Active anticorrosion and self-healing coatings: A review with focus on multi-action smart coating strategies

doi:10.1016/j.jmst.2021.11.042

Abstract

Abstract:

The development of smart coatings with potential for active anticorrosion and self-healing protection of metals is essential for long-term performance of metallic structures in aggressive chemical environments. Presently, emphasis has been placed on the development of advanced smart coatings for corrosion protection in different applications. Innovative multifunctional coatings with fascinating stimuli-responsive functionalities are considered “smart”. The stimuli-responsive functionalities of these smart coatings when properly harnessed result in a class of coatings with inherent autonomous control of corrosion. Fundamentally, when metals are exposed to aggressive environments, occurrences at the metal-solution interface cause environmental changes. These changes can be controlled when triggers from external environment set off active components of smart coating, thereby enhancing coating's life and functionality. Common triggers include the availability of moisture, concentration of chloride ion, pH gradient, mechanical damage, impact, fatigue, light, redox activity and temperature. In this review, recent technological trends in active anticorrosion and self-healing coatings as functional routes for metal protection are summarized, stimuli responsiveness and mechanisms of inhibition are discussed, and recent multi-action protective systems are particularly focused on.

Key words: Smart coating, Active anticorrosion protection, Self-healing, Multi-action, Protection mechanism

Inime Ime Udoh, Hongwei Shi, Enobong Felix Daniel, Jianyang Li, Songhua Gu, Fuchun Liu, En-Hou Han. Active anticorrosion and self-healing coatings: A review with focus on multi-action smart coating strategies[J]. J. Mater. Sci. Technol., 2022, 116: 224-237.

Figures/Tables 16

Fig. 1. Schematic representation of three ways of achieving self-healing at defect site. (a) Polymer network of the coating itself fills up the defect site and restores coating barrier, (b) reactive monomers released from microcapsules polymerize and seal up defect site, and (c) released corrosion inhibitors from preloaded nano-/micro-containers passivate the metal surface.

Fig. 2. Images of coating after immersion in 0.1 M NaCl solution for 20 days: blank coating (a), coatings with MSNs (b), MSNs-BTA (c), and MSNs-BTA@PDA (d). Adapted with permission from [49] (https://pubs.acs.org/doi/10.1021/acsami.8b21197), Copyright (2019), American Chemical Society.

Table 1. Summary of nano/microcontainers, active substances and assessment methods in active anticorrosion coatings.

Nano/microcontainers	Active substance	Assessment method (s)	Ref.
Zeolitic imidazolate	polyethylene glycol-tannic acid complex	EIS	[53]
Halloysite nanotubes	imidazole, dodecylamine	EIS	[54]
Graphene oxide nanoplatform	Tamarindus indiaca extract, Zn²⁺	EIS, FE-SEM, SST	[55]
Mesoporous silica nanoparticles	benzotriazole, benzalkonium chloride	SVET, EIS	[56]
Silica nanocapsules	2-mercaptobenzothiazole	EIS	[57]
Dendrimer-like mesoporous silica nanocontainer	8- hydroxyquinoline	EIS, SVET, SFIM	[58]
Zeolitic imidazolate framework-8	benzotriazole, tannic acid	EIS	[59]
Ceria nanoparticles	Zirconium	Tafel polarization, EIS	[60]
Poly(urea-formaldehyde)-based microcapsules	oleyl phosphate	UV irradiation, SEM, PDP, EIS	[61]
Poly methyl methacrylate nanocapsules	triethanolamine	OM, SEM, EIS	[62]
Polydopamine modified mesoporous silica/graphene oxide,	benzotriazole	EIS, SEM	[63]
Graphene/halloysite nanotubes	L-histidine	EIS	[64]
Phenylene-bridged hollow periodic mesoporous organosilica	2-Mercaptobenzothiazole	EIS, PDP, SEM, AFM, MD	[65]
Metal organic frameworks	tetraethyl orthosilicate, graphene oxide, benzotriazole	EIS	[66]
Graphene	carbon dot	EIS, SVET, LSCM, SEM, XPS	[67]
Zn-Al layered double hydroxides	Nitrates	XRD, IC	[68]
Hollow carbon spheres	Zn²⁺	FESEM, ICP-OES, EIS, PDP	[69]
Nano-ZrO₂,	tannic acid, d-limonene	Raman, SEM, EIS	[70]
Mesoporous silica nanoparticles	1,10-phenanthroline, Chitosan-sodium tripolyphosphate	SEM, EIS, LEIS	[71]
Mesoporous silica core@layered double hydroxide	2-mercaptobenzothiazole	EIS, visual observation	[72]
Layered double hydroxide	N-alkyl-N, N-dimethyl-N-(3-thienylmethylene) ammonium bromides	PDP, DFT	[73]

Fig. 3. (a) Schematic representation of self-healing after scratch. (b) SEM image of scratched epoxy coating without microcapsules, (c) SEM image of scratched epoxy coating with microcapsules displaying self-healing effect [89].

Fig. 4. Infrared Rays (IR) intensity maps of 1690 cm-1 band of scratched film at specified locations for different healing time: (a) 0 h, (b) 1 h and (c) 2 h. Reprinted from [90], Copyright (2021), with permission from Elsevier.

Table 2. Summary of defect-filling materials and assessment methods in self-healing coatings.

Defect-filling Materials/Polymers	Assessment method(s)	Ref.
Nanofibers (polyacrylonitrile), TA and tung oil	SEM, XPS, Scanning Kelvin Probe (SKP), EIS	[91]
Polycaprolactone microspheres, cerium(III) nitrate	SEM, EIS	[92]
Urea-formaldehyde microcapsules, fluorosilane	SEM, accelerated weathering, EIS, SVET	[93]
Polydopamine, graphene oxide, Zn (II)	SEM, EIS, PDP	[94]
Poly(urea-urethane)-graphitic carbon nitride nanosheet	Transmission electron microscopy (TEM), XRD, AFM, EIS	[95]
Polyurea/polyaniline hybrid shell microcapsules, isophorone diisocyanate	SEM, EIS	[96]
Gelatin-gum Arabic/urea-formaldehyde microcapsules, vinyl ester resin and benzoyl peroxide	SEM, OM, EIS	[97]
Polyaspartamide	SEM, DSC, EIS	[98]
Furan-capped aniline trimer, maleimide compounds	SEM, PDP, EIS	[99]
Coumarin	Accelerated weathering, SEM, TEM	[100]
Polydimethylsiloxane, meldrum's acid	SEM, PDP, EIS	[101]
2,2-azobis(2-methylpropionamidine), dimethylaminoethyl methacrylate, methoxy polyethylene glycol acrylate, acrylic acid	SAXS, OM, load bearing, photoluminescence emission	[102]
Lignin nanoparticle, isophorone diisocyanate	OM, SEM, EIS	[103]
Polydopamine, 2-hydroxypropyltrimethyl ammonium chloride, chitosan, sodium alginate, Ca²⁺	FESEM, EIS	[104]
Polyurea/poly(urea-formaldehyde)/Al₂O₃ hybrid microcapsules, 4,4′-methylenebis cyclohexyl isocyanate	SEM, XPS	[105]
1h,1h,2h,2h-perfluorooctyl triethoxysilane	SEM, EIS	[106]
Sulfate-doped polyaniline	SEM, SVET, EIS, salt spray	[107]
Tolylene 2,4-diisocynate terminated polypropylene glycol, 1-(3-aminopropyl) imidazole, trimethylolpro-pane tris[poly(propylene glycol),	SEM, STEM, Raman, XPS, OM, SVET	[108]

Fig. 5. Schematic illustration of (a) inhibitor release from a pH responsive microcontainer with polyelectrolyte shell; (b) inhibitor release after mechanical rupture; (c) porous structure showing time-dependent release; and (d) inhibitor release by ion-exchange mechanism in the presence of aggressive ions.

Fig. 6. (a) Ratio between the maximum admittance values determined at the defect at certain time (A) and the initial maximum admittance values (A0) for each coated sample (Coat-I and Coat-II) during immersion in 0.005 mol L-1 NaCl. Inset: Coat-I (magnified scale). (b, c) SEM images and EDS analysis of Coat-I and Coat-II obtained after LEIS measurements performed in 0.005 mol L-1 NaCl for 24 h. Reprinted from [134], Copyright (2020), with permission from Elsevier.

Fig. 7. Illustration of self-healing process of Coat-I in NaCl solution. Reprinted from [134], Copyright (2020), with permission from Elsevier.

Fig. 8. (a) Scheme of multifunctional Pickering emulsions and their response to mechanical damage or pH change; Investigation of self-healing performance of the coatings (b) Optical images of the acrylate coating, acrylate coatings containing 45 wt.% soybean oil or linseed oil Pickering droplets before and after scratching the coating. Adapted with permission from [153] (https://pubs.acs.org/doi/10.1021/acsami.0c11866), Copyright (2020), American Chemical Society.

Fig. 9. Schematic representation of preparation of (A) FcCA-Cys and (B) TSR-SNs. (C) Construction route of TSR-SN-based SF-SHAC. Adapted with permission from [154], Copyright (2019), American Chemical Society.

Fig. 10. Optical micrograph (a) and SVET current density maps of (A) coating I, (B) coating II, and (C) coating III for immersion of 4 (b), 30 (c), 60 (d) h, and (e) maximum anodic and cathodic current densities over the defect area during monitoring time of 150 h in 0.05 M NaCl solution. Adapted with permission from [154], Copyright (2019), American Chemical Society.

Fig. 11. (a) Impedance values for specimens measured around the defect (Y = 2.5 mm) and (b) Raman spectrum of the scratched coatings after 20 h of immersion; (c) optical micrographs of steel electrodes beneath the coating after LEIS test: (c1) pure EP, (c2) rGO-CD/EP, and (c3) rGO-CD-BTA/EP coatings. Adapted with permission from [155], Copyright (2018), American Chemical Society.

Fig. 12. Schematic representation of self-healing mechanism for graphene-based containers composite coatings. Adapted with permission from [155], Copyright (2018), American Chemical Society.

Fig. 13. SEM image and EDS mapping image of CP-SFAC sample (A) before immersion, (B) after immersion in 0.05 M NaCl solution for 24 h; SEM image and EDS mapping image of the control coating sample (C) before immersion, (D) after immersion in 0.05 M NaCl solution for 24 h. Adapted with permission from [156], Copyright (2017), American Chemical Society.

Fig. 14. Schematic representation of corrosion protection mechanism of (A) CP-SFAC, and (B) CP-SFAC-RD(random distribution of CP-SNCs within CP-SFAC); (C) corrosion potential induced process of 8-HQ from CP-SNCs. CP-SNCs close to the surface of AZ31B can quickly accept the electrons generated from dissolution of magnesium, while CP-SNCs far from the surface of AZ31B cannot accept the electrons. Adapted with permission from [156], Copyright (2017), American Chemical Society.

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