Preparation and thermoelectric properties of Sc-doped Ti<sub>1–<i>x</i></sub>NiSb half-Heusler alloys

Liu Rong-Tao; Wang Chen-Yang; Huang Jia-Mian; Luo Peng-Fei; Liu Xin; Ye Song; Dong Zi-Rui; Zhang Ji-Ye; Luo Jun

doi:10.7498/aps.72.20230035

Abstract

The nominal composition TiNiSb with 19 valence electrons is demonstrated to be composed of off-stoichiometric half-Heusler phase and impurities. In this work, the Ti_1–xNiSb (x = 0, 0.10, 0.15, 0.20, 0.25) samples are prepared by ball milling and spark plasma sintering. The single-phase Ti_0.9NiSb sample, deviating from the theoretical composition Ti_0.75NiSb base on 18-electron rule, is obtained, which might be ascribed to the small defect formation energy of Ti filling the vacancy as well as our ball-milling preparation method. With the single-phase Ti_0.9NiSb sample used as the base material, a small amount of Sc is used to partially replace Ti in order to further reduce the carrier concentration. Thus, the Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) samples are designed to investigate the effect of Sc doping on the thermoelectric properties. The X-ray powder diffraction (XRD) and scanning electron microscopy (SEM) analysis confirm the single-phase nature of the Ti_1–x–ySc_yNiSb samples. Energy-dispersive X-ray spectroscopy (EDS) results indicate that the actual compositions of the Ti_1–x–ySc_yNiSb samples are consistent well with their nominal compositions, and all elements are distributed uniformly in the sample. Moreover, the doping of Sc can increase the content of Ti vacancy while maintaining the single-phase structure, which could be attributed to the higher binding energy between Sc and Sb because the electronegativity of Sc is less than that of Ti. Both the substitution of Sc for Ti and the increase of the Ti vacancies significantly reduce the carrier concentration, which decreases from ~13.6 × 10²¹ cm^–3 for Ti_0.9NiSb to ~3.4 × 10²¹ cm^–3 for Ti_0.8Sc_0.05NiSb. The reduced carrier concentration results in greatly increased Seebeck coefficient, therefore the Ti_0.8Sc_0.05NiSb sample achieves a power factor as high as 17.7 μW·cm^-1·K^-2 at 973 K. Although the lattice thermal conductivity of Sc-doped sample increases slightly due to the reduction of electron–phonon scattering and the enhancement of chemical bonds, the total thermal conductivity decreases dramatically due to the electronic thermal conductivity decreasing greatly. Finally, the Ti_0.8Sc_0.05NiSb sample reaches a ZT value of ~0.42 at 973 K, which is 180% higher than that of Ti_0.9NiSb sample. Despite the fact that the thermoelectric performance of our sample is still inferior to those of the state-of-the-art off-stoichiometric 19-electron half-Heusler alloys, this work demonstrates that the thermoelectric performance of Ti_1–xNiSb can be further improved by non-isoelectronic doping.

Keywords:

Authors and contacts

School of Material Science and Engineering, Shanghai University, Shanghai 200444, China

Corresponding author: Dong Zi-Rui, zirui@shu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51902194, 52272226).

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References

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Cited By

图 1 Ti_1–xNiSb (0 ≤ x ≤ 0.25) 和Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) 样品的XRD图谱(a), (c)与晶格常数(b), (d)

Figure 1. XRD patterns (a), (c) and lattice constant (b), (d) of Ti_1–xNiSb (0 ≤ x ≤ 0.25) and Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05)

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图 2 Ti_0.85NiSb和Ti_0.8Sc_0.05NiSb样品的XPS能谱

Figure 2. XPS spectra of Ti_0.85NiSb and Ti_0.8Sc_0.05NiSb samples.

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图 3 样品Ti_0.8Sc_0.05NiSb的SEM (a)和BSE (b) 图像 (插图为EDS面扫描元素分布图)

Figure 3. SEM image (a) and BSE image (b) of the Ti_0.8Sc_0.05NiSb samples (The insets are the EDS elemental mappings).

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图 4 Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05)的电输运特性随温度的变化　(a) 电导率σ; (b) 塞贝克系数S; (c) 功率因子. (d) Ti_1–x–ySc_yNiSb样品的载流子浓度n_H和迁移率μ_H

Figure 4. Temperature dependent electrical transport properties of Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) samples: (a) Electrical conductivity σ; (b) Seebeck coefficients S; (c) power factor. (d) Room-temperature Hall carrier concentration n_H and mobility μ_H of Ti_1–x-ySc_yNiSb samples.

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图 5 Ti_1–x–ySc_yNiSb样品的塞贝克系数S随载流子浓度n_H的变化

Figure 5. Carrier concentration dependent Seebeck coefficient for Ti_1–x–ySc_yNiSb samples at room temperature.

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图 6 (a), (b) Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) 样品的总热导率κ和晶格热导率κ_l随温度的变化 (图(b)中的虚线为T^–0.5关系)

Figure 6. (a), (b) Temperature dependence of total thermal conductivity (κ) and lattice thermal conductivity (κ_l) of Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) samples (The dashed lines in Fig. (b) represent the T^–0.5 relationship).

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图 7 (a) Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) 样品的ZT值随温度的变化; (b) Ti_0.8Sc_0.05NiSb样品的ZT值与文献数据对比^[39,40]

Figure 7. (a) Temperature dependence of ZT value for Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) samples; (b) comparison of ZT value of Ti_0.8Sc_0.05NiSb sample with literature data^[39,40].

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表 1 Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) 样品的名义成分和EDS实际成分

Table 1. Nominal and actual atomic contents for Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) detected by EDS.

名义成分	实际成分
Ti_0.9NiSb	Ti_0.87NiSb_1.04
Ti_0.87Sc_0.03NiSb	Ti_0.85Sc_0.03NiSb_1.02
Ti_0.85Sc_0.05NiSb	Ti_0.85Sc_0.06NiSb_1.15
Ti_0.80Sc_0.05NiSb	Ti_0.80Sc_0.06NiSb_1.04

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表 2 室温下Ti_1–x–ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) 样品的横波${{v}}_{\text{l}}$和纵波声速${{v}}_{\text{t}}$, 以及利用公式^①计算得到的平均声速${{v}}_{\text{s}}$

Table 2. Measured longitudinal${{v}}_{\text{l}}\text{}$and transverse${{v}}_{\text{t}}$ sound velocities for Ti_1–x–_ySc_yNiSb (x = 0.10, 0.15; y = 0.03, 0.05) samples at room temperature. The average sound velocity ${{v}}_{\text{s}}$ is calculated by the formula^①

样品	${ {v} }_{{\rm{l}} }$/(m·s^–1)	${v} _{{\rm{t}}}$/(m·s^–1)	${v}_{{\rm{s}}}$/(m·s^–1)
Ti_0.9NiSb	3085	5887	3451
Ti_0.87Sc_0.03NiSb	3094	5841	3458
Ti_0.85Sc_0.05NiSb	3100	5844	3464
Ti_0.80Sc_0.05NiSb	3121	5977	3491
注: ① ${ {v} }_{\text{s} }=\left[\dfrac{\text{1} }{\text{3} }\text{}\left(\dfrac{\text{1} }{ { {v} }_{\text{l} }^{\text{3} } }+\dfrac{\text{2} }{ { {v} }_{\text{t} }^{\text{3} } }\right)\right] ^{ {-1/3} }.$

DownLoad: CSV

[1]	Bell L E 2008 Science 321 1457 Google Scholar
[2]	Jia N, Cao J, Tan X Y, Dong J F, Liu H F, Tan C K I, Xu J W, Yan Q Y, Loh X J, Suwardi A 2021 Energy Environ. Sci. 21 100519 Google Scholar
[3]	Min R A, Wang Y X, Jiang X, Chen R C, Kang H J, Guo E Y, Chen Z N, Yang X, Wang T M 2022 Chem. Eng. J. 449 137898 Google Scholar
[4]	Joshi G, Dahal T, Chen S, Wang H Z, Shiomi J, Chen G, Ren Z F 2013 Nano Energy 2 82 Google Scholar
[5]	Yu C, Zhu T J, Shi R Z, Zhang Y, Zhao X B, He J 2009 Acta Mater. 57 2757 Google Scholar
[6]	Fu C G, Zhu T J, Liu Y T, Xie H H, Zhao X B 2015 Energy Environ. Sci. 8 216 Google Scholar
[7]	Pei Y Z, Shi X Y, LaLonde A, Wang H, Chen L D, Snyder G J 2011 Nature 473 66 Google Scholar
[8]	Fu C G, Zhu T J, Pei Y Z, Xie H H, Wang H, Snyder G J, Liu Y, Liu Y T, Zhao X B 2014 Adv. Energy Mater. 4 1400600 Google Scholar
[9]	Tan C, Wang H X, Yao J, Chen T T, Wang L, Sun Y Q, Khan M, Wang H C, Wang C L 2022 J. Eur. Ceram. Soc. 42 7010 Google Scholar
[10]	Biswas K, He J Q, Blum I D, Wu C I, Hogan T P, Seidman D N, Dravid V P, Kanatzidis M G 2012 Nature 489 414 Google Scholar
[11]	Sun Y J, Shuai Z G, Wang D 2019 J. Phys. Chem. C 123 12001 Google Scholar
[12]	He R, Gahlawat S, Guo C F, Chen S, Dahal T, Zhang H, Liu W S, Zhang Q, Chere E, White K, Ren Z F 2015 Phys. Status. Solidi. A 212 2191 Google Scholar
[13]	Graf T, Felser C, Parkin S S P 2011 Prog. Solid. State Ch. 39 1 Google Scholar
[14]	Sakurada S, Shutoh N 2005 Appl. Phys. Lett. 86 082105 Google Scholar
[15]	Uher C, Yang J, Hu S, Morelli D T, Meisner G P 1999 Phys. Rev. B 59 8615 Google Scholar
[16]	王鹏将, 康慧君, 杨雄, 刘颖, 程成, 王同敏 2022 无机材料学报 37 717 Google Scholar Wang P J, Kang H J, Yang X, Liu Y, Cheng C, Wang T M 2022 J. Inorg. Mater. 37 717 Google Scholar
[17]	Sekimoto T, Kurosaki K, Muta H, Yamanaka S 2006 Mater. Trans. 47 1445 Google Scholar
[18]	Sekimoto T, Kurosaki K, Muta H, Yamanaka S 2005 Mater. Trans. 46 1481 Google Scholar
[19]	Sekimoto T, Kurosaki K, Muta H, Yamanaka S 2007 Jpn. J. Appl. Phys. 46 L673 Google Scholar
[20]	Huang Y, Hayashi K, Miyazaki Y 2020 Chem. Mater. 32 5173 Google Scholar
[21]	Joshi G, He R, Engber M, Samsonidze G, Pantha T, Dahal E, Dahal K, Yang J, Lan Y C, Kozinsky B, Ren Z F 2014 Energy Environ. Sci. 7 4070 Google Scholar
[22]	Zhu H T, Mao J, Li Y W, et al. 2019 Nat. Commun. 10 270 Google Scholar
[23]	Xia K, Liu Y, Anand S, Snyder G J, Xin J, Yu J, Zhao X, Zhu T 2018 Adv. Funct. Mater. 28 1705845 Google Scholar
[24]	Li S, Bai F X, Wang R F, Chen C, Li X F, Cao F, Yu B, Sui J H, Liu X J, Ren Z F, Zhang Q 2020 Ann. Phys. 532 1900440 Google Scholar
[25]	Miranda J, Gruhn T 2022 J. Electron. Mater. 51 2043 Google Scholar
[26]	Huang L H, Wang J C, Mo X B, Lei X B, Ma S D, Wang C, Zhang Q Y 2019 Materials 12 1637 Google Scholar
[27]	Kainuma R, Umino R, Xu X, Han K, Omori T 2020 J. Phase. Equilibria. Diffus. 41 116 Google Scholar
[28]	Romaka V V, Rogl P, Romaka L, Stadnyk Y, Melnychenko N, Grytsiv A, Falmbigl M, Skryabina N 2013 J. Solid State Chem. 197 103 Google Scholar
[29]	Anand S, Xia K Y, Zhu T J, Wolverton C, Snyder G J 2018 Adv. Energy Mater. 8 1801409 Google Scholar
[30]	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
[31]	Anand S, Xia K Y, Hegde V I, Aydemir U, Kocevski V, Zhu T J, Wolverton C, Snyder G J 2018 Energy Environ. Sci. 11 1480 Google Scholar
[32]	Romaka V V, Rogl G, Grytsiv A, Rogl P 2020 Comput. Mater. Sci. 172 109307 Google Scholar
[33]	Zhou M, Chen L D, Feng C D, Wang D L, Li J F 2007 J. Appl. Phys. 101 113714 Google Scholar
[34]	Zhao D G, Wang L, Bo L, Wu D 2018 Metals 8 61 Google Scholar
[35]	Tavassoli A, Failamani F, Grytsiv A, Rogl G, Heinrich P, Müller H, Bauer E, Zehetbauer M, Rogl P 2017 Acta Mater. 135 263 Google Scholar
[36]	Kim H S, Gibbs Z M, Tang Y L, Wang H, Snyder G J 2015 APL Mater. 3 041506 Google Scholar
[37]	沈家骏, 方腾, 傅铁铮, 忻佳展, 赵新兵, 朱铁军 2019 无机材料学报 34 260 Google Scholar Shen J J, Fang T, Fu T Z, Xin J Z, Zhao X B, Zhu T J 2019 J. Inorg. Mater. 34 260 Google Scholar
[38]	Zhu T J, Yu G T, Xu J, Wu H J, Fu C G, Liu X H, He J Q, Zhao X B 2016 Adv. Electron. Mater. 2 1600171 Google Scholar
[39]	Karati A, Hariharan V S, Ghosh S, Prasad A, Nagini M, Guruvidyathri K, Mallik R C, Shabadi R, Bichler L, Murty B S, Varadaraju U V 2020 Scr. Mater. 186 375 Google Scholar
[40]	Hasan R, Park T, Kim S I, Kim H S, Jo S, Lee K H 2022 Adv. Energy Sustainability Res. 3 2100206 Google Scholar
[41]	Zhang X Y, Bu Z L, Shi X M, Chen Z W, Lin S Q, Shan B, Wood M, Snyder A H, Chen L D, Snyder G J, Pei Y Z 2020 Sci. Adv. 6 eabc0726 Google Scholar

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Preparation and thermoelectric properties of Sc-doped Ti_1–xNiSb half-Heusler alloys

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Corresponding author: Dong Zi-Rui, zirui@shu.edu.cn

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Preparation and thermoelectric properties of Sc-doped Ti1–xNiSb half-Heusler alloys

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Corresponding author: Dong Zi-Rui, zirui@shu.edu.cn

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Preparation and thermoelectric properties of Sc-doped Ti_1–xNiSb half-Heusler alloys