Hydrothermal synthesis of Zn-Mg-based layered double hydroxide coatings for the corrosion protection of copper in chloride and hydroxide media

Abstract

Layered double hydroxides (LDHs) hinder corrosive elements by forming a double layer and locking them between its layers. Hence, LDHs are interesting materials in corrosion inhibition. In this work, Zn-Mg-based LDHs are grown over a copper substrate by using a hydrothermal method. Two types of Zn-Mg-based LDH coating are prepared based on hydrothermal reaction time. Both types are characterized through Fourier transform infrared spectroscopy, Raman spectroscopy, high-resolution scanning electron microscopy, energy dispersive X-ray analysis, atomic force microscopy, and X-ray diffraction. Results show that the two types of LDH coating are successfully grown on copper; however, they differ in thickness and structural configuration. Corrosion testing of the LDH coatings is executed in 0.1 M NaCl and 0.1 M NaOH through alternating current impedance measurements and Tafel polarization curves. Results show that L48 gives more than 90% protection to copper, which is higher than the protection provided by L24. However, both LDH coatings (L24 and L48) are more effective corrosion inhibitors in NaCl than in NaOH, suggesting that the LDH coatings can more efficiently exchange Cl ions than OH ions.

Keywords

hydrothermal synthesis / layered double hydroxides / anticorrosion coating / ion exchange / copper substrate

References

[1] Jafari Y, Ghoreishi SM, Shabani-Nooshabadi M. Polyaniline/graphene nanocomposite coatings on copper: Electro-polymerization, characterization, and evaluation of corrosion protection performance. Synth. Met., 2016, 217, 220.

[2] Zhang DQ, Cai QR, He XM, Gao LX, Zhou GD. Inhibition effect of some amino acids on copper corrosion in HCl solution. Mater. Chem. Phys., 2008, 112(2): 353.

[3] Sherif ESM. Corrosion mitigation of copper in acidic chloride pickling solutions by 2-amino-5-ethyl-1,3,4-thiadiazole. J. Mater. Eng. Perform., 2010, 19(6): 873.

[4] Zhang DQ, Xie B, Gao LX, Cai QR, Joo HG, Lee KY. Intramolecular synergistic effect of glutamic acid, cysteine and glycine against copper corrosion in hydrochloric acid solution. Thin Solid Films, 2011, 520(1): 356.

[5] El-Etre AY. Natural honey as corrosion inhibitor for metals and alloys. I. Copper in neutral aqueous solution. Corros. Sci., 1998, 40(11): 1845.

[6] Wazzan NA. DFT calculations of thiosemicarbazide, arylisothiocynates, and 1-aryl-2,5-dithiohydrazodicarbonamides as corrosion inhibitors of copper in an aqueous chloride solution. J. Ind. Eng. Chem., 2015, 26, 291.

[7] Karthik N, Lee YR, Sethuraman MG. Hybrid sol-gel/thiourea binary coating for the mitigation of copper corrosion in neutral medium. Prog. Org. Coat., 2017, 102, 259.

[8] Farahati R, Ghaffarinejad A, Mousavi-Khoshdel SM, Rezania J, Behzadi H, Shockravi A. Synthesis and potential applications of some thiazoles as corrosion inhibitor of copper in 1 M HCl: Experimental and theoretical studies. Prog. Org. Coat., 2019, 132, 417.

[9] Alibakhshi E, Ghasemi E, Mahdavian M, Ramezanzadeh B, Farashi S. Active corrosion protection of ${\rm{Mg}} - {\rm{Al}} - {\rm{PO}}_4^{3 - }$ LDH nanoparticle in silane primer coated with epoxy on mild steel. J. Taiwan Inst. Chem. Eng., 2017, 75, 248.

[10] Alibakhshi E, Ghasemi E, Mahdavian M, Ramezanzadeh B. A comparative study on corrosion inhibitive effect of nitrate and phosphate intercalated Zn-Al-layered double hydroxides (LDHs) nanocontainers incorporated into a hybrid silane layer and their effect on cathodic delamination of epoxy topcoat. Corros. Sci., 2017, 115, 159.

[11] Alibakhshi E, Ghasemi E, Mahdavian M, Ramezanzadeh B. Fabrication and characterization of layered double hydroxide/silane nanocomposite coatings for protection of mild steel. J. Taiwan Inst. Chem. Eng., 2017, 80, 924.

[12] Mishra G, Dash B, Pandey S, Sethi D. Ternary layered double hydroxides (LDH) based on Cu-substituted Zn-Al for the design of efficient antibacterial ceramics. Appl. Clay Sci, 2018, 165, 214.

[13] Zeng RC, Li XT, Liu ZG, Zhang F, Li SQ, Cui HZ. Corrosion resistance of Zn-Al layered double hydroxide/poly(lactic acid) composite coating on magnesium alloy AZ₃₁. Front. Mater. Sci., 2015, 9(4): 355.

[14] Zhang F, Liu ZG, Zeng RC, Li SQ, Cui HZ, Song L, Han EH. Corrosion resistance of Mg-Al-LDH coating on magnesium alloy AZ31. Surf. Coat. Technol., 2014, 258, 1152.

[15] Lin JK, Jeng KL, Uan JY. Crystallization of a chemical conversion layer that forms on AZ91D magnesium alloy in carbonic acid. Corros. Sci., 2011, 53(11): 3832.

[16] Lin JK, Hsia CL, Uan JY. Characterization of Mg,Al-hydrotalcite conversion film on Mg alloy and Cl⁻ and ${\rm{CO}}_3^{2 - }$ an-ion-exchangeability of the film in a corrosive environment. Scr. Mater., 2007, 56(11): 927.

[17] Ji G, Shukla SK, Dwivedi P, Sundaram S, Prakash R. Inhibitive effect of argemone mexicana plant extract on acid corrosion of mild steel. Ind. Eng. Chem. Res., 2011, 50(21): 11954.

[18] Ji G, Dwivedi P, Sundaram S, Prakash R. Inhibitive effect of chlorophytum borivilianum root extract on mild steel corrosion in HCl and H₂SO₄ solutions. Ind. Eng. Chem. Res, 2013, 52(31): 10673.

[19] Tiwari M, Gupta VK, Singh RA, Ji G, Prakash R. Donor-π-acceptor-type configured, dimethylamino-based organic push-pull chromophores for effective reduction of mild steel corrosion loss in 1 M HCl. ACS Omega, 2018, 3(4): 4081.

[20] Ishizaki T, Chiba S, Watanabe K, Suzuki H. Corrosion resistance of Mg-Al layered double hydroxide container-containing magnesium hydroxide films formed directly on magnesium alloy by chemical-free steam coating. J. Mater. Chem. A, 2013, 1(31): 8968.

[21] Wang LD, Zhang KY, Sun W, Wu TT, He HR, Liu GC. Hydrothermal synthesis of corrosion resistant hydrotalcite conversion coating on AZ91D alloy. Mater. Lett., 2013, 106, 111.

[22] Kloprogge JT, Hickey L, Frost RL. FT-Raman and FT-IR spectroscopic study of synthetic Mg/Zn/Al-hydrotalcites. J. Raman Spectrosc., 2004, 35(11): 967.

[23] Tiwari P, Srivastava M, Mishra R, Ji G, Prakash R. Economic use of waste Musa paradisica peels for effective control of mild steel loss in aggressive acid solutions. J. Environ. Chem. Eng., 2018, 6(4): 4773.

[24] Srivastava M, Tiwari P, Srivastava SK, Kumar A, Ji G, Prakash R. Low cost aqueous extract of Pisum sativum peels for inhibition of mild steel corrosion. J. Mol. Liq., 2018, 254, 357.

[25] Ji G, Anjum S, Sundaram S, Prakash R. Musa paradisica peel extract as green corrosion inhibitor for mild steel in HCl solution. Corros. Sci., 2015, 90, 107.

[26] Ferreira ES, Giacomelli C, Giacomelli FC, Spinelli A. Evaluation of the inhibitor effect of _L-ascorbic acid on the corrosion of mild steel. Mater. Chem. Phys, 2004, 83(1): 129.

[27] Li WH, He Q, Zhang ST, Pei CL, Hou BR. Some new triazole derivatives as inhibitors for mild steel corrosion in acidic medium. J. Appl. Electrochem., 2008, 38(3): 289.

[28] Ji G, Dwivedi P, Sundaram S, Prakash R. Aqueous extract of Argemone mexicana roots for effective protection of mild steel in an HCl environment. Res. Chem. Intermed., 2016, 42(2): 439.

[29] Xiang TF, Zheng SL, Zhang M, Sadig HR, Li C. Bioinspired slippery zinc phosphate coating for sustainable corrosion protection. ACS Sustainable Chem. Eng., 2018, 6(8): 10960.

[30] Lgaz H, Salghi R, Jodeh S, Hammouti B. Effect of clozapine on inhibition of mild steel corrosion in 1.0 M HCl medium. J. Mol. Liq., 2017, 225, 271.

[31] E. Alibakhshi, E. Ghasemi, M. Mahdavian, B. Ramezanzadeh, and M. Yasaei, The effect of interlayer spacing on the inhibitor release capability of layered double hydroxide based nanocontainers, J. Cleaner Prod., 251(2020), art. No. 119676.

[32] Solomon MM, Umoren SA, Abai EJ. Poly(methacrylic acid)/silver nanoparticles composites: In-situ preparation, characterization and anticorrosion property for mild steel in H₂SO₄ solution. J. Mol. Liq., 2015, 212, 340.

[33] Ji G, Macía LF, Allaert B, Hubin A, Terryn H. Odd random phase electrochemical impedance spectroscopy to study the corrosion behavior of hot dip Zn and Zn-alloy coated steel wires in sodium chloride solution. J. Electrochem. Soc., 2018, 165(5): 246.

[34] Arenas MA, García I, de Damborenea J. X-ray photoelectron spectroscopy study of the corrosion behaviour of galvanised steel implanted with rare earths. Corros. Sci., 2004, 46(4): 1033.

[35] Deslouis C, Duprat M, Tournillon C. The kinetics of zinc dissolution in aerated sodium sulphate solutions. A measurement of the corrosion rate by impedance techniques. Corros. Sci., 1989, 29(1): 13.

[36] Xu JX, Song YB, Zhao YH, Jiang LH, Mei YJ, Chen P. Chloride removal and corrosion inhibitions of nitrate, nitrite-intercalated Mg-Al layered double hydroxides on steel in saturated calcium hydroxide solution. Appl. Clay Sci., 2018, 163, 129.