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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, TiNiCoxSn (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 TiNiCoxSn samples is 3.19 W/(m·K). Therefore, Co doping can significantly reduce the κl values 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 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.
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Keywords:
- TiNiSn /
- thermoelectric materials /
- melt spinning /
- half-Heusler
[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 物理学报 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
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Google Scholar
[8] Jiang B B, Wang W, Liu S X, Wang Y, Wang C F, Chen Y N, Xie L, Huang M Y, He J Q 2022 Science 377 208
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[9] Gelbstein Y, Rosenberg Y, Sadia Y, Dariel M P 2010 J. Phys. Chem. C. 114 13126
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[11] Liu H T, Sun Q, Zhong Y, Deng Q, Gan L, Lü F L, Shi X L, Chen Z G, Ang R 2022 Nano Energy 91 106706
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Google Scholar
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Google Scholar
[36] Cho J, Park T, Bae K W, Kim H S, Choi S M, Kim S I, Kim S W 2021 Materials 14 4029
Google Scholar
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[38] Wang J F, Luo F, Zhu C, Zhang S, Yang Z, Wang J F, He X, Zhang Y, Sun Z G 2022 J. Appl. Phys. 132 135103
Google Scholar
[39] Dresselhaus M S, Chen G, Tang M Y, Yang R, Lee H, Wang D, Ren Z F, Fleurial J P, Gogna P 2007 Adv. Mater. 19 1043
Google Scholar
[40] Dresselhaus M, Chen G, Ren Z F, Dresselhaus G, Henry A, Fleurial J P 2009 JOM 61 86
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[48] 罗丰2023 博士学位论文 (武汉: 武汉理工大学)
Luo F 2023 Ph. D. Dissertation (Wuhan: Wuhan University of Technology
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[50] Drymiotis F, Lashley J C, Fisk Z, Peterson E, Nakatsuji S 2003 Philos. Mag. 83 3169
Google Scholar
[51] Kim H S, Gibbs Z M, Tang Y L, Wang H, Snyder G J 2015 APL Mater. 3 041506
Google Scholar
[52] Baranovskiy A, Harush M, Amouyal Y 2019 Adv. Theor. Simul. 2 54
[53] Chi H, Liu W, Sun K, Su X L, Wang G Y, Lošt'ák P, Kucek V, Drašar Č, Uher C 2013 Phys. Rev. B 88 045202
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Google Scholar
[58] Liu Y T, Xie H H, Fu C G, Snyder G J, Zhao X B, Zhu T J 2015 J. Mater. Chem. A 3 22716
Google Scholar
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图 1 TiNiCoxSn样品的(a) XRD图谱和(b)晶格常数
Figure 1. (a) XRD patterns and (b) lattice constants of TiNiCoxSn samples.
图 2 TiNiCoxSn样品的背散射图 (a) x = 0; (b) x = 0.01; (c) x = 0.03; (d) x = 0.05
Figure 2. Backscattering images of TiNiCoxSn samples: (a) x = 0; (b) x = 0.01; (c) x = 0.03; (d) x = 0.05.
图 3 TiNiCoxSn薄带的SEM图 (a) TiNiSn微观图; (b) TiNiSn局部放大图; (c) TiNiCo0.03Sn微观图; (d) TiNiCo0.03Sn局部放大图
Figure 3. SEM images of TiNiCoxSn ribbons: (a) Microscopic image of TiNiSn; (b) local enlarged image of TiNiSn ribbon; (c) microscopic image of TiNiCo0.03Sn; (d) local enlarged image of TiNiCo0.03Sn ribbon.
图 4 TiNiCoxSn块体截面的EPMA图 (a) TiNiSn微观图; (b) TiNiSn局部放大图; (c) TiNiCo0.03Sn微观图; (d) TiNiCo0.03Sn局部放大图
Figure 4. EPMA diagrams of TiNiCoxSn block section: (a) Microscopic image of TiNiSn; (b) local enlarged image of TiNiSn sample; (c) microscopic image of TiNiCo0.03Sn; (d) local enlarged image of TiNiCo0.03Sn sample.
图 5 TiNiCoxSn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
Figure 5. Variation of TiNiCoxSn samples parameters with temperature and the doping amount x: (a), (b) Seebeck coefficients; (c), (d) conductivities; (e), (f) power factors.
图 6 TiNiCoxSn样品加权迁移率μw随温度(a)与掺杂量x (b)的变化关系
Figure 6. Relation of weighted mobility μw with temperature (a) and doping amount x (b) of TiNiCoxSn samples.
图 7 TiNiCoxSn样品的载流子浓度 nH和载流子迁移率μH
Figure 7. Hall carrier concentrations (nH) and carrier mobilities (μH) of TiNiCoxSn samples.
图 8 (a) TiNiCoxSn样品在室温下磁化强度随磁场的变化关系; (b) TiNiCoxSn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
Figure 8. (a) Room temperature M-H curves of TiNiCoxSn samples, (b) the ferromagnetic singals of TiNiCoxSn samples, (c) the enlarged M-H curves near zero point; (d) relation of saturation magnetization with doping amount x.
图 9 (a) 热导率κtot随温度变化的关系; (b) κtot随掺杂量x的变化关系; (c) 电子热导率κe随温度的变化关系; (d) κe随掺杂量x的变化关系; (e)晶格热导率κl随温度的变化关系; (f) κl随掺杂量x的变化关系
Figure 9. (a) Thermal conductivities κtot as a function of temperature; (b) κtot as a function of doping amount x; (c) electronic thermal conductivities κe as a function of temperature; (d) κe as a function of doping amount x; (e) lattice thermal conductivities κl as a function of temperature; (e) thermal conductivities κl as a function of temperature; (f) dependence of κl on doping amount x.
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[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 物理学报 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
[7] Xiao F, Hangarter C, Yoo B, Rheem Y, Lee K H, Myung N V 2008 Electrochimica Acta 53 8103
Google Scholar
[8] Jiang B B, Wang W, Liu S X, Wang Y, Wang C F, Chen Y N, Xie L, Huang M Y, He J Q 2022 Science 377 208
Google Scholar
[9] Gelbstein Y, Rosenberg Y, Sadia Y, Dariel M P 2010 J. Phys. Chem. C. 114 13126
[10] Komisarchik G, Gelbstein Y, Fuks D 2017 Intermetallics 89 16
Google Scholar
[11] Liu H T, Sun Q, Zhong Y, Deng Q, Gan L, Lü F L, Shi X L, Chen Z G, Ang R 2022 Nano Energy 91 106706
Google Scholar
[12] Pochet P, Caliste D 2012 Mat. Sci. Semicon. Proc. 15 675
Google Scholar
[13] Khan M R, Gopidi H R, Wlazło M, Malyi O I 2023 J. Phys. Chem. Lett. 14 1962
Google Scholar
[14] Kaller M, Fuks D, Gelbstein Y 2017 J. Alloy Compd. 729 446
Google Scholar
[15] Chauhan N S, Bathula S, Vishwakarma A, Bhardwaj R, Gahtori B, Kumar A, Dhar A 2018 ACS Appl. Energy Mater. 1 757
Google Scholar
[16] Lim W Y S, Zhang D, Duran S S F, Tan X Y, Tan C K I, Xu J, Suwardi A 2021 Front Mater. 8 745
[17] Wang J, Luo F, Zhu C, Wang J, He X, Zhang Y, Liu H, Sun Z G 2023 J. Mater. Chem. 11 4056
Google Scholar
[18] Zhu C, Wang J, Zhu X Q, Zhang S, Xu F, Luo F, Wang J F, Zhang Y, Liu H X, Sun Z G 2023 J. Mater. Chem. A 11 1268
Google Scholar
[19] 陈树权, 王剑, 杨振, 朱璨, 罗丰, 祝鑫强, 徐峰, 王嘉赋, 张艳, 刘虹霞, 孙志刚 2023 物理学报 72 068401
Google Scholar
Chen S Q, Wang J, Yang Z, Zhu C, Luo F, Zhu X Q, Xu F, Wang J F, Zhang Y, Liu H X, Sun Z G 2023 Acta Phys. Sin. 72 068401
Google Scholar
[20] Santos R, Yamini S A, Dou S X 2018 J. Mater. Chem. A 6 3328
Google Scholar
[21] Berry T, Fu C, Auffermann G, Fecher G H, Schnelle W, Serrano-Sanchez F, Yue Y, Liang H, Felser C 2017 Chem. Mater. 29 7042
Google Scholar
[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
[30] Pei Y Z, Shi X Y, Lalonde A, Wang H, Chen L D, Snyder G J 2011 Nature 473 66
Google Scholar
[31] Poudel B, Hao Q, Ma Y, Lan Y C, Minnich A, Yu B, Yan X, Wang D Z, Muto A, Vashaee D, Chen X Y, Liu J M, Dresselhaus M S, Chen G, Ren Z F 2008 Science 320 634
Google Scholar
[32] Zhao L D, Tan G J, Hao S Q, He J Q, Pei Y L, Chi H, Wang H, Gong S K, Xu H B, Dravid V P, Uher C, Snyder G J, Wolverton C, Kanatzidis M G 2016 Science 351 141
Google Scholar
[33] Hohl H, Ramirez A P, Goldmann C, Ernst G, Wölfing B, Bucher E 1999 J. Phys. Condens. Mat. 11 1697
Google Scholar
[34] Chauhan N S, Raghuvanshi P R, Tyagi K, Johari K K, Tyagi L, Gahtori B, Bathula S, Bhattacharya A, Mahanti S D, Singh V N 2020 J. Phys. Condens. Mat. 124 8584
[35] Shutoh N, Sakurada S 2005 J. Alloy Compd. 389 204
Google Scholar
[36] Cho J, Park T, Bae K W, Kim H S, Choi S M, Kim S I, Kim S W 2021 Materials 14 4029
Google Scholar
[37] He J S, Shen Y C, Zhai L J, Luo F, Zhang Y, Liu H X, Hu J F, Sun Z G 2024 J. Alloy Compd. 975 172808
Google Scholar
[38] Wang J F, Luo F, Zhu C, Zhang S, Yang Z, Wang J F, He X, Zhang Y, Sun Z G 2022 J. Appl. Phys. 132 135103
Google Scholar
[39] Dresselhaus M S, Chen G, Tang M Y, Yang R, Lee H, Wang D, Ren Z F, Fleurial J P, Gogna P 2007 Adv. Mater. 19 1043
Google Scholar
[40] Dresselhaus M, Chen G, Ren Z F, Dresselhaus G, Henry A, Fleurial J P 2009 JOM 61 86
Google Scholar
[41] Yang J, Yip H L, Jen A K Y 2013 Adv. Energy Mater. 3 549
Google Scholar
[42] Kim K S, Kim Y M, Mun H, Kim J, Park J, Borisevich A Y, Lee K H, Kim S W 2017 Adv. Mater. 29 1702091
Google Scholar
[43] Katayama T, Kim S W, Kimura Y, Mishima Y 2003 J. Electron. Mater. 32 1160
Google Scholar
[44] Li C C, Zhao W Y, Zhang Q J 2022 Sci. Bull. 67 891
Google Scholar
[45] Zhao W Y, Liu Z Y, Sun Z G, Zhang Q J, Wei P, Mu X, Zhou H Y, Li C C, Ma S F, He D Q, Ji P X, Zhu W T, Nie X L, Su X L, Tang X F, Shen B G, Dong X L, Yang J H, Liu Y, Shi J 2017 Nature 549 247
Google Scholar
[46] Luo F, Wang J, Zhu C, He X, Zhang S, Wang J F, Liu H X, Sun Z G 2022 J. Mater. Chem. A 10 9655
Google Scholar
[47] Romaka V, Stadnyk Y V, Fruchart D, Dominuk T, Romaka L, Rogl P, Goryn A M 2009 Semiconductors 43 1124
Google Scholar
[48] 罗丰2023 博士学位论文 (武汉: 武汉理工大学)
Luo F 2023 Ph. D. Dissertation (Wuhan: Wuhan University of Technology
[49] An D C, Wang J J, Zhang J, Zhai X, Kang Z P, Fan W H, Yan J, Liu Y Q, Lu L, Jia C L, Wuttig M, Cojocaru-Mirédin O, Chen S P, Wang W X, Snyder G J, Yu Y 2021 Energy Environ. Sci. 14 5469
Google Scholar
[50] Drymiotis F, Lashley J C, Fisk Z, Peterson E, Nakatsuji S 2003 Philos. Mag. 83 3169
Google Scholar
[51] Kim H S, Gibbs Z M, Tang Y L, Wang H, Snyder G J 2015 APL Mater. 3 041506
Google Scholar
[52] Baranovskiy A, Harush M, Amouyal Y 2019 Adv. Theor. Simul. 2 54
[53] Chi H, Liu W, Sun K, Su X L, Wang G Y, Lošt'ák P, Kucek V, Drašar Č, Uher C 2013 Phys. Rev. B 88 045202
Google Scholar
[54] Lkhagvasuren E, Fu C, Fecher G H, Auffermann G, Kreiner G, Schnelle W, Felser C 2017 J. Phys. D Appl. Phys. 50 425502
Google Scholar
[55] Gong B, Li Y, Liu F S, Zhu J X, Wang X, Ao W Q, Zhang C H, Li J Q, Xie H P, Zhu T J 2019 ACS Appl. Mater. Interface 11 13397
Google Scholar
[56] Mao J, Zhou J, Zhu H, Liu Z, Zhang H, He R, Chen G, Ren Z F 2017 Chem. Mater. 29 14
[57] Yan J X, Liu F S, Ma G H, Gong B, Zhu J X, Wang X, Ao W Q, Zhang C H, Li Y, Li J Q 2018 Scripta Mater. 157 129
Google Scholar
[58] Liu Y T, Xie H H, Fu C G, Snyder G J, Zhao X B, Zhu T J 2015 J. Mater. Chem. A 3 22716
Google Scholar
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