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Enhanced Electrical Transport Properties via Defect Control for

Screen-Printed Bi2Te3 Films over a Wide Temperature Range
Jingjing Feng, Wei Zhu,* Zhiwei Zhang, Lili Cao, Yuedong Yu, and Yuan Deng*

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ABSTRACT: The application of screen-printed thin-film thermo-

electric (TE) devices is still in its infancy, mainly due to low TE
Downloaded via UNIV OF WOLLONGONG on July 18, 2020 at 07:36:36 (UTC).

performance of screen-printed films and especially the poor

electrical transport properties. Herein, we design and prepare a
high-performance screen-printed Bi2Te3 film through introducing
excessive Te-based nanosolder (Te-NS) to simultaneously realize
the conduction channel construction and defect control. On one
hand, the promoted carrier migration makes the electrical
conductivity dramatically rise about 7 times, with a maximum
power factor of 4.65 μW cm −1 K −2. Meanwhile, the defect
formation mechanism in the screen-printed Bi2Te3 film after the introduction of Te-NS is also in-depth studied, and the bipolar
conduction is reduced by increased generation of Te•Bi and/or more suppression of BiTe
′ , resulting in a postponed temperature of the
maximum Seebeck coefficient. Hence, the large engineering power factor is achieved with excellent temperature linearity, indicating a
possibility of screen-printed film application in a large temperature region. A TE device with a single leg has been fabricated to
further demonstrate the generation validity. An open-circuit voltage of 11.34 mV and a maximum output power of 27.1 μW at a
temperature gradient of 105 K have been achieved over a wide temperature range from 303 to 478 K. This study provides a
theoretical and practical basis for the performance improvement of screen-printed TE films and devices.
KEYWORDS: thermoelectric film, screen printing, electrical transport property, wide temperature range, defect control

1. INTRODUCTION channel and the improvement of carrier mobility.7 In addition,

Thermoelectric (TE) devices have garnered tremendous
interest in energy conversion field through interconverting
temperature gradients (ΔT) with electric potential.1−3
Conventional approaches to manufacture TE devices generally
involve ingot fabrication, dicing, and etching, which are time-
consuming and energy intensive. In this light, high-throughput
and low-cost screen printing has recently emerged as a
promising manufacturing technology.4−6 The bottleneck of
screen-printed TE devices still lies in low TE performance of
the screen-printed films, especially the electrical transport
property, which is due to the low crystallinity and poor density
of the screen-printed film caused by the evaporation of solvent
and binder during the sintering process.6 In addition, TE
materials with high performance maintained in a large
temperature region are essential for electrical generation
application. Thus, more efforts need to be made toward
raising the electrical transport property of screen-printed films
over a wide temperature range.
The construction of a conduction channel is of much
significance for TE materials to facilitate the carrier transport.
In a previous report, the grains of Bi0.5Sb1.5Te3 film grow and
gradually “sinter” together through increasing the annealing
temperature, thus resulting in the construction of a conduction
a liquid-phase hot deformation procedure is applied in the
fabrication of Bi2(Te,Se)3 ingots with excessive Te powder
with a low melting point, which optimizes the conduction
channel by improving the texture with (00l) orientation,
leading to the enhancement of carrier mobility in TE bulks.8
Recently, nanosolder has been proven to be an effective
additive through facilitating grain crystallization and interfacial
bonding at lower temperatures.9−11 For example, the densities
and electrical conductivities of the brush-painted TE materials
were significantly improved by introducing the Sb2Te3-based
chalcogenidometalate (nanosolder).9 Meanwhile, Sb2Te3-
based nanosolder has also been introduced into the screen-
printed n-type Bi2Te3 material to optimize the electrical
conductivity.12 The carrier concentration is a vital parameter
that greatly influences the electrical transport properties of TE
materials,13 and any deviation from stoichiometry strongly
Received: January 21, 2020
Accepted: March 20, 2020
Published: March 20, 2020

© 2020 American Chemical Society https://dx.doi.org/10.1021/acsami.0c01049

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Figure 1. SEM images of the screen-printed Bi2Te3 films with different contents of Te-NS: (a1, a2) 0 wt %, (b1, b2) 4 wt %, (c1, c2) 8 wt %, (d1,
d2) 12 wt %, and (e1, e2) 16 wt %.
affects the carrier concentration of Bi2Te3 materials.14−16
However, the role of nanosolder on carrier type and
concentration in screen-printed TE films is still deficient and
less investigated so far.
In addition, owing to the higher vapor pressure of Te, Bi2Te3
films inevitably undergo segregation of chemical components
during the sintering process, resulting in changes in carrier
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concentration and intrinsic point defects in the film.7,12 For
example, after high temperature annealing, the Bi2Te2.7Se0.3
film changed from a Te-rich state to a Te-deficient state,
causing a change in ionized defects and reducing the carrier
concentration.17 Experimental results have also shown that the
intrinsic point defects (like antisite defects) dominate the n-
type and p-type Bi2Te3-based materials, playing an important
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Figure 2. (a) XRD patterns of unsintered and sintered Bi2Te3 films with 12 wt % Te-NS (inset is the enlarged part of the gray frame). (b) XRD
patterns of sintered Bi2Te3 films with different content of Te-NS.
role in optimizing the carrier concentration and improving the
TE performance.15,18,19 Harman et al. explained that the main
intrinsic point defects of the Bi2Te3 ingot are positively
charged antisite defects (TeBi •
) on the Te-rich side and
′ ) on the Te-deficient
negatively charged antisite defects (BiTe
side.20 Meanwhile, through controlling the carrier concen-
tration by point defects and suppressing intrinsic excitation, the
TE performance of Bi2Te3 alloys at elevated temperatures is
enhanced.21 Therefore, regulating the carrier concentration of
screen-printed films through intrinsic point defects is an
effective method for improving the electrical transport and TE
properties of screen-printed films.
Hence, in order to further improve the electrical transport
property of screen-printed TE films, we prepared a low-melting
Te-based nanosolder (Te-NS) applied to screen-printed
Bi2Te3 films to facilitate the construction of conduction
channels during the sintering process. Then the effect of
nanosolder on intrinsic point defect control and carrier
transport mechanism is discussed in-depth and clarified.
Additionally, the electrical transport properties of screen-
printed films were systematically studied over a wide
temperature range. On this basis, a TE device with a single
leg has been fabricated to further demonstrate the generation
validity in different temperature ranges, verifying its potential
generation applications in a wide temperature range.
2. EXPERIMENTAL PROCEDURES
2.1. Screen-Printed Bi2Te3 Films and TE Device. Bi2Te3 pastes
were fabricated by thoroughly mixing Bi2Te3 powder, organic binder,
dispersant, solvent, and Te-NS. High purity Bi2Te3 powder (99.999%)
was purchased from Prmat (Shanghai) Technology Co., Ltd. The
organic binder was made by heating (80 °C) and stirring (300 rpm)
the mixture of ethyl cellulose (1 g), diethylene glycol butyl ether
acetate (9 g), and dibutyl phthalate (2 g) until the ethyl cellulose
dissolved thoroughly. It determines the viscosity and rheology of the
paste and affects the printing resolution of screen-printed films.
Tween 80 was used as a dispersant, and as a solvent diethylene glycol
butyl ether acetate was added to adjust the viscosity of the paste.
Using a thiol-diamine method,22,23 Te-NS was synthesized by
dissolving Te powder (1 g) in a cosolvent of ethanethiol (2 mL)
and ethylenediamine (8 mL) at room temperature. Subsequently, it
was stirred until it was completely dissolved to produce a dark purple
solution. Then Te-NS was precipitated by the addition of acetonitrile
(50 mL) and obtained by centrifugation (10,000 rpm, 10 min.). The
Bi2Te3 powder, organic binder, dispersant, and solvent account for 80,
14, 1, and 5 wt % of the paste, and on this basis the extra Te-NS for
different pastes is 0, 4, 8, 12, and 16 wt %, respectively. Once the paste
is prepared, it can be printed on polyimide or AlN substrate via a
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screen-printing technique. Then drying at 150 °C was performed for
60 min to slowly remove the solvent in the printed films, and sintering
at 400 °C was conducted in a furnace tube for about 30 min under N2
atmosphere. To verify the actual generation application of the film
with Te-NS in a wide temperature range, a single leg TE device with
an effective length, width, and thickness of 10 mm, 5 mm, and 166 μm
was fabricated by using the Bi2Te3 paste with 12 wt % Te-NS and Ag
paste as electrode.
2.2. Measurement and Characterization. The morphologies of
the screen-printed films were confirmed by field emission scanning
electron microscopy (FE-SEM, Sirion 200, FEI), and the correspond-
ing energy-dispersive X-ray spectroscopy (EDS) was utilized to
determine the chemical compositions of screen-printed films. An X-
ray diffractometer (XRD, D/MAX 2200 PC, Rigaku) with Cu Kα
radiation (λ = 0.154 nm) was used to characterize the crystal structure
and phase composition of screen-printed films. The electrical
conductivity and Seebeck coefficient of the screen-printed films
were examined simultaneously via a thermoelectric measurement
system (ZEM-3, Ulvac Riko, Inc.) in the temperature range from 300
to 660 K. And a four-probe Hall measurement system (Accent
HL5500, Nanometrics, Inc.) was used to investigate the room
temperature carrier concentration and mobility. The output character-
istics of the device were measured using a high and low temperature
control platform which consists of a cooler on the cold side and a
heater on the hot side. The thermocouple meter was used to calibrate
the temperature difference across the TE device. Once the
temperature gradient was in a thermally steady state, the output
characteristics were simultaneously measured as a function of the
temperature gradient through a program with the LabVIEW
controlled source meter (Keithley 2400).
3. RESULTS AND DISCUSSION
3.1. Microstructure Evolution. The surface morphologies
of screen-printed films after sintering with different contents of
Te-NS are shown in Figure 1. The sintering process of the
screen-printed film not only contains the pyrolysis evaporation
of binders but also includes the sintering crystallization of
Bi2Te3 particles.24 As illustrated in Figure 1a, the Bi2Te3
particles in the film without Te-NS are only slightly sintered,
showing small particle size and large porosity. Particles in the
film with 4 wt % Te-NS (Figure 1b) grow larger, and the
surface and interface of the film contain tiny layer structures.
These tiny layer structures are replaced by small grains in the
film with 8 wt % Te-NS (Figure 1c). In Figure 1d, when the
Te-NS content is 12 wt %, the particle size is significantly
increased, while the porosity drops obviously. The morphology
of the film with 16 wt % Te-NS (Figure 1e) is similar to that of
the film with 12 wt % Te-NS, having larger particle size and
smaller porosity. These differences in the morphology of
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screen-printed films are mainly attributed to the addition of
different Te-NS contents, which may be related to the
improvement of mass transfer along and across grain
boundaries.25
Pure solid-state sintering occurs in the film without Te-NS,
which has higher sintering barrier so that only slight sintering
can occur at the sintering temperature of 400 °C.26 Nanosolder
usually attaches well to the surface of Bi2Te3 particles,12,27 and
its introduction can improve the surface energy of Bi2Te3
particles and promote sintering. Additionally, it can also form a
solid solution with Bi2Te3 in the sintering process, cause the
main lattice distortion, change the point defect concentration,
and thus promote the mass transport, enabling it to sinter and
crystallize even at a lower temperature (400 °C).28−30 The
microscopic origin of the screen-printed films with different
contents of Te-NS should be related to the difference in mass
transfer.29,31 When the Te-NS content is no less than 12 wt %,
the particle size in the films is enlarged obviously, the porosity
drops apparently, and the electrical conduction channel is
significantly improved. That is, Te-NS promotes the sintering
crystallization of the Bi2Te3 film, and some grains may
agglomerate to form larger particles, thus building the
conduction channels.
3.2. Crystallinity and Preferential Orientation
Change. The XRD patterns in Figure 2a indicate that the
sintered Bi2Te3 film has a pure rhombohedral R3̅m phase,
while the unsintered Bi2Te3 film with 12 wt % Te-NS has a tiny
Te (102) peak, attributing to a Te second phase. In Figure 2b,
the XRD patterns display that all the sintered Bi2Te3 films with
different content of Te-NS are pure Bi2Te3 phase without any
detectable Te-rich phase remaining. Therefore, the above
results indicate that there will be enthalpy evaporation during
the sintering process. In order to systematically study the
influence of Te-NS content on the crystal structure of screen-
printed films, the full width at half-maximum (fwhm) of the
main diffraction peak (015) and the orientation factor of (00l)
plane were summarized, as shown in Table 1. The value of
Table 1. FWHM Values of the (015) Plane, Orientation
Factors of the (00l) Plane, and Lattice Parameters for
Screen-Printed Bi2Te3 Films with Different Te-NS Content
lattice parameters/Å
Te/wt % (015) FWHM/deg F (00l) a-axis c-axis
0 0.191 0.038 4.392 30.61
4 0.184 0.068 4.392 30.54
8 0.172 0.051 4.391 30.53
12 0.169 0.128 4.385 30.48
16 0.164 0.094 4.383 30.45
fwhm in (015) decreases monotonously with the increase of
Te-NS content, which indicates that Te-NS improves the
degree of crystallization and facilitates the crystallization of the
screen-printed film. The orientation factor calculated by the
Lotgering method32 is used to evaluate the texture degree. As
shown in Table 1, the F (00l) for films with different Te-NS
content are 0.038 (0 wt %), 0.068 (4 wt %), 0.051 (8 wt %),
0.128 (12 wt %), and 0.094 (16 wt %), respectively, which
basically correspond to the morphological structures. These
Te-NS induced morphology and structure changes are
beneficial to the electrical transport properties of the screen-
printed film.
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The lattice parameters calculated from the XRD peak shift
are also illustrated in Table 1. As the Te-NS content increases,
the lattice parameters of c-axis of screen-printed films show a
downward trend, while the lattice parameters of the a-axis are
basically the same. Combining the different atomic radii of Bi
(1.6 Å) and Te (1.4 Å), it is confirmed that the decrease of c-
axis lattice constants is caused by the increase of the major
• 14,15,33,34
antisite defect (TeBi ). Moreover, the changes of
intrinsic point defects would affect carrier concentration
significantly in screen-printed Bi2Te3 films, thus influencing
the electrical transport.
3.3. Defect Control and Carrier Transport Mecha-
nism. To verify the change in intrinsic point defects, EDS was
used to analyze the chemical compositions of unsintered and
sintered Bi2Te3 films, as shown in Figure 3a. With the increase
of Te-NS content, the contents of Te increase both in
unsintered and sintered films. However, due to the high
saturated vapor pressure of Te, it is inevitably volatilized
during the sintering process. Thus, the Te content in the
sintered films is obviously lower than that in unsintered films.
According to the lattice parameters in Table 1, the evaporation
of Te in Bi2Te3 films during the sintering process decreases
Te•Bi or increases BiTe′ and the addition of Te-NS inhibits the
change in intrinsic point defects.
The following four kinds of intrinsic point defects are mainly
included in Bi2Te3: (1) the Te site lacks one atom to form two
positively charged anion vacancy defects (V•• Te ); (2) the Bi site
lacks an atom to form three negatively charged cation vacancy
defects (V‴ Bi ); (3) Bi occupies the Te site forming a negatively
charged antisite defect (Bi’Te); (4) Te occupies a Bi site and
forms a positively charged antisite defect (Te•Bi). They can be
expressed by the following defect equations:
••
TeTe → VTe + Te ↑ +2e′ (1)
••
BiBi + VTe + 2e′ F BiTe ′′
′ + V Bi + 4h• (2)
′′′
TeTe + V Bi + 3h• F VTe
•• •
+ TeBi + 3e′ (3)
In the sintering process, the evaporation of Te increases V••Te in
Bi2Te3 as shown in eq 1. The increase in V•• Te tends to promote
eq 2 from the left side to the right side, generating more Bi′Te
and VBi‴, and makes eq 3 shift from the right side to the left
side, inhibiting the generation of Te•Bi. The formed BiTe′ and VBi
‴
have acceptor behavior, which increases the concentration of
vacancies and decreases the dangling bonds which donate
electrons. As illustrated in Figure 3b, the film without Te-NS
exhibits p-type conductive behavior. With the increase of Te-
NS addition, the concentration of V•• Te is decreased, and the
acceptor behavior is suppressed. In other words, the decrease
in V••
Te tends to promote the eq 3 shift from the left side to the
right side generating more Te•Bi and inhibits the generation of
Bi’Te (in eq 2), showing a donor effect. Thus, the carrier
concentration increases gradually with the increase of Te-NS
content. Meanwhile, the mobility of screen-printed films
increases basically as the content of Te-NS increases, mainly
due to the decreased porosity and increased texture. In
addition to the above factors, the decrease in mobility of the
film with 16 wt % Te-NS is related to the degradation of
texture.35
3.4. Electrical Transport Properties. Figure 4 displays
the electrical transport properties of screen-printed Bi2Te3
films. The electrical conductivity of screen-printed films with
different Te-NS content is shown in Figure 4a-b. With the
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Figure 3. (a) Element composition of unsintered and sintered Bi2Te3 films and (b) room-temperature carrier concentration (n) and mobility (μ) of
screen-printed Bi2Te3 films.

Figure 4. Electrical transport properties of screen-printed Bi2Te3 films: (a) electrical conductivity, (b) room-temperature electrical conductivity, (c)
Seebeck coefficient, (d) power factor, (e) engineering power factor, and (f) output power density.

increase of Te-NS content, the room-temperature electrical
conductivity first basically increases from 4.75 × 103 S m−1 (0
wt %) and 3.71 × 103 S m−1 (4 wt %) to 31.57 × 103 S m−1
(12 wt %) and then slightly decreases to 24.63 × 103 S m−1 (16
wt %), signifying an initially enhanced and then weakened
room-temperature electrical conductivity in screen-printed
films. The poor electrical conductivity for films with Te-NS
content less than 8 wt % is attributed to less construction of
conduction channels, that is, poor electrical contact between
16634
adjacent Bi2Te3 particles. Furthermore, the enhanced electrical
conductivity for films with Te-NS is related to the enhanced
mobility and carrier concentration, which are shown in Figure
3b. The lower electrical conductivity for the film with 16 wt %
Te-NS should be explained by its lower mobility. As the test
temperature increased, the electrical conductivity of the film
without Te-NS obviously increased, which is mainly due to the
aggravated intrinsic excitation electron−hole pair at elevated
temperatures. With the increase of Te-NS content, this trend
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gradually weakens. The films with more than 12 wt % Te-NS,
especially the film with 16 wt % Te-NS, basically show a
decreasing trend in electrical conductivity with the increase of
test temperature, which indicates that the introduction of Te-
NS is beneficial to suppress the intrinsic excitation at elevated
temperatures.
Figure 4c shows the temperature-dependent Seebeck
coefficient of screen-printed films, which is mainly dependent
on the carrier concentration and is thus sensitive to the point
defects. Because of the change in intrinsic point defects caused
by the evaporation of Te during the sintering process, p-type
conduction occurs in the film without Te-NS, while n-type
conduction occurs in films with Te-NS due to the
compensation of evaporated Te. The absolute values of the
room temperature-Seebeck coefficient decrease slightly with
the increase of Te-NS content, which are 177.6 μV K −1 (0 wt
%), 165.7 μV K −1 (4 wt %), 153.3 μV K −1 (8 wt %), 118.2 μV
K −1 (12 wt %), and 106.6 μV K −1 (16 wt %). The Seebeck
coefficient of the film without Te-NS decreases sharply with
increasing test temperature, and this trend is significantly
suppressed with increasing Te-NS content. This also confirms
that the introduction of Te-NS is beneficial to inhibit the
intrinsic excitation at elevated temperatures via defect control.
In order to further study the mechanism of Te-NS on the
electrical transport of screen-printed films, the energy bands
(calculated by the Goldsmid−Sharp equation of Eg = 2e|
S|maxTmax36,37) and room-temperature reduced Fermi levels
(estimated using a single parabolic band model) of screen-
printed films are summarized in Table 2. We note that, with
Table 2. Estimated Band Gaps and Room-Temperature
Reduced Fermi Levels of Screen-Printed Bi2Te3 Films
Te/wt % Tmax/K Smax/(μV/K) Eg/eV ηF
0 333.5 179.9 0.1200 0.465
4 334.6 −169.8 0.1136 0.693
8 363.6 −156.6 0.1139 0.947
12 454.6 −127.3 0.1157 1.824
16 481.8 −127.5 0.1229 2.188
the increase of Te-NS content, the peak Seebeck coefficient is
postponed, but the Seebeck coefficient is decreased. Accord-
ingly, the estimated band gap shows little change. Meanwhile,
the reduced Fermi levels shift from 0.465 (0 wt %) and 0.693
(4 wt %) to 2.188 (16 wt %), which means the degeneracy is
increased with the increase of Te-NS content. In other words,
the Fermi energy level rises gradually in the conduction band
owing to rapidly increased majority carriers as the Te-NS
content increases, strongly suppressing the intrinsic excitation
and bipolar conduction at the elevated temperature, which is
conducive to the application in a wide temperature range. The
temperature-dependent power factor of screen-printed films is
illustrated in Figure 4d. The power factor of the film with 12
wt % Te-NS is superior to that of others. At 395 K, it achieves
the highest value of 4.65 μW cm−1 K−2. In addition, even at
elevated temperatures, such as 660 K, the power factor is still
higher than that of other films. This is because the adverse
effect of minority carriers on the Seebeck coefficient is
suppressed by increasing the majority carrier concentra-
tion.38,39
The engineering power factor can correctly indicate the
intrinsic characteristics for the output performance of TE
materials. To further evaluate the practicability of the screen-
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printed films, we estimated the engineering power factor as a
function of hot side temperature (Th; cold side temperature
(Tc) is about 310 K) using the eq 4.40,41 In Figure 4e, owing to
the engineering power factor depends on a cumulative
temperature effect, they have quite different trends from
power factors (Figure 4d), which only points to the
momentary characteristic at a temperature. As expected, the
engineering power factor of the film with 12 wt % Te-NS is
superior compared to that of other films. It reaches 0.14 W
m−1 K−1 when Th is about 660 K. In addition, the engineering
power factor of the film with 12 wt % Te-NS shows a linear
relationship with Th in the first half part, mainly due to the
nearly constant electrical conductivity and Seebeck coefficient,
indicating a possibility of application in a wide temperature
range. Accordingly, the output power densities at the
maximum efficiency with respect to Th (Tc = 310 K, leg
length (L) is 8 mm) were calculated via eq 5.40,41 As illustrated
in Figure 4f, the output power density has a similar quadratic
relationship to temperature, and it achieves 152 mW cm−2 for
the film contents 12 wt % Te-NS at Th = 660 K.
2
T
(S2σ )eng =
(∫T h S(T ) dT
c
)
Th
∫T ρ(T ) dT (4)
c
(S2σ )eng (Th − Tc)
Pd =
4L (5)
3.5. Output Performance of Te-NS Based TE Devices.
In order to verify the generation application in a wide
temperature range, a single leg TE device with effective length,
width and thickness of 10 mm, 5 mm, and 166 μm was
fabricated by Bi2Te3 paste with 12 wt % Te-NS and Ag paste as
electrode. Output characteristics of the device with ΔT ranging
from 21 to 105 K are summarized in Figure 5. Figure 5a
presents the typical superimposed voltage−current curves for
different ΔT and generated output power. The maximum
open-circuit voltage of 11.34 mV is achieved, and the
maximum output power of 27.1 μW is generated for a
maximum ΔT value of 105 K. The maximum open-circuit
voltage, output power, and output power density according to
the ΔT of the device is depicted in Figure 5b. A linear
correlation between the maximum open-circuit voltage and ΔT
is observed. Meanwhile, the variation of ΔT shows quadratic
behavior with the maximum output power and maximum
output power density (PD). It is worth noting that the
maximum output power density is as high as 3.265 mW cm−2
for a ΔT value of 105 K.
To further test the hypothesis of the application in a wide
temperature range, we measured the output characteristics of
the device at a fixed ΔT (ΔT = Th − Tc) of 105 K in different
temperature regions (Tc = 273−373 K, Th = 378−478 K),
which are shown in Figure 5c and d. Four nearly parallel lines
are depicted in Figure 5c, and the relatively stable maximum
open-circuit voltages of 11.13 mV (Tc = 273 K, Th = 378 K),
11.34 mV (Tc = 303 K, Th = 408 K), 11.57 mV (Tc = 333 K,
Th = 438 K), and 11.76 mV (Tc = 373 K, Th = 478 K) are
obtained. Figure 5d illustrates the plot of output power−
current curves for different Th. The maximum output powers
in different temperature regions are similar, which are 24.5 μW
(Tc = 273 K, Th = 378 K), 27.1 μW (Tc = 303 K, Th = 408 K),
27.0 μW (Tc = 333 K, Th = 438 K), and 27.7 μW (Tc = 373 K,
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Figure 5. Output characteristics of the single leg TE device. (a) Voltage−current (U−I) curves and output power (P) with respect to different ΔT.
(b) U, P, and PD as a function of ΔT. Insets show the prototype and the thickness of the TE device. (c) U−I curves at a fixed ΔT value of 105 K
with respect to different Th. (d) P−I curves at a fixed ΔT value of 105 K with respect to different Th.
Th = 478 K), indicating stable output power in a wide
temperature range from 303 to 478 K.
4. CONCLUSION
In summary, we have successfully prepared a wide temperature
range screen-printed Bi2Te3 film via conduction channel
construction and defect control. The introduction of Te-NS
can facilitate the construction of conduction channels through
grain growth and boundary bridging, which makes the
electrical conductivity dramatically rise by about 7 times,
with a maximum power factor of 4.65 μW cm−1 K−2.
Meanwhile, the introduction of Te-NS is beneficial for
reducing bipolar conduction via defect control by additional
generation of Te•Bi and/or more suppression of BiTe
′ . As a result,
the temperature of the maximum Seebeck coefficient is
postponed, due to the enlarged band gap, and the intrinsic
excitation and bipolar conduction are suppressed. The
excellent engineering power factor and strong linearity with
temperature indicate a great possibility of application over a
wide temperature range. Furthermore, a single leg TE device
has been fabricated by Bi2Te3 paste with 12 wt % Te-NS. The
maximum open-circuit voltage of 11. 34 mV and the maximum
output power of 27.1 μW were obtained for a larger ΔT value
of 105 K, and the relatively stable output characteristics were
achieved in a large temperature region (303−478 K) at a fixed
ΔT of 105 K. These results open up a simple and effective
direction for the development of screen-printed TE materials
suitable for a wide temperature range, which will greatly
promote the application of screen printing in TE energy
conversion.
■
AUTHOR INFORMATION
Corresponding Authors
Wei Zhu − School of Materials Science and Engineering and
Beijing Advanced Innovation Center for Biomedical Engineering,
Beihang University, Beijing 100083, China; orcid.org/
0000-0002-9887-9804; Email: zhu_wei@buaa.edu.cn
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Yuan Deng − School of Materials Science and Engineering and
Beijing Advanced Innovation Center for Biomedical Engineering,
Beihang University, Beijing 100083, China; orcid.org/
0000-0002-1454-2965; Email: dengyuan@buaa.edu.cn
Authors
Jingjing Feng − School of Materials Science and Engineering,
Beihang University, Beijing 100083, China
Zhiwei Zhang − AECC Aero Engine Academy of China, Beijing
101304, China
Lili Cao − Key Laboratory of the Ministry of Education for
Optoelectronic Measurement Technology and Instrument,
Beijing Information Science and Technology University, Beijing
100101, China; orcid.org/0000-0002-1392-7273
Yuedong Yu − School of Materials Science and Engineering,
Beihang University, Beijing 100083, China
Complete contact information is available at:
https://pubs.acs.org/10.1021/acsami.0c01049
Notes
The authors declare no competing financial interest.
■ ACKNOWLEDGMENTS
The work was supported by the National Key R&D Program
of China (Grant No. 2018YFA0702100), Beijing Natural
Science Foundation (Grant No. 2182032), the Joint Funds of
the National Natural Science Foundation of China (Grant No.
U1601213), the National Natural Science Foundation of
China (Grant No. 51601005), Beijing Nova Programme
Interdisciplinary Cooperation Project (Grant No.
Z191100001119013), and the Fundamental Research Funds
for the Central Universities.
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