Adhesion Improvements of Thermal Barrier Coatings
Adhesion Improvements of Thermal Barrier Coatings
Adhesion Improvements of Thermal Barrier Coatings
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Abstract
Thermal barrier coatings (TBC) are an effective engineering solution for the improvement of in service performance of gas turbines and diesel
engine components. The quality and further performance of TBC, likewise all thermally sprayed coatings or any other kind of coating, is strongly
dependent on the adhesion between the coating and the substrate as well as the adhesion (or cohesion) between the metallic bond coat and the
ceramic top coat layer. The debonding of the ceramic layer or of the bond coat layer will lead to the collapse of the overall thermal barrier system.
Though several possible problems can occur in coating application as residual stresses, local or net defects (like pores and cracks), one could say
that a satisfactory adhesion is the first and intrinsic need for a good coating. The coating adhesion is also dependent on the pair substrate-coating
materials, substrate cleaning and blasting, coating application process, coating application parameters and environmental conditions. In this work,
the general characteristics and adhesion properties of thermal barrier coatings (TBCs) having bond coats applied using High Velocity Oxygen Fuel
(HVOF) thermal spraying and plasma sprayed ceramic top coats are studied. By using HVOF technique to apply the bond coats, high adherence
and high corrosion resistance are expected. Furthermore, due to the characteristics of the spraying process, compressive stresses should be induced
to the substrate. The compressive stresses are opposed to the tensile stresses that are typical of coatings applied by plasma spraying and eventually
cause delamination of the coating in operational conditions. The evaluation of properties includes the studies of morphology, microstructure,
microhardness and adhesive/cohesive resistance. From the obtained results it can be said that the main failure location is in the bond coat/ceramic
interface corresponding to the lowest adhesion values.
© 2006 Elsevier B.V. All rights reserved.
Table 2
General thermal spraying parameters
HVOF Oxygen Propylene Air Powder feed rate Stand off
(g/min) distance (mm)
Pressure (bar) Flow rate (SLPM) Pressure (bar) Flow rate (SLPM) Pressure (bar) Flow rate (SLPM)
CoNiCrAlY 10.3 139 6.9 89 7.2 384 38 250
NiCoCrAlTaY 10.3 139 6.9 89 7.2 384 38 250
NiCrAlY 10.3 189 6.9 89 7.2 384 38 250
NiCr 10.3 189 6.9 89 7.2 384 38 250
APS Ar flow rate (l/min) H2 flow rate (l/min) Amperage (A) Voltage (V) Passes Stand off
distance (mm)
ZrO2–8%Y2O3 40 12 630 68 20 120
ZrO2–20%Y2O3 42 18 630 68 29 120
the studies of morphology, microstructure, microhardness and was used as cooling media, directed to the back surface of the
adhesive/cohesive resistance. substrate. The powders were characterized for particle size
distribution by Laser Scattering (Microtrac SRA150), Scanning
2. Experimental procedure Electron Microscopy (SEM) and flow rate test (ASTM B-213-
90). X-ray diffraction (XRD) was employed to reveal phase
Table 1 shows the matrix of TBC systems (S) applied to low content of the starting powder and deposits. The diffractometer
carbon steel substrates specifying the materials used as bond used was a SIEMENS model D-500 with a Cu Kα = 1.5418 Å
coats and top coats. The ceramic top coats used were ZrO2– and working power of 40 Kv–30 mA.
8 wt.%Y2O3 (203-NS — Sulzer Metco) and ZrO2–20wt.% Samples characterization included cross-sectional Optical
Y2O3 (202-NS — Sulzer Metco). The bond coats were Microscopy – OM – (Olympus BH-2-UMA) and Scanning
produced by using an HVOF spraying system Model DJ- Electron Microscopy – SEM – (JEOL-JSM-5310) images, as
2600/2700 (Sulzer Metco Inc., Westbury, NY, USA). The well as phase analysis by Energy Dispersive Spectroscopy –
ceramic top coats were applied by atmospheric plasma spray EDS – (Quantum, Kevex). Cross-sectional Vickers microhard-
(APS) with an F4 gun (Plasma Technik, Sulzer Metco, ness measurements were performed on polished samples
Westbury, USA). (Matsuzawa MTX-α microhardness tester) at 300-g load.
Spraying parameters are presented in Table 2 for metallic and Coating surface roughness was measured for each sample
ceramic materials. These parameters were selected from the (Mitutoyo Surftest 301). Both microhardness and roughness
conditions indicated by the manufacturers of the powders trying values quoted are an average of 20 measurements for each
to guarantee the best deposition characteristics for all the coating. Adhesion of the systems was measured according the
systems as well as similar energy for the flame. ASTM-C-633-01 tensile adhesion test standard [28]. The
The materials were sprayed onto 100 mm × 20 mm × 5 mm adhesive used in the adhesion test was the HTK Ultrabond
UNS G41350 steel coupons for sample characterization and ∅ 100 (HTK Hamburg, Hamburg-Sasel, Germany) cured for 1 h at
25.4 mm × 25.4 mm steel cylinders for the tensile adhesion tests. 170 °C and 35 N of pressure.
Just before spraying, the substrates were degreased with acetone
and grit blasted with white corundum at 5.6 bar, 45° blasting 3. Results and discussion
incidence angle and using a blasting distance of 250 mm. The
grit blasted substrates had a mean roughness (Ra) of 5 μm. The 3.1. General characteristics of the coatings
samples for each coating system were placed in a circular
sample holder and were simultaneously sprayed for every The general characteristics of the powder materials used in
material with a rotational speed producing 500 mm·s− 1 in the this investigation are presented in Table 3. It can be observed
substrate surface. When applying the ceramic coatings, air jet that the bond coat powder materials have presented differences
Table 3
Characterization of metallic and ceramic powders
Powder Composition (wt.%) Particle Grain size (μm) Morphology
size (μm)
Co Ni Cr Al Ta Y ZrO2 Y2O3 x σ
Amdry 9951 38.5 32 21 8 – 0.5 – – − 37 + 5 21.5 9.2 Spheroidal
Amdry 997 23 43.9 20 8.5 4 0.6 – – − 37 27.0 11.6 Spheroidal
TAFA NI 343 – 69.2 20 10 – 0.8 – – − 45 + 10 38.2 12.8 Spheroidal
TAFA N 1262 – 80 20 – – – – – − 53 + 20 41.3 11.3 Spheroidal
203-NS – – – – – – 92 8 − 125 + 16 65.3 30.2 Spheroidal
202-NS – – – – – – 80 20 − 106 + 16 62.2 32.4 Spheroidal
x = mean value σ = standard deviation.
C.R.C. Lima, J.M. Guilemany / Surface & Coatings Technology 201 (2007) 4694–4701 4697
in average grain size that reach more than 90% when comparing
CoNiCrAlY with NiCr powders. The morphology of powders is
spheroidal for the four powder materials tested with a lightly
more regular shape for CoNiCrAlY and NiCoCrAlTaY. Both
ceramic materials used are spheroidal and have very similar
average grain sizes. Typical images of the morphology of the
powders can be observed in Fig. 2.
Typical microstructure of the coating systems can be
observed in Fig. 3. A very dense and homogeneous coating
with very low oxidation was obtained for all the coating systems
at the metallic layers. Ceramic layers have a more porous
microstructure as expected for APS spraying of such materials.
X-ray diffraction results for the bond coats and for ceramic
deposits are shown in Fig. 4. X-ray diffraction results have not
evidenced relevant presence of undesirable phases as it was also
confirmed with EDS. Ceramic deposits shown to be mainly
constituted of non-transformable tetragonal zirconia phases (t′).
Fig. 3. Typical cross sectional optical micrographies of the coating systems with
(A) ZrO2–8wt.%Y2O3 and (B) ZrO2–20wt.%Y2O3 top coat. A general porous
ceramic microstructure can be observed in contrast to a very dense metallic
deposit.
Fig. 4. X-ray diffractograms of the bond coat powders (A) and the top coat ceramic deposits (B). The systems showed in (B) represent the four distinctive bond coats
applied and the two distinctive ceramic top coats.
tested samples with each respective dispersion bar. As usual, a 30% lower than the other systems. But this simple observation
huge dispersion of values can be observed mainly due to the did not represent the exact behavior of each distinctive coating
nature of the metal-ceramic coatings. The locations of coating system. A deep analysis can bring up much more information and
failures in the test are described in Table 5 for better under- lead to a better understanding of each individual behavior.
standing of such dispersed results and for further discussion. Looking to the maximum values, highlighted in Table 5 with a
It can be observed from Fig. 5 and Table 5 that the mean values gray background, it can be observed that in general the coating
are in a very good agreement for the eight tested coating systems, failure location is at the interface between bond coat and
except for the systems S3 and S4, that have a mean value around substrate. This means an adhesive failure. The highest values are
Table 4
Thickness, roughness and microhardness measurements of the coating systems
Coating system S1 S2 S3 S4 S5 S6 S7 S8 BC1 BC2 BC3 BC4
Thickness (SD = 30μm S1 to S8) 410 410 410 410 410 410 410 410 120 120 120 120
Roughness (μm) Ra (SD = 0.3 μm) 6.8 6.8 6.8 6.9 7.6 7.2 7.3 7.0 5.8 6.5 5.6 8.4
HV0.3 mean (x) (SD = 36 μm) 638 650 618 624 711 692 753 683 368 369 432 337
SD = Standard Deviation.
C.R.C. Lima, J.M. Guilemany / Surface & Coatings Technology 201 (2007) 4694–4701 4699
Table 5
Coating systems adhesion and failure location in ASTM-C-633 test
Fig. 6. Fracture surfaces of a TBC system after ASTM C633 tensile test showing
C/S = Bond coat/substrate interface (Adhesive failure); C/Z = Bond coat/ceramic the bond coat ceramic interface (A) with no defects and (B) with a singular defect.
interface (Cohesive failure). It should be noted that the ceramic remaining intact (right side of “A”) if tested
Glue = failure within the glue (poor test). again would present an adhesion higher than that found in that specific test.
4700 C.R.C. Lima, J.M. Guilemany / Surface & Coatings Technology 201 (2007) 4694–4701
system S5 (7.6 μm), that also presents one of the highest coating adhesion but also increasing the number of coating
adhesion mean values (34.0 MPa). However, system S1 with an layers for the same thickness tends to diminish coating adhesion.
average roughness of 6.8 μm presents a very similar mean In that work, increasing the number of layers indicated a greater
adhesion (33.3) and one of the three highest individual adhesion interruption time for the spraying of the subsequent layer due to
values (52.8 MPa for sample 2). It should be observed that the the necessary arrangements. In the present work, the only
standard deviation of the roughness values shown in Table 4 is difference for the tested coating systems was a greater number of
0.3 μm thus implying a very similar roughness for all the passes to deposit ZrO2–20%Y2O3 (systems S5, S6, S7 and S8)
systems that can explain such variations in the adhesion of the compared with ZrO2–8%Y2O3 as shown in Table 2. That almost
individual samples. fifty percent higher number of passes implies an increased
Another issue to be observed is that the highest roughness number of ceramic interfaces as well as a more homogeneous
(8.4 μm) just after bond coat application shown in Table 4 is that ceramic coating with thinner subsequent layers.
of systems S4 and S8, corresponding to bond coat 4 (NiCr) but
showing no high adhesion values. This could be due to residual 3.8. Effect of thermal expansion
stresses at bond coat/substrate and bond coat/ceramic interfaces.
According to Khan et al. [30] the adhesion of the coatings From the point of view of thermal expansion differences
increases with the increase of substrate roughness (or bond coat between the four used bond coats, it has to be said that NiCrAlY
surface roughness for a ceramic coating deposition) up to presents the lowest expansion (11.73 mm/m at 825 °C),
certain limits (about 5 μm in their work) and then decreases. compared with CoNiCrAlY (13.84 mm/m at 825 °C), NiCo-
With the increase of substrate roughness there is an increase in CrAlTaY (13.48 mm/m at 825 °C) and NiCr (13.42 mm/m at
interfacial toughness due to high compressive stresses associ- 825 °C). These values were found by Taylor and Walsh [33] in a
ated with high rough surfaces but further temperature and systematic study with several MCrAlY bond coats including
pressure from the spray process effect the residual stress profile bond coats with the same composition of the ones used in the
and thus the interfacial toughness of the coatings [30]. present study. They stated that the expansion differences
between NiCrAlY and the other tested coatings were greater
3.6. Effect of powder particle size than the standard deviation of the used method and have to be
considered as significant. Moreover the authors related
Limarga et al. [31] working with multilayered thermal barrier expansion to chemical composition trying to get directions for
coatings found adhesion strengths between 5 and 23 MPa longer life of TBCs by modifying composition for low
depending on the proportion of bond coat, Al2O3 and ZrO2 in the expansivity. According to their results, thermal expansion
coating systems. The majority of failures have occurred inside mismatch at bond coat/top coat interface can be reduced from
the ceramic layer. When interfacial bond coat/ceramic failure 2.2 mm/m for a CoNiCrAlY/ZrO2–7%Y2O3 pair to a 1.4 mm/m
occurred, the highest adhesion values were registered. The used for a NiCrAlY/ZrO2–7%Y2O3 pair mainly due to the increasing
bond coat was a 200 μm thick NiCoCrAlY. According to the of Al content but the strongest expansion reduction would be
authors, the very low bond strength exhibited for some coating obtained by increasing Cr at the expense of Ni or Co [33].
systems is due to a low surface roughness of the sprayed ceramic, Such discussion should predict that thermal expansion
where the mechanical interlocking is negligible. Furthermore, residual stresses would be higher for CoNiCrAlY, NiCoCrAlY
they concluded that the low surface roughness correspond to the and NiCr, respectively. This would influence in coating
small particle size of materials used for plasma spraying. adhesion. But from the observation of the results shown in
Using the same analysis for the present work and considering Table 5, it can be said that the lowest adhesion values were
just the final ceramic layer, it can be observed in Table 4 that the obtained for samples of NiCrAlY and NiCr (systems S3, S7 and
highest roughness values are found in systems S5 to S8, S4) that have the lowest expansion and the fracture location is at
corresponding to powder 202-NS (ZrO2–20%Y2O3) which bond coat/top coat interface. A possible explanation for this is
have a slightly lower grain size compared with powder 203-NS that some stress relaxation mechanism occurs, probably creep or
(ZrO2–8%Y2O3) that corresponds to systems S1 to S4, as it can metallic yield, that are stated by Tsui and Clyne [34] as the
be seen in Table 3. This would partially confirm Limarga's major stress relaxation for metallic coatings, thus modifying the
trend. In fact, those powder grain size values (65.3 and 62.2 μm) expected stress influence on adhesion, at least at the
should be taken as very similar values mainly due to their temperatures experienced for the tested coatings which are as-
statistical standard deviation. However, the trend of adhesion/ sprayed coatings without thermal cycling.
roughness correlation can be really observed since the highest
adhesion mean values in Table 5 are basically those of systems 4. Conclusions
S5 to S8, corresponding to ZrO2–20%Y2O3 which presents the
highest roughness. In the present work, eight distinctive TBC coating systems
have been compared. Microstructure, hardness, roughness and
3.7. Effect of number of spraying passes adhesion were measured. For adhesion measurement, ASTM-
C633 tensile adhesion test was used and proved to be effective
Lima and Trevisan [32] working with graded TBCs have for general level of comparison but deeper analysis of the
found that not only increasing thickness tends to decrease individual results has to be done in order to know specific
C.R.C. Lima, J.M. Guilemany / Surface & Coatings Technology 201 (2007) 4694–4701 4701
characteristics of true coating adhesion. From the obtained [9] N.P. Padture, M. Gell, E.H. Jordan, Science 296 (2002) 280.
results it can be said that the main failure location is in the bond [10] R.N. Katz, Ceram. Ind. 151 (4) (2001) 22.
[11] J.P. Huchin, in: C. Coddet (Ed.), Thermal Spray: Meeting the Challenges
coat/ceramic interface corresponding to the lowest adhesion of the 21st Century, Proceedings of the 15th International Thermal Spray
values. For the highest adhesion values, coating failure is Conference, Nice, France, ASM International, Materials Park, Ohio, 1998,
mainly located in the bond coat/substrate interface. Mean p. 931.
adhesion values can be higher for systems that have higher [12] W.J. Brindley, R.A. Miller, Adv. Mater. Process. 136 (2) (1989) 29.
[13] Y. Itoh, M. Saitoh, M. Tamura, J. Eng. Gas Turbine Power 122 (2000) 43.
roughness but this trend is not always observed when analyzing
[14] P. Vuoristo, S. Ahmaniemi, S. Tuurna, T. Mantyla, E. Cordano, F. Fignino,
individual samples. When focusing individual sample adhesion G.C. Gualco, Proceedings of ITSC 2002 — International Thermal Spray
values, samples with the lowest roughness show the highest Conference and Exposition, Essen, Germany, vol. 1, ASM-International/
adhesion values. Furthermore, thermal expansion, powder grain DVS, Dusseldorf, Germany, 2002, p. 470.
size and number of spraying passes can modify the building [15] V.V. Sobolev, J.M. Guilemany, J. Nutting, High Velocity Oxy-fuel
process of each individual coating system thus showing Spraying: Theory, Structure–Property Relationships and Applications,
Maney Publishing, London, 2004, 397 pp.
different values of coating adhesion. [16] A.G. Evans, D.R. Mumm, J.W. Hutchinson, G.H. Meier, F.S. Pettit, Prog.
Mater. Sci. 46 (2001) 505.
Acknowledgments [17] M.D. Hill, Ceram. Ind. 153 (10) (2003) 17.
[18] D. Stover, G. Pracht, H. Lehmann, M. Dietrich, J.E. Doring, R. Vaben, in:
The authors would like to thank M. Torrel and N. Cinca for B. Marple, C. Moureau (Eds.), Thermal Spray 2003: Advancing the
Science and Applying the Technology, ASM International, Materials Park,
helping in metallographic preparation and tensile adhesion tests Ohio, USA, 2003, p. 1455.
and J. R. Miguel for helping in the evaluation of coatings. [19] A.W.S., Thermal Spraying: Practice, Theory and Application, American
Carlos Lima acknowledges the sabbatical concession of CNPq– Welding Society, Miami, FL, 1985.
Conselho Nacional de Desenvolvimento Científico e Tecnoló- [20] V.V. Sobolev, J.M. Guilemany, J. Nutting, J.R. Miguel, Int. Mater. Rev. 42
gico — Brazil. CPT thanks to Generalitat de Catalunya for the (3) (1997) 117.
[21] M.F. Bahbou, P. Nylén, J. Wigren, J. Therm. Spray Technol. 3 (4) (2004)
project 2001SGR00145. 508.
[22] C.C. Berndt, Mater. Sci. Forum 34–36 (1988) 457.
References [23] H. Era, F. Otsubo, T. Uchida, S. Fukuda, K. Kishitake, Mater. Sci. Eng., A
Struct. Mater.: Prop. Microstruct. Process. 251 (1998) 166.
[1] F. Kassabji, J.P. Durand, G. Jacq, in: Christian Coddet (Ed.), Thermal [24] Y.L. Zhu, S.N. Ma, B.S. Xu, J. Therm. Spray Technol. 8 (2) (1999) 328.
Spray: Meeting the Challenges of the 21st Century, ASM International, [25] S. Siegman, M. Dvorak, H. Grutzner, K. Nassenstein, A. Walter, in: E.
Ohio, USES, 1998, p. 1677. Lugscheider (Ed.), Thermal Spray Connects: Explore its Surface Potential,
[2] W. Hangong, W. Liuying, in: E. Lugscheider (Ed.), Thermal Spray Proceedings of the International Thermal Spray Conference ITSC, Basel,
Connects: Explore its Surface Potential, Proceedings of the International Switzerland, ASM International/DVS, Dusseldorf, Germany, 2005, p. 823.
Thermal Spray Conference ITSC, Basel, Switzerland, ASM International/ [26] M. Hadad, G. Marot, J. Lesage, J. Michler, S. Siegmann, in: E. Lugscheider
DVS, Dusseldorf, Germany, 2005, p. 29. (Ed.), Thermal Spray Connects: Explore its Surface Potential, Proceedings of
[3] K. Neufuss, P. Chráska, B. Kolman, S. Sampath, Z. Trávnicek, J. Therm. the International Thermal Spray Conference ITSC, Basel, Switzerland, ASM
Spray Technol. 6 (4) (1997) 434. International/DVS, Dusseldorf, Germany, 2005, p. 759.
[4] J.M. Guilemany, J. Nin, J.R. Miguel, in: E. Lugscheider (Ed.), Thermal [27] R.E. Trevisan, H.C. Fals, C.R.C. Lima, Inf. Tecnol., Chile 11 (4) (2000)
Spray Connects: Explore its Surface Potential, Proceedings of the 103.
International Thermal Spray Conference-ITSC, Basel, Switzerland, ASM [28] Standard test method for adhesion or cohesion strength of thermal spray
International/DVS, Dusseldorf, Germany, 2005, p. 36. coatings, ASTM Standard C 633-01, ASTM, West Conshocken, PA, USA,
[5] T. Mckechnie, in: C.C. Berndt (Ed.), Thermal Spray: Surface Engineering 2001.
Through Applied Research, ASM Intl., Materials Park, OH, 2000, p. 1105. [29] H.D. Steffens, B. Wielage, J. Drozak, Surf. Coat. Technol. 45 (1991) 299.
[6] J. Streeter, E.R. Sampson, in: C.C. Berndt (Ed.), Thermal Spray: Surface [30] A.N. Khan, J. Lu, H. Liao, Surf. Coat. Technol. 168 (2003) 291.
Engineering Through Applied Research, ASM Intl., Materials Park, OH, [31] A.M. Limarga, S. Widjaja, T.H. Yip, Surf. Coat. Technol. 197 (2005) 93.
2000, p. 1145. [32] C.R.C. Lima, R.E. Trevisan, J. Therm. Spray Technol. 6 (2) (1997) 199.
[7] W. Mallèner, W. Hohenauer, D. Stover, in: C.C. Berndt (Ed.), Thermal [33] T.A. Taylor, P.N. Walsh, Surf. Coat. Technol. 177–178 (2004) 24.
Spray: Practical Solutions goes Engineering Problems, ASM Intl., Ohio, [34] Y.C. Tsui, T.W. Clyne, Thin Solid Films 306 (1997) 23.
1996, p. 1.
[8] Y. Wang, K.A. Khor, P. Cheang, J. Therm. Spray Technol. 7 (1) (March
1998) 50.