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The preparation and thermoelectric properties of Ti0.5Zr0.25Hf0.25Co1-xNixSb

half-Heusler compounds

Article in Journal of Applied Physics · March 2008

DOI: 10.1063/1.2885113 · Source: IEEE Xplore

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The preparation and thermoelectric properties of
Ti0.5Zr0.25Hf0.25Co1−xNixSb half-Heusler compounds
Wenjie Xie, Qiao Jin, and Xinfeng Tang

Citation: J. Appl. Phys. 103, 043711 (2008); doi: 10.1063/1.2885113

View online: http://dx.doi.org/10.1063/1.2885113
View Table of Contents: http://jap.aip.org/resource/1/JAPIAU/v103/i4
Published by the American Institute of Physics.

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 JOURNAL OF APPLIED PHYSICS 103, 043711 共2008兲

The preparation and thermoelectric properties of Ti0.5Zr0.25Hf0.25Co1−xNixSb

half-Heusler compounds
Wenjie Xie,1 Qiao Jin,1 and Xinfeng Tang1,a兲
1
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University
of Technology, Wuhan 430070, People’s Republic of China
共Received 23 October 2007; accepted 20 December 2007; published online 26 February 2008兲
Ni doping Ti0.5Zr0.25Hf0.25Co1−xNixSb 共x = 0 – 0.05兲 half-Heusler compounds have been fabricated by
combining high-frequency induction melting with spark plasma sintering technique, and their
thermoelectric transport properties have been investigated in the temperature range of 300– 900 K.
With the increase of Ni doping content, the electrical conductivity increases significantly, and withal
the Seebeck coefficient of all doped samples improve to some extent compared with the undoped
Ti0.5Zr0.25Hf0.25CoSb compound. These lead to a great improvement in the power factor, and the
highest power factor of 1.63⫻ 10−3 W m−1 K−1 is obtained at 715 K for
Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb compound. Furthermore, thermal conductivity of
Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds decrease remarkably due to Zr and Hf substitutions on Ti
site and Ni doping on Co site. Compared with ternary TiCoSb compound, the thermal conductivity
of Ti0.5Zr0.25Hf0.25Co1−xNixSb compound decreases 415%–430% at room temperature, and
compared with undoped Ti0.5Zr0.25Hf0.25CoSb compound, the thermal conductivity of
Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb decreases 34% at 300 K and 21% at 900 K, respectively. A maximum
dimensionless figure of merit ZT of 0.51 has been achieved for Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb
compound at 813 K. © 2008 American Institute of Physics. 关DOI: 10.1063/1.2885113兴

I. INTRODUCTION key problem as to how to decrease the thermal conductivity

of TiCoSb-based compounds with the maintaining good elec-
Thermoelectric materials draw much attention of world- trical transport properties.
wide researchers1–7 due to the fact that it can convert thermal Both theoretical calculation28,29 and experimental
energy directly into electrical energy by using the Seebeck results7,14–16,30,31 show that isoelectronic alloy of Ti, Zr, and
effect.8 The efficiency of a thermoelectric material is related Hf on M site will significantly reduce the lattice thermal
to the dimensionless figure of merit ZT, which is expressed conductivity of half-Heusler compounds. Zhou et al.29 inves-
as ZT = ␣2␴T / ␬, where ␣, ␴, T, and ␬ are Seebeck coeffi- tigated the thermal conductivity of Ti0.5Zr0.5CoSb compound
and confirmed that lattice thermal conductivity of
cient, electrical conductivity, absolute temperature, and ther-
Ti0.5Zr0.5CoSb compound is about 3 W / m K. It indicates
mal conductivity, respectively.
that Zr substitution on Ti site can effectively decrease the
The half-Heusler intermetallics compounds possessed
lattice thermal conductivity. However, up to now, it has not
MgAgAs-type structure9 have a small gap in the density of been reported how the isoelectronic alloy of Ti, Zr, and Hf on
states and a considerable effective mass;10–13 therefore, they M site affect on the thermoelectric properties of MCoSb-
have been intensively investigated owing to their potential based half-Heusler compounds. Furthermore, compared with
application in the thermoelectric field. Recently, MNiSn-based compounds, electrical transport properties of
MNiSn-based14–20 and MCoSb-based21–27 half-Heusler com- MCoSb-based compounds should be further improved.
pounds 共M = Ti, Zr, and Hf兲 have been paid more attention Therefore, in this research work, using Zr and Hf substitu-
than other half-Heusler compounds. For MNiSn-based half- tions on Ti site to reduce thermal conductivity and Ni doping
Heusler compounds, lots of good results7,14,16,17 have been on Co site to adjust electrical transport properties and further
reported and the highest ZT value of 1.5 has been obtained at decrease thermal conductivity, Ti0.5Zr0.25Hf0.25Co1−xNixSb
700 K for 共Zr0.5Hf0.5兲0.5Ti0.5NiSn0.998Sb0.002. However, the compounds have been fabricated, and their thermoelectric
reported greatest ZT value of TiCoSb-based half-Heusler properties have been investigated. We attempt to optimize
compounds is only 0.30 关Ti0.92Ta0.08CoSb 共Ref. 24兲兴, which the thermoelectric performance of TiCoSb-based half-
Heusler compounds by combining the isoelectronic alloy of
is much lower than that of MNiSn-based half-Heusler com-
Ti, Zr, and Hf with Ni doping on Co site.
pound. The main reason for the low ZT value of TiCoSb-
based compounds is that they have high thermal conductiv-
II. EXPERIMENT DETAILS
ity, which can achieve 24 W / m K 共Ref. 23兲 at the room
temperature for TiCoSb compound. Consequently, it is the Starting materials were commercial powders of Ti
共99.99%兲, Zr 共99%兲, Hf 共99%兲, Co 共99.99%兲, and Sb
a兲
Author to whom correspondence should be addressed. Electronic mail: 共99.999%兲. The mixed powders which were weighed accord-
tangxf@whut.edu.cn. ing to stoichiometric proportion of

0021-8979/2008/103共4兲/043711/5/$23.00 103, 043711-1 © 2008 American Institute of Physics

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043711-2 Xie, Jin, and Tang J. Appl. Phys. 103, 043711 共2008兲

Ti0.5Zr0.25Hf0.25Co1−xNixSb 共x = 0 , 0.01, 0.03, 0.05兲 were

pressed to disk and put into alumina crucible in the high-
frequency induction melting system 共VF-HMF100, Makabe
R&D Co., Ltd兲, and then the disks were melted three times
under the protection of argon to ensure homogeneity. Finally,
the obtained ingots were pulverized and sintered by spark
plasma sintering 共SPS兲 共SPS-1050, Sumitomo Coal Mining
Co., Ltd兲 technique to get bulk materials at 1323 K for
10 min. The obtained bulk materials were cut into rectangu-
lar bars with the approximate dimensions of 2 ⫻ 2
⫻ 10 mm3 for electrical transport properties measurement
共electrical conductivity and Seebeck coefficient兲. Addition-
ally, approximately 1.5-mm-thick disks with a diameter of
10.0 mm were cut for testing thermal conductivity.
Phase structures of the bulk materials were determined
by x-ray diffraction 共XRD兲 共PANalytical X’Pert Pro x-ray
diffraction兲. The chemical composition of FIG. 1. 共Color online兲 XRD patterns of Ti0.5Zr0.25Hf0.25Co1−xNixSb com-
pounds with different Ni doping contents 共x兲.
Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds were obtained by
electron probe microanalysis 共EPMA兲 共JXA-8800R兲, and the shown in Fig. 2共b兲 indicates that there is no obvious segre-
morphology and element distribution of bulk material sin- gation of any elements and all elements are distributed ho-
tered by SPS were analyzed by field emitted scanning elec- mogeneously in the matrix.
tron microscopy 共Hitachi S-4800兲. The electrical conductiv- B. Electrical transport properties
ity 共␴兲 and Seebeck coefficient 共␣兲 were measured
simultaneously using ZEM-1 共ULVAC Co. Ltd.兲. The carrier Figure 3 shows the temperature dependence of electrical
concentration 共N兲 and carrier mobility 共␮H兲 of the samples conductivity of Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds. The
with the approximate dimensions of 8 ⫻ 8 ⫻ 0.4 mm3 at the
room temperature were measured by Accent HL5500PC sys-
tem with the magnetic field strength of 0.513 T. The thermal
conductivity 共␬兲 was calculated from the measured thermal
diffusivity 共D兲, specific heat 共C p兲, and density 共d兲 using the
relationship ␬ = DC pd. D and C p were measured by a laser
flash method 共Shinkuriko: TC-7000兲 in a vacuum. The actual
density of obtained bulk Ti0.5Zr0.25Hf0.25Co1−xNixSb com-
pounds is measured by Archimedes principle, and the rela-
tive density of bulk materials is over 96%. The measure-
ments of all thermoelectric properties were performed within
the temperature range of 300– 900 K.

III. RESULTS AND DISCUSSIONS

A. Structure and microstructure
Figure 1 shows the typical XRD patterns of the final
Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds with different Ni
doping contents 共x兲. As shown in Fig. 1, all bulk materials
have a single MgAgAs-type lattice structure. Because the
atomic radius of Co 共0.167 nm兲 is very close to that of Ni
共0.162 nm兲, a paucity of Ni doping on Co site has little effect
on lattice parameter of Ti0.5Zr0.25Hf0.25Co1−xNixSb com-
pounds.
The microstructure and element distribution of
Ti0.5Zr0.25Hf0.25Co0.95Ni0.5Sb compound are obtained and
shown in Fig. 2. The grain and grain boundary structure are
observed in Fig. 2共a兲 and the grain sizes are about 5 – 10 ␮m.
From the energy dispersive spectroscopy 共EDS兲 results, both
the grain and grain boundary are composed of the half-
Heusler compound with a little different deviation of nomi- FIG. 2. Microstructure and element distribution of the
nal composition. The element distribution of the compound Ti0.5Zr0.25Hf0.25Co0.95Ni0.5Sb compound.

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043711-3 Xie, Jin, and Tang J. Appl. Phys. 103, 043711 共2008兲

FIG. 4. 共Color online兲 Temperature dependence of Seebeck coefficient for

FIG. 3. 共Color online兲 Temperature dependence of electrical conductivity
Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds.
for the Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds.

electrical conductivity of Ti0.5Zr0.25Hf0.25Co1−xNixSb com- tive, which is consistent with the Hall coefficient. It indicates
pounds increase significantly with the increasing of the Ni that Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds possess n-type
doping content. At room temperature, the electrical conduc- conduction. The absolute values of Seebeck coefficient ini-
tivity of Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb 共1.78⫻ 104 S m−1兲 is tially increase with temperature, and then reach their maxi-
about six times larger than that of Ti0.5Zr0.25Hf0.25CoSb mum at the temperature of intrinsic excitation, and followed
共3.0⫻ 103 S m−1兲. The EPMA analyzed composition, carrier by the decrease with temperature increasing. The maximum
concentration 共N兲, and carrier mobility 共␮H兲 for of Seebeck coefficient shifts to high temperature with the
Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds at room temperature increase of Ni doping content, which indicates that the tem-
are presented in Table I. With the increase of Ni doping perature of intrinsic excitation rises with the increase of Ni
content, the carrier concentration increases significantly. It doping content. At the same temperature, the Seebeck coef-
can be seen from the Table I that the carrier concentration of ficient increases with the increasing of Ni doping content and
Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb compound is nearly 200 times reaches the maximum when Ni doping content is x = 0.03,
higher than that of undoped Ti0.5Zr0.25Hf0.25CoSb compound. and followed by the decrease with Ni doping content increas-
Although the carrier mobility of doped compounds de- ing. However, with the rise of x, the change of Seebeck
creases, the electrical conductivity increases due to the high coefficient is not consistent with the increased electrical con-
carrier concentration. This remarkable improvement is ductivity as a result of the increased carrier concentration. It
caused by the fact that the Ni doping on Co site can intro- can be explained by the multiband conduction caused by
duce one more electron and thus the carrier 共electron兲 con- doping. For Ti0.5Zr0.25Hf0.25CoSb compound, both electrons
centration increases. As shown in the Fig. 3, with the in- and holes should contribute to the Seebeck coefficient; when
crease of temperature, the electrical conductivity of the Ni doped on Co site in Ti0.5Zr0.25Hf0.25Co1−xNixSb sys-
Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds rise, and then keep tem, basically a single band contributes to Seebeck coeffi-
steady or decrease a little when the temperature reaches cient. Therefore, the Seebeck coefficient of
500– 600 K. These results are due to the fact that the Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds could increase for
Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds appear to enter the small amount of Ni doping 共x 艋 0.03兲 and then it should
intrinsic conduction regime at high temperature. This transi- decrease for larger amount of doping 共x = 0.05兲 due to the
tional phenomenon is also observed in the TiCo1−xNixSb increase in carrier concentration.
compounds25 and some ZrNiSn-based half-Heusler The power factor values of all samples are obtained us-
compounds.14,31 ing the above electrical conductivity and Seebeck coefficient.
The temperature dependence of the Seebeck coefficient Figure 5 describes the temperature dependence of the power
of Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds is shown in Fig. 4. factor of Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds. Compared
The sign of the Seebeck coefficient of all samples is nega- with undoped Ti0.5Zr0.25Hf0.25CoSb compound, the power

TABLE I. EPMA analyzed composition, Hall coefficient 共RH兲, carrier concentration 共N兲, and carrier mobility 共␮H兲 for Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds
at the room temperature.

RH ␮H N
Nominal composition EPMA analyzed composition 共cm3 C−1兲 共cm2 V−1 s−1兲 共cm−3兲

Ti0.5Zr0.25Hf0.25CoSb Ti0.51Zr0.26Hf0.23CoSb −5.52⫻ 10−1 14.6 1.13⫻ 1019

Ti0.5Zr0.25Hf0.25Co0.99Ni0.01Sb Ti0.52Zr0.25Hf0.23Co0.995Ni0.005Sb −6.29⫻ 10−2 2.47 9.92⫻ 1019
Ti0.5Zr0.25Hf0.25Co0.97Ni0.03Sb Ti0.51Zr0.26Hf0.23Co0.977Ni0.023Sb −1.51⫻ 10−2 1.61 4.14⫻ 1020
Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb Ti0.51Zr0.25Hf0.24Co0.958Ni0.042Sb −2.99⫻ 10−3 0.52 2.09⫻ 1021

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043711-4 Xie, Jin, and Tang J. Appl. Phys. 103, 043711 共2008兲

FIG. 7. 共Color online兲 Temperature dependence of ZT values for

FIG. 5. 共Color online兲 Temperature dependence of power factor for Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds.
Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds.

with isoelectronic alloy of Ti, Zr, and Hf is much lower than

factor of all doped samples increases owing to the signifi-
that of TiCo0.95Ni0.05Sb 共Ref. 25兲 compound. It is for this
cantly improvement of electrical conductivity. The power
reason that isoelectronic alloying on Ti site introduces pho-
factor of Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb compound achieves
non mass-fluctuation scattering due to the mass differences
1.63⫻ 10−3 W m−1 K−1 at 715 K. Compared with
between Ti 共atomic mass= 47.867兲, Zr 共atomic mass
Ti0.5Zr0.25Hf0.25CoSb compound, it increases by about 270%.
= 91.224兲, and Hf 共atomic mass= 178.49兲 and phonon strain
field fluctuation scattering owing to the size and interatomic
C. Thermal transport properties
coupling force differences of Ti, Zr, and Hf atoms. The ther-
Figure 6 presents the temperature dependence of the to- mal conductivity of Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds
tal thermal conductivity of Ti0.5Zr0.25Hf0.25Co1−xNixSb com- decreases further due to the fact that Ni doping on Co site
pounds. In order to compare, some reported data21,24,25 of can induce disorder in the crystal lattice, which will also
TiCoSb-based compounds are summarized in the inset of increase the phonon scattering. Therefore, the combined ef-
Fig. 6. As shown in Fig. 6, the thermal conductivity of fect of isoelectronic alloying on Ti site and Ni doping on Co
Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb at 300 and 900 K are 3.35 and site reduce the thermal conductivity remarkably.
2.29 W m−1 K−1. Compared with undoped
Ti0.5Zr0.25Hf0.25CoSb compound, they decrease 34% and D. Dimensionless thermoelectric figure of merit ZT
21%, respectively. At room temperature, the thermal conduc- The dimensionless thermoelectric figure of merit ZT val-
tivity of Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds are about ues is calculated from the above measured electrical conduc-
3.35– 4.50 W m−1 K−1, which decreases 415%–430% com- tivity, the Seebeck coefficient, and the thermal conductivity
pared with the reported data of ternary TiCoSb compound and shown in Fig. 7. Because of the significant increase of
关about 18 W m−1 K−1 共Ref. 24兲兴 in the inset. Furthermore, the power factor and the considerable decrease of the thermal
when the Ni doping content x is the same 共0.05兲, the thermal conductivity, the ZT value of Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb
conductivity of Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb compound compound is much higher than that of Ti0.5Zr0.25Hf0.25CoSb.
As shown in Fig. 7, the greatest ZT value of 0.51 is obtained
at 813 K for the Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb compound.

IV. CONCLUSIONS
Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds have been syn-
thesized by combining high-frequency induction melting
technique and spark plasma sintering method, and the effect
of Ni doping content on their thermoelectric transport prop-
erties have been investigated. The XRD result shows that the
obtained Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds are signal
phase with MgAgAs structure. The EPMA and EDS map-
ping analyses show that all elements distribute homoge-
neously. With the increasing Ni doping content, the electrical
conductivity increases significantly, and the Seebeck coeffi-
cient of doped compounds increases to some extent com-
pared with the undoped compound. When the Ni doping con-
FIG. 6. 共Color online兲 Temperature dependence of thermal conductivity for
Ti0.5Zr0.25Hf0.25Co1−xNixSb compounds 共the inset shows the reported data of tent x is 0.05, the power factor of
TiCoSb-based compounds兲. Ti0.5Zr0.25Hf0.25Co0.95Ni0.05Sb compound reaches maximum

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043711-5 Xie, Jin, and Tang J. Appl. Phys. 103, 043711 共2008兲

14
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