Journal of The Electrochemical Society, 155 共12兲 C583-C587 共2008兲 C583

0013-4651/2008/155共12兲/C583/5/$23.00 © The Electrochemical Society

Influence of the Alloying Elements on Pitting Corrosion

of Stainless Steels: A Modeling Approach
B. Malki,z T. Souier, and B. Baroux*
Science et Ingénierie des Matériaux et Procédés, Centre National de la Recherche Scientifique
UMR 5266-INP–UJF, 38402 Saint-Martin d’Hères, France

Modeling of corrosion pit chemistry in applied polarization mode is carried out using finite element method calculations. The
results lead to the formulation of critical conditions for pit stabilization in terms of the pit geometry and the applied potential.
More detailed computing is performed to compare the behavior of both ferritic and austenitic stainless steels. The results fairly
predict the beneficial effects of nickel on pitting resistance of 304 stainless steels, attributed to nickel-induced changes in
dissolution laws.
© 2008 The Electrochemical Society. 关DOI: 10.1149/1.2996565兴 All rights reserved.

Manuscript submitted May 14, 2008; revised manuscript received September 12, 2008. Published October 17, 2008.

Extensive works have been devoted to pit stability in conven-
tional stainless steels.1-13 Most of these studies portray various phe-
nomenological aspects of the pit active/passive transition. Many in-
vestigations have suggested that during pit growth a thick film,
mainly composed of salts, may cover the pit mouth.4,5 It is proposed
that it plays the role of an extra barrier to diffusion, keeping the
local medium rather corrosive.6,7 The pit in this case is regarded as
stable when the cover remains intact for a period long enough to
allow for salt film precipitation. Thus, pit growth is largely con-
trolled by the ohmic resistance of the porous cover, and only its
breakdown leads to a dilution of the pit medium, followed by step-
wise current decreases, and then repassivation.9 Regarding pit chem-
istry, Pistorius and Burstein affirm that a critical concentration of
metal chlorides is required to form the salt films.5,7 Laycock and
Newman8 have shown elsewhere that salt precipitation is not a nec-
essary condition for stabilization provided that the pit environment
is sufficiently concentrated to avoid repassivation. Williams et al.9
state that active/passive transition is the result of a local decrease in
the concentration of an anolyte inside the pit, while Sato3 argues in
favor of the existence of a critical ion concentration for the pit
electrolyte 共⌬c*兲 above which the pit will stabilize.
From another point of view, Pistorius and Burstein5,7,14 quanti-
fied the critical condition for pit stability in terms of the product of
pit radius 共r兲 and dissolution current density 共 j兲: 共r·j兲 as stipulated
in the Williams, Wescott, and Fleischman models.9 The latter works
are worth studying, because they put the emphasis on the possible
formulation of a meaningful link between pit chemistry and pit ge-
ometry. However, troublesome points remain. Pit chemistry and in
particular the local acidity is likely to control the passive film sta-
bility and in turn the current density. Moreover, regarding the pit
morphology and the chemically heterogeneous stainless steel sub-
strate, little information is known about the critical repassivation
conditions as a function of the stainless steel chemical composition.
All these effects are encapsulated in the current density parameter
共 j兲, and it is then hardly practical to sort out the pros and cons of the
multiple physicochemical parameters. An appropriate mechanistic
description of pit repassivation conditions still awaits new develop-
ments. The question of how far a possible combination of both pit
geometry and chemistry can control the stability transition needs to
be examined more closely. In this regard, the present paper aims to
investigate the critical conditions of active/passive transition, focus-
ing on the influence of pit geometry and the stainless steel chemical
composition. Particular attention is paid to the ferritic and austenitic
stainless steel alloys.
In a previous work,15 a simplified analytical description of pit
chemistry has shown, without referring to any salt formation, that
stable pits can survive when the critical acidity level at the active/
passive transition point reaches the depassivation pHd of the stain-
less steel. A linear relationship is found between a geometrical factor
共log L2 /r, L and r are, respectively, pit depth and pit mouth兲 and a
critical applied potential Vc above which pits will stabilize. In this
paper we propose an extension of the model to include realistic pit
chemistry for a better application to stainless steels systems. Nu-
merical simulations using the finite elements method 共FEM兲 seem
the appropriate method to employ. We use it to examine the applied
potential mode under which pit initiation is supposed to occur. We
focus particularly on the evolution of acidity at the transition point
共pHt兲 as a function of the pit geometry and the applied potential.
More detailed calculations are made to compare pit stabilization of
both ferritic and austenitic stainless steels. The consequences of the
established critical repassivation conditions are explored to throw
light particularly on the role of alloying elements, a key question as
far as the durability of stainless steels is concerned.
Model
Pit reactive system.— We study two typical stainless steel grades
in dilute chloride solution: the ferritic grade 共AISI 430兲 and the
austenitic ones 共AISI 304 and 316兲 共see Table I兲. Most of the re-
ported calculations are performed on AISI 430 considered as a pro-
totype system. We investigate in particular the relevance of the two
following parameters: the repassivation variable noted p/L 共see Fig.
1兲 and the applied potential Vapp. The advantage of using the FEM
technique is that it avoids numerous assumptions inherent to any
analytical approach.15-21 This requires taking into account all the
chemical species involved in a real material as well as their corre-
sponding chemical and electrochemical reactions. Nevertheless, we
still need to make two assumptions particularly about the anodic
dissolution and the hydrolysis reactions:
1. Due to a lack of information on the anodic dissolution law for
the boundary conditions, we use empirical current densities 共see
Table II兲, which are drawn from measurements in deaerated bulk
electrolyte NaCl 共2 M兲 pH 1 at room temperature, and are believed
to reflect the anodic dissolution in slightly growing stabilized pits.
Indeed, the important point is not to obtain absolute quantitative
predictions but to compare the behavior of the three stainless steel
grades under investigation
Table I. Chemical composition of the investigated materials in wt
%.
AISI C Mn Cr Ni Mo Cu S 共ppm兲 N

430 0.042 0.38 16.39 0.16 0.032 0.038 15 0.028

* Electrochemical Society Active Member. 304 0.016 1.2 18.5 8.1 0.15 0.18 5 0.04
z
E-mail: brahim.malki@ltpcm.inpg.fr
316 0.02 1.7 17.6 11.2 2.1 0.08 2 0.03

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C584 Journal of The Electrochemical Society, 155 共12兲 C583-C587 共2008兲

ci = ci ,0 Table III. Diffusion coefficients and initial concentrations used in

the simulation. These kinetics values are quite reasonable in rela-
ci = ci ,0 ci = ci ,0 tively dilute aqueous solutions.

z Species D cm2 s−1 Electrolyte concentration mol L−1

N i .n = 0 N i .n = 0 H+ 9.3 ⫻ 10−5 10−7
r OH− 5.3 ⫻ 10−5 10−7
Na+ 1.3 ⫻ 10−5 Estimated
p Cl− 2.0 ⫻ 10−5 0.1
Fe2+ 7.1 ⫻ 10−6 0
Cr3+ 7.5 ⫻ 10−6 0
ϕ(z) L Ni2+ 5.9 ⫻ 10−6 0
CrOH2+ 7.3 ⫻ 10−6 0
⎛ αi J⎞ FeOH+ 5.9 ⫻ 10−6 0
N i .n = ⎜ × ⎟
⎝ 2 + αi F ⎠ NiOH+ 7.3 ⫻ 10−6 0

Figure 1. 2D axis-symmetric pit geometry used for finite element calcula-
tions. The repassivation variable is defined by ratio p/L corresponding to
nonactive walls. Given the chemical composition ␣i, of the stainless steel,
the dissolution flux of species is calculated using an empirical current density
J 共see Table II兲, n being the outward normal vector from the pit wall and ␸
the electrostatic potential. Far from the pit reactive system, the species con-
centration is assumed to be constant, ci = ci,0.
2. In the second, only one hydrolysis reaction is considered for
each dissolved cation. No significant changes in the acidity are ex-
pected from more complicated hydrolysis reactions.
The pit reactive systems include the following ionic species:
Fe2+, Cr3+, CrOH2+, FeOH+, H+, Na+, and Cl− for the AISI 430
steel; and, Ni++ and NiOH+ for the AISI 304 grade. The correspond-
ing chemical and electrochemical reactions are the following
Fe → Fe2+ + 2e− 关1兴
k1,f
Fe2+ + H2O
FeOH+ + H+ 关2兴
k1,b
k3,f
Ni2+ + H2O →
NiOH+ + H+ 关7兴
k3,b
ki represents the kinetic constant rates. Tables III and IV summarize
all kinetic and thermodynamic data used in the calculations.
Master equations.— The governing equations are deduced first
from the mass balance principle, neglecting the advection term and
in the case of dilute aqueous solutions, the so-called Nernst–Planck
equation
⳵ci
+ ⵜ 共− Di ⵜ ci − zi␻iFci ⵜ ␸兲 = Ri 关8兴
⳵t
where the parameters ci, Di, zi, ␻i, and ␸ are, respectively, concen-
tration, diffusion coefficient, valence number, and ionic mobility of
species “i” in SI units. Ri is the corresponding net creation rate
共mol L−1 s−1兲. Extended Nernst–Planck equation analysis in the
case of deviations from dilute aqueous solutions hypothesis22 show
slight shifts in the potential profiles that can be treated in a second
step of this work to give a more complete picture. Second, from the
electroneutrality condition

Cr → Cr3+ + 3e− 关3兴 兺zc i

i i =0 关9兴

k2,f
this condition is made possible by assuming that the diffusion relax-
Cr3+ + H2O
CrOH2+ + H+ 关4兴 ation time 共␶d ⬃ 1 ms兲 is much greater than the charge relaxation
k2,b
one 共␶c ⬃ 1 ns兲. Given these master equations, the mathematical
kw,f description of the transport phenomena inside the pit reactive system
H2O
H+ + OH− 关5兴 is well-posed. FEM can now be used to solve the stationary prob-
kw,b lem.
for the AISI 430 grade, supplemented by the following two reactions
for the AISI 304 grade Boundary conditions.— We chose to work on axis-symmetric
two-dimensional 共2D兲 pit geometries as illustrated in Fig. 1. The pit
Ni → Ni 2+
+ 2e −
关6兴
size ranges from 1 to 200 ␮m, a length scale well above the lower
limit required for the validity of the continuum approximation. The
boundary conditions are fixed as follows:

Table II. Empirical parameters used in the calculations. The Taf- 1. On the pit walls, dissolution of Fe, Cr, and Ni species obeys
el’s law coefficients are obtained in 2 M NaCl at pH 1 and at an empirical Tafel’s law under charge-transfer-controlled
room temperature and the depassivation pHd are taken from Ref. conditions18
24.

AISI Vcorr 共V/SCEa兲 J0共␮A cm−2兲 b 共V/dec兲 pHd J = J0 exp关− b共Vapp兲 − Vcor − ␸兴 关10兴

430 −0.56 130 0.06 3

where the corrosion current J0, the corrosion potential Vcorr, and the
304 −0.45 35 0.06 2.4 Tafel slope b are fitted from experimental data. The applied potential
316 −0.39 29 0.11 1.8 Vapp is considered as a control parameter. Depending on the stainless
steel chemical composition 共␣i兲, the net flux of each species is given
a
Saturated calomel electrode. by

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 Journal of The Electrochemical Society, 155 共12兲 C583-C587 共2008兲 C585

Table IV. Equilibrium constants „Keq… of the used hydrolysis reactions Eq. 2, 4, and 7 and the corresponding kinetics rate constants.16 The latter
are estimated from equilibrium constants „ki,b = Keq Õki,f… assuming fast forward reaction rates.

Keq ki,f ki,b

Fe2+ 5 ⫻ 10−9 共mol L−1兲 103 s−1 2 ⫻ 1011 共mol L−1兲−1 s−1
Cr3+ 10−4 共mol L−1兲 107 s−1 1011 共mol L−1兲−1 s−1
Ni2+ 1.38 ⫻ 10−10 共mol L−1兲 103 s−1 7.2 ⫻ 1012 共mol L−1兲−1 s−1
H 2O 10−14 共mol L−1兲2 10−3 共mol L−1兲s−1 1011 共mol L−1兲−1 s−1

Ni·n =
where n is the normal direction to the boundary and F the Faraday
constant.
2. Passivation is expected to occur when dissolution fluxes is
null
3. Finally, within the electrolyte and at an infinite distance from
the pit, the concentration of all species as well as the electrostatic
potential are assumed to be constants of the so-called Dirichlet con-
ditions: ci = ci,0 and ␸ = 0.
The numerical implementation of the resulting partial differential
equations is performed using the software Comsol Multiphysics that
is practical for this kind of nonlinear problem.23 For a given pit
depth 共L兲 the stationary state for each repassivation state p/L is
calculated. In so doing, we obtain a variation of the transition pHt as
a function of p/L that can be considered as an average estimation of
the acidity level for a given pit geometry. By comparing this curve
to a given depassivation pHd, one should be able to verify if the
growth of a given pit is stable or not. Furthermore, a parametric
study of the influence of the pit geometry 共in terms of L and r兲 for
every applied potential Vapp is required to demarcate between pas-
sive and active zones in the 共L2 /r, Vapp兲 plane. Last, one alternative
to the use of pHt as a criterion for transition is simply to use the
minimum pHmin inside the pit to reach the same conclusions. The
gap in between can be considered as a transition zone given that the
冉 ␣i
2 + ␣i
⫻
J
F
冊 关11兴
pit repassivation mechanism is not yet elucidated. Such diagrams are
expected to illustrate more clearly the different behavior between
different stainless steels.
Results and Discussion
Figure 2 illustrates the simulated species concentration distribu-
tion along the pit depth for a given pit geometry: r = 1 ␮m, L
= 10 ␮m, and p/L = 0.5, which follows a nonuniform profile near
the pit mouth. This is because of the high concentration gradients
Ni·n = 0 关12兴 between the pit and the electrolyte outside the pit. As expected, this
distribution is strongly dependent on the pit geometry and the pas-
sive area, making the working point of the pit reactive system highly
sensitive to any change in these two major parameters. Note that the
relatively high concentration of chloride anions in this case suggests
a possible salt precipitation which may cause an additional shift of
the working point. This is not taken into account in our model as
mentioned above.
Figure 3 reports the various calculated transition pHt as a func-
tion of p/L and Vapp for a pit size of r = 1 ␮m and L = 10 ␮m. Two
observations emerge from these results. First, a parabolic shape of
the transition function pHt共p/L兲 is found by this method as predicted
by the analytical model.15 Given a critical pH 共pHd兲 and depending
on the repassivation variable p/L, this function presents two saddle
points, typically the hallmark of multiple steady states. This is pri-
marily related to a competition between dissolution and repassiva-
tion kinetics. Accordingly, during the propagation step pits may ex-
perience transient regimes, leading to unpredictable dynamical
effects encountered in some corrosion situations. Second, the aver-
age acidity level reached in the pit is lowered with increasing the
applied potential Vapp. Any increase in Vapp 共indirectly the dissolu-

6
2
10
-
-0,56 V
Cl
-1

0
10
specie concentration /mol.L

++
Cr
+++ Fe 5 -0,46 V
-2
10 +
H
T

+
CrOH
pH

-4 -0,36 V
10
4
-6
10 FeOH
+
-0,26 V

-8
10 +
Na 3
-0,16 V
-10 pH
10 d
0 2 4 6 8 10
Distance (µm)
Active wall Passive wall (p) 2
0 0,2 0,4 0,6 0,8 1
p/L
Pit buttom
z
Figure 3. 共Color online兲 Evolution of the pH at the active/passive transition
Figure 2. Simulation of concentration distributions along the pit depth ob- 共pHt兲 for a pit size of r = 1 ␮m and L = 10 ␮m as a function of the repas-
tained for r = 1 ␮m, L = 10 ␮m, p/L = 0.3, and for AISI 430 in 0.05 M sivation variable p/L and the applied potential Vapp for AISI 430 in 0.05 M
NaCl at Vapp = 0.16 V/ECS. NaCl.

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C586 Journal of The Electrochemical Society, 155 共12兲 C583-C587 共2008兲

-0,1 0,25

(Active zone) 0,2

-0,15 1E-4 M

(V/ECS)
(V/ECS)

0,15
-0,2
(Transition zone) 0,1

Critical
Critical

-0,25

V
0,05 0,02 M
V

-0,3 0
(Passive zone)
-0,35 -0,05
0 0,5 1 1,5 2 2,5 3 3,5 0 0,5 1 1,5 2 2,5 3 3,5
2 2
log(L /r) log(L /r)

Figure 4. 共Color online兲 Plot of the critical applied potential for pit stabili-
zation as a function of the pit geometry. Given a depassivation pHd 共case of
AISI 430 in 0.05 M NaCl兲, there is a threshold of the pit acidity above which
the pit repassivates, i.e., when pHt ⬍ pHd the pit is entirely active, when
pHtmin ⬎ pHd the pit is entirely passive, and in between a transition zone can
be defined.
tion current兲 will necessarily lead to more stable pits. Thus, given a
pit geometry 共L2 /r兲 and depassivation pHd, it is always possible to
define a critical applied potential above which pits can stabilize. In
this way, one can build a stability diagram as mentioned above for
each stainless steel 共see Fig. 4兲. This figure clearly illustrates that
small pits are more difficult to stabilize than the large ones, as they
require higher potentials to cross the active zone. Moreover, it is
tempting to link the critical potential Vc to the pitting potential 共Vpit兲
obtained experimentally. Although they are undoubtedly correlated,
this correlation depends on the pit’s geometry distribution,23 and
only the knowledge of this distribution should allow for a formal
connection between Vc and Vpit.
Notice that the active/passive transitions follow various “path
transitions” with regard to pit geometry and polarization conditions.
That is, the shape and the position of the parabolic curves depend on
the environmental variables. Figures 5 and 6 illustrate examples of
such effects. For example, as one enlarges the pit opening 共break-
down of the pit cover兲, the increase of the outward proton fluxes
leads to a reduction of the local acidity and hence to a possible pit
repassivation 共Fig. 5a兲. Moreover, the pit shape 共in the case of a
spherical morphology; see Fig. 5b兲, as well as the initial chloride
concentration 共Fig. 6兲, together lead to a significant shift in the
working point. Therefore, for realistic materials one can logically
expect deviations from the proposed linear relationship between Vc
and log共L2 /r兲. This is due to the above nonlinear contributions be-
sides those not taken into account in the model 共dissolution aniso-
Figure 6. 共Color online兲 Confirmation of the enhancing chlorides effect on
pit stabilization.
tropy, salts precipitation, etc.兲. Nevertheless, it is still possible to
provide valuable insights into the role of alloying elements using the
above linear approximation.
Indeed, if one compares the transition curves of ferritic AISI 430
and austenitic AISI 304 stainless steels, given their depassivation
pHd 共see Table II兲, AISI 430 exhibits a low transition curve 共see Fig.
7兲. Low applied potentials are sufficient to bring the working point
of a given pit 共L2 /r兲 to stable regimes. To answer the question
whether this can be attributed to nickel-induced change in the dis-
solution behavior or to nickel hydrolysis reactions, we have checked
the response of both ferritic and austenitic stainless steels when
inverting their empirical dissolution laws. Surprisingly, the transi-
tion curves also have been inverted. This confirms the predominant
role of nickel-induced change in the dissolution embodied by the
large difference in the empirical dissolution laws 共see Table II兲. The
case of AISI 316 grade appears to behave in the same way: the
passivity zone is wider than the previous grades. The only dissolu-
tion law 共implicitly the effect of alloying elements兲 is enough to
determine the stability behavior of the grade, although no assump-
tion has been made on molybdenum chemistry.
Conclusions
We have presented a corrosion pit reactive system from FEM
calculations. Our findings capture correctly the major asymptotic
behaviors and yield thresholds of the critical parameters in qualita-
tive agreement with experimental knowledge. Both pit chemistry
and topology are linked together to build a stability diagram portray-
ing the critical pit stabilization conditions. A linear relationship be-
tween a “critical propagation potential” Vc and log共L2 /r兲 共L and r
are, respectively, pit depth and pit mouth兲 has been established. This

4,5 3,8

(a) (b)
V = - 0,16 V/ECS
Vapp = - 0,16 V/ECS app
3,6 Figure 5. 共Color online兲 Transition pHt
4 dependence: 共a兲 on the pit opening where
cylindrical the reduction of the local acidity may lead
pHT

pHT

3,4
to pit repassivation, 共b兲 on the pit mor-
3,5 phology: in this case a spherical pit is used
pit mouth 3µm 3,2 instead of a cylinder and the principle of
calculations is exactly the same. The
3
simulation was performed for AISI 430 in
3 0.05 M NaCl at Vapp = 0.16 V/SCE and
spherical
pit mouth 1µm for a pit size of r = 1 ␮m and L
= 10 ␮m.
2,5 2,8
0 0,2 0,4 0,6 0,8 1 0 0,2 0,4 0,6 0,8 1
p/L p/L

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 Journal of The Electrochemical Society, 155 共12兲 C583-C587 共2008兲 C587

Centre National de la Recherche Scientifique assisted in meeting the

0,8 AISI 316 publication costs of this article.

0,6 References
V (V/ECS)

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