研究论文

La掺杂PCeyFe3CoSb12 热电材料及涂层的热电性能

  • 李斗 ,
  • 徐长江 ,
  • 李旭光 ,
  • 李双明 ,
  • 钟宏
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  • 西北工业大学 凝固技术国家重点实验室 西安 710072
李 斗,男,1993年生,博士生

收稿日期: 2021-05-19

  修回日期: 2021-12-04

  网络出版日期: 2022-01-26

基金资助

国家自然科学基金项目(51774239)

Thermoelectric Properties of P-Type CeyFe3CoSb12 Thermoelectric Materials and Coatings Doped with La

  • Dou LI ,
  • Changjiang XU ,
  • Xuguang LI ,
  • Shuangming LI ,
  • Hong ZHONG
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  • State Key Laboratory of Solidification Processing, Northwestern Polytechnical University, Xi'an 710072, China
LI Shuangming, professor, Tel: (029)88493264, E-mail: lsm@nwpu.edu.cn

Received date: 2021-05-19

  Revised date: 2021-12-04

  Online published: 2022-01-26

Supported by

National Natural Science Foundation of China(51774239)

摘要

采用熔融-退火-放电等离子烧结工艺合成P型CoSb3基热电材料,研究Ce掺杂量对CoSb3基热电材料显微组织和热电性能的影响,以及La掺杂对解耦热电关系的作用。结果表明,掺杂元素La和Ce降低了热导率,使La0.1Ce0.8Fe3CoSb12在整个测温区间的热导率保持在1 W/(m·K)左右,对应的最高热电优值在723 K时达到0.45。以磁控溅射法制备Al-Ni涂层,通过对溅射Al-Ni防护涂层的P型La0.1Ce0.8Fe3CoSb12材料热电性能进行测试,发现涂层的介入并未造成材料热电性能的衰退,且涂层与基底结合良好,元素分布均匀。以钎料Ag40Cu60对P型热电元件La0.1Ce0.8Fe3CoSb12与电极片Mo50Cu50接头进行焊接行为研究,发现界面处宏观结合效果良好。

本文引用格式

李斗 , 徐长江 , 李旭光 , 李双明 , 钟宏 . La掺杂PCeyFe3CoSb12 热电材料及涂层的热电性能[J]. 金属学报, 2023 , 59(2) : 237 -247 . DOI: 10.11900/0412.1961.2021.00215

Abstract

During the use of fossil fuels, about two-thirds of the energy that is discharged into the environment in the form of waste heat are barely utilized and cause considerable environmental pollution and intense CO2 emission. Thermoelectric materials directly convert heat energy to electricity, thus, improving the utilization efficiency of fossil energy and reducing environmental pollution. Skutterudite CoSb3 has been widely studied as one of the materials for thermoelectric applications in the middle-temperature region. CoSb3-based skutterudites are narrow bandgap semiconductors with a high-electrical conductivity and Seebeck coefficient. Meanwhile, thermoelectric performance of bulk CoSb3 has been considerably improved via doping and design of nano structures. Herein, P-type CoSb3 was synthesized via melt-annealing-spark plasma sintering process. The effect of Ce-doping content on microstructure and thermoelectric properties of CoSb3 and the effect of La doping on decoupled thermoelectric performance were studied. Compared with Ce0.8Fe3CoSb12, the Seebeck coefficient of La0.1Ce0.8Fe3CoSb12 increased with temperature, electrical resistivity decreased from 25 μΩ·m to 15 μΩ·m at 300 K, and power factor simultaneously increased from 480 μW/(m·K2) to 642 μW/(m·K2) at 673 K. The La0.1Ce0.8Fe3CoSb12 thermal conductivity decreased with La or Ce doping to ~1 W/(m·K), and the corresponding thermoelectric figure of merit reached 0.45 at 723 K in the temperature range from 300 K to 723 K. Al-Ni coating was deposited on the sintered bulk skutterudite via magnetron sputtering method. It was demonstrated that the coating did not degrade the thermoelectric performance, while the coating elements were uniformly distributed across the sintered bulk La0.1Ce0.8Fe3CoSb12. The welding behavior of P-type La0.1Ce0.8Fe3CoSb12 was studied using a Ag40Cu60 solder and a Mo50Cu50 electrode sheet. The interface of this thermoelectric material was prone to cracking and pore formation, while the elements at the interface have not demonstrated remarkable diffusion. This indicates an efficiency of the interface bonding, which may be used in the fabrication technologies of thermoelectric devices.

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