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粉末冶金制备技术是制备兼具优异力学性能和热电性能Bi2Te3基块状材料的重要途径，但是粉末冶金制备过程中样品取向损失导致材料热电性能不高，开发具有强板织构、细晶粒Bi2Te3基热电材料的制备技术是高性能Bi2Te3基热电材料研究的重点。本文采用垂直转角挤压制备技术制备了系列p型Bi2Te3基材料，系统研究了挤压温度对材料微结构和织构特征的影响规律以及其对材料热电性能的影响规律，在垂直转角挤压过程中，材料经历了剧烈的塑性变形，导致材料内部晶粒的破碎、重排及偏转，同时挤压过程中高温有助于材料中晶粒的动态再结晶和生长过程，实现了晶粒的细化，773 K挤压样品在垂直于压力方向和平行于压力方向上分别取得了F(00l) = 0.51和F(110) = 0.30的高取向因子，即从热压样品中面织构向挤压样品中板织构的转变，这种微结构特征显著提升了样品的载流子迁移率，773 K挤压样品室温下载流子迁移率高达345.4 cm2·V-1·s-1，与区熔样品相当，表现出优异的电输运性能，室温下功率因子达到4.43 mW·m-1·K-2，与此同时，773 K挤压样品的晶格热导率和双极热导率之和在323 K时降低至最小值0.78 W·m-1·K-1，最终773 K挤压样品在323 K时获得最大ZT值1.13，较热压样品提高了近70 %。该研究为高性能强板织构、细晶粒Bi2Te3基热电材料的制备提供了新途径，为微型热电器件的制造奠定了重要基础。
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关键词:
- 垂直转角挤压制备技术 /
- 挤压温度 /
- 微结构 /
- 热电性能
The preparation technology of powder metallurgy is an important way to prepare Bi2Te3-based bulk materials with excellent mechanical properties and thermoelectric properties. However, the loss of sample orientation during the preparation of powder metallurgy results in low thermoelectric properties of the materials. The development of high-performance Bi2Te3-based thermoelectric materials with strong plate texture and fine grains is the focus of research on high-performance Bi2Te3-based thermoelectric materials. In this paper, a series of p-type Bi2Te3-based materials were prepared by vertical corner extrusion preparation technology. The influence of extrusion temperature on the microstructure and texture characteristics of the material and its influence on the thermoelectric properties of the material were systematically studied. During the vertical corner extrusion process, the grain preferentially grows along the minimum resistance direction in the direction perpendicular to the pressure, that is, along the extrusion direction, so that the (00l) texture of the original hot-pressed sample is further enhanced; while in the direction parallel to the pressure, due to the existence of friction with the inner wall of the die during the extrusion process, this frictional resistance will promote the inversion of the grain, so that the grain is arranged in a directional manner to achieve the effect of reducing the frictional resistance, thus forming the (110) texture that is not in the original hot-pressed sample in the extruded sample, and finally completing the surface weaving from the hot-pressed sample The transition of the structure to the plate texture of the extruded sample. When the extrusion temperature is low, the atomic diffusion rate is low, which limits the dynamic recrystallization of the grain, the grain growth process and the grain deflection speed. With the increase of the extrusion temperature, these processes can be carried out rapidly, so a more obvious plate texture characteristic is formed.The 773 K extruded sample achieved high orientation factors of F(00l) = 0.51 and F(110) = 0.30 in the direction perpendicular to the pressure and parallel to the pressure, respectively, and the carrier mobility was as high as 345.4 cm2·V-1·s-1 at room temperature, which was comparable to the zone melt sample and showed excellent electrical transport performance. The power factor reached 4.43 mW·m-1·K-2 at room temperature. At the same time, the sum of lattice thermal conductivity and bipolar thermal conductivity of the 773 K extruded sample decreased to a minimum value of 0.78 W·m-1·K-1 at 323 K. Finally, the 773 K extruded sample obtained a maximum ZT value of 1.13 at 323 K, which was nearly 70 % higher than that of the hot-pressed sample. This research provides a new way for the preparation of high-performance strong plate textures and fine-grained Bi2Te3-based thermoelectric materials, and lays an important foundation for the fabrication of micro thermoelectric devices.-
Keywords:
- vertical angular extrusion preparation technology /
- extrusion temperature /
- microstructure /
- thermoelectric properties
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