Journal of Inorganic Materials ›› 2024, Vol. 39 ›› Issue (8): 903-910.DOI: 10.15541/jim20240057
Special Issue: 【能源环境】热电材料(202409)
• RESEARCH ARTICLE • Previous Articles Next Articles
MIAO Xin1(), YAN Shiqiang1, WEI Jindou1, WU Chao1, FAN Wenhao2, CHEN Shaoping1(
)
Received:
2024-01-30
Revised:
2024-02-20
Published:
2024-08-20
Online:
2024-04-19
Contact:
CHEN Shaoping, professor. E-mail: chenshaoping@tyut.edu.cnAbout author:
MIAO Xin (1999-), male, Master candidate. E-mail: miaoxin0242@link.tyut.edu.cn
Supported by:
CLC Number:
MIAO Xin, YAN Shiqiang, WEI Jindou, WU Chao, FAN Wenhao, CHEN Shaoping. Interface Layer of Te-based Thermoelectric Device: Abnormal Growth and Interface Stability[J]. Journal of Inorganic Materials, 2024, 39(8): 903-910.
Fig. 1 Microstructure and composition of Te0.985Sb0.015 precursor powder (a) Backscattered SEM image; (b) XRD patterns and quasi-1D chain crystal structure of Te and Te0.985Sb0.015 powders; Colorful figures are available on website
Fig. 3 (a) Thicknesses of the interface reaction layers (IRLs) at the Te0.985Sb0.015/NixTe interfaces, and (b) formation Gibbs free energies in molar (ΔrGT) of the interface products at the Te0.985Sb0.015/NixTe interfaces
Total migration of atoms | x=0.500 | x=0.563 | x=0.667 | x=0.833 | x=0.908 | Te0.985Sb0.015/Ni |
---|---|---|---|---|---|---|
CN·l/(mol·cm-2) | 0 | 0.1297 | 0.2134 | 0.2810 | 0.3154 | 0.5653 |
Table 1 Total migration of atoms (CN·l) at Te0.985Sb0.015/NixTe interface
Total migration of atoms | x=0.500 | x=0.563 | x=0.667 | x=0.833 | x=0.908 | Te0.985Sb0.015/Ni |
---|---|---|---|---|---|---|
CN·l/(mol·cm-2) | 0 | 0.1297 | 0.2134 | 0.2810 | 0.3154 | 0.5653 |
Fig. 5 Microstructures of Te0.985Sb0.015/NixTe interfaces after aging at 473 K for 6 and 12 d Backscattering SEM images for (a) x=0.500, (b) x=0.563, and (c) x=0.667
Fig. 6 Performance of NixTe/Te0.985Sb0.015/NixTe (x=0.500, 0.563, 0.667) single-leg devices (a, b) Room temperature V-I curves and contact resistivity, ρc, before aging; (c) Time-dependent room temperature ρc; (d) Time-dependent efficiency, η, under a temperature difference of 180 K (hot end: 473 K, cold end: 293 K)
Fig. S2 Thermoelectric performance of Te0.985Sb0.015 in the direction parallel to the sintering pressure (a) Total thermal conductivity, κ; (b) Carrier concentration, n; (c) Resistivity; (d) Seebeck coefficient; (e) Power factor, PF; (f) Dimensionless ZT of Te0.985Sb0.015; The test results of Pei et al.[15] are also drawn in the figures for comparison
Fig. S4 Microstructures and element distributions of sintered Te0.985Sb0.015/NixTe interfaces Backscatter SEM images and EDS spectra for (a) x=0.500, (b) x=0.563, (c) x=0.667, (d) x=0.833, and (e) x=0.908
Phase lable | Formula in reference | Formula used here | Temperature/K | ST/(J·mol-1·K-1) | HT/(kJ·mol-1) | GT/(kJ·mol-1) | Ref. |
---|---|---|---|---|---|---|---|
δ(-NiTe2-x, 52.2%-66.7% (in atom) Te) | Ni0.476Te0.524 | Ni0.908Te | 298.15 | 76.393 | -51.908 | -74.685 | [ |
600.00 | 112.729 | -36.120 | -103.758 | ||||
700.00 | 121.397 | -30.494 | -115.472 | ||||
Ni0.4Te0.6 | Ni0.667Te | 298.15 | 66.917 | -47.833 | -67.785 | [ | |
600.00 | 98.732 | -33.987 | -93.226 | ||||
700.00 | 106.415 | -29.000 | -103.491 | ||||
Ni0.333Te0.667 | Ni0.5Te | 298.15 | 60.135 | -43.778 | -61.707 | [ | |
600.00 | 88.253 | -31.552 | -84.504 | ||||
700.00 | 95.001 | -27.172 | -93.673 | ||||
Te | Te | Te | 298.15 | 49.497 | 0.000 | -14.757 | [ |
600.00 | 69.537 | 8.766 | -32.956 | ||||
700.00 | 74.694 | 12.114 | -40.171 | ||||
Ni | Ni | Ni | 298.15 | 29.874 | 0.000 | -8.907 | [ |
600.00 | 50.419 | 9.008 | -21.243 | ||||
700.00 | 55.546 | 12.326 | -26.557 |
Table S1 Thermodynamic data. Values of entropy (ST), enthalpy (HT), and Gibbs free energy (GT) at 298.15, 600.00 and 700.00 K, respectively
Phase lable | Formula in reference | Formula used here | Temperature/K | ST/(J·mol-1·K-1) | HT/(kJ·mol-1) | GT/(kJ·mol-1) | Ref. |
---|---|---|---|---|---|---|---|
δ(-NiTe2-x, 52.2%-66.7% (in atom) Te) | Ni0.476Te0.524 | Ni0.908Te | 298.15 | 76.393 | -51.908 | -74.685 | [ |
600.00 | 112.729 | -36.120 | -103.758 | ||||
700.00 | 121.397 | -30.494 | -115.472 | ||||
Ni0.4Te0.6 | Ni0.667Te | 298.15 | 66.917 | -47.833 | -67.785 | [ | |
600.00 | 98.732 | -33.987 | -93.226 | ||||
700.00 | 106.415 | -29.000 | -103.491 | ||||
Ni0.333Te0.667 | Ni0.5Te | 298.15 | 60.135 | -43.778 | -61.707 | [ | |
600.00 | 88.253 | -31.552 | -84.504 | ||||
700.00 | 95.001 | -27.172 | -93.673 | ||||
Te | Te | Te | 298.15 | 49.497 | 0.000 | -14.757 | [ |
600.00 | 69.537 | 8.766 | -32.956 | ||||
700.00 | 74.694 | 12.114 | -40.171 | ||||
Ni | Ni | Ni | 298.15 | 29.874 | 0.000 | -8.907 | [ |
600.00 | 50.419 | 9.008 | -21.243 | ||||
700.00 | 55.546 | 12.326 | -26.557 |
Chemical reaction equation | Temperature/K | ΔrST/(J·mol-1·K-1) | ΔrHT/(kJ·mol-1) | ΔrGT/(kJ·mol-1) |
---|---|---|---|---|
0.25Te+0.75Ni0.667Te→Ni0.5Te | 298.15 | -2.427 | -7.903 | -7.180 |
600.00 | -3.180 | -8.253 | -6.345 | |
700.00 | -3.484 | -8.451 | -6.012 | |
0.449Te+0.551Ni0.908Te→Ni0.5Te | 298.15 | -4.182 | -15.177 | -13.930 |
600.00 | -5.083 | -15.586 | -12.536 | |
700.00 | -5.426 | -15.809 | -12.010 | |
1.5Ni+Te→Ni1.5Te | 298.15 | 5.692 | -57.500 | -59.197 |
600.00 | 5.969 | -57.318 | -60.899 | |
700.00 | 8.110 | -56.023 | -61.700 |
Table S2 Molar formation Gibbs free energies (ΔrGT) of interface products at 298.15, 600.00 and 700.00 K, respectively
Chemical reaction equation | Temperature/K | ΔrST/(J·mol-1·K-1) | ΔrHT/(kJ·mol-1) | ΔrGT/(kJ·mol-1) |
---|---|---|---|---|
0.25Te+0.75Ni0.667Te→Ni0.5Te | 298.15 | -2.427 | -7.903 | -7.180 |
600.00 | -3.180 | -8.253 | -6.345 | |
700.00 | -3.484 | -8.451 | -6.012 | |
0.449Te+0.551Ni0.908Te→Ni0.5Te | 298.15 | -4.182 | -15.177 | -13.930 |
600.00 | -5.083 | -15.586 | -12.536 | |
700.00 | -5.426 | -15.809 | -12.010 | |
1.5Ni+Te→Ni1.5Te | 298.15 | 5.692 | -57.500 | -59.197 |
600.00 | 5.969 | -57.318 | -60.899 | |
700.00 | 8.110 | -56.023 | -61.700 |
Item | NiTe2 (Ni0.5Te) | NiTe1.776 (Ni0.563Te) | NiTe1.5 (Ni0.667Te) | NiTe1.2 (Ni0.833Te) | NiTe1.1 (Ni0.908Te) | Ni | Te | NiTe0.667 (Ni1.5Te) |
---|---|---|---|---|---|---|---|---|
M/(g·mol-1) | 313.893 | 285.311 | 250.093 | 211.813 | 199.053 | 58.693 | 127.600 | 143.802 |
n | 2.000 | 1.776 | 1.500 | 1.200 | 1.100 | 0.000 | - | 0.667 |
ρ/(g·cm-3) | 7.701 | 7.565 | 7.363 | 7.086 | 6.976 | 8.910 | - | 8.126 |
Table S3 Density (ρ), molar mass (M) and moles of the bound Te per mole substance
Item | NiTe2 (Ni0.5Te) | NiTe1.776 (Ni0.563Te) | NiTe1.5 (Ni0.667Te) | NiTe1.2 (Ni0.833Te) | NiTe1.1 (Ni0.908Te) | Ni | Te | NiTe0.667 (Ni1.5Te) |
---|---|---|---|---|---|---|---|---|
M/(g·mol-1) | 313.893 | 285.311 | 250.093 | 211.813 | 199.053 | 58.693 | 127.600 | 143.802 |
n | 2.000 | 1.776 | 1.500 | 1.200 | 1.100 | 0.000 | - | 0.667 |
ρ/(g·cm-3) | 7.701 | 7.565 | 7.363 | 7.086 | 6.976 | 8.910 | - | 8.126 |
Fig. S6 Performance of Ni0.5Te/Te0.985Sb0.015/Ni0.5Te single-leg devices under a temperature difference of 180 K (Hot end: 473 K, Cold end: 293 K) (a) Current-dependent output voltage, Uout; (b) Current-dependent heat flux, Q
Fig. S7 Aging-time dependent performance of Ni0.5Te/Te0.985Sb0.015/Ni0.5Te single-leg devices under a temperature difference of 180 K (Hot end: 473 K, Cold end: 293 K) (a, c) Current-dependent output voltages, Uout and (b, d) current-dependent heat flux, Q, after aging for (a, b) 3 and (c, d) 6-15 d; Aging-time dependent (e) open-circuit voltage, Uo and (f) internal resistance, Rin with inset in (f) showing internal resistivity, R, of the devices
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