Metals and metal oxides polymer frameworks as advanced anticorrosive materials: design, performance, and future direction

Chandrabhan Verma; Chaudhery Mustansar Hussain; Mumtaz A. Quraishi; Kyong Yop Rhee

doi:10.1515/revce-2022-0039

Open Access Published by De Gruyter December 21, 2022

Metals and metal oxides polymer frameworks as advanced anticorrosive materials: design, performance, and future direction

Chandrabhan Verma

Chandrabhan Verma works at the IRC for Advanced Materials, KFUPM, Dhahran, 31261, Saudi Arabia. He is a member of the American Chemical Society (ACS). His research is mainly focused on the synthesis and designing of environmentally-friendly corrosion inhibitors useful for several industrial applications. Dr. Verma is the author of several research and review articles and has edited many books. He has a total citation of more than 8200. Dr. Verma has received many awards.
, Chaudhery Mustansar Hussain

Chaudhery Mustansar Hussain, PhD, is an adjunct professor and director of laboratories in the Department of Chemistry and Environmental Sciences at the New Jersey Institute of Technology, Newark, NJ, USA. His research is focused on the applications of nanotechnology and advanced materials, environmental management, analytical chemistry, and other various industries. Dr. Hussain is the author of numerous papers in peer-reviewed journals as well as a prolific author and editor of around 100 books.
, Mumtaz A. Quraishi

Dr. Mumtaz A. Quraishi is a Chair Professor at IRC for Advanced Materials, KFUPM, Saudi Arabia. Before joining KFUPM, he was an Institute Professor at IIT-BHU, Varanasi, India. He also served as Head of Department of Chemistry at IIT-BHU. He has teaching experience of more than 35 years. He has published more than 400 papers having a total citation rate of more than 30000. He has also authored and edited many books.
and Kyong Yop Rhee

Dr. Kyong Yop Rhee is a professor of Mechanical Engineering at Kyung Hee University (South Korea) since 1999. His main research interests are nanocomposites, surface treatment, fracture, and composite materials. He has published more than 451 scientific papers and has led 67 R&D projects. He earned his BS and MS degrees in Mechanical Engineering from Seoul National University (South Korea). He earned his PhD in Mechanical Engineering at the Georgia Institute of Technology.

From the journal Reviews in Chemical Engineering

https://doi.org/10.1515/revce-2022-0039

Abstract

Metals (Ms) and metal oxides (MOs) possess a strong tendency to coordinate and combine with organic polymers to form respective metal–polymer frameworks (MPFs) and metal oxide polymer frameworks (MOPFs). MPFs and MOPFs can be regarded as composites of organic polymers. MPFs and MOPFs are widely used for industrial and biological applications including as anticorrosive materials in the aqueous phase as well as in the coating conditions. The presence of the Ms and MOs in the polymer coatings improves the corrosion inhibition potential of MPFs and MOPFs by improving their self-healing properties. The Ms and MOs fill the micropores and cracks through which corrosive species such as water, oxygen, and corrosive ions and salts can diffuse and destroy the coating structures. Therefore, the Ms and MOs enhance the durability as well as the effectiveness of the polymer coatings. The present review article is intended to describe the corrosion inhibition potential of some MPFs and MOPFs of some most frequently utilized transition metal elements such as Ti, Si, Zn, Ce, Ag, and Au. The mechanism of corrosion inhibition of MPFs and MOPFs is also described in the presence and absence of metal and metal oxides.

Keywords: anti-corrosive coatings; composite coatings; corrosion protection; metal-polymer frameworks (MPFs); nanofillers; self-healing

1 Introduction

1.1 Corrosion: basics and a journey corrosion control

Metals and their alloys have a natural propensity to experience corrosive humiliation by the environmental constituents (Comizzoli et al. 1986, Frankel 1998). Corrosion is an exceedingly dangerous and pricey event as various corrosion allied failures have been reported worldwide. According to NACE’s (National association of corrosion engineers) assessment, the existing universal cost of corrosion is roughly US $2.505 trillion (≈3.4% of the world’s GDP; gross domestic product) out of which 15% (US $375)–35% (US $875) can be saved using formerly documented methods (Hou et al. 2017; Koch 2017; Song and Mishra 2017; Yeganeh et al. 2020). Some widespread corrosion preclusion strategies embrace coatings, alloying and dealloying, paintings, and cathodic protection and make use of corrosion inhibitors (Ahmad 2006; Shreir 2013; Smith and Virmani 2000). These methods comprise their profits and disadvantages. For aqueous phase inhibition, the use of organic corrosion inhibitors is the most popular method as their synthesis, preservation, implementation, and discharge are easy, effective, and cost-friendly (Guo et al. 2020a,b; Nmai 2004; de Souza and Spinelli 2009; Tan et al. 2022). Depending upon the character of the metal/electrolyte system and rising ecological welfare, a variety of alternatives are chronologically developed to substitute the existing less successful and ecological malignant corrosion inhibitors. Inorganic species including chromates, molybdates, phosphate, nitrates, etc. can be regarded as the oldest corrosion inhibitors. However, they were replaced by organic, principally heterocyclic corrosion inhibitors (Ahmed et al. 2019; Babić-Samardžija et al. 2005; Singh et al. 2017), because of the emerging interest of 4E, i.e. ecology, effectivity, economy, and energy. Recently, the use of natural polymers and compounds synthesized from energy-efficient methods is gaining attention.

Recently, the use of polymers and nanopolymers as anticorrosive materials is withdrawing significant attention as they provide excellent surface protection (Umoren and Solomon 2014; Umoren et al. 2006; Verma et al. 2020, 2021b). However, their applications were cut short through their insolubility. Functionalization of the polymers helps in their solubility enhancement as well as inhibition potential (Figure 1). Literature investigation shows that chemically modified polymers are widely used as corrosion inhibitors (Chauhan et al. 2021; Fazayel et al. 2018). These species become useful through building inhibitive films. The polymers and nanopolymers contain numerous peripheral functional groups through which they easily adsorption. Their adsorption depends upon numerous factors such as temperature and moisture. Similar to the heterocyclic corrosion inhibitors, adsorption of polymers and nanopolymers on the metal surface followed physiochemisorption i.e. both physical and chemical bondings. Chemical bonding occurs by the charge sharing between metal and electron-rich centers of the polymers. On the other hand, physical or ionic bonding occurs through electrostatic bonding between the charged metal surfaces and charged polymers (Ituen et al. 2017; Kuznetsov 2015). Noticeably, in aqueous solutions, metal surface and polar functional groups of the polymers acquire specific charges. The number and nature of polar functional groups in polymers and nanopolymers can be suitably modified using chemical derivatization or functionalization.

Figure 1:

Diagrammatic illustration of chronological growth of corrosion inhibitors and enhanced solubility of polymers and nanopolymers using functionalization.

1.2 Metals and metal oxides polymer frameworks (MPFs/MOPFs): fundamental and corrosion inhibition properties

MPFs and MOPFs are an important class of compounds in which Ms and MOs bind with polymer matrix using different covalent and noncovalent bondings including coordination bonding (Khan et al. 2013; Kitagawa 2014; Silva et al. 2015; Stock and Biswas 2012). MPFs and MOPFs can be regarded as members of metal-organic frameworks (MOFs) in which organic compounds are replaced by organic polymers. MPFs and MOPFs are composites in which polymers coordinate with a metal and metal oxide instead of organic ligands. MPFs and MOPFs can be regarded as coordination polymers or metallopolymers as they are metal and metal oxide-containing polymers. Since their development, MPFs and MOPFs have withdrawn substantial awareness in materials science and inorganic chemistry. The MPFs and MOPFs have been used widely for different industrial applications including in the isolation, purification, and storage of gases (e.g. H₂ and CO₂), in catalysis, and as supercapacitors. Recently, the use of MPFs and MOPFs as anticorrosive materials is acquiring immense attention as they provide excellent surface protection. The MPFs and MOPFs can be effective by adsorbing on the metal surface thereby forming the hydrophobic protective film. The anticorrosive applications of polymers are long known (Umoren 2009; Umoren et al. 2006). They are widely used corrosion inhibitors, especially as anticorrosive coating materials. A literature survey suggests that numerous natural and synthetic polymers and their degradants, such as oligomers and macromolecules, are used as aqueous phase corrosion inhibitors (APCIs) (Tiu and Advincula 2015). However, many of the polymers experience solubility problems otherwise their use would have been more explored. Therefore, attempts have been made to enhance their aqueous phase by chemical functionalization. Chemically modified/functionalized polymers, especially naturally originated polymers, are extensively used as APCIs (Chauhan et al. 2020, 2021; Dagdag et al. 2020b; Fazayel et al. 2018; Shirazi et al. 2020). The addition of the polar functional groups and heterocyclic moieties in the polymer matrix increases their solubility and corrosion inhibition performance by behaving as adsorption centers (Figure 2a).

Figure 2:

(a) Diagrammatic presentation of solubilization of insoluble polymer through chemical functionalization and (b) the effect of metal and metal oxide on corrosion inhibition performance of a polymer coating.

Natural and synthetic polymers are extensively employed as anticorrosive coatings in their purified and composite forms. Generally, composite-based coatings exhibit better anticorrosive performance as compared to pure polymer coatings. MPFs and MOPFs represent two common examples of polymer composites that have been widely used as anticorrosive formulations. MPFs and MOPFs show better anticorrosive activities than their pure polymer-based coatings which are attributed to the self-healing and curing properties of the MPFs and MOPFs. The presence of metal and metal oxide in the MPFs and MOPFs fills the micropores and cracks of polymer coatings and avoids the penetration of corrosive species such as oxygen, water, corrosive salts, and ions. Alternatively, the presence of the Ms and MOs in MPFs and MOPFs avoids the direct penetration of corrosive species and chemicals that penetration feels no hinder in the absence of Ms and MOs (Figure 2b). Literature study indicates that currently few reports have limited description of corrosion inhibition potential of only a few series of metal oxide/polymer composites (Basik and Mobin 2022; Verma et al. 2021a, 2022). These reports do not provide any background about their synthesis, properties, and corrosion inhibition mechanism. In the present article, the entire aspects of corrosion inhibition using metal and metal oxides/polymer frameworks (MPFs and MOPFs) including their bonding (coordination), properties, and a plethora of other possible uses are documented. The mechanism of enhancement in the durability and effectiveness of polymer coatings is also documented with suitable illustrations. The anti-corrosive effect of numerous series of MPFs and MOPFs has also been comprehensively described with possible challenges and future outlooks. The literature study suggests that this is one of the primary reports on the anticorrosive effect of MPFs and MOPFs. In the present report, the anticorrosive effect of some Ms and MOs such as TiO₂, SiO₂, ZnO, Ag/Au, and CeO₂-based formulations is described extensively.

2 Corrosion control using MPFs and MOFs: literature survey

2.1 TiO₂-based MPFs and MOPFs in corrosion control

Polyaniline (PANI or PAni) is an important member of the rod-polymer family. PANI represents an example of an organic semiconductor or conducting polymer that possesses excellent mechanical properties and electrical conductivity (Cho et al. 2004; Kim et al. 2006; Valentová and Stejskal 2010; Wang et al. 2016). Generally, PANI exists in three idealized oxidation states, namely, leucoemeraldine [(C₆H₄NH)_n], emeraldine [([C₆H₄NH]₂[C₆H₄N]₂)_n], and (per)nigraniline [(C₆H₄N)_n] that are present colorless/white, green/blue, and blue/violate color, respectively. PANI can be synthesized by oxidation of any generic oxidant and ammonium persulfate in 1 M HCl (or other acids) (Bhagwat et al. 2016; Zhang et al. 2021).

(1) n C 6 H 5 NH 2 + [ O ] → [ C 6 H 4 NH ] n + H 2 O

(2) { [ C 6 H 4 NH ] 2 [ C 6 H 4 N ] 2 } n + RCO 3 H → [ C 6 H 4 N ] n + H 2 O + RCO 2 H

PANI possesses potential applications and is widely used as a precursor for the synthesis of N-doped carbon materials such as quantum dots (QDs) (Lyu et al. 2018; Zhu et al. 2014). PANI has also been used in ESD coatings, sensing, aerosol printings, and corrosion mitigation (Bhadra et al. 2009; Coltevieille et al. 1999; Kazemi et al. 2021). PANI acquires insufficient solubility which limits its use as an aqueous phase inhibitor (Gao et al. 2021). Nevertheless, oligoaniline which is a smaller fraction of PANI has been successfully employed (Syed et al. 2015; Yadav et al. 2013). Because of its polymeric character, PANI provides sufficient surface coverage and protection, especially in the coating phase. Anticorrosive application of PANI and its composites is very rarely reported. Although PANI furnishes excellent surface coverage when applied as surface protective coating however PANI based coatings are highly unstable and susceptible to reacting with the environmental components which cut short the durability of PANI-based coatings. After a specific time interval, PANI-based coatings get ruptured resulting in the formation of coating pores and cracks through which corrosive species including moisture, air, electrolyte molecules, and salts can penetrate and accelerate the metallic corrosion rate. Therefore, corrosion scientists and engineers are devoted to developing highly durable anti-corrosive coatings. One such major attempt is the incorporation of metal and metal oxide(s) (in small amounts) in the anticorrosive formulations (Islam et al. 2021; Viswanathan et al. 2014; Yeong et al. 2018). Metal and metal oxides fill the micropores and cracks generated over the surface of the metal. Thereby, they enhance the effectiveness as well as durability of the coatings.

Literature study suggests that PANI-TiO₂-based composites are widely investigated as anticorrosive formulations (Al-Dulaimi et al. 2011; Atta et al. 2017b; Sulistyaningsih and Lestari 2020; Yan et al. 2015). The PANI-TiO₂ coating can be applied on metal surfaces using various methods including film applicator, electrodeposition, salt spray, and dipping methods (Sørensen et al. 2009). Out of various methods, the use of solution dipping is a very common and peculiar method in which metal surface is allowed to coat uniformly in the homogenized solution of coating materials. Numerous methods such as SEM, TEM, FT-IR, UV–vis, XRD, and XPS are widely employed for coating characterization and thickness measurements. Noticeably, PANI polymerized in HCl solution acquires a diameter of 100–150 nm whereas its composites acquire a diameter of about 40 nm. A summary of some major studies on PANI-TiO₂-based anticorrosive coatings is illustrated in Table 1. The PANI-TiO₂ effectively serves as anticorrosive formulations for mild steel (Mahulikar et al. 2011), 304 stainless steel (Abaci and Nessark 2015), carbon steel (Pagotto et al. 2016), 316LN stainless steel (Rathod et al. 2013), Al1050 alloy (Ates and Topkaya 2015), Q235 steel (Wang et al. 2019a,b), and cold rolled carbon steel (Jadhav and Gelling 2015) etc. in various electrolytes. In these solutions, PANI-TiO₂ becomes effective by building a protective surface covering through their adsorption. SEM, TEM, FT-IR, UV–vis, XRD, and XPS methods have been used to demonstrate the adsorption of PANI-TiO₂.

Table 1:

Summary of some major reports on TiO₂-based MPFs and MOPFs as anticorrosive formulations for different metals/electrolyte systems.

S/N	Nature of composite	Metal/electrolyte	References	S/N	Nature of composite	Metal/electrolyte	References
1	Polyaniline/TiO₂	Mild steel/5% HCl, 5% NaOH, and 3.5% NaCl	Mahulikar et al. (2011)	2	PANI + TiO₂	304 stainless steel/n H₂O/(0.1 M LiClO₄ + 0.5 M H₂SO₄)	Abaci and Nessark (2015)
3	PAni and PAni/n-TiO₂	Carbon steel and welded CS/3% NaCl	Pagotto et al. (2016)	4	PANI/TiO₂	316LN SS/3% NaCl	Rathod et al. (2013)
5	PANI, PANI-TiO₂, PANI/Zn, and PANI/Ag	Al1050 alloy/3.5% NaCl s	Ates and Topkaya (2015)	6	Polydopamine modified GO-TiO₂ (nano-PDA@GO-TiO₂)	Q235 steel/3.5% NaCl	Wang et al. (2019a,b)
7	TiO₂/PANI composite, and TiO₂/PPy	Cold rolled carbon steel/5% NaCl	Jadhav and Gelling (2015) and Liu et al. (2018a)	8	Polyaniline–nano-TiO₂	Stainless steel/3.5% NaCl	Radhakrishnan et al. (2009)
9	Polyaniline (PANI)-TiO₂	Carbon steel/3.5% NaCl	Huang et al. (2020)	10	Poly(aniline-co-o-toluidine)/TiO₂	Carbon steel/3.5% NaCl	Aslam et al. (2018)
11	Nb-doped TiO₂ -polyaniline	316 stainless steel/1 M H₂SO₄	Wang et al. (2019a,b)	12	TiO₂/GO/PANI	Q235 carbon steel/3.5% NaCl	(Chen et al. 2021a,b)
13	TiO₂ nanosheets/CdSe/polyaniline/graphene (TCPG)	304 stainless steel/photocathodic protective	Xu et al. (2020)	14	TiO₂/poly(indole-co-aniline)	Stainless steel/3.5% NaCl	Döşlü et al. (2018)
15	PPy, PPy/TiO_2, and PPy/TiO₂@Mo	304 stainless steel/3.5% NaCl	Chen et al. (2020)	16	Polypyrrole/TiO₂	AISI 1010 steel/0.1 M H₂C₂O₄ + 0.1 M pyrrole	Ferreira et al. (2001)
17	PPy/TiO₂	Copper/3.5% NaCl	Beikmohammadi et al. (2018)	18	Co-doped TiO₂/polypyrrole	AISI 1018 steel/3.5% NaCl	Ladan et al. (2017)
19	TiO₂/PPy and V-TiO₂/PPy	Carbon steel/0.1 M HCl	Chen et al. (2019)	20	PPy–TiO₂–phenylalanine	Fe–C steel/3.5% NaCl	Pahuja et al. (2020)
21	Polypyrrole/TiO₂	AISI 1010 steel (mild steel)/3.5% NaCl	Lenz et al. (2003)	22	Polypyrrole nanowire/TiO₂	Ti and 304 SS/photocathodic protection	Cui et al. (2015)
23	PDMAS/TiO₂	Carbon steel/5% NaCl	Fadl et al. (2020a)	24	DGEDDS-MDA and DGEDDS-MDA-TiO₂	Carbon steel/3% NaCl	Dagdag et al. (2020a)
25	Epoxy, epoxy/BTA, epoxy/TiO₂/ and epoxy/TiO₂/BTA/(PEI/PSS)₂.	Carbon steel/0.5 M NaCl	Liu et al. (2020a,b)	26	Epoxy, Epoxy-8HQ and epoxy-ncTiO₂-8HQ	2024-T3/0.0 M NaCl	Balaskas et al. (2012)
27	Bis[triethoxysilylpropyl]-tetrasulfide (BTESPT)/TiO₂	304 stainless steel/3.5% NaCl	Chen et al. (2015)	28	Polytetrafluoroethylene (PTFE)/TiO₂	Titanium alloy/3.5%	Wang et al. (2020)
29	[TiO₂ NFs/SBP]	Mild steel/1 M HCl	Abd El-Lateef et al. (2020)	30	DGPMDAP/MDA/TiO₂	Carbon steel/1 M HCl	Hsissou et al. (2019)
31	Poly(urethane-esteramide)/TiO₂	Mild steel/3.5% HCl, 3.5% NaOH, and 5% NaOH	Shaik et al. (2015)	32	TiO₂-NIPAm/AAm, TiO₂-AA/AAm, and TiO₂-NIPAm/AA	Carbon steel/sea and distil water	Atta et al. (2017a)
33	Poly (butyl methacrylate-late)/GO/TiO₂ (poly(BMA)/GO/TiO₂)	Magnesium alloy (AZ31)/3.5% NaCl	Nazeer et al. (2019)	34	Polyvinyl alcohol(PVA)/TiO₂	Mild steel/3.5% NaCl	Devikala et al. (2018)
35	Epoxy-TiO₂	CR mild steel/3.5% NaCl	Shafaamri et al. (2020)	36	TiO₂-APTAC/AMPS- Na, TiO₂-APTAC/AA and TiO₂-APTAC/NIPAm	Mild steel/3.5% NaCl	Kumar et al. (2018)
37	MT-AA/AMPSs	St-37 steel/3.5% NaCl	Ghomi et al. (2020)	38	TiO₂/polyvinylidene fluoride	Copper/3.5 wt% NaCl	Qing et al. (2016)
39	BTESPT, BTSEPT/TiO₂ and BTSEPT/TiO₂/MWCNT	AA 2024/3.5% NaCl	Zhang et al. (2016)	40	Hydroxyapatite (HA, Ca₁₀(PO₄)₆(OH)₂)/TiO₂	Ti–6Al–4V/0.05 g iodine in 50 mL EtOH	Farnoush et al. (2015)
41	Cu(II)–Schiff base complex (CuSB@Fe₃O₄, CuSB@Fe₃O₄/TiO₂ and CuSB@Fe₃O₄/SiO₂)	Carbon steel/3.0 N HCl	Khalaf and Abd El-Lateef (2020)	42	TiO₂/g-C₃N₄ and 3-(aminopropyl)triethoxysilane functionalized hybrid	Q235 carbon steel/3.5% NaCl	Pourhashem et al. (2020)
43	TiO₂-epoxy	Steel (Fe-500 grade)/3.5% NaCl solution and 1 M H₂SO₄	Ramganesh et al. (2020)	44	Epoxy, epoxy/modified TiO₂ and Epoxy/MBI	Carbon steel/0.05 M NaCl	Liu et al. (2018a)
45	Poly(3-amino-1, 2, 4-triazole) + TiO₂	Copper/1% NaCl	Rajkumar and Sethuraman (2013)	46	TiO₂–vinylester polymer composite	Aluminum/3% NaCl	Yabuki et al. (2011)
47	2-Amino-5-mercapto-1,3,4-thiadiazole/TiO₂	Copper/3.5% NaCl	Vinothkumar and Sethuraman (2018)	28	TiO₂ encapsulated with dodecylamine (DOC).	Carbon steel/3.5%NaCl	Ubaid et al. (2019)
49	Octadecylamine-functionalized graphene/TiO₂	Copper/0.5 M H₂SO₄	Sadeghian et al. (2020)	50	Polystyrene/TiO₂	Aluminum alloy 2024-T3/3.5% NaCl	Zhang and Zhang (2019)
51	Al₂O₃ anchored QDs/TiO₂ (Al/C/TNRs)	Q235 CS/3.5% NaCl	Feng et al. (2020)	52	Ni/rGO-TiO₂	Mild steel/0.1 M acetic acid & 0.06 M citric acid	El-Sayed et al. (2019)
53	r-GO/TiO₂	Magnesium/0.1 M Na₂SO₄	Gandhi et al. (2018)	54	TiO₂-rGO	304 stainless steel/3.5% NaCl	Azadeh et al. (2019)
55	TiO₂–GO and TiO₂–GO/epoxy	Carbon steel/3.5% NaCl	Yu et al. (2015)	56	PbS & CdS cosensitized graphene/TiO₂	304 stainless steel/3.5% NaCl	Yang et al. (2018a,b)
57	r-GO/TiO₂	Magnesium/3.5% NaCl	Kavimani et al. (2018)	58	Ni-phosphorus – TiO₂ – rGO (NiP-TiO₂ sol-RGO)	Mild steel/3.5% NaCl	Promphet et al. (2017)
59	DA/meso-TiO₂	Carbon steel/3.5% NaCl	Wang et al. (2018)	60	BPTA with 0.001 g, of TiO₂-NPs	Mild steel/1 M HCl	Al-Taweel et al. (2019)
61	Chitosan-doped-hybrid/TiO₂	Aluminum/3.5% NaCl	Balaji and Sethuraman (2017)	62	Chitosan/TiO₂	Mild steel/0.1 M HCl	John et al. (2019)

PDMAS, poly-dimethylamino siloxane; DGEDDS, diglycidyl ether 4,4′-dihydroxydiphenylsulfone; MDA, 4,4′-methylene dianiline; NFs/SBP, nanofibers/Schiff base phenylalanine composite; DGPMDAP, decaglycidyl pentamethylene dianiline of phosphorus; PANI, polyaniline; rGO, reduced graphene oxide; PPy, polypyrrole; PSS, poly(sodium-4-styenesulfonate); BTA, benzotriazole; PEI, polyethyleneimine; BTESPT, bis-[triethoxysilylpropyl]tetrasulfide; 8HQ, 8-hydroxyquinoline; NIPAm, N-isopropyl acrylamide; AA, acrylic acid (AA); AAm, acrylamide; QDs, quantum dots; APTAC, 3-(acrylamidopropyl) trimethylammonium chloride; AMPS-Na, 2-acrylamido-2-metylpropane sulfonate sodium salt; PVA, polyvinyl alcohol; PDMS, polydimethylsiloxane; BPTA, N-benzylidene-5-phenyl-1,3,4-thiadiazol-2-amine.

Ates and Topkaya (2015) studied the anticorrosive effect o PANI, PANI-TiO₂, PANI/Zn, and PANI/Ag for Al1050 alloy in 3.5% NaCl solution and through SEM analysis they observed that these composites become effective by adsorbing on the surface. The inhibition effectiveness of the tested species followed the sequence: PANI/Ag (97.54%) > PANI/Zn (92.52%) > PANI/TiO₂ (91.91%) > PANI (91.41%). SEM study suggests that among the different coatings, the PANI/Ag coating is the most uniform while PANI, PANI/TiO_2, and PANI/Zn coatings are highly rough with extensively distributed grains. From this observation, it can be concluded that for effective anticorrosive activity, a uniformly distributed coating is essentially required. Apart from PANI-TiO₂, PANI-TiO₂-based other coatings such as Nb-doped TiO₂–polyaniline (Wang et al. 2019a,b), TiO₂/GO/PANI (Chen et al. 2021a,b), TiO₂ nanosheets/CdSe/polyaniline/graphene (Xu et al. 2020), and TiO₂/poly(indole-co-aniline) (Döşlü et al. 2018) have also been tested.

Polypyrrole (PPy) is another polymer that has been used extensively for the production of anticorrosive coating formulations (Duchet et al. 1998; Ma et al. 2011). PPy is produced by oxidative polymerization of pyrrole. Similar to PANI, PPy is a good conductor of electricity and is used for different applications including in biological, electronic, optical, and medical fields. There are numerous methods for PPy synthesis that have been reported but electrochemical synthesis using chemical oxidation is the most common and peculiar method. Synthesis of PPy from the chemical oxidation of pyrrole and p-doping (to enhance electrical conductance) is illustrated as follows (Duchet et al. 1998; Ma et al. 2011):

(3) n C 4 H 4 NH + 2 n FeCl 3 → ( C 4 H 2 NH ) n + 2 n FeCl 2 + 2 n HCl

(4) ( C 4 H 2 NH ) n + 0.2 X → [ ( C 4 H 2 NH ) n X 0.2 ]

The chemical oxidation and the p-doping can be affected and controlled electrochemically. PPy is extensively used in the manufacturing of chemical sensors and electronic devices. Literature investigation suggests that pyrrole and its derivatives have been used as effective APCIs (Stupnišvek-Lisac et al. 1992; Verma et al. 2015; Zarrouk et al. 2015). Nevertheless, the use of PPy as an anticorrosive material in the solution phase is highly limited because of its restricted solubility. Therefore, PPy and its composites are mainly employed as anticorrosive coating formulations. TiO₂-based PPy composites are also used effectively for different metals and alloys in various electrolytes. Due to its polymer nature, PPy provides excellent surface protection and the presence of TiO₂ enhances durability as well as inhibition potential of the PPy coatings. Through its self-healing property, TiO₂ fills the surface micropores and cracks and avoids the leakage of corrosive species inside the coating structures. A summary of major reports on PPy-TiO₂-based anticorrosive coatings is presented in Table 1. Chen et al. (2020) demonstrated the relative anticorrosive potential of PPy, its TiO₂ composite (PPy/TiO₂), and molybdate-loaded PPy/TiO₂ composite (PPy/TiO₂@Mo) for 304 stainless steel in 3.5% NaCl. SEM analysis suggests that PPy/TiO₂@Mo coating was much thicker and smoother than that of PPy and PPy/TiO₂ coatings. The thickness of various coatings followed the sequence: PPy/TiO₂@Mo (5.59 ± 0.42 μm) > PPy/TiO₂ (4.16 ± 0.51 μm) > PPy (2.27 ± 0.57 μm). It was also derived that PPy/TiO₂@Mo coating contains around double thickness as compared to the PPy coating (Figure 3). Based on this outcome, the authors concluded that PPy/TiO₂@Mo furnishes long-term protection from corrosion as it forms a relatively stronger anticorrosive barrier.

Figure 3:

SEM morphologies and subsequent cross-section micrographs of the (a), (d) PPy, (b), (e) PPy/TiO₂ and (c), (f) PPy/TiO₂@Mo coatings (Chen et al. 2020). Reproduced with permission @copyright Elsevier, 2020.

The corrosion inhibition potential of PPy, PPy/TiO_2, and PPy/TiO₂@Mo was assessed electrochemically using EIS, CV, and OCP methods. The OCP measurements show that in all coated specimens, OCP curves shifted in the positive direction concerning the noncoated specimen which indicates the formation of passive and corrosion protective film by PPy, PPy/TiO_2, and PPy/TiO₂@Mo. EIS study suggested an increase in the magnitude of diameter of Nyquist curves in the presence of PPy, PPy/TiO_2, and PPy/TiO₂@Mo, and this increase was consistent with their order of inhibition effectiveness. Figure 4 represents the Nyquist and Bode (frequency and phase angle) plots for 304 stainless steel dissolution in 3.5% NaCl with and without PPy, PPy/TiO_2, and PPy/TiO₂@Mo presented in Figure 4. Noticeably, in the presence of PPy, PPy/TiO_2, and PPy/TiO₂@Mo diameter of Nyquist curves increases significantly indicating that they build a protective physical barrier at the interface of 304 stainless steel and 3.5% NaCl. Careful observation of Nyquist curves indicates that in the absence of PPy, PPy/TiO_2, and PPy/TiO₂@Mo, 304 SS corrosion involves a single charge transfer mechanism as uninhibited Nyquist curves reveal a single semicircle. On the hand, in the presence of PPy, PPy/TiO_2, and PPy/TiO₂@Mo, 304 SS corrosion involves two charge transfer mechanisms.

Figure 4:

Nyquist (left side), Bode frequency (middle), and phase angle (right side) plots for 304 stainless corrosion in 3.5% in the absence of coatings (a), in the presence of PPy coating (b), in the presence of PPy/TiO₂ coating (c), and the presence of PPy/TiO₂@Mo coating (d) (Chen et al. 2020). Reproduced with permission @copyright Elsevier, 2020.

The involvement of two charge transfer processes was further supported by two maximum in the Bode phase angle plots of inhibited metallic specimens. Corrosion inhibition using adsorption of PPy, PPy/TiO_2, and PPy/TiO₂@Mo was further supported by SEM and AFM studies where 304 SS surfaces in different coating conditions are allowed to corrode in 3.5% NaCl for 30 days (720 h). It was observed that surface bare metal is badly corroded and damaged with a huge number of micropores and cracks. However, in the presence of PPy, PPy/TiO_2, and PPy/TiO₂@Mo coatings, surface morphologies become smoother, especially in the presence of PPy/TiO₂ and PPy/TiO₂@Mo. The PPy/TiO₂ and PPy/TiO₂@Mo coatings remain compact and dense. A similar observation was reported by the AFM study. The average roughness (R _a) of the metal surface coated with PPy/TiO₂@Mo, PPy/TiO₂, PPy, and bare surfaces were 16.9, 61.13, 110.64, and 320.07 nm, respectively.

In another study, polypyrrole nanocomposites (PPy NTCs) doped with TiO₂ and Co/TiO₂ were evaluated as anticorrosive formulations for AISI 1018 steel in 3.5% NaCl (Ladan et al. 2017). Similar conclusions were derived. Careful observation of FESEM images of TiO₂, TiO₂/PPy, and Co-doped TiO₂/PPy NTCs suggests that TiO₂ and Co are uniformly distributed in The PPy matrix. The anticorrosive effect of TiO₂-doped PPy has also been reported elsewhere (Chen et al. 2019; Cui et al. 2015; Lenz et al. 2003; Pahuja et al. 2020). Epoxy resins/TiO₂ and organic compounds/TiO₂ composites have also been investigated as anticorrosive formulations (Fadl et al. 2020a) and a summary of major reports is illustrated in Table 1. Recently, our research group (Dagdag et al. 2020a), reported the corrosion inhibition potential of a DGEDDS and MDA-based resin, designated as DGEDDS-MDA, and its TiO₂ composites for carbon steel corrosion in 3.5% NaCl solution using computational and experimental demonstrations. Results showed that DGEDDS-MDA and DGEDDS-MDA/TiO₂ act as effective anticorrosive materials even after exposing the metal specimens for 2000 h to UV radiation. It was also observed that the presence of TiO₂ in the epoxy resin enhances its durability as well as anticorrosive potential. Computational studies suggest that DGEDDS-MDA interacts with donor–acceptor mode (DFT outcomes) and acquires a flat orientation on the metallic surface (MDS results). Figure 5 represents the FMOs and orientation of DGEDDS-MDA acquired on the carbon steel surface.

Figure 5:

FMOs (HOMO and LUMO; upper) and side- and top-views of DGEDDS-MDA adsorption on Fe(110) surface (Dagdag et al. 2020a). Reproduced with permission @copyright Elsevier, 2020.

Similar to this, numerous studies on the anticorrosive effect of epoxy resins/TiO₂ and organic compounds/TiO₂ composites have been evaluated. These compounds become effective by building physical passive film. Their adsorption and corrosion inhibition measurements are carried out using various surface investigations including SEM, EDX, TEM, FESEM, UV–vis, FT-IR, XPS, XRD, EDX, etc. methods. Recently, the formulation and use of GOTiO₂-based composites for anticorrosive applications is gaining attention (Azadeh et al. 2019; El-Sayed et al. 2019; Gandhi et al. 2018; Kavimani et al. 2018; Promphet et al. 2017; Yang et al. 2018a,b; Yu et al. 2015). Noticeably, GO/TiO₂ composites exhibit better anti-corrosive properties as compared to TiO₂ and GO separately. This can be attributed to the self-healing properties of TiO₂ in GO-based anticorrosive coatings. Chitosan is a bio-based polymer that consists of repeating units of D-glucosamine and N-acetyl-D-glucosamine joint together by β-1, 4-glycosidic linkage. The use of chitosan and its derivatives as anticorrosive materials is acquiring special attention. Given this currently, chitosan/TiO₂ composite has been tested as anticorrosive formulations in a few studies (Balaji and Sethuraman 2017; John et al. 2019).

2.2 ZnO-based MPFs and MOPFs in corrosion control

Zinc oxide (ZnO) is a white power that is insoluble in water (Ahmad and Zhu 2011; Coleman and Jagadish 2006; Djurišić et al. 2012). ZnO has been used as an additive in various materials such as rubbers, food supplements, cosmetics, plastics, ceramics, lubricants, glass, and cement. ZnO is also employed as adhesives, pigments, fire retardants, batteries, ointments, sealants, paints, ferrites, foods, and first-aid tapes (Ahmad and Zhu 2011; Coleman and Jagadish 2006; Djurišić et al. 2012). ZnO exists naturally as the mineral zincite however it is commercially derived from synthesis. ZnO acquires various properties that make it useful for numerous industrial applications. Literature investigation suggests that ZnO combines with organic compounds and polymers to form corresponding composites (Artifon et al. 2019; Bakhsheshi-Rad et al. 2017; Guo et al. 2020a,b; Kadri et al. 2021; Kumari et al. 2021; Quadri et al. 2017; Ramezanzadeh et al. 2017; Verma et al. 2019). These composites are extensively employed as corrosion inhibitors, especially in coating formulations. The presence of Zn or ZnO in the polymer matrix enhances their corrosion inhibition performance by filling the micropores and cracks present in the coating structures through which corrosion species including moisture, salts, and corrosive gases can penetrate and initiate and propagate the corrosion (Ezzat et al. 2021; Kamburova et al. 2021; Loto et al. 2015; El Saeed et al. 2015). ZnO can also reinforce the binding of polymers with the metal surface. Theoretically, the coating formulations uniformly distributed with Zn or ZnO would act as a better anticorrosive barrier as compared to the formulation in which they are not uniformly distributed (Selvam et al. 2016; Somoghi et al. 2021; Zhu et al. 2020).

Selim et al. (2021) while studying the anticorrosive potential of polydimethylsiloxane (PDMS)/GO nanosheets decorated with ZnO nanorods (GO-ZnO NRs) for carbon steel in 3.5% NaCl showed that ZnO NRs are uniformly distributed in the matrix of GO nanosheets. The GO-ZnO NRs were allowed to distribute in the PDMS matrix followed by the air-assisted spray coating of PDMS/GO-ZnO. The characterization and morphology distribution of PDMS/GO-ZnO was carried out using FESEM, EDX, TEM, XRD, FTIR, and AFM methods. The anti-corrosive effect of PDMS/GO-ZnO coating was achieved using EIS and PDP methods. Synthesis of the ZnO NRs, GO nanosheets, and PDMS coatings are illustrated in Figure 6. The authors determined that the presence of polar functional groups such as hydroxyl (–OH), carboxyl (–COOH), and epoxy-moieties help ZnO to interact with GO nanosheets and form GO-ZnO NRs. It is important to mention that similar protocols have been adopted for the synthesis of other ZnO composites with GO and other polymers. Apart from that ZnO NRs can also interact with GO nanosheets using physical interactions such as hydrogen bonding.

Figure 6:

Synthesis of GO nanosheets and ZnO nanorods (upper) and preparation of PDMS/GO-ZnO coating on carbon steel surface through air-spray method (lower) (Selim et al. 2021). Reproduced with permission @copyright Elsevier, 2021.

Similarly, Asaldoust and Ramezanzadeh (2020) developed a benzimidazole-zinc phosphate (ZP-BIM) tailored GO formulation for an additive in the epoxy-based coating on mild steel in 3.5% NaCl solution. The authors showed that different elements were uniformly distributed in the GO matrix (Figure 7). The chemical composition, morphology, and characterization of the GO-ZP-BIM were achieved using various spectral techniques including FE-SEM, EDX, Raman, FT-IR, RDX, and XPS methods. The magnitude of released inhibitive species including BMI, zinc cation, and phosphate anions were analyzed using the UV–vis method. Electrochemical analyses indicate that GO-ZP and GO-ZP-BMI-based coatings exhibit the highest inhibition activities of 62.2 and 86.5%, respectively. FESEM and EDX studies indicate that GO-ZP and PDMS/GO-ZnO become effective by building a passive film over the metal surface.

Figure 7:

Diagrammatic illustration for the synthesis of GO-ZP and GO-ZP-BMI (Asaldoust and Ramezanzadeh 2020). Reproduced with permission @copyright Elsevier, 2020.

An electrochemical impedance spectroscope (EIS) study was carried out to demonstrate the relative anticorrosive activities of GO-ZP and GO-ZP-BMI coatings. Nyquist and Bode (phase angle and frequency) plots for carbon steel corrosion with and without GO-ZP and GO-ZP-BMI coatings are illustrated in Figure 8. It can be seen that the diameters of Nyquist curves for CS corrosion in 3.5% NaCl without GO-ZP and GO-ZP-BMI coatings are much smaller as compared to the diameter of Nyquist curves in the presence of GO-ZP and GO-ZP-BMI coatings. This observation indicates that GO-ZP and GO-ZP-BMI coatings behave the barrier to the charge transfer process. Further, diameters of Nyquist curves protected by GO-ZP-BMI coating are much bigger as compared to the diameter of Nyquist curves inhibited by GO-ZP coating indicating that GO-ZP-BMI-based coating is much more effective as compared to the GO-ZP coating. The presence of a single semicircle in the inhibited and non-inhibited Nyquist curves indicates that CS corrosion in 3.5% NaCl involves a single charge transfer mechanism irrespective of the presence or absence of GO-ZP and GO-ZP-BMI coatings. The single charge transfer mechanism of the CS/3.5% NaCl system was also supported by a single maximum in the inhibited and non-inhibited Bode curves. It can also be seen that phase angle values of inhibited Bode curves are higher than that of the non-inhibited Bode curve.

Figure 8:

Nyquist (left side) and Bode (frequency and phase angle) plots for CS corrosion in the absence (a1), (b1) and presence of GO-ZP (a2), (b2) and GO-ZP-BIM (a3), (b3) (Asaldoust and Ramezanzadeh 2020). Reproduced with permission @copyright Elsevier, 2020.

The anticorrosive effectiveness of ZnO composites based on GO (Asaldoust et al. 2020; Azar et al. 2020; Ebrahimi et al. 2020; Habibiyan et al. 2020; Mohammadkhani et al. 2020; Othman et al. 2020; Taheri et al. 2019; Xiao et al. 2018; Xing et al. 2019; Zhang et al. 2020a,b,c; Zhou et al. 2019), MWCTNs (Gujjar et al. 2000), and quantum dots (Behgam et al. 2020; Liu et al. 2020c) are also demonstrated extensively. In these formulations, ZnO is uniformly distributed in the GO matrix and provides excellent anticorrosive activities. The composites are characterized using various spectral techniques. Along with GO, composites of ZnO with polymers such as polyurethane (Ariffin et al. 2020; Christopher et al. 2015; Mousa et al. 2018; Rashvand and Ranjbar 2013), poly(lactic acid) (Mousa et al. 2018), polypyrrole (Jlassi et al. 2020; Satpal et al. 2020), polyaniline (Kumar et al. 2020; Rouhollahi and Barzegar Khaleghi 2018), polyacrylamide (Morsi et al. 2016), poly(glycerol succinate) (Unnisa et al. 2018), poly methyl methacrylate (Potdar et al. 2020), epoxy resins (Alibakhshi et al. 2018; Banczek et al. 2006; Dagdag et al. 2020a,b,c; Ibrahim et al. 2020; Majd et al. 2020; Palimi et al. 2018; Ramezanzadeh et al. 2014; Yang et al. 2018a,b), chitosan (John et al. 2015; Vathsala et al. 2010), and other (AL-Mosawi et al. 2021; Chen et al. 2021a,b; Ji and Prakash 2019) are also tested as effective anticorrosive coatings, especially for steel alloys in neutral sodium chloride solution. A summary of such major reports is illustrated in Table 2. Noticeably, most of the ZnO-based formulations of composites are used as anticorrosive coatings. Reports on aqueous phase corrosion protection of ZnO/Zn composites are very few.

Table 2:

Summary of some major reports on Zn/ZnO-based MPFs and MOPFs as anticorrosive formulations for different metals/electrolyte systems.

S/N	Nature of composite	Metal/electrolyte	References	S/N	Nature of composite	Metal/electrolyte	References
1	GO-ZnO nanorodes-based nanocomposites	Carbon steel/3.5% NaCl	Selim et al. (2021)	2	Benzimidazole-(ZP-BIM) tailored GO/epoxy resin	Mild steel/3.5% NaCl	Asaldoust and Ramezanzadeh (2020)
3	Polydopamine (PDA)-Zn (II) complex on GO framework	Mild steel/3.5% NaCl	Habibiyan et al. (2020)	4	Zn and Zn-GO nanocomposite	Mild steel/3.5% NaCl	Azar et al. (2020)
5	rGO/ZnO hybrid composites	Zinc/3.5% NaCl	Ebrahimi et al. (2020)	6	GO/Zn rich epoxy composite	Carbon steel/3.5% NaCl	Zhou et al. (2019)
7	GO nanosheets/polyaniline/Zn cations	Mild steel/3.5% NaCl	Taheri et al. (2019)	8	Zinc-rich epoxy composite using SiO₂-GO	Q235 steel/3.5% NaCl	Zhang et al. (2020a,b,c)
9	GO@Zn₃PO₄/epoxy composite	Carbon steel/3.5% NaCl	Asaldoust et al. (2020)	10	GO/Zn doped-PPy nanoparticles	Carbon steel/3.5% NaCl	Mohammadkhani et al. (2020)
11	ZnMoO₄/rGO composite	Q235 steel/3.5% NaCl	Xing et al. (2019)	12	GO-ZnO/epoxy nanohybrids	Carbon steel/3.5% NaCl	Othman et al. (2020)
13	Zn-based PANI/GO composite	Carbon steel/3.5% NaCl	Xiao et al. (2018)	14	MWCNTs/nano ZnO/epoxy resin	Mild steel/3.5% NaCl	Gujjar et al. (2000)
15	Molybdenum-ZnO quantum dots	Stainless steel/3.5% NaCl	Liu et al. (2020c)	16	Carbon spheres doped with Zn cations	Mild steel/3.5% NaCl	Behgam et al. (2020)
17	Polyurethane/ZnO nanocomposites	Mild steel/3.5% NaCl	Christopher et al. (2015)	18	Polyurethane acrylate/ZnO coating	Mild steel/3.5% NaCl	Ariffin et al. (2020)
19	Nano-ZnO/polyurethane coatings	Carbon steel/3.5% NaCl	Rashvand and Ranjbar (2013)	20	ZnO/poly(lactic acid) nanocomposite	Magnesium (Mg) AZ31 alloy/Biocorrosion	Mousa et al. (2018)
21	Polymer epoxy acrylate/ZnO	Mild steel/3.5% NaCl	Aung et al. (2020)	22	Clay/PPy decorated Ag and ZnO nanoparticles	Mild steel/3.5% NaCl	Jlassi et al. (2020)
23	ZnO-PPy microcomposite	Mild steel/3.5% NaCl	Satpal et al. (2020)	24	PANI-metal oxide-nano-composite	Mild steel/0.1 M HCl	Kumar et al. (2020)
25	PANI/ZnO/glass fiber nanocomposite	Carbon steel/3.5% NaCl	Rouhollahi and Barzegar Khaleghi (2018)	26	ZnO/polyacrylamide nanocomposite	Carbon steel/1 M HCl	Morsi et al. (2016)
27	Poly(glycerol succinate) (PGS)/ZnO, CuO, SnO	Mild steel/0.5 M H₂SO₄	Unnisa et al. (2018)	28	ZnO-poly methyl methacrylate hybrid	Mild steel/3.5% NaCl	Potdar et al. (2020)
29	Epoxy resins/zinc composites	Copper/3% NaCl	Dagdag et al. (2020a,b,c)	30	Epoxy-zinc oxide nanocomposite	316L stainless steel/3.5% NaCl	Ibrahim et al. (2020)
31	Epoxy-ester/Zn kaolin nanocontainer	Carbon steel/3.5% NaCl	Majd et al. (2020)	32	Epoxy Zn-rich composite coating with Zn, Al and FeO	St-37 steel/3.5% NaCl	Ramezanzadeh et al. (2014)
33	Zn phosphate/epoxy coating	Mild steel/3.5% NaCl	Alibakhshi et al. (2018)	34	Zn acetyl acetonate/epoxy-ester polymer	Mild steel/3.5% NaCl	Palimi et al. (2018)
35	Zn-rich epoxy/sulfonated polyaniline	Q235 steel/3.5% NaCl	Yang et al. (2018a,b)	36	Benzotriazole/zinc phosphate	Carbon steel/3.5% NaCl	Banczek et al. (2006)
37	Chitosan/ZnO nanoparticle	Mild steel/0.M HCl	John et al. (2015)	38	Zn-chitosan composite	Mild steel/3.5% NaCl	Vathsala et al. (2010)
39	3-((3-acetylphenyl)imino)indolin-2-one/ZnO	Mild steel/1 M HCl	AL-Mosawi et al. (2021)	40	ECDPA/ZnO nanosheets	Copper/1 M HCl	Ji and Prakash (2019)
41	Mn-MOFs loaded Zn phosphate composite	Mild steel/3.5% NaCl	Chen et al. (2021a,b)

PDMS, polydimethylsiloxane; ECDPA, ethyl-2-cyano-3-(4-(dimethylamino) phenyl) acrylate; MWCNTs, multi-walled carbon nanotubes; GO, graphene oxide.

2.3 SiO₂-based MPFs and MOPFs in corrosion control

Silicon dioxide (SiO₂) or silica most commonly exists as quartz in nature and in numerous living organisms (Duan et al. 1998; Künzelmann and Böttcher 1997; Mallakpour and Naghdi 2018). It is one of the major constituents of sand and it is present in various products such as aerogels, silica gel, fumed silica, and fused quartz. SiO₂ is widely used in making structural materials and microelectronics and constitutes in pharmaceutical and food industries (Duan et al. 1998; Künzelmann and Böttcher 1997). The chemical structure, properties, and application of SiO₂ and its derivatives are discussed elsewhere. SiO₂ is mainly used (almost 95%) for the production of concrete. Various methods of SiO₂ synthesis have been developed however its synthesis using organosilicon compounds is one of the most common and frequently used methods. Some of the common syntheses of SiO₂ are illustrated in the following schemes (Anderson and Bard 1995; Kim et al. 2013; Watanabe et al. 1999; Zhu et al. 2011):

(5) N a 2 S i 3 O 7 + H 2 S O 4 → 3 S i O 2 + N a 2 S O 4 + H 2 O ( F r o m s o d i u m s i l i c a t e )

(6) S i + O 2 → S i O 2 ( T h e r m a l o x i d a t i o n o f S i )

(7) S i + 2 H 2 O → S i O 2 + 2 H 2 ( W e t o x i d a t i o n o f S i )

(8) S i H 4 + 2 O 2 → S i O 2 + 2 H 2 O ( O x i d a t i o n o f s i l a n e )

(9) S i ( O C 2 H 5 ) 4 → S i O 2 + 2 O ( C 2 H 5 ) 2 ( H e a t i n g o f t e t r a e t h y l o r t h o s i l i c a t e ( T E O S )

(10) S i ( O C 2 H 5 ) 4 + 12 O 2 → S i O 2 + 10 H 2 O + 8 C O 2 ( O x i d a t i o n o f T E O S )

(11) S i ( O C 2 H 5 ) 4 + 2 H 2 O → S i O 2 + 4 C H 3 C H 2 O H ( H y d r o l y s i s o f T E O S )

SiO₂ possesses a strong ability of binding with the polymers and organic compounds to form composites that acquire unique anticorrosive properties for various metals and alloys in different electrolytes, especially in the sodium chloride-based electrolytes (El-Din et al. 2021; Gómez-Magallón et al. 2020; Olya et al. 2020; Tavakoli et al. 2019; Xie et al. 2018a,b; Xu et al. 2021). SiO₂ itself and its polymer composites are widely used as self-healing materials in epoxy-based coatings. The presence of SiO₂ enhances the toughness, durability, and effectiveness of the polymer coatings. SiO₂ fills and blocks the surface micropores and cracks of polymer coatings and thereby hinders the diffusion of corrosive species in the polymer matrixes. The SiO₂-based composites can be achieved using various methods similar to the TiO₂-based anticorrosive coatings. Generally, the anticorrosive effect of SiO₂-based polymer composites greatly depends upon the size distribution of SiO₂ and its relative proportion. A high proportion of SiO₂ is associated with high protection effectiveness. Xie et al. (2018a,b) developed a polydimethylsiloxane/silicon dioxide (PDMS/SiO₂) composite coating for AZ31 magnesium alloy to demonstrate the effect of the proportion of 40 nm and 50–250 nm of SiO₂ on wear, wettability, and anticorrosive effect in 3.5% NaCl. The synthesis of the PDMS/SiO₂ composite and its subsequent coating on the AZ31 Mg alloy using the glass slide method is illustrated in Figure 9.

Figure 9:

Diagrammatic illustration of the preparation of f PDMS/SiO₂ super hydrophobic coating on AZ31 Mg alloy (Xie et al. 2018a,b). Reproduced with permission @copyright Elsevier, 2018.

For the preparation of PDMS/SiO₂ super hydrophobic coating, TTFOS were allowed to hydrolyze in ethanol (C₂H₅OH) to form a flurosilane hydroxyl polymer. Meanwhile, the hydroxyl group (–OH) grow on the surface of SiO₂ and enhances its solubility/dispersion ability. It is important to report that PDMS is attached to the SiO₂ surface whereas the organic–inorganic mixture adheres to the AZ31 Mg alloy surface.

Noticeably, SiO₂ mixed with other inorganic oxide and their polymer composites are also widely investigated as anticorrosive coatings. Recently, Abd El-Lateef and Khalaf (2019) developed two Tl₂O₃-SiO₂/polyaniline-based formulations having 5% of Tl₂O₃ (5 T-S/PANI) and 10% of Tl₂O₃ (10 T-S/PANI) and tested them as anticorrosive materials for carbon steel corrosion in 2N HCl solution. The formation and structures of 5 T-S/PANI and 10 T-S/PANI were determined using XRD, UV–vis, FT-IR, EDX, HR-TEM, and DLS methods. Relative corrosion inhibition potential of PANI, 5 T-S/PANI, and 10 T-S/PANI was tested using polarization, EIS, and SEM methods. Using these methods, the inhibition efficiencies of tested species followed the sequence: PANI < 5 T-S/PANI < 10 T-S/PANI. Potentiodynamic polarization study indicated that in the presence of PANI, 5 T-S/PANI, and 10 T-S/PANI in the 2 N HCl solution, the nature of polarization (anodic and cathodic) curves changes greatly indicating that they exert a significant effect on anodic and cathodic Tafel reactions. A significant decrease in the values of current density (i _corr) was observed in the presence of PANI, 5 T-S/PANI, and 10 T-S/PANI. This observation indicated that PANI, 5 T-S/PANI, and 10 T-S/PANI become effective by adsorbing on the metal surface thereby blocking the active sites.

An electrochemical impedance spectroscope (EIS) study was also conducted to furnish the corrosion inhibition potential of PANI, 5 T-S/PANI, and 10 T-S/PANI for carbon steel in 2 N HCl solution (Figure 10). The Nyquist curves in all situations furnish a single semicircle indicating that carbon steel corrosion in 2N HCl with and without PANI, 5 T-S/PANI, and 10 T-S/PANI involve the single charge transfer process. This observation was further supported by single maxima in the Bode phase angle curves. The increase in the diameter of Nyquist curves in the presence of PANI, 5 T-S/PANI, and 10 T-S/PANI and the rise in their concentration indicated that magnitudes of charge transfer resistance follow the same sequence. This observation also suggests that PANI, 5 T-S/PANI, and 10 T-S/PANI act as interface-type corrosion inhibitors.

Figure 10:

Nyquist curves for carbon steel corrosion in 2 N HCl in the absence and presence of different (10–150 ppm) concentrations of (a) PANI, (b) 5 T-S/PANI, and (c) 10 T-S/PANI (Abd El-Lateef and Khalaf 2019). Reproduced with permission @copyright Elsevier, 2019.

Literature study suggests that various other polymer composites of SiO₂ are tested as anticorrosive coating materials. The structure and morphology of SiO₂-based polymer composites are characterized using various surface monitoring techniques using XRD, XPS, UV–vis, FT-IR, Raman, EDX, HR-TEM, and DLS methods. A summary of the nature of SiO₂-based polymer composites such as polyaniline, polypyrrole, polyamide, poly(urea−formaldehyde), etc., metal/alloy, and electrolyte of some major reports are illustrated in Table 3.

Table 3:

Summary of some major reports on SiO₂-based MPFs and MOPFs as anticorrosive formulations for different metals/electrolyte systems.

S/N	Nature of composite	Metal/electrolyte	References	S/N	Nature of composite	Metal/electrolyte	References
1	PDMS/SiO₂ superhydrophobic coatings	AZ31 magnesium alloys/3.5% NaCl	Xie et al. (2018a,b)	2	Tl₂O₃-SiO₂/polyaniline nanocomposites	Carbon steel/0.1 M NaCl	Abd El-Lateef and Khalaf (2019)
3	Nano-SiO₂-polyaniline (PANI)	Carbon steel/3.5% NaCl	Cruz et al. (2019)	4	Polyaniline-SiO₂- coating	Mg-Li alloy/3% NaCl	Chen et al. (2010)
5	Polyaniline (PANI)/modified SiO₂ coatings	Q235 carbon steel/0.1 M H₂SO₄	Shi et al. (2017)	6	Polyaniline–SiO₂ composite	Mild steel/1 M HCl	Kumar et al. (2013)
7	Poly(aniline-co-phenetidine)/SiO₂ composites	Mild steel/3.5% NaCl	Sambyal et al. (2016)	8	HPC-PANI/SIO₂/poly(vinyl acetate)	Mild steel/3.5% NaCl and 1 M HCl	Khademian et al. (2015)
9	Poly(aniline-anisidine)/chitosan/SiO₂ composite	Mild steel/3.5% NaCl	Sambyal et al. (2018a)	10	Poly(2,3-dimethylaniline) modified by nano-SiO₂	SS steel/3.5% NaCl	Ma et al. (2014)
11	Poly(o-anisidine)-SiO₂ nanocomposites	Mild steel/3.5% NaCl	Rajkumar and Vedhi (2020)	12	Poly (o-phenitidine)/SiO₂/Epoxy coating	Mild steel/3.5% NaCl	Sambyal et al. (2018b)
13	Polyp-phenylendiamine-SiO₂ nanocomposite (PSC)	Carbon steel/1.0 M HCl	Emamgholizadeh et al. (2015a,b)	14	Polypyrrole/SiO₂ composite	Mild steel/3.5% NaCl	Ruhi et al. (2014)
15	Chitosan-polypyrrole-SiO₂ composite	Mild steel/3.5% NaCl	Ruhi et al. (2015)	16	Polyimide/SiO₂ composites	Cold-rolled steel (CRS)/3.5% NaCl	Chou et al. (2014)
17	Poly(urea−formaldehyde)/SiO₂	Steel/3.5% NaCl	Li et al. (2019a,b)	18	(HL)/epoxy/SiO₂ nanocomposite	Carbon steel/5% NaCl	Fadl et al. (2020b)
19	EP/PpPDA and EP/PpPDA/SiO₂ nanocomposite	Carbon steel/1.0 M HCl	Emamgholizadeh et al. (2015a,b)	20	SiO₂-PMMA composite	SS steel/3.5% NaCl	Kumar et al. (2015)
21	g-C3N4@SiO₂ and g-C3N4@SiO₂/epoxy	Mild steel/3.5% NaCl	Xia et al. (2020)	22	SiO₂/polydimethylsiloxane films	Mild steel/3.5% NaCl	Zhang et al. (2020a,b,c)
23	Polyglycerol-decorated Fe3O4@SiO₂	Mild steel/1.0 M HCl	Amiri et al. (2020)	24	SB metal complex/SiO₂ hybrid epoxy nanocomposite	Carbon steel/5% NaCl	Fadl et al. (2019)
25	SiO₂-GO/epoxy composite coating	Mild steel/3.5% NaCl	Ramezanzadeh et al. (2016)	26	ZnO/SiO₂/epoxy coatings	Mild steel/3.5% NaCl	Abdus Samad et al. (2020)
27	SiO₂/fluorine-containing epoxy coatings	Carbon steel/3.5% NaCl	Liu et al. (2017)	28	Graphene@SiO₂ composites	Copper sheet/3.5% NaCl and 1 M HCl	Sun et al. (2015)
29	F-SiO₂@PDMS composite	Aluminum sheet/3.5% NaCl	Shen et al. (2021)	30	SiO₂-GO nanohybrids/epoxy	Mild steel/3.5% NaCl	Pourhashem et al. (2017)
31	TMES-modified SiO₂ composite	Aluminum alloy/3.5% NaCl	Tong et al. (2020)	32	Polybenzoxazine/SiO₂ nanocomposite	Mild steel/1 M HCl	Zhou et al. (2014)

HL, p-phenylamine-N(4-chloro salicylaldenemine); SB, Schiff base; F-SiO₂, fluorinated silica; PDMS, polydimethylsiloxane; CRS, cold-rolled steel; TTFOS or C₈F₁₃H₄Si(OCH₂CH₃, Triethoxy-1H,1H,2H,2H-tridecafluoro-n-octylsilane).

2.4 Ag/Au-based MPFs and MOPFs in corrosion control

Silver is a chemical element, illustrated by Ag, having atomic number 47. Ag is a white, soft, and lustrous transition metal element that possesses the highest thermal and electrical conductivity. Ag may be found in pure and alloy forms. Most of the commercially useful silver is derived as the byproduct of zinc, copper, lead, and gold refining (Lansdown 2002). On the other hand, gold which is presented by Au is a reddish yellowish, soft, ductile, and malleable transitional element metal. Similar to Ag, the Au may be present either in pure or combined form. Both Ag and Au possess a strong tendency of forming complexes/composites with organic compounds and polymers. The Ag and Au composites are extensively used for various industrial and biological applications (Bayat et al. 2015; Navratil and Kopanica 2002; Palanisamy et al. 2016; Sabury et al. 2015; Wu et al. 2012). These composites have also been used as anticorrosive materials in the coating as well as in the solution phase (Atta et al. 2014; Badr et al. 2020; El-Faham et al. 2018; Ituen et al. 2021c; Patil et al. 2019; Saugo et al. 2015; Solomon and Umoren 2016; Thulasi et al. 2021; Venkateswarlu et al. 2012). In the polymer coating, the Ag and Au metals act as nanofillers and they fill the surface micropores and cracks present in the polymer coatings. Thereby, they avoid the penetration and leakage of corrosive species such as moisture and salt solution. Therefore, in the polymer coatings, the Ag and Au metals enhance their durability as well as anticorrosive effectiveness. Unlike most of the other metal-polymer composites, Ag and Au-based composites/nanocomposites are widely used as anticorrosive materials in the solution phase.

Hefni and coworkers (Hefni et al. 2016) reported the corrosion inhibition potential of chitosan (Ch) grafted on PEG (polyethylene glycol) (Ch-g-mPEG) and its silver nanocomposite for carbon steel in 1 M HCl using various methods. The composite was characterized using numerous methods. Through electrochemical analyses, it was derived that Ch-g-PEG/AgNPs exhibit a higher anticorrosive effect as compared to the Ch-g-PEG. Both Ch-g-PEG and Ch-g-PEG/AgNPs act as mixed-type corrosion inhibitors with slight cathodic predominance. In another investigation, the corrosion mitigating potential of poly(methacrylic acid)/silver nanocomposites (PMAA/AgNPs) was demonstrated for mild steel in 0.5 M H₂SO₄ solution (Solomon et al. 2015a,b). The characterization of the composite was achieved using TEM, EDX, XRD, FT-IR, and UV–vis spectroscope methods. Electrochemical measurements suggest that PMAA/AgNPs behave as mixed-type corrosion inhibitors and their adsorption on metal surfaces follows the Temkin adsorption isotherm model. PMAA/AgNPs exhibit the highest efficiency of 76.7% at 1000 ppm concentration. Using SEM and EDX methods it was observed that PMAA/AgNPs become effective by adsorbing on the metallic surface thereby forming the surface protective film. Results clearly show that the metallic surface greatly smoothened in the presence of PMAA/AgNPs as compared to in its absence. This observation indicates that PMAA/AgNPs form surface protective film through their adsorption. Change in the composition of elements present over the metallic surface observed through EDX analysis also validates this conclusion.

Recently, Ituen et al. (2021a) described the relative corrosion inhibition potential of red onion peels extract, illustrated as AROPE (1000 ppm), and its silver composite (AqAgNPs) for X80 steel in 1 M HCl solution. Electrochemical demonstrations suggest that AROPE and AqAgNPs act as excellent corrosion inhibitors. It was also derived that the presence of 15 and 25% of AqAgNPs in the AROPE enhances its corrosion protection effectively. The AROPE, 15% AqAgNPs and 25% AqAgNPs exhibit the highest protection efficiencies of 63.7, 81.9 and 87.8%, respectively. AROPE, 15% AqAgNPs, and 25% AqAgNPs act as mixed-type inhibitors with some anodic domino effect.

The increase in the diameter of Nyquist curves in the presence of AROPE, 15% AqAgNPs, and 25% AqAgNPs than that of their absence indicates that AROPE, 15% AqAgNPs, and 25% AqAgNPs act as interface-type corrosion inhibitors i.e. they become effective by adsorbing at the interface of metal and electrolyte. This conclusion was supported by SEM, EDX, and AFM analyses where a significant improvement in the surface morphology of protected metallic specimens was observed in the presence of AROPE and AqAgNPs. SEM, AFM (2D and 3D), and EDX spectra of X80 surface in various situations are presented in Figure 11. The corrosion inhibition potential of other silver composites has also been reported extensively. Reports on the anticorrosive effect of Ag and Au composites for different metals and alloys in various electrolytes are summarized in Table 4.

Figure 11:

SEM (uppermost), AFM [middle (Fetouh et al. 2020); upper 3D and lower 2D] and EDX (lowermost spectra of mild steel surface (a) corroded in 1 M HCl without inhibitors, (b) corroded in 1 M HCl in the presence of AROPE, and (c) corroded in 1 M HCl in the presence of AqAgNPs (Ituen et al. 2021a). Open access publication, copyright permission not required.

Table 4:

Summary of some major reports on Ag/Au-based MPFs and MOPFs as anticorrosive formulations for different metals/electrolyte systems.

S/N	Nature of composite	Metal/electrolyte	References	S/N	Nature of composite	Metal/electrolyte	References
1	Chitosan-g-PEG assembled Ag nanoparticles (Ch-g-(PEG/AgNPs)	Carbon steel/1 M HCl	Hefni et al. (2016)	2	Poly(methacrylic acid)/silver nanocomposites (PMAA/AgNPs)	Mild steel/0.5 M H₂SO₄	Solomon et al. (2015a,b)
3	Biomass-mediated Ag nanoparticles (AqAgNPs)	X80 steel/1 M HCl	Ituen et al. (2021a)	4	Silver-polyurea nanocomposite	ASTM A194 steel/3.5% NaCl	Beiki and Mosavi (2020)
5	Gum Arabic-silver nanocomposite (GA-AgNPs)	St37 steel/15% HCl and 15% H₂SO₄	Solomon et al. (2018)	6	Chitosan-silver nanoparticles (AgNPs-Chi)	St37 steel/15% H₂SO₄	Solomon et al. (2017a)
7	Chitosan/silver nanoparticles (AgNPs/chitosan)	St37 steel/15% HCl	Solomon et al. (2017b)	8	GO/silver nanostructure	X60 steel/microbial corrosion	Taghavi Kalajahi et al. (2021)
9	Poly (methacrylic acid)/silver nanocomposite	Aluminum/0.5 M H₂SO₄	Solomon and Umoren (2015)	10	Cysteine-silver-gold nanocomposite (Cys/Ag-Au NCz)	Mild steel/1 M HCl	Basik et al. (2020)
11	Polypropylene glycol-silver nanocomposites (PPG/AgNPs)	Aluminum/0.5 M H₂SO₄	Solomon et al. (2015a,b)	12	Allium cepa peels extract-silver nanocomposite (Et-AgNPs)	X80 steel/1 M HCl	Ituen et al. (2021b)
13	Polyvinyl alcohol (PVA) and Ag nanoparticles (nAg/PVA)	Copper/0.1 M HCl	Grecu et al. (2019)	14	Chitosan-silver nanocomposite (SNPs-CT NC)	Mil steel/chilled water circuits	Fetouh et al. (2020)
15	Elaeis guineensis/silver nanoparticles (EG/AgNPs)	Carbon steel/seawater	Asaad et al. (2018)	16	pPoly(ethylene glycol)thiol (PEGSH-AgNPs) and poly(vinyl pyrrolidone) (PVP/PEGSH-AgNPs)	Carbon steel/1 M HCl	Atta et al. (2013)
17	Graphene oxide/chitosan/silver NPs (AgNPs/GO/CS)	Stainless steel utensils/universal buffer (pH = 11)	Bioumy et al. (2020)	18	GO-chitosan-silver composite coating	Cu–Ni specimens/3.5 wt% NaCl	Jena et al. (2020)
19	Silver-polyaniline nanoparticles (PANI-AgNPs)	6061 aluminum alloy/1 M HCl	Badi et al. (2020)	20	Polyvinyl alcohol- silver nanoparticles (PVA/nAg)	304L stainless steel/0.1 M HCl	Samide et al. (2019)

2.5 CeO₂-based MPFs and MOPFs in corrosion control

Cerium (IV) oxide, CeO₂ is also known as ceric dioxide, ceric oxide, cerium oxide, cerium dioxide, and ceria, which is a pale yellow–white powder (Caixiang et al. 2008; Korotcenkov 2019). Cerium oxide naturally occurs in combination with other rare-earth elements, especially in monazite and bastnesite ores. CeO₂ is widely used in catalysis, polishing, decolorizing glass, welding, and various biomedical applications. CeO₂ possesses a strong affinity to binding with polymer matrix and organic compounds, through coordination bonding, to form various industrially and biologically useful composites (Lara-López et al. 2017; Parvatikar et al. 2006; Phokha et al. 2018). These composites have also been extensively studied as anticorrosive materials in aqueous as well as coating conditions (Gong et al. 2021; González et al. 2021; Habib et al. 2020; Nassaj et al. 2020; Qian et al. 2021; Rahman et al. 2020; Wu et al. 2021). Similar to the other metal oxides, including TiO₂ and ZnO, CeO₂ also acquires self-healing properties in the polymer coatings. The presence of CeO₂ in the polymer coatings increases their protection performance as well as durability. CeO₂ molecules fill the micropores and cracks produced by the rupturing of the metallic coatings. Thereby, they avoid the penetration or leakage of corrosive species inside the coating matrix. Using the AFM technique, Eduok et al. (2017a) showed that in the presence of CeO₂, epoxy-silica (SG) coating remains unaffected even after immersion in the highly aggressive electrolyte of 0.6 wt% NaCl + 0.6 wt% (NH₄)₂SO₄ for two weeks (Figure 12).

Figure 12:

AFM images of mild steel surface corroded in 0.6 wt% NaCl + 0.6 wt% (NH₄)₂SO₄ for two weeks (a) coated with epoxy-silica (SG) with 1 wt% CeO₂ and (b), (c) coated with epoxy-silica (SG) without CeO₂ (Eduok et al. 2017a). Reproduced with permission @copyright Elsevier, 2017.

Careful observation of Figure 12 suggests that coating structures are highly damaged in the absence of CeO₂ as the surface contains various cracks-like appearances. On the other hand, in the presence of CeO₂ coating structure remains highly smoothened and relatively less damaged. In the polymer coatings, CeO₂ molecules uniformly distribute and provide excellent self-healing properties. Ramezanzadeh and coworkers (Ramezanzadeh et al. 2018) recently developed a graphene oxide (GO), polyaniline (PANI), and CeO₂-based epoxy coating, designated as GO-PAni-CeO₂/epoxy, for corrosion protection of mild steel in 3.5% NaCl. It can be seen clearly that CeO₂ molecules are uniformly distributed in the polymer matrix of GO-PAni. The GO-PAni-CeO₂ composite was incorporated into the epoxy coatings. Through EIS analysis, it was derived that GO-PAni-CeO₂/epoxy-based coatings exhibit remarkably high anticorrosive activities as compared to the neat epoxy coatings. The corrosion protection of neat epoxy, as well as GO-PAni-CeO₂/epoxy coatings, was tested at different time intervals (2–48 h). The anti-corrosive activity of neat epoxy and GO-PAni-CeO₂/epoxy coatings decreases with time. A similar observation was also observed while investigating the anticorrosive effect of CeO₂/PU, CNTs/PU, PDA-CNTs/PU, and CeO₂-CNTs/PU coatings for AA7075 Al alloy in 3.5% NaCl (Cai et al. 2021).

Literature investigation suggests that CeO₂-based organic compound/polymer composites are widely used as anticorrosive materials (Cai et al. 2021; Hasannejad and Molavi 2014; Hasanzadeh et al. 2015; Hosseini and Aboutalebi 2018, 2019; Kumar et al. 2017; Lei et al. 2020; Li et al. 2015, 2019a,b, 2020; Liu et al. 2018b, 2020a,b,c, 2021a,b; Shetty et al. 2020; Zhang et al. 2020a,b,c). Their characterization has been achieved using various techniques including SEM, TEM, AFM, EDX, XRD, XPS, Raman, UV–Vis, and FT-IR. They are mostly tested as anticorrosive coating formulations. However, few reports on the anticorrosive effect of CeO₂-based composites in aqueous electrolytes have also been investigated. Eduok et al. (2017c) studied the inhibition potential of the ceria/acrylic polymer composite (PAA/CeO₂) for API 5L X70 steel corrosion in 0.5 M HCl using numerous methods. An electrochemical polarization study indicates that PAA/CeO₂ acts as an effective corrosion inhibitor and its presence adversely affects the overall Tafel reaction. PAA/CeO₂ acts as a mixed type inhibitor as its presence does not cause any appreciable shift in the E _corr values. Using PDP and EIS methods, it was established that the anticorrosive property of PAA/CeO₂ increase by increasing the proportion of CeO₂ as PAA/CeO₂ containing 1 wt% CeO₂ exhibits the lowest inhibition efficiency and PAA/CeO₂ containing 5 wt% CeO₂ exhibits the highest efficiency. EIS study further suggests that API 5L X70 steel corrosion in 0.5 M HCl with and without PAA/CeO₂ involves the single charge transfer mechanism and an increase in the diameter of Nyquist curves in the presence of PAA/CeO₂ is due to an increase in the value of charge transfer process. This observation indicates that PAA/CeO₂ behaves as an interface-type inhibitor and it becomes effective by adsorbing on the metal surface.

The adsorption mechanism of corrosion inhibition using PAA/CeO₂ was also investigated by SEM analysis. SEM images of polished and corroded API 5L X70 steel with and without PAA/CeO₂ showed that the morphology of polished API 5L X70 steel was highly smooth without any significant corroded and damaged areas. However, after immersing the metal surface in 0.M HCl it becomes highly damaged and corroded due to free acidic aggressive attacks. In the presence of PAA/CeO₂, especially with 5.0 wt% CeO₂, metal surface morphologies were significantly improved. This observation indicated that PAA/CeO₂ becomes effective by adsorbing on the metal surface. A similar observation has also been reported elsewhere (Eduok et al. 2017b; Sasikumar et al. 2015; Umoren and Madhankumar 2016). A summary of the nature of CeO₂/polymer composites used as anticorrosive materials, metal/alloy, and electrolyte is given in Table 5.

Table 5:

Summary of some major reports on CeO₂-based MPFs and MOPFs as anticorrosive formulations for different metals/electrolyte systems.

S/N	Nature of composite	Metal/electrolyte	References	S/N	Nature of composite	Metal/electrolyte	References
1	Epoxy-silica/CeO₂	Mild steel/0.6 wt% NaCl + 0.6 wt% (NH₄)₂SO₄	Eduok et al. (2017a)	2	GO/epoxy and GO-PAni-CeO₂/epoxy	Mild steel/3.5% NaCl	Ramezanzadeh et al. (2018)
3	CeO₂/PU, CNTs/PU, PDA-CNTs/PU and CeO₂-CNTs/PU	AA7075 aluminum alloy/3.5% NaCl	Cai et al. (2021)	4	CeO₂/organic silicon epoxy (EP)/PVDF	Q235 low carbon steel/3.5% NaCl	Zhang et al. (2020a,b,c)
5	Urea-formaldehyde microcapsules/CeO₂	Carbon steel/0.5 m HCl	Hasanzadeh et al. (2015)	6	Waterborne acrylic/CeO₂ composite coating	Carbon steel/3.5% NaCl	Li et al. (2015)
7	CHIT, CHIT-CE, and CeO₂-CHIT-CE	AA5083-H321 (aluminum)/3.5% NaCl	Hasannejad and Molavi (2014)	8	CeO₂@PANI@MBT and EP/CeO₂@PANI@MBT	Mild steel/3.5% NaCl	Hosseini and Aboutalebi (2019)
9	Gr, CeO_2, and Gr(3%)-P-CeO₂	Carbon steel/3.5% NaCl	Li et al. (2020)	10	Stearic acid (SA)/CeO₂ bilayer coating	AZ31B magnesium alloy/3.5% NaCl	Liu et al. (2020a,b,c)
11	Polyaniline (PANI)/CeO₂ in alkyd coating	Carbon steel/3.5% NaCl	Li et al. (2019a,b)	12	Epoxy coatings/imidazole modified CeO₂	Mild steel/3.5% NaCl	Hosseini and Aboutalebi (2018)
13	CeO₂-GO/EP nanocomposite coating	Q235 carbon steel/simulated seawater	Liu et al. (2021b)	14	Polyaniline (PANI)/cerium dioxide(CeO₂)	Steel 316/0.25 M HCl	Shetty et al. (2020)
15	EP-GO and EP/CeO₂-GO	Q235 carbon steel/simulated concrete pore solution	Liu et al. (2021a)	16	EP/CeO₂ nanocontainers	Carbon steel/0.5MNaCl	Liu et al. (2018b)
17	Polypyrrole-CeO₂ nanocomposite	AA2024 alloy/0.6 M NaCl	Kumar et al. (2017)	18	Polyaniline/CeO₂ nanocomposites	Carbon steel/3.5% NaCl	Lei et al. (2020)
19	Ceria/acrylic polymer composite	API 5L X70 steel/0.5 M HCl	Eduok et al. (2017c)	20	Aniline(PANI)/CeO₂ nanoparticles	Mild steel/0.5 M HCl	Sasikumar et al. (2015)
21	Chitosanic hydrogel/nano-CeO₂	API 5L X70 steel/4% NaCl (pH = 1.5)	Eduok et al. (2017b)	22	Pectin-CeO₂ mixtures	X60 steel/0.5 M HCl	Umoren and Madhankumar (2016)

PDA, polydopamine; CNTs, carbon nanotubes; AA, acrylic acid; AAP, acrylic acid polymer; PVDF, poly (vinylidene fluoride); CHIT, chitosan; CE, cerium (III) ion; MBT, mercaptobenzotiazole; EP, epoxy; PU, polyurethane; Gr, graphene; Gr-P, graphene-based acrylic coating; SA, stearic acid.

3 Concluding remarks: challenges and future prospects

Metal-polymer frameworks (MPFs) and metal oxide polymer frameworks (MOPFs) are widely used for biological and industrial applications. The MPFs and MOPFs possess strong anticorrosive properties in both aqueous phases as well as in coating conditions. One of the biggest challenges of using these materials in aqueous solutions is their limited solubility. They are mostly used as fillers in polymer-based coating formulations. Their dispersity in the aqueous phase and subsequent consumption can be enhanced by chemical modification such as attachment of the polar functional groups. Therefore, future studies should be focused on designing and synthesis relatively more soluble MPFs and MOPFs. More so, most of these materials and their syntheses are highly expensive and eco-friendly as they are synthesized by traditional hot-plat heating methods. Therefore, in future studies, MPFs and MOPFs derived from nontraditional heatings such as microwave (MW) and ultrasound (US) should be explored. Another area where research on the anticorrosive effect of MPFs and MOPFs should be focused is the implementation of nonferrous metals and alloys as literature investigation suggests that in most of the studies, MPFs and MOPFs are mainly tested as anticorrosive materials for ferrous alloys. More so, the MPFs and MOPFs are mainly employed as anticorrosive materials for sodium chloride solutions. Therefore, the use of MPFs and MOPFs as anticorrosive materials should also be explored for other media, especially in basic electrolytes e.g. NaOH and NH₄OH. In the solution phase, the presence of metal and metal oxide is supposed to enhance the adsorption tendency of organic/polymer compounds. However, in the organic/polymer coatings, their role is entirely different. In such coatings, Ms and MOs are expected to fill and block the micropores and cracks thereby they avoid the penetration of corrosive species such as salts, oxygen, moisture and gases. We herein describe the corrosion inhibition potential of TiO₂, SiO₂, ZnO, CeO_2, and Ag/Au organic/polymer composites.

Corresponding authors: Chandrabhan Verma, Center of Research Excellence in Corrosion, Research Institute, King Fahd University of Petroleum and Minerals, Dhahran 31261, Saudi Arabia, E-mail: chandraverma.rs.apc@itbhu.ac.in; and Kyong Yop Rhee, Department of Mechanical Engineering (BK21 four), College of Engineering, Kyung Hee University, Yongin, Republic of Korea, E-mail: rheeky@khu.ac.kr

About the authors

Chandrabhan Verma

Chandrabhan Verma works at the IRC for Advanced Materials, KFUPM, Dhahran, 31261, Saudi Arabia. He is a member of the American Chemical Society (ACS). His research is mainly focused on the synthesis and designing of environmentally-friendly corrosion inhibitors useful for several industrial applications. Dr. Verma is the author of several research and review articles and has edited many books. He has a total citation of more than 8200. Dr. Verma has received many awards.

Chaudhery Mustansar Hussain

Chaudhery Mustansar Hussain, PhD, is an adjunct professor and director of laboratories in the Department of Chemistry and Environmental Sciences at the New Jersey Institute of Technology, Newark, NJ, USA. His research is focused on the applications of nanotechnology and advanced materials, environmental management, analytical chemistry, and other various industries. Dr. Hussain is the author of numerous papers in peer-reviewed journals as well as a prolific author and editor of around 100 books.

Mumtaz A. Quraishi

Dr. Mumtaz A. Quraishi is a Chair Professor at IRC for Advanced Materials, KFUPM, Saudi Arabia. Before joining KFUPM, he was an Institute Professor at IIT-BHU, Varanasi, India. He also served as Head of Department of Chemistry at IIT-BHU. He has teaching experience of more than 35 years. He has published more than 400 papers having a total citation rate of more than 30000. He has also authored and edited many books.

Kyong Yop Rhee

Dr. Kyong Yop Rhee is a professor of Mechanical Engineering at Kyung Hee University (South Korea) since 1999. His main research interests are nanocomposites, surface treatment, fracture, and composite materials. He has published more than 451 scientific papers and has led 67 R&D projects. He earned his BS and MS degrees in Mechanical Engineering from Seoul National University (South Korea). He earned his PhD in Mechanical Engineering at the Georgia Institute of Technology.

Author contribution: All the authors collectively wrote and contributed to the entire manuscript and have agreed to its publication.
Research funding: None declared.
Conflict of interest statement: 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.

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Received: 2022-06-29

Accepted: 2022-10-25

Published Online: 2022-12-21

Published in Print: 2024-01-29

This work is licensed under the Creative Commons Attribution 4.0 International License.

Metals and metal oxides polymer frameworks as advanced anticorrosive materials: design, performance, and future direction

Abstract

1 Introduction

1.1 Corrosion: basics and a journey corrosion control

1.2 Metals and metal oxides polymer frameworks (MPFs/MOPFs): fundamental and corrosion inhibition properties

2 Corrosion control using MPFs and MOFs: literature survey

2.1 TiO₂-based MPFs and MOPFs in corrosion control

2.2 ZnO-based MPFs and MOPFs in corrosion control

2.3 SiO₂-based MPFs and MOPFs in corrosion control

2.4 Ag/Au-based MPFs and MOPFs in corrosion control

2.5 CeO₂-based MPFs and MOPFs in corrosion control

3 Concluding remarks: challenges and future prospects

About the authors

References

Journal and Issue

Articles in the same Issue

Metals and metal oxides polymer frameworks as advanced anticorrosive materials: design, performance, and future direction

Abstract

1 Introduction

1.1 Corrosion: basics and a journey corrosion control

1.2 Metals and metal oxides polymer frameworks (MPFs/MOPFs): fundamental and corrosion inhibition properties

2 Corrosion control using MPFs and MOFs: literature survey

2.1 TiO2-based MPFs and MOPFs in corrosion control

2.2 ZnO-based MPFs and MOPFs in corrosion control

2.3 SiO2-based MPFs and MOPFs in corrosion control

2.4 Ag/Au-based MPFs and MOPFs in corrosion control

2.5 CeO2-based MPFs and MOPFs in corrosion control

3 Concluding remarks: challenges and future prospects

About the authors

References

Journal and Issue

Articles in the same Issue

2.1 TiO₂-based MPFs and MOPFs in corrosion control

2.3 SiO₂-based MPFs and MOPFs in corrosion control

2.5 CeO₂-based MPFs and MOPFs in corrosion control