Multifunctional hopeite nanocoating on Ti64 substrates by pulsed laser deposition and radio frequency magnetron sputtering for orthopedic implant applications: A comparative study

Abstract

Functionalized implants demonstrate an upgraded approach in orthopedic implants, aiming to achieve long term success through improved bio integration. Bioceramic coatings with multifunctionality have arisen as an effective substitute for conventional coatings, owing to their combination of various properties that are essential for bio-implants, such as osteointegration and antibacterial character. In the present study, thin hopeite coatings were produced by Pulsed laser deposition (PLD) and radio frequency magnetron sputtering (RFMS) on Ti64 substrates. The obtained hopeite coatings were annealed at 500 °C in ambient air and studied in terms of surface morphology, phase composition, surface roughness, adhesion strength, antibacterial efficacy, apatite forming ability, and surface wettability by scanning electron microscope (SEM), X-ray diffraction (XRD), atomic force microscope (AFM), tensometer, fluorescence-activated cell sorting (FACS), simulated body fluid (SBF) immersion test and contact angle goniometer, respectively. Furthermore, based on promising results obtained in the present work it can be summarized that the new generation multifunctional hopeite coating synthesized by two alternative new process routes of PLD and RFMS on Ti64 substrates, provides effective alternatives to conventional coatings, largely attributed to strong osteointegration and antibacterial character of deposited hopeite coating ensuring the overall stability of metallic orthopedic implants.

Keywords

hopeite / Ti64 alloy / pulsed laser deposition / magnetron sputtering / coating / implant

References

[1] YangW H, XiX F, SiY, HuangS, WangJ F, CaiK Y. Surface engineering of titanium alloy substrates with multilayered biomimetic hierarchical films to regulate the growth behaviors of osteoblasts [J]. Acta Biomaterialia, 2014, 10(10): 4525-4536

[2] HallabN J, VermesC, MessinaC, RoebuckK A, GlantT T, JacobsJ J. Concentration and composition dependent effects of metal ions on human MG-63 osteoblasts [J]. Journal of Biomedical Materials Research, 2002, 60(3): 420-433

[3] SunZ L, WatahaJ C, HanksC T. Effects of metal ions on osteoblast like cell metabolism and differentiation [J]. Journal of Biomedical Materials Research, 1997, 34(1): 29-37

[4] ThompsonG J, PueloD A. TC4 ion solution inhibition of osteogenic cell phenotype as a function of differentiation time course in vitro [J]. Biomaterials, 1996, 17(20): 1949-1954

[5] WangJ Y, WicklundB H, GustiloR B, TsukayamaD T. Prosthetic metals interfere with the functions of human osteoblast cells in vitro [J]. Clinical Orthopaedics and Related Research, 1997, 339: 216-226

[6] MohammedM T, KhanZ A, SiddiqueeA NTitanium and its alloys the imperative materials for biomedical applications [C], 2012, India, ICRTET. Meerut, 9195

[7] YuJ, ChuX, CaiY, TongP, YaoJ. Preparation and characterization of antimicrobial nano hydroxyapatite composites [J]. Materials Science and Engineering C, 2014, 37: 54-59

[8] ParkJ W, ParkK B, SuhJ Y. Effects of calcium ion incorporation on bone healing of Ti6Al4V alloy implants in rabbit tibiae [J]. Biomaterials, 2007, 28(22): 3306-3313

[9] SridharT M, ArumugamT K, RajeswariS, SubbaiyanM. Electrochemical behaviour of hydroxyapatite-coated stainless-steel implants [J]. Journal of Materials Science Letters, 1997, 16(22): 1964-1966

[10] YamaguchiM, OishiH, SuketaY. Stimulatory effect of zinc on bone formation in tissue culture [J]. Journal of Materials Science Letters, 1987, 36(22): 4007-4012

[11] EberleJ, SchmidmayerS, ErbenR G, StangassingerM, RothH P. Skeletal effects of zinc deficiency in growing rats [J]. Journal of Trace Elements in Medicine and Biology, 1999, 13(1): 21-262

[12] ChenD, WaiteL C, PierceW M. In vitro effects of zinc on markers of bone formation [J]. Biological Trace Element Research, 1999, 68(3): 225-234

[13] ShibliS M A, JayalekshmiA C. Development of phosphate inter layered hydroxyapatite coating for stainless steel implant [J]. Applied Surface Science, 2008, 254(13): 4103-4110

[14] HerschkeL, RottsteggeJ, LieberwirthI, WegnerG. Zinc phosphate as versatile material for potential biomedical applications, Part 1 [J]. Journal of Materials Science: Materials in Medicine, 2006, 17(1): 81-94

[15] NriaguJ O. Solubility equilibrium constant of α-hopeite [J]. Geochimica et Cosmochimica Acta, 1973, 37(6): 2357-2361

[16] UoM, SjorenG, SundhA, WatariF, BergmanM, LernerU. Cytotoxicity and bonding property of dental ceramics [J]. Dental Materials, 2003, 19(6): 487-492

[17] AttarN, TamL E, MccombD. Mechanical and physical properties of contemporary dental luting agents [J]. Journal of Prosthetic Dentistry, 2003, 89(2): 127-134

[18] HoriuchiS, AsaokaK, TanakaE. Development of a novel cement by conversion of hopeite in set zinc phosphate cement into biocompatible apatite [J]. Bio-Medical Materials and Engineering, 2009, 19(2): 121-1313

[19] LinF H, HsuY S, LinS H, SunJ S. The effect of Ca/P concentration and temperature of simulated body fluid on the growth of hydroxyapatite coating on alkali-treated 316L stainless steel [J]. Biomaterials, 2002, 23(19): 4029-4038

[20] KokuboT, ItoS, SakkaS, YamamuroT. Formation of a high strength bioactive glass-ceramic in the system MgO-CaO-SiO₂-P₂O₅ [J]. Journal of Materials Science, 1986, 21: 536-540

[21] KokuboT, HayashiT, SakkaS, KitsugiT, YamamuroT. Bonding between bioactive glasses, glass-ceramics or ceramics in simulated body fluid [J]. Journal of the Ceramic Association, 1987, 95: 785-791

[22] KokuboT, KushitaniH, SakkaS, KitsugiT, YamamuroT. Solutions able to reproduce in vivo surface-structure changes in bioactive glass-ceramics A-W3 [J]. Journal of Biomedical Materials Research, 1990, 24(6): 721-734

[23] KokuboT. Surface chemistry of bioactive glass-ceramics [J]. Journal of Non-Crystalline Solids, 1990, 120(1–3): 138-151

[24] AzaP N D, GuitianF, AzaS D. Bioactivity of wollastonite ceramics: In vitro evaluation [J]. Scripta Metallurgica et Materialia, 1994, 31: 1001-1005

[25] LiuD M. Bioactive glass-ceramic: Formation, characterization and bioactivity [J]. Materials Chemistry and Physics, 1994, 36: 294-303

[26] AzaP N D, LuklinskaZ B, AnseauM R, GuitianF, AzaS D E. Bioactivity of pseudowollastonite in human saliva [J]. Journal of Dentistry, 1999, 27: 107-113

[27] AzaP N D, LuklinskaZ. Effect of the glass-ceramic microstructure on its in vitro bioactivity [J]. Journal of Materials Science: Materials in Medicine, 2003, 14: 891-898

[28] AzaP N D, LuklinskaZ B, AnseauM R. Bioactivity of diopside ceramic in human parotid saliva [J]. Journal of Biomedical Materials Research, 2005, 73: 54-60

[29] AlemanyM I, VelasquezP, de la Casa-LilloM A, AzaP N D. Effect of materials processing methods on the in vitro bioactivity of wollastonite glass-ceramic materials [J]. Journal of Non-Crystalline Solids, 2005, 351: 1716-1726

[30] KhanA N, LuJ. Thermal cyclic behavior of air plasma sprayed thermal barrier coatings sprayed on stainless steel substrates [J]. Surface and Coatings Technology, 2007, 201(8): 4653-4658

[31] OskuieA A, AfsharA, HasannejadH. Effect of current density on DC electrochemical phosphating of stainless steel 316 [J]. Surface and Coatings Technology, 2010, 205(7): 2302-2306

[32] IonitaD, UngureanuC, DemetrescuI. Electrochemical and antibacterial performance of CoCrMo alloy coated with hydroxyapatite or silver nanoparticles [J]. Journal of Materials Engineering and Performance, 2013, 22: 3584-3591

[33] KavithaC, NarayananT S N S, RavichandranK, ParkI L S, LeeM H. Deposition of zinc-zinc phosphate composite coatings on steel by cathodic electrochemical treatment [J]. Journal of Coatings Technology and Research, 2014, 11(3): 431-442

[34] ValanezhadA, TsuruK, MarutaM, KawachiG, MatsuyaS, IshikawaK. Zinc phosphate coating on 316L-type stainless steel using hydrothermal treatment [J]. Surface and Coatings Technology, 2010, 205(7): 2538-2541

[35] RadH R B, HamzahE, KadirM R A, SaudS. The mechanical properties and corrosion behavior of double-layered nano hydroxyapatite-polymer coating on Mg-Ca alloy [J]. Journal of Materials Engineering and Performance, 2015, 24: 4010-4021

[36] CarradoA. Nano-crystalline pulsed laser deposition hydroxyapatite thin films on Ti substrate for biomedical application [J]. Journal of Coatings Technology and Research, 2011, 8: 749-755

[37] KhaliliV, AllafiJ K, GhalehH M, PaulsenA, FrenzelJ, EggelerG. The influence of Si as reactive bonding agent in the electrophoretic coatings of HA-Si-MWCNTs on NiTi alloys [J]. Journal of Materials Engineering and Performance, 2016, 25(2): 390-400

[38] FoersterC E, SerbenaF C, Da Silva SlR, LepienskiC M, DeM, SiqueiraC J, UedaM. Mechanical and tribological properties of AISI 304 stainless steel nitrided by glow discharge compared to ion implantation and plasma immersion ion implantation [J]. Nuclear Physics B, 2007, 257(1): 732-7362

[39] KheimehsariH, IzmanS, ShirdarM R. Effects of HA-coating on the surface morphology and corrosion behavior of a Co-Cr-based implant in different conditions [J]. Journal of Materials Engineering and Performance, 2015, 24(6): 2294-2302

[40] AksakalB, GavgaliM, DikiciB. The effect of coating thickness on corrosion resistance of hydroxyapatite coated Ti6Al4V and 316L SS implants [J]. Journal of Materials Engineering and Performance, 2010, 19(6): 894-899

[41] TlotlengM, AkinlabiE, ShuklaM, PityanaS. Microstructures, hardness and bioactivity of hydroxyapatite coatings deposited by direct laser melting process [J]. Materials Science and Engineering C, 2014, 43: 189-198

[42] GarciaS F J, MayorM B, AriasJ L, PouJ, LeonB, PerezA M. Hydroxyapatite coatings: A comparative study between plasmaspray and pulsed laser deposition techniques [J]. Journal of Materials Science: Materials in Medicine, 1997, 8(12): 861-865

[43] BaoQ, ChenC, WangD, JiQ, LeiT. Pulsed laser deposition and its current research status in preparing hydroxyapatite thin films [J]. Applied Surface Science, 2005, 252(5): 1538-1544

[44] BigiA, BracciB, CuisinierF, ElkaimR, FiniM, MayerI, MihailescuIN, SocolG, SturbaL, TorricelliP. Human osteoblast response to pulsed laser deposited calcium phosphate coatings [J]. Biomaterials, 2005, 26(15): 2381-2389

[45] FernandezP J M, GarciaC M V, CleriesL, SardinG, MorenzaJ L. Influence of the interface layer on the adhesion of pulsed laser deposited hydroxyapatite coatings on titanium alloy [J]. Applied Surface Science, 2002, 195(1–4): 31-37

[46] ZengH, LacefieldW R. XPS, EDX and FTIR analysis of pulsed laser deposited calcium phosphate bioceramic coatings: The effects of various process parameters [J]. Biomaterials, 2000, 21(1): 23-30

[47] RajeshP, MuraleedharanC V, KomathM, VarmaH. Pulsed laser deposition of hydroxyapatite on titanium substrate with titania interlayer [J]. Journal of Materials Science: Materials in Medicine, 2011, 22(3): 497-505

[48] WonY J, KiH. Fabricating functionally graded films with designed gradient profiles using pulsed laser deposition [J]. Journal of Applied Physics, 2013, 113: 174910

[49] TanaskovicD, JokicB, SocolG, PopescuA, MihailescuI N, PetrovicR, JanackovicD. Synthesis of functionally graded bioactive glass-apatite multistructures on Ti substrates by pulsed laser deposition [J]. Applied Surface Science, 2007, 254(4): 1279-1282

[50] ShiJ Z, ChenC Z, YuH J, ZhangS J. Application of magnetron sputtering for producing bioactive ceramic coatings on implant materials [J]. Bulletin of Materials Science, 2008, 31877-884

[51] SurmenevR A. A review of plasma-assisted methods for calcium phosphate-based coatings fabrication [J]. Surface and Coatings Technology, 2012, 206(8): 2035-20569

[52] RusopM, UmaK, SogaT, JimboT. Structural properties of pulsed laser deposited zinc oxide thin films annealed at various temperatures [J]. Surface Engineering, 2007, 23(3): 230-233

[53] YangY, KimK H, OngJ L. A review on calcium phosphate coatings produced using a sputtering process-an alternative to plasma spraying [J]. Biomaterials, 2005, 26(3): 327-337

[54] KuppusamiP, RaghunathanV S. Status of pulsed laser deposition: Challenges and opportunities [J]. Surface Engineering, 2006, 22(2): 81-83

[55] KhandelwalH, SinghG, AgrawalK, PrakashS, AgarwalR D. Characterization of hydroxyapatite coating by pulse laser deposition technique on stainless steel 316L by varying laser energy [J]. Applied Surface Science, 2013, 265: 30-35

[56] ZengH, LacefieldW R, MirovS. Structural and morphological study of pulsed laser deposited calcium phosphate bioceramic coatings: Influence of deposition conditions, laser parameters, and target properties [J]. Journal of Biomedical Materials Research, 2000, 50(2): 248-258

[57] DAS A, SHUKLA M. Surface morphology and adhesion studies of pulsed laser deposited hydroxyapatite thin film coatings on SS254 stainless steel [C]// 24th DAE BRNS National Laser Symposium (NLS-24), 2015.

[58] DasA, ShuklaM. Surface morphology, bioactivity, and antibacterial studies of pulsed laser deposited hydroxyapatite coatings on stainless steel 254 for orthopedic implant applications [J]. Journal of Materials: Design and Applications, 2016, 233(2): 120-127

[59] ConstantinoM E, CampilloB, StaiaM H, SernaS, Juarez-IslasJ, SudarshanT S. Pulsed electrode deposition of super hard coatings on steel substrates: microstructural and chemical study [J]. Surface Engineering, 2006, 22(3): 212-218

[60] ZHANG S. Hydroxyapatite coatings for biomedical applications [M]. CRC Press, 2018.

[61] WASA K. Handbook of sputtering technology [M]. Elsevier, 2012. DOI: https://doi.org/10.1016/C2010-0-67037-4.

[62] SwannS. Magnetron sputtering [J]. Physics in Technology, 1988, 19(2): 67-75

[63] DRIVER M. Coatings for biomedical applications [M]. Woodhead Publishing Limited, 2012.

[64] WanT, AokiH, HikawaJ, LeeJ H. RF-magnetron sputtering technique for producing hydroxyapatite coating film on various substrates [J]. Bio-Medical Materials and Engineering, 2007, 17(5): 291-297

[65] DasA, ShuklaM. Surface morphology and in vitro bioactivity of biocompatible hydroxyapatite coatings on medical grade S31254 steel by RF magnetron sputtering deposition [J]. International Journal of Surface Engineering and Coatings, 2017, 95(5): 276-281

[66] WOLKOWICZ R. Fluorescence-activated cell sorting, Brenner’s encyclopedia of genetics [M]. Academic Press, 2013.

[67] KASSING R, PETKOV P, KULISCH W, POPOV C. Functional properties of nanostructured materials series II: Mathematics physics and chemistry [M]. Springer, 2006.

[68] NELEA V, MOROSANU C, ILIESCU M, MIHAILESCU I N. Hydroxyapatite thin films grown by pulsed laser deposition and radio-frequency magnetron sputtering: comparative study [J]. Applied Surface Science, 228(1): 346–356. DOI: https://doi.org/10.1016/j.apsusc.2004.01.029.

[69] ThianE S, HuangJ, BestS M, BarberZ H, BonfieldW. Magnetron co-sputtered silicon-containing hydroxyapatite thin films — An in vitro study [J]. Biomaterials, 2005, 26(16): 2947-2956

[70] DindaG P, ShinJ, MazumderJ. Pulse laser deposition of hydroxyapatite thin coatings on TC4: Effect of heat treatment on structure and properties [J]. Acta Biomaterialia, 2009, 5(5): 1821-1830

[71] BlindO, KleinL H, DaileyB, JordanL. Characterization of hydroxyapatite films obtained by pulsed-laser deposition on Ti and TC4 substrates [J]. Dental Materials, 2005, 21(11): 1017-1024

[72] TorrisiL. Structural investigations on laser deposited hydroxyapatite films [J]. Thin Solid Films, 1994, 237(1): 12-152

[73] ZhangX, XiaoG Y, JiaoY, ZhaoX C, LuY P. Facile preparation of hopeite coating on stainless steel by chemical conversion method [J]. Surface and Coatings Technology, 2014, 240: 361-364

[74] LopezE O, MelloA, SendaoH, CostaL T, RossiA L, OspinaO R, BorghiF F, FilhoJ G S, RossiA M M. Growth of crystalline hydroxyapatite thin films at room temperature by tuning the energy of the RF-Magnetron sputtering plasma [J]. ACS Applied Materials & Interfaces, 2013, 5(19): 9435-9445

[75] AnselmeK, BigerelleM, NoelB, DufresneE, JudasD, IostA, HardouinP. Qualitative and quantitative study of human osteoblast adhesion on materials with various surface roughnesses [J]. Journal of Biomedical Materials Research, 2000, 49(2): 155-166

[76] PriceR L, WaidM C, HaberstrohK M, WebsterT J. Selective bone cell adhesion on formulations containing carbon nanofibers [J]. Biomaterials, 2003, 24(11): 1877-1887

[77] WashburnN R, YamadaK M, SimonC G, KennedyS B, AmisE J. High-throughput investigation of osteoblast response to polymer crystallinity: Influence of nanometer-scale roughness on proliferation [J]. Biomaterials, 2004, 25(7): 1215-12248

[78] WebsterT J, HellenmeyerE L, PriceR L. Increased osteoblast functions on theta plus delta nanofiber alumina [J]. Biomaterials, 2005, 26(9): 953-960

[79] WilsonC J, CleggR E, LeavesleyD I, PearcyM J. Mediation of biomaterial-cell interactions by adsorbed proteins: A review [J]. Tissue Engineering, 2005, 11(1): 1-182

[80] YANG L. Nanotechnology-enhanced orthopedic materials fabrications, applications and future trends [M]. Woodhead Publishing, 2015. DOI: https://doi.org/10.1016/C2013-0-16378-7.

[81] GeX, LengY, BaoC, XusL, WangR, RenF. Antibacterial coatings of fluoridated hydroxyapatite for percutaneous implants [J]. Journal of Biomedical Materials Research Part A, 2010, 95(2): 588-599

[82] SarithaK, RajeshA, ManjulathaK, SettyO H, YenuguS. Mechanism of antibacterial action of the alcoholic extracts of Hemidesmus indicus (L.) R. Frontiers in Microbiology, 2015, 6: 1-9

[83] DasA, ShuklaM. Hydroxyapatite coatings on high nitrogen stainless steel by laser rapid manufacturing [J]. Journal of the Minerals, Metals & Materials Society, 2017, 69(11): 2292-2296

[84] DasA, ShuklaM. Pulsed laser-deposited hopeite coatings on titanium alloy for orthopaedic implant applications: surface characterization, antibacterial and bioactivity studies [J]. Journal of the Brazilian Society of Mechanical Sciences and Engineering, 2019, 41(5): 214

[85] PuckettS D, TaylorE, RaimondoT, WebsterT J. The relationship between the nanostructure of titanium surfaces and bacterial attachment [J]. Biomaterials, 2010, 314706-713

[86] YiW, SunX, NiuD, HuX. In vitro bioactivity of 3D Ti-mesh with bioceramic coatings in simulated body fluid [J]. Journal of Asian Ceramic Societies, 2014, 2(3): 210-214

[87] KokuboT, TakadamaH. How useful is SBF in predicting in vivo bone bioactivity? [J]. Biomaterials, 2006, 27(15): 2907-2915

[88] ManH C, ChiuK Y, ChengF T, WongK H. Adhesion study of pulsed laser deposited hydroxyapatite coating on laser surface nitrided titanium [J]. Thin Solid Films, 2009, 517(18): 5496-5501

[89] NeoM, KotaniS, NakamuraT, YamamuroT, OhtsukiC, KokuboT, BandoY A. A comparative study of ultrastructures of the interfaces between four kinds of surface-active ceramic and bone [J]. Journal of Biomedical Materials Research, 1992, 26(11): 1419-1432

[90] ChavanP N, BahirM M, MeneR U, MahaboleM P, KhairnarR S. Study of nano biomaterial hydroxyapatite in simulated body fluid: formation and growth of apatite [J]. Material Science & Engineering B, 2010, 168(1): 224-230

[91] GuY W, KhorK A, CheangP. Bone-like apatite layer formation on hydroxyapatiteprepared by spark plasma sintering (SPS) [J]. Biomaterials, 2004, 25(18): 4127-4134

[92] WangY X, RobertsonJ L, SpillmanW B, ClausR O. Effects of the chemical structure and the surface properties of polymeric biomaterials and their biocompatibility [J]. Journal of Pharmaceutical Research, 2004, 21(18): 1362-1373

[93] WangJ, PanC J, HuangN, SunH, YangP, LengX Y, ChenJ Y, WanG J, ChuP K. Surface characterization and blood compatibility of poly (ethylene terephthalate) modified by plasma surface grafting [J]. Surface and Coatings Technology, 2005, 196(1–3): 307-311

[94] HiguchiA, ShiranoK, HarashimaM, YoonB O, HaraM, HattoriM, ImamuraK. Chemically modified polysulfone hollow fibers with vinylpyrrolidone having improved blood compatibility [J]. Biomaterials, 2002, 23(13): 2659-2666