Enhanced thermoelectric performance in n-type Mg3.2Sb1.5Bi0.5 doping with lanthanides at the Mg site

doi:10.1016/j.jmst.2022.02.054

Abstract

Abstract:

Mg-based thermoelectric materials have attracted more and more attention because of their rich composition elements, green environmental protection, and lower price. In recent years, the thermoelectric properties of n-type Mg₃Sb₂ materials have been optimized by doping chalcogenide elements (S, Se, and Te) at the anionic position. In this work, n-type Mg_3.2A_xSb_1.5Bi_0.5 (A = Gd, Ho; x = 0.01, 0.02, 0.03, and 0.4) samples were prepared by the cation site doping of lanthanide elements (Gd and Ho). The research results show that Gd and Ho doped n-type Mg_3.2Sb_1.5Bi_0.5 samples are entirely comparable to the S, Se, and Te doped n-type Mg_3.2Sb_1.5Bi_0.5 samples, demonstrating more excellent thermoelectric properties. Doping with lanthanides (Gd and Ho) at the Mg site increases the carrier concentration of the material to 8.161 × 10¹⁹ cm⁻³. Doping induces the contribution of more electron, thus obtaining higher conductivity. The maximum zT value of the Mg_3.2Gd_0.02Sb_1.5Bi_0.5 and the Mg_3.2Ho_0.02Sb_1.5Bi_0.5 samples reaches 1.61 and 1.55, respectively. This work theoretically and experimentally demonstrates Gd and Ho are efficient n-type dopants for Mg_3.2Sb_1.5Bi_0.5 thermoelectric material.

Key words: Thermoelectric material, First-principles calculation, Mg_3.2Sb_1.5Bi_0.5

Lu Yu, Zipei Zhang, Juan Li, Wenhao Li, Shikai Wei, Sitong Wei, Guiwu Lu, Weiyu Song, Shuqi Zheng. Enhanced thermoelectric performance in n-type Mg_3.2Sb_1.5Bi_0.5 doping with lanthanides at the Mg site[J]. J. Mater. Sci. Technol., 2022, 127: 108-114.

Figures/Tables 9

Fig. 1. Band-structure by element-weights of (a) Mg24Sb16, (b) Mg23Gd1Sb16, and (c) Mg23Ho1Sb16 samples.

Fig. 2. (a) XRD pattern of n-type Mg3.2GdxSb1.5Bi0.5 (x = 0.01, 0.02, 0.03, and 0.04), and (b) XRD pattern of n-type Mg3.2HoxSb1.5Bi0.5 (x = 0.01, 0.02, 0.03, and 0.04).

Fig. 3. (a) SEM image of the fractured cross section of n-type Mg3.2Gd0.02Sb1.5Bi0.5 sample and (b-f) SEM-EDS images of the polished surface of n-type Mg3.2Gd0.02Sb1.5Bi0.5 sample.

Fig. 4. (a) SEM image of the fractured cross section of n-type Mg3.2Ho0.02Sb1.5Bi0.5 sample and (b-f) SEM-EDS images of the polished surface of n-type Mg3.2Ho0.02Sb1.5Bi0.5 sample.

Fig. 5. Temperature dependence of n-type Mg3.2GdxSb1.5Bi0.5 (x = 0.01, 0.02, 0.03, and 0.04) samples: (a) Seebeck coefficient, (b) conductivity, and (c) power factor.

Fig. 6. Temperature dependence of (a) total thermal conductivity, (b) lattice thermal conductivity, (c) electrical thermal conductivity, and (d) figure of merit zT of n-type Mg3.2GdxSb1.5Bi0.5(x = 0.01, 0.02, 0.03, and 0.04) samples.

Fig. 7. Temperature dependence of n-type Mg3.2HoxSb1.5Bi0.5 (x = 0.01, 0.02, 0.03, and 0.04) samples: (a) Seebeck coefficient, (b) conductivity, and (c) power factor.

Fig. 8. Temperature dependence of (a) total thermal conductivity, (b) lattice thermal conductivity, (c) electrical thermal conductivity, and (d) figure of merit zT of n-type Mg3.2HoxSb1.5Bi0.5 (x = 0.01, 0.02, 0.03, and 0.04) samples.

Fig. 9. (a) The relationship between the carrier concentration of Mg3Sb2-based compounds and the doping content of Gd, Ho, S, Se, and Te at 300 K [19,30,31], and (b) the maximum zT values comparison of n-type Mg3.2Ho0.02Sb1.5Bi0.5, Mg3.2Gd0.02Sb1.5Bi0.5 and other Mg3Sb2-based thermoelectric materials [32, 33, 34].

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