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Xingye Guo
Zhe Lu
Yeon-Gil Jung
Jing Zhang
Novel Lanthanum
Zirconate-based
Thermal Barrier
Coatings for Energy
Applications
Novel Lanthanum Zirconate-based Thermal Barrier
Coatings for Energy Applications
Xingye Guo • Zhe Lu
Yeon-Gil Jung • Jing Zhang
Novel Lanthanum
Zirconate-based Thermal
Barrier Coatings for Energy
Applications
Xingye Guo Zhe Lu
Faculty of Materials and Manufacturing School of Materials and Metallurgical
Beijing University of Technology Engineering
Beijing, China University of Science and Technology
Liaoning
Yeon-Gil Jung Anshan, Liaoning, China
School of Materials Science and
Engineering Jing Zhang
Changwon National University Department of Mechanical and Energy
Changwon, Republic of Korea Engineering
Indiana Univ Purdue Univ Indianapolis
Indianapolis, IN, USA
ISBN 978-3-030-58694-2 ISBN 978-3-030-58695-9 (eBook)

https://doi.org/10.1007/978-3-030-58695-9
© Springer Nature Switzerland AG 2021

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Preface
Thermal barrier coatings (TBCs) are refractory materials deposited on gas turbine
components, which provide thermal protection for metallic components at operat-
ing conditions. Recently, lanthanum zirconate has emerged as a promising candi-
date material for TBC applications, due to its lower thermal conductivity and higher
thermal stability compared to traditional TBC systems, such as yttria-stabilized
zirconia.
This book describes the latest developments of lanthanum zirconate–based
thermal barrier coatings. Chapter 1 summarizes the manufacturing techniques of
lanthanum zirconate powder and thermal barrier coatings. Chapter 2 presents the
physical, thermal, and mechanical properties of lanthanum zirconate powder and
coatings. Processing and characterizations of lanthanum zirconate powder and
coatings under various conditions are also examined. Theoretical studies on the
powder and coating’s mechanical properties are presented in Chap. 3. Chapter 4
discusses the modeling work of the thermal properties of the powder and coat-
ings. Chapter 5 focuses on the theoretical studies of the mechanical properties at
the interface between the ceramic top coat and metallic substrate. Future research
directions of lanthanum zirconate as the next-generation thermal barrier applica-
tions are proposed in Chap. 6.
This work is the fruit of international scientific collaboration. Xingye Guo
acknowledges the support by the National Natural Science Foundation of China
(No. 51901006) and Scientific Research Program of Beijing Municipal Education
Committee (KM202010005006). Zhe Lu acknowledges the support by the National
Natural Science Foundation of China (No. 51702145). Yeon-Gil Jung acknowledges
the financial support by the “Human Resources Program in Energy Technology”
of the Korea Institute of Energy Technology Evaluation and Planning (KETEP),
which is granted from the Ministry of Trade, Industry & Energy, Republic of Korea
(No. 20194030202450), and by the National Research Foundation of Korea (NRF)
grant funded by the Korea government (MSIP) (2018R1A5A6075959). Jing Zhang
acknowledges the support by the U.S. Department of Energy (No. DE-FE0008868).
v
vi Preface
Any comments and suggestions about the work are greatly appreciated. Please
send the message to Jing Zhang, jz29@iupui.edu.
Beijing, China Xingye Guo

Anshan, China Zhe Lu
Changwon, Republic of Korea Yeon-Gil Jung
Indianapolis, IN, USA Jing Zhang
Contents
1 Overview of Lanthanum Zirconate-Based Thermal Barrier

Coatings�� 1
1.1 Thermal Barrier Coatings �� 1
1.2 Synthesis of Lanthanum Zirconate Powder�� 3
1.3 Crystal Structure of Lanthanum Zirconate �� 4
1.4 Deposition Techniques of Lanthanum Zirconate-Based
Coatings�� 5
References�� 10
2 Properties of Lanthanum Zirconate–Based Thermal Barrier
Coatings�� 13
2.1 Physical Properties�� 13
2.1.1 Coating Density and Porosity �� 13
2.1.2 Sintering Behavior�� 14
2.1.3 Morphology of Coating Cracks and Pores�� 15
2.2 Mechanical Properties�� 15
2.2.1 Elastic Modulus�� 15
2.2.2 Hardness and Fracture Toughness�� 16
2.2.3 Erosion Resistance�� 17
2.3 Thermal Properties�� 18
2.3.1 Melting Point Temperature and Specific Heat Capacity�� 18
2.3.2 Thermal Conductivity �� 20
2.3.3 Coefficient of Thermal Expansion�� 22
2.3.4 Furnace Cycling Test (FCT) and Jet Engine Thermal
Shock (JETS) Test�� 24
References�� 25
3 Modeling of Mechanical Properties of Lanthanum Zirconate
Crystal�� 29
3.1 Motivation and Introduction �� 29
3.2 Theoretical LZ Model �� 30
3.2.1 DFT Model�� 30
vii
viii Contents
3.2.2 MD Model�� 33

3.3 LZ Crystal Constant Optimization�� 34
3.4 Stress-Strain Analysis and Anisotropic Elastic Moduli�� 36
3.4.1 Large Deformation Stress-Strain Analysis�� 36
3.4.2 Small Deformation Elastic Moduli Calculation�� 37
3.4.3 Bader Charge Analysis and Charge Density
Distribution �� 40
3.4.4 MD Tensile and Shear Simulations�� 41
3.5 Summary �� 43
References�� 45
4 Modeling of Thermal Properties of Lanthanum Zirconate
Crystal�� 47
4.1 Introduction of Thermal Properties Calculations�� 47
4.2 Thermodynamic Energy and Specific Heat of LZ�� 48
4.3 Thermal Conductivity of LZ �� 50
4.3.1 Thermal Conductivity of Single Crystal LZ Using
MD Simulation �� 50
4.3.2 Thermal Conductivity of Polycrystalline LZ Coating
By Using FE Method�� 53
References�� 56
5 Modeling of Mechanical Properties of Zirconia Top Coat
and Bond Coat Interface �� 59
5.1 Introduction of Interface Modeling�� 59
5.2 DFT Methods of ZrO2/Ni Interface Model �� 60
5.2.1 ZrO2 (111)/Ni (111) Interface Model�� 60
5.2.2 Adiabatic Work of Adhesion�� 62
5.2.3 Stress-Strain Behaviors in Tensile
and Shear Deformations�� 62
5.2.4 Bader Charge Analysis�� 62
5.3 DFT Interface Modeling Results and Discussion �� 62
5.3.1 Adiabatic Work of Adhesion�� 62
5.3.2 Stress-Strain Behaviors in Tensile
and Shear Deformations�� 63
5.3.3 Charge Density and Bader Charge Analyses�� 69
5.4 MD Tensile and Shear Simulations of ZrO2/Ni Interface
Model�� 72
References�� 77
6 Concluding Remarks and Future Research Directions�� 79
6.1 Concluding Remarks�� 79
6.2 Outlook of Future Work�� 81
Index�� 83
Author Biographies
Xingye Guo is an assistant professor in the Faculty of

Materials and Manufacturing at Beijing University of
Technology, China. He obtained his PhD in mechanical
engineering from Purdue University. Dr. Guo is the
recipient of the International Thermal Spray Association
(ITSA) scholarship for thermal barrier coating studies
in 2017. His research interests include thermal/environ-
mental barrier coatings and multi-scale modeling. Dr.
Guo’s research is supported by the National Natural
Science Foundation of China and Scientific Research
Program of Beijing Municipal Education Committee.
Zhe Lu is an assistant professor of materials and met-
allurgical engineering at the University of Science and
Technology Liaoning, China. He received his PhD
from Changwon National University. Dr. Zhe is active
in the research fields of fracture mechanics in nano- and
micro-structured materials, material design and fabri-
cation of advanced structural ceramics, ceramic-matrix
composites, and thermal and mechanical properties in
thermal barrier coatings. His research is supported by
the National Natural Science Foundation of China.
Yeon-Gil Jung is a professor of materials science
and engineering at Changwon National University. He
received his PhD in inorganic materials science and engi-
neering from Hanyang University. Professor Jung was a
visiting scientist at NIST during 1997–1999 and 2003–
2004. He has an h-index of 29, an i10-index of 91, and
his works have been cited 3678 times (Google Scholar,
2020). Professor Jung has contributed to over 330 publi-
cations and acts as a reviewer on 10 international journals.
ix
x Author Biographies
Jing Zhang is an associate professor of mechanical

and energy engineering at Indiana University – Purdue
University. He received his PhD in materials science
and engineering from Drexel University. Professor
Zhang’s research interests include high-temperature
materials and additive manufacturing. His research has
been funded by the U.S. DOE, NSF, NASA, AFRL, and
the industry.
Chapter 1
Overview of Lanthanum Zirconate-Based
Thermal Barrier Coatings
1.1 Thermal Barrier Coatings
The development of gas turbine engines relates to a great variety of engineering

disciplines including turbine design, combustion, and cutting-edge materials. The
application of thermal barrier coatings (TBCs) on turbine components has dramati-
cally increased the operation temperature and lifetime of the alloy components in
gas turbine engine [1]. The engine efficiency of gas turbines is increased due to the
increase of operation temperature [2]. TBCs were initially introduced to the gas-
turbine industry in the mid-1970s [3]. Nowadays, TBCs are widely used in aeronau-
tics, astronautics, motor industry, and heat power stations. They are extensively
applied in high-temperature components of gas turbines to protect the surface of
metallic parts, such as combustor wall, rotating blades, stationary guide vanes,
blade outer air seals, and afterburners in the tail section of jet engines and so on,
because, in general, superalloy materials used as substrate of high-temperature
components allow a temperature below 1100 °C [4–7]. TBCs are multilayered coat-
ing systems deposited on the turbine components, especially the turbine blade,
which can thermally insulate them and protect them against hot and corrosive gas
stream [1, 6, 8].
The typical structure of TBCs includes four layers: (1) superalloy substrate, (2)
bond coat, (3) thermally grown oxide (TGO), and (4) ceramic top coat. The bond
coat consists of an MCrAlN intermetallic alloy with a thickness of 100–300 μm,
where M is an element selected from nickel, cobalt, iron, and their mixture, and N
is an element selected from yttrium, zirconium, hafnium, ytterbium, and mixture
thereof [9]. Typically, the ceramic top coat can be deposited directly on the substrate
using various techniques, such as air plasma spraying (APS), high-velocity oxygen-
fuel (HVOF) spraying, vacuum plasma spraying, low-pressure plasma spraying,
and diffusion deposition method [10–13]. In high-temperature operation conditions,
the bond coat is inevitably oxidized and a TGO layer is formed at the interface
between the bond and the top coats with a thickness of 1–10 μm. The main
© Springer Nature Switzerland AG 2021 1

X. Guo et al., Novel Lanthanum Zirconate-based Thermal Barrier Coatings for
Energy Applications, https://doi.org/10.1007/978-3-030-58695-9_1
2 1 Overview of Lanthanum Zirconate-Based Thermal Barrier Coatings
composition of TGO is α-alumina (α-Al2O3), which can work as a good oxygen dif-
fusion barrier to protect the bond coat and substrate from further oxidation. On the
other hand, the growth of the TGO layer can lead to TBC failure [14]. The ceramic
top coat is one or multiple low-thermal conductivity ceramic layers with a typical
thickness of 100–600 μm, which is deposited by the APS or electron-beam physical
vapor deposition (EB-PVD) methods [5, 8]. The criteria for TBCs material selection
include high melting point, low thermal conductivity, high CTEs, good thermal and
chemical stability, no phase change, low sintering activity, good erosion resistance,
and good foreign objective damage (FOD) or calcium–magnesium–alumino-silicate
(CMAS) resistance [15].
Currently, the state-of-the-art TBCs are 7–8wt % yttria (Y2O3)-stabilized zirco-
nia (ZrO2) (8YSZ). The 8YSZ has a metastable tetragonal phase (t′), and Y2O3 is
used to stabilize the ZrO2 structure. The 8YSZ has a relatively high melting point
(2680 °C) [15], relatively low thermal conductivity about 2.0–2.3 W/m/K around
1000 °C for a fully dense status (0.9–1.2 W/m/K for 10–15% porosity) [16, 17], a
relatively high CTEs (11 × 10−6 /K at 1000 °C) [15], and good thermal and chemical
stability [18]. However, the maximum surface temperature that can be employed as
TBCs of 8YSZ is limited to 1200 °C for long-time operation. At temperatures above
1200 °C, two important degradation mechanisms occur in 8YSZ. The first mecha-
nism is that the t′ phase of YSZ will decompose to two equilibrium phases: tetrago-
nal (t) and cubic (c) phases. During the cooling process, the t phase will transform
to the monoclinic (m) phase, causing ~4% volume expansion. The second mecha-
nism is the sintering of coating, which will change the microstructure as well as the
mechanical and thermal properties. The phase change and sintering, and the associ-
ated thermal and mechanical property changes will finally lead to high thermally
induced stress and shorten the coating’s lifetime [15]. However, some approaches
can be chosen to enhance TBCs’ performance: (1) find a new feedstock powder with
a higher sintering resistance or no phase change and (2) control the porosity of
TBCs [19]. In addition, increasing the thickness of top coat can reduce the substrate
temperature, although the performance of TBC still remains the same.
Lanthanum zirconate (La2Zr2O7, LZ) is a typical pyrochlore structure ceramic
material. The general chemical formula of the pyrochlore structure is A2B2O7.
The A element in A2B2O7 generally is a rare earth or an element with an inert
single pair of electrons and the B element typically is a transition metal or a post-
transition metal with a variable oxidation state [10, 20]. Compared to 8YSZ, LZ
is more advantageous in the application of TBCs: (1) no phase transformation
from room temperature to its melting temperature is noted, (2) has a considerably
high sintering resistance, (3) has a very low thermal conductivity (1.5–1.8 W/m/K
at 1000 °C for a fully dense material), and (4) has a lower oxygen ion diffusivity,
which protects the bond coat and the substrate from oxidation [15]. The principal
drawback of LZ is its small CTE, which does not match the high CTE of the
bond coat.
1.2 Synthesis of Lanthanum Zirconate Powder 3
1.2 Synthesis of Lanthanum Zirconate Powder
There are several ways to synthesize LZ powder, which can be used in thermal spray
process, including solid state reaction method, co-precipitation method, and the sol-
gel method [15, 21–23].
LZ powder can be synthesized by solid state reaction method from a mixture of
lanthanum oxide (La2O3, 99.9%) and ZrO2 (99%) powders at high temperatures
(T = 1773 K) under an argon atmosphere for 10 h [21, 22]. The pure La2O3 is typi-
cally prepared by dissolving La2(CO3)3·8H2O in nitric acid and subsequently pro-
ducing a precipitate by adding NH3. The precipitate is dried in air and then heated
in oxygen at 1173 K to remove the nitrogen-containing fragments. The La2O3
obtained is heated at 1473 K to remove any absorbed water [21]. The LZ powder
thus obtained is spherical or ellipsoidal in shape with a porous microstructure on the
surface. The theoretical chemical composition of LZ powder coating is La 48.6 wt%,
Zr 31.9 wt%, O 19.5 wt%, which is equivalent to 1:2 molar ratios of La2O3 and
ZrO2 [18].
In the co-precipitation method, an aqueous solution of lanthanum nitrate hexahy-
drate (La(NO3)3·6H2O) and zirconium oxychloride (ZrOCl2·8H2O) with a diluted
NH3 solution is used to prepare LZ powder [15]. During this preparation process,
La(NO3)3·6H2O and ZrOCl2·8H2O are dissolved in distilled water in equimolar
amounts. The liquid mixtures are slowly added under stirring to an ammonium
hydrate solution at pH 12.5. The precipitate obtained is filtered, washed with dis-
tilled water, and then dried at 120 °C overnight. The remaining solid is then calcined
at 900 °C for 5 h.
The sol-gel method is another way to synthesize nanostructured powders, which
have high sintering ability for the A2Zr2O7 (A = La, Nd, Sm) system [23]. Tang et al.
fabricated LZ fibers by a sol-gel combined electrospinning method [24]. LaCl3·7H2O
(9 mmol) was dissolved in zirconium acetate solution in an equimolar ratio and
0.4 g silica sol (SiO2, 22%, pH = 3.2) was added with magnetic stirring for 6 h. The
transparent sol was added to absolute ethanol (8.0 ml) with polyvinylpyrrolidone
(PVP, 0.4 g). The sol was transferred into a syringe and 20 kV power was supplied
between the syringe tip and a stainless steel collector. The LZ gel fibers were fabri-
cated on the collector under the electrostatic force, after the dry and calcination
processes at high temperatures.
In addition to the aforementioned three commonly used methods, other methods
also can fabricate LZ powders. Tong et al. prepared LZ nanopowder using stearic
acid combustion method [25]. La(NO3)3·nH2O and Zr(NO3)4·9H2O were used as
the precursors, and stearic acid (C17H35COOH) was used as the solvent and disper-
sant. The mixed solution was ignited in the air, and the obtained powder was cal-
cined at a series of increasing temperatures ranging from 600 to 900 °C for 5 h in
the air.
1.3 Crystal Structure of Lanthanum Zirconate
LZ is a typical ZrO2-Ln2O3 system (Ln is lanthanide elements, Ln = La → Gd),

which has a pyrochlore structure with space group Fd 3 m [26]. Although the com-
pounds Ln2Zr2O7 (Ln = La → Gd) are stable at room temperature, an order-disorder
transition occurs at high temperatures (>1500 °C). For example, the compounds get
transferred from pyrochlore to defect fluorite structure, with the only exception of
LZ (actually Ln2Zr2O7, Ln = Tb → Lu adopt the defect fluorite structure) [20]. The
transition temperature depends on the radius of Ln ions (La, no transition; Nd,
2300 °C, Sm 2000 °C, and Gd 1530 °C) [27].
X-ray diffraction is widely used to identify crystal structures. Figure 1.1 shows
the X-ray diffraction patterns of several Ln2Zr2O7 materials at room temperature
[23]. Two peaks indexed (331) and (511) shown in the LZ pattern originate from the
pyrochlore structure, which are also observed in Nd2Zr2O7, Sm2Zr2O7, and Gd2Zr2O7
patterns. Other peaks are commonly observed for pyrochlore and defect fluorite
structures [23].
The Ln2Zr2O7 pyrochlore crystal is a cubic structure in space group Fd 3 m (ori-
gin choice 2) with four crystallographically independent atom sites (rare earth ion
1 1 1 1 1
Ln, in 16d at ( , , ), Zr in 16c at (0,0,0), O1 in 48f at (x, , ), and O2 in 8b
2 2 2 8 8
3 3 3
at ( , , ). The structure type can be considered as an ordered defect fluorite
8 8 8
structure with the trivalent rare earth Ln3+ and quadrivalent Zr4+ cations forming an
7
ordered, face-centered cubic eutectic cation array. Oxygen ions are located in of
8
the tetrahedral interstices: O1 in an off-center position within the Ln2Zr2 tetrahedral
and O2 in the Zr tetrahedral [28]. The x values of O1 can be varied from 0.3125 to
0.375. The x values 0.3125 and 0.375 correspond to the regular octahedral oxygen
environment around the Zr4+ ion and regular cubic oxygen environment around
Ln3+, respectively. Tabira et al. determined the x value of LZ using systematic row
wide-angle convergent beam electron diffraction (CBED) techniques [28]. The
results showed that the x value varied systematically with the rare earth ion radius,
the larger radius corresponding to the larger x value. The experimental result of x
value in LZ is 0.333, according to Tabira’s work [28].
The lattice parameter of a conventional cubic LZ cell can be calculated using
XRD results based on Bragg’s law [29]. Shimamura et al. reported that the lattice
parameters of Ln2Zr2O7 pyrochlores increased with the ionic radius of Ln, as shown
in Fig. 1.2 [23]. The lattice parameter of LZ is 10.8 Å in Shimamura’s experiments
and 10.802 Å in Tabira’s work [28].
As discussed from the XRD pattern in Fig. 1.1, the LZ has a cubic phase at room
temperature. As shown in the ZrO2-La2O3 phase diagram of Fig. 1.3, the LZ has no
phase transformation from room temperature to its melting point [30–32]. When the
molar ratio of ZrO2 and La2O3 reaches 2:1, which corresponds to 33.3% La2O3, only
a single LZ cubic phase is available from room temperature to its melting point.
1.4 Deposition Techniques of Lanthanum Zirconate-Based Coatings 5
Fig. 1.1 X-ray diffraction patterns of Ln2Zr2O7 [23]
1.4 Deposition Techniques of Lanthanum

Zirconate-Based Coatings
Air plasma spray (APS) is the most widely used thermal spray technique for LZ
deposition. Plasma normally consists of neutral atoms, positive ions, and free elec-
trons. Plasma is produced by transferring energy into the gas until the energy level
Fig. 1.2 Lattice parameters of Ln2Zr2O7 as a function of ionic radius of Ln. Solid and open sym-
bols stand for pyrochlore and defect fluorite structures, respectively [23]
is large enough to ionize the gas, allowing the electrons and ions to move indepen-
dently of one another. As a result, plasma is often called the fourth state of matter.
The plasma state is achieved when the current can be sustained under an electric
field and the free electron can move through the ionized gas [10]. The plasma tem-
perature in the core of the heating gas exceeds 20,000 °C, which depends on the gas
properties. During the APS process, feedstock powders are carried by some noble
gasses, such as argon and nitrogen, to the APS torch. The thermal plasma can be
generated using electric arcs. Natural air can be used as the source of the plasma gas
for the LZ spray. The essential APS parameters include current, carrier air flow rate,
primary air flow rate, spray distance, powder feed rate, substrate tangential speed,
etc. [33].
As shown in Fig. 1.4, the APS-sprayed LZ has many amorphous pores and
cracks, which is well known as the “splat” grain [33]. The thermal conductivity of
the APS deposited coating is lower than the EB-PVD deposited one, due to its
“splat” grain morphology. The porosity of the LZ coating can be easily controlled
by changing the spray parameters, which results in changing the thermal and
mechanical properties.
Another commonly used deposition technology is EB-PVD. The term PVD
denotes those vacuum deposition processes where the coating material is
Fig. 1.3 Phase diagram of ZrO2 and La2O3 in mole percentage [30–32]
evaporated by various mechanisms (resistant heating, high-energy ionized gas bom-

bardment, or electron gun) under vacuum, and the vapor phase is transported to the
substrate, forming a coating [34]. The main EB-PVD deposition parameters include
vacuum pressure, substrate distance, power supply, average substrate temperature
(1223 ± 25 K, 950 ± 25 °C), substrate rotate speed, etc. [35, 36]. As shown in
Fig. 1.5, the EB-PVD-deposited LZ coating microstructure has a fine columnar
microstructure that results in a higher strain tolerance [37]. Typically, the EB-PVD-
deposited coatings have a higher thermal conductivity than the APS-sprayed coat-
ings at the same porosity level. This is because the splat boundaries of the
APS-deposited coatings act as scattering centers perpendicular to the direction of
heat flux, which weakens the heat transfer process. However, the columnar grain
boundaries in EB-PVD-deposited coating are parallel to the direction of heat flux.
As a result, the EB-PVD-deposited coating has a good performance and consider-
ably longer operating lifetimes [12].
Fig. 1.4 Cross-sectional microstructure of APS-sprayed LZ coating [33]
Fig. 1.5 Cross-sectional microstructure of EB-PVD-deposited LZ coating [37]
However, the main disadvantages of EB-PVD technique are its low deposition
rate, high investment costs, high thermal conductivity, and vapor pressure
requirements.
In addition to the two methods mentioned above, there are other techniques to
deposit LZ coatings, such as suspension plasma spray (SPS) and spray pyrolysis
[12, 38, 39].
Wang et al. deposited an LZ coating using SPS method [38] and a suspension of
30 wt.% nano-LZ particles in (99.5%) ethanol was produced. Meanwhile, an elec-
trostatic dispersant of 1 wt.% polyethylene glycol (PEG1000) was added to the
suspension. The suspension was injected into the plasma spray jet and the LZ coat-
ing was deposited. The main deposition parameters are standoff distance of the
substrate and the concentration of the suspension feedstock. A liquid solution was
used as a feedstock material instead of powder, which provided the possibility of
tailoring the coating composition easily and facilitating the doped, multilayered,
and graded coatings [39]. As shown in Fig. 1.6a, b, many pores and cracks were
spotted in the microstructure of SPS-deposited coatings [38]. Weber et al. fabricated
the LZ coating using spray pyrolysis method [39]. Zirconyl oxynitrate hydrate
(ZrO(NO3)2·xH2O) and lanthanum nitrate hexahydrate (La(NO3)3·6H2O) were dis-
solved in deionized water and further mixed in a molar ratio of 1:1 of La to Zr. The
precursor solution was sprayed at a flow rate of 1 ml/min at 240 °C. The deposited
coatings were dried at 500–600 °C after the deposition process. As shown in
Fig. 1.6c, d, a lot of cracks were observed in the coating layer [39].
Fig. 1.6 Cross-sectional microstructure of LZ coatings: (a) SPS deposited with standoff 40 mm,
(b) SPS deposited with standoff 50 mm, and (c) surface view and (d) cross-section view of spray
pyrolysis-deposited LZ coatings [38, 39]
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Chapter 2
Properties of Lanthanum Zirconate–Based
Thermal Barrier Coatings
2.1 Physical Properties
2.1.1 Coating Density and Porosity
The theoretical density of LZ material can be calculated using the molecular weight
and the number of formula units per elementary cell [1]. Lehmann et al. calculated
the theoretical density of LZ material as 6050 kg/m3 [1].
The porous LZ coating density can be measured following the ASTM standard
B328-96, which is based on the Archimedes’ principle [2]. Freestanding samples,
which were peeled off from the substrate without the bond coat, were used in the
coating density measurements. Engine oil was used to seal the pores on the sample
surface by dipping the sample with the oil, so the volume of the sample can be mea-
sured by Archimedes’ principle. Density (D, g/cm3) of the sample can be calcu-
lated by [2]:
A
D D (2.1)
B C E w
where A is the mass of oil-free specimen in the air, B is mass of oil-impregnated
specimen, C is mass of oil-impregnated specimen and wire in water, E is the mass
of wire in water, and Dw is density of water at specific immersion temperature.
The porosity of the coating (φ) can be measured by the ratio of coating density
to the theoretical density (Dt), which can be expressed by:
D
1 100% (2.2)
Dt
© Springer Nature Switzerland AG 2021 13

X. Guo et al., Novel Lanthanum Zirconate-based Thermal Barrier Coatings for
Energy Applications, https://doi.org/10.1007/978-3-030-58695-9_2
14 2 Properties of Lanthanum Zirconate–Based Thermal Barrier Coatings
The porosity of the LZ coating varies with the deposition parameters, such as depo-
sition power, powder feed rate, and substrate standoff distance. For the APS-
deposited coating, the higher the power used in the torch, and the larger the powder
feed ratio and the shorter standoff distance used in the deposition process, the denser
the coating will be. The commercial APS-deposited coating shows a porosity of
15–25%. However, it is important to tailor the porosity of the LZ coating in a range
of 8–19% to acquire good thermal and mechanical properties [3].
2.1.2 Sintering Behavior
Sintering in the porous ceramic coating is the process by which the coating will be
densified by the reduction in surface energy associated with the excess surface area
of the pores and cracks [4]. Sintering of the porous TBCs normally occurs at ele-
vated temperature. When the sintering occurs, the densification process inevitably
increases the elastic modulus and thereby decreases the strain compliance of the
coating. Meanwhile, the thermal conductivity of the coating increases due to the
decrease of the porosity [4].
Many experimental approaches can be used to describe the sintering behavior:
(1) record the dimension change of the coating sample using a high-temperature
dilatometer, (2) detect the porosity distribution change using mercury porosimetry,
(3) measure the relative density of the coating during the sintering process, and (4)
monitor the thermal conductivity increases during a long time heating period at
various temperatures [5–7]. Vassen et al. investigated the sintering behavior of APS-
deposited LZ coating at temperatures as high as 1650 °C using the high-temperature
dilatometer and the mercury porosimetry [5, 6]. The higher porosity the coating
had, the higher sintering rate it had. The coating with high porosity level (20%)
densified strongly during the annealing process at 1250 °C [5]. Vassen et al. indi-
cated that decrease porosity might lead to a better thermomechanical behavior [6].
Zhu investigated the sintering behavior by continuously monitoring the thermal
conductivity [7]. Zhu found that the LZ coating showed significant thermal conduc-
tivity increase (from 0.55 W/m/K to 0.95 W/m/K in 20 h) at 1575 °C, suggesting the
coating was undergoing substantial sintering. Nair et al. systematically studied the
sintering of the LZ coating [8]. They found that the major mechanism of the sinter-
ing process in the temperature range of 800–1100 °C is surface diffusion. The sin-
tering above 1100 °C is mainly because of grain boundary diffusion combined with
the surface diffusion. The contribution from surface diffusion becomes negligible as
the sintering temperature increases.
In general, the sintering resistance of LZ coating is higher than that of YSZ coat-
ing, and also BaZrO3 and SiZrO3 coatings [5, 6]. The low-sintering activity of the
LZ is beneficial for TBC applications.
2.2 Mechanical Properties 15
2.1.3 Morphology of Coating Cracks and Pores
The crack and pore morphology of TBC is a crucial parameter affecting the thermal
and mechanical properties of the coatings. The cracks can be categorized as the
horizontal, vertical, and spherical forms. Zhang et al. studied the crack morphology
of the APS-deposited LZ coating using a quantitative imaging analysis method [9].
It was found that the cracks were primarily horizontal in the top and middle regions
of the cross-section area, while vertical cracks became dominant in the bottom
region. In addition, the calculated porosities showed a nonuniformity in the cross-
section area.
Weber et al. indicated that vertical crack is beneficial in TBC application due to
enhanced thermomechanical compliance [10, 11]. The LZ-based TBCs were depos-
ited using the spray pyrolysis method, and the vertical cracks were introduced by
decomposing the dried coating layer at 575 °C, as shown in Fig. 1.6d. Moreover, the
multilayer coating with vertical cracks was fabricated by the successive deposition
and decomposition of multiple thin layers. The heat conduction is slowed in this
multilayer coating due to the generated cracks, and the thermal durability can be
increased due to the increased thermomechanical compliance [11].
2.2 Mechanical Properties
2.2.1 Elastic Modulus
Elastic moduli include Young’s modulus (E), bulk modulus (K), shear modulus (G),
and Poisson’s ratio (ν). These elastic moduli can be measured by a depth-sensing
micro- and nanoindentation technique or an ultrasound pulse-echo method [6, 12].
In the micro-indentation technique, E can be obtained from the unloading slope by
adopting Sneddon’s flat-ended cylindrical punch model [6]. Shimamura et al. stud-
ied the moduli for a series of Ln2Zr2O7 material using ultrasound pulse-echo mea-
surement [12]. Shimamura found that the elastic moduli (except for Poisson’s ratio)
strongly depend on the atomic radius of rare earth elements for the lanthanide zir-
conate pyrochlore Ln2Zr2O7. The larger atomic radius corresponds to larger E, K,
and G values. La has larger atomic radius than Nd, Sm, and Gd, so LZ has larger
elastic modulus than Nd2Zr2O7, Sm2Zr2O7, and Gd2Zr2O7 [12].
Many researchers successfully measured the elastic moduli of the LZ powder
and coating, as summarized in Table 2.1. The sample used in Vassen’s work was
prepared by pressing the LZ powders at 1350~1400 °C. In this chapter, the Young’s
modulus of APS-deposited LZ coating with porosity of 7.53% were measured
(detailed discussion in Sect. 2.2.2) [13]. Xu et al. investigated the E of EB-PVD-
deposited LZ coating [14]. Shimamura et al. measured the LZ powder using the
ultrasound pulse-echo method [12]. Girolamo et al. tested the APS-deposited LZ
coating, which was exposed at 1350 °C for 50 h [15].
Table 2.1 Mechanical properties of LZ coating versus YSZ coating

Properties LZ YSZ
Young’s modulus 175 ± 11 GPa (densified powder, Vassen 210 ± 10 GPa
[6]) (densified powder, Vassen
156 ± 10 GPa (coating, Zhang [13]) [6])
153 GPa (coating, Xu [14])
280 GPa (powder, Shimamura [12])
141 GPa (porous coating, Girolamo [15])
Bulk modulus 216 GPa (Shimamura [12]) –
Shear modulus 109 GPa (Shimamura [12]) –
Poisson’s ratio 0.28 (Shimamura [12]) –
Vicker’s hardness 5.51 ± 0.25 GPa (coating, Zhang [13]) –
8.83 GPa (coating, Xu [14])
Microindentation 9.9 ± 0.4 GPa (densified powder, Vassen 13 ± 1 GPa
hardness [6]) (densified powder, Vassen
[6])
Nanoindentation 8.8 ± 2.1 GPa (coating, Zhang [13]) –
hardness
Fracture toughness 1.1 ± 0.2 MPa m1/2 (densified powder, 2.0–3.3 MPa·m1/2 (Beshish
Vassen [6]) [17])
1.84 MPa m1/2 (coating, Xu [14])
0.9 MPa m1/2 (densified powder, Jiang
[16])
The Young’s modulus of the hot-pressed LZ sample is about 15% lower than that
of the hot-pressed 8YSZ, which is 210 ± 10 GPa. The low Young’s moduli of LZ are
advantageous for reducing thermal stresses, which might compensate CTE mis-
match in coatings [6].
2.2.2 Hardness and Fracture Toughness
The hardness test can be classified into three categories according to the length scale
applied in the measurement: macroindentation hardness, microindentation hard-
ness, and nanoindentation hardness. The measured hardness results of LZ are listed
in Table 2.1. The hardness of LZ varies significantly due to the sample density
change. The hardness increases with increasing coating density.
Fracture toughness is a material property, which describes the ability of fracture
resistance to maintain cracks in the material without elongation of cracks. The defi-
nition of fracture toughness is that if a sample has a crack in loading, the stress
intensity factor increases with increasing load until the unstable crack propagation
occurs at a critical value of KI [18]. This critical value is fracture toughness (KIC).
The standard measurement method of fracture toughness is the four-point bending
test of the bulk sample. Another alternative technique is the indentation method,
which is widely used to evaluate the fracture toughness of ceramic and coating
2.2 Mechanical Properties 17
systems [19]. The fracture toughness can be estimated from the indentation test, and
the relationship between fracture toughness and hardness can be expressed by the
following equation [18]:
E P
K IC 0.16 (2.3)
H c1.5
where E is the elastic modulus, H is the hardness, P is the applied load, and c is the
sum of the crack length and one-half of the indenter imprint diagonal. The fracture
toughness of LZ powders and coatings summarized in Table 2.1.
Hot-pressed 8YSZ has higher hardness and fracture toughness than LZ (micro-
indentation hardness of densified 8YSZ is 13 ± 1, fracture toughness of densified
8YSZ is 2.0–3.3 MPa·m1/2) [6, 17]. The low fracture toughness is the major disad-
vantage of LZ, which leads to a severe limit on its application as a TBC material.
To improve the fracture toughness of LZ material, a composite or multilayer LZ
coating can be used. Jiang et al. studied the microstructure and mechanical proper-
ties of LZ/Zr0.92Y0.08O1.96 composite ceramics, which were prepared by spark plasma
sintering at 1450 °C. The results revealed that the composite ceramics had a higher
fracture toughness than single-phase LZ [16]. Jiang et al. also showed that the frac-
ture toughness of composite LZ and 4YSZ coatings increased with increasing the
content of 4YSZ. The fracture toughness reached to a value of 1.8 ± 0.1 MPa m1/2
for 50% 4YSZ plus 50% LZ composite coating, which is about two times of that of
single-phase LZ coating.
In this chapter, we compared single LZ and double-layer LZ/8YSZ coatings
[20]. The results showed that the double-layer coating composed of LZ plus porous
8YSZ substantially improved the durability in thermal cycling tests, suggesting the
bilayer design is a feasible solution to improve the fracture toughness in LZ-based
coatings.
2.2.3 Erosion Resistance
Erosion is regarded as a secondary cause of failure of TBCs by deteriorating the

coating through progressive removal of the coating material due to the mechanical
interaction between the coating surface and the impinging solid particles [21]. The
erosion tests by solid particle impingement were standardized by ASTM G76-13
[22]. Typically, the Al2O3 medium with the particle size of 50 μm is used as the
abrasive particles, and the abrasive particles are accelerated by the high-velocity
carrier gas through a particle-gas supply system. Finally, the abrasive particles are
impacted on the surface of the coating at a specific impinging angle. The average
erosion rate (mg/g or g/kg) is used to evaluate the erosion resistance performance,
which is determined by the slope of TBC mass loss (mg) versus the mass (g) of
erodent. Many variables such as velocity, working distance, impact angle, abrasive
particles properties, coating hardness, and mechanical properties of coating (H and
KIC) affect the erosion results.
Ramachandran et al. studied the erosion of APS-deposited YSZ and LZ coatings
with different coating porosity, abrasive particles’ velocity, and impact angle [23].
They found that the porosity level is the most predominant factor affecting the ero-
sion rate of the coatings. High porosity in the coating increased erosion rate. The
erosion rate increased with the increasing of the abrasive particles’ velocity.
One method of improving erosion test performance is microstructure modifica-
tion. For instance, the columnar microstructure of EB-PVD-deposited coating typi-
cally provides the improvement of erosive resistance compared to the “splat” grain
microstructure of APS-deposited coating [21]. In addition, the aging of the APS
coating decreases the erosion rate and therefore enhances the erosion performance.
However, the aging of the EB-PVD coating results in a significant increase of ero-
sion rate due to the sintering of columns [21].
2.3 Thermal Properties
2.3.1 Melting Point Temperature and Specific Heat Capacity
The high melting point is an important criterion for TBC material, which is good for
the thermal stability during the high-temperature operation environment. Thermal
analysis is the commonly used method to detect the melting point, which is per-
formed in sealed tungsten crucibles, and the sample temperature is monitored by a
spectro-pyrometer. In addition, high-temperature X-ray diffraction experiments (the
Advanced Photon Source, Argonne National Laboratory) can also be used to deter-
mine the melting temperature by monitoring the pyrochlore (111) peaks [24, 25]. As
shown in Table 2.2, the experimentally measured melting point of the LZ is about
2523–2573 K (2250–2300 °C), which is lower than that of YSZ (2953 K, 2680 °C)
[5, 6, 24]. Although the melting point of LZ is lower than that of YSZ, it is still high
sufficient for most TBC applications.
Differential scanning calorimetry (DSC) is the most widely used technique to
precisely measure the specific heat capacity (Cp). Several researchers investigated
the specific heat capacity of LZ in different conditions, as shown in Fig. 2.1 [6, 15,
26, 27]. The samples tested in Vassen ‘s work were the densified LZ powder using
hot pressing technique at the temperature around 1350~1400 °C. LZ samples in
powder form were used in Bolech and Sedmidubsky’s work. In Girolamo’s work,
the specific heat of the LZ coating with a porosity of 11% was measured. The spe-
cific heat of 8YSZ is ~ 0.55–0.65 J/g/K in the temperature range of 300–1200 °C,
which is larger than that of the LZ [28]. For the TBC materials, small Cp values are
preferred to reduce thermal diffusivity.
2.3 Thermal Properties 19
Table 2.2 Thermal properties of LZ coating versus YSZ coating

Properties LZ YSZ
Melting point 2523–2573 K (Vassen [5, 6], Hong 2953 K
[24]) (Vassen [6])
Specific heat capacity 0.48 J/g/K (@ 1200 K, Vassen [6]) 0.65 J/g/K (@ 1200 K, Khor
0.41 J/g/K (@ 400 K, Bolech [26]) [28])
0.42 J/g/K (@ 400 K, Sedmidubsky
[27])
0.44 J/g/K (@ 1200 K, Girolamo
[15])
Thermal conductivity 1.55 W/m/K (dense, @1273 K, 2.25 W/m/K (dense @1273 K,
Vassen [6]) Vassen [6])
2.15 W/m/K (dense, @ 1273 K, Zhu 0.88 W/m/K (Porous, @
[7]) 1173 K, this work, Guo [20])
0.68 W/m/K (porosity 11.54%, @ 1.38 W/m/K (porous, @
1173 K, this work, Guo [20]) 1273 K, Bobzin [29])
0.87 W/m/K (EB-PVD, @ 1273 K,
Bobzin [29])
Coefficients of 9.45 × 10−6 /K (273–1473 K, Chen 11 × 10–6 /K (dense @ 1273 K,
thermal expansion [30]) Vassen [6]
9–10 × 10–6 /K (400–1600 K, this
work, [20])
9.0–9.7 × 10–6 /K (400–1600 K,
Zhang [31])
7.6–9.1 × 10–6 /K (400–1400 K,
Lehmann [1])
Fig. 2.1 Specific heat capacity (Cp) of LZ in the temperature range from 0 to 1600 K [6, 15, 26, 27]
2.3.2 Thermal Conductivity
For TBC materials, thermal conductivity is the most important material property.
Thermal conductivity is a measurement of heat flux in a temperature gradient
according to Fourier’s law, which provides the fundamental theory for heat conduc-
tion analysis [32].
q
(2.4)
dT / dx
Later, Debye used the phonon gasses analogy to explain the heat conduction process
and derived an expression for thermal conductivity, which shows that thermal con-
ductivity is related to the phonon mean free path (Λ) [33, 34].
cv vs
(2.5)
3
where cv is the specific heat capacity (about constant volume) and vs is the speed of
sound. As a result, the thermal conductivity is related to the amount of energy that
is carried by a particle, the phonon travel speed, and the distance the phonon travels
before scattering [19]. The phonon scattering effect would decrease the thermal
conductivity, and the point defect (e.g., oxygen vacancies) would substantially
increase the phonon scattering, so the Ln2Zr2O7 pyrochlore structure and doped
pyrochlore can have a lower thermal conductivity than that of fluorite structure
materials.
The most widely used experimental method to measure thermal conductivity is
the laser-flash method, which was first proposed by Parker in 1961 [35]. Thermal
conductivity can be determined using thermal diffusivity (Dth), specific heat capac-
ity (cp), and density (ρ), which can be independently measured experimentally.
During the experiment process, the front surface of the sample is irradiated by a
high-energy laser pulse (usually duration time less than 1 ms). The temperature at
the back surface of the sample is monitored by an infrared detector [19]. The ther-
mal diffusivity (Dth) can be determined by the bottom surface temperature and time
curves using Parker’s theory [35]:
1.38 L2
Dth (2.6)
2 t0.5
where L is the sample thickness and t0.5 is the time required for the bottom surface
to reach half of the maximum temperature rise. The measurement error of the stan-
dard flash method is less than 5%. Subsequently, the thermal conductivity (κ) of the
LZ coating with given density can be determined according to the following
Eq. (2.6):
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This lute music must have been usually played in rooms of limited
size, for the delicate tone quality of the lute would scarcely render it
practical for accompaniments to dances. Hence we may conclude
that this early lute music was played for its own sake. It is the earliest
form of true chamber music and represents the beginning of
absolute instrumental music in general.
We find already in this early chamber music the elements of artistic

form. It is evident from the examination of numerous collections from
the sixteenth century that composers for the lute applied the principle
of contrast, being impelled thereto by a natural artistic sense. In
Petrucci’s lute collection (1507-08), for example, a Ricercar is
preceded by a sort of prelude-like Tartar le corde that in its rapid
passages forms an evident contrast to the even and more simple
style of the Ricercar. It is this tendency toward artistic contrast that
helped to build up the cyclical forms of the suite and of the sonata.
Lutenists, in fact, preferred to combine their favorite songs and

dances in groups of two, three, or more, which thus constituted the
earliest suites. A suite of three dances is to be found in Petrucci’s
collection. It contains a Pavane, a Saltarello, and a Piva. The
Pavane (in common time) gives the melodic material for the two
other movements (in triple time), a crude example of the use of a
leading theme in the different movements. Attaignat’s French
collection (1529) also contains a suite of three dances: Bassedance,
Recoupe, and Tordion. Some German suites consisted of a slow
movement (in triple time), and a second, more rapid, on the melody
of the first. The individual pieces sometimes had no names, but
frequently the slow movement was called Hoftanz, while the fast
movement bore the designation Hupfauff. Other combinations of
movements were Ein guter Hoftanz (in common time), Proportz
darauf (in triple time), and Pavana, or Ein kunstreicher Gassenhauer,
Ander Thyl, Proportz dritt Thyl. Toward the middle of the century,
when movements increased in number, the suites ended with a
postlude, such as a Toccata. The relation between the movements
was evident not only in the common thematic material, but also in
the use of the same key throughout. Later the dances were grouped
under their different titles—all the Pavanes and Allemandes, for
instance, being brought together. Not every kind of dance was
regarded as suitable for combination with others. Such dances as
Caluta a la Spagnola or a la Italiana, the Branle, the Morino, the
Balletti, the Polish, ‘Welsh,’ French, Swiss, Hungarian, Bavarian, and
Swabian dances are always found alone. The contrasted tempi of
the better suites lent them a certain variety and lightness.
Lute music gradually ‘went out of fashion,’ as Thomas Mace, himself
a composer for the lute, remarked, because it was ‘a very
chargeable instrument’ and ‘the hardest instrument in the world.’ In
the meantime certain composers were writing chamber music for
which no special instrument was indicated. Of this class of
instrumental compositions we may mention especially a Canzon da
sonare a 4, by Florentino Maschera from his Libro primo de canzoni
da sonare a 4 (1593). It is called La Capriola and is written for basso,
tenore, alto, e canto. Maschera’s canzonas are among the earliest
printed specimens of independent instrumental compositions. Their
phrase structure is very irregular. One canzona, for instance, has an
introduction of twenty-one measures, followed by a longer piece of
six periods of 22, 21, 18, 19, and 23 measures. On the whole,
Maschera’s instrumental compositions are vocal in character and
polyphonic in style. Almost the same may be said of the Canzoni and
Sacræ Symphoniæ of Giov. Gabrieli (1597), although his Sonata con
tre violini and canzoni a 6 (two violins, cornetto, tenore, trombone
and bass) (1615) show an advance in instrumental writing. In
Gabrieli’s Sonata piano e forte, we meet for the first time the term
‘Sonata.’ This composition is scored for a double choir of
instruments, the first consisting of a cornet and three trombones, and
the second of a violin and three trombones. These two choirs are
employed antiphonally. Gabrieli usually preferred to score his
sonatas and canzonas for eight instruments in two choirs, but not
infrequently he wrote from four to twenty-two parts in one or three
choirs.
In comparing Gabrieli with Maschera we get the impression that

while Maschera’s canzonas are song-like, Gabrieli’s polyphonic style
represents rudimentary symphonic music.
A link in the evolution of chamber music form is to be found in the

Fantasie overo Canzoni alla Francese per suonare nell’organo ed
altri stromenti musicali a 4, by Adriano Banchieri (1603). In some of
these pieces the first part corresponds with the third, the second part
appearing as a kind of middle movement, an arrangement that
shows the elements of the three-part form of the modern sonata.
We have seen that chamber music included dances (single and in

suites) and compositions of free invention. The names of the former
class of pieces clearly expressed and described the character of the
music. The terms applied to compositions of free invention, however,
were not strictly defined, and compositions with scarcely any
difference between them were variously entitled Sonata, Fantasia,
Simphonia and Canzona. To illustrate the uncertain terminology of
the time we may quote the following from Prætorius’ Syntagma
Musicum (1618): ‘In my personal opinion there is still some
difference between Sonatas and Canzonas. Namely, Sonatas
contain serious, solemn and pompous music, in the manner of
Motettes; while the Canzonas briskly, quickly, and merrily pass
away.’ Sometimes, however, the term ‘Sonata’ conveyed the idea of
music that was played at banquets and for dancing.
Currently with the rise of music of free invention, dances and suites
were further cultivated, as we see from the large number of such
compositions extant. The dances of Melchior Franck (1603) were
sometimes of polyphonic phraseology, sometimes of lively flowing
melodies, with irregular structure, and we find a Galliarde by Johann
Ghro (1604) consisting of periods of 13—11—11 measures. Similar
pieces by Brade (1607), Thomas Simpson (1617), Erasmus Widman
(1618), and others, showed more or less skill in handling their
musical materials. Besides single dances, we find also several
interesting and valuable collections of suites. I. H. Schein’s
Banchetto musicale, 1617, a series of twenty suites, contains very
characteristic examples of the suite in five movements. We may
quote here the beginnings of the five movements of his tenth suite:
Similar to Schein’s suites in the character of their variations are
those by Paul Bäuerl, edited six years earlier. Variations in suites
were so popular that in a work by Andreas Hammerschmidt (1639)
the author gave instructions for playing ‘Gaillarde on the 1, 2, 7,
Pavane.’ Change in the order and in the number of the single
movements is to be found in the suites of Johann Neubauer (1649).
They contain only four movements, Pavane, Gaillarde, Balletto, and
Courante. The Balletto stands for the Allemanda and Tripla, having
two parts, the first in common, the second in triple, time.
The four movement form of suite was adopted by Froberger (1649),

and by K. Briegel (1652). After the middle of the century composers
began to include in their suites movements that were not dances,
such as Canzonas, Symphonias, Sonatas, Sonatinas or Præludia.
The earliest examples of those are by I. R. Ahle (1650), Martin
Rubert, Joh. Jak. Löwe (1658), Diedrich Becker (Musikalische
Frühlingsfrüchte, 1668), Joh. Rosenmüller (Sonata da camera,
1667), Joh. Petzolds (Leipzigische Abendmusik, 1669), Esajas
Reusser (Suites for two violins with continuo, containing the following
movements: Allemande, Courante, Sarabande or Gavotte, Gigue,
with an Adagio—called Sonata—as introduction, 1670). Thus
through the mixture of ‘suites’ with ‘sonatas’ the way was prepared
for the classical chamber-sonata.
II
It must not be forgotten that an important part of early chamber
music consisted of various compositions in the form of vocal pieces
—madrigals, canons, rounds, and catches. As far as we know the
earliest printed collection of such music extant is a volume entitled
Pammelia (o) Musicks Misscellane (1609). The mixed variety of
these ‘pleasant and delightful Roundelays’ shows skillful
counterpoint and good harmony. The names of the composers are
not mentioned in the book, but since the style of the compositions
suggests great antiquity, this collection may represent the oldest
printed vocal chamber music. With the striking progress of
instrumental music, purely vocal compositions were less and less
used as chamber music, since instruments were being used to play
in unison with the voices. Such performances were called concertati.
Significant vocal compositions with instrumental accompaniments
were produced by Peri (1561-1633) and Caccini (d. 1618), whose
Cantate da camera or Madrigali da camera were mostly pieces for a
single voice accompanied by a single instrument. On the whole,
however, it is not necessary to emphasize the vocal music here,
since chamber music as we know it today represents a purely
instrumental development.
We have already referred to Gabrieli’s use of the term sonata and to

the first specimens of canzonas. Besides these we may mention a
Canzon francese a risposta by Viadana (1602) for ‘violino, cornetto,
two tromboni, and basso continuo.’ The parts of the instruments that
lead the melodies are handled here as in a dialogue. The treatment
of the melody is monodic rather than contrapuntal.
Of much more interest and value are a Sonata in dialogo for violin,
with basso continuo, and a Sonata detto la moderna, from the Varie
Sonate (1613) of Salomone Rossi. Rossi’s sonatas contain good
examples of variations on a basso ostinato (Sopra l’Aria della
Romanesca and Sopra l’Aria di Ruggiero). The basses, however, are
not always strictly carried out. Rossi also cultivated variations on
melodies not in the bass. He is noted for his first attempts in the form
of the trio sonata (two violins with basso continuo), where, as in his
simpler and shorter ‘Sinfonias,’ the homophonic style is predominant.
His compositions have thematic unity, and he sometimes demands
the changing of his tempi (Si replica l’ultima parte ma piu presto).
Similar to Rossi’s trio sonatas are those by Buonamente (1626), who

is likewise fond of variations and of writing in dialogues for two
violins. In his Sonate a 3 (for two violins and string-bass) the bass
has a more important rôle than a mere accompaniment; it also helps
to carry the themes, showing a tendency toward independent
movement. A sonata (113 measures long) arouses our interest by
the development of the first three notes of its theme that
reappears in the following manner reminding us of the C
minor symphony of Beethoven. Some of Buonamente’s sonatas end
with the complete form of the original themes as if to unify the whole
composition—a characteristic we again find in Beethoven (i.e., at the
end of the first movement of the eighth symphony). The single
themes and the lack of variety in tempi lend a certain monotony to
Buonamente’s compositions, though otherwise they are very
interesting.
Another writer of sonatas in Rossi’s manner is Francesco Turini

(Tanto tempo hormai, 1624). His compositions, too, are in the form of
variation suites, where the same bass, with slight changes in rhythm
and character, is used in all movements. For the sake of
completeness we may also mention G. Allegri’s sonatas for four
string instruments, which may be considered crude early specimens
of the string quartet.
An important advance in chamber music compositions is marked by

B. Marini, who introduced into the trio sonata a second theme,
contrasting strongly in rhythm with the first. This new second theme
is announced simultaneously with the first when the latter appears
for the second time thus:
Marini is also notable for the use of chromatics in his later works
(1651) and his effective instrumental writing. He did not, however, lay
special stress upon developing the idea of the new theme nor upon
giving more independence to the two leading instruments.
Frescobaldi also failed to recognize the possibilities of the second
motive in his trio sonatas (1628). The idea, however, was well
developed by Tarquinio Merula (especially in a sonata called La
Pedrina, 1637), whose works (Canzoni da sonar, 1615, Canzoni
overo Sonate concertate da chiesa e camera a 2 e 3, 1637, etc.)
show not only more proficiency in instrumental writing, but also
greater independence in the single parts and more individuality in the
bass parts. Merula’s compositions have a sort of jovial humor, and
on the whole they produce a more satisfactory general effect than
those of his predecessors.
Of minor importance are the Sinfonie ad uno e duoi violini, a duoi

trombone, con il partimento per l’organo con alcune quattro viole,
1629, by Mont’Albano, and the few chamber music compositions
(besides solo sonatas) by Fontana (1630, 1641), whose graceful
melodies are suggestive of the coming era. In further developing the
forms of chamber music (mostly in trio sonatas) an important place
belongs to Maurizio Cazzati (d. 1677), who is distinguished
especially for his clear-cut melodies. The following from his sonata,
La Lucilla (1648), is a good example:
Here the contrasting second theme is brought in before the

exposition of the first is completed. La Lucilla has repose and
thoughtfulness instead of the restlessness usual in similar
compositions. It is in four parts and ends with the first theme without
the contrasting second motive.
"The concert"; painting by Terborch.
Among other chamber music composers of the middle of the
seventeenth century, we may point out Massimiliano Neri, who first
used the terms sonata and canzona without any distinction. After his
time the term canzona was less and less used and the name sonata
finally became general for all instrumental chamber music
compositions. Neri’s works are characteristic products of the century.
His scoring for three to twelve instruments, his restless changing of
rhythm and tempo, his lack of unity and ‘development,’ are the ever-
present signs of the age in which he wrote. Still, his construction of
phrase, his modulations, his more graceful figures show an
improvement upon the writing of his predecessors. The following
analysis of his Sonata in nine movements (1651) for two violins, viola
and bass—another ancestor of the modern string quartet—shows
the looseness of form which was characteristic of all contemporary
instrumental music:
Movement I: in 4/4—46 measures

Movement II: Adagio in 3/2—20 measures
Movement III: Allegro in 4/4—26 measures
Movement IV: Adagio in 4/4—8 measures
Movement V: Allegro in 6/4—22 measures
Movement VI: Adagio in 4/4—6 measures
Movement VII: Allegro in 3/4—24
56 measures
Adagio in 3/4—32
Movement VIII: Allegro in 4/4—5 measures
Movement IX: Presto in 4/4—9 measures
Among writers of sonatas who varied less the number of movements

we may notice Nicolaus Kempi (Sonatas and ‘Symphonies’ for 1-3
violins, 1-5 instruments, 1644, 1647, 1669), who employed the four
movements of the modern cyclical sonata form, thus:
I. A pathetic movement (in the style of the Pavane).

II. An Allegro movement (imitative).
III. Gaillarde or Courante.
IV. Similar to the first movement (with figurative elements).
Although Kempi’s compositions show some improvement in fluency,

they are otherwise of little interest.
Of far more eminence is Giovanni Legrenzi, the first composer of

chamber music who abandoned entirely the term canzone. He is
rightly called a ‘master of first rank,’ and his harmonies, chromatics
(in the Sonata La Cornava, 1655), and modulations are noteworthy.
In his trio sonatas (La Rosetta, 1671) and in his Sonata a 5: La
Fugazza, he demonstrated that a few instruments could be made to
express musical ideas of genuine value.
Among the minor sonata writers of this period we may mention

Mazzolini (Sonate per camera a 3, containing preludes and dances),
Mazzaferrata (Sonate a due violini: con un basetto viola, 1674, all in
four movements), Bononcini (Sonate da chiesa and ‘Symphonie’ for
two to eight instruments 1666, 1678), Tonini, C. A. Marini, Grossi,
Taglietti, Rugieri, Vinacesi, Zanata, Charelli, and Gighi.
Practically all the compositions we have noticed possess for us little

interest apart from their significance in the evolution of chamber
music. To a modern ear their appeal is very slight. Historically,
however, they are of importance, constituting as it were the
substructure upon which the edifice of chamber music has been
reared. Between them and the music which has a genuine artistic
appeal and an emotional content lies a sort of transition stage in
which the most notable names are Giovanni Battista Vitali, Antonio
Veracini, and Giovanni Bassani.
III
Vitali is the dance composer par excellence of the seventeenth
century. His Correnti e balletti da camera a 2 violini col suo basso
continuo (1666) have melodic value and clarity of structure and form.
In his Balletti correnti, e capricci per camera for two violins and bass
(1683), in his Sonate da camera for two violins and bass (1667), and
in sonatas for two to five instruments (1669) we find inspiration,
expression, and a dignified style. Vitali’s sonatas consist of three
movements. The first and the last are in fast 4/4 time, and in fugal
style; the middle, in 3/4 or 3/2 time, is more tranquil in character.
Sometimes a short largo precedes the first movement, sometimes a
largo is inserted before or after the middle movement. The two
allegros are thematically connected. In one sonata Vitali uses the
same theme through all three movements with a dexterity that
suggests the influence of his teacher, Cazzati.
Antonio Veracini (1690) was not a fertile composer, and he is

important rather for his personal influence than for the volume of his
work. His Sonate a 3, Sonate da chiesa a violino e violoncello and
Sonate da camera a 2, possess nobility and individuality of style,
with a certain melodic originality. His forms are clear, his
contrapuntal combinations not unattractive, and all his details with a
few exceptions show careful workmanship. His adagios are
especially fine.[60]
Giovanni Battista Bassani, too, derives his importance largely from

his personal influence, especially as the teacher of Arcangelo Corelli.
Bassani’s chamber music compositions include Balletti, Correnti,
Gighue e Sarabande a violino e violono overo spinetta, con il
secondo violino (1673); twelve sonate da camera (each containing
four dances in the following order: 1—Balletto, 2—Corrento, 3—
Gigha, and 4—Sarabanda); Sinfonie a due o tre instrumenti con il
basso continuo per l’organo (1638), in which each single piece bears
the title of ‘sonata.’ All these compositions are interesting rather than
attractive; though while emphasizing and broadening the technique
and form of his predecessors, Bassani improved upon their harmony
and exhibited more fluency and smoothness through better
modulations and transitional passages. We may note especially his
independent part-writing, his rythmic steadiness, and his ingenious
working-out of motives taken from the main theme. The device of
developing themes in contrapuntal works had been variously used
since Gabrieli, but the credit for first resolving a theme into its
motives and working with them skillfully belongs to Bassani. The
following examples will clearly show Bassani’s skill in thematic
development.
The theme of a Sonata (for two violins, violoncello ad libitum and

organ, 1683):
The motives:
and
Here again we are reminded of Beethoven’s Fifth Symphony.
The large amount of chamber music composed toward the end of

the seventeenth century is eloquent of the popularity of this class of
composition. In fact chamber music was so much favored that a
certain Thomas Britton (in London) formed a chamber music club
(1678) and gave weekly concerts for thirty-six years, at first free of
charge but afterwards at a subscription fee of ten shillings. Later,
similar and stronger organizations came to play an important part in
the development of music.
IV
We now arrive at an epoch in chamber music where for the first time
we meet with works that are today deemed worthy of performance
for their purely musical value. The beginning of this era is marked by
the name of Arcangelo Corelli (1653-1713). Corelli’s music is simple
and expressive in style and is distinguished by a peculiarly ascetic
and spiritual quality suggestive of the church. It is plastic and concise
in thought and dignified and noble in utterance. Corelli was not a
pioneer. It was his mission to synthesize into a more logical and
graceful whole the musical effects discovered by his many
predecessors, and his highly individual genius enabled him to do this
with a distinction which makes his name a landmark in the progress
of the art of music. In analyzing Corelli’s compositions we find
graceful harmonies, fluent modulations and pleasingly regular, well-
balanced phrase structures. His musical ideas, especially in the
adagio movements, have dignity, grace and lucidity. His allegros,
although not lacking in dignity, do not stand on the high artistic level
of his slow movements.
Corelli’s earliest chamber works are included in a collection of XII

Sonate a tre, due violini e violone col Basso per l’organo, op. 1
(1683). In these church-sonatas his strong individuality is already
apparent, although Bassani’s influence is clearly recognizable. Some
passages lack beauty and are not very pleasing to the ear. The
sonatas consist of four movements, as follows: adagio, allegro,
adagio, allegro. Sometimes the first slow movement is replaced by
an allegro, and the second movement is in a related key. The
seventh sonata has only three movements: allegro, adagio and
allegro.
The next series, XII Sonate a camera a tre, due violini e violone e
cembalo, op. 2 (1685), consists of idealized dances with a prelude
(largo or adagio). The third sonata of this collection has the following
movements: Prelude (largo), Allemande (allegro), adagio (of free
invention), and Allemande. The twelfth sonata has a Ciaccona and a
longer allegro movement. Corelli’s talent appears to better
advantage in his Sonate da chiesa a 3 (1689) and in Sonate da
camera a 3 (1694) which in form are similar to his previous sonatas.
Most of them are in the suite form; some consist of movements of
abstract nature, some show a combination of different forms.
The period of chamber music composition inaugurated by Corelli

lasted until about the middle of the eighteenth century. It is
characterized by a mixture of contemporary and older monodic and
polyphonic styles, with a strong tendency toward independent,
individual part writing. In this period Corelli’s pupils and imitators
produced valuable works, though they could not surpass their
master. Among his more prominent pupils may be mentioned F.
Geminiani (1680-1782) and P. A. Locatelli (1690-1764). Geminiani’s
works (sonatas for two violins and 'cello, and sonatas for two violins
and bass) possess neither individuality nor enduring merit, but they
claim attention for the careful marking of dynamic nuances. In
Locatelli’s sonatas for two violins and cembalo, the virtuoso element
is too strong to make them good examples of pure ensemble writing.
The same may be said of Torelli’s (d. 1708) Concerti da camera for
two violins and bass, Sinfonie for two, three and four instruments,
Balletti da camera for three violins and bass, Sinfonie a 3, Conzerti a
4, Conzerti musicali a 4, and Caprici musicali per camera, for violin,
viola and archlute. Torelli helped to fuse the Sonata da camera with
the Sonata da chiesa and is notable as the first to use the term
concerto. In general the violinist-composers of the period preferred
to cultivate solo sonatas and concertos which would demonstrate the
virtuosity of the performers. The elevation of chamber music through
serious and pure ensemble writing was not at all their aim. This was
notably the case with F. M. Veracini (1685-1750), a pupil and cousin
of Antonio Veracini, and with T. Antonio Vitali—Sonate da chiesa for
violin and 'cello (1693), Sonate for two violins and bass, Conzerto di
Sonate a violino e violoncello e cembalo (1701).
The most prominent and gifted of Corelli’s immediate successors
was Antonio Vivaldi (died 1743). His early compositions were ‘wild
and irregular,’ but later, under the influence of Corelli’s pure style, he
acquired an ‘elegant manner of writing’ that was often entirely free
from contrapuntal phraseology. His works (Sinfonie, Sonate, etc.)
became the models of his time and exercised a strong influence
even upon Bach. On the whole, however, he pandered chiefly to the
prevailing passion for virtuosity. His sonatas are written in three
movements. The opening movement still lacks the ‘song-like’ second
theme of the modern sonata-movement, and its first theme is long,
consisting of several brief, slightly-developed motives. His second
movements closely resemble the preludes of his fellow-composers.
Up to the time of Haydn and Boccherini we find very few important

works in ensemble chamber music. The solo sonata was chiefly
cultivated and from it the sonata form really was developed. So we
find that the instrumental compositions of Alessandro Scarlatti (1659-
1725) are not of much value (sonata for two flutes, two violins and
continuo, sonatas for flute, sonatas for three flutes and continuo). His
Sonate a quattro (string-quartets of archaic style) in which tediously
developed figures are the principal movements and only the little
‘brisk minuettos’ have a certain modernity, are below the artistic
standard established by Corelli. Much the same may be said of
François Couperin’s (1668-1733) trio sonatas entitled La Parnasse
ou l’apothéose de Corelli, and other trios for two violins and bass,
and Pièces de viole, published in 1724-26.
The two great composers, John Sebastian Bach and George

Frederick Handel, also produced more valuable works in the form of
solo sonatas, suites, and concertos than in ensembles. Bach’s
concertos are often classified as chamber music and indeed the
grouping of the solo instruments of his Brandenburg concertos
resembles chamber music combinations. In his trio sonatas for two
violins and thorough-bass, or for flute, violin and thorough-bass,
Bach employed the three movement form of Vivaldi. Handel[61]
cultivated the four and five movement form of Corelli.

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Novel Lanthanum Zirconate-based

Thermal Barrier Coatings for Energy

Thermal Energy : Sources, Recovery, and Applications

Thermal sprayed coatings and their tribological

Energy-Based Control of Electromechanical Systems: A

Research on Chemical Mechanical Polishing Mechanism of

Polymers Coatings: Technology and Applications 1st

Thin Film Coatings for Biomaterials and Biomedical

Thermal Energy Systems: Design and Analysis Steven G

Thermal Energy Systems: Design and Analysis Second

ISBN 978-3-030-58694-2 ISBN 978-3-030-58695-9 (eBook)

© Springer Nature Switzerland AG 2021

Beijing, China Xingye Guo

1 Overview of Lanthanum Zirconate-Based Thermal Barrier

3.2.2 MD Model������������������������������������������������������������������������������ 33

Xingye Guo is an assistant professor in the Faculty of

Jing Zhang is an associate professor of mechanical

1.1 Thermal Barrier Coatings

The development of gas turbine engines relates to a great variety of engineering

© Springer Nature Switzerland AG 2021 1

1.2 Synthesis of Lanthanum Zirconate Powder

1.3 Crystal Structure of Lanthanum Zirconate

LZ is a typical ZrO2-Ln2O3 system (Ln is lanthanide elements, Ln = La → Gd),

Fig. 1.1 X-ray diffraction patterns of Ln2Zr2O7 [23]

1.4 Deposition Techniques of Lanthanum

evaporated by various mechanisms (resistant heating, high-energy ionized gas bom-

Fig. 1.4 Cross-sectional microstructure of APS-sprayed LZ coating [33]

Fig. 1.5 Cross-sectional microstructure of EB-PVD-deposited LZ coating [37]

2.1 Physical Properties

2.1.1 Coating Density and Porosity

© Springer Nature Switzerland AG 2021 13

2.1.2 Sintering Behavior

2.1.3 Morphology of Coating Cracks and Pores

2.2 Mechanical Properties

2.2.1 Elastic Modulus

Table 2.1 Mechanical properties of LZ coating versus YSZ coating

2.2.2 Hardness and Fracture Toughness

2.2.3 Erosion Resistance

Erosion is regarded as a secondary cause of failure of TBCs by deteriorating the

2.3 Thermal Properties

2.3.1 Melting Point Temperature and Specific Heat Capacity

Table 2.2 Thermal properties of LZ coating versus YSZ coating

2.3.2 Thermal Conductivity

We find already in this early chamber music the elements of artistic

Lutenists, in fact, preferred to combine their favorite songs and

In comparing Gabrieli with Maschera we get the impression that

A link in the evolution of chamber music form is to be found in the

We have seen that chamber music included dances (single and in

The four movement form of suite was adopted by Froberger (1649),

We have already referred to Gabrieli’s use of the term sonata and to

Similar to Rossi’s trio sonatas are those by Buonamente (1626), who

Another writer of sonatas in Rossi’s manner is Francesco Turini

An important advance in chamber music compositions is marked by

Of minor importance are the Sinfonie ad uno e duoi violini, a duoi

Here the contrasting second theme is brought in before the

Movement I: in 4/4—46 measures

Among writers of sonatas who varied less the number of movements

I. A pathetic movement (in the style of the Pavane).

Although Kempi’s compositions show some improvement in fluency,

Of far more eminence is Giovanni Legrenzi, the first composer of

Among the minor sonata writers of this period we may mention

Practically all the compositions we have noticed possess for us little

Antonio Veracini (1690) was not a fertile composer, and he is

Beijing, China Xingye Guo

1 Overview of Lanthanum Zirconate-Based Thermal Barrier

3.2.2 MD Model�� 33

1.1 Thermal Barrier Coatings

1.2 Synthesis of Lanthanum Zirconate Powder

1.3 Crystal Structure of Lanthanum Zirconate

1.4 Deposition Techniques of Lanthanum

2.1 Physical Properties

2.1.1 Coating Density and Porosity

2.1.2 Sintering Behavior

2.1.3 Morphology of Coating Cracks and Pores

2.2 Mechanical Properties

2.2.1 Elastic Modulus

2.2.2 Hardness and Fracture Toughness

2.2.3 Erosion Resistance

2.3 Thermal Properties

2.3.1 Melting Point Temperature and Specific Heat Capacity

2.3.2 Thermal Conductivity