Interface performance of Bi<sub>2</sub>Te<sub>3</sub>-based micro thermoelectric devices optimized synergistically by surface modification engineering

Tang Hao; Bai Hui; Lü Jia-Nan; Hua Si-Heng; Yan Yong-Gao; Yang Dong-Wang; Wu Jin-Song; Su Xian-Li; Tang Xin-Feng

doi:10.7498/aps.71.20220549

Abstract

The miniaturization of thermoelectric devices raises a strong requirement for the excellent interfacial properties of thermoelectric elements. Thus, achieving a heterogeneous interface with low interfacial contact resistivity and high interfacial bonding strength is a prerequisite for the successful fabrication of high-performance and high-reliability Bi₂Te₃-based micro thermoelectric devices. In this work, we adopt the acid pickling method to modify the surface structure of Bi_0.4Sb_1.6Te₃ material to synergistically optimize the interfacial properties of Bi_0.4Sb_1.6Te₃/Ni thermoelectric elements. The acid pickling process effectively modulates the work function of Bi_0.4Sb_1.6Te₃ material, which dramatically reduces the contact barrier height of Ni/Bi_0.4Sb_1.6Te₃ heterojunction from 0.22 to 0.02 eV. As a consequence, the corresponding interfacial contact resistivity of the element is greatly reduced from 14.2 to 0.22 μΩ·cm². Moreover, the acid pickling process effectively adjusts the surface roughness of the matrix, forming a V-shaped pit of 2–5 μm in depth on the substrate surface and leading to a pinning effect. This significantly enhances the physical bonding between the material surface and the Ni layer, which, together with the metallurgical bond formed by the interfacial diffusion reaction zone of about 50-nm-thick Ni/Bi_0.4Sb_1.6Te₃, greatly enhances the interfacial bond strength from 7.14 to 22.34 MPa. The excellent interfacial properties are further validated by the micro-thermoelectric devices. The maximum cooling temperature difference of 4.7 mm× 4.9 mm micro thermoelectric device fabricated by this process achieves 56.5 K, with hot side temperature setting at 300 K, and the maximum output power reaches 882 μW under the temperature gradient of 10 K. This work provides a new strategy for realizing the synergetic optimization of interfacial properties and opens up a new avenue for improving the performance of micro thermoelectric devices.

Keywords:

Authors and contacts

1.
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China
2.
Nanostructure Research Center, Wuhan University of Technology, Wuhan 430070, China

Corresponding author: Tang Xin-Feng, tangxf@whut.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 52122108, 51972256), and the National Key Research and Development Program of China (Grant No. 2019YFA0704900).

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References

[1]	Snyder G J, Toberer E S 2008 Nat. Mater. 7 105 Google Scholar
[2]	陶颖, 祁宁, 王波, 陈志权, 唐新峰 2018 67 197201 Google Scholar Tao Y, Qi N, W B, Chen Z Q, Tang X F 2018 Acta Phys. Sin. 67 197201 Google Scholar
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Cited By

图 A1 不同酸洗时间后的材料表面3D形貌及面粗糙度S_a

Figure A1. 3D surface topography and surface-roughness of the materials under different pickling time from 0 min to 10 min.

DownLoad: Full-Size Img PowerPoint

图 A2 Bi₂Te₃基热电材料的　(a) 电导率, (b) Seebeck系数, (c) 总热导率和(d) 热电优值ZT随温度的变化

Figure A2. Temperature dependences of (a) electrical conductivity, (b) Seebeck coefficient, (c) total thermal conductivity and (d) ZT value for Bi₂Te₃-based thermoelectric materials.

DownLoad: Full-Size Img PowerPoint

图 A3 不同酸洗时间后的Bi_0.4Sb_1.6Te₃/Ni界面接触电阻率测试结果　(a) 0 min; (b) 2 min; (c) 4 min; (d) 6 min; (e) 8 min; (f) 10 min

Figure A3. The results of interfacial contact resistivity of Bi_0.4Sb_1.6Te₃/Ni thermoelectric elements after different pickling time: (a) 0 min; (b) 2 min; (c) 4 min; (d) 6 min; (e) 8 min; (f) 10 min.

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图 A4 N-Bi₂Te₃/Ni热电元件的界面接触电阻率测试结果

Figure A4. The results of interfacial contact resistivity of N-Bi₂Te₃/Ni thermoelectric element.

DownLoad: Full-Size Img PowerPoint

图 1 Bi_0.4Sb_1.6Te₃/Ni热电元件的(a) 界面结合强度和(b) 界面接触电阻率随酸洗时间变化的关系, 其中红色虚线代表现有商业化水平; (c) 器件内阻随酸洗时间的变化关系, 其中右上角为微型热电器件实物照片; (d) 器件的最大制冷温差随酸洗时间的变化关系; 不同酸洗时间制备的器件在10 K温差下的 (e) 开路电压和(f) 输出功率随电流的变化关系

Figure 1. The pickling time dependences of (a) the interfacial bonding strength and (b) the interfacial contact resistivity for Bi_0.4Sb_1.6Te₃/Ni thermoelectric elements, the red dotted line represents the commercial level. (c) The relationship between the internal resistance of the devices and the pickling time, the upper right corner is the photograph of the micro thermoelectric device; (d) the relationship between the maximum cooling temperature difference of the device and pickling time; the current dependences of (e) open-circuit voltage and (f) output power of the devices prepared by different pickling time under 10 K temperature difference.

DownLoad: Full-Size Img PowerPoint

图 2 材料表面粗糙度随酸洗时间的变化关系

Figure 2. The relationship between the surface-roughness and pickling time.

DownLoad: Full-Size Img PowerPoint

图 3 (a) 不同酸洗时间后的材料表面FESEM图像; (b) 不同酸洗时间后热电元件抛光界面FESEM图像

Figure 3. FESEM images of (a) materials surface and (b) polishing interface of the thermoelectric elements after different pickling time.

DownLoad: Full-Size Img PowerPoint

图 4 (a) Bi_0.4Sb_1.6Te₃/Ni热电元件的界面HAADF-STEM图像, 区域1和区域2分别表示界面区域和基体的选区电子衍射; (b) 界面区域的元素面分布图谱, 其中紫色为Ni, 绿色为Te, 红色为Bi和蓝色为Sb; (c)—(f) 区域1的TEM图像, 界面相为Ni₃Te₂ and NiTe₂

Figure 4. (a) HAADF-STEM images of the Ni/Bi_0.4Sb_1.6Te₃ thermoelectric element contact interface, area 1 and 2 represents the selected area electron diffraction of the interface and the matrix, respectively; (b) EDS mapping of (a), purple: Ni, green: Te, red: Bi, blue: Sb; (c)–(f) TEM images of area 1 in Figure (a) and the interface phases are Ni₃Te₂ and NiTe₂ compounds.

DownLoad: Full-Size Img PowerPoint

图 5 不同酸洗时间后的材料表面的(a) UPS光谱以及(b) 截止边强度的结合能微分; (c) 材料表面功函数随酸洗时间变化的关系; 酸洗8 min前后的(d) Bi_0.4Sb_1.6Te₃/Ni热电元件的I-V曲线和(e) 能带结构示意图以及(f) 与Ni层界面接触势垒高度的变化示意图

Figure 5. (a) UPS spectra and (b) the binding energy differential of the cut-off edge intensity for the materials surface after different pickling time; (c) I-V curve for the Bi_0.4Sb_1.6Te₃/Ni thermoelectric elements and (d) surface energy band structure diagram and (e) schematic diagram of the height change of the contact barrier at the interface with Ni layer before and after pickling for 8 min.

DownLoad: Full-Size Img PowerPoint

表 A1 不同酸洗时间制备出的Bi_0.4Sb_1.6Te₃/Ni热电元件和N-Bi₂Te₃/Ni热电元件的五次界面结合强度测试结果

Table A1. The five repeated results of interfacial bonding strength for Bi_0.4Sb_1.6Te₃/Ni thermoelectric elements with different pickling time and N-Bi₂Te₃/Ni thermoelectric elements.

Sample	1#	2#	3#	4#	5#	Average/MPa
0 min	7.25	6.75	7.50	6.93	7.27	7.14
2 min	14.00	13.73	13.25	13.75	13.50	13.65
4 min	16.25	14.75	14.95	15.50	15.00	15.29
6 min	17.55	18.08	17.25	14.75	16.00	16.73
8 min	22.05	20.75	23.75	23.25	21.90	22.34
10 min	13.13	14.28	12.00	13.03	13.75	13.24
N-Bi₂Te₃/Ni	14.33	13.85	16.40	14.28	16.80	15.13

DownLoad: CSV

map

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[2]	陶颖, 祁宁, 王波, 陈志权, 唐新峰 2018 67 197201 Google Scholar Tao Y, Qi N, W B, Chen Z Q, Tang X F 2018 Acta Phys. Sin. 67 197201 Google Scholar
[3]	Mao J, Chen G, Ren Z 2020 Nat. Mater. 20 454 Google Scholar
[4]	范人杰, 江先燕, 陶奇睿, 梅期才, 唐颖菲, 陈志权, 苏贤礼, 唐新峰 2021 70 137102 Google Scholar Fan R J, Jiang X Y, Tao Q R, Mei Q C, Tang Y F, Chen Z Q, Su X L, Tang X F 2021 Acta Phys. Sin. 70 137102 Google Scholar
[5]	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
[6]	Tang X, Li Z, Liu W, Zhang Q, Uher C 2022 Interdisciplin. Mater. 1 88 Google Scholar
[7]	Venkatasubramanian R, Watkins C, Stokes D, Posthill J, Caylor C 2007 IEEE International Electron Devices Meeting Washington, USA, December 10–12, 2007, p367
[8]	Liu D, Zhao F Y, Yang H X, Tang G F 2015 Energy 83 29 Google Scholar
[9]	Yan J, Liao X, Yan D, Chen Y 2018 J. Microelectromech. Syst. 27 1 Google Scholar
[10]	Liu Q L, Li G D, Zhu H T, Zhao H Z 2022 Chin. Phys. B 31 047204 Google Scholar
[11]	Yu Y, Guo Z, Zhu W, Zhou J, Guo S, Wang Y, Deng Y 2022 Nano Energy 93 106818 Google Scholar
[12]	Aswal D K, Basu R, Singh A 2016 Energy Convers. Manage. 114 50 Google Scholar
[13]	Zhang Q H, Huang X Y, Bai S Q, Shi X, Uher C, Chen L D 2016 Adv. Eng. Mater. 18 194 Google Scholar
[14]	He R, Schierning G, Nielsch K 2018 Adv. Mater. Technol. 3 1700256 Google Scholar
[15]	Liu W, Bai S 2019 J. Materiomics 5 321 Google Scholar
[16]	胡晓凯, 张双猛, 赵府, 刘勇, 刘玮书 2019 无机材料学报 34 269 Google Scholar Hu X K, Zhang S M, Zhao F, Liu Y, Liu W S 2019 J. Inorg. Mater. 34 269 Google Scholar
[17]	Hatzikraniotis E, Zorbas K, Samaras I, Kyratsi T, Paraskevopoulos K 2010 J. Electron. Mater. 39 2112 Google Scholar
[18]	Park W, Barako M T, Marconnet A M, Asheghi M, Goodson K E 13 th InterSociety Conference on Thermal and Thermomechanical Phenomena in Electronic Systems San Diego, USA, May 30–June 1, 2012, p107
[19]	Barako M T, Park W, Marconnet A M, Asheghi M, Goodson K E 13 th InterSociety Conference on Thermal and Thermomechanical Phenomena in Electronic Systems San Diego, USA, May 30–June 1, 2012, p86
[20]	Gupta R, White J, Iyore O, Chakrabarti U, Alshareef H N, Gnade B 2009 Electrochem. Solid-State Lett. 12 H302 Google Scholar
[21]	Iyore O D, Lee T H, Gupta R P, White J B, Alshareef H N, Kim M J, Gnade B E 2010 Surf. Interface Anal. 41 440 Google Scholar
[22]	Feng H-P, Yu B, Chen S, Collins K, He C, Ren Z, Chen G 2011 Electrochim. Acta 56 3079 Google Scholar
[23]	Taylor P J, Maddux J R, Meissner G, Venkatasubramanian R, Bulman G, Pierce J, Gupta R, Bierschenk J, Caylor C, D’Angelo J 2013 Appl. Phys. Lett. 103 043902 Google Scholar
[24]	Weitzman L H 1967 US Patent 3 338 765
[25]	Kozlov A O, Korchagin E P, Mustafoev B R, Babich A V, Rogachev M S 2021 IEEE Conference of Russian Young Researchers in Electrical and Electronic Engineering (ElConRus) St. Petersburg, Moscow, Russia, January 26–29, 2021, p2451
[26]	Vikhor L M, Anatychuk L I, Gorskyi P V 2019 J. Appl. Phys. 126 164503 Google Scholar
[27]	Schottky W 1938 Naturwissenschaften 26 843 Google Scholar
[28]	Monroy E, Calle F, Ranchal R, Palacios T, Moerman I 2002 Semicond. Sci. Technol. 17 L47 Google Scholar
[29]	Kim H S, Lee K H, Yoo J, Shin W H, Roh J W, Hwang J Y, Kim S W, Kim S I 2018 J. Alloys Compd. 741 869 Google Scholar
[30]	Liu W, Jie Q, Kim H S, Ren Z 2015 Acta Mater. 87 357 Google Scholar
[31]	Tang H, Bai H, Yang X, Cao Y, Tang K, Zhang Z, Chen S, Yang D, Su X, Yan Y 2022 J. Alloys Compd. 896 163090 Google Scholar
[32]	Liu W, Wang H, Wang L, Wang X, Joshi G, Chen G, Ren Z 2013 J. Mater. Chem. A 1 13093 Google Scholar

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Interface performance of Bi₂Te₃-based micro thermoelectric devices optimized synergistically by surface modification engineering

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Corresponding author: Tang Xin-Feng, tangxf@whut.edu.cn

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Interface performance of Bi2Te3-based micro thermoelectric devices optimized synergistically by surface modification engineering

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Corresponding author: Tang Xin-Feng, tangxf@whut.edu.cn

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Interface performance of Bi₂Te₃-based micro thermoelectric devices optimized synergistically by surface modification engineering