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Cu2Se类液态热电材料扩散阻挡层的研究
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中国科学院 上海硅酸盐研究所

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国家重点基础研究发展计划项目(2018YFB0703600);国家自然科学基金面上项目(51872314);. 中科院重点部署项目(KFZD-SW-421))


Investigation on the barrier layer of Cu2Se liquid-like thermoelectric material
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Shanghai Institute of Ceramics, Chinese Academy of Sciences

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    摘要:

    近年来,以Cu2Se为代表的类液态热电材料在热电领域获得了高度关注。相对于Cu2Se类液态材料电、热输运性质方面的诸多研究,目前热电领域对Cu2Se基热电器件的研究则很少。扩散阻挡层作为热电器件的重要组成部分,可用于阻止热电材料和电极材料在高温下的快速反应,保证热电器件长时间稳定服役。本工作首先选用Mo作为Cu2Se的扩散阻挡层材料,通过一步法热压烧结制备了Cu2Se/Mo/Cu2Se三明治结构样品,发现Cu2Se/Mo界面具有极低的界面接触电阻率。但是,Cu2Se/Mo界面结合强度较差,不利于器件的长时间稳定工作。随后,通过在Mo层中引入活性元素Mn,利用Mn在Cu2Se中易于扩散的特点,在保持极低界面接触电阻率的同时,显著提高了界面的结合强度。高温长时间老化后, Cu2Se/Mo-Mn界面仍然保持良好的界面结合和低的界面接触电阻率。本工作表明Mo-Mn金属混合相是与Cu2Se材料相匹配的扩散阻挡层,可用以开发具有良好服役性能的Cu2Se基热电器件。

    Abstract:

    Recently, Cu2Se-based liquid-like materials with high thermoelectric performance have attracted great attention from the thermoelectric community. However, as compared with the extensive study on the electrical and thermal transport properties of Cu2Se, few investigations were reported on the Cu2Se-based thermoelectric device. Barrier layer is an imperative component for thermoelectric power generators (TEG)since it can effectively depress drastic reactions between the thermoelectric material and the electrode at hot side. In this work, we firstly chose Mo as the barrier layer for Cu2Se and fabricated Cu2Se/Mo/Cu2Se thermoelectric joints with the one-step hot pressing method. It is found that the Cu2Se/Mo interface has ultralow electrical contact resistivity but poor tensile strength. Via introducing 5 wt.% Mn in Mo, we successfully improved the tensile strength by three times while still maintaining low electrical contact resistivity, which are attributed to the diffusion of Mn into Cu2Se during the hot pressing process. The evolutions of microstructure and contact resistivity at the interface during long-term aging at high temperatures (650℃ and 800℃) were investigated. After aging experiments, the interface remains integrity and with low contact resistivity which proves that the Mo-Mn mixed phase is a promising candidate as the the barrier layer for Cu2Se-based TEGs.

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黄仲夫,顾明,仇鹏飞,邵笑,任都迪,柏胜强,史迅,陈立东. Cu2Se类液态热电材料扩散阻挡层的研究[J].稀有金属材料与工程,2020,49(4):1352~1359.[Huang Zhongfu, Gu Ming, Qiu Pengfei, Shao Xiao, Ren Dudi, Bai Shengqiang, Shi Xun, Chen Lidong. Investigation on the barrier layer of Cu2Se liquid-like thermoelectric material[J]. Rare Metal Materials and Engineering,2020,49(4):1352~1359.]
DOI:10.12442/j. issn.1002-185X.20190046

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  • 收稿日期:2019-01-12
  • 最后修改日期:2019-03-07
  • 录用日期:2019-03-15
  • 在线发布日期: 2020-05-07
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