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Numerical modeling of corrosion pit propagation using the combined

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Comput Mech (2014) 54:613–627
DOI 10.1007/s00466-014-1010-8
ORIGINAL PAPER
Numerical modeling of corrosion pit propagation using the
combined extended finite element and level set method
Ravindra Duddu
Received: 7 November 2013 / Accepted: 19 March 2014 / Published online: 19 April 2014
© Springer-Verlag Berlin Heidelberg 2014
Abstract A sharp-interface Eulerian formulation for
modeling the propagation of localized pitting corrosion is
presented. This formulation allows for an accurate repre-
sentation of the corrosion front independent of the underly-
ing finite element mesh and handles complex morphological
transitions such as pit merging without requiring remeshing
or mesh-moving procedures. First, the governing equations
of the moving interface problem associated with pit growth
are derived for the two-phase (metal-solution) system. Next,
the implementation of the combined extended finite element
and level set method and the procedure to enforce interface
conditions are discussed. Finally, the method is validated by
conducting several benchmark numerical studies, and com-
paring the results with published experimental data and exist-
ing numerical studies. Simulation studies indicate that: dur-
ing diffusion-controlled corrosion an isolated pit grows as
a semi-circular shape, whereas closely spaced pits merge
and grow into an elongated elliptical shape; and only during
activation-controlled corrosion the initial pit morphology is
preserved.
Keywords Pitting corrosion · XFEM · Level sets ·
Moving interface · Interface constraints
1 Introduction
Alloys of steel, nickel and aluminum are commonly used as
structural materials and are susceptible to pitting corrosion,
a form of extremely localized corrosion that leads to the for-
R. Duddu (B)
Department of Civil and Environmental Engineering,
Vanderbilt University, 400 24th Avenue South, 274 Jacobs Hall,
Nashville, TN 37212, USA
e-mail: rduddu@gmail.com; ravindra.duddu@vanderbilt.edu
mation of pits on the metal surface. A major problem with
this localized form of corrosion is that it is difficult to detect
and often leads to sudden and catastrophic failures by induc-
ing fatigue cracks or stress corrosion cracks near the pits
[1]. Thus, pitting corrosion poses a formidable threat to the
durability and integrity of industrial, civil infrastructure and
military systems [2]. Computational modeling of corrosion,
together with accelerated laboratory experiments, can yield
quantitative tools for scientists and engineers to better under-
stand and predict corrosion, and develop efficient strategies
for mitigating corrosion. Therefore, corrosion modeling has
been an active area of research, and for a detailed literature
review of the various empirical, stochastic and deterministic
models the reader is referred to [2]. The purpose and scope of
this article is to present a novel extended finite element and
level set formulation for modeling pitting corrosion propa-
gation based on continuum mechanics and electrochemical
theory.
Pitting corrosion, or simply pitting, progresses primar-
ily by the anodic dissolution of metal atoms as metal ions
(loss of electrons or oxidation) into the pit solution (elec-
trolyte) [3]. Isaacs [4] distinguished three basic stages of
pitting corrosion of stainless steels: nucleation, metastable
growth and stable pit growth. In this article, only the stable
growth (or propagation) stage is studied, when the pit inter-
face (separating the solid metal phase from the liquid pit
solution phase) acts as a sharp moving electrode boundary
across which there are jumps or discontinuities in both the
atom/ion concentrations and their normal derivatives. Thus,
the pit propagation problem belongs to the class of moving
free boundary problems. It is well known from experimental
studies that the rate of pit propagation is not only dependent
on the compositional variables (e.g. alloy, inter-metallic par-
ticles composition) but also dependent on the environmental
variables (e.g. pH, concentration of ionic and neutral species
123
614
in the pit solution) [5]. The need for tracking the concen-
trations of multiple ionic (anions and cations) and neutral
species in the pit solution using electro-diffusion equations,
arising from either Nernst-Planck or Stefan-Maxwell theo-
ries [6], tremendously increases the computational burden.
Additionally, corrosion pits can evolve into different com-
plex morphologies over time that can range from narrow-
deep to wide-shallow shapes owing to the different pit sur-
face and environments and local microstructure features, as
identified by ASTM [7]. Thus, the challenges associated with
numerical simulation of pitting corrosion are significant due
to the presence of a sharp moving interface, discontinuous
concentrations and gradients across the interface, complex
pit geometries, and heterogeneous microstructure. Conse-
quently, specialized methods for handling moving bound-
aries and for solving elliptic/parabolic partial differential
equations (PDEs) on irregularly shaped domains are needed
for producing accurate simulations.
Early efforts on numerical modeling of localized corro-
sion focussed on one-dimensional pit growth using either
the finite difference method [8,9] or the finite element
method [10]. Recent modeling studies simulated pit growth
in higher dimensions (mostly in 2D) using either the finite
volume method [11,12] or the finite element method [13–
16]. Scheiner and Hellmich [11,12] simulated pit propaga-
tion in two-dimensions using the finite volume method, but
the pit interface was not consistently tracked; consequently,
the reported pit shapes were zigzagged. The finite element
method (FEM) was employed to study pitting in higher
dimensions; however, simulating pit propagation using the
FEM can be cumbersome as it relies either on remeshing
[16], moving mesh techniques [17], or arbitrary Lagrangian-
Eulerian techniques (ALE) [14]. To overcome the limitations
of the FEM, herein an efficient and accurate method based on
the extended finite element method (XFEM) [18,19] and the
level set method (LSM) [20–24] is presented. In the literature,
many investigations employed the XFEM to study a variety
of embedded interface problems related to: crack propaga-
tion [25,26], phase transformation [27–29], fluid structure
interaction [30], hydrogels [31–33], biological cells [34–37],
finite deformations with arbitrary inclusions or voids [38,39],
and nano-composites [40]. The above cited work only con-
sidered the level set representation of the embedded inter-
face, but did not employ the full LSM along with the fast
marching scheme to consistently simulate its time evolution.
With the goal of consistently simulating complex interface
morphology evolution and shape transitions, the author and
co-workers developed the combined extended finite element
and level set method (XFE-LSM) to study microbial biofilm
growth [41,42] and precipitate evolution in Ni-Al alloys [43–
45].
In this article, a model for pitting corrosion propagation is
proposed within the XFE-LSM framework and is validated
123
Comput Mech (2014) 54:613–627
using published experimental data on stainless steel alloys.
In addition, an improved numerical implementation of the
XFE-LSM is presented. Unlike the original implementation
described in [41], herein Heaviside functions are employed
to enrich the finite element basis and Lagrange multipliers
are used to enforce the Dirichlet interface condition on the
evolving interface during diffusion-controlled corrosion.The
generalized Heaviside enrichment or step enrichment is cho-
sen as it allows for the jumps in both the concentration field
and its normal derivative at the pit interface. The rest of the
article is organized as follows: in Sect. 2 the strong form of
the elliptic interface problem governing metal dissolution is
derived using the continuum theory of two-phase interfaces
described by Gurtin et al. [46,47], and the corresponding
weak or variational formulation is presented; in Sect. 3 the
XFE-LSM discretization and strategies for enforcing interfa-
cial constraints and for evaluating the interface propagation
speed are detailed; in Sect. 4 numerical results are presented
that demonstrate the viability of this approach for studying
localized pitting corrosion in two-dimensions; and finally,
Sect. 5 presents some concluding remarks.
2 Model formulation
2.1 Governing equations
2.1.1 Domain description
Let us consider a regular domain  ∈ R3 bounded by a
smooth boundary ∂ =  that consists of two phases:
the solid metal domain s (t) and the pit solution domain
p (t). The solid and the solution domains are separated by
a sharp moving interface  int (t) at all times t, as shown
in Fig. 1. Herein, the general 3D problem is reduced to
2D by considering uniformity in the out of plane direc-
tion. The two phases are assumed exist in closed regions
with their union  = s (t) ∪ p (t) and their intersection
 int (t) = s (t) ∩ p (t) is a smoothly propagating inter-
face. The interface orientation is defined by the outward unit
normal n(x, t) pointing away from the pit solution domain
p (t), where x denotes the spatial Cartesian system of coor-
dinates. Let V (x, t) denote the normal interface speed of
 int (t) in the direction n at any spatial location x and time
t. The Dirichlet boundary at pit mouth and the Neumann
boundary enclosing the metal solid domain are denoted by
p p
hs (t) and d (t), respectively. Note that  = hs ∪ d at all
times.
2.1.2 Continuum mechanics of phase interfaces
Following the two-phase continuum theory and the notation
introduced by Gurtin et al. [46,47], let us derive the govern-
Comput Mech (2014) 54:613–627 615

Fig. 1 A schematic diagram of the pitting corrosion problem. The
interface  int (blue) partitions the sub-domains s (light grey) and p
p
(white). The Dirichlet boundary d (red) and the Neumann boundary
hs (black) are shown. The outward interface normal n points away from
the pit solution domain. The outward normal to the domain boundary
is denoted by n0 . A control volume R ∈  with outward unit normal
n R on ∂ R is considered to derive the governing equations. (Color figure
online)

 
ing equations in three-dimensions in the bulk domains and J · n R da → [[ J]] · n da. (5)
at the interfaces. Let c(x, t) denote the metal atom/ion con-
∂R r (t)
centration of a particular species in  that is function of the
spatial coordinates x and time t, and let c denote its mate-
rial time derivative. For this bulk field, let cp and cs denote 2.1.3 Mass balance
the limits of c when the interface is approached from the pit
solution and solid domains, respectively, and [[c]] denotes the The balance of metal atom/ion mass for all control volumes
jump in c across the interface: for x ∈  int (t) R is given by,
cp (x, t) = lim c( y, t), cs (x, t) = lim c( y, t), (1) ⎧ ⎫
y→x y→x
y∈p (t) y∈s (t) ⎨ ⎬ 
[[c]] = c − c .
s p
(2) Mc dv =− M J · n R da, (6)
⎩ ⎭
R ∂R
Now, consider a control volume R ∈  with n R the out-
ward unit normal on ∂ R, as shown in Fig. 1. Let R contain
a portion of the interface r such that r (t) = R ∩  int (t). An where M is the mass of one mole of metal atoms/ions. By
important transport identity [47], valid for the bulk field c is, applying the above equation to control volumes that exclude
the interface and using the divergence theorem, the standard
⎧ ⎫
⎨ ⎬   bulk relation can written as,
c dv = c dv − [[c]]V da, (3)
⎩ ⎭
R R r (t) c = −∇ · J (7)

where V is the normal interface speed, dv is an infinitesimally

small volume element in  and da is an infinitesimally small where ∇· is the divergence operator. The above relation must
area element on the moving interface. Note that the above be satisfied in each of the bulk regions s (t) and p (t) at
identity can be expressed in 2D by replacing volume integrals all times. Shrinking the control volume R (with r = ∅) to
by area integrals and area integrals by line integrals. As R the interface in (6) and using the identities in (4) and (5), the
shrinks to the interface the above Eq. (3) yields the limiting interfacial mass balance can be written as,
relation,
⎧ ⎫ [[c]]V = [[ J]] · n, (8)
⎨ ⎬ 
c dv →− [[c]]V da. (4)
⎩ ⎭
R r (t) which must be satisfied on the interface  int (t) at all times.
Note that the above equation is the Rankine-Hugoniot jump
As ∂ R approaches the interface from the solution or the condition in Eulerian description [48]. In the case of multiple
solid phase, the normal n R has the limit −n or n, respectively. species, bulk mass balance for each of the species in solution
Thus, for the bulk molar flux vector field J the following and interface mass balance for all the dissolving solid species
relation is obtained, needs to be considered.

123
616 Comput Mech (2014) 54:613–627

2.1.4 Diffusive flux
The driving force for diffusion is the gradient of the chemical
potential μ and the total atomic/ionic flux associated with c
is given by,
Note that i 0 is dependent on the temperature T and the pH of
the pit solution (electrolyte). During the activation-controlled
corrosion i A can be related to the molar flux of metal atoms
J m dissolving into the pit solution or to the normal interface
speed V according to Faraday’s laws of electrolysis as,

Dc i A = z F J m · n = z F V cs . (13)
J =− ∇μ, μ = μ0 + kB T ln (γ c) + z F E, (9)
kB T
Combining Eqs. (8), (10) and (13), the interface condition
where μ0 is the chemical potential at a reference state, kB for activation-controlled corrosion can be written as,
is the Boltzmann’s constant, T is the absolute temperature,
D is the diffusion coefficient or diffusivity, γ is the activ-
ity coefficient, z is the number of electrons involved in the
reaction, F is the Faraday constant, E is the electric poten-
tial and ∇ denotes the gradient operator. In this study, D is
assumed to vary linearly with temperature T as given by the
Einstein’s relation. For dilute solutions (i.e. γ ≈ 1), assum-
ing zero thermal gradients (i.e. ∇T = 0) and zero electric
potential gradient in the domain (i.e. ∇ E = 0), except for a
sharp potential drop across the pit interface  int , the diffusive
flux for the bulk field c is simply given by Fick’s first law,
J = −D∇c, (10)
2.1.5 Electrochemical kinetics
Metal corrosion usually occurs through electrochemical reac-
tions at the pit interface,  int , which acts as an anodic site.
When an anodic activation overpotential η A is applied, gener-
ally referred to as polarizing the metal, a current is established
and corrosion progresses due to the dissolution of the metal
at the anode. The overpotential is related to applied potential
E according to the relation η A = E − E corr , where E corr
is a material parameter called the corrosion or open-circuit
potential. The magnitude of the anodic current density i A is
given by the Bulter-Volmer equation, but when η A is not too
small, i A may be approximated by the Tafel equation [3],
in the solid domain:
αzη A F
i A = i 0 exp (11)
kB T
where i 0 is the exchange current density and α is the dimen-
sionless anodic charge transfer coefficient. The exchange cur-
rent density i 0 is a parameter that represents the current in the
absence of net electrolysis and at zero overpotential. Math-
ematically, i 0 can be thought of as a background current to
which the observed current i A at various overpotentials η A
is normalized. According to [12], i 0 can be related to the
dissolution affinity Adiss as,
 
iA
[[D∇c]] · n + [[c]] = 0. (14)
z Fcs
2.2 Modeling assumptions
The following assumptions were made for simplifying the
pit growth problem:
1. The motion of the pit interface is due to the dissolution
and diffusion of a single independent chemical compo-
nent in the pit solution [11,12]. Since only one charged
species (Fe2+ in aqueous solution) is considered, electro-
migration effects can be modeled by simply choosing an
appropriate diffusion coefficient. Also, the aqueous pit
solution is assumed to be under stagnant conditions, so
mass transport is purely via diffusion. In a more gen-
eral case scenario, one should track the concentrations
of all the corrosion rate limiting species by considering
the flux contribution from electric potential gradient and
advection in addition to that from concentration gradient
[15,16]. Since the focus here is on developing the XFE-
LSM for modeling pit propagation only Fickian diffusion
of one rate-limiting species is considered.
2. The solid domain is homogeneous and local microstruc-
ture features such as precipitates are ignored. The con-
centration of metal atoms is therefore assumed a constant
c = csolid in s . (15)
Thus, there is no need to solve for mass balance in s
and the interface concentration cs = csolid at all times.
3. The diffusion rate of ions in pit solution is relatively much
faster compared to corrosion (dissolution) rate; so it is
reasonable to assume that the concentration of ions in
p at any time t is at a steady state, that is, c = 0. Using
this in Eq. (7) and combining with Eq. (10) gives the
steady state diffusion equation for Fe2+ ions in solution:

z F E corr
i 0 = z F Adiss exp (12) ∇ · J = ∇ · (D∇c) = 0 (16)
kB T

123
Comput Mech (2014) 54:613–627 617

For corrosion of stainless steels, it can be shown that rior Laplace problem. For activation controlled corrosion,
the steady-state assumption holds, using the analytical the variational or weak form can be written as follows:
solution of the 1D moving interface problem [11,49]. Find c ∈ C for all v ∈ V such that,
4. The temperature T and the applied overpotential η A  
are spatially constant at the pit interface  int , so the iA
− D ∇v · ∇c d + v d
molar flux J m is a constant along the interface during zF
 p
 int
activation-controlled corrosion. In addition, the precipi- 
i Ac
tation reaction products are assumed to be infinitely sol- = v d if cp < csat , (20)
z Fcsolid
uble in the solution, so the formation of a salt layer on  int
the pit interface is neglected. The formation of hydrogen
gas and changes in pH are also ignored. For this simple where C and V are spaces of sufficiently smooth functions for
case, the current density i A during activation-controlled the bulk field and their variations. For diffusion controlled
corrosion is spatially constant along the interface. corrosion, the use of Lagrange multipliers to enforce the
interfacial Dirichlet constraint results in the following mixed
2.3 Strong form of the free boundary problem variational form:
Find c ∈ C and λ ∈ L for all v ∈ V and u ∈ L such that,
The strong form of the boundary value problem for the metal   ⎫
 
concentration in the pit solution is given by, − D∇v · ∇c d+ λ c−csat d = 0,⎪ ⎬
⎫  p   int
∇ · (D∇c) = 0 in p , ⎬ u c d = u csat d, ⎪
⎭
p
c=0 on d , (17)  int  int
⎭
D∇c · n0 = 0 on h .s if cp = csat , (21)
When corrosion is activation-controlled, the normal inter- where L defines an admissible space for the Lagrange mul-
face speed V is directly known from the current density i A , as tipliers.
given by Eq. (13). When corrosion is diffusion-controlled, the
concentration at pit interface is given by the saturation limit
csat . This gives a Robin type condition (activation-controlled
process) or a Dirichlet type interface condition (diffusion- 3 Numerical implementation
controlled process) on the moving boundary  int depending
upon the local interface concentration cp as follows: In this section, the details of the XFE-LSM and the algo-
rithm are provided. The numerical implementation, herein,
  ⎫ is different from [41] in following ways: (1) The step enrich-
iA iA ⎪
if cP < csat −D∇cp · n + cp = ,⎪⎬ ment function is used instead of the discontinuous deriva-
z Fcsolid zF
on  int (t)
⎪
⎪ tive enrichment function; (2) the Lagrange multiplier method
⎭
else cP = csat , is employed for enforcing the Dirichlet interface condition,
(18) instead of the variationally inconsistent penalty method; (3)
a nonlocal domain integral scheme is used for evaluating the
By solving the above two Eqs. (17) and (18), the con- normal interface speed, instead of a direct evaluation scheme
centration field c(x, t) can be established in the pit solution based on the local concentration gradient; and (4) a bilinear
domain p (t). The normal interface speed under activation- rectangular finite element (FE) mesh is employed instead of
controlled cp < csat ) and diffusion-controlled corrosion a triangular FE mesh. The current XFEM-LSM implemen-
regimes (cp = csat ) is given by: tation uses a structured finite difference (FD) grid for the
⎧ level set evolution, whose nodes coincide with the nodes of
⎪ iA
⎪
⎪ if c p < csat ,
the structured bilinear FE (four-noded quadrilateral) mesh;
⎨ z Fcsolid
V = (19) therefore interpolation of the level set function φ between the
⎪
⎪ p·n
⎪
⎩− D∇c FD grid and the FE mesh is avoided at every time step. Since
if cp = csat , φ is continuous across the interface standard FE shape func-
c solid −c sat
tions are used to interpolate φ within finite elements. If the
2.4 Weak form FE mesh is unstructured or is composed of different order
elements (e.g. triangles or nine-noded quadrilaterals) or if
The above described boundary value problem along with the the FD grid is of finer resolution, then a bicubic interpolation
interface conditions belongs to the class of elliptic inter- scheme can be used to project φ from the FD grid to the FE
face problems. When D is constant it reduces to an inte- mesh.

123
618
3.1 The level set method
The level set method (LSM) for moving interfaces was orig-
inally introduced by Osher and Sethian [20,21], wherein the
interface location at any time t is given by the zero contour
of the scalar level set function, φ(x, t), that is,
 int = {x ∈  | φ(x, t) = 0}. (22)
Following this approach, the interface is implicitly repre-
sented by φ, such that φ = 0 on the pit interface  int , φ < 0
in the pit solution domain p , and φ > 0 in the solid domain
s . As corrosion progresses,  int (t) moves in the normal
direction with speed V and the level set function φ satisfies
the level set evolution equation in the whole domain,
∂φ
+ Vext
∇φ
= 0 in . (23)
∂t
where Vext is the extended normal interface speed. The above
level set evolution equation is a first order hyperbolic PDE
and is subjected to the following initial and boundary condi-
tions:
φ(x, 0) = ± min ||x − x  || in , (24)
x  ∈ int (0)
∇φ · n = 0 on . (25)
The above equations specify that φ is initialized using the
signed distance function to the interface and that the normal
flux is zero on the exterior boundary . The normal speed
is defined in the entire computational domain using velocity
extensions as, [22–24],

∇Vext · ∇φ = 0 in ,
(26)
Vext = V on  int .
The velocity extension procedure is necessary because the
normal interface speed V is known only at points that lie on
the interface; however, the LSM requires that V be defined
at all nodes in the FD grid. Note that Eq. (26) is derived such
that it preserves the signed distance property of the level set
function as it is evolved [23]; therefore, reinitialization of the
level set function is seldom required.
The level set evolution equation is solved using an upwind
finite difference scheme and the fast marching method [24].
The explicit forward Euler scheme is employed to update
φ using a stable adaptive time step given by the Courant-
Friedrichs-Lewy (CFL) condition [50],
h min
t ≤ , (27)
Vmax
where h min is the minimum FD grid size and the maximum
interface speed Vmax = max{V (x  , t)} for all x  ∈  int (t).
The motivation for using the LSM rather than an explicit
123
Comput Mech (2014) 54:613–627
tracking method (e.g. marker particle method [51]) is that
the LSM can handle arbitrary topological transitions such as
corrosion pit merging (see Fig. 8c). This is important as corro-
sion pit morphologies can evolve into complex shapes due to
undercutting, subsurface pitting, and vertical and horizontal
grain attack [7]. The LSM is relatively expensive compared to
the particle methods due to the solution of hyperbolic level set
equation and the CFL condition (27) for stability; however,
one needs to pay this extra cost for a more robust handling
of interface topology. An alternative numerical implementa-
tion of the LSM could utilize a Stream-line Upwind Petrov-
Galerkin (SUPG) finite element scheme. Although the SUPG
finite element level set scheme completely avoids the need
for interpolation of φ and is second order accurate [52], it will
be computationally much more expensive than the LSM.
3.2 The extended finite element method (XFEM)
The XFEM is used to discretize the weak form of the interior
Laplace problem defined by (20) and (21). Note that the con-
centration field c(x, t) and its normal derivative ∇c · n(x, t)
are discontinuous across the pit interface  int (t) due to the
different metal ion concentrations and fluxes in the solid and
solution phases. Therefore, the enriched approximation is
defined as,

n e (t)
n
c(x, t) = N (x)c (t) +
A A
S B (x, t)a B (t), (28)
A=1 B=1
where N A (x) are the standard finite element shape functions,
c A are nodal degrees of freedom (DOFs), n is the total number
of nodes in the mesh, a B are the nodal enrichment DOFs
(which are additional DOFs at the enriched nodes), n e (t) is
the total number of enriched nodes in the mesh at time step t,
and the step enrichment function corresponding to enriched
node B, is defined as,
 
S B (x, t) = N B (x) H(φ(x, t)) − H(−φ(x, t)) , (29)
where H(φ) is the Heaviside step function given by,

1 i f φ > 0,
H(φ) = (30)
0 i f φ < 0.
Unlike the discontinuous derivative enrichment function
used in [41], S incorporates a discontinuity in the value of
the unknown field across the interface; however, S itself does
not enforce the jump in value or normal derivative across
the interface, so interface conditions need to be enforced
for the problem to be well-posed. In the pitting corrosion
problem, since the concentration is only changing in p ,
during diffusion-controlled corrosion the jump in concentra-
tion is captured by enforcing a one-sided Dirichlet constraint
Comput Mech (2014) 54:613–627
cp = csat on the moving interface using Lagrange multipli-
ers as described in Sect. 3.3; and during activation-controlled
corrosion the jump in the normal derivative is captured by
adding interface line source terms corresponding to a one-
sided normal flux (i.e. f c and f a ) to the right hand side of the
system matrix, defined in Sect. 3.4. A more detailed account
on incorporating intra-element strong and weak discontinu-
ities is given in [53].
3.3 Imposition of the interfacial constraints
In order for the pitting corrosion problem to be well-posed,
boundary conditions must be enforced on the moving inter-
face. Previously in [41], the penalty method was used to
enforce Dirichlet conditions on the moving interface, but
this approach is variationally inconsistent. For the sake of
accuracy, one must choose the penalty parameter to be sev-
eral orders of magnitude larger than the diffusion coefficient;
however, choosing a large penalty parameter often leads to ill-
conditioning of the system matrix which could lead to erro-
neous results or even singular systems. Instead, herein the
variationally consistent Lagrange multiplier (LM) method
is employed to enforce the Dirichlet conditions on the pit
solution side of the interface under diffusion-controlled cor-
rosion. In the current scheme, a 2D mesh consisting of four-
noded (bilinear) square finite elements is used to discretize
the bulk concentration field. Next, a 1D interface mesh that is
independent of the underlying 2D mesh is constructed such
that there is only one LM node per interface segment con-
tained in a bulk enriched element, as shown in Fig. 2. If the
length of the interface segment in an enriched element is
small then LM node is not added for this segment, so as to
improve stability. On this interface mesh, the LMs are inter-
polated using piecewise linear functions as [54],

m(t)
λ= N̂ A λ A , (31)
A=1
Fig. 2 The 2D XFE mesh and the corresponding 1D Lagrange multi-
plier mesh used for the initially circular pit interface are shown. Notice
that the XFE-LSM bulk mesh is independent of the embedded interface,
so there is no need to remesh or move the mesh as the pit grows, which
leads to computational efficiency
619
where N̂ A are the standard 1D FE shape functions, λ A are
LM nodal DOFs and m(t) is the total number of LM nodes
at time step t. This strategy for generating the LM mesh
[54] has many similarities with the mortared finite element
method presented in [55].
A key challenge in using Lagrange multipliers (LMs) for
enforcing Dirichlet constraints on embedded interfaces in
conjunction with the XFEM lies in the construction of a sta-
ble discrete LM space L. A poor choice of L often leads to
spurious oscillations in the multipliers referred to as bound-
ary locking effect, which has been reported in several of the
studies cited below. To resolve this issue, the vital-vertex
algorithm was proposed in [56–58], which constructs a sta-
ble reduced LM space that passes the numerical inf-sup test;
however, its implementation is relatively complex compared
to our implementation. Although some oscillations in the LM
values were noticed in the current implementation, the mag-
nitude of these oscillations was relatively small; and by using
a smoothing procedure based on the domain integral scheme
[31] interface fluxes can be recovered accurately, as described
in sect. 3.5. An alternative approach for imposing the inter-
face Dirichlet condition involves the Nitsche’s formulation
[59], which could be computationally more efficient and be
readily extensible to three-dimensions; moreover, it can lead
to optimal convergence [60–65], and possibly, eliminate the
need for the smoothing procedure.
3.4 Discrete equations
Upon introducing the XFE and FE approximations into the
weak form (20) and (21), the following linear algebraic sys-
tem is obtained: for activation-controlled corrosion,
Kcc Kca c fc
= , (32)
Kac Kaa a fa
and for diffusion-controlled corrosion,
⎡ ⎤⎡ ⎤ ⎡ ⎤
Kcc Kca Gc c 0
⎣ Kac Kaa Ga ⎦ ⎣ a⎦ = ⎣ 0 ⎦ , (33)
(Gc )T (Ga )T 0 λ g
where c, a, and λ are the arrays containing the stan-
dard, enriched and Lagrange multiplier DOFs, respectively;
Kcc , Kca , Kac and Kaa are the standard and enriched tangent
matrix terms; f c and f a are the standard and enriched vec-
tors of the line source terms, respectively; Gc , Ga , and g are
the matrix and vector terms corresponding to the Lagrange
multipliers. The domain integrals corresponding to all these
matrices and vectors are given in Appendix A. The concentra-
tion field c(x, t) is obtained by solving the above linear sys-
tem. The interface speed can then be computed as described
in the next section.
123
620
3.5 Domain integral evaluation of the normal interface
speed
As described in Sect.2, for diffusion-controlled corrosion
(cp = csat ), the normal interface speed V is given in terms of
the normal interface flux D∇cp · n on the pit solution side,
according to Eq. (19). However, a direct evaluation of the flux
using the local concentration gradient at a point on the inter-
face, as previously proposed in [41], can give rise to errors
in V and will yield a poor quality interface topology [66].
Although the LM nodal values can be interpreted as interface
fluxes, they do not provide a good estimate because the 1D
interface mesh is chosen to be sufficiently coarse for stability
reasons. Also, there could be minor oscillations in the LM
nodal values as discussed Sect. 3.3. Instead a domain integral
scheme proposed in [31] gives a better approximation of the
normal interface flux, which is used herein to calculate V .
Let us now briefly review the procedure to approximate the
flux D∇cp · n at a point x ∗ on the pit interface  int using the
domain integral scheme. Consider a section of the interface
∗int containing the point x ∗ , within compact support ∗ of a
scalar weight function w∗ . Upon multiplying the first equa-
tion in (17) by w ∗ , integrating over ∗ by parts and then
applying the divergence theorem, one can obtain the follow-
ing relation:
 
D ∇w ∗ · ∇c d = w ∗ D∇cp · n d. (34)
∗ ∗int
Next, let us adopt a first order approximation by assum-
ing the normal derivative D∇cp · n to be constant over ∗int .
Thus, a simple approximation for the normal component of
the concentration flux at x ∗ ∈ ∗int , when the interface is
approached from p , can be written as,
 with the aim of validating the approach by comparing our
 ∗ ∇w ∗ D · ∇c d
D∇c · n x ∗ =
p 
∗
. (35)
 int w d
∗ [67] and numerical studies [12]. Second, accelerated foil cor-
As noted in [31], the above result is independent of the par-
ticular choice of the weight function w ∗ , so there are several
 in two-dimensions.
ways to construct the approximation. Herein, D∇cp · n x ∗ is
evaluated by: (1) identifying the nodes of the finite element
containing x ∗ ; (2) evaluating the contribution of those nodes
to the normal flux on the pit solution side; and (3) interpolat-
ing the value at x ∗ using these nodal contributions according
to the standard finite element approximation as,
 
NA ∇w ∗ D · ∇c d
 A  in electrolyte solution so that only one end of the wire was
D∇cp · n x ∗ =  
A
(36)
w ∗ d
e∈ A int
A
123
Comput Mech (2014) 54:613–627
where  A denotes the support of the FE node A and  int A is
the interface segment contained in an element e that belongs
to the support  A . Finally, the interface speed at point x ∗ is
calculated according to Eq. (19) as,

∗
D∇cp · n x ∗
V (x , t) = − . (37)
csolid − csat
The above procedure is a nonlocal scheme for calculating
V and yields a better approximation compared to the local
scheme implemented in [41].
3.6 Algorithm
The strategy here is to adopt a staggered explicit time scheme,
and the algorithm for evolving the corrosion front at time t
is:
1. Project the level set function φ from the FD grid onto the
XFE mesh;
2. Assemble the linear systems in Eq. (32) or (33) using the
XFEM and solve for the concentration field c(x, t) in p ;
3. Compute the normal interface speed V according to Eq.
(37) using the domain integral scheme, as described in
Sect. 3.5;
4. Solve the interface evolution Eq. (23) using the LSM and
the explicit forward Euler method, as described in Sect.
3.1;
5. If t < tfinal then go to step 1, else end computation.
4 Numerical results
In this section, two types of numerical experiments are simu-
lated. First, the pencil electrode corrosion tests are simulated
numerical results with those from published experimental
rosion tests are simulated to predict corrosion morphologies
with the goal of demonstrating the viability of the approach
4.1 Pencil electrode corrosion test
4.1.1 Experimental validation
Let us first simulate the 1D pencil electrode experiments
described in [67], wherein a stainless steel (304 SS) wire
of 50 μm diameter is mounted in epoxy resin and immersed
exposed to the solution. In this case, the concentration gradi-
ent is only along the longitudinal axis of the wire (i.e. a 1D
problem), so it is reasonable to model this as a flat interface
Comput Mech (2014) 54:613–627 621

Table 1 Model parameters and constants used in this study

Parameter Value Units Source

Adiss 4.0 mol/cm2 /s [12]

csat 5.1 mol/l [68]
csolid 143 mol/l [9]
D(T = 25 ◦ C) 0.824 × 10−5 cm2 /s [9]
E corr −0.24 mV [69]
F 96485.53 C/mol -
kB 8.314 J/mol./K -
z 2.19 - [11]
α 0.65 - [12]
Fig. 3 A schematic diagram of the pencil electrode corrosion test. The
side walls are made of non-corrosive epoxy resin and so they serve as
zero flux boundaries. The pit depth d is the distance between the pit
mouth and the metal surface to the anodic metal dissolution, the anodic current density i A
provides a good estimate of the rate of corrosion. Figure 4d
shows that pit depth increases linearly with the inverse of the
in a rectangular domain with gradients only in the x2 direc-
current density i A , which is also consistent with experiments.
tion. Figure 3 shows the schematic diagram of the test set-up
along with the domain–boundary definitions. The numeri-
cal results are obtained using a 2D computational domain 4.1.2 Numerical validation
that is 0.16 mm (length x1 ) × 0.16 mm (height x2 ) with
a flat initial interface of height x2 = 0.157 mm and a flat Let us next consider three different values of overpotential
pit mouth boundary at x2 = 0.16 mm. The initial pit depth η A =100 mV, 140 mV, 200 mV and compare our numerical
d = 3 μm is the distance between the pit mouth and the metal results with those of [12] obtained from a finite volume model
surface. Thus, the 2D numerical problem is constrained to (FVM). For this study, D = 0.85 × 10−5 cm2 /s, according to
mimic 1D experimental set-up. The experiments were con- [12]. The same domain and mesh discretization as described
ducted at a constant applied potential of E = +600 mV above is employed. The scatter (diamonds, circles, squares)
versus the reference Saturated Calomel Electrode (SCE) at a of the numerical curves shown in Fig. 5 is obtained from Fig.
temperature of T = 15 ◦ C so that diffusion-controlled sta- 6 in [12]. For the low overpotential η A = 100 mV, corrosion
ble pitting occurs. The diffusion coefficient at T = 25 ◦ C is activation-controlled, so the current density i A is constant
is reported to be D25 = 0.824 × 10−5 cm2 /s by Gaudet et throughout the simulation. Therefore, the pit depth versus
al. [9], and using Einstein’s relation (kinetic theory) one can time plot is a straight line as shown in Fig. 5a and b. For
obtain D15 = 0.796 × 10−5 cm2 /s. The concentration on the intermediate overpotential η A = 140 mV, corrosion is
p initially activation controlled, although after 40 seconds the
the pit mouth d = {x ∈  | x2 = 0.16 mm} is fixed at
zero and the concentration at the pit interface  int is fixed process becomes diffusion-controlled. This is evident from
at csat = 5.1 mol/l [68]. All the model parameter values are the kink in the pit growth rate and current density curves
listed in Table 1. In all the simulations, the finite difference in Fig. 5. For the high overpotential η A = 200 mV, corro-
(FD) grid for the level set method is chosen so that the spa- sion process is diffusion-controlled right from the beginning,
tial coordinates of the FD nodes coincide with those of XFE and the current density is inversely is proportional to time.
nodes. For this problem, an XFE mesh consisting of 200 × As expected the XFE-LSM results match exactly with those
200 elements is employed, so the FD grid consists of 201 × from the FVM, which validates the proposed approach. The
201 nodes. Under the steady state assumption, the average main advantage of the XFE-LSM over the FVM is its ability
ion concentration field in the pit solution varies linearly with to accurately evolve realistic corrosion pit morphology.
depth in p as shown in Fig. 4a. The numerical results of
real-time pit growth and current density are compared with 4.2 Accelerated foil corrosion test
the experimental data of [67] in Fig. 4b and c. The scatter of
the experimental data points is obtained from Figs. 2 and 5 in 4.2.1 Growth of an isolated pit
[67], and the data was adjusted by taking time t = 25 seconds
as t = 0 so as to only consider the regime when η A is truly Let us next simulate the growth of a single isolated pit
constant in the experiment. As expected, during diffusion- similar to the experiment conducted by Ernst and Newman
controlled corrosion the pit depth increases linearly with the [67], wherein a thin stainless steel (SS) foil was sandwiched
square root of time (see Fig. 4b). Since pit formation is due between two optical glass plates so that only one edge is

123
622 Comput Mech (2014) 54:613–627

(a) (b)

(c) (d)
Fig. 4 Comparison of our numerical results (lines) with the experi- depth increases linearly with the square root of time and with the inverse
ments results (scatter) reported in Figs. 2 and 5 in [67]. The excellent of current density as expected for a diffusion-controlled corrosion
agreement of the results demonstrates the validity of the model. The pit

80
10

60 8

6
40
4

20
2

0 0
0 20 40 60 80 100 0 20 40 60 80 100

(a) (b)

Fig. 5 Comparison of our numerical results obtained using the circles, squares) in subfigure (a) is obtained from Fig. 6 in [12] and
extended finite element and level set method (XFE-LSM) with the the lines show our numerical results. The current density is constant
numerical results of Scheiner and Hellmich [12] obtained using the with time during activation-controlled corrosion and is inversely pro-
finite volume method (FVM). The scatter of the data points (diamonds, portional to time during diffusion-controlled corrosion

exposed to the solution. The exposed surface of the foil 2D idealization of the problem is reasonable as experimen-
was coated with lacquer leaving only a small square area tal observations support the assumption of uniformity in the
of 250 μm2 in contact with the pit solution. In this case, a x3 (thickness) direction. The test set-up can be described

123
Comput Mech (2014) 54:613–627
(a)
0.6
0.55
0.5
0.45
0.2 0.3 0.4
(c)
Fig. 6 Comparison of semi-circular shape pit growth with experiments of Ernst and Newman [67]. The pit is grown from the edge of a 304 stainless
steel (SS) foil where the edge was covered with lacquer except for a small hole that is ≈ 250 μm2
by the schematic diagram in Fig. 1, except that the inter-
face shape is semi-circular. The experiment was conducted
at a constant applied potential of E = +600 mV versus
the reference Saturated Calomel Electrode (SCE) at temper-
ature T = 20 ◦ C so that diffusion-controlled stable pitting
occurs. Using Einstein’s relation, the diffusion coefficient at
T = 20 ◦ C is calculated to be D20 = 0.8102 × 10−5 cm2 /s.
The 2D computational domain is taken to be 0.6 mm (length
x1 ) × 0.6 mm (height x2 ) with an initial pit of diameter 0.016
mm so as to mimic the physical experimental set-up of [67].
As corrosion progresses the pit grows wider and deeper, but
the pit mouth is assumed to remain 0.016 mm wide and the
rest of the top boundary is a zero flux boundary because it
is coated with lacquer. The concentration at the pit mouth
p
d = {x ∈  | 0.292 mm ≤ x1 ≤ 0.308 mm, x2 = 0.6 mm}
is fixed at zero and the concentration at the pit interface  int
is fixed at csat = 5.1 mol/l using Lagrange multipliers. The
numerical results were obtained using an XFE mesh consist-
ing of 600 × 600 elements. A typical field plot of the average
ion concentration in the solution domain is shown in Fig. 6a.
The maximum pit depth is plotted as a function of time in Fig.
6b, which plateaus as the corrosion rate decreases with time
under diffusion-control. Next, a numerical convergence study
of the XFE-LSM is conducted by considering 3 different XFE
mesh resolutions consisting of 600 × 600, 400 × 400, 200
623
200
150
100
50
0
0 250 500 750 1000
(b)
(d)
× 200 elements. The results from these 3 meshes overlap
with each other demonstrating good convergence; however,
the simulation predicted smaller pit depth at t = 720 seconds
compared to the experiment, as indicated by data point (red
square) in Fig. 6b. This discrepancy could be arising because
of: (1) uncertainty in the value of diffusion coefficient at dif-
ferent temperatures; and (2) factors such as electro-migration
and activity of ions in the saturated or super-saturated pit
solution. To address this discrepancy, the model may need to
be extended by incorporating the Nernst-Planck-Poisson for
electro-diffusion as opposed to Fickian diffusion, in conjunc-
tion with more details experiments. Finally, from Fig. 6c it
is evident that an isolated pit grows as a semi-circular shape
throughout the diffusion-controlled corrosion process, which
is qualitatively consistent with the observations of Ernst and
Newman [67] shown in Fig. 6d.
4.2.2 Pit shape evolution
Let us next examine the morphology evolution of an iso-
lated semi-elliptical (crack-like) pit during activation- and
diffusion- controlled corrosion processes. The same domain
and XFEM mesh as above is employed and initialized with a
semi-elliptical pit with a major axis length 0.032 mm and a
minor axis length 0.008 mm. For activation-controlled cor-
123
624
0.6
0.58
0.56
0.54
0.25 0.3 0.35
(a)
0.6
0.59
0.58
0.57
0.28 0.3 0.32
(c)
Fig. 7 Comparison of pit morphologies under activation- and
diffusion-controlled corrosion processes. The numerical results of pit
interface evolution show that the activation-controlled process (a, c) pre-
serves the semi-elliptical shape of the pit, whereas diffusion-controlled
rosion η A = 100 mV and for diffusion-controlled corrosion
csat = 5.1 mol/l. The numerical results of pit interface evo-
lution, in Fig. 7a and b, show that the semi-elliptical shape
of the pit is preserved during activation-controlled corro-
sion, whereas the pit morphology transitions into a semi-
circular shape during diffusion-controlled corrosion. This
happens because the corrosion rate at the interface during
an activation-controlled process is spatially constant for a
given T and η A . Therefore, V is constant along the interface,
as indicated by length of the arrows in Fig. 7c. On the other
hand, in a diffusion-controlled process the corrosion rate at a
point on the interface is inversely proportional to its distance
to the pit mouth, so V is larger at points on the interface that
are closer to the pit mouth, as shown in Fig. 7d. Thus, the
pit shape is preserved only during an activation-controlled
process, which was also pointed out in [12,70].
4.2.3 Growth of multiple pits
Let us next investigate the morphology evolution of multi-
ple closely spaced pits during diffusion-controlled corrosion.
Ernst and Newman [67] experimentally observed pits that
123
Comput Mech (2014) 54:613–627
0.6
0.58
0.56
0.54
0.25 0.3 0.35
(b)
0.6
0.59
0.58
0.57
0.28 0.3 0.32
(d)
process (b, d) smoothens the pit into a semi-circular shape. The nor-
mal interface speed is spatially constant during the activation-controlled
corrosion
grow as elongated elliptical shapes with lacy metal cover
formation on the top boundary. The mechanisms behind the
formation of the lacy cover are complex; however, the perfo-
rated cover leads to the evolution of elongated pit shapes. To
illustrate the role of the perforated metal cover, a 2D com-
putational domain that is 0.36 mm (length x1 ) × 0.36 mm
(height x2 ) is initialized with several small semi-circular pits,
each of diameter 0.004 mm, along the top boundary of the
domain. The domain is discretized using an XFE mesh con-
sisting of 200 × 200 elements. In this case, since there was
lacy cover formation on the exposed surface due to numerous
small pits, the assumption of uniformity in x3 direction is not
strictly valid, and so the 2D idealization of the problem is a
simplifying approximation. Another assumption here is that
there is no change in the protective layer on the metal surface
as corrosion progresses via metal dissolution inside the pit
beneath the lacy cover. Therefore, the pit mouth of each pit
remains 0.004 mm wide even as the pits grow and coalesce,
which can be clearly seen from the field plot of the concen-
tration variable as shown in Fig. 8a. The pit is evolved under
a diffusion-controlled corrosion process at T = 15 ◦ C and
E = +600 mV (SCE) for about 300 seconds and the corre-
Comput Mech (2014) 54:613–627
(a)
0.36
0.3
0.24
0 0.06 0.12 0.18 0.24 0.3
(c)
Fig. 8 Multiple pit growth in SS foils with partially broken passive layer on the top surface. The coalescence of nearby pits leads to the formation
of elongated elliptical pits. The numerical pit shapes are in qualitative agreement with the experimental shapes
sponding maximum pit depth is plotted as a function of time
in Fig. 8b. The model seems to predict a faster rate of corro-
sion as compared to the experiment at t = 240 seconds, as
indicated the data point (red square) in Fig. 8b. This discrep-
ancy may be attributed to the 2D idealization and arbitrary
choice of the initial pit locations and sizes. Figure 8c shows
that the individual pits initially grow as circular shapes but
soon coalesce to form an elongated elliptical shape. Thus,
this simulation study provides an explanation for the mecha-
nism behind the formation of elongated pits experimentally
observed by Ernst and Newman [67] shown in Fig. 8d.
5 Conclusion
A simple yet robust sharp interface formulation for model-
ing corrosion pit propagation in alloys is presented, within
the framework of the XFE-LSM. In contrast with existing
approaches based on the standard FEM or the FVM, the pro-
posed approach allows for an accurate representation of the
geometry of the corrosion front independent of the underly-
ing finite element mesh. The method is convergent and can
capture complex morphological transitions such as pit merg-
ing without requiring remeshing. The generalized Heaviside
or step function allows for the jumps in both the concentration
field and its normal derivative across the pit interface. The
domain integral scheme yields a good approximation of the
625
150
100
50
0
0 50 100 150 200 250 300
(b)
0.36
(d)
normal interface speed in conjunction with the Lagrange mul-
tiplier method. The numerical results from the pencil elec-
trode test are in excellent quantitative agreement with both
experimental and numerical results in the literature, demon-
strating the validity of the model for simpler pit geometries.
The foil corrosion test results are qualitatively consistent with
experiments, illustrating that the model is able to capture the
mechanisms of pit propagation under diffusion-controlled
corrosion. Only one experimental data point in time is avail-
able from the foil corrosion tests reported in [67], and the
predicted pit growth rates in the case of an isolated pit or
multiple pits do not agree quantitatively with the data. This
discrepancy could be arising because of the 2D idealization
and because the model does not consider complex phenom-
ena associated with activity of ions in concentrated solutions,
electro-migration, reactions, local microstructural features
and the effects of chloride ion concentration in pit solution.
Also, there is uncertainty associated with the model parame-
ters and experimental data that could be another source of
the discrepancy. Clearly, this work is only a first step toward
developing a comprehensive extended finite element model
for localized corrosion, and future work will focus on improv-
ing the model in conjunction with more detailed experimen-
tation.
Acknowledgments This work was supported by a start-up grant from
Vanderbilt University. The author is grateful to Dr. Chandrasekhar
123
626 Comput Mech (2014) 54:613–627

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 predicting localized pitting corrosion in a brine water-CO2 system.
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I
where superscripts A, B denote the nodal indices; N A is the
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