Zheng, Y., and Chu, P.K.: Corrosion resistance of dicalcium phosphate dihydrate/poly(lactic-co-glycolic acid) hybrid coating on AZ31 magnesium alloy. Corros. Sci. 102, 209 (2016).CrossRefGoogle Scholar
Bakhsheshi-Rad, H., Hamzah, E., Abdul-Kadir, M., Saud, S.N., Kasiri-Asgarani, M., and Ebrahimi-Kahrizsangi, R.: The mechanical properties and corrosion behavior of double-layered nano hydroxyapatite-polymer coating on Mg–Ca alloy. J. Mater. Eng. Perform. 24, 4010 (2015).CrossRefGoogle Scholar
Zeng, R-C., Qi, W-C., Song, Y-W., He, Q-K., Cui, H-Z., and Han, E-H.: In vitro degradation of MAO/PLA coating on Mg–1.21Li–1.12Ca–1.0Y alloy. Front. Mater. Sci. 8, 343 (2014).CrossRefGoogle Scholar
Yamamoto, A. and Hiromoto, S.: Effect of inorganic salts, amino acids and proteins on the degradation of pure magnesium in vitro. Mater. Sci. Eng., C 29, 1559 (2009).CrossRefGoogle Scholar
Song, Y.W., Shan, D.Y., Chen, R.S., Zhang, F., and Han, E.H.: Biodegradable behaviors of AZ31 magnesium alloy in simulated body fluid. Mater. Sci. Eng., C 29, 1039 (2009).CrossRefGoogle Scholar
Meng, E., Guan, S., Wang, H., Wang, L., Zhu, S., Hu, J., Ren, C., Gao, J., and Feng, Y.: Effect of electrodeposition modes on surface characteristics and corrosion properties of fluorine-doped hydroxyapatite coatings on Mg–Zn–Ca alloy. Appl. Surf. Sci. 257, 4811 (2011).CrossRefGoogle Scholar
Seuss, F., Seuss, S., Turhan, M.C., Fabry, B., and Virtanen, S.: Corrosion of Mg alloy AZ91D in the presence of living cells. J. Biomed. Mater. Res., Part B 99, 276 (2011).CrossRefGoogle ScholarPubMed
Bakhsheshi-Rad, H., Hamzah, E., Daroonparvar, M., Ebrahimi-Kahrizsangi, R., and Medraj, M.: In vitro corrosion inhibition mechanism of fluorine-doped hydroxyapatite and brushite coated Mg–Ca alloys for biomedical applications. Ceram. Int. 40, 7971 (2014).CrossRefGoogle Scholar
Jalota, S., Bhaduri, S.B., and Tas, A.C.: In vitro testing of calcium phosphate (HA, TCP, and biphasic HA-TCP) whiskers. J. Biomed. Mater. Res., Part A 78, 481 (2006).CrossRefGoogle ScholarPubMed
Fathi, M. and Zahrani, E.M.: Mechanical alloying synthesis and bioactivity evaluation of nanocrystalline fluoridated hydroxyapatite. J. Cryst. Growth 311, 1392 (2009).CrossRefGoogle Scholar
Jalota, S., Bhaduri, S.B., and Tas, A.C.: Effect of carbonate content and buffer type on calcium phosphate formation in SBF solutions. J. Mater. Sci. Mater. Med. 17, 697 (2006).CrossRefGoogle ScholarPubMed