Trigger and response mechanisms for controlled release of corrosion inhibitors from micro/nanocontainers interpreted using endogenous and exogenous stimuli: A review

doi:10.1016/j.jmst.2022.02.037

Abstract

Abstract:

Metallic corrosion can lead to both economic losses and environmental pollution due to undesired chemical and biochemical reactions. Furthermore, there are a number of drawbacks associated with different corrosion prevention and mitigation techniques. In view of these challenges, corrosion inhibitor-based smart micro/nanocontainers (CISCs) with stimuli-responsive functionality emerge as an important alternative technical approach in dealing with metallic corrosion. The development of CISCs involves controlled release corrosion inhibitors and self-healing coatings. This review focuses on the trigger and response mechanisms of controlling the discharge of corrosion inhibitors from micro/nanocontainers (a core-shell or layered structure) into aqueous solution under endogenous (pH, redox, and ion-exchange), exogenous (temperature, magnetic field, and light), and multiple stimuli. When these CISCs are embedded into coating materials, the self-healing effect of the coating can manifest to protect various types of metals. In this review effort, different types of CISCs are classified for the first time into the following three categories: inorganic, organic, and organic-inorganic hybrid. We also discuss application scope, future perspectives, and research strategies for CISCs in the hopes of increasing the life of corrosion protection and providing inspiration in related fields.

Key words: Smart micro/nanocontainers, Stimuli-responsive, Controlled release, Corrosion protection, Mechanism

Shan Chen, Zhongyu Huang, Mingzhe Yuan, Guang Huang, Honglei Guo, Guozhe Meng, Zhiyuan Feng, Ping Zhang. Trigger and response mechanisms for controlled release of corrosion inhibitors from micro/nanocontainers interpreted using endogenous and exogenous stimuli: A review[J]. J. Mater. Sci. Technol., 2022, 125: 67-80.

Figures/Tables 16

Table 1. Anodic and cathodic reactions of common metals.

Metal	Anodic reactions	Cathodic reactions
Zn	Zn → Zn²⁺ + 2e^-Zn²⁺ + mH₂O → [Zn(OH)_m]^(2-^m⁾⁺ + mH⁺ (m = 1-2)	Neutral or alkaline solution:2H₂O + 2e^- → 2OH^- +H₂↑O₂ + 2H₂O + 4e^- → 4OH^-Acidic solution:2H⁺ + 2e^- → H₂↑O₂ + 4H⁺ + 4e^- = 2H₂O
Al	Al → Al³⁺ + 3e^-Al³⁺ + nH₂O → [Al(OH)_n]^(3-ⁿ⁾⁺ + nH⁺ (n = 1-3)
Mg	Mg → Mg²⁺ + 2e^-Mg²⁺ + 2H₂O → Mg(OH)₂ + 2H⁺
Fe	Fe → Fe²⁺ + 2e^-Fe²⁺ → Fe³⁺ + e^-xFe²⁺ + yO₂ + H₂O → Fe₃O₄, Fe₂O₃, Fe(OH)₃, Fe(OH)₃·3H₂OFe³⁺ + nH₂O → [Fe(OH)_n]^(3-ⁿ⁾⁺ + nH⁺ (n = 1-3)

Table 2. List of micro/nanocontainers controlled release inhibitors with different stimuli-responsive types for corrosion protection of metals.

Stimuli	Micro/nanocontainer	Container type	Inhibitor	Coating	Substrate	Refs.
alkali	SiO₂/PEI/PSS/BTA/PSS/BTA	Hybrid	BTA	ZrO₂/SiO₂	Al alloy AA2024	[9]
alkali	SiO₂/PEI/PSS/PEI/PSS	Hybrid	2-(benzothiazol-2-ylsulfanyl)-succinic acid	SiO_x-ZrO_x	Al alloy AA2024	[103]
alkali	PSS-BTA/PEI	Organic	BTA	SiO_x/ZrO_y	carbon steel	[104]
alkali,or acid	HMSNs with CB[6]/bisammonium or α-CD/aniline supramolecular nanovalves	Hybrid	BTA	ZrO₂-SiO₂	Al alloy AA2024	[102]
acid	CaCO₃ microbeads	Inorganic	Ce³⁺, Sal, DMTD	epoxy	Al alloy AA2024-T3	[107]
acid	HAP microparticles	Inorganic	Ce³⁺, La³⁺, Sal, 8-HQ	SiO₂-ZrO₂	Al alloy AA2024-T3	[55]
alkali	MSNs	Inorganic	NaF	Ni	Mg alloy AZ31	[108]
redox	PANI,PPy	Organic	PDMS-DE, PDMS-DC	PVA, acrylate	/	[117]
redox	RTSNs 1	Organic	CA	Ce⁴⁺-doped and RTSNs 1 incorporated bi-layered ZrO₂-SiO₂ coating	Al alloy AA2024	[109]
redox	TESPT-based SiO₂ nanocapsules	Hybrid	MBT	/	/	[113]
redox	PANI shell with AuNPs	Hybrid	3-NisA	PVB	Zn plates	[11]
ion-exchange	Zn-Al LDHs	Inorganic	VO_x, H_xPO₄, MBT	epoxy	Al alloy AA2024	[127]
ion-exchange	Na⁺-MMT	Inorganic	BIA⁺, Zn²⁺	epoxy ester	mild steel panels	[52]
ion-exchange	Mg₂Al₆ LDH,CeMo	Inorganic	MBT	epoxy	galvanized steel	[12]
ion-exchange	Zn₂Al LDH	Inorganic	MoO₄^2-	epoxy	galvanized steel	[128]
ion-exchange	MgAl LDH	Inorganic	MBT	/	Mg alloy AZ31	[132]
temperature,alkali,or redox	SiO₂/polymer double-walled hybrid nanotubes	Hybrid	BTA	SiO_x/ZrO_y	carbon steel	[95]
magnetic field	MWCNTs/BTA-poly(urea-formaldehyde)	Hybrid	BTA	epoxy resin	Cu	[28]
light	TiO₂/PEI/PSS/8-HQ/PSS/PEI	Hybrid	8-HQ	/	Al alloy AA6061-T6	[143]
light	TiO₂/PEI/PSS/PEI/PSS	Hybrid	BTA	SiO_x-ZrO_x	Al alloy AA2024	[46]
light	TiO₂ core with AgNPs/PEI/PSS/PEI/PSS	Hybrid	BTA	SiO_x-ZrO_x	Al alloy AA2024	[45]
light	TiN NPs/mesoporous SiO₂	Inorganic	BTA	epoxy	Al alloy AA2024-T3	[135]
light	HMSNs with Azo	Hybrid	BTA	alkyd	Al alloy AA2024	[146]
alkali,Mg²⁺	MSNPs	Hybrid	HMAP	SNAP	Mg alloy AZ31B	[30]
acid,alkali,reduction potential	TSR-SNs	Hybrid	BTA	SiO₂-ZrO₂	Al alloy AA2024	[150]
acid,alkali,reduction potential	QSR-MSNPs	Hybrid	BTA	sol-gel	Al alloy AA2024	[151]
alkali,reduction potential	PANI shell with AuNPs	Hybrid	3-NisA, MBT	/	/	[152]

Table 2. List of micro/nanocontainers controlled release inhibitors with different stimuli-responsive types for corrosion protection of metals.

Stimuli	Micro/nanocontainer	Container type	Inhibitor	Coating	Substrate	Refs.
alkali	SiO₂/PEI/PSS/BTA/PSS/BTA	Hybrid	BTA	ZrO₂/SiO₂	Al alloy AA2024	[9]
alkali	SiO₂/PEI/PSS/PEI/PSS	Hybrid	2-(benzothiazol-2-ylsulfanyl)-succinic acid	SiO_x-ZrO_x	Al alloy AA2024	[103]
alkali	PSS-BTA/PEI	Organic	BTA	SiO_x/ZrO_y	carbon steel	[104]
alkali,or acid	HMSNs with CB[6]/bisammonium or α-CD/aniline supramolecular nanovalves	Hybrid	BTA	ZrO₂-SiO₂	Al alloy AA2024	[102]
acid	CaCO₃ microbeads	Inorganic	Ce³⁺, Sal, DMTD	epoxy	Al alloy AA2024-T3	[107]
acid	HAP microparticles	Inorganic	Ce³⁺, La³⁺, Sal, 8-HQ	SiO₂-ZrO₂	Al alloy AA2024-T3	[55]
alkali	MSNs	Inorganic	NaF	Ni	Mg alloy AZ31	[108]
redox	PANI,PPy	Organic	PDMS-DE, PDMS-DC	PVA, acrylate	/	[117]
redox	RTSNs 1	Organic	CA	Ce⁴⁺-doped and RTSNs 1 incorporated bi-layered ZrO₂-SiO₂ coating	Al alloy AA2024	[109]
redox	TESPT-based SiO₂ nanocapsules	Hybrid	MBT	/	/	[113]
redox	PANI shell with AuNPs	Hybrid	3-NisA	PVB	Zn plates	[11]
ion-exchange	Zn-Al LDHs	Inorganic	VO_x, H_xPO₄, MBT	epoxy	Al alloy AA2024	[127]
ion-exchange	Na⁺-MMT	Inorganic	BIA⁺, Zn²⁺	epoxy ester	mild steel panels	[52]
ion-exchange	Mg₂Al₆ LDH,CeMo	Inorganic	MBT	epoxy	galvanized steel	[12]
ion-exchange	Zn₂Al LDH	Inorganic	MoO₄^2-	epoxy	galvanized steel	[128]
ion-exchange	MgAl LDH	Inorganic	MBT	/	Mg alloy AZ31	[132]
temperature,alkali,or redox	SiO₂/polymer double-walled hybrid nanotubes	Hybrid	BTA	SiO_x/ZrO_y	carbon steel	[95]
magnetic field	MWCNTs/BTA-poly(urea-formaldehyde)	Hybrid	BTA	epoxy resin	Cu	[28]
light	TiO₂/PEI/PSS/8-HQ/PSS/PEI	Hybrid	8-HQ	/	Al alloy AA6061-T6	[143]
light	TiO₂/PEI/PSS/PEI/PSS	Hybrid	BTA	SiO_x-ZrO_x	Al alloy AA2024	[46]
light	TiO₂ core with AgNPs/PEI/PSS/PEI/PSS	Hybrid	BTA	SiO_x-ZrO_x	Al alloy AA2024	[45]
light	TiN NPs/mesoporous SiO₂	Inorganic	BTA	epoxy	Al alloy AA2024-T3	[135]
light	HMSNs with Azo	Hybrid	BTA	alkyd	Al alloy AA2024	[146]
alkali,Mg²⁺	MSNPs	Hybrid	HMAP	SNAP	Mg alloy AZ31B	[30]
acid,alkali,reduction potential	TSR-SNs	Hybrid	BTA	SiO₂-ZrO₂	Al alloy AA2024	[150]
acid,alkali,reduction potential	QSR-MSNPs	Hybrid	BTA	sol-gel	Al alloy AA2024	[151]
alkali,reduction potential	PANI shell with AuNPs	Hybrid	3-NisA, MBT	/	/	[152]

Fig. 2. (A) Schematic representations of CISC synthesis and alkali-responsive CISCs releasing BTA. (B) Schematic representations of CISC synthesis and acid-responsive CISCs releasing BTA. Reprinted with permission from Ref. [102]. Copyright 2012 IOP Publishing Ltd.

Fig. 3. Schematic mechanism of CaCO3 microbeads releasing corrosion inhibitors at different fractions of Ca2+ containing ions and pH value in solution. Reprinted with permission from Ref. [107]. Copyright 2012 Elsevier.

Fig. 5. (A) Schematic preparation of RTSNs 1. (B) Schematic depicting of the release mechanism of redox-responsive CISCs. Reprinted with permission from Ref. [109]. Copyright 2017 Royal Society of Chemistry.

Fig. 6. (A) Cumulative release of PDMS-DE from PANI capsules under different oxidized and/or reduced conditions and schematic representation of the release mechanism. (B) Cumulative release of 3-NisA from PANI capsules under reduced (gray-shaded area, b and d) and oxidized conditions (white background, a and c) and schematic representation of the release mechanism. Reprinted with permission from Refs. [117] and [11], respectively. Copyright 2013 American Chemical Society and Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim, respectively.

Fig. 7. Schematic release mechanism of LDHs for entrapping aggressive species (Cl-) from the environment and releasing anionic inhibitors (Inh-) onto metallic substrate surfaces to achieve self-healing. Reprinted with permission from Ref. [127]. Copyright 2010 American Chemical Society.

Fig. 12. Schematic self-healing mechanism of the smart coating immobilized with alkali/Mg2+ dual stimuli-responsive CISCs. Reprinted with permission from Ref. [30]. Copyright 2016 Royal Society of Chemistry.

Fig. 13. (A) Reduction potential-triggered release profiles of BTA from CISCs. (B) Alkali-triggered release profiles of BTA from CISCs under different alkalinity values. (C) Acid-triggered release profiles of BTA from CISCs under different acidity values. Reprinted with permission from Ref. [150]. Copyright 2019 American Chemical Society.

Fig. 14. Schematic illustration of the selective release mechanism of 3-NisA or MBT in the dual-responsive CISCs upon pH change or reduction. Reprinted with permission from Ref. [152]. Copyright 2014 American Chemical Society.

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