Abstract
The present work fits into the efforts deployed to minimize the huge problems related to corrosion phenomena. As several industries are affected by the deterioration of metallic materials, new solutions need to be offered by the scientific community. In this context, we describe, in this paper, the electrochemical synthesis of polydiphenylamine coating (PDPA) on steel in an organic solution consisting of CH2Cl2 as solvent and N(Bu)4PF6 as supporting electrolyte. The electrolytic medium has been retained after a preliminary electrogravimetric study has shown that it can inhibit the working electrode dissolution without preventing the PDPA film formation. Spectroscopic and microscopic analyses were then achieved for the elaborated coatings. Analyses by X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FTIR) have allowed a detailed characterization of the polymer (molecular structure, doping rate, chain length, …). In addition, morphological characterization by scanning electron microscope (SEM) confirmed that the value of the applied current density has a direct influence on the properties of the obtained polymer. The homogeneity and high adherence of the prepared PDPA film allow its use as a protective coating against steel dissolution. For this, corrosion tests were performed by studying the open-circuit potential (OCP), linear polarization curve (Tafel) as well as electrochemical impedance spectroscopy (EIS). The studies achieved in 3% NaCl solution have confirmed that the potential of the steel electrode shifts towards its passivation domain with the presence of PDPA coating. The latter is stable over time in contact with an aggressive solution and the inhibitory efficiency reached 97.2%.
Similar content being viewed by others
Explore related subjects
Discover the latest articles, news and stories from top researchers in related subjects.References
Aouzal Z et al (2020) Improvement of the anticorrosion resistance of nickel by polypyrrole coating electrosynthesized in salicylate medium. Mater Today Proc 31:S89–S95. https://doi.org/10.1016/j.matpr.2020.06.237
Jadi SB et al (2020) Electropolymerization and corrosion resistance of polypyrrole on nickel bipolar plate for PEM fuel cell application. Mater Today Proc 22:52–56. https://doi.org/10.1016/j.matpr.2019.08.072
El Jaouhari A et al (2017) Corrosion resistance and antibacterial activity of electrosynthesized polypyrrole. Synth Met 226:15–24. https://doi.org/10.1016/j.synthmet.2017.01.008
El Jaouhari A et al (2018) Comparison study between corrosion protection of polypyrrole synthesized on stainless steel from phthalate and saccharinate aqueous medium. Polym Test 67:302–308. https://doi.org/10.1016/j.polymertesting.2018.03.022
González MB, Saidman SB (2015) Electrodeposition of bilayered polypyrrole on 316 L stainless steel for corrosion prevention. Prog Org Coatings 78:21–27. https://doi.org/10.1016/J.PORGCOAT.2014.10.012
Nautiyal A, Qiao M, Cook JE, Zhang X, Huang TS (2018) High performance polypyrrole coating for corrosion protection and biocidal applications. Appl Surf Sci 427:922–930. https://doi.org/10.1016/J.APSUSC.2017.08.093
Yin Y, Prabhakar M, Ebbinghaus P, Corrêa da Silva C, Rohwerder M (2022) Neutral inhibitor molecules entrapped into polypyrrole network for corrosion protection. Chem Eng J 440:135739. https://doi.org/10.1016/J.CEJ.2022.135739
Mehandzhiyski Y, Zhao X, Liu X, Fan B, Zheng X (2022) Optimized Anticorrosion of Polypyrrole Coating by Inverted-Electrode Strategy: Experimental and Molecular Dynamics Investigations. mdpi.com. https://doi.org/10.3390/polym14071356
Feliú S, Emelyanenko A, Zhu H, Liu X, Hao H, Zheng X (2022) Influence of Surface Pretreatments on the Anticorrosion of Polypyrrole Electro-Polymerized Coatings for Copper in Artificial Seawater. mdpi.com. https://doi.org/10.3390/met12030383
Sang Y et al (2022) Synthetic polyaniline-boron nitride-aqueous epoxy resin composite coating for improving the corrosion resistance of hot-dip galvanized steel plates. Appl Surf Sci 592:153229. https://doi.org/10.1016/J.APSUSC.2022.153229
Pan W, Dong J, Gui T, Liu R, Liu X, Luo J (2022) Fabrication of dual anti-corrosive polyaniline microcapsules via Pickering emulsion for active corrosion protection of steel. Soft Matter 18(14):2829–2841. https://doi.org/10.1039/D2SM00062H
Wu K, Gui T, Dong J, Luo J, Liu R (2022) Synthesis of robust polyaniline microcapsules via UV-initiated emulsion polymerization for self-healing and anti-corrosion coating. Prog Org Coatings 162:106592. https://doi.org/10.1016/J.PORGCOAT.2021.106592
Fuseini M, Mahmoud M, Zaghloul Y, Elkady MF, El-Shazly AH (2022) Evaluation of synthesized polyaniline nanofibres as corrosion protection film coating on copper substrate by electrophoretic deposition. J Mater Sci 57(10):6085–6101. https://doi.org/10.1007/S10853-022-06994-3
Wang Q (2022) Preparation of Polyaniline/Epoxy Composite and Its Anti-Corrosion Performance. Int J Electrochem Sci 17:220416. https://doi.org/10.20964/2022.04.26
Li X, Liu X, Liu H, Liu X, He R, Meng S (2022) Structure, morphology and anti-corrosion performance of polyaniline modified molybdenum sulfide/epoxy composite coating. Colloids Surf A Physicochem Eng Asp 639:128345. https://doi.org/10.1016/J.COLSURFA.2022.128345
Bouabdallaoui M et al (2020) Influence of polythiophene overoxidation on its physicochemical properties and corrosion protection performances. Mater Today Proc 31:S69–S74. https://doi.org/10.1016/j.matpr.2020.06.067
Conde-Nicho J, Nicho ME, Rodríguez JA, León-Silva U, Rodríguez-Lelis JM (2022) Corrosion protection by poly(3-hexylthiophene)/poly(methyl-methacrylate) coating of cracked 410 stainless steel. Anti-Corrosion Methods Mater. https://doi.org/10.1108/ACMM-07-2021-2507 (ahead-of-print)
Xavier JR (2021) Corrosion protection performance and interfacial interactions of polythiophene/silanes/MnO2 nanocomposite coatings on magnesium alloy in marine environment. Int J Polym Anal Charact 26(4):309–329. https://doi.org/10.1080/1023666X.2021.1887627
Yadav PK, Prakash O, Ray B, Maiti P (2021) Functionalized polythiophene for corrosion inhibition and photovoltaic application. J Appl Polym Sci 138(44):51306. https://doi.org/10.1002/APP.51306
Zhao Y, Chen M, Liu X, Xu T, Liu W (2005) Electrochemical synthesis of polydiphenylamine nanofibrils through AAO template. Mater Chem Phys 91:518–523. https://doi.org/10.1016/j.matchemphys.2004.12.019
Athawale AA, Deore BA, Chabukswar VV (1999) Studies on poly(diphenylamine) synthesized electrochemically in nonaqueous media. Mater Chem Phys 58:94–100. https://doi.org/10.1016/S0254-0584(98)00258-2
Bitew Z, Kassa A, Misgan B (2022) Poly(diphenylamine-4-sulfonic acid) modified glassy carbon electrode for voltammetric determination of gallic acid in honey and peanut samples. Arab J Chem 15:103853. https://doi.org/10.1016/J.ARABJC.2022.103853
Obrezkov FA, Shestakov AF, Vasil’ev SG, Stevenson KJ, Troshin PA (2021) Polydiphenylamine as a promising high-energy cathode material for dual-ion batteries. J Mater Chem A 9(5):2864–2871. https://doi.org/10.1039/D0TA09427G
Ozkan SZ et al (2021) One-step synthesis, characterization and properties of novel hybrid electromagnetic nanomaterials based on polydiphenylamine and Co–Fe particles in the absence and presence of single-walled carbon nanotubes. RSC Adv 11(40):24772–24786. https://doi.org/10.1039/D1RA03114G
Khatoon H, Ahmad S (2019) Vanadium Pentoxide-Enwrapped Polydiphenylamine/Polyurethane Nanocomposite: High-Performance Anticorrosive Coating. ACS Appl Mater Interfaces 11(2):2374–2385. https://doi.org/10.1021/ACSAMI.8B17861/SUPPL_FILE/AM8B17861_SI_001.PDF
Lingam R (2019) Synthesis and Electrochemical Characterisation of Novel Hybrid Copper/Poly (diphenylamine) (PDPA) Nanocomposites. Int J Recent Technol Eng 8:2277–3878. https://doi.org/10.35940/ijrte.D1156.1284S219
Hu J-Q, Yang SZ, Zhang JJ, Guo L, Xu X (2019) Synthesis and Anti-Oxidative Properties of Poly(diphenylamine) Derivative as Lubricant Antioxidant. Pet Chem 59(9):1037–1042. https://doi.org/10.1134/S0965544119090081
Muthusankar E, Lee SC, Ragupathy D (2019) Enhanced Electron Transfer Characteristics of Surfactant Wrapped SnO 2 Nanorods Impregnated Poly(diphenylamine) Matrix. Sens Lett 16(12):911–917. https://doi.org/10.1166/SL.2018.4031
Bazzaoui M, Bazzaoui EA, Martins JI, Martins L (2004) Electrochemical Synthesis of Polythiophene Coatings on Zinc and a Zinc Alloy in Organic Media. Mater Sci Forum 455–456:484–488. https://doi.org/10.4028/www.scientific.net/MSF.455-456.484
Petitjean J, Aeiyach S, Ferreira CA, Lacaze PC, Takenouti H (1995) A new oscillatory electrocheical phenomenon observed in the electropolymerization of pyrrole in MeCN+N(Bu)4PF6 on an Iron electrode studied by the ring-disk-electrode technique. J Electrochem Soc 142(1):136–142
Ferreira CA, Aeiyach S, Delamar M, Lacaze PC (1990) Electropolymerization of pyrrole on iron electrodes Influence of solvent and electrolyte on the nature of the deposits. J Electroanal Chem 284:351–369. https://doi.org/10.1016/j.jelechem.2005.02.001
Tourillon G, Garnier F (1984) Morphology of conducting organic polymers: Polythiophene and poly(3-methyl thiophene). J Polym Sci 22:33–39. https://doi.org/10.1002/pol.1984.180220103
Tourillon G, Garnier F (1983) Stability of Conducting Polythiophene and Derivatives. J Electrochem Soc 130(10):2042–2044. https://doi.org/10.1149/1.2119517
Aeiyach S, Bazzaoui EA, Lacaze PC (1997) Electropolymerization of thiophene on oxidizable metals in organic media. J Electroanal Chem 434:153–162. https://doi.org/10.1016/S0022-0728(97)00044-2
Odziemkowski M, Krell M, Irish DE (1992) A Raman Microprobe In Situ and Ex Situ Study of Film Formation at Lithium/Organic Electrolyte Interfaces. J Electrochem Soc 139(11):3052–3063. https://doi.org/10.1149/1.2069032
Chan HSO, Ng SC, Sim WS, Tan KL, Tan BTG (1992) Preparation and Characterization of Electrically Conducting Copolymers of Aniline and Anthranilic Acid: Evidence for Self-Doping by X-ray Photoelectron Spectroscopy. Macromolecules 25:6029–6034. https://doi.org/10.1021/ma00048a026
Golczak S, Kanciurzewska A, Fahlman M, Langer K, Langer JJ (2008) Comparative XPS surface study of polyaniline thin films. Solid State Ionics 179:2234–2239. https://doi.org/10.1016/j.ssi.2008.08.004
Chang C-F, Chen W-C, Wen T-C, Gopalan A (2002) Electrochemical and Spectroelectrochemical Studies on Copolymerization of Diphenylamine with 2,5-Diaminobenzenesulfonic Acid. J Electrochem Soc 149(8):E298–E305. https://doi.org/10.1149/1.1491984
Kilmartin PA, Wright GA (1997) Photoelectrochemical and spectroscopic studies of sulfonated polyanilines Part I. Copolymers of orthanilic acid and aniline. Synth Met 88:153–162. https://doi.org/10.1016/S0379-6779(97)03854-X
Wu M-S, Wen T-C, Gopalan A (2001) Electrochemical Copolymerization of Diphenylamine and Anthranilic Acid with Various Feed Ratios. J Electrochem Soc 148(5):D65–D73. https://doi.org/10.1149/1.1366625
Bouabdallaoui M et al (2017) X-ray photoelectron and in situ and ex situ resonance Raman spectroscopic investigations of polythiophene overoxidation. J Solid State Electrochem 21(12):3519–3532. https://doi.org/10.1007/s10008-017-3698-9
Eshkenazi V, Peled E, Burstein L, Golodnitsky D (2004) XPS analysis of the SEI formed on carbonaceous materials. Solid State Ion 170:83–91. https://doi.org/10.1016/S0167-2738(03)00107-3
Ugalde L, Bernede JC, Del Valle MA, Díaz FR, Leray P (2002) SEM study of the growth of electrochemically obtained polythiophene thin films: Effect of electrolyte and monomer concentration in acetonitrile. J Appl Polym Sci 84:1799–1809. https://doi.org/10.1002/app.10291
Abraham KM, Goldman JL, Natwig DL (1982) Characterization of Ether Electrolytes for Rechargeable Lithium Cells. J Electrochem Soc 129(11):2404–2409. https://doi.org/10.1149/1.2123556
Shifler DA, Moran PJ, Kruger J (1991) The passivity of iron and carbon steel in anhydrous propylene carbonate solutions. Corros Sci 32(5/6):475–496. https://doi.org/10.1016/0010-938X(91)90102-U
Nelson AJ, Glenis S, Frank AJ (1987) XPS and UPS investigation of PF6 doped and undoped poly 3methyl thiophene. J Chern Phys 87(8):5002–5006. https://doi.org/10.1063/1.452815
Cai M, Liang Y, Zhou F, Liu W (2011) Tribological Properties of Novel Imidazolium Ionic Liquids Bearing Benzotriazole Group as the Antiwear/Anticorrosion Additive in Poly(ethylene glycol) and Polyurea Grease for Steel/Steel Contacts. ACS Appl Mater Interfaces 3:4580–4592
Bazzaoui EA, Bazzaoui M, Aubard J, Lomas JS, Félidj N, Lévi G (2001) Surface-enhanced Raman scattering study of polyalkylthiophenes on gold electrodes and in silver colloids. Synth Met 123:299–309. https://doi.org/10.1016/S0379-6779(01)00299-5
Bazzaoui EA, Lévi G, Aeiyach S, Aubard J, Marsault JP, Lacaze PC (1995) SERS spectra of polythiophene in doped and undoped states. J Phys Chem 99:6628–6634. https://doi.org/10.1021/j100017a052
Bazzaoui EA, Marsault JP, Aeiyach S, Lacaze PC (1994) Resonance Raman study of polythiophene films in the doped and undoped states. Relations between spectral data and physicochemical properties. Synth Met 66:217–224. https://doi.org/10.1016/0379-6779(94)90070-1
Bazzaoui EA, Aubard J, Félidj N, Laurent G, Lévi G (2005) Ex situ and in situ SERS analyses of polybithiophene using roughened Ag and Cu electrodes and multilayer SERS-active systems. J Raman Spectrosc 36:817–823. https://doi.org/10.1002/jrs.1368
Bazzaoui EA, Aeiyach S, Lacaze PC (1996) Electropolymerization of bithiophene on Pt and Fe electrodes in an aqueous sodium dodecylsulfate (SDS) micellar medium. Synth Met 83:159–165. https://doi.org/10.1016/S0379-6779(97)80070-7
Showkat AM, Cao XT, Kim DW, Islam MR, Lim KT (2015) Characterization of poly(diphenylamine)-gold nanocomposites obtained by self-assembly. IOP Conf Ser Mater Sci Eng 77:1–8. https://doi.org/10.1088/1757-899X/77/1/012007
Kim SB, Harada K, Yamamoto T (1998) Preparation of poly(diphenylamine-4,4′-diyl) and related random copolymers by organometallic polycondensation. Electrical, electrochemical, and optical properties. Macromolecules 31:988–993. https://doi.org/10.1021/ma971244f
Showkat AM, Cao XT, Kim DW, Kim YH, Lim KT (2016) Self-Assembly Directed One-Step Synthesis of Conducting Poly(diphenylamine)/Gold Nanocomposites. Sci Adv Mater 8:318–321. https://doi.org/10.1166/sam.2016.2486
Tang J, Jing X, Wang B, Wang F (1988) Infrared spectra of soluble polyaniline. Synth Met 24:231–238. https://doi.org/10.1016/0379-6779(88)90261-5
Dong S, Song FY, Li Z (1992) Electrochemical Synthesis and Characterization of polydiphenylamine. Chin J Chem 10(1):10–16. https://doi.org/10.1088/1742-6596/431/1/012003
Md Showkat A, Md Showkat KP, Gopalan AI, Kim SH, Choi SH, Sohn SH (2006) Characterization and preparation of new multiwall carbon nanotube/conducting polymer composites by in situ polymerization. J Appl Polym Sci 101:3721–3729. https://doi.org/10.1002/app.23359
Ozkan SZ, Dzidziguri EL, Karpacheva GP, Bondarenko GN (2011) Synthesis, structure, and properties of new Cu/polydiphenylamine metallopolymer nanocomposites. Nanotechnologies Russ 6(11–12):750–756. https://doi.org/10.1134/S1995078011060115
Ozkan SZ, Dzidziguri EL, Chernavskii PA, Karpacheva GP, Efimov MN, Bondarenko GN (2013) Metal-polymer nanocomposites based on polydiphenylamine and cobalt nanoparticles. Nanotechnologies Russ 8(7–8):452–460. https://doi.org/10.1134/S1995078013040113
Fenelon AM, Breslin CB (2005) The Formation of Polypyrrole at Iron from 1-Butyl-3-methylimidazolium Hexafluorophosphate. J Electrochem Soc 152(1):D6–D11. https://doi.org/10.1149/1.1831211
Gambino D et al (1999) Synthesis, Characterization, and Crystal Structure of [ReO(Me4tu)4](PF6)3 (tu = thiourea). Z Anorg Allg Chem 625:813–819
Heinze J, Frontana-uribe BA, Ludwigs S (2010) Electrochemistry of Conducting Polymers s Persistent Models and New. Chem Rev 110:4724–4771
Kraljić M, Mandić Z, Duić L (2003) Inhibition of steel corrosion by polyaniline coatings. Corros Sci 45(1):181–198. https://doi.org/10.1016/S0010-938X(02)00083-5
Minh L, Quoc V (2013) Layers of Inhibitor Anion – Doped Polypyrrole for Corrosion Protection of Mild Steel. Materials Science - Advanced Topics. InTech
Roberge PR, Pierre R (1999) Handbook of Corrosion Engineering. McGraw-Hill
Sathiyanarayanan S, Muthukrishnan S, Venkatachari G (2006) Synthesis and anticorrosion properties of polydiphenylamine blended vinyl coatings. Synth Met 156:1208–1212. https://doi.org/10.1016/j.synthmet.2006.08.008
Beck F, Barsch U, Michaelis R (1993) Corrosion of conducting polymers in aqueous media. J Electroanal Chem 351(1–2):169–184. https://doi.org/10.1016/0022-0728(93)80232-7
Christensen PA, Hamnett A (1991) In situ spectroscopic investigations of the growth, electrochemical cycling and overoxidation of polypyrrole in aqueous solution. Electrochim Acta 36(8):1263–1286. https://doi.org/10.1016/0013-4686(91)80005-S
Hien NTL, Garcia B, Pailleret A, Deslouis C (2005) Role of doping ions in the corrosion protection of iron by polypyrrole films. Electrochim Acta 50(7–8):1747–1755. https://doi.org/10.1016/j.electacta.2004.10.072
Inzelt G (2018) Conducting polymers: past, present, future. J Electrochem Sci Eng 8(1):3–37. https://doi.org/10.5599/jese.448
Deshpande PP, Jadhav NG, Gelling VJ, Sazou D (2014) Conducting polymers for corrosion protection : a review. J Coat Technol Res. https://doi.org/10.1007/s11998-014-9586-7
Paliwoda-Porebska G, Rohwerder M, Stratmann M, Rammelt U, Duc LM, Plieth W (2006) Release mechanism of electrodeposited polypyrrole doped with corrosion inhibitor anions. J Solid State Electrochem 10(9):730–736. https://doi.org/10.1007/s10008-006-0118-y
Plieth W, Bund A, Rammelt U, Neudeck S, Duc LM (2006) The role of ion and solvent transport during the redox process of conducting polymers. Electrochim Acta 51(11):2366–2372. https://doi.org/10.1016/j.electacta.2005.03.087
Rammelt U, Duc LM, Plieth W (2005) Improvement of protection performance of polypyrrole by dopant anions. J Appl Electrochem 35(12):1225–1230. https://doi.org/10.1007/s10800-005-9033-7
Shinde VP (2017) Study of water transport characteristics of poly ( o -ethylaniline ) coatings : corrosion mechanism. Ionics. https://doi.org/10.1007/s11581-017-2213-8
Sangaj NS, Malshe VC (2004) Permeability of polymers in protective organic coatings. Prog Org Coatings 50(1):28–39. https://doi.org/10.1016/j.porgcoat.2003.09.015
Herrasti P, del Rio AI, Recio J (2007) Electrodeposition of homogeneous and adherent polypyrrole on copper for corrosion protection. Electrochim Acta 52:6496–6501. https://doi.org/10.1016/j.electacta.2007.04.074
Funding
This work was supported by the MESRSFC and CNRST (Morocco) under grant No. PPR/30/2015.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interests
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Bouabdallaoui, M., El Guerraf, A., Aouzal, Z. et al. Extremely adherent and protective polymeric coating based on polydiphenylamine electrodeposited on steel in an organic electrolytic medium. J Polym Res 29, 357 (2022). https://doi.org/10.1007/s10965-022-03215-y
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s10965-022-03215-y