Home Comprehensive investigation of corrosion resistance of magnesium–titanium, aluminum, and aluminum–vanadium alloys in dilute electrolytes under zero-applied potential conditions
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Comprehensive investigation of corrosion resistance of magnesium–titanium, aluminum, and aluminum–vanadium alloys in dilute electrolytes under zero-applied potential conditions

  • Roland Tolulope Loto EMAIL logo , Joshua Olusegun Okeniyi , Morounfoluwa John , Christopher Chintua Enweremadu , Ayomide Oluwaseyi Olaolorun , Daniel Ikhionose Igenuma , David Ayobami Sonde , Emmanuel Eberechukwu Achonwa , Afolami Erastus Fanifosi and Tobechukwu Bravohenshaw Okoroji
Published/Copyright: April 16, 2025
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Open Engineering
From the journal Open Engineering Volume 15 Issue 1

Abstract

MgTi alloy exhibited the highest corrosion values (0.242–6.081 mm/year) in H2SO4 compared to values obtained for Al4032, Al4004, and AlV alloys which varied from 0.270 to 1.795, 0.233 to 2.002, and −0.125 to 3.779 mm/year. The plot configuration of MgTi and other alloys showed a decrease in corrosion values with respect to exposure time. Corrosion of MgTi, Al4032, Al4004, and AlV in NaCl were significantly lower compared to H2SO4. The highest corrosion rate occurred at 0.5% NaCl and the lowest at 4.5% NaCl. MgTi alloy exhibited the highest corrosion rate with the optimal value from 0.180 to 0.794 mm/year compared to Al4032 (−0.141 and −0.458 mm/year). The corrosion rate of the alloys in acid–chloride is visibly higher compared to NaCl but significantly lower than H2SO4. MgTi exhibits the most electronegative open circuit potentials (OCPs) in acid, NaCl, and acid–chloride solution with final potential values of −1.591 and −0.233 V from 0.00625 M H2SO4 and 0.1 M H2SO4, −1.631 and −1.542 V from 0.5 and 4.5% NaCl, and −1.598 and −1.576 V from acid–chloride solution. Al4032 displayed the most electropositive OCPs at −0.464 and 2.418 V from H2SO4 and 2.710 and −0.650 V from NaCl solution. Optical microscopy shows MgTi and Al4004 depicting morphological degradation over its surface. Al4032 shows extensive localized deterioration while AlV depicts flake-like deterioration. Extensive morphological deterioration is visible on MgTi, Al4032, Al4004, and AlV alloys from the acid, chloride, and acid–chloride solution. The degree and type of deterioration vary with the electrolyte, electrolyte concentration, and metallurgical properties of the alloys.

Keywords: corrosion; magnesium; aluminum; acid; chloride; pitting

1 Introduction

Aluminium (Al) makes up over 8% of the Earth’s crust. The industrial significance of the metal is second to ferrous alloys due to its exceptional engineering properties such as its heat and electrical conductivity, high- and low-temperature stability, reflectivity, non-toxicity, specific strength, weldability, toughness, corrosion resistance, formability, impact strength, reusability, strength to density ratio and density to weight fraction [1,2]. The Al industry is worth about $174 billion in the United States [3]. Al-based alloys are used in the manufacture of parts and components for automobile, electricity generation, chemical production, marine and aeronautical industries, etc. [4,5,6,7]. The mechanical, heat, and electrical properties of Al can be adjusted to fulfill the requisite demand of industrial applications, e.g., the automobile and aerospace industries utilize Al due to its high strength-to-weight ratio and high-temperature stability [8]. Corrosion of Al significantly reduces its mechanical strength leading to cracks, pits, and fracture prior to failure. Pure Al is reasonably resistant to corrosion due to the formation of a continuous invisible oxide in most environments [9]. However, their structural strength is lower than their alloyed counterparts. The presence of alloying elements invariably increases their vulnerability to corrosion [10,11,12,13,14]. The corrosion resistance properties of Al-based alloys have been of utmost importance due to the evolution of complex technologies for application in demanding environments. Al surface exhibits amphoteric properties and its oxide deteriorates at certain concentrations of Cl−, SO 4 2 − , NO 3 − anions, etc. [15,16,17,18,19]. Previous research has theorized the breakdown of the protective oxide on Al in the presence of corrosive anions. Some research concluded that corrosive anions are responsible for the dissolution of the oxide due to the formation of metallic precipitates [20,21]. Solange et al. [22] stated that corrosion of Al alloys is associated with the intermetallic second phase and composition. Results of Al corrosion in HCl, HNO3, H2SO4, and H3PO4 solutions show that an increase in corrosion rate is proportional to solution concentration and temperature [23]. A study on the corrosion resistance of Al-based galvanic anodes in Cl− and SO 4 2 − indicates pitting potential lowers with an increase in Cl− anion concentration while SO 4 2 − exhibits a passivating effect [24]. Investigation by Oya et al. [25] shows that the pitting potential of Al becomes more noble with an increase in sulfate and sulfite concentrations. Wu and Wu analyzed the effect of SO 4 2 − ions on the corrosion of AA7075 alloy in a chloride solution [26]. Other causative factors responsible for Al corrosion to specific degrees are temperature, alloying elements mechanical properties, cost, availability, maintainability, compatibility with other system components, operating lifetime, reliability, appearance, and appropriate materials selection.

Materials selection for applications in corrosive environments is a key factor in Al corrosion control strategy. Other metallic alloys have been utilized in some applications where Al and ferrous alloys have been primarily used. Medically, magnesium (Mg) and Mg alloys have received attention for orthopedic and cardiovascular implant applications due to their corrosion resistance [27]. Mg alloys are also extensively used in the automobile industry due to their low density and high strength-to-weight ratio. However, they are prone to corrosion due to the formation of intermetallic phases with other alloying elements which have higher free corrosion potential than the Mg substrate [28,29,30]. Titanium (Ti) and its alloys have seen extensive application recently in the automobile industry [31,32]. They are used as bio-compatible materials in mechanical applications due to their high corrosion resistance and high fatigue strength. MgTi composite combines the bioactivity of Mg and the good mechanical properties of Ti. MgTi alloy improves the osseointegration property of Ti and improves the structural problem of Mg implants. They cannot be fabricated by powder metallurgy method due to differences in solubility of the alloys and their melting points [33,34,35]. However, they can be alloyed together by non-equilibrium processes [36–42]. Previous research on the influence of Ti content on the mechanical properties of MgTi composites by powder metallurgy shows a slight decrease in yield strength and a significant increase in ductility with an increase in Ti content [43]. Mg and Ti were used to fabricate functionally graded materials at specific weight ratios for quasi-isotropic compression waves in dynamic high-pressure technology. Results show full density was achieved with a sintering temperature of 560°C up to 75 wt% Ti, with the materials being physical mixtures of Mg and Ti [44]. Al alloys with vanadium (V) content have recently been utilized as structural components of vehicles. This is due to their ability to absorb kinetic energy, an important feature when evaluating the properties of vehicle components subjected to strong deformation. Al-V master alloys are used as reducing agents and additives in the metallurgical industry. The alloy is employed for high-temperature alloy applications and super Ti alloy productions [45]. They act as intermediate alloys by improving their heat resistance, cold workability, as well as their mechanical strength, hence their important addition to the aerospace, automobile, and civil industries [46–50]. It is generally believed that the V acts as a grain refiner, reduces the conductivity, and increases the temperature of recrystallization [51].

Research to improve the corrosion resistance of Mg by identifying metal fluorides resistant to dissolution in H2O, before alloying with Ti, led to the development of MgTi alloy. The alloy exhibited significant corrosion resistance in weak acid solutions containing F− ions for dental implants due to the formation of a thin, insoluble film of metal fluoride. Ti moderately dissolves in the presence of F− ions, creating problems with dental implants [52]. The effect of the addition of Mg and Mg alloys (AZ91 and WE43) with Ti6Al4V alloy on their corrosion resistance was studied in simulated body fluid by H2 evolution and electrochemical characterization techniques. Mg with Ti6Al4V alloy enhanced the formation of galvanic corrosion due to the initiation of microcracks from H2 evolution. However, Ti6Al4V-AZ91 composites, displaying a new TiAl3 interface layer maintained their mechanical and corrosion properties [53]. Xu et al. [39] investigated the corrosion resistance of binary MgTi alloys fabricated in a wide range of compositions by magnetron sputtering deposited on glass slides. Results showed that the MgTi alloy was more corrosion resistant than pure Mg in saturated Mg(OH)2 solutions with and without low concentrations of NaCl. The higher the Ti content the greater the corrosion resistance. Ozdemir and Gupta [54] studied the effect of V content on the hardness and corrosion resistance properties of Al alloy 2024 produced by high-energy ball milling. The alloy was observed to enhance the solid solubility of V elements and ultrafine grains. V also improved the corrosion resistance of Al 2024 alloy. Corrosion studies on binary Al alloys have shown that V provides an excellent combination of strength and corrosion resistance [55–57].

The influence of V additions on the precipitation of Mg2Si and Al2Cu phases in 6xxx series Al alloys shows that higher V content reduced the degree of strengthening with Mg2Si and Al2Cu phases and increased the content of AlFeSi and AlMgV particles in the range of sizes from 50 to 500 nm [58]. Investigation of Al 6063 alloy with 0.1 wt% addition of V showed that V enhanced the precipitation kinetics of Mg-Si phases, which invariably influenced the tensile and yield strength of the alloy. Al 6063 with 0.038 wt% of V did not show these phases [59]. Camero et al. [60] reported that the incorporation of 0.1% vanadium influenced the precipitation behavior and enhanced the mechanical properties of Al 6063 alloy. Cvetković et al. [61] investigated the electrodeposition of aluminum–vanadium alloys from chloroaluminate-based molten salts containing vanadium ions. Their findings indicated that the controlled co-deposition of vanadium and aluminum represents a promising approach for the development of advanced synthesis technologies for Al3V and AlV3 intermetallic alloys. In a related study, Wang et al. [62] examined the influence of vanadium addition on the hot deformation behavior of aluminum alloy 5083. The results demonstrated that vanadium additions in the range of 0–0.10 wt.% did not significantly alter the grain size of alloy 5083 in either the as-cast or homogenized states. However, the formation of fine Al3V precipitates in the alloy with 0.05 wt.% vanadium was found to enhance flow stress. Esquivel and Gupta [63] observed that the hardness of Al-V alloys increased with an increase in V addition due to the solid solution strengthening effect. Shi and Chen [64] studied the hot deformation properties of Al alloy 7150 at various V additions. Results show that the flow stress increased substantially with V additions. Shi and Chen [65] investigated the influence of Zr and V contents on the hot deformation properties of Al alloy 7150. Results show that adding 0.05 wt% V substantially increased the activation energy of the alloy. The effective application of Al-based alloys and metallic alloys closely aligned in properties and applications strongly depends on a thorough understanding of the environments responsible for corrosion and the most appropriate corrosion prevention methods. However, the corrosion reaction mechanism, rate of deterioration, equilibrium conditions, metal–solution interaction at the interface, and the specific types of corrosion must be investigated. Localized corrosion is primarily determined by the properties, size, and distribution of intermetallic components and secondarily by the solid-solution microstructure of the alloy. The information obtained will significantly influence the selection of appropriate metallic alloy with the matching environment resulting in minimizing the costly impact of corrosion damage.

Recent advancements in corrosion research for MgTi and aluminum-based alloys, such as Al4032 and Al4004, highlight their pivotal roles in aerospace, automotive, and biomedical fields. These alloys balance strength, weight, and corrosion resistance, making them integral for high-performance applications. The study of corrosion in these alloys is critical due to their susceptibility to electrochemical degradation in aggressive environments like chloride and sulfate-rich solutions. This degradation undermines structural integrity, limiting their application in demanding environments. Previous research largely focuses on generalized corrosion mechanisms in Mg and aluminum alloys but inadequately explores the nuanced interaction of metallurgical properties with specific corrosive ions (e.g., sulfate, chloride) and the long-term stability of dual passive oxide films in MgTi alloys and the selective role of vanadium in aluminum alloys. This study fills these gaps by analyzing corrosion behaviors under varied electrolyte concentrations and coupling these findings with microscopic and thermodynamic evaluations. Specifically, it investigates discrepancies in degradation dynamics, oxide stability, and anion interactions. In light of the above, this research investigates the corrosion resistance properties of Al4032 and Al4004 alloys, MgTi alloy, and Al-V alloy in neutral chloride and sulfate–environment electrolytes.

2 Experimental methods

2.1 Materials and method

MgTi, Al3032, Al4004, and AlV alloys were retrieved from automobile scrap components. These alloys were then manually sectioned with a hacksaw into 15 specimens each, with dimensions of 1 cm in length, 1 cm in width, and 0.75 cm in thickness, for the purpose of gravimetric analysis and open circuit potential (OCP) assessment. Elemental examination of the alloys was conducted using a PhenomWorld high-resolution electron microscope at the Covenant University Central Instrumentation Research Facility in Ota, Ogun State, Nigeria. The findings (weight percent compositions) of the analysis are presented in Table 1. Cu wires were affixed to the alloy specimens using soft solder before being embedded in pre-solidified acrylic paste. The surface of the specimens was polished with silicon carbide sheets (60–1,500 grits), refined with a 3 µm diamond suspension, and cleaned with demineralized water and acetone. Three sets of electrolyte solutions were prepared. Set 1 consist of 0.1 M H2SO4, 0.05 M H2SO4, 0.025 M H2SO4, 0.0125 M H2SO4, and 0.00625 M H2SO4 solution. Set 2 consists of 0.5% NaCl, 1.5% NaCl, 2.5% NaCl, 3.5% NaCl, and 4.5% NaCl solution while set 3 consists of 0.00625 M H2SO4/0.5% NaCl, 0.00625 M H2SO4/1.5% NaCl, 0.00625 M H2SO4/2.5% NaCl, 0.00625 M H2SO4/3.5% NaCl, and 0.00625 M H2SO4/4.5% NaCl solution at 200 mL each. They were prepared by dilution of analaR grade of H2SO4 (98% H2SO4) and recrystallized NaCl with distilled H2O.

Table 1

Elemental wt% composition of Al4032, MgTi, Al4004 and Al-V alloys

Al 4032 MgTi Al 4004 Al-V
Element symbol wt% conc. Element symbol wt% conc. Element symbol wt% conc. Element symbol wt% conc.
Al 85.08 Mg 73.26 Al 89.05 V 89.41
Si 14.18 Ti 22.34 Si 10.04 Al 9.25
Fe 0.74 Dy 3.51 Fe 0.5 N 0.82
Cu 0.41 C 0.89 Cu 0.41 C 0.52
Cu 0.41 — —

2.2 OCP evaluation

Corrosion thermodynamics was assessed through an OCP analysis. The experiment was conducted at room temperature (308 K) using a Digi-Ivy 2311 potentiostatic device with a step potential of 0.1 V maintained for 5,400 s. The apparatus, comprising a triple cord electrode (alloy working electrode, Ag/AgCl electrode, and Pt cord counter electrode), was connected to a laptop computer.

2.3 Weight loss measurement

The weights of Al 4032, Al 4004, AlV, and MgTi specimens were measured and then fully immersed in the prepared electrolytes for a period of 480 h at ambient room temperature. Each alloy sample was weighed individually every 24 h using an Ohaus analytical weighing balance. The corrosion rate was calculated using the following equation:

C R = 87.6 W D A T ,

where W signifies the weight loss in grams, D denotes the density in g/cm2, A represents the area in cm2, and T indicates the time of exposure in hours. W was determined by subtracting the final weight of each sample measured at 24-h intervals for a total of 480 h, from its initial weight (maintained for 480 h).

2.4 Optical microscopy analysis

Optical microscopic images of MgTi, Al3032, Al4004, and AlV alloy specimens were captured using an Omax trinocular metallurgical microscope before and after the corrosion test. These images were then analyzed following the weight loss assessment.

3 Results and discussion

3.1 Gravimetric studies

3.1.1 Corrosion in 0.00625–0.1 M H2SO4

Figure 1a–d shows the plots of corrosion rates versus exposure time for MgTi, Al4032, Al4004, and AlV alloys in 0.00625–0.1 M H2SO4 solution. Figures 2a–d and 3a–d shows the corresponding plots for the alloys in 0.5–4.5% NaCl and 0.00625 M H2SO4/0.5% NaCl to 0.00625 M H2SO4/4.5% NaCl solution. The alloys were studied in these media to assess their corrosion resistance properties over extended time periods. H2 ion reduction and cathodic H2 overpotential play a major role in the corrosion process of the four alloys. The reaction processes on the alloy’s surfaces involve the anodic and cathodic reaction processes. While the anodic reaction is specific to the constituent ionic species of elements within the alloys studied, the cathodic reaction processes (H2 evolution and O2 reduction reactions) apply to all the alloys as shown in the equation below;

(1) 2 H + + 2 e − → H 2 ,

(2) O 2 + 2 H 2 O + 4 e − → 4 OH − ,

(3) O 2 + 4 H + + 4 e − → 2 H 2 .

Figure 1 Plot of corrosion rate versus exposure time for (a) MgTi, (b) Al4032, (c) Al4004, and (d) AlV alloys in 0.0625 M H2SO4 to 0.1 M H2SO4.
Figure 1

Plot of corrosion rate versus exposure time for (a) MgTi, (b) Al4032, (c) Al4004, and (d) AlV alloys in 0.0625 M H2SO4 to 0.1 M H2SO4.

Figure 2 Plot of corrosion rate versus exposure time for (a) MgTi, (b) Al4032, (c) Al4004, and (d) AlV alloys in 0.5% NaCl to 4.5% NaCl.
Figure 2

Plot of corrosion rate versus exposure time for (a) MgTi, (b) Al4032, (c) Al4004, and (d) AlV alloys in 0.5% NaCl to 4.5% NaCl.

Figure 3 Plot of corrosion rate versus exposure time for (a) MgTi, (b) Al4032, (c) Al4004, and (d) AlV alloys in 0.00625 M H2SO4/0.5% NaCl to 0.00625 M H2SO4/4.5% NaCl.
Figure 3

Plot of corrosion rate versus exposure time for (a) MgTi, (b) Al4032, (c) Al4004, and (d) AlV alloys in 0.00625 M H2SO4/0.5% NaCl to 0.00625 M H2SO4/4.5% NaCl.

MgTi alloy generally exhibited the highest corrosion rate values in H2SO4 solution at all concentrations studied compared to Al4032, Al4004, and AlV alloys. Corrosion rate initiated at values between 4.689 and 9.234 mm/year (0.00625–0.1 M H2SO4) at 24 h and progressively decreased to values between 0.242 and 6.081 mm/year at 480 h. The rate of decrease varies with H2SO4 concentration. The relatively weak corrosion behavior of MgTi alloy in H2SO4 solution is due to the highly reactive nature of the Mg constituents of the alloy [66]. These assertions are due to factors such as the selectively weak passive hydroxide film, lattice defects, flaws, and galvanic effects on grain boundaries with Ti constituent [67,68]. Previous research has stated that the oxide film on Mg has a porous structure, which significantly influences the electrochemical properties of the oxide [69]. Mg is also known to have a lower electrode potential than Ti and hence will significantly corrode relative to Ti [70]. According to Gore et al. [71]. Mg alloys are susceptible to H2 evolution in corrosive conditions. The reaction of Mg with the H₂SO₄ media occurs as a single displacement reaction as shown below. MgSO₄ and H₂ are the products of the reaction.

(4) Mg ( s ) + H 2 SO 4 ( aq ) → MgSO 4 ( aq ) + H 2 ( g ) .

However, despite the susceptibility of Mg to corrosion, the plot configuration of MgTi shows a decrease in corrosion rate values as earlier mentioned before 120 h of exposure. Beyond these, the corrosion rate was relatively stable with respect to exposure time at most concentrations. This is probably due to the metallurgical interaction of Mg with Ti metal whereby an oxide film forms on the MgTi surface, i.e., MgO and TiO oxide layer; though this does not negate the effect of galvanic coupling at the grain boundaries, the dual passive film has been credited with significantly reducing corrosion attacks [39,72]. Ti does not generally react with H2SO4 at low concentrations due to the formation of a highly resistant protective oxide layer on its surface. The corrosion resistance of Ti is primarily due to the evolution of TiO2, according to the equation below whereby Ti interacts with dissolved O2 to produce the strong adherent oxide layer on its surface as shown below [73,74]. With regard to these assertions, there is a strong possibility that selective deterioration of MgTi occurred.

(5) Ti + O 2 → TiO 2 .

Al4032, Al4004, and AlV alloys exhibited higher corrosion resistance behavior from observation of the corrosion rate values in Figures 1b–d. However, their corrosion resistance is highly dependent on the concentration of H2SO4. At the 0.1 and 0.05 M H2SO4 concentration, Al4032 exhibited the lowest corrosion rate values (1.245 and 1.795 mm/year) while AlV exhibited the highest values (3.779 and 2.543 mm/year). However, at 0.00625 and 0.0125 M H2SO4 concentration, AlV alloy displays the highest corrosion resistance at −0.106 and −0.125 mm/year while the corresponding values for Al4004 and Al4032 are comparable. The plot configuration for Al4032 generally showed a decrease in corrosion rate with respect to exposure time. However, at 0.1 and 0.05 M H2SO4 concentration corrosion rate was generally constant with respect to exposure time before decreasing at 312 and 144 h to lower values. The same was observed for Al4004 generally after 144 h of exposure. After an initial increase in corrosion at specific concentrations, the corrosion rate decreased significantly. AlV alloy displayed a significant increase in corrosion rate for 144 h of exposure from initiation at 0.1 and 0.05 M H2SO4 concentration before significantly decreasing to the end of the exposure hours. At 0.00625–0.125 M H2SO4 concentration, the corrosion rate was generally constant. Generally, an oxide layer of Al2O3 forms on Al-based alloys making it highly resistant and responsible for the decrease in corrosion rate with exposure time in H2SO4 [75–78]. However, it is in a continual state of collapse and reformation. SO 4 2 − anions are known to hinder the repair of the passive film within the electrolyte [79,80]. In the presence of the SO 4 2 − anions, the Al alloys oxidize according to the equation below:

(6) Al → Al 3 + + 3 e − .

The presence of O2 changes the dynamics of the Al oxidation process to Al(OH)3 as follows:

(7) Al + 3 OH − → Al ( OH ) 3 + 3 e − .

However, complexes resulting from SO 4 2 − ionic interaction with the Al alloy surface shown in the equations below likely have a passivating effect on Al alloys. Research from Bolzoni et al. [81] has shown that SO 4 2 − anions display a limited passivating effect on some Al alloys [82]

(8) Al 3 + + SO 4 2 − → AlSO 4 2 − ,

(9) Al ( OH ) − 2 + SO 4 2 − → Al ( OH ) SO 4 2 − .

Si is the major alloying element for Al4032 and Al4004 alloys. It rapidly forms a thin layer of SiO₂ on its surface (as shown in the equation below) in aqueous media. The oxide is passive and protects the substrate metal. Hence, galvanic action at grain boundaries and localized corrosion reactions are likely to be prevalent on the Al alloy surfaces:

(10) Si + O 2 → SiO 2 .

The unusual characteristics of AlV exhibiting the highest corrosion rate values at 0.1 and 0.05 M H2SO4 and the lowest corrosion rate at 0.00625, 0.0125, and 0.025 M H2SO4 among Al alloys are probably due to the presence of V element in the alloy. V has been proven to enhance the corrosion resistance of Al alloys as it changes the chemical composition of the passive film. V is known to decrease the concentration and mobility of point defects and releases vanadates which are known to inhibit corrosion and cause grain refinement [58,83]. There are factors under which the protective effect of V in AlV alloy is disrupted. In a more reactive state, alteration in the dynamics of the electrochemical process, changes in pH conditions, percentage concentration of V within, and its interaction with the alloy and galvanic effects, V reacts within the electrolyte to form VSO₄ as follows;

(11) V ( s ) + H 2 SO 4 ( aq ) → VSO 4 ( aq ) + H 2 ( g ) .

3.1.2 Corrosion in 0.5–4.5% NaCl Solution

Corrosion rates of MgTi, Al4032, Al4004, and AlV in Figure 2a–d are proportional with NaCl concentration. The alloys generally exhibited the highest corrosion rate values in 0.5% NaCl concentration while the lowest corrosion rate occurred at 4.5% NaCl. Second, the corrosion rate of the alloys in the NaCl solution is significantly lower than the values obtained in the H2SO4 solution. However, MgTi alloy exhibited the highest corrosion rate values among the alloys with optimal corrosion rates of 0.794 and 0.180 mm/year (0.5 and 4.5% NaCl concentration) at 480 h. At 0.5% NaCl concentration, the plot configuration of MgTi shows a significant increase in corrosion rate for the first 264 h of exposure before marginally decreasing. At other concentrations beyond 0.5% NaCl, the plot configuration was generally stable with minimal alterations. Mg alloys are known to corrode in Cl− ion-containing solutions [84–87]. The corrosion reaction process of Mg in a neutral chloride solution is shown below:

(12) Mg + 2 H 2 O → Mg ( OH ) 2 + H 2 .

The oxidation reaction process is as follows:

(13) Mg → Mg 2 + + 2 e − ( anodic ) .

Mg(OH)2 occurs as a result of recombination of oxidized Mg ions with OH− ions [88,89]:

(14) Mg 2 + + 2 OH − → Mg ( OH ) 2 .

The corrosion protection properties of Mg(OH)2 are limited [90]. In Cl− ion solutions, the reaction processes of Mg are known to be complex. Mg(OH)2 is easily infiltrated by Cl− ion and transformed to MgCI according to the equation below. MgCI is easily broken down by the Cl− ion leading to further corrosion [91,92].

(15) Mg ( OH ) 2 + 2 CI − → MgCl 2 + 2 OH − .

The effect of Cl− ions on the corrosion resistance of Al4032, Al4004, and AlV alloys is limited with respect to corrosion rate results when compared to the values obtained for MgTi. The corrosion rate of Al4032, Al4004, and AlV initiated at values between 1.425 and −1.696 mm/year, −0.0004 and −0.0011 mm/year, and −0.085 and −1.310 mm/year at 24 h of exposure. However, the plot configuration of Al4032 differs from Al4004 and AlV alloys. Al4004 and AlV alloys plot configuration showed a decrease in corrosion rate at all concentrations (though marginal at very few concentrations) to 480 h, the plot configuration for Al4032 significantly decreased at 0.5, 1.5, and 3.5% while at 2.5 and 4.5% increase in corrosion rate was observed for 48 h of exposure. Generally, corrosion rates were marginally stable after 120 h of exposure. At 480 h of exposure, the final corrosion rate values for the alloys are −0.141 and −0.458 mm/year, −0.0003 and −0.0004 mm/year, and −0.0004 and −0.0004 mm/year. Overall, Al4004 and AlV displayed relatively strong resistance to corrosion throughout the exposure hours compared to the other alloys. The high corrosion resistance of the Al alloys does not negate the electrochemical effects of the Cl− ion on the protective oxide of Al due to the diffusion of the Al3+ ion [93,94]. The equations below show the effect of Cl− ion concentration on the corrosion rate of Al alloys:

(16) Al → Al 3 + + 3 e − ,

(17) Al 3 + + H 2 O → Al ( OH ) 2 + + H + ,

(18) Al 3 + + Cl → AICl 2 + ,

(19) Al ( OH ) 2 + + Cl − → Al ( OH ) CI − ,

(20) AlCl 2 + 2 H 2 O → Al ( OH ) 2 Cl + 2 H + ,

(21) Al ( OH ) Cl − + H 2 O → Ai ( OH ) 2 Cl + H + ,

(22) Al ( OH ) 2 Cl + H 2 O Al ( OH ) 3 + H + + Cl − ,

(23) 2 Al ( OH ) 3 ( amorphous ) → Al 2 O 3 ⋅ H 2 O ( boehmite ) + 2 H 2 O .

V in AlV probably forms a passivating oxide layer, such as V₂O₅ which can slow down further corrosion.

(24) 2 V + 5 H 2 O → V 2 O 5 + 10 H + + 10 e − .

However, in Cl− ion solution, there is the possibility of V oxidizing leading to the formation of V²⁺, V³⁺ as shown in the equation below. This is due to disruption of the passivation layer resulting in the initiation of localized corrosion on AlV alloys [95–97].

(25) V → V 3 + + 3 e − .

The V ions released into the electrolyte interact with Cl− ions, potentially forming VCl2+ complexes as shown below:

(26) V 3 + + Cl − → VCl 2 + .

This reaction mechanism results in the dissolution of V and accelerates the corrosion process due to disruption of the passive oxide layer by Cl− leading to the initiation of localized corrosion.

The presence of Si in the Al alloy significantly enhances the formation of localized corrosion due to galvanic action. SiO₂ tends to be chemically inert but changes in pH condition, the presence of impurities, other electrochemical factors, and most importantly the presence of Cl− cause the formation of localized corrosion due to weakening of the protective oxide layer though Si is much more resistant than some metals.

3.1.3 Corrosion in 0.00625 M H2SO4/0.5% NaCl–0.00625 M H2SO4/4.5% NaCl

Corrosion rate values for MgTi, Al4032, Al4004, and AlV alloys from the acid chloride media in Figure 3a–d are visibly higher (marginal at some concentrations) than the values obtained in Figure 2a–d. The combined action of SO 4 2 − and Cl− ions reacted with the alloy surfaces. However, the combined effect is significantly lower than the singular effect of SO 4 2 − ions but more than the effect of Cl− ions on the alloys. There is the possibility that SO 4 2 − ions may slightly mitigate the aggressive behavior of Cl− ions, but this effect is limited and often not enough to prevent significant corrosion due to the formation of stable corrosion products, e.g., Al₂(SO₄)₃ that are less damaging compared to chlorides [98,99]. Second, SO 4 2 − ions are known to provide protection through competitive adsorption with Cl− ions on adsorption sites on the alloy’s surfaces. However, this is often insufficient to prevent significant corrosion [100–103]. MgTi alloy generally exhibited the highest corrosion rate values throughout the exposure hours compared to the other alloys. Its corrosion rates initiated (24 h) at values between 0.072 and 6.240 mm/year. The plot configuration shows a significant decrease in corrosion rate values at 0.5% NaCl/H2SO4 to 2.5% NaCl/H2SO4 solution for 120 h of exposure. Beyond 120 h, the plot configuration indicates the relative stability of the alloy surface and attainment of equilibrium conditions. At 3.4 and 4.5% NaCl/H2SO4 concentration, relative stability occurred from onset to the end of the exposure hours (480 h). The plot configuration and corrosion rate values of Al4032 and Al4004 are comparable and show a significant decrease in corrosion rate unto 96 h (Al4004) and 120 h (Al4032). Although corrosion rates of Al4032 are slightly higher, alloys show relative stability in plot configuration to 480 h due to the stability of the protective oxide. AlV displayed the lowest corrosion rate values among the alloys throughout the exposure hours signifying higher corrosion resistance. However, corrosion rate is not proportional to NaCl concentration neither was a significant or direct decrease in corrosion observed at all NaCl concentrations.

3.2 OCP measurement

3.2.1 0.00625–0.1 M H2SO4 concentration

The OCP plots for MgTi, Al4032, Al4004, and AlV alloy in 0.00625 and 0.1 M H2SO4, 0.5 and 4.5% NaCl, and 0.00625 M H2SO4/0.5% NaCl and 0.00625 M H2SO4/4.5% NaCl solutions are shown in Figures 4a and b, 5a and b, and 6a and b. Generally, the plot configuration of MgTi in the acid, neutral chloride, and acid–chloride solution (Figures 3a, 4a, and 5a) is significantly electronegative relative to the plots of the other alloys. This observation agrees with the results obtained from gravimetric analysis. The electronegativity signifies an electroactive surface, breakdown of the protective oxide, and a high tendency to corrode [104,105]. The OCP plot for MgTi in Figure 4a and b initiated at −1.728 and −0.439 V and terminated at −1.591 and −0.233 V. This shows that MgTi is relatively more resistant or has a lower tendency to corrode in 0.1 M H2SO4 solution compared to 0.00625 M H2SO4. It indicates the formation of more dense oxide to withstand the electrochemical action of SO 4 2 − ions on the alloy surface [106–108]. This assertion is further proven by the plot configuration for MgTi in Figure 4b which shows the stability of the oxide film compared to the plot configuration of MgTi in Figure 4a with significant potential transients. The potential transients are due to the active nature of the alloy surface due to the active–passive transition behavior of the alloy surface [109]. The plot configuration of Al4032 in Figure 4a and b proves it has the lowest tendency to corrode or possibly the most corrosion-resistant oxide. The corresponding potential values are the most electropositive which relates to oxide formation. In Figure 4a, the Al4032 plot initiated at −0.686 V and significantly increased to −0.359 V at 500 s. Beyond this most, there was visible active–passive transition behavior till 2,400 s where relative stability was observed (−0.423). The dynamic equilibrium state continued to 5,400 s (−0.464). The corresponding plot for Al4032 in Figure 4b shows significant thermodynamic instability throughout the exposure hours. However, the corresponding corrosion potential is significantly more electropositive than the values obtained in Figure 4a probably due to the formation of reaction complexes with SO 4 2 − ions which provides pseudo passivity [110–112]. The OCP plots for Al4004 and AlV in Figure 4a and b were relatively stable with no visible potential transient, although the plots in Figure 4a tend to electro-positivity signifying a marginal increase in the protective oxide. In Figure 4b, there was a visible but marginal transition of AlV plots to electronegative values signifying weakening of the protective oxide. The plots initiated at −0.591 and −0.628 V and −0.514 and −0.467 V in 0.00625 and 0.1 M H2SO4 solution at 0 s and culminated at −0.484 and −0.562 V and at −0.433 and −0.722 V at 5,400 s.

Figure 4 OCP plots for (a) MgTi, Al4032, Al4004, and AlV alloys in (a) 0.0625 M H2SO4 and (b) 0.1 M H2SO4.
Figure 4

OCP plots for (a) MgTi, Al4032, Al4004, and AlV alloys in (a) 0.0625 M H2SO4 and (b) 0.1 M H2SO4.

Figure 5 OCP plots for (a) MgTi, Al4032, Al4004, and AlV alloys in (a) 0.5% NaCl and (b) 4.5% NaCl.
Figure 5

OCP plots for (a) MgTi, Al4032, Al4004, and AlV alloys in (a) 0.5% NaCl and (b) 4.5% NaCl.

Figure 6 OCP plots for (a) MgTi, Al4032, Al4004, and AlV alloys in (a) 0.00625 M H2SO4/0.5% NaCl and (b) 0.00625 M H2SO4/4.5% NaCl.
Figure 6

OCP plots for (a) MgTi, Al4032, Al4004, and AlV alloys in (a) 0.00625 M H2SO4/0.5% NaCl and (b) 0.00625 M H2SO4/4.5% NaCl.

3.2.2 0.5% NaCl to 4.5% NaCl concentration

The plot configuration of Al4032 in 0.5 and 4.5% NaCl solution relative to other alloys (Figure 5a and b) shows that it has the least tendency to corrode due to anodic passivation and growth of oxide formed on the alloy surface. However, it must be noted that the Al4032 plot in Figure 5a occurred at higher potentials hence greater oxide formation on its surface compared to Figure 5b. The OCP plot for Al4032 in Figure 5a and b initiated at −0.268 and −0.648 V and terminated at 2.711 and −0.650 V. However, the plot configuration in Figure 5a shows that it is thermodynamically unstable due to the electrochemical action of Cl− ions at low concentrations [113,114]. This contrasts the plot configuration in Figure 5b which indicates stable passive film and thermodynamic stability throughout the exposure hours in the presence of high Cl− ion concentration. The OCP plots for Al4004 and AlV in Figure 5a and b though significantly more electronegative than the plots for Al4032 were thermodynamically stable for 5,400 s. Despite their higher tendency to corrode compared to Al4032, the consistency of their plot configuration shows their protective oxide has attained dynamic equilibrium at the metal–solution interface where Cl− ions consistently interact with the ionized alloy surfaces [115,116]. MgTi in agreement with the results for gravimetric analysis exhibited the most electronegative plots in Figure 5a and b indicating a higher tendency to corrode. The plot configuration for MgTi in Figure 5a shows significant instability of the protective oxide in the presence of Cl− ions at 0.5% concentration, whereas Figure 5b shows significant stability of the protective oxide at 4.5% NaCl concentration. The observation for the alloys in Figure 5a and b shows that Cl− ions at low concentrations are more deleterious to their protective oxide due to their ability to penetrate through the oxide. However, at high Cl− ion concentrations (probably due to solute saturation) the protective oxides are stable.

3.2.3 0.00625 M H2SO4/0.5% NaCl to 0.00625 M H2SO4/4.5% NaCl concentration

The OCP plots in Figure 6a and b illustrate the influence of SO₄²⁻ and Cl⁻ ions on the corrosion resistance and thermodynamic properties of the alloys. Despite higher corrosion tendencies from gravimetric data, the combined action of reactive species promotes a stable oxide film. MgTi alloy exhibits the weakest corrosion resistance, with OCP values starting at −1.665 and −1.715 V (0 s) and rising to −1.598 and −1.576 V at 5,400 s. Figure 6a indicates thermodynamic stability, while Figure 6b shows marginal instability. Over time, the plots shift anodically, suggesting protective oxide growth and metallic complex formation. Al4004 demonstrates the highest corrosion resistance and stability, followed by AlV in Figure 6a and Al4032 in Figure 6b.

3.3 Optical microscopy analysis

3.3.1 Corrosion in 0.00625–0.1 M H2SO4

Optical images of MgTi, Al4032, Al4004, and AlV alloys after gravimetric analysis are shown in Figures 7a–10dii at magnification ×20. Figure 7a–d shows the images of MgTi, Al4032, Al4004, and AlV alloys before corrosion. Figure 8ai–dii shows the optical images of the alloys from 0.00625 M H2SO4 and 0.1 M H2SO4 solution. Figure 9ai–dii shows the optical images of the alloys from 0.5% NaCl and 4.5% NaCl solution while Figure 10ai–dii shows the optical images of the alloys from 0.00625 M H2SO4/0.5% NaCl and 0.00625 M H2SO4/4.5% NaCl solution. Variation in morphological features of the alloys from the H2SO4 solution is due to differences in their metallurgical structure and their respective electrochemical interaction with the anionic species in the electrolyte. Extensive morphological deterioration is visible on MgTi, Al4004, and AlV alloy at 0.00625 M H2SO4 compared to the surface morphology at 0.1 M H2SO4. This is debatable for AlV alloy (Figure 7di). However, for the alloys earlier mentioned the nature of deterioration differs. MgTi and Al4004 (Figure 8ai and ci) depict morphological degradation over the entire surface. Al4032 (Figure 8bi) shows extensive localized deterioration over the entire surface in the form of corrosion pits while AlV (Figure 8di) depicts flake-like deterioration or deterioration in layers. The corresponding images in Figure 8aii, bii, cii, and dii show that the degradation mechanisms of the alloys differ with respect to the electrolyte concentration. A limited number of large micro-pits are present on the MgTi (Figure 8aii) surface while the adjacent areas show toned-down deterioration compared to Figure 8ai. The same was observed for Al4032 (Figure 8bii) where the extent of deterioration was limited compared to Figure 8bi. The morphology of AlV (Figure 7dii) remains unchanged compared to Figure 8di while localized corrosion deterioration dominated the morphology of Al4004 (Figure 8cii) from 0.1 M H2SO4.

Figure 7 Optical images of (a) MgTi alloy, (b) Al4032 alloy, (c) Al4004, and (d) AlV before corrosion test.
Figure 7

Optical images of (a) MgTi alloy, (b) Al4032 alloy, (c) Al4004, and (d) AlV before corrosion test.

Figure 8 Optical images of MgTi (ai and aii), Al4032 (bi and bii), Al4004 (ci and cii), and AlV (di and dii) from 0.00625 M H2SO4 and 0.1 M H2SO4 solution.
Figure 8

Optical images of MgTi (ai and aii), Al4032 (bi and bii), Al4004 (ci and cii), and AlV (di and dii) from 0.00625 M H2SO4 and 0.1 M H2SO4 solution.

3.3.2 Corrosion in 0.5–4.5% NaCl solution

The extent of the morphological deterioration of MgTi alloy in 0.5 and 4.5% NaCl (Figure 9ai and aii) differs to a certain degree from the morphology in Figure 8ai and aii. Although the degree of variation is much more visible when comparing Figures 8aii and 9aii, Cl− ions undoubtedly interacted with the MgTi surface, deteriorating the alloy. The extent of localized surface deterioration increased significantly at 4.5% NaCl concentration (Figure 9aii) compared to Figure 8aii. Al4032 (Figure 9bi) exhibited significant morphological deterioration in the presence of Cl− ions over the entire surface compared to localized surface degradation (Figure 8bi) in the presence of SO 4 2 − ions. This shows that the dynamics of electrochemical reactions in the presence of Cl− and SO 4 2 − ions significantly differs. Al4004 alloy (Figure 9cii) underwent general surface deterioration in the presence of Cl− ions. This contrasts its morphology (Figure 8ci) in the presence of SO 4 2 − ions which showed extensive localized deterioration as earlier mentioned. AlV alloy proves more resilient in the presence of Cl− ions (Figure 9di and dii) compared to SO 4 2 − ions (Figure 8di and dii). The extensive degradation visible in Figure 8di and dii was largely in the presence of Cl− ions.

Figure 9 Optical images of MgTi (ai and aii), Al4032 (bi and bii), Al4004 (ci and cii), and AlV (di and dii) from 0.5% NaCl and 4.5% NaCl solution.
Figure 9

Optical images of MgTi (ai and aii), Al4032 (bi and bii), Al4004 (ci and cii), and AlV (di and dii) from 0.5% NaCl and 4.5% NaCl solution.

3.3.3 Corrosion in 0.00625 M H2SO4/0.5% NaCl–0.00625 M H2SO4/4.5% NaCl

The combined action of SO 4 2 − and Cl− ions significantly deteriorated the morphology of MgTi, Al4032, and Al4004 compared to their separate electrochemical action. Extensive general surface degradation and localized corrosion are present in Figure 10ai and aii, bi and bii, and ci and cii, whereas the counterparts exhibited general or localized corrosion degradation. However, AlV (Figure 10ci and cii) proves to be more resilient in the presence of both anions compared to its morphology in Figure 8ai and aii. However, the morphology in Figure 10ai and aii showed large micro-pits due to localized deterioration while the general surface deterioration is marginal.

Figure 10 Optical images of MgTi (ai and aii), Al4032 (bi and bii), Al4004 (ci and cii), and AlV (di and dii) from 0.00625 M H2SO4/0.5% NaCl and 0.1 M H2SO4/4.5% NaCl solution.
Figure 10

Optical images of MgTi (ai and aii), Al4032 (bi and bii), Al4004 (ci and cii), and AlV (di and dii) from 0.00625 M H2SO4/0.5% NaCl and 0.1 M H2SO4/4.5% NaCl solution.

3.4 Implications of research outcome and recommendations for future investigation

The study presents significant insights into the corrosion performance of various alloys and their potential applications in different aggressive environments. The MgTi alloy demonstrated the highest corrosion rates in acidic (H₂SO₄), chloride-rich (NaCl), and mixed acid–chloride environments. This performance suggests that MgTi alloys are best suited for applications requiring controlled degradation, such as biomedical implants, where exposure to aggressive electrolytes can be minimized. Furthermore, applying protective coatings or employing anodization techniques could enhance their performance by stabilizing the oxide layer. Mitigating galvanic coupling at grain boundaries may also reduce localized degradation.

In contrast, Al4032, Al4004, and AlV alloys exhibited significantly superior corrosion resistance compared to MgTi, particularly in chloride-rich environments. These characteristics make them ideal candidates for structural and automotive applications, especially in marine or coastal conditions where chloride exposure is prevalent. The incorporation of vanadium and silicon in these aluminum alloys was found to enhance their corrosion resistance, indicating that alloy design optimization can further improve their performance in aggressive environments.

These findings underscore the need for tailored corrosion prevention strategies. For MgTi alloys, optimizing surface protection methods could extend their utility in biomedical applications. For aluminum alloys, the excellent chloride resistance of AlV, combined with its vanadium-enhanced pitting resistance, positions it as a promising material for marine structural components. Additionally, Al4032 and AlV alloys demonstrate potential for use in lightweight, high-strength automotive components, particularly in environments with significant exposure to corrosive elements. The results highlight the critical role of material selection and alloy optimization in engineering applications. It is recommended that future research should focus on several key areas to enhance material performance and broaden application possibilities. Advanced coatings for MgTi alloys should be investigated to improve their durability and usability across diverse environments. Additionally, exploring the long-term behavior of aluminum alloys in mixed-ion environments will provide insights to refine material selection for more demanding conditions. Hybrid alloys that combine the favorable properties of aluminum and Mg should also be examined to achieve an optimal balance between mechanical strength and corrosion resistance.

4 Conclusion

MgTi, Al4032, Al4004, and Al-V alloys were studied for their corrosion resistance properties. MgTi alloy exhibited the weakest corrosion resistance in H2SO4, NaCl, and H2SO4-NaCl solution from corrosion rate values obtained compared to Al4032, Al4004, and AlV alloy. Plot configuration from the gravimetric analysis showed the corrosion rate of the alloys generally decreased with respect to exposure time. OCP plots showed that MgTi all displayed the most electronegative potential throughout the exposure hours compared to the other alloys while Al4032 proved to be the most electropositive, thermodynamically stable, and more resistant to corrosion tendency. Images from optical microscopy depict extensive morphological degradation. However, the degree of degradation varies with the type of electrolyte, electrolyte concentration, and metallurgical properties of the alloy.

Acknowledgments

The authors of this research appreciate Covenant University Center for Research Innovation and Discovery (CUCRID) for supporting this work.

  1. Funding information: Authors state no funding involved.

  2. Author contributions: All authors have accepted responsibility for the entire content of this manuscript and consented to its submission to the journal, reviewed all the results and approved the final version of the manuscript. Roland Tolulope Loto, Joshua Olusegun Okeniyi, and Morounfoluwa John are responsible for supervision, conceptualization, and writing – original draft preparation. Ayomide Oluwaseyi Olaolorun, Daniel Ikhionose Igenuma, David Ayobami Sonde, Emmanuel Eberechukwu Achonwa, Afolami Erastus Fanifosi, and Tobechukwu Bravohenshaw Okoroji are responsible for visualization, investigation, validation, methodology, data curation, and writing – original draft preparation.

  3. Conflict of interest: Authors state no conflict of interest.

  4. Data availability statement: The datasets generated during and/or analyzed during the current study are available from the corresponding author on reasonable request.

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Received: 2024-10-16
Revised: 2024-12-23
Accepted: 2025-02-21
Published Online: 2025-04-16

© 2025 the author(s), published by De Gruyter

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

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https://doi.org/10.1515/eng-2025-0110
Keywords for this article
corrosion; magnesium; aluminum; acid; chloride; pitting
Creative Commons
BY 4.0

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