Application of g-C₃N₄/sol—gel nanocomposite on AM60B magnesium alloy and investigation of its properties

Abstract

To protect the AM60B magnesium alloy from corrosion, a sol—gel coating containing hydroxylated g-C₃N₄ nanoplates was applied. The chemical composition of the hydroxylated g-C₃N₄ nanoplates was investigated using X-ray photoelectron spectroscopy (XPS). The hydroxylation process did not affect the crystal size, specific surface area, pore volume, average pore diameter, and thermal stability of the g-C₃N₄ nanoplates. After incorporating pristine and hydroxylated g-C₃N₄ nanoplates, dense sol-gel coatings were obtained. Transmission electron microscopy (TEM) revealed the uniform distribution of the modified g-C₃N₄ in the coating. The average roughness of the coating was also reduced after adding the modified nanoplates due to the decreased aggregation tendency. Electrochemical impedance spectroscopy (EIS) examinations in simulated acid rain revealed a significant improvement in the anticorrosion properties of the sol—gel film after the addition of the modified g-C₃N₄ due to the chemical bonding of the coating to the nanoplates.

Keywords

Mg alloy / corrosion protection / sol—gel / g-C₃N₄ nanocomposite / electrochemical impedance spectroscopy

References

[1] Z. Yin, R.H. He, Y. Chen, et al., Effects of surface micro-galvanic corrosion and corrosive film on the corrosion resistance of AZ91—xNd alloys, Appl. Surf. Sci., 536(2021), art. No. 147761.

[2] X. Dai, L. Wu, Y. Xia, et al., Intercalation of Y in Mg—Al layered double hydroxide films on anodized AZ31 and Mg—Y alloys to influence corrosion protective performance, Appl. Surf. Sci., 551(2021), art. No. 149432.

[3] G.L. Yang, Y.J. Ouyang, Z.H. Xie, Y. Liu, W.X. Dai, and L. Wu, Nickel interlayer enables indirect corrosion protection of magnesium alloy by photoelectrochemical cathodic protection, Appl. Surf. Sci., 558(2021), art. No. 149840.

[4] D.D. Zhang, F. Peng, and X.Y. Liu, Protection of magnesium alloys: From physical barrier coating to smart self-healing coating, J. Alloys Compd., 853(2021), art. No. 157010.

[5] P. Predko, D. Rajnovic, M.L. Grilli, et al., Promising methods for corrosion protection of magnesium alloys in the case of Mg—Al, Mg—Mn—Ce, and Mg—Zn—Zr: A recent progress review, Metals, 11(2021), No. 7, art. No. 1133.

[6] Hu RG, Zhang S, Bu JF, Lin CJ, Song GL. Recent progress in corrosion protection of magnesium alloys by organic coatings. Prog. Org. Coat., 2012, 73(2–3): 129.

[7] Ke C, Song MS, Zeng RC, et al. Interfacial study of the formation mechanism of corrosion resistant strontium phosphate coatings upon Mg—3Al—4.3Ca—0.1Mn. Corros. Sci., 2019, 151, 143.

[8] Saran D, Kumar A, Bathula S, Klaumünzer D, Sahu KK. Review on the phosphate-based conversion coatings of magnesium and its alloys. Int. J. Miner. Metall. Mater., 2022, 29(7): 1435.

[9] Kaseem M, Zehra T, Dikici B, Dafali A, Yang HW, Ko YG. Improving the electrochemical stability of AZ31 Mg alloy in a 3.5wt.% NaCl solution via the surface functionalization of plasma electrolytic oxidation coating. J. Magnes. Alloys, 2022, 10(5): 1311.

[10] Jin SY, Ma XC, Wu RZ, et al. Effect of carbonate additive on the microstructure and corrosion resistance of plasma electrolytic oxidation coating on Mg—9Li—3Al alloy. Int. J. Miner. Metall. Mater., 2022, 29(7): 1453.

[11] H. Chen, J. Shen, J.Z. Deng, Y.D. Hu, and Y.H. Zhang, Sol—gel coatings with hydrothermal hydroxylation as pre-treatment for 2198-T851 corrosion protection performance, Appl. Surf. Sci., 508(2020), art. No. 145285.

[12] Tarzanagh YJ, Seifzadeh D, Samadianfard R. Combining the 8-hydroxyquinoline intercalated layered double hydroxide film and sol—gel coating for active corrosion protection of the magnesium alloy. Int. J. Miner. Metall. Mater., 2022, 29(3): 536.

[13] A. Suárez-Vega, C. Agustín-Sáenz, L.A. O’dell, F. Brusciotti, A. Somers, and M. Forsyth, Properties of hybrid sol—gel coatings with the incorporation of lanthanum 4-hydroxy cinnamate as corrosion inhibitor on carbon steel with different surface finishes, Appl. Surf. Sci., 561(2021), art. No. 149881.

[14] I. Milošev, D. Hamulić, P. Rodič, et al., Siloxane polyacrylic sol—gel coatings with alkly and perfluoroalkyl chains: Synthesis, composition, thermal properties and long-term corrosion protection, Appl. Surf. Sci., 574(2022), art. No. 151578.

[15] Hernández-Barrios CA, Cuao CA, Jaimes MA, Coy AE, Viejo F. Effect of the catalyst concentration, the immersion time and the aging time on the morphology, composition and corrosion performance of TEOS—GPTMS sol—gel coatings deposited on the AZ31 magnesium alloy. Surf. Coat. Technol., 2017, 325, 257.

[16] C.A. Hernández-Barrios, J.A. Saavedra, S.L. Higuera, A.E. Coy, and F. Viejo, Effect of cerium on the physicochemical and anticorrosive features of TEOS—GPTMS sol—gel coatings deposited on the AZ31 magnesium alloy, Surf. Interfaces, 21(2020), art. No. 100671.

[17] Tiringer U, Milošev I, Durán A, Castro Y. Hybrid sol—gel coatings based on GPTMS/TEOS containing colloidal SiO₂ and cerium nitrate for increasing corrosion protection of aluminium alloy 7075-T6. J. Sol—Gel Sci. Technol., 2018, 85(3): 546.

[18] Izadi M, Shahrabi T, Ramezanzadeh B. Active corrosion protection performance of an epoxy coating applied on the mild steel modified with an eco-friendly sol—gel film impregnated with green corrosion inhibitor loaded nanocontainers. Appl. Surf. Sci., 2018, 440, 491.

[19] Zheludkevich ML, Salvado IM, Ferreira MGS. Sol—gel coatings for corrosion protection of metals. J. Mater. Chem., 2005, 15(48): 5099.

[20] Hammer P, dos Santos FC, Cerrutti BM, Pulcinelli SH, Santilli CV. Carbon nanotube-reinforced siloxane—PMMA hybrid coatings with high corrosion resistance. Prog. Org. Coat., 2013, 76(4): 601.

[21] Maeztu JD, Rivero PJ, Berlanga C, Bastidas DM, Palacio JF, Rodriguez R. Effect of graphene oxide and fluorinated polymeric chains incorporated in a multilayered sol—gel nanocoating for the design of corrosion resistant and hydrophobic surfaces. Appl. Surf. Sci., 2017, 419, 138.

[22] Akhtar S, Matin A, Kumar AM, Ibrahim A, Laoui T. Enhancement of anticorrosion property of 304 stainless steel using silane coatings. Appl. Surf. Sci., 2018, 440, 1286.

[23] S. Pourhashem, J.Z. Duan, F. Guan, N. Wang, Y. Gao, and B.R. Hou, New effects of TiO₂ nanotube/g-C₃N₄ hybrids on the corrosion protection performance of epoxy coatings, J. Mol. Liq., 317(2020), art. No. 114214.

[24] Kang SF, Zhang L, He MF, et al. “Alternated cooling and heating” strategy enables rapid fabrication of highly-crystalline g-C₃N₄ nanosheets for efficient photocatalytic water purification under visible light irradiation. Carbon, 2018, 137, 19.

[25] Pourhashem S, Rashidi A, Alaei M, Moradi MA, Maklavany DM. Developing a new method for synthesizing amine functionalized g-C₃N₄ nanosheets for application as anti-corrosion nanofiller in epoxy coatings. SN Appl. Sci., 2018, 1(1): 1.

[26] Y.Q. Xia, Y. He, C.L. Chen, Y.Q. Wu, F. Zhong, and J.Y. Chen, Co-modification of polydopamine and KH560 on g-C₃N₄ nanosheets for enhancing the corrosion protection property of waterborne epoxy coating, React. Funct. Polym., 146(2020), art. No. 104405.

[27] Y.Q. Xia, N.G. Zhang, Z.P. Zhou, et al., Incorporating SiO₂ functionalized g-C₃N₄ sheets to enhance anticorrosion performance of waterborne epoxy, Prog. Org. Coat., 147(2020), art. No. 105768.

[28] Yan SC, Li ZS, Zou ZG. Photodegradation performance of g-C₃N₄ fabricated by directly heating melamine. Langmuir, 2009, 25(17): 10397.

[29] Zheng Y, Zhang ZS, Li CH, Proulx S. Surface hydroxylation of graphitic carbon nitride: Enhanced visible light photocatalytic activity. Mater. Res. Bull., 2016, 84, 46.

[30] H.A. Zheng, Y. Liu, Y.H. Zhou, et al., Improved photocathodic protection performance of g-C₃N₄/rGO/ZnS for 304 stainless steel, J. Phys. Chem. Solids, 148(2021), art. No. 109672.

[31] Bu YY, Chen ZY, Yu JQ, Li WB. A novel application of g-C₃N₄ thin film in photoelectrochemical anticorrosion. Electrochim. Acta, 2013, 88, 294.

[32] C.L. Chen, Y. He, G.Q. Xiao, F. Zhong, Y.Q. Xia, and Y.Q. Wu, Graphic C₃N₄-assisted dispersion of graphene to improve the corrosion resistance of waterborne epoxy coating, Prog. Org. Coat., 139(2020), art. No. 105448.

[33] Yang DX, Velamakanni A, Bozoklu G, et al. Chemical analysis of graphene oxide films after heat and chemical treatments by X-ray photoelectron and micro-Raman spectroscopy. Carbon, 2009, 47(1): 145.

[34] Thomas A, Fischer A, Goettmann F, et al. Graphitic carbon nitride materials: Variation of structure and morphology and their use as metal-free catalysts. J. Mater. Chem., 2008, 18(41): 4893.

[35] Xu QX, Xu GQ, Yu QB, Yang K, Li HQ. Nitrogen self-doped high specific surface area graphite carbon nitride for photocatalytic degradating of methylene blue. J. Nanoparticle Res., 2019, 21(11): 1.

[36] J.H. Shi, T. Chen, C.L. Guo, et al., The bifunctional composites of AC restrain the stack of g-C₃N₄ with the excellent adsorption-photocatalytic performance for the removal of RhB, Colloids Surf. A, 580(2019), art. No. 123701.

[37] R. Samadianfard, D. Seifzadeh, A. Habibi-Yangjeh, and Y. Jafari-Tarzanagh, Oxidized fullerene/sol—gel nanocomposite for corrosion protection of AM60B magnesium alloy, Surf. Coat. Technol., 385(2020), art. No. 125400.

[38] R. Samadianfard, D. Seifzadeh, and A. Habibi-Yangjeh, Sol—gel coating filled with SDS-stabilized fullerene nanoparticles for active corrosion protection of the magnesium alloy, Surf. Coat. Technol., 419(2021), art. No. 127292.

[39] Nezamdoust S, Seifzadeh D. Application of Ce—V/sol—gel composite coating for corrosion protection of AM60B magnesium alloy. Trans. Nonferrous Met. Soc. China, 2017, 27(2): 352.

[40] N.J. Huang, Q.Q. Xia, Z.H. Zhang, et al., Simultaneous improvements in fire resistance and alarm response of GO paper via one-step 3-mercaptopropyltrimethoxysilane functionalization for efficient fire safety and prevention, Composites Part A, 131(2020), art. No. 105797.

[41] Ramezanzadeh B, Ahmadi A, Mahdavian M. Enhancement of the corrosion protection performance and cathodic delamination resistance of epoxy coating through treatment of steel substrate by a novel nanometric sol—gel based silane composite film filled with functionalized graphene oxide nanosheets. Corros. Sci., 2016, 109, 182.

[42] M. Mao, H. Xu, K.Y. Guo, et al., Mechanically flexible, super-hydrophobic and flame-retardant hybrid nanosilica/graphene oxide wide ribbon decorated sponges for efficient oil/water separation and fire warning response, Composites Part A, 140(2021), art. No. 106191.

[43] V. Kumar and B. Kandasubramanian, Ionic-liquid-assisted three-dimensional caged silica ablative nanocomposites, J. Appl. Polym. Sci., 134(2017), No. 38, art. No. 45328.

[44] Yu M, Qiao XY, Dong XJ, Sun K. Effect of particle modification on the shear thickening behaviors of the suspensions of silica nanoparticles in PEG. Colloid Polym. Sci., 2018, 296(11): 1767.

[45] Vivar Mora L, Taylor A, Paul S, et al. Impact of silica nanoparticles on the morphology and mechanical properties of sol-gel derived coatings. Surf. Coat. Technol., 2018, 342, 48.

[46] Y.H. Gao, W.L. Zhao, and Y. Chen, g-C₃N₄ modified by hydroxyl group on the surface prepared by double salt enhanced the visible light photocatalytic activity, Diam. Relat. Mater., 116(2021), art. No. 108425.

[47] R.Y. He, B.Y. Wang, J.H. Xiang, and T.J. Pan, Effect of copper additive on microstructure and anti-corrosion performance of black MAO films grown on AZ91 alloy and coloration mechanism, J. Alloys Compd., 889(2021), art. No. 161501.

[48] Song YW, Shan DY, Chen RS, Han EH. Corrosion characterization of Mg—8Li alloy in NaCl solution. Corros. Sci., 2009, 51(5): 1087.

[49] Sun L, Ma Y, Fan BF, Wang S, Wang ZY. Investigation of anti-corrosion property of hybrid coatings fabricated by combining PEC with MAO on pure magnesium. J. Magnes. Alloys, 2022, 10(10): 2875.

[50] Zhang CY, Zhang SY, Liu XP, He HC. Microstructure and corrosion properties of calcium phosphate coating on magnesium alloy prepared by hydrothermal treatment at various pH values. Rare Met. Mater. Eng., 2018, 47(10): 2993.

[51] Ayata S, Ensinger W. Ion beam sputter coating in combination with sol—gel dip coating of Al alloy tube inner walls for corrosion and biological protection. Surf. Coat. Technol., 2018, 340, 121.

[52] Nezamdoust S, Seifzadeh D. Email protected]/hybrid sol—gel nanocomposite for corrosion protection of 2024 aluminum alloy. Prog. Org. Coat., 2017, 109, 97.

[53] King AD, Birbilis N, Scully JR. Accurate electrochemical measurement of magnesium corrosion rates, a combined impedance, mass-loss and hydrogen collection study. Electrochim. Acta, 2014, 121, 394.

[54] M.A. Ashraf, Z.L. Liu, W.X. Peng, and N. Yoysefi, Amino acid and TiO₂ nanoparticles mixture inserted into sol—gel coatings: An efficient corrosion protection system for AZ91 magnesium alloy, Prog. Org. Coat., 136(2019), art. No. 105296.

[55] Li J, Cui JC, Yang JY, Ma Y, Qiu HX, Yang JH. Silanized graphene oxide reinforced organofunctional silane composite coatings for corrosion protection. Prog. Org. Coat., 2016, 99, 443.

[56] Hu JY, Li Q, Zhong XK, Zhang L, Chen B. Composite anticorrosion coatings for AZ91D magnesium alloy with molybdate conversion coating and silicon sol—gel coatings. Prog. Org. Coat., 2009, 66(3): 199.

[57] Ashassi-Sorkhabi H, Moradi-Alavian S, Kazempour A. Salt-nanoparticle systems incorporated into sol—gel coatings for corrosion protection of AZ91 magnesium alloy. Prog. Org. Coat., 2019, 135, 475.

[58] Ashassi-Sorkhabi H, Moradi-Alavian S, Jafari R, Kazempour A, Asghari E. Effect of amino acids and montmorillonite nanoparticles on improving the corrosion protection characteristics of hybrid sol—gel coating applied on AZ91 Mg alloy. Mater. Chem. Phys., 2019, 225, 298.

[59] Hu TT, Xiang B, Liao SG, Huang WZ. Corrosion of AM60B magnesium alloy in simulated acid rain. Anti-Corros. Methods Mater., 2010, 57(5): 244.

[60] Y.J. Tarzanagh, D. Seifzadeh, Z. Rajabalizadeh, A. Habibi-Yangjeh, A. Khodayari, and S. Sohrabnezhad, Sol—gel/MOF nanocomposite for effective protection of 2024 aluminum alloy against corrosion, Surf. Coat. Technol., 380(2019), art. No. 125038.