<i>MAX</i>及其衍生<i>MX</i>ene相碳化物的热电性能及展望

刘超; 杨岳洋; 南策文; 林元华

doi:10.7498/aps.70.20211050

摘要

热电材料无需提供其他能量就能直接实现热能和电能的相互转换, 是一种新型能源材料, 然而当前热电材料的发展现状严重制约了热电器件的工程化应用, 提高现有热电材料的热电性能或研发具有优异性能的新型热电材料是热电领域永恒的研究主题. 近年来, MAX及其衍生MXene相材料由于特有的结构性能而逐渐进入了科研工作者的视线, MAX 相的晶体结构由M_n+1X_n 结构单元与A 元素单原子面交替堆垛排列而成, MAX中A层原子被刻蚀之后可以制备得到对应的衍生二维MXene相, MAX及其衍生MXene相陶瓷兼具金属和陶瓷的特性, 具有良好的导热导电性能, 有望成为一种非常有前景的热电材料. 本文简要综述了近年来MAX相及其衍生MXene相材料的制备技术和热电性能的发展现状, 并针对MAX及其衍生MXene相材料的特性提出了一些改善热电性能的可行性方案, 据此展望了MAX相以及MXene材料在未来的发展方向和前景.

关键词:

热电材料 /
MAX /
MXene /
综述

Abstract

Thermoelectric materials, a kind of new energy material, can directly convert heat energy into electric energy, and vice versa, without needing any other energy conversion. However, the present development status of thermoelectric materials severely restricts their engineering applications in thermoelectric devices. Improving the thermoelectric performances of existing thermoelectric materials and exploring new thermoelectric materials with excellent performance are eternal research topics in thermoelectricity field. In recent years, the MAX phases and their derived MXene phases have gradually received the attention of researchers due to their unique microstructures and properties. The crystal structure of MAX phases is comprised of M_n+1X_n structural units and the single atomic plane of A stacked alternately. The two-dimensional MXene phase derived can be prepared after the atoms in the A-layer of MAX have been etched. The MAX phases and their derived MXene phases have both metal feature and ceramic feature, and also have good thermal conductivity and electric conductivity, and they are anticipated to be the promising thermoelectric materials. In this paper, the present development status of the preparation technology and the thermoelectric properties of MAX phases and MXene are reviewed. Finally, some feasible schemes to improve the thermoelectric properties of MAX and its derived MXene phase materials are proposed, and the development direction and prospect of MAX phases and MXene are prospected as well.

Keywords:

作者及机构信息

1.
清华大学, 新型陶瓷与精细工艺国家重点实验室, 北京　100084

2.
中南大学, 轻质高强结构材料国家级重点实验室, 长沙　410083

通信作者: 林元华, linyh@tsinghua.edu.cn

基金项目: 国家自然科学基金(批准号: 51729201, 51788104, 51672155) 和国家重点研发计划(批准号: 2016YFA0201003)资助的课题

Authors and contacts

1.
State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing 100084, China

2.
National Key Laboratory of Science and Technology for National on High-strength Structural Materials, Central South University, Changsha 410083, China

Corresponding author: Lin Yuan-Hua, linyh@tsinghua.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 51729201, 51788104, 51672155) and the State Key R&D Program of China (Grant No. 2016YFA0201003).

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施引文献

图 1 热电材料的塞贝克效应和珀尔帖效应示意图^[6]

Fig. 1. Schematic diagram of Seebeck effect and Peltier effect in thermoelectric materials^[6].

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图 2 M_n+1AX_n相的晶体结构^[11]

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图 3 Cr₂AlC的组织和性能　(a)晶体结构; (b)热导率; (c)测量电阻率; (d)预测面外电阻率^[21]

Fig. 3. Microtructure and properties of Cr₂AlC: (a) Atomic structure; (b) thermal conductivity, compared to the values found in the literature; (c) measurements resistivity; (d) predicted out-of-plane resistivity. Plane reprinted with permission from Ref. [21]. Copyright © 2020 American Chemical Society.

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图 4 Ti₂AlC的组织和性能　(a)蚀刻表面; (b)电导率和电阻率; (c)热导率、热容和热扩散率; (d)总热导率、电子热导率和声子热导率^[33]

Fig. 4. Microtructure and properties of Cr₂AlC: (a) Etched surface; (b) electrical conductivity and resistivity; (c) thermal conductivity, heat capacity, and thermal diffusivity; (d) total, electronic and phonon thermal conductivity. Plane reprinted with permission from Ref. [33]. Copyright © 2011 John Wiley and Sons.

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图 5 Ti₃AlC₂的热电性能　(a)电阻率; (b)热导率^[34]

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图 6 MXene的制备方法　(a) HF刻蚀法^[12]; (b) LiF+HCl刻蚀法^[49]; (c) Li扩张法^[52]; (d)电化学刻蚀法^[57]; (e)路易斯酸刻蚀法^[62]; (f)碘刻蚀法^[65]

Fig. 6. Preparation methods of MXene: (a) Etching method via HF^[12]; (b) etching method via LiF+HCl^[49]; (c) lithiation expansion^[52]; (d) electrochemical etching^[57]; (e) Lewis acid etching^[62]; (f) iodine‐assisted etching^[65]. Panel (a) reprinted from Ref. [12], Copyright 2011 John Wiley and Sons. Panel (b) reprinted from Ref. [49] with the permission of John Wiley and Sons. Panel (c) reprinted with permission from Ref. [52]. Copyright © 2019 American Chemical Society. Panel (e) reprinted with permission from Ref. [62], Copyright © 2019 American Chemical Society. Panel (f) reprinted from Ref. [65] with the permission of John Wiley and Sons

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图 7 MXene的界面工程及热电性能　(a)−(c) Ti₃C₂T_x/SWCNTs (M/S), Ti₃C₂T_x-SWCNTs-Ti₃C₂T_x (MSM)和 SWCNTs-Ti₃C₂T_x-SWCNTs (SMS) 多层膜及能量过滤效应示意图^[69]; (d)−(f) 3种结构下对应的功率因子随SWCNTs百分比的变化图^[69]; (g) MXene和PEDOT复合后形成内建电场示意图; MXene/PEDOT:PSS中不同MXene质量分数下的(h)塞贝克系数和电导率以及(i)功率因子^[70]

Fig. 7. Interface engineering and thermoelectric properties of MXene. The schematic energy diagrams of (a) Ti₃C₂T_x/SWCNTs (M/S), (b) Ti₃C₂T_x-SWCNTs-Ti₃C₂T_x (MSM), and (c) SWCNTs-Ti₃C₂T_x-SWCNTs (SMS) showing the different energy-filtering effects^[69]-. Power factor of (d) Ti₃C₂T_x/SWCNTs (M/S), (e) Ti₃C₂T_x-SWCNTs-Ti₃C₂T_x (MSM), and (f) SWCNTs-Ti₃C₂T_x-SWCNTs (SMS) films^[69]. (g) Schematic diagrams for the interfacial effect between MXene and PEDOT^[70]. (h) Seebeck coefficient and electrical conductivity and (i) power factor of MXene/PEDOT: PSS as a function of the MXene loading^[70]. Panels (a)−(f) are reprinted from Ref. [69] with the permission of John Wiley and Sons. Panels (g)−(i) are adapted with permission from Ref. [70], Copyright © 2020 American Chemical Society.

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图 8 含有0.81% O空位的Ti₂CO₂在(a)单轴和(b)双轴应变下的电子能带结构; (c) Ti₂CO₂带隙随应力的变化^[72]

Fig. 8. Electronic band structure of the O-vacacy Ti₂CO₂ structure (for 0.81% defect concentration) as a function of (a) uniaxial and (b) biaxial strain. (c) Variation of band gap with respect to strain. Reprinted from Ref. [72], Copyright © 2020 John Wiley and Sons

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图 9 MXene的缺陷工程　(a) Mo_1.33C^[75]; (b) W_1.33C^[76]

Fig. 9. Defect engineering of MXene: (a) Mo_1.33C; (b) W_1.33C. Panel (a) is reprinted with permission from Ref. [75], Springer Nature. Panel (b) is adapted from Ref. [76], Copyright © 2016 John Wiley and Sons.

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图 10 MXene的合金化工程及热电性能 Mo基MXene的 (a)电导率、(b)塞贝克系数和(c)功率因子随温度变化图^[78]; (d) Cr基MXene的理论晶格和电子热导率^[67]; (e) Cr基MXene的理论ZT值^[67]; (f) TiMo基MXene的理论晶格和电子热导率^[66]; (g) TiMo基MXene的理论ZT值^[66]

Fig. 10. Alloying engineering and thermoelectric properties of MXene. Temperature dependent thermoelectric properties of Mo-based MXene papers during the first thermal cycle: (a) Electrical conductivity; (b) Seebeck coefficient; (c) thermoelectric power factor^[78]. (d) Lattice and electron thermal conductivities of Cr-based MXene^[67]. (e) Thermoelectric figure of merit (ZT) of Cr-based MXene ^[67]. (f) Temperature-dependent electronic and lattice thermal conductivities of TiMo-based MXene ^[66]. (g) Thermoelectric figure of merit (ZT) effificiency for passivated TiMo-based MXene ^[66]. Panels (a) (c) are reprinted with permission from Ref. [78], Copyright © 2017 American Chemical Society. Panels (d), (e) are reprinted with permission from Ref. [67], Copyright © 2019 American Chemical Society. Panels (f), (g) are reprinted from Ref. [66] with permission from American Physical Society.

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图 11 MXene体系热电性能研究现状, 图中表示的是M位元素组成, 紫色代表理论具有一定的热电性能, 蓝色代表实验上成功制备的MXene相, 红色代表实际已经测得热电性能, 下划线代表具有潜在热电性能的体系

Fig. 11. Status of thermoelectric research of MXene system. Purple elements represent the constituent MXene have certain thermoelectric properties theoretically. Blue elements represent the constituent MXene synthesized experimentally. Red represents the thermoelectric properties of theses MXene being reported. The lanthanides on the underscore represent a class of MXene that may have thermoelectric properties.

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表 1 常见单相MAX的热电性能^{[14,34,36,37]}

Table 1. Thermoelectric properties of single-phase MAX^{[14,34,36,37]}.

物相种类		测试温度 /K	热膨胀系数 /(10^-6 K^-1)	热导率 /(W·m^–1·K^–1)	电导率 /(10⁶ S·m^–1)	塞贝克系数/(μV·K^–1)
211相	Cr₂AlC	473	12.50	17.5	1.8	—
	Ti₂AlC	300	(8.10 ± 0.50)	46.0	2.8	—
	Nb₂AlC	300	8.10	20.0		—
	Ti₂SnC	300	10.00 ± 2.00	—	14.0	—
	Ti₂SC	300	8.40	60..0	1.8	–12.7
312相	Ti₃AlC₂	85	9.00 ± 0.20	26.5		0.22
312相	Ti₃SiC₂	300	9.20	46.0		—
413相	Nb₄AlC₃	300	5.75	13.5		—

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表 2 MXene的带隙以及载流子迁移率^[80-99]

Table 2. Bandgap and carrier mobility of MXene^[80-99].

MXene	带隙/eV	迁移率/(cm²·V^–1·s^–1)	计算方法/实验值	参考文献
Sc₂CF₂	1.0	1000—5000 (e) 200—500 (h)	PBE	[80-83]
Sc₂CF₂	1.85		HSE06	[82]
Sc₂(OH)₂	0.45	2000 (e) 50—240 (h)	PBE	[80-83]
Sc₂(OH)₂	0.845		HSE06	[82]
Sc₂CO₂	1.8		PBE	[80, 82]
Sc₂CO₂	2.87		HSE06	[82]
Sc₃(CN)F₂	1.18	200—1300 (e) 80—1000 (h)	HSE06	[84]
Ti₂CO₂	0.17—0.26	250—610 (e) 20000—74000 (h)	PBE	[80-82, 85]
	0.9	70—150 (e) 10000—40000 (h)	HSE06	[82, 86, 87]
	1.03	2—900 (e) 4000—8000 (h)	HSE06	[88]
Ti₃C₂T_x(T = O, OH, F)		0.7±0.2 (e)	Experimental	[89]
		1.06 (e)	Experimental	[90]
	0.66		Experimental	[91]
Zr₂CO₂	0.88—0.97		PBE	[80, 82]
	0.66		PBE	[81]
	1.70	150 (e) 1400—17500 (h)	HSE06	[82, 87]
	1.58	14—376 (e) 770—1950 (h)	HSE06	[88]
	1.34		mBJ	[92]
Hf₂CO₂	0.8—1.0		PBE	[80-82]
	1.66	77—330 (e) 1000—34000 (h)	HSE06	[82, 87]
	1.78	24—700 (e) 620—1300 (h)	HSE06	[88]
(Zr_0.5Hf_0.5)₂CO₂	1.74	45—1460 (e) 1500—6200 (h)	PBE	[93]
Mo₂CF₂	0.25—0.30		PBE	[81, 82]
Mo₂CF₂	0.86		HSE06	[82]
Mo₂CCl₂	0.05		PBE	[81]
Mo₂C(OH)₂	0.1		PBE	[81]
W₂CO₂	0.0683		HSE06	[82]
Mo₂TiC₂O₂	0.04		PBE	[94, 95]
Mo₂TiC₂O₂	0.10—0.17		HSE06	[94-96]
Mo₂TiC₂(OH)₂	0.05		PBE	[97]
Cr₂CF(OH)	0.383		PBE	[98]
Cr₂CF₂	1.105		PBE	[98]
Cr₂C(OH)₂	0.396		PBE GGA	[98]
Mo₂ZrC₂O₂	0.066		PBE	[95]
Mo₂ZrC₂O₂	0.11—0.13		HSE06	[95, 96]
Mo₂HfC₂O₂	0.154		PBE	[95]
Mo₂HfC₂O₂	0.20—0.24		HSE06	[95, 96]
W₂TiC₂O₂	0.29		HSE06	[96]
W₂ZrC₂O₂	0.28		HSE06	[96]
W₂HfC₂O₂	0.41		HSE06	[96]
Lu₂CF₂	2.07	200—1000 (e) 14—6000 (h)	HSE06	[99]
Lu₂C(OH)₂	1.28	100000—200000 (e) 12—14000 (h)	HSE06	[99]

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MAX及其衍生MXene相碳化物的热电性能及展望