Mg-Si-Sn基热电器件电极材料的优化选择与连接工艺

doi:10.15541/jim20140623

无机材料学报 ›› 2015, Vol. 30 ›› Issue (6): 639-646.DOI: 10.15541/jim20140623

Mg-Si-Sn基热电器件电极材料的优化选择与连接工艺

陈耿^1,2, 刘桃香^1,2, 唐新峰², 苏贤礼², 鄢永高²

(武汉理工大学 1. 材料科学与工程学院; 2. 材料复合新技术国家重点实验室, 武汉 430070)

收稿日期:2014-12-01 修回日期:2015-02-04 出版日期:2015-06-04 网络出版日期:2015-05-22
作者简介:陈耿(1987–), 男, 硕士研究生. E-mail: chengeng17@126.com
基金资助:
国家重大基础研究计划973项目(2013CB632502);国家自然科学基金(51402222, 51172174, 51401153);国家111计划(B07040)

Optimization of Electrode Material and Connecting Process for Mg-Si-Sn Based Thermoelectric Device

CHEN Geng^1,2, LIU Tao-Xiang^1,2, TANG Xin-Feng², SU Xian-Li², YAN Yong-Gao²

(1. School of materials science and engineering, Wuhan University of Technology, Wuhan 430070, China; 2. StateKey Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China)

Received:2014-12-01 Revised:2015-02-04 Published:2015-06-04 Online:2015-05-22
About author:CHEN Geng. E-mail: chengeng17@126.com
Supported by:
National Basic Research Program of China (973 Program) (2013CB632502);National Natural Science Foundation of China (51402222, 51172174, 51401153);111 Project of China (B07040)

摘要/Abstract

摘要：

研究了采用不同放电等离子烧结(SPS)工艺获得的单质金属(Ni、Cu、Ag、Al)电极与Mg-Si-Sn基热电材料结合界面的微观形貌和成分分布特征, 测试了合金(Ni-Al、Cu-Al)、金属/合金复合电极材料的热膨胀系数、电导率和热导率等物性参数。实验结果表明: 通过SPS烧结可以有效实现电极材料与Mg-Si-Sn基材料的连接, 复合电极材料Ni-Al/Al(60:40)和Cu-Al/Cu(45:55)具有高的电导率和热导率, 并且热膨胀系数与Mg-Si-Sn基热电材料相匹配, 有可能成为Mg-Si-Sn基材料的较理想电极材料。

关键词: 镁硅锡, 热电材料, 电极材料

Abstract:

Metal (Ni, Cu, Ag, Al) electrode was connected with Mg-Si-Sn based thermoelectric materials by Spark Plasma Sintering (SPS) process. Microstructure of interface, sintering process and transport properties, including electrical conductivity, thermal conductivity and thermal expansion coefficient, of electrode materials were investigated. The results showed that composites of Ni-Al /Al (60:40) and Cu-Al/Cu (45:55) displayed high electrical conductivity, high thermal conductivity and suitable thermal expansion coefficient to Mg-Si-Sn based materials. It is indicated that the two composites have potential to be used as good electrode materials for, and to be connected by SPS sintering to, Mg-Si-Sn based materials.

Key words: Mg-Si-Sn, thermoelectric material, electrode material

中图分类号:

TB34

陈耿, 刘桃香, 唐新峰, 苏贤礼, 鄢永高. Mg-Si-Sn基热电器件电极材料的优化选择与连接工艺[J]. 无机材料学报, 2015, 30(6): 639-646.

CHEN Geng, LIU Tao-Xiang, TANG Xin-Feng, SU Xian-Li, YAN Yong-Gao. Optimization of Electrode Material and Connecting Process for Mg-Si-Sn Based Thermoelectric Device[J]. Journal of Inorganic Materials, 2015, 30(6): 639-646.

图/表 10

图1 Ni电极与Mg-Si-Sn基材料结合界面背散射和线扫描成分分布图

Fig. 1 Back scattering images and line profiles of the interface between Ni and Mg-Si-Sn by EMPA (a-b) BSE photographs of the joint between Ni and Mg-Si-Sn; (c) BSE photographs of Mg-Si-Sn; (d-e) Line profiles of the joint Arrows point to the cracks

图2 金属电极和Mg-Si-Sn基材料的热膨胀系数(CTE)随温度的变化关系

Fig. 2 Temperature dependence of CTE for metal electrodes and Mg-Si-Sn

图3 一步法烧结的电极材料与Mg-Si-Sn基材料样品照片

Fig. 3 Pictures of samples sintered by one step SPS (a) Sectional view of Cu/Mg-Si-Sn; (b) Sectional view of Ag/Mg-Si- Sn; (c) Mg-Si-Sn of Al/Mg-Si-Sn

图4 Cu电极与Mg-Si-Sn基材料结合界面背散射和线扫描成分分布图

Fig. 4 Back scattering images and line profiles of the interface between Cu and Mg-Si-Sn by EMPA (a-c) Holding for 10 min and with cooling rate of 20 K/min; (a) BSE photograph; (b-c) line profiles; Inset photograph in (a) is BSE photograph of the joint with rapid cooling process; (d-f) Holding for 20 min and with cooling rate of 10 K/min; (d) BSE photograph; (e-f) line profiles

图5 Ag电极与Mg-Si-Sn基材料结合界面背散射和线扫描成分分布图

Fig. 5 Back scattering images and line profiles of the interface between Ag and Mg-Si-Sn by EMPA (a-c) Holding for 5 min with cooling rate of 20 K/min; (a) BSE photograph; (b-c) Line profiles; Circles represent the region of Ag and Mg rich area; (d-f) Holding for 10 min with cooling rate of 10 K/min; (d) BSE photograph; (e-f) Line profiles

图6 Al电极与Mg-Si-Sn基材料结合界面背散射和线扫描成分分布图

Fig. 6 Back scattering images and line profiles of the interface between Al and Mg-Si-Sn by EMPA (a-c) Holding for 5 min with cooling rate of 20 K/min; (a) BSE photograph; (b-c) Line profiles (d-f) Holding for 10 min with cooling rate of 10 K/min; (d) BSE photograph; (e-f) Line profiles

图7 合金原料粉末的XRD图谱

Fig. 7 XRD patterns of raw materials.

图8 SPS烧结合金块体的基本物性与温度关系

Fig. 8 Temperature dependence of basic physical properties for alloy material

图9 Ni-Al/Al的基本物性随温度的变化关系

Fig. 9 Physical properties as a function of temperature for Ni-Al/Al

图10 Cu-Al/Cu的基本物性随温度的变化关系

Fig. 10 Physical properties as a function of temperature for Cu-Al/Cu

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Mg-Si-Sn基热电器件电极材料的优化选择与连接工艺

Optimization of Electrode Material and Connecting Process for Mg-Si-Sn Based Thermoelectric Device

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