Fast synthesis and improved electrical stability in n-type Ag2Te thermoelectric materials

doi:10.1016/j.jmst.2021.01.097

Abstract

Abstract:

Cu- and Ag-based superionic conductors are promising thermoelectric materials due to their good electrical properties and intrinsically low thermal conductivity. However, the poor electrical and thermal stability restrict their application. In this work, n-type pure phase Ag2Te compound is synthesized by simply grinding elemental powders at room temperature and compacted by spark plasma sintering. It is found that, because of the migration of Ag+ after the phase transition around 425 K, submicron pores are formed inside the samples during the electrical performance measurement, resulting in poor electrical stability and repeatability of Ag2Te samples. However, Pb-doped Ag2-xPbxTe (x = 0-0.05) specimens exhibit improved electrical stability by the precipitation of the secondary phase PbTe in the Ag2Te matrix, which is confirmed via cyclic electrical property measurement and microstructure characterization. A maximum zT = 0.72 is obtained at 570 K for x = 0.03 mainly due to the increased power factor.

Key words: Thermoelectric, Superionic conductor, Silver telluride, Phase transition, Stability

Huiping Hu, Kaiyang Xia, Yuechu Wang, Chenguang Fu, Tiejun Zhu, Xinbing Zhao. Fast synthesis and improved electrical stability in n-type Ag₂Te thermoelectric materials[J]. J. Mater. Sci. Technol., 2021, 91: 241-250.

Figures/Tables 11

Fig. 1. (a) Pictures of Ag and Te powder with different grinding time. (b) XRD patterns of Ag-Te powder with grinding time of 5 min, 10 min, 30 min, and 60 min. (c) DSC and TG curves of Ag2Te sample synthesized by manual mixing in the temperature range of 300-573 K. (d) XRD patterns of Ag2Te bulks synthesized by melting, ball-milling, and manual mixing.

Fig. 2. Temperature dependences of (a) electrical conductivity, (b) Seebeck coefficient, (c) total thermal conductivity, and (d) the figure of merit zT for Ag2Te bulks synthesized by melting (M), ball milling (BM), and manual mixing (MM). The magenta short dash line is the literature data of Ag2Te synthesized by melting and SPS [27]. We have eliminated those values in the temperature range of 400-450 K where the phase transition occurs, which causes a great fluctuation in the results.

Table 1 Actual chemical compositions, density, carrier concentration, and carrier mobility for MM samples with different electrical property measuring cycles at room temperature.

Electrical property measuring cycles	EPMA composition	ρ (g cm^-3)	n_H (10¹⁸ cm^-3)	µ_H (10³ cm² V^-1 s^-1)
0	Ag_2.018Te	8.37	1.20	5.12
1	Ag_1.979Te	8.31	1.47	4.46
2	Ag_1.955Te	8.23	1.01	3.58
3	Ag_1.928Te	8.19	1.32	2.35

Fig. 3. Temperature dependences of (a) electrical conductivity and (b) Seebeck coefficient of pristine Ag2Te prepared by manual-mixing and SPS with cyclic electrical property measurements for 3 cycles.

Fig. 4. (a-d) SEM images of the polished surface for MM samples with different electrical property measurement cycles. (e-h) BSE images of polished surface for MM samples with different electrical property measurement cycles. Moreover, images denoted as Before measurement are obtained from MM sample without electrical property measurement, and so on. In BSE images, the gray regions are Ag2Te phase, and the actual compositions detected by EPMA are shown in the bottom left corner as well as in Table 1. The black regions are confirmed to be pores.

Fig. 5. SEM images of fresh fracture surface for MM samples with different annealing cycles. (a) Unannealed, (b) annealing 1 cycle, (c) annealing 2 cycles, (d) annealing 3 cycles. The annealing temperature and time (t) of each cycle are identical to the electrical property measurement with temperature ranging from ambient temperature to 573 K and t = 250 min.

Fig. 6. SEM images of fresh fracture surface for MM samples with different annealing temperatures. (a) Annealed at 373 K, (b) annealed at 473 K, and (c) annealed at 573 K for 420 min.

Fig. 7. Phase structure and microstructure for Ag2-xPbxTe specimens. (a) Powder XRD patterns of Ag2-xPbxTe (x = 0-0.05) specimens. (b) SEM image and (c) BSE image of polished surface for Ag1.96Pb0.04Te sample after 3 times cyclic electrical property measurement. (d-f) SEM images of fresh fracture surface for Ag1.96Pb0.04Te sample with no anneal treatment and 3 cycles anneal treatment respectively. Anneal temperature (T) and time (t) of each cycle are identical to the electrical property measurement.

Fig. 8. Temperature dependences of electrical conductivity (a, c, e and g) and Seebeck coefficient (b, d, f and h) for Ag2-xPbxTe (x = 0.005, 0.01, 0.02, and 0.04) specimens with cyclic electrical property measurements for 3 times. We have eliminated those Seebeck coefficient values in the temperature range of 400-450 K where phase transition occurs to cause great fluctuation in the results.

Fig. 9. Temperature dependences of (a) electrical conductivity, (b) Seebeck coefficient, (c) power factor and (d) thermal conductivity of the Ag2-xPbxTe specimens (x = 0-0.05). We have repeatedly measured the TE properties for three cycles and then chosen the data from the last cycle.

Fig. 10. Temperature dependence of zT for Ag2-xPbxTe specimens.

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Fast synthesis and improved electrical stability in n-type Ag₂Te thermoelectric materials

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