Defect structure regulation and thermoelectric transfer performance in n-type Bi2–x SbxTe3–ySey-based compounds

Li Rui-Ying; Luo Ting-Ting; Li Mao; Chen Shuo; Yan Yong-Gao; Wu Jin-Song; Su Xian-Li; Zhang Qing-Jie; Tang Xin-Feng

doi:10.7498/aps.73.20240098

Abstract

Bi₂Te₃-based compounds are thermoelectric materials with the best performance near room temperature. The existence of a large number of complex defects makes defect engineering a core stratagem for adjusting and improving the thermoelectric performance. Therefore, understanding and effectively controlling the existence form and concentration of defects is crucial for achieving high-thermoelectric performance in Bi₂Te₃-based alloy. Herein, a series of Cl doped n-type quaternary Bi_2–x Sb_xTe_3–ySe_y compounds is synthesized by the zone-melting method. The correlation between defect evolution process and thermoelectric performance is systematically investigated by first-principles calculation and experiments. Alloying Sb on Bi site and Se on Te site induce charged structural defects, leading to a significant change in the carrier concentration. For Bi_2–x Sb_xTe_2.994Cl_0.006 compounds, alloying Sb on Bi site reduces the formation energy of the ${\mathrm{S}}{{\text{b}}_{{\mathrm{Te}}}}_{_2}$ antisite defect, which generates the antisite defect ${\mathrm{S}}{{\text{b}}_{{\mathrm{Te}}}}_{_2}$ and accompanied with the increase of the minority carrier concentration from 2.09×10¹⁶ to 3.99×10¹⁷ cm^–3. The increase of the minority carrier severely deteriorates the electrical transport properties. In contrast, alloying Se in the Bi_1.8Sb_0.2Te_2.994–ySe_yCl_0.006 compound significantly lowers the formation energy of the complex defect ${\mathrm{S}}{{\mathrm{e}}_{{\mathrm{Te}}}}$+${\mathrm{S}}{{\mathrm{b}}_{{\mathrm{Bi}}}}$, which becomes more energetically favorable and suppresses the formation of the antisite defect ${\mathrm{S}}{{\text{b}}_{{\mathrm{Te}}}}_{_2}$. As a result, the concentration of minority carriers decreases to 1.46×10¹⁶ cm^–3. This eliminates the deterioration effect of the minority carrier on the electrical transport properties of the material and greatly improves the power factor. A maximum power factor of 4.49 mW/(m·K²) is achieved for Bi_1.8Sb_0.2Te_2.944Se_0.05Cl_0.006 compound at room temperature. By reducing thermal conductivity through intensifying the phonon scattering via alloying Sb and Se, the maximum ZT value of 0.98 is attained for Bi_1.8Sb_0.2Te_2.844Se_0.15Cl_0.006 compound at room temperature. Our finding provides an important guidance for adjusting point defects, carrier concentrations, and thermoelectric performances in Bi₂Te₃-based compounds with complex compositions.

Keywords:

Authors and contacts

1.
Longzhong Laboratory in Hubei Province, Xiangyang Demonstration Zone of Wuhan University of Technology, Xiangyang 441000, China
2.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
3.
Nanostructure Research Center, Wuhan University of Technology, Wuhan 430070, China

Corresponding author: Luo Ting-Ting, luotingting27@whut.edu.cn ; Tang Xin-Feng, tangxf@whut.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 52122108), the National Key Research and Development Program of China (Grant No. 2018YFB0703600), and the Independent and Innovative Project of Longzhong Laboratory in Hubei Province, China (Grant No. 2022ZZ-07).

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References

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Cited By

图 1 (a) 区熔法制备Bi_2–x Sb_xTe_2.994Cl_0.006和Bi_1.8Sb_0.2Te_2.994–ySe_yCl_0.006样品粉末X射线衍射图谱; (b) Bi_1.8Sb_0.2Te_2.694Se_0.3Cl_0.006样品垂直于提拉方向自由断裂截面的场发射扫描电子显微镜照片; (c) Bi_1.8Sb_0.2Te_2.694Se_0.3Cl_0.006样品抛光表面背散射电子图像(单位原子百分比)以及对应区域Bi, Sb, Se和Te等元素的面分布图像

Figure 1. (a) Powder XRD patterns of Bi_2–x Sb_xTe_2.994Cl_0.006 and Bi_1.8Sb_0.2Te_2.994–ySe_yCl_0.006 samples prepared by zone melting method; (b) field emission scanning electron microscope images of freshly fractured surfaces of the Bi_1.8Sb_0.2Te_2.694Se_0.3Cl_0.006 sample measured perpendicular to the travel direction during zone melting; (c) backscattered electron image of polished surfaces for Bi_1.8Sb_0.2Te_2.694Se_0.3Cl_0.006 sample and the corresponding elemental mapping images for Bi, Sb, Se and Te, respectively.

DownLoad: Full-Size Img PowerPoint

图 2 Bi_2–x Sb_xTe_2.994Cl_0.006和Bi1_.8Sb_0.2Te_2.994–ySe_yCl_0.006样品的电输运性能　(a), (b) 电导率; (c), (d) Seebeck系数; (e), (f) 功率因子

Figure 2. Temperature-dependent electronic transport properties for Bi_2–x Sb_xTe_2.994Cl_0.006 and Bi_1.8Sb_0.2Te_2.994–ySe_yCl_0.006 samples: (a), (b) Electrical conductivity; (c), (d) Seebeck coefficient; (e), (f) power factor.

DownLoad: Full-Size Img PowerPoint

图 3 (a), (b) 室温载流子浓度及迁移率随Sb, Se含量的变化; (c) 室温下样品的塞贝克系数与载流子浓度的关系, 图中紫色实线、红色实线、黄色实线为不同态密度有效质量下基于单抛带模型计算的塞贝克系数与载流子浓度关系曲线

Figure 3. (a), (b) Hall carrier mobility and concentration change with respect to the Sb, Se content; (c) Seebeck coefficients as a function of the charge carrier concentration at 300 K, where the colored dash lines are Pisarenko plots based on the single parabolic band model with different effective mass.

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图 4 Bi₂Te₃基化合物中不同点缺陷形成能　(a) Bi_2–x Sb_xTe₃固溶体; (b) Bi_2–x Sb_xTe_3–ySe_y固溶体

Figure 4. Theoretically calculated formation energies of different point defects in (a) Bi_2–x Sb_xTe₃ and (b) Bi_2–x Sb_xTe_3–ySe_y solid solution as a function of the Fermi level under the Te-poor condition.

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图 5 在200 K下, 不同样品(a) 两种载流子浓度及其比值随组分变化情况, 以及(b) 两种载流子迁移率及其比值随组分变化情况; (c) Bi_2–x Sb_xTe_3–ySe_y固溶体缺陷演化过程示意图

Figure 5. Composition dependence of (a) n_e, n_h, and n_h/n_e, (b) μ_e, μ_h, and μ_e/μ_h of different samples at 200 K. (c) Defect evolution process for Bi_2–x Sb_xTe_3–ySe_y solid solution.

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图 6 Bi_1.8Sb_0.2Te_2.994–ySe_yCl_0.006样品的(a) 总热导率κ、(b) 热导率κ－κ_e和(c) 无量纲热电优值ZT随温度的变化

Figure 6. Temperature-dependent (a) Total thermal conductivity, (b) thermal conductivity κ－κ_e, (c) ZT for Bi_1.8Sb_0.2Te_2.994–ySe_yCl_0.006 samples.

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表 1 Bi_2–x Sb_xTe_2.994Cl_0.006和Bi_1.8Sb_0.2Te_2.994–ySe_yCl_0.006样品的室温物理性能参数

Table 1. Room-temperature physic properties of Bi_2–x Sb_xTe_2.994Cl_0.006 and Bi_1.8Sb_0.2Te_2.994–ySe_yCl_0.006 samples.

Samples	σ/(10⁴ S·m^–1)	S/(μV·K^–1)	n/(10¹⁹ cm^–3)	μ/(cm²·V^–1·s^–1)	κ/(W·m^–1·K^–1)	m*/m₀
x = 0	11.2	–214.0	1.06	568	1.84	0.51
x = 0.05	11.0	–209.6	0.91	750	1.75	0.45
x = 0.10	9.94	–216.4	0.88	706	1.72	0.45
x = 0.15	9.16	–223.2	0.82	698	1.58	0.45
x = 0.20	5.79	–210.0	0.64	661	1.66	0.36
y = 0.05	8.97	–223.1	1.16	481	1.42	0.57
y = 0.10	8.46	–223.6	1.95	271	1.41	0.80
y = 0.15	9.94	–209.9	2.35	264	1.35	0.86
y = 0.20	8.82	–215.8	2.57	214	1.45	0.94
y = 0.25	8.68	–217.4	1.92	282	1.33	0.66
y = 0.30	9.15	–207.2	1.80	318	1.30	0.70

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[1]	Liu S X, Tian J L, Wu S, Zhang W, Luo M Y 2022 Nano Energy 93 106812 Google Scholar
[2]	Hu B X, Shi X L, Zou J, Chen Z G 2022 Chem. Eng. J. 437 135268 Google Scholar
[3]	Chen W Y, Shi X L, Zou J, Chen Z G 2022 Mater. Sci. Eng., R 151 100700 Google Scholar
[4]	Han C G, Qian X, Li Q K, Deng B, Zhu Y B, Han Z J, Zhang W Q, Wang W C, Feng S P, Chen G, Liu W S 2020 Science 368 1091 Google Scholar
[5]	Zhang Q, Yuan M, Pang K, Zhang Y, Wang R, Tan X, Wu G, Hu H, Wu J, Sun P, Liu G Q, Jiang J 2023 Adv. Mater. 35 2300338 Google Scholar
[6]	Xie H Y, Hao S Q, Bao J K, Slade T J, Snyder G J, Wolverton C, Kanatzidis M G 2020 J. Am. Chem. Soc. 142 9553 Google Scholar
[7]	Xie H, Zhao L D, Kanatzidis M G 2024 Interdiscip. Mater. 1 24 Google Scholar
[8]	Liu Z, Hong T, Xu L, Wang S, Gao X, Chang C, Ding X, Xiao Y, Zhao L D 2022 Interdiscip. Mater. 2 161 Google Scholar
[9]	Suh J, Yu K M, Fu D Y, Liu X Y, Yang F, Fan J, Smith D J, Zhang Y H, Furdyna J K, Dames C, Walukiewicz W, Wu J Q 2015 Adv. Mater. 27 3681 Google Scholar
[10]	Tang X, Li Z, Liu W, Zhang Q, Uher C 2022 Interdiscip. Mater. 1 88 Google Scholar
[11]	Medlin D L, Yang N, Spataru C D, Hale L M, Mishin Y 2019 Nat. Commun. 10 1820 Google Scholar
[12]	Cheng Y, Cojocaru-Mirédin O, Keutgen J, Yu Y, Küpers M, Schumacher M, Golub P, Raty J Y, Dronskowski R, Wuttig M 2019 Adv. Mater. 31 1904316 Google Scholar
[13]	Shen J J, Hu L P, Zhu T J, Zhao X B 2011 Appl. Phys. Lett. 99 124102 Google Scholar
[14]	Zhu T J, Hu L P, Zhao X B, He J 2016 Adv. Sci. 3 1600004 Google Scholar
[15]	Horak J, Stary Z, Lošťák P, Pancíř J 1990 J. Phys. Chem. Solids 51 1353 Google Scholar
[16]	Starý Z, Horak J, Stordeur M, Stölzer M 1988 J. Phys. Chem. Solids 49 29 Google Scholar
[17]	Horak J, Čermák K, Koudelka L 1986 J. Phys. Chem. Solids 47 805 Google Scholar
[18]	Miller G R, Li C Y 1965 J. Phys. Chem. Solids 26 173 Google Scholar
[19]	Gobrecht H, Pantzer G, Boeters K E 1964 Z. Phys. 177 68 Google Scholar
[20]	Offergeld G, Van Cakenberghe J 1959 J. Phys. Chem. Solids 11 310 Google Scholar
[21]	鲁志强, 刘可可, 李强, 胡芹, 冯丽萍, 张清杰, 吴劲松, 苏贤礼, 唐新峰 2023 无机材料学报 38 1331 Google Scholar Lu Z Q, Liu K K, Li Q, Hu Q, Feng L P, Zhang Q J, Wu J S, Su X L, Tang X F 2023 J. Inorg. Mater. 38 1331 Google Scholar
[22]	李强, 陈硕, 刘可可, 鲁志强, 胡芹, 冯丽萍, 张清杰, 吴劲松, 苏贤礼, 唐新峰 2023 72 097101 Google Scholar Li Q, Chen S, Liu K K, Lu Z Q, Hu Q, Feng L P, Zhang Q J, Wu J S, Su X L, Tang X F 2023 Acta Phys. Sin. 72 097101 Google Scholar
[23]	Zhang Q, Cao F, Liu W, Lukas K, Yu B, Chen S, Opeil C, Broido D, Chen G, Ren Z 2012 J. Am. Chem. Soc. 134 10031 Google Scholar
[24]	Mehta R J, Zhang Y L, Karthik C, Singh B, Siegel R W, Borca-Tasciuc T, Ramanath G 2012 Nat. Mater. 11 233 Google Scholar
[25]	Heremans J P, Wiendlocha B, Chamoire A M 2012 Energy Environ. Sci. 5 5510 Google Scholar
[26]	Pei Y Z, Heinz N A, LaLonde A, Snyder G J 2011 Energy Environ. Sci. 4 3640 Google Scholar
[27]	Xie W J, Tang X F, Yan Y G, Zhang Q J, Tritt T M 2009 Appl. Phys. Lett. 94 102111 Google Scholar
[28]	Navratil J, Starý Z, Plechacek T 1996 Mater. Res. Bull. 31 1559 Google Scholar
[29]	Shen J J, Zhu T J, Zhao X B, Zhang S N, Yang S H, Yin Z Z 2010 Energy Environ. Sci. 3 1519 Google Scholar
[30]	Oh T S, Hyun D B, Kolomoets N V 2000 Scr. Mater. 42 849 Google Scholar
[31]	Hao F, Qiu P, Tang Y, Bai S, Xing T, Chu H S, Zhang Q, Lu P, Zhang T, Ren D, Chen J, Shi X, Chen L 2016 Energy Environ. Sci. 9 3120 Google Scholar
[32]	Hwang J Y, Kim J, Kim H S, Kim S I, Lee K H, Kim S W 2018 Adv. Energy Mater. 8 1800065 Google Scholar
[33]	Qin B, Wang D, Liu X, Qin Y, Dong J F, Luo J, Li J W, Liu W, Tan G J, Tang X F, Li J F, He J, Zhao L D 2021 Science 373 556 Google Scholar
[34]	Su X L, Wei P, Li H, Liu W, Yan Y G, Li P, Su C Q, Xie C J, Zhao W Y, Zhai P C, Zhang Q J, Tang X F, Uher C 2017 Adv. Mater. 29 23 Google Scholar
[35]	陶颖, 祁宁, 王波, 陈志权, 唐新峰 2018 67 197201 Google Scholar Tao Y, Qi N, Wang B, Chen Z Q, Tang X F 2018 Acta Phys. Sin. 67 197201 Google Scholar
[36]	杨东旺, 罗婷婷, 苏贤礼, 吴劲松, 唐新峰 2021 无机材料学报 36 991 Google Scholar Yang D W, Luo T T, Su X L, Wu J S, Tang X F 2021 J. Inorg. Mater. 36 991 Google Scholar
[37]	Kim H S, Gibbs Z M, Tang Y L, Wang H, Snyder G J 2015 APL Mater. 3 041506 Google Scholar
[38]	Witting I T, Ricci F, Chasapis T C, Hautier G, Snyder G J 2020 Research 2020 4361703 Google Scholar

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Vol. 73, Issue 9 - 2024-05-05

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