Materials Science for Energy Technologies 2 (2019) 96–103

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Materials Science for Energy Technologies

CHINESE ROOTS
GLOBAL IMPACT
journal homepage: www.keaipublishing.com/en/journals/materials-science-for-energy-technologies

Flexible ceramic film capacitors for high-temperature power

electronics q
Beihai Ma a,⇑, Tae H. Lee a, Stephen E. Dorris a, Rachel E. Koritala b, Uthamalingam Balachandran a
a
Applied Materials Division, Argonne National Laboratory, Argonne, IL 60439, United States
b
Nanoscience and Technology Division, Argonne National Laboratory, Argonne, IL 60439, United States

a r t i c l e i n f o a b s t r a c t

Article history: Flexible ceramic film capacitors with high dielectric constant and high breakdown strength hold special
Received 24 September 2018 promise for applications in power electronics. We deposited lanthanum-doped lead zirconate titanate
Revised 21 November 2018 (PLZT) films on aluminum-metallized polyimide films at room temperature by an aerosol deposition
Accepted 22 November 2018
(AD) process and examined the electrical and dielectric properties of the PLZT films over a wide temper-
Available online 28 November 2018
ature range between
55 and 175 °C. The PLZT film capacitors fabricated by high deposition rate AD pro-
cess not only satisfy X8R temperature rating but also exhibit superior volumetric and gravimetric specific
Keywords:
capacitance. At room temperature, we measured a dielectric constant of 85, dielectric loss of 0.012,
Ceramic coating
Aerosol deposition
energy density of 13.2 J/cm3 with an applied voltage of 1000 V. A mean dielectric breakdown field
Film capacitor strength (EB) of 1.25 MV/cm was determined by Weibull analysis for the 8-lm-thick PLZT film capac-
Energy conversion itors fabricated on flexible aluminum-metallized polyimide substrates. These results revealed that the
Power electronics PLZT-based ceramic film capacitors meet the requirements for advanced high-temperature power invert-
ers. Our results demonstrated that AD process offers the greatest potential for producing low-cost, robust,
compact and light-weight ceramic film capacitors with enhanced reliability for power inverters of elec-
trical drive vehicles and various power electronic devices that are critical for high-efficiency energy con-
version and renewable energy systems.
Ó 2018 The Authors. Production and hosting by Elsevier B.V. on behalf of KeAi Communications Co., Ltd.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-
nd/4.0/).

1. Introduction Therefore, a dedicated secondary cooling system is often required

Rapid advancement in power electronics for the control and
power conversion (AC to DC and vice versa) requires passive com-
ponents that are capable of handling high power density with low
self-energy-consumption, compact size, light weight, improved
switching speed, enhanced reliability, low cost, and increased
operating efficiency. These requirements are especially important
for distributed energy systems and on-board automotive applica-
tions. Capacitors are vital components of power electronic systems,
such as power inverters for electrical drive vehicles (EDV), and con-
verters for distributed energy storage systems [1,2]. DC bus capac-
itors that are currently in use in the inverter systems are made of
polypropylene (PP) films coated with metal films for electrodes.
The so called metallized polymer film capacitors lack the ability
to handle high ripple current at temperatures above 100 °C.
q
This work was supported by the U.S. Department of Energy, Vehicle Technolo-
gies Program, under Contract No. DE-AC02-06CH11357.
⇑ Corresponding author.
E-mail address: bma@anl.gov (B. Ma).
to provide further cooling capability to the power electronics in
EDVs. Having the secondary cooling system adds weight, increases
operational load, and reduces operation efficiency. In addition, the
polymer films in these capacitors exhibit low dielectric constant of
2–3. Therefore, it requires large volume of material to produce a
functional capacitor with the required capacitance. Ceramic ferro-
electric materials, such as barium titanate and lead zirconate tita-
nate, exhibit high dielectric constant and they can be operated at
elevated temperatures [3–5]. Recent development in multilayer
ceramic capacitor (MLCC) technology has attracted significant
research interest in developing high temperature ceramic capaci-
tors. Although relatively high capacitance density has been
achieved, the low field strength of surface mounted MLCCs pre-
vented their widespread application for the next generation power
electronic devices [4–6].
New technology development has been focused on making
capacitors that are not only suitable for higher temperatures but
also capable of high electric field operation for various of functions
in pulse power and power electronics applications, such as pulse
discharge, coupling/decoupling, filtering, DC blocking, power

https://doi.org/10.1016/j.mset.2018.11.005
2589-2991/Ó 2018 The Authors. Production and hosting by Elsevier B.V. on behalf of KeAi Communications Co., Ltd.
This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
 B. Ma et al. / Materials Science for Energy Technologies 2 (2019) 96–103
conditioning, snubbing, electromagnetic interference suppression,
and commutation in power electronics. Specific requirements need
to be satisfied according to their intended applications. For exam-
ple, snubber capacitors are used for minimizing power dissipation
in silicon and silicon carbide-based switching devices and for
power smoothing in switch-mode power supplies. This type of
capacitors typically possess relatively small capacitance (10 nF to
1 lF), operate at high frequency (10 kHz–1 MHz), and are placed
close to the switches that they protect. The snubber capacitor
experiences full voltage transients, from 0 V to the bus voltage
(700 V). Therefore, dielectric materials with low hysteresis losses
are desirable for this type of capacitors. Snubber capacitors are
designed for low self-inductance and high ripple current handling.
On the other hand, DC bus capacitors act as an energy source to
stabilize the DC bus voltage in power electronic circuits such as
DC/AC inverters of hybrid electric systems. DC bus capacitors pos-
sess large capacitance (2 mF) and operate under a stable DC bias
with a superimposed AC transient voltage. Bus capacitors are gen-
erally the largest capacitors in the power electronic circuit, and
high-energy density is very important. Filter capacitors are used
to remove the spurious signals from the fundamental output fre-
quency and are placed at the inverter output. Dielectrics for filter
capacitors must also be linear with low hysteresis loss. The energy
storage capacity of a capacitor is proportional to the applied elec-
tric field and the resulting dielectric polarization [7,8]. In general,
for power electronic applications, capacitors are required to have
adequate capacitance, high breakdown voltage, low dielectric
losses, low leakage current density, and minimal thermal runaway.
The ceramic film capacitors that we developed exhibit high dielec-
tric constant, low dielectric losses, high breakdown field strength,
and thus high energy density capacity. They can operate at high
temperatures with high voltage loads and still exhibit low equiva-
lent series resistance (ESR). These properties allow them to be
operated under high ripple currents and at elevated temperatures.
Ceramic capacitors hold great promise for high temperature appli-
cations that require swift delivery of large amounts of electric
energy, such as for use in DC/AC inverters of hybrid electric sys-
tems that require to have not only high energy density but also
high-power density and high-temperature operation [9,10].
Driven by the increasing demand for passive power electronics
with improved performance, high reliability, and reduced size and
weight, much attention has been paid to the so-called ‘‘film-on-
foil” technology, with which ceramic films on metal foils are
embedded into a printed circuit board. Our research [11–14] has
shown that lead lanthanum zirconate titanate (PLZT) films depos-
ited on base metal foils possess excellent dielectric properties that
are promising for high power applications. The stacked and
embedded capacitors approaches significantly reduce component
footprint, improve device performance, provide greater design
flexibility, and offer an economic advantage for commercialization.
Use of film-on-foil technology can lead to high degree of packaging
volumetric efficiency with less weight. For power electronics appli-
cations, capacitors with high capacitance are required to work
under high voltage (several hundred volts) conditions. This
requirement imposes additional challenges to the fabrication of
thicker (>5 mm) film-on-foil capacitors. Due to the well-known crit-
ical thickness effect, the per-layer thickness that can be achieved
by a chemical solution deposition (CSD) process is generally lim-
ited to 0.2 mm per coating. And it requires high temperature
pyrolysis (450 °C) and crystallization (650 °C). These required
processing conditions make the CSD method unattractive to indus-
try production when thicker films are needed to meet the opera-
tion voltage requirement [15]. Therefore, a processing
methodology capable of high rate deposition of ceramic PLZT films
with good dielectric properties is highly desirable. This technology
will fulfill the needs for massive production of high quality ceramic
97
film capacitors to meet the market needs for electric drive vehicles
and other renewable energy devices.
Fabrications of lead zirconate titanate (PZT) and barium titanate
(BT) related thick films by aerosol deposition (AD) process were
reported by several research groups in recent years [16–19]. Akedo
et al. reported PZT and PLZT films of greater than 10 lm in thick-
nesses that were deposited on Si substrates using AD process with
a deposition rate up to 25 lm/min. Good ferroelectric properties
were measured on these samples after annealing at 800 °C in air
for 4 hrs [16]. Wang et al. reported AD processing of 30 lm thick
PZT films on Si substrates for microelectronic applications. These
films also require post deposition annealing at temperatures above
400 °C to exhibit good piezoelectric properties [17]. Han et al.
reported deposition of PZT-PVDF composite films up to 130 lm
thick by AD process on Si substrates. To achieve desirable ferro-
electric and piezoelectric properties, all the PZT films prepared
by AD need 700 °C annealing in air [18]. Kawakami et al. reported
deposition of BaTiO3 (BT) thick films on ceramics and stainless
steel substrates by AD process [19]. These BT films produced by
AD process once again require heat treatment at high temperatures
(above 800 °C) to exhibit good piezoelectric properties. None of
these publications had reported dielectric breakdown strength of
the ceramic thick films deposited by AD process.
With this paper, we report our recent development of a high
deposition rate and high throughput AD process that can produce
thick PLZT films with desirable good dielectric properties. The AD
process we developed at Argonne can produce high-quality cera-
mic film capacitors at room temperature without the need for high
temperature heat treatments. This makes the process amenable for
depositing PLZT films on various types of substrates including
polymer films, ultra-thin glass, and thin metal foils. With this
paper, for the first time, we report systematic characterizations
of thick PLZT films deposited on flexible metallized polymer sub-
strates by AD process. Physical properties discussed including high
electric field tenability, leakage current density, temperature
dependent ferroelectric properties, and dielectric breakdown
strength, and temperature dependent stability. Our results demon-
strated that the technology development of combining film-on-foil
approach with high deposition rate AD process enables a cost-
effective and high throughput method for the industrial production
of ceramic film capacitors to meet the needs in power electronics
such as inverters for EDVs. Our work has shown the feasibility of
making flexible ceramic film capacitors on flexible metallized poly-
mer films which are readily adaptable for applications in stretch-
able devices and wearable electronics [20].
2. Experiment
We deposited dense PLZT films with thickness up to 30 lm on
various substrates by AD process. A PLZT film of 8-lm-thick
could be prepared in minutes by the room temperature AD process.
Fig. 1 shows a schematic illustration of the experimental setup of
the AD system used for this study. Submicron PLZT powder was
baked at 600 °C for 2 hrs in air prior to loading into the aerosol
generation chamber which was maintained at an operation pres-
sure of 100–300 torr. A mass flow controller controlled the flow
of carrier gas (N2, Ar, He, air) into the aerosol generation chamber
at a rate of 5–7 standard liters per minute (lpm). Fluidized submi-
cron PLZT particles were accelerated to velocities in the range of
200–500 m/s by flowing the aerosol into the deposition chamber
through a nozzle with slit opening of 7 mm  0.4 mm. The depo-
sition chamber pressure was maintained at <5 torr by high capac-
ity rotary pumps. The distance between the nozzle and substrate
was fixed at 3 mm. The sample stage was controlled by a com-
puter for XY motion to accomplish the desired deposition pattern.
98 B. Ma et al. / Materials Science for Energy Technologies 2 (2019) 96–103

Fluka silicone oil (Sigma-Aldrich) during measurements of high-

XYZ field hysteresis loops. A Keithley 237 high-voltage source meter
measured the current-voltage characteristics. The leakage current
density was determined by fitting the current density relaxation
data to the Curie-von Schweidler equation [22]. Dielectric break-
down measurements were conducted using Keithley 237 high-
voltage source meter with step increase of voltage. Each applied
voltage was applied to the testing capacitor, which was
immersed in Fluka silicone oil, for a time duration of one second
before the voltage increases to the next value, or until a dielectric
breakdown occurred. The applied voltage level at which the
dielectric breakdown occurred was recorded as the breakdown
voltage for the capacitor being tested. Weibull analysis was
applied to determine the mean breakdown voltage of the speci-
MFC mens. Particle size distributions of the PLZT powders used for
the AD processing were measured by a CILAS 1064 particle size
analyzer.

Fig. 1. Schematic illustration of the aerosol deposition system developed at

Argonne for the fabrication of dense PLZT films at room temperature. 3. Results and discussion

Fig. 2a shows an SEM micrograph of PLZT powder that was used

Experimental conditions that were used in our AD process are
for the AD process, and Fig. 2b shows its particle size distribution.
summarized in Table 1.
An X-ray diffraction pattern of the powder is shown in Fig. 2c. All
During the AD process, PLZT particles are accelerated when they
diffraction peaks can be indexed according to a pseudo-cubic per-
are subjected to the pressure difference between the aerosol cham-
ovskite structure for PLZT (JCPDS 56-0900). A low degree of
ber and the deposition chamber. The flow of the PLZT particles is
agglomeration is evident from the SEM image. More than 90% of
directed toward the substrate affixed to the sample stage. When
the particle population is within the size range of 0.2–2 lm, which
their speed exceeds a critical value, the particles consolidate and
is the desirable particle size range for producing high quality dense
fused upon impact without the need of heating. Because AD is done
oxide films by AD process [23]. An average particle size of 0.8 lm
without heating the substrate, flexible materials such as metalized
was measured.
polymer films, plastics, thin metal foils, thin glass, etc. can all be
Plan-view and cross-sectional view SEM micrographs are
used as the substrates. By using flexible substrates, PLZT-based
shown in Fig. 3a and 3b, respectively for a 8-lm-thick AD PLZT
capacitors can be produced in a wound configuration [21], similar
film deposited on a (1 1 1) oriented platinum coated silicon (PtSi)
to the currently used polymer-based capacitors that can exhibit
substrate. Fig. 3c shows a photograph of an as-deposited PLZT film
benign failure.
(10 mm  15 mm) coated on a glass slide by the AD process with-
The phase integrity of PLZT films made by AD was studied by
out any post-deposition heat treatment. The PLZT film on glass is
a Bruker AXS D8 with GADDS diffraction system. Microstructures
transparent, which illustrates the nature of highly dense and good
were analyzed by a Hitachi S-4700-II field-emission electron
optical property. The AD ceramic film is made of close-packed par-
microscope. For dielectric characterizations, platinum (Pt) or alu-
ticles that collided at high speed and fused together upon impact
minum (Al) top electrodes with thickness of 100 nm were
with the substrate. The as-deposited films are polycrystalline and
deposited by electron-beam evaporation onto the PLZT films
have no preferred orientation, as illustrated by the X-ray diffrac-
through shadow masks to define the appropriate size of capaci-
tion pattern shown in Fig. 3d. All peaks can be indexed in accor-
tors for testing. A Signatone QuieTempÒ probe system with heat-
dance with pseudo-cubic PLZT (JCPDS 56-0900) and cubic Pt
able sample stage (Lucas Signatone Corp., Gilroy, CA) was used
(JCPDS 01-087-0646). The peak broadening observed in Fig. 3d is
for dielectric characterization. For electrical testing and polariza-
due to the film’s small crystalline size and the elevated level of
tion measurements, the top electrode was connected with one
mechanical stress caused by the elastic distortion of PLZT crystal-
probe and the metallized film (bottom electrode) with the other.
lites upon impact with the substrate during the AD process.
A positive applied voltage corresponds to a configuration where
Fig. 4a shows the frequency dependence of the dielectric con-
the top electrode is at a higher potential than the bottom elec-
stant for a 8-lm-thick PLZT film deposited by the AD process
trode. An Agilent E4980A precision LCR meter was used to deter-
on an 100-nm-thick aluminum-metallized polyimide film. The
mine the capacitance and dissipation factor under an applied bias
aluminum-metallized polyimide films for this study were provided
field. A Radiant Technologies Precision Premier II tester measured
by Sigma Technologies International, LLC, Tucson, AZ. At room
the hysteresis loops. The capacitor samples were immersed in
temperature and 10 kHz, we measured a dielectric constant of
85 and dielectric loss of 0.012. The dielectric constant exhibits
a good linear dependence on the logarithm of frequency, indicating
Table 1
Summary of processing conditions used in AD process.
that the frequency response of domain motion in AD PLZT dielec-
tric films is not strongly affected by the applied bias field [24].
Parameters Values
To understand the dielectric response of AD PLZT films in bias field,
Pressure in deposition chamber 2–5 Torr we measured the dielectric properties as a function of applied
Pressure in aerosol chamber 100–300 Torr bias voltage up to 300 V (corresponding to an electric field of
Dimension of nozzle orifice 7 mm  0.4 mm
Carrier gas type N2, Ar, He, Air
400 KV/cm), as shown in Fig. 4b. Again, we observed low dielec-
Gas flow rate 1000–7000 sccm tric loss (1%) that is nearly independent of applied bias voltage.
Nozzle to substrate distance 2–10 mm The little hump in the dielectric constant curve (Fig. 4b at 50 V)
Substrate moving speed 0.1–10 mm/s is related to the initial polarization. Further increase in the applied
Substrate temperature Room temperature
electric field leads to a gradual decrease in dielectric constant.
 B. Ma et al. / Materials Science for Energy Technologies 2 (2019) 96–103 99

Fig. 2. (a) SEM image, (b) particle size distribution, and (c) X-ray diffraction pattern of the PLZT powder used in the deposition of PLZT films by AD process.

(d)
Pt(111)
PLZT(110)
Intensity (a.u.)

Pt(111) Cu-K

PLZT(211)
PLZT(200)
PLZT(111)

PLZT(210)

PLZT(220)
PLZT(100)

20 30 40 50 60 70
2 (o )

Fig. 3. (a) Plan view and (b) cross-sectional view SEM micrographs of AD PLZT film on PtSi substrate, (c) photograph of AD PLZT on glass slide, and (d) X-ray diffraction pattern
of AD PLZT film on PtSi substrate.
100 B. Ma et al. / Materials Science for Energy Technologies 2 (2019) 96–103

100 0.2 100 0.2

Dielectric Constant 80 80

Dielectric Constant
0.15 0.15

Dielectric Loss

Dielectric Loss
60 60
0.1 0.1
40 40

0.05 0.05
20 20

0 0 0 0
4 5
1000 10 10 0 50 100 150 200 250 300 350
Frequency (Hz) Bias Voltage (V)

Fig. 4. (a) Frequency dependence and (b) bias voltage dependence of dielectric properties of AD PLZT deposited on aluminum-metallized polyimide films.

Dielectric constant displayed a weak dependence on applied bias Fig. 5 shows polarization–electric field (PE) hysteresis loops
voltage for bias voltage >00 V. measured at different temperatures for a 8-lm-thick PLZT film
It is worth noting that the PLZT films fabricated by room tem- fabricated by AD process on aluminum-metallized polyimide film.
perature AD process exhibit much lower tunability as defined by, The data in Fig. 5 illustrate paraelectric behavior, i.e. nearly linear
dependence of dielectric polarization on the applied voltage. The


eðEÞ enclosed area within the PE loop, which is related to energy dissi-
sðEÞ ¼ 1
 100% ð1Þ
eð0Þ pation and hysteresis loss, slowly increases with increasing
temperature.
where e(0) and e(E) are dielectric constant under zero-field and at Fig. 6a shows the time relaxation in leakage current density
applied field E, respectively. While high tunability is desirable for measured with various levels of applied voltage for a 8 lm-
sensor applications, low tunability is advantageous for DC bus thick AD PLZT film fabricated on aluminum-metallized polyimide
capacitor application in power inverters due to the minimal change film. Steady-state leakage current density can be extracted by fit-
in the circuit impedance at different voltage load levels. ting the relaxation data to Curie–von Schweidler equation [22],

1.5 1.5 1.5

1 1 1
Polarization (µC/cm )

Polarization (µC/cm )

Polarization (µC/cm )
2

0.5 0.5 0.5

0 0 0

-0.5 -0.5 -0.5

-1 -1 -1

-1.5 -1.5 -1.5

-100 -50 0 50 100 -100 -50 0 50 100 -100 -50 0 50 100

Applied Voltage (V) Applied Voltage (V) Applied Voltage (V)

1.5 1.5 1.5

1 1 1
Polarization (µC/cm )
Polarization (µC/cm )

Polarization (µC/cm )
2
2

0.5 0.5 0.5

0 0 0

-0.5 -0.5 -0.5

-1 -1 -1

-1.5 -1.5 -1.5

-100 -50 0 50 100 -100 -50 0 50 100 -100 -50 0 50 100

Applied Voltage (V) Applied Voltage (V) Applied Voltage (V)

Fig. 5. PE hysteresis loops measured at different temperatures for 8 lm-thick PLZT film deposited on aluminum-metallized polyimide film.
 B. Ma et al. / Materials Science for Energy Technologies 2 (2019) 96–103 101

Applied Field (kV/cm)

-6 0 100 200 300 400 500 600
10
0.1
80V
160V
240V
320V
-7 400V
10 480V
J (A/cm )

J ( A/cm )
2

2
0.01

s
-8
10

-9
10 0.001
1 10 100 1000 0 100 200 300 400 500

Time (s) Applied Voltage (V)

Fig. 6. (a) Time relaxation in current density and (b) field-dependence of leakage current density for 8 lm-thick AD PLZT film on aluminum-metallized polyimide film.

JðtÞ ¼ J S þ J 0  t
n ð2Þ 2

where JS is the leakage current density, J0 is a fitting constant, t is
relaxation time in seconds and n is the slope of the log–log plot. Weibull Parameter, ln(ln(1/(1-p)))
The steady-state leakage current density is plotted as a function 1
of applied voltage in Fig. 6b. The leakage current density increases
exponentially with increasing applied field. At room temperature,
we measured a leakage current density of 2 nA/cm2 at 100 V
0
and <0.1 lA/cm2 at 500 V for a 8 lm-thick AD PLZT film capac-
itor on aluminum-metallized polyimide film.
-1
The dielectric breakdown of AD PLZT films on Al-metallized
polyimide was investigated by means of Weibull analysis [25–
27]. Each sample was tested at room temperature with a step
-2
increase in applied voltage and 1 s holding time until the leakage
current exceeded 1 lA. Results of the breakdown voltage measure-
ments were fit with the following two-parameter Weibull distribu- VB = 990 V
-3
tion function, = 7.43
"
 #
v b
Fðv Þ ¼ 1
exp
ð3Þ -4
g 100 1000 10
4

where b and g are fitting parameters of the measured values of the
observable, v . The mean voltage to failure (MVTF) value, i.e., the
mean breakdown voltage, (V B ), can be extracted from points where
the fitting lines intersect with the horizontal line going through
lnðlnð1=ð1
pÞÞÞ = 0. Using Bernard’s approximation, the sampling
cumulative distribution parameter, p, is calculated from the follow-
ing formula [28] for each set of experimental data:
r
0:3
p¼
N þ 0:4
where N is the total sample number, and r is the sample sequential
number. Fig. 7 shows a two parameter Weibull plot of dielectric
breakdown strength measured on a group of 30 samples of AD PLZT
film capacitors (8-lm-thick) on aluminum-metallized polyimide
films. All 30 samples displayed breakdown voltage greater than
600 V at room temperature. We measured mean breakdown voltage
of 1000 V and Weibull modulus b of 7.4 with two-parameter
Weibull analysis. A high value of Weibull modulus indicates a low
level of fluctuation associated with the samples, i.e., a good homo-
geneity among samples. Our results demonstrated that PLZT film
capacitors produced by AD process not only meet the specification
for next generation power inverter applications [9] but also provide
a method for cost-effective manufacturing of high-temperature
capacitors.
Breakdown Voltage (V)
Fig. 7. Weibull plot of breakdown strength of PLZT deposited by AD process on
aluminum-metallized polyimide films.
The energy conversion/storage capability of AD PLZT on metal-
lized polyimide foils was investigated by high-field polarization
(PE) measurements. Fig. 8a shows PE hysteresis loops measured
ð4Þ at various maximum applied fields on 8-lm-thick AD PLZT film
capacitors on aluminum-metallized polyimide films. As the data
in Fig. 8a illustrate, the polarization of AD PLZT film capacitors
exhibits good linear dependence on applied electric field even at
a high field level of 1 MV/cm. This behavior is desirable for energy
conversion/storage applications as it directly translate to lower
dissipation losses. As shown in Fig. 8b, the recoverable energy
density increases with increasing applied field. We measured
recoverable energy density URec  8 J/cm3 with an applied voltage
Vmax  800 V (corresponding to Emax  1 MV/cm) and
URec  13.2 J/cm3 with a 1000 V applied voltage (corresponding
to Emax  1.25 MV/cm). This energy density value is substantially
higher than that of the state-of-the-art polymer film capacitors
[29,30] which typically have URec around 0.2 J/cm3 and are rated
for operation up to 85 °C. AD PLZT ceramic film capacitors, on
the other hand, can operate at much higher temperatures
102 B. Ma et al. / Materials Science for Energy Technologies 2 (2019) 96–103

Applied Voltage (V) V (V)

max
-1000 0 1000 0 200 400 600 800 1000
20 15
Polarization (µC/cm )
2

(J/cm )
3
10

Rec
U
5

-20 0
-1000 0 1000 0 200 400 600 800 1000 1200 1400
E (KV/cm) E (KV/cm)
max

Fig. 8. (a) PE hysteresis loops and (b) recoverable energy density as a function of applied field for a PLZT film deposited by AD process on aluminum-metallized polyimide
substrate.

100 0.2 30

80
TCC, ( C/C ) x 100

0.15 15
Dielectric Constant

X8R
Dielectric Loss

60
0

0.1 0
40

0.05 -15
20

0 0 -30
-50 0 50 100 150 200 -50 0 50 100 150 200
o o
Temperature ( C) Temperature ( C)

Fig. 9. (a) Temperature-dependent dielectric properties of AD PLZT film on aluminum-metallized polyimide substrate, and (b) plot of TCC measured at 10 kHz illustrating that
the AD PLZT film capacitor meets the X8R specification.

(200 °C) without deterioration in their ability to withstand ripple 4. Conclusions

currents. The AD PLZT film capacitors can be used in high-
temperature power electronics such as power inverter for EDVs. We produced dense ceramic films by room temperature aerosol
Fig. 9a shows the dielectric properties measured at 10 kHz as a deposition process on a variety of substrates. AD PLZT film capac-
function of temperature for a PLZT film capacitor 8-lm-thick itors exhibit superior volumetric and gravimetric specific capaci-
deposited on aluminum-metallized polyimide substrate by AD tance when compared to the current-in-use polymer film
process. The data in Fig. 9a indicate that the PLZT-based film capac- capacitors. The measured properties showed that the PLZT-based
itors are suitable for applications in a broad temperature range ceramic film capacitors meet the requirements for advanced
from
55 °C to above 175 °C. Fig. 9b shows the temperature coef- high-temperature capacitors. We successfully fabricated
ficient of capacitance (TCC) measured at 10 kHz for a 8-lm-thick 8-lm-thick PLZT film capacitors by the AD process on flexible
AD PLZT film. The temperature variation property of the AD PLZT aluminum-metallized polyimide films. PLZT films fabricated by
film capacitor satisfies the X8R rating requirement (
55/+150, the AD process exhibited high dielectric constant, low dielectric
DC/C0 = ±15%) as highlighted by the shaded area shown in the fig- loss, weak dependence on applied field, high recoverable energy
ure inset; this again indicates that PLZT-based film capacitors fab- density, and were found suitable for high-field and high-
ricated by the high-rate AD process possess desirable thermal temperature operation. At room temperature, we measured
properties that meet the next generation power inverter require- dielectric constant of 85, dielectric loss of 0.012, energy
ments. From the slope of the linear fitting to the experimental data, density of 13.2 J/cm3 with a maximum applied Field of
we observed a temperature-dependent capacitance variation coef- Emax  1.25 MV/cm. The mean dielectric breakdown voltage of
ficient (a) of 560 ppm/K for PLZT film capacitors on aluminum- 1000 V was determined by Weibull analysis for AD PLZT film
metallized polyimide films. capacitors of 8-lm-thick deposited on aluminum-metallized
 B. Ma et al. / Materials Science for Energy Technologies 2 (2019) 96–103
polyimide substrates. The temperature variation of AD PLZT film
capacitors satisfy the X8R rating requirement. The AD process
offers the greatest potential for producing flexible, low-cost,
robust, compact and light-weight ceramic film capacitors for
high-temperature operation in power inverters for electrical drive
vehicles and green energy applications.
Conflict of interest
None.
Acknowledgment
This work was supported by the U.S. Department of Energy,
Vehicle Technologies Program, under Contract No. DE-AC02-
06CH11357. Microstructure analysis was done at the Electron
Microscopy Center for Materials Research at Argonne National Lab-
oratory, a U.S. Department of Energy Office of Science Laboratory
operated under Contract No. DE-AC02-06CH11357 by UChicago
Argonne, LLC. The authors would like to thank Mr. Chris Hohmann
and Dr. Angelo Yializis, Sigma Technologies International, LLC, Tuc-
son, Arizona for providing the aluminium metallized polymer films
that were used in this study.
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.mset.2018.11.005.
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