Skip to main content
SpringerLink
Log in

Mechanical properties and decohesion of sol–gel coatings on metallic and glass substrates

  • Original Paper: Characterization methods of sol-gel and hybrid materials
  • Published:
Journal of Sol-Gel Science and Technology Aims and scope Submit manuscript

Abstract

The sol–gel coating method is considered to be simple and easy to implement to lead to organic/inorganic hybrid coatings. In addition, the application of thin films by this technique is inexpensive and applicable on large substrates without form restriction. In this context, thin sol–gel coatings based on a mixture of three alkoxysilanes and synthesized in purely aqueous phase with different thicknesses and with the presence or not of ZrO2 nanoparticles, were applied on metallic and glass substrates. After application and curing, the mechanical properties of sol–gel coatings were characterized by Berkovich nanoindentation with continuous stiffness measurement mode (CSM). The effective elastic moduli as well as the hardness values were estimated for each coating along the indentation depth and as a function of the substrate material and sol–gel characteristics. The effect of a annealing at higher temperature was also studied. Then, the failure modes of sol–gel coatings were investigated using both Berkovich nanoindentation and nanoscratch technique with a 5 µm radius spherical diamond tip. Careful microscopic observations of residual imprints and residual grooves both exhibit chipping in case of thick coating especially on glass substrate and no dramatic failure for thin coating applied on both substrates. It is shown in this work that the mechanical properties of the sol–gel and the mechanical stability of coatings on substrates are influenced dramatically by the presence of nanoparticles and the thermal treatment. Finally, interfacial fracture toughness of sol–gel coatings on substrate was estimated using analytical model from the literature and Ashby map based on experimental results was created using performance indices in order to proceed to sol–gel coating selection.

Highlights

  • Mechanical characterization of sol–gel coatings using a combination of different nanomechanical experiments.

  • Effects of nanoparticles addition and thermal treatment on mechanical coating stability.

  • Construction of Ashby map using experimental results for sol–gel coating selection.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7
Fig. 8
Fig. 9
Fig. 10
Fig. 11
Fig. 12
Fig. 13
Fig. 14
Fig. 15
Fig. 16
Fig. 17

Similar content being viewed by others

References

  1. Aparicio M et al. (2016) Corrosion Protection of AISI 304 Stainless Steel with Melting Gel Coatings. Electrochim Acta 202(Supplement C):325–332

    CAS  Google Scholar 

  2. Ćurković L, Ćurković HO, Salopek S, Renjo MM, Šegota S (2013) Enhancement of corrosion protection of AISI 304 stainless steel by nanostructured sol–gel TiO2 films. Corros Sci 77:176–184

    Google Scholar 

  3. Feng Z, Liu Y, Thompson GE, Skeldon P (2010) Sol–gel coatings for corrosion protection of 1050 aluminium alloy. Electrochim Acta 55(10):3518–3527

    CAS  Google Scholar 

  4. Vignesh RB, Edison TNJI, Sethuraman MG (2014) ‘Sol–Gel coating with 3-Mercaptopropyltrimethoxysilane as precursor for corrosion protection of aluminium metal. J Mater Sci Technol 30(8):814–820

    CAS  Google Scholar 

  5. Nezamdoust S, Seifzadeh D (2017) Application of CeH–V/ sol–gel composite coating for corrosion protection of AM60B magnesium alloy. Trans Nonferrous Met Soc China 27(2):352–362

    CAS  Google Scholar 

  6. Martini C, Ceschini L (2011) A comparative study of the tribological behaviour of PVD coatings on the Ti-6Al-4V alloy. Tribol Int 44(3):297–308

    CAS  Google Scholar 

  7. Damasceno JC, Camargo SS, Cremona M (2002) Deposition and evaluation of DLC–Si protective coatings for polycarbonate materials. Thin Solid Films 420–421:195–199

    Google Scholar 

  8. Dave BC, Hu X, Devaraj Y, Dhali SK (2004) Sol–gel-derived corrosion-protection coatings. J Sol–Gel Sci Technol 32(1–3):143–147

    CAS  Google Scholar 

  9. Wang D, Bierwagen GordonP (2009) Sol–gel coatings on metals for corrosion protection. Prog Org Coat 64(4):327–338

    CAS  Google Scholar 

  10. Zheng S, Li J (2010) Inorganic–organic sol gel hybrid coatings for corrosion protection of metals. J Sol–Gel Sci Technol 54(2):174–187

    CAS  Google Scholar 

  11. Fabes BD, Uhlmann DR (1990) Strengthening of glass by sol-gel coatings. J Am Ceram Soc 73(no. 4):978–988

    CAS  Google Scholar 

  12. Guglielmi M (1997) Sol-Gel Coatings on Metals. J Sol–Gel Sci Technol 8(1–3):443–449

    CAS  Google Scholar 

  13. Mammeri F, Le Bouhris E, Rozes L, Sanchez C (2005) Mechanical properties of hybrid organic–inorganic materials. J Mater Chem 15(35–36):3787–3811

    CAS  Google Scholar 

  14. S Zhang (2010) Nanostructured thin films and coatings: mechanical properties. CRC Press, USA

  15. Levy D, Zayat M (2015) The sol–gel handbook: synthesis, characterization and applications, 3–volume set. Wiley VCH, Weinheim

    Google Scholar 

  16. Tlili B, Barkaoui A, Walock M (2016) Tribology and wear resistance of the stainless steel. The sol–gel coating impact on the friction and damage. Tribol Int 102:348–354

    CAS  Google Scholar 

  17. F-X Perrin, ‘Films inorganiques et hybrides protecteurs obtenus par voie sol-gel’, Techniques de l’ingénieur Traitements de surface des métaux en milieu aqueux. vol. base documentaire: TIB359DUO, no. ref. article: m1722, 2007.

  18. Osborne JH et al. (2001) Testing and evaluation of nonchromated coating systems for aerospace applications. Prog Org Coat 41(4):217–225

    CAS  Google Scholar 

  19. Yang Y-Q, Liu L, Hu J-M, Zhang J-Q, Cao C-N (2012) Improved barrier performance of metal alkoxide-modified methyltrimethoxysilane films. Thin Solid Films 520(6):2052–2059

    CAS  Google Scholar 

  20. Rauter A, Slemenik Perše L, Orel B, Bengű B, Sunetci O, Šurca Vuk A (2013) Ex situ IR and Raman spectroscopy as a tool for studying the anticorrosion processes in (3-glycidoxypropyl)trimethoxysilane-based sol–gel coatings. J Electroanal Chem 703:97–107

    CAS  Google Scholar 

  21. Kunst SR et al. (2014) Corrosion resistance of siloxane–poly(methyl methacrylate) hybrid films modified with acetic acid on tin plate substrates: Influence of tetraethoxysilane addition. Appl Surf Sci 298:1–11

    CAS  Google Scholar 

  22. Dias SAS, Lamaka SV, Nogueira CA, Diamantino TC, Ferreira MGS (2012) Sol–gel coatings modified with zeolite fillers for active corrosion protection of AA2024. Corros Sci 62:153–162

    CAS  Google Scholar 

  23. Lamaka SV et al. (2008) Novel hybrid sol–gel coatings for corrosion protection of AZ31B magnesium alloy. Electrochim Acta 53(14):4773–4783

    CAS  Google Scholar 

  24. Garcia RBR, da Silva FS, Kawachi EY (2013) New sol–gel route for SiO2/ZrO2 film preparation. Colloids Surf A Physicochem Eng Asp 436:484–488

    CAS  Google Scholar 

  25. Capelossi VR, Poelman M, Recloux I, Hernandez RPB, de Melo HG, Olivier MG (2014) Corrosion protection of clad 2024 aluminum alloy anodized in tartaric-sulfuric acid bath and protected with hybrid sol–gel coating. Electrochim Acta 124:69–79

    CAS  Google Scholar 

  26. Roussi E, Tsetsekou A, Skarmoutsou A, Charitidis CA, Karantonis A (2013) Anticorrosion and nanomechanical performance of hybrid organo-silicate coatings integrating corrosion inhibitors. Surf Coat Technol 232:131–141

    CAS  Google Scholar 

  27. Fedel M, Olivier M, Poelman M, Deflorian F, Rossi S, Druart M-E (2009) Corrosion protection properties of silane pre-treated powder coated galvanized steel. Prog Org Coat 66(2):118–128

    CAS  Google Scholar 

  28. Nicolay A et al. (2015) Elaboration and characterization of a multifunctional silane/ZnO hybrid nanocomposite coating. Appl Surf Sci 327:379–388

    CAS  Google Scholar 

  29. Sabzi M, Mirabedini SM, Zohuriaan-Mehr J, Atai M (2009) Surface modification of TiO2 nano-particles with silane coupling agent and investigation of its effect on the properties of polyurethane composite coating. Prog Org Coat 65(2):222–228

    CAS  Google Scholar 

  30. Peng B, Huang Y, Chai L, Li G, Cheng M, Zhang X (2007) Influence of polymer dispersants on dispersion stability of nano-TiO2 aqueous suspension and its application in inner wall latex paint. J Cent South Univ Technol 14(4):490–495

    CAS  Google Scholar 

  31. Luo K, Zhou S, Wu L (2009) High refractive index and good mechanical property UV-cured hybrid films containing zirconia nanoparticles. Thin Solid Films 517(21):5974–5980

    CAS  Google Scholar 

  32. Piwoński I, Soliwoda K (2010) The effect of ceramic nanoparticles on tribological properties of alumina sol–gel thin coatings. Ceram Int 36(1):47–54

    Google Scholar 

  33. Banerjee DA, Kessman AJ, Cairns DR, Sierros KA (2014) Tribology of silica nanoparticle-reinforced, hydrophobic sol–gel composite coatings. Surf Coat Technol 260:214–219

    CAS  Google Scholar 

  34. Song J, Liu Y, Liao Z, Wang S, Tyagi R, Liu W (2016) Wear studies on ZrO2-filled PEEK as coating bearing materials for artificial cervical discs of Ti6Al4V. Mater Sci Eng C 69:985–994

    CAS  Google Scholar 

  35. Atanacio AJ, Latella BA, Barbé CJ, Swain MV (2005) Mechanical properties and adhesion characteristics of hybrid sol–gel thin films. Surf Coat Technol 192(2–3):354–364

    CAS  Google Scholar 

  36. Fabes BD, Oliver WC (1990) Mechanical properties of sol-gel coatings. J Non-Cryst Solids 121(1):348–356

    CAS  Google Scholar 

  37. Chan CM, Cao GZ, Fong H, Sarikaya M, Robinson T, Nelson L (2000) Nanoindentation and adhesion of sol-gel-derived hard coatings on polyester. J Mater Res 15(01):148–154

    CAS  Google Scholar 

  38. Latella BA, Gan BK, Barbé CJ, Cassidy DJ (2008) Nanoindentation hardness, Young’s modulus, and creep behavior of organic–inorganic silica-based sol-gel thin films on copper. J Mater Res 23(09):2357–2365

    CAS  Google Scholar 

  39. J Hay (2009) Mechanical characterization of sol–gel coatings using a nano indenter G200. Application Notes from Agilent Technologies. https://www.agilent.com/

  40. Piombini H, Ambard C, Compoint F, Valle K, Belleville PSanchez C (2015) Indentation hardness and scratch tests for thin layers manufactured by sol–gel process. In: CLEO: Applications and Technology

  41. Ballarre J, Jimenez-Pique E, Anglada M, Pellice SA, Cavalieri AL (2009) Mechanical characterization of nano-reinforced silica based sol–gel hybrid coatings on AISI 316L stainless steel using nanoindentation techniques. Surf Coat Technol 203(20–21):3325–3331

    CAS  Google Scholar 

  42. Malzbender J, de With G, den Toonder JMJ (2000) Determination of the elastic modulus and hardness of sol–gel coatings on glass: influence of indenter geometry. Thin Solid Films 372(1–2):134–143

    CAS  Google Scholar 

  43. BA Latella, MV Swain, M Ignat (2012) Indentation and fracture of hybrid sol-gel silica films. In: J Nemecek (ed.) Nanoindentation in materials science, IntechOpen, London (UK)

  44. Latella BA, Ignat M (2012) Interface fracture surface energy of sol–gel bonded silicon wafers by three-point bending. J Mater Sci Mater Electron 23(1):8–13

    CAS  Google Scholar 

  45. Den Toonder JD, Malzbender J, With GD, Balkenende R (2002) Fracture toughness and adhesion energy of sol–gel coatings on glass. J Mater Res 17(01):224–233

    Google Scholar 

  46. BA Latella, M Ignat, CJ Barbé, DJ Cassidy, H Li (2004) Cracking and decohesion of sol–gel hybrid coatings on metallic substrates. J Sol–Gel Sci Technol 31(1–3):143–149

    CAS  Google Scholar 

  47. Malzbender J, Den Toonder JMJ, Balkenende AR, De With G (2002) Measuring mechanical properties of coatings: a methodology applied to nano-particle-filled sol–gel coatings on glass Mater Sci Eng R Rep 36(2):47–103

    Google Scholar 

  48. Chen L, Yeap KB, She CM, Liu GR (2011) A computational and experimental investigation of three-dimensional micro-wedge indentation-induced interfacial delamination in a soft-film-on-hard-substrate system. Eng Struct 33(12):3269–3278

    Google Scholar 

  49. Mercier D, Mandrillon V, Parry G, Verdier M, Estevez R, Bréchet Y, Maindron T (2017) Investigation of the fracture of very thin amorphous alumina film during spherical nanoindentation. Thin Solid Films 638:34–47. https://doi.org/10.1016/j.tsf.2017.07.040

    CAS  Google Scholar 

  50. Thouless MD (1998) An analysis of spalling in the microscratch test. Eng Fract Mech 61(1):75–81

    Google Scholar 

  51. Malzbender J, de With G (2002) A model to determine the interfacial fracture toughness for chipped coatings. Surf Coat Technol 154(1):21–26

    CAS  Google Scholar 

  52. Xie Y, Hawthorne HM (2003) Measuring the adhesion of sol–gel derived coatings to a ductile substrate by an indentation-based method. Surf Coat Technol 172(1):42–50

    CAS  Google Scholar 

  53. Bull SJ, Berasetegui EG (2006) An overview of the potential of quantitative coating adhesion measurement by scratch testing. Tribol Int 39(2):99–114

    CAS  Google Scholar 

  54. Granta Design Ltd. (2019) CES Selector version 2019, Cambridge (UK). https://grantadesign.com

  55. MF Ashby (2011) Materials selection in mechanical design, 4th edn. Butterworth-Heinemann, Oxford (UK)

  56. Oliver WC, Pharr GM (1992) An improved technique for determining hardness and elastic modulus using load and displacement sensing indentation experiments. J Mater Res 7(06):1564–1583

    CAS  Google Scholar 

  57. Oliver WC, Pharr GM (2004) Measurement of hardness and elastic modulus by instrumented indentation: advances in understanding and refinements to methodology. J Mater Res 19(1):3–20

    CAS  Google Scholar 

  58. King RB (1987) Elastic analysis of some punch problems for a layered medium. Int J Solids Struct 23(12):1657–1664

    Google Scholar 

  59. Makishima A, Mackenzie JD (1975) Calculation of bulk modulus, shear modulus and Poisson’s ratio of glass. J Non-Cryst Solids 17(2):147–157

    CAS  Google Scholar 

  60. Ledbetter HM (1981) Stainless‐steel elastic constants at low temperatures. J Appl Phys 52(3):1587–1589

    CAS  Google Scholar 

  61. Fischer-Cripps AC (2011) Nanoindentation, 3rd edn. Springer-Verlag, New York (USA)

    Google Scholar 

  62. Mercier D et al. (2010) Mesure de module d’Young d’un film mince à partir de mesures expérimentales de nanoindentation réalisées sur des systèmes multicouches, Matériaux & Techniques 99. https://doi.org/10.1051/mattech/2011029

    CAS  Google Scholar 

  63. Mercier D (2016) NIMS version 3.2. https://github.com/DavidMercier/NIMS, https://doi.org/10.13140/RG.2.2.13901.03045

  64. Lawn BR, Evans AG (1977) A model for crack initiation in elastic/plastic indentation fields. J Mater Sci 12:2195–2199

    CAS  Google Scholar 

  65. Malzbender J, de With G (2001) The use of the indentation loading curve to detect fracture of coatings. Surf Coat Technol 137(1):72–76

    CAS  Google Scholar 

  66. Li X, Bhushan B (1998) Measurement of fracture toughness of ultra-thin amorphous carbon films. Thin Solid Films 315(1):214–221

    CAS  Google Scholar 

  67. Attar F, Johannesson T (1996) Adhesion evaluation of thin ceramic coatings on tool steel using the scratch testing technique. Surf Coat Technol 78(1–3):87–102

    CAS  Google Scholar 

  68. Burnett PJ, Rickerby DS (1987) The relationship between hardness and scratch adhesion. Thin Solid Films 154(1–2):403–416

    CAS  Google Scholar 

  69. Bull SJ, Rickerby DS, Matthews A, Leyland A, Pace AR, Valli J (1988) The use of scratch adhesion testing for the determination of interfacial adhesion: the importance of frictional drag. Surf Coat Technol 36(1):503–517

    CAS  Google Scholar 

  70. Bull SJ, Rickerby DS (1990) New developments in the modelling of the hardness and scratch adhesion of thin films. Surf Coat Technol 42(2):149–164

    CAS  Google Scholar 

  71. Bull SJ, Berasetegui EG (2006) An overview of the potential of quantitative coating adhesion measurement by scratch testing. Tribol Int 39(2):99–114

    CAS  Google Scholar 

  72. Lai C-M, Lin K-M, Rosmaidah S (2012) Effect of annealing temperature on the quality of Al-doped ZnO thin films prepared by sol–gel method. J Sol–Gel Sci Technol 61(1):249–257

    CAS  Google Scholar 

  73. Bull SJ (1997) Failure mode maps in the thin film scratch adhesion test. Tribol Int 30(7):491–498

    CAS  Google Scholar 

Download references

Acknowledgements

The authors would like to thank the MecaTech Cluster and the Walloon region for the financial support, in the frame of the Nanosol project. The authors would also like to thank the Walloon region for financial support in the frame of the INDMAT project (BEWARE FELLOWSHIPS), co-funded by the European Union (FP7—Marie Curie Actions). The authors are grateful to Luiza Bonin (UMons) for the 3D microscopic visualization and to Recayi Bilgic (CRM Group) for the AFM observations of residual indents and scratches.

Author information

Authors and Affiliations

  1. CRM Group, Liege, Belgium

    David Mercier, Xavier Vanden Eynde, Laure Libralesso & Alain Daniel

  2. Ansys, Inc.—Granta Education Team, Lyon, France

    David Mercier

  3. University of Mons, Faculty of Engineering, Mons, Belgium

    Arnaud Nicolay & Marjorie Olivier

  4. Materia Nova, Mons, Belgium

    Arnaud Nicolay & Abdelhamid Boudiba

  5. Ionics Group, Mons, Belgium

    Arnaud Nicolay

Authors
  1. David Mercier
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Arnaud Nicolay
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Abdelhamid Boudiba
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Xavier Vanden Eynde
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Laure Libralesso
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Alain Daniel
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Marjorie Olivier
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to David Mercier.

Ethics declarations

Conflict of interest

The authors declare that they have no conflict of interest.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Mercier, D., Nicolay, A., Boudiba, A. et al. Mechanical properties and decohesion of sol–gel coatings on metallic and glass substrates. J Sol-Gel Sci Technol 93, 229–243 (2020). https://doi.org/10.1007/s10971-019-05196-9

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10971-019-05196-9

Keywords

Search

Navigation