Vietnam Journal of Science and Technology 56 (1A) (2018) 1-13

THERMOELECTRIC MATERIALS: FUNDAMENTAL,

APPLICATIONS AND CHALLENGES

Bui Duc Long1, *, Duong Ngoc Binh1, Le Minh Hai1, Le Hong Thang2, Tran Duc Huy3
1
Department of Non-ferrous Metals and Composites, School of Materials Science and
Engineering, HUST, 1 Dai Co Viet, Ha Noi
2
Central Laboratory of Metals Technology, School of Materials Science and Engineering,
HUST, 1 Dai Co Viet, Ha Noi
3
Department of Materials and Foundry Technology,
School of Materials Science and Engineering, HUST, 1 Dai Co Viet, Ha Noi
*
Email: long.buiduc@hust.edu.vn

Received: 15 August 2017; Accepted for publication: 21 February 2018

ABSTRACT

Energy and the environment are popular themes in the 21st century because both are closely
interlinked. The current technologies are focusing on finding new, clean, safe and renewable
energy sources for a better environment. Thermoelectric (TE) materials are able to generate
electricity when applied a temperature different at a junction of two dissimilar materials. This is
a promising technology to directly convert waste heat into electricity without any gas emission,
thus providing one of the most clean and safe energy. However, the applications of TE devices
are still limited due to its low energy conversion efficiency and high material cost. As a result,
researches in TE materials are mainly focusing on the improving of efficiency and developing
cheap materials. In this paper, the fundamental, challenges and applications of thermoelectric
materials were reviewed. In addition, currently research in thermoelectric materials and
improving their efficiency will also be reviewed.

Keywords: thermoelectric materials, energy conversion, energy materials, and clean energy.

1. INTRODUCTION

The world projected population and rapid economic growth lead to dramatically increase
the demand for energy in the next decades [1]. According to the U.S Energy Information
Administration [2], total world energy consumption will be double rate from 2012 to 2040. It
was also estimated that by the end of this century the world energy consumption would be triple
increase compare to that of 2012 [3]. Currently, the world energy resources are mostly from
fossil fuel [2, 4]. However, the use of fossil fuel has led to serious environmental problems such
as global warming, greenhouse gas emission, and climate change [5, 6]. Besides, the safety of
nuclear energy is recently raising question and many European countries have shut down their
nuclear plants [7]. Therefore, broad societal needs focused attention on the discovery of new,
clean and renewable energy sources, and improving the existing energy efficiency [1, 5-10]. It is
 Bui Duc Long, Duong Ngoc Binh, Le Minh Hai, Le Hong Thang, Tran Duc Huy

reported that the world’s hunger for coal to abate starting around 2026 as governments work to
reduce emissions in step with promises under the Paris Agreement on climate change. By 2040
more than 60 % of electricity will come from solar, wind and other renewable resources, less
than 40 % of the electricity will produce from the fossil fuel [11]. In Vietnam, the government
has adopted various policies and measures to provide a reliable and clean energy supply
including provisions for the promotion of renewable and sustainable energies from different
sources such as wind energy, biomass and biogas, as well as solar and hydropower [12].
Thermoelectric (TE) devices or thermoelectric generators (TEGs), which are based on TE
materials, are solid-state devices with no moving parts; they are silent, reliable, scalable and no
gas emission, making them ideal for small power generation, as shown in Figure 1. TEGs have
greatly attracted attention from scientists, academia and industrialists as having the potential to
make important contributions to improving energy efficiency and providing cleaner forms of
energy without gas emissions [9, 12, 13]. TEGs can be used to recover or directly convert
waste heat from home heating, automotive exhaust, and industrial processes into electric power
[7, 12, 14]. For instance, by developing an automotive TEG that can be used to convert waste
heat into useable electricity, the engine will burn less fuel to power the vehicle's electrical
components and resulting in releasing fewer emissions. Currently, leading car manufacturers are
working on the development of this possibility [15].

Figure 1. Conversion heat energy from automobiles, industrial processes, home heating, sun and other
waste heat resources into electricity.

2. WORKING PRINCIPLES

Thermoelectric phenomenon or Seebeck effect was discovered by Thomas Johann Seebeck

in 1821. The fundamental of thermoelectric is very simple, when the temperature difference is
applied on a TE junction of two dissimilar metals, a voltage difference (∆V) will be produced
proportionally to the temperature difference (∆T) [5, 13,16], as shown in Figure 2a. The
proportional constant related to the intrinsic property of the material is known as the Seebeck
coefficient (denoted as S or α) [5, 13], where
α = ∆V/∆T. (1)

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Thermoelectric materials: fundamental, applications and challenges

Solid-state TE devices based on Seebeck effect can be used to generate electric power. TE
devices or TEGs are solid-state devices which is composed both n-, p-types materials. For
practical TEGs, a connection of large numbers of junctions in series is needed to increase
operating voltage, as shown in Figure 3.

Figure 2. A schematic of thermoelectric effect (a) Seebeck effect, ∆T = Thot –Tcold, (b) Peltier effect.

Likewise, a current flowing across a TE junction, either cooling or heating can occur at the
junction (Figure 2b), which depends on the direction of the current [5, 13]. This phenomenon is
named as Peltier effect, which was discovered by Jeans Charles Athanase Peltier in 1843. The
Peltier effect has been widely used in the applications such as thermal couple, air conditioning,
and refrigeration.

Figure 3. TE module composing of both n, p-types materials.

This figure is reproduced from [9] with copyright permission.

The performance of TE material is evaluated by a dimensionless figure of merit (ZT),

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 Bui Duc Long, Duong Ngoc Binh, Le Minh Hai, Le Hong Thang, Tran Duc Huy

defined as [1, 13]:

ZT = (S2σ/k)T (2)
where S, σ, k and T are the Seebeck coefficient (μVK ), electrical conductivity (Ω cm-1),
-1

thermal conductivity (Wm-1K-1) and absolute temperature (K). ZT is a function of temperature

(T) and depending on the intrinsic material properties (S, σ, k). For commercialization of
thermoelectric power generation (TEG), high-ZT value (≥3) materials are needed [1].
The efficiency (η) of a TE device for power generation is given by [1, 13]:

η= (3)

where Th, Tc are the temperatures of hot and cold sides of the TE material, respectively. ZT M is
average figure-of-merit over the whole working temperature range. For practical application, a
high ZTM value is required to have high efficiency TE devices or generators.

3. APPLICATIONS OF THERMOELECTRIC MATERIALS

3.1. Thermoelectric power for space applications

Thermoelectric power generations have shown their extraordinary reliability and long-life
for deep space science and exploration missions [17,18]. Radioisotope thermoelectric generators
(RTGs) were developed in the United State during the late 1950s [19]. The first RTGs were
lunched into space in 1961 and continuously operated for more than 30 years using high-
temperature heat sources (up to 1000 oC). The RTGs used by the U.S. space program were made
from alloys of lead telluride, TAGS, or SiGe [18].

3.2. Potential application in automobiles

Figure 4. Typical energy path for vehicles with gasoline-fueled internal combustion engines.
This figure is reprinted from [22] with copyright permission.

Extremely large amounts of waste heat energy are generated from transportation vehicles,
typically, heat produced by automotive engine [20]. Yu and Chau [21] reported that as for
internal combustion engine, only 25 % of the energy generated by fuel combustion was used to
run vehicle, whilst 70 % of the energy was lost as the waste heat, and 5 % of energy was
dissipated as friction, as shown in Figure 4. By recovering parts of the waste heat to produce

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Thermoelectric materials: fundamental, applications and challenges

electricity, which leads to improve fuel efficiency, reduce the fuel consumption and greenhouse
gas emissions [17]. Many car manufacturers, for example Toyota, Honda, Nissan, BMW, Ford
and GM, are interested in developing automotive TEGs with the target of improving 5 % of
consumption efficiency [22-25]. For instance, in 2008, a German automotive engineering
company developed a prototype TEG device for the Volkswagen Golf with an output power of
600 W [23]. It was reported that General Motors achieved TEGs with output of 350 W and 600
W in a Chevrolet Suburban under city and highway driving conditions, respectively [24].
Recently, BMW developed high temperature automotive TEGs which produces 750 W [25].

3.3. Recovery waste heat from industrial sectors

A huge amount of waste heat energy is generated from power plants and industries
processes. It is reported that manufacturing industries overall reject about 33 % of their energy
as waste heat directly to the atmosphere or to thermal management systems. In the U.S.
manufacturing sector alone, more than 3,000 TWh of waste heat energy is lost each year, an
amount equivalent to more than 1.72 billion barrels of oil [17]. TEGs can be used to recover
waste heat from many manufacturing processes such as biomass boiler, furnaces, cement kiln,
metal casting and steel manufacturing [1, 9, 17, 26, 27]. Recently, Alphabet energy developed
E1-C TEG which is the world largest TEG for exhaust heat recovery generator as large as a
container [28].

3.4. Stove-powered thermoelectric generator

Figure 5: A schematic of stove-power thermoelectric generation.

It is reported that more than three billion people, especially in some parts of developing
countries or rural area, are dependent on solid fuels, particularly biomass fuels, for their daily
cooking, heating, and even lighting [29]. In addition, electric supply in these areas is also
unreliable, and in some cases power can be failed due to natural disasters such as earthquake,
snowstorm, etc. Small power generators would be very useful to convert housing waste heat
into electricity, which is called the stove-powered thermoelectric generator. These stove-TEGs
consist of three parts: the stove system, the TEG system and the load system, as shown in Figure
5. When the biomass is burned and apart of waste heat can transfer to the TEGs and is converted
into electricity. This electric power can be stored or power the fan, light, radio or charge a

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 Bui Duc Long, Duong Ngoc Binh, Le Minh Hai, Le Hong Thang, Tran Duc Huy

mobile phone.

3.5. New applications of thermoelectric generator

Harvesting solar energy based - TEG is another important way to capture low temperature
heat. The amount of energy emitted from sun is gigantic, around 3 × 1024J/year, which are a few
hundred-fold times greater than what we use at the present. It is estimated that with a conversion
of 0.1 % of solar energy into useful energy with 10 % efficiency is more than enough to meet
our current energy needs [30]. Thus it has been proposed the concept of hybrid solar power
systems, which combines solid-state photovoltaic (PV) and TEGs [17]. This concept consists of
concentrating and splitting the solar energy spectrum into a low wavelength portion directed at
PV cells and a high wavelength portion directed at TE modules. Based on this idea, PV will
convert the ultraviolet and visible light and removing the infrared portion of the spectrum to
maximize their conversion efficiency by maintaining low operating temperatures [17]. Recently,
researchers at Massachusetts Institute of Technology (MIT) and their collaborators have
developed a high-performance and possibly less expensive way to convert solar heat into
electricity using flat-panel solar-thermoelectric power combined with hot water systems [30].

4. RECENT RESEARCH ON THERMOELECTRIC MATERIALS

Each TE material works with high performance at a certain temperature range. Thus in this
paper we review different TE materials based on different temperature ranges. As mentioned
previously, the available waste heat sources can be came from electronics, sun, geothermal
energy, the exhausted waste heat of transportation vehicles, industrial heat-generating processes
etc. [1, 34]. The waste heat sources can be classified at different temperature ranges, i.e. low
temperature (< 250 oC), middle temperature (250-650 oC), and high temperature (> 650 oC)
[1, 34].

Low temperature TE materials

Bi2Te3 is among the most outstanding TE materials for application at the vicinity of the
room temperature [35,36]. Besides, Bi2Te3-based alloys also can be good candidates for power
generation applications from room temperature to 230 oC [37]. For a long time, ZT value of
Bi2Te3 is around 1.0 [38]. Xie et al. applied melt spinning method combined with subsequent
spark plasma sintering to fabricate nanostructured p-type (Bi,Sb)2Te3 that exhibits a maximum
ZT of 1.5 at about 390 K [39]. However, Te is considered a toxic and expensive element. Thus,
researchers are searching for other non-toxic TE such as binary (Bi2S3, CdS, TiS2, Ag2S, Mg3Sb2
etc.) [16, 40]. Recently, H. Zhao et al. reported the discovery of high performance room
temperature TE material based on MgAgSb. As reported, the ZT values of this TE material are
close to 1.0 at room temperature and reached a maximum of 1.4 at 475 K [41].

Middle temperature TE materials

Cu - S based minerals appeared as potential candidates for TE materials due to their

advantages: earth abundant, low cost, and less toxic constituent elements, and high TE
performances at 400 oC. This trend in the research of TE materials was triggered by the
pioneering works on kesterite Cu2ZnSnS4, digenite Cu1.8S, and chalcopyrite CuFeS2. These

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Thermoelectric materials: fundamental, applications and challenges

works were followed by several reports on tetrahedrites Cu12-xTrxSb4S13 (Tr: 3d transition metals
and Zn) [42]. On other hand, lead telluride, clathrates, silicides, skutterudites have good
performance at temperature range of ~500 - 600 °C [1, 34, 43, 44, 45]. Skutterudites systems
have attracted great attention from TE community due to its high Seebeck coefficient, excellent
electrical transport properties and special lattice structure. Skutterudites have the cubic structure,
which has eight formula units per cubic cell. The two that are empty are called voids. Although
it is still controversial hypothesis, it has been believed that thermal conductivity of skutterudites
was reduced by filling impurity atoms in the voids. The “filler” atoms acted as the center
scattering phonons, consequently thermal conductivity will be decrease while electrical
conductivity can be increased due to the reduction of the band gap of the compound [1].
Recently, a remarkable ZT value of 1.7 was achieved for n-type filled skutterudites [46].
The following silicides have favorable properties as thermoelectric: CrSi2, MnSi1.75, β-FeSi2,
Ru2Si3, ReSi1.75, and Mg2X (X = Si, Ge, and Sn) [42, 43]. These TE material have energy gaps
and melting temperatures suitable for middle temperature range which is 300 - 600 °C. Silicides
have generated interest due to their low cost, abundant and non-toxic materials [32, 43]. Among
all semiconductor silicides, Mg2IV - based TE materials and higher manganese silicides (HMS)
are the most popular choices due to their promising n-type and p-type TE performance,
respectively [39, 47]. Currently, the highest ZT values obtained with the n-type and p-type
Mg2IV-based TE materials ~ 800 K are about 1.5 and 0.7, respectively [44, 45].

High temperature TE materials

Half-Heusler materials, denoted as XYZ, are semiconductors which consisting of a

covalent and an ionic part. The X and Y atoms have a distinct cationic character, whereas Z can
be seen as the anionic counterpart [48, 49]. Half-Heuslers have 18 valence electrons, they
consist of a late transition metal, an early transition metal or a rare earth element, and a main
group element [50, 51]. Half-Heusler compounds that can be used to directly convert the waste
heat to clean electric energy at relatively high temperatures around 700 oC [51]. There are two
types of half-Heusler which are n- (MNiSn where M = Ti, Zr, Hf, NbCoSn) [50, 51] and p-types
(MCoSb, where M is Ti, Zr, or Hf) [52, 53]. Many research groups focused on the n-type half-
Heusler MNiSn (M = Ti,Zr,Hf) system, since MNiSn based alloys due to their high power factor
[50, 51, 54, 55].
Si-Ge system is well known for high temperature (up to 1000 oC) thermoelectric power
generation, which is used for space mission [17]. Si-Ge system has high Seebeck coefficient but
also has large thermal conductivity. Thus many research works have been focused on the
reduction of lattice thermal conductivity [56-62].
Oxide semiconductors, which are thermally and chemically stable in air at high temperature,
which are promising the candidates for high temperature TE applications. However, their ZT value
has remained low, around 0.1–0.4 for more than 20 years. The poor performance in oxides is due
to their low electrical conductivity and high thermal conductivity [63]. In Japan, the rapid increase
in performance of oxide materials has made more than 10 times in the ZT value within the last two
decades due to the change in the guiding principles of TE materials research [64]. Some strategies
of lowering thermal conductivity of oxides materials are nanostructures, enhancing the phonon
scattering by introducing ‘‘impurity’’ atoms which serve as scattering centers [63, 64]. Recently
several oxide-based TE materials have been developed such as Ca3Co4O9 [65], CaMnO3 [66],
SrTiO3 [67], BiCuSeO [68], ZnO [69], In2O3 [70] and NiO [71] due to their structural and chemical
stabilities, oxidation resistance, easy processing, and low cost. Up-to-date, maximum ZT values of

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 Bui Duc Long, Duong Ngoc Binh, Le Minh Hai, Le Hong Thang, Tran Duc Huy

0.5 - 0.7 have been achieved for oxide TE materials [72].

5. IMPROVING EFFICIENCY APPROACHES

The efficiency of TE device is mainly determined by the value ZT. Other factors also affect
the efficiency of TE device such as resistances of the intermediate surface between TE material
and substrate, heat exchanger etc. This review was focus on the challenges and improving
approaches ZT of materials, which is led to improving the TE device performance. From Eq.
(2), having a high-ZT value, TE material needs to have large Seebeck coefficient, high electrical
conductivity, and low thermal conductivity. However, a material has large Seebeck coefficient,
which has low carrier concentration (see Eq. (4)), will have low electrical conductivity (see Eq.
(5)) [12].

(4)
where κB is the Boltzmann constant, e is the charge carrier, h is Planck’s constant, m* is the
effective mass of the charge carrier, and n is the carrier concentration. The relationship between
electrical conductivity and carrier concentration can be defined as:
(5)

where µ is the carrier mobility.

A material has high electrical conductivity, will also have high thermal conductivity (see
Eq. (5) and (7)). Therefore, it is really a challenge to improve ZT or the efficiency of the TE
material. Thermal conductivity of materials comes from two sources: (1) electrons and holes
transporting heat (ke) and (2) phonons travelling through the lattice (kl) [12].
K = ke + kl (6)

According to the Wiedemann-Franz law, the relationship between electrical conductivity

and electric thermal conductivity is defined as:
= (7)
Despite of difficulty, recently TE technology has made a big improvement via
nanostructuring approach, including nanocomposites [1, 7, 12, 36, 39, 63]. Here are the briefly
review of some main improving ZT approaches. The traditional approach is finding new TE
materials with high ZT values. In this method, the concept of “phonon-glass-electron-crystal”
(PGEC) with the ideal that TE material should have low thermal conductivity like in glass, high
Seebeck coefficient like in semiconductors, and high electrical conductivity like in crystal
material such as metals. The PGEC concept can be found in the materials with complex
symmetry and crystal structure such as skutterudites, zintl phases and clatharates [12, 13]. The
second approach is to enhance the powder factor (S2σ) (see Eq.2) by doping to optimize the
carrier concentration in the range of 1019 - 1021 carriers/cm3 [12, 73, 74]. The third approach is to
reduce the thermal conductivity (k) (see Eq. 2) via nanostructuring. In fact, bot improvement in
the power factor (S2σ) and reduction in lattice thermal conductivity are possible in
nanostructures. Particularly, theories and experiments indicated that a larger reduction in thermal
conductivity can be achieved in nanometer-sized low-dimensional structures as well as bulk
nanograined materials, arising from similar boundary and interface phonon-scattering
mechanisms [75].

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Thermoelectric materials: fundamental, applications and challenges

6. CONCLUSION

Thermoelectric is a promising technology to convert waste heat into electricity.

Thermoelectric generators, which are based on thermoelectric materials, are able to apply in
many different areas such as automobile, industrial processes, space, home heating, sun energy
etc. Although thermoelectric technology has made a big improvement in recent years, the
application of the technology is still limited by the low energy conversion efficiency of the
materials. There are a few enhanced efficiency approaches such as finding new materials with
high ZT value, doping, and nanostructures. The current high ZT materials usually contain toxic
and expensive elements, and therefore researchers now are paying more attention on the
development of non-toxic and cheap TE materials.

Acknowledgement. This work is supported by National Foundation for Science and Technology
Development (Nafosted), grant No.103.02-2016.18.

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