Accepted Manuscript Not Copyedited

Journal of Heat Transfer.
Received May 24, 2014;

Accepted manuscript posted April 01, 2015. doi:10.1115/1.4030243
Copyright (c) 2015 by ASME
A Comparative Experimental Study on Radiative Properties of
EB-PVD and APS Thermal Barrier Coatings

G Yang, C Y Zhao*
Institute of Engineering Thermophysics, School of Mechanical Engineering,
Shanghai Jiao Tong University, Shanghai, 200240, China.
d
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*Corresponding author, Email: changying.zhao@sjtu.edu.cn; Tel:+86(0)21 34204541
Abstract
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In this paper, the radiative properties of electron beam physical deposition (EB-PVD)
py
and air plasma sprayed (APS) partially yttria stabilized zirconia (YSZ) thermal barrier
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coatings (TBCs) have been comparatively studied for the first time by measuring the
spectral diffuse reflectance and transmittance in a broad spectral band ranging from
ot
250nm to 15μm. The radiation transfer mechanisms inside the coatings are explored
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based on the experimental data and theoretical model. The results indicate that the
distinctive micro-nanostructures of APS and EB-PVD coatings have an important
rip
effect on the radiative heat transfer. In particular, the larger grain boundary and the
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total porosity strongly affect the volume scattering properties of the coatings, and the
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scattering coefficient is closely related to the arrangement of grain boundary as well

as the pore architecture (i.e., its size, morphology, and its distribution). Compared to
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the laminar microstructure of APS thermal barrier coatings, the columnar

microstructure of EB-PVD freestanding coatings exhibits a higher transmittance, a
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lower reflectance and a larger absorption in the spectral region from 400nm to 10μm,
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which leads to an increase of the total heat flux. By modifying the microstructure of
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TBCs properly, the radiative heat flux can be reduced and thereby providing a better
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thermal protection for the metallic substrate.
Keywords: Radiative property, Reflectance; Transmittance; Heat transfer; Thermal

Barrier Coatings (TBCs); Thermal radiation; Microstructure;
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Journal of Heat Transfer. Received May 24, 2014;
Nomenclature
A absorptance
E emittance
eλ b blackbody spectral flux, W/m2
convective heat transfer coefficients on high temperature inside, W/(m2·K)
d
hgas
ite
hair convective heat transfer coefficient on the cold air side, W/(m2·K)
ed
I radiative source function, W/m2
py
G flux quantity, W/m2
spectral extinction coefficient, αλ+σsλ, m-1
Co
Kλ
kc thermal conductivity of coatings, W/(m·K)

ot
k sub thermal conductivity of metal substrate, W/(m·K)
tN
n refractive index of coatings

rip
qrλ radiative heat flux, W/m2

sc
qtot total heat flux, W/m2

nu
p porosity
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T absolute temperature, K
T gas gas temperature, K

ed
Tsurr surrounding temperature, K

pt
x coordinate in semitransparent coatings, mm

ce
Ac
Greek Symbols
αλ absorption coefficient, m-1
δc coating thickness, mm
ε gas emissivity of high temperature gas

ε sub emissivity of metal substrate
ε surr emissivity of hot surrounding
λ wavelength, μm
ρi reflectivity of interface for internally incident radiation
d
ρo reflectivity of interface for externally incident radiation
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σ sλ scattering coefficient, m-1
ed
Ω scattering albedo
py
Co
Subscripts
s relate to scattering
λ relate to wavelength
ot
tN
tot relate to total flux
i, o quantity incident from inside or outside

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+, − flux in positive or negative x direction

sc
nu
Ma
ed
pt
ce
Ac

1. Introduction
Thermal barrier coatings (TBCs) used on advanced turbine blades can considerably
increase engine efficiency and improve the performance of the highly loaded blades
[1-3]. 8 wt.% yttria partially stabilized zirconia (8YSZ) is widely used today as
ceramic top coatings to reduce the Ni-based superalloy temperature because of its low
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density, low thermal conductivity, high melting point, good thermal shock resistance
ite
and excellent erosion resistant properties[4, 5]. Traditionally, there are two processes
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as viable ways to fabricate TBCs under industrial conditions, and they are air plasma
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spray (APS) and electron beam physical vapor deposition (EB-PVD). These two
methods produce characteristic microstructures under certain desirable conditions [6,
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7]. The structure of APS coatings is typically laminar and consists of splats with pores
or cracks parallel to the surface of coatings[8], while EB-PVD top coat consists of
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columnar grains, which are separated by channels normal to the ceramic/metal
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interface. In addition to the micro-sized inter-columnar channels, the YSZ grains

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contain nanometer scale intra-columnar pores[9]. The main advantage of this

microstructure is its superior tolerance against stresses, erosion and thermo shock,
sc
thus giving it a major edge in lifetime. Apart from that, EB-PVD technique also leads
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to aerodynamically favorable smooth surface of the turbine blades, thus eliminating

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the need for final polishing or conditioning of the cooling holes. As a result, EB-PVD
is not only widely used for making TBCs for high pressure turbine blades and but also
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becomes increasingly important for turbine blades of land based industrial gas
turbines [10-13].
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The heat transfer inside TBCs is one of the most critical issues for the application of
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coatings. So far, the majority of studies on the heat transfer inside TBCs mainly focus
on the conduction [14-16]. However, the material of TBCs is semitransparent over a
spectral region where thermal radiation tends to be concentrated (0.35~8μm)[17, 18].
The radiative heat transfer behavior inside the coatings includes volume emission,
absorption and scattering[19], which will become significant at a high temperature

circumstance. In order to obtain the radiative properties in such participating media, it

is highly necessary to conduct experimental measurements on the spectral reflectance,
transmittance and emittance/absorption. Moreover, further research shows that
radiative properties within TBCs depend on the grain structure and pore
architecture[20]. Similar to the phonon scattering, the microstructures would also
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scatter the photon and further affect the radiative heat transfer across the coating.
ite
Since scattering of radiation by particles, fibers, cracks or pores is one of the main
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features of radiative transfer in such disperse systems [21-23], therefore, a
fundamental experimental research on the relationship between microstructures and
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radiative properties is extremely important.
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Although several detailed studies for the microstructural effects on radiative
ot
properties of APS have been reported [24-26], the effects of microstructure on
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radiative properties of EB-PVD freestanding coating are not yet reported. The
comparative study on the radiative properties of APS and EB-PVD TBCs is very
rip
important not only for engineering applications but also for exploring the radiation
sc
transfer mechanisms inside TBCs，since the volume scattering is mainly caused by

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different microstructures inside coatings. Dombrovsky et al. studied the infrared

radiative properties of APS TBCs, and the results indicated that volume scattering is
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closely related to the pore and cracks inside the coatings[27, 28]. It should be pointed
out that the microstructure of APS coating is mainly lamellar, and the general
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distribution of splat boundaries, pores and microcracks is along the coating surface.
pt
However, compared to the APS TBCs, the microstructure of EB-PVD TBCs is

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columnar. The large grain boundaries and intra-columnar pores are mostly
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perpendicular to the substrate, even penetrating through the thickness [29-31]. In

addition, the shadowing effects during deposition together with gas entrapment give
rise to nanoscale intracolumnar porosity consisting of featherlike and globular
pores[32]. Consequently, the volume scattering inside EB-PVD TBCs will be
significantly different from APS TBCs. To the best of our knowledge, there is no
detailed experimental study on the radiative properties of EB-PVD freestanding

micrographs of feather striations for the coatings are shown in Fig. 4.
This type of feathery striations is most evident near the periphery of the larger grain.
It extends inwards to about 1/3 to 1/2 the grain radius, and mostly oriented at 50°~60°
to the substrate plane. As shown in Fig. 4(b), additional presences of intracolumnar
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pores toward the center of the columns can be observed, and these pores are elongated
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spheroids [32, 35]. Image analysis shows that the 400~500nm feathery cracks have a
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typical aspect ratio of 1/10. Besides the feathery striations, another significant feature
of EB-PVD TBCs is that the grain contains a larger number of closed nanometer
py
pores with the size of 20 ~ 200 nm[35], and the quantity of closed nanometer pores
Co
inside the grain will be increased as the grain grows, leading to an important result
that the quantity of nanometer pores will increase with the thickness of coatings.
ot
tN
3.2 APS Freestanding Coatings
The microstructure of air plasma sprayed (APS) thermal barrier coating strongly
rip
depends on the spraying parameters, however, it always shows some certain features.
sc
Standard air plasma sprayed thermal barrier coatings have a typical laminar structure
nu
[36]. The coating has a specific morphology with a lot of cracks parallel to the
substrate as well as orthogonal cracks to the top coating surface [8]. Meanwhile, as
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porous materials, there are a lot of open pores and closed pores existing in the coating
[37]. The SEM images of air plasma sprayed coating under different resolutions are
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shown in Fig. 5.
pt
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The microstructures of APS coatings with various porosities were examined using
Ac
SEM image J software. The result indicates that the APS coatings with a lower
porosity (A4) exhibit a numerous thin lamella structure including enormous
submicron-sized spherical pores with the size of 0.1~0.5μm, while the APS coating
with a medium porosity (A5) displays a multiplayer structure consisting of micro
scale horizontal cracks and spheroid pores with the pore size of 0.8~1.2μm. The high
porosity APS coating (A6) exhibits an irregular microstructure with randomly

measurements are performed by optical microscopy on cross-section samples after the

polishing. Morphological features of APS and EB-PVD PYSZ freestanding coatings
were recorded using a digital scanning electron microscope (FEI-Sirion 200). The
porosity was obtained by using the Archimedes methods and was further validated by
SEM image analysis. The specifications of samples are reported in Table 1.
d
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The EB-PVD and APS freestanding coating samples are illuminated by normally
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incident beam. The cone angle is less than 2º. The experimental system consists of
two main parts, reflectance and transmittance subsystems. The spectral
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directional-hemispherical reflectance and transmittance of the EB-PVD 8YSZ
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freestanding coatings are measured in the ultraviolet and visible region
(250nm<λ<2.5μm) by using Lambda 750S UV/Vis spectrometer with a 60 mm
ot
integrating sphere. Spectrum in the 250nm~860nm wavelength range is collected
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using deuterium lamp source and a high sensitivity R928 photomultiplier detector,
while spectrum in the 860nm~2500nm is collected using a quartz halogen lamp
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source and a lead sulphide (PBS) detector. Fourier transform infrared (FTIR)
sc
spectrometer (Perkin Elmer, Frontier) with a gold-coated integrating sphere accessory

nu
(PIKE) is used to measure the hemispherical transmittance and reflectance in the

infrared region. Spectrum in 2μm~15μm wavelength range are collected using
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proprietary hot-spot stabilization source and KBr beam-splitter, and all spectral
quantities in the Mid-IR are acquired using liquid nitrogen cooled mercury cadmium
ed
telluride (MCT) detector. Every measurement is repeated three times and the average
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value is obtained. Meanwhile, in order to further reduce the H2O and CO2 absorption
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line in the Mid-IR, we purge the FTIR bench with high purity N2 in the measurement
Ac
[33, 34]. In addition, we strictly checked the experimental errors before and after each
measurement, and the average relative error is less than 0.5%. The essential principles
of transmittance and reflectance measurements are shown in Fig. 1.
3. Microstructure Analysis
3.1 EB-PVD Freestanding Coatings

SEM images, conducted to observe microstructural features of EB-PVD freestanding

coatings with two different thicknesses, are presented in Fig. 2. The surfaces of 8YSZ
EB-PVD freestanding coatings have a distinct pyramid or cone-like morphology, and
the arrangement of tip is regular. SEM analyses indicate that the surface roughness of
EB-PVD coating is much smaller compared to the APS thermal barrier coatings. At a
d
larger scale, it can be observed that EB-PVD ceramic coating has a unique columnar
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morphology, and the columnar grains grow almost perpendicular to the substrate and
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extend through the entire thickness, resulting in intercolumnar voids (1 to 3μm wide),
as shown in Figs.2(b).
py
Co
In fact, typical microstructure of 8YSZ EB-PVD coatings can be divided into two
zones (see Figs. 2(a)). inner zone( Ⅰ ) is the early stage of deposition. In
ot
zone(Ⅰ)there are many small nucleate columns, resulting in a high density of
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nanometer-sized intercolumnar pores. With continuous deposition, the small grains
will grow, and the coating structure is characterized by a dominant crystallographic
rip
texture, leading to larger intercolumnar pores as well as larger grain boundaries. In the
sc
outer zone(Ⅱ), the columnar structure becomes more coarse grain and the number of
nu
oblique columnar boundaries decreases. The columns and the elongated intercolumnar
porosity become predominantly aligned perpendicular to the plane of the coating as its
Ma
thickness increases [11, 15, 29]. At the TBCs/bond coating interface, the size of the
columnar grain is very small (<1μm), and it will increase as grain grows. For a
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coating with the thickness of 100μm, the diameter of the columns varies from about
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0.8μm at the roots to about 5μm at the upper part, while for the 200μm thick coating,
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the diameter of the columnar varies from about 1.5μm at the roots to about 7μm at the
Ac
upper part (see Fig. 3). One distinct feature is that the porosity will change from 10%
near the substrate to 20% near the top coating surface due to the increase of the
intercolumnar pores.
Meanwhile, overshadowing effects and gas entrapment give rise to feathery striation
and evenly distributed nanometer pores within the primary columns [30-32]. The

micrographs of feather striations for the coatings are shown in Fig. 4.
This type of feathery striations is most evident near the periphery of the larger grain.
It extends inwards to about 1/3 to 1/2 the grain radius, and mostly oriented at 50°~60°
to the substrate plane. As shown in Fig. 4(b), additional presences of intracolumnar
d
pores toward the center of the columns can be observed, and these pores are elongated
ite
spheroids [32, 35]. Image analysis shows that the 400~500nm feathery cracks have a
ed
typical aspect ratio of 1/10. Besides the feathery striations, another significant feature
of EB-PVD TBCs is that the grain contains a larger number of closed nanometer
py
pores with the size of 20 ~ 200 nm[35], and the quantity of closed nanometer pores
Co
inside the grain will be increased as the grain grows, leading to an important result
that the quantity of nanometer pores will increase with the thickness of coatings.
ot
tN
3.2 APS Freestanding Coatings
The microstructure of air plasma sprayed (APS) thermal barrier coating strongly
rip
depends on the spraying parameters, however, it always shows some certain features.
sc
Standard air plasma sprayed thermal barrier coatings have a typical laminar structure
nu
[36]. The coating has a specific morphology with a lot of cracks parallel to the
substrate as well as orthogonal cracks to the top coating surface [8]. Meanwhile, as
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porous materials, there are a lot of open pores and closed pores existing in the coating
[37]. The SEM images of air plasma sprayed coating under different resolutions are
ed
shown in Fig. 5.
pt
ce
The microstructures of APS coatings with various porosities were examined using
Ac
SEM image J software. The result indicates that the APS coatings with a lower
porosity (A4) exhibit a numerous thin lamella structure including enormous
submicron-sized spherical pores with the size of 0.1~0.5μm, while the APS coating
with a medium porosity (A5) displays a multiplayer structure consisting of micro
scale horizontal cracks and spheroid pores with the pore size of 0.8~1.2μm. The high
porosity APS coating (A6) exhibits an irregular microstructure with randomly

oriented spheroid pores, and the mean pore size is also larger, about 1.6~2.3μm.
4. Experimental Results and Discussions

4.1 Normal hemispherical reflectance and transmittance of EB-PVD and APS
TBCs with various thickness.
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In this experiment, the wavelength region which is measured using different
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equipment contains an overlap region (2μm<λ<2.5μm). Experimental results show
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that there is a very good agreement in the overlap region with the maximum
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differenceless than 1%. The measured normal-hemispherical reflectance and
transmittance for different specimen thickness of APS and EB-PVD freestanding
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coatings are presented in Figs. 6 and 7, respectively.
ot
It's worth noting that the two large absorption peaks near 2.96μm and 6.15μm is
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attributed to the OH bound in the 8YSZ coating, while the small absorption at 4.25μm
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is due to residual CO2 in the IR spectrometer. It can be seen from Fig. 6 that the
normal-hemispherical reflectance for both APS and EB-PVD freestanding coatings
sc
increase with coatings thickness in the spectral region from 500nm to 5.7μm, and the
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trend is more obvious in the short-wave band(600nm~2μm). Meanwhile, it can also

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be observed from Fig.6 that the normal-hemispherical reflectance decreases

monotonically with increasing wavelength in the spectral region from 600nm to 10μm.
ed
However, it is noticeable that the normal-hemispherical reflectance spectra of

EB-PVD freestanding coatings is far below that of APS coatings in the spectral region
pt
from 600nm to 7μm, and the average difference is up to 40% in this specific region.
ce
The large difference on the normal-hemispherical reflectance between APS and

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EB-PVD coatings can only be attributed to their distinctive microstructures, which are
closely related to the arrangement of grain boundaries and the pore architecture (pore
size, morphology as well as distribution), since the volume scattering effects in the
APS and EB-PVD coatings are mainly caused by these specific defects.

It can also be observed from Fig. 7 that both of APS and EB-PVD freestanding
coatings exhibit a considerable transmission in the spectral region from 1μm to 8μm.
However, through a comparative analysis, it can be found that the EB-PVD
freestanding coating presents an even higher transmission than APS coatings, for the
same thickness of APS and EB-PVD coatings, and the average normal-hemispherical
d
transmission reach a difference up to 30% in the Mid-IR region, leading to an even
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higher normal-hemispherical transmission for 200μm EB-PVD coatings than 100μm
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APS freestanding coatings. This result can also be attributed to the distinctive
microstructures of APS and EB-PVD coatings. For the laminar structure of APS
py
coatings, the larger splats boundaries as well as the long and narrow micro crack are
Co
mostly parallel to the coating surface, and this kind of microstructures make scattering
tend to be backscattering, leading to a higher reflectively and a lower transmittance.
ot
On the contrary, for the columnar structure of EB-PVD coatings, the larger grain
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boundaries as well as larger pores (micro level) are mainly perpendicular to coatings
surface (parallel to incident direction), the scattering caused by grain boundary and
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pores dramatically decreases, and this leads to a lower reflectance and a higher
sc
transmittance in the Mid-IR region. In addition, the increasing porosity from the
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substrate surface to the top surface makes the transmittance of EB-PVD coatings
different from APS coatings in the short wavelength range (500nm~2μm).
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Spectral absorptance/emittance is obtained according to closure relationship and

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Kirchhoff’s law. The mathematical expression is as follows:

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E = A = 1− R − T (1)
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Where E is the hemispherical emittance, A is the absorptance, R is the

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hemispherical reflectance, and T is the hemispherical transmittance. The

emittance/absorptance spectra are shown in Fig. 8.
It can be seen from Fig. 8 that absorption/emittance spectra of the 8YSZ APS and
EB-PVD freestanding coatings exhibit strong lattice vibration absorption in the
wavelength region from 5.5 to 8 μm[38], in the spectral region from 8 to 12 μm, both

APS and EB-PVD freestanding coatings present a near blackbody’s behavior, the
absorptivity/emissivity close to unity. While in the short wavelength region, there is a
weak onset of absorption from 500nm, followed by a sharp absorption edge which is
probably attributed to electronic band to band transitions[39, 40]. Moreover, it can be
seen from Fig. 8 that the absorption/emittance spectra of APS freestanding coatings
d
increase with the thickness over the entire spectral range, but for the EB-PVD
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coatings, the absorption/emittance spectra increases with coating thickness only in the
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spectral region that larger than 2.5μm. In the short wavelength region (600 nm~2.5
μm), the absorption/emittance for the 200 μm sample is lower than that of 100 μm,
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and this behavior is believed to be closely related to gradient porosity across the
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thickness for the EB-PVD coatings.
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4.2 Effects of grain boundary and porosity on the normal-hemispherical
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reflectance and transmittance
In order to explore the radiation transfer mechanism and to examine the effects of
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grain boundaries and pore architectures on the radiative properties of TBCs, a

sc
comparative study is performed, and the results are presented in Figs. 9, 10,
nu
respectively.
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Combining Fig.9 and Fig.10, it can be found that increasing the porosity can enhance
the normal hemispherical reflectance and reduce the normal-hemispherical
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transmittance for the APS coatings in a certain range of porosity. According to the
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previous SEM analysis, the quantity of horizontal splats boundaries, microcracks and
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spheroid pores will be increased with the porosity of APS coatings, and it strengthens
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the backscattering. However, for the same porosity, the arrangement of larger grain
boundaries as well as pores perpendicular to coatings surface (EB-PVD TBCs) makes
coatings exhibit a lower reflectance and a higher transmittance than that parallel to
coating surface (APS TBCs), and this effect becomes obvious in the Mid-IR region
(2~6μm). Similarly, the spectral emittance/absorptance of APS and EB-PVD coatings
can be obtained according to Eq. 1. The absorptance/emittance spectra are shown in

Fig.11.
It can be observed from Fig.11 that the spectral absorption/emittance of EB-PVD

coatings is much higher than APS coatings in the spectral region from 500nm to 8μm,
and this result indicates that different arrangement of microstructures not only affects
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the scattering properties but also affects the absorption of thermal barrier coatings.
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Considering the internal volume scattering, this kind of vertical arrangement of larger
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grain will probably increase horizontal absorption [41]. Therefore, the distribution of
grain boundaries has a significant effect on the absorption properties of the coatings.
py
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5. Theoretical Modeling of Radiative Properties
For the disperse media, the simplification of the RTE is focused mainly on transport
ot
approximation and diffusion-based model [22, 42-44]. In this paper, the
tN
Kubelka-Munk four-flux model is used to identify the scattering and absorption

rip
coefficients. More importantly, the relation between these specific radiative properties
and microstructures of APS and EB-PVD thermal barrier coatings will be explored.
sc
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The detailed mathematical description and corresponding solution for the classical
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Kubelka-Munk four flux model is given by Ishimaru[45]. A final correlation between

the model and experimental data is given as follows:
ed
⎧⎪ Rmod el (α λ , σ sλ ) = Rmeasure
⎨ (2)
⎪⎩Tmod el (α λ , σ sλ ) = Tmeasure
pt
Where α λ , σ sλ are absorption and scattering coefficients, Rmod el , Tmod el are normal
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hemispherical reflectance and transmission given by four-flux model, Rmeasure , Tmeasure

Ac
are the reflectance and transmission coming from experimental data. In order to solve
these nonlinear equations, a fitting procedure is used, and the results for the
absorption and scattering coefficient are presented as follows.
5.1 Absorption and scattering coefficients of EB-PVD coatings

In view of the fact that the microstructure of EB-PVD TBCs varies across the coatings
thickness, it is necessary to give the radiative properties of EB-PVD coatings with
different thickness. The obtained results for the spectral scattering and absorption
coefficients in the translucent range (250 nm~8 μm) are shown in Figs. 12 and 13,
respectively.
d
ite
It can be observed from Fig.12 that scattering coefficient decreases dramatically in
ed
spectral region from 250nm to 3 μm, and this is a typical behavior for radiation
scattering by pores with size less than the wavelength[26]. While for the wavelength
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regime from 4 to 8μm, the scattering coefficient is close to zero, and this confirms the
Co
fact that normal-hemisphere reflectance is determined by the front and back surface
reflectance in this specific spectral region. It is noted that in the short wavelength
ot
band (250~1000 nm), scattering coefficient increases with thickness of coatings. As
tN
previously described for microstructures of EB-PVD coatings, the quantity of
micro-nanoscale pores will increase as larger grains grow, and this causes a significant
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scattering for the similar size wavelength. Larger grain boundaries are mostly
sc
perpendicular to the substrate/surface of coatings and the majority of pores in the

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coatings are in nanometer level, therefore, the internal volume scattering caused by
vertical microspores isn’t noticeable, as shown in Fig. 12, the scattering coefficient
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decreases lightly in the spectral region from 2 to 5.5μm.

ed
Fig. 13 displays the absorption coefficient of EB-PVD coatings over the entire
pt
spectrum from 250nm to 8μm. An important result observed is that the absorption
ce
coefficient of 100μm coatings is larger than that of 200μm in the wavelength range
Ac
from 500nm to 2.5μm. This result can be attributed to various microstructures across
coating thickness, especially linked with the gradual transition of porosity.
5.2 A comparison on absorption and scattering coefficients for APS and EB-PVD
thermal barrier coatings
Based on the experimental measurement data and four flux model, the obtained

results for the absorption and scattering coefficient for the APS and EB-PVD coatings
are compared in Figs. 14 and 15, respectively.
It can be observed from Fig.14 that scattering coefficient of APS coatings is obviously
larger than EB-PVD coatings over the entire spectrum from 250nm to 8μm. For the
d
APS thermal barrier coatings, the microstructure is laminar, the splats boundary,
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microcracks and pores are along the coating surface. As previously indicated, this
ed
kind of arrangement makes the scattering tend to be backscattering, which leads to a
higher reflectivity and a lower transmittance. On the contrary, the microstructure of
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EB-PVD coating is columnar, and the larger grain boundaries inside the EB-PVD
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coatings are along the direction perpendicular to coating surface, and this makes the
scattering (which occurs on the grain boundaries) more tend to be forward scattering
ot
which leads to a lower reflectivity and a higher transmittance. One common
tN
microstructure feature shared by APS and EB-PVD coatings is that there are plenty of
nanometer pores existing in coatings, and this will result in a stronger scattering for
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the nanoscale wavelength. Therefore, the arrangement of grain boundary, pore size
sc
and pore distribution will have significant effects on the scattering coefficient, as
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predicted by Zhang et al.[26].

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Similarly, it can be seen from Fig. 15 that absorption coefficient of APS coatings is
lower than EB-PVD coatings over the entire spectrum from 250nm to 8μm, especially
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it becomes significant in the spectrum region from 3 to 7μm. Actually, the 8YSZ
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material with random pores is anisotropic. It means that such a material is

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characterized by different scattering and absorption properties in different

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directions[46]. The vertical-align of larger grain will probably increase horizontal

absorption due to the multiple scattering effects in the Mid-IR region. Hence, the
different microstructure of APS and EB-PVD coatings will also affect the absorption
coefficient.

6. Stationary Temperature Distributions and Radiative Flux

A two-flux model was used to quantitatively evaluate the influence of the
microstructure of EB-PVD and APS coatings on the stationary temperature
distribution and radiative flux across the coatings. The total heat flux within the
coatings is the sum of conduction and radiation, as given by integrating energy
d
equation[19]:
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dT ( x ) ∞
qtot ( x) = −kc + ∫ qrλ ( x, λ )d λ (3)
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dx 0
The radiative flux qrλ ( x) is obtained by the Milne-Eddington two-flux equation
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assuming that the direction dependence of intensity is reduced to two main directions,
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forward ( I λ+ ( x ) ) and backward ( I λ− ( x ) ). Hence, the flux quantity Gλ ( x ) , the radiative
flux qrλ ( x) , and their correlation are given as follows: ot

(
⎧G ( x ) = π I + ( x ) + I − ( x ) )
tN
⎪ λ λ λ
⎨ rλ
(
⎪⎪q ( x ) = π I + ( x ) − I − ( x )
λ λ )
rip
⎪ 1 dGλ ( x )
⎪− ⋅ = qrλ ( x ) (4)
⎪⎩ 3 ⋅ K λ dx
sc
According to the radiative transfer equation (RTE), the flux quantity Gλ ( x ) is

nu
obtained by solving a second-order differential equation including local blackbody

Ma
emission:
d 2Gλ ( x )
− 3K λ2 ⋅ (1 − Ωλ ) ⋅ Gλ ( x ) = −3Kλ2 ⋅ (1 − Ωλ ) ⋅ 4n 2 eλb (T ( x ) ) (5)
ed
2
dx
The boundary conditions are given as follow:
pt
⎧ 2 1 + ρi dGλ ( x ) 1 − ρ0
⎪Gλ ( 0 ) - ⋅ ⋅ = 4⋅ ( (
⋅ ε surr eλb (Tsurr ) + ε gas eλb Tgas ))
ce
⎪⎪ 3K λ 1 − ρ i dx 1 − ρi
x=0
⎨ (6)
⎞ dGλ ( x )
Ac
⎪ 2 ⎛ 2
⎪Gλ (δ c ) + 3K ⋅ ⎜ ε − 1⎟ ⋅ dx = 4n 2 eλb Tδc( )
⎪⎩ λ ⎝ sub ⎠ x =δ c
Where ρo and ρi denote the outward and inward reflectivity at the coating
interface, and they are given as[19]:

1 ( 3n + 1)( n − 1) n ( n − 1) ⎛ n − 1 ⎞ 2n ( n + 2n − 1) 8n4 ( n 4 + 1)
2 2 3 2
ρo = + + ⋅ ln ⎜ ⎟− + ln(n) (7)
6 ( n + 1) ( n2 + 1) ⎝ n + 1 ⎠ ( n2 + 1)( n4 −1) ( n2 + 1)( n4 −1)
2 3 2
2
1
ρi = 1 − (1 − ρo ) (8)
n2
Finally, the temperature distribution in the coating can be derived by integrating the
energy equation to give the form:
d
ite
1 ⎡ 1 ∞ Gλ ( 0 ) − Gλ ( x ) ⎤
T ( x ) = T ( 0) − ⋅ ⎢ qtot ⋅ x − ∫ dλ⎥ (9)
kc ⎣⎢ 3 λ =0 Kλ ⎦⎥
ed
In order to solve the total flux and the temperature, an iterative solution procedure
py
was used by guessing the boundary temperature T ( 0 ) and T (δ c ) , first to obtain Gλ ( x )
Co
according to equation (5), and then obtain the new temperature distribution according
to equation (9), finally the successive iterative values are adjusted to conform to
ot
energy conservation. As an additional final step, the radiative fraction to total flow is
tN
calculated according to equation (3).
rip
In this paper, TBCs material is assumed opaque in the spectral region λ > 8 μm
sc
according to Fig.11. We divide the translucent spectral region into three bands, and
nu
the scattering and absorption coefficient are averaged and considered as constants in
each band. Moreover, we remove the OH band and CO2 bands and extrapolate the
Ma
results based on polynomial fitting. The model parameters are given in Table 2.
ed
The obtained stationary temperature distributions as well as total heat flux across the
pt
APS and EB-PVD coatings are presented in Fig. 16. It can be seen from Fig. 16 that
ce
the higher translucence of 8YSZ EB-PVD coatings increases the total heat flux,
Ac
leading to a higher temperature distribution at the metal wall. In addition, the results
show that the radiative heat flux could account for total heat flux up to 40% for the
EB-PVD coatings and 30% for the APS coatings. The above results can be attributed
to the microstructural effects of APS and EB-PVD TBCs. For practical engineering
applications, we can effectively reduce the radiative heat flux as well as substrate
metal temperature by optimizing the microstructures of TBCs.

7. Conclusions
The radiative properties of 8YSZ EB-PVD and APS freestanding coatings have been
experimentally investigated in a broad wavelength region from 250 nm to 15 μm.
Comparative results reveal that the microstructure of TBCs has a significant effect on
d
their radiative properties. Compared to the laminated structure of APS TBCs, the
ite
columnar structure of EB-PVD TBCs exhibits a higher transmittance and a lower
ed
reflectance in a broad spectral region from 400 nm to 10 μm. The study shows that the
py
volume scattering inside TBCs closely depends on pore architecture and distribution
of grain boundaries. The scattering coefficient of EB-PVD TBCs is strongly affected
Co
by the micro or nanoscale pores (400 nm~1 μm) which is characterized by feathery
striation and closed pores inside the grain, while the scattering coefficient of APS
ot
TBCs is mainly determined by the horizontal cracks as well as the oblate spheroids
tN
with the size of 400 nm~3 μm. Compared to the laminated APS TBCs, the vertical
rip
arrangement of larger grains inside the EB-PVD coatings can cause a stronger
absorption in the Mid-IR region (3μm~7μm). For practical engineering applications,
sc
the radiative heat flux and substrate temperature can be effectively reduced by
nu
optimizing the pore microstructure of TBCs.

Ma
Acknowledgments
ed
This work is supported by the National Natural Science Foundation of China (Grant
Nos: 51476097 and 51176110).
pt
ce
Reference
Ac
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List of Tables
Table1 Thermal barrier coatings samples investigated
Table 2 The parameters used in two flux model
Table1.Thermal barrier coatings samples investigated
d
ite
Sample Name
ed
A1 A2 A3 A4 A5 A6
Deposition EB-PVD EB-PVD APS APS APS APS
py
Thickness(μm) 100±2 200±4 100±2 200±4 200±4 200±4
Porosity (%) 12.5 17.3 16.7 5.5 17.1 25.3
Co
ot
Table 2. The parameters used in two flux model
tN
Name kc(W/m·K) Bands(μm) σ sλ (m-1) α λ (m-1) Ω

rip
0.3~1 63995 490 0.9924

EB-PVD 1.5 1~5 5115 820 0.861824
sc
5~8 51 9650 0.005165

0.3~1 104705 1590 0.985041
nu
APS 0.8 1~5 49690 125 0.997489

Ma
5~8 8690 9065 0.48944

ed
pt
ce
Ac

Figure Captions
Fig. 1 Measurement principle of hemispherical transmittance/reflectance
Fig. 2 SEM micrographs of 8YSZ EB-PVD freestanding coatings with thickness of 200μm; (a) Cross
section of coating, (b) Top surface of coating
Fig. 3 Microstructure feature of cross section of 8YSZ EB-PVD coatings; (a) Bottom features of
d
200μm freestanding coatings, (b) Top features of 200μm freestanding coatings
ite
Fig. 4 Cross-sectional SEM micrographs revealing feathery striations; (a) The primary columns with
ed
feathery structure, (b) Feathery striations at a higher resolution
Fig. 5 SEM micrographs of air plasma sprayed coating with the porosity of 15%; (a) Surface section
py
(A5), (b) Cross section (A5)
Co
Fig. 6 Spectral normal-hemispherical reflectance of 8YSZ APS and EB-PVD freestanding coatings
Fig. 7 Spectral normal-hemispherical transmittance of 8YSZ APS and EB-PVD freestanding coatings
ot
Fig. 8 Emittance/absorptance spectra of 8YSZ APS and EB-PVD freestanding coatings
tN
Fig. 9 Effects of grain boundary and porosity on the normal-hemispherical reflectance of 8YSZ
rip
APS and EB-PVD freestanding coatings
Fig. 10 Effects of grain boundary and porosity on the normal-hemispherical transmittance of 8YSZ
sc

nu
Fig. 11 Effects of grain boundary and porosity on the emittance/absorptance spectra of 8YSZ APS and
EB-PVD freestanding coatings

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Fig. 12 Spectral scattering coefficients of EB-PVD coatings
Fig. 13 Spectral absorption coefficients of EB-PVD coatings

ed
Fig. 14 Spectral scattering coefficients for APS and EB-PVD thermal barrier coatings
pt
Fig. 15 Spectral absorption coefficients for APS and EB-PVD thermal barrier coatings
ce
Fig.16 Temperature distribution in the coating-metallic systems

Ac

d
ite
ed
py
Fig. 1 Measurement principle of hemispherical transmittance/reflectance
Co
ot
tN
rip
sc
nu
(a) Cross section of coating (b) Top surface of coating
Fig. 2 SEM micrographs of 8YSZ EB-PVD freestanding coatings with thickness of 200μm
Ma
ed
pt
ce
Ac
(a) Bottom features of 200μm freestanding coatings (b) Top features of 200μm freestanding coatings
Fig. 3 Microstructure feature of cross section of 8YSZ EB-PVD coatings

d
ite
(a) The primary columns with feathery structure (b) Feathery striations at a higher resolution
ed
Fig. 4 Cross-sectional SEM micrographs revealing feathery striations
py
Co
ot
tN
rip
(a) Surface section (A5) (b) Cross section (A5)

sc
Fig. 5 SEM micrographs of air plasma sprayed coating with the porosity of 15%
nu
Ma
ed
pt
ce
Ac

80
Thickness=100μm, Porosity=12.5%, EB-PVD Thickness=200μm, Porosity=17.3%, EB-PVD
Normal-Hemispherical Reflectance R/% Thickness=100μm, Porosity=16.7%, APS Thickness200μm, Porosity=17.1% APS
70 80
Normal-Hemispherical Reflectance R/%

70
60
60
50
40
50
30
d
20
ite
40 10
0
200 400 600 800 1000 1200 1400 1600 1800 2000
ed
30 Wavelength λ/nm
py
20
Co
10
0 ot
0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16
Wavelength λ/μm
tN
Fig. 6 Spectral normal-hemispherical reflectance of 8YSZ APS and EB-PVD freestanding coatings
rip
80
sc
Thickness=100μm, Porosity=12.5%, EB-PVD Thickness=200μm, Porosity=17.3%, EB-PVD

Thickness=100μm, Porosity=16.7%, APS Thickness=200μm, Porosity=17.1%, APS
Normal-Hemispherical Transmittance T/%
70
nu
Hemispherical Transmittance T/%
60
50
60
Ma
40
30
50
20
ed
40 10
pt
0
0 200 400 600 800 1000 1200 1400 1600 1800 2000
30 Wavelength λ/nm
ce
20
Ac
10
0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16
Wavelength λ/μm
Fig. 7 Spectral normal-hemispherical transmittance of 8YSZ APS and EB-PVD freestanding coatings

100
90
80
Absorption/Emittance A/%
70
60
d
ite
50
40
ed
30
py
20 Thickness=100μm, Porosity=12.5%, EB-PVD
Co
Thickness=200μm, Porosity=17.3%, EB-PVD
10 Thickness=100μm, Porosity=16.7%, APS
Thickness=200μm, Porosity=17.1%, APS
0 ot
0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16
Wavelength λ/μm
tN
Fig. 8 Emittance/absorptance spectra of 8YSZ APS and EB-PVD freestanding coatings

rip
90
Thickness=200μm, Porosity~17.3% EB-PVD
Thickness=200μm, Porosity~5.5% APS
80
sc

70
nu
90
80
70
60
Ma
60
50
50 40
30
ed
40 20
10
0
pt
30 0 200 400 600 800 1000 1200 1400 1600 1800 2000
Wavelength λ/nm
ce
20
Ac
10
0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16
Wavelength λ/μm
Fig. 9 Effects of grain boundary and porosity on the normal-hemispherical reflectance of 8YSZ

60
Normal-Hemispherical Transmittance T/%
50
50
Hemispherical Transmittance T/%

40
40
d
30
30
ite
20
ed
10
20
0
py
0 200 400 600 800 1000 1200 1400 1600 1800 2000
Wavelength λ/nm
10
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0
0 1 2 3 4 5 6 7 8
ot
9 10 11 12 13 14 15 16
Wavelength λ/μm
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Fig. 10 Effects of grain boundary and porosity on the normal-hemispherical transmittance of 8YSZ
rip

sc
nu
Ma
ed
pt
ce
Ac

100
90
80
Absorption/Emittance A/%
70
60
d
ite
50
ed
40
30
py
20 Thickness=200μm, Porosity~5.5% APS
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10
0
0 1 2 3 4 5 6 7 8
ot9 10 11 12 13 14 15 16
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Wavelength λ/μm
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Fig. 11 Effects of grain boundary and porosity on the emittance/absorptance spectra of 8YSZ

sc
nu
Ma
ed
pt
ce
Ac

5
1.2x10
5
1.0x10
-1
5
Scattering coefficient σsλ/m
1.2x10
Scattering coefficient σsλ/m-1

5
4 1.0x10
8.0x10
4
8.0x10
d
4
ite
6.0x10 4
6.0x10
ed
4.0x10
4
4.0x10
4
2.0x10
py
4 0.0
2.0x10 0 400 800 1200 1600 2000
Co
Wavelength λ/nm
0.0
0 1 2 3 ot 4 5 6 7 8
Wavelength λ/μm
tN
Fig. 12 Spectral scattering coefficients of EB-PVD coatings

rip
4
sc
2.1x10
Thickness=200μm, 5000
-1
Porosity=17.3%, EB-PVD
Absorption coefficient aλ/m
nu
4 Thickness=100μm, 4000
1.8x10
-1
Porosity=12.5%, EB-PVD
3000
Ma
4
1.5x10 2000
1000
4
1.2x10
ed
0
0 500 1000 1500 2000 2500
Wavelength λ/nm
pt
3
9.0x10
ce
3
6.0x10
Ac
3
3.0x10
0.0
0 1 2 3 4 5 6 7 8
Wavelength λ/μm
Fig. 13 Spectral absorption coefficients of EB-PVD coatings

5
1.6x10
5 Thickness=200μm, Porosity~5.5% APS
1.4x10 Thickness=200μm, Porosity~17.1% APS
-1

Scattering coefficient σsλ/m
5 5
1.2x10 1.6x10
-1
Scattering coefficient σ /m
5
1.4x10
sλ
5
5 1.2x10
1.0x10 5
1.0x10
d
4
8.0x10
4
ite
8.0x10 6.0x10
4
4
4.0x10
4
ed
4
6.0x10 2.0x10
0.0
200 400 600 800 1000 1200 1400 1600 1800 2000
4 Wavelength λ/nm
py
4.0x10
4
2.0x10
Co
0.0
0 1 2 3 ot4 5 6 7 8
Wavelength λ/μm
tN
Fig. 14 Spectral scattering coefficients for APS and EB-PVD thermal barrier coatings
rip
4
sc
2.4x10 750
Thickness=200μm,
Absorption coefficient aλ/m-1
Porosity~17.3%, EB-PVD
4
nu
600
2.1x10 Thickness=200μm,
Porosity~5.5%, APS
-1
4
1.8x10
Ma
Porosity~17.1%, APS
Porosity~25.3%, APS
4
1.5x10 150
ed
4 0
1.2x10 400 800 1200 1600 2000
Wavelength λ/nm
pt
3
9.0x10
ce
3
6.0x10
Ac
3
3.0x10
0.0
0 1 2 3 4 5 6 7 8
Wavelength λ/μm
Fig. 15 Spectral absorption coefficients for APS and EB-PVD thermal barrier coatings

1650
APS
EB-PVD
Temperature distribution T(x), K
1600 Metal Wall
1550
2
qtot=1462590,W/m
d
ite
1500
ed
1450
2
qtot=1230780,W/m
py
8YSZ TBCs
1400
Co
n=2.1
1350
0.0 0.1 0.2 0.4 ot 0.6 0.8 1.0
Position within coating and metal, x, mm
tN
Fig.16 Temperature distribution in the coating-metallic systems

rip
Parameter: Tgas=1950K, Tsurr=1700K, hgas=2200W/ (m2.K), hair=1000W/ (m2.K), εgas=0.3,
εsurr=1.0, εsub=0.6, ksub=25.4 W/(m·K), n=2.1. Porosity=17.1 %( APS), Porosity=17.3 %( EB-PVD),

sc
Thickness=200μm (TBCs), Thickness=0.8mm (metal)

nu
Ma

ed
pt
ce
Ac

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Journal of Heat Transfer.

Received May 24, 2014;

A Comparative Experimental Study on Radiative Properties of

EB-PVD and APS Thermal Barrier Coatings

scattering coefficient is closely related to the arrangement of grain boundary as well

the laminar microstructure of APS thermal barrier coatings, the columnar

thermal protection for the metallic substrate.

Keywords: Radiative property, Reflectance; Transmittance; Heat transfer; Thermal

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eλ b blackbody spectral flux, W/m2

convective heat transfer coefficients on high temperature inside, W/(m2·K)

spectral extinction coefficient, αλ+σsλ, m-1

kc thermal conductivity of coatings, W/(m·K)

n refractive index of coatings

qrλ radiative heat flux, W/m2

qtot total heat flux, W/m2

T gas gas temperature, K

Tsurr surrounding temperature, K

x coordinate in semitransparent coatings, mm

αλ absorption coefficient, m-1

ε gas emissivity of high temperature gas

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ε sub emissivity of metal substrate

ε surr emissivity of hot surrounding

ρi reflectivity of interface for internally incident radiation

i, o quantity incident from inside or outside

+, − flux in positive or negative x direction

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interface. In addition to the micro-sized inter-columnar channels, the YSZ grains

contain nanometer scale intra-columnar pores[9]. The main advantage of this

to aerodynamically favorable smooth surface of the turbine blades, thus eliminating

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circumstance. In order to obtain the radiative properties in such participating media, it

transfer mechanisms inside TBCs，since the volume scattering is mainly caused by

different microstructures inside coatings. Dombrovsky et al. studied the infrared

However, compared to the APS TBCs, the microstructure of EB-PVD TBCs is

perpendicular to the substrate, even penetrating through the thickness [29-31]. In

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micrographs of feather striations for the coatings are shown in Fig. 4.

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measurements are performed by optical microscopy on cross-section samples after the

spectrometer (Perkin Elmer, Frontier) with a gold-coated integrating sphere accessory

(PIKE) is used to measure the hemispherical transmittance and reflectance in the

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SEM images, conducted to observe microstructural features of EB-PVD freestanding

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micrographs of feather striations for the coatings are shown in Fig. 4.

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4. Experimental Results and Discussions

trend is more obvious in the short-wave band(600nm~2μm). Meanwhile, it can also

be observed from Fig.6 that the normal-hemispherical reflectance decreases

However, it is noticeable that the normal-hemispherical reflectance spectra of

The large difference on the normal-hemispherical reflectance between APS and

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Spectral absorptance/emittance is obtained according to closure relationship and

Kirchhoff’s law. The mathematical expression is as follows:

Where E is the hemispherical emittance, A is the absorptance, R is the

hemispherical reflectance, and T is the hemispherical transmittance. The

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grain boundaries and pore architectures on the radiative properties of TBCs, a

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It can be observed from Fig.11 that the spectral absorption/emittance of EB-PVD

Kubelka-Munk four-flux model is used to identify the scattering and absorption