无机材料学报 ›› 2026, Vol. 41 ›› Issue (3): 303-310.DOI: 10.15541/jim20250264 CSTR: 32189.14.jim20250264
李鹏1(
), 仇鹏飞2(
), 江彬彬1(
), 肖杰2, 史迅2
收稿日期:2025-06-23
修回日期:2025-08-11
出版日期:2025-08-26
网络出版日期:2025-08-26
通讯作者:
仇鹏飞, 研究员. E-mail: qiupf@mail.sic.ac.cn;作者简介:李 鹏(1995-), 男, 博士. E-mail: pengli@whu.edu.cn
基金资助:
LI Peng1(
), QIU Pengfei2(
), JIANG Binbin1(
), XIAO Jie2, SHI Xun2
Received:2025-06-23
Revised:2025-08-11
Published:2025-08-26
Online:2025-08-26
Contact:
QIU Pengfei, professor. E-mail: qiupf@mail.sic.ac.cn;About author:LI Peng (1995-), male, PhD. E-mail: pengli@whu.edu.cn
Supported by:摘要:
基于埃廷豪森效应的热磁制冷是一种低温固态制冷技术, 具有控温精确、体积小、无振动、无噪声等优点。近年来, 拓扑半金属因兼具电子与空穴两种载流子及高迁移率, 在低温下表现出优异的热磁性能, 成为潜在候选材料。本研究采用固相反应与放电等离子烧结工艺制备了高致密度多晶TaSb2, 并系统测试其低温热磁输运性质。结果表明, 多晶TaSb2的能斯特热电势(Syx)在27 K附近达到最大值, 且表现出与磁场的正相关关系。多晶TaSb2在9 T、26 K条件下的能斯特功率因子((PF)N)达到315.1 μW·cm-1·K-2, 在9 T、22 K条件下的能斯特热电优值(zN)达到7.1×10-4 K-1, 均优于大部分已报道的多晶热磁材料。机理分析发现, 强双极效应、高载流子迁移率及显著的声子曳引效应共同提升了其热电势, 从而赋予材料优异的热磁性能。此外, 磁场可显著抑制低温下的电子热导率, 导致磁场下总热导率主要来自于晶格贡献。本研究为低温固态制冷提供了新的材料选择和设计思路, 然而得到的材料晶格热导率较高, 在一定程度上限制了材料性能, 未来通过声子工程降低晶格热导率有望进一步优化性能。
中图分类号:
李鹏, 仇鹏飞, 江彬彬, 肖杰, 史迅. 多晶TaSb2的热磁性能研究[J]. 无机材料学报, 2026, 41(3): 303-310.
LI Peng, QIU Pengfei, JIANG Binbin, XIAO Jie, SHI Xun. Thermomagnetic Performance of Polycrystalline TaSb2[J]. Journal of Inorganic Materials, 2026, 41(3): 303-310.
图1 多晶TaSb2的晶体结构、能带结构和物相分析
Fig. 1 Crystal structure, band structure and phase analysis of polycrystalline TaSb2 (a) Schematic representation of the unit cell; (b) Band structure with spin-orbit coupling considered; (c) Powder XRD pattern and Rietveld refinement results; (d) Secondary electron images of cross-section after acid pickling (upper left) and polished surface (upper right), and corresponding elemental mappings (lower)
图2 多晶TaSb2的电输运性质
Fig. 2 Electrical transport properties of polycrystalline TaSb2 Temperature dependences of (a) Seebeck thermopower Sxx, (b) Nernst thermopower Syx, (c) electrical resistivity ρyy, and (d) Nernst power factor (PF)N of polycrystalline TaSb2 under different magnetic fields
图3 多晶TaSb2的电输运性能分析
Fig. 3 Analysis of the electrical transport properties of polycrystalline TaSb2 (a, b) Comparison between experimental data and two-carrier model fitting results for (a) resistivity ρyy and (b) Hall resistivity ρyx of polycrystalline TaSb2 (dots representing experimental data and lines representing fitting results); (c) Temperature dependences of electron concentration ne and hole concentration nh in polycrystalline TaSb2 with inset showing temperature dependences of electron mobility μe and hole mobility μh; (d, e) Comparison between experimental and theoretical values of Nernst thermopower Syx at (d) low temperatures (15, 25, 35 and 50 K) and (e) high temperatures (above 150 K); (f) Contributions of thermal diffusion and phonon drag to the thermopower of electrons (${S}_{\text{d}}^{\text{e}}$ and ${S}_{\text{p}}^{\text{e}}$) and holes (${S}_{\text{d}}^{\text{h}}$ and ${S}_{\text{p}}^{\text{h}}$)
图4 多晶TaSb2的热输运性质与性能评价
Fig. 4 Thermal transport properties and performance evaluation of polycrystalline TaSb2 (a) Temperature dependence and (b) magnetic field dependence of thermal conductivity κxx of polycrystalline TaSb2; (c) Temperature dependence and (d) magnetic field dependence of Nernst figure-of-merit zN of polycrystalline TaSb2
| T/K | κl/(W·m-1·K-1) | κc(0, T)/(W·m-1·K-1) | η/T-1 | s |
|---|---|---|---|---|
| 5 | 1.17 | 5.92 | 1.190 | 1.41 |
| 15 | 13.71 | 11.68 | 0.790 | 1.58 |
| 25 | 36.81 | 12.72 | 0.400 | 1.54 |
| 50 | 45.83 | 9.26 | 0.114 | 1.45 |
| 100 | 29.66 | 7.14 | 0.043 | 1.56 |
| 150 | 21.47 | 7.85 | 0.033 | 1.88 |
| 200 | 17.51 | 8.34 | 0.029 | 1.81 |
| 250 | 15.49 | 8.41 | 0.026 | 1.91 |
| 300 | 14.90 | 8.53 | 0.023 | 1.90 |
表1 TaSb2热导率的拟合参数
Table 1 Parameters used to fit the thermal electric conductivity of polycrystalline TaSb2
| T/K | κl/(W·m-1·K-1) | κc(0, T)/(W·m-1·K-1) | η/T-1 | s |
|---|---|---|---|---|
| 5 | 1.17 | 5.92 | 1.190 | 1.41 |
| 15 | 13.71 | 11.68 | 0.790 | 1.58 |
| 25 | 36.81 | 12.72 | 0.400 | 1.54 |
| 50 | 45.83 | 9.26 | 0.114 | 1.45 |
| 100 | 29.66 | 7.14 | 0.043 | 1.56 |
| 150 | 21.47 | 7.85 | 0.033 | 1.88 |
| 200 | 17.51 | 8.34 | 0.029 | 1.81 |
| 250 | 15.49 | 8.41 | 0.026 | 1.91 |
| 300 | 14.90 | 8.53 | 0.023 | 1.90 |
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