Research progress of metal organic framework materials in anti-corrosion coating

Chengwei Yang; Yin Zhu; Tao Wang; Xu Wang; Yubin Wang

doi:10.1515/polyeng-2023-0144

Article Publicly Available

Research progress of metal organic framework materials in anti-corrosion coating

Chengwei Yang , Yin Zhu , Tao Wang , Xu Wang and Yubin Wang

Published/Copyright: November 24, 2023

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From the journal Journal of Polymer Engineering Volume 44 Issue 1

Abstract

In recent decades of research, organic coatings have been considered the most effective and economical measure for corrosion protection of metals. However, defects in organic coatings created during the curing reaction provide corrosion channels for corrosive media, which in turn accelerate the failure of metallic materials. Functional nanomaterials are considered to be the key to solving this challenge. Metal organic frameworks (MOFs) materials, as an emerging nanomaterial, show great potential as a durable and efficient nano-corrosion filler in organic anti-corrosion coatings. Therefore, this paper reviews the application of MOFs materials as solid corrosion inhibitors, small molecule corrosion inhibitor vehicles and modified graphene oxide in anti-corrosion coatings and looks forward to the prospect of research on their application in engineering practice.

Keywords: organic coating; corrosion; metal-organic frame materials; nano-corrosion filler

1 Introduction

Metal corrosion occurs earliest on the surface of the material, so the treatment of metal material surface is the key measure to prevent metal corrosion, such as corrosion inhibitor protection [1], [2], [3], [4], metal plating protection [5, 6], and organic coating protection [7], [8], [9], [10]. Organic coating protection method is considered to be efficient, economical and green protection measure. However, organic coatings produce defects inside the coating during the curing process, and corrosive media will penetrate through these defects to the metal surface after a long period of use, which makes the protective performance significantly reduced [11]. In order to solve the defects arising from the curing of organic coatings and to enhance the protective properties of the coatings. Functional nano fillers such as graphene and its derivatives [12], [13], [14], [15], MXene [16, 17], cerium dioxide [18, 19], and mesoporous silica [20], have been extensively studied in the field of anti-corrosion coatings. Metal-organic frameworks (MOFs) materials are an important novel class of porous materials with a “microcapsule” like structure of cavities [21, 22]. It has been widely used in drug release retardation [23], catalytic oxidation [24, 25], battery energy storage [26], and adsorption separation [27]. In the field of organic anti-corrosion coatings, MOFs materials contain heteroatoms such as nitrogen, sulfur, and oxygen that can participate in adsorption reactions as well as unsaturated metal sites, which can adsorb with metal ions on metal surfaces to form protective films, thus improving the corrosion resistance of coatings [28]. It can be seen that MOFs materials in organic anti-corrosion coatings have been a hot research topic in recent years.

This paper reviews the application of common types of MOFs materials as functional fillers in organic anti-corrosion coatings with coordination ions and organic ligands as shown in Table 1. Finally, the application and development of MOFs materials in the field of anticorrosive coatings are prospected.

Table 1:

Coordination ions and organic ligands corresponding to different MOFs materials in this paper.

MOF	Coordination ions	Organic ligands
ZIF-7	Zn²⁺	Benzimidazole
ZIF-8	Zn²⁺	2-Methylimidazole
ZIF-67	Co³⁺	2-Methylimidazole
La-MOF	La³⁺	1,4-Dicarboxybenzene
MOF-5	Zn²⁺	1,4-Dicarboxybenzene
Cu-TCPP	Cu²⁺	Tetra(4-carboxyphenyl)porphine
UIO-66	Zr⁴⁺	1,4-Dicarboxybenzene

2 Zeolite-imidazolate framework MOFs materials in organic coating applications

Zeolite imidazole frameworks (ZIFs) are self-assembled by transition metal ions with organic imidazole ligands through complexation [29, 30]. It has stable thermodynamic properties, pH responsiveness, porous structure and “microcapsule” cavities, and synthesis ease, it is a molecularly delivered and stimulus-responsive nanomaterial [31, 32]. The researches shows that ZIFs were considered as a polymer multifunctional cross-linker with polymer matrix with reversible ligand cross-linking, and the introduction of MOFs material into polymer matrix could enhance the mechanical properties of the material [33]. Moreover, the high specific surface area confers excellent adsorption capacity to ZIFs, which are expected to trap corrosive ions during their erosion phase as functional fillers for anticorrosive coatings to achieve corrosion inhibition [34].

2.1 Applications as solid corrosion inhibitors

Liquid corrosion inhibitors have a short maintenance time of effective content and significant application defects in special cases, which limit their application. While the solid corrosion inhibitor maintenance time is long, and can improve the coating microporous and cracking, which has important significance for corrosion-resistant coatings. Xu et al. [35], in their study of polyetheretherketone composite membranes, found that. Water uptake and swelling rate of membranes doped with ZIF-8 was lower than pure membrane. This was mainly because ZIF-8 was hydrophobic and had a rigid skeleton. These could inhibit membranes from absorbing water. Besides, membranes doped with ZIF-8 showed better mechanical properties. The main reason might be that ZIF-8 had a good rigid structure. Thus, it can be seen that ZIF-8 with hydrophobicity has great potential in the field of organic metal anti-corrosion coatings.

Ramezanzadeh et al. [36], studied the release characteristics of ZIF-8 in 3.5 wt% NaCl solution and found that ZIF-8 can partially dissolve in NaCl solution and dissociate Zn²⁺ and 2-methylimidazole ligands, which would facilitate the active corrosion inhibition of metals. The solution phase corrosion study of bare steel sheets immersed in NaCl solution and NaCl solution containing ZIF-8 dissociated extract found that: the steel sheets immersed in NaCl solution containing ZIF-8 dissociated extract showed excellent corrosion resistance, which can be attributed to the recombination of ZIF-8 dissociated substances with corrosion products to form a dense protective film extending the erosion path of the corrosive medium. Lashgari et al. [37], prepared ZIF-67 nanoparticles by co-precipitation of Co (NO₃)₂.6H₂O with 2-methylimidazole in methanol solution, and surface modification with 3-aminopropyltriethoxysilane (APTES) denoted as (ZIF-67@APTES). As shown in Figure 1. Then, ZIF-67@APTES was ultrasonically dispersed in epoxy resin and physically blended with a curing agent to obtain ZIF-67@APTES/epoxy resin coating. The results indicate that Co²⁺ acts as a cathodic inhibitor with the OH⁻ that can be generated on the cathode to form a complex film on the metal surface. The 2-methylimidazole can be adsorbed in the anodic region, providing a superior barrier/active inhibition for the substrate. Meanwhile, ZIF-67@APTES improved the dense density of the epoxy resin and decreased its water absorption, further enhancing the abrasion and corrosion resistance of the coating. After up to 50 days of immersion, the electrochemical impedance spectroscopy(EIS) impedance of the composite coating was |Z|_0.01 Hz = 5.78 × 10⁹ Ω cm⁻², which was nearly three orders of magnitude higher than that of the epoxy coating.

Figure 1:

Modification of ZIF-67 and anticorrosion mechanism of composite coatings. (a) APTES modified ZIF-67 preparation procedure; (b) mechanism of corrosion protection of ZIF-67@APTES/epoxy resin coating [37] (Lashgari et al. 2021; reprinted with permission, copyright 2021 Elsevier).

Lei et al. [38], modified ZIF-67 with dodecyltrimethoxysilane (DTMS) and used epoxy resin as the coating matrix. Found that the long hydrophobic carbon-chains in the DTMS structure could improve the interfacial compatibilities of the nanoparticles in the epoxy matrix and prevent the aggregation between the particles, and the modified ZIF-67 was still stably dispersed in the epoxy resin even after 24 h. The stability in epoxy resin for 24 h before and after modification is shown in Figure 2a. In the EIS impedance test it was found that the resistance of ZIF-67/epoxy and ZIF-67@DTMS/epoxy coatings at |Z|_0.01 Hz were 7.45 × 10⁸ Ω cm⁻² and 2.46 × 10⁹ Ω cm⁻² after 25 days of immersion were always greater than that of pure epoxy at |Z|_0.01 Hz of 3.99 × 10⁸ Ω cm⁻², as shown in Figure 2b. Duan et al. [39], prepared a series of ZIF-8/epoxy composite coatings with different ZIF-8 mass fractions to study the effect of ZIF-8 content on the corrosion resistance of the coatings. It was shown that the amine group in ZIF-8 could react with the epoxy group in the epoxy resin by ring opening. With the increase of ZIF-8 content and epoxy resin cross-link density, the cured ZIF-8/epoxy resin has higher densities. After 54 days of immersion, the composite coating (ZIF-8 0.5 wt%) exhibited an optimal corrosion resistance of EIS impedance |Z|_0.01 Hz = 9.86 × 10¹⁰ Ω cm⁻², which was nearly three orders of magnitude higher than that of the pure epoxy resin |Z|_0.01 Hz = 1.01 × 10⁸ Ω cm⁻², greatly improving the corrosion resistance of the composite coating.

Figure 2:

Stability of ZIF-67 in epoxy resin and impedance of composite coatings. (a) ZIF-67 stability in epoxy resin for 24 h before and after modification; (b) EIS impedance of the coating after 25 days of immersion in 3.5 wt% NaCl solution [38] (Lei et al. 2023; reprinted with permission, copyright 2023 Elsevier).

Yang et al. [40], synthesized a series of ZIF-8 nanoparticles of different sizes (50 nm, 100 nm, 500 nm) and compounded them with a polyurethane matrix to investigate the resistance of the composite coatings to biofouling and cavitation erosion in a simulated marine environment. It was found that the anti-biofouling and anti-cavitation erosion of the composite coating were enhanced when small size of ZIF-8 made the coating resistant to biofouling and cavitation erosion, but the hydrophobicity of the coating was almost unaffected; in further studies, it was found that small size of ZIF-8 could dissociate more Zn²⁺ and 2-methylimidazole ligands, so the anti-biofouling and anti-cavitation erosion of the coating were also improved. In addition, the mechanical properties of the composite coatings, tended to decrease with the increase of ZIF-8 size, indicating that the small size of ZIF-8 nanoparticles could combine with more molecular chains in the polymer matrix, thus enhancing the crosslink density of the composite coatings, which also contributed to the cavitation erosion resistance of the coatings. In conclusion, it can be seen that ZIFs is a solid corrosion inhibitor with high performance, and its anti-corrosion application is shown in Table 2. The anti-corrosion mechanism mainly utilizes hydrophobic MOFs fillers to enhance the hydrophobicity of the composite coating, which can effectively block the corrosive medium from entering the coating. Besides, due to the dissociation of MOFs, the dissociated material can react with cathode and anode ions to generate a passivation film, which can effectively improve the corrosion resistance of composite coatings.

Table 2:

Applications of MOFs materials as solid corrosion inhibitors.

Fillers	Modified materials	Polymer matrix	Metals	Corrosion conditions	References
ZIF-8	/	/	Q235	3.5 wt% NaCl 6 h	[36]
ZIF-67	APTES	Epoxy resin	Q235	3.5 wt% NaCl 50 d	[37]
ZIF-67	DTMS	Epoxy resin	Q235	3.5 wt% NaCl 25 d	[38]
ZIF-8	/	Epoxy resin	Q235	3.5 wt% NaCl 54 d	[39]

ZIFs as solid corrosion inhibitors have been widely studied and applied to anticorrosive coatings, and its problems are focused on dispersion in the coating matrix and long-term preservation of composite coatings. Therefore, researchers should proceed to solve the above problems to bring a better development prospect for ZIFs composite coatings.

2.2 Corrosion inhibitor vehicle

Numerous studies in drug delivery retardation have demonstrated that ZIFs are ideal drug encapsulation containers [41]. Therefore, it is reasonable to use them as vehicles for corrosion inhibitors. According to the report dissolving zinc gluconate (ZnG) in 3.5 wt% NaCl solution provided corrosion inhibition in mild steel [42]. Therefore, Ren et al. [43], prepared a ZnG@ZIF-8/epoxy composite coating. By using ZnG as a single source of zinc for the preparation of ZnG@ZIF-8, and cleverly encapsulating the corrosion inhibitor ZnG in the internal cavity of ZIF-8 by a one-pot method. Then, ZnG@ZIF-8 was dispersed in a methanol solution, and the epoxy resin and curing agent were mixed into xylene and n-butanol solvents. The above mixture was ultrasonically dispersed for 2 h until it was dispersed well. The design strategy is shown in Figure 3a. It was shown that ZIF-8 is compatible with epoxy resin, and ZnG@ZIF-8 could be well dispersed in the epoxy resin matrix. In a 3.5 wt% NaCl solution, the ZnG@ZIF-8/epoxy composite coating exhibited excellent corrosion resistance compared to the control, even after 30 days of immersion the EIS impedance of the composite coating|Z|_0.01 Hz = 1 × 10⁷ Ω cm⁻² was 3 orders of magnitude higher than that of the pure epoxy|Z|_0.01 Hz = 1.0 × 10⁴ Ω cm⁻² and about 2 orders of magnitude higher than that of the ZIF-8/epoxy resin|Z|_0.01 Hz = 1.4 × 10⁶ Ω cm⁻² by about 2 orders of magnitude. The mechanism of corrosion inhibition is that: firstly, the hydrophobicity of ZIF-8 enhances the hydrophobicity of the composite coating; secondly, ZnG@ZIF-8 reduces the defects generated by the curing of the coating; finally, ZIF-8 releases ZnG adsorbed on the substrate surface to form a dense protective film, which resists the erosion of corrosive substances. In addition, Guo et al. [44], used a ligand exchange method to incorporate the organic corrosion inhibitor benzotriazole (BTA) into ZIF-7 and prepared a pH-responsive composite coating to improve the corrosion resistance, and it was found that the nanocomposite particles could rapidly dissociate and release BTA within 10 min under acidic conditions BTA adsorbs to the metal substrate to form a protective film, enabling the composite coating to provide 99.4 % inhibition efficiency under acidic conditions, as shown in Figure 3b.

Figure 3:

ZnG@ZIF-8/epoxy preparation and pH response. (a) Design strategy of ZnG@ZIF-8/epoxy composite coating [43] (Ren et al. 2020; reprinted with permission, copyright 2020 Elsevier); (b) release rates of BTA under acidic conditions [44] (Guo et al. 2019; reprinted with permission, copyright 2019 Elsevier).

Yang et al. [45], using the pH responsiveness of ZIF-8, combined with the hollow “microcapsule” structure, encapsulated BTA in the ZIF-8 cavities and hydrophilically modified the surface of ZIF-8 using tannic acid (TA), obtained BTA@ZIF-8@TA, the preparation process is shown in Figure 4a. The BTA@ZIF-8@TA/epoxy composite coatings were prepared procedures is firstly, a certain percentage of BTA@ZIF-8@TA was added into waterborne hardener, and the mixture was treated with mechanical stirring for 30 min and sonicated for another half an hour; then waterborne epoxy resin was added and stirred for 10 min. It was found that BTA@ZIF-8@TA has acid and base dual responsiveness, and the release rate of BTA at pH = 5 and pH = 7 was 90 % and 85 %, as shown in Figure 4b, respectively. BTA@ZIF-8@TA/epoxy composite coating is showing excellent corrosion resistance in the early stages of immersion. The EIS impedance of the composite coating at |Z|_0.01 Hz decreases and then increases with the extension of the immersion time, indicating that with the erosion of the corrosive medium the collapse of the ZIF-8 structure releases the BTA adsorbed on the surface of the mild steel sheet to form a film, resulting in the enhancement of the corrosion resistance of the coating. In addition, the hydrophilic modifier TA can react with corrosion products to produce iron tannate, which can further inhibit corrosion; even after up to 20 days of immersion BTA@ZIF-8@TA/epoxy composite coating EIS impedance|Z|_0.01 Hz = 1.45 × 10⁸ Ω cm⁻², which is nearly two orders of magnitude higher than the pure epoxy coating.

Figure 4:

Synthesis and pH-response of BTA@ZIF-8@TA. (a) Synthesis procedure of BTA@ZIF-8@TA nanomaterials; (b) release rate of BTA at different pH conditions [45] (Yang et al. 2021; reprinted with permission, copyright 2021 Elsevier).

Zhou et al. [46], report on a new corrosion inhibitor-encapsulated nanocontainer, Firstly, the hollow mesoporous silica nanoparticles (HMSN) were constructed by using ZIF-8 as a sacrificial template, and then coated with corrosion inhibitor BTA, finally the surface of HMSN was modified with ZIF-8 (denoted as HMSN@BTA@ZIF-8). Then they prepared an HMSN@BTA@ZIF-8/epoxy composite coating. It was shown that HMSN@BTA@ZIF-8 also has dual responsiveness to acids and bases, and its release curves at different pH conditions are shown in Figure 5a. HMSN@BTA@ZIF-8 could be distributed well in the epoxy resin matrix and improve the crosslink density of the composite coating. The corrosion potential of the HMSN@BTA@ZIF-8/epoxy composite coating was significantly higher than that of the pure epoxy resin coating after 30 days of immersion as shown in Figure 5b from the polarization curve. Therefore, the composite coating exhibited stronger corrosion resistance.

Figure 5:

HMSN@BTA@ZIF-8 pH response and polarization curves of composite coatings. (a) HMSN@BTA@ZIF-8 release BTA curves at different pH conditions; (b) epoxy and HMSN@BTA@ZIF-8/epoxy polarization curve plot for 30 days of immersion in 3.5 wt% NaCl solution [46] (Zhou et al. 2020; reprinted with permission, copyright 2020 Elsevier).

Yan et al. [47] used the green corrosion inhibitor zinc phytate (ZnPA) to provide in-situ synthesis of Zn²⁺and dimethylimidazole ZnPA@ZIF-8 and water-based polyacrylate was used as the coating substrate to prepare ZnPA@ZIF-8/Waterborne polyacrylate composite coating. The results indicate that ZnPA@ZIF-8 particles dissociate under the stimulation of salt solution and can release ZnPA rapidly within 8 h. After immersion in the salt solution for 3 days, the EIS impedance of the composite coating at |Z|_0.01 Hz was about 3 orders of magnitude higher than that of the pure aqueous polyacrylate, with a corrosion inhibition rate of 99.9 %, and the corrosion voltage of the composite coating increased by about 0.341 V, as can be obtained from the polarization curve plots.

In summary, pH-responsive anti-corrosion coating has the following anti-corrosion characteristics: when the coating is damaged by external factors, the corrosion inhibitor vehicle actively releases the corrosion inhibitor to form a passivated protective film in the damaged area to prevent further corrosion from occurring, so that the coating defects can be repaired and in the case of corrosive media erosion to form a passive barrier; their applications are shown in Table 3. This provides a certain basis for smart nanocontainers to be applied in anticorrosive coatings and for the preparation of self-healing, smart anticorrosive coatings.

Table 3:

Applications of MOFs materials as corrosion inhibitor supports in coatings.

Vehicle	Corrosion inhibitors	Modified materials	Polymer matrix	Metals	Corrosion conditions	References
ZIF-8	ZnG	/	Epoxy resin	AZ31B	3.5 wt% NaCl 30 d	[43]
ZIF-7	BTA	/	Epoxy resin	Q235	0.1 M HCl 120 h	[44]
ZIF-8	BTA	TA	Waterborne epoxy resin	Q235	3.5 wt% NaCl 20 d	[45]
ZIF-8	BTA	HMSN	Epoxy resin	Q235	3.5 wt% NaCl 30 d	[46]
ZIF-8	ZnPA	/	Waterborne polyacrylate	Q235	3.5 wt% NaCl 3 d	[47]

2.3 Graphene oxide modification

ZIFs could be used to modify graphene oxide (GO) for synergistic corrosion protection, in addition to acting as a carrier for solid corrosion inhibitors and organic corrosion inhibitors. GO has the property of preventing the diffusion of water, oxygen, and ions and is an excellent filler in organic coatings [48]. As the surface of GO contains abundant oxygen groups, there is a large polarity its dispersion state in organic coatings is poor and the compatibility with the polymer matrix is poor [49, 50]. Secondly, the electrical conductivity that GO has, uneven dispersion is very easy to pit on the steel surface, which seriously affects the service life of the coating. It was found that GO was modified by zeolite-imidazolate framework MOFs material and its conductivity was reduced, and it could exist stably in the organic matrix, which could achieve a good anti-corrosion effect with the nature of the modifier. Ramezanzadeh et al. [36], successfully anchored ZIF-8 on GO using a one-pot method. GO@ZIF-8/epoxy composite coatings were prepared. It was found that the addition of GO@ZIF-8 enhanced the adhesion and corrosion resistance of the composite coating, and the corrosion resistance was substantially improved compared to the pure epoxy resin after 70 days of immersion, as shown in Figure 6.

Figure 6:

Pure epoxy resin and GO@ZIF-8/ epoxy resin EIS impedance. (a) Epoxy EIS impedance plot for 70 days of immersion in 3.5 wt% NaCl solution; (b) GO@ZIF-8/epoxy EIS impedance plot for 70 days of immersion in 3.5 wt% NaCl solution [36] (Ramezanzadeh et al. 2020; reprinted with permission, copyright 2020 Elsevier).

In addition, encapsulating the corrosion inhibitor in ZIF-8 and then anchoring it on the GO surface is also an important measure to enhance the corrosion resistance of the composite coating, Xiong et al. [51], anchored ZIF-8 containing the corrosion inhibitor salicylaldehyde (SA) on GO by a one-pot method, and then, dispersed it in ethanol solution, added polyvinyl butyral ester powder to the solution, and stirred for 1 h to obtain SA@ZIF-8@GO/polyvinyl butyral ester composite coating, and the preparation process is shown in Figure 7. SA@ZIF-8@GO is distributed uniformly in the polyvinyl butyral ester matrix and adsorbs on the substrate surface by releasing corrosion inhibitor through pH response, which, together with the anti-permeability of GO, simultaneously makes the composite coating with passive barrier and active protection properties, significantly improving the corrosion resistance of the composite coating, and after 6 days of immersion, the EIS impedance of SA@ZIF-8@GO/polyvinyl butyral ester coating is about |Z|_0.01Hz = 4.90 × 10⁶ Ω cm⁻², which is much larger than the pure polyvinyl butyral ester coating |Z|_0.01Hz = 7.94 × 10⁴ Ω cm⁻². Subsequently, Xiong et al. [52], modified SA@ZIF-8@GO with 3-aminopropyltriethoxysilane (APTES). Comparison with the filler without APTES modification revealed that the modified SA@ZIF-8@GO could maintain stable dispersion in the epoxy resin after up to 480 h. This would be beneficial to improve its compatibility and interfacial bonding in the epoxy coating, and the excellent corrosion resistance of the composite coating was further improved, with an impedance two orders of magnitude higher than that of the pure epoxy coating after 20 days of immersion.

Figure 7:

Li et al. [53], modified ZIF-8 containing 2-mercaptobenzimidazole (2-M) on GO and compounded it with epoxy resin and investigated the corrosion resistance of the coating on mild steel surface, and found that after the filler was added to the epoxy resin and immersed in the salt solution for 60 days, the impedance of 2-M@ZIF-8@GO/epoxy resin coating|Z|_0.01 Hz = 3.30 × 10⁹ Ω cm⁻² was four orders of magnitude higher than that of the epoxy resin coating|Z|_0.01 Hz = 2.00 × 10⁵ Ω cm⁻².

It can be seen that ZIFs can enhance the corrosion resistance of anticorrosion coatings after modifying GO, and its anti-corrosion mechanism is that: ZIFs can be either solid corrosion inhibitors or vehicles of small molecule corrosion inhibitors, which can react quickly at the early stage of corrosion occurrence, and then GO have attracted extensive attention and show the superior barrier effect because of large specific area and excellent impermeability to oxygen and water; and its application is shown in Table 4.

Table 4:

Applications of graphene oxide modified by MOFs materials.

Fillers	Corrosion inhibitors	Modified materials	Polymer matrix	Metals	Corrosion conditions	References
ZIF-8@GO	/	/	/	Q23Z	3.5 wt% NaCl 6 h	[36]
ZIF-8@GO	SA	/	Polyvinylbutyral ester	2024-T3	3.5 wt% NaCl 6d	[51]
ZIF-8@GO	SA	APTES	Epoxy resin	2024-T3	3.5 wt% NaCl 25d	[52]
ZIF-8	2-M	/	Epoxy resin	Q235	3.5 wt% NaCl 60d	[53]

Noticeably, when ZIFs anchor GO, their interfacial compatibility with the coating substrate remains a critical factor restricting the long-term protective performance of the coating. T Therefore, modified interfacial compatibility is the direction of future research.

3 Application of other MOFs materials in anti-corrosion coatings

As mentioned above, ZIFs have been extensively studied in anticorrosive coatings, which have greatly improved the corrosion resistance of organic coatings. In addition to zeolite imidazole framework MOFs materials, other MOFs materials are also widely used in the field of corrosion protection, and the current status of research on other types of MOFs materials in corrosion resistant coatings is reviewed below.

Keramatinia et al. [54], first reported La-MOF synthesized with La³⁺ as a metal source and 1,4-dicarboxybenzene as a ligand. It was found that La-MOF was compatible with epoxy polyamide coatings and could fill the defects generated by curing. The corrosion results showed that La³⁺ released from La-MOF could bind to OH⁻ in the cathode region to form a film, and the bonding of oxygen heteroatoms in the ligand to the anode region could effectively inhibit the corrosion reaction at the anode, which could be observed under SEM test and EDS test as shown in Figure 8a. The composite coating has excellent corrosion protection even after 12 weeks of immersion, the EIS impedance at |Z|_0.01 Hz still exceeds 10¹⁰ Ω cm⁻² by two orders of magnitude higher than that of the pure epoxy polyamide coating. Wang et al. [55], reported the application of dopamine-modified MOF-5 (DA-MOF-5) in aqueous epoxy resin coatings. The results showed that dopamine could produce strong cross-linking with the aqueous epoxy resin, as shown in Figure 8b. DA-MOF-5 with a mass fraction of only 0.5 % effectively enhanced the adhesion of the coating to the substrate and gave the coating the best anti-corrosion performance. Qiu et al. [56], reported the synthesis of ultrathin MOF Nano sheets Cu-TCPP using surfactant-assisted synthesis and filled with epoxy resin coatings. The results showed that Cu-TCPP is a two-dimensional nanomaterial with good water stability and permeation resistance, and it is well dispersed in epoxy resin at 0.5 % mass fraction, and its flake structure enhances the “labyrinth effect” of the composite coating, resulting in stable barrier properties and ion resistance, which enhances the corrosion resistance of the coating. The lamellar structure enhances the “labyrinth effect” of the composite coating, resulting in stable barrier properties and ion resistance, and enhancing the corrosion resistance of the coating. Chen et al. [57], used UIO-66 as a nano-vessel loaded with corrosion inhibitor and anchored on graphene oxide nano sheets to enable the composite coating to achieve dual active and passive protection functions. This is mainly due to the dual active protection by the release of corrosion inhibitor from UIO-66 under alkaline conditions to form a protective film and dissociation of Zr⁴⁺ to generate a metal passivation film, and the passive protection by the excellent barrier function of graphene oxide. Sun et al. [58], reported the modification of 2D Co-MOF by polydopamine as a measure to enhance the corrosion resistance of epoxy composite coatings and showed that only 0.5 wt% Co-MOF-PDA was required to make the composite coating three orders of magnitude higher than the pure epoxy coating even after 60 d of immersion in 3.5 wt% NaCl solution.

Figure 8:

SEM and EDS of scratched area and reaction of DA-MOFs-5 with waterborne epoxy resin. (a) SEM and EDS of La-MOF/epoxy scratch area after corrosion [43] (Keramatinia et al. 2022; reprinted with permission, copyright 2022 Elsevier); (b) DA-MOFs-5 reaction with waterborne epoxy [44] (Wang et al. 2017; reprinted with permission, copyright 2017 Elsevier).

In conjunction with the current research, there are four main mechanisms for MOFs materials to enhance the corrosion resistance in organic coatings: 1. Using the dissociable character of MOFs materials, ions and organic complexes with corrosion inhibition are dissociated and combined with cathodic and anodic corrosion products to form passivation films, respectively. 2. Using its pH responsiveness and cavity structure, the corrosion inhibitor is introduced into the structural cavity, and when the coating is eroded, the corrosion inhibitor is then released, forming a protective film on the substrate surface to resist the erosion of corrosive media. 3. Using the anti-permeability of two-dimensional MOFs material, it can effectively block the erosion of corrosive media, such as Cl⁻, to extend the erosion path of corrosive media and effectively improve the “labyrinth effect” of the composite coating. 4. The passive and active anti-corrosion functions of the composite coatings were achieved by modifying graphene oxide. In order to better exploit the anti-corrosion function of the above nano-functional fillers, enhancing their dispersion in organic coatings and strengthening the cross-link density of the coatings are crucial to enhance the performance of the coatings. Therefore, surface modification of nano-functional fillers is also one of the hot spots of research.

4 Conclusion and outlook

As an emerging nanomaterial, MOFs materials play a crucial role in the field of composite coating protection of metals because of their simple preparation process, low production cost and excellent anti-corrosion properties. In addition, MOFs materials act as excellent pH-responsive containers, which help to control the release of corrosion inhibitors and improve the long-term usability of corrosion inhibitors in coatings; the modifiability of MOFs to graphene oxide not only enhances the corrosion resistance of coatings, but also drastically reduces the amount of graphene oxide used, and the production cost of coatings is significantly reduced, giving active/passive corrosion resistance to coatings. However, the current research also has certain limitations: the main goal focuses on MOFs material to enhance the corrosion resistance of the coating, the weather resistance, radiation resistance, temperature resistance and chemical damage resistance of the coating and other aspects of the research are yet to be in-depth; only a single anti-corrosion properties of the composite coating is far from the current industrial generation of the actual use of standards. Therefore, multi-functional composite anti-corrosion coating will become a hot spot for future research. In recent years, two-dimensional metal organic framework materials (2D MOFs) have gradually appeared on the horizon of researchers. 2D MOFs have been used as Nano-fillers, such as the above-mentioned Cu-TCPP and Co-MOF, as a new type of 2D nanomaterials, which have ultra-thin thickness and nanoscale dimensions and play an important role in blocking corrosion erosion. It has also been shown that 2D MOFs are a graphene-like conductive material. Therefore, in future research, it can be tried to be compounded with zinc-rich epoxy resin to replace graphene filler, which is of great significance in reducing the cost of commercial anti-corrosion coatings.

Corresponding author: Xu Wang, School of New Energy and Materials, Southwest Petroleum University, No. 8 Xindu Avenue Chengdu, Chengdu, Sichuan 610500, China, E-mail: wwxx1969@163.com

Funding source: Institute of Engineering Technology, PetroChina Coalbed Methane Company Limited

Award Identifier / Grant number: GCY22008CQ02

Acknowledgments

Yang Chengwei would like to thank his graduate advisor, Professor Wang Xu from the School of New Energy and Materials, Southwest Petroleum University for his valuable comments and guidance as well as his continuous encouragement and support during the writing of this thesis. Yang Chengwei would like to thank the Institute of Engineering Technology, PetroChina Coalbed Methane Company Limited for their support of this article.

Research ethics: Not applicable.
Author contributions: All the authors have accepted responsibility for the entire content of this submitted manuscript and approved submission.
Competing interests: The authors state no conflict of interest.
Research funding: This work was supported by Institute of Engineering Technology, PetroChina Coalbed Methane Company Limited (project no. GCY22008CQ02).
Data availability: Not applicable.

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Received: 2023-06-20

Accepted: 2023-10-05

Published Online: 2023-11-24

Published in Print: 2024-01-29

Articles in the same Issue

https://doi.org/10.1515/polyeng-2023-0144

Keywords for this article

organic coating; corrosion; metal-organic frame materials; nano-corrosion filler