熔融旋甩制备Co掺杂TiNiCo<sub><i>x</i></sub>Sn合金的热电性能

何俊松; 罗丰; 王剑; 杨士冠; 翟立军; 程林; 刘虹霞; 张艳; 李艳丽; 孙志刚; 胡季帆

doi:10.7498/aps.73.20240112

摘要

TiNiSn基 half-Heusler高温热电材料具有较高的功率因子, 但其也具有较高的晶格热导率, 这极大地阻碍了其热电性能的提升. 本文采用熔融旋甩快淬与放电等离子烧结工艺制备TiNiCo_xSn (x = 0—0.05)样品, 研究磁性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TiNiCo_xSn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, TiNiCo_xSn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3.19 W/(m·K), 最大降幅约为42.6%. 随着Co掺杂量x的增大TiNiCo_xSn样品出现n/p转变, 电导率随x增大而逐渐下降, 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29.56 W/(m·K²)的最高功率因子. ZT值随Co掺杂量x的增大而逐渐降低, 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.

关键词:

Abstract

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 work, TiNiCo_xSn (x = 0–0.05) samples are 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 any other impurity phases are found, indicating that the high purity single phase can be prepared by rapid quenching process combined with SPS process. In 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 grain sizes in a range of 200–600 nm. The grain sizes 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 Co-doping sample has the thermal conductivity that decreases significantly, and the maximum decrease can reach about 38.9%. The minimum value of lattice thermal conductivity of TiNiCo_xSn samples is 3.19 W/(m·K). Therefore, Co doping can significantly reduce the κ_l values of TiNiCo_xSn (x = 0.01–0.05) samples. With the increase of Co doping amount x, n/p transition is observed in the TiNiCo_xSn samples, resulting in gradually reducing the conductivity and the power factor, and finally deteriorating the electrical transport performance, of which, the TiNiSn sample obtains the highest power factor of 29.56 W/(m·K²) at 700 K. The ZT value decreases with the Co doping amount x increasing, 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:

作者及机构信息

1.
太原科技大学材料科学与工程学院, 太原　030024

2.
太原科技大学, 山西省磁电功能材料与应用重点实验室, 太原　030024

3.
武汉理工大学, 材料复合新技术国家重点实验室, 武汉　430070

4.
武汉理工大学襄阳示范区, 湖北隆中实验室, 襄阳　441000

通信作者: 孙志刚, sun_zg@whut.edu.cn ; 胡季帆, 2019064@tyust.edu.cn

基金项目: 国家自然科学基金 (批准号: 12174297, 12204342)、山西省基础研究计划 (批准号: 202103021224283, 202203021212323)、太原科技大学科研启动基金项目(批准号: 20222015, 20222002)、来晋工作优秀博士奖励项目(批准号: 20222039, 20222040)和山西省高等学校科技创新项目(批准号: 2022L288)资助的课题.

Authors and contacts

1.
College of Materials Science and Engineering, Taiyuan University of Science and Technology, Taiyuan 030024, China

2.
Shanxi Key Laboratory of Magnetoelectric Functional Materials and Application, Taiyuan University of Science and Technology, Taiyuan 030024, China

3.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China

4.
Hubei Longzhong Laboratory, Xiangyang Demonstration Zone of Wuhan University of Technology, Xiangyang 441000, China

Corresponding author: Sun Zhi-Gang, sun_zg@whut.edu.cn ; Hu Ji-Fan, 2019064@tyust.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 12174297, 12204342), the Basic Research Program of Shanxi Province, China (Grant Nos. 202103021224283, 202203021212323), the Scientific Research Start-up Fund of Taiyuan University of Science and Technology (Grant Nos. 20222015, 20222002), the Outstanding Doctoral Award Program for Working in Shanxi Province (Grant Nos. 20222039, 20222040), and the Science and Technology Innovation Project of Higher Education Institutions in Shanxi Province, China (Grant No. 2022L288).

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参考文献

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施引文献

图 1 TiNiCo_xSn样品的(a) XRD图谱和(b)晶格常数

Fig. 1. (a) XRD patterns and (b) lattice constants of TiNiCo_xSn samples.

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图 2 TiNiCo_xSn样品的背散射图　(a) x = 0; (b) x = 0.01; (c) x = 0.03; (d) x = 0.05

Fig. 2. Backscattering images of TiNiCo_xSn samples: (a) x = 0; (b) x = 0.01; (c) x = 0.03; (d) x = 0.05.

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图 3 TiNiCo_xSn薄带的SEM图　(a) TiNiSn微观图; (b) TiNiSn局部放大图; (c) TiNiCo_0.03Sn微观图; (d) TiNiCo_0.03Sn局部放大图

Fig. 3. SEM images of TiNiCo_xSn ribbons: (a) Microscopic image of TiNiSn; (b) local enlarged image of TiNiSn ribbon; (c) microscopic image of TiNiCo_0.03Sn; (d) local enlarged image of TiNiCo_0.03Sn ribbon.

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图 4 TiNiCo_xSn块体截面的EPMA图　(a) TiNiSn微观图; (b) TiNiSn局部放大图; (c) TiNiCo_0.03Sn微观图; (d) TiNiCo_0.03Sn局部放大图

Fig. 4. EPMA diagrams of TiNiCo_xSn block section: (a) Microscopic image of TiNiSn; (b) local enlarged image of TiNiSn sample; (c) microscopic image of TiNiCo_0.03Sn; (d) local enlarged image of TiNiCo_0.03Sn sample.

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图 5 TiNiCo_xSn样品参数随温度及掺杂量x的变化　(a), (b) Seebeck系数; (c), (d)电导率; (e), (f)功率因子

Fig. 5. Variation of TiNiCo_xSn samples parameters with temperature and the doping amount x: (a), (b) Seebeck coefficients; (c), (d) conductivities; (e), (f) power factors.

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图 6 TiNiCo_xSn样品加权迁移率μ_w随温度(a)与掺杂量x (b)的变化关系

Fig. 6. Relation of weighted mobility μ_w with temperature (a) and doping amount x (b) of TiNiCo_xSn samples.

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图 7 TiNiCo_xSn样品的载流子浓度 n_H和载流子迁移率μ_H

Fig. 7. Hall carrier concentrations (n_H) and carrier mobilities (μ_H) of TiNiCo_xSn samples.

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图 8 (a) TiNiCo_xSn样品在室温下磁化强度随磁场的变化关系; (b) TiNiCo_xSn样品的铁磁性; (c) 零点附近局部放大图; (d) 最大饱和磁化强度随掺杂量的关系

Fig. 8. (a) Room temperature M-H curves of TiNiCo_xSn samples, (b) the ferromagnetic singals of TiNiCo_xSn samples, (c) the enlarged M-H curves near zero point; (d) relation of saturation magnetization with doping amount x.

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图 9 (a) 热导率κ_tot随温度变化的关系; (b) κ_tot随掺杂量x的变化关系; (c) 电子热导率κ_e随温度的变化关系; (d) κ_e随掺杂量x的变化关系; (e)晶格热导率κ_l随温度的变化关系; (f) κ_l随掺杂量x的变化关系

Fig. 9. (a) Thermal conductivities κ_tot as a function of temperature; (b) κ_tot as a function of doping amount x; (c) electronic thermal conductivities κ_e as a function of temperature; (d) κ_e as a function of doping amount x; (e) lattice thermal conductivities κ_l as a function of temperature; (e) thermal conductivities κ_l as a function of temperature; (f) dependence of κ_l on doping amount x.

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图 10 (a) TiNiCo_xSn样品的ZT随温度的变化关系; (b) TiNiSn样品的ZT值与其他工作的对比^[54–58]

Fig. 10. (a) Relation of ZT of TiNiCo_xSn samples with the temperature; (b) comparison of ZT value of TiNiSn samples in this work with other works^[54–58].

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map

[1]	杨士冠, 林鑫, 何俊松, 翟立军, 程林, 吕明豪, 刘虹霞, 张艳, 孙志刚 2023 72 228401 Google Scholar Yang S G, Lin X, He J S, Zhai L J, Cheng L, Lü M H, Liu H X, Zhang Y, Sun Z G 2023 Acta Phys. Sin. 72 228401 Google Scholar
[2]	Luo F, Zhu C, Wang J, He X, Yang Z, Ke S, Zhang Y, Liu H, Sun Z G 2022 ACS Appl. Mater. Interfaces. 14 45503 Google Scholar
[3]	Ma S F, Li C C, Wei P, Zhu W T, Nie X L, Sang X H, Zhang Q J, Zhao W Y 2020 J. Mater. Chem. A 8 4816 Google Scholar
[4]	Shi L, Chen J, Zhang G, Li B 2012 Phys. Lett. A 376 978 Google Scholar
[5]	Ouyang Y, Zhang Z, Li D, Chen J, Zhang G 2019 Ann. Phys. Berlin 531 4 Google Scholar
[6]	He J, Hu Y X, Li D F, Chen J 2021 Nano Res. 15 3804
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[22]	Downie R, Maclaren D, Bos J W 2014 J. Mater. Chem. A 2 6107 Google Scholar
[23]	Sanad M F, Shalan A E, Abdellatif S O, Serea E S A, Adly M S, Ahsan M A 2020 Top Curr. Chem. 378 48 Google Scholar
[24]	Wang J, Zhu C, Luo F, Wang J F, He X, Zhang Y, Liu H X, Sun Z G 2023 ACS Appl. Mater. Interfaces 15 8105 Google Scholar
[25]	Lü W Y, Liu W D, Li M, Hong M, Guo K, Luo J, Xing J, Sun Q, Xu S, Zou J 2022 Chem. Eng. J. 446 137278 Google Scholar
[26]	Hu B, Shi X L, Zou J, Chen Z G 2022 Chem. Eng. J. 437 135268 Google Scholar
[27]	Liu H X, Zhang S, Zhang Y, Zong S T, Li W, Zhu C, Luo F, Wang J, Sun Z G 2022 ACS Appl. Energy Mater. 5 15093 Google Scholar
[28]	Zhu T J, Liu Y T, Fu C G, Heremans J P, Snyder J G, Zhao X B 2017 Adv. Mater. 29 1605884 Google Scholar
[29]	Van Du N, Nam W H, Cho J Y, Binh N V, Huy P T, Tuan D A, Shin W H, Lee S 2021 J. Alloy Compd. 886 161293 Google Scholar
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