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Review

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Advanced Thermoelectric Materials for Flexible Cooling


Application
Jiamin Ding, Wenrui Zhao, Wenlong Jin, Chong-an Di,* and Daoben Zhu

patterns. In addition, novel solid-state


Flexible cooling devices, which aim to fulfill the essential requirement of cooling systems such as thermoacoustic
complex working environments and enable local heat dissipation, have refrigeration,[2] magnetic refrigeration,[3]
and electrocaloric refrigeration[4] exhibit
become the cutting-edge area of refrigeration technology. Thermoelectric
great potential for small-scale cooling.
(TE) material represents a promising candidate for various flexible cooling In recent years, along with the booming
applications, including wearable personal thermoregulation devices. With the development of wearable electronics,
increasing interest in the Peltier effect of conductive polymers and inorganic flexible cooling applications have garnered
films on flexible substrates, flexible cooling devices have undergone rapid significant attention in regard to refrig-
development. Herein, the fundamental mechanisms, basic parameters, and eration with arbitrary geometries such as
the human body, curved pipes, or other
temperature measurement techniques for evaluating the cooling performance
nonplanar electronic devices. However,
are summarized. Moreover, recent progress on TE materials, such as flex- until now, universal and efficient flexible
ible inorganic and organic materials for Peltier cooling studies, is reviewed. cooling technologies remain considerably
More importantly, insights are provided into the key strategies for high- challenging.
performance Peltier devices. The final part details the existing challenges and Under these circumstances, thermoelec-
tric coolers (TECs) provide an alternative
perspectives on flexible TE cooling to inspire additional research interests
option. The basic TEC is a solid-state active
toward the advancement of refrigeration technology. heat pump based on the Peltier effect,
which was discovered in early 1834.[5]
During the Peltier cooling process, direct
1. Introduction current flows through the TEC circuit, creating hot and cold sides
by transferring heat from one side to another.[6] TECs with rela-
Refrigeration refers to the cooling of an object in the definite tively simple structures can easily realize miniaturized and light
time and space for reducing its temperature below the ambient refrigeration equipment due to their favorable properties such
temperature. In modern society, refrigeration devices account as light weight, compact size, and no working fluid or mechan-
for 25–30% of the global consumption of electricity.[1] These ical moving parts. In addition, the power of the Peltier devices
devices have penetrated virtually all production technolo- can be readily adjusted by modifying the current. Given these
gies and scientific research fields. Further, they are integral to advantages, Thermoelectric (TE) cooling has attracted signifi-
improving the quality of human life, such as low-temperature cant interest since the 1950s and the TE refrigeration effect was
storage and cold-chain transportation, temperature control of first experimentally demonstrated in bulky Bi2Ti3 (Figure 1).[7]
instruments, and indoor environment. The emergence and In recent years, benefitting from the rapid development of con-
assessment evaluation of mechanical refrigeration technology ductive polymers, flexible TECs based on organic TE (OTE)
enable large-scale commercial cooling applications, which have materials come into focus. Meanwhile, reduction in the dimen-
a considerable impact on industry, lifestyle, and settlement sions of TE materials and the vigorously development of Peltier
devices based on soft substrates have facilitated the achieve-
ment of flexible cooling applications of intrinsically rigid inor-
J. M. Ding, W. R. Zhao, W. L. Jin, Prof. C.-A. Di, Prof. D. B. Zhu ganic counterparts.
Beijing National Laboratory for Molecular Sciences There have been many reviews dealing with Peltier cooling
CAS Key Laboratory of Organic Solids or flexible TE power generation.[6,12] For example, Zhao et al.
Institute of Chemistry
Chinese Academy of Sciences
overviewed modeling approaches and applications on TE
Beijing 100190, China cooling,[6] Du et al. summarized different classes of flexible TE
E-mail: dicha@iccas.ac.cn materials and devices for power sources.[12b] Nonetheless, to the
J. M. Ding, W. R. Zhao, W. L. Jin best of our knowledge, there is no systematic review focusing
School of Chemical Sciences on flexible cooling application based on TE materials. Our aim
University of Chinese Academy of Sciences is to present a comprehensive insight into the fundamental
Beijing 100049, China
mechanisms, recent progress and key strategies of flexible
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adfm.202010695.
TECs. First, we introduce the operating mechanisms and basic
parameters involved in TECs. Second, we summarize several
DOI: 10.1002/adfm.202010695 common Peltier measurement techniques. Third, we discuss

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Figure 1. The development of TE material for Peltier cooling. Peltier refrigeration was first realized in inorganic TE materials and undergone a change
from bulk material to flexible film.[7,8] Images reproduced with permission from Ref. [8c,d]. Copyright 2014, Wiley-VCH.[8c] Copyright 2011, Nature Pub-
lishing Group.[8d] In terms of organics, Peltier devices based on PPy was developed in 2005 but it exhibited a weak and unstable cooling signal.
Reproduced with permission.[9] Copyright 2005, Elsevier. In 2012, Zhu et al. fabricated a thermoelectric module by combining n-type poly[Nax(Ni-ett)]
and p-type poly[Cux(Ni-ett)]. Reproduced with permission.[10] Copyright 2012, Wiley-VCH. Recently, advanced measurement techniques and device struc-
ture design realized the observation of single molecular Peltier effect in molecular-metal junction or the separation of Peltier cooling in poly(Ni-ett),
which deepen basic understanding of Peltier effect in organics and provide new possibilities for flexible refrigeration. Images reproduced with permis-
sion.[11] Copyright 2018, Nature Publishing Group.[11a] Copyright 2018, Nature Publishing Group.[11b]

the development of TE materials which have been applied in The Peltier coefficients of n-type material are negative, whereas
flexible TECs, including organics and inorganics to offer a dis- those of p-type materials are positive. Moreover, the magni-
tinct map of the development status. Then, optimizing strate- tude of Π is extremely dependent on the doping level of the
gies for state-of-the-art thermoelectric materials and Peltier materials. As the doping level increases, the Fermi level is
devices are presented. Last, we propose our perspectives to approaching closer to the valence/conduction band, leading to
stimulate more research interests in this emerging area. a stronger p-type/n-type doping and a smaller absolute value of
the Peltier coefficient.
Conventional Peltier coolers consist of unipolar p- or n-type
2. Mechanism and Basic Parameters thermoelements (Figure 2a). Each TE couple is arranged elec-
trically in series and thermally in parallel. When an electric bias
2.1. Mechanism of the Peltier Effect is applied, the carriers move between near-equilibrium distribu-
tions on either side of each semiconductor/metal junction and
The Peltier effect was named after a French physicist, J.C.A. exchange heat energy with the lattice (Figure 2b). The absorbed/
Peltier, who observed heating or cooling at a junction of two released energy at junctions almost entirely arises from the
different conductors when the current was applied.[13] This transport of majority carriers (holes for p-type materials, elec-
phenomenon comes from the variation in the average energy trons for n-type materials), whereas that of the minority carriers
of carriers between different materials. When transitioning is negligible. Since holes and electrons have opposite charges,
between materials, carriers compensate for the energy differ- the fabrication of TE modules with π-shaped p-n legs will pro-
ence by exchanging heat energy with the surrounding lattice. mote the overall heat flux achieved from one side to the other.
The amount of energy transported per unit carrier is reflected In contrast to conventional Peltier coolers, the minority car-
by the Peltier coefficient.[14] For a semiconductor whose carriers riers of bipolar Peltier devices play a crucial role in current
follow the Fermi–Dirac distribution function (feq), the Peltier and heat flow.[15] In this case, the p- and n-type semiconduc-
coefficient can be expressed by Equation (1). tors are directly connected to form a p-n junction (Figure 2c,d).
When no voltage is applied, there is a large built-in potential
 ∂f  opposing the flow of both holes and electrons across the junc-
∫ σ (E )(E − E F ) − eq  dE
 ∂E  tion. A suitable positive voltage could reduce the potential bar-
Π= (1)
 ∂f  rier and supply free electrons and holes. Subsequently, carriers
q ∫ σ (E ) − eq  dE that diffuse against the built-in potential will remove energy
 ∂E 
from the lattice, leading to Peltier cooling at the p-n inter-
where q is the unit charge, EF is the Fermi energy, and σ(E) face.[16] Notably, the effective Peltier coefficients for both p- and
is the contribution of the conductivity of a carrier at energy E. n-type semiconductor are bias-dependent. As the bias voltage

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Figure 2. Schematic diagram of the Peltier effect. a) Structure diagram and b) band structure of conventional Peltier device. c) Structure diagram and
d) band structure of bipolar Peltier devices.

increases, additional minority carriers are injected and the dis- thermoelements, electrical resistivity (ρ) or thermal conduc-
tance between the quasi-Fermi level and band edge decreases, tivity (κ) of the TE material, which can be written as:
which contributes to a smaller Peltier coefficient.[14]
ln l
R= ρn + P ρ p (4)
An Ap
2.2. Basic Parameters of Peltier Devices
An A
Considering that p-n bipolar device is difficult to implement K= κn + p κ p (5)
ln lP
practical external cooling application, the performance of the
Peltier cooler was analyzed based on the conventional device When the TE module is at zero heat load (Qc = 0), the max-
architecture. Cooling capacity (Qc), temperature difference (ΔT), imum temperature difference (ΔTmax) between the cold and hot
heat flux density (q), and coefficient of performance (COP) are sides can be obtained as follows:
four commonly used parameters for performance evaluation.
As current flows through the thermocouple, heat is pumped 1 (6)
∆ Tmax = ZDTc2
from one side to the other. The heat absorbed or released per 2
unit time is equivalent to the following:
The maximum cooling capacity (Qc,max) is specified at ΔT = 0
dQ /dt = Πnp I (2) and expressed as:
2
where Πnp is the Peltier coefficient of the module SnpTc2 (7)
Q c ,max =
(Πnp = Πp − Πn) and I is the electric current. 2R
However, apart from Peltier cooling, heat sources such as
Joule heating (Q J = 0.5 I2 R) and heat conduction (Q J = K(Th − Tc)) where Snp is the Seebeck coefficient of the module
are non-negligible during the heat pumping process.[12c] (Snp = Sp − Sn).
Therefore, the energy balance equation at the cooling side can The heat flux density (q), which is calculated from the
be represented as follows: cooling power per unit area, is another essential parameter
because high-heat-flux cooling devices are urgently desirable in
Q c = Πnp I − 0.5 I 2R − K (Th − Tc ) (3) the thermal management of high-power electronic devices. The
formulation of qmax can be written as:
where R and K are the electrical resistance and thermal
1  1 2 2  
 SnpTc / ρ  − [K (Th − TC )]
conductance of the TE module, respectively. They are closely qmax = (8)
related to the length (l) and cross-sectional area (A) of the l   2  

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According to Equation (8), qmax can be improved by opti- desirable thermoelectric materials should have a high Seebeck
mizing the performance of the TE material or reducing the coefficient, high electrical conductivity but low thermal conduc-
length of the thermoelements. tivity toward achieving a higher ZMT of the thermocouple.
As for the cooling efficiency, the input power (P) of the Pel-
tier device is not only consumed by Joule heating, but also used
to overcome the Seebeck voltage resulting from the tempera- 3. Measurement Techniques
ture difference between the two sides of the thermocouple. The
input power is given by: The Peltier effect describes the process of absorbing or releasing
heat; hence, accurate temperature measurement is crucial for
P = Snp (Th − Tc ) I + I 2R (9) reliably evaluating the device performance. However, Joule
heating also occurs as charge carriers dissipate energy within
Therefore, the COP can be obtained from Equations (3) and (9): the lattice and contributes to the temperature change in the Pel-
tier device. As a result, the coupling of thermal signals makes it
Q ΠnpI − 0.5 I 2R − K (Th − Tc ) extremely challenging to separate that caused by Peltier effect.
COP = = (10)
P Snp (Th − Tc ) I + I 2R To resolve the aforementioned limitations, several high-preci-
sion contact/non-contact temperature measurement techniques
For a given (Th − Tc), the COP varies with the applied cur- along with the frequency-resolved method have been employed
rents. Solving the equation dCOP/dI = 0, the optimum current for Peltier cooling characterization, which will be introduced in
(Icop) for maximum COP can be expressed as: the following section.
(Sn − SP )(Th − Tc )
I cop = (11)
R  1 + ZMT − 1 3.1. Contact Temperature Measurements

The maximum COP is given by: Contact temperature measurement involves sensors that are in
physical contact with the object and utilize heat conduction to
Th monitor the temperature changes. Thermocouples are the most
1 + ZMT −
Tc Tc (12) widely used contact thermometers owning to their low cost
COPmax = ×
Th − Tc 1 + ZMT + 1 and high accuracy. A thermocouple consists of two different
metals with a large difference in the Seebeck coefficient. When
where ZM T is the figure-of-merit of the TE module, which can a temperature difference (ΔT) exists at the metal junction with
be written as: respect to the reference temperature (T0), an open circuit poten-
tial V = (Smetal1−Smetal2) ΔT is detected and then could be con-
2
SnpT verted to sample temperature. Wees et al. employed a NiCu/Au
ZMT = (13)
KR thermocouple junction (SNiCu≈ 30 μV K–1 and SAu≈ 2 μV K–1)
to investigate the Peltier effect of the graphene-metal junction
According to Equation (12), a flexible TE module with high (Figure 3a).[17] This sensitive thermometry can reflect the tem-
ZMT is beneficial for high cooling efficiency. For example, the perature changes in the mK magnitude. Furthermore, when a
COP is significantly improved from 0.05 to 0.4 when ZMT low frequency AC current is introduced to generate Peltier sig-
changes from 0.5 to 1 with fixed cold and hot side temperatures nals at the junction and a lock-in technique is used to measure
of 250 and 300 K, respectively. Furthermore, the efficiency of the thermocouple voltage, the Peltier (∝I) and Joule heating
flexible Peltier coolers could even be comparable with home (∝I2) effects could be distinguished by separating the first har-
refrigeration once their ZMT values increase to 4,[12c] but dis- monic response to the heat modulation at the junction. How-
couragingly, it remains a formidable challenge and is hard to ever, despite the high sensitivity and applicability for extracting
see how such a high ZMT can be realized in the foreseeable temperature values from miniature devices, thermocouple fails
future. Therefore, thermoelectric cooling should be regard as to realize thermal imaging.
a complementary technique for specialized application such as Scanning thermal microscopy (SThM) is another contact
small-scale cooling and hot-spot cooling, rather than a compet- temperature measurement technique and can generate a
itor to the conventional methods. In spite of this, great efforts thermal map with a high spatial resolution of 0.3–0.5 µm by
have been devoted to improve the ZMT of the thermocouple. integrating a small thermocouple on the tips of the atomic force
According to Equations (4) and (5), ignoring the metallic con- microscope (AFM).[18] When the tip is brought into contact
nections and interfacial resistance, ZMT could be calculated with the surface, the resistance of the thermistor will change
from the properties of TE materials. For a single component as a function of temperature. However, in previous studies,
material, the TE properties can be evaluated in terms of ZT: the thermal contact resistance between the sample and tip
(Rts) would significantly reduce the measurement accuracy and
S 2σ inevitably leads to systematic errors. Furthermore, Rts not only
ZT = T (14)
K varies with the contact area of the tip and sample, but is also
influenced by different tribological effects when the sample
where S, σ, and κ are the Seebeck coefficient, electrical con- changes. To address this issue, Gotsmann et al. extracted Rts
ductivity, and thermal conductivity, respectively. Therefore, from the ratio of the temperature senor to the measured heat

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Figure 3. Temperature measurement techniques of Peltier device. a) Illustration of temperature measurement of Au/NiCu thermocouple. Reproduced
with permission.[17] Copyright 2016, Nature Publishing Group. b) Illustration of temperature measurement by SThM. The insert figure is instantaneous
Peltier and Joule induced temperature distributions. Reproduced with permission.[19] Copyright 2016, Nature Publishing Group. c) Illustration of ther-
moreflectance for Peltier effect measurements. d) Illustration of LIT for Peltier effect measurements. Reproduced with permission.[24] Copyright 2018,
Nature Publishing Group.

flux then corrected the temperature map.[19] As shown in microscopy to characterize the cooling performance of inte-
Figure 3b, the instantaneous Peltier and Joule distributions of grated µ-TECs.[21] When an electric current of 21 mA was
nanowires, which eliminated the false signals caused by rough applied, a significant cooling effect was observed from the
surfaces or different material compositions, were obtained thermal image and ΔT attained to 4 K. Upon switching the cur-
from the improved SThM. In most cases, SThM is satisfactory rent direction, the top side was heated with a ΔT of 3 K. Notably,
for macroscale thermometry. However, the limitations such as the data were extracted from the smooth area of n-type BiTeSe
high cost, limited device size, considerable acquisition time legs because the thermoreflectance measurement is sensitive to
for thermal images, and complex temperature calibration pro- the surface roughness.
cesses must be considered for practical applications.[20] As for IR thermography, the detection mechanism is funda-
mentally different from the previous one. IR thermography is
based on Planck’s law—the radiation intensity emitted by the
3.2. Non-Contact Temperature Measurements object surface is temperature dependent at a specific wave-
length, which can be translated into the absolute temperature.
Thermoreflectance microscopy and IR thermography are non- However, the Planck’s law for specific objects needs to be scaled
contact temperature measurement techniques with advantages by emissivity because few objects are true blackbodies.[18] The
of being nondestructive, full-filed and real-time. Thermoreflec- application of IR thermography is classified into passive or
tance microscopy provides thermal images by analyzing the active methods. In the passive IR test, the object is characterized
surface reflectivity of the sample. The temperature variation by its naturally emitted temperature field without an external
(ΔT) can be extracted from the reflectivity change (ΔR), which heat source.[22] However, it is unable to produce frequency-
can be expressed as: dependent signals and thus can hardly meet the requirements
of Peltier cooling and Joule heating separation. Active infrared
∆T = ∆R / (R0C th ) (15) thermography, such as lock-in thermography (LIT), is more
popular for analyzing the heat sources in the Peltier devices.[23]
where Cth is the thermoreflectance coefficient of the surface Saitoh et al. directly observed the anisotropic magneto-Peltier
material and R0 is the reflectivity at reference temperature (T0) effect in nickel using this method.[24] During the experiment,
(Figure 3c). In principle, Cth must be calibrated with reference a periodic rectangular AC current was applied. Joule heating is
samples such as Au surfaces to promote the reliability and accu- not influenced by current direction (∝I2) and remains constant,
racy of the result. Nielsch et al. conducted thermoreflectance whereas the temperature modulation induced by Peltier effect

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oscillates with f. The thermal images oscillating with the same of wrinkles is beneficial for reducing the thermal conductivity
frequency as the perturbation were extracted and then trans- by less than 50%.[28] In addition, the existence of structural
formed into the lock-in amplitude and phase images by Fou- defects,[29] carbon isotopes,[30] and domain boundaries[31] will
rier analysis. Subsequently, the separated Peltier signal can be also contribute to lower thermal conductivity and improved ZT
obtained from the phase image (Figure 3d). By this way, LIT value to promote practical refrigeration applications. Although
enables visualizing the spatial distribution of temperature mod- majority of the current Peltier devices based on graphene are
ulation with high temperatures (< 0.1 mK) and spatial resolu- fabricated on glass or silicon substrates, the mechanical flexi-
tions (3–5 µm, determined by the wavelength of the detected bility and potentially high TE performance render them capable
light). of achieving flexible cooling.
Additionally, flexible inorganic Peltier cooling greatly ben-
efits from the unrivaled combination of device physics and
4. Development of Thermoelectric Materials mechanics. For example, vapor deposition or inkjet printing
of inorganics on soft polymeric or plastic substrates are prev-
The exploration of state-of-the-art TE materials is essential for alent methods. In these cases, polyimide (PI) is a commonly
achieving high-performance flexible Peltier cooling devices used substrate because of its low thermal conductivity, high
(Figure 1). One effective strategy is developing 2D inorganic TE mechanical performance, and excellent tensile strength. Based
materials such as graphene, which can be efficiently exfoliated on this polymer substrate, Rowe et al. fabricated a microcooler
and dispersed in solvents to form flexible TE films. In addition, with vacuum-deposited p-type Sb2Te3 and n-type Bi2Te3.[8a]
the deposition of inorganic TE thin films on flexible substrates When a current of 4 mA was supplied, the temperature differ-
is also widely employed to enhance flexibility. Another poten- ence reaches ≈4 K under vacuum. Hng et al. also synthesized
tial method is utilizing intrinsic flexible OTE materials, which p-type Sb1.5Bi0.5Te3 and n-type Bi2Te2.7Se0.3 nanoparticles and
have advantages of low toxicity, low cost and easy synthesis for printed them on a PI substrate.[8c] The flexible device consisted
industrial applications. Although their relatively poor electric of three pairs of p-n legs and supplied steady state cooling when
transport properties may partly limit practical application in the electric voltage was 1.5 V. However, because of the limited
Peltier cooling, the properties could be improved by enhancing tolerance temperature of the flexible organic substrates, high-
the film crystallinity and efficient doping process. In the fol- temperature deposited techniques or annealing is not suitable
lowing section, the recent progresses on flexible Peltier devices in these cases. For example, zinc antimonide film must be
based on inorganic and organic thermoelectric materials are annealed at 325 °C to improve the TE performance, whereas
highlighted and discussed. PI degrades when exposed to such high temperatures for pro-
longed periods.[32]
Furthermore, many inorganic TE materials exhibit high
4.1. Inorganic Flexible Thermoelectric Thin-Film Materials ZT at room temperature and excellent bendability, indicating
their great potential in cooling application. An example is
Although the Peltier effect was discovered in 1834, the first Pel- CuI thin film, which is generally fabricated on a flexible PET
tier device was not realized until 1954. Many inorganics with substrate,[33] shows a high ZT value of 0.21 at 300 K via opti-
high ZT values at medium and high temperature regions have mizing the sputtering rate of iodide. In addition, the rapid
been developed over past decades, but the progress in low- development of medium- and high-temperature inorganic flex-
temperature and room-temperature inorganic materials for TE ible TE materials, such as silver chalcogenide Ag2X (X = S, Se,
cooling is still unsatisfactory. Bi2Se0.3Te2.7,[25] Bi0.5Sb1.5Te3,[26] Te), carbon-nanotube-based composites, ternary cobalt oxides
and Bi2Te3/Sb2Te3 superlattices[8b] exhibit a high ZT (>1) at (Ca3Co4O9), or ZnO based on mica substrate, is also significant
room temperature and are considered as promising candidates to the advances of flexible TE cooling.[34]
for Peltier devices. However, the inherent rigidity and brittle-
ness of inorganic TE materials restrict their applicability to
flexible cooling. Therefore, great efforts have been devoted to 4.2. OTE Materials
the search for flexibility in state-of-the-art low-temperature and
room-temperature inorganic thermoelectric materials. Different from strong covalent or ionic bonds in inorganics,
2D inorganic materials such as graphene have great potential OTE materials form regular and tight packing between neigh-
for flexible Peltier cooling due to their outstanding mechanical boring molecules with relatively weak non-covalent bonds,
flexibility and favorable combination of electrical and thermal such as van der Waals forces, hydrogen bonds, and π–π inter-
transport properties. Wees et al. observed a ΔT of 15 mK at actions, which endow the materials with excellent flexibility.
the Au-graphene-Au junction when the applied current was Furthermore, considering the favorable features of low thermal
20 µA.[17] The direct measurement of the Peltier effect in gra- conductivity, light weight, and solution processability, OTE are
phene provides a complementary method for comprehending desirable for flexible cooling applications. Over the past few
the nanoscale thermoelectric transport of 2D materials. More years, a series of conductive polymers such as PEDOT:PSS and
recently, Di et al. combined graphene wrinkles with nanobubble poly[Kx(Ni-ett)] have been employed to develop organic flexible
engineering and demonstrated a remarkably enhanced Peltier TE devices, demonstrating their great potential in power gen-
effect with improved current density.[27] It is worth noting that eration.[10,35] Whereas, studies in organic Peltier cooling are still
the overall ZT value of graphene is generally quite low due in their infancy with limited progresses (Figure 3). In 2005, Hu
to its ultrahigh thermal conductivity. However, the introduction et al. tried to demonstrate the organic Peltier device based on

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polypyrrole (PPy).[9] Given the unstable electrical properties and (μcal < E < μcal + e|Vp|), as well as in a small range of energies
poor thermal insulation between the two sides of the device, (E) above the chemical potential of the probe (E > μcal + e|Vp|)
the temperature difference of the device gradually decreased or below the chemical potential of the calorimeter (E < μcal).
to zero in ambient environment. In 2012, Zhu et al. fabricated In this HOMO-dominated junction, an appropriate negative
a thermoelectric module by combining n-type poly[Nax(Ni-ett)] bias caused electrons to flow below the chemical potential of
and p-type poly[Cux(Ni-ett)].[10] However, due to the fast heat the calorimeter, causing cooling and heating in the calorim-
dissipation into the ambient environment, the TE module dis- eter (E − μcal) and the probe (μcal + e|Vp|−E), respectively. The
play negligible cooling effect. In spite of these initial studies, experimental results showed the expected heating or cooling
the Peltier effect in organic materials are poorly understood of the calorimeter when the voltage was applied in the probe
and their potential in flexible cooling applications has not been shifted from +VP to −VP (Figure 4d,e). Similar results were
demonstrated successfully. observed in the lowest unoccupied molecular orbital (LUMO)-
Experimental observations of the Peltier effect in organic dominated Au−4,4′-bipyridine (BP)–Au molecular junctions (n-
molecular junctions are crucial for understanding the elec- type) (Figure 4c). In this case, a positive bias contributes to net
trical, thermoelectric, and energy dissipation characteristics at cooling in the calorimeter. However, due to the relatively small
the molecular scale. However, the low Π of molecular junction Seebeck coefficient (−6.9 ± 0.4 μV K–1), Peltier cooling was only
and picowatt-level cooling signal lead to technical challenges in detected in a narrow range of positive voltages (Figure 4f).
their detection. Reddy et al. developed an experimental platform In previous reports, majority of the studies on OTE cooling
by integrating conducting-probe AFM with custom-fabricated failed to precisely extract the Peltier signal and quantitatively
calorimetric microdevices, enabling probing of molecular- study the cooling effect because severe Joule heating effect
scale refrigeration.[11a] For highest occupied molecular orbital induced by the relatively low electrical conductivity of OTE
(HOMO)-dominated Au–biphenyl-4,4′-dithiol (BPDT)–Au junc- materials. Besides, internal heat conduction and various heat
tions (p-type), as the probe was applied with a negative bias (−Vp), dissipation processes also significantly influence tempera-
electrons are injected into the electrode at an energy of μcal + e|Vp| ture distribution, thus making studies on the Peltier effect in
(μcal is the chemical potential of the calorimeter electrode, e is organics particularly challenging. To address this problem,
the elementary charge) and leave the calorimeter electrode at Zhu et al. employed a parylene-based suspended device and a
an energy of μcal (Figure 4a,b). Owing to the thermal broad- high vacuum degree of 6 × 10−4 Pa to minimize heat dissipa-
ening of the Fermi–Dirac functions, charge transfer occurs at tion (Figure 5a).[11b] In addition, utilizing difference of the func-
the energies between the chemical potentials of the electrodes tion relationships between Peltier or Joule effect with current,

Figure 4. Peltier effect in molecular junctions. a) A schematic illustration of the AFM-based platform for probing Peltier effect. Mechanism of the origin
of the Peltier effect in a molecular junction in which transport is dominated by the b) HOMO and c) LUMO. d) The heating and cooling power in
Au–BPDT–Au junctions. Voltage-dependent thermal power for e) Au–BPDT–Au and f) Au–BP–Au junctions. Reproduced with permission.[11a] Copyright
2018, Nature Publishing Group.

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Figure 5. Peltier effect in poly(Ni-ett) thin films. a) A schematic illustration of poly(Ni-ett) Peltier device on the suspended perylene film. b) The mecha-
nism for separating the Peltier cooling and Joule heating by a rectangular alternating current. c) Temperature distribution of the poly(Ni-ett) device and
the separate contributions of Peltier cooling and Joule heating. The temperature distribution induced by Peltier effect with various current densities at
d) 0.01 s and e) 3 s. f) Current-density-dependent temperature differences at the two contacts of the device. Reproduced with permission.[11b] Copyright
2018, Nature Publishing Group.

an alternating current bias with rectangular wave modulation and leg spacing. Besides, some novel cooling mechanisms such
was used to extract the Peltier effect signal (Figure 5b,c). On this as the Thomson effect provide new insights into enhancing the
basis, the experimental results from transient IR characteriza- cooling performance.
tion clearly revealed the Peltier-effect-induced temperature dis-
tribution in a poly(Ni-ett) device. As shown in Figure 5d, a slight
temperature change of < 0.1 K was measured at 0.01 s near the 5.1. Developing Low-Dimensional Materials
semiconductor/metal junction when the applied current density
was 0.3 A mm−2. As the operating time continued to increase, Dimensionality is essential for controlling the properties of
the internal heat conduction contributed to the diffusion of materials. For 3D TE candidates, three TE parameters of ZT are
heating or cooling energy into the central part of the film and strongly coupled and mutually contra-indicated. S is inversely
achieved a thermal balance with the Peltier effect less than 3 s proportional to σ, which in turn is related to the electronic
(Figure 5e). Furthermore, in real-time measurements, an unex- thermal conductivity (κe) via the Wiedemann–Franz law, thus
pected ΔT of ≈40 K was observed when a large current density making it particularly challenging to optimize ZT value.[36]
of 5 A mm−2 was applied (Figure 5f), suggesting that OTE mate- However, this scenario is quite different in low-dimensional
rials are promising candidates for flexible cooling devices. materials. With reduced dimensionality, the motion of carriers
is restricted in a certain direction and the electronic spectrum
drastically changes. These so-called quantum confinement effect
5. Optimizing Strategy is beneficial for a great enhancement in ZT.[37] The improve-
ment mainly originated from two aspects: 1) the enhanced den-
Practical flexible cooling applications put forward urgent sity of states (DOS) near EF leads to an increase in S; 2) a strong
requirements of state-of-the-art TE materials with high ZT and modification of phonon group velocities, a significant enhance-
rational designs of the device structure. To achieve high-perfor- ment in the phonon relaxation rate together with increased
mance TE materials, dimensionality reduction provides an possibility of phonons scattering at the interface reduce the
effective route due to the decoupling of three TE parameters by lattice thermal conductivity. For the past two decades, excep-
enhancing S and reducing κ, without significantly impacting σ. tionally high ZT values in low-dimensional materials such as
In addition, considering the cooling features of flexible Peltier quantum well superlattices (2D) and nanowires (1D) have been
devices, OTE materials are outstanding candidates for low-tem- demonstrated. In addition, coupled quantum dots (0D) are also
perature TE applications because some of them could maintain promising because they provide adequate conduction paths for
high performance at ultra-low temperature. In terms of the carriers but less effective heat conduction paths for phonons.
device design, current strategies focus on decreasing the elec- Hicks et al. prepared Pb1−xEuxTe/PbTe quantum well
trical and thermal contact resistance, regulating leg geometries superlattices with varying thicknesses.[38] As the thickness of

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Figure 6. Quantum size effects on TE performance of inorganics. a) DOS for a 2D quantum well. Reproduced with permission.[38] Copyright 2016,
Nature Publishing Group. b) S2n of PbTe/Pb0.927Eu0.073Te quantum wells as a function of well thickness at 300 K. Reproduced with permission.[39]
Copyright 1996, American Physical Society. c) Thermal conductivity of GaAs/AlAs superlattices as a function of the layer thickness at 300 K. Reproduced
with permission.[38] Copyright 2016, Nature Publishing Group. d) The heterojunction band diagram for Bi2Te3/Sb2Te3 superlattice. e) Transmission
electron micrograph of a Bi2Te3/Sb2Te3 (10 Å/50 Å) superlattice. f) Potential COP as a function of ZT with various material size. Reproduced with
permission.[8b] Copyright 2001, Nature Publishing Group.

the material decreased to nanometers, the DOS of the quantum promoting a high conductivity of 790 S cm–1. Besides, the cou-
wells changed to a step function and the steps occurred at the pling between inorganic and organic parts has an negative
energy of each quantized level (Figure 6a).[37b] Meanwhile, as influence on phonon transport in the in-plane direction; thus, a
the well thickness decreased from 55 to 17 Å, S2n increased low total κ of 0.45 W m–1 K–1 was achieved in the hybrid superla-
exponentially and the maximum value nearly triple that of ttice, which is approximately one-sixth that of TiS2 single crystal
bulk PbTe (Figure 6b). As for thermal conductivity, Chen et al. (Figure 7c). As a result, the ZT of TiS2[(HA)0.08(H2O)0.22(DMSO)0.03]
observed a significant reduction in the κ of GaAs/AlAs super- can reach up to 0.28 at 373 K (Figure 7d). Noteworthy, these
lattices (Figure 6c).[38] Notably, the partially specular or dif- hybrid inorganic/organic superlattices also exhibited excellent
fuse interface scattering model demonstrated good agreement flexibility, indicating great potential in flexible modules.
with the experimental data of κ, indicating that the interfacial
phonon scattering by atomic scale interface roughness in super-
lattices also contribute to decreased thermal conductivity.[40] 5.2. Enabling High Performance at Low Temperatures
Venkatasubramanian et al. further confirmed a large enhance-
ment of ZT in p-type Bi2Te3/Sb2Te3 superlattice (Figure 6d,e).[8b] In most cases, flexible Peltier devices have to operate below
Owing to the high Seebeck coefficient of ≈238 μV K–1 and ambient temperatures owing to the cooling effect. Therefore,
ultra-low lattice thermal conductivity of 0.22 W m–1 K–1, candidate materials that can function well at low temperature
the ZT reached 2.4 at room temperature. Furthermore, the fab- are highly desirable for TE cooling.[42] However, it is extremely
ricated Peltier device exhibited a significant cooling ability of challenging to search for promising low-temperature TE mate-
30 K at 300 K (Figure 6f), demonstrating that low-dimensional rials.[43] Although considerable progress has been made in the
materials have great potential for cooling applications. ZT enhancement of inorganics, majority of them only exhibit
Similar with inorganics, a low-dimensional structure in optimal TE performance at a relatively narrow range of high
hybrid inorganic/organic is also regarded as an effective temperatures (>500 K). Besides, strategies such as band engi-
strategy to enhance ZT. Koumoto et al. prepared a hybrid neering for inorganic materials to enhance ZT of medium- and
superlattice by intercalating hexylamine (HA) molecules into high-temperature may be not appropriate at low temperatures.
titanium disulfide (TiS2) layers.[41] The electrochemical interca- Instead, OTE materials could potentially contribute to attaining
lation and solvent exchange process enabled a stable structure this goal. The optimum TE performance of organic materials
with HA, which was confined within a narrower space of inor- usually achieves at room temperature and some of them can
ganic layers (Figure 7a,b). After intercalation, the carrier density even be well maintained at ultra-low temperatures through rea-
of the hybrid material increased from 3.4 × 1020 to 7.59 × 1020 cm–3, sonable molecular design.[44]

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Figure 7. a) A schematic diagram of TiS2 based hybrid superlattice. b) HAADF-STEM images of the layered structure. Temperature dependent c) κ and
d) ZT value of TiS2 single crystal and its hybrid superlattice. Reproduced with permission.[41] Copyright 2015, Nature Publishing Group.

Pflaum et al. synthesized DCNQI2Cu and TTF-I3, and meas- in DCNQI2Cu than that of TTF-I3 (WTTF−I3 = 632 meV).
ured the temperature-dependent TE properties (Figure 8a,b).[45] Besides, for TTF-I3, the electronic thermal conductivity (κe)
The electrical resistivity of both materials declines rapidly with can be estimated via Wiedemann–Franz law κe = σL0T, where
temperature, exhibiting strong temperature dependence and L0 is the Lorenz number and T is the operating temperature.
correlating with typical low-dimensional organic metals. Notably, The difference between κ and κe is a temperature-independent
the phonon drag effect enabled a smaller slope of the temper- parameter (κph) caused by heat-carrying phonons. However,
ature-dependent Seebeck cofficient (WDCNQI2Cu = 333 meV) a weaker temperature dependence of κ was observed for

Figure 8. Low temperature TE performance of TTF2-I3 and DCNQI2Cu. Crystal structure of a) TTF2-I3 (top) and b) DCNQI2Cu (below). Temperature
dependent c) ρ, S, ĸ and d) PF, ZT of TTF2-I3 (yellow) and DCNQI2Cu (blue). Reproduced with permission.[45] Copyright 2017, Wiley-VCH.

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DCNQI2Cu than that expected from the Wiedemann–Franz computational results indicate that the introduction of Rth and
law, which resulted from different relaxation times for thermal Rele result in an elevated hot spot temperature in the TE module,
and electric field perturbations of the electronic system. There- so a large thermal energy loss at the interface and deterioration
fore, combined the high Seebeck and low κ at low tempera- of the cooling performance are observed (Figure 9b). This is due
ture, DCNQI2Cu exhibits particularly high PF and ZT ≥ 0.15 to the fact that Peltier cooling occurs at the interface, whereas the
(< 40 K) (Figure 8c). However, considering the brittleness of existence of Rth and Rele increases the unwanted Joule heating
organic crystals, promising crystal growth techniques on flex- and reduces the heat conduction of solid bodies in thermal con-
ible substrates or transfer strategies enabling the separation of tact.[48] Therefore, lowering the contact resistance is significant
substrate and crystals are indispensable for achieving their full for optimizing the cooling performance especially in flexible
potential in low-temperature flexible cooling devices.[46] cooling applications, where severe deformation of the Peltier
device might induce poorer connections at various interfaces.
Kumar et al. attempted to determine the appropriate range
5.3. Minimizing Thermal and Electrical Contact Resistances of Rth and Rele for the cooling effect by measuring the max-
imum temperature drop at a hot spot with different contact
When two solid bodies come in contact, the thermal and elec- resistances (Figure 9c,d).[48] As Rth increased from 1 × 10−6 to
trical contact resistances (Rth and Rele) account for the tem- 7.5 × 10−6 m2 K W–1, ΔTmax suffered from a sharp decline from
perature drop at the interfaces and increment of the total 6.5 to 1 K, whereas the declining trend reduced as Rth increased
electric resistances (Figure 9a).[47] Both the experimental and from 1 × 10−7 to 1 × 10−6 m2 K W–1. This indicates that the

Figure 9. Electrical and thermal contact resistances in Peltier device. a) Schematic of a realistic single thermocouple Peltier module with electrical
and thermal contact resistances. b) Experimental and computation result of hot-spot temperature at the bottom surface of the chip. ΔTmax of hot spot
as a function of c) thermal contact resistances or d) electric contact resistances. Reproduced with permission.[47] Copyright 2011, IEEE. e) Schematic
illustrating the wearable TEC placed on human skin. f) The effect of TE parameters on cooling behavior of Peltier device. Reproduced with permis-
sion.[5] Copyright 2019, Nature Publishing Group.

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maximum desirable value of Rth is < 1 × 10−7 m2 K W–1. Simi- As expected, the lowest ZT resulted in a minimum cooling
larly, an acceptable Rele value of < 10–11 Ω m2 can be obtained capacity. Nevertheless, ZT is not a decisive parameter. TEC 4,
due to the slight improvement in ΔT as Rele decreases from 10–11 which exhibited a high ZT by lowering the thermal conductivity,
to 10–12 Ω m2. To achieve this goal, the contact surface should generated a much higher cooling performance than the others
be perfectly clean and smooth, without oxides and impurities. (Figure 9f). However, as h increased to 1000 W m−2 K−1, which
In addition, reducing the distance between the contact mem- means a lower external Rth, TEC with a high ZT by improving
bers and increasing the contact area will also make a difference. Seebeck coefficient exhibits much better performance. There-
For a typical TEC module, thermoelectric interface materials fore, the values of the three parameters of ZT should be taken
(TEiM) are beneficial to reduce the thermal and electrical con- into consideration according to the variation external thermal
tact resistivity, maintaining low energy loss transport of heat resistance.
and electricity between electrode and TE material. To meet the
requirements, a proper TEiM should have matched the coeffi-
cient of thermal expansion and work function with TE mate- 5.4. Tuning Geometries and Spacing of the TE Legs
rial.[49] Generally, Transition metals such as Fe, NiFe, and Ti
alloy are good choices for TEiM in TE devices. Despite these The cooling performance of a flexible Peltier device is also
progresses, interface materials for organic materials have not closely related to the geometries and spacing of the legs. The
been investigated in a systematic way and deserve focus atten- aspect ratio (AR) and fill factor (FF, the amount of space in a
tion in the future. Peltier module taken up by thermoelectric elements) are typical
However, with the exception of the internal contact resistance, dimensionless parameters to describe leg features (Figure 10a),
the external Rth, which is induced by the thermal conductivity of which can be expressed by
the object to be cooled, also presents a fundamental challenge
to cooling efficiency (Figure 9e). Priya et al. designed four TEC l
AR = (16)
modules with same dimensions and employed them to cool w
human skin, which exhibited a large external Rth with a heat
transfer coefficient (h) of 20–100 W m−2 K−1 (R = 1/hA, where A Nw 2
FF = (17)
is the cross section of the TE leg).[5] TEC 1 was fabricated from A
TE materials with a low ZT value of 0.62 at 25 °C, whereas the
others had the same ZT value of 1.25, but varied in terms of where l and w are the leg length and leg width, respectively.
their Seebeck coefficients (TEC 2), conductivities (TEC 3), N is the total number of legs, and A is the module base area.
or thermal conductivities (TEC 4). In their experiment, the Increases in the AR are typically beneficial for suppressing the
source and sink were maintained at 22 and 27 °C, respectively. effect of contact resistance and acquiring a larger ΔT, but it will

Figure 10. The effect of device design on Peltier cooling performance. a) Schematic of AR and FF of TECs. b) Calculated cold-side temperature of the
wearable TECs at different FF and AR. c) Experimental cold side temperature and d) temperature difference of Peltier devices with a high-fill factor
(FF = 36% and AR = 1.0), low-fill factor (FF = 12% and AR = 1.0), ultra-low fill factor (FF = 5.2% and AR = 1.6). Reproduced with permission.[5] Copyright
2019, Nature Publishing Group.

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induce more Joule heating loss at the same time. A smaller FF, thermal conduction, Joule heating accumulated inside the sem-
which suggests that a limited number of TE legs comprise the iconductor and caused a higher temperature in the middle of
module, leads to less material consumption and allows a higher the TE leg. The Thomson heat can be described as β ddθξ , where θ
sustainable ΔTmax across the Peltier device, whereas a larger FF and ξ are the dimensionless temperature and distance, respec-
might promote a higher cooling capacity. In addition, external tively. A positive β resulted in an improved cooling power of
load resistance or external thermal resistance will also make a 5 ≈ 7% (Figure 11b). In contrast, a decline in the performance
difference on optimal AR and FF of device. The theoretical cal- was observed when β was negative (Figure 11c). This phenom-
culation is an effective strategy to determine the compromise enon became more evident as β increased. Therefore, if ther-
among multiple parameters and acquire optimal device design. moelectric materials with properly designed β are employed,
Priya et al. performed simulations of the TEC module for on- a higher cooling power can be obtained. Additionally, Snyder
body cooling applications.[5] Considering the high external et al. proposed a novel concept of “Thomson coolers”, which
resistance of the operating condition, the optimum cold-side had an exponentially rising Seebeck coefficient with increasing
temperature was achieved when FF was < 15% and AR was temperature.[53] They predicted that the Thomson cooler was
2.0 (Figure 10b), which was further confirmed by experimental able to exhibit twice the ΔTmax compared to the traditional Pel-
data. By testing different devices with various AR and FF, an tier device with the same ZT value.
ultra-low FF TEC (FF = 5.2%, AR = 2.0) device exhibited the
maximum temperature difference (Figure 10c,d).
6. Conclusions and Perspectives
5.5. Taking Advantage of the Thomson Effect Inorganic TE refrigeration has been commercialized in portable
refrigerators, space exploration, and power electronics. Over
The Thomson effect, which originates from the relationship the past decade, the explosive growth of wearable devices has
between the Seebeck and Peltier effect, describes the absorbed brought great opportunities for flexible Peltier cooling. In spite
or liberated heat (Q) of the conductor as the current (I) and of a few preliminary explorations, the development of thin-film
temperature gradient (ΔT) are applied to it simultaneously.[50] Peltier devices is still in infancy stage. Aiming at boosting their
It can be expressed as rapid development of in the future, the improvement in ZT of
TE materials are always of vital importance. From the viewpoint
dQ /d t = βI∆T (18) of cooling applications, the devices should focus on realizing
the high heat flux, large temperature difference, and low power
where β is the Thomson coefficient with a unit of V/K. When consumption (Figure 12). As for the mechanical property of
the current direction coincides with the temperature gradient materials and devices, reducing the thickness represents the
and the conductor absorbs heat, β is positive; otherwise, it is conventional method to improve the flexibility. The exploration
negative. Optimization of the material properties by taking the of novel way to manipulate the intrinsic flexibility will enable
Thomson effect into account is beneficial for improving cooling more fascinating applications in the future.
performance of Peltier devices.[51] A positive β will improve Peltier devices with high heat flux can alleviate the heat
cooling power because the Thomson effect causes heat absorp- dissipation problem of nonplanar and integrated electronic
tion on the Peltier cooling side and liberates heat on the hot devices. To meet the requirement, exploring high-performance
side. TE materials, particularly those with low thermal conductivity,
Lee et al. conducted numerical simulations of the commer- deserves focus attention. OTE materials are promising can-
cial thermoelectric module to reveal the effect of Thomson didates. However, owing to the anisotropic TE properties of
cooling or heating on its cooling performance.[52] Figure 11a OTE materials, the utilization of in-plane properties to con-
depicts the temperature distribution in the TE cooler when ΔT struct vertical structure devices is a favorable choice. In addi-
is 10 K. As a result of the large electrical resistance and low tion to high heat flux, maintaining the temperature difference

Figure 11. Cooling performance of Peltier device when taking Thomson effect into account. a) Illustration of thermoelectric module with Thomson
effect. Dimensionless temperature as a function of dimensionless distance as b) β > 0 and c) β < 0. Reproduced with permission.[52] Copyright 2013,
Elsevier.

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Figure 12. Strategies and prospects for high-performance flexible Peltier cooling devices.

between the hot and cold sides of Peltier devices is another offers more opportunities to achieve high-performance, low-
challenge. Except for the development of low thermal conduc- cost, and wearable Peltier devices in the near future.
tivity TE materials, increasing interest will be paid to modulate
the device geometry. At present, most Peltier devices possess
single-stage structure. Although the construction of multi- Acknowledgements
stage devices can overcome the limitation, it can be hardly
This research was financially supported by the National Key Research
achieved especially for OTE candidates. Low power consump- and Development Program of China (2017YFA0204700, 2018YF-
tion is significant for achieving wearable and portable personal E0200702) and the Key Research Program of Frontier Sciences of CAS
cooling. With this in mind, more attention should be not only (QYZDY-SSW-SLH024).
devoted to developing high performance TE materials with
superior electrical conductivity to suppress Joule heating, but
also to introducing adhesive layer with decreased electrical and Conflict of Interest
thermal contact resistance.
The authors declare no conflict of interest.
So far, the flexibility in Peltier devices are still far from sat-
isfactory. For inorganic TE materials, constructing ultrathin,
low-dimensional and amorphous candidates can promote the Keywords
mechanical properties and TE performance simultaneously.[54]
In addition, introducing nanostructure tailor to create a void device design, flexible thermoelectric cooling, inorganic thermoelectric
films, organic thermoelectric materials, peltier effect
space between the grains[55] or involving a carbon nanotube net-
work to guide the growth of layer-structured inorganic films[34b] Received: December 13, 2020
offers alternative way to fabricate freestanding films. Although Revised: January 22, 2021
OTE materials have been widely considered to possess good Published online: March 5, 2021
flexibility, more research attention will focus on fabricating
ultrathin, wearable, and stretchable devices toward a variety
of realistic applications. To satisfy the requirement of flexible
cooling device, searching for electrodes materials with high [1] F. Birol, International Energy Agency (www.iea.org) OECD/IEA
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Stretchable multilayer graphene/graphene scrolls[56] or organics [2] M. E. H. Tijani, J. C. H. Zeegers, A. T. A. M. d. Waele, Cryogenics
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Adv. Funct. Mater. 2021, 31, 2010695 2010695 (15 of 17) © 2021 Wiley-VCH GmbH
16163028, 2021, 20, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/adfm.202010695 by HONG KONG POLYTECHNIC UNIVERSITY HU NG HOM, Wiley Online Library on [08/01/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advancedsciencenews.com www.afm-journal.de

Jiamin Ding received her B.S. degree in chemistry from Lanzhou University in 2017. Currently, she
is pursuing her Ph.D. degree at the Institute of Chemistry, Chinese Academy of Sciences (ICCAS).
Her research interest is on organic thermoelectric materials and devices.

Wenrui Zhao received his B.S. degree in chemistry from Lanzhou University (2016). Since 2016, he has
been at the Key Laboratory of Organic Solids in ICCAS for a Ph.D. degree. His main research interest
focuses on organic transistors and organic thermoelectric devices.

Wenlong Jin received his B.S. degree in applied chemistry from East China University of Science and
Technology (2015). Then, he joined ICCAS and obtained his Ph.D. in 2020. His research focus is on
organic thermoelectric and Peltier devices.

Chong-An Di received his Ph.D. degree in Chemistry from ICCAS in 2008. He was appointed to the
associate professor position in 2010 and promoted to professor in 2016 at ICCAS. His research cur-
rently focuses on the investigation of organic thin-film transistors and organic thermoelectric devices.

Adv. Funct. Mater. 2021, 31, 2010695 2010695 (16 of 17) © 2021 Wiley-VCH GmbH
16163028, 2021, 20, Downloaded from https://onlinelibrary.wiley.com/doi/10.1002/adfm.202010695 by HONG KONG POLYTECHNIC UNIVERSITY HU NG HOM, Wiley Online Library on [08/01/2024]. See the Terms and Conditions (https://onlinelibrary.wiley.com/terms-and-conditions) on Wiley Online Library for rules of use; OA articles are governed by the applicable Creative Commons License
www.advancedsciencenews.com www.afm-journal.de

Daoben Zhu is a professor and director of the Organic Solids Laboratory in the Institute of
Chemistry, CAS. He finished his graduate courses at the East China University of Science and
Technology in 1968. He was selected as an academician of the CAS in 1997. His research interests
include molecular materials and devices.

Adv. Funct. Mater. 2021, 31, 2010695 2010695 (17 of 17) © 2021 Wiley-VCH GmbH

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