WO2017208929A1 - Module de conversion thermoélectrique - Google Patents

Module de conversion thermoélectrique Download PDF

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Publication number
WO2017208929A1
WO2017208929A1 PCT/JP2017/019352 JP2017019352W WO2017208929A1 WO 2017208929 A1 WO2017208929 A1 WO 2017208929A1 JP 2017019352 W JP2017019352 W JP 2017019352W WO 2017208929 A1 WO2017208929 A1 WO 2017208929A1
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Prior art keywords
thermoelectric conversion
layer
type thermoelectric
conversion layer
module
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PCT/JP2017/019352
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English (en)
Japanese (ja)
Inventor
鈴木　秀幸
真二 今井
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富士フイルム株式会社
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Priority to JP2018520836A priority Critical patent/JP6659836B2/ja
Publication of WO2017208929A1 publication Critical patent/WO2017208929A1/fr

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    • H—ELECTRICITY
    • H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
    • H02N—ELECTRIC MACHINES NOT OTHERWISE PROVIDED FOR
    • H02N11/00—Generators or motors not provided for elsewhere; Alleged perpetua mobilia obtained by electric or magnetic means
    • 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
    • H10N10/10—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects
    • H10N10/17—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects operating with only the Peltier or Seebeck effects characterised by the structure or configuration of the cell or thermocouple forming the device

Definitions

  • the present invention relates to a thermoelectric conversion module folded in a bellows shape.
  • thermoelectric conversion materials that can mutually convert thermal energy and electrical energy are used for thermoelectric conversion elements such as power generation elements and Peltier elements that generate electricity by heat.
  • the thermoelectric conversion element can convert heat energy directly into electric power, and has an advantage that a movable part is not required. For this reason, a thermoelectric conversion module (power generation device) formed by connecting a plurality of thermoelectric conversion elements is provided in a portion where heat is exhausted, such as an incinerator or various facilities in a factory, so that it is not necessary to incur operation costs and is simple. Can get power.
  • thermoelectric conversion elements are usually used as thermoelectric conversion modules in which a plurality of thermoelectric conversion elements are connected in series.
  • thermoelectric conversion module a so-called ⁇ -type thermoelectric conversion module using a thermoelectric conversion material such as Bi-Te is known.
  • p-type and n-type thermoelectric conversion materials are processed into blocks, arranged alternately on a substrate such as ceramics, and the arranged thermoelectric conversion materials are connected in series. That is how it is made.
  • thermoelectric conversion module takes time and effort to process block-shaped thermoelectric conversion materials, arrangement of thermoelectric conversion materials, connection of thermoelectric conversion materials by electrodes, and the like.
  • a thermoelectric conversion module has been reported in which a resin film or the like is used as an insulating substrate, and an ink-like thermoelectric conversion material is formed on the insulating substrate by a coating or printing process. This thermoelectric conversion module is easy to manufacture, and many thermoelectric conversion elements can be continuously manufactured by printing or the like.
  • thermoelectric conversion module thermoelectric thin film device having a thermoelectric thin film element that generates power by forming a temperature difference is described.
  • Patent Document 2 discloses that a flexible insulating sheet folded in a bellows shape having a plurality of formation regions where thermocouples are formed and a non-formation region where thermocouples are not formed, and formation of the insulation sheet
  • a thermoelectric conversion module thermoelectric generator
  • thermoelectric generator thermoelectric generator
  • thermoelectric conversion is performed by a coating method using an ink-like thermoelectric conversion material or an electrode material, a printing method, or a vacuum film formation method such as vacuum deposition. Conversion layers and electrodes can be formed. Therefore, this thermoelectric conversion module is easy to manufacture and can be manufactured at a lower cost than a ⁇ -type thermoelectric conversion module using a block-shaped thermoelectric conversion material. Moreover, since the electromotive force per thermoelectric conversion element is very small, the thermoelectric conversion module needs to connect several hundred or more thermoelectric conversion elements in series to increase the voltage and the amount of power generation. On the other hand, if it is a thermoelectric conversion module using a resin film etc. as a support body, formation of many thermoelectric conversion elements can be easily coped with by manufacture by printing etc.
  • JP 2012-212838 A Japanese Patent Laid-Open No. 2008-130813
  • thermoelectric conversion module In such a flexible bellows-like thermoelectric conversion module, various methods are conceivable as methods for improving the performance such as the amount of power generation.
  • thermoelectric conversion module having a shape folded in a conventional bellows shape has an inclined surface of the bellows on which a thermoelectric conversion layer or the like is formed, and an inclined surface facing each other. It is in a separated state.
  • a bellows-like thermoelectric conversion module can reduce the size, improve the heat transfer efficiency, improve the mounting density of the thermoelectric conversion elements, and the like. It is advantageous that the bellows be closed as much as possible by compressing in the arrangement direction.
  • thermoelectric conversion module when the bellows is closed, the electrodes and the thermoelectric conversion layers come into contact with each other, short-circuiting, and no power is generated. Therefore, in the conventional bellows-shaped thermoelectric conversion module, in order to close the bellows, it is necessary to combine insulating members, to form an insulating layer covering the electrodes and the thermoelectric conversion layer, etc. There is a possibility of causing a decrease in the property.
  • An object of the present invention is to solve such problems of the prior art, and prevent short-circuiting of electrodes and thermoelectric conversion layers without combining insulating members or forming an insulating layer. It is in providing the thermoelectric conversion module which can be closed.
  • thermoelectric conversion module of the present invention is formed by alternately forming a plurality of first layers folded in a bellows shape and spaced apart in a bellows-like folding direction on one surface of the first layer.
  • thermoelectric conversion layer and the n-type thermoelectric conversion layer are electrically connected by an electrode pair, Furthermore, in the bellows-like folding direction, It has a pattern of p-type thermoelectric conversion layer-p-type thermoelectric conversion layer-first layer-first layer-n-type thermoelectric conversion layer-n-type thermoelectric conversion layer-second layer-second layer.
  • a thermoelectric conversion module is provided.
  • thermoelectric conversion module of the present invention the p-type thermoelectric conversion layer and the n-type thermoelectric conversion layer formed on one surface of the first layer are electrically connected by an electrode pair, and It is preferable that the p-type thermoelectric conversion layer and the n-type thermoelectric conversion layer formed on one surface of the two layers are electrically connected by an electrode pair.
  • the first layer is the first substrate
  • the second layer is the second substrate
  • the p-type thermoelectric conversion layer formation surface of the first substrate and the p-type thermoelectric conversion layer formation surface of the second substrate.
  • the first substrate and the second substrate are laminated facing each other. Further, it is preferable that one substrate becomes the first layer and the second layer by bending one substrate.
  • a flexible linear member is inserted through the first layer and the second layer.
  • the linear member is a place other than the formation part of the first p-type thermoelectric conversion layer and the n-type thermoelectric conversion layer and the formation part of the second p-type thermoelectric conversion layer and the n-type thermoelectric conversion layer. It is preferable to pass through.
  • the linear member is at the same position in the bellows-like folding direction with respect to the electrode pair formed on one surface of the first layer and the electrode pair formed on one surface of the second layer, And it is preferable to penetrate the 1st layer and the 2nd layer in the outside of the longitudinal direction of the ridgeline by the bellows-like folding.
  • the heat conductive member is inserted into at least one of the first layer and the first layer and the second layer and the second layer in the pattern. Further, the heat conducting member faces in an accordion-like folded direction with respect to at least one of the electrode pair formed on one surface of the first layer and the electrode pair formed on one surface of the second layer. It is preferably inserted at a position where Furthermore, it is preferable to have at least one of a plate-like heat conduction member and a bellows-like heat conduction member as the heat conduction member.
  • thermoelectric conversion module in the bellows-shaped thermoelectric conversion module, it is possible to close the bellows by preventing short-circuiting of the electrodes and the thermoelectric conversion layer without combining insulating members, forming an insulating layer, or the like. it can.
  • FIG. 1 is a diagram conceptually illustrating an example of the thermoelectric conversion module of the present invention.
  • FIG. 2 is a conceptual diagram for explaining the thermoelectric conversion module shown in FIG. 1.
  • FIG. 3 is a conceptual diagram for explaining the thermoelectric conversion module shown in FIG. 1.
  • FIG. 4 is an equivalent circuit of the thermoelectric conversion module of the present invention.
  • FIG. 5 is a diagram conceptually illustrating another example of the thermoelectric conversion module of the present invention.
  • FIG. 6 is a diagram conceptually illustrating another example of the thermoelectric conversion module of the present invention.
  • FIG. 7 is a conceptual diagram for explaining the thermoelectric conversion module shown in FIG. 6.
  • FIG. 8 is a diagram conceptually showing a usage pattern of the thermoelectric conversion module of the present invention.
  • FIG. 9 is a diagram conceptually showing another usage pattern of the thermoelectric conversion module of the present invention.
  • FIG. 10 is a diagram conceptually showing another example of the thermoelectric conversion module of the present invention.
  • thermoelectric conversion module of the present invention will be described in detail based on a preferred embodiment shown in the accompanying drawings.
  • a numerical range expressed using “to” means a range including numerical values described before and after “to” as a lower limit value and an upper limit value.
  • FIG. 1 conceptually shows an example of the thermoelectric conversion module of the present invention.
  • the thermoelectric conversion module 10 shown in FIG. 1 includes a first module 10A in which a thermoelectric conversion layer or the like is formed on one surface of a first substrate 12A folded in a bellows shape, and a thermoelectric conversion on one surface of a second substrate 12B folded in a bellows shape. This is a combination of the second module 10B on which a conversion layer or the like is formed.
  • FIG. 1 shows a state in which the bellows is closed by compressing the thermoelectric conversion module of the present invention in the folding direction of the bellows, that is, in the longitudinal direction of the first substrate 12A and the second substrate 12B (lateral direction in the figure).
  • FIG. 1 shows the bellows-like folded portion in a rectangular shape so that the configuration and each member of the thermoelectric conversion module 10 can be clearly shown.
  • the state in which the bellows is closed is a state in which the bellows-like thermoelectric conversion module as shown in FIG. 2 is compressed in the folding direction of the bellows.
  • FIG. 1 is a conceptual diagram to the last, and the relationship between thickness, size, length, and the like between the members is different from that of an actual thermoelectric conversion module.
  • thermoelectric conversion module 10 shown in FIG. 1 is a combination of the first module 10A and the second module 10B.
  • the first module 10A includes a first substrate 12A, a p-type thermoelectric conversion layer 14p, an n-type thermoelectric conversion layer 16n, and a connection electrode 18.
  • the first substrate 12A is the first layer in the thermoelectric conversion module of the present invention.
  • the second module 10B includes a second substrate 12B, a p-type thermoelectric conversion layer 14p, an n-type thermoelectric conversion layer 16n, and a connection electrode 18.
  • the second substrate 12B is the second layer in the thermoelectric conversion module of the present invention.
  • the first substrate 12A and the second substrate 12B are hatched, and the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n are shaded. .
  • thermoelectric conversion module 10 and the thermoelectric conversion module 10 of the present invention are disassembled into a first module 10A and a second module 10B, and a state in which the first module 10A and the second module 10B are extended in a planar shape.
  • the upper stage is a state where the first module 10 ⁇ / b> A and the second module 10 ⁇ / b> B are extended in a planar shape
  • the middle stage is a state where the thermoelectric conversion module 10 is disassembled
  • the lower stage is the thermoelectric conversion module 10. .
  • FIG. 3 is a view of the first module 10A and the second module 10B extending in a planar shape, as viewed from above (second module 10B) and below (first module 10A) in the middle and lower parts of FIG. is there. That is, the middle stage and the lower stage (FIGS. 1 and 2) of FIG. 3 fold back the first module 10A and the second module 10B extended in a planar shape shown in the upper stage of FIG. It is the figure seen in the up-down direction in the figure.
  • the first module 10A, the second module 10B, and the first substrate 12A have basically the same configuration except that the bellows-like folding direction of the first substrate 12A is different from the bellows-like folding direction of the second substrate 12B. Therefore, except for the case where it is necessary to distinguish the two, the description will be made with the first module 10A as a representative example.
  • the first module 10A (second module 10B) is fixed on one surface of the long first substrate 12A (second substrate 12B) at a constant interval in the longitudinal direction of the first substrate 12A.
  • a connection electrode 18 having a length is formed, and p-type thermoelectric conversion layers 14p and n-type thermoelectric conversion layers 16n having a certain length are alternately arranged on the same surface of the first substrate 12A in the longitudinal direction of the first substrate 12A. Is formed.
  • the “longitudinal direction of the first substrate 12A” that is, the bellows-like folding direction is also referred to as “longitudinal direction”.
  • the width direction of the first substrate 12A that is, the direction orthogonal to the longitudinal direction is also referred to as “width direction”. Therefore, the width direction is a direction perpendicular to the paper surface in the middle and lower stages of FIG. 1 (FIG. 2) and FIG.
  • the length and interval in the longitudinal direction are the length and interval in a state where the first module 10A (first substrate 12A) is extended in a planar shape.
  • the first module 10A has a bellows-like shape that is alternately folded into a mountain fold and a valley fold by a fold line (broken line in the upper part of FIG. 3) parallel to the width direction of the first substrate 12A at the center of the connection electrode 18 in the longitudinal direction. It has become. Therefore, the first module 10A has alternately the mountain folds and the valley folds in the longitudinal direction, and alternately has the top and the bottom by accordion-like folding. Therefore, the longitudinal direction coincides with the inclination direction of the inclined surface by the bellows-like folding.
  • the first substrate 12A is folded inward on the inner side, that is, the side on which the connection electrode 18 is convex, and the first substrate 12A is on the outer side, ie, on the side in which the connection electrode 18 is concave, by valley folding.
  • the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n are spaced apart and alternately arranged in the longitudinal direction, and the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n adjacent to each other in the longitudinal direction.
  • the connection electrode 18 is connected in series by the connection electrode 18.
  • the first module 10 ⁇ / b> A is folded in a mountain fold and a valley fold at the longitudinal center of the connection electrode 18 to have a bellows shape.
  • a high temperature heat source is provided on the lower side of FIG. 1 (lower stage in FIG.
  • thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n formed on the inclined surface of the first substrate 12A generate power by generating a temperature difference in the thermoelectric conversion layer in the longitudinal direction.
  • the first substrate 12A (second substrate 12B) is long, flexible, and insulative.
  • a long sheet-like material (film) used in a known thermoelectric conversion module using a flexible support. ) Can be used in various ways.
  • polyester resins such as polyethylene terephthalate, polyethylene isophthalate, polyethylene naphthalate, polybutylene terephthalate, poly (1,4-cyclohexylenedimethylene terephthalate), polyethylene-2,6-phthalenedicarboxylate, polyimide
  • the sheet-like material are polycarbonate, polypropylene, polyethersulfone, cycloolefin polymer, polyetheretherketone (PEEK), triacetylcellulose (TAC), and other resins, glass epoxy, liquid crystalline polyester, and the like.
  • the sheet-like material which consists of a polyimide, a polyethylene terephthalate, a polyethylene naphthalate etc. is utilized suitably by points, such as thermal conductivity, heat resistance, solvent resistance, availability, and economical efficiency.
  • the thickness of the first substrate 12A may be set as appropriate so that sufficient flexibility can be obtained and the thickness that functions as the first substrate 12A can be set according to the forming material of the first substrate 12A.
  • the length and width of the first substrate 12A may be set as appropriate according to the size and application of the first module 10A.
  • thermoelectric conversion layer On one surface of the first substrate 12A, p-type thermoelectric conversion layers 14p and n-type thermoelectric conversion layers 16n having a certain length are alternately arranged at regular intervals in the longitudinal direction.
  • thermoelectric conversion layer when it is not necessary to distinguish between the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n, both are collectively referred to as “thermoelectric conversion layer”.
  • thermoelectric conversion layers 14p and n-type thermoelectric conversion layers 16n made of known thermoelectric conversion materials can be used.
  • the thermoelectric conversion material constituting the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n include nickel or a nickel alloy.
  • nickel alloys that generate electricity by generating a temperature difference can be used. Specific examples include nickel alloys mixed with one component or two or more components such as vanadium, chromium, silicon, aluminum, titanium, molybdenum, manganese, zinc, tin, copper, cobalt, iron, magnesium, and zirconium.
  • the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n have a nickel content of 90 atomic% or more.
  • the nickel content is more preferably 95 atomic% or more, and particularly preferably made of nickel.
  • the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n made of nickel include those having inevitable impurities.
  • thermoelectric conversion material of the p-type thermoelectric conversion layer 14p When nickel alloy is used as the thermoelectric conversion material of the p-type thermoelectric conversion layer 14p, chromel containing nickel and chromium as main components is typical. In addition, when a nickel alloy is used as the thermoelectric material of the n-type thermoelectric conversion layer 16n, constantan mainly composed of copper and nickel is typical. When nickel or a nickel alloy is used as the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n, and when nickel or a nickel alloy is also used as the connection electrode 18, the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n and the connection electrode 18 may be integrally formed.
  • thermoelectric conversion materials that can be used for the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n include the following materials in addition to nickel and nickel alloys.
  • thermoelectric conversion material used for the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n a pasteable material capable of forming a film by coating or printing can be used.
  • thermoelectric conversion materials include organic thermoelectric conversion materials such as conductive polymers or conductive nanocarbon materials.
  • the conductive polymer include a polymer compound having a conjugated molecular structure (conjugated polymer).
  • conjugated polymer include known ⁇ -conjugated polymers such as polyaniline, polyphenylene vinylene, polypyrrole, polythiophene, polyfluorene, acetylene, and polyphenylene.
  • polydioxythiophene can be preferably used.
  • the conductive nanocarbon material include carbon nanotubes, carbon nanofibers, graphite, graphene, and carbon nanoparticles. These may be used alone or in combination of two or more. Among these, carbon nanotubes are preferably used because the thermoelectric characteristics are better. In the following description, “carbon nanotube” is also referred to as “CNT”.
  • CNT is a single-layer CNT in which one carbon film (graphene sheet) is wound in a cylindrical shape, two-layer CNT in which two graphene sheets are concentrically wound, and a plurality of graphene sheets in a concentric circle
  • multi-walled CNTs wound in a shape In the present invention, single-walled CNTs, double-walled CNTs, and multilayered CNTs may be used alone, or two or more kinds may be used in combination.
  • single-walled CNT and double-walled CNT having excellent properties in terms of conductivity and semiconductor properties are preferably used, and single-walled CNT is more preferably used.
  • Single-walled CNTs may be semiconducting or metallic, and both may be used in combination. When using both semiconducting CNT and metallic CNT, the content ratio of both can be adjusted suitably.
  • the CNT may contain a metal or the like, or may contain a molecule such as fullerene.
  • the average length of the CNT is not particularly limited and can be selected as appropriate. Specifically, although it depends on the distance between the electrodes, the average length of the CNT is preferably 0.01 to 2000 ⁇ m, more preferably 0.1 to 1000 ⁇ m from the viewpoints of manufacturability, film formability, conductivity, and the like. 1 to 1000 ⁇ m is particularly preferable.
  • the diameter of the CNT is not particularly limited, but is preferably 0.4 to 100 nm, more preferably 50 nm or less, and particularly preferably 15 nm or less from the viewpoint of durability, transparency, film formability, conductivity, and the like.
  • the diameter of the CNT is preferably 0.5 to 2.2 nm, more preferably 1.0 to 2.2 nm, and particularly preferably 1.5 to 2.0 nm.
  • CNT may contain defective CNT. Such CNT defects are preferably reduced in order to reduce the conductivity of the thermoelectric conversion layer.
  • the amount of CNT defects can be estimated by the ratio G / D between the G-band and D-band of the Raman spectrum. It can be estimated that the higher the G / D ratio, the less the amount of defects, the CNT material.
  • the CNT preferably has a G / D ratio of 10 or more, more preferably 30 or more.
  • CNTs modified or treated with CNTs can be used. Modification or treatment methods include a method of encapsulating a ferrocene derivative or nitrogen-substituted fullerene (azafullerene), a method of doping an alkali metal (such as potassium) or a metal element (such as indium) into the CNT by an ion doping method, CNT in a vacuum The method etc. which heat this are illustrated.
  • nanocarbon such as carbon nanohorn, carbon nanocoil, carbon nanobead, graphite, graphene, and amorphous carbon may be included.
  • the thermoelectric conversion layer preferably contains a p-type dopant or an n-type dopant.
  • P-type dopant As p-type dopants, halogens (iodine, bromine, etc.), Lewis acids (PF 5 , AsF 5 etc.), proton acids (hydrochloric acid, sulfuric acid etc.), transition metal halides (FeCl 3 , SnCl 4 etc.), metal oxides (Molybdenum oxide, vanadium oxide, etc.), organic electron accepting substances and the like are exemplified.
  • organic electron accepting substance examples include 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane, 2,5-dimethyl-7,7,8,8- Tetracyanoquinodimethane such as tetracyanoquinodimethane, 2-fluoro-7,7,8,8-tetracyanoquinodimethane, 2,5-difluoro-7,7,8,8-tetracyanoquinodimethane (TCNQ) derivatives, 2,3-dichloro-5,6-dicyano-p-benzoquinone, benzoquinone derivatives such as tetrafluoro-1,4-benzoquinone, etc., 5,8H-5,8-bis (dicyanomethylene) quinoxaline, Preferred examples include dipyrazino [2,3-f: 2 ′, 3′-h] quinoxaline-2,3,6,7,10,11-hexacarbonitrile.
  • organic electron-accepting substances such as TCNQ (tetracyanoquinodimethane) derivatives or benzoquinone derivatives are preferably exemplified in terms of material stability, compatibility with CNTs, and the like.
  • TCNQ tetracyanoquinodimethane
  • benzoquinone derivatives are preferably exemplified in terms of material stability, compatibility with CNTs, and the like.
  • Each of the p-type dopant and the n-type dopant may be used alone or in combination of two or more.
  • N-type dopant include (1) alkali metals such as sodium and potassium, (2) phosphines such as triphenylphosphine and ethylenebis (diphenylphosphine), and (3) polymers such as polyvinylpyrrolidone and polyethyleneimine. These materials can be used.
  • polyethylene glycol type higher alcohol ethylene oxide adducts such as phenol or naphthol
  • fatty acid ethylene oxide adducts polyhydric alcohol fatty acid ester ethylene oxide adducts, higher alkylamine ethylene oxide adducts, fatty acids Amide ethylene oxide adduct, fat and oil ethylene oxide adduct, polypropylene glycol ethylene oxide adduct, dimethylsiloxane-ethylene oxide block copolymer, dimethylsiloxane- (propylene oxide-ethylene oxide) block copolymer, etc.
  • thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n a thermoelectric conversion layer in which a thermoelectric conversion material is dispersed in a resin material (binder) is also preferably used.
  • distributing a conductive nano carbon material to a resin material is illustrated more suitably.
  • a thermoelectric conversion layer in which CNT is dispersed in a resin material is particularly preferably exemplified in that high conductivity is obtained.
  • Various known non-conductive resin materials (polymer materials) can be used as the resin material. Specific examples include vinyl compounds, (meth) acrylate compounds, carbonate compounds, ester compounds, epoxy compounds, siloxane compounds, and gelatin.
  • examples of the vinyl compound include polystyrene, polyvinyl naphthalene, polyvinyl acetate, polyvinyl phenol, polyvinyl butyral, and the like.
  • examples of the (meth) acrylate compound include polymethyl (meth) acrylate, polyethyl (meth) acrylate, polyphenoxy (poly) ethylene glycol (meth) acrylate, polybenzyl (meth) acrylate and the like.
  • examples of the carbonate compound include bisphenol Z-type polycarbonate and bisphenol C-type polycarbonate. As the ester compound, amorphous polyester is exemplified.
  • Preferred examples include polystyrene, polyvinyl butyral, (meth) acrylate compounds, carbonate compounds, and ester compounds, and more preferred are polyvinyl butyral, polyphenoxy (poly) ethylene glycol (meth) acrylate, polybenzyl (meth) acrylate, and amorphous.
  • An example is a reactive polyester.
  • the quantity ratio of the resin material to the thermoelectric conversion material is the material used, the required thermoelectric conversion efficiency, the viscosity or solid content concentration of the solution affecting printing, etc. It may be set appropriately according to the above.
  • thermoelectric conversion layer mainly composed of CNT and a surfactant is also preferably used.
  • the thermoelectric conversion layer can be formed with a coating composition to which a surfactant is added. Therefore, the thermoelectric conversion layer can be formed with a coating composition in which CNTs are reasonably dispersed. As a result, good thermoelectric conversion performance can be obtained by the thermoelectric conversion layer containing many CNTs that are long and have few defects.
  • the surfactant a known surfactant can be used as long as it has a function of dispersing CNTs. More specifically, various surfactants can be used as long as they have a group that dissolves in water, a polar solvent, or a mixture of water and a polar solvent and adsorbs CNTs. Accordingly, the surfactant may be ionic or nonionic. The ionic surfactant may be any of cationic, anionic and amphoteric.
  • anionic surfactant examples include alkylbenzene sulfonates such as dodecylbenzene sulfonic acid, aromatic sulfonic acid surfactants such as dodecyl phenyl ether sulfonate, monosoap anionic surfactants, ether sulfates Surfactants, phosphate surfactants and carboxylic acid surfactants such as sodium deoxycholate or sodium cholate, carboxymethylcellulose and salts thereof (sodium salt, ammonium salt, etc.), ammonium polystyrene sulfonate, Examples thereof include water-soluble polymers such as polystyrene sulfonate sodium salt.
  • Examples of the cationic surfactant include alkylamine salts and quaternary ammonium salts.
  • amphoteric surfactants include alkyl betaine surfactants and amine oxide surfactants.
  • examples of nonionic surfactants include sugar ester surfactants such as sorbitan fatty acid esters, fatty acid ester surfactants such as polyoxyethylene resin acid esters, ether surfactants such as polyoxyethylene alkyl ether, and the like. Is exemplified. Among these, ionic surfactants are preferably used, and among them, cholate or deoxycholate is preferably used.
  • the surfactant / CNT mass ratio is preferably 5 or less, and more preferably 3 or less. Setting the mass ratio of surfactant / CNT to 5 or less is preferable in that higher thermoelectric conversion performance can be obtained.
  • thermoelectric conversion layer made of an organic material, optionally, SiO 2, TiO 2, Al 2 O 3, may have an inorganic material such as ZrO 2.
  • a thermoelectric conversion layer contains an inorganic material, it is preferable that the content is 20 mass% or less, and it is more preferable that it is 10 mass% or less.
  • thermoelectric conversion layer 14p and n-type thermoelectric conversion layer 16n may be formed by a known method.
  • the following method is illustrated as an example.
  • a coating composition for forming a thermoelectric conversion layer containing a thermoelectric conversion material and necessary components such as a surfactant is prepared.
  • the coating composition used as the thermoelectric conversion layer prepared is patterned and apply
  • the coating composition may be applied by a known method such as a method using a mask or a printing method. After applying the coating composition, the coating composition is dried by a method according to the resin material to form a thermoelectric conversion layer.
  • thermoelectric conversion layer may be patterned by etching or the like after coating the prepared coating composition to be the thermoelectric conversion layer on the entire surface of the insulating support and drying it.
  • thermoelectric conversion layer mainly composed of CNT and a surfactant
  • the thermoelectric conversion layer is immersed in a solvent that dissolves the surfactant
  • the thermoelectric conversion layer is preferably formed by washing the thermoelectric conversion layer with a solvent that dissolves the surfactant and then drying. Thereby, the surfactant is removed from the thermoelectric conversion layer, and a thermoelectric conversion layer in which the surfactant / CNT mass ratio is extremely small, more preferably no surfactant is present, can be formed.
  • the thermoelectric conversion layer is preferably patterned by printing.
  • thermoelectric conversion layer As the printing method, various known printing methods such as screen printing, metal mask printing, and inkjet can be used. In addition, when pattern-forming a thermoelectric conversion layer using the coating composition containing CNT, it is more preferable to use metal mask printing.
  • the printing conditions may be appropriately set depending on the physical properties (solid content concentration, viscosity, viscoelastic physical properties) of the coating composition to be used, the opening size of the printing plate, the number of openings, the opening shape, the printing area, and the like.
  • thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n are formed of the inorganic material such as nickel, nickel alloy, or BiTe-based material, other than the forming method using such a coating composition.
  • the thermoelectric conversion layer can be formed by using a film forming method such as sputtering, CVD (Chemical Vapor Deposition), vapor deposition, plating, or aerosol deposition.
  • the sizes of the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n may be appropriately set according to the size of the first module 10A, the width of the first substrate 12A, the size of the connection electrode 18, and the like. . In the present invention, the size is the size in the surface direction of the first substrate 12A. As described above, the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n have the same length in the longitudinal direction. Further, since the thermoelectric conversion layers are formed at regular intervals, the p-type thermoelectric conversion layers 14p and the n-type thermoelectric conversion layers 16n are alternately formed at the same intervals.
  • the thicknesses of the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n may be appropriately set according to the material for forming the thermoelectric conversion layer, but are preferably 1 to 20 ⁇ m, and more preferably 3 to 15 ⁇ m. By setting the thicknesses of the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n within this range, it is preferable in terms of obtaining good electrical conductivity and good printability.
  • the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n may have the same or different thicknesses, but basically have the same thickness.
  • the connection electrode 18 is formed on the formation surface of the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n of the first substrate 12A.
  • the connection electrode 18 is an electrode pair in the present invention.
  • the connection electrode 18 electrically connects the p-type thermoelectric conversion layers 14p and the n-type thermoelectric conversion layers 16n alternately formed in the longitudinal direction in series.
  • the thermoelectric conversion layer is formed with a certain length in the longitudinal direction at regular intervals. Accordingly, the connection electrodes 18 having a certain length are formed at regular intervals.
  • the first module 10 ⁇ / b> A is folded back at the center in the longitudinal direction of the connection electrode 18 by a mountain fold and a valley fold along a fold line parallel to the width direction.
  • connection electrode 18 Any material can be used for the connection electrode 18 as long as it has a necessary conductivity.
  • various materials such as copper, silver, gold, platinum, nickel, aluminum, constantan, chromium, indium, iron, copper alloy, and other devices such as indium tin oxide (ITO) and zinc oxide (ZnO) Examples include materials used as transparent electrodes.
  • ITO indium tin oxide
  • ZnO zinc oxide
  • the connection electrode 18 may be a laminated electrode such as a configuration in which a copper layer is formed on a chromium layer.
  • connection electrode 18 may be patterned by a known method according to the material for forming the connection electrode 18 such as a vapor deposition method such as vacuum deposition or sputtering or a coating method such as printing. .
  • the size of the connection electrode 18 is the size of the first module 10A, the width of the first substrate 12A, the sizes of the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n, the p-type thermoelectric conversion layer 14p and the n-type thermoelectric. What is necessary is just to set suitably according to the space
  • the thickness of the connection electrode 18 may be appropriately set to a thickness that can ensure sufficient conductivity between the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n in accordance with the forming material.
  • the first module 10A (second module 10B) can be manufactured by a known method.
  • the thermoelectric conversion layer and the connection electrode 18 are formed by patterning on a long plate-like first substrate 12A by a known method according to a forming material such as a printing method. Thereafter, a known sheet-like material is bent, such as pressing or a process using a roll using protrusions, and folded into a bellows shape to form a bellows-like first module 10A.
  • These operations are preferably performed by so-called roll-to-roll, in which various processes are continuously performed while the first substrate 12A (substrate to be processed) is conveyed in the longitudinal direction.
  • thermoelectric conversion module 10 of the present invention shown in FIGS. 1 to 3 is a combination of the first module 10A and the second module 10B.
  • the bellows-like folding direction is reversed between the first module 10A and the second module 10B. That is, the order of mountain folding and valley folding is reversed.
  • the accordion-like folds in the connection electrodes 18 between the thermoelectric conversion layers start from the left side in the figure from the valley fold-mountain fold-valley. Fold-mountain fold-valley fold.
  • the bellows-like folds in the connection electrodes 18 between the thermoelectric conversion layers are mountain fold-valley fold-mountain fold-valley fold-mountain fold from the left side in the figure.
  • the first module 10A on the right side is turned upside down, and the first substrate 12A is set to the upper side in the figure. Furthermore, as shown in the lower part of FIG. 3 (FIGS. 1 and 2), the p-type thermoelectric conversion layer 14p of the first module 10A and the p-type thermoelectric conversion layer 14p of the second module 10B face each other, and the first module 10A
  • the n-type thermoelectric conversion layer 16n of the second module 10B and the n-type thermoelectric conversion layer 16n of the second module 10B face each other, and a valley fold (valley) of the first module 10A and a mountain fold (
  • the first module 10A and the second module 10B are stacked by matching the mountain fold (top) of the first module 10A with the valley fold (valley) of the second module 10B. To do.
  • thermoelectric conversion module 10 of this invention is formed.
  • a thermoelectric conversion module of the present invention is a thermoelectric conversion module in which parallel parallel thermoelectric conversion elements are connected as shown in the equivalent circuit of FIG.
  • the thermoelectric conversion module 10 of this invention seals the edge part of the width direction with a well-known material with high gas barrier property in the state which accumulated the 1st module 10A and the 2nd module 10B.
  • the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n can be prevented from deterioration caused by moisture, sulfide gas, nitrogen oxides, etc. in the atmosphere, and the durability of the thermoelectric conversion module 10 is improved. Can be made.
  • thermoelectric conversion module 10 includes: “p-type thermoelectric conversion layer 14p-p-type thermoelectric conversion layer 14p—first substrate 12A (first layer) —first substrate 12A (first layer) —n-type thermoelectric conversion.
  • the layer 16n-n type thermoelectric conversion layer 16n-second substrate 12B (second layer) -second substrate 12B (second layer) "pattern is repeatedly formed.
  • thermoelectric conversion module 10 of the present invention is “p-type thermoelectric conversion layer 14p of the second module 10B—p-type thermoelectric conversion layer 14p of the first module 10A—first substrate 12A—first substrate 12A— The pattern of the n-type thermoelectric conversion layer 16n of the first module 10A—the n-type thermoelectric conversion layer 16n of the second module 10B—the second substrate 12B—the second substrate 12B ”is repeated.
  • thermoelectric conversion module 10 of the present invention is such that the p-type thermoelectric conversion layers 14p face each other with the first substrate 12A and the second substrate 12B on the outside, and The first module 10A and the second module 10B are stacked with the n-type thermoelectric conversion layers 16n facing each other. Therefore, it is possible to prevent a short circuit between the thermoelectric conversion layer and the connection electrode 18 when the bellows is compressed and closed in the longitudinal direction without providing an insulating member such as an insulating sheet and an insulating layer separately. In addition, the utilization efficiency of the substrate can be improved.
  • thermoelectric conversion module since it is basically composed of only the first module 10A and the second module 10B folded back in a bellows shape, that is, it is possible to realize an efficient thermoelectric conversion module without any extra members that do not contribute to power generation. Moreover, since the outer side is the first substrate 12A and the second substrate 12B, this acts as a protective member, so that the p-type thermoelectric conversion layer 14p, the n-type thermoelectric conversion layer 16n, and the connection electrode 18 can be prevented from being damaged. Further, since the first module 10A and the second module 10B can be in a state where the thermoelectric conversion materials or the connection electrodes are in contact with each other, even if a disconnection or the like occurs in one module, electricity can flow through the other. Therefore, disconnection failure and the like can be greatly reduced.
  • thermoelectric conversion module 10 is formed using the flexible first substrate 12A and the second substrate 12B, it has good flexibility. Therefore, it can be bent in the longitudinal direction, and can be attached to a heat source of various shapes, for example, attached to a tubular heat source in a curved state.
  • thermoelectric conversion layer and the like can be formed by printing or the like using roll-to-roll, productivity is also good.
  • thermoelectric conversion module 10 shown in FIGS. 1 to 3 uses the two layers as the first layer and the second layer of the present invention, the present invention is not limited to this. As an example, the configuration shown in FIG. 5 is illustrated.
  • this configuration is the same as the first module 10A and the second module 10B in the width direction (direction perpendicular to the bellows-like fold) on one substrate 20.
  • An array of conversion layer 14p, connection electrode 18, and n-type thermoelectric conversion layer 16n is formed.
  • the middle of the arrangement of the p-type thermoelectric conversion layer 14p, the connection electrode 18 and the n-type thermoelectric conversion layer 16n (dashed line) is a fold line, and the thermoelectric conversion layer forming surface faces inward.
  • the substrate 20 is bent.
  • one substrate 20 becomes the first layer 20A on the upper side in the drawing and the second layer 20B on the lower side in the drawing.
  • thermoelectric conversion module 24 has the same configuration as that of the thermoelectric conversion module 10 shown in FIGS. 1 to 3 except that it includes a single substrate 20.
  • the substrate 20 can use various kinds of flexible and insulating sheet-like materials similar to the first substrate 12A described above.
  • thermoelectric conversion module 10 thermoelectric conversion module 24 of the present invention penetrates through the through-holes 28 formed in the first substrate 12A and the second substrate 12B, thereby providing flexibility. You may have the wire (linear member) 26 to have.
  • the first module 10A and the second module 10B can be prevented from dissociating. That is, by having such a wire 26, the first layer 20A and the second layer 20B can be prevented from being unnecessarily separated. Further, since not only the thermoelectric conversion module 10 but also the wire 26 has flexibility, it can be bent in the longitudinal direction. For example, it can be bent in a curved shape and attached to a tubular heat source. It is possible to attach to a heat source of any shape.
  • the bellows can be easily closed by pressing in the longitudinal direction, and the degree of compression by the pressed state, that is, the interval between the irregularities of the bellows
  • the (bellows interval) can also be easily changed in whole or in part. Therefore, by having the wire 26, the thermoelectric conversion module can be mounted with good workability even when mounted on a heat source having various shapes such as a curved surface or a refracted surface by being handled easily. Is obtained.
  • the wire 26 can be a variety of flexible linear members. Specifically, metal wires such as threads (strings) and wires, metal wires coated with an insulating material, and the like are exemplified.
  • the insertion position of the wire 26 in the first substrate 12A and the second substrate 12B that is, the position of the through hole 28 through which the wire 26 is inserted is not particularly limited.
  • the position of the through hole 28 is other than the formation part of the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n.
  • the portion other than the portion where the connection electrode 18 is formed it can prevent that the area of a thermoelectric conversion layer or an electrode reduces, and the intensity
  • the insertion position of the wire 26, that is, the through hole 28 through which the wire 26 is inserted is conceptually shown in FIG. 7, outside the connection electrode 18 in the width direction and the same as the connection electrode 18 in the longitudinal direction.
  • the position is preferred. That is, the width direction is the longitudinal direction of the ridge line in the bellows-like folding.
  • the longitudinal direction is a bellows-like folding direction.
  • connection electrode 18 when the bellows is closed by inserting the wire 26 outside the connection electrode 18 in the width direction and at the same position as the connection electrode 18 in the longitudinal direction as in the illustrated example, it is usually formed of a metal material.
  • the connecting electrode 18 can be brought into close contact with each other, and the temperature unevenness of the thermoelectric conversion layer in the width direction and the longitudinal direction can be reduced, so that efficient power generation can be performed.
  • the through hole 28 through which the wire 26 is inserted is preferably formed at a position that is linear in the longitudinal direction when the first substrate 12A and the second substrate 12B are folded back in a bellows shape. That is, the through hole 28 is preferably formed at a position where a single straight line elongated in the longitudinal direction can be inserted when the first substrate 12A is folded in a bellows shape. Furthermore, the through hole 28 is a position where the through hole 28 of the first substrate 12A and the through hole 28 of the second substrate 12B are linear in the longitudinal direction when the first module 10A and the second module 10B are stacked. It is preferable to form it.
  • symbol 28a is a reinforcement member for reinforcing the through-hole 28 provided as needed.
  • the reinforcing member 28a may be formed using a known hole reinforcing member such as a metal or a resin material.
  • the first substrate 12 ⁇ / b> A and the second substrate 12 ⁇ / b> B have the mountain fold and the valley fold reversed at the position where the through hole 28 is formed.
  • thermoelectric conversion module 10 thermoelectric conversion module 24 of the present invention may have a heat conducting member such as a heat radiating fin.
  • the heat conductive member may be a plate-like heat conductive member 32 as conceptually shown in FIG. 8, or may be a bellows-like heat conductive member 36 as conceptually shown in FIG. Alternatively, the plate-like heat conducting member 32 and the bellows-like heat conducting member 36 may be used in combination.
  • the material for forming the heat conducting member 32 and the heat conducting member 36 various materials used for so-called heat radiating fins can be used. Specific examples include various metal materials such as copper and aluminum, inorganic compounds such as alumina, boron nitride, and aluminum nitride, and carbon materials such as graphite. Among these, metal materials such as copper and aluminum are preferably used.
  • the bellows-like heat conductive member 36 may be manufactured by a known sheet-like material bending process such as a press process or a process using a roll using protrusions.
  • the heat conducting member 32 and the heat conducting member 36 may be provided on the heat radiating side, may be provided on the high temperature heat source side, or may be provided on both the heat radiating side and the high temperature heat conducting side.
  • both the plate-like heat conducting member 32 and the bellows-like heat conducting member 36 are disposed between the first substrate 12A and the first substrate 12A and / or the first substrate 12A. It is preferable to insert between the two substrates 12B and the second substrate 12B.
  • both the plate-like heat conducting member 32 and / or the bellows-like heat conducting member 36 be provided at a position facing the connection electrode 18 in the longitudinal direction (the bellows-like folding direction).
  • thermoelectric conversion module 10 and the heat conducting member are provided by inserting the heat conducting member between the first substrate 12A and the first substrate 12A and / or between the second substrate 12B and the second substrate 12B. It is possible to improve the efficiency of heat conduction (heat exchange) between the heat source and the heat utilization efficiency and heat dissipation efficiency from the heat source. Furthermore, as described above, since the connection electrode 18 is usually metallic, by providing the heat conducting member facing the connection electrode 18 in the longitudinal direction, the heat conduction efficiency can be greatly improved, and the heat source can be separated from the heat source. The heat utilization efficiency and heat dissipation efficiency can be greatly improved.
  • the connection electrode 18 includes the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n in both the first module 10A and the second module 10B (first layer and second layer). Connected.
  • the present invention is not limited to this, and is not the connection electrode 18 that connects the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n in any one of the first module 10A and the second module 10B.
  • the electrode pair sandwiching the p-type thermoelectric conversion layer 14p and the electrode pair sandwiching the n-type thermoelectric conversion layer 16n may be used.
  • the second module 10Ba does not have a connection electrode that connects the p-type thermoelectric conversion layer 14p and the n-type thermoelectric conversion layer 16n, and the longitudinal direction (accordion-like shape) It may be configured to have an electrode 38 constituting an electrode pair sandwiching the p-type thermoelectric conversion layer 14p in the folding direction and an electrode 38 constituting an electrode pair sandwiching the n-type thermoelectric conversion layer 16n in the longitudinal direction. .
  • the connection electrode 18 of the first module 10A and the second module 10Ba can be electrically connected by contacting the electrodes 38 constituting the electrode pair.
  • thermoelectric conversion modules of the present invention the p-type thermoelectric conversion layers 14p, the n-type thermoelectric conversion layers 16n, and the connection electrodes 18 that face each other are in contact with each other.
  • the present invention is not limited to this, and various configurations can be used.
  • at least one set of the facing p-type thermoelectric conversion layers 14p, the n-type thermoelectric conversion layers 16n, and the connection electrodes 18 may be completely separated, Or you may contact partially.
  • thermoelectric conversion module of the present invention has a configuration in which the p-type thermoelectric conversion layers 14p facing each other and the n-type thermoelectric conversion layers 16n are in contact with each other and the connection electrodes 18 facing each other are separated from each other, or the n-type thermoelectric conversion facing each other.
  • the layers 16n are in contact with each other, and the facing p-type thermoelectric conversion layers 14p and the connection electrodes 18 are separated from each other, or the facing p-type thermoelectric conversion layers 14p are in contact with each other and the facing n-type thermoelectric conversion layers 16n are in contact with each other.
  • the connection electrodes 18 may be separated from each other.
  • thermoelectric conversion module of the present invention has been described above.
  • the present invention is not limited to the above-described example, and various modifications and changes may be made without departing from the scope of the present invention. It is.
  • thermoelectric conversion module 10A first module 10B, 10Ba second module 12A first substrate 12B second substrate 14p p-type thermoelectric conversion layer 16n n-type thermoelectric conversion layer 18 connection electrode 20 substrate 20A first layer 20B second Layer 26 Wire 28 Through-hole 28a Reinforcing member 32, 36 Heat conducting member 38 Electrode

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Abstract

La présente invention aborde le problème de fournir un module de conversion thermoélectrique de type soufflet qui peut être replié comme un soufflet, sans devoir être combiné à un élément d'isolation, tout en empêchant un court-circuit. La présente invention résolvant ce problème comprend : une première couche en forme de soufflet ; une couche de conversion thermoélectrique de type p et une couche de conversion thermoélectrique de type n qui sont agencées en alternance à intervalles dans la direction de pliage de la première couche ; et une paire d'électrodes qui prend en sandwich les couches de conversion thermoélectrique. La présente invention comprend également : une deuxième couche en forme de soufflet ; une couche de conversion thermoélectrique de type p et une couche de conversion thermoélectrique de type n qui sont agencées en alternance à intervalles dans la direction de pliage de la deuxième couche ; et une paire d'électrodes qui prend en sandwich les couches de conversion thermoélectrique. Les couches de conversion thermoélectrique de la première couche ou de la deuxième couche sont connectées électriquement, et un motif « couche de conversion thermoélectrique de type p - couche de conversion thermoélectrique de type p - première couche - première couche - couche de conversion thermoélectrique de type n - couche de conversion thermoélectrique de type n - deuxième couche - deuxième couche » est répété.
PCT/JP2017/019352 2016-05-31 2017-05-24 Module de conversion thermoélectrique WO2017208929A1 (fr)

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JP2020140985A (ja) * 2019-02-26 2020-09-03 日本ゼオン株式会社 熱電変換モジュール
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