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晶粒细化是提高Bi2Te3基热电材料力学性能的重要方法, 但晶粒细化过程中伴随的类施主效应严重劣化了材料的热电性能, 并且一旦产生类施主效应, 就很难通过简单的热处理等工艺消除. 本文系统研究n型Bi2Te3基化合物烧结前粉体颗粒尺寸对材料类施主效应和热电性能的影响规律. 随着颗粒尺寸减小, 氧诱导的类施主效应明显增强, 载流子浓度从10 M烧结样品的3.36×1019 cm–3急剧增加到120 M烧结样品的7.33×1019 cm–3, 严重偏离最佳载流子浓度2.51×1019 cm–3, 热电性能严重劣化. 当粉体颗粒尺寸为1—2 mm时, 烧结样品的Seebeck系数为–195 μV/K, 载流子浓度为3.36×1019 cm–3, 与区熔样品沿着ab面方向的Seebeck系数为–203 μV/K和载流子浓度为2.51×1019 cm–3相近, 未表现出明显的类施主效应, 可作为粉末冶金工艺的优质原料. 18 M烧结样品获得最大ZT值为0.75, 进一步增强织构有望获得优异的热电性能. 本研究为调控和有效抑制类施主效应的产生提供了新方法和途径, 为采用粉末冶金工艺制备具有优异热电性能和力学性能材料提供了重要指导.
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关键词:
- Bi2Te3基化合物 /
- 颗粒尺寸 /
- 类施主效应 /
- 热电性能
Grain size refinement is the vital stratagem for improving mechanical properties of Bi2Te3-based thermoelectric material. However, the donor-like effect induced by grain size refinement seriously deteriorates the thermoelectric properties especially near room temperature. Once the donor-like effect is generated, it is very difficult to eliminate the donor-like effect by the simple heat treatment process and other processes. In this study, the influences of particle size on the donor-like effect and thermoelectric properties are systematically studied for Bi2Te3-based compounds. As the particle size decreases, the donor-like effect is enhanced significantly. The oxygen-induced donor-like effect dramatically increases the carrier concentration from 3.36× 1019 cm–3 for 10 M sintered sample to 7.33×1019 cm–3 for 120 M sintered sample, which is largely beyond the optimal carrier concentration of 2.51×1019 cm–3 and seriously deteriorates the thermoelectric properties. However, when the particle size of the powder is 1–2 mm, the Seebeck coefficient of –195 μV/K and the carrier concentration of 3.36×1019 cm–3 near room temperature are achieved, which are similar to those of the ZM sample with the Seebeck coefficient of –203 μV/K and the carrier concentration of 2.51×1019 cm–3. The powders without the obvious donor-like effect can be used as the excellent raw material for powder metallurgy process. A maximum ZT value of 0.75 is achieved for the 18 M sintered sample. The excellent thermoelectric properties are expected to be obtained by enhancing the texture further. This study provides a new way to regulate and effectively suppress the generation of the donor-like effect, and provides an important guidance for the preparation of materials with excellent thermoelectric and mechanical properties by powder metallurgy process.-
Keywords:
- Bi2Te3-based compound /
- particle size /
- donor-like effect /
- thermoelectric properties
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图 1 (a) 不同粉体颗粒尺寸Bi2Te2.79Se0.21烧结样品的粉体XRD图谱; (b) 垂直于烧结压力方向的块体XRD图谱
Fig. 1. (a) Powder XRD patterns of Bi2Te2.79Se0.21 samples sintered with different particle sizes of powders; (b) bulk XRD patterns of samples measured perpendicular to the pressing direction.
图 2 (a), (b) 10 M样品沿着垂直和平行于烧结压力方向断裂截面的场发射扫描电子显微镜图像(FESEM); (c) 10 M样品抛光表面的背散射电子图像; (d)—(f) 图(c)中Bi-Te-Se元素的能谱面扫描图(EDS-Map)
Fig. 2. (a), (b) Field emission scanning electron microscope images of fractured surfaces of the 10 M sample measured perpendicular to and parallel to the pressing direction; (c) backscattered electron images of polished surfaces of the 10 M sample; (d)–(f) EDS elemental mapping of Bi, Te, and Se of Fig. 2 (c).
图 3 区熔锭体沿ab面方向和Bi2Te2.79Se0.21烧结样品沿着(a), (c), (e)垂直和(b), (d), (f)平行于压力方向的电输运性能与温度的关系曲线 (a), (b) 电导率; (c), (d) Seebeck系数; (e), (f) 功率因子
Fig. 3. Temperature dependence of (a), (b) the electrical conductivity, (c), (d) Seebeck coefficient, and (e), (f) power factor for the zone melt (ZM) sample measured along the ab-plane and Bi2Te2.79Se0.21 sintered samples measured (a), (c), (e) perpendicular to and (b), (d), (f) parallel to the pressing direction, respectively.
图 4 室温下Bi2Te2.79Se0.21烧结样品沿垂直于烧结压力方向的性质 (a)载流子浓度n和迁移率μ与颗粒尺寸的关系; (b)样品Seebeck系数与载流子浓度的关系曲线, 以及单抛带模型计算载流子有效质量
Fig. 4. Properties for Bi2Te2.79Se0.21 sintered samples measured perpendicular to the pressing direction at room temperature: (a) The relationship of carrier concentration n and carrier mobility μ to the size of powder; (b) Seebeck coefficients as a function of the charge carrier concentration, where the solid lines are Pisarenko plots based on the single parabolic band model.
图 5 区熔锭体沿着ab面方向和Bi2Te2.79Se0.21烧结样品沿着(a), (c), (e)垂直和(b), (d), (f)平行于烧结压力方向的热输运性能和热电优值与温度的关系曲线 (a), (b) 总热导率; (c), (d) 晶格热导率; (e), (f) 无量纲热电优值ZT
Fig. 5. Temperature dependence of (a), (b) total thermal conductivity, (c), (d) lattice thermal conductivity, and (e), (f) dimensionless thermoelectric figure of merit ZT value for the ZM sample measured along the ab-plane and Bi2Te2.79Se0.21 sintered samples measured (a), (c), (e) perpendicular to and (b), (d), (f) parallel to the pressing direction, respectively.
表 1 烧结块体样品垂直于压力方向的取向因子、密度和致密度
Table 1. Orientation factor F value, density, and relative density of sintered bulk samples perpendicular to the pressing direction.
目数 10 M 18 M 35 M 50 M 65 M 120 M F(0 0 l) 0.43 0.36 0.39 0.30 0.25 0.20 密度 6.98 7.06 7.13 7.27 7.42 7.69 致密度/% 89.2 90.3 91.2 93.0 94.9 98.3 
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[1] Wang Y, Liu W D, Shi X L, Hong M, Wang L J, Li M, Wang H, Zou J, Chen Z G 2020 Chem. Eng. J. 391 123513
Google Scholar
[2] Deng R G, Su X L, Zheng Z, Liu W, Yan Y G, Zhang Q, Dravid V P, Uher C, Kanatzidis M G, Tang X F 2018 Sci. Adv. 4 5606
Google Scholar
[3] Liu W S, Zhang Q, Lan Y, Chen S, Yan X, Zhang Q, Wang H, Wang D, Chen G, Ren Z 2011 Adv. Energy Mater. 1 577
Google Scholar
[4] Sun M, Tang G W, Wang H F, Zhang T, Zhang P Y, Han B, Yang M, Zhang H, Chen Y C, Chen J, Chen D D, Gan J L, Qian Q, Yang Z M 2022 Adv. Mater. 34 2202942
Google Scholar
[5] Hu L P, Zhu T J, Liu X H, Zhao X B 2014 Adv. Funct. Mater. 24 5211
Google Scholar
[6] Tao Q R, Deng R G, Li J, Yan Y G, Su X L, Poudeu P F P, Tang X F 2020 ACS Appl. Mater. Interfaces 12 26330
Google Scholar
[7] Hu L P, Wu H J, Zhu T J, Fu C G, He J Q, Ying P J, Zhao X B 2015 Adv. Energy Mater. 5 1500411
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[8] Zhao L D, Zhang B P, Li J F, Zhang H L, Liu W S 2008 Solid State Sci. 10 651
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[9] Liu Y, Zhang Y, Lim K H, Ibáñez M, Ortega S, Li M, David J, Martí-Sánchez S, Ng K M, Arbiol J, Kovalenko M V, Cadavid D, Cabot A 2018 ACS Nano 12 7174
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[12] Tao Q R, Wu H J, Pan W F, Zhang Z K, Tang Y F, Wu Y T, Fan Y J, Chen Z Q, Wu J S, Su X L, Tang X F 2021 ACS Appl. Mater. Interfaces 13 60216
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Google Scholar
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Google Scholar
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Google Scholar
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Hu W W, Sun J C, Zhang Y, Gong Y, Fan Y T, Tang X F, Tan G J 2022 Acta Phys. Sin. 71 047101
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