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. 2023 May 18;16(10):3819.
doi: 10.3390/ma16103819.

Investigation of the Effect of Double-Filler Atoms on the Thermoelectric Properties of Ce-YbCo4Sb12

Nguyen Vu Binh  1 , Nguyen Van Du  2 , Nayoung Lee  1 , Minji Kang  1 , So Hyeon Ryu  1 , Munhwi Lee  1 , Deokcheol Seo  3 , Woo Hyun Nam  1 , Jong Wook Roh  4 , Soonil Lee  5 , Se Yun Kim  6 , Sang-Mo Koo  7 , Weon Ho Shin  7 , Jung Young Cho  1
Affiliations

Investigation of the Effect of Double-Filler Atoms on the Thermoelectric Properties of Ce-YbCo4Sb12

Nguyen Vu Binh et al. Materials (Basel). .

Abstract

Skutterudite compounds have been studied as potential thermoelectric materials due to their high thermoelectric efficiency, which makes them attractive candidates for applications in thermoelectric power generation. In this study, the effects of double-filling on the thermoelectric properties of the CexYb0.2-xCo4Sb12 skutterudite material system were investigated through the process of melt spinning and spark plasma sintering (SPS). By replacing Yb with Ce, the carrier concentration was compensated for by the extra electron from Ce donors, leading to optimized electrical conductivity, Seebeck coefficient, and power factor of the CexYb0.2-xCo4Sb12 system. However, at high temperatures, the power factor showed a downturn due to bipolar conduction in the intrinsic conduction regime. The lattice thermal conductivity of the CexYb0.2-xCo4Sb12 skutterudite system was clearly suppressed in the range between 0.025 and 0.1 for Ce content, due to the introduction of the dual phonon scattering center from Ce and Yb fillers. The highest ZT value of 1.15 at 750 K was achieved for the Ce0.05Yb0.15Co4Sb12 sample. The thermoelectric properties could be further improved by controlling the secondary phase formation of CoSb2 in this double-filled skutterudite system.

Keywords: double-filled; skutterudite; thermoelectric.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Figure 1
Figure 1
(a) Powder XRD of CexYb0.2−xCo4Sb12 after SPS, (b) the secondary phase peak of CoSb2, (c) zoomed in XRD pattern between 31° and 31.8°, and (d) calculated lattice parameter of CexYb0.2−xCo4Sb12 samples as a function of Ce content.
Figure 2
Figure 2
FE-SEM images of CexYb0.2−xCo4Sb12 samples after SPS for (a) x = 0.000, (b) x = 0.025, (c) x = 0.050, (d) x = 0.075, and (e) x = 0.100.
Figure 3
Figure 3
FE-SEM images of ribbons from the RSP process. (a) The cross section, (b) contact surface, and (c) free surface of sample Ce0.025Yb0.175Co4Sb12; (d) the cross section, (e) contact, and (f) free surface of sample Ce0.1Yb0.1Co4Sb12.
Figure 4
Figure 4
EDS images of sample Ce0.025Yb0.175Co4Sb12. (a) The SEM image, the distribution of (b) Co, (c) Sb, (d) Ce, (e) Yb and (f) O (EDS images of other compositions are displayed in Figures S1–S5).
Figure 5
Figure 5
(a) The carrier concentration and mobility of CexYb0.2−xCo4Sb12 (x = 0, 0.025, 0.05, 0.075, and 0.1) at room temperature, and (b) the temperature dependence of electrical conductivity.
Figure 6
Figure 6
The temperature dependence of (a) the Seebeck coefficient and (b) the power factor of CexYb0.2−xCo4Sb12 (x = 0, 0.025, 0.05, 0.075, and 0.1).
Figure 7
Figure 7
The effective mass m*/m0 at room temperature as a function of carrier concentration for CexYb0.2−xCo4Sb12.
Figure 8
Figure 8
The temperature dependence of (a) the total thermal conductivity and (b) the lattice thermal conductivity of sample CexYb0.2−xCo4Sb12 (x = 0, 0.025, 0.05, 0.075, and 0.1).
Figure 9
Figure 9
The temperature dependence of the ZT of sample CexYb0.2−xCo4Sb12 (x = 0, 0.025, 0.05, 0.075, and 0.1).
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