Se掺杂量对n型Bi2Te3-xSex微结构及热电性能的影响

doi:10.15541/jim20140085

摘要/Abstract

摘要：

通过水热法合成不同Se掺杂量的Bi₂Te_3-_xSe_x (0 ≤x ≤0.45)纳米粉体, 采用放电等离子烧结技术, 制备出致密度较高的块体材料。通过X射线衍射、扫描电镜、透射电镜等测试手段对材料的微结构进行了表征, 并重点研究了含有不同Se掺杂量块体材料的显微结构和热电性能。结果表明: Se元素的掺杂使得粉体XRD特征衍射峰向高角度偏移, 并且衍射峰出现宽化, 晶粒尺寸变小。随着Se掺杂量的增加, 块体材料的电导率先增大后减小; Se元素的掺杂有效地降低了材料的热导率, 并提高了材料的Seebeck系数。研究结果表明: 在整个测试温度区间, 所有经过Se掺杂的样品ZT值都高于未掺杂样品。当Se掺杂量为0.3时, 样品具有最大的ZT值, 平均约为0.51, 并在475 K时达到最大值0.57, 相比未经Se掺杂的Bi₂Te₃提高了159%。

关键词: 碲化铋, 硒掺杂, 水热合成, 放电等离子体烧结, 热电性能

Abstract:

A hydrothermal method combined with a subsequent spark plasma sintering technique was successfully utilized to synthesize selenium (Se) doped bismuth telluride (Bi₂Te_3-_xSe_x) (0≤x≤0.45). The influence of Se-doping on the composition and morphology of n-type Bi₂Te_3-_xSe_x was studied by X-ray diffraction, scanning electron microscope and transmission electron microscope. Thermoelectric properties of the as-prepared bulk Bi₂Te_3-_xSe_x nanocomposites were investigated in detail. Results showed that the grain became finer by the Se-doping. With increasing Se doping content, the electrical conductivity of bulk Bi₂Te_3-_xSe_x increased firstly and then decreased. Se-doping effectively reduced the thermal conductivity and improved the Seebeck coefficient to some extent. Consequently, a maximum ZT value of 0.57 was obtained from bulk Bi₂Te_2.7Se_0.3 at 475 K, which was increased by 159% as compared with pure bulk Bi₂Te₃.

Key words: bismuth telluride, Se-doping, hydrothermal synthesis, spark plasma sintering, thermoelectric properties

中图分类号:

TN304

张骐昊, 徐磊磊, 王连军, 江莞. Se掺杂量对n型Bi₂Te_3-_xSe_x微结构及热电性能的影响[J]. 无机材料学报, 2014, 29(11): 1139-1144.

ZHANG Qi-Hao, XU Lei-Lei, WANG Lian-Jun, JIANG Wan. Effects of Different Amount of Se-doping on Microstructures and Thermoelectric Properties of n-type Bi₂Te_3-_xSe_x[J]. Journal of Inorganic Materials, 2014, 29(11): 1139-1144.

图/表 8

图1 不同Se掺杂量的Bi2Te3-xSex纳米粉体的XRD图谱

Fig. 1 XRD patterns of Bi2Te3-xSex nanopowders being doped with different Se-doping contents

图2 不同Se掺杂量的Bi2Te3-xSex纳米粉体的场发射扫描电镜和透射电镜照片

Fig. 2 FE-SEM and HRTEM images of Bi2Te3-xSex nano-powder being doped with different Se contents SEM images of (a) Bi2Te2.9Se0.1, (b) Bi2Te2.7Se0.3 and (c) Bi2Te2.55Se0.45, HRTEM image of (d) Bi2Te2.55Se0.45 nanopowder

图3 不同Se掺杂量的Bi2Te3-xSex块体的断面形貌

Fig. 3 Fractured surfaces′ morphologies of bulk Bi2Te3-xSex being doped with different Se contents (a) Bi2Te3; (b) Bi2Te2.9Se0.1; (c) Bi2Te2.85Se0.15; (d) Bi2Te2.7Se0.3; (e) and (f) Bi2Te2.55Se0.45

表1 不同Se掺杂量的Bi2Te3-xSex块体密度及相对密度

Tables 1 Densities and relative densities of Bi2Te3-xSex bulk samples being doped with different Se contents

Sample	Bi₂Te₃	Bi₂Te_2.9Se_0.1	Bi₂Te_2.85Se_0.15	Bi₂Te_2.7Se_0.3	Bi₂Te_2.55Se_0.45
Density/(g·cm^-3)	7.820	7.755	7.760	7.753	7.759
Relative density	99.52%	98.92%	98.98%	99.02%	99.16%

图4 不同Se掺杂量的Bi2Te3-xSex块体的电导率随温度的变化关系

Fig. 4 Temperature dependence of electrical conductivity for Bi2Te3-xSex bulk samples being doped with different Se contents

图5 不同Se掺杂量的Bi2Te3-xSex块体的Seebeck系数随温度的变化关系

Fig. 5 Temperature dependence of Seebeck coefficient for Bi2Te3-xSex bulk samples being doped with different Se contents

图 6 不同Se掺杂量的Bi2Te3-xSex块体(a)热导率和(b)晶格热导率随温度的变化关系

Fig. 6 Temperature dependence of (a) thermal conductivity and (b) lattice thermal conductivity for Bi2Te3-xSex bulk samples being doped with different Se contents

图7 不同Se掺杂量的Bi2Te3-xSex块体的ZT值随温度的变化关系

Fig. 7 Temperature dependence of ZT for Bi2Te3-xSex bulk samples being doped with different Se contents

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Se掺杂量对n型Bi₂Te_3-_xSe_x微结构及热电性能的影响

Effects of Different Amount of Se-doping on Microstructures and Thermoelectric Properties of n-type Bi₂Te_3-_xSe_x

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