Yb0.3Co4Sb12/Mo-Cu热电元件的界面结构与界面电阻

doi:10.15541/jim20140378

无机材料学报 ›› 2015, Vol. 30 ›› Issue (3): 256-260.DOI: 10.15541/jim20140378 CSTR: 32189.14.10.15541/jim20140378

Yb_0.3Co₄Sb₁₂/Mo-Cu热电元件的界面结构与界面电阻

唐云山^{1, 2}, 柏胜强², 任都迪², 廖锦城², 张澜庭¹, 陈立东²

(1. 上海交通大学材料科学与工程学院, 上海200240; 2. 中国科学院上海硅酸盐研究所能源材料研究中心, 上海200050)

收稿日期:2014-07-22 修回日期:2014-10-20 出版日期:2015-03-20 网络出版日期:2015-03-06
作者简介:唐云山(1984–), 男, 硕士研究生. E-mail: tys280@mail.sic.ac.cn
基金资助:
国家973计划项目 (2013CB632504);国家自然科学基金(51102260);国家国际科技合作项目(2011DFB60150);上海市科委技术标准专项基金(13DZ0501803)

Interface Structure and Electrical Property of Yb_0.3Co₄Sb₁₂/Mo-Cu Element Prepared by Welding Using Ag-Cu-Zn Solder

TANG Yun-Shan^{1, 2}, BAI Sheng-Qiang², REN Du-Di², LIAO Jin-Cheng², ZHANG Lan-Ting¹, CHEN Li-Dong²

(1. School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai 200240, China; 2. CAS Key Laboratory of Energy-conversation Materials, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China)

Received:2014-07-22 Revised:2014-10-20 Published:2015-03-20 Online:2015-03-06
About author:TANG Yun-Shan. E-mail: tys280@mail.sic.ac.cn
Supported by:
National Basic Research Program of China (2013CB632504);National Natural Science Foundation of China (51102260);International S＆T Cooperation Program of China(2011DFB60150);Program of Shanghai Science Technology Committee (Special Technical Standards 13DZ0501803)

摘要/Abstract

摘要： 通过放电等离子烧结(SPS)实现阻挡层Ti-Al、过渡焊接层Ni与热电臂Yb_0.3Co₄Sb₁₂的一体化烧结, 使用Ag-Cu-Zn共晶合金完成热电元件Yb_0.3Co₄Sb₁₂/Ti-Al/Ni与Mo-Cu电极的钎焊连接。扫描电镜(SEM)显示出Yb_0.3Co₄Sb₁₂/Ti-Al/Ni/Ag-Cu-Zn/Mo-Cu接头中各界面结合良好, 无裂纹, 成分分析发现Yb_0.3Co₄Sb₁₂/Ti-Al界面存在AlCo、TiCoSb及TiSb₂等金属间化合物(IMC)。500℃下等温时效30 d后, Yb_0.3Co₄Sb₁₂/Ti-Al界面处的金属间化合物厚度无明显变化; Ag-Cu-Zn/Ni界面处Cu、Zn扩散趋于稳定, Cu-Zn扩散层厚度达到约40 μm。界面接触电阻测试结果表明, 等温时效前后Yb_0.3Co₄Sb₁₂/Ti-Al/Ni/Ag-Cu-Zn/Mo-Cu元件的界面接触电阻率均低于10 μΩ·cm²。

null

关键词: 热电元件, 放电等离子烧结, 钎焊, 接触电阻率

Abstract:

The barrier layer of Ti-Al and the contact layer of Ni were joined to Yb_0.3Co₄Sb₁₂ simultaneously by using spark plasma sintering (SPS) technique. The Mo-Cu electrode was then welded to thermoelectric element Yb_0.3Co₄Sb₁₂/Ti-Al/Ni by using Ag-Cu-Zn alloy as solder. SEM results show that there are no cracks at the interfaces of Yb_0.3Co₄Sb₁₂/Ti-Al/Ni/Ag-Cu-Zn/Mo-Cu thermoelectric joints. The EDS analysis shows that intermetallic compounds (IMCs) layer containing AlCo, TiCoSb and TiSb₂ phases are formed at the interface between Yb_0.3Co₄Sb₁₂ and Ti-Al. After thermal aging at 500℃ for 30 d, the inter-diffusions at both Yb_0.3Co₄Sb₁₂/Ti-Al interface and Ag-Cu-Zn/Ni interface tend to be steady. The contact electrical resistivity of the Yb_0.3Co₄Sb₁₂/ Ti-Al/Ni/Ag-Cu-Zn/Mo-Cu thermoelectric joints are about 6.1 μΩ·cm²after welding, and it maintained as low as 10 μΩ·cm² even after thermal aged for 30 d.

Key words: thermoelectric element, SPS, braze, contact electrical resistivity

中图分类号:

TN377

唐云山, 柏胜强,任都迪,廖锦城,张澜庭, 陈立东. Yb_0.3Co₄Sb₁₂/Mo-Cu热电元件的界面结构与界面电阻[J]. 无机材料学报, 2015, 30(3): 256-260.

TANG Yun-Shan, BAI Sheng-Qiang, REN Du-Di, LIAO Jin-Cheng, ZHANG Lan-Ting, CHEN Li-Dong. Interface Structure and Electrical Property of Yb_0.3Co₄Sb₁₂/Mo-Cu Element Prepared by Welding Using Ag-Cu-Zn Solder[J]. Journal of Inorganic Materials, 2015, 30(3): 256-260.

图/表 8

图1 SPS烧结得到的Yb0.3Co4Sb12/Ti-Al/Ni断面SEM照片

Fig. 1 SEM image of Yb0.3Co4Sb12/Ti-Al/Ni cross section after SPS

图2 SPS烧结后的Yb0.3Co4Sb12/Ti-Al/Ni界面A点至B点线扫描图像

Fig. 2 SEM image and line-scan EDS of Yb0.3Co4Sb12/ Ti-Al/Ni interface from A to B after SPS

图3 SPS烧结后的Yb0.3Co4Sb12/Ti-Al界面不同位置处IMC能谱分析结果

Fig. 3 EDS analyses of IMC layer at Yb0.3Co4Sb12/Ti-Al interface region after SPS

图4 SPS烧结得到的Yb0.3Co4Sb12/Ti-Al/Ni界面电阻

Fig. 4 Electrical resistance of Yb0.3Co4Sb12/Ti-Al/Ni interface after SPS

图5 500℃下不同时间热时效热电元件的SEM照片

Fig. 5 SEM images of thermoelectric elements after thermal aging at 500℃ for different period (a) 0 d; (b) 10 d; (c) 20 d; (d) 30 d

图6 500℃热时效30 d后的Mo-Cu/Ag-Cu-Zn/Ni界面C点至D点线扫描图像

Fig. 6 Line analysis of Mo-Cu/Ag-Cu-Zn/Ni interface from C to D after thermal aging at 500℃ for 30 d

图7 不同时间热时效钎焊后元件的电阻扫描图

Fig. 7 Electrical resistance of thermoelectric elements after thermal aging at 500℃ for different period

表1 钎焊热电元件500℃热时效后界面接触电阻率

Table1 Contact electrical resistivity of thermoelectric elements after thermal aging at 500℃

Time/d	0	10	20	30
Contact electrical resistivity/ (μΩ·cm²)	6.1	8.0	8.9	9.8

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Yb_0.3Co₄Sb₁₂/Mo-Cu热电元件的界面结构与界面电阻

Interface Structure and Electrical Property of Yb_0.3Co₄Sb₁₂/Mo-Cu Element Prepared by Welding Using Ag-Cu-Zn Solder

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