WO2013179840A1 - 熱電変換装置の製造方法、熱電変換装置を備える電子装置の製造方法、熱電変換装置 - Google Patents
熱電変換装置の製造方法、熱電変換装置を備える電子装置の製造方法、熱電変換装置 Download PDFInfo
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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
- H10N10/10—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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L23/00—Details of semiconductor or other solid state devices
- H01L23/34—Arrangements for cooling, heating, ventilating or temperature compensation ; Temperature sensing arrangements
- H01L23/38—Cooling arrangements using the Peltier effect
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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
- H10N10/01—Manufacture or treatment
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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
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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
- H10N10/82—Connection of interconnections
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L2924/00—Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
- H01L2924/0001—Technical content checked by a classifier
- H01L2924/0002—Not covered by any one of groups H01L24/00, H01L24/00 and H01L2224/00
Definitions
- the present invention relates to a method for manufacturing a thermoelectric conversion device, a method for manufacturing an electronic device including the thermoelectric conversion device, and a thermoelectric conversion device.
- Patent Document 1 proposes a method for manufacturing a thermoelectric conversion device as follows.
- first, through holes are formed in an insulating mold, and the first conductive paste regularly formed of Bi, Te, Se, etc., and Bi, Sb, Te, etc. are formed in the through holes. Fill with the second conductive paste.
- a plurality of surface conductive layers are formed on the surface of the insulating mold so as to be in contact with the adjacent first and second conductive pastes. Also, a back conductive layer that contacts the first conductive paste and a second conductive paste that contacts a surface conductive layer different from the surface conductive layer that contacts the first conductive paste on the back of the insulating mold A plurality of are formed.
- the insulating mold is heat-treated at 460 ° C. for 10 hours in an Ar gas atmosphere to form an N-type thermoelectric conversion element from a conductive paste composed of Bi, Te, Se, etc., and Bi, Sb, Te
- a P-type thermoelectric conversion element is formed from a conductive paste composed of the like.
- the N-type thermoelectric conversion element and the P-type thermoelectric conversion element are also connected to the front surface conductive layer and the back surface conductive layer. Thereby, a thermoelectric conversion device in which a plurality of N-type thermoelectric conversion elements and a plurality of P-type thermoelectric conversion elements are alternately connected in series is manufactured.
- the N-type thermoelectric conversion element and the P-type thermoelectric conversion element have a melting point of Bi and Te lower than 460 °. It is formed by doing.
- the alloy formed by liquid phase sintering has a problem that the crystal structure of metal atoms is random, so that it is difficult to generate power in practice.
- the applied pressure is equally applied not only to the first and second conductive pastes but also to the insulating mold located around the first and second conductive pastes (through holes).
- the first and second conductive pastes cannot be pressurized efficiently. For this reason, when the pressure applied to the first and second conductive pastes is insufficient, the N-type thermoelectric conversion element and the P-type thermoelectric conversion element cannot be formed from the first and second conductive pastes. There is a problem that there is.
- thermoelectric conversion device having an N-type thermoelectric conversion element and a P-type thermoelectric conversion element. That is, the thermoelectric effect occurs when two different types of metals are connected. For this reason, for example, the through holes are filled only with a conductive paste composed of Bi, Te, Se, etc., and the surface conductive layer and the back surface conductive layer are made of a material different from the alloy in which the conductive paste is solid-phase sintered. The above problem also occurs in the formed thermoelectric conversion device.
- An object of the present invention is to provide a method for manufacturing a thermoelectric conversion device capable of efficiently applying pressure to a conductive paste, a method for manufacturing an electronic device including a thermoelectric conversion device, and a thermoelectric conversion device.
- a plurality of first and second via holes (11, 12) penetrating in the thickness direction are formed, including a thermoplastic resin, and the first conductive paste ( 41) and a step of preparing the insulating base material 10 in which the second via hole is filled with the second conductive paste (51), and predetermined first and second conduction on the surface 10a of the insulating base material.
- the first conductive paste an alloy powder in which a plurality of metal atoms maintain a predetermined crystal structure is added to an organic solvent to make a paste, and the second conductive paste is used as a different metal from the alloy.
- cavities 13 to 17 are formed inside the laminate, and in the integration step, the cavities Application in the laminating direction acting on the laminate by absorbing pressure in a direction different from the laminating direction acting on the first conductive paste by acting to promote the flow of the thermoplastic resin
- the first interlayer connecting member is configured by increasing the pressure and solid-phase sintering the first conductive paste.
- the applied pressure around the first via hole (the portion where the thermoplastic resin is flowing) is reduced.
- the pressurizing force which should be originally applied to this part is applied to the 1st conductive paste, and the pressurizing force applied to the 1st conductive paste becomes large. That is, the applied pressure can be efficiently applied to the first conductive paste. Therefore, it can suppress that a 1st conductive paste is not solid-phase-sintered.
- a pressurizing force can be efficiently applied also to a 2nd conductive paste, when solid-phase sintering a 2nd conductive paste, it can also suppress that a 2nd conductive paste is not solid-phase sintered. .
- a plurality of via holes (11, 12) penetrating in the thickness direction are formed and filled with a conductive paste (41).
- a paste prepared by adding an organic solvent to an alloy powder in which a plurality of metal atoms maintain a predetermined crystal structure is prepared.
- cavities 13 to 17
- the integration step what is the stacking direction that acts on the conductive paste by the cavities acting to promote the flow of the thermoplastic resin?
- the applied pressure in the stacking direction acting on the stacked body is increased, and the conductive paste is solid-phase sintered to form an interlayer connection member.
- thermoelectric conversion device in which only one kind of interlayer connection member is arranged on the insulating base material is manufactured. And also in such a thermoelectric conversion apparatus, since the integration process is performed while allowing the thermoplastic resin to flow into the cavity, it is possible to efficiently apply pressure to the conductive paste as in the first embodiment. It is possible to prevent the conductive paste from being solid-phase sintered.
- the first and second via holes (11, 12) are formed to include a thermoplastic resin and penetrate in the thickness direction.
- a step of preparing an insulating base material (10) filled with the first conductive paste (41) and the second via hole filled with the second conductive paste (51); and a surface (10a) of the insulating base material A surface protective member (20) having a surface conductive layer (21) in contact with the predetermined first and second conductive pastes and including a thermoplastic resin, and a back surface of the insulating substrate.
- a back surface protective member (30) having a back surface conductive layer (31) in contact with predetermined first and second conductive pastes and including a thermoplastic resin is disposed to form a laminate ( 80) and lamination while heating the laminate
- the first and second interlayer connection members (40, 50) are formed from the first and second conductive pastes, and the first and second interlayer connection members are electrically connected to the surface conductive layer and the back surface conductive layer. And an integration step of connecting them together.
- the first conductive paste an alloy powder in which a plurality of metal atoms maintain a predetermined crystal structure is added to an organic solvent to make a paste, and the second conductive paste is used as a different metal from the alloy.
- a hollow portion (90a) is formed in at least one of the portion facing the surface of the insulating base material and the portion facing the back surface of the insulating base material.
- the laminated body is pressed using the pair of pressed plates (90), and at least one of the thermoplastic resins constituting the surface protection member and the back surface protection member is caused to flow into the recess, and the thermoplastic resin constituting the insulating base material
- the first conductive paste is solid-phase sintered to make the first interlayer connection member.
- thermoplastic resin which comprises an insulating base material flows, it is the 1st like the 1st form.
- the applied pressure can be efficiently applied to the conductive paste. For this reason, it can suppress that a conductive paste is not solid-phase sintered.
- a plurality of first and second via holes (11, 12) penetrating in the thickness direction are formed, and a first via hole is formed in the first via hole.
- a step of preparing an insulating base material (10) filled with the first conductive paste (41) and the second via hole filled with the second conductive paste (51); and a surface (10a) of the insulating base material A surface metal plate (21a) and a back surface metal plate (31a) on the back surface (10b) of the insulating substrate to form a laminate (80), and a laminating direction while heating the laminate
- the first and second interlayer connection members (40, 50) are formed from the first and second conductive pastes, and the first and second interlayer connection members are electrically connected to the front surface metal plate and the back surface metal plate. Integration process to connect to the surface metal plate and And dicing the back metal plate to form a plurality of front surface conductive layers (21) and back surface conductive layers (31) electrically connected to predetermined first and second interlayer connection
- the first conductive paste an alloy powder in which a plurality of metal atoms maintain a predetermined crystal structure is added to an organic solvent to make a paste, and the second conductive paste is used as a different metal from the alloy.
- cavities 13 to 17 are formed inside the laminate, and in the integration step, the cavities Application in the laminating direction acting on the laminate by absorbing pressure in a direction different from the laminating direction acting on the first conductive paste by acting to promote the flow of the thermoplastic resin
- the first interlayer connecting member is formed by increasing the pressure and solid-phase sintering the first conductive paste.
- the front surface metal plate is disposed on the surface of the insulating base material
- the back surface metal plate is disposed on the back surface of the insulating base material
- the surface conductive layer and the back surface conductive layer are formed after the laminate is integrated.
- the integration process is carried out while allowing the thermoplastic resin to flow into the cavity, it is possible to efficiently apply pressure to the conductive paste as in the first embodiment, and the conductive paste is solid phase. It can suppress that it is not sintered.
- the surface protection member (20) which has a some surface conductive layer (21), the back surface protection member (30) which has a some back surface conductive layer (31), and thickness direction A plurality of first and second via holes (11, 12) penetrating through the insulating base material (10) including a thermoplastic resin, and the first via hole (11) filled with a plurality of metals
- the first interlayer connecting member and the second interlayer The surface protection member is disposed in a state where the connecting member is in contact with the same surface conductive layer in the plurality of surface conductive layers for each set, and the first con
- the back surface protection member is disposed in a state where the conductive paste and the second conductive paste of the other set are in contact with the same back surface conductive layer in the plurality of back surface conductive layers, and around the first interlayer connection member and the second interlayer connection member Is characterized by being surrounded by an insulating substrate.
- the insulation base material comprised including the thermoplastic resin is arrange
- FIG. 1 is a plan view of the thermoelectric conversion device according to the first embodiment of the present invention.
- FIG. 2 is a cross-sectional view taken along line II-II in FIG.
- FIG. 3 is a cross-sectional view taken along line III-III in FIG. 4 (a) to 4 (i) are cross-sectional views showing manufacturing steps of the thermoelectric conversion device shown in FIG.
- FIG. 5 is a plan view of the surface side of the insulating base shown in FIG.
- FIG. 6 is a diagram showing manufacturing conditions in the integration step shown in FIG. 7 (a) to 7 (d) are detailed cross-sectional views in the integration process shown in FIG. 4 (i).
- FIG. 8 is a cross-sectional view corresponding to FIG. 4E in the second embodiment of the present invention.
- FIG. 8 is a cross-sectional view corresponding to FIG. 4E in the second embodiment of the present invention.
- FIG. 9 is a plan view of the surface side of the insulating base shown in FIG.
- FIG. 10 is a cross-sectional view corresponding to FIG. 4H in the third embodiment of the present invention.
- FIG. 11 is a cross-sectional view corresponding to FIG. 4E in the fourth embodiment of the present invention.
- FIG. 12 is a cross-sectional view corresponding to FIG. 4E in the fifth embodiment of the present invention.
- FIGS. 13A to 13C are cross-sectional views when performing the step of FIG. 4H in the sixth embodiment of the present invention.
- 14 (a) to 14 (c) are cross-sectional views showing manufacturing steps for preparing an insulating base material according to the seventh embodiment of the present invention.
- FIG. 10 is a cross-sectional view corresponding to FIG. 4H in the third embodiment of the present invention.
- FIG. 11 is a cross-sectional view corresponding to FIG. 4E in the fourth embodiment of the present invention.
- FIG. 12 is a cross-sectional view
- thermoelectric conversion device 15 is a cross-sectional view of the thermoelectric conversion device according to the eighth embodiment of the present invention.
- 16 (a) to 16 (c) are cross-sectional views corresponding to FIG. 4 (i) showing the manufacturing process of the thermoelectric conversion device of FIG.
- FIG. 17 is a cross-sectional view of the thermoelectric conversion device according to the ninth embodiment of the present invention.
- FIG. 18 is a cross-sectional view corresponding to FIG. 4H illustrating the manufacturing process of the thermoelectric conversion device illustrated in FIG. 17.
- FIG. 19 is a cross-sectional view of the thermoelectric conversion device according to the tenth embodiment of the present invention.
- FIG. 20 is a plan view of the surface side of the thermoelectric conversion device according to the eleventh embodiment of the present invention.
- FIG. 21 is a plan view of the back side of the thermoelectric conversion device shown in FIG.
- FIG. 22 is a cross-sectional view of a thermoelectric conversion device according to a twelfth embodiment of the present invention.
- FIG. 23 is a developed plan view of the front surface protection member and the back surface protection member.
- FIG. 24 is a cross-sectional view of an electronic device according to a thirteenth embodiment of the present invention.
- FIG. 25 is a cross-sectional view of an electronic device having a thermoelectric conversion device.
- FIG. 26 is a cross-sectional view of a modified example of an electronic device having a thermoelectric conversion device.
- FIG. 27 is a cross-sectional view of another modified example of an electronic device having a thermoelectric conversion device.
- thermoelectric conversion device 1 includes an insulating base material 10, a surface protection member 20, a back surface protection member 30, and a plurality of first and second interlayer connection members 40 and 50.
- the insulating base material 10, the surface protection member 20, and the back surface protection member 30 are connected to each other, that is, integrated in a multilayer form.
- a plurality of connection member arrays comprising first and second interlayer connection members 40 and 50 for connecting the front surface protection member 20 and the rear surface protection member 30 are formed in the horizontal direction of the drawing. It extends to.
- Each first interlayer connection member 40 and each second interlayer connection member 50 are made of different metals. In each connection member arrangement, the first and second interlayer connection members 40 and 50 are alternately connected in series.
- FIG. 1 the surface protecting member 20 is omitted for easy understanding. Further, FIG. 1 is not a cross-sectional view.
- the first interlayer connection member 40 and the second interlayer connection member 50 are indicated by hatching composed of lines in different directions.
- the insulating substrate 10 is made of a planar rectangular thermoplastic resin film containing polyetheretherketone (PEEK) or polyetherimide (PEI).
- the insulating base 10 is formed with a plurality of first and second via holes 11 and 12 penetrating in the thickness direction.
- the plurality of first and second via holes 11 and 12 are alternately arranged in each of the horizontal arrays extending in the left-right direction in FIG.
- the first and second via holes 11 and 12 have a cylindrical shape whose diameter is constant from the front surface 10a to the back surface 10b of the insulating base material 10, but the first and second via holes 11 and 12 are
- the taper may have a diameter that decreases from the front surface 10a toward the back surface 10b, or may have a rectangular tube shape.
- first interlayer connection member 40 is disposed in each first via hole 11.
- second interlayer connection member 50 is disposed in each second via hole 12.
- the second interlayer connection member 50 is formed of a metal different from that of the first interlayer connection member 40. That is, as described above, the insulating base material 10 includes the first and second interlayer connection members 40 and 50 that are alternately arranged in each of the horizontal arrays extending in the horizontal direction in FIG. Also in FIG. For example, in the lowermost array in FIG. 1, the second interlayer connection member 50, the first interlayer connection member 40, and the second interlayer connection member 50 are arranged in this order from the right. In the second arrangement, the first interlayer connection member 40, the second interlayer connection member 50, and the first interlayer connection member 40 are arranged from the right in the order of “middot; ··”.
- the first interlayer connection member 40 is made of a conductive paste containing powder (metal particles) of a Bi—Sb—Te alloy constituting P-type.
- the second interlayer connection member 50 is made of a conductive paste containing powder (metal particles) of Bi-Te alloy constituting N type.
- a surface protection member 20 made of a flat rectangular thermoplastic resin film containing polyetheretherketone (PEEK) or polyetherimide (PEI) is disposed on the surface 10a of the insulating substrate 10.
- the surface protection member 20 has the same planar shape as the insulating base material 10.
- a plurality of surface conductive layers 21 made of a patterned copper foil or the like are formed on one surface 20a of the surface protection member 20 facing the insulating substrate 10. The plurality of surface conductive layers 21 are separated from each other. Each surface conductive layer 21 is electrically connected to the first and second interlayer connection members 40 and 50, respectively.
- a set 60 is constituted by one adjacent first interlayer connection member 40 and one second interlayer connection member 50.
- the first and second interlayer connection members 40 and 50 of each set 60 are connected to the same surface conductive layer 21. That is, the first and second interlayer connection members 40 and 50 of each set 60 are electrically connected via the surface conductive layer 21.
- each set 60 includes one first interlayer connection member 40 and one second interlayer connection member 50 that are adjacent to each other along the long side direction of the insulating substrate 10 (the left-right direction in FIG. 1). It consists of.
- a flat rectangular back surface protection member 30 made of a thermoplastic resin film containing polyether ether ketone (PEEK) or polyether imide (PEI) is disposed on the back surface 10b of the insulating base material 10.
- the back surface protection member 30 has the same size as that of the insulating base material 10 in plan view.
- a plurality of back surface conductive layers 31 made of a patterned copper foil or the like are formed on one surface 30a side of the back surface protection member 30 facing the insulating base material 10. The plurality of back surface conductive layers 31 are separated from each other. Each back surface conductive layer 31 is electrically connected to the first and second interlayer connection members 40 and 50.
- one first interlayer connection member 40 of each of the two adjacent sets 60 and the second interlayer connection member 50 of the other set 60 are connected to the same back surface conductive layer 31. That is, the first and second interlayer connection members 40 and 50 of two sets 60 adjacent in the horizontal direction are electrically connected via the back surface conductive layer 31.
- two sets 60 arranged along the long side direction of the insulating base material 10 are adjacent sets 60.
- two sets 60 arranged along the short side direction are adjacent sets 60.
- the first and second interlayer connection members 40 and 50 are connected in series as shown in FIG. Is done.
- the first interlayer connection member 40 or the second interlayer connection member 50 located at either one of the left and right ends of each horizontal array is the second interlayer connection member 50 or the first interlayer adjacent in the vertical direction.
- the connecting member 40 Connected to the connecting member 40.
- the 1st interlayer connection member 40 and the 2nd interlayer connection member 50 are connected in series as a whole.
- thermoelectric conversion device 1 is different from that of the thermoelectric conversion device 1.
- the back surface protection member 30 is electrically connected to the back surface conductive layer 31 and opposite to the insulating base material 10.
- An interlayer connection member exposed from one surface of the side rear surface protection member 30 is formed.
- the interlayer connection member can be electrically connected to the outside.
- the thermoelectric conversion device 1 has a structure as described above.
- the diameter of the first and second via holes 11 and 12 is ⁇ 0.7 mm
- the thickness of the insulating base material 10 is 1 mm
- the first and second interlayer connection members 40 and 50 are combined.
- a power of about 2.5 mW can be obtained at a temperature difference of 10 ° C.
- thermoelectric conversion device 1 Next, a method for manufacturing the thermoelectric conversion device 1 will be described with reference to FIGS. 4 (a) -4 (i).
- 4 (a) -4 (i) are cross-sectional views taken along the line II-II in FIG.
- an insulating substrate 10 is prepared, and a plurality of first via holes 11 are formed by a drill or the like.
- each first via hole 11 is filled with a first conductive paste 41.
- the insulating base material 10 is arranged on a holding table (not shown) with the suction paper 70 interposed therebetween so that the back surface 10 b faces the suction paper 70.
- the adsorbing paper 70 may be made of a material that can absorb the organic solvent of the first conductive paste 41, and general high-quality paper or the like is used. Then, the first conductive paste 41 is filled into the first via hole 11 while the first conductive paste 41 is melted. As a result, most of the organic solvent of the first conductive paste 41 is adsorbed by the adsorbent paper 70, and the alloy powder is placed in close contact with the first via hole 11.
- the first conductive paste 41 is a paste obtained by adding an organic solvent such as paraffin having a melting point of 43 ° C. to an alloy powder in which metal atoms maintain a predetermined crystal structure. It is done. For this reason, when the first conductive paste 41 is filled, the surface 10a of the insulating base 10 is heated to about 43 ° C.
- the alloy powder constituting the first conductive paste 41 is, for example, Bi—Sb—Te formed by mechanical alloying.
- a plurality of second via holes 12 are formed in the insulating base material 10 by a drill or the like. As described above, the second via holes 12 are alternately formed with the first via holes 11 and are formed to form a staggered pattern together with the first via holes 11.
- the insulating base material 10 is again disposed on the holding table (not shown) with the suction paper 70 interposed therebetween so that the back surface 10 b faces the suction paper 70.
- the second conductive paste 51 is filled in the second via hole 12 in the same manner as when the first conductive paste 41 is filled.
- most of the organic solvent of the second conductive paste 51 is adsorbed by the adsorbent paper 70, and the alloy powder is placed in close contact with the second via hole 12.
- the second conductive paste 51 an organic solvent such as terpine which has a melting point of room temperature is added to an alloy powder in which metal atoms different from the metal atoms constituting the first conductive paste 41 maintain a predetermined crystal structure.
- the organic solvent constituting the second conductive paste 51 a solvent having a melting point lower than that of the organic solvent constituting the first conductive paste 41 is used.
- the second conductive paste 51 is filled in a state where the organic solvent contained in the first conductive paste 41 is solidified.
- the second conductive paste 51 is suppressed from being mixed into the first via hole 11.
- the alloy powder constituting the second conductive paste 51 for example, Bi-Te formed by mechanical alloying is used.
- the insulating base material 10 filled with the first and second conductive pastes 41 and 51 is prepared.
- a plurality of through holes 13 as cavities are formed in the insulating base material 10 by a drill or a laser.
- the through holes 13 are preferably spaced at equal intervals in the circumferential direction on concentric circles centering on the first and second via holes 11 and 12.
- each through-hole 13 is cylindrical, it is good also as a taper shape where a diameter becomes small toward the back surface 10b from the surface 10a.
- each set 60 includes the first conductive paste 41 filled in one adjacent first via hole 11 and the second conductive paste 51 filled in one second via hole 12.
- the surface protection member 20 is arranged on the surface 10a of the insulating base 10 so that the first and second conductive pastes 41 and 51 of each set 60 are in contact with the same surface conductive layer 21.
- the first conductive pastes 41 and 1 filled in one first via hole 11 adjacent along the long side direction of the insulating base material 10 (the left-right direction in FIG. 1).
- the second conductive paste 51 filled in the two second via holes 12 constitutes each set 60.
- the first conductive paste 41 of one set 60 and the second conductive paste 51 of the other set 60 in the two adjacent sets 60 on the back surface 10b of the insulating base 10 are the same as the back conductive layer 31.
- the back surface protection member 30 is disposed so as to come into contact.
- the adjacent sets 60 are two sets 60 arranged in the long side direction of the insulating base material 10 (left and right direction in FIG. 1).
- two sets 60 arranged along the short side direction (up and down direction in FIG. 1) are adjacent sets 60.
- thermoelectric conversion device 1 is completed by applying pressure while integrating the insulating base material 10, the surface protection member 20, and the back surface protection member 30.
- buffer materials such as rock wool paper
- the laminated body 80 is heated to about 320 ° C. and pressurized at 0.1 Mpa until time T1, and the organic solvent contained in the first and second conductive pastes 41 and 51 is evaporated. (See FIG. 7 (a)).
- the time between T0 and T1 is about 10 minutes.
- the organic solvent contained in the first and second conductive pastes 41 and 51 is an organic solvent remaining without being adsorbed on the adsorbing paper 70 in the steps of FIGS. 4B and 4D. It is.
- the laminated body 80 (that is, the assembly of the insulating base material 10, the surface protection member 20, and the back surface protection member 30 is heated to a temperature equal to or higher than the softening point of the thermoplastic resin. And pressurizing at 10 MPa until time T2 while maintaining at about 320 ° C. At this time, the thermoplastic resin constituting the insulating base material 10 melts and flows, whereby the first and second via holes 11 and 12 The first and second conductive pastes 41 and 51 (alloy powder) are pressed from the lateral direction (radial direction), so that the first and second via holes 11 and 12 are formed as shown in FIG.
- thermoplastic resin flows and the through-hole 13 is deformed to reduce its volume, whereby the pressure applied to the periphery of the first and second via holes 11 and 12 is absorbed and reduced.
- the pressure drops, It becomes possible to increase the pressure that can be applied from above and below the second conductive pastes 41 and 51. That is, the pressure applied from the press plate to the first and second conductive pastes 41 and 51 is increased.
- the pressing direction of the laminate 80 at 10 MPa is the direction in which the insulating base material 10, the surface protection member 20, and the back surface protection member 30 are overlapped, that is, the lamination.
- the alloy powders, the alloy powder, the front surface conductive layer 21 and the back surface conductive layer 31 are pressed and solid-phase sintered, so that the first and second layers Connection members 40 and 50 are formed.
- the first and second interlayer connecting members 40 and 50 are electrically connected to the front surface conductive layer 21 and the back surface conductive layer 31.
- the time between T1 and T2 is about 10 minutes.
- a space is formed in the first and second via holes 11 and 12 by evaporating the organic solvent. However, since this space is very small, the solid-phase sintering of the first and second interlayer connection members 40 and 50 is not hindered by these.
- the laminated body 80 is cooled until time T ⁇ b> 3 while maintaining the pressure applied to the laminated body 80 including the insulating base material 10, the surface protection member 20, and the back surface protection member 30 at 10 MPa.
- the thermoelectric conversion device 1 shown in FIG. 1 in which the insulating base material 10, the surface protection member 20, and the back surface protection member 30 are integrated is manufactured.
- the time between T2 and T3 is about 8 minutes.
- the plurality of through holes 13 are formed in the insulating base material 10.
- the insulating substrate 10 is heated to cause the thermoplastic resin that is the material of the insulating substrate 10 to flow.
- the through-hole 13 is deformed to have a small volume, further increasing the flow of the thermoplastic resin.
- the pressure applied around the first and second via holes 11 and 12 is reduced.
- the pressure applied to the first and second conductive pastes 41 and 51 can be increased by the reduced amount. That is, pressure can be efficiently applied to the first and second conductive pastes 41 and 51. Therefore, the first and second conductive pastes 41 and 51 can reliably perform solid-phase sintering.
- the plurality of through holes 13 are arranged at equal intervals in the circumferential direction on concentric circles centering on the first and second via holes 11 and 12, respectively. For this reason, when the laminated body 80 is formed, the thermoplastic resin around the first and second via holes 11 and 12 is likely to flow so as to make the through-holes 13 isotropically smaller, and the first and second The bias of the two via holes 11 and 12 in the planar direction of the stacked body 80 is suppressed. Therefore, the stability of conduction between the first and second interlayer connection members 40 and 50 formed from the first and second conductive pastes 41 and 51 and the front surface conductive layer 21 and the back surface conductive layer 31 is ensured.
- thermoelectric device having a desired conversion efficiency can be obtained simply by appropriately changing the size and thickness of the planar shape of the insulating base material 10, the number of first and second via holes 11 and 12, the diameter, and the like.
- the converter 1 can be manufactured, and the manufacturing process is not particularly increased or complicated depending on the use of the thermoelectric converter 1. That is, the degree of freedom in designing the thermoelectric conversion device 1 can be improved.
- thermoelectric conversion device 1 generates large electric power because the first and second interlayer connection members 40 and 50 are formed of an alloy in which a plurality of metal atoms maintain a predetermined crystal structure. Can be made. And since the insulating base material 10 comprised including the thermoplastic resin is arrange
- the insulating base material 10 is arrange
- a multilayer board in which a via hole having a wiring pattern such as a copper foil is formed on the bottom and a plurality of resin films in which interlayer connection members are arranged in the via hole are laminated.
- a via hole having a wiring pattern such as a copper foil as a bottom surface is formed, and a plurality of resin films in which a conductive paste is filled in the via hole are prepared.
- the conductive paste contains Sn.
- a plurality of resin films are superposed to form a film laminate (stack).
- the film laminate is pressed and integrated while being heated in a vacuum state to form a stack body.
- the conductive paste is sintered to form an interlayer connection member, and the interlayer connection member is electrically connected to the wiring pattern.
- the conductive paste contains Sn
- the Sn is diffused into the wiring pattern to bond the interlayer connection member (conductive paste) and the wiring pattern. That is, since the metal particles cannot be directly pressed, the laminate is formed using a pressure of about 4 MPa at the maximum. Therefore, the multilayer substrate having such a configuration cannot be formed by the manufacturing method of this embodiment in which the thermoelectric conversion device 1 is manufactured using a large applied pressure.
- the first conductive paste 41 is formed from Bi—Sb—Te alloy powder
- the second conductive paste 51 is Bi—Te alloy powder.
- the powder of the alloy constituting the first and second conductive pastes 41 and 51 is appropriately selected from those in which copper, constantan, chromel, alumel, etc. are alloyed with iron, nickel, chromium, copper, silicon, etc. May be.
- thermoelectric conversion device 1 of the present embodiment differs from the first embodiment in the shape of the cavity formed in the insulating base material 10 and is otherwise the same as that of the first embodiment, so the description thereof is omitted here. .
- a closed-loop square groove 14 surrounding each of the first and second via holes 11 and 12 is formed in the insulating base material 10.
- the grooves 14 are formed on the surface 10 a of the insulating base 10 so that the first and second via holes 11 and 12 enter one groove 14.
- the groove 14 is formed on the back surface 10 b of the insulating base material 10 so that the first and second via holes 11 and 12 enter the single groove 14.
- the groove 14 forms a cavity.
- the plurality of grooves 14 surrounding the first and second via holes 11 and 12 are arranged in a lattice shape, but the shape of the grooves 14 may be other than a square.
- the groove 14 may be formed to extend directly.
- the grooves 14 formed on the front surface 10a and the back surface 10b of the insulating base material 10 have the same size.
- the first and second via holes 11 and 12 are located at the center in the groove 14.
- the groove 14 of the insulating base material 10 is deformed in its own shape with the flow of the thermoplastic resin, and absorbs pressure acting on the groove 14.
- the pressure applied to the first and second conductive pastes 41 and 51 can be increased, and the same effect as in the first embodiment can be obtained.
- the grooves 14 are formed on the front surface 10a and the back surface 10b of the insulating base material 10, but the grooves 14 may be formed only on one of the front surface 10a and the back surface 10b of the insulating base material 10. .
- thermoelectric conversion device 1 of the present embodiment is different from the first embodiment in the shape of the cavity, and the other aspects are the same as those of the first embodiment, and thus the description thereof is omitted here.
- the step of FIG. 4 (e) is omitted, and in the steps of FIGS. 4 (f) and 4 (g), the first and second conductive properties of the front surface conductive layer 21 and the back surface conductive layer 31 are omitted.
- a recess 15 is formed in a portion different from the portion in contact with the pastes 41 and 51. That is, the laminated body 80 in which the concave portion 15 is formed in a portion of the front surface conductive layer 21 and the back surface conductive layer 31 facing the thermoplastic resin constituting the insulating base material 10 is formed.
- the concave portion 15 functions as a cavity.
- the concave portion 15 formed in the front surface conductive layer 21 and the back surface conductive layer 31 is deformed in its own shape with the flow of the thermoplastic resin and absorbs pressure acting on the concave portion 15. By doing so, the pressure applied to the 1st, 2nd conductive pastes 41 and 51 can be enlarged, and the effect similar to the said 1st Embodiment can be acquired.
- the formation of the recess 15 in the front surface conductive layer 21 and the back surface conductive layer 31 has been described.
- the recess 15 is formed only in one of the front surface conductive layer 21 and the back surface conductive layer 31. Also good.
- thermoelectric conversion device 1 of the present embodiment differs from the first embodiment in the cavities formed in the insulating base material 10 and is otherwise the same as in the first embodiment, so the description thereof is omitted here.
- thermoplastic resin film 10c As shown in FIG. 11, in this embodiment, a thermoplastic resin film 10c, a glass cloth 10d having a plurality of cavities 16 therein, and a thermoplastic resin film 10c are laminated in this order as the insulating base material 10, and these are at a low temperature. What was temporarily joined with a press or the like is used.
- the glass cloth 10d functions as a porous member.
- the thermoplastic resin flows (impregnates) into the cavity 16 in the glass cloth 10d in the step of FIG. 4 (i).
- the cavity 16 increases the flow of the thermoplastic resin, that is, promotes the absorption of pressure acting on the cavity 16. For this reason, the pressure applied to the 1st, 2nd conductive paste 41 and 51 can be enlarged, and the effect similar to the said 1st Embodiment can be acquired.
- an aramid nonwoven fabric may be used as the porous member.
- thermoelectric conversion device 1 (Fifth embodiment) A fifth embodiment of the present invention will be described.
- the thermoelectric conversion device 1 according to the present embodiment is different from the first embodiment in the cavity and is otherwise the same as in the first embodiment, and thus the description thereof is omitted here.
- the insulating base material 10 is made of a porous member in which a plurality of holes 17 are formed in a thermoplastic resin film.
- the thermoplastic resin flows into (impregnates) the plurality of holes 17 in the step of FIG.
- the pressure applied to the first and second conductive pastes 41 and 51 can be increased by absorbing the pressure acting on the holes 17 as the holes 17 flow with the thermoplastic resin. The same effect as in the first embodiment can be obtained.
- thermoelectric conversion apparatus 1 of this embodiment has the laminated body 80 in which the through-hole 13 is not formed with respect to 1st Embodiment. Since this laminated body 80 is formed using a press plate in which a hollow portion is formed, and the other parts are the same as those in the first embodiment, the description thereof is omitted here.
- the through hole 13 is not formed in the laminated body 80. That is, the laminate 80 is formed by the steps of FIGS. 4A to 4D and 4F to 4H.
- the laminated body 80 (that is, the assembly made up of the insulating base material 10, the surface protection member 20, and the back surface protection member 30) has a recess 90a formed in a portion different from the portion facing the front surface conductive layer 21 and the back surface conductive layer 31.
- the pair of press plates 90 are pressurized.
- thermoplastic resin constituting the surface protection member 20 and the back surface protection member 30 flows into the respective recessed portions 90 a of the pair of press plates 90, and the thermoplastic resin Following, the thermoplastic resin of the insulating base material 10 flows.
- the lateral pressure acting on the first and second conductive pastes 41 and 51 is absorbed, and the pressure applied from the press plate 90 to the first and second conductive pastes 41 and 51 is increased.
- the first and second conductive pastes 41 and 51 are solid-phase sintered to form the first and second interlayer connection members 40 and 50.
- thermoplastic resin constituting the insulating base material 10 is allowed to flow, whereby the first and first The pressure applied to the two conductive pastes 41 and 51 can be increased, and the same effect as in the first embodiment can be obtained.
- thermoelectric conversion apparatus 1 manufactured by this embodiment, a convex part is formed with the thermoplastic resin which flowed in the hollow part 90a.
- thermoplastic resin which flowed in the hollow part 90a.
- hollow part 90a is formed in each of a pair of press plates 90, you may use the press plate 90 in which the hollow part 90a was formed only in either one of a pair of press plates 90.
- a pair of press plates 90 in which recessed portions 90a are formed in portions different from the portions facing the front surface conductive layer 21 and the back surface conductive layer 31 are used.
- FIG. Also by this, since the flow of each thermoplastic resin which comprises the insulating base material 10, the surface protection member 20, and the back surface protection member 30 is permitted, the effect similar to the said Example can be acquired.
- a seventh embodiment of the present invention will be described.
- the present embodiment is different from the first embodiment in the manufacturing process of preparing the insulating base material 10 filled with the first and second conductive pastes 41 and 51, and the other aspects are the first embodiment. Therefore, the description is omitted here.
- first and second via holes 11 and 12 are formed in the insulating base material 10 at the same time.
- a mask 91 having an area corresponding to the first via hole 11 is disposed on the surface 10 a of the insulating base material 10. Then, only the first via hole 11 is filled with the first conductive paste 41.
- thermoelectric conversion device 1 shown in FIG. 1 is manufactured by performing the same steps as in the first embodiment.
- the first and second via holes 11 and 12 are simultaneously formed in the insulating base material 10.
- the first and second via holes are formed in a single process.
- a mask having an opening corresponding to the second via hole 12 may be disposed on the surface 10 a of the insulating substrate 10.
- the second conductive paste 51 is filled in the second via hole 12
- the second conductive paste 51 is suppressed from being mixed into the first via hole 11 by the mask. Therefore, as the organic solvent that constitutes the second conductive paste 51, a material in which the first conductive paste 41 melts when the second conductive paste 51 is filled can be used. Paraffin can be used similarly to the organic solvent of the paste 41.
- the present embodiment differs from the first embodiment in the configuration of the insulating base material 10 and in the shapes of the first and second via holes 11 and 12 (first and second interlayer connection members 40 and 50). Since other aspects are the same as those in the first embodiment, description thereof is omitted here.
- the insulating base material 10 is configured by laminating a thermosetting resin film 10e, a thermoplastic resin film 10c, and a thermosetting resin film 10e in this order.
- the diameters of the portions near the front surface 10a and the rear surface 10b of the insulating base 10 are larger than the diameter of the central portion. ing.
- thermoelectric conversion device 1 is manufactured as follows. That is, the thermosetting resin film 10e, the thermoplastic resin film 10c, and the thermosetting resin film 10e are laminated in order, and these assemblies are pressed at a low temperature and temporarily joined to form the insulating substrate 10.
- thermosetting resin film 10e that forms the front surface 10a of the insulating substrate 10 and the thermosetting resin film 10e that forms the back surface 10b are thermoplastic.
- a plurality of large-diameter holes reaching the surface of the resin film 10c are formed.
- the 1st, 2nd via-holes 11 and 12 are formed by forming the small diameter hole smaller in diameter in the large diameter hole than the several large diameter hole formed in the thermosetting resin film 10e in the thermoplastic resin film 10c. .
- the laminated body 80 is formed by performing the process of FIG. That is, as shown in FIG. 16 (a), when pressure is applied from the upper and lower surfaces in the stacking direction of the laminate 80, as shown in FIG. 16 (b), the thermoplastic resin (thermoplastic resin film 10c) is It flows and pressurizes the first and second conductive pastes 41 and 51 and flows into the through holes 13. However, the thermosetting resin (thermosetting resin film 10e) does not flow. For this reason, as shown in FIG. 16C, the thermoplastic resin flows into the gap and the through hole 13 formed between the thermosetting resin film 10 e and the first and second interlayer connection members 40 and 50. .
- the thermoplastic resin flows into the through-hole 13 and the through-hole 13 is deformed, the radial (lateral direction in the drawing) force applied to the first and second conductive pastes 41 and 51 is absorbed.
- the pressure applied to the first and second conductive pastes 41 and 51 is increased. Even with such a manufacturing method, the same effect as in the first embodiment can be obtained.
- thermosetting resin does not flow, the displacement of the first and second via holes 11 and 12 in the plane direction of the laminate 80 due to the thermoplastic flow is suppressed. And since the thermosetting resin film 10e becomes a flow resistance when the thermoplastic resin flows, it is possible to suppress the thermoplastic resin from flowing out particularly at the outer edge portion of the insulating base material 10.
- the first and second via holes 11 and 12 have the diameters of the portions near the front surface 10a and the back surface 10b of the insulating base material 10 larger than the diameter of the central portion. For this reason, the contact area of the 1st, 2nd interlayer connection members 40 and 50, the surface conductive layer 21, and the back surface conductive layer 31 can fully be ensured, and it can suppress that a conduction
- the insulating base material 10 of this embodiment is comprised as a laminated body which consists of three resin films of the thermosetting resin film 10e, the thermoplastic resin film 10c, and the thermosetting resin film 10e, it is two sheets Or you may comprise by the laminated body of four or more resin films.
- thermoelectric conversion device 1 of the present embodiment is different from the first embodiment in that the front surface protection member 20 and the back surface protection member 30 are not provided, and the other aspects are the same as those of the first embodiment. Therefore, the description is omitted here.
- thermoelectric conversion device 1 is manufactured as follows. That is, as shown in FIG. 18, the front surface metal plate 21 a and the rear surface metal plate 31 a such as a copper plate having the same size as the planar shape of the insulating base material 10 are arranged on the front surface 10 a and the back surface 10 b of the insulating base material 10. Thus, the laminated body 80 is configured.
- the surface metal plate 21a so that only the first and second interlayer connection members 40, 50 of each set 60 are connected to the same surface conductive layer 21. Dicing. Further, in the two adjacent sets 60, the back surface metal so that only the first interlayer connection member 40 of one set 60 and the second interlayer connection member 50 of the other set 60 are connected to the same back surface conductive layer 31. The plate 31a is diced. Thereby, the thermoelectric conversion apparatus 1 shown in FIG. 17 is completed.
- thermoelectric conversion device 1 in which only the surface conductive layer 21 is disposed on the front surface 10a of the insulating base material 10 and only the back surface conductive layer 31 is disposed on the back surface 10b is also formed by the manufacturing method of any of the above embodiments. can do.
- thermoelectric conversion device 1 of the present embodiment is different from the first embodiment in the second interlayer connection member 50, and the other parts are the same as those in the first embodiment, and thus the description thereof is omitted here.
- the second interlayer connection member 50 is configured by sintering a second conductive paste 51 containing metal particles such as Ag—Sn. That is, the second interlayer connection member 50 is not intended mainly for exerting the thermoelectric effect, but is intended to conduct. For this reason, the diameter of the second via hole 12 is made smaller than the diameter of the first via hole 11. In other words, the cross-sectional area along the plane parallel to the surface of the insulating base material 10 in the second via hole 12 is made smaller than the cross-sectional area along the plane parallel to the surface of the insulating base material 10 in the first via hole 11.
- thermoelectric conversion device 1 As well, the first interlayer connection member 40, the front surface conductive layer 21, and the back surface conductive layer 31 are made of different metals. A thermoelectric effect can be obtained with the conductive layer 31.
- thermoelectric conversion apparatus 1 is manufactured using the conductive paste containing metal particles, such as Ag-Sn type
- thermoelectric conversion device 1 configured so that the second interlayer connection member 50 mainly conducts can also be formed by the manufacturing method of any of the above-described embodiments.
- the second interlayer connection member 50 is not connected to the front surface conductive layer 21 and the back surface conductive layer 31 by solid phase sintering, but is connected to the front surface conductive layer 21 and the back surface conductive layer 31 by metal (diffusion) bonding. Is done.
- thermoelectric conversion device 1 according to an eleventh embodiment of the present invention will be described with reference to FIGS. 20 and 21.
- the thermoelectric conversion device 1 is different from the tenth embodiment in the arrangement of the first and second via holes 11 and 12, and the rest is the same as in the tenth embodiment, so the description thereof is omitted here.
- FIG. 20 shows the surface of the insulating substrate 10 on which the surface conductive layer 21 is disposed.
- FIG. 21 shows the back surface of the insulating base material 10 on which the back surface conductive layer 31 is disposed.
- the first interlayer connection member 40 and the second interlayer connection member 50 are indicated by hatching composed of lines in different directions.
- the first via hole 11 and the second via hole 12 have a plurality of horizontal arrays (horizontal arrays) extending in the long side direction of the insulating base material 10 (left and right direction in FIG. 20 and FIG. 21). ).
- the second via holes 12 are formed only at one end of each horizontal array. More specifically, in each of the left and right of the vertical array extending in the short side direction on the insulating base material 10 (the vertical direction in FIG. 20 and FIG. 21), the first and second via holes 11 and 12 are provided. Alternatingly arranged.
- the first and second interlayer connection members 40 in each horizontal array are connected to the same surface conductive layer 21. Further, as is apparent from FIG. 23, the first interlayer connection members 40 in each horizontal array are connected to the same back surface conductive layer 31.
- Each of the back surface conductive layers 31 has an L shape, as is apparent from FIG. 21, and each of the second interlayer connection members 50 is connected to the adjacent first interlayer connection members 40 in the horizontal arrangement. The back surface conductive layer 31 is connected.
- the first interlayer connection members 40 in each horizontal array are connected in parallel, and those connected in parallel are adjacent to each other through the second interlayer connection member 50.
- the member 40 is connected in series.
- the surface protecting member 20 is omitted for easy understanding.
- the first and second interlayer connection members 40 and 50 are hatched as described above.
- FIG. 21 does not show the back surface protection member 30 for easy understanding.
- the first and second interlayer connection members 40 and 50 are hatched.
- thermoelectric conversion device 1 Although the manufacture of such a thermoelectric conversion device 1 is not particularly illustrated, the locations where the first via holes 11 and the second via holes 12 are formed are changed in the steps of FIGS. 4A and 4C. (F) and the process of FIG.4 (g) are performed by forming the said surface conductive layer 21 and the back surface conductive layer 31 in a shape as shown to FIG.
- thermoelectric conversion device 1 in which the first and second via holes 11 and 12 are not alternately formed, the thermoelectric conversion device 1 can be formed by any one of the manufacturing methods of the above embodiments.
- thermoelectric conversion device 1 of the present embodiment is different from the first embodiment in that only the first via hole 11 is provided and the front surface protection member 20 and the back surface protection member 30 are integrated. Since it is the same as the embodiment, the description thereof is omitted here.
- FIG. 23 is a development view of FIG.
- only the first via hole 11 is formed in the insulating base material 10. That is, only the first interlayer connection member 40 is disposed on the insulating base material 10. Moreover, the surface protection member 20 and the back surface protection member 30 are integrated. In other words, the front surface conductive layer 21 and the back surface conductive layer 31 are continuous as is apparent from FIG.
- Each of the plurality of surface conductive layers 21 is connected to the first interlayer connection member 40 in each lateral arrangement, as is apparent from FIG. Further, each of the back surface conductive layers 31 formed continuously with the surface conductive layer 21 has a horizontal arrangement adjacent to the horizontal arrangement of the first interlayer connection members 40 connected to the surface conductive layer 21 connected thereto. The first interlayer connection member 40 is connected.
- the first interlayer connection members 40 arranged in the horizontal direction along the long side direction of the insulating base material 10 are connected in parallel.
- thermoelectric conversion device 1 is not particularly shown, but only the first via hole 11 is formed in the insulating base material 10 in the step of FIG. 4A, and the surface in the steps of FIGS. 4F and 4G. It is manufactured by integrally forming the protection member 20 and the back surface protection member 30.
- thermoelectric conversion device 1 of this embodiment can also be completed using any of the manufacturing methods of the above embodiments.
- thermoelectric conversion device 1 heats or cools the electronic device 100 to maintain the electronic device 100 at a desired temperature or generate power using the heat of the electronic device 100.
- the electronic device 100 includes a multilayer substrate 110 on the surface protection member 20 in the thermoelectric conversion device 1.
- the multilayer substrate 110 includes a laminate composed of a plurality of (four in this embodiment) resin films 120 each including the wiring pattern 121 and the interlayer connection member 122, and the inside of the laminate and the surface opposite to the thermoelectric conversion device 1.
- Semiconductor chips 131 to 133 are provided on the top. And the thermoelectric conversion apparatus 1 and the multilayer substrate 110 are directly joined.
- thermoelectric conversion device 1 provided in the electronic device 100 functions to cool the multilayer substrate 110 and generate power to be supplied to the chips 131 to 133.
- thermoelectric conversion device 1 can also be used to supply power to the multilayer substrate 110.
- the thermoelectric conversion device 1 and the multilayer substrate 110 are each provided with an interlayer connection member or the like as described in the above embodiment, and are electrically connected to each other.
- the back surface protection member 30, the insulating base material 10, the surface protection member 20, and the plurality of resin films 120 are stacked on each other to form a stack 80, and the stack 80 is heated while being heated.
- the thermoelectric conversion device 1 and the multilayer substrate 110 are bonded simultaneously with the manufacture of the thermoelectric conversion device 1.
- thermoelectric conversion device 1 when the thermoelectric conversion device 1 is manufactured, the thermoelectric conversion device 1 and the multilayer substrate 110 are simultaneously bonded. Therefore, the manufacturing process of the electronic device 100 can be simplified as compared with the case where the thermoelectric conversion device 1 is bonded to the multilayer substrate 110 via an adhesive or the like after the thermoelectric conversion device 1 is formed.
- the electronic device 100 is configured by directly joining the thermoelectric conversion device 1 and the multilayer substrate 110. That is, no extra inclusions are present between the thermoelectric conversion device 1 and the multilayer substrate 110. For this reason, the heat of the multilayer substrate 110 is easily transferred to the thermoelectric conversion device 1, and the electronic device 100 having high heat transfer between the multilayer substrate 110 and the thermoelectric conversion device 1 can be obtained.
- the multilayer substrate 110 of the electronic device 100 has the laminated body which consists of the some resin film 120
- the multilayer substrate 110 may be formed first, and the back surface protection member 30, the insulating base material 10, the surface protection member 20, and the multilayer substrate 110 may be laminated to form the laminate 80.
- the above embodiments can be combined as follows. That is, the first and second embodiments may be combined with the third embodiment to form the through hole 13 or the groove 14 while forming the recess 15. Further, the second embodiment may be combined with the seventh to twelfth embodiments, and the groove 14 may be formed instead of the through hole 13. Further, the third embodiment may be combined with the seventh to twelfth embodiments, and the recess 15 may be formed instead of the through hole 13.
- the fourth embodiment may be combined with the seventh to twelfth embodiments, and the glass cloth 10d may be used instead of the through hole 13, or the fifth embodiment may be combined with the seventh to twelfth embodiments to Instead, a thermoplastic resin film 10c in which a plurality of holes 17 are formed may be used.
- channel 14, the recessed part 15, or all can also be formed.
- the sixth embodiment may be combined with the first to fifth embodiments, and the laminate 80 may be integrated using a pair of press plates 90 in which the recessed portions 90a are formed.
- the eighth embodiment may be combined with the ninth to twelfth embodiments, and the insulating substrate 10 may be a laminate of a thermoplastic resin film 10c and a thermosetting resin film 10e. Moreover, when using the insulating base material 10 which laminated
- thermoelectric conversion device 1 described above can have a structure of several combinations of the above embodiments, and the thermoelectric conversion device 1 is manufactured by any one of the manufacturing methods of the above embodiments. Can do.
- the electronic device 100 is configured by the thermoelectric conversion device 1 and the multilayer substrate 110, but the attachment target of the thermoelectric conversion device is not limited to the multilayer substrate 110.
- the electronic device 100 may further include fins 140 on the surface protection member 20 in the thermoelectric conversion device 1.
- the heat dissipation effect can be improved by the fins 140.
- the electronic device 100 includes a laminated body 80 including the fins 140 and is integrally manufactured by pressing the laminated body 80 while heating.
- the electronic device 100 may be configured by joining the thermoelectric conversion device 1 to a circular cross-section such as a pipe 150 as shown in FIG.
- thermoelectric conversion device 1 used in the electronic device 100 is manufactured by using, for example, a pair of press plates that have a curved surface as a pair of press plates for heating the laminated body 80 in the integration step of FIG.
- the In the integration step stress is applied to the first and second via holes 11 and 12 by the flow of the resin constituting the insulating base 10 as described above, so that the metal particles, the metal particles and the surface conductive layer 21, and the back surface conductive Since the layer 31 is press-contacted, a stable bonding can be obtained even when the shape has a curved surface.
- the thermoelectric conversion device 1 and the target object may be joined.
- the insulating base material 10, the surface protection member 20, and the back surface protection member 30 are made of resin, and the thermoelectric conversion device 1 has flexibility. For this reason, after manufacturing the thermoelectric conversion apparatus 1, you may bend
- the electronic device 100 can also be composed of a thermoelectric conversion device 1 and an electronic device 190.
- the thermoelectric conversion device 1 is disposed on the base 160.
- the electronic device 190 has a communication device 180.
- the communication device 180 has a control IC chip 170 disposed on the substrate 160.
- the thermoelectric conversion device 1 generates power and supplies it to the communication device 180.
- the communication apparatus 180 may be arrange
- thermoelectric conversion apparatus 1 of this invention and the electronic apparatus 100 containing this thermoelectric conversion apparatus 1 are provided in the roof and wall which partition indoor and the outdoor, for example, and generate
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Abstract
Description
本発明の第1実施形態の熱電変換装置1について図面を参照しつつ説明する。図1~図3に示されるように、熱電変換装置1は、絶縁基材10、表面保護部材20、裏面保護部材30、および複数の第1、第2層間接続部材40、50を有する。絶縁基材10、表面保護部材20、裏面保護部材30は、多層形態で、互いに接続、すなわち一体化される。この一体化された組立体(assembly)内において、表面保護部材20と裏面保護部材30を接続する第1、第2層間接続部材40、50からなる複数の接続部材配列(arrays)が図面左右方向に延在している。各第1層間接続部材40と各第2層間接続部材50は互いに異なる金属からなる。各接続部材配列において、第1、第2層間接続部材40、50は交互に直列に接続されている。
つまり、絶縁基材10には、上記したように、第1、第2層間接続部材40、50が、図1の左右方向に延びる横配列の各々において互い違いに配置され、上下方向に延びる縦配列においても、互い違いに配置される。例えば、図1の一番下の配列においては、右から、第2層間接続部材50、第1層間接続部材40、第2層間接続部材50···の順で配置され、下から2番目の配列においては、右から第1層間接続部材40、第2層間接続部材50、第1層間接続部材40···の順で配置されている。
本発明の第2実施形態について説明する。本実施形態の熱電変換装置1は、第1実施形態に対して、絶縁基材10に形成する空洞の形状において異なり、その他に関しては第1実施形態と同様であるため、ここでは説明を省略する。
本発明の第3実施形態について説明する。本実施形態の熱電変換装置1は、第1実施形態に対して、空洞の形状において異なるものであり、その他に関しては第1実施形態と同様であるため、ここでは説明を省略する。
本発明の第4実施形態について説明する。本実施形態の熱電変換装置1は、第1実施形態に対して、絶縁基材10に形成する空洞において異なり、その他に関しては第1実施形態と同様であるため、ここでは説明を省略する。
本発明の第5実施形態について説明する。本実施形態の熱電変換装置1は、第1実施形態に対して、空洞において異なるものであり、その他に関しては第1実施形態と同様であるため、ここでは説明を省略する。
積層体80を形成する際に、図4(i)の工程において、複数の穴17に熱可塑性樹脂が流れ込む(含浸する)。言い換えれば、穴17が熱可塑性樹脂の流動に伴い、穴17へ作用する圧力を吸収することにより、第1、第2伝導性ペースト41、51に印加される圧力を大きくすることができ、上記第1実施形態と同様の効果を得ることができる。
本発明の第6実施形態について説明する。本実施形態の熱電変換装置1は、第1実施形態に対して、貫通孔13が形成されていない積層体80を有している。この積層体80は窪み部が形成されたプレス板を用いて形成されるものであり、その他に関しては第1実施形態と同様であるため、ここでは説明を省略する。
本発明の第7実施形態について説明する。本実施形態は、第1実施形態に対して、第1、第2伝導性ペースト41、51が充填された絶縁基材10を用意する製造工程において異なるものであり、その他に関しては第1実施形態と同様であるため、ここでは説明を省略する。
本発明の第8実施形態について説明する。本実施形態は、第1実施形態に対して、絶縁基材10の構成が異なるとともに、第1、第2ビアホール11、12(第1、第2層間接続部材40、50)の形状が異なるものであり、その他に関しては第1実施形態と同様であるため、ここでは説明を省略する。
本発明の第9実施形態について説明する。本実施形態の熱電変換装置1は、第1実施形態に対して、表面保護部材20および裏面保護部材30を有さないという点で異なるものであり、その他に関しては第1実施形態と同様であるため、ここでは説明を省略する。
本発明の第10実施形態について説明する。本実施形態の熱電変換装置1は、第1実施形態に対して、第2層間接続部材50において異なるものであり、その他に関しては第1実施形態と同様であるため、ここでは説明を省略する。
本発明の第11実施形態の熱電変換装置1について図20および図21を用いて説明する。熱電変換装置1は、第10実施形態に対して、第1、第2ビアホール11、12の配列において異なるものであり、その他に関しては第10実施形態と同様であるため、ここではその説明を省略する。なお、図20は、絶縁基材10の表面導電層21が配置された表面を示す。図21は、絶縁基材10の裏面導電層31が配置された裏面を示す。なお、図20,21において、第1層間接続部材40と第2層間接続部材50とを、異なる向きの線からなるハッチングで示してある。
本発明の第12実施形態について説明する。本実施形態の熱電変換装置1は、第1実施形態に対して、第1ビアホール11のみを有すると共に表面保護部材20と裏面保護部材30とを一体化した点において異なり、その他に関しては第1実施形態と同様であるため、ここではその説明を省略する。図23は図22の展開図である。
本発明の第13実施形態について説明する。本実施形態は、第1実施形態の熱電変換装置1を有する電子装置100に関するものである。熱電変換装置1の構造の詳細は第1実施形態と同様であるため、ここでは説明を省略する。熱電変換装置1は、電子装置100を加熱あるいは冷却することにより、電子装置100を所望の温度に保ったり、電子装置100の熱を利用して発電したりする。
本発明は上記した実施形態に限定されるものではなく、特許請求の範囲に記載した範囲内において上記実施例の可能な数の組み合わせや、変形例を含むものである。
10a 表面
10b 裏面
11 第1ビアホール
12 第2ビアホール
20 表面保護部材
21 表面導電層
30 裏面保護部材
31 裏面導電層
40 第1層間接続部材
41 第1伝導性ペースト
50 第2層間接続部材
51 第2伝導性ペースト
60 組
80 積層体
Claims (18)
- 熱可塑性樹脂を含んで構成されており、厚さ方向に貫通する複数の第1、第2ビアホール(11、12)が形成され、前記第1ビアホールに第1伝導性ペースト(41)が充填されていると共に前記第2ビアホールに第2伝導性ペースト(51)が充填されている絶縁基材(10)を用意する工程と、
前記絶縁基材の表面(10a)に所定の前記第1、第2伝導性ペーストと接触する表面導電層(21)を有する表面保護部材(20)を配置すると共に、前記絶縁基材の裏面(10b)に所定の前記第1、第2伝導性ペーストと接触する裏面導電層(31)を有する裏面保護部材(30)を配置して積層体(80)を形成する工程と、
前記積層体を加熱しながら積層方向から加圧し、前記第1、第2伝導性ペーストから第1、第2層間接続部材(40、50)を構成すると共に前記第1、第2層間接続部材と前記表面導電層および前記裏面導電層とを電気的に接続する一体化工程と、を行い、
前記第1伝導性ペーストとして、複数の金属原子が所定の結晶構造を維持している合金の粉末に有機溶剤を加えてペースト化したものを用い、
前記第2伝導性ペーストとして、前記合金と異種金属の粉末に有機溶剤を加えてペースト化したものを用い、
前記積層体を構成する工程では、前記積層体の内部に空洞(13~17)が形成されており、
前記一体化工程では、前記空洞が前記熱可塑性樹脂の流動を助長させるように作用することにより前記第1導電ペーストに対して作用する積層方向とは異なる方向への圧力を吸収することにより、前記積層体に作用する積層方向への印加圧力を増大させ、前記第1伝導性ペーストを固相焼結して前記第1層間接続部材を構成することを特徴とする熱電変換装置の製造方法。 - 前記積層体を構成する工程の前に、前記絶縁基材に貫通孔(13)を形成することを特徴とする請求項1に記載の熱電変換装置の製造方法。
- 前記貫通孔を形成する工程では、前記第1、第2ビアホールのそれぞれを中心とする同心円上において周方向に等間隔に複数の前記貫通孔を形成することを特徴とする請求項2に記載の熱電変換装置の製造方法。
- 前記積層体を構成する工程の前に、閉ループ状の溝部(14)を当該溝部の閉ループ内に前記第1、第2ビアホールのいずれか一方が1つずつ位置するように形成することを特徴とする請求項1に記載の熱電変換装置の製造方法。
- 前記積層体を構成する工程では、前記表面導電層および前記裏面導電層の少なくとも一方のうち前記第1、第2伝導性ペーストと接触する部分と異なる部分に凹部(15)が形成されている前記表面保護部材および前記裏面保護部材を用いることを特徴とする請求項1ないし4のいずれか1つに記載の熱電変換装置の製造方法。
- 前記絶縁基材として、内部に空洞(16)を有する多孔質部材(10d)を含有するものを用いることを特徴とする請求項1ないし5のいずれか1つに記載の熱電変換装置の製造方法。
- 前記絶縁基材として、内部に穴(17)が形成された多孔質性のものを用いることを特徴とする請求項1ないし5のいずれか1つに記載の熱電変換装置の製造方法。
- 前記絶縁基材を用意する工程では、
前記絶縁基材に前記第1ビアホールを形成する工程と、
前記第1ビアホールに前記第1伝導性ペーストを充填する工程と、
前記第1伝導性ペーストを充填する工程の後に行う前記絶縁基材に前記第2ビアホールを形成する工程と、
前記第2ビアホールに前記第2伝導性ペーストを充填する工程と、を行い、
前記第2伝導性ペーストとして、前記第1伝導性ペーストを構成する有機溶剤より融点が低い有機溶剤にて構成されるものを用い、
前記第2伝導性ペーストを充填する工程では、前記絶縁基材を前記第1伝導性ペーストに含まれる有機溶剤の融点より低い温度であって、前記第2伝導性ペーストに含まれる有機溶剤の融点より高い温度に維持しつつ行うことを特徴とする請求項1ないし7のいずれか1つに記載の熱電変換装置の製造方法。 - 前記絶縁基材を用意する工程では、
前記絶縁基材に前記第1、第2ビアホールを同時に形成する工程と、
前記絶縁基材の表面上に、前記第1ビアホールに対応する領域が開口されたマスクを配置する工程と、
前記絶縁基材の表面側から前記第1ビアホールに前記第1伝導性ペーストを充填する工程と、
前記マスクを除去する工程と、
前記第2ビアホールに前記第2伝導性ペーストを充填する工程と、を行い、
前記第2伝導性ペーストとして、前記第1伝導性ペーストを構成する有機溶剤より融点が低い有機溶剤にて構成されるものを用い、
前記第2伝導性ペーストを充填する工程では、前記絶縁基材を前記第1伝導性ペーストに含まれる有機溶剤の融点より低い温度であって、前記第2伝導性ペーストに含まれる有機溶剤の融点より高い温度に維持しつつ行うことを特徴とする請求項1ないし7のいずれか1つに記載の熱電変換装置の製造方法。 - 前記絶縁基材として、熱硬化性樹脂フィルム(10e)、熱可塑性樹脂フィルム(10c)、熱硬化性樹脂フィルム(10e)が順に積層されたものを用いることを特徴とする請求項1ないし9のいずれか1つに記載の熱電変換装置の製造方法。
- 前記絶縁基材を用意する工程では、前記第1、第2ビアホールが互い違いに形成されたものを用意し、
前記積層体を構成する工程では、隣接する1つの前記第1ビアホールに充填された前記第1伝導性ペーストと1つの前記第2ビアホールに充填された前記第2伝導性ペーストとを組(60)としたとき、前記絶縁基材の表面側に、前記第1伝導性ペーストおよび前記第2伝導性ペーストが前記組毎に前記複数の表面導電層における同じ表面導電層に接触する状態で前記表面保護部材を配置すると共に、前記絶縁基材の裏面側に、隣接する組における一方の組の前記第1伝導性ペーストおよび他方の組の前記第2伝導性ペーストが前記複数の裏面導電層における同じ前記裏面導電層に接触する状態で前記裏面保護部材を配置することを特徴とする請求項1ないし10のいずれか1つに記載の熱電変換装置の製造方法。 - 前記絶縁基材を用意する工程では、前記第2ビアホールにおける前記絶縁基材の表面と平行な平面に沿った断面積が前記第1ビアホールにおける前記絶縁基材の前記平面に沿った断面積より小さいものを用意し、
前記第2伝導性ペーストとして前記表面導電層と前記裏面導電層とを接続するためのものを用いることを特徴とする請求項1ないし10のいずれか1つに記載の熱電変換装置の製造方法。 - 前記積層体を構成する工程では、前記表面保護部材および前記裏面保護部材が一体化されているものを用いることを特徴とする請求項1ないし12のいずれか1つに記載の熱電変換装置の製造方法。
- 熱可塑性樹脂を含んで構成されており、厚さ方向に貫通する複数のビアホール(11、12)が形成され、前記ビアホールに伝導性ペースト(41)が充填されている絶縁基材(10)を用意する工程と、
前記絶縁基材の表面(10a)に所定の前記伝導性ペーストと接触する表面導電層(21)を有する表面保護部材(20)を配置すると共に、前記絶縁基材の裏面(10b)に所定の前記伝導性ペーストと接触する裏面導電層(31)を有する裏面保護部材(30)を配置して積層体(80)を形成する工程と、
前記積層体を加熱しながら積層方向から加圧し、前記伝導性ペーストから層間接続部材(40)を構成すると共に当該層間接続部材と前記表面導電層および前記裏面導電層とを電気的に接続する一体化工程と、を行い、
前記伝導性ペーストとして、複数の金属原子が所定の結晶構造を維持している合金の粉末に有機溶剤を加えてペースト化したものを用意し、
前記積層体を構成する工程では、前記積層体の内部には空洞(13~17)が形成されており、
前記一体化工程では、前記空洞が前記熱可塑性樹脂の流動を助長させるように作用することにより前記導電ペーストに対して作用する積層方向とは異なる方向への圧力を吸収することにより、前記積層体に作用する積層方向への印加圧力を増大させ、前記伝導性ペーストを固相焼結して層間接続部材を構成することを特徴とする熱電変換装置の製造方法。 - 請求項1ないし14のいずれか1つに記載の熱電変換装置の製造方法を電子装置の製造方法として適用し、
前記積層体を構成する工程では、前記表面保護部材上に被対象物(110、140、150)を積層した積層体を構成し、
前記一体化工程では、前記表面保護部材と前記被対象物とを直接接合することを特徴とする電子装置の製造方法。 - 熱可塑性樹脂を含んで構成されており、厚さ方向に貫通する複数の第1、第2ビアホール(11、12)が形成され、前記第1ビアホールに第1伝導性ペースト(41)が充填されていると共に前記第2ビアホールに第2伝導性ペースト(51)が充填されている絶縁基材(10)を用意する工程と、
前記絶縁基材の表面(10a)に、所定の前記第1、第2伝導性ペーストと接触する表面導電層(21)を有し、熱可塑性樹脂を含んで構成された表面保護部材(20)を配置すると共に、前記絶縁基材の裏面(10b)に、所定の前記第1、第2伝導性ペーストと接触する裏面導電層(31)を有し、熱可塑性樹脂を含んで構成された裏面保護部材(30)を配置して積層体(80)を形成する工程と、
前記積層体を加熱しながら積層方向から加圧し、前記第1、第2伝導性ペーストから第1、第2層間接続部材(40、50)を構成すると共に前記第1、第2層間接続部材と前記表面導電層および前記裏面導電層とを電気的に接続する一体化工程と、を行い、
前記第1伝導性ペーストとして、複数の金属原子が所定の結晶構造を維持している合金の粉末に有機溶剤を加えてペースト化したものを用い、
前記第2伝導性ペーストとして、前記合金と異種金属の粉末に有機溶剤を加えてペースト化したものを用い、
前記一体化工程では、前記絶縁基材の表面と対向する部分および前記絶縁基材の裏面と対向する部分の少なくとも一方に窪み部(90a)が形成された一対のプレス板(90)を用いて前記積層体を加圧し、前記表面保護部材および前記裏面保護部材を構成する熱可塑性樹脂の少なくとも一方を前記窪み部に流動させると共に前記絶縁基材を構成する熱可塑性樹脂を流動させつつ、前記第1伝導性ペーストを固相焼結して前記第1層間接続部材を構成することを特徴とする熱電変換装置の製造方法。 - 熱可塑性樹脂を含んで構成されており、厚さ方向に貫通する複数の第1、第2ビアホール(11、12)が形成され、前記第1ビアホールに第1伝導性ペースト(41)が充填されていると共に前記第2ビアホールに第2伝導性ペースト(51)が充填されている絶縁基材(10)を用意する工程と、
前記絶縁基材の表面(10a)に表面金属板(21a)を配置すると共に、前記絶縁基材の裏面(10b)に裏面金属板(31a)を配置して積層体(80)を形成する工程と、
前記積層体を加熱しながら積層方向から加圧し、前記第1、第2伝導性ペーストから第1、第2層間接続部材(40、50)を構成すると共に前記第1、第2層間接続部材と前記表面金属板および前記裏面金属板とを電気的に接続する一体化工程と、
前記表面金属板および前記裏面金属板をダイシングし、所定の前記第1、第2層間接続部材と電気的に接続される複数の表面導電層(21)および裏面導電層(31)を形成する工程と、を行い、
前記第1伝導性ペーストとして、複数の金属原子が所定の結晶構造を維持している合金の粉末に有機溶剤を加えてペースト化したものを用い、
前記第2伝導性ペーストとして、前記合金と異種金属の粉末に有機溶剤を加えてペースト化したものを用い、
前記積層体を構成する工程では、前記積層体の内部に空洞(13~17)が形成されており、
前記一体化工程では、前記空洞が前記熱可塑性樹脂の流動を助長させるように作用することにより前記第1導電ペーストに対して作用する積層方向とは異なる方向への圧力を吸収することにより、前記積層体に作用する積層方向への印加圧力を増大させ、前記第1伝導性ペーストを固相焼結して第1層間接続部材を構成することを特徴とする熱電変換装置の製造方法。 - 複数の表面導電層(21)を有する表面保護部材(20)と、
複数の裏面導電層(31)を有する裏面保護部材(30)と、
厚さ方向に貫通する複数の第1、第2ビアホール(11、12)を有し、熱可塑性樹脂を含んで構成された絶縁基材(10)と、
前記第1ビアホール(11)に充填され、複数の金属原子が所定の結晶構造を維持している合金で形成された第1層間接続部材(40)と、
前記第2ビアホール(12)に充填され、前記合金に対して異種金属で形成された第2層間接続部材(50)と、を備え、
隣接する1つの前記第1ビアホールに充填された前記第1層間接続部材と1つの前記第2ビアホールに充填された前記第2層間接続部材とを組(60)としたとき、前記絶縁基材の表面側に、前記第1層間接続部材および前記第2層間接続部材が前記組毎に前記複数の表面導電層における同じ表面導電層に接触する状態で前記表面保護部材が配置されている共に、前記絶縁基材の裏面側に、隣接する組における一方の組の前記第1伝導性ペーストおよび他方の組の前記第2伝導性ペーストが前記複数の裏面導電層における同じ前記裏面導電層に接触する状態で前記裏面保護部材が配置されており、
前記第1層間接続部材および前記第2層間接続部材の周囲は、前記絶縁基材で囲まれていることを特徴とする熱電変換装置。
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US14/404,705 US9680079B2 (en) | 2012-05-30 | 2013-04-26 | Production method of thermoelectric converter, production method of electronic device equipped with thermoelectric converter, and thermoelectric converter |
CN201380028113.6A CN104335374B (zh) | 2012-05-30 | 2013-04-26 | 热电变换装置的制造方法、具备热电变换装置的电子装置的制造方法、热电变换装置 |
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EP2858134B1 (en) | 2017-09-20 |
US20150144171A1 (en) | 2015-05-28 |
EP2858134A8 (en) | 2015-05-27 |
CN104335374B (zh) | 2017-05-24 |
CN104335374A (zh) | 2015-02-04 |
CN106876570A (zh) | 2017-06-20 |
US9871181B2 (en) | 2018-01-16 |
US9680079B2 (en) | 2017-06-13 |
JP2014007376A (ja) | 2014-01-16 |
EP2858134A1 (en) | 2015-04-08 |
US20170213953A1 (en) | 2017-07-27 |
KR101716559B1 (ko) | 2017-03-14 |
EP2858134A4 (en) | 2016-04-20 |
KR20150002865A (ko) | 2015-01-07 |
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