WO2020255898A1 - Matériau thermoélectrique - Google Patents

Matériau thermoélectrique Download PDF

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Publication number
WO2020255898A1
WO2020255898A1 PCT/JP2020/023300 JP2020023300W WO2020255898A1 WO 2020255898 A1 WO2020255898 A1 WO 2020255898A1 JP 2020023300 W JP2020023300 W JP 2020023300W WO 2020255898 A1 WO2020255898 A1 WO 2020255898A1
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Prior art keywords
thermoelectric
thermoelectric material
carbon
material according
nanoparticles
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PCT/JP2020/023300
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English (en)
Japanese (ja)
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崇人 小野
ファズリ ビン サマト カイル
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国立大学法人東北大学
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Priority to JP2021528195A priority Critical patent/JPWO2020255898A1/ja
Publication of WO2020255898A1 publication Critical patent/WO2020255898A1/fr

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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/80—Constructional details
    • H10N10/85—Thermoelectric active materials
    • H10N10/851—Thermoelectric active materials comprising inorganic compositions
    • H10N10/855—Thermoelectric active materials comprising inorganic compositions comprising compounds containing boron, carbon, oxygen or nitrogen
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L29/00—Semiconductor devices specially adapted for rectifying, amplifying, oscillating or switching and having potential barriers; Capacitors or resistors having potential barriers, e.g. a PN-junction depletion layer or carrier concentration layer; Details of semiconductor bodies or of electrodes thereof ; Multistep manufacturing processes therefor
    • H01L29/02—Semiconductor bodies ; Multistep manufacturing processes therefor
    • H01L29/06—Semiconductor bodies ; Multistep manufacturing processes therefor characterised by their shape; characterised by the shapes, relative sizes, or dispositions of the semiconductor regions ; characterised by the concentration or distribution of impurities within semiconductor regions
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/80—Constructional details
    • H10N10/85—Thermoelectric active materials
    • H10N10/851—Thermoelectric active materials comprising inorganic compositions
    • H10N10/852—Thermoelectric active materials comprising inorganic compositions comprising tellurium, selenium or sulfur
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
    • H10N10/80—Constructional details
    • H10N10/85—Thermoelectric active materials
    • H10N10/857—Thermoelectric active materials comprising compositions changing continuously or discontinuously inside the material

Definitions

  • the present invention relates to thermoelectric materials.
  • Bi 2 Te 3 is known as a thermoelectric conversion material that can be plated on the surface of an object to be treated and has excellent thermoelectric characteristics in a low temperature region of about room temperature.
  • the electrodeposited Bi 2 Te 3 has a dimensionless figure of merit ZT (where Z is a figure of merit and T is an absolute temperature) of about 0.1 to 0.16, which is smaller than that of a bulk-like one. The value is shown (see, for example, Non-Patent Document 1 or 2). Therefore, in order to enhance the thermoelectric characteristics, a composite material in which Pt nanoparticles or carbon nanotubes (CNTs) are dispersed in Bi 2 Te 3 has been developed.
  • ZT dimensionless figure of merit
  • T is an absolute temperature
  • thermoelectric material composed of a composite material of Bi 2 Te 3 and Pt nanoparticles
  • it is formed by electrodeposition coating by an electrochemical reaction, and power factor S 2 ⁇ (where S is Seebeck).
  • S power factor
  • a coefficient (the coefficient, ⁇ is an electrical conductivity) of 1800 ⁇ W / m ⁇ K 2 and a dimensionless performance index ZT of 0.61 have been developed by the present inventor (see, for example, Non-Patent Document 3).
  • thermoelectric material composed of a composite material of Bi 2 Te 3 and multi-walled carbon nanotubes (MWCNT)
  • MWCNT multi-walled carbon nanotubes
  • thermoelectric material described in Non-Patent Document 3 has excellent thermoelectric characteristics because the values of the output factor S 2 ⁇ and the dimensionless performance index ZT are increased by dispersing Pt nanoparticles in the thermoelectric conversion material. However, considering applications such as power generation, cooling, and exhaust heat recovery, the development of thermoelectric materials having better thermoelectric characteristics is desired. Further, the thermoelectric material described in Non-Patent Document 4 can reduce the electric resistance by dispersing the multilayer carbon nanotubes in the thermoelectric conversion material, but is compared with the thermoelectric material described in Non-Patent Document 3, Seebeck. Since it is considered that the absolute value of the coefficient S is small and the thermal conductivity ⁇ is large, the values of the output factor S 2 ⁇ and the dimensionless performance index ZT are small, and there is a problem that the thermoelectric characteristics are inferior.
  • the present invention has been made focusing on such a problem, and an object of the present invention is to provide a thermoelectric material capable of obtaining more excellent thermoelectric characteristics.
  • thermoelectric material according to the present invention is characterized by being composed of a thermoelectric conversion material, a carbon nanomaterial having one or more pores, and a composite material containing metal nanoparticles.
  • thermoelectric material according to the present invention is composed of a thermoelectric conversion material, a carbon nanomaterial having one or more pores, and a composite material containing metal nanoparticles, conventionally, only Pt nanoparticles are dispersed in the thermoelectric conversion material.
  • the values of the output factor S 2 ⁇ and the dimensionless performance index ZT are larger than those of the conventional one in which only the multilayer carbon nanotubes are dispersed in the thermoelectric conversion material, and more excellent thermoelectric characteristics can be obtained.
  • the carbon nanomaterial is preferably porous carbon particles and / or carbon nanotubes. More specifically, the carbon nanomaterial may be composed of single-walled carbon nanotubes having a diameter of 20 nm or less, or may be composed of porous carbon particles having a porosity of 8 or more. Further, the carbon nanomaterial may be made of porous carbon black having a particle size of 100 nm or less. In these cases, particularly excellent thermoelectric characteristics can be obtained.
  • the metal nanoparticles are preferably composed of particles containing at least one of Ni, Pt, Ag, Au, Co, Fe, Cu and Pd. Further, the metal nanoparticles preferably have a particle diameter of 50 nm or less, more preferably 40 nm or less, and further preferably 20 nm or less. In these cases, particularly excellent thermoelectric characteristics can be obtained.
  • thermoelectric material according to the present invention preferably contains the carbon nanomaterial in an amount of 6 wt% to 9 wt% and the metal nanoparticles in an amount of 0.5 wt% to 1 wt%. In this case, particularly excellent thermoelectric characteristics can be obtained.
  • the thermoelectric conversion material preferably comprises a substance that can be plated on the surface of the object to be treated.
  • a substance that can be plated on the surface of the object to be treated for example, Bi, Te and Sb such as Bi 2 Te 3 and Sb 2 Te 3 It may be a substance containing at least two or more of them.
  • the plating process forms a thin film on the surface of the object to be treated, so that the surface of the object to be processed can be covered. As a result, a film having excellent thermoelectric characteristics can be obtained.
  • the thermoelectric conversion material comprises a substance used for a plating process such as electroplating, hot-dip plating, electroless plating, vacuum plating, vapor phase plating, and electroplating (electroplating).
  • thermoelectric material according to the present invention has, for example, an output factor S 2 ⁇ (where S is a Seebeck coefficient and ⁇ is an electrical conductivity) of 1000 ⁇ W / m ⁇ K 2 or more, and has a dimensionless figure of merit ZT (here). (Z is a figure of merit and T is an absolute temperature) is 0.65 or more.
  • the thermoelectric material according to the present invention has more excellent thermoelectric characteristics than the conventional one, and is effective when used for power generation, cooling, waste heat recovery, and the like.
  • thermoelectric material capable of obtaining more excellent thermoelectric characteristics.
  • thermoelectric material of the Bi 2 Te 3 thin film (A) Scanning electron microscope (SEM) photograph of the thermoelectric material of the Bi 2 Te 3 thin film, (b) Scanning electron micrograph of the thermoelectric material according to the embodiment of the present invention, (c) Part of (b). It is a magnified scanning electron micrograph.
  • SEM Scanning electron microscope
  • ⁇ Seebeck coefficient S and electrical conductivity ⁇ of the thermoelectric material and Bi 2 Te 3 thin film of the embodiment of the present invention and the content of Pt nanoparticles
  • PF power factor
  • thermoelectric material of the Bi 2 Te 3 thin film (A) Scanning electron micrograph of the thermoelectric material of the Bi 2 Te 3 thin film, (b) Scanning electron micrograph of the thermoelectric material in which carbon black is dispersed in Bi 2 Te 3 according to the embodiment of the present invention. ..
  • the relationship between the content of Bi 2 Te 3 in which carbon black is dispersed thermoelectric material and Bi 2 Te 3 thin film (a) the Seebeck coefficient (Seebeck coefficient) S and carbon (Carbon) The graph shown, (b) the graph showing the relationship between the electrical conductivity ⁇ and the carbon (Carbon) content, (c) the power factor (PF) and the carbon (Carbon) content. It is a graph which shows the relationship.
  • thermoelectric material of the embodiment of the present invention comprises a thermoelectric conversion material, a carbon nanomaterial having one or more pores, and a composite material containing metal nanoparticles.
  • the thermoelectric material of the embodiment of the present invention contains 6 wt% to 9 wt% of carbon nanomaterials and 0.5 wt% to 1 wt% of metal nanoparticles.
  • thermoelectric conversion material is composed of a substance that can be plated on the surface of the object to be treated, and is used for plating such as electroplating, hot-dip plating, electroless plating, vacuum plating, vapor phase plating, and electroplating (electroplating). Consists of the substances used.
  • the thermoelectric conversion material is preferably a substance containing at least two or more of Bi, Te and Sb, and a specific example is Bi 2 Te 3 and Sb 2 Te 3 which can be electrodeposited.
  • Carbon nanomaterials consist of porous carbon particles or carbon nanotubes.
  • the carbon nanomaterial is a single-walled carbon nanotube having a diameter of 20 nm or less, or a porous carbon black having a porosity of 8 or more and a particle diameter of 100 nm or less.
  • the metal nanoparticles have a particle diameter of 20 nm or less and are composed of particles containing at least one of Ni, Pt, Ag, Au, Co, Fe, Cu and Pd.
  • thermoelectric material of the embodiment of the present invention is composed of a thermoelectric conversion material, a carbon nanomaterial having one or more pores, and a composite material containing metal nanoparticles, only Pt nanoparticles are dispersed in the thermoelectric conversion material.
  • the values of the output factor S 2 ⁇ and the dimensionless performance index ZT are larger, and more excellent thermoelectric characteristics can be obtained. Can be done. Therefore, for example, it is effective when used for power generation, cooling, waste heat recovery, and the like.
  • thermoelectric material according to the embodiment of the present invention is formed into a thin film on the surface of the object to be treated by the plating treatment, and can cover the surface of the object to be treated. As a result, a film having excellent thermoelectric characteristics can be obtained.
  • thermoelectric material in which carbon nanotubes and Pt nanoparticles are dispersed in Bi 2 Te 3 Using Bi 2 Te 3 as the thermoelectric conversion material, single-walled carbon nanotubes (SWCNT) as the carbon nanomaterial, and Pt nanoparticles as the metal nanoparticles, the thermoelectric material was produced as follows. That is, first, single-walled carbon nanotubes and Pt nanoparticles were added to an acidic aqueous solution (electrolyte solution) containing Bi-Te ions, and the atmosphere was stirred while being replaced with nitrogen gas.
  • acidic aqueous solution electrophilic aqueous solution
  • a working electrode (WE), a counter electrode (CE), and a reference electrode (RE) are placed in the stirred solution, and the potential between the working electrode and the reference electrode is controlled by a potentiostat while facing the working electrode. Electroplating was performed by passing a current between the electrode and the electrode. In this way, a thin-film thermoelectric material was formed on the surface of the working electrode.
  • the electrolytic solution used was a solution of Te 2 O 3 and Bi 2 O 4 in an aqueous solution of nitric acid (HNO 3 ). Further, the aqueous solution is not limited to the nitric acid aqueous solution, and an aqueous solution of Ni (NO 3 ) 2 or (NH 4 ) 2 PtCl 6 can also be used.
  • a gold-coated silicon substrate was used as the working electrode, platinum was used as the counter electrode, and silver chloride was used as the reference electrode.
  • thermoelectric material samples Pt-SWCNTs / Bi 2 Te 3- I, II, III with different Pt nanoparticles content were used to measure the thermoelectric properties of the thermoelectric material.
  • Each sample has a Pt nanoparticle content of 0.4 wt%, 0.6 wt%, and 0.9 wt%, and a single-walled carbon nanotube (SWCNT) content of 5.7 to 7.8 wt%.
  • SWCNT single-walled carbon nanotube
  • FIGS. 1 (b) and 1 (c) Scanning electron microscope (SEM) photographs of the prepared samples Pt-SWCNTs / Bi 2 Te 3- I and Bi 2 Te 3 thin films are shown in FIG.
  • the sample Pt-SWCNTs / Bi 2 Te 3- I to which the single-walled carbon nanotubes and Pt nanoparticles were added is the Bi 2 Te 3 thin film of FIG. 1 (a).
  • the crystals of Bi 2 Te 3 were finer.
  • FIG. 1 (c) it was also confirmed that in the sample Pt-SWCNTs / Bi 2 Te 3- I, crystals of Bi 2 Te 3 were grown on the surface of the single-walled carbon nanotubes.
  • the output factor PF becomes 1000 ⁇ W / m ⁇ K 2 or more when the content of Pt nanoparticles is 0.6 wt% and 0.9 wt%, which is 0.6 wt%. It was confirmed that it sometimes showed a peak.
  • the peak value of the output factor PF is about 1800 ⁇ W / m ⁇ K 2 .
  • the value of thermal conductivity ⁇ decreases as the content of Pt nanoparticles increases. It was also confirmed that the dimensionless figure of merit ZT was 0.85 or more when the content of Pt nanoparticles was 0.6 wt% and 0.9 wt%, and peaked at 0.6 wt%. The peak value of the dimensionless figure of merit ZT is 0.99.
  • thermoelectric material sample (thickness; 4.5 ⁇ m) having a Pt nanoparticle content of 0.9 wt% and a single-walled carbon nanotube (SWCNT) content of 6.8 to 8.5 wt% was produced. Then, the hardness was measured by the nanoindentation method. For comparison, the hardness of the Bi 2 Te 3 thin film (thickness: 9.5 ⁇ m) was measured in the same manner. As a result of the measurement, the content of Pt nanoparticles 0.9 wt% of the samples, the hardness was from 39.2 to 42.0 in terms 0.67 ⁇ 0.73 GPa, and the Vickers hardness H V.
  • thermoelectric material was hardened by adding the single-walled carbon nanotubes and Pt nanoparticles.
  • Bi 2 Te 3 as the thermoelectric conversion material
  • carbon black powder as the carbon nanomaterial
  • the thermoelectric material was produced in the same manner as each sample in Table 1.
  • the thermoelectric material produced does not contain metal nanoparticles.
  • porous Ketjen Black (“EC600JD” manufactured by Lion Specialty Chemicals Co., Ltd .; Porousness 13.7) was used.
  • carbon black was used after being coated with PDDA (polydiallyldimethylammonium chloride).
  • thermoelectric properties of the thermoelectric material As shown in Table 2, in order to measure the thermoelectric properties of the thermoelectric material, three types of samples (CB / Bi 2 Te 3- I, II, III) with different carbon (C) contents were prepared. .. Each sample has a carbon content of 3.4 wt%, 3.7 wt% and 4.3 wt%, respectively.
  • CB / Bi 2 Te 3- I, II, III three types of samples with different carbon (C) contents were prepared. ..
  • CB / Bi 2 Te 3- I, II, III three types of samples (CB / Bi 2 Te 3- I, II, III) with different carbon (C) contents were prepared. .. Each sample has a carbon content of 3.4 wt%, 3.7 wt% and 4.3 wt%, respectively.
  • the Bi 2 Te 3 thin films in Table 1 are also shown in Table 2.
  • thermoelectric materials were produced in the same manner as in each sample in Table 1.
  • the thermoelectric material produced does not contain metal nanoparticles.
  • thermoelectric properties of thermoelectric materials As shown in Table 3, three types of samples (SWCNTs / Bi 2 Te 3- I, II, III, and MWCNTs / Bi) with different carbon contents were used to measure the thermoelectric properties of thermoelectric materials. 2 Te 3- I, II, III) was manufactured. Each sample has a carbon content of 3.8 wt%, 4.1 wt%, 4.4 wt%, 3.6 wt%, 4.1 wt% and 4.8 wt%, respectively.
  • the Bi 2 Te 3 thin films in Table 1 are also shown in Table 3.
  • the output factor PF is about 790 to 950 ⁇ W / m ⁇ K 2 in the sample to which carbon black is added, which is larger than that in the sample to which carbon nanotubes are added. It was confirmed that it was. Further, as shown in Table 2, it was confirmed that the dimensionless figure of merit ZT was 0.64 in the sample to which carbon black was added, which was larger than that of the Bi 2 Te 3 thin film.
  • thermoelectric material in which carbon nanotubes and Pt nanoparticles are dispersed in Bi 2 Te 3 (see, for example, FIGS. 2 and 3) and a thermoelectric material in which carbon black or carbon nanotubes are dispersed in Bi 2 Te 3
  • the thermoelectric material in which both carbon nanotubes and Pt nanoparticles are dispersed has an output factor PF of 1000 ⁇ W / m ⁇ K 2 by adjusting their contents.
  • the dimensionless performance index ZT is 0.65 or more, and it can be said that excellent thermoelectric characteristics can be obtained as compared with the thermoelectric material to which only one of carbon black and carbon nanotube is added.

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Abstract

Le problème décrit par la présente invention est de fournir un matériau thermoélectrique qui peut obtenir de meilleures caractéristiques thermoélectriques. La solution selon la présente invention porte sur un matériau thermoélectrique qui est composé d'un matériau composite qui contient un matériau de conversion thermoélectrique, un nanomatériau de carbone ayant un ou plusieurs pores, et des nanoparticules métalliques. Il est préférable que le matériau de conversion thermoélectrique soit composé d'une substance qui peut être plaquée sur la surface d'un objet à traiter. Il est préférable que le nanomatériau de carbone soit composé de particules de carbone poreux et/ou de nanotubes de carbone. Il est préférable que les nanoparticules métalliques soient composées de particules qui contiennent au moins un élément parmi Ni, Pt, Ag, Au, Co, Fe, Cu et Pd. Il est préférable que le matériau thermoélectrique contienne de 6 % en poids à 9 % en poids du nanomatériau de carbone et de 0,5 % en poids à 1 % en poids de la nanoparticule métallique.
PCT/JP2020/023300 2019-06-20 2020-06-12 Matériau thermoélectrique WO2020255898A1 (fr)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN116589253A (zh) * 2023-05-31 2023-08-15 山东交通学院 一种碳微球复合水泥基热电材料及其制备方法

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JP2008523614A (ja) * 2004-12-07 2008-07-03 トヨタ テクニカル センター，ユー．エス．エー．，インコーポレイティド ナノ構造のバルク熱電材料
JP2013058531A (ja) * 2011-09-07 2013-03-28 Toyota Industries Corp 熱電変換材料
JP2015228498A (ja) * 2014-05-30 2015-12-17 三星電子株式会社Ｓａｍｓｕｎｇ Ｅｌｅｃｔｒｏｎｉｃｓ Ｃｏ．，Ｌｔｄ． 伸縮性熱電複合体、及びそれを含む熱電素子
WO2017122805A1 (fr) * 2016-01-15 2017-07-20 日本ゼオン株式会社 Composition pour élément de conversion thermoélectrique, procédé de production de nanotubes de carbone qui portent des nanoparticules de métal, corps moulé pour élément de conversion thermoélectrique et son procédé de production, et élément de conversion thermoélectrique
US20180108449A1 (en) * 2014-11-12 2018-04-19 Korea Institute Of Machinery & Materials Thermoelectric composite material and method for preparing thermoelectric composite material

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2008523614A (ja) * 2004-12-07 2008-07-03 トヨタ テクニカル センター，ユー．エス．エー．，インコーポレイティド ナノ構造のバルク熱電材料
JP2013058531A (ja) * 2011-09-07 2013-03-28 Toyota Industries Corp 熱電変換材料
JP2015228498A (ja) * 2014-05-30 2015-12-17 三星電子株式会社Ｓａｍｓｕｎｇ Ｅｌｅｃｔｒｏｎｉｃｓ Ｃｏ．，Ｌｔｄ． 伸縮性熱電複合体、及びそれを含む熱電素子
US20180108449A1 (en) * 2014-11-12 2018-04-19 Korea Institute Of Machinery & Materials Thermoelectric composite material and method for preparing thermoelectric composite material
WO2017122805A1 (fr) * 2016-01-15 2017-07-20 日本ゼオン株式会社 Composition pour élément de conversion thermoélectrique, procédé de production de nanotubes de carbone qui portent des nanoparticules de métal, corps moulé pour élément de conversion thermoélectrique et son procédé de production, et élément de conversion thermoélectrique

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN116589253A (zh) * 2023-05-31 2023-08-15 山东交通学院 一种碳微球复合水泥基热电材料及其制备方法

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