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TiNiSn基half-Heusler高温热电材料具有较高的功率因子，但其较高的晶格热导率极大地阻碍了热电性能的提升。本文采用熔融旋甩快淬与放电等离子烧结工艺制备TiNiCoxSn (x=0~0.05)样品，研究了磁性Co元素掺杂对材料的相组成、微观结构和热电性能。结果表明，该制备工艺能够直接获得纳米晶的TiNiCoxSn样品。在纳米晶影响下的样品的热导率明显低于块体材料的热导率，平均降幅约为17.8%。在Co掺杂后样品的晶粒尺寸进一步降低，与TiNiSn基体相比TiNiCoxSn样品的热导率显著降低，最大降幅约为38.9%，其中晶格热导率最低值为3.19W/mK，最大降幅约为42.6%。随着Co掺杂量x的增加TiNiCoxSn样品出现n/p转变，电导率随x增加而逐渐下降，电输运性能劣化，功率因子缓慢减小，其中TiNiSn样品在700 K时获得29.56W/mK2的最高功率因子。zT值随Co掺杂量x的增加而逐渐降低，TiNiSn样品在900 K时的最大zT值为0.48。本工作表明采用熔融旋甩制备工艺及磁性Co掺杂能够有效降低TiNiSn材料的热导率。
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关键词:
- TiNiSn /
- 热电材料 /
- 熔融旋甩 /
- half-Heusler
Although TiNiSn-based half-Heusler thermoelectric materials obtain high power factors, their high lattice thermal conductivity greatly hinders the improvement of thermoelectric properties. In this paper, TiNiCoxSn (x=0~0.05) samples were prepared by melt spinning combined with spark plasma sintering method and their phase, microstructure and thermoelectric properties are studied. The XRD results show that the main phase of all samples is TiNiSn phase, and no other impurity phases are found, indicating that the high purity single phase can be prepared by rapid quenching process combined with SPS process. During the solidification process, the large cooling rate (105-106 K/s) is conducive to obtaining the uniform nanocrystalline structure. The grains are closely packed with a grain size of 200-600 nm. The grain size decrease to 50-400 nm for the Co-doping samples, which indicates that Co doping can reduce the grain size. For the x=0 sample, the thermal conductivity of the rapid quenching sample is significantly lower than that of bulk sample, with an average decrease of about 17.8%. Compared with the TiNiSn matrix, the thermal conductivity of the Co-doping samples are significantly reduced, and the maximum decrease is about 38.9%. The minimum value of lattice thermal conductivity of TiNiCoxSn samples is 3.19 W/mK. Therefore, Co doping can significantly reduce the кl of TiNiCoxSn (x=0.01~0.05) samples. With the increase of Co doping amount x, n/p transition is observed in the TiNiCoxSn samples, resulting in a gradually decrease of the conductivity and the power factor, and finally the deterioration of the electrical transport performance. Among them, the TiNiSn sample obtains the highest power factor of 29.56 W/mK2 at 700 K. The zT value decreases with the Co doping amount x, and the maximum zT value of TiNiSn sample at 900 K is 0.48. This work shows that the thermal conductivity of TiNiSn can be effectively reduced by using the melt spinning process and magnetic Co doping.-
Keywords:
- TiNiSn /
- thermoelectric materials /
- melt spinning /
- half-Heusler
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