Journal of Coatings Technology and Research

, Volume 16, Issue 2, pp 477–489 | Cite as

Composite PCL/HA/simvastatin electrospun nanofiber coating on biodegradable Mg alloy for orthopedic implant application

  • Abdelrahman I. Rezk
  • Hamouda M. Mousa
  • Joshua Lee
  • Chan Hee ParkEmail author
  • Cheol Sang KimEmail author


Recently, magnesium (Mg) and its alloys have attracted more attention because of their biodegradability and fascinating mechanical properties in the medical field. However, their low corrosion resistance and high degradability in the body have a great effect on mechanical stability and cytocompatibility, which hinders its clinical applications. Therefore, here we introduce a bifunctional composite coating composed of polycaprolactone and synthesized hydroxyapatite nanoparticles (HA-NPs) loaded with simvastatin deposited on the AZ31 alloy via electrospinning technique. The synthesized HA-NPs and composite nanofibers layer were characterized using TEM, FE-SEM, FTIR, and XRD to understand the physiochemical properties of the composite nanofibers compared to pristine polymer and bare alloy. Corrosion resistance was evaluated electrochemically using potentiodynamic polarization and EIS measurements, and biodegradability was evaluated in terms of pH and Mg ions release in SBF solution. The as-prepared coating was found to retard the corrosion and increased the osteocompatibility as resulted in cell culture test, a higher cell attachment and proliferation on the implant biointerface, in addition to releasing simvastatin in a controlled platform.


Magnesium alloys Composite nanofibers Simvastatin HA nanoparticles Biodegradable metal Drug release Surface coating 



This paper was supported by a grant from the Basic Science Research Program through the National Research Foundation of Korea (NRF) by Ministry of Education, Science and Technology (Project No. 2016R1A2A2A07005160) and also partially supported by the program for fostering next-generation researchers in engineering of the National Research Foundation of Korea (NRF) funded by the Ministry of Science, (Project No. 2017H1D8A2030449).


  1. 1.
    Czerwinski, F, “Controlling the Ignition and Flammability of Magnesium for Aerospace Applications.” Corros. Sci., 86 1–16 (2014)Google Scholar
  2. 2.
    Kulekci, MK, “Magnesium and its Alloys Applications in Automotive Industry.” Int. J. Adv. Manuf. Technol., 39 (9) 851–865 (2008)Google Scholar
  3. 3.
    Hu, BH, Tong, KK, Niu, XP, Pinwill, I, “Design and Optimisation of Runner and Gating Systems for the Die Casting of Thin-Walled Magnesium Telecommunication Parts through Numerical Simulation.” J. Mater. Process. Technol., 105 (1) 128–133 (2000)Google Scholar
  4. 4.
    Waizy, H, Seitz, J-M, Reifenrath, J, Weizbauer, A, Bach, F-W, Meyer-Lindenberg, A, Denkena, B, Windhagen, H, “Biodegradable Magnesium Implants for Orthopedic Applications.” J. Mater. Sci., 48 (1) 39–50 (2013)Google Scholar
  5. 5.
    Mousa, HM, Hussein, KH, Woo, HM, Park, CH, Kim, CS, “One-Step Anodization Deposition of Anticorrosive Bioceramic Compounds on AZ31B Magnesium Alloy for Biomedical Application.” Ceram. Int., 41 (9, Part A) 10861–10870 (2015)Google Scholar
  6. 6.
    Mordike, BL, Ebert, T, “Magnesium: Properties—Applications—Potential.” Mater. Sci. Eng. A, 302 (1) 37–45 (2001)Google Scholar
  7. 7.
    Kotoka, R, Yamoah, NK, Mensah-Darkwa, K, Moses, T, Kumar, D, “Electrochemical Corrosion Behavior of Silver Doped Tricalcium Phosphate Coatings on Magnesium for Biomedical Application.” Surf. Coat. Technol., 292 99–109 (2016)Google Scholar
  8. 8.
    Zhao, MJ, Cai, C, Wang, L, Zhang, Z, Zhang, JQ, “Effect of Zinc Immersion Pretreatment on the Electro-Deposition of Ni onto AZ91D Magnesium Alloy.” Surf. Coat. Technol., 205 (7) 2160–2166 (2010)Google Scholar
  9. 9.
    Mousa, HM, Hussein, KH, Pant, HR, Woo, HM, Park, CH, Kim, CS, “In Vitro Degradation Behavior and Cytocompatibility of a Bioceramic Anodization Films on the Biodegradable Magnesium Alloy.” Colloids Surf. A, 488 82–92 (2016)Google Scholar
  10. 10.
    Xue, D, Yun, Y, Schulz, MJ, Shanov, V, “Corrosion protction of biodgradable Magnesium Implants using Anodization.” Mater. Sci. Eng. C, 31 (2) 215–223 (2011)Google Scholar
  11. 11.
    Mousa, HM, Park, CH, Kim, CS, Surface Modification of Magnesium and its Alloys Using Anodization for Orthopedic Implant Application. Magnesium Alloys, InTech (2017)Google Scholar
  12. 12.
    Luo, X, Cui, XT, “Electrochemical Deposition of Conducting Polymer Coatings on Magnesium Surfaces in Ionic Liquid.” Acta Biomater., 7 (1) 441–446 (2011)Google Scholar
  13. 13.
    Wong, HM, Yeung, KWK, Lam, KO, Tam, V, Chu, PK, Luk, KDK, Cheung, KMC, “A Biodegradable Polymer-Based Coating to Control the Performance of Magnesium Alloy Orthopaedic Implants.” Biomaterials, 31 (8) 2084–2096 (2010)Google Scholar
  14. 14.
    Staiger, MP, Pietak, AM, Huadmai, J, Dias, G, “Magnesium and Its Alloys as Orthopedic Biomaterials: A Review.” Biomaterials, 27 (9) 1728–1734 (2006)Google Scholar
  15. 15.
    Hanas, T, Sampath Kumar, TS, Perumal, G, Doble, M, “Tailoring Degradation of AZ31 Alloy by Surface Pre-Treatment and Electrospun PCL Fibrous Coating.” Mater. Sci. Eng. C, 65 43–50 (2016)Google Scholar
  16. 16.
    Soujanya, GK, Hanas, T, Chakrapani, VY, Sunil, BR, Kumar, TSS, “Electrospun Nanofibrous Polymer Coated Magnesium Alloy for Biodegradable Implant Applications.” Proc. Mater. Sci., 5 817–823 (2014)Google Scholar
  17. 17.
    Kim, J, Mousa, HM, Park, CH, Kim, CS, “Enhanced Corrosion Resistance and Biocompatibility of AZ31 Mg Alloy using PCL/ZnO NPs via Electrospinning.” Appl. Surf. Sci., 396 249–258 (2017)Google Scholar
  18. 18.
    Yasin, AS, Mohamed, IMA, Mousa, HM, Park, CH, Kim, CS, “Facile Synthesis of TiO2/ZrO2 Nanofibers/Nitrogen Co-Doped Activated Carbon to Enhance the Desalination and Bacterial Inactivation via Capacitive Deionization.” Sci. Rep., 8 (1) 541 (2018)Google Scholar
  19. 19.
    Jose, MV, Thomas, V, Johnson, KT, Dean, DR, Nyairo, E, “Aligned PLGA/HA Nanofibrous Nanocomposite Scaffolds for Bone Tissue Engineering.” Acta Biomater., 5 (1) 305–315 (2009)Google Scholar
  20. 20.
    Mousa, HM, Abdal-hay, A, Bartnikowski, M, Mohamed, IMA, Yasin, AS, Ivanovski, S, Park, CH, Kim, CS, “A Multifunctional Zinc Oxide/Poly(Lactic Acid) Nanocomposite Layer Coated on Magnesium Alloys for Controlled Degradation and Antibacterial Function.” ACS Biomater. Sci. Eng., 4 (6) 2169–2180 (2018)Google Scholar
  21. 21.
    Kim, H-W, Lee, H-H, Chun, G-S, “Bioactivity and Osteoblast Responses of Novel Biomedical Nanocomposites of Bioactive Glass Nanofiber Filled Poly(Lactic Acid).” J. Biomed. Mater. Res. Part A, 85A (3) 651–663 (2008)Google Scholar
  22. 22.
    Bianco, A, Di Federico, E, Moscatelli, I, Camaioni, A, Armentano, I, Campagnolo, L, Dottori, M, Kenny, JM, Siracusa, G, Gusmano, G, “Electrospun Poly(ε-caprolactone)/Ca-Deficient Hydroxyapatite nanohybrids: Microstructure, Mechanical Properties and Cell Response by Murine Embryonic Stem Cells.” Mater. Sci. Eng. C, 29 (6) 2063–2071 (2009)Google Scholar
  23. 23.
    Fabbri, P, Bondioli, F, Messori, M, Bartoli, C, Dinucci, D, Chiellini, F, “Porous Scaffolds of Polycaprolactone Reinforced with In Situ Generated Hydroxyapatite for Bone Tissue Engineering.” J. Mater. Sci. Mater. Med., 21 (1) 343–351 (2010)Google Scholar
  24. 24.
    Tian, P, Xu, D, Liu, X, “Mussel-Inspired Functionalization of PEO/PCL Composite Coating on a Biodegradable AZ31 Magnesium Alloy.” Colloids Surf. B, 141 327–337 (2016)Google Scholar
  25. 25.
    Bakhsheshi-Rad, HR, Hamzah, E, Kasiri-Asgarani, M, Jabbarzare, S, Iqbal, N, Abdul Kadir, MR, “Deposition of Nanostructured Fluorine-Doped Hydroxyapatite–Polycaprolactone Duplex Coating to Enhance the Mechanical Properties and Corrosion Resistance of Mg Alloy for Biomedical Applications.” Mater. Sci. Eng. C, 60 526–537 (2016)Google Scholar
  26. 26.
    Zomorodian, A, Santos, C, Carmezim, MJ, Silva, TME, Fernandes, JCS, Montemor, MF, “ ‘In-Vitro’ Corrosion Behaviour of the Magnesium Alloy with Al and Zn (AZ31) Protected with a Biodegradable Polycaprolactone Coating Loaded with Hydroxyapatite and Cephalexin.” Electrochim. Acta, 179 431–440 (2015)Google Scholar
  27. 27.
    Mousa, HM, Tiwari, AP, Kim, J, Adhikari, SP, Park, CH, Kim, CS, “A Novel In Situ Deposition of Hydroxyapatite Nanoplates using Anodization/Hydrothermal Process Onto Magnesium Alloy Surface Towards Third Generation Biomaterials.” Mater. Lett., 164 144–147 (2016)Google Scholar
  28. 28.
    Abdal-hay, A, Vanegas, P, Hamdy, AS, Engel, FB, Lim, JH, “Preparation and Characterization of Vertically Arrayed Hydroxyapatite Nanoplates on Electrospun Nanofibers for Bone Tissue Engineering.” Chem. Eng. J., 254 612–622 (2014)Google Scholar
  29. 29.
    Shikinami, Y, Okuno, M, “Bioresorbable Devices Made of Forged Composites of Hydroxyapatite (HA) Particles and Poly l-lactide (PLLA). Part II: Practical Properties of Miniscrews and Miniplates.” Biomaterials, 22 (23) 3197–3211 (2001)Google Scholar
  30. 30.
    Fang, R, Zhang, E, Xu, L, Wei, S, “Electrospun PCL/PLA/HA Based Nanofibers as Scaffold for Osteoblast-Like Cells.” J. Nanosci. Nanotechnol., 10 (11) 7747–7751 (2010)Google Scholar
  31. 31.
    Dong, H, Li, Q, Tan, C, Bai, N, Cai, P, “Bi-Directional Controlled Release of Ibuprofen and Mg2 + from Magnesium Alloys Coated by Multifunctional Composite.” Mater. Sci. Eng. C, 68 512–518 (2016)Google Scholar
  32. 32.
    Yoo, HS, Kim, TG, Park, TG, “Surface-Functionalized Electrospun Nanofibers for Tissue Engineering and Drug Delivery.” Adv. Drug Deliv. Rev., 61 (12) 1033–1042 (2009)Google Scholar
  33. 33.
    Rezk, AI, Rajan Unnithan, A, Hee Park, C, Sang Kim, C, “Rational Design of Bone Extracellular Matrix Mimicking Tri- Layered Composite Nanofibers for Bone Tissue Regeneration.” Chem. Eng. J., 350 812 (2018)Google Scholar
  34. 34.
    Thylin, MR, McConnell, JC, Schmid, MJ, Reckling, RR, Ojha, J, Bhattacharyya, I, Marx, DB, Reinhardt, RA, “Effects of Simvastatin Gels on Murine Calvarial Bone.” J. Periodontol., 73 (10) 1141–1148 (2002)Google Scholar
  35. 35.
    Tang, ZG, Black, RA, Curran, JM, Hunt, JA, Rhodes, NP, Williams, DF, “Surface Properties and Biocompatibility of Solvent-Cast Poly[ε-Caprozlactone] Films.” Biomaterials, 25 (19) 4741–4748 (2004)Google Scholar
  36. 36.
    Gautam, S, Dinda, AK, Mishra, NC, “Fabrication and Characterization of PCL/Gelatin Composite Nanofibrous Scaffold for Tissue Engineering Applications by Electrospinning Method.” Mater. Sci. Eng. C, 33 (3) 1228–1235 (2013)Google Scholar
  37. 37.
    Mousa, HM, Lee, DH, Park, CH, Kim, CS, “A Novel Simple Strategy for In Situ Deposition of Apatite Layer on AZ31B Magnesium Alloy for Bone Tissue Regeneration.” Appl. Surf. Sci., 351 55–65 (2015)Google Scholar
  38. 38.
    Kouhi, M, Morshed, M, Varshosaz, J, Fathi, MH, “Poly (ε-Caprolactone) Incorporated Bioactive Glass Nanoparticles and Simvastatin Nanocomposite Nanofibers: Preparation, Characterization and In Vitro Drug Release for Bone Regeneration Applications.” Chem. Eng. J., 228 1057–1065 (2013)Google Scholar
  39. 39.
    Rehman, I, Bonfield, W, “Characterization of Hydroxyapatite and Carbonated Apatite by Photo Acoustic FTIR Spectroscopy.” J. Mater. Sci. Mater. Med., 8 (1) 1–4 (1997)Google Scholar
  40. 40.
    Fujihara, K, Kotaki, M, Ramakrishna, S, “Guided Bone Regeneration Membrane Made of Polycaprolactone/Calcium Carbonate Composite Nano-fibers.” Biomaterials, 26 (19) 4139–4147 (2005)Google Scholar
  41. 41.
    Lebourg, M, Suay Antón, J, Gomez Ribelles, JL, “Characterization of Calcium Phosphate Layers Grown on Polycaprolactone for Tissue Engineering Purposes.” Compos. Sci. Technol., 70 (13) 1796–1804 (2010)Google Scholar
  42. 42.
    Mousa, HM, Hussein, KH, Raslan, AA, Lee, J, Woo, HM, Park, CH, Kim, CS, “Amorphous Apatite Thin Film Formation on a Biodegradable Mg Alloy for Bone Regeneration: Strategy, Characterization, Biodegradation, and In Vitro Cell Study.” RSC Adv., 6 (27) 22563–22574 (2016)Google Scholar
  43. 43.
    Gu, Y, Bandopadhyay, S, Chen, C-F, Guo, Y, Ning, C, “Effect of Oxidation Time on the Corrosion Behavior of Micro-Arc Oxidation Produced AZ31 Magnesium Alloys in Simulated Body Fluid.” J. Alloy. Compd., 543 109–117 (2012)Google Scholar
  44. 44.
    Wen, C, Guan, S, Peng, L, Ren, C, Wang, X, Hu, Z, “Characterization and Degradation Behavior of AZ31 Alloy Surface Modified by Bone-Like Hydroxyapatite for Implant Applications.” Appl. Surf. Sci., 255 (13) 6433–6438 (2009)Google Scholar
  45. 45.
    Ayukawa, Y, Yasukawa, E, Moriyama, Y, Ogino, Y, Wada, H, Atsuta, I, Koyano, K, “Local Application of Statin Promotes Bone Repair Through the Suppression of Osteoclasts and the Enhancement of Osteoblasts at Bone-Healing Sites in Rats.” Oral Surg. Oral Med. Oral Pathol. Oral Radiol. Endod., 107 (3) 336–342 (2009)Google Scholar

Copyright information

© American Coatings Association 2018

Authors and Affiliations

  1. 1.Department of Bionanosystem EngineeringChonbuk National UniversityJeonjuRepublic of Korea
  2. 2.Deptment of Engineering Materials and Mechanical Design, Faculty of EngineeringSouth Valley UniversityQenaEgypt
  3. 3.Division of Mechanical Design EngineeringChonbuk National UniversityJeonjuRepublic of Korea

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