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J. Coat. Technol. Res.

, 8 (2) 255263, 2011


DOI 10.1007/s11998-010-9296-8

Determination of epoxy coating wet-adhesive strength using


a standardized ASTM/ISO scratch test
Han Jiang, Robert Browning, Peng Liu,
T. A. Chang, Hung-Jue Sue

ACA and OCCA 2010


Abstract A new approach for evaluating the wetadhesive strength of epoxy-based coatings was carried
out based on a recently standardized ASTM/ISO
scratch test. A linearly increasing scratch normal load
was applied during scratch to induce progressively
increased delamination stress at the coating and steel
substrate interface. Thus, the applied critical load to
cause coating debonding can be experimentally determined. To find out the corresponding stress magnitude
to incur coating debonding, finite element methods
(FEM) modeling was conducted to analyze the stress
fields around the scratch tip during scratching. The
wet-adhesive strength is then quantitatively determined. Based on the above methodology, investigation
on a set of model coating systems suggests that the
critical load for coating delamination is significantly
influenced by water exposure time, coating thickness,
and substrate surface roughness. By combining the
standardized scratch tests and FEM modeling, the
proposed approach is found to be effective for quantitative assessment of epoxy coating wet-adhesive
strength and for the development of high performance
protective coatings for various industrial applications.
Keywords Epoxy coating, Wet-adhesive strength,
Debonding, Scratch, Finite element modeling

H. Jiang, R. Browning, P. Liu, H.-J. Sue (&)


Department of Mechanical Engineering, Polymer
Technology Center, Texas A&M University, College
Station, TX 77843-3123, USA
e-mail: hjsue@tamu.edu
T. A. Chang
PolyLab LLC, Houston, TX 77042, USA

Introduction
Polymeric coating adhesion to metal substrate is critically
important for various industrial applications.18 It is
particularly true when the coating systems are subjected
to environmental degradation, thermal degradation, and
mechanical impact, which can further weaken the coating
adhesive strength.1,2 One such example is the utilization
of fusion-bonded epoxy (FBE) coating to protect steel
pipes against corrosion for oil and gas pipeline applications. The integrity of FBE coating adhesion on steel
substrate is critically important for preventing corrosion
and for extending service life of steel pipes.
Numerous research efforts have been carried out
and many methodologies, such as impact tests, bend
tests, pull-off tests, blister test, acoustic emission, etc.,
have been employed to evaluate coating adhesive
strengths.38 Assessment of the wet-adhesive strength,
i.e., the adhesion performance under wet condition of
FBE coatings on steel substrate is crucial for the
pipeline coating industry. While quantitative assessment of adhesive strength under dry condition can be
easily made by most of the above test methods, their
usage for coating adhesive strength measurement
under wet environment is not considered reliable due
to their difficulties in sample preparation and in data
analysis. Thus, these methods are only suitable for pass
or fail evaluation of the coating wet adhesion performance. A reliable test method that can provide
quantitative assessment of the coating-metal adhesive
strength under a wet environment is still lacking.
Although significant research efforts have been
performed on scratch of metallic/ceramic coatings,912
few have been focused on the study of scratch behavior
of polymeric coatings. A recent development of the
polymer scratch test method (ASTM D7027-05 and
ISO 19252:2008),1315 which has been demonstrated to
be effective for quantitative scratch performance
evaluation of bulk polymers,1518 can also be adopted

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J. Coat. Technol. Res., 8 (2) 255263, 2011

for polymer coating study. Our previous effort on


scratching of acrylic coatings on steel substrate showed
that various types of coating damage modes, including
coating delamination,19 were observed (Fig. 1). Since
coating wet-adhesive strength is highly sensitive to how
the samples are prepared, the proposed scratch test,
which requires little or no special sample preparation
or handling, is suitable for investigating the wetadhesive strength of coatings. It is thus anticipated
that the above scratch approach will work for quantitative determination of the wet-adhesive strength of
FBE coatings on steel substrate.
Three-dimensional (3-D) finite element methods
(FEM) analysis has been adopted to simulate a
progressively increasing normal load scratching process
and shown to be effective for understanding the
scratch-induced damage mechanisms.2022 To quantitatively determine the coating adhesive strength, the
onset normal load of scratch-induced debonding can be
experimentally obtained. By a correlation between
the experimentally observed coating delamination and
the corresponding stress state and magnitudes obtained
by FEM modeling, it becomes possible for quantitative
determination of the coating wet-adhesive strengths.
The objective of this study is to establish an effective
test method for the quantitatively measurement of wetadhesive strength of FBE coating on steel substrates. It
is anticipated that the testing methodology proposed in
this research will assist coating formulators as well as
pipeline fabricators to develop high performance
coatings that will meet the demands of the oil and
gas pipeline industries.

Experimental

50 and 100 lm, applied on both smooth (Ra = 3.5 lm)


and roughened (Ra = 64 lm) steel surfaces. System II
is based on 3M Scotchkote 626-140 FBE (dry Tg =
140C and wet Tg = 134C) with DFT of 100, 200, and
300 lm, which was prepared by spray coating on a flat,
smooth steel substrate preheated at 177C. The samples were then post-cured for 10 min at 249C,
followed by air cooling.
Sample water immersion conditioning
The coating panels were exposed to hot water at 80C
for System I and 95C for System II, respectively, using
a custom-built water immersion set-up. Thermal couples were installed for temperature reading and control. Foam insulation layers were incorporated to help
maintain the designated temperatures for a specified
period of time from 1 day to 2 weeks to probe the
coating residual adhesive strength.
Determination of adhesive strength via scratch test
After the prespecified time of water immersion at
elevated temperatures, the specimens were removed
from the hot water tank and rinsed with tap water and
wiped dry before scratch testing. The scratch tests were
performed immediately using a commercially available
scratch test apparatus (Surface Machine Systems,
Model G4, www.surfacemachines.com). A linearly
increasing normal load scratch test, ranging from 1 to
95 N, was conducted on most samples. The scratch
velocity and length were set at 100 mm/s and 100 mm,
respectively. A 2-mm diameter spherical tungsten
carbide tip was chosen for the scratch test.

Model coating systems


Two commercially available high Tg epoxy coating
systems were chosen for this study. System I is
an experimental bisphenol A epoxy-based coating
(Tuboscope), having a dry-film-thickness (DFT) of

Determination of critical load of coating


debonding
To experimentally detect the critical load of coating
debonding, three different methods were chosen: (1)

Fig. 1: Typical scratch-induced damage patterns of an acrylic coating system. (a) Three damage zones are observed:
zone 1coating debonding, zone 2in-layer cracking, and zone 3buckling damage, (b) onset of in-layer cracking,
and (c) onset of buckling damage18

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J. Coat. Technol. Res., 8 (2) 255263, 2011

direct visual observation, (2) exposure of the scratched


samples to oxidative liquid, and (3) laser confocal
scanning microscopy (LSCM) examination of surface
profile changes. For a linearly increasing normal load
scratch test, once the onset of the scratch-induced
debonding is detected based on the above methods, the
critical load value for coating delamination can be
easily determined by measuring the distance of onset
delamination from either the start or the end of the
scratch point.
Similar to the scratching of transparent coatings,19
the delamination onset of thin opaque coatings can be
readily detected by visual observation. Upon coating
debonding, the light can penetrate through the thin
opaque coating and scatter more light on the delaminated surface. The very first location of such a visual
change in appearance is the onset of coating delamination. Figure 2 shows the onset delamination phenomena for Systems I and II after 1 day of water immersion.
The yellow circles indicate the location of onset of
sample color change, i.e., coating delamination.
For thicker opaque coatings, their delamination
phenomenon cannot be directly observed by the naked
eye. Alterative methods have to be employed. One
approach is to expose the scratched samples to oxidative liquid by which the delaminated region will be
oxidized easily. With an open cut on a more severely
scratched coating region, the sample was then
immersed in DI water containing 5 vol.% chlorine
bleach for 6 h. If coating debonding is present along
the scratch path, the steel surface will be directly
exposed to the oxidative liquid and rust readily.
Subsequently, the rust can be observed after peeling
off the coating layer. Figure 3 shows the rusted scratch
region of the sample shown in Fig. 2b. Here, the onset
of coating delamination can be indentified as the
location of the very first rusted spot.
KEYENCE VK-9700K LSCM was also used to
observe the subtle surface profile change by scratchinduced delamination. As illustrated in Fig. 4a, the
lowest point (valley) of the scratched profile is always
below the original coating surface if there is no
debonding. However, if delamination occurs, the

debonded coating layer will bulge and induce a surface


profile change as shown in Fig. 4b, which can be
nondestructively observed using LSCM. Actually, the
bulging phenomenon has been observed upon the
coating debonding for both thin opaque coatings
(Fig. 2) and transparent coatings.18

Determination of coating wet-adhesive strength


via FEM
To determine the corresponding stresses induced by
the progressively increasing normal load scratch test, a
3-D FEM simulation approach was used here similar to
Jiang et al.s work.22 ABAQUS/Explicit 6.4.5 is
employed to simulate the scratch process of a polymeric coating.23 As shown in Fig. 5,22 the mesh is
assumed to be symmetrical about the 2-axis. The
typical size of an eight-node tri-linear brick element along the scratch path is 0.05 mm 9 0.05 mm 9
0.05 mm and is chosen to give converging simulation
results and assure numerical accuracy. The spherical
stainless steel tip is assumed to be a rigid surface. The
perfect bonding between the coating layer and substrate exists before the occurrence of debonding. The
elastic-pure-plastic material type is adopted for the
steel substrate, and the epoxy coating is described by
piecewise linear elasticplastic stressstrain curves.
The normal load applied on the indenter is linearly
increased from 1 to 95 N during the scratch process.
The adaptive remeshing methodology provided in
ABAQUS is performed to preserve mesh quality
during the scratch simulation.
Although the scratch always induces multiaxial
stress components at the interface, the Mode I stress
component (i.e., r33) of the debonding stress is always
dominant and is an order of magnitude larger than
other stress components (Fig. 6). Thus, Mode I debonding stress is expected to be the dominant damage
mode at the interface.
If the adhesive strength is higher than the cohesive
strength of the coating, the in-layer coating cracking

Fig. 2: Direct visual detection of onset coating debonding (normal load 180 N) after 1 day water immersion: (a) System I
(smooth substrate surface) and (b) System II (smooth substrate surface)

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J. Coat. Technol. Res., 8 (2) 255263, 2011

Fig. 3: Detection of onset coating debonding (normal load 180 N) by oxidative liquid exposure

Debonding

Bonded interface

Polymer
coating

Steel
substrate

Polymer
coating

Steel
substrate

Fig. 4: Surface profile change with and without coating debonding

Coating layer

Substrate

Fig. 5: 3-D FEM modeling of polymer coating scratch22

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J. Coat. Technol. Res., 8 (2) 255263, 2011


3
S, Max. Principal
(Avg: 75%)
+9.8e+07
+9.0e+07
+8.2e+07
+7.4e+07
+6.5e+07
+5.7e+07
+4.9e+07
+4.1e+07
+3.3e+07
+2.4e+07
+1.6e+07
+7.9e+06
2.7e+05

31

+1.4e+07
+1.2e+07
+9.1e+06
+6.5e+06
+3.9e+06
+1.3e+06
1.3e+06
3.9e+06
6.5e+06
9.1e+06
1.2e+07
1.4e+07
1.7e+07

3
1

S, S23
(Avg: 75%)

S, S13
(Avg: 75%)

33

+2.3e+07
+2.0e+07
+1.6e+07
+1.3e+07
+9.4e+06
+6.0e+06
+2.6e+06
8.0e+06
4.2e+06
7.6e+06
1.1e+07
1.4e+07
1.8e+07

3
2

32

Fig. 6: Stress components corresponding to possible debonding modes (I, II, and III)

coating debonding gives good reproducibility and


follows the expected trend of coating adhesion degradation due to environmental exposure. In this case, the
onset of delamination can be visually observed. Under
a higher normal load, the in-layer coating cracking and
buckling damage are also observed, which is consistent
with our previous studies.19

80
In-layer tensile stress

70
Interfacial stress

Stress (MPa)

60
50

Tip diameter = 2 mm
Coating thickness = 100 microns

40
30

Substrate surface roughness effect

20
10
0
0

10

20

30

40

50

60

70

80

Scratch normal load (N)

Fig. 7: Debonding stress and in-layer tensile stress vs


scratch normal load

may occur.19,21 Figure 7 shows the stress magnitude


variations of both debonding stress and the in-layer
tensile stress as a function of the increasing scratch
normal load. The occurrence of either in-layer cracking
or coating delamination depends on many factors, such
as the coating ductility, Youngs modulus, yield stress,
coating thickness, cohesive strength, and adhesive
strength.
Once the debonding stress exceeds the interfacial
adhesive strength, the coating debonding will take
place. With the known critical load for coating
debonding from the scratch experiment, FEM modeling can then be utilized to determine the corresponding
wet-adhesive strength of the coatings.

Results and discussion


Scratch test
Scratched coating samples of System II having a DFT
of 100 lm after an immersion time of up to 5 days are
shown in Fig. 8. The results suggest that the proposed
scratch methodology for determining the onset of

For System I with a smooth steel substrate surface


(Ra = 3.5 lm), the scratched samples are shown in
Fig. 9. After 3 days of water immersion, the coating
wet-adhesive strength is weakened and the scratchinduced coating debonding can be detected using
LSCM surface profile analysis. Meanwhile, for the
rougher steel substrate (Ra = 64 lm) counterpart, no
coating debonding was observed even after 21 days of
hot water immersion. Only in-layer cracking was
found. The degradation of wet-adhesive strength is
known to be partially due to the deposit of water at the
metal/coating interface.24 The absence of detectable
debonding for the coating system that contains rough
steel surface implies that the effect of substrate
roughness is important for maintaining good coating
wet-adhesive strength. This study also suggests that the
proposed scratch test is an effective method for
evaluating steel surface treatment effect on coating
wet-adhesive strength.
Coating thickness effect
To investigate the coating thickness effect, System II
with coating thicknesses of 100, 200, and 300 lm on a
smooth steel substrate was immersed in water at 95C
for up to 2 weeks. The samples were then scratched
and evaluated by the three detection methods mentioned above. The onset locations for debonding are
marked for direct visual comparison, as shown in
Figs. 10, 11, and 12.
The onset location and critical normal load values
for all the System II samples are reported in Table 1.

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J. Coat. Technol. Res., 8 (2) 255263, 2011

Fig. 8: Scratch of immersed coating System II (DFT = 100 lm)

Fig. 9: Surface roughness effect on coating adhesive strength (System I with smooth substrate surface)

1 day
2 day

3 day
4 day
1 week
Fig. 10: Scratch of System II after up to 2 weeks of hot water exposure (DFT = 100 lm)

It is evident that interfacial degradation is more severe


for thin coatings and for longer hot water exposure
time. For the sample with 100 lm in coating thickness,
the coating becomes extremely weak after 2 weeks of
water immersion. Cohesive coating damage occurs so
readily upon scratching that only in-layer coating
damage is observed. One can also find that the STDV
of the test results is considered acceptable (<9%),
which suggests that the proposed coating scratch test

260

can generate reliable, reproducible results for wetadhesive strength evaluation.


It is interesting to note that the size of the
delamination area and its onset location are quite
different for coating samples with different thicknesses.
A thicker coating slows the adhesion degradation rate
early on. This is because a longer time is needed for
sufficient water to diffuse to the coating/steel interface
to cause damage. Furthermore, a thicker coating

J. Coat. Technol. Res., 8 (2) 255263, 2011

2 day
3 day
4 day
1 week
2 week
Fig. 11: Scratch of System II after up to 2 weeks of hot water exposure (DFT = 200 lm)

2 day
3 day
4 day
1 week
2 week
Fig. 12: Scratch of System II after up to 2 weeks of hot water exposure (DFT = 300 lm)

Table 1: Onset location and critical normal load for debonding of FBE coating
Immersion
time (days)
0
1
2
3
4
7
14

DFT = 100 lm

DFT = 200 lm

Location (mm)

Load (N)

X
77.8
49.6
44.7
33.7
25.1
O

81.7
51.7
46.5
34.7
25.6

0.6
3.1
1.4
2.1
2.3

Location (mm)
X
X
79.0
69.5
63.5
61.5
56.5

1.4
0.7
2.1
2.1
0.7

DFT = 300 lm

Load (N)
X
X
75.3
66.3
60.7
58.8
54.1

Location (mm)
X
X
82.5
80.8
79.0
77.5
69.5

0.7
1.8
2.8
3.6
0.7

Load (N)
X
X
78.6
76.9
75.3
73.9
66.3

X: no damage and O: in-layer cracking occurs first

lowers the stress magnitude generated at the interface


under the same applied scratch normal load level.
Consequently, a higher scratching load is needed to
achieve similar stress level at the interface to induce
debonding for thicker coatings. Similar effects on
immersion time and coating thickness have also been
observed for System I.
Coating wet-adhesive strength determination
by FEM
After experimentally determining the onset location of
coating delamination and the critical debonding load

level (Table 1), FEM is performed to obtain the


corresponding wet-adhesive strengths under different
immersion time periods. Here, only the coating material properties of System II are available, the FEM
work focuses mostly on this system. The results with
three different thicknesses immersed at 95C are
shown in Table 2. The calculated adhesive strength
values and their trend due to extended water exposure
time are shown. The degradation of wet-adhesion
strength as a function of water exposure time is quite
significant. The thicker coating does slow the degradation rate in the early stage of immersion due to longer
time requirement for water permeation to the interface. With longer immersion time, the water will

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J. Coat. Technol. Res., 8 (2) 255263, 2011

Table 2: Degradation of wet-adhesive strength


System II with various FBE coating thicknesses

of

Adhesive
Adhesive
Immersion
Adhesive
time (days) strength (MPa) strength (MPa) strength (MPa)
DFT = 100 lm DFT = 200 lm DFT = 300 lm
0
1
2
3
4
7
14

X
58
41
30
18
8
O

X
X
47
35
21
13
10

X
X
50
38
23
14
11

X: no damage and O: in-layer cracking occurs first

eventually diffuse further into coating and reaches the


interface. The eventual degradation of interface will
occur. The wet-adhesive strength after degradation
tends to level off and shows similar values for all the
coating samples after long exposure time.
While the wet-adhesive strength of the coating
degrades severely upon high temperature water
immersion, the mechanical properties of FBE coating
itself can deteriorate significantly as well. Upon the
scratch test, eventually the coating will fail either
adhesively or cohesively, depending on the relative
rate of adhesion strength degradation at the coating
steel interface and on the coating itself. For the coating
with a thickness of 100 lm, in-layer cohesive failure
occurred first after 14 days of hot water immersion.
Even though debonding was also observed at a higher
scratch normal load, it was no longer feasible to
reliably determine the adhesive strength of the coating
once coating cohesive failure took place.
This study has clearly demonstrated the usefulness
of the scratch tests for quantitative determination of
the residual wet-adhesive strengths of coatings after
their exposure to hot water. The calculated delamination stress values and their trends shown in Table 2 are
quite plausible, suggesting the effectiveness of the
proposed scratch test methodology for development of
optimized coating formulation and substrate surface
treatment for various industrial coating applications.
The reason for such a good FEM finding is likely
because of the brittle nature of the FBE coatings. Only
a small amount of plastic deformation is observed
during scratch. This allows for fairly accurate simulation of the scratch process using FEM. However, if the
coating layer is ductile, then significant ductile deformation of the coating will take place and make the
FEM analysis more complicated, which may result in
the assessment of coating delamination stress less
accurate. Furthermore, if the degradation at the
interface due to water immersion is not uniform, which
may be caused by uneven coating thicknesses or
nonuniform substrate surface treatment, then the
scratch test results may exhibit significant data scattering. Therefore, care should be taken in sample

262

preparation and in carrying out the proposed tests for


the determination of wet-adhesive strength of coatings.

Conclusion
Based on the standardized scratch test method and FEM
modeling, a new approach has been established to
quantitatively determine the wet-adhesive strength of
FBE coating on steel substrate. With the experimentally
determined critical scratching load of coating debonding, the wet-adhesive strength can be calculated and
determined via FEM. The influences of coating thickness and steel surface roughness on the degradation of
coating adhesive strength have also been investigated.
A rougher substrate surface leads to greatly enhanced
wet-adhesive strength. A thicker coating provides a
better resistance against interfacial adhesion degradation and lowers the debonding stress at the interface.
This study has demonstrated that the proposed testing
protocol is effective for evaluation of epoxy coating wetadhesive strength and for development of optimized
coating systems for industrial applications.
Acknowledgments The authors would like to acknowledge the financial support from the Department of
Transportation (DTPH56-06-T-000022). Significant
inputs, discussion, and experimental assistance from
NOV Tuboscope, 3M, Dow Chemical, and ShawCor in
this research endeavor are also greatly appreciated.

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