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Effects of Cerium on the Inclusions and Pitting Corrosion Behavior of 434 Ferritic Stainless Steel

  • Y. C. Yu , S. H. Zhang and S. B. Wang EMAIL logo
Published/Copyright: September 25, 2018
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High Temperature Materials and Processes
From the journal High Temperature Materials and Processes Volume 37 Issue 9-10

Abstract

The effects of Ce addition on the inclusions and the pitting corrosion behavior of ferritic stainless steel were investigated. The results showed that Ce2O3·SiO2 and Ce2O2S inclusions were mainly found in 434 ferritic stainless steel containing 0.011% or 0.023 wt% Ce, which is the most appropriate addition of Ce that could contribute to produce the dispersive and fine rare earth inclusions. According to the thermodynamic analysis, Ce inclusions could be produced by rare earth elements combining with oxygen, sulfur, or preexisting SiO2. While the kinetic analysis and mechanism for formation of inclusions suggested that the area ratio of the pure SiO2 inclusion decreased with Ce increasing, and the difference of [Ce] concentration between the original inclusion interface and the SiO2 solid unreacted nuclear interface is the main reason to cause the different process of inclusion modification. Meanwhile, when the content of Ce was 0.011% or 0.023%, the resistance to pitting corrosion increased with the interface areas between the inclusions and the steel matrix decreasing. However, the excessive Ce addition resulted in the increase of size and quantity of inclusions, which would reduce the resistance to pitting corrosion.

Keywords: ferritic stainless steel; cerium; inclusions; pitting corrosion

1 Introduction

Ferritic stainless steels approximately constitute one-half of the AISI type 400 series stainless steels. These steels contain 10% to 30% Cr except other alloying elements. Ferritic stainless steels are noted for their excellent stress corrosion cracking resistance and good resistance to pit and crevice corrosion in chloride environments [1, 2, 3, 4]. However, the relatively developed columnar structure leads to the weakness of the mechanical properties of ferritic stainless steels, and the application of this group of alloys is limited. It is well known that the addition of rare earth in stainless steels could suppress the detrimental action of inclusions by forming stable and globular rare earth inclusions, and then improve the mechanical properties of steels [5, 6, 7, 8]. However, corrosion is certainly an issue in steels and hence the corrosion properties of ferritic stainless steels are of high interest for their potential applications. Importantly, the alloying elements in these steels can alter the corrosion behavior due to the differences in their electrochemical properties, and the addition of alloying elements, such as rare earth Ce, may influence its original corrosion resistance. It was also reported in previous studies that stainless steels may suffer from pitting corrosion due to the presence of nonmetallic inclusions, and these inclusions, such as manganese sulfides, act as initiation sites for pitting corrosion [9, 10, 11, 12]. Some studies showed that the improvement of the corrosion resistance of the austenitic stainless steels by adding rare earth elements is due to modified inclusions inhibiting the occurrence of pitting corrosion.

However, up to now, few papers have specifically focused on the relationship between the corrosion behavior and inclusions in 434 ferritic stainless steels. Therefore, it is definitely worthwhile to study the formation mechanism of inclusions and the effect of inclusions on the corrosion behavior of 434 ferritic stainless steels.

In this paper, morphology, compositions, and size distributions of rare earth Ce inclusions in 434 ferritic stainless steel have been investigated; moreover, the thermodynamic possibility and kinetic mechanism analysis for the formation of rare earth inclusions have been discussed. Meanwhile, the corrosion behavior of 434 ferritic stainless steel with different Ce contents in 3.5 wt% NaCl solution was studied by using potentiodynamic polarization method.

2 Experimental procedure

Approximately 3 kg of alloy with different rare earth content were smelted in a vacuum induction furnace protected by argon at a temperature of 1,873K. The rare earth lined on a pure iron wire was inserted into a liquid steel after deoxidization with Si–Mn, and the molten steel was then refined for 3 min. When the temperature and composition were uniform, the molten steel was cast into the iron mold with dimensions of 55 mm at a pouring temperature of 1,823K, and finally, air cooled to room temperature. The chemical compositions of 434 ferritic stainless steel and Ce-containing steels are shown in Table 1.

Table 1:

Chemical composition of tested 434 ferritic stainless steels in wt%.

SampleCSiMnPSCrMoOCeN
10.0880.480.410.0210.03115.640.820.011–0.039
20.0880.500.420.0210.01715.570.820.0080.0110.035
30.0930.560.440.0220.01115.590.830.0070.0230.034
40.0910.570.430.0210.01015.620.820.0060.0340.034

The steel samples were grounded and polished to observe the inclusions of ferritic stainless steels. The inclusions in ferritic stainless steels were studied using scanning electron microscopy (SEM). The corresponding spectrum analysis of inclusions in the steels was undertaken by energy spectrum analysis (EDS).

To analyze the effect of Ce addition on the corrosion resistance of 434 ferritic stainless steel, the potentiodynamic polarization test of the experimental steel samples was conducted in the deaerated 3.5 wt% NaCl solution at 298 K. The test samples were welded with copper wire through solder and then embedded by the epoxy resin. The side of sample used in this test was polished with 1,200-grit silicon carbide abrasive papers until previous coarse scratches were removed, then rinsed, and dried.

3 Experimental results

3.1 Effect of Ce on the characteristics of inclusions

The morphology of inclusions in 1# steel sample was observed through SEM and the chemical composition of inclusions was analyzed by using EDS, as shown in Figure 1. It could be concluded that the types of inclusions in 1# steel mainly were SiO2, (Cr, Mn, Si) oxides, and MnS, which have a negative effect on properties of steels.

Figure 1: SEM image and EDS analysis of inclusions in 1# steel (a) complex inclusions (Cr, Mn, Si oxides); (b) SiO2 inclusions; (c) MnS inclusions.
Figure 1:

SEM image and EDS analysis of inclusions in 1# steel (a) complex inclusions (Cr, Mn, Si oxides); (b) SiO2 inclusions; (c) MnS inclusions.

Figure 2 represents the morphology, energy spectrum, and element distribution of the rare earth complex inclusion SiO2·Ce2O3. It is SiO2 inclusion in the center in this inclusion, surrounded by Ce2O3•SiO2 complex inclusion outside.

Figure 2: SEM image, EDS analysis, and element distribution of inclusions (Ce2O3·SiO2) in 2# steel.
Figure 2:

SEM image, EDS analysis, and element distribution of inclusions (Ce2O3·SiO2) in 2# steel.

Figure 3 represents the morphology, energy spectrum, and element distribution of inclusions in 3# steel. Primary inclusions were mostly transformed to Ce inclusions with the increase of Ce content in 3# steel sample, such as Ce2O3, Ce2O2S, and Ce2O3•SiO2, as shown in Figure 3. In addition, the area ratio of the pure SiO2 inclusion is very little compared to that of 2# steel and the shape of the inclusions has become globular.

Figure 3: SEM image, EDS analysis, and element distribution of inclusions (Ce2O2S) in 3# steel.
Figure 3:

SEM image, EDS analysis, and element distribution of inclusions (Ce2O2S) in 3# steel.

Figure 4 represents the morphology, energy spectrum, and element distribution of inclusions in 4# steel. Ce oxides or oxy-sulfides gathered because of the strong affinity of rare earth Ce to oxygen and sulfur when the content of rare earth Ce in the molten steel was 0.034%. As can be seen in Figure 4, clusters of rare earth inclusions with the strip shape were observed in the 4# steel.

Figure 4: SEM image, EDS analysis, and element distribution of reunited Ce complex inclusions in 4# steel.
Figure 4:

SEM image, EDS analysis, and element distribution of reunited Ce complex inclusions in 4# steel.

It can be concluded that Ce addition could change the morphology and type of inclusions. Ce reacted with SiO2 or MnS, which generated rare earth Ce inclusions (Ce2O3•SiO2 or Ce2O2S), and the pure SiO2 and MnS inclusions disappeared. So, rare earth Ce has played a great role of inclusion modification.

Image-Pro Plus software, statistic analysis was performed to determine the average size, size distribution, and quantity of inclusions per frame area of inclusions in the experimental steels, as shown in Figure 5. The size of inclusions decreases first with the content of rare earth Ce increasing; however, the size represents an increase when the content of rare earth Ce is 0.034%, as shown in Figure 5(a), which suggests that the addition of rare earth Ce plays an important role in the size distribution of inclusions. Figure 5(b) shows the effect of Ce on the area of inclusions per unit area. When 0.023% Ce was added, the area percentage of inclusions per unit area was much smaller than that of other stainless steel samples. So the appropriate content of Ce in steels could contribute to producing the dispersive and fine rare earth Ce inclusions.

Figure 5: Effects of rare earth Ce on the size distribution, number, and area of inclusions per unit area.
Figure 5:

Effects of rare earth Ce on the size distribution, number, and area of inclusions per unit area.

3.2 Effect of the Ce addition on the pitting corrosion behavior of 434 ferritic stainless steel

Figure 6 shows the effect of the rare earth Ce addition on the potentiodynamic polarization behavior of the experimental steels in deaerated 3.5 wt.% NaCl solution. In general, the pitting potential (Ep) is defined as the breakdown potential for destroying a passive film. The resistance to pitting corrosion of the experimental steel increases with the Ep increasing. The resistance to pitting corrosion of 2# steel and 3# steel containing rare earth Ce was superior to that of 1# steel without rare earth Ce because the pitting potential of 2# steel and 3# steel containing rare earth Ce is much higher than that of 1# steel. However, the pitting potential of 4# steel containing 0.034% Ce is similar to that of 1# steel.

4 Analysis and discussion

4.1 Thermodynamic analysis of rare earth inclusions

According to the results mentioned above, rare earth oxides or oxy-sulfides are main inclusions in Ce-containing experimental steels. Henrian activity coefficients and Henrian activities (1 wt% standard state) of O, S, Si, and Ce in liquid steel can be calculated by interaction coefficients with Wagner’s model. The corresponding interaction coefficients of O, S, Si, and Ce at 1,873K are shown in Table 2. Taking the experimental steel containing 0.023 wt% rare earth elements as an example, Henrian activity coefficients and Henrian activities of O, S, Si, and Ce in molten steel at 1,873K are calculated in Table 3.

Table 2:

Interaction coefficient eji of various elements in liquid steel at 1,873K [13, 14].

ejiCNOSiSPCeCrMnMo
S0.110.01–0. 270.063–0.0280.029–2.36–0.01–0.0260.0027
O–0.450.057–0. 2–0.131–0.1330.07–0.57–0.04–0.0210.0035
Si0.180.09–0.230.1030.0560.11––0.00030.002–
Ce0.397–6.612–5.03––10.341.77–0.008–––
Table 3:

Henrian activity coefficients and activities (1 wt% standard state) of different elements in liquid steel at 1,873K.

iSiSOCe
fi1.1890.6610.1740.504
ai0.6660.00730.00120.012

Standard Gibbs free energy change for formation of Ce2O3 and Ce2O2S in liquid steel is expressed by Eq. (1) and (2) [15], respectively

(1)Ce+32O=12Ce2ΔG10=−714380+179.74T.
(2)[Ce]+12[O]+[S]=12Ce2O2SΔG20=−675700+165.50T.

At 1,873K, corresponding Gibbs free energy changes of eqs. (1) and (2) are –151.775 kJ·mol-1 and –167.875 kJ·mol–1, respectively. So Ce2O3 and Ce2O2S in 434 ferritic stainless steel can be produced at 1,873K. However, the affinity of rare earth Ce and sulfur is less than that of oxygen, so Ce2O2S may be oxidized to Ce2O3 in some conditions.

In addition to simple rare earth oxides or oxy-sulfides, there also exist many Ce2O3•SiO2 complex inclusions in 434 ferritic stainless steel. Under current experimental conditions, the formation of Ce2O3•SiO2 under current experimental conditions may be expressed by Eq. (3)

(3)[Ce]+52[O]+12[Si]=12Ce2O3•SiO2ΔG30=−1106635+286.11T .

According to the activities of O, Ce, and Si in liquid steel, as shown in Table 3, the value of Gibbs free energy change at 1,873K is –236.885kJ·mol–1. The result shows that Ce2O3•SiO2 is stable under the condition.

Ce2O3, Ce2O2S, and Ce2O3•SiO2 are main inclusions in 3# steel, and inclusions of 434 ferritic stainless steel have been modified by adding rare earth Ce. It can be found from Figure 2 to Figure 4 that there are many rare earth Ce inclusions Ce2O3, Ce2O2S, and Ce2O3•SiO2 in the Ce-containing steels. Meanwhile, it suggests that the thermodynamic results and experimental results are basically in agreement.

4.2 Kinetic analysis of formation mechanism of rare earth Ce inclusion

Based on the inclusions observation, a dynamic model of SiO2 inclusion modification was deduced, and the corresponding model parameters were established by thermodynamic analysis to understand deeply SiO2 inclusion modification process after adding different contents of rare earth Ce.

SiO2 inclusion modification process can be divided into the following steps.

(1) [Ce] in molten steel diffused to the SiO2 inclusion surface.

(2) The reaction of [Ce] on the surface of SiO2 inclusion for Eq. (4) and (5) at 1,873K

(4)4 Ce+3 SiO2=2 Ce2O3+3 Si,
(5) Ce2O3+SiO2=Ce2O3∙SiO2.

(3) [Si] Generation diffused outward.

Figure 7 is the dynamic model of SiO2 inclusion modification. r0 represents the initial radius of SiO2 inclusion (m); r indicates the radius of unreacted nuclear (m); i1 and i2 represent the original inclusion interface and the SiO2 solid unreacted nuclear interface, respectively. The mixing of the molten steel is obvious in the refining process due to using medium-frequency vacuum induction furnace, and the diffusion of [Si] and [Ce] in liquid steel is relatively easy and the speed of chemical reaction is very fast at high temperature. So before the process of SiO2 inclusion modification, the main controlled step is the diffusion of [Si] or [Ce] in the middle of rare earth inclusion layers.

Figure 6: Effects of Ce addition on the potentiodynamic polarization behavior of the experimental steels in 3.5wt% NaCl solution.
Figure 6:

Effects of Ce addition on the potentiodynamic polarization behavior of the experimental steels in 3.5wt% NaCl solution.

Figure 7: The dynamic model of SiO2 inclusion modification.
Figure 7:

The dynamic model of SiO2 inclusion modification.

(1) The diffusion rate of [Si] in the rare earth Ce inclusion layer can be expressed by Eq. (6)

(6)vSi=−dnSidt=4 πr2DSidcSidr.

In Eq. (6), n[Si] and c[Si] represent the amount of substance of [Si] (mol) and the concentration of [Si] (mol·m-3), respectively. t represents time (s) and DSi represents the diffusion coefficient of [Si] (m2•s), which can be regarded as a constant.

Equation (7) can be derived by separating variables in Eq. (6)

(7) dcSi=−14πDSi⋅dnSidt⋅drr.

Getting Eq. (8) and Eq. (9) by integrating:

(8)∫cSi, i2cSi, i1dcSi=−14 πDSi⋅dnSidt⋅∫rr0drr2,
(9)vSi=−dnSidt=4 πDSir0rr0−rcSi, i2−cSi, i1.

cSi, i1 represents the concentration of [Si] in layer i1, while cSi, i2 represents the concentration of [Si] in layer i2.

The consumption rate of SiO2 in modification reaction can be expressed by Eq. (10)

(10)−dnSidt=−dnSiO2dt=−xSiO2dnCe inclusionsdt=−4 πr2ρCe inclusions⋅drdt.

ρCe inclusions represent the density of rare earth Ce inclusion layers.

Simultaneous equations above can be calculated to get Eq. (11)

(11)t=ρCe inclusions⋅r23 MCe inclusions⋅DSicSi,i2−cSi,i1.

Because ρCe inclusions and MCe inclusions are constants, the time of SiO2 inclusion modification is determined by the particle size and the concentration difference of [Si] between the interface i1 and the interface i2.

(2) The diffusion rate of [Ce] in the rare earth Ce inclusion layer can be expressed by the Eq. (12)

(12) vCe=−dnCedt=4 πr02DCecCe, i2−cCe, i1.

DCe represents the diffusion coefficient of [Ce], which can be regarded as a constant, and r0 is a fixed value. So the diffusion rate of [Ce] in the rare earth inclusion layers is proportional to the concentration difference of [Ce] between the interface i1 and the interface i2.

In the smelting process of ferrite stainless steel, all other conditions are the same except for the different content of rare earth Ce. So in the SiO2 inclusion modification process, the concentration difference of [Ce] between the interface i1 and the interface i2 is the main reason to cause the different process of inclusion modification in different steels, and, as is shown from Figure 1 to Figure 3, the area ratio of the pure SiO2 inclusion decreases with the increasing content of Ce. The kinetic results and experimental results are basically in agreement.

(3) It can be seen from Table 1 that the content of S decreases from 0.031 to 0.010. The Ce inclusions with low standard enthalpies of formation and melting points (Ce2O3 1,690°C, Ce2O2S 1,950°C) will nucleate and grow up if proper concentration and energy are given.

From above, it can be concluded that rare earth Ce inclusions nucleate and grow up separately centering on oxides and oxy-sulfides with high melting point. Just because of such a mechanism of nucleation, the dimension of rare earth Ce inclusions formed in steels exceeded in the current standard as shown in Figure 4. The process is as follows: first, rare earth Ce inclusions nucleate on oxides and sulfides with high melting points in liquid phase, and chemical potential gradient will drive atoms to diffuse because of high activity of rare earth Ce. The concentration gradient between the nucleus and its neighboring vicinity accelerates the diffusion of rare earth Ce. The surface activity of the impurity elements remains very high, and these impurities absorb other impurities in the steel and formed Ce-containing oxides and oxy-sulfides, which promote the aggregation of these elements on the particles. The more the rare earth Ce elements, the more impurities being absorbed. So the dimension of the inclusions relates to the degree of aggregation and the size of the inclusion in 4# steel is more than 10 μm.

4.3 Mechanism of the effect of Ce addition on the pitting corrosion behavior of 434 ferritic stainless steel

Wranglen [16] proposed the pit corrosion model originating from the sulfides and analyzed the mechanism of propagation of corrosion pits in steel by the microcorrosion test. The sulfides and its surrounding dispersion also play a role of cathode sites. In addition, due to the hydrolysis of iron ions, the anodic areas tend to become acidic, which accelerates the corrosion reactions with the formation of H2S, H+, and HS- ions. When the sulfide inclusion is destroyed and falls away, the micropits form in this way. If the proportion of inclusions is large as shown in Figure 7c, the corrosion of steel matrix around an inclusion may expose a new active volume around an underlying inclusion. When the depth of pits reaches a certain level, the initiation stage has been passed and the process of corrosion enters the propagation stage. At this time, an oxygen concentration cell as a small anode is formed in the interior of corrosion pits and its surrounding steel as the large cathode. This is called the cell of “small anode–large cathode.” Under this condition, the density of current is larger and the corrosion rate is accelerated.

It was reported that the addition of Ce can modify the types of inclusions from the soluble active sulfides or (Si, Mn) oxides to uncreative rare earth inclusions, which can avoid the pitting initiation from the other inclusions. [16, 17]

Meanwhile, the interface area between the inclusion and the substrate in 2# steel and 3# steel was smaller than that of 1# steel without rare earth Ce, as shown in Figure 7(c). In other words, the preferential sites for the initiation of pitting corrosion in the steel containing 0.011% or 0.023% Ce compared to other steel samples will decrease. However, there is the presence of stress field around the large inclusions with 0.034% Ce, and the pitting corrosion first appears in the interface between inclusions and steel matrix, which will contribute to the local corrosion and the formation of cracks.

5 Conclusions

(1) Ce has played a great role in inclusion modification. Ce reacted with SiO2 and generated Ce2O3•SiO2 complex inclusions, while Ce reacted with sulfide inclusions and generated globular Ce oxy-sulfides (Ce2O2S) inclusions.

(2) The kinetic analysis and mechanism of formation of inclusions suggest that the area ratio of the pure SiO2 inclusion decreases with the increasing content of Ce, and the concentration difference of [Ce] between the original inclusion interface and the SiO2 solid unreacted nuclear interface is the main reason to cause the different process of inclusion modification in different steels.

(3) When the content of rare earth Ce is 0.011% or 0.023%, the preferential sites for the initiation of pitting corrosion decrease with the interface areas between the inclusions and the steel matrix decreasing. However, the excessive Ce addition results in the increase of size and quantity of inclusions, which will reduce the resistance to pitting corrosion.

Acknowledgements

The authors are grateful for the support of the Natural Science Foundation of Shanxi Province (Grant No. 2015011068) and Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi (Grant No. 2017138).

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Received: 2017-07-02
Accepted: 2017-10-11
Published Online: 2018-09-25
Published in Print: 2018-10-25

© 2018 Walter de Gruyter GmbH, Berlin/Boston

This article is distributed under the terms of the Creative Commons Attribution Non-Commercial License, which permits unrestricted non-commercial use, distribution, and reproduction in any medium, provided the original work is properly cited.

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https://doi.org/10.1515/htmp-2017-0094
Keywords for this article
ferritic stainless steel; cerium; inclusions; pitting corrosion
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BY-NC-ND 3.0

Articles in the same Issue

  1. Frontmatter
  2. Research Articles
  3. Numerical Simulation of the Electron Beam Welding and Post Welding Heat Treatment Coupling Process
  5. Effect of Ti and Ta on Oxidation Kinetic of Chromia Forming Ni-Base Superalloys in Ar-O2-Based Atmosphere
  6. Effects of Cerium on the Inclusions and Pitting Corrosion Behavior of 434 Ferritic Stainless Steel
  7. Critical Assessment of Activities of Structural Units in Fe–Al Binary Melts Based on the Atom and Molecule Coexistence Theory
  8. A Yield Stress Model for a Solution-Treated Ni-Based Superalloy during Plastic Deformation
  9. Stress Relaxation Behaviour and Creep Constitutive Equations of SA302Gr.C Low-Alloy Steel
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  11. Experimental and Numerical Investigations on Hot Deformation Behavior and Processing Maps for ASS 304 and ASS 316
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  14. A Thermodynamic Study of the Reduction of a Limonitic Laterite Ore by Methane
  15. Electrochemical and Phase Analysis of Si(IV) on Fe Electrode in Molten NaCl-NaF-KCl-SiO2 System
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