Thermal Stability of Nb/Mg3SbBi Interface

doi:10.15541/jim20230006

Abstract

Abstract:

Zintl-phase Mg₃(Sb,Bi)₂-based thermoelectric (TE) compounds have attracted extensive attention due to their excellent TE performance in the medium and low temperature region (27-500 ℃). However, the reactive nature of Mg and Sb elements leads to violent interfacial diffusion reactions with electrodes during long-term high-temperature service, degrading TE performance and shortening lifespan of TE devices. Consequently, it is crucial to select diffusion barrier layer (DBL) with low interfacial contact resistivity to block violent interdiffusion of components. In this work, the n-type Mg₃SbBi (Mg_3.2SbBi_0.996Se_0.004) sample, with ZT~1.4@300 ℃, and the “sandwich” structure of Mg₃SbBi/Nb/ Mg₃SbBi was prepared by hot pressing sintering process. Composition and microstructure of the interfacial layer and evolution of resistance with aging time were investigated systematically. Accelerated aging results (525 ℃/70 h, 525 ℃/170 h, 525 ℃/360 h) indicated that Mg-Sb/Bi components segregation occurred in the Mg₃SbBi-Nb DBL junctions, and cracks formed on the surface. However, the interfaces were well conjunctive after polishing the pellets. And the thickness of diffusion layer slowly increased to 1.6 μm after aging. Besides, resistivity of the Nb/Mg₃SbBi interface slightly increased from initial 12.9 μΩ·cm² to 19.8, 27.4 and 31.8 μΩ·cm², respectively, indicating the Nb DBL still displaying excellent barrier properties except for the faint diffusion during aging. Based on these data, Nb is a better choice to effectively suppress the diffusion of Mg and Sb elements achieving reliable connection, to be the DBL material in the Mg₃(Sb,Bi)₂-based TE families. In conclusion, Nb can effectively improve the Mg₃(Sb,Bi)₂-based devices' thermal stability and promote the application over the medium temperature power generation.

Key words: Mg₃(Sb,Bi)₂, diffusion barrier layer, interface stability, interface resistivity

CLC Number:

TQ174

HU Zhongliang, FU Yuntian, JIANG Meng, WANG Lianjun, JIANG Wan. Thermal Stability of Nb/Mg₃SbBi Interface[J]. Journal of Inorganic Materials, 2023, 38(8): 931-937.

Figures/Tables 8

Fig. 1 (a) Loading diagram and (b) physical particle picture of Mg3SbBi/Nb/Mg3SbBi sample

Fig. 2 (a) Powder and bulk XRD patterns and (b) block decent scanning element distribution mappings of Mg3SbBi sample

Fig. 3 Thermoelectric properties of hot-pressed 750 ℃ sintered samples with various holding time as a function of test temperature (a) Electrical conductivity; (b) Seebeck coefficient; (c) Lattice thermal conductivity; (d) ZT

Fig. 4 (a) BSE image of Mg3SbBi/Nb/Mg3SbBi sample before aging and (b, c) magnified images of corresponding areas in (a)

Table 1 EDS point analysis results of the points in Fig.4(c) (in atomic)

Point	Mg/%	Sb/%	Bi/%	Nb/%
1	59.75	9.25	29.64	1.36
2	51.88	8.35	25.57	14.20
3	1.19	0.14	0.13	98.54
4	58.78	19.85	20.22	1.15

Fig. 5 BSE images of the interface of Mg3SbBi/Nb/Mg3SbBi after aging at 525 ℃ for 70, 160 and 360 h (a-c) Before polished; (d-f) After polished

Fig. 6 Backscatter (up) and line sweep (down) results of Nb /Mg3SbBi interface aged at 525℃for different time (a) 70; (b) 170 h; (c) 360 h; Colorful figures are available on website

Fig. 7 Interface resistivities of Nb/Mg3SbBi (a) Comparison with literature [13,17⇓-19]; (b) Relationship of interface resistivity with thermal aging time

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Thermal Stability of Nb/Mg₃SbBi Interface

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