Improvement of thermoelectric performance of SnTe-based solid solution by entropy engineering

Li Meng-Rong; Ying Peng-Zhan; Li Xie; Cui Jiao-Lin

doi:10.7498/aps.71.20221247

Abstract

SnTe is a good alternative to PbTe in the thermoelectric (TE) applications, in that it is a compound with no toxic element Pb. Besides, the compound SnTe has a relatively narrow bandgap (0.3–0.4 eV) and high Sn vacancy concentration (Sn_v) as well. Accordingly, it gives a high carrier concentration (10²¹ cm^–3) at room temperature (RT), which is not favorable for thermoelectrics, therefore the regulation of both the electronic and phonon scattering mechanisms is strongly required. Up to date, there have been many approaches to improving its TE performance. The typical examples are those involving the valence band convergence, nanostructuring, substitutional and interstitial defects, and lattice softening, which are all practical and effective to improve the TE performance of SnTe. However, in this work the entropy is taken as an indicator to design the SnTe-based TE material with multicomponents and then optimize its TE performance. The detailed scheme involves the chemical composition design step by step. At first, SnTe alloys with 5% GaTe to form a solid solution Sn_0.95Ge_0.05Te, aiming to increase the solubility of the foreign species. The second step is to form another solid solution (Sn_0.95Ge_0.05Te)_0.95(Ag₂Se)_0.05 via the alloying Sn_0.95Ge_0.05Te with 5% Ag₂Se. The purpose of this step is to reduce the p-type carrier concentration of the system, for the species Ag₂Se is a typical n-type semiconductor. The last step is to form a series of solid solutions (Sn_0.95–xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 by substituting different amounts of Bi on Sn in (Sn_0.95Ge_0.05Te)_0.95(Ag₂Se)_0.05, to further enhance the configurational entropy (ΔS). Because of the above approaches, both the carrier concentration and thermal conductivity decrease while the highest TE figure of merit (ZT) increases from 0.22 for the pristine SnTe to ~0.8 for the alloy (Sn_0.95–xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 (x = 0.075). This result proves that the entropy engineering is a practical way to improve the TE performance of SnTe, and at the same time it illustrates that it is very important to harmonize the entropy engineering with other electronic and phonon scattering mechanisms, in order to improve the TE performance of SnTe effectively.

Keywords:

Authors and contacts

1.
School of Materials Scienc and Chemical Engineering, Ningbo University of Technology, Ningbo 315211, China
2.
School of Materials Science and Engineering, China University of Mining and Technology, Xuzhou 221116, China

Corresponding author: Cui Jiao-Lin, cuijiaolin@163.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 51671109).

[1]	Zhang Q, Liao B, Lan Y C, Lukas K, Liu W, Esfarjani K, Opeil C, Broido D, Chen G, Ren Z 2013 PNAS 110 13261 Google Scholar
[2]	Rogers L 1968 J. Phys. D:Appl. Phys. 1 845 Google Scholar
[3]	Brebrick R 1963 J. Phys. Chem. Solids 24 27 Google Scholar
[4]	Li M, Ying P, Du Z, Liu X, Li X, Fang T, Cui J 2022 ACS Appl. Mater. Interfaces 14 8171 Google Scholar
[5]	Banik A, Shenoy U S, Saha S, Waghmare U V, Biswas K 2016 J. Am. Chem. Soc. 138 13068 Google Scholar
[6]	Tan G, Shi F, Hao S, Chi H, Bailey T P, Zhao L, Uher C, Wolverton C, Dravid V P, Kanatzidis M G 2015 J. Am. Chem. Soc. 137 11507 Google Scholar
[7]	Zhou M, Gibbs Z M, Wang H, Han Y, Xin C, Li L 2014 Phys. Chem. Chem. Phys. 16 20741 Google Scholar
[8]	Pei Y, Shi X, LaLonde A, Wang H, Chen L, Snyder G J 2011 Nature 473 66 Google Scholar
[9]	Pei Y, Wang H, Snyder G J 2012 Adv. Mater. 24 6125 Google Scholar
[10]	Moshwan R, Yang L, Zou J, Chen Z G 2017 Adv. Funct. Mater. 27 1703278 Google Scholar
[11]	Wang L, Tan X, Liu G, Xu J, Shao H, Yu B, Jiang H, Yue S, Jiang J 2017 ACS Energy Lett. 2 1203 Google Scholar
[12]	Tan G, Hao S, Hanus R C, Zhang X, Anand S, Bailey T P, Rettie A J E, Su X, Uher C, Dravid V P, Snyder G J, Wolverton C, Kanatzidis M G 2018 ACS Energy Lett. 3 705 Google Scholar
[13]	Banik A, Vishal B, Perumal S, Datta R, Biswas K 2016 Energy Environ. Sci. 9 2011 Google Scholar
[14]	Zhao L D, Lo S H, Zhang Y, Sun H, Tan G, Uher C, Wolverton C, Dravid V P, Kanatzidis M G 2014 Nature 508 373 Google Scholar
[15]	Zheng L, Li W, Lin S, Li J, Chen Z, Pei Y 2017 ACS Energy Lett. 2 563 Google Scholar
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[17]	Roychowdhury S, Biswas R K, Dutta M, Pati S K, Biswas K 2019 ACS Energy Lett. 4 1658 Google Scholar
[18]	Tan G, Zeier W G, Shi F, Wang P, Snyder G J, Dravid V P, Kanatzidis M G 2015 Chem. Mater. 27 7801 Google Scholar
[19]	Tang J, Gao B, Lin S, Wang X, Zhang X, Xiong F, Li W, Chen Y, Pei Y 2018 ACS Energy Lett. 3 1969 Google Scholar
[20]	Yao Z, Li W, Tang J, Chen Z, Lin S, Biswas K, Burkov A, Pei Y 2019 InfoMat 1 571 Google Scholar
[21]	Liu R, Chen H, Zhao K, Qin Y, Jiang B, Zhang T, Sha G, Shi X, Uher C, Zhang W, Chen L 2017 Adv. Mater. 29 1702712 Google Scholar
[22]	Hu L, Zhang Y, Wu H, Li J, Li Y, Mckenna M, He J, Liu F, Pennycook S, Zeng X 2018 Adv. Energy Mater. 8 1802116 Google Scholar
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[26]	Mi W, Qiu P, Zhang T, Lv Y, Shi X, Chen L 2014 Appl. Phys. Lett. 104 133903 Google Scholar
[27]	Snyder G J, Toberer E S 2008 Nat. Mater. 7 105 Google Scholar
[28]	Kim H, Gibbs Z, Tang Y, Wang H, Snyder G J 2015 APL Mater. 3 041506 Google Scholar
[29]	Roychowdhury S, Shenoy U S, Waghmare U V. Biswas K 2017 J. Mater. Chem. C 5 5737 Google Scholar
[30]	Song S, Lo C, Aminzare M, Tseng Y, Valiyaveettil S, Mozharivskyj Y 2020 Dalton Trans. 49 6135 Google Scholar
[31]	Tan G, Shi F, Sun H, Zhao L, Uher C, Dravid V P, Kanatzidis M G 2014 J. Mater. Chem. A 2 20849 Google Scholar
[32]	Guo X, Chen Z, Tang J 2020 Appl. Phys. Lett. 116 103901 Google Scholar
[33]	Chen Z, Guo X, Zhang F, Shi Q, Tang M, Ang R 2020 J. Mater. Chem. A 8 16790 Google Scholar
[34]	Chen R, Qiu P F, Jiang B B, Hu P, Zhang Y M, Yang J, Ren D, Shi X, Chen L 2018 J. Mater. Chem. A 6 6493 Google Scholar
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[38]	Cahill D G, Watson S K, Pohl R O 1992 Phys. Rev. B 46 6131 Google Scholar
[39]	You L, Zhang J, Pan S, Jiang Y, Wang K, Yang J, Pei Y, Zhu Q, Agne M T, Snyder G. J, Ren Z, Zhang W, Luo J 2019 Energy Environ. Sci. 12 3089 Google Scholar
[40]	Zhu H, Zhao T, Zhang B, An Z, Mao S, Wang G, Han X, Lu X, Zhang J, Zhou X 2021 Adv. Energy Mater. 11 2003304 Google Scholar
[41]	Li S, Li J, Yang L, Liu F, Ao W, Li Y 2016 Mater. Des. 108 51 Google Scholar
[42]	Guo F, Cui B, Geng H, Zhang Y, Wu H, Zhang Q, Yu B, Pennycook S J, Cai W, Sui J 2019 Small 15 1902493 Google Scholar

Cited By

图 1 (Sn_0.95-xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 (x = 0—0.1)的构型熵(ΔS)与Bi含量(x)的关系. ΔS₁和ΔS₂代表添加摩尔分数5% Ge和5% Ag₂Se后的熵增

Figure 1. Dependence of the configurational entropy (ΔS) on the Bi content (x) in (Sn_0.95-xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 (x = 0–0.1), where the ΔS₁ and ΔS₂ represent the increased entropy after addition of 5% Ge and 5% Ag₂Se (mole fraction), respectively.

DownLoad: Full-Size Img PowerPoint

图 2 (a) 各组材料的XRD谱图; (b) XRD的放大图(28°—29°); (c) 晶格常数a与Bi含量x的关系

Figure 2. (a) XRD diffraction patterns of different materials; (b) close-up view XRD patterns between 28°–29°; (c) lattice constants a as a function of Bi content x.

DownLoad: Full-Size Img PowerPoint

图 3 样品 (x = 0.05)的透射电镜图　(a) 低倍TEM图; (b) 高倍透射电镜图(HRTEM); (c) 选区电子衍射花样(SAED); (d) 能谱分析图(EDS)

Figure 3. Transmission electron microscopy (TEM) images observed on the sample (Sn_0.95-xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 (x = 0.05): (a) TEM image; (b) HRTEM image; (c) the selected area electron diffraction (SAED) pattern; (d) EDS analysis.

DownLoad: Full-Size Img PowerPoint

图 4 室温条件下本征SnTe, Sn_0.95Ge_0.05Te和(Sn_0.95–xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 (x = 0, 0.025, 0.050, 0.075, 0.100 样品的(a)载流子浓度(n_H); (b)载流子迁移率(μ)

Figure 4. (a) Hall hole concentration (n_H) and (b) carrier mobility (μ) of the pristine SnTe, Sn_0.95Ge_0.05Te, (Sn_0.95–xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 (x = 0, 0.025, 0.050, 0.075, 0.100) at room temperature (RT).

DownLoad: Full-Size Img PowerPoint

图 5 SnTe, Sn_0.95Ge_0.05Te和(Sn_0.95-xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 (x = 0, 0.025, 0.050, 0.075, 0.100)热电性能随温度的变化　(a) Seebeck系数(α); (b) 电导率 (σ), 插图为功率因子 (PF); (c) 晶格热导率 (κ_L), 插图为总热导率 (κ_total); (d) 热电优值(ZT )

Figure 5. Temperature dependence of the TE properties for SnTe, Sn_0.95Ge_0.05Te and (Sn_0.95-xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 (x = 0, 0.025, 0.050, 0.075, 0.100): (a) Seebeck coefficients (α); (b) electrical conductivities (σ), the insert is the power factors (PF); (c) lattice thermal conductivities. (κ_L), the insert is the κ_total; (d) Figure of the merit ZT

DownLoad: Full-Size Img PowerPoint

图 6 室温下各热电参数与(Sn_0.95-xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 (x = 0—0.1)构型熵(ΔS)的关系　(a) Seebeck系数与ΔS的关系; (b) 电导率与ΔS的关系; (c) 晶格热导率与ΔS的关系; (d) 热电优值与ΔS的关系

Figure 6. Dependence of the TE performance on the configurational entropy (ΔS) of (Sn_0.95-xGe_0.05Bi_xTe)_0.95(Ag₂Se)_0.05 (x = 0–0.1): (a) Dependence of the Seebeck coefficient (α) on the configurational entropy (ΔS); (b) dependence of the electrical conductivity (σ) on the configurational entropy (ΔS); (c) dependence of the lattice thermal conductivity (κ_L) on the configurational entropy (ΔS); (d) dependence of the ZT value on the configurational entropy (ΔS).

DownLoad: Full-Size Img PowerPoint

map

[1]	Zhang Q, Liao B, Lan Y C, Lukas K, Liu W, Esfarjani K, Opeil C, Broido D, Chen G, Ren Z 2013 PNAS 110 13261 Google Scholar
[2]	Rogers L 1968 J. Phys. D:Appl. Phys. 1 845 Google Scholar
[3]	Brebrick R 1963 J. Phys. Chem. Solids 24 27 Google Scholar
[4]	Li M, Ying P, Du Z, Liu X, Li X, Fang T, Cui J 2022 ACS Appl. Mater. Interfaces 14 8171 Google Scholar
[5]	Banik A, Shenoy U S, Saha S, Waghmare U V, Biswas K 2016 J. Am. Chem. Soc. 138 13068 Google Scholar
[6]	Tan G, Shi F, Hao S, Chi H, Bailey T P, Zhao L, Uher C, Wolverton C, Dravid V P, Kanatzidis M G 2015 J. Am. Chem. Soc. 137 11507 Google Scholar
[7]	Zhou M, Gibbs Z M, Wang H, Han Y, Xin C, Li L 2014 Phys. Chem. Chem. Phys. 16 20741 Google Scholar
[8]	Pei Y, Shi X, LaLonde A, Wang H, Chen L, Snyder G J 2011 Nature 473 66 Google Scholar
[9]	Pei Y, Wang H, Snyder G J 2012 Adv. Mater. 24 6125 Google Scholar
[10]	Moshwan R, Yang L, Zou J, Chen Z G 2017 Adv. Funct. Mater. 27 1703278 Google Scholar
[11]	Wang L, Tan X, Liu G, Xu J, Shao H, Yu B, Jiang H, Yue S, Jiang J 2017 ACS Energy Lett. 2 1203 Google Scholar
[12]	Tan G, Hao S, Hanus R C, Zhang X, Anand S, Bailey T P, Rettie A J E, Su X, Uher C, Dravid V P, Snyder G J, Wolverton C, Kanatzidis M G 2018 ACS Energy Lett. 3 705 Google Scholar
[13]	Banik A, Vishal B, Perumal S, Datta R, Biswas K 2016 Energy Environ. Sci. 9 2011 Google Scholar
[14]	Zhao L D, Lo S H, Zhang Y, Sun H, Tan G, Uher C, Wolverton C, Dravid V P, Kanatzidis M G 2014 Nature 508 373 Google Scholar
[15]	Zheng L, Li W, Lin S, Li J, Chen Z, Pei Y 2017 ACS Energy Lett. 2 563 Google Scholar
[16]	Tang J, Gao B, Lin S, Li J, Chen Z, Xiong F, Li W, Chen Y, Pei Y 2018 Adv. Funct. Mater. 28 1803586 Google Scholar
[17]	Roychowdhury S, Biswas R K, Dutta M, Pati S K, Biswas K 2019 ACS Energy Lett. 4 1658 Google Scholar
[18]	Tan G, Zeier W G, Shi F, Wang P, Snyder G J, Dravid V P, Kanatzidis M G 2015 Chem. Mater. 27 7801 Google Scholar
[19]	Tang J, Gao B, Lin S, Wang X, Zhang X, Xiong F, Li W, Chen Y, Pei Y 2018 ACS Energy Lett. 3 1969 Google Scholar
[20]	Yao Z, Li W, Tang J, Chen Z, Lin S, Biswas K, Burkov A, Pei Y 2019 InfoMat 1 571 Google Scholar
[21]	Liu R, Chen H, Zhao K, Qin Y, Jiang B, Zhang T, Sha G, Shi X, Uher C, Zhang W, Chen L 2017 Adv. Mater. 29 1702712 Google Scholar
[22]	Hu L, Zhang Y, Wu H, Li J, Li Y, Mckenna M, He J, Liu F, Pennycook S, Zeng X 2018 Adv. Energy Mater. 8 1802116 Google Scholar
[23]	Acharya S, Anwar S, Mori T, Soni A 2018 J. Mater. Chem. C 6 6489 Google Scholar
[24]	Sarkar D, Ghosh T, Banik A, Roychowdhury S, Sanyal D, Biswas K 2020 Angew Chem. Int. Ed. 59 11115 Google Scholar
[25]	Jood P, Ohta M 2020 ACS Appl. Energy Mater. 3 2160
[26]	Mi W, Qiu P, Zhang T, Lv Y, Shi X, Chen L 2014 Appl. Phys. Lett. 104 133903 Google Scholar
[27]	Snyder G J, Toberer E S 2008 Nat. Mater. 7 105 Google Scholar
[28]	Kim H, Gibbs Z, Tang Y, Wang H, Snyder G J 2015 APL Mater. 3 041506 Google Scholar
[29]	Roychowdhury S, Shenoy U S, Waghmare U V. Biswas K 2017 J. Mater. Chem. C 5 5737 Google Scholar
[30]	Song S, Lo C, Aminzare M, Tseng Y, Valiyaveettil S, Mozharivskyj Y 2020 Dalton Trans. 49 6135 Google Scholar
[31]	Tan G, Shi F, Sun H, Zhao L, Uher C, Dravid V P, Kanatzidis M G 2014 J. Mater. Chem. A 2 20849 Google Scholar
[32]	Guo X, Chen Z, Tang J 2020 Appl. Phys. Lett. 116 103901 Google Scholar
[33]	Chen Z, Guo X, Zhang F, Shi Q, Tang M, Ang R 2020 J. Mater. Chem. A 8 16790 Google Scholar
[34]	Chen R, Qiu P F, Jiang B B, Hu P, Zhang Y M, Yang J, Ren D, Shi X, Chen L 2018 J. Mater. Chem. A 6 6493 Google Scholar
[35]	Qiu Y, Jin Y, Wang D Y, Guan M, He W, Peng S, Liu R, Gao X, Zhao L 2019 J. Mater. Chem. A 7 26393 Google Scholar
[36]	Jiang B, Qiu P, Chen H, Huang J, Mao T, Wang Y, Song Q, Ren D, Shi X, Chen L 2018 Mater. Today Phys. 5 20 Google Scholar
[37]	Orabi R A R A, Mecholsky N A, Hwang J, Kim W, Rhyee J, Wee D, Fornari M 2016 Chem. Mater. 28 376 Google Scholar
[38]	Cahill D G, Watson S K, Pohl R O 1992 Phys. Rev. B 46 6131 Google Scholar
[39]	You L, Zhang J, Pan S, Jiang Y, Wang K, Yang J, Pei Y, Zhu Q, Agne M T, Snyder G. J, Ren Z, Zhang W, Luo J 2019 Energy Environ. Sci. 12 3089 Google Scholar
[40]	Zhu H, Zhao T, Zhang B, An Z, Mao S, Wang G, Han X, Lu X, Zhang J, Zhou X 2021 Adv. Energy Mater. 11 2003304 Google Scholar
[41]	Li S, Li J, Yang L, Liu F, Ao W, Li Y 2016 Mater. Des. 108 51 Google Scholar
[42]	Guo F, Cui B, Geng H, Zhang Y, Wu H, Zhang Q, Yu B, Pennycook S J, Cai W, Sui J 2019 Small 15 1902493 Google Scholar

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