Hygrothermal Stability of Bi2Te3-based Thermoelectric Materials

doi:10.15541/jim20220736

Abstract

Abstract:

Bi₂Te₃-based thermoelectric (TE) materials have already been commercialized, of which the hygrothermal stability has a direct impact on the service reliability of TE devices, but is still confronted many challenges. This work investigated the degradation behavior of commercial n-type Bi₂Se_0.21Te_2.79 and p-type Bi_0.4Sb_1.6Te₃ TE materials during storage in 85 ℃, 85% RH hygrothermal environment for 600 h. The surfaces of n-type Bi₂Se_0.21Te_2.79 and p-type Bi_0.4Sb_1.6Te₃ TE materials were oxidized with reaction process of Bi₂Te₃+O₂→Bi₂O₃+TeO₂ and Bi₂Te₃+Sb₂Te₃+O₂→Bi₂O₃+Sb₂O₃+TeO₂, respectively. The oxidation process creates nanoscale holes and even microcracks inside the material, which leads to an overall deterioration of the electrical and thermal properties. At room temperature, the electrical conductivity of the n-type Bi₂Se_0.21Te_2.79 material drops from 9.45×10⁴ S·m^-1 to 7.79×10⁴ S·m^-1 after exposure, and ZT decreases from 0.97 to 0.79, while Seebeck coefficient of the p-type Bi_0.4Sb_1.6Te₃ material declines from 243 μV·K^-1to 220 μV·K^-1, correspondingly, ZT decreases from 1.24 to 0.97. In conclusion, Bi₂Te₃-based TE materials have extremely poor hygrothermal stability, and their corresponding micro-TE devices need to be strictly encapsulated in service to prevent complex redox reactions between the TE materials themselves and the environmental water vapor and air.

Key words: Bi₂Te₃, thermoelectric material, hygrothermal stability

CLC Number:

TQ174

XIAO Yani, LYU Jianan, LI Zhenming, LIU Mingyang, LIU Wei, REN Zhigang, LIU Hongjing, YANG Dongwang, YAN Yonggao. Hygrothermal Stability of Bi₂Te₃-based Thermoelectric Materials[J]. Journal of Inorganic Materials, 2023, 38(7): 800-806.

Figures/Tables 9

Table 1 Room temperature thermoelectric performance of n-type Bi2Se0.21Te2.79 and p-type Bi0.4Sb1.6Te3 materials before and after storage in hygrothermal environment (85 ℃, 85% RH) for 600 h

Parameter at room temperature	n-type Bi₂Se_0.21Te_2.79
Parameter at room temperature	0 h	600 h	0 h	600 h
σ / (×10⁴, S·m^-1)	9.45	7.79	9.12	8.69
S / (μV·K^-1)	219	224	243	220
n / (×10¹⁹, cm^-3)	1.25	1.32	1.52	1.47
μ / (cm²·V^-1·s^-1)	470	369	375	370
PF / (mW·m^-1·K^-2)	4.54	3.90	5.41	4.21
κ / (W·m^-1·K^-1)	1.40	1.48	1.31	1.29
ZT	0.97	0.79	1.24	0.97

Fig. 1 (a1, b1) XRD patterns of samples after storage in hygrothermal environment for different time with (a2, b2) EDS results of material surface after storage in hygrothermal environment for 600 h (a1, a2) n-type Bi2Se0.21Te2.79; (b1, b2) p-type Bi0.4Sb1.6Te3

Fig. 2 Surface XPS spectra of n-type Bi2Se0.21Te2.79 material (a1-b1) before and (a2-b2) after storage in hygrothermal environment for 600 h (a1, a2) Bi4f; (b1, b2) Te3d

Fig. 3 Surface XPS spectra of p-type Bi0.4Sb1.6Te3 material (a1-c1) before and (a2-c2) after storage in hygrothermal environment for 600 h (a1, a2) Bi4f; (b1, b2) Te3d; (c1, c2) Sb3d

Fig. 4 FESEM images of (a1, a2) n-type Bi2Se0.21Te2.79 and (b1, b2) p-type Bi0.4Sb1.6Te3 material (a1, b1) before and (a2, b2) after storage in hygrothermal environment for 600 h

Fig. 5 (a) TEM image of the area close to the surface of n-type Bi2Se0.21Te2.79 material exposed to hygrothermal environment for 600 h; (b) elemental surface distribution profiles of the square region in (a); (c) HRTEM image of the square region in (a); (d) IFFT image of (c); (e) HAADF-STEM image of the area close to the surface of p-type Bi0.4Sb1.6Te3 material exposed to hygrothermal environment and (f) its elemental surface distribution profiles of the region (b1, f1) O; (b2, f2) Bi; (b3, f3) Te; (b4)Se; (f4) Sb

Fig. S1 Thermoelectric performance of n-type Bi2Se0.21Te2.79 in hygrothermal environment (85 ℃, 85% RH) (a) Electrical conductivity; (b) Seebeck coefficient; (c) Room temperature carrier concentration and carrier mobility; (d) Power factor; (e) Thermal conductivity; (f) ZT

Fig. S2 Thermoelectric performance of p-type Bi0.4Sb1.6Te3 in hygrothermal environment (85 ℃, 85% RH) (a) Electrical conductivity; (b) Seebeck coefficient; (c) Room temperature carrier concentration and carrier mobility; (d) Power factor; (e) Thermal conductivity; (f) ZT

Fig. S3 FESEM images of samples exposed to hygrothermal environment for different time n-type Bi2Se0.21Te2.79: (a1) 200 h; (a2) 400 h; p-type Bi0.4Sb1.6Te3: (b1) 200 h; (b2) 400 h

References 38

[1]	CORNETT J, CHEN B, HAIDAR S, et al. Fabrication and characterization of Bi₂Te₃-based chip-scale thermoelectric energy harvesting devices. Journal of Electronic Materials, 2016, 46(5):2844. DOI URL
[2]	LIU C, ZHAO K, FAN Y, et al. A flexible thermoelectric film based on Bi₂Te₃ for wearable applications. Functional Materials Letters, 2021, 15(1):2251005. DOI URL
[3]	NOZARIASBMARZ A, DYCUS J H, CABRAL M J, et al. Efficient self-powered wearable electronic systems enabled by microwave processed thermoelectric materials. Applied Energy, 2021, 283: 116211.
[4]	HOU C C, VAN TOAN N, ONO T. High density micro-thermoelectric generator based on electrodeposition of Bi₂Te₃ and Sb₂Te₃. 2022 IEEE 35th International Conference on Micro Electro Mechanical Systems Conference (MEMS), Tokyo, 2022: 600-603.
[5]	YAN Q, KANATZIDIS M G. High-performance thermoelectrics and challenges for practical devices. Nature Materials, 2022, 21(5):503. DOI
[6]	YUAN X, L Z, SHAO Y, et al. Bi₂Te₃-based wearable thermoelectric generator with high power density: from structure design to application. Journal of Materials Chemistry C, 2022, 10: 6456.
[7]	FRANCIOSO L, DE PASCALI C, FARELLA I, et al. Flexible thermoelectric generator for ambient assisted living wearable biometric sensors. Journal of Power Sources, 2011, 196(6):3239. DOI URL
[8]	LU Z, ZHANG H, MAO C, et al. Silk fabric-based wearable thermoelectric generator for energy harvesting from the human body. Applied Energy, 2016, 164: 57.
[9]	WANG Y, SHI Y, MEI D, et al. Wearable thermoelectric generator to harvest body heat for powering a miniaturized accelerometer. Applied Energy, 2018, 215: 690.
[10]	ZOU Q, SHANG H, HUANG D, et al. Bi₂Te₃-based flexible thermoelectric generator for wearable electronics. Applied Physics Letters, 2022, 120(2):023903. DOI URL
[11]	YOU H, LI Z, SHAO Y, et al. Flexible Bi₂Te₃-based thermoelectric generator with an ultra-high power density. Applied Thermal Engineering 2022, 202: 117818.
[12]	XU Z, YANG D, YUAN X, et al. Objective evaluation of wearable thermoelectric generator: from platform building to performance verification. Review of Scientific Instruments, 2022, 93(4):045105. DOI URL
[13]	HENDRICKS T J, KARRI N K. Micro- and nano-technology: a critical design key in advanced thermoelectric cooling systems. Journal of Electronic Materials, 2009, 38(7):1257. DOI URL
[14]	TANG X, LI Z, LIU W, et al. A comprehensive review on Bi₂Te₃- based thin films: thermoelectrics and beyond. Interdisciplinary Materials, 2022, 1(1):88. DOI URL
[15]	MAMUR H, BHUIYAN M R A, KORKMAZ F, et al. A review on bismuth telluride (Bi₂Te₃) nanostructure for thermoelectric applications. Renewable and Sustainable Energy Reviews, 2018, 82: 4159.
[16]	ZHU W, WEI P, ZHANG J, et al. Fabrication and excellent performances of bismuth telluride-based thermoelectric devices. ACS Applied Materials & Interfaces, 2022, 14(10):12276.
[17]	LIN Y, WU X, LI Y, et al. Revealing multi-stage growth mechanism of Kirkendall voids at electrode interfaces of Bi₂Te₃-based thermoelectric devices with in-situ TEM technique. Nano Energy, 2022, 102: 107736.
[18]	TASHIRO M, SUKENAGA S, IKEMOTO K, et al. Interfacial reactions between pure Cu, Ni, and Ni-Cu alloys and p-type Bi₂Te₃bulk thermoelectric material. Journal of Materials Science, 2021, 56(29):16545. DOI
[19]	CHEN L, BAI S, SHI X, et al. High temperature interfacial stability of Fe/Bi_0.5Sb_1.5Te₃thermoelectric elements. Journal of Inorganic Materials, 2021, 36(2):197. DOI URL
[20]	ZHENG Y, TAN X Y, WAN X, et al. Thermal stability and mechanical response of Bi₂Te₃-based materials for thermoelectric applications. ACS Applied Energy Materials, 2019, 3(3): 2078. DOI URL
[21]	LIN C F, HAU N Y, HUANG Y T, et al. Synergetic effect of Bi₂Te₃ alloys and electrodeposition of Ni for interfacial reactions at solder/Ni/Bi₂Te₃ joints. Journal of Alloys and Compounds, 2017, 708: 220.
[22]	JIANG C, FAN X A, HU J, et al. Thermal stability of zone melting p-type (Bi, Sb)₂Te₃ ingots and comparison with the corresponding powder metallurgy samples. Journal of Electronic Materials, 2018, 47(7):4038. DOI
[23]	JIANG C, FAN X A, FENG B, et al. Thermal stability of p-type polycrystalline Bi₂Te₃-based bulks for the application on thermoelectric power generation. Journal of Alloys and Compounds, 2017, 692: 885.
[24]	HU X, FAN X A, JIANG C, et al. Thermal stability of n-type zone- melting Bi₂(Te, Se)₃ alloys for thermoelectric generation. Materials Research Express, 2018, 6(3):035907. DOI URL
[25]	TANG H, HUI B, YANG X, et al. Thermal stability and interfacial structure evolution of Bi₂Te₃-based micro thermoelectric devices. Journal of Alloys and Compounds, 2022, 896: 163090.
[26]	ARUN P, TYAGI P, VEDESHWAR, et al. Ageing effect of Sb₂Te₃ thin films ageing effect of Sb₂Te₃ thin films. Physica B: Condensed Matter, 2001, 307: 105.
[27]	BANDO H, KOIZUMI K, OIKAWA Y, et al. The time-dependent process of oxidation of the surface of Bi₂Te₃ studied by X-ray photoelectron spectroscopy. Journal of Physics: Condensed Matter, 2000, 12: 5607.
[28]	GUO J H, QIU F, ZHANG Y, et al. Surface oxidation properties in a topological insulator Bi₂Te₃ film. Chinese Physics Letters, 2013, 30: 106801.
[29]	MUSIC D, CHANG K, SCHMIDT P, et al. On atomic mechanisms governing the oxidation of Bi₂Te₃. Journal of Physics: Condensed Matter, 2017, 29: 485705.
[30]	SIROTINA A P, CALLAERT C, VOLYKHOV A A, et al. Mechanistic studies of gas reactions with multicomponent solids: what can we learn by combining NAP XPS and atomic resolution STEM/EDX? The Journal of Physical Chemistry C, 2019, 123: 26201.
[31]	THOMAS C R, VALLON M K, FRITH M G, et al. Surface oxidation of Bi₂(Te,Se)₃ topological insulators depends on cleavage accuracy. Chemistry of Materials, 2016, 28: 35.
[32]	QU Q, LIU B, LIANG J, et al. Expediting hydrogen evolution through topological surface states on Bi₂Te₃. ACS Catalysis, 2020, 10: 1656.
[33]	SHARMA P A, OHTA T, BRUMBACH M T, et al. Ex Situ photoelectron emission microscopy of polycrystalline bismuth and antimony telluride surfaces exposed to ambient oxidation. Applied Materials & Interfaces, 2021, 13: 18218.
[34]	LU B, HU S, LI W E, et al. Preparation and characterization of Sb₂Te₃ thin films by coevaporation. International Journal of Photoenergy, 2010, 4: 476589.
[35]	NORIMASA O, KUROKAWA T, EGUCHI R, et al. Evaluation of thermoelectric performance of Bi₂Te₃ films as a function of temperature increase rate during heat treatment. Coatings, 2021, 11(1):38. DOI URL
[36]	LI A, NAN P, WANG Y, et al. Chemical stability and degradation mechanism of Mg₃Sb₂-Bi thermoelectrics towards room-temperature applications. Acta Materialia, 2022, 239: 118301.
[37]	ZHAO Y, BURDA C. Chemical synthesis of Bi_(0.5)Sb_(1.5)Te₃ nanocrystals and their surface oxidation properties. ACS Applied Materials & Interfaces, 2009, 1(6):1259.
[38]	JEONG K, PARK D, MAENG I, et al. Modulation of optoelectronic properties of the Bi₂Te₃nanowire by controlling the formation of selective surface oxidation. Applied Surface Science, 2021, 548: 149069.

Hygrothermal Stability of Bi₂Te₃-based Thermoelectric Materials

RichHTML

PDF (PC)

Knowledge

Abstract

Cite this article

share this article

Figures/Tables 9

References 38

Related Articles 15

Recommended Articles

Metrics

Comments

[1]	CHENG Jun, ZHANG Jiawei, QIU Pengfei, CHEN Lidong, SHI Xun. Preparation and Thermoelectric Transport Properties of P-doped β-FeSi₂ [J]. Journal of Inorganic Materials, 2024, 39(8): 895-902.
[2]	CHEN Hao, FAN Wenhao, AN Decheng, CHEN Shaoping. Improvement of Thermoelectric Performance of SnTe by Energy Band Optimization and Carrier Regulation [J]. Journal of Inorganic Materials, 2024, 39(3): 306-312.
[3]	ZHANG Zhe, SUN Tingting, WANG Lianjun, JIANG Wan. Flexible Thermoelectric Films with Different Ag₂Se Dimensions: Performance Optimization and Device Integration [J]. Journal of Inorganic Materials, 2024, 39(11): 1221-1227.
[4]	MENG Yuting, WANG Xuemei, ZHANG Shuxian, CHEN Zhiwei, PEI Yanzhong. Single- and Two-band Transport Properties Crossover in Bi₂Te₃ Based Thermoelectrics [J]. Journal of Inorganic Materials, 2024, 39(11): 1283-1291.
[5]	SU Haojian, ZHOU Min, LI Laifeng. Optimization of Thermoelectric Properties of SnTe via Multi-element Doping [J]. Journal of Inorganic Materials, 2024, 39(10): 1159-1166.
[6]	HE Danqi, WEI Mingxu, LIU Ruizhi, TANG Zhixin, ZHAI Pengcheng, ZHAO Wenyu. Heavy-Fermion YbAl₃ Materials: One-step Synthesis and Enhanced Thermoelectric Performance [J]. Journal of Inorganic Materials, 2023, 38(5): 577-582.
[7]	HUA Siheng, YANG Dongwang, TANG Hao, YUAN Xiong, ZHAN Ruoyu, XU Zhuoming, LYU Jianan, XIAO Yani, YAN Yonggao, TANG Xinfeng. Effect of Surface Treatment of n-type Bi₂Te₃-based Materials on the Properties of Thermoelectric Units [J]. Journal of Inorganic Materials, 2023, 38(2): 163-169.
[8]	LI Jianbo, TIAN Zhen, JIANG Quanwei, YU Lifeng, KANG Huijun, CAO Zhiqiang, WANG Tongmin. Effects of Different Element Doping on Microstructure and Thermoelectric Properties of CaTiO₃ [J]. Journal of Inorganic Materials, 2023, 38(12): 1396-1404.
[9]	WANG Pengjiang, KANG Huijun, YANG Xiong, LIU Ying, CHENG Cheng, WANG Tongmin. Inhibition of Lattice Thermal Conductivity of ZrNiSn-based Half-Heusler Thermoelectric Materials by Entropy Adjustment [J]. Journal of Inorganic Materials, 2022, 37(7): 717-723.
[10]	CHENG Cheng, LI Jianbo, TIAN Zhen, WANG Pengjiang, KANG Huijun, WANG Tongmin. Thermoelectric Property of In₂O₃/InNbO₄ Composites [J]. Journal of Inorganic Materials, 2022, 37(7): 724-730.
[11]	LOU Xunuo, DENG Houquan, LI Shuang, ZHANG Qingtang, XIONG Wenjie, TANG Guodong. Thermal and Electrcial Transport Properities of Ge Doped MnTe Thermoelectrics [J]. Journal of Inorganic Materials, 2022, 37(2): 209-214.
[12]	JIN Min, BAI Xudong, ZHANG Rulin, ZHOU Lina, LI Rongbin. Metal Sulfide Ag₂S: Fabrication via Zone Melting Method and Its Thermoelectric Property [J]. Journal of Inorganic Materials, 2022, 37(1): 101-106.
[13]	ZHANG Cencen, WANG Xue, PENG Liangming. Thermoelectric Transport Characteristics of n-type (PbTe)_1-_x_-_y(PbS)_x(Sb₂Se₃)_y Systems via Stepwise Addition of Dual Components [J]. Journal of Inorganic Materials, 2021, 36(9): 936-942.
[14]	YANG Qingyu, QIU Pengfei, SHI Xun, CHEN Lidong. Application of Entropy Engineering in Thermoelectrics [J]. Journal of Inorganic Materials, 2021, 36(4): 347-354.
[15]	KANG Huijun,ZHANG Xiaoying,WANG Yanxia,LI Jianbo,YANG Xiong,LIU Daquan,YANG Zerong,WANG Tongmin. Effect of Rare-earth Variable-valence Element Eu doping on Thermoelectric Property of BiCuSeO [J]. Journal of Inorganic Materials, 2020, 35(9): 1041-1046.