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Some Recent Trends in Research and Technology of Advanced Thermal Barrier

Coatings

Article in Aerospace Science and Technology · January 2003

DOI: 10.1016/S1270-9638(02)00003-2

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Some recent trends in research and technology

of advanced thermal barrier coatings ✩

Aktuelle Forschungs- und Entwicklungstrends

bei Wärmedämmschichten für die Gasturbine
Uwe Schulz a,∗ , Christoph Leyens a , Klaus Fritscher a , Manfred Peters a , Bilge Saruhan-Brings a ,
Odile Lavigne b , Jean-Marc Dorvaux b , Martine Poulain b , Remy Mévrel b , Michaël Caliez b
a Deutsches Zentrum für Luft- und Raumfahrt (DLR), Institute of Materials Research, D-51170 Köln, Germany
b Office National d’Etudes et de Recherches Aérospatiales (ONERA), Department of Metallic Materials and Processing, 29, avenue de la Division Leclerc,
F-92322 Châtillon Cedex, France
Received 3 May 2002; received in revised form 17 September 2002; accepted 14 October 2002

Abstract
Ceramic thermal barrier coatings (TBCs) offer the potential to significantly improve efficiencies of aero engines as well as stationary
gas turbines for power generation. On internally cooled turbine parts temperature gradients of the order of 100 to 150 ◦ C can be achieved.
Today, state-of-the-art TBCs, typically consisting of an yttria-stabilised zirconia top coat and a metallic bond coat deposited onto a superalloy
substrate, are mainly used to extend lifetime. Further efficiency improvements require TBCs being an integral part of the component which,
in turn, requires reliable and predictable TBC performance. Presently, TBCs produced by electron beam physical vapour deposition are
favoured for high performance applications. The paper highlights critical R&D needs for advanced TBC systems with a special focus on
reduced thermal conductivity and life prediction needs.
 2002 Éditions scientifiques et médicales Elsevier SAS. All rights reserved.
Zusammenfassung
Keramische Wärmedämmschichten ermöglichen eine deutliche Steigerung der Effizienz von Flugtriebwerken und stationären Gasturbinen
für die Energieerzeugung. Bei innengekühlten Turbinenbauteilen lässt sich eine Temperaturabsenkung um 100 bis 150 ◦ C erreichen.
Standardwärmedämmschichtsysteme, welche aus einer keramischen Außenschicht aus Yttriumoxid-stabilisiertem Zirkonoxid und einer
metallischen Haftvermittlerschicht auf der Nickel-Superlegierung bestehen, werden bisher zumeist nur zur Lebensdauerverlängerung der
Turbinenschaufeln verwendet. Die notwendige weitere Steigerung der Effizienz erfordert jedoch Wärmedämmschichten, die ein integraler
Bestandteil des Bauteildesigns sind. Dafür ist ein zuverlässiges und vorhersagbares Verhalten der Schichtsysteme im Einsatz unabdingbar.
Für hochbelastete Bauteile wie z.B. Turbinenlaufschaufeln wird zur Schichtherstellung bevorzugt das EB-PVD-Verfahren eingesetzt. Der
Artikel fasst wesentliche Entwicklungsrichtungen für neue Wärmedämmschichtsysteme zusammen mit den Schwerpunkten Verringerung
der Wärmeleitfähigkeit sowie Erfordernisse der Lebensdauervorhersage.
 2002 Éditions scientifiques et médicales Elsevier SAS. Alle Rechte vorbehalten.

Keywords: Thermal barrier coatings; EB-PVD; Thermal conductivity; Lifetime prediction

Schlüsselwörter: Wärmedämmschicht; EB-PVD; Wärmeleitfähigkeit; Lebensdauervorhersage

1. Introduction

✩
This article was presented at ODAS 2002.
High pressure turbine blades and vanes of aeroengines are
* Corresponding author. among the most highly loaded parts in engineering compo-
E-mail address: [Link]@[Link] (U. Schulz). nents. For these demanding applications only high temper-
1270-9638/02/$ – see front matter  2002 Éditions scientifiques et médicales Elsevier SAS. All rights reserved.
PII: S 1 2 7 0 - 9 6 3 8 ( 0 2 ) 0 0 0 0 3 - 2
74 U. Schulz et al. / Aerospace Science and Technology 7 (2003) 73–80

Fig. 2. Typical thermal barrier coating system: materials selection and

Fig. 1. Increase of operational temperature of turbine components made function.
possible by alloy development, manufacturing technology and TBCs.

ature Ni-base superalloys can be considered. As shown in

Fig. 1 these alloys have matured over the years from wrought
to cast, then to directionally solidified alloys, whereas in the
latest generation of turbines for the most demanding appli-
cations, like the rotating turbine components, single crystal
material is employed [38].
In today’s engines, the hot gas temperatures exceed
the melting point of the Ni-base alloys by more than
250◦ C. The only way the airfoils can survive in such an
environment is by excessive internal and external cooling,
which, however, reduces the overall thermal efficiency
of the aero engine. The extreme conditions such airfoils Fig. 3. TEM picture of interface between NiCoCrAlY bond coat and YPSZ
operate in are clearly expressed by the fact that creep TBC in as-coated condition [53].
life of turbine blades is halved for every 10 to 15◦ C
increase in metal peak temperature [21]. Actual metal coefficient of thermal expansion, which comes close to
surface temperatures are about 1000◦C with short-term that of the metal substrate, and which, for this reason,
peaks as high as 1100◦C. Obviously the melting point of upon thermal cycling allows to accommodate straining
the alloys clearly marks the limit for future developments. without spalling immediately. In-between the TBC and the
Nevertheless, further increases in thrust-to-weight ratio of substrate a metallic corrosion resistant coating is applied,
next generation aero engines will require even higher gas which protects the substrate from oxidation and/or high
temperatures [62]. There is no doubt that this ambitious goal temperature corrosion and provides the necessary adhesion
can only be met by either usage of uneconomically extensive of the ceramic to the airfoil material. These bond coatings
cooling or – from a materials standpoint – advanced high are either overlay (MCrAlY-type) or diffusion coatings (Pt-
temperature materials such as new generations of Ni-base modified aluminides). During processing and in service a
superalloys [10], primarily, however, by use of advanced thermally grown oxide (TGO) layer forms as a result of bond
coating systems, in particular thermal barrier coatings [14, coat oxidation which often plays the most important role for
27,29,38,51,56]. The paper highlights the present status and the adherence of the TBC. Fig. 3 shows a TEM micrograph
sheds some light on future developments in the area of of the interface between a NiCoCrAlY bond coat and YPSZ
thermal barrier coatings (TBCs). TBC, where a thin TGO has already developed during the
deposition process [53].
The potential benefits of TBC application on turbine
2. Thermal barrier coatings blades in aeroengines are schematically outlined in Fig. 4
[28]. The insulating properties of these coatings may lead
TBCs usually consist of a duplex system as schematically to performance improvements by allowing a reduced cool-
shown in Fig. 2. The actual thermal barrier is a ceramic top ing air flow at a given metal temperature or may improve
coating with the prime function to reduce the heat transfer lifetime of the components by reducing the metal tempera-
to the metallic substrate. For many years yttria partially ture at a given cooling air flow. Furthermore, higher engine
stabilised zirconia (YPSZ) has been the prime choice, thrust can be achieved by allowing higher gas temperatures
because it reveals a thermal conductivity which is more than at a given cooling air flow. Currently, engine design still pri-
an order of magnitude below that of the Ni-base superalloy. marily relies on lifetime extension benefits of TBCs. It is,
Furthermore, as a ceramic, it also shows a relatively high however, obvious that prime reliant TBCs with predictable
 U. Schulz et al. / Aerospace Science and Technology 7 (2003) 73–80 75

Fig. 6. Results of burner rig tests of candidate ceramic coatings within the
US ATS program [41].
Fig. 4. Potential benefits in gas turbines for the use of TBCs: depending
on operating conditions and requirements, TBCs can improve engine
lifetime. A recent study performed within the Advanced Tur-
performance and thrust as well as component lifetime [42].
bine Systems Program (ATS) in the United States docu-
mented the superiority in lifetime during burner rig testing
of EB-PVD over PS TBCs candidate coatings as outlined
in Fig. 6 [41]. A similar ranking was reported for the ther-
mal fatigue behaviour of TBCs, where plasma sprayed TBCs
reached only 30 to 40% of the lifetime of an evaporated coat-
ings [13]. Finally it was observed, that apart from reduced
life, the scatter of lifetime data is considerably higher for the
sprayed coatings [5].
Apart from that, the EB-PVD technology leads to aerody-
namically smooth surfaces of the turbine blades, thus elim-
inating the need for final polishing or conditioning of the
cooling holes, which are not blocked by EB-PVD process-
ing of TBCs [50]. Therefore, today EB-PVD is the process
of choice as far as TBCs for high pressure turbine blades for
Fig. 5. YPSZ thermal barrier coating with strain-tolerant columnar mi- aeroengines are concerned, and becomes increasingly im-
crostructure fabricated by EB-PVD. portant also for turbine blades of land-based industrial gas
turbines for power generation [5,12,30].
life-time performance are required to implement TBCs as During EB-PVD processing a high energy electron beam
designed-in components and in this way to fully exploit their melts and evaporates a ceramic source ingot in a vacuum
potential for significant performance improvements [33]. chamber. During evaporation the ingots are bottom-fed into
the crucibles to ensure continuous growth of the ceramic
coating. Preheated substrates are positioned in the vapour
3. Competing technologies for TBC deposition cloud and the vapour is deposited onto the substrates
at deposition rates of 4–10 µm/min. To achieve defined
There are essentially two processes which have emerged stoichiometry of the zirconia a controlled amount of oxygen
as viable ways to fabricate TBCs under industrial condi- is bled into the deposition chamber.
tions. Plasma-spraying (PS) has been widely applied since Fig. 7 shows a GE Aircraft Engines CF6 high pressure
the 1960s to produce TBCs on hot components like burner turbine blade with an EB-PVD ceramic coating, TBCs were
cans or combustion chambers. The evaporation technology manufactured in a semi-commercial 150 kW dual-source
by means of electron beam physical vapour deposition (EB- jumping beam von Ardenne Anlagentechnik EB-PVD coater
PVD) technology has emerged in the 1980s. This latter de- shown in Fig. 8 [42,43]. State-of-the-art commercial produc-
position process is particularly favoured for applications on tion facilities are aimed at reducing the overall coating costs
more mechanically loaded parts, i.e. rotating parts like high per coated article by increasing the number of coated compo-
pressure turbine blades. The typical columnar microstruc- nents per coating charge, by extending the production cycle
ture of EB-PVD TBCs is shown in the SEM micrograph in between maintenance stops, by simultaneously minimising
Fig. 5. the latter and by optimising the processing steps per coating
The specific microstructure reveals a certain pseudo- run. Recently, some process improvements have been intro-
plasticity which translates into superior tolerance against duced such as electron-beam pre-heating for large industrial
straining and thermoshock, thus giving it a major edge in components or in-line trolley installation for higher flexibil-
76 U. Schulz et al. / Aerospace Science and Technology 7 (2003) 73–80

weight, high temperatures and humidity. As a result the en-

gines’ turbine blade life was reduced to only 20%. In this sit-
uation TBC “band-aids” applied to the highly stressed parts
of the airfoil prevented the aircraft from being grounded. So
these abnormal engine operation conditions paved the way
for EB-PVD thermal barrier coatings.
Today EB-PVD thermal barrier coatings are widely used
in engine technology as part of advanced designs, like in
the Pratt & Whitney 4000 family, General Electric/Snecma’s
CFM56-7 version and a great variety of other aeroengine
types. They also have been successfully introduced into
industrial gas turbines for power generation via the latest
Westinghouse and Siemens designs [5,13].
Fig. 7. GE Aircraft Engines CF6 high pressure turbine blade with EB-PVD
thermal barrier coating. Note that cooling holes remain open after deposi-
tion. 5. Future research and development needs

Although TBCs are flying in today’s advanced aero-

engines and are introduced into first land-based gas turbines,
a lot of research issues still have to be addressed until TBCs
qualify to become prime reliant, i.e. an integral part of tur-
bine blades and vanes and thus exploit their full potential
[43]. Furthermore, advanced TBC systems have to be de-
veloped in order to accommodate the further anticipated in-
crease in engine performance. In a recent workshop [58] crit-
ical R&D needs of TBCs in future gas turbine systems have
been described as follows (in random order):
• reduced thermal conductivity;
• higher temperature capability;
• improved hot corrosion resistance;
Fig. 8. Dual-source von Ardenne Anlagentechnik EB-PVD coater. • long-term thermal cycle testing in a thermal gradient;
• lifetime prediction modelling;
ity and throughput [5,16,48] or dual-source jumping beam • non-destructive inspection technique development;
evaporation for generation of new types of TBC [31,52,54]. • coatings on ceramics;
In recent years, a number of alternative coating processes • process modelling/validation;
have been investigated, based on chemical vapour deposi- • modelling of long-term TBC system stability.
tion, a technique with which columnar YPSZ coatings can In the following, some recent investigations related to
be produced with a good throwing power and high deposi- thermal conductivity and lifetime prediction modelling are
tion rates if metalorganic precursors [61] or a plasma assis- summarised.
tance [45,46] are employed. Such processes could provide
an easy way to evaluate new and/or complex ceramic com-
positions. 6. Thermal conductivity

Although thermal conductivity is one of the physical key

4. From invention to application properties of TBCs, it has not been a major research and
development topic until the early 1990s, compared to work
Only few other inventions in the aerospace sector have related to thermomechanical behaviour for instance. Today,
experienced such a short time from “invention” to “appli- increasing the thermal barrier coating insulation capability
cation” as EB-PVD thermal barrier coatings have done. In clearly emerges as a technical and economical challenge for
the early 1980s first process and product patents were filed engine manufacturers [1]. Lowering TBCs thermal conduc-
in the United States [57]. The breakthrough came already tivity would increase the engine performance by improv-
less than ten years later when South African Airlines expe- ing the combustion efficiency (higher Turbine Entry Tem-
rienced severe problems with their aircraft engines [8]. Due perature), reduce the specific fuel consumption, allow a re-
to apartheid, SAA aircraft had no right to land in continen- duction of internal cooling, reduce the metallic component
tal Africa with the consequence that they had to take-off un- temperature and extend their lifetime [3]. Thermal conduc-
der extreme conditions, like high altitude, maximum take-off tivity of standard 6 to 8 wt.% yttria partially stabilised zir-
 U. Schulz et al. / Aerospace Science and Technology 7 (2003) 73–80 77

on specially prepared dense materials, showing that signif-

icant decrease in thermal conductivity (up to 40%) can be
achieved, compared to the standard 8 wt.% yttria partially
stabilised zirconia [32].
Thermal barrier coatings with alternative compositions
have been deposited by PECVD [47] or EBPVD: most of
these new systems are simple tetragonal or cubic zirconia
based coatings [2,26,39,40,49] whose thermal conductiv-
ity proved to be as low as 1.0 W·m−1 ·K−1 . Some other
ceramics with more complex crystallographic structures,
like pyrochlores [34,60], garnets [59], magnetoplumbites
[19], . . . are emerging, which combine very promising ther-
mal insulation capabilities (thermal conductivities as low as
half the thermal conductivity of yttria partially stabilised zir-
Fig. 9. Calculated thermal conductivity at 300 K of Zr1−x Xx O2−x/2 as
a function of X ion radius (diamond: partially stabilised zirconia x = 0.08;
conia) with increased high temperature stability.
square: fully stabilised zirconia x = 0.18).
6.2. Influence of porous architecture
conia EBPVD coatings is typically 1.8 to 2.0 W·m−1 ·K−1 .
Reducing this value to that observed for standard plasma Another efficient way to decrease the thermal conductiv-
sprayed TBCs (0.9 to 1.0 W·m−1 ·K−1 ) could ensure further ity of a material is to deliberately introduce microstructural
benefits from the use of EBPVD coatings. defects such as pores, voids, microcracks which constitute
The thermal conductivity of a porous ceramic layer obstacles against the through-thickness heat transfer propa-
depends on: gation. This approach turned out to be very fruitful in case of
– the intrinsic thermal conductivity of the bulk ceramic, plasma sprayed coatings by use of specially designed feed-
which is linked with its composition and its structure, stock powders or by control of spray parameters [23]. In
– the architecture of the porous structure, i.e. pore volume the case of EBPVD coatings a gain in thermal insulation
fraction, geometry and distribution. has also been obtained with particular columnar architec-
Moreover, in the case of a multiphase ceramic materi- tures [22,23], although lower than the one achieved with op-
als (for example a multilayer insulating coating), thermal timised chemical composition. The introduction of layered
boundary resistance and phase topology have to be taken into structures that introduces porosity in YPSZ [39,40] or that
account. creates alternating layers of different chemical composition
Thus lowering thermal conductivity of the ceramic layer [29,31] has also been reported. The layered coatings provide
can be achieved by engineering chemical composition and/or barriers to the through thickness heat transfer that can result
coating microstructure. in a substantial reduced thermal Conductivity.
Moreover, Since the end of the 19th century several meth-
6.1. Influence of chemical composition ods have been proposed to estimate the thermal conductiv-
ity of multiphased solids, in particular in porous materials
Dense zirconia based materials already exhibit low ther- (see review article [18]). Most of the analytical calculations
mal conductivity. The introduction of a stabiliser, required are derived from the earliest models of Maxwell and Eucken
to avoid the detrimental effect of monoclinic to tetrago- [35]: they all assume the material constituted of a dispersion
nal phase transformation at typical service temperature, is of a randomly distributed, more or less concentrated, more
accompanied by the incorporation of a substantial amount or less spherically shaped, second phase. This oversimpli-
of vacancies providing an efficient source of scattering of fication of the porosity description (by a restricted number
phonons. This explains why the thermal conductivity of yt- of parameters like pore volume fraction and some adjustable
tria doped zirconia is a decreasing function of the yttria con- parameters) limits the predictive capacity of these models
tent (at least for relatively low stabiliser contents) [7,39,40]. for complex interconnected porous structures. In those cases
Further thermal conductivity decrease may be achieved with numerical schemes appear to be more promising as they in-
stabilisers having different atomic mass and/or ionic radius. volve a description of the material structure which is close to
A model based on solid state physics considerations regard- the real structure. Bakker [4] and more recently Staicu [55]
ing heat conduction mechanisms in disordered oxide ceram- used a finite element method to compute the conductivity of
ics has been developed for calculating the thermal conduc- a matrix containing dispersed pores. However, this method
tivity of zirconia based materials doped with trivalent ions may be difficult to apply, in terms of meshing and memory
(see Fig. 9) and codoped with pentavalent metallic ions. Rel- storage, on complex microstructures with very fine features
atively good fits, given the experimental uncertainties and like those encountered in plasma sprayed or EBPVD thermal
assumptions made, are obtained with experimental results barrier coatings.
78 U. Schulz et al. / Aerospace Science and Technology 7 (2003) 73–80

7. Lifetime prediction modelling

7.1. Modelling

Most lifetime prediction models currently employed by

designers [64] are based on the approach proposed by Miller
[37], involving cumulative damages linked to oxidation of
the bondcoat and mechanical cycling, and later substantiated
by [36]. Improvements of these approaches have been
included within proprietary models, taking into account
service experience. These models involve fitting parameters
obtained by testing, generally under simpler experimental
conditions than those experienced by engine components,
although in recent years, efforts have been devoted to
understand the behaviour and degradation of TBCs under
combined mechanical and thermal loadings [6,63].

Fig. 10. Calculated heat flux through an EBPVD coating [18]. 7.2. Failure mechanisms

To appreciate how relevant these descriptions are and how

these models can be extrapolated to a wider range of condi-
Alternative approaches have been proposed by Dorvaux tions than the testing conditions, an active research must lead
[17] (finite difference method) and Fuller et al. [20] (finite to understand and describe the damage mechanisms. Gener-
element method) for computing the thermal conductivity ally, high stresses are present in the interfacial zone, due to
of porous coatings, using as input digitised micrographs of oxide growth, to thermal misfit and to applied loads. As a re-
coating cross sections. In that way the real porous structure sult, cracks can initiate and propagate, causing the ceramic
of the material, as complex as it can be, is taken into layer to spall off, leading to the system degradation. A phys-
account. In the field of thermal barrier coatings, Dorvaux’s ical description of these phenomena requires in particular to
calculation has been used [17,18,23] (see an example on know the fine structure and properties of the various con-
Fig. 10): stituents as well as their evolution as a function of time and
– as an alternative to diffusivity measurements for rank- temperature.
ing coatings according to their thermal insulation efficiency At the moment, there is no adequate global description
with regard to the porous structure, integrating all these data but several aspects are being
– to determine the contribution to thermal insulating ca- investigated in a detailed manner, for example:
– The determination of the residual stresses in the
pabilities of each pore family (globular pores, fine inter-
alumina layer by piezospectroscopy [11].
lamellar defects, cracks, . . . ) in the case of plasma sprayed
– The determination of the mechanical behaviour of
coatings, thus providing a guideline for engine manufactur-
bondcoats [15].
ers for designing more efficient coatings with optimised ther-
– The coupling of oxidation and mechanical aspects, in
mal properties,
finite element calculations of the stress field (see Fig. 11),
– for studying the relationship between sintering effects
leading to a description of crack initiation modes in agree-
and thermal conductivity increase [44], ment with experimental observations [25].
– to put into light the influence of pressure on thermal – The delamination of compressed films in relation with
barrier coating thermal conductivity, especially in service imperfections and the interface geometry [24].
conditions where no experimental data are available, The knowledge derived from all these approaches, and its
– to estimate the effective thermal conductivity in the case integration in a more physically-based model should serve
of multiphase or multilayer materials. designers and coaters to optimise actual and future thermal
It must be emphasised that the reliability of the results barrier systems with respect to given service conditions.
depends highly on the quality of the various input data:
digital images, thermal conductivity values of the solid
material phases and of the gas inside the pores. In particular, 8. Outlook and conclusion
2D images must be representative of the material structure.
This is generally the case for plasma sprayed coatings but To exploit the full potential of TBCs on highly stressed
may not be the case for anisotropic EBPVD coatings. To rotating turbine components further work has to be directed
overcome this limitation, an extension of this approach is to substantial improvement of the thermal barrier coating
being developed to treat 3D images. system itself. Future research must generate an increased
 U. Schulz et al. / Aerospace Science and Technology 7 (2003) 73–80 79

Fig. 11. Numerical simulation (FEM) of crack initiation and propagation at the alumina/interface in a TBC [9].

understanding of the processing-property interplay of these [7] J.-F. Bisson, D. Fournier, M. Poulain, O. Lavigne, R. Mévrel, J. Am.
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