热电发电器件与应用技术: 现状、挑战与展望

doi:10.15541/jim20180465

摘要/Abstract

摘要：

热电发电技术在特种电源、绿色能源、环境能量收集与工业余热发电等领域具有重要的应用价值。近年来, 热电材料zT值的纪录不断被刷新, 为热电器件应用技术的发展奠定了坚实的基础。然而, 目前热电应用技术远滞后于热电材料科学的发展, 特别是热电发电技术的大规模应用仍面临着技术瓶颈和挑战。本文介绍了热电器件设计与集成的基本原理及其关键科学与技术问题, 着重总结了器件集成中的界面结构设计与优化、电极连接与器件一体化制备技术、器件服役性能与寿命评价等方面的最新研究进展。同时, 分析和展望了热电发电技术规模化应用面临的挑战与发展策略。

关键词: 热电发电器件, 设计与集成, 界面优化, 服役性能, 失效机制, 综述

Abstract:

Thermoelectric (TE) power generation technology is highly expected for various applications such as special power supply, green energy, energy harvesting from the environment and harvesting of industrial waste heat. Over the past years, the record of zT values of TE materials has been continuously updated, which would bode well for widespread practical applications of TE technology. However, the TE device as the core technology for the TE application lags behind the development of TE materials. Especially, the large-scale application of TE power generation technology is facing bottlenecks and new challenges. This reviewpresents an overview of the recent progress on TE device design and integration with particular attentions on device optimization design, electrode fabrication, interface engineering, and service behavior. The future challenges and development strategies for large-scale application ofthermoelectric power generation are also discussed.

Key words: thermoelectric power generation devices, design and integration, interface engineering, service behavior, failure mechanism, review

中图分类号:

TQ174

张骐昊, 柏胜强, 陈立东. 热电发电器件与应用技术: 现状、挑战与展望[J]. 无机材料学报, 2019, 34(3): 279-293.

ZHANG Qi-Hao, BAI Sheng-Qiang, CHEN Li-Dong. Technologies and Applications of Thermoelectric Devices: Current Status, Challenges and Prospects[J]. Journal of Inorganic Materials, 2019, 34(3): 279-293.

图/表 12

图1 热电材料与器件发展态势(a)热电材料zT值[6,7], (b)热电发电器件转换效率[10,11,12,13,14,15,16,17,18,19,20,21,22,23,24,25,26,27,28,29,30,31,32,33,34,35,36,37,38,39,40]

Fig. 1 Timelines underscoring the improvement in (a) zT value of typical thermoelectric materials[6,7] and (b) conversion efficiency of typical thermoelectric power generation devices[10,11,12,13,14,15,16,17,18,19,20,21,22,23,24,25,26,27,28,29,30,31,32,33,34,35,36,37,38,39,40]

图2 热电转换技术的研发链示意图

Fig. 2 Schematic diagram of the full-chain development of thermoelectric conversion technology

图3 热电器件设计与集成中的关键科学与技术问题

Fig. 3 Diagram of key scientific and technical issues in the design and integration of TE devices

图4 热电发电器件能量转换过程示意图[45]

Fig. 4 Schematic diagram of energy conversion process for thermoelectric power generation devices[45]

图5 (a)具有不同接触热阻的热电单偶转换效率随热电偶臂高度H的变化关系和(b)具有不同热电偶臂高度的热电单偶相对输出功率随接触电阻参数n的变化关系[46]

Fig. 5 (a) Conversion efficiency as a function of thermoelectricelement height for different thermal contact parameter,r,and (b) power output ratio Pc/Pmax as a function of the electrical contact parameter,n, for different thermoelectric element height[46]

图6 热电器件内部各种热损失示意图

Fig. 6 Schematic diagram of various thermal losses in thermoelectric devices

图7 热电效应的等效示意图(热容 $C_{n}=\rho ·n·C_{p_{n}}·\frac{H}{N}·A$ , 热导${{K}_{n}}=\frac{{{k}_{n}}\cdot A}{H\text{/}N}$) [55]

Fig. 7 Analogical scheme of the thermoelectric phenomena with the thermal capacitances $C_{n}=\rho ·n·C_{p_{n}}·\frac{H}{N}·A$ and thermal conductances $K_{n}=\frac{k_{n}·A}{H/N}$ [55]

图8 热电器件全参数优化设计逻辑框架[40]

Fig. 8 Logical framework for the full-parameter optimization of a thermoelectric power generation module[40]

表1 典型热电发电元件的电极材料、过渡层材料及其连接方式

Table 1 Electrode, interface layer and joining method of typical thermoelectric devices

Thermoelectric material	(T_h/T_c)/℃	Electrode	Interface layer	Joining method	Ref.
Bismuth telluride	240/22	Cu	Ni	Soldering	[59-60]
Bismuth telluride	-	-	Ni	One-step hot press sintering	[61]
Bismuth telluride	200/-	Cu	Ni	Solid-liquid diffusion welding	[62]
Bismuth telluride	250/50	Al	Mo	Plasma spraying	[63]
Bismuth telluride	240/20	Cu	Mo	Arc spraying	[64]
MgAg_0.965Ni_0.005Sb_0.99	245/20	Ag	-	Diffusion welding	[65]
Poly[A_x(M-ett)]	147/67	Hot side: Al	Au		[66]
Poly[A_x(M-ett)]	147/67	Cold side: Ag	Au		[66]
n-type PbTe + p-type TAGS 85	500/100	Ag	Ag/Fe/Ag + Fe	Diffusion welding	[25]
Skutterudite	500/40	Al	Mo	Brazing	[67]
Skutterudite	550/70		n-type: CoSi₂		[31]
Skutterudite	550/70		p-type: Co₂Si		[31]
Skutterudite	600/35	Hot side: Mo-Cu Cold side: Cu	Ti-Al	Brazing	[17]
n-type Bi₂Te₃/PbTe + p-type Sb₂Te₃/PbTe	600/10	Cu	Hot side: Co_0.8Fe_0.2	Liquid InGa eutectic alloy	[35]
n-type Bi₂Te₃/PbTe + p-type Sb₂Te₃/PbTe	600/10	Cu	Cold side: Ni	Liquid InGa eutectic alloy	[35]
Bismuth telluride/ Skutterudite	600/35	Hot side: Mo-Cu	Hot side: Ti-Al	Welding	[40]
Bismuth telluride/ Skutterudite	600/35	Cold side: Cu	Cold side: Ni	Welding	[40]
Half-Heusler	718/63	Hot side: Mo-Cu		Brazing	[18]
Half-Heusler	718/63	Cold side: Cu		Brazing	[18]
n-type Fe_0.93Co_0.07Si_1.99Al_0.01 + p-type MnSi_1.73	700/100	TiSi₂		Welding	[19]
SiGealloy	870/31	Mo	Pressure contact	Cold side In welding	[68]
SiGe alloy	553/44	Mo	C	Brazing	[69]
SiGe alloy	1000/300	With Ti layer		Diffusion welding	[70]
n-type Ca_0.92La_0.08MnO₃ + p-type Ca_2.75Gd_0.25Co₄O₉	773 /383	Silver electrode		Silver paste	[71]
p-type Mg₂Si_0.53Sn_0.4Ge_0.05Bi_0.02+ n-type MnSi_1.75Ge_0.01	735/50	Hot side: Mo	p-type: Ni/Pb/Ni	Spring contact	[37]
	735/50	Cold side: Cu	n-type: Cu	Spring contact	[37]

图9 热电发电器件主要失效模式框架图

Fig. 9 Diagram of main failure modes of thermoelectric devices

图10 在550 ℃不同老化时间下的CoSb3/Ti/Mo-Cu界面扫描电镜照片[115]

Fig. 10 Scanning electron microscope images of CoSb3/Ti/Mo-Cu interface after thermal aging at 550 ℃ for different periods[115](a) 0; (b) 8 d; (c) 20 d; (d) 30 d

图11 (a)Ti(100-x)Alx-Yb0.6Co4Sb12界面结构形成示意图; (b)600 ℃、真空条件下Ti(100-x)Alx-Yb0.6Co4Sb12元件界面扩散层厚度随热持久时间的演化; (c)600 ℃、真空条件下Ti(100-x)Alx-Yb0.6Co4Sb12元件接触电阻率随热持久时间的演化[79]

Fig. 11 (a) Schematic diagram of the formation of Ti(100-x)Alx-Yb0.6Co4Sb12 interface, (b) the diffusion layer thickness and (c) specificcontact resistivity of the Ti(100-x)Alx-Yb0.6Co4Sb12 interface as a function of the thermal aging time under 600 ℃ and vacuum condition[79]

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