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Surface Chemistry and Corrosion of Light Alloys

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A special issue of Metals (ISSN 2075-4701). This special issue belongs to the section "Corrosion and Protection".

Deadline for manuscript submissions: closed (31 January 2021) | Viewed by 77183

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Dr. Sebastian Feliú, Jr.

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Centro Nacional de Investigaciones Metalúrgicas CSIC, Avda. Gregorio del Amo 8, 28040 Madrid, Spain
Interests: magnesium alloys; corrosion; surface chemistry; electrochemistry; XPS; EIS
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Special Issue Information

Dear Colleagues,

Light alloys have attracted increasing scientific and technical interest during the last two decades. From a practical point of view, aluminum- and magnesium-based alloys are among the lighter structural metals, with densities of less than 3–4 g cm⁻³, which make their utilization very attractive in the transport industry, where weight is important, to lower fuel consumption and CO₂ emissions. On the other hand, titanium alloys are commonly used materials for permanent implants and the biocompatibility and biodegradability of magnesium alloys are interesting for temporary implants. Nevertheless, corrosion and wear resistance of these alloys is one of the key points that limit its utilization in service.

Although, the corrosion of metals begins on a portion of the surface film and then expands due to its breakdown, the influence of surface chemistry is generally considered less relevant than the composition or microstructure of the bulk material on their corrosion behavior. However, the surface films on titanium and aluminum alloys are continuous, uniform and greatly retard the corrosion of the chemically active metal substrate. In contrast, most of the naturally formed surface films on Mg alloys are considered to be discontinuous, providing considerably less protection and are consequently a primary factor that explains the poor corrosion resistance of this material. Any attempt to improve the corrosion resistance of light alloys requires a profound understanding of the relationship between the composition, structure and the protective properties of the surface films and how these relationships are modified by surface and interface engineering or under different environmental factors.

This Special Issue addresses the nature of the surface films formed on commercial light alloys, corrosion protection strategies and the changes in their chemical composition induced by exposure to aggressive environments, with the aim of elucidating the protective properties of these films.

Dr. Sebastian Feliú Jr.
Guest Editor

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Keywords

Magnesium alloys
Aluminum alloys
Titanium alloys
Surface chemistry
Electrochemistry at surfaces
Corrosion behavior
Protective properties
Surface engineering

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Published Papers (12 papers)

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Research

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19 pages, 6685 KiB

Open AccessEditor’s ChoiceArticle

Improved Corrosion Behavior of AZ31 Alloy through ECAP Processing

by A. I. Alateyah, Talal A. Aljohani, Majed O. Alawad, H. Abd El-Hafez, A. N. Almutairi, E. S. Alharbi, R. Alhamada, B. W. El-Garaihy and W. H. El-Garaihy

Metals 2021, 11(2), 363; https://doi.org/10.3390/met11020363 - 21 Feb 2021

Cited by 37 | Viewed by 3849

Abstract

This study aims to establish the effects of equal channel angular pressing (ECAP) processing on the corrosion behavior and hardness values of the AZ31 Mg alloy. The AZ31 billets were processed through ECAP successfully at 250 °C and their microstructural evolution was studied using optical and field emission scanning electron microscopy. The corrosion resistance of the AZ31 alloy was studied before and after processing through ECAP. The homogeneity of the hardness distribution was studied using both sections cut parallel and perpendicular to the extrusion direction. ECAP processing resulted in highly deformed central regions with elongated grains aligned parallel to the extrusion direction, whereas the peripheral regions showed an ultra-fine-grain recrystallized structure. After processing, small ultra-fine secondary particles were found to be homogeneously dispersed alongside the grain boundaries of the α-Mg matrix. Regarding the corrosion properties, measurements showed that ECAP processing through 1-P and 2-Bc resulted in decreasing their corrosion rate to 67.7% and 78.3%, respectively, of their as-annealed counterpart’s. The corrosion resistance of the ECAPed Mg alloy increased with the number of processing passes. This was due to the refinement of the grain size of the α-Mg matrix and secondary phases till ultra-fine size, caused by the accumulation of strain during processing. On the other hand, ECAP processing through 2-Bc resulted in increasing the Vickers hardness values by 132% and 71.8% at the peripheral and central areas, respectively, compared to the as-annealed counterpart. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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8 pages, 3484 KiB

Open AccessArticle

Effect of Laser Power on Microstructure and Micro-Galvanic Corrosion Behavior of a 6061-T6 Aluminum Alloy Welding Joints

by Huiling Zhou, Fanglian Fu, Zhixin Dai, Yanxin Qiao, Jian Chen and Wen Liu

Metals 2021, 11(1), 3; https://doi.org/10.3390/met11010003 - 22 Dec 2020

Cited by 22 | Viewed by 3266

Abstract

The 6061-T6 aluminum alloy welding joints were fabricated using gas metal arc welding (GMAW) of various laser powers, and the effect of laser power on the microstructure evolution of the welding joints was investigated. The corrosion behaviors of 6061-T6 aluminum alloy welding joints were investigated in 3.5 wt% NaCl solution using scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDS). The results showed that the micro-galvanic corrosion initiation from Mg₂Si or around the intermetallic particles (Al-Fe-Si) is observed after the immersion test due to the inhomogeneous nature of the microstructure. The preferential dissolution of the Mg₂Si and Al-Fe-Si is believed to be the possible cause of pitting corrosion. When the laser power reached 5 kW, the microstructure of the welded joint mainly consisted of Al-Fe-Si rather than the Mg₂Si at 2 kW. The relatively higher content of Al-Fe-Si with increasing in laser power would increase the volume of corrosion pits. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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15 pages, 3361 KiB

Open AccessArticle

Synthesis and Electrochemical Characterisation of Magnetite Coatings on Ti6Al4V-ELI

by Adriana Montiel, Edgar Onofre Bustamante and María Lorenza Escudero

Metals 2020, 10(12), 1640; https://doi.org/10.3390/met10121640 - 5 Dec 2020

Cited by 4 | Viewed by 2338

Abstract

Titanium alloys have been widely employed in implant materials owing to their biocompatibility. The primary limitation of these materials is their poor performance in applications involving surfaces in mutual contact and under load or relative motion because of their low wear resistance. The aim of this work is to synthesis magnetite coatings on the Ti6Al4V-ELI alloy surface to increase corrosion resistance and to evaluate its electrochemical behaviour. The coatings were obtained using potentiostatic pulse-assisted coprecipitation (PP-CP) on a Ti6Al4V-ELI substrate. The preliminary X-Ray Diffraction (XRD) results indicate the presence of the magnetite coating with 8–10 nm crystal sizes, determined for the (311) plane. Using X-ray photoelectron spectroscopy (XPS), the presence of the magnetite phase on the titanium alloy was observed. Magnetite coating was homogeneous over the full surface and increased the roughness with respect to the substrate. For the corrosion potential behaviour, the Ti6Al4V-ELI showed a modified E_corr that was less active from the presence of the magnetite coating, and the impedance values were higher than the reference samples without coating. From the polarization curves, the current density of the sample with magnetite was smaller than of bare titanium. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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23 pages, 13462 KiB

Open AccessFeature PaperArticle

PEO of AZ31 Mg Alloy: Effect of Electrolyte Phosphate Content and Current Density

by Branislav Hadzima, Daniel Kajánek, Michal Jambor, Juliána Drábiková, Matěj Březina, Joseph Buhagiar, Jana Pastorková and Martina Jacková

Metals 2020, 10(11), 1521; https://doi.org/10.3390/met10111521 - 17 Nov 2020

Cited by 24 | Viewed by 3933

Abstract

In this work, the quality of coatings prepared by plasma electrolytic oxidation (PEO) on an AZ31 magnesium alloy were evaluated. This was done by studying the effects of the chemical composition of phosphate-based process electrolytes in combination with different applied current densities on coating thickness, porosity, micro-cracking and corrosion resistance in 0.1 M NaCl. Both processing parameters were studied in four different levels. Mid-term corrosion resistance in 0.1 M NaCl was examined by electrochemical impedance spectroscopy and based on this, corrosion mechanisms were hypothesized. Results of performed experiments showed that the chosen processing parameters and electrolyte composition significantly influenced the morphology and corrosion performance of the prepared PEO coatings. The PEO coating prepared in an electrolyte with 12 g/L Na₃PO₄·12H₂O and using an applied current density 0.05 A/cm² reached the highest value of polarization resistance. This was more than 11 times higher when compared to the uncoated counterpart. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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26 pages, 6088 KiB

Open AccessArticle

Enhancing the Corrosion Protection of AA2024-T3 Alloy by Surface Treatments Based on Piperazine-Modified Hybrid Sol–Gel Films

by Diógenes J. Carbonell, Rodrigo Montoya, Victoria J. Gelling, Juan Carlos Galván and Antonia Jiménez-Morales

Metals 2020, 10(4), 539; https://doi.org/10.3390/met10040539 - 21 Apr 2020

Cited by 3 | Viewed by 4077

Abstract

The aim of this study was to develop new chrome-free surface pretreatments for AA2024-T3 aluminum alloy. These pretreatments were based on hybrid organic–inorganic sol–gel thin films prepared from mixtures of γ-methacryloxypropyltrimethoxysilane (MAPTMS) and tetramethylorthosilicate (TMOS). Different MAPTMS/TMOS molar ratios were used for optimizing the physical–chemical characteristics of the sol–gel films. The formulation of a set of these sols was modified by incorporating piperazine (1,4-diazacyclohexane) as a corrosion inhibitor. The resulting sol–gel films were characterized by using Fourier transform infrared spectroscopy (FTIR), liquid-state ²⁹Si nuclear magnetic resonance spectroscopy (²⁹Si-NMR) and viscosity measurements. The corrosion performance of the sol–gel films was analyzed by using electrochemical impedance spectroscopy (EIS) and local electrochemical impedance mapping (LEIM). The characterization techniques indicated that piperazine behaved as a catalyst for the condensation reaction during the formation of the MAPTMS/TMOS organopolysiloxane network and produces an increase of the crosslinking degree of the sol–gel films. EIS and LEIM results showed that piperazine is an effective corrosion inhibitor, which can be used to enhance the active corrosion protection performance of sol–gel films. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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15 pages, 2189 KiB

Open AccessFeature PaperArticle

Improvement of the Corrosion Resistance of Biomedical Zr-Ti Alloys Using a Thermal Oxidation Treatment

by Javier Izquierdo, Daniel Mareci, Georgiana Bolat, Juan J. Santana, Raquel Rodríguez-Raposo, Luis C. Fernández-Mérida, Liviu Burtan, Lucia C. Trincă and Ricardo M. Souto

Metals 2020, 10(2), 166; https://doi.org/10.3390/met10020166 - 22 Jan 2020

Cited by 5 | Viewed by 2845

Abstract

Binary Zr-Ti alloys spontaneously develop a tenacious and compact oxide layer when their fresh surface is exposed either to air or to aqueous environments. Electrochemical impedance spectroscopy (EIS) analysis of Zr-45Ti, Zr-25Ti, and Zr-5Ti exposed to simulated physiological solutions at 37 °C evidences the formation of a non-sealing bilayer oxide film that accounts for the corrosion resistance of the materials. Unfortunately, these oxide layers may undergo breakdown and stable pitting corrosion regimes at anodic potentials within the range of those experienced in the human body under stress and surgical conditions. Improved corrosion resistance has been achieved by prior treatment of these alloys using thermal oxidation in air. EIS was employed to measure the corrosion resistance of the Zr-Ti alloys in simulated physiological solutions of a wide pH range (namely 3 ≤ pH ≤ 8) at 37 °C, and the best results were obtained for the alloys pre-treated at 500 °C. The formation of the passivating oxide layers in simulated physiological solution was monitored in situ using scanning electrochemical microscopy (SECM), finding a transition from an electrochemically active surface, characteristic of the bare metal, to the heterogeneous formation of oxide layers behaving as insulating surfaces towards electron transfer reactions. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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17 pages, 21336 KiB

Open AccessArticle

Effect of Temperature on the Corrosion Behavior of Biodegradable AZ31B Magnesium Alloy in Ringer’s Physiological Solution

by Sebastian Feliu, Jr., Lucien Veleva and Federico García-Galvan

Metals 2019, 9(5), 591; https://doi.org/10.3390/met9050591 - 22 May 2019

Cited by 11 | Viewed by 4548

Abstract

In this work, the corrosion behaviors of the AZ31B alloy in Ringer’s solution at 20 °C and 37 °C were compared over four days to better understand the influence of temperature and immersion time on corrosion rate. The corrosion products on the surfaces of the AZ31B alloys were examined by scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS) and X-ray diffraction (XRD). Electrochemical impedance spectroscopy (EIS) provided information about the protective properties of the corrosion layers. A significant acceleration in corrosion rate with increasing temperature was measured using mass loss and evolved hydrogen methods. This temperature effect was directly related to the changes in chemical composition and thickness of the Al-rich corrosion layer formed on the surface of the AZ31B alloy. At 20 °C, the presence of a thick (micrometer scale) Al-rich corrosion layer on the surface reduced the corrosion rate in Ringer’s solution over time. At 37 °C, the incorporation of additional Mg and Al compounds containing Cl into the Al-rich corrosion layer was observed in the early stages of exposure to Ringer’s solution. At 37 °C, a significant decrease in the thickness of this corrosion layer was noted after four days. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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15 pages, 6166 KiB

Open AccessArticle

Effect of Si Content on the Corrosion Behavior of 420 MPa Weathering Steel

by Rui Sun, Qiang Yu, Yue Zhang, Xuqiang Yan, Yuchen Lu, Chunling Zhang and Qingfeng Wang

Metals 2019, 9(5), 486; https://doi.org/10.3390/met9050486 - 26 Apr 2019

Cited by 13 | Viewed by 4419

Abstract

The effect of Si content (0.12%, 0.34%, and 0.48%) on the corrosion behavior of weathering steel in a simulated marine environment was investigated in a dry/wet alternating cycle corrosion experiment. Corrosion weight gain, X-ray diffraction (XRD), scanning electron microscope (SEM), energy dispersive spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), and electrochemical methods were used to measure the regularity and nature of the rust. The results show that the corrosion process could be divided into an initial stage where the corrosion rate increased and a later stage where the corrosion rate decreased before remaining stable. The corrosion rate was the lowest for a Si content in the weathering steel of 0.48%. The corrosion products of all three steel groups contains α-FeOOH, β-FeOOH, γ-FeOOH, Fe₃O₄, and large amounts of amorphous compounds. Furthermore, Si benefits the transformation of β-FeOOH and γ-FeOOH to stable phases. The addition of the Si alloying element is beneficial to the formation of dense and compact rust layers that enhance the electrochemical resistance of weathering steel and silicon oxide influences the self-corrosion potential of the corrosion products. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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21 pages, 4577 KiB

Open AccessArticle

Influence of Aerospace Standard Surface Pretreatment on the Intermetallic Phases and CeCC of 2024-T3 Al-Cu Alloy

by Juan Jesús Alba-Galvín, Leandro González-Rovira, Manuel Bethencourt, Francisco Javier Botana and José María Sánchez-Amaya

Metals 2019, 9(3), 320; https://doi.org/10.3390/met9030320 - 12 Mar 2019

Cited by 16 | Viewed by 4098

Abstract

A standard three-step surface pretreatment employed in the aerospace sector for Al alloys have been investigated prior to the generation of cerium conversion coatings (CeCC) on aluminium-copper alloy 2024. Two pretreatments were analysed, one without final acid etching (Pretreatment 1) and another with this step (Pretreatment 2). Both pretreatments affect the alloy intermetallic phases, playing a key role in the development of the CeCC, and also in the susceptibility to localised corrosion in NaCl medium. Scanning electron microscopy coupled with energy-dispersive X-ray analysis (SEM-EDX) revealed that after Pretreatment 2, Al(Cu,Mg) phases were partially or totally removed through dealloying with their subsequent copper enrichment. Conversely, none of these intermetallic phases were affected when the final acid step was not employed (Pretreatment 1). Meanwhile, Al-Cu-Fe-Mn-(Si) phases, the other major Al–Cu alloys intermetallics, suffers minor changes through the whole pretreatments chain. The protective efficiency of CeCC was evaluated using electrochemical techniques based on linear polarisation (LP) and electrochemical impedance spectroscopy (EIS). Samples with CeCC deposited after the Pretreatment 1 gave higher polarisation resistance and impedance module than CeCC deposited after Pretreatment 2. SEM-EDX and X-ray photoelectron spectroscopy analysis (XPS) indicate that the main factors explaining the corrosion resistance of the coatings is the existence of Al(Cu,Mg) intermetallics in the surface of the alloy, which promote the deposition of a cerium-based coating rich in Ce⁴⁺ compounds. These Al(Cu,Mg) intermetallics were kept in the 2024 alloy when acid etching was not employed (Pretreatment 1). Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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Review

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37 pages, 10702 KiB

Open AccessEditor’s ChoiceReview

Promising Methods for Corrosion Protection of Magnesium Alloys in the Case of Mg-Al, Mg-Mn-Ce and Mg-Zn-Zr: A Recent Progress Review

by Pavel Predko, Dragan Rajnovic, Maria Luisa Grilli, Bogdan O. Postolnyi, Vjaceslavs Zemcenkovs, Gints Rijkuris, Eleonora Pole and Marks Lisnanskis

Metals 2021, 11(7), 1133; https://doi.org/10.3390/met11071133 - 18 Jul 2021

Cited by 46 | Viewed by 9425

Abstract

High specific strength characteristics make magnesium alloys widely demanded in many industrial applications such as aviation, astronautics, military, automotive, bio-medicine, energy, etc. However, the high chemical reactivity of magnesium alloys significantly limits their applicability in aggressive environments. Therefore, the development of effective technologies for corrosion protection is an urgent task to ensure the use of magnesium-containing structures in various fields of application. The present paper is aimed to provide a short review of recent achievements in corrosion protection of magnesium alloys, both surface treatments and coatings, with particular focus on Mg-Al-Mn-Ce, Mg-Al-Zn-Mn and Mg-Zn-Zr alloys, because of their wide application in the transport industry. Recent progress was made during the last decade in the development of protective coatings (metals, ceramics, organic/polymer, both single layers and multilayer systems) fabricated by different deposition techniques such as anodization, physical vapour deposition, laser processes and plasma electrolytic oxidation. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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23 pages, 6092 KiB

Open AccessReview

Electrochemical Impedance Spectroscopy for the Measurement of the Corrosion Rate of Magnesium Alloys: Brief Review and Challenges

by Sebastián Feliu, Jr.

Metals 2020, 10(6), 775; https://doi.org/10.3390/met10060775 - 10 Jun 2020

Cited by 157 | Viewed by 21111

Abstract

From a technological point of view, measurement of the corrosion rate of magnesium (Mg) and its alloys is critical for lifetime predictions of Mg-based structures and for comparative assessments of their corrosion protection ability. Whilst weight loss, hydrogen evolution, and polarization curves methods are frequently used for measuring the corrosion rate, the determination of values by electrochemical impedance spectroscopy (EIS) is relatively scarce and has only been realized recently. This technique seems to be the most suitable for monitoring corrosion rate values due to its “non-destructive” character, its reproducibility, and its reliable determination of small corrosion rates, much lower than those measured by other techniques. This review aims to picture the state-of-the-art technique of using EIS for measuring the corrosion rate of Mg. This paper starts by introducing some fundamental aspects of the most widely used methods for monitoring the corrosion rate of Mg/Mg alloy and continues by briefly explaining some of the fundamental concepts surrounding EIS, which are essential for the user to be able to understand how to interpret the EIS spectra. Lastly, these concepts are applied, and different approaches that have been proposed to obtain quantitative values of corrosion rate since the 1990s are discussed. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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33 pages, 18310 KiB

Open AccessReview

A Review on Adhesively Bonded Aluminium Joints in the Automotive Industry

by Francesca Cavezza, Matthieu Boehm, Herman Terryn and Tom Hauffman

Metals 2020, 10(6), 730; https://doi.org/10.3390/met10060730 - 1 Jun 2020

Cited by 74 | Viewed by 11996

Abstract

The introduction of adhesive bonding in the automotive industry is one of the key enabling technologies for the production of aluminium closures and all-aluminium car body structures. One of the main concerns limiting the use of adhesive joints is the durability of these system when exposed to service conditions. The present article primarily focuses on the different research works carried out for studying the effect of water, corrosive ions and external stresses on the performances of adhesively bonded joint structures. Water or moisture can affect the system by both modifying the adhesive properties or, more importantly, by causing failure at the substrate/adhesive interface. Ionic species can lead to the initiation and propagation of filiform corrosion and applied stresses can accelerate the detrimental effect of water or corrosion. Moreover, in this review the steps which the metal undergoes before being joined are described. It is shown how the metal preparation has an important role in the durability of the system, as it modifies the chemistry of the substrate’s top layer. In fact, from the adhesion theories discussed, it is seen how physical and chemical bonding, and in particular acid-base interactions, are fundamental in assuring a good substrate/adhesive adhesion. Full article

(This article belongs to the Special Issue Surface Chemistry and Corrosion of Light Alloys)

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