Materials and Corrosion 2012, 63, No.

9999

DOI: 10.1002/maco.201106404

Unified model for blister growth in coating degradation

using weight function and diffusion concepts
Y. Prawoto*
This paper discusses new conceptual and mathematical models for blistering
propagation especially useful for coating life assessment. It proposes new
equations governing blister development that combines fracture mechanics and
diffusion based concepts. The fracture mechanics concept is used to treat blister
growth as crack propagation, while the diffusion concept is used to treat the
ionic transport that eventually causes corrosion and blistering to occur. The new
equations are expected to be useful in coating development as well as coating
life assessment. Furthermore, with little modification, the equations are also
beneficial for other surface engineering methods.

1 Introduction
In general, coating deterioration and degradation could be
modeled in three ways [1]:

As a black-box statistical time to failure (such as lifetime
distribution);

As a grey-box stress-strength model based on a measurable
quantity indicating time-dependent deterioration and
failure;

As a white-box model through simulation of the physics of
measurable deterioration and failure.

In this research, the focus is on both the second and the third
methods with some manipulation similar to that of life
assessment methodology for metal structures [24]. A number
of papers have been written on the degradation of systems
exposed to outdoor weathering conditions. For example, Chan
and Meeker [5] relate degradation to environmental factors, such
as the weather. These factors are transformed into a degradation
rate. A time series modeling approach is proposed to predict daily
degradation. Other researchers describe how the maintenance
methodology from other field [6] is applied to protective paint
systems. The lifetime-extending maintenance model, in which
deterioration is modeled by a gamma process with expected
deterioration non-linear in time, is applied successfully to
optimize maintenance of the coating.
Physically among other deterioration parameters, the
adhesive strength is one of the most critical to use in life
Y. Prawoto
Faculty of Mechanical Engineering. University Technology Malaysia,
81310 UTM, Skudai, Johor (Malaysia)
E-mail: yunan.prawoto@gmail.com

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assessment, taking the advantage of the blister formation and

development as a symptom of the coating deterioration.
Although the surface engineering has developed beyond
coating [713], blistering remains one of serious problems and
important parameters [1417]. Therefore, an understanding on
the physical and metallurgical phenomena of blistering is
important from both scientific and engineering point of view.
However, many experimental researches on this subject results
solely in qualitative analyses [1823]. As such, this research aims
to develop new unified-governing equations for blistering
development that are easy to use. At the same time these
equations can be related to and compared with the existing
models [2432], which were started byQ2 Evans and Hutchinson
[26] with their conceptual observation published [33]. The fracture
mechanics concept is used to treat blister growth as crack
propagation [34], while the diffusion concept is used to treat the
ionic substance transport that eventually causes corrosion and
blistering to occur. The new equations are expected to be useful in
coating development as well as coating life assessment.

2 Blistering in coating degradation

Blisters are local defects that form because of the pressure exerted
by an accumulation of substrate at the coating-substrate interface
in conjunction with loss of adhesion and distention of the coating.
When impurity ions are present on the surface or leachable ions
are present in the coating, with sufficient amounts of water,
blisters or local osmotic cells can initiate in the coatings [24, 25,
35]. Typically the loss of coating adhesion is related with the
development of a cathodic area underneath the coating adjacent
to the defect. Oxygen also infuses the coating while ionic
materials are leached from the substrate or from the coating and
these all concentrate to make an electrochemical corrosion cell
beneath the blister. Several preliminary qualitative experiments
have been conducted and published (e.g. [36]), see Fig. 1.

2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Prawoto

Materials and Corrosion 2012, 63, No. 9999

defect:
1
H2 O O2 2e ! 2OH
2

(2)

The cathodic and anodic sites are connected by an electrolyte

layer. The corrosion products are formed and concentration
gradients of corrosive species are established, eventually, the
reaction sites separate and localize. This is a well-known
mechanism for the formation of blistering. The concentration
of sodium ions within the blister remains the same with that of
background levels during the initial stage as a moving interface
travels across channel between the scribe and blister. The time
taken for the interface to reach the blister is the initiation time,
blister formation time.
Once a blister is formed, the cathodic site grows to push the
coating layer away from the base metal appearing as blister
growing. The blister development in general is known by the
combination of internal pressure due to the cathodic reaction and
reduction of adhesion [12, 16, 18, 22, 24, 25, 35]. At this stage, ions
enter the blister as a result of both diffusion and transport caused
by the applied electric field [24, 25, 35]. Ions accumulate within
the blister but no longer only within the channel. The
concentration of ion rises within the blister during this period.
At the same time, the quality of the adhesion also decreases. As a
result, the blister size proliferates.
In this research, the mathematical model of the blistering
development is the focus. Figure 2 shows the two approaches
used in this research.
Figure 1. Blister formation on steel material coated with organic
coating [36]

One of the most severe forms of blistering is termed cathodic

blistering, which can occur when a coated metal with defects in
the coating is exposed to a deleterious environment, such as salt
spray or immersion in a salt solution [10, 16, 2325]. After
sufficient time, the blisters may enlarge to a point where adjacent
blisters coalesce. This can lead to complete detachment of the
coating from the substrate causing premature failure of the
organic coating system by delamination.

3 Analytical approach
3.1 Basic Concept
The growing anodic character at the defect area stimulates the
cathodic reactions adjacent to it. Cathodic blistering also can
occur when an electric potential is applied across the coated
objects. The defect serves as the anode where the iron is oxidized
by the half-cell reaction:
Fe ! Fe 2e

(1)

The other half-cell corrosion reaction, where the oxygen is

reduced, occurs under the coating a distance away from the

2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

equation missing. I
resupply with new
figure (see
attachement)

Figure 2. Introduction of weight function to simplify problems in

blister development

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Unified model forQ1 blister growth in coating degradation

Materials and Corrosion 2012, 63, No. 9999

3.2 Fracture mechanics and weight function approach

to blister development
The fracture mechanics part of the equation is discussed in detail
elsewhere [34] based on the strain energy density (SED) principle
using the weight function concept [3739]. Nonetheless, the
equations are briefly discussed for the sake of readers
convenience. When the polynomial curve fitting can be made
for the blister shape, the displacement can be expressed as:
ux; r yc 

Xn
xi
i0 r

(3)

where yc is the height of the blister, r is the blister radius, and x is

the distance from the center
R r of the blister. In this case, the value of
Kr2 a  yc , where a is 0 @ux; r=@r dx. Therefore, the weight
function becomes [34]:
H
hx; r p
a  yc

Zr

@ux; r
dx
@r

(4)

where H is the generalized modulus of elasticity. For the case

where the internal and external pressure difference is p, the SIF
(stress intensity factor) becomes:
E=1  v2
K p
a  yc

Zr

@ux; r
dx
@r

(5)

Therefore, the SIF for mode I and II can be written as:

p
p
a  E  py yc
a  E  px yc
KI
;
K

II
1  v2
1  v2

Figure 3. Experimental observation of the blister shape and

polynomial curve fitting

(6)

E is the modulus of elasticity. px and py are horizontal and vertical

components of the pressure, respectively. a can be computed
easily by curve fitting the shape of the blister by sectioning the
blistered sample (see Fig. 3). Our SED factor is as follows:
p
a  E yc
a11  px 2a12  px  py a22  py
S
1  v2

(7)

where a11, a12, and a22 are constants depending on the values of
the modulus and the Poissons ratio. Equation (7) can therefore be
used as part of governing equation for blistering development.
Figure 4 shows the comparison of the current model with
currently existing models, while Table 1 shows the tabular list of
the available models.
3.3 Diffusion concept to blister development
Diffusion describes the spread of particles through random
motion from regions of higher concentration to regions of lower
concentration [40]. The time dependence of the statistical
distribution in space is given by the diffusion equation. The
concept of diffusion is tied to that of mass transfer driven by a
concentration gradient, although diffusion can still occur when

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there is no concentration gradient. The following equation is the

basic diffusion concept [40]:
@fr; t
r  Df; rrfr; t
@t

(8)

where the f(r,t) is the density of the diffusing material at location

r and time t. Diffusion coefficient is D(f,r) for density f at
location r. The nabla symbol r is the del operator, which is
n
P
usually known as
ei @=@xi for general Cartesian space.
i1

Equation (8) shows that the diffusion equation is a partial

differential equation that describes density fluctuations in a
material undergoing diffusion.
While the previous part discusses about the blister
propagation purely from mechanics point of view, this part
discusses about the diffusion that causes the corrosion to occur
(see the upper part of Figs. 2 and 5). Referring to the figures,
corrosion products are formed at point A and concentration
gradients of corrosive species are established, eventually, the
reaction sites separate and localize. Once a blister is formed,
the cathodic site grows to push the coating layer away from the
base metal thus appearing as blister growing, pressure p.
The blister development in here is conceptually defined by the
combination of internal pressure due to the cathodic reaction and

2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Prawoto

Materials and Corrosion 2012, 63, No. 9999

Figure 4. Simplified normalized comparison of the current model with other available models varying the blister size and pressure [36]

Table 1. Available models that can be used for blister development/propagation [34]

Model

Developer

p
p  1  v2  t
, where t is the coating thickness
2

Bresser

p
p  C  yc  E, where C is the
constant dependent upon geometry

Galindo

p
p 1  v2

Jahnsen

2yc

 4 4 5 1=6
p r E
, where t is the coating thickness
17:4t

Kappes

reduction of adhesion, which is expressed as Scrit reduction. At

this stage, ions enter the blister as a result of both diffusion
and transportation, which is caused by other factors. This other
factors are later on be explored experimentally. This other factor
rectifies the value of the concentration gradient as our preliminary
experiment shows that blister keeps growing despite the

2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Model
p
a  E yc

1  v2
a11  px 2a12  px  py a22  py
p
p  yc 1  v2
, where f is the constant
2f

Developer
Prawoto

Volinsky

dependent upon geometry

p
E
Wan
5  C  p  yc , where C is the constant
2
dependent upon geometry
In alphabetical order. General description: p blister pressure,
yc blister height, t coating thickness, E Youngs modulus,
r blister radius.

concentration gradient shown in the equation shows otherwise.

Furthermore, it is also worth noting that the quality of the adhesion
also decreases. As a result, the blister size proliferates.
Therefore, mimicking the equation developed by earlier
researchers [24, 25], Equation (8) can be manipulated to
accommodate the physical observation here. The situation is

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Unified model forQ1 blister growth in coating degradation

Materials and Corrosion 2012, 63, No. 9999

The 3rd term,



1 @2 fr; t
;
r2
@u
vanishes in our model due to its characteristic and its magnitude.
Therefore, Equation (9) can be simplified to:
 2
 
@f
@ f 1 @f
@f
D 2
C1 C2
@t
@r
r @r
@t

(12)

The graphical representation of Equation (12) is shown in

Fig. 6, with the initial condition of corrosive ion concentration 100
and variation of C1 and C2. The simulation shown in this figure
was done by the following conditions:

At r 1, the concentration was 100, fr1 ; t 100.

The initial condition was that the concentration at r 1 was
close to 100 with the Dirac Delta function used. (Alternatively,
user can also use a normal distribution with the variance
of 1 to avoid the discontinuity of using step function,
fr1 ; t0 norm  dist100; 10; r )

The values of C1 varies from 0 to 0.1

The values of C2 varies from 0.1 to 0.1

Figure 5. Simplified conditions of the diffusion described with

cylindrical coordinate approach. The circle ring (upper) or the small
circle (lower) is the scribe that provides corrosive elements

shown in Fig. 5, where the model of concentration takes the

form of:
@fr; t
@fr; t
r  Df; rrfr; t C1
C2
(9)
@t
@t
where C1 and C2 are constants introduced here to accommodate
the combination of the electrolytic anodecathode system to
synergize with osmotically driven diffusion. This agrees to the
fact that physical observation of the blistering that the source of
the ion is also through the coating and it continuously grows
despite its obvious diffusional saturation. Therefore, for a start
these terms are independent of diffusion coefficient, D.
Similar approach was also used [24, 25]:
@fr; t
@fr; t
r  Df; rrfr; t mE
@t
@t

It is worth noting that the values of C1 and C2 vary depending

on the coating types, based materials to which the coating is
applied, and the environment. Experiment is needed to obtain
these constants. MathematicaTM [41] was used to numerically
solve the equation and subsequently graph the solutions. These
numerical trials (Fig. 6) show that with C1 and C2 being positive, a
more realistic model can be obtained. It is possible to simulate the
fact that the blister continues to grow despite the saturation of
the diffusion time.
Afterward, Equation (11), which was derived based on the
diffusion theory, can be related to Equation (7), which was derived
based on fracture mechanics. To do this some mathematical
manipulation was accordingly performed. Assuming that the
pressure built up underneath the blister, p  C3  fr; t.
Furthermore, the stress intensity factor is used as a conditional
judgment in which two different conditions are possible here.
Case 1, Blister propagation occurs.
If fr; t >

1  v2  Scrit
p
C3  a  E yc

(13a)

(10)
Case 2, Blister propagation does not occur

where m is the average mobility of ions and E is the strength of the

imposed unscreened electrical field.
Using the cylindrical coordinate, and assuming that D is a
constant, Equation (9) is given as:
2 2

 3
@ fr; t 1 @fr; t
7

6 @r 2
r
@r
@fr; t
@fr; t
6
7
D6  2
C2

7 C1
4 1 @ fr; t
5
@t
@t
r2
@u
(11)

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If fr; t 

1  v2  Scrit
p
C3  a  E yc

(13b)

where f(r,t) is the solution to Equation (11), and the rest of

the symbols are consistently the same with that of Equations (6)
and (7) and Equations (13a) and (13b) are comparable with
available solutions [26, 2833]. It is worth noting here that value
of the Scrit is a dynamic one, with a physical meaning that
its value decreases as the coating is used and exposed to

2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Prawoto

Materials and Corrosion 2012, 63, No. 9999

Figure 6. Implementation of Equation (9) with variation of constants

detrimental environments. To use the equations for coating

evaluation, profiling of the Scrit with respect to its lifetime
can be done for particular coating. The constants C1, C2,
and C3 are experimentally obtainable for almost any kind of
surface engineering and not limited to coating blistering.
These constant values for various conditions are to be reported
separately as the experiment is planned to be performed in the
near future.

2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

4 Conclusions
Equations (13a) and (13b) are the general solutions for this study
derived using the weight function concept combined with
diffusional principle. Despite accommodating modes I and II, the
equations are not complicated. They are as simple as the existing
ones, which neglect the mode II effect. The equations developed
in this research can be summarized as follow:

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Materials and Corrosion 2012, 63, No. 9999

Blistering propagation condition, expressed in Equation (7).

Blistering phenomenal cause, expressed in Equation (11).

Unified blistering propagation, expressed in Equations (13a)
and (13b).
Equations (7) and (11) can be used independently, in
conjunction with other available solutions, or as a unified model
expressed in Equations (13a) and (13b). The limitation of the
linear elastic fracture mechanics is carried over to the equations
derived; although the SED was proven to be applicable equally
well for the plastic case with and without dissipation [37, 38]. For
damage accumulation and material in homogeneity effects,
modification can be done to mimic [42, 43]. It is also worth noting
that preparation for large-scale experimental verification for
various conditions using various surface engineering methods is
undergoing.
Acknowledgements: This work was funding by the Government
of Malaysia through Research University Grant (RUG-GUP)
UTM number Q.J130000. 7124. 00H14, under the title of
Degradation of corrosion protective coatings on steel: computational and experimental approaches to blistering formation and
development is gratefully acknowledged.

5 References
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[13] C. Courcier, V. Maurel, L. Remy, S. Quilici, I. Rouzou,
A. Phelippeau, Surf. Coat. Technol. 2011, 205, 3763.

Unified model forQ1 blister growth in coating degradation

[14] K. Wan, K. Liao, Thin Solid Films 1999, 352, 167.

[15] J. H. Liang, C. H. Hu, C. M. Lin, Surf. Coat. TechnolQ3. (in
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J. Giridhar, Surf. Coat. Technol. 1998, 107, 1.
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Mater. 1992, 40, 295.
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[29] H. M. Jahnsen, Delamination of Coatings, in: J. Lemaitre,
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[39] Y. Prawoto, Application of Linear Elastic Fracture Mechanics in
Materials Science and Engineering, Lulu Enterprise, Morrisville 2011.
[40] W. Bolton, M. Philip, Technology of Engineering Materials,
Butterworth-Heinemann, Oxford 2002.
[41] M. L. Abell, J. P. Braselton, The Mathematica Handbook,
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(Received: October 13, 2011)
(Accepted: January 23, 2012)

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W6404

2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Prawoto

Materials and Corrosion 2012, 63, No. 9999

Keywords: coating degradation

fracture
interfaces
life assessment
micromechanics

Q1: Author: A running head short title was not supplied; please
check if this one is suitable and, if not, please supply
a short title that can be used instead.
Q2: Author: Please check the reference citations [26] and [33]
here.
Q3: Author: Please update year of publication, volume and page
number.
Q4: Author: Please update year of publication, volume and page
number.

2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

A1: Thats fine with me.

A2: Yup, they are fine.
A3: correction made.
A4: correction made.
Additional corrections:
1. My institution is Universiti
Teknologi Malaysia
2. Equation (7) is inaccurate, see
attachement
3. Table 1 also there is some inacuracy
in the equation, see attachement
4. Figure 2 also appeared wrong. It
does not display the symbol correctly.
see attachement for the replacement of
this.
5. Text for graphical abstract:
This is a new unified model for blister
growth in coating degradation utilizing
the fracture mechanics and diffusion
concepts.

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