WO2019146990A1 - 열전소자 및 그의 제조 방법 - Google Patents

열전소자 및 그의 제조 방법 Download PDF

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Publication number
WO2019146990A1
WO2019146990A1 PCT/KR2019/000893 KR2019000893W WO2019146990A1 WO 2019146990 A1 WO2019146990 A1 WO 2019146990A1 KR 2019000893 W KR2019000893 W KR 2019000893W WO 2019146990 A1 WO2019146990 A1 WO 2019146990A1
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WIPO (PCT)
Prior art keywords
resin layer
metal substrate
region
disposed
inorganic filler
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Ceased
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PCT/KR2019/000893
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English (en)
French (fr)
Korean (ko)
Inventor
노명래
이종민
조용상
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LG Innotek Co Ltd
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LG Innotek Co Ltd
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Application filed by LG Innotek Co Ltd filed Critical LG Innotek Co Ltd
Priority to US16/962,606 priority Critical patent/US11417816B2/en
Priority to EP19743973.0A priority patent/EP3745479B1/en
Priority to CN201980009569.5A priority patent/CN111630671B/zh
Priority to JP2020540286A priority patent/JP7344882B2/ja
Priority to CN202410510951.7A priority patent/CN118434250A/zh
Publication of WO2019146990A1 publication Critical patent/WO2019146990A1/ko
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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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
    • H10N10/81—Structural details of the junction
    • 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
    • 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
    • H10N10/01—Manufacture or treatment
    • 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
    • H10N10/13—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 heat-exchanging means at the junction
    • 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
    • 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
    • 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
    • H10N10/856—Thermoelectric active materials comprising organic compositions

Definitions

  • thermoelectric element and more particularly, to a thermoelectric element junction structure.
  • Thermoelectric phenomenon is a phenomenon caused by the movement of electrons and holes inside a material, which means direct energy conversion between heat and electricity.
  • Thermoelectric elements are collectively referred to as elements utilizing thermoelectric phenomenon and have a structure in which a p-type thermoelectric material and an n-type thermoelectric material are bonded between metal electrodes to form a PN junction pair.
  • thermoelectric element can be classified into a device using a temperature change of electrical resistance, a device using a Seebeck effect that generates electromotive force by a temperature difference, a device using a Peltier effect that is a phenomenon in which heat is generated by heat or a heat is generated .
  • thermoelectric devices are widely applied to household appliances, electronic components, and communication components.
  • a thermoelectric element can be applied to a cooling device, a heating device, a power generation device, and the like.
  • thermoelectric performance of thermoelectric elements there is a growing demand for thermoelectric performance of thermoelectric elements.
  • thermoelectric element includes a substrate, an electrode, and a thermoelectric leg, wherein a plurality of thermoelectric legs are arranged in an array between the upper substrate and the lower substrate, a plurality of upper electrodes are disposed between the plurality of thermoelectrons and the upper substrate, A plurality of lower electrodes are disposed between the thermoelectric leg and the lower substrate.
  • thermoelectric element can be placed on a metal support.
  • the upper substrate and the lower substrate included in the thermoelectric element are ceramic substrates, heat loss may occur due to thermal resistance at the interface between the thermoelectric elements and the metal support.
  • the present invention provides a bonding structure of a thermoelectric element.
  • thermoelectric device includes a first metal substrate, a first resin layer disposed on the first metal substrate and in direct contact with the first metal substrate, a plurality of A plurality of P-type thermoelectric legs and a plurality of N-type thermoelectric legs disposed on the plurality of first electrodes, a plurality of P-type thermoelectric legs arranged on the plurality of P- And a second metal substrate disposed on the second resin layer, wherein the first metal layer and the second metal layer are disposed on the first metal layer, Wherein the surface comprises a first region and a second region disposed within the first region, wherein a surface roughness of the second region is greater than a surface roughness of the first region, .
  • the first resin layer comprises an epoxy resin and an inorganic filler
  • the inorganic filler comprises a first inorganic filler and a second inorganic filler
  • the particle size D50 of the first inorganic filler is a particle size of the second inorganic filler D50.
  • the surface roughness of the second region may be greater than a particle size D50 of the first inorganic filler and less than a particle size D50 of the second inorganic filler.
  • the surface roughness of the second region may be 1.05 to 1.5 times the particle size D50 of the first inorganic filler.
  • the surface roughness of the second region may be 0.04 to 0.15 times the particle size D50 of the second inorganic filler.
  • the second inorganic filler may have a surface roughness of 10 to 50 ⁇ ⁇ , a particle size D50 of the first inorganic filler of 10 to 30 ⁇ ⁇ , and a particle size D50 of the second inorganic filler of 250 to 350 ⁇ ⁇ .
  • the first resin layer comprises an epoxy resin and an inorganic filler and the content of the epoxy resin and the inorganic filler in the groove formed by the surface roughness of the second region is between the first metal substrate and the plurality of first electrodes
  • the content of the epoxy resin and the inorganic filler may be different from each other.
  • a part of the epoxy resin and a part of the first inorganic filler may be disposed in at least a part of the groove formed by the surface roughness of the second region.
  • a surface of the first metal substrate facing the first resin layer further includes a third region disposed inside the second region, and the first resin layer includes a portion of the second region, And the surface roughness of the second region may be larger than the surface roughness of the third region.
  • an adhesive layer disposed between the first metal substrate and the first resin layer, wherein a portion of the adhesive layer may be disposed on at least a part of the groove corresponding to the surface roughness of the second region.
  • thermoelectric device includes a first metal substrate, a first resin layer disposed on the first metal substrate, a plurality of first electrodes disposed on the first resin layer, A plurality of P-type thermoelectric legs and a plurality of N-type thermoelectric legs disposed on the electrode, a plurality of second electrodes disposed on the plurality of P-type thermoelectric legs and the plurality of N-type thermoelectric legs, A second metal substrate disposed on the second resin layer, and a sealing portion disposed between the first metal substrate and the second metal substrate, wherein the first resin layer, the second resin layer, Wherein the surface of the first metal substrate includes a first region and a second region disposed within the first region, wherein the sealing portion is disposed on the first region, Area.
  • the sealing part may include a sealing case disposed at a predetermined distance from a side surface of the first resin layer and a side surface of the second resin layer, and a sealing material disposed between the sealing case and the first area.
  • the width of the first metal substrate may be greater than the width of the second metal substrate.
  • the first metal substrate emits heat, and the second metal substrate can absorb heat.
  • the thickness of the first metal substrate may be less than the thickness of the second metal substrate.
  • the first resin layer may be spaced a predetermined distance from the boundary between the first region and the second region.
  • the first resin layer may be formed to be in direct contact with the first metal substrate.
  • thermoelectric device includes a first metal substrate, a first resin layer disposed on the first metal substrate, a plurality of first electrodes disposed on the first resin layer, A plurality of P-type thermoelectric legs and a plurality of N-type thermoelectric legs disposed on one electrode, a plurality of second electrodes disposed on the plurality of P-type thermoelectric legs and the plurality of N-type thermoelectric legs, And a second metal substrate disposed on the second resin layer, wherein the first resin layer comprises an epoxy resin composition comprising an epoxy resin and an inorganic filler, The filler comprises at least one of aluminum oxide and nitride, and the inorganic filler is contained in an amount of 68 to 88 vol% of the epoxy resin composition.
  • the nitride may be included in an amount of 55 to 95 wt% of the inorganic filler.
  • the nitride may comprise at least one of boron nitride and aluminum nitride.
  • the boron nitride may be a boron nitride aggregate in which plate-shaped boron nitride is aggregated.
  • the inorganic filler may include aluminum oxide having a particle size D50 of 10 to 30 ⁇ ⁇ and boron nitride aggregates having a particle size D50 of 250 to 350 ⁇ ⁇ .
  • the first resin layer may be formed to be in direct contact with the first metal substrate.
  • a method of manufacturing a thermoelectric device includes the steps of bonding a resin layer and a metal layer, etching the metal layer to form a plurality of electrodes, forming a first region, Forming a surface roughness in the second region in one surface of the metal substrate including the first region and the second region; arranging the second region of the metal substrate and the resin layer so as to be in contact with each other; And thermocompression bonding.
  • the method may further include disposing an adhesive layer in an uncured state between the metal substrate and the resin layer before arranging the resin layer and the second region of the metal substrate in contact with each other.
  • the step of disposing the adhesive layer comprises the steps of applying the adhesive layer in an uncured state on the release film, disposing the resin layer on the adhesive layer, compressing the resin layer and the adhesive layer, Removing the release film, and disposing a surface on which the release film has been removed, on a second area of the metal substrate.
  • the resin layer may include an epoxy resin composition
  • the adhesive layer may include the same epoxy resin composition as the epoxy resin composition contained in the resin layer.
  • thermoelectric device includes a first resin layer, a plurality of first electrodes disposed on the first resin layer, a plurality of P-type thermoelectric legs disposed on the plurality of first electrodes, and a plurality of A plurality of second electrodes disposed on the plurality of P-type thermoelectric legs and the plurality of N-type thermoelectric legs, and a second resin layer disposed on the plurality of second electrodes, At least one of the plurality of first electrodes includes a first surface facing the first resin layer, a second surface facing the pair of P-type thermoelectric legs and the N-type thermoelectric leg, and a width of the first surface And the length is different from the width length of the second surface.
  • the width of the second surface may be 0.8 to 0.95 times the width of the first surface.
  • the side surface between the first surface and the second surface may include a curved surface having a predetermined curvature.
  • thermoelectric device having excellent thermal conductivity, low heat loss, and high reliability.
  • thermoelectric element according to the embodiment of the present invention has high bonding strength with the metal support, and the manufacturing process is simple.
  • thermoelectric device 1 is a cross-sectional view of a thermoelectric device according to an embodiment of the present invention.
  • thermoelectric device 2 is a top view of a metal substrate included in a thermoelectric device according to an embodiment of the present invention.
  • thermoelectric device 3 is a cross-sectional view of a thermoelectric device on a metal substrate side according to an embodiment of the present invention.
  • FIG. 4 is an enlarged view of one area of Fig.
  • thermoelectric device 7 is a top view of a metal substrate included in a thermoelectric device according to another embodiment of the present invention.
  • thermoelectric element 8 is a cross-sectional view of the thermoelectric element including the metal substrate of Fig. 7 on the metal substrate side.
  • thermoelectric device 9 is a cross-sectional view of a thermoelectric device according to another embodiment of the present invention.
  • thermoelectric device 10 is a perspective view of the thermoelectric device according to Fig.
  • thermoelectric device 11 is an exploded perspective view of the thermoelectric device according to Fig.
  • thermoelectric device 12 to 13 show a method of manufacturing a thermoelectric device according to an embodiment of the present invention.
  • FIG. 14 is a diagram illustrating an example in which a thermoelectric element according to an embodiment of the present invention is applied to a water purifier.
  • FIG. 15 is a view illustrating an example in which a thermoelectric element according to an embodiment of the present invention is applied to a refrigerator.
  • the terms including ordinal, such as second, first, etc. may be used to describe various elements, but the elements are not limited to these terms. The terms are used only for the purpose of distinguishing one component from another.
  • the second component may be referred to as a first component, and similarly, the first component may also be referred to as a second component.
  • / or < / RTI &gt includes any combination of a plurality of related listed items or any of a plurality of related listed items.
  • FIG. 2 is a top view of a metal substrate included in a thermoelectric device according to an embodiment of the present invention.
  • FIG. 3 is a cross-sectional view of a thermoelectric device according to an embodiment of the present invention.
  • Fig. 4 is an enlarged view of one region of Fig. 3, and Figs. 5 to 6 are enlarged views of another region of Fig.
  • thermoelectric element 100 includes a first resin layer 110, a plurality of first electrodes 120, a plurality of P-type thermoelectric legs 130, a plurality of N-type thermoelectric legs 140, The second electrode 150 and the second resin layer 160 of FIG.
  • the plurality of first electrodes 120 are disposed between the first resin layer 110 and the lower surfaces of the plurality of P-type thermoelectric legs 130 and the plurality of N-type thermoelectric legs 140, Are disposed between the second resin layer 160 and the upper surfaces of the plurality of P-type thermoelectric legs 130 and the plurality of N-type thermoelectric legs 140. Accordingly, the plurality of P-type thermoelectric legs 130 and the plurality of N-type thermoelectric legs 140 are electrically connected by the plurality of first electrodes 120 and the plurality of second electrodes 150. A pair of the P-type thermoelectric legs 130 and the N-type thermoelectric legs 140, which are disposed between the first electrode 120 and the second electrode 150 and are electrically connected to each other, may form a unit cell.
  • a pair of P-type thermoelectric legs 130 and N-type thermoelectric legs 140 may be disposed on each of the first electrodes 120 and disposed on each of the first electrodes 120 on the second electrodes 150
  • a pair of N-type thermoelectric legs 140 and a pair of P-type thermoelectric legs 130 may be disposed so that one of a pair of P-type thermoelectric legs 130 and N-type thermoelectric legs 140 overlaps.
  • the P-type thermoelectric leg 130 and the N-type thermoelectric leg 140 may be bismuth telluride (Bi-Te) thermoelectric legs containing bismuth (Bi) and tellurium (Te) as main raw materials.
  • the P-type thermoelectric leg 130 is formed of a material selected from the group consisting of antimony (Sb), nickel (Ni), aluminum (Al), copper (Cu), silver (Ag), lead (Pb), boron 99 to 99.999 wt% of a bismuth telluride (Bi-Te) based raw material containing at least one of gallium (Ga), tellurium (Te), bismuth (Bi) and indium (In) and 0.001 Lt; / RTI > to 1 wt%.
  • the base material may be Bi-Se-Te, and may further contain Bi or Te in an amount of 0.001 to 1 wt% of the total weight.
  • the N-type thermoelectric leg 140 is made of selenium (Se), nickel (Ni), aluminum (Al), copper (Cu), silver (Ag), lead (Pb), boron (B) 99 to 99.999 wt% of a bismuth telluride (Bi-Te) based raw material containing at least one of gallium (Ga), tellurium (Te), bismuth (Bi) and indium (In) and 0.001 Lt; / RTI > to 1 wt%.
  • the base material may be Bi-Sb-Te and may further contain Bi or Te in an amount of 0.001 to 1 wt% of the total weight.
  • the P-type thermoelectric leg 130 and the N-type thermoelectric leg 140 may be formed in a bulk or laminated form.
  • the bulk type P-type thermoelectric leg 130 or the bulk N-type thermoelectric leg 140 is manufactured by heat-treating the thermoelectric material to produce an ingot, pulverizing and sieving the ingot to obtain a thermoelectric leg powder, Sintered body, and cutting the sintered body.
  • the laminated P-type thermoelectric leg 130 or the laminated N-type thermoelectric leg 140 is formed by applying a paste containing a thermoelectric material on a sheet-shaped substrate to form a unit member, then stacking and cutting the unit member Can be obtained.
  • the pair of the P-type thermoelectric legs 130 and the N-type thermoelectric legs 140 may have the same shape and volume, or may have different shapes and volumes. Since the electrical conduction characteristics of the P-type thermoelectric leg 130 and the N-type thermoelectric leg 140 are different from each other, the height or the cross-sectional area of the N-type thermoelectric leg 140 may be set to a height or a cross- May be formed differently.
  • thermoelectric device The performance of a thermoelectric device according to an embodiment of the present invention can be represented by a Gebeck index.
  • the whiteness index (ZT) can be expressed by Equation (1).
  • ⁇ is the Seebeck coefficient [V / K]
  • ⁇ is the electric conductivity [S / m]
  • ⁇ 2 ⁇ is the power factor (W / mK 2 ).
  • T is the temperature
  • k is the thermal conductivity [W / mK].
  • k is a ⁇ c p ⁇ ⁇ where a is the thermal diffusivity [cm 2 / S], c p is the specific heat [J / gK], and ⁇ is the density [g / cm 3 ].
  • the Z value (V / K) is measured using a Z meter, and the Zebek index (ZT) can be calculated using the measured Z value.
  • the plurality of second electrodes 150 disposed between the legs 130 and the N-type thermoelectric legs 140 may include at least one of copper (Cu), silver (Ag), and nickel (Ni).
  • the sizes of the first resin layer 110 and the second resin layer 160 may be different.
  • the volume, thickness, or area of one of the first resin layer 110 and the second resin layer 160 may be formed larger than the other volume, thickness, or area.
  • the heat absorption performance or the heat radiation performance of the thermoelectric element can be enhanced.
  • the P-type thermoelectric leg 130 or the N-type thermoelectric leg 140 may have a cylindrical shape, a polygonal columnar shape, an elliptical columnar shape, or the like.
  • the P-type thermoelectric leg 130 or the N-type thermoelectric leg 140 may have a laminated structure.
  • the P-type thermoelectric leg or the N-type thermoelectric leg may be formed by stacking a plurality of structures coated with a semiconductor material on a sheet-like base material and then cutting the same. Thus, it is possible to prevent the loss of the material and improve the electric conduction characteristic.
  • the P-type thermoelectric leg 130 or the N-type thermoelectric leg 140 may be manufactured according to a zone melting method or a powder sintering method.
  • a zone melting method an ingot is produced using a thermoelectric material, refined to heat the ingot slowly in a single direction, and slowly cooled to obtain a thermoelectric leg.
  • a powder sintering method an ingot is produced using a thermoelectric material, and then the ingot is pulverized and sieved to obtain a thermoelectric material powder, and the thermoelectric material is obtained by sintering the thermoelectric material.
  • the first resin layer 110 may be disposed on the first metal substrate 170 and the second metal substrate 180 may be disposed on the second resin layer 160.
  • the first metal substrate 170 and the second metal substrate 180 may be made of aluminum, an aluminum alloy, copper, a copper alloy, or the like.
  • the first metal substrate 170 and the second metal substrate 180 are formed of a first resin layer 110, a plurality of first electrodes 120, a plurality of P-type thermoelectric legs 130, and a plurality of N-type thermoelectric legs 140, a plurality of second electrodes 150, a second resin layer 160, and the like, and may be a region directly attached to an application to which the thermoelectric element 100 according to the embodiment of the present invention is applied . Accordingly, the first metal substrate 170 and the second metal substrate 180 can be mixed with the first metal substrate and the second metal substrate, respectively.
  • the area of the first metal substrate 170 may be larger than the area of the first resin layer 110 and the area of the second metal substrate 180 may be larger than the area of the second resin layer 160. That is, the first resin layer 110 may be disposed in a region spaced a predetermined distance from the edge of the first metal substrate 170, and the second resin layer 160 may be disposed in a region separated from the edge of the second metal substrate 180 And can be disposed in an area spaced apart by a predetermined distance.
  • the width of the first metal substrate 170 may be greater than the width of the second metal substrate 180, or the thickness of the first metal substrate 170 may be greater than the thickness of the second metal substrate 180 .
  • the first metal substrate 170 may be a heat dissipating unit that dissipates heat and the second metal substrate 180 may be a heat absorbing unit that absorbs heat.
  • the first resin layer 110 and the second resin layer 160 may be made of an epoxy resin composition including an epoxy resin and an inorganic filler.
  • the inorganic filler may be contained in an amount of 68 to 88 vol% of the epoxy resin composition. If the inorganic filler is contained in an amount less than 68 vol%, the heat conduction effect may be low. If the inorganic filler is contained in an amount exceeding 88 vol%, the adhesion between the resin layer and the metal substrate may be lowered and the resin layer may break easily.
  • the thickness of the first resin layer 110 and the second resin layer 160 may be 0.02 to 0.6 mm, preferably 0.1 to 0.6 mm, more preferably 0.2 to 0.6 mm, and the thermal conductivity may be 1 W / mK or more , Preferably 10 W / mK or more, and more preferably 20 W / mK or more. If the thicknesses of the first resin layer 110 and the second resin layer 160 satisfy these numerical ranges, the first resin layer 110 and the second resin layer 160 repeatedly shrink and expand according to the temperature change The bonding between the first resin layer 110 and the first metal substrate 170 and the bonding between the second resin layer 160 and the second metal substrate 180 may not be affected.
  • the epoxy resin may include an epoxy compound and a curing agent.
  • the curing agent may be contained in a ratio of 1 to 10 parts by volume of the epoxy compound 10 parts by volume.
  • the epoxy compound may include at least one of a crystalline epoxy compound, amorphous epoxy compound, and silicone epoxy compound.
  • the crystalline epoxy compound may include a mesogen structure. Mesogen is a basic unit of liquid crystal and includes a rigid structure.
  • the amorphous epoxy compound may be a conventional amorphous epoxy compound having two or more epoxy groups in the molecule, for example, a glycidyl ether compound derived from bisphenol A or bisphenol F.
  • the curing agent may include at least one of an amine curing agent, a phenol curing agent, an acid anhydride curing agent, a polymercaptan curing agent, a polyaminoamide curing agent, an isocyanate curing agent and a block isocyanate curing agent, May be mixed and used.
  • the inorganic filler may comprise aluminum oxide and nitride, and the nitride may be comprised between 55 and 95 wt% of the inorganic filler, and more preferably between 60 and 80 wt%.
  • the thermal conductivity And the bonding strength can be increased.
  • the nitride may include at least one of boron nitride and aluminum nitride.
  • the surface of the aggregate of boron nitride may be coated with a polymer having the following unit 1, or at least a part of the voids in the aggregate of boron nitride may be coated on a polymer having the following unit 1 .
  • Unit 1 is as follows.
  • R 1 , R 2 , R 3 and R 4 is H and the remainder is selected from the group consisting of C 1 -C 3 alkyl, C 2 -C 3 alkene and C 2 -C 3 alkyne
  • R 5 May be a linear, branched, or cyclic divalent organic linker having 1 to 12 carbon atoms.
  • one of R 1 , R 2 , R 3 and R 4 , except H, is selected from C 2 -C 3 alkenes, the other and the other is selected from C 1 -C 3 alkyl Can be selected.
  • the polymer according to an embodiment of the present invention may include the following monomer unit 2:
  • the remainder of the R 1 , R 2 , R 3 and R 4 may be selected to be different from each other in the group consisting of C 1 -C 3 alkyl, C 2 -C 3 alkene and C 2 -C 3 alkyne have.
  • the air layer in the aggregate of the boron nitride is minimized, The heat conduction performance can be enhanced and cracking of the boron nitride aggregate can be prevented by increasing the bonding force between the plate-like boron nitride.
  • the coating layer is formed on the boron nitride aggregate in which the plate-shaped boron nitride is aggregated, functional groups are easily formed, and when a functional group is formed on the coating layer of the boron nitride aggregate, the affinity with the resin can be increased.
  • the particle size D50 of the boron nitride aggregate may be 250 to 350 mu m, and the particle size D50 of aluminum oxide may be 10 to 30 mu m.
  • the particle size D50 of the aggregate of boron nitride and the particle size D50 of the aluminum oxide satisfy these numerical ranges, the boron nitride agglomerate and the aluminum oxide may be uniformly dispersed in the epoxy resin composition, whereby the uniform heat conduction effect and adhesion performance Lt; / RTI >
  • the first resin layer 110 when the first resin layer 110 is disposed between the first metal substrate 170 and the plurality of first electrodes 120, the first metal substrate 170 and the plurality of first electrodes 120, The first resin layer 110 can be thermally transferred between the first resin layer 110 and the second resin layer 120, and no adhesive or physical fastening means are required due to the adhesive property of the first resin layer 110 itself. Accordingly, the overall size of the thermoelectric element 100 can be reduced.
  • the first metal substrate 170 may be in direct contact with the first resin layer 110.
  • the surface of the first metal substrate 170 on which the first resin layer 110 is disposed that is, the surface of the first metal substrate 170 facing the first resin layer 110, has a surface roughness . Accordingly, the first resin layer 110 can be prevented from being floated during thermal compression between the first metal substrate 170 and the first resin layer 110.
  • the surface roughness means irregularities and may be mixed with the surface roughness.
  • the first region 172 may include a first region 172 and the second region 174 and the second region 174 may be disposed within the first region 172. That is, the first region 172 may be disposed within a predetermined distance from the edge of the first metal substrate 170 toward the center region, and the first region 172 may surround the second region 174.
  • the surface roughness of the second region 174 is larger than the surface roughness of the first region 172, and the first resin layer 110 can be disposed on the second region 174.
  • the first resin layer 110 may be disposed to be spaced apart from the boundary between the first region 172 and the second region 174 by a predetermined distance. That is, the first resin layer 110 may be disposed on the second region 174, and the edge of the first resin layer 110 may be located within the second region 174.
  • a portion of the first resin layer 110, that is, the epoxy resin 600 included in the first resin layer 110, and the epoxy resin 600 included in the first resin layer 110 are formed in at least a part of the groove 400 formed by the surface roughness of the second region 174, A part of the inorganic filler 604 can permeate and the adhesion between the first resin layer 110 and the first metal substrate 170 can be increased.
  • the surface roughness of the second region 174 may be formed to be larger than a particle size D50 of a part of inorganic fillers included in the first resin layer 110 and smaller than a particle size D50 of another portion.
  • the particle size D50 means a particle size corresponding to 50% of the weight percentage in the particle size distribution curve, that is, a particle size at which the percentage of the passing mass is 50%, and can be mixed with the average particle size.
  • the aluminum oxide does not affect the adhesion performance between the first resin layer 110 and the first metal substrate 170
  • the boron nitride has a smooth surface, which may adversely affect the bonding performance between the first resin layer 110 and the first metal substrate 170.
  • the surface roughness of the second region 174 is formed to be larger than the particle size D50 of the aluminum oxide included in the first resin layer 110 but smaller than the particle size D50 of the boron nitride, Since only aluminum oxide is disposed in the groove formed by the surface roughness and boron nitride can not be disposed, the first resin layer 110 and the first metal substrate 170 can maintain a high bonding strength.
  • the surface roughness of the second region 174 can be adjusted by the inorganic filler 604 having a relatively small size among the inorganic fillers contained in the first resin layer 110, for example, 1.05 to 1.5 And may be 0.04 to 0.15 times the particle size D50 of the inorganic filler 602 having a relatively large size among inorganic fillers contained in the first resin layer 110, for example, boron nitride.
  • the surface roughness of the second region 174 may be 1 to 50 mu m . Accordingly, only the aluminum oxide is disposed in the groove formed by the surface roughness of the second region 174, and the boron nitride aggregate may not be disposed.
  • the content of the epoxy resin and the inorganic filler in the groove formed by the surface roughness of the second region 174 can be controlled by adjusting the surface roughness of the epoxy resin and the inorganic filler in the middle region between the first metal substrate 170 and the plurality of first electrodes 120. [ The content of the filler may be different.
  • This surface roughness can be measured using a surface roughness meter.
  • the surface roughness meter measures the cross-sectional curve using a probe, and the surface roughness can be calculated using the peak line, the bottom line of the cross-sectional curve, the average line and the reference length.
  • the surface roughness can mean an arithmetic average roughness (Ra) by the center line average calculation method.
  • the arithmetic mean roughness (Ra) can be obtained by the following equation (2).
  • At least one of the plurality of first electrodes 120 includes a first surface 121 disposed to face the first resin layer 110, that is, a first resin layer 110, The first face 121 and the second face 122 disposed toward the opposite face of the first face 121, i.e., a pair of the P-type thermoelectric legs 130 and the N-type thermoelectric leg 140, And a second surface 122 opposed to the pair of P type thermoelectric legs 130 and the N type thermoelectric legs 140.
  • the width W1 of the first surface 121 and the width W2 of the second surface 122 The width W2 may be different.
  • the width W2 of the second surface 122 may be 0.8 to 0.95 times the width W1 of the first surface 121. [ If the width W1 of the first surface 121 is larger than the width W2 of the second surface 122 as described above, the contact area with the first resin layer 110 becomes wider, The bonding strength between the first electrode 110 and the first electrode 120 can be increased.
  • the side surface 123 between the first surface 121 and the second surface 122 may include a curved surface having a predetermined curvature.
  • a round shape having a predetermined curvature may be used. According to this, it is easy to fill the spaces between the plurality of first electrodes 120 with the insulating resin, so that the plurality of first electrodes 120 can be stably supported on the first resin layer 110, Even if the electrodes 120 are arranged at a close distance, the neighboring electrodes may not have an electric influence.
  • the first electrode 120 may be formed of a Cu layer, or may have a structure in which Cu, Ni, and Au are sequentially stacked, or may have a structure in which Cu, Ni, and Sn are sequentially stacked.
  • FIG. 7 is a top view of a metal substrate included in a thermoelectric device according to another embodiment of the present invention
  • FIG. 8 is a cross-sectional view of a thermoelectric device including the metal substrate of FIG. 7 on a metal substrate side. The same contents as those described in Figs. 1 to 6 will not be repeatedly described.
  • the surface of the first metal substrate 170 on which the first resin layer 110 is disposed that is, the surface facing the first resin layer 110 of the first metal substrate 170, Includes a second region (174) surrounded by a first region (172) and a first region (172) and having a greater surface roughness than the first region (172), further comprising a third region can do.
  • the third region 176 may be disposed inside the second region 174. That is, the third region 176 may be arranged to be surrounded by the second region 174.
  • the surface roughness of the second region 174 may be larger than the surface roughness of the third region 176.
  • the first resin layer 110 is spaced apart from the first region 172 by a predetermined distance from the boundary between the first region 172 and the second region 174 and the first resin layer 110 is a portion of the second region 174 and / And may cover the third region 176.
  • An adhesive layer 800 may be further disposed between the first metal substrate 170 and the first resin layer 110 to increase the bonding strength between the first metal substrate 170 and the first resin layer 110.
  • the adhesive layer 800 may be the same epoxy resin composition as the epoxy resin composition constituting the first resin layer 110.
  • the same epoxy resin composition as the epoxy resin composition constituting the first resin layer 110 is applied between the first metal substrate 170 and the first resin layer 110 in an uncured state, The first metal substrate 170 and the first resin layer 110 can be bonded together by laminating the first resin layer 110 of the first resin layer 110 and pressing at a high temperature.
  • a part of the adhesive layer 800 for example, a part of the epoxy resin of the epoxy resin composition constituting the adhesive layer 800 and a part of the inorganic filler may be disposed in at least a part of the groove according to the surface roughness of the second region 174 .
  • FIG. 9 is a cross-sectional view of a thermoelectric transducer according to another embodiment of the present invention
  • FIG. 10 is a perspective view of the thermoelectric transducer according to FIG. 9
  • FIG. 11 is an exploded perspective view of the thermoelectric transducer according to FIG. The same contents as those described in Figs. 1 to 8 will not be duplicated.
  • thermoelectric element 100 according to an embodiment of the present invention includes a sealing portion 190.
  • the sealing portion 190 may be disposed on the side of the first resin layer 110 and the side of the second resin layer 160 on the first metal substrate 170. That is, The plurality of P-type thermoelectric legs 130 and the plurality of N-type thermoelectric legs 140 are disposed at the outermost portion of the plurality of first electrodes 120, the plurality of P-type thermoelectric legs 130, and the plurality of N-type thermoelectric legs 140 disposed between the substrate 170 and the second metal substrate 180 The outermost periphery of the second electrode 150, and the side surface of the second resin layer 160. As shown in FIG.
  • the resin layer may be sealed from external moisture, heat, contamination, and the like.
  • the sealing portion 190 may be disposed on the first region 172.
  • the sealing portion 190 is disposed on the first region 172 having a small surface roughness, the sealing effect between the sealing portion 190 and the first metal substrate 170 can be enhanced.
  • the sealing portions 190 are formed on the side surfaces of the first resin layer 110, the outermost portions of the plurality of first electrodes 120, the plurality of P-type thermoelectric legs 130, and the plurality of N-type thermoelectric legs 140
  • a sealing case 192, a sealing case 192 and a first metal substrate 170 which are disposed at a predetermined distance from the outermost periphery of the plurality of second electrodes 150 and the side surface of the second resin layer 160,
  • a sealing member 194 disposed between the first region 172 of the first metal substrate 180 and a sealing member 196 disposed between the sealing case 192 and the side surfaces of the second metal substrate 180.
  • the sealing case 192 can contact the first metal substrate 170 and the second metal substrate 180 via the sealing members 194 and 196.
  • sealing case 192 when the sealing case 192 is in direct contact with the first metal substrate 170 and the second metal substrate 180, thermal conduction occurs through the sealing case 192, resulting in a problem of lowering ⁇ T .
  • a part of the inner wall of the sealing case 192 is formed to be inclined, and the sealing material 196 is disposed on the side of the second metal substrate 180, (Not shown). Accordingly, the volume between the first metal substrate 170 and the second metal substrate 180 becomes large, and heat exchange becomes active, so that a higher ⁇ T can be obtained.
  • the sealing members 194 and 196 may include at least one of an epoxy resin and a silicone resin, or may include a tape on which at least one of an epoxy resin and a silicone resin is applied on both sides.
  • the sealing members 194 and 196 serve to seal between the sealing case 192 and the first metal substrate 170 and between the sealing case 192 and the second metal substrate 180.
  • the first resin layer 110, The sealing effect of the plurality of first electrodes 120, the plurality of P-type thermoelectric legs 130, the plurality of N-type thermoelectric legs 140, the plurality of second electrodes 150, and the second resin layer 160 is And can be mixed with a finishing material, a finish layer, a waterproofing material, a waterproof layer, and the like.
  • the sealing case 192 may be formed with a guide groove G for drawing the wires 200 and 202 connected to the electrodes.
  • the sealing case 192 may be an injection-molded article made of plastic or the like, and may be mixed with a sealing cover.
  • the first metal substrate 170 may be a heat radiating portion or a heat generating portion for emitting heat
  • the second metal substrate 180 may be a heat absorbing portion or a cooling portion for absorbing heat.
  • the width of the first metal substrate 170 may be greater than the width of the second metal substrate 180 or the thickness of the first metal substrate 170 may be less than the thickness of the second metal substrate 180 have. Accordingly, the first metal substrate 170, which is a heat radiating portion or a heat generating portion, can be realized with a small thermal resistance, and the sealing portion 190 can be stably disposed.
  • the first metal substrate 170 may be formed to be larger than the second metal substrate 180 by an area corresponding to the first region 172 to stably arrange the sealing portion 190.
  • the second metal substrate 180 which is a heat absorbing portion or a cooling portion, can be brought into contact with an object to be contacted with a minimum area, so that heat loss can be minimized.
  • the thickness of the second metal substrate 180 may vary depending on the required heat capacity of the cooling system.
  • FIG. 9-11 The embodiment described in Figures 9-11 is similar to the embodiment of Figures 1-6 in which the first metal substrate 170 includes the first region 172 and the second region 174 as well as the first metal substrate 170 May also be applied to the embodiment of Figures 7 through 8 including the first region 172, the second region 174, and the third region 176.
  • thermoelectric device Accordingly, a method of manufacturing a thermoelectric device according to an embodiment of the present invention will be described with reference to the drawings.
  • thermoelectric device 12 to 13 show a method of manufacturing a thermoelectric device according to an embodiment of the present invention.
  • a metal layer is bonded to a resin layer (S1200), and a plurality of electrodes are formed by etching the metal layer (S1210).
  • a plurality of electrode-shaped masks may be disposed on the metal layer, and then the etchant may be sprayed.
  • the electrode may include at least one of Cu, Ni, Au, and Sn.
  • the electrode may be made of a Cu layer.
  • the electrode may have a structure in which Cu, Ni, and Au are sequentially stacked, or Cu, Ni, and Sn are sequentially stacked.
  • the metal layer bonded on the resin layer in step S 1200 may include a plated Ni layer and Au layer on the Cu layer, or a Ni layer and a Sn layer plated on the Cu layer.
  • the metal layer bonded on the resin layer is a Cu layer, and the Cu layer is etched to form a plurality of electrodes. Then, the Ni layer and the Au layer are sequentially plated on the plurality of electrodes, Can be successively plated.
  • a surface roughness is formed on one of both surfaces of the metal substrate (S1220).
  • Surface roughness can be accomplished by a variety of methods including, but not limited to, sandblasting, sawing, casting, forging, turning, milling, boring, drilling, As described above, the surface roughness can be performed only in a partial area on one side of both surfaces of the metal substrate.
  • the surface roughness may be measured in a region including the edge of the metal substrate, that is, a region other than the first region, such as the embodiment of Figs. 1 to 6, .
  • the surface roughness may be adjusted to some extent including the edge of the metal, i.e., the first region and the middle region of the metal substrate, i.e., the remaining region except for the third region, May be performed in the second area.
  • the metal substrate on which the surface roughness is formed and the resin layer are bonded (S1230).
  • the metal substrate and the resin layer may be thermocompression-bonded after one surface of the surface roughness is formed and the opposite surface of the surface of the resin layer opposite to the surface on which the plurality of electrodes are formed.
  • the method may further include disposing an adhesive layer in an uncured state between the metal substrate and the resin layer before disposing the resin layer and the second region of the metal substrate in contact with each other.
  • a resin layer is applied on a Cu layer, an adhesive layer is applied on the release film, and a surface roughness Respectively.
  • the epoxy resin composition constituting the resin layer and the epoxy resin composition constituting the adhesive layer may be the same epoxy resin composition.
  • a Cu layer for electrode formation is further disposed on the resin layer applied in Fig. 13 (a), and then thermally pressed, the resin layer is cured to form a structure Can be obtained.
  • a plating layer can be formed on a plurality of electrodes as shown in Fig. 13 (g).
  • the adhesive layer applied on the release film is disposed on the opposite side of the surface of the resin layer opposite to the surface on which the plurality of electrodes are formed, and then the release film can be removed. At this time, the adhesive layer may be in a semi-cured state.
  • the surface from which the release film has been removed is placed on the surface of the metal substrate on which the surface roughness is formed, and the metal substrate and the resin layer can be bonded by pressing.
  • a part of the semi-hardened adhesive layer can penetrate into the groove according to the surface roughness on the metal substrate.
  • thermoelectric element according to an embodiment of the present invention is applied to a water purifier
  • thermoelectric device 14 is a block diagram of a water purifier to which a thermoelectric device according to an embodiment of the present invention is applied.
  • a water purifier 1 to which a thermoelectric device according to an embodiment of the present invention is applied includes a raw water supply pipe 12a, a purified water tank inflow pipe 12b, a purified water tank 12, a filter assembly 13, a cooling fan 14, 15, a cold water supply pipe 15a, and a thermoelectric device 1000.
  • the raw water supply pipe 12a is a supply pipe for introducing water to be purified water from the water source into the filter assembly 13 and the purified water tank inflow pipe 12b is a pipe for introducing purified water from the filter assembly 13 into the purified water tank 12
  • the cold water supply pipe 15a is a supply pipe in which cold water cooled at a predetermined temperature by the thermoelectric device 1000 in the purified water tank 12 is finally supplied to the user.
  • the purified water tank 12 is cleaned by passing through the filter assembly 13 and temporarily stores purified water to store and supply the water that has flowed through the purified water tank inflow pipe 12b.
  • the filter assembly 13 is composed of a precipitating filter 13a, a pre-carbon filter 13b, a membrane filter 13c, and a post-carbon filter 13d.
  • the water flowing into the raw water supply pipe 12a can be purified through the filter assembly 13.
  • a heat storage tank 15 is disposed between the water purification tank 12 and the thermoelectric device 1000 to store cool air formed in the thermoelectric device 1000.
  • the cool air stored in the thermal storage tank 15 is applied to the purified water tank 12 to cool the water contained in the purified water tank 120.
  • the thermal storage tank 15 may be in surface contact with the purified water tank 12 so that cold air can be smoothly transmitted.
  • thermoelectric device 1000 has a heat absorbing surface and a heat generating surface, and one side is cooled and the other side is heated by electron movement on the P type semiconductor and the N type semiconductor.
  • one side may be the purified water tank 12 side and the other side may be the opposite side of the purified water tank 12.
  • thermoelectric device 1000 has excellent waterproof and dustproof performance, and the heat flow performance is improved, so that the water tank 12 can be efficiently cooled in the water purifier.
  • thermoelectric element according to an embodiment of the present invention is applied to a refrigerator.
  • thermoelectric device 15 is a block diagram of a refrigerator to which a thermoelectric device according to an embodiment of the present invention is applied.
  • the refrigerator includes a deep-room evaporation chamber cover 23, an evaporation chamber partition wall 24, a main evaporator 25, a cooling fan 26, and a thermoelectric device 1000 in the deep-room evaporation room.
  • the inside of the refrigerator is divided into the deep room storage room and the deep room evaporation room by the deep room evaporation room cover (23).
  • the inner space corresponding to the front of the deep evaporation room cover 23 is defined as a deep room storage room, and the inner space corresponding to the rear of the deep room evaporation room cover 23 can be defined as a deep room evaporation room.
  • a discharge grille 23a and a suction grille 23b may be formed on the front surface of the deep-drawing room seal cover 23, respectively.
  • the evaporation chamber partition wall 24 is provided at a position spaced forward from the rear wall of the inner cabinet to define a space where the core room storage system is placed and a space where the main evaporator 25 is placed.
  • the cool air cooled by the main evaporator 25 is supplied to the freezing chamber and then returned to the main evaporator.
  • thermoelectric device 1000 is accommodated in the deep-room evaporation chamber, and the heat absorbing surface is directed toward the drawer assembly of the deep-room storage compartment and the heat generating surface is directed toward the evaporator. Accordingly, the heat absorption phenomenon occurring in the thermoelectric device 1000 can be used to rapidly cool the food stored in the drawer assembly to a cryogenic temperature of minus 50 degrees Celsius.
  • thermoelectric device 1000 is excellent in waterproof and dustproof performance, and the heat flow performance is improved, so that the drawer assembly can be efficiently cooled in the refrigerator.
  • thermoelectric device can be applied to a power generation device, a cooling device, a thermal device, and the like.
  • the thermoelectric device according to an embodiment of the present invention mainly includes an optical communication module, a sensor, a medical instrument, a measuring instrument, an aerospace industry, a refrigerator, a chiller, a ventilation sheet, a cup holder, a washing machine, , A water purifier, a power supply for a sensor, a thermopile, and the like.
  • thermoelectric element according to the embodiment of the present invention is applied to a medical instrument
  • a PCR (Polymerase Chain Reaction) device there is a PCR (Polymerase Chain Reaction) device.
  • the PCR device is a device for amplifying DNA to determine the DNA sequence and is a device that requires precise temperature control and thermal cycling.
  • a Peltier based thermoelectric element can be applied.
  • thermoelectric element according to an embodiment of the present invention is applied to a medical instrument
  • the photodetector includes an infrared / ultraviolet detector, a CCD (Charge Coupled Device) sensor, an X-ray detector, and a TTRS (Thermoelectric Thermal Reference Source).
  • a Peltier-based thermoelectric device can be applied for cooling the photodetector.
  • an immunoassay field an immunoassay field
  • an in vitro diagnostics field a general temperature control and cooling system
  • Physiotherapy field a general temperature control and cooling system
  • liquid chiller system liquid chiller system
  • blood / plasma temperature control field blood / plasma temperature control field.
  • thermoelectric element according to an embodiment of the present invention is applied to a medical instrument.
  • a medical instrument is an artificial heart.
  • power can be supplied to the artificial heart.
  • thermoelectric devices examples include star tracking systems, thermal imaging cameras, infrared / ultraviolet detectors, CCD sensors, Hubble Space Telescopes and TTRS. Accordingly, the temperature of the image sensor can be maintained.
  • thermoelectric element according to the embodiment of the present invention is applied to the aerospace industry include a cooling device, a heater, a power generation device, and the like.
  • thermoelectric device according to the embodiment of the present invention can be applied to power generation, cooling, and heating in other industrial fields.

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  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Cooling Or The Like Of Semiconductors Or Solid State Devices (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
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EP19743973.0A EP3745479B1 (en) 2018-01-23 2019-01-22 Thermoelectric element
CN201980009569.5A CN111630671B (zh) 2018-01-23 2019-01-22 热电元件及其制造方法
JP2020540286A JP7344882B2 (ja) 2018-01-23 2019-01-22 熱電素子およびその製造方法
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KR101981629B1 (ko) 2019-05-24
EP3745479A1 (en) 2020-12-02
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EP3745479B1 (en) 2025-09-24
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CN111630671A (zh) 2020-09-04
CN111630671B (zh) 2024-05-24

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