Te基热电器件反常界面层生长行为及界面稳定性研究

doi:10.15541/jim20240057

无机材料学报 ›› 2024, Vol. 39 ›› Issue (8): 903-910.DOI: 10.15541/jim20240057

Te基热电器件反常界面层生长行为及界面稳定性研究

苗鑫¹(), 闫世强¹, 韦金豆¹, 吴超¹, 樊文浩², 陈少平¹()

1.太原理工大学材料科学与工程学院, 太原 030024
2.太原理工大学物理学院, 太原 030024

收稿日期:2024-01-30 修回日期:2024-02-20 出版日期:2024-08-20 网络出版日期:2024-04-19
通讯作者: 陈少平, 教授. E-mail: chenshaoping@tyut.edu.cn
作者简介:苗鑫(1999-), 男, 硕士研究生. E-mail: miaoxin0242@link.tyut.edu.cn
基金资助:
国家自然科学基金(52202277);山西省科技合作与交流专项项目(202104041101007);山西省省筹资金资助回国留学人员科研项目(2023-083)

Interface Layer of Te-based Thermoelectric Device: Abnormal Growth and Interface Stability

MIAO Xin¹(), YAN Shiqiang¹, WEI Jindou¹, WU Chao¹, FAN Wenhao², CHEN Shaoping¹()

1. College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, China
2. College of Physics, Taiyuan University of Technology, Taiyuan 030024, China

Received:2024-01-30 Revised:2024-02-20 Published:2024-08-20 Online:2024-04-19
Contact: CHEN Shaoping, professor. E-mail: chenshaoping@tyut.edu.cn
About author:MIAO Xin (1999-), male, Master candidate. E-mail: miaoxin0242@link.tyut.edu.cn
Supported by:
National Natural Science Foundation of China(52202277);Special Project of Science and Technology Cooperation and Exchange of Shanxi Province(202104041101007);Shanxi Scholarship Council of China(2023-083)

摘要/Abstract

摘要：

单质Te具有优异的热电优值(ZT), 但其与金属电极连接界面处的剧烈元素交互扩散及反应会引入较大的接触电阻率(ρ_c), 导致器件的转换效率(η)较低。因此, 寻找合适的阻挡层来优化Te与金属电极间的连接至关重要。本研究基于梯度结构报道了一种宽相场Ni-Te合金阻挡层NiTe_2-_m (Ni_xTe(x=0.500~0.908))。结果表明, 当x=0.500时, Ni_0.5Te/Te_0.985Sb_0.015/Ni_0.5Te器件的界面处无任何反应层及微观缺陷, ρ_c小于10 μΩ·cm², η在180 K温差(热端温度473 K)时达到了理论值的75%。同时, 界面具有良好的热稳定性, 在473 K老化期间, 界面微观组织、ρ_c以及η无明显变化。当x>0.500时, 界面反应层厚度随x增大而逐渐减小, 即主导界面反应层生长行为的因素并非常规的界面反应能及浓度梯度等热力学因素。进一步分析表明, 反常生长源于动力学因素中的“原子空位”对反应层生成的迟滞作用。

关键词: Te, 热电器件, 扩散动力学, 阻挡层, 热稳定性

Abstract:

Though Te has excellent figure of merit (ZT), the severe element diffusion and reaction at the Te/metallic-electrodes interface render high contact resistivity (ρ_c) and low device conversion efficiency (η). Therefore, it is critical to develop suitable barrier layers for optimizing the bonding between Te and metallic electrodes. In this work, an appropriate barrier layer, NiTe_2-_m (Ni_xTe (x=0.500~0.908)), was screened based on gradient structure. No reaction layers and defects at the interface of Ni_0.5Te/Te_0.985Sb_0.015/Ni_0.5Te were detected before and after aging at 473 K. Low ρ_c (less than 10 μΩ·cm²) and high η (about 75% of the theoretical value under a temperature difference of 180 K (hot end: 473 K)) were achieved and maintained stable during aging, showing excellent thermal stability of the interface. When x>0.500, the thickness of the interface reaction layer decreased with x increasing, showing the retarding effect dominating the growth behavior of interface reaction layer not from the usual thermodynamic factors, such as interface reaction energy and composition gradient, but from the “atom vacancy” on formation of the reaction layer.

Key words: Te, thermoelectric device, diffusion dynamic, barrier, thermal stability

中图分类号:

TN377

苗鑫, 闫世强, 韦金豆, 吴超, 樊文浩, 陈少平. Te基热电器件反常界面层生长行为及界面稳定性研究[J]. 无机材料学报, 2024, 39(8): 903-910.

MIAO Xin, YAN Shiqiang, WEI Jindou, WU Chao, FAN Wenhao, CHEN Shaoping. Interface Layer of Te-based Thermoelectric Device: Abnormal Growth and Interface Stability[J]. Journal of Inorganic Materials, 2024, 39(8): 903-910.

图/表 17

图1 Te0.985Sb0.015前驱粉末的微观形貌及成分组成

Fig. 1 Microstructure and composition of Te0.985Sb0.015 precursor powder (a) Backscattered SEM image; (b) XRD patterns and quasi-1D chain crystal structure of Te and Te0.985Sb0.015 powders; Colorful figures are available on website

图2 NixTe样品的成分及晶格参数

Fig. 2 Composition and lattice parameters of NixTe samples (a) XRD patterns; (b) Lattice constant a changed with x

图3 (a) Te0.985Sb0.015/NixTe各界面反应层(Interface Reaction Layers, IRLs)的厚度, (b)各界面产物的摩尔生成吉布斯自由能ΔrGT

Fig. 3 (a) Thicknesses of the interface reaction layers (IRLs) at the Te0.985Sb0.015/NixTe interfaces, and (b) formation Gibbs free energies in molar (ΔrGT) of the interface products at the Te0.985Sb0.015/NixTe interfaces

图4 Te/NiTe2-m界面反应层(Interface Reaction Layer, IRL)生长行为模型图

Fig. 4 Diagram of the growth of the interface reaction layer (IRL) at Te/NiTe2-m interface

表1 Te0.985Sb0.015/NixTe界面处原子的总迁移量CN·l

Table 1 Total migration of atoms (CN·l) at Te0.985Sb0.015/NixTe interface

Total migration of atoms	x=0.500	x=0.563	x=0.667	x=0.833	x=0.908	Te_0.985Sb_0.015/Ni
C_N·l/(mol·cm^-2)	0	0.1297	0.2134	0.2810	0.3154	0.5653

图5 473 K老化6及12 d后的Te0.985Sb0.015/NixTe界面微观结构

Fig. 5 Microstructures of Te0.985Sb0.015/NixTe interfaces after aging at 473 K for 6 and 12 d Backscattering SEM images for (a) x=0.500, (b) x=0.563, and (c) x=0.667

图6 NixTe/Te0.985Sb0.015/NixTe (x=0.500, 0.563, 0.667)单臂器件的性能

Fig. 6 Performance of NixTe/Te0.985Sb0.015/NixTe (x=0.500, 0.563, 0.667) single-leg devices (a, b) Room temperature V-I curves and contact resistivity, ρc, before aging; (c) Time-dependent room temperature ρc; (d) Time-dependent efficiency, η, under a temperature difference of 180 K (hot end: 473 K, cold end: 293 K)

图S1 烧结态Te0.985Sb0.015的断口形貌及元素分布

Fig. S1 Fracture microstructure and element distribution of sintered Te0.985Sb0.015 (a, b) Backscattered SEM images; (c) Corresponding EDS mapping

图S2 平行于烧结压力方向上的Te0.985Sb0.015的热电性能

Fig. S2 Thermoelectric performance of Te0.985Sb0.015 in the direction parallel to the sintering pressure (a) Total thermal conductivity, κ; (b) Carrier concentration, n; (c) Resistivity; (d) Seebeck coefficient; (e) Power factor, PF; (f) Dimensionless ZT of Te0.985Sb0.015; The test results of Pei et al.[15] are also drawn in the figures for comparison

图S3 NixTe样品的电性能

Fig. S3 Electrical performance of NixTe samples (a) Resistivity; (b) Seebeck coefficient

图S4 烧结态Te0.985Sb0.015/NixTe界面的微观形貌以及元素分布

Fig. S4 Microstructures and element distributions of sintered Te0.985Sb0.015/NixTe interfaces Backscatter SEM images and EDS spectra for (a) x=0.500, (b) x=0.563, (c) x=0.667, (d) x=0.833, and (e) x=0.908

图S5 烧结态Te0.985Sb0.015/Ni界面的背散射SEM照片

Fig. S5 Backscatter SEM image of sintered Te0.985Sb0.015/Ni interface

表S1 热力学数据

Table S1 Thermodynamic data. Values of entropy (ST), enthalpy (HT), and Gibbs free energy (GT) at 298.15, 600.00 and 700.00 K, respectively

Phase lable	Formula in reference	Formula used here	Temperature/K	S_T/(J·mol^-1·K^-1)	H_T/(kJ·mol^-1)	G_T/(kJ·mol^-1)	Ref.
δ(-NiTe_2-_x, 52.2%-66.7% (in atom) Te)	Ni_0.476Te_0.524	Ni_0.908Te	298.15	76.393	-51.908	-74.685	[40]
			600.00	112.729	-36.120	-103.758
			700.00	121.397	-30.494	-115.472
	Ni_0.4Te_0.6	Ni_0.667Te	298.15	66.917	-47.833	-67.785	[40]
			600.00	98.732	-33.987	-93.226
			700.00	106.415	-29.000	-103.491
	Ni_0.333Te_0.667	Ni_0.5Te	298.15	60.135	-43.778	-61.707	[40]
			600.00	88.253	-31.552	-84.504
			700.00	95.001	-27.172	-93.673
Te	Te	Te	298.15	49.497	0.000	-14.757	[41]
			600.00	69.537	8.766	-32.956
			700.00	74.694	12.114	-40.171
Ni	Ni	Ni	298.15	29.874	0.000	-8.907	[41]
			600.00	50.419	9.008	-21.243
			700.00	55.546	12.326	-26.557

表S2 298.15, 600.00和700.00 K条件下各界面反应产物的摩尔生成吉布斯自由能∆rGT

Table S2 Molar formation Gibbs free energies (ΔrGT) of interface products at 298.15, 600.00 and 700.00 K, respectively

Chemical reaction equation	Temperature/K	Δ_rS_T/(J·mol^-1·K^-1)	Δ_rH_T/(kJ·mol^-1)	Δ_rG_T/(kJ·mol^-1)
0.25Te+0.75Ni_0.667Te→Ni_0.5Te	298.15	-2.427	-7.903	-7.180
	600.00	-3.180	-8.253	-6.345
	700.00	-3.484	-8.451	-6.012
0.449Te+0.551Ni_0.908Te→Ni_0.5Te	298.15	-4.182	-15.177	-13.930
	600.00	-5.083	-15.586	-12.536
	700.00	-5.426	-15.809	-12.010
1.5Ni+Te→Ni_1.5Te	298.15	5.692	-57.500	-59.197
	600.00	5.969	-57.318	-60.899
	700.00	8.110	-56.023	-61.700

表S3 各层材料的密度ρ、摩尔质量M以及每摩尔物质中结合态Te的物质的量n

Table S3 Density (ρ), molar mass (M) and moles of the bound Te per mole substance

Item	NiTe₂ (Ni_0.5Te)	NiTe_1.776 (Ni_0.563Te)	NiTe_1.5 (Ni_0.667Te)	NiTe_1.2 (Ni_0.833Te)	NiTe_1.1 (Ni_0.908Te)	Ni	Te	NiTe_0.667 (Ni_1.5Te)
M/(g·mol^-1)	313.893	285.311	250.093	211.813	199.053	58.693	127.600	143.802
n	2.000	1.776	1.500	1.200	1.100	0.000	-	0.667
ρ/(g·cm^-3)	7.701	7.565	7.363	7.086	6.976	8.910	-	8.126

图S6 老化前在180 K温差(热端473 K, 冷端293 K)条件下Ni0.5Te/Te0.985Sb0.015/Ni0.5Te单臂器件的性能

Fig. S6 Performance of Ni0.5Te/Te0.985Sb0.015/Ni0.5Te single-leg devices under a temperature difference of 180 K (Hot end: 473 K, Cold end: 293 K) (a) Current-dependent output voltage, Uout; (b) Current-dependent heat flux, Q

图S7 180 K温差 (热端473 K, 冷端293 K)条件下Ni0.5Te/Te0.985Sb0.015/Ni0.5Te单臂器件的性能随老化时间的变化

Fig. S7 Aging-time dependent performance of Ni0.5Te/Te0.985Sb0.015/Ni0.5Te single-leg devices under a temperature difference of 180 K (Hot end: 473 K, Cold end: 293 K) (a, c) Current-dependent output voltages, Uout and (b, d) current-dependent heat flux, Q, after aging for (a, b) 3 and (c, d) 6-15 d; Aging-time dependent (e) open-circuit voltage, Uo and (f) internal resistance, Rin with inset in (f) showing internal resistivity, R, of the devices

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Te基热电器件反常界面层生长行为及界面稳定性研究

Interface Layer of Te-based Thermoelectric Device: Abnormal Growth and Interface Stability

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