Ag掺杂SnSe化合物的制备及热电性能

doi:10.15541/jim20150599

无机材料学报 ›› 2016, Vol. 31 ›› Issue (7): 751-755.DOI: 10.15541/jim20150599 CSTR: 32189.14.10.15541/jim20150599

Ag掺杂SnSe化合物的制备及热电性能

李松浩¹, 张忻¹, 刘洪亮¹, 郑亮¹, 张久兴^{1, 2}

(1. 北京工业大学材料科学与工程学院, 新型功能材料教育部重点实验室北京 100124; 2. 合肥工业大学材料科学与工程学院, 合肥 230009)

收稿日期:2015-12-01 修回日期:2016-01-13 出版日期:2016-07-20 网络出版日期:2016-06-22
作者简介:李松浩(1990–), 男, 硕士研究生. E-mail: vinceli1990@hotmail.com
基金资助:
北京市教育委员会科技计划面上项目(KM201510005001)

Synthesis and Thermoelectric Properties of Ag-doped SnSe

LI Song-Hao¹, ZHANG Xin¹, LIU Hong-Liang¹, ZHENG Liang¹, ZHANG Jiu-Xing^1,2

(1. The Key Laboratory of Advanced Functional Material of Education Ministry, School of Materials Science and Engineering, Beijing University of technology, Beijing 100124, China. 2. School of Materials Science and Engineering, Hefei University of technology, Hefei 230009, China)

Received:2015-12-01 Revised:2016-01-13 Published:2016-07-20 Online:2016-06-22
About author:LI Song-Hao. E-mail: vinceli1990@hotmail.com

摘要/Abstract

摘要：

SnSe是一种潜在的极具应用前景的热电材料。采用机械合金化结合放电等离子烧结的方法制备了Ag掺杂的Sn_1-_xAg_xSe (0.005≤x≤0.03)多晶块体热电材料, 并借助XRD、SEM、电热输运测试系统研究了其物相组成、微结构与电热输运性能。XRD分析结果表明, 少量Ag(0.005≤x≤0.01)掺杂仍然能够成功制备出单相斜方结构SnSe化合物, 但随着Ag掺杂量的增加, 基体中出现SnAgSe₂第二相, 且第二相含量逐渐增加。掺杂Ag大幅度提高了载流子浓度, 从而使材料的综合电输运性能(功率因子)显著提高, 当Ag掺杂量x=0.02时, 功率因子提高至4.95×10^-4W/(m·K²), 较未掺杂SnSe样品提高了36%。尽管掺杂样品的热导率均有小幅升高, 无量纲热电优值(ZT)仍获得一定改善。当Ag掺杂量x=0.02时, Sn_0.98Ag_0.02Se成分样品具有较高的热电优值, 并在823 K附近达到最高值0.82。

关键词: SnSe, Ag掺杂, 放电等离子烧结, 热电性能

Abstract:

SnSe material is one of the most promising state-of-art thermoelectric materials. The polycrystalline Ag-doped Sn_1-_xAg_xSe (0.005≤x≤0.03) bulks were prepared by mechanical alloying and spark plasma sintering technique, and the composition, microstructure and thermoelectric properties were systematically studied by XRD, SEM and thermoelectric performance measurement. XRD results show that single-phase orthorhombic SnSe-based compounds can be prepared with small amount of Ag-doping (0.005≤x≤0.01), but with Ag doping amount increasing, small quantity of secondary phase, SnAgSe₂, can be detected in the matrix. The carrier concentration and overall electrical properties (power factor) are significantly enhanced as a result of Ag doping. The power factor of Sn_0.98Ag_0.02Se increases up to 0.495×10^-3W/(m·K²), which is about 36% higher than that of SnSe material. Although the thermal conductivity increases slightly, the dimensionless figure of merit, ZT is still optimized for the Ag-doped samples. Sn_0.98Ag_0.02Se bulk shows optimal ZT value and the highest ZT of 0.82 is obtained at 823 K, which is the highest value reported for the polycrystalline SnSe-based thermoelectric materials.

Key words: SnSe, Ag-doped, Spark plasma sintering, thermoelectric property

中图分类号:

TB34

李松浩, 张忻, 刘洪亮, 郑亮, 张久兴. Ag掺杂SnSe化合物的制备及热电性能[J]. 无机材料学报, 2016, 31(7): 751-755.

LI Song-Hao, ZHANG Xin, LIU Hong-Liang, ZHENG Liang, ZHANG Jiu-Xing. Synthesis and Thermoelectric Properties of Ag-doped SnSe[J]. Journal of Inorganic Materials, 2016, 31(7): 751-755.

图/表 4

图1 Sn1-xAgxSe合金烧结块体的XRD图谱

Fig. 1 XRD patterns of the sintered Sn1-xAgxSe alloys bulks

图2 (a)烧结的SnSe样品和(b)Ag掺杂量x=0.02样品的断口SEM照片

Fig. 2 Fractured surface images of (a) SnSe and (b) Sn0.98Ag0.02Se

图3 Sn1-xAgxSe合金的热电性能与温度的关系

Fig. 3 Temperature dependence of thermoelectric properties for Sn1-xAgxSe alloys (a) Electrical resistivity; (b) Seebeck coefficient; (c) Power factor; (d) Thermal conductivity; (e) Lattice thermal conductivity; (f) Figure of merit ZT

表1 样品的部分物理参数

Table 1 Some physical properties of the samples prepared

Component		Carrier concentration, n/cm³	Mobility, μ_h/(cm²·V^-1·s^-1)
SnSe	14,.95	4.185×10¹⁷	1.370
Sn_0.995Ag_0.005Se	3.02	2.065×10¹⁸	0.827
Sn_0.99Ag_0.01Se	2.21	2.972×10¹⁸	1.121
Sn_0.985Ag_0.015Se	1.65	3.793×10¹⁸	1.194
Sn_0.98Ag_0.02Se	1.19	4.566×10¹⁸	1.251
Sn_0.97Ag_0.03Se	0.88	5.854×10¹⁸	1.376

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Ag掺杂SnSe化合物的制备及热电性能

Synthesis and Thermoelectric Properties of Ag-doped SnSe

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