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Coupling of the electrocaloric and electromechanical effects for solid-state

refrigeration
A. Bradeko, . Jurii, M. Santo Zarnik, B. Mali, Z. Kutnjak, and T. Rojac

Citation: Applied Physics Letters 109, 143508 (2016); doi: 10.1063/1.4964124


View online: http://dx.doi.org/10.1063/1.4964124
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APPLIED PHYSICS LETTERS 109, 143508 (2016)

Coupling of the electrocaloric and electromechanical effects for solid-state


refrigeration
A. Bradesko,1,2,a) D
- . Juricic,1,2 M. Santo Zarnik,1 B. Malic,1,2 Z. Kutnjak,1,2 and T. Rojac1,2
1
Jozef Stefan Institute, Jamova cesta 39, 1000 Ljubljana, Slovenia
2
Jozef Stefan International Postgraduate School, Jamova cesta 39, 1000 Ljubljana, Slovenia
(Received 17 February 2016; accepted 21 September 2016; published online 4 October 2016)
Electrocaloric (EC) materials have shown the potential to replace some of the technologies in
current commercial refrigeration systems. The key problem when fabricating an efficient EC
refrigerator is the small adiabatic temperature change that current bulk materials can achieve.
Therefore, such a solid-state EC refrigerator should be engineered to enhance the EC temperature
change by rectifying the induced EC heat flow. Here, we present a numerical study of a device that
couples the EC and electromechanical (EM) effects in a single active material. The device consists
of several elements made from a functional material with coupled EC and EM properties, allowing
the elements to bend and change their temperature with the application of an electric field. The
periodic excitation of these elements results in a temperature span across the device. By assuming
heat exchange with the environment and a low thermal contact resistivity between the elements, we
show that a device with 15 elements and an EC effect of 1.2 K achieves a temperature span between
the hot and cold sides of the device equal to 12.6 K. Since the temperature span can be controlled
by the number of elements in the device, the results suggest that in combination with the so-called
giant EC effect (DTEC  10 K), a very large temperature span would be possible. The results of
this work should motivate the development of efficient EC refrigeration systems based on a cou-
pling of the EC and EM effects. Published by AIP Publishing.
[http://dx.doi.org/10.1063/1.4964124]

Electrocaloric (EC) cooling technology has the potential removal of the electric field (adiabatic depolarization), the
for a broad range of applications, such as on-chip cooling heat must be absorbed from the heat source. Jia and
and body-worn chillers, due to its high efficiency and scal- Sungtaek Ju8 for example, separated the EC heat flux by
ability. The main problem of putting EC refrigeration into attaching an EC element to a motorized z-stage, which was
practice is the small temperature change typically induced in moved vertically to achieve thermal contacts with the heat
bulk EC materials (DTEC  3 K).13 The temperature change sink and the heat source during the EC cycle. This mechani-
(or span) in an EC-based cooling device, however, can be cal motion of the EC material separated the heat flows during
made larger than the EC effect of the material itself, leading the EC cooling cycle; however, the authors stressed the criti-
to an effective regenerative process.4 Several studies have cal importance of the thermal contact resistance. Ju9 further
reported EC coolers with significant regeneration and, conse- developed the idea of introducing electrostatic elements to
quently, an increased temperature span in the device relative mechanically displace a plate with EC elements, with which
to the adiabatic EC temperature change induced by the EC they separated the heat flows and created a temperature span
material. For example, Gu et al.5 reported on an EC oscilla- in the device.
tory refrigeration (ECOR) device in which the EC elements, In this study, we propose the coupled use of the EC and
driven by a stepper motor, slide laterally on a substrate, cre- electromechanical (EM) properties of a material in a device.
ating a temperature span in the substrate. Numerical studies The application of an electric field to these materials simulta-
of the ECOR cooler revealed a temperature span of 52 K neously induces the EC and EM effects, and thus enables the
with a DTEC 16 K (regeneration factor DT/DTEC 3.3). separation of the adiabatic polarization and depolarization by
Plaznik et al.6 demonstrated a cooling device with active EC displacing or bending the material and making a contact with
regeneration (AER).7 The device exhibited a regeneration the heat source or heat sink during the EC cycle. The concept
factor of 3.7, which is currently the largest measured value would in principle allow the heat flow in the device without
reported in the literature. external mechanical motions as previously suggested.5,810
The key problem that needs to be addressed in order to Examples of materials that exhibit high EC and EM effects
achieve a large temperature span in cooling devices is the are polymers11,12 and ceramics13,14 belonging to the group of
effective separation of the heat flows during an EC cycle. ferroelectrics and relaxor-ferroelectrics.1517 The ceramic
When the EC material is heated by DTEC as a result of the 0.65Pb(Mg1/3Nb2/3)O3-0.35PbTiO3 (PMN-35PT) is an
applied electric field (adiabatic polarization), the generated example of such a material with large measured EC and EM
heat must be directed to the heat sink. On the other hand, effects.18,19
when the EC material is cooled by DTEC as a result of the The concept of the device on which we demonstrate our
idea is shown schematically in Fig. 1. The device consists of
a)
andraz.bradesko@ijs.si PMN-35PT elements in a form of cantilevers (one-side

0003-6951/2016/109(14)/143508/5/$30.00 109, 143508-1 Published by AIP Publishing.

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143508-2 Bradesko et al. Appl. Phys. Lett. 109, 143508 (2016)


clamped) that exhibit both EC and EM (i.e., piezoelectric) in contact Rcontact ; if itc < t < i 1tc
Ri
properties.2022 When an electric field is applied to such a can- not in contact infinite R; else;
tilever, it will simultaneously heat up by DTEC and bend (1)
because of the EC and piezoelectric responses, respectively.
Then, when the electric field is removed, the cantilever will where i is the cantilever number, counted from the bottom to
return to its initial position and cool down by DTEC.23 This the top of the array, and tc is the time during which the two
means that by using an array of such cantilevers and by pro- cantilevers are in contact.
viding periodic contacts between them, the device can, in Depending on the position in the array (number i), it is
principle, transfer the heat generated during adiabatic polari- assumed that the cantilever can be in three different states. If
zation through the device, leading to a temperature span larger the simulation time (t) matches the elements time interval
than DTEC between the ends of the device. between itc and itc tp, during which the EC cycle begins,
We investigated the time-dependent behavior of the the cantilever generates the EC heat (Qeci). This step simu-
device with finite-element modelling using the commercial lates the adiabatic polarization of the material. After a cer-
software COMSOL Multiphysics.24 The devices geometry tain time tc, the adiabatic depolarization follows. In the time
was considered to be two dimensional as temperature varia- between (i 1)tc and (i 1)tc tp the material cools down.
tions are only expected in two directions. The cantilever ele- Before and after these two steps, there is no heat generation
ments, clamped on one side onto Al holders, were 20 mm or termination in the material. These steps of the devices
long and consisted of a 50-lm-thick EC layer, i.e., PMN- operation were described with Eq. (2)
35PT, and a 10-lm-thick bottom Pt electrode.20 The upper 8
electrode of the cantilever is sputtered Au and was thus < mcp DTEC ;
> if itc < t < itc tp
neglected in the model due to its small thickness (200 nm). Qeci mcp DTEC ; if i 1tc < t < i 1tc tp
To avoid a multi-field description of the device, we >
:
0; else;
modelled only its thermal aspects. The contacts between the
cantilevers were described as thin resistive layers that work (2)
as thermal switches. This means that in the time frame of the where m is the mass of the EC layer, tp is the time duration
mechanical contact between the cantilevers, the thermal con- of the heat generation or termination, cp is the specific heat
tact (R) was assumed to have a finite thermal resistance capacity, and DTEC is the EC temperature change induced by
(Rcontact), while in the absence of a mechanical contact, the the cantilever.
thermal contact resistivity was set to be infinitely high. Thus, The time tc was determined based on the thermal time
the thermal resistivity of the contacts between the cantilevers constant (s), which is the time necessary for two cantilevers
along the structure was mathematically described using the to stabilize their temperatures. The time constant s was esti-
following expressions: mated using an equivalent thermal circuit of two cantilevers
in contact25

s Rtotal Ctotal ; (3)

where Rtotal is the sum of the contacting cantilever thermal


resistances and contact resistance. Ctotal is the total thermal
capacity. Rtotal is 0.68 K/W and Ctotal is 1.35  103 J/K.
For tc the value of 10s was considered, which in our
case is 0.01 s. This value is calculated for the best-case sce-
nario, where the contacts between the cantilevers are ideally
conductive. We estimated the actual thermalization time
using two 100-lm-thick PMN-10PT plates and a small bead
thermistor. We compared the experimental time response of
a single plate and two plates in contact (see inset of Fig. 2).
While a similar time response was observed for these two
cases, compared to the single plate, we observed a reduction
of the measured DTEC in the case of the two plates in contact.
FIG. 1. Schematics of the refrigeration cycle using cantilever elements This indicates that the transfer between the plates is faster
exhibiting both an EC and EM (piezoelectric) response. The operating cycle
of the refrigeration device consists of three steps: (i) application of the elec-
than the response time of the thermistor (estimated as
tric field (E) to a single cantilever with an initial temperature Ti, causing the <0.7 s). From the observed temperature responses, we esti-
cantilever heat above its initial temperature (Ti DTEC) and bend according mated the time needed for the thermalization of the 100-lm-
to, respectively, the EC and EM effects, (ii) heat transfer between the canti- thick plates as 0.17 s. By scaling the results to 60-lm-thick
levers until a stationary state is achieved (Ti DT), which occurs through
the contact of the i-th and upper neighboring (i 1) cantilever, and (iii) plates (which is the cantilever thickness proposed here for
removal of the electric field causing the cantilever to return to its initial posi- the device), we obtained the time of the temperature equili-
tion, while its temperature decreases below the initial temperature (Ti DT bration of 0.06 s (see experimental details in supplemen-
 DTEC) due to the adiabatic depolarization. This cycle is repeated sequen-
tary material).18,26
tially through the device from the first to the last cantilever in a vertical cas-
cade and results in a temperature span larger than DTEC across the device For each cantilever, we assumed a DTEC of 0.2 K, which
(central schematic). is the value measured on the PMN-35PT thick film.27 The
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143508-3 Bradesko et al. Appl. Phys. Lett. 109, 143508 (2016)

In the next step, we investigated how repeated excitations


of the elements (cycles) affect the temperature span in a
device with three, five, and ten elements (Fig. 3). In the device
with three elements, the temperature span converges to
DT Tlast  Tfirst 0.32 K after six cycles. The device with
five elements reaches a steady DT 0.56 K after eight cycles.
The DT further increases with the number of elements, and
the device with ten elements reaches DT 1.32 K after thirty
cycles.
As shown in Fig. 4 (circles), the converged temperature
span between the first and last elements follows a linear rela-
tionship with the number of elements. This is due to the ideal
heat-transfer conditions assumed in these initial simulations.
To simulate the devices operation in a realistic environment,
FIG. 2. Simulated temperature in the first cycle as a function of operating
we included in the models: (i) the heat exchange between the
time for the EC device with three elements in ideal conditions. The tempera- elements and surrounding (air and the element holders), and
ture was calculated in the center of each EC (PMN-35PT) layer. The inset (ii) the partial overlapping of the elements (see the bottom
shows the measured temperature response of a 100-lm-thick plate either schematic in Fig. 4). The heat exchange with the air was
measured as a single plate or in contact with a plate of the same dimensions
(details are reported in the supplementary material). modelled using Fouriers law. The characteristic thermal dif-
fusion length was calculated as25
p
d atc : (4)
values of cp and k for the materials in the device were taken
from Refs. 28 and 29. The air diffusivity (a) was taken from the literature,29 while
We investigated how the number of elements (n) influen- the air temperature was 293.15 K. The heat exchange with
ces the overall EC temperature span in the device. We built the Al holders was calculated in a similar way. In the realis-
models of the devices with three, five, and ten cantilevers tic description, we also assumed that the overlapping area of
(these cantilevers are subsequently referred to as elements, the elements is reduced by a half.
since we modeled only their thermal aspect). We first investi- Fig. 4 (squares) shows the dependence of the converged
gated an ideal case where any heat exchange with the environ- DT on the number of elements, n, for realistic conditions. In
ment is neglected and where the thermal contacts between the these realistic models, DT increases with the number of ele-
elements are ideal. For this case, we assumed no contact resis- ments, but only up to ten elements, in which case the trend is
tance during the time of contact between the elements and an similar to that predicted for ideal conditions (Fig. 4, circles).
ideal contact equal to the whole area of the elements. With a further increase of n above ten elements, DT deviates
After building the numerical models, we simulated the from the linear trend. This is due to the longer idle time of
device with three elements and probed the temperature in the the elements during which they do not contribute to the heat
middle of each EC element during the first operation cycle. transfer across the device. The time for one cycle of the
While the temperature of the element increased, a simulta- device was, in fact, longer due to the larger number of ele-
neous contact was made with the second element. These two ments in the device, operating in sequence (one after the
steps were used as a part of the simulation procedure that other). In addition, the number of cycles for the temperature
emulated the application of the electric field to the first ele- span to converge increases with the number of elements,
ment. In this way, the first element exchanged the generated thus prolonging the total operating time of the device. Both
EC heat with the second element. After tc elapsed, the con-
tact was closed and the first element cooled by DTEC. The
second and third elements followed the same procedure. The
third element had no upper neighbor to further transfer the
generated heat, so even after heating and cooling, the tem-
perature of the third element remained the same as it was at
the beginning of its cycle.
Figure 2 shows the results of the simulations of the
device with three elements under ideal heat-transfer condi-
tions. The results clearly show that in the first cycle, a tem-
perature span of 0.18 K is established across the EC device
between the first and the last element. If the simulation pro-
cedure is repeated, starting again with the first element, the
temperature span across the device continues to increase. FIG. 3. Simulated temperature as a function of the number of operating
However, the heat exchange stopped after several cycles cycles for the ideal EC device with 3, 5, and 10 elements. The inset shows a
schematic of the cantilever array with indicated temperatures for the first
when the temperature span between the element neighbors (Tfirst) and last (Tlast) elements. The temperature spans (DT) between the first
became larger than the EC temperature change of the single and last elements achieved with 3, 5, and 10 elements that are indicated on
element. the graph.

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143508-4 Bradesko et al. Appl. Phys. Lett. 109, 143508 (2016)

FIG. 4. Simulated temperature span (DT) between the first and last elements
in the cantilever array as a function of the number of elements (n) in the EC
device for ideal (full line connecting circles) and realistic (dashed line con- FIG. 5. Ratio of the temperature span between the first and the last element
necting squares) operating conditions. The lines are drawn as a guide to the in the array for a finite contact resistance (DT) and that of the ideal contact
eye. The insets show the temperature distribution in the devices with 10 ele- with no resistance (DTic) as a function of the contact resistance (Rcontact)
ments for ideal and realistic operating conditions. For the realistic device, between the cantilevers. On the secondary x-axis, the corresponding change
the temperature profiles for the first and last element are plotted above and of tc with the Rcontact is shown. The dependence of the regeneration factor on
below the elements. The temperature profile across the center of the ele- the contact resistance (Rcontact) is shown on the secondary (right) axis. The
ments is shown on the right side. dashed line is drawn as a guide to the eye. The schematic shows Pt and
PMN-35PT in contact with the indicated Rcontact.

of these effects provide sufficient time for heat exchange to method, we apply an electric field first to the odd and then, in
occur with the cantilever holders and air, which reduces the the second step, to the even elements (see inset of Fig. 6).
effectiveness of the refrigerator. The partial element overlap- Using such an odd/even excitation, the DT increases com-
ping during contact, on the other hand, leads to an inhomoge- pared to the periodic excitation. As shown in Fig. 6, the
neous distribution of the temperature in the elements along device with 15 elements excited with the odd/even method
the lateral direction (compare the temperature distribution in shows a DT 1.87 K (Fig. 6, diamonds), while the periodic
the insets of Fig. 4), so reducing the effective cooling area. excitation results in a DT 1.42 K (Fig. 4, squares).
To reveal the important features of the realistic device, For use in commercial applications, DT must be increased
we further introduced in the realistic model, the contact resis- further. This can be done either by increasing the number of
tance between the elements as a critical parameter that deter- elements in the device and/or by replacing the EC material. To
mines the performance of the device. In the literature, we study both possibilities, we simulated the behavior of the
found values for the contact resistances (in the case of low- device as a function of the number of elements using PMN-
pressure contacts) ranging from 102 m2K/W to 106 m2K/ 10PT as the EC material, which in bulk form exhibits a high
W.3033 We used these values in our model as Rcontact (see EC effect and better energy efficiency (DTEC 1.2 K at 57 kV/
Equation (1)) and simulated the temperature span (DT) at a cm).22,34 The comparison with PMN-35PT (DTEC 0.2 K at
finite contact resistivity, which is plotted in Fig. 5 as the ratio 25 kV/cm) is shown in Fig. 6. The device with fifteen elements
to the ideal, zero contact resistivity (DTic, as calculated in the
previous example with ten elements; Fig. 4, squares). By
using a contact resistance of 106 m2K/W, no differences
were observed as compared to the ideal case; the regeneration
factor (DT/DTEC) is approximately 6. By increasing Rcontact,
the DT/DTic ratio reduces; at 103 m2K/W, the values fall
drastically below 0.2 and the regenerative factor falls to 1.
Thus, liquid interfaces, carbon-nanotube coatings and other
surface-engineering methods that ensure a good thermal con-
tact should be considered when designing this type of
refrigerator.
We next address the problem of the smaller increase in
DT(n) by increasing the number of elements, n, to more than
ten (Fig. 4, squares), while assuming an engineered contact
thermal resistivity between the elements of 106 m2K/W. As
this effect is related to the long idle time of individual ele- FIG. 6. Comparison of temperature span evolution as a function of the num-
ber of cycles between the 15-element device with PMN-35PT and PMN-
ments, excited sequentially along the array, we introduce a
10PT EC materials.34 The simulations were performed by driving the ele-
different excitation procedure that increases the working time ments with the optimum odd/even excitation method, as indicated in the
of the elements during a single EC cycle. With this excitation inset.

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143508-5 Bradesko et al. Appl. Phys. Lett. 109, 143508 (2016)

6
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