[en] The sol-gel sealing method is widely recognized as a simple and effective technique for enhancing the protective performance of plasma electrolytic oxidation (PEO) coatings. While sol-gel coatings are already known for their reliability and corrosion resistance, incorporating nanoparticles has been shown to further improve their barrier properties. Our objective was to validate the positive impact of incorporating nanosheets and assess the influence of h-BN functionalization in the sol-gel/PEO coating system on AA2024. Specifically, as-received, oxidized, and functionalized nanopowders at two concentrations were added to the sol-gel solution. (3-Aminopropyl)triethoxysilane (APTES) was selected as the suitable candidate for h-BN functionalization, given that the sol-gel sealing comprises a combination of (3-glycidyloxypropyl)trimethoxysilane (GPTMS) and tetraethoxysilane (TEOS). Consequently, higher compatibility between the nanopowders and the sol-gel matrix was achieved, thereby improving the barrier properties. Various chemical techniques, such as zeta potential (ZP) measurement and Fourier Transform Infrared Spectroscopy (FTIR), were employed to confirm the successful oxidation and functionalization processes. Rheology evaluation further affirmed the influence of h-BN functionalization on its compactness and the viscosity of the network. The trace of nanosheets within the sol-gel coating on top of the PEO layer was visualized using Field Emission Scanning Electron Microscopy (FE-SEM). Finally, Electrochemical Impedance Spectroscopy (EIS) analysis reported that the modified sol-gel coating with functionalized h-BN exhibited the greatest corrosion resistance after exposure to 0.1 M NaCl electrolyte for 14 days.
Disciplines :
Materials science & engineering
Author, co-author :
Akbarzadeh, Sajjad ; Université de Mons - UMONS > Faculté Polytechnique > Service de Science des Matériaux
Batjargal, Zorigtbaatar; Materials Science Department, Faculty of Engineering, University of Mons, Mons, Belgium
Ölmez, Vedi; Belgian Ceramic Research Centre (BCRC), Mons, Belgium
Olivier, Marjorie ; Université de Mons - UMONS > Faculté Polytechnique > Service de Science des Matériaux
Language :
English
Title :
Modified sol-gel layer incorporating hexagonal boron nitride (h-BN) nanosheets for improved corrosion resistance in plasma electrolytic oxidation coatings on AA2024
R400 - Institut de Recherche en Science et Ingénierie des Matériaux
Name of the research project :
4573 - SEALCERA - Corrosion and tribocorrosion performance of sealed ceramic coatings obtained by plasma electrolytic oxidation - Fédération Wallonie Bruxelles
Funders :
FWB - Fédération Wallonie-Bruxelles
Funding text :
The authors are thankful to the University of Mons for its financial
support as part of the ARC (Actions de Recherche Concertées) SEALCERA project funded by the Fédération Wallonie-Bruxelles and the Materials Institute of UMONS.
Zhao, D., Sun, J., Zhang, L., Tan, Y., Li, J., Corrosion behavior of rare earth cerium based conversion coating on aluminum alloy. J. Rare Earths 28 (2010), 371–374.
Mokaddem, M., Volovitch, P., Rechou, F., Oltra, R., Ogle, K., The anodic and cathodic dissolution of Al and Al–Cu–Mg alloy. Electrochim. Acta 55 (2010), 3779–3786.
Cavanaugh, M.K., Li, J.-C., Birbilis, N., Buchheit, R.G., Electrochemical characterization of intermetallic phases common to aluminum alloys as a function of solution temperature. J. Electrochem. Soc. 161 (2014), C535–C543.
Queiroz, F.M., Magnani, M., Costa, I., de Melo, H.G., Investigation of the corrosion behaviour of AA 2024-T3 in low concentrated chloride media. Corros. Sci. 50 (2008), 2646–2657.
Lacroix, L., Blanc, C., Pébère, N., Thompson, G.E., Tribollet, B., Vivier, V., Simulating the galvanic coupling between S-Al2CuMg phase particles and the matrix of 2024 aerospace aluminium alloy. Corros. Sci. 64 (2012), 213–221.
Vander Kloet, J., Hassel, A.W., Stratmann, M., Effect of pretreatment on the intermetallics in aluminum alloy 2024-T3. Zeitschrift Fur Phys. Chemie 219 (2005), 1505–1518.
Klumpp, R.E., Akbarzadeh, S., de Sousa Araujo, J.V., Gonon, M.F., Delaunois, F., Costa, I., Olivier, M.G., Correlating corrosion modes with the microstructure of the 2XXX series alloys: a comparative approach. Surf. Interface Anal. 56 (2024), 643–653.
Vukmirovic, M.B., Dimitrov, N., Sieradzki, K., Dealloying and corrosion of Al alloy 2024-T3. J. Electrochem. Soc., 149, 2002, B428.
Akbarzadeh, S., Coelho, L.B., Dangreau, L., Lanzutti, A., Fedrizzi, L., Olivier, M.G., Self-healing plasma electrolytic oxidation (PEO) coating developed by an assembly of corrosion inhibitive layer and sol-gel sealing on AA2024. Corros. Sci., 222, 2023, 111424.
Khalid, H.A., Akbarzadeh, S., Paint, Y., Vitry, V., Olivier, M.G., Comparison of tribological characteristics of AA2024 coated by plasma electrolytic oxidation (PEO) sealed by different sol–gel layers. Coatings, 13, 2023, 871.
Capelossi, V.R., Poelman, M., Recloux, I., Hernandez, R.P.B., De Melo, H.G., Olivier, M.G., Corrosion protection of clad 2024 aluminum alloy anodized in tartaric-sulfuric acid bath and protected with hybrid sol–gel coating. Electrochim. Acta 124 (2014), 69–79.
Wang, L.F., Sun, J., Yu, X.L., Shi, Y., Zhu, X.G., Cheng, L.Y., Liang, H.H., Yan, B., Guo, L.J., Enhancement in mechanical properties of selectively laser-melted AlSi10Mg aluminum alloys by T6-like heat treatment. Mater. Sci. Eng. A 734 (2018), 299–310.
Haixiang, C., Dejun, K., Comparison on electrochemical corrosion performances of arc and laser thermal sprayed Al–Ti–Ni coatings in marine environment. Mater. Chem. Phys., 251, 2020, 123200.
Ryabchikov, A.I., Kashkarov, E.B., Shevelev, A.E., Obrosov, A., Sivin, D.O., Surface modification of Al by high-intensity low-energy Ti-ion implantation: microstructure, mechanical and tribological properties. Surf. Coatings Technol. 372 (2019), 1–8.
Rao, G.M., Dilkush, Gopal, A.V., Effect of physical vapour deposition coated and uncoated carbide tools in turning aluminium alloy-AA6063. Mater. Today Proc. 41 (2021), 1212–1219.
Yu, F., Camilli, L., Wang, T., Mackenzie, D.M.A., Curioni, M., Akid, R., Bøggild, P., Complete long-term corrosion protection with chemical vapor deposited graphene. Carbon N. Y. 132 (2018), 78–84.
Verdalet-Guardiola, X., Fori, B., Bonino, J.P., Duluard, S., Blanc, C., Nucleation and growth mechanisms of trivalent chromium conversion coatings on 2024-T3 aluminium alloy. Corros. Sci. 155 (2019), 109–120.
del Olmo, R., Mohedano, M., Visser, P., Matykina, E., Arrabal, R., Flash-PEO coatings loaded with corrosion inhibitors on AA2024. Surf. Coatings Technol., 402, 2020, 126317.
Molaeipour, P., Allahkaram, S.R., Akbarzadeh, S., Corrosion inhibition of Ti6Al4V alloy by a protective plasma electrolytic oxidation coating modified with boron carbide nanoparticles. Surf. Coatings Technol., 430, 2022, 127987.
Xie, H. Jun, Cheng, Y. Liang, Li, S. Xian, Cao, J. Hui, Cao, L., Wear and corrosion resistant coatings on surface of cast A356 aluminum alloy by plasma electrolytic oxidation in moderately concentrated aluminate electrolytes. Trans. Nonferrous Met. Soc. China 27 (2017), 336–351.
Li, K., Li, W., Zhang, G., Zhu, W., Zheng, F., Zhang, D., Wang, M., Effects of Si phase refinement on the plasma electrolytic oxidation of eutectic Al-Si alloy. J. Alloys Compd. 790 (2019), 650–656.
Pezzato, L., Akbarzadeh, S., Settimi, A.G., Moschin, E., Moro, I., Olivier, M.G., Brunelli, K., Dabalà, M., Corrosion and antifouling properties of copper-containing PEO coatings produced on steels. Surf. Coatings Technol., 482, 2024, 130631.
Wang, L., Chen, L., Yan, Z., Fu, W., Optical emission spectroscopy studies of discharge mechanism and plasma characteristics during plasma electrolytic oxidation of magnesium in different electrolytes. Surf. Coatings Technol. 205 (2010), 1651–1658.
Snizhko, L.O., Yerokhin, A.L., Pilkington, A., Gurevina, N.L., Misnyankin, D.O., Leyland, A., Matthews, A., Anodic processes in plasma electrolytic oxidation of aluminium in alkaline solutions. Electrochim. Acta 49 (2004), 2085–2095.
Treviño, M., Mercado-Solis, R.D., Colás, R., Pérez, A., Talamantes, J., Velasco, A., Erosive wear of plasma electrolytic oxidation layers on aluminium alloy 6061. Wear 301 (2013), 434–441.
Joo, J., Kim, D., Moon, H.S., Kim, K., Lee, J., Durable anti-corrosive oil-impregnated porous surface of magnesium alloy by plasma electrolytic oxidation with hydrothermal treatment. Appl. Surf. Sci., 509, 2020, 145361.
Mashtalyar, D.V., Nadaraia, K.V., Imshinetskiy, I.M., Belov, E.A., Filonina, V.S., Suchkov, S.N., Sinebryukhov, S.L., Gnedenkov, S.V., Composite coatings formed on Ti by PEO and fluoropolymer treatment. Appl. Surf. Sci., 536, 2021, 147976.
Pezzato, L., Babbolin, R., Cerchier, P., Marigo, M., Dolcet, P., Dabalà, M., Brunelli, K., Sealing of PEO coated AZ91magnesium alloy using solutions containing neodymium. Corros. Sci., 173, 2020, 108741.
Akbarzadeh, S., Naderi, R., Mahdavian, M., Fabrication of a highly protective silane composite coating with limited water uptake utilizing functionalized carbon nano-tubes. Compos. Part B Eng., 175, 2019, 107109.
Akbarzadeh, S., Akbarzadeh, K., Ramezanzadeh, M., Naderi, R., Mahdavian, M., Olivier, M.G., Corrosion resistance enhancement of a sol-gel coating by incorporation of modified carbon nanotubes: artificial neural network (ANN) modeling and experimental explorations. Prog. Org. Coatings., 174, 2023, 107296.
Mackenzie, J.D., Bescher, E.P., Physical properties of sol-gel coatings. J. Sol-Gel Sci. Technol. 19 (2000), 23–29.
Mehner, A., Zoch, H.W., Datchary, W., Pongs, G., Sol-gel coatings for high precision optical molds. CIRP Ann. 55 (2006), 589–592.
Akbarzadeh, S., Ramezanzadeh, M., Ramezanzadeh, B., Mahdavian, M., Naderi, R., Fabrication of highly effective polyaniline grafted carbon nanotubes to induce active protective functioning in a silane coating. Ind. Eng. Chem. Res. 58 (2019), 20309–20322.
Akbarzadeh, S., Klumpp, R.E., Mégret, A., Ölmez, V., Vitry, V., Olivier, M.G., Breakthrough in aluminum protection: electrochemical and wear insights into sol-gel sealed PEO-coated AA2024-T3 and AA2198-T851. Surf. Coatings Technol., 494, 2024, 131510.
Wang, H., Akid, R., A room temperature cured sol–gel anticorrosion pre-treatment for Al 2024-T3 alloys. Corros. Sci. 49 (2007), 4491–4503.
Samadianfard, R., Seifzadeh, D., Habibi-Yangjeh, A., Sol-gel coating filled with SDS-stabilized fullerene nanoparticles for active corrosion protection of the magnesium alloy. Surf. Coatings Technol., 419, 2021, 127292.
Samadianfard, R., Seifzadeh, D., Habibi-Yangjeh, A., Jafari-Tarzanagh, Y., Oxidized fullerene/sol-gel nanocomposite for corrosion protection of AM60B magnesium alloy. Surf. Coatings Technol., 385, 2020, 125400.
Zhang, S., Liang, X., Gadd, G.M., Zhao, Q., A sol–gel based silver nanoparticle/polytetrafluorethylene (AgNP/PTFE) coating with enhanced antibacterial and anti-corrosive properties. Appl. Surf. Sci., 535, 2021, 147675.
Nezamdoust, S., Seifzadeh, D., Habibi-Yangjeh, A., Nanodiamond incorporated sol−gel coating for corrosion protection of magnesium alloy. Trans. Nonferrous Met. Soc. China. 30 (2020), 1535–1549.
Xue, B., Yu, M., Liu, J., Liu, J., Li, S., Xiong, L., Corrosion protection of AA2024-T3 by sol-gel film modified with graphene oxide. J. Alloys Compd. 725 (2017), 84–95.
Uddin, F., Uddin, F., Montmorillonite: An Introduction to Properties and Utilization. 2018, IntechOpen.
Montemor, M.F., Ferreira, M.G.S., Analytical characterization of silane films modified with cerium activated nanoparticles and its relation with the corrosion protection of galvanised steel substrates. Prog. Org. Coatings. 63 (2008), 330–337.
Kim, H., Hwang, T., Corrosion protection enhancement effect by mixed silica nanoparticles of different sizes incorporated in a sol-gel silica film. J. Sol-Gel Sci. Technol. 63 (2012), 563–568.
Shi, Y., Yuan, S., Ter-Ovanessian, B., Hermange, K., Huo, Y., Normand, B., Enhancing the barrier effect of sol-gel derived inorganic coating by doping h-BN nanosheet. Appl. Surf. Sci., 544, 2021, 148849.
Coan, T., Barroso, G.S., Motz, G., Bolzána, A., Machado, R.A.F., Preparation of PMMA/hBN composite coatings for metal surface protection. Mater. Res. 16 (2013), 1366–1372.
Huang, Y.C., Lo, T.Y., Chao, C.G., Whang, W.T., Anti-corrosion characteristics of polyimide/h-boron nitride composite films with different polymer configurations. Surf. Coatings Technol. 260 (2014), 113–117.
Husain, E., Narayanan, T.N., Taha-Tijerina, J.J., Vinod, S., Vajtai, R., Ajayan, P.M., Marine corrosion protective coatings of hexagonal boron nitride thin films on stainless steel. ACS Appl. Mater. Interfaces 5 (2013), 4129–4135.
TabkhPaz, M., Park, D.Y., Lee, P.C., Hugo, R., Park, S.S., Development of Nanocomposite Coatings With Improved Mechanical, Thermal, and Corrosion Protection Properties. 52, 2017, Sage, 1045–1060.
Golberg, D., Bando, Y., Huang, Y., Terao, T., Mitome, M., Tang, C., Zhi, C., Boron nitride nanotubes and nanosheets. ACS Nano 4 (2010), 2979–2993.
Kim, K., Kim, M., Hwang, Y., Kim, J., Chemically modified boron nitride-epoxy terminated dimethylsiloxane composite for improving the thermal conductivity. Ceram. Int. 40 (2014), 2047–2056.
Yu, J., Zhao, W., Liu, G., Wu, Y., Wang, D., Anti-corrosion mechanism of 2D nanosheet materials in waterborne epoxy coatings. Surf. Topogr. Metrol. Prop., 6, 2018, 034019.
Ysiwata-Rivera, A.P., Hernández-Hernández, E., Cadenas-Pliego, G., Ávila-Orta, C.A., González-Morones, P., Velásquez-de Jesús, J.A., Cuara-Díaz, E., Gallardo-Vega, C.A., Mata-Padilla, J.M., Effect of modified hexagonal boron nitride nanoparticles on the emulsion stability, viscosity and electrochemical behavior of nanostructured acrylic coatings for the corrosion protection of AISI 304 stainless steel. Coatings, 10, 2020, 488.
Lee, C.Y., Bae, J.H., Kim, T.Y., Chang, S.H., Kim, S.Y., Using silane-functionalized graphene oxides for enhancing the interfacial bonding strength of carbon/epoxy composites. Compos. Part A Appl. Sci. Manuf. 75 (2015), 11–17.
Akbarzadeh, S., Paint, Y., Olivier, M.-G., A comparative study of different sol-gel coatings for sealing the plasma electrolytic oxidation (PEO) layer on AA2024 alloy. Electrochim. Acta, 443, 2023, 141930.
Akbarzadeh, S., Sopchenski Santos, L., Vitry, V., Paint, Y., Olivier, M.G., Improvement of the corrosion performance of AA2024 alloy by a duplex PEO/clay modified sol-gel nanocomposite coating. Surf. Coatings Technol., 434, 2022, 128168.
Sopchenski, L., Robert, J., Touzin, M., Tricoteaux, A., Olivier, M.G., Improvement of wear and corrosion protection of PEO on AA2024 via sol-gel sealing. Surf. Coatings Technol., 417, 2021, 127195.
Ramezanzadeh, B., Haeri, Z., Ramezanzadeh, M., A facile route of making silica nanoparticles-covered graphene oxide nanohybrids (SiO2-GO); fabrication of SiO2-GO/epoxy composite coating with superior barrier and corrosion protection performance. Chem. Eng. J. 303 (2016), 511–528.
Huang, K., Liang, L., Chai, S., Tumuluri, U., Li, M., Wu, Z., Sumpter, B.G., Dai, S., Aminopolymer functionalization of boron nitride nanosheets for highly efficient capture of carbon dioxide. J. Mater. Chem. A 5 (2017), 16241–16248.
Majoul, N., Aouida, S., Bessaïs, B., Progress of porous silicon APTES-functionalization by FTIR investigations. Appl. Surf. Sci. 331 (2015), 388–391.
Yan, Y., Liao, K., Hu, J., Qin, M., He, T., Ou, T., Fan, Y., Leng, J., He, G., Effects of h-BN content and silane functionalization on thermal conductivity and corrosion resistance of h-BN/EPN coating. Surf. Coatings Technol., 476, 2024, 130185.
Ramezanzadeh, M., Dashan, A., Norouzi, F., Ramezanzadeh, B., Integration of metal co-dopted cysteine builted in porous covalent organic framework (COF) decorated 2D hexagonal boron nitride (h-BN) for multi-functional smart coatings. J. Colloid Interface Sci. 680 (2024), 311–331.
Ren, J., Stagi, L., Innocenzi, P., Hydroxylated boron nitride materials: from structures to functional applications. J. Mater. Sci. 56 (2020), 4053–4079.
Du, M., Wu, Y., Hao, X., A facile chemical exfoliation method to obtain large size boron nitride nanosheets. CrystEngComm 15 (2013), 1782–1786.
Rana, P., Dixit, R., Sharma, S., Dutta, S., Yadav, S., Sharma, A., Kaushik, B., Rana, P., Adholeya, A., Sharma, R.K., Enhanced catalysis through structurally modified hybrid 2-D boron nitride nanosheets comprising of complexed 2-hydroxy-4-methoxybenzophenone motif. Sci. Rep. 11 (2021), 1–13.
Kim, Y.J., Shin, T.S., Do Choi, H., Kwon, J.H., Chung, Y.C., Yoon, H.G., Electrical conductivity of chemically modified multiwalled carbon nanotube/epoxy composites. Carbon N. Y. 43 (2005), 23–30.
Shevelev, V.O., Bokai, K.A., Vilkov, O.Y., Makarova, A.A., Usachov, D.Y., Oxidation of h-BN on strongly and weakly interacting metal surfaces. Nanotechnology, 30, 2019, 234004.
Rho, H., Chon, K., Cho, J., Surface charge characterization of nanofiltration membranes by potentiometric titrations and electrophoresis: functionality vs. zeta potential. Desalination 427 (2018), 19–26.
Jia, K., Meng, X., Wang, W., Study on the preparation of high-temperature resistant and electrically insulating h-BN coating in ethanol solution by electrophoretic deposition. Processes, 9, 2021, 871.
Molaeipour, P., Ramezanzadeh, M., Ramezanzadeh, B., Stachys byzantina extract: a green biocompatible molecules source for graphene skeletons generation on the carbon steel for superior corrosion mitigation. Bioelectrochemistry, 143, 2022, 107970.
Parhizkar, N., Ramezanzadeh, B., Shahrabi, T., Enhancement of the corrosion protection properties of a hybrid sol-gel based silane film through impregnation of functionalized graphene oxide nanosheets. J. Electrochem. Soc. 164 (2017), C1044–C1058.
Li, C.P., Weng, M.C., Huang, S.L., Preparation and characterization of pH sensitive chitosan/3-glycidyloxypropyl trimethoxysilane (GPTMS) hydrogels by sol-gel method. Polymers (Basel), 12, 2020, E1326.
Ciobotaru, I.A., Maior, I., Vaireanu, D.I., Cojocaru, A., Caprarescu, S., Ciobotaru, I.E., The determination of the optimum hydrolysis time for silane films deposition. Appl. Surf. Sci. 371 (2016), 275–280.
Studer, K., Decker, C., Beck, E., Schwalm, R., Overcoming oxygen inhibition in UV-curing of acrylate coatings by carbon dioxide inerting, part I. Prog. Org. Coatings. 48 (2003), 92–100.
Sitthiracha, M., Kilmartin, P.A., Edmonds, N.R., Novel organic–inorganic hybrid materials based on epoxy-functionalized silanes. J. Sol-Gel Sci. Technol. 76 (2015), 542–551.
Otalvaro, J.O., Avena, M., Brigante, M., Adsorption of organic pollutants by amine functionalized mesoporous silica in aqueous solution. Effects of pH, ionic strength and some consequences of APTES stability. J. Environ. Chem. Eng., 7, 2019, 103325.
Alexander, C.L., Tribollet, B., Orazem, M.E., Contribution of surface distributions to constant-phase-element (CPE) behavior: 1. Influence of roughness. Electrochim. Acta 173 (2015), 416–424.
Liu, W., Pu, Y., Liao, H., Lin, Y., He, W., Corrosion and wear behavior of PEO coatings on D16T aluminum alloy with different concentrations of graphene. Coatings, 10, 2020, 249.
Zhu, M., Song, Y., Dong, K., Shan, D., Han, E.H., Correlation between the transient variation in positive/negative pulse voltages and the growth of PEO coating on 7075 aluminum alloy. Electrochim. Acta, 411, 2022, 140056.
Amand, S., Musiani, M., Orazem, M.E., Pébère, N., Tribollet, B., Vivier, V., Constant-phase-element behavior caused by inhomogeneous water uptake in anti-corrosion coatings. Electrochim. Acta 87 (2013), 693–700.
Yang, F., Liu, T., Li, J., Qiu, S., Zhao, H., Anticorrosive behavior of a zinc-rich epoxy coating containing sulfonated polyaniline in 3.5% NaCl solution. RSC Adv. 8 (2018), 13237–13247.
Akbarzadeh, S., Ramezanzadeh, M., Ramezanzadeh, B., Bahlakeh, G., A green assisted route for the fabrication of a high-efficiency self-healing anti-corrosion coating through graphene oxide nanoplatform reduction by Tamarindus indiaca extract. J. Hazard. Mater., 390, 2020, 122147.