WO2018235408A1 - Electricity storage device - Google Patents

Electricity storage device Download PDF

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Publication number
WO2018235408A1
WO2018235408A1 PCT/JP2018/015494 JP2018015494W WO2018235408A1 WO 2018235408 A1 WO2018235408 A1 WO 2018235408A1 JP 2018015494 W JP2018015494 W JP 2018015494W WO 2018235408 A1 WO2018235408 A1 WO 2018235408A1
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WO
WIPO (PCT)
Prior art keywords
active material
layer
storage device
inorganic filler
electrolyte
Prior art date
Application number
PCT/JP2018/015494
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French (fr)
Japanese (ja)
Inventor
恭丈 福田
上田　安彦
将之 神頭
法久 青木
Original Assignee
株式会社村田製作所
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Publication of WO2018235408A1 publication Critical patent/WO2018235408A1/en

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/10—Multiple hybrid or EDL capacitors, e.g. arrays or modules
    • H01G11/12—Stacked hybrid or EDL capacitors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/78—Cases; Housings; Encapsulations; Mountings
    • H01G11/80—Gaskets; Sealings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G4/00—Fixed capacitors; Processes of their manufacture
    • H01G4/30—Stacked capacitors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/04—Construction or manufacture in general
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a power storage device.
  • Patent Document 1 describes an example thereof.
  • Patent Document 1 describes a power storage device in which the periphery of an active material layer is covered with a separator having an insulating property.
  • the storage characteristic of the storage device decreases as the amount of the electrolyte held in the electrolyte layer decreases. For this reason, it is necessary to reliably hold the electrolytic solution in the electrolyte layer from the viewpoint of maintaining the excellent storage characteristics of the storage device.
  • the main object of the present invention is to provide a storage device in which storage characteristics are unlikely to deteriorate.
  • An electricity storage device comprises a first internal electrode, a first electrolyte layer, a first insulating adhesive layer, a second internal electrode, a second electrolyte layer, and a second insulating property. And an adhesive layer.
  • the first inner electrode extends along the length direction and the width direction.
  • the first inner electrode has a first current collector and a first active material layer.
  • the first active material layer is provided on the first current collector.
  • the first electrolyte layer is disposed on the first active material layer.
  • the first insulating adhesive layer covers the periphery of the first active material layer and the first electrolyte layer.
  • the first insulating adhesive layer is made of a resin composition in which an inorganic filler is dispersed.
  • the second inner electrode is stacked in the thickness direction with respect to the first inner electrode.
  • the second inner electrode has a second current collector and a second active material layer.
  • the second active material layer is provided on the second current collector.
  • the second electrolyte layer is disposed on the second active material layer.
  • the second electrolyte layer is in contact with the first electrolyte layer.
  • the second insulating adhesive layer covers the periphery of the second active material layer and the second electrolyte layer.
  • the second insulating adhesive layer is made of a resin composition in which an inorganic filler is dispersed.
  • the second insulating adhesive layer is bonded to the first insulating adhesive layer.
  • the first insulating adhesive layer has a first portion and a second portion.
  • the first portion covers the periphery of the first active material layer.
  • the second portion covers the periphery of the first electrolyte layer.
  • the second portion is bonded to the second insulating adhesive layer.
  • the second insulating adhesive layer has a third portion and a fourth portion.
  • the third portion covers the periphery of the second active material layer.
  • the fourth portion covers the periphery of the second electrolyte layer.
  • the fourth portion is bonded to the second portion.
  • the content of the inorganic filler in the second part is less than the content of the inorganic filler in the first part.
  • the content of the inorganic filler in the fourth part is less than the content of the inorganic filler in the third part.
  • the inorganic filler is contained in the insulating adhesive layer made of the resin composition. For this reason, it is suppressed that the electrolyte solution contained in an electrolyte layer infiltrates in the insulating contact bonding layer, and swelling of the insulating contact bonding layer.
  • the whole of the insulating adhesive layer preferably contains many inorganic fillers.
  • the adhesive strength between the second portion and the fourth portion decreases. For this reason, there is a possibility that the electrolytic solution may leak from between the second portion and the fourth portion, or the second portion and the fourth portion may peel, and the electrolytic solution may leak from the peeled portion.
  • the content of the inorganic filler in the second part is smaller than the content of the inorganic filler in the first part.
  • the content of the inorganic filler in the fourth part is less than the content of the inorganic filler in the third part. That is, the content of the inorganic filler in the second and fourth portions is relatively low, and the content of the resin is relatively high.
  • the second part and the fourth part are firmly bonded. Therefore, the leakage of the electrolytic solution from between the second portion and the fourth portion is also effectively suppressed. For this reason, it is difficult for the electrolytic solution to leak from the electrolyte layer. Therefore, the storage characteristic of the storage device according to the present invention is unlikely to deteriorate.
  • the second and fourth portions may not contain the inorganic filler.
  • each of the first and second electrolyte layers may contain an electrolytic solution.
  • the resin contained in the first and second insulating adhesive layers may be a resin which is swelled by the electrolytic solution.
  • the thickness of the first part when the thickness of the first part is t1, the thickness of the second part is t2, the thickness of the third part is t3, and the thickness of the fourth part is t4.
  • T2 / t1 and t4 / t3 are each preferably 0.55 or less.
  • each of the first and second active material layers may contain an active material.
  • the oil absorption of the inorganic filler is lower than the oil absorption of the active material.
  • the inorganic filler includes aluminum oxide, silicon oxide, titanium oxide, magnesium oxide, zirconium oxide, zircon, silicon carbide, aluminum phosphate, aluminum nitride, silicon nitride, steatite, cordierite, mullite and the like It may contain at least one selected from the group consisting of sialon.
  • FIG. 1 is a schematic perspective view of a power storage device according to an embodiment of the present invention.
  • FIG. 2 is a schematic cross-sectional view taken along line II-II in FIG.
  • FIG. 3 is a schematic cross-sectional view taken along line III-III of FIG.
  • FIG. 1 is a schematic perspective view of a power storage device according to the present embodiment.
  • FIG. 2 is a schematic cross-sectional view taken along line II-II in FIG.
  • FIG. 3 is a schematic cross-sectional view taken along line III-III of FIG.
  • the power storage device 1 shown in FIGS. 1 to 3 is, for example, a device that constitutes an electric double layer capacitor or a secondary battery.
  • the storage device 1 includes a device body 10. As shown in FIGS. 2 and 3, the device body 10 includes a functional unit 10A and an exterior body 10B.
  • the functional unit 10A is a portion at least a part of which exhibits a function as a power storage device.
  • the functional unit 10A is provided in a rectangular shape.
  • the functional unit 10A has first and second main surfaces 10a and 10b, first and second side surfaces 10c and 10d (see FIG. 3), and first and second end surfaces 10e and 10f (FIG. 2). See)).
  • the first and second major surfaces 10 a and 10 b extend along the length direction L and the width direction W.
  • the first major surface 10 a and the second major surface 10 b are opposed in the thickness direction T.
  • the first and second side surfaces 10 c and 10 d extend along the length direction L and the thickness direction T.
  • the first side surface 10 c and the second side surface 10 d face each other in the width direction W.
  • the first and second end faces 10 e and 10 f extend in the width direction W and the thickness direction T.
  • the first end face 10 e and the second end face 10 f are opposed in the length direction L.
  • the “cuboid shape” includes a rectangular shape having a chamfered shape or a rounded shape at a corner portion or a ridge portion.
  • the functional unit 10 ⁇ / b> A includes a first inner electrode 11, a second inner electrode 12, and an electrolyte layer 13.
  • the first inner electrode 11 extends along the length direction L and the width direction W.
  • the first inner electrode 11 is provided in parallel to the first and second main surfaces 10a and 10b.
  • the first inner electrode 11 has a first current collector 11a and a first active material layer 11b.
  • the first current collector 11a can be made of, for example, a metal foil made of at least one metal such as aluminum and copper.
  • metal includes alloys.
  • a first active material layer 11 b is provided on the surface on one side of the first current collector 11 a.
  • the first active material layer 11 b contains an active material.
  • the first active material layer 11 b constitutes a polarizable electrode.
  • the first active material layer 11b as the polarizable electrode contains, for example, a carbon material such as activated carbon as an active material.
  • the first inner electrode 11 is drawn to the first end face 10e, but is not drawn to the first and second side faces 10c and 10d and the second end face 10f. Specifically, in the present embodiment, as shown in FIG. 2, only the first current collector 11a of the first inner electrode 11 is exposed at the first end face 10e.
  • the second inner electrode 12 extends along the length direction L and the width direction W.
  • the second inner electrode 12 is provided in parallel to the first and second main surfaces 10a and 10b.
  • the second inner electrode 12 is stacked in the thickness direction T with respect to the first inner electrode 11.
  • the portion excluding the second end face 10 f side end portion of the second inner electrode 12 is opposed in the thickness direction T to the portion excluding the first end face 10 e side end portion of the first inner electrode 11.
  • the second inner electrode 12 includes a second current collector 12a and a second active material layer 12b.
  • the second current collector 12a can be made of, for example, a metal foil made of at least one metal such as aluminum and copper.
  • the second active material layer 12 b is provided on the surface of the second current collector 12 a on the first inner electrode 11 side. Therefore, a part of the second active material layer 12 b is opposed to a part of the first active material layer 11 b in the thickness direction T.
  • the second active material layer 12 b contains an active material.
  • the second active material layer 12 b constitutes a polarizable electrode.
  • the second active material layer 12 b as the polarizable electrode contains, for example, a carbon material such as activated carbon as an active material.
  • the second inner electrode 12 is drawn to the second end face 10f, but is not drawn to the first and second side faces 10c and 10d and the first end face 10e. Specifically, in the present embodiment, as shown in FIG. 2, only the second current collector 12a of the second inner electrode 12 is exposed at the second end face 10f.
  • An electrolyte layer 13 is provided between the first active material layer 11 b of the first inner electrode 11 and the second active material layer 12 b of the second inner electrode 12.
  • the electrolyte layer 13 is a layer containing an electrolytic solution.
  • the electrolyte layer 13 may be constituted by a gel electrolyte which is a gel electrolyte containing an electrolytic solution, or may be constituted by a porous body such as a separator impregnated with the electrolytic solution.
  • a gel electrolyte high molecular polyethylene oxide containing an electrolyte etc. are mentioned, for example.
  • electrolyte examples include, for example, ionic liquids such as EMITFSI (1-ethyl-3-methylimidazolium bis (trifluoromethanesulfonyl) imide), EMIBF4 (1-ethyl-3-methylimidazolium borofluoride), or A solution obtained by dissolving the ionic liquid in an organic solvent such as propylene carbonate or acetonitrile can be used. Only one of these electrolytes may be used, or a plurality of types may be mixed and used.
  • ionic liquids such as EMITFSI (1-ethyl-3-methylimidazolium bis (trifluoromethanesulfonyl) imide), EMIBF4 (1-ethyl-3-methylimidazolium borofluoride), or A solution obtained by dissolving the ionic liquid in an organic solvent such as propylene carbonate or acetonitrile can be used. Only one of these electrolytes may be used, or a
  • the electrolyte layer 13 has a first electrolyte layer 13a and a second electrolyte layer 13b.
  • the first electrolyte layer 13a is provided on the first active material layer 11b.
  • the second electrolyte layer 13 b is provided on the second active material layer 12 b.
  • the first electrolyte layer 13a and the second electrolyte layer 13b are in contact with each other so that the electrolytes can move relative to each other. It is preferable that the first electrolyte layer 13a and the second electrolyte layer 13b be in close contact with each other.
  • the storage device 1 further includes a first insulating adhesive layer 15a and a second insulating adhesive layer 15b.
  • the first insulating adhesive layer 15a covers the periphery of the first active material layer 11b and the first electrolyte layer 13a. For this reason, the first active material layer 11 b and the first electrolyte layer 13 a are formed of the first insulating adhesive layer 15 a from the first and second side faces 10 c and 10 d and the first and second end faces 10 e and 10 f. It is isolated by
  • the second insulating adhesive layer 15 b covers the periphery of the second active material layer 12 b and the second electrolyte layer 13 b.
  • the second active material layer 12b and the second electrolyte layer 13b are formed of the second insulating adhesive layer 15b from the first and second side faces 10c and 10d and the first and second end faces 10e and 10f. It is isolated by The second insulating adhesive layer 15 b and the first insulating adhesive layer 15 a are bonded.
  • Each of the first and second insulating adhesive layers 15a and 15b is made of a resin composition in which an inorganic filler is dispersed.
  • a resin used preferably, a urethane resin, an acrylic resin, an epoxy resin, a polyimide resin, a silicone resin etc. are mentioned. Only one of these resins may be used, or a plurality of resins may be used.
  • the inorganic filler preferably used for the first and second insulating adhesive layers 15a and 15b include, for example, aluminum oxide, silicon oxide, titanium oxide, magnesium oxide, zirconium oxide, zircon, silicon carbide, aluminum phosphate , Aluminum nitride, silicon nitride, steatite, cordierite, mullite, sialon and the like. Only one type of these inorganic fillers may be used, or a plurality of types may be used.
  • the first insulating adhesive layer 15a has a first portion 15a1 and a second portion 15a2.
  • the first portion 15a1 covers the periphery of the first active material layer 11b.
  • the second portion 15a2 is provided on the first portion 15a1 and covers the first electrolyte layer 13a.
  • the second portion 15a2 is bonded to the second insulating adhesive layer 15b.
  • the first portion 15a1 and the second portion 15a2 may be provided integrally or separately. In this embodiment, an example in which the first portion 15a1 and the second portion 15a2 are provided separately will be described.
  • the second insulating adhesive layer 15 b has a third portion 15 b 1 and a fourth portion 15 b 2.
  • the third portion 15b1 covers the periphery of the second active material layer 12b.
  • the fourth portion 15b2 is provided on the third portion 15b1 and covers the second electrolyte layer 13b.
  • the fourth portion 15b2 is bonded to the second portion 15a2.
  • the third portion 15b1 and the fourth portion 15b2 may be provided integrally or separately. In this embodiment, an example in which the third portion 15b1 and the fourth portion 15b2 are separately provided will be described.
  • the pair of first and second inner electrodes 11 and 12, the electrolyte layer 13, and the first and second insulating adhesive layers 15a and 15b constitute one storage unit 17.
  • a plurality of storage units 17 are stacked, and the stack of the plurality of storage units 17 constitutes the functional unit 10A.
  • the storage units 17 adjacent in the stacking direction T are bonded by the adhesive layer 16.
  • the storage units 17 located in the uppermost layer and the lowermost layer in the stacking direction T are bonded to the inner surface of the exterior body 10B by the adhesive layer 16.
  • the present invention is not limited to the above configuration.
  • the power storage device according to the present invention may have only one power storage unit.
  • the storage unit may be formed of a laminate of a plurality of pairs of first and second inner electrodes 11 and 12 sandwiching the electrolyte layer.
  • An exterior body 10B is provided outside the functional unit 10A.
  • the exterior body 10B has a function of suppressing the intrusion of water or the like into the functional unit 10A, and a function of suppressing the leakage of the electrolytic solution from the functional unit 10A.
  • the exterior body 10B can be made of, for example, an epoxy resin such as a naphthalene epoxy resin, a liquid crystal polymer, or the like.
  • the exterior body 10B is provided to cover the first and second main surfaces 10a and 10b and the first and second side surfaces 10c and 10d of the functional unit 10A.
  • the first and second end faces 10e and 10f of the functional unit 10A are exposed from the exterior body 10B.
  • a first external electrode 18 electrically connected to the first internal electrode 11 is provided on the first end face 10 e.
  • the first external electrode 18 has a first electrode film 18a, a first conductive adhesive layer 18b, and a first metal cap 18c.
  • a first electrode film 18a is provided on the first end face 10e. Substantially the entire first end face 10 e is covered by the first electrode film 18 a.
  • the first metal cap 18 c covers a portion on the first end face 10 e side of the device body 10. Specifically, the first metal cap 18c includes the first end face 10e, the first and second main faces 10a and 10b, and the first and second side faces 10c and 10d, respectively. Cover the side part.
  • a first conductive adhesive layer 18 b is provided between the first metal cap 18 c and the first electrode film 18 a. The first metal cap 18c and the first electrode film 18a are electrically connected and bonded together by the first conductive adhesive layer 18b.
  • a second outer electrode 19 electrically connected to the second inner electrode 12 is provided on the second end face 10 f.
  • the exposed portion from the exterior body 10B of the functional portion 10A is covered by the second external electrode 19 and the first external electrode 18.
  • the second external electrode 19 has a second electrode film 19a, a second conductive adhesive layer 19b, and a second metal cap 19c.
  • a second electrode film 19a is provided on the second end face 10f.
  • the second electrode film 19a covers substantially the entire second end face 10f.
  • the second metal cap 19 c covers a portion on the second end face 10 f side of the device body 10.
  • the second metal cap 19c includes the second end face 10f, the first and second main faces 10a and 10b, and the first and second side faces 10c and 10d, respectively. Cover the side part.
  • a second conductive adhesive layer 19b is provided between the second metal cap 19c and the second electrode film 19a. The second metal cap 19c and the second electrode film 19a are electrically connected and bonded together by the second conductive adhesive layer 19b.
  • Each of the first and second electrode films 18a and 19a is formed of a sprayed film.
  • the first and second electrode films 18a and 19a can be made of, for example, at least one metal selected from the group consisting of Al, Cu, and Al-Si.
  • the first and second metal caps 18c and 19c are, for example, a base material containing an alloy (Fe-42Ni alloy), a base material made of aluminum or an aluminum alloy, a base material made of copper or a copper alloy, It can be comprised by Ni / Ag plating which covers the surface, or Ni / Au plating.
  • a base material containing an alloy Fe-42Ni alloy
  • a base material made of aluminum or an aluminum alloy a base material made of copper or a copper alloy
  • It can be comprised by Ni / Ag plating which covers the surface, or Ni / Au plating.
  • the first and second insulating adhesive layers 15a and 15b are made of a resin composition containing a resin. For this reason, the electrolytic solution contained in the first and second electrolyte layers 13a and 13b permeates into the first and second insulating adhesive layers 15a and 15b, and the first and second insulating adhesive layers 15a and 15b, There is a possibility that 15b may swell. When the electrolyte solution contained in the first and second electrolyte layers 13a and 13b penetrates into the first and second insulating adhesive layers 15a and 15b, the electrolyte solution in the first and second electrolyte layers 13a and 13b The amount decreases. Therefore, the storage characteristic of the storage device 1 is degraded.
  • an inorganic filler is added to at least first and third portions 15a1 and 15b1 of the first and second insulating adhesive layers 15a and 15b. For this reason, it is suppressed that the electrolyte solution contained in 1st and 2nd electrolyte layer 13a, 13b infiltrates in the 1st and 2nd insulating contact bonding layer 15a, 15b. From the viewpoint of suppressing the permeation of the electrolytic solution into the first and second insulating adhesive layers 15a and 15b, many inorganic fillers are added to the entire first and second insulating adhesive layers 15a and 15b. Is preferred.
  • the adhesive strength between the second portion 15a2 and the fourth portion 15b2 may be reduced.
  • the electrolyte leaks from between the second portion 15a2 and the fourth portion 15b2, and the first and second electrolyte layers are produced. There is a possibility that the amount of electrolytic solution in 13a and 13b may decrease.
  • the content of the inorganic filler in the second portion 15a2 is smaller than the content of the inorganic filler in the first portion 15a1, and the content of the inorganic filler in the fourth portion 15b2 is It is less than the content of the inorganic filler in the portion 15 b 1 of 3. Therefore, it is effectively suppressed that the electrolytic solution infiltrates into the first and second insulating adhesive layers 15a and 15b by adding the inorganic filler to the first and second insulating adhesive layers 15a and 15b. While the adhesive strength between the second portion 15a2 and the fourth portion 15b2 is increased, and the leakage of the electrolyte from between the second portion 15a2 and the fourth portion 15b2 is effectively suppressed. . Therefore, the reduction of the electrolytic solution in the first and second electrolyte layers 13a and 13b can be suppressed. As a result, it is possible to realize the storage device 1 in which storage characteristics are not easily deteriorated.
  • the content of the inorganic filler in the first portion 15a1 is 5% by mass or more and 40% by mass or less Is preferable, and 10% by mass or more and 30% by mass or less is more preferable. Further, the electrolytic solution leakage from the second portion 15a2 and the fourth portion 15b2 can be more effectively suppressed to further reduce the electrolytic solution in the first and second electrolyte layers 13a and 13b.
  • the content of the inorganic filler in 2nd and 4th part 15a2 and 15b2 is set from the viewpoint of more effectively suppressing the electrolyte solution from invading the first and second insulating adhesive layers 15a and 15b.
  • the content is preferably 5% by mass or more, and more preferably 10% by mass or more.
  • each of t2 / t1 and t4 / t3 is preferably 1.0 or less, and more preferably 0.55 or less. However, if t2 / t1 and t4 / t3 are too small, the adhesive strength between the second portion 15a2 and the fourth portion 15b2 may be too low. Therefore, each of t2 / t1 and t4 / t3 is preferably 0.1 or more, and more preferably 0.25 or more.
  • t1 thickness of first portion 15a1, 18 to 22 ⁇ m t2: Thickness of second portion 15a2, 6 to 8 ⁇ m t3: Thickness of third portion 15b1, 18 to 22 ⁇ m t4: Thickness of second portion 15b2, 6 to 8 ⁇ m It is.
  • T1 to t4 can be measured using an ultrasonic thickness gauge or the like.
  • the preferable average particle diameter of the inorganic filler in the first and second insulating adhesive layers 15a and 15b is preferably 0.2 ⁇ m to 0.9 ⁇ m, and more preferably 0.5 ⁇ m to 3.0 ⁇ m. Is more preferred.
  • the average particle size of the inorganic filler can be determined by measuring the particle size distribution using LA-960 (laser diffraction / scattering type particle size distribution measuring device) manufactured by Horiba, Ltd.
  • the storage device 1 when the storage device 1 is reflow-mounted, heat is applied to the storage device 1, and when the temperature rises, the internal pressure in the storage device 1 rises.
  • the internal pressure of the storage device 1 depends on the amount of gasification of impurities and water present inside the storage device 1. Then, as the internal stress of the storage device 1 becomes higher, the amount of deformation of the storage device 1 (in particular, the amount of deformation of the exterior body 10B) becomes larger. Therefore, the higher the internal stress of the storage device 1, the easier it is to be damaged when the temperature of the storage device 1 rises.
  • the first insulating adhesive layer 15 a covers both sides in the length direction L of the first electrolyte layer 13 a and both sides in the width direction W.
  • the second insulating adhesive layer 15 b covers both sides in the length direction L of the second electrolyte layer 13 b and both sides in the width direction W.
  • the first and second insulating adhesive layers 15a and 15b contain an inorganic filler. Therefore, the first and second active material layers 11b and 12b are covered with the first and second insulating adhesive layers 15a and 15b at both sides in the length direction L and at both sides in the width direction W from the outside. Moisture and impurities do not easily enter. Thus, the amount of water in the storage device 1 is difficult to increase.
  • the entry of moisture, impurities and the like into the storage device 1 is more effectively suppressed. Therefore, when the temperature of the storage device 1 rises, damage to the storage device 1 caused by the increase in the internal pressure of the storage device 1 is more effectively suppressed. In other words, the storage device 1 is unlikely to be damaged even when the temperature of the storage device rises. That is, the storage device 1 has excellent temperature durability.
  • the inorganic filler contained in the first and second insulating adhesive layers 15 a and 15 b is less than the oil absorption of the active material (active material particles) contained in the active material layers 11 b and 12 b.
  • the active material active material particles contained in the active material layers 11 b and 12 b.
  • the oil absorption can be measured in accordance with the test method defined in JIS K5101-13-2.
  • the oil absorption of the inorganic filler is preferably 5% by mass or less, and 4% by mass or less It is more preferable to do.
  • the oil absorption of the inorganic filler is preferably 0.5 times or less of the oil absorption of the active material (active material particles) contained in the active material layers 11b and 12b, and more preferably 0.1 times or less.
  • each of the first and second insulating adhesive layers 15a and 15b is preferably 20 ⁇ m or more and 25 ⁇ m or less.
  • the strength of the first and second insulating adhesive layers 15a and 15b can be improved. .
  • the strength of the power storage device 1 is improved. Therefore, breakage of the storage device 1 is more effectively suppressed in the manufacturing process, mounting process, and the like of the storage device 1.
  • first portion 15a1 and the second portion 15a2 are separate bodies.
  • first part and the second part may be integrally provided.
  • the content of the inorganic filler in the first insulating adhesive layer may be decreased stepwise or gradually toward the second insulating adhesive layer side.
  • the third part and the fourth part may be integrally provided. In that case, the content of the inorganic filler in the second insulating adhesive layer may be decreased stepwise or gradually toward the first insulating adhesive layer side.
  • Method of Manufacturing Storage Device 1 (Method of Manufacturing Storage Device 1)
  • an example of the manufacturing method of the electrical storage device 1 will be described.
  • the method of manufacturing the electricity storage device according to the present invention is not limited to the following manufacturing method.
  • a paste containing active material particles, a conductive material, and the like is printed on a current collector made of aluminum foil or the like using a printing method such as screen printing, and the electrode is formed by drying.
  • a paste containing an inorganic filler and a resin is printed using a printing method such as a screen printing method so as to cover the outer periphery of the active material layer, and then dried. Form a first or third part of the layer.
  • a paste containing an inorganic filler and a resin is printed using a printing method such as screen printing and dried to form a second or fourth portion of the insulating adhesive layer.
  • a paste used for formation of this 2nd or 4th part the paste in which content of an inorganic filler is smaller than the paste used in order to form a 1st or 3rd part is used.
  • a paste containing an electrolytic solution is printed using a printing method such as a screen printing method to form an electrolyte layer on the active material layer.
  • the active material layers of the two laminates produced as described above are in contact with each other, and the current collector of one laminate is exposed at one end face in the lengthwise direction, and the collection of the other laminate is performed.
  • the electricity storage unit is manufactured by stacking and pressing so that the current collector is exposed on the other end surface in the lengthwise direction.
  • a plurality of power storage units are stacked with an adhesive interposed, and the adhesive is cured to produce a functional unit.
  • the exterior body can be provided, for example, by a resin mold or a resin case.
  • an electrode film is formed on each end face where the current collector is exposed, using a thin film forming method such as thermal spraying or sputtering.
  • a conductive adhesive is applied on each electrode film and then covered with a metal cap, and the conductive adhesive is cured, whereby the storage device 1 can be completed.
  • first storage device 10 device body 10A: functional unit 10B: exterior body 10a: first main surface 10b: second main surface 10c: first side 10d: second side 10e: first end 10f: Second end face 11: first inner electrode 11a: first current collector 11b: first active material layer 12: second inner electrode 12a: second current collector 12b: second active material layer 13: electrolyte layer 13a: first electrolyte layer 13b: second electrolyte layer 15a: first insulating adhesive layer 15a1: first portion 15a2: second portion 15b: second insulating adhesive layer 15b1: Third portion 15b2: fourth portion 16: adhesive layer 17: storage unit 18: first external electrode 18a: first electrode film 18b: first conductive adhesive layer 18c: first metal cap 19: Second outside Part electrode 19a: second electrode film 19b: second conductive adhesive layer 19c: second metal cap

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Abstract

Provided is an electricity storage device which is not susceptible to deterioration in the electricity storage characteristics. With respect to an electricity storage device 1 according to the present invention, a first insulating bonding layer 15a comprises a first portion 15a1 that covers the periphery of a first active material layer 11b and a second portion 15a2 that covers the periphery of a first electrolyte layer 13a. The second portion 15a2 is bonded to a second insulating bonding layer 15b. The second insulating bonding layer 15b comprises a third portion 15b1 that covers the periphery of a second active material layer 12b and a fourth portion 15b2 that covers the periphery of a second electrolyte layer 13b. The fourth portion 15b2 is bonded to the second portion 15a2. The content of an inorganic filler in the second portion 15a2 is lower than the content of the inorganic filler in the first portion 15a1. The content of the inorganic filler in the fourth portion 15b2 is lower than the content of the inorganic filler in the third portion 15b1.

Description

蓄電デバイスPower storage device
　本発明は、蓄電デバイスに関する。 The present invention relates to a power storage device.
　従来、電気二重層コンデンサや二次電池などの蓄電デバイスが種々知られている。例えば特許文献１には、その一例が記載されている。特許文献１には、活物質層の周囲が絶縁性を有するセパレータで覆われた蓄電デバイスが記載されている。 Conventionally, various storage devices such as an electric double layer capacitor and a secondary battery are known. For example, Patent Document 1 describes an example thereof. Patent Document 1 describes a power storage device in which the periphery of an active material layer is covered with a separator having an insulating property.
国際公開第２０１３／０９９５４１号公報International Publication 2013/099541
　蓄電デバイスの蓄電特性は、電解質層に保持されている電解液の量が減少すると低下する。このため、蓄電デバイスの優れた蓄電特性を維持する観点からか、電解質層に電解液を確実に保持しておく必要がある。 The storage characteristic of the storage device decreases as the amount of the electrolyte held in the electrolyte layer decreases. For this reason, it is necessary to reliably hold the electrolytic solution in the electrolyte layer from the viewpoint of maintaining the excellent storage characteristics of the storage device.
　本発明の主な目的は、蓄電特性が劣化し難い蓄電デバイスを提供することにある。　 The main object of the present invention is to provide a storage device in which storage characteristics are unlikely to deteriorate.
　本発明に係る蓄電デバイスは、第１の内部電極と、第１の電解質層と、第１の絶縁性接着層と、第２の内部電極と、第２の電解質層と、第２の絶縁性接着層とを備える。第１の内部電極は、長さ方向及び幅方向に沿って延びている。第１の内部電極は、第１の集電体と、第１の活物質層とを有する。第１の活物質層は、第１の集電体の上に設けられている。第１の電解質層は、第１の活物質層の上に配されている。第１の絶縁性接着層は、第１の活物質層及び第１の電解質層の周囲を覆っている。第１の絶縁性接着層は、無機フィラーが分散した樹脂組成物からなる。第２の内部電極は、第１の内部電極に対して厚み方向に積層されている。第２の内部電極は、第２の集電体と、第２の活物質層とを有する。第２の活物質層は、第２の集電体の上に設けられている。第２の電解質層は、第２の活物質層の上に配されている。第２の電解質層は、第１の電解質層と接触している。第２の絶縁性接着層は、第２の活物質層及び第２の電解質層の周囲を覆っている。第２の絶縁性接着層は、無機フィラーが分散した樹脂組成物からなる。第２の絶縁性接着層は、第１の絶縁性接着層と接着されている。第１の絶縁性接着層は、第１の部分と、第２の部分とを有する。第１の部分は、第１の活物質層の周囲を覆っている。第２の部分は、第１の電解質層の周囲を覆っている。第２の部分は、第２の絶縁性接着層と接着されている。第２の絶縁性接着層は、第３の部分と、第４の部分とを有する。第３の部分は、第２の活物質層の周囲を覆っている。第４の部分は、第２の電解質層の周囲を覆っている。第４の部分は、第２の部分と接着されている。第２の部分における無機フィラーの含有量は、第１の部分における無機フィラーの含有量よりも少ない。第４の部分における無機フィラーの含有量は、第３の部分における無機フィラーの含有量よりも少ない。 An electricity storage device according to the present invention comprises a first internal electrode, a first electrolyte layer, a first insulating adhesive layer, a second internal electrode, a second electrolyte layer, and a second insulating property. And an adhesive layer. The first inner electrode extends along the length direction and the width direction. The first inner electrode has a first current collector and a first active material layer. The first active material layer is provided on the first current collector. The first electrolyte layer is disposed on the first active material layer. The first insulating adhesive layer covers the periphery of the first active material layer and the first electrolyte layer. The first insulating adhesive layer is made of a resin composition in which an inorganic filler is dispersed. The second inner electrode is stacked in the thickness direction with respect to the first inner electrode. The second inner electrode has a second current collector and a second active material layer. The second active material layer is provided on the second current collector. The second electrolyte layer is disposed on the second active material layer. The second electrolyte layer is in contact with the first electrolyte layer. The second insulating adhesive layer covers the periphery of the second active material layer and the second electrolyte layer. The second insulating adhesive layer is made of a resin composition in which an inorganic filler is dispersed. The second insulating adhesive layer is bonded to the first insulating adhesive layer. The first insulating adhesive layer has a first portion and a second portion. The first portion covers the periphery of the first active material layer. The second portion covers the periphery of the first electrolyte layer. The second portion is bonded to the second insulating adhesive layer. The second insulating adhesive layer has a third portion and a fourth portion. The third portion covers the periphery of the second active material layer. The fourth portion covers the periphery of the second electrolyte layer. The fourth portion is bonded to the second portion. The content of the inorganic filler in the second part is less than the content of the inorganic filler in the first part. The content of the inorganic filler in the fourth part is less than the content of the inorganic filler in the third part.
　本発明に係る蓄電デバイスでは、樹脂組成物からなる絶縁性接着層に無機フィラーが含まれている。このため、電解質層に含まれる電解液が絶縁性接着層内に浸入し、絶縁性接着層が膨潤することが抑制されている。電解質層に含まれる電解液が絶縁性接着層内に浸入することを抑制する観点からは、絶縁性接着層の全体が多くの無機フィラーを含むことが好ましい。但し、その場合は、第２及び第４の部分における無機フィラーの含有量が多くなる分、第２の部分と第４の部分との接着強度が低くなる。このため、第２の部分と第４の部分との間から電解液が漏洩したり、第２の部分と第４の部分とが剥離し、その剥離部から電解液が漏洩する虞がある。 In the electricity storage device according to the present invention, the inorganic filler is contained in the insulating adhesive layer made of the resin composition. For this reason, it is suppressed that the electrolyte solution contained in an electrolyte layer infiltrates in the insulating contact bonding layer, and swelling of the insulating contact bonding layer. From the viewpoint of suppressing the infiltration of the electrolytic solution contained in the electrolyte layer into the insulating adhesive layer, the whole of the insulating adhesive layer preferably contains many inorganic fillers. However, in such a case, since the content of the inorganic filler in the second and fourth portions increases, the adhesive strength between the second portion and the fourth portion decreases. For this reason, there is a possibility that the electrolytic solution may leak from between the second portion and the fourth portion, or the second portion and the fourth portion may peel, and the electrolytic solution may leak from the peeled portion.
　それに対して本発明に係る蓄電デバイスでは、第２の部分における無機フィラーの含有量は、第１の部分における無機フィラーの含有量よりも少ない。第４の部分における無機フィラーの含有量は、第３の部分における無機フィラーの含有量よりも少ない。すなわち、第２及び第４の部分の無機フィラーの含有量が相対的に低く、樹脂の含有量が相対的に高い。よって、第２の部分と第４の部分とが強固に接着されている。よって、第２の部分と第４の部分との間からの電解液の漏洩も効果的に抑制されている。このため、電解質層から電解液が漏洩しにくい。従って、本発明に係る蓄電デバイスの蓄電特性は劣化し難い。 On the other hand, in the electricity storage device according to the present invention, the content of the inorganic filler in the second part is smaller than the content of the inorganic filler in the first part. The content of the inorganic filler in the fourth part is less than the content of the inorganic filler in the third part. That is, the content of the inorganic filler in the second and fourth portions is relatively low, and the content of the resin is relatively high. Thus, the second part and the fourth part are firmly bonded. Therefore, the leakage of the electrolytic solution from between the second portion and the fourth portion is also effectively suppressed. For this reason, it is difficult for the electrolytic solution to leak from the electrolyte layer. Therefore, the storage characteristic of the storage device according to the present invention is unlikely to deteriorate.
　本発明に係る蓄電デバイスでは、第２及び第４の部分が無機フィラーを含まなくてもよい。 In the electricity storage device according to the present invention, the second and fourth portions may not contain the inorganic filler.
　本発明に係る蓄電デバイスでは、第１及び第２の電解質層は、それぞれ、電解液を含んでいてもよい。その場合、第１及び第２の絶縁性接着層に含まれる樹脂が電解液により膨潤する樹脂であってもよい。 In the electricity storage device according to the present invention, each of the first and second electrolyte layers may contain an electrolytic solution. In that case, the resin contained in the first and second insulating adhesive layers may be a resin which is swelled by the electrolytic solution.
　本発明に係る蓄電デバイスでは、第１の部分の厚みをｔ１とし、第２の部分の厚みをｔ２とし、第３の部分の厚みをｔ３とし、第４の部分の厚みをｔ４としたときに、ｔ２／ｔ１及びｔ４／ｔ３が、それぞれ０．５５以下であることが好ましい。 In the electric storage device according to the present invention, when the thickness of the first part is t1, the thickness of the second part is t2, the thickness of the third part is t3, and the thickness of the fourth part is t4. , T2 / t1 and t4 / t3 are each preferably 0.55 or less.
　本発明に係る蓄電デバイスでは、第１及び第２の活物質層が、それぞれ、活物質を含んでいてもよい。その場合、無機フィラーの吸油量が活物質の吸油量よりも低いことが好ましい。 In the electricity storage device according to the present invention, each of the first and second active material layers may contain an active material. In that case, it is preferable that the oil absorption of the inorganic filler is lower than the oil absorption of the active material.
　本発明に係る蓄電デバイスでは、無機フィラーが、酸化アルミニウム、酸化ケイ素、酸化チタン、酸化マグネシウム、酸化ジルコニウム、ジルコン、炭化ケイ素、リン酸アルミニウム、窒化アルミニウム、窒化ケイ素、ステアタイト、コージライト、ムライト及びサイアロンからなる群から選ばれた少なくとも一種を含んでいてもよい。 In the electricity storage device according to the present invention, the inorganic filler includes aluminum oxide, silicon oxide, titanium oxide, magnesium oxide, zirconium oxide, zircon, silicon carbide, aluminum phosphate, aluminum nitride, silicon nitride, steatite, cordierite, mullite and the like It may contain at least one selected from the group consisting of sialon.
　本発明によれば、蓄電特性が劣化し難い蓄電デバイスを提供することができる。 According to the present invention, it is possible to provide an electricity storage device in which the electricity storage characteristic is not easily deteriorated.
図１は、本発明の一実施形態に係る蓄電デバイスの模式的斜視図である。FIG. 1 is a schematic perspective view of a power storage device according to an embodiment of the present invention. 図２は、図１の線ＩＩ－ＩＩにおける模式的断面図である。FIG. 2 is a schematic cross-sectional view taken along line II-II in FIG. 図３は、図２の線ＩＩＩ－ＩＩＩにおける模式的断面図である。FIG. 3 is a schematic cross-sectional view taken along line III-III of FIG.
　以下、本発明を実施した好ましい形態の一例について説明する。但し、下記の実施形態は、単なる例示である。本発明は、下記の実施形態に何ら限定されない。 Hereinafter, an example of the preferable form which implemented this invention is demonstrated. However, the following embodiments are merely illustrative. The present invention is not at all limited to the following embodiments.
　また、実施形態等において参照する各図面において、実質的に同一の機能を有する部材は同一の符号で参照することとする。また、実施形態等において参照する図面は、模式的に記載されたものである。図面に描画された物体の寸法の比率などは、現実の物体の寸法の比率などとは異なる場合がある。図面相互間においても、物体の寸法比率等が異なる場合がある。具体的な物体の寸法比率等は、以下の説明を参酌して判断されるべきである。 Moreover, in each drawing referred in the embodiment etc., members having substantially the same functions are referred to by the same reference numerals. The drawings referred to in the embodiments and the like are schematically described. The ratio of dimensions of objects drawn in the drawing may differ from the ratio of dimensions of real objects. The dimensional ratio of the object may differ between the drawings. Specific dimensional ratios and the like of objects should be determined in consideration of the following description.
　図１は、本実施形態に係る蓄電デバイスの模式的斜視図である。図２は、図１の線ＩＩ－ＩＩにおける模式的断面図である。図３は、図２の線ＩＩＩ－ＩＩＩにおける模式的断面図である。 FIG. 1 is a schematic perspective view of a power storage device according to the present embodiment. FIG. 2 is a schematic cross-sectional view taken along line II-II in FIG. FIG. 3 is a schematic cross-sectional view taken along line III-III of FIG.
　図１～図３に示す蓄電デバイス１は、例えば、電気二重層コンデンサや、二次電池を構成するデバイスである。 The power storage device 1 shown in FIGS. 1 to 3 is, for example, a device that constitutes an electric double layer capacitor or a secondary battery.
　蓄電デバイス１は、デバイス本体１０を備えている。図２及び図３に示すように、デバイス本体１０は、機能部１０Ａと、外装体１０Ｂとを有する。 The storage device 1 includes a device body 10. As shown in FIGS. 2 and 3, the device body 10 includes a functional unit 10A and an exterior body 10B.
　機能部１０Ａは、少なくとも一部が蓄電デバイスとしての機能を発現する部分である。機能部１０Ａは、直方体状に設けられている。機能部１０Ａは、第１及び第２の主面１０ａ、１０ｂと、第１及び第２の側面１０ｃ、１０ｄ（図３を参照。）と、第１及び第２の端面１０ｅ、１０ｆ（図２を参照。）とを有する。第１及び第２の主面１０ａ、１０ｂは、長さ方向Ｌ及び幅方向Ｗに沿って延びている。第１の主面１０ａと第２の主面１０ｂとは、厚み方向Ｔにおいて対向している。図３に示すように、第１及び第２の側面１０ｃ、１０ｄは、長さ方向Ｌ及び厚み方向Ｔに沿って延びている。第１の側面１０ｃと第２の側面１０ｄとは、幅方向Ｗにおいて対向している。図２に示すように、第１及び第２の端面１０ｅ、１０ｆは、幅方向Ｗ及び厚み方向Ｔに沿って延びている。第１の端面１０ｅと第２の端面１０ｆとは、長さ方向Ｌにおいて対向している。 The functional unit 10A is a portion at least a part of which exhibits a function as a power storage device. The functional unit 10A is provided in a rectangular shape. The functional unit 10A has first and second main surfaces 10a and 10b, first and second side surfaces 10c and 10d (see FIG. 3), and first and second end surfaces 10e and 10f (FIG. 2). See)). The first and second major surfaces 10 a and 10 b extend along the length direction L and the width direction W. The first major surface 10 a and the second major surface 10 b are opposed in the thickness direction T. As shown in FIG. 3, the first and second side surfaces 10 c and 10 d extend along the length direction L and the thickness direction T. The first side surface 10 c and the second side surface 10 d face each other in the width direction W. As shown in FIG. 2, the first and second end faces 10 e and 10 f extend in the width direction W and the thickness direction T. The first end face 10 e and the second end face 10 f are opposed in the length direction L.
　なお、本発明において、「直方体状」には、角部や稜線部が、面取り状や丸められた形状を有する直方体状が含まれるものとする。 In the present invention, the “cuboid shape” includes a rectangular shape having a chamfered shape or a rounded shape at a corner portion or a ridge portion.
　機能部１０Ａは、第１の内部電極１１と、第２の内部電極１２と、電解質層１３とを有する。 The functional unit 10 </ b> A includes a first inner electrode 11, a second inner electrode 12, and an electrolyte layer 13.
　第１の内部電極１１は、長さ方向Ｌ及び幅方向Ｗに沿って延びている。第１の内部電極１１は、第１及び第２の主面１０ａ、１０ｂと平行に設けられている。 The first inner electrode 11 extends along the length direction L and the width direction W. The first inner electrode 11 is provided in parallel to the first and second main surfaces 10a and 10b.
　第１の内部電極１１は、第１の集電体１１ａと、第１の活物質層１１ｂとを有する。 The first inner electrode 11 has a first current collector 11a and a first active material layer 11b.
　第１の集電体１１ａは、例えば、アルミニウム、銅等の少なくとも一種の金属からなる金属箔等により構成することができる。 The first current collector 11a can be made of, for example, a metal foil made of at least one metal such as aluminum and copper.
　なお、本発明において、「金属」には、合金が含まれるものとする。 In the present invention, "metal" includes alloys.
　第１の集電体１１ａの一方側の表面の上には、第１の活物質層１１ｂが設けられている。第１の活物質層１１ｂは、活物質を含む。蓄電デバイス１が電気二重層コンデンサを構成している場合には、第１の活物質層１１ｂは、分極性電極を構成している。蓄電デバイス１が電気二重層コンデンサを構成している場合は、分極性電極としての第１の活物質層１１ｂは、例えば、活性炭などの炭素材料を活物質として含んでいることが好ましい。 A first active material layer 11 b is provided on the surface on one side of the first current collector 11 a. The first active material layer 11 b contains an active material. When the storage device 1 constitutes an electric double layer capacitor, the first active material layer 11 b constitutes a polarizable electrode. When the storage device 1 constitutes an electric double layer capacitor, it is preferable that the first active material layer 11b as the polarizable electrode contains, for example, a carbon material such as activated carbon as an active material.
　第１の内部電極１１は、第１の端面１０ｅに引き出されている一方、第１及び第２の側面１０ｃ、１０ｄ並びに第２の端面１０ｆには引き出されていない。具体的には、本実施形態では、図２に示すように、第１の内部電極１１のうち、第１の集電体１１ａのみが第１の端面１０ｅに露出している。 The first inner electrode 11 is drawn to the first end face 10e, but is not drawn to the first and second side faces 10c and 10d and the second end face 10f. Specifically, in the present embodiment, as shown in FIG. 2, only the first current collector 11a of the first inner electrode 11 is exposed at the first end face 10e.
　第２の内部電極１２は、長さ方向Ｌ及び幅方向Ｗに沿って延びている。第２の内部電極１２は、第１及び第２の主面１０ａ、１０ｂと平行に設けられている。第２の内部電極１２は、第１の内部電極１１に対して厚み方向Ｔに積層されている。第２の内部電極１２の第２の端面１０ｆ側端部を除いた部分は、第１の内部電極１１の第１の端面１０ｅ側端部を除いた部分と厚み方向Ｔにおいて対向している。 The second inner electrode 12 extends along the length direction L and the width direction W. The second inner electrode 12 is provided in parallel to the first and second main surfaces 10a and 10b. The second inner electrode 12 is stacked in the thickness direction T with respect to the first inner electrode 11. The portion excluding the second end face 10 f side end portion of the second inner electrode 12 is opposed in the thickness direction T to the portion excluding the first end face 10 e side end portion of the first inner electrode 11.
　第２の内部電極１２は、第２の集電体１２ａと、第２の活物質層１２ｂとを有する。 The second inner electrode 12 includes a second current collector 12a and a second active material layer 12b.
　第２の集電体１２ａは、例えば、アルミニウム、銅等の少なくとも一種の金属からなる金属箔により構成することができる。 The second current collector 12a can be made of, for example, a metal foil made of at least one metal such as aluminum and copper.
　第２の活物質層１２ｂは、第２の集電体１２ａの第１の内部電極１１側表面上に設けられている。従って、第２の活物質層１２ｂの一部は、第１の活物質層１１ｂの一部と厚み方向Ｔにおいて対向している。第２の活物質層１２ｂは、活物質を含む。蓄電デバイス１が電気二重層コンデンサを構成している場合には、第２の活物質層１２ｂは、分極性電極を構成している。蓄電デバイス１が電気二重層コンデンサを構成している場合は、分極性電極としての第２の活物質層１２ｂは、例えば、活性炭などの炭素材料を活物質として含んでいることが好ましい。 The second active material layer 12 b is provided on the surface of the second current collector 12 a on the first inner electrode 11 side. Therefore, a part of the second active material layer 12 b is opposed to a part of the first active material layer 11 b in the thickness direction T. The second active material layer 12 b contains an active material. When the storage device 1 constitutes an electric double layer capacitor, the second active material layer 12 b constitutes a polarizable electrode. When the storage device 1 constitutes an electric double layer capacitor, it is preferable that the second active material layer 12 b as the polarizable electrode contains, for example, a carbon material such as activated carbon as an active material.
　第２の内部電極１２は、第２の端面１０ｆに引き出されている一方、第１及び第２の側面１０ｃ、１０ｄ並びに第１の端面１０ｅには引き出されていない。具体的には、本実施形態では、図２に示すように、第２の内部電極１２のうち、第２の集電体１２ａのみが第２の端面１０ｆに露出している。 The second inner electrode 12 is drawn to the second end face 10f, but is not drawn to the first and second side faces 10c and 10d and the first end face 10e. Specifically, in the present embodiment, as shown in FIG. 2, only the second current collector 12a of the second inner electrode 12 is exposed at the second end face 10f.
　第１の内部電極１１の第１の活物質層１１ｂと、第２の内部電極１２の第２の活物質層１２ｂとの間には、電解質層１３が設けられている。電解質層１３は、電解液を含む層である。電解質層１３は、電解液を含むゲル状の電解質であるゲル電解質により構成されていてもよいし、電解液が含浸したセパレータ等の多孔質体により構成されていてもよい。ゲル電解質の具体例としては、例えば、電解質を含む高分子ポリエチレンオキサイド等が挙げられる。 An electrolyte layer 13 is provided between the first active material layer 11 b of the first inner electrode 11 and the second active material layer 12 b of the second inner electrode 12. The electrolyte layer 13 is a layer containing an electrolytic solution. The electrolyte layer 13 may be constituted by a gel electrolyte which is a gel electrolyte containing an electrolytic solution, or may be constituted by a porous body such as a separator impregnated with the electrolytic solution. As a specific example of a gel electrolyte, high molecular polyethylene oxide containing an electrolyte etc. are mentioned, for example.
　電解質の具体例としては、例えば、ＥＭＩＴＦＳＩ（１－エチル－３－メチルイミダゾリウムビス（トリフルオロメタンスルホニル）イミド）、ＥＭＩＢＦ４（ホウフッ化１－エチル－３－メチルイミダゾリウム）等のイオン性液体、又は、そのイオン性液体をプロピレンカーボネート、アセトニトリル等の有機溶媒に溶かしたものを用いることができる。これらの電解質のうちの１種のみを用いてもよいし、複数種類を混合して用いてもよい。 Specific examples of the electrolyte include, for example, ionic liquids such as EMITFSI (1-ethyl-3-methylimidazolium bis (trifluoromethanesulfonyl) imide), EMIBF4 (1-ethyl-3-methylimidazolium borofluoride), or A solution obtained by dissolving the ionic liquid in an organic solvent such as propylene carbonate or acetonitrile can be used. Only one of these electrolytes may be used, or a plurality of types may be mixed and used.
　具体的には、本実施形態では、電解質層１３は、第１の電解質層１３ａと、第２の電解質層１３ｂとを有する。第１の電解質層１３ａは、第１の活物質層１１ｂの上に設けられている。一方、第２の電解質層１３ｂは、第２の活物質層１２ｂの上に設けられている。第１の電解質層１３ａと第２の電解質層１３ｂとは、電解質が相互に移動可能なように接触している。第１の電解質層１３ａと第２の電解質層１３ｂとは、密着していることが好ましい。 Specifically, in the present embodiment, the electrolyte layer 13 has a first electrolyte layer 13a and a second electrolyte layer 13b. The first electrolyte layer 13a is provided on the first active material layer 11b. On the other hand, the second electrolyte layer 13 b is provided on the second active material layer 12 b. The first electrolyte layer 13a and the second electrolyte layer 13b are in contact with each other so that the electrolytes can move relative to each other. It is preferable that the first electrolyte layer 13a and the second electrolyte layer 13b be in close contact with each other.
　蓄電デバイス１は、第１の絶縁性接着層１５ａ及び第２の絶縁性接着層１５ｂをさらに備えている。 The storage device 1 further includes a first insulating adhesive layer 15a and a second insulating adhesive layer 15b.
　第１の絶縁性接着層１５ａは、第１の活物質層１１ｂ及び第１の電解質層１３ａの周囲を覆っている。このため、第１の活物質層１１ｂ及び第１の電解質層１３ａは、第１及び第２の側面１０ｃ、１０ｄ並びに第１及び第２の端面１０ｅ、１０ｆから、第１の絶縁性接着層１５ａにより隔離されている。 The first insulating adhesive layer 15a covers the periphery of the first active material layer 11b and the first electrolyte layer 13a. For this reason, the first active material layer 11 b and the first electrolyte layer 13 a are formed of the first insulating adhesive layer 15 a from the first and second side faces 10 c and 10 d and the first and second end faces 10 e and 10 f. It is isolated by
　一方、第２の絶縁性接着層１５ｂは、第２の活物質層１２ｂ及び第２の電解質層１３ｂの周囲を覆っている。このため、第２の活物質層１２ｂ及び第２の電解質層１３ｂは、第１及び第２の側面１０ｃ、１０ｄ並びに第１及び第２の端面１０ｅ、１０ｆから、第２の絶縁性接着層１５ｂにより隔離されている。第２の絶縁性接着層１５ｂと、第１の絶縁性接着層１５ａとは、接着されている。 On the other hand, the second insulating adhesive layer 15 b covers the periphery of the second active material layer 12 b and the second electrolyte layer 13 b. For this reason, the second active material layer 12b and the second electrolyte layer 13b are formed of the second insulating adhesive layer 15b from the first and second side faces 10c and 10d and the first and second end faces 10e and 10f. It is isolated by The second insulating adhesive layer 15 b and the first insulating adhesive layer 15 a are bonded.
　第１及び第２の絶縁性接着層１５ａ、１５ｂは、それぞれ、無機フィラーが分散した樹脂組成物からなる。 Each of the first and second insulating adhesive layers 15a and 15b is made of a resin composition in which an inorganic filler is dispersed.
　好ましく用いられる樹脂としては、ウレタン樹脂、アクリル樹脂、エポキシ樹脂、ポリイミド樹脂、シリコーン樹脂等が挙げられる。これらの樹脂のうちの１種のみを用いてもよいし、複数種類の樹脂を用いてもよい。 As a resin used preferably, a urethane resin, an acrylic resin, an epoxy resin, a polyimide resin, a silicone resin etc. are mentioned. Only one of these resins may be used, or a plurality of resins may be used.
　第１及び第２の絶縁性接着層１５ａ、１５ｂに好ましく用いられる無機フィラーの具体例としては、例えば、酸化アルミニウム、酸化ケイ素、酸化チタン、酸化マグネシウム、酸化ジルコニウム、ジルコン、炭化ケイ素、リン酸アルミニウム、窒化アルミニウム、窒化ケイ素、ステアタイト、コージライト、ムライト、サイアロン等が挙げられる。これらの無機フィラーの１種のみを用いてもよいし、複数種類を用いてもよい。 Specific examples of the inorganic filler preferably used for the first and second insulating adhesive layers 15a and 15b include, for example, aluminum oxide, silicon oxide, titanium oxide, magnesium oxide, zirconium oxide, zircon, silicon carbide, aluminum phosphate , Aluminum nitride, silicon nitride, steatite, cordierite, mullite, sialon and the like. Only one type of these inorganic fillers may be used, or a plurality of types may be used.
　詳細には、第１の絶縁性接着層１５ａは、第１の部分１５ａ１と、第２の部分１５ａ２とを有する。第１の部分１５ａ１は、第１の活物質層１１ｂの周囲を覆っている。第２の部分１５ａ２は、第１の部分１５ａ１の上に設けられており、第１の電解質層１３ａを覆っている。第２の部分１５ａ２は、第２の絶縁性接着層１５ｂと接着されている。なお、第１の部分１５ａ１と第２の部分１５ａ２とは、一体に設けられていてもよいし、別体に設けられていてもよい。本実施形態では、第１の部分１５ａ１と第２の部分１５ａ２とが別体に設けられている例について説明する。 In detail, the first insulating adhesive layer 15a has a first portion 15a1 and a second portion 15a2. The first portion 15a1 covers the periphery of the first active material layer 11b. The second portion 15a2 is provided on the first portion 15a1 and covers the first electrolyte layer 13a. The second portion 15a2 is bonded to the second insulating adhesive layer 15b. The first portion 15a1 and the second portion 15a2 may be provided integrally or separately. In this embodiment, an example in which the first portion 15a1 and the second portion 15a2 are provided separately will be described.
　第２の絶縁性接着層１５ｂは、第３の部分１５ｂ１と、第４の部分１５ｂ２とを有する。第３の部分１５ｂ１は、第２の活物質層１２ｂの周囲を覆っている。第４の部分１５ｂ２は、第３の部分１５ｂ１の上に設けられており、第２の電解質層１３ｂを覆っている。第４の部分１５ｂ２は、第２の部分１５ａ２と接着されている。なお、第３の部分１５ｂ１と、第４の部分１５ｂ２とは、一体に設けられていてもよいし、別体に設けられていてもよい。本実施形態では、第３の部分１５ｂ１と、第４の部分１５ｂ２とが別体に設けられている例について説明する。 The second insulating adhesive layer 15 b has a third portion 15 b 1 and a fourth portion 15 b 2. The third portion 15b1 covers the periphery of the second active material layer 12b. The fourth portion 15b2 is provided on the third portion 15b1 and covers the second electrolyte layer 13b. The fourth portion 15b2 is bonded to the second portion 15a2. The third portion 15b1 and the fourth portion 15b2 may be provided integrally or separately. In this embodiment, an example in which the third portion 15b1 and the fourth portion 15b2 are separately provided will be described.
　本実施形態の蓄電デバイス１では、一対の第１及び第２の内部電極１１，１２、電解質層１３並びに第１及び第２の絶縁性接着層１５ａ、１５ｂがひとつの蓄電ユニット１７を構成している。蓄電デバイス１では、蓄電ユニット１７が複数積層されており、この複数の蓄電ユニット１７の積層体が機能部１０Ａを構成している。なお、積層方向Ｔにおいて隣り合う蓄電ユニット１７は、接着層１６により接着されている。また、積層方向Ｔにおける最上層及び最下層のそれぞれに位置する蓄電ユニット１７は、外装体１０Ｂの内面に対して、接着層１６により接着されている。 In the storage device 1 of the present embodiment, the pair of first and second inner electrodes 11 and 12, the electrolyte layer 13, and the first and second insulating adhesive layers 15a and 15b constitute one storage unit 17. There is. In the storage device 1, a plurality of storage units 17 are stacked, and the stack of the plurality of storage units 17 constitutes the functional unit 10A. The storage units 17 adjacent in the stacking direction T are bonded by the adhesive layer 16. Further, the storage units 17 located in the uppermost layer and the lowermost layer in the stacking direction T are bonded to the inner surface of the exterior body 10B by the adhesive layer 16.
　もっとも、本発明は、上記構成に限定されない。例えば、本発明に係る蓄電デバイスは、蓄電ユニットをひとつのみ有していてもよい。蓄電ユニットは、電解質層を挟持する複数対の第１及び第２の内部電極１１，１２の積層体により構成されていてもよい。 However, the present invention is not limited to the above configuration. For example, the power storage device according to the present invention may have only one power storage unit. The storage unit may be formed of a laminate of a plurality of pairs of first and second inner electrodes 11 and 12 sandwiching the electrolyte layer.
　機能部１０Ａの外側には、外装体１０Ｂが設けられている。この外装体１０Ｂは、機能部１０Ａへの水分等の侵入を抑制する機能や、機能部１０Ａからの電解液の漏洩を抑制する機能を有している。外装体１０Ｂは、例えば、ナフタレン系エポキシ樹脂等のエポキシ樹脂、液晶ポリマーなどにより構成することができる。 An exterior body 10B is provided outside the functional unit 10A. The exterior body 10B has a function of suppressing the intrusion of water or the like into the functional unit 10A, and a function of suppressing the leakage of the electrolytic solution from the functional unit 10A. The exterior body 10B can be made of, for example, an epoxy resin such as a naphthalene epoxy resin, a liquid crystal polymer, or the like.
　外装体１０Ｂは、機能部１０Ａの第１及び第２の主面１０ａ、１０ｂ並びに第１及び第２の側面１０ｃ、１０ｄを覆うように設けられている。機能部１０Ａの第１及び第２の端面１０ｅ、１０ｆは、外装体１０Ｂから露出している。 The exterior body 10B is provided to cover the first and second main surfaces 10a and 10b and the first and second side surfaces 10c and 10d of the functional unit 10A. The first and second end faces 10e and 10f of the functional unit 10A are exposed from the exterior body 10B.
　図２に示すように、第１の端面１０ｅの上には、第１の内部電極１１に電気的に接続された第１の外部電極１８が設けられている。第１の外部電極１８は、第１の電極膜１８ａと、第１の導電性接着層１８ｂと、第１の金属キャップ１８ｃとを有する。 As shown in FIG. 2, a first external electrode 18 electrically connected to the first internal electrode 11 is provided on the first end face 10 e. The first external electrode 18 has a first electrode film 18a, a first conductive adhesive layer 18b, and a first metal cap 18c.
　第１の端面１０ｅの上には、第１の電極膜１８ａが設けられている。この第１の電極膜１８ａにより、第１の端面１０ｅの実質的に全体が覆われている。 A first electrode film 18a is provided on the first end face 10e. Substantially the entire first end face 10 e is covered by the first electrode film 18 a.
　第１の金属キャップ１８ｃは、デバイス本体１０の第１の端面１０ｅ側の部分を覆っている。具体的には、第１の金属キャップ１８ｃは、第１の端面１０ｅと、第１及び第２の主面１０ａ、１０ｂ並びに第１及び第２の側面１０ｃ、１０ｄのそれぞれの第１の端面１０ｅ側の部分を覆っている。第１の金属キャップ１８ｃと第１の電極膜１８ａとの間には、第１の導電性接着層１８ｂが設けられている。この第１の導電性接着層１８ｂにより、第１の金属キャップ１８ｃと第１の電極膜１８ａとが電気的に接続されていると共に、接着されている。 The first metal cap 18 c covers a portion on the first end face 10 e side of the device body 10. Specifically, the first metal cap 18c includes the first end face 10e, the first and second main faces 10a and 10b, and the first and second side faces 10c and 10d, respectively. Cover the side part. A first conductive adhesive layer 18 b is provided between the first metal cap 18 c and the first electrode film 18 a. The first metal cap 18c and the first electrode film 18a are electrically connected and bonded together by the first conductive adhesive layer 18b.
　第２の端面１０ｆの上には、第２の内部電極１２に電気的に接続された第２の外部電極１９が設けられている。この第２の外部電極１９と上記第１の外部電極１８とにより機能部１０Ａの外装体１０Ｂからの露出部が覆われている。第２の外部電極１９は、第２の電極膜１９ａと、第２の導電性接着層１９ｂと、第２の金属キャップ１９ｃとを有する。第２の端面１０ｆの上には、第２の電極膜１９ａが設けられている。この第２の電極膜１９ａにより、第２の端面１０ｆの実質的に全体が覆われている。 A second outer electrode 19 electrically connected to the second inner electrode 12 is provided on the second end face 10 f. The exposed portion from the exterior body 10B of the functional portion 10A is covered by the second external electrode 19 and the first external electrode 18. The second external electrode 19 has a second electrode film 19a, a second conductive adhesive layer 19b, and a second metal cap 19c. A second electrode film 19a is provided on the second end face 10f. The second electrode film 19a covers substantially the entire second end face 10f.
　第２の金属キャップ１９ｃは、デバイス本体１０の第２の端面１０ｆ側の部分を覆っている。具体的には、第２の金属キャップ１９ｃは、第２の端面１０ｆと、第１及び第２の主面１０ａ、１０ｂ並びに第１及び第２の側面１０ｃ、１０ｄのそれぞれの第２の端面１０ｆ側の部分を覆っている。第２の金属キャップ１９ｃと第２の電極膜１９ａとの間には、第２の導電性接着層１９ｂが設けられている。この第２の導電性接着層１９ｂにより、第２の金属キャップ１９ｃと第２の電極膜１９ａとが電気的に接続されていると共に、接着されている。 The second metal cap 19 c covers a portion on the second end face 10 f side of the device body 10. Specifically, the second metal cap 19c includes the second end face 10f, the first and second main faces 10a and 10b, and the first and second side faces 10c and 10d, respectively. Cover the side part. A second conductive adhesive layer 19b is provided between the second metal cap 19c and the second electrode film 19a. The second metal cap 19c and the second electrode film 19a are electrically connected and bonded together by the second conductive adhesive layer 19b.
　第１及び第２の電極膜１８ａ、１９ａは、それぞれ、溶射膜により構成されている。第１及び第２の電極膜１８ａ、１９ａは、例えば、Ａｌ、Ｃｕ、Ａｌ－Ｓｉからなる群から選ばれた少なくとも一種の金属により構成することができる。 Each of the first and second electrode films 18a and 19a is formed of a sprayed film. The first and second electrode films 18a and 19a can be made of, for example, at least one metal selected from the group consisting of Al, Cu, and Al-Si.
　第１及び第２の金属キャップ１８ｃ、１９ｃは、例えば、アロイ（Ｆｅ－４２Ｎｉ合金）を含む母材やアルミニウム又はアルミニウム合金からなる母材、銅又は銅合金からなる母材と、母材の外表面を覆うＮｉ／Ａｇめっき、又はＮｉ／Ａｕめっきとにより構成することができる。 The first and second metal caps 18c and 19c are, for example, a base material containing an alloy (Fe-42Ni alloy), a base material made of aluminum or an aluminum alloy, a base material made of copper or a copper alloy, It can be comprised by Ni / Ag plating which covers the surface, or Ni / Au plating.
　ところで、第１及び第２の絶縁性接着層１５ａ、１５ｂは、樹脂を含む樹脂組成物により構成されている。このため、第１及び第２の電解質層１３ａ、１３ｂに含まれる電解液が第１及び第２の絶縁性接着層１５ａ、１５ｂ内に浸入し、第１及び第２の絶縁性接着層１５ａ、１５ｂが膨潤する虞がある。第１及び第２の電解質層１３ａ、１３ｂに含まれる電解液が第１及び第２の絶縁性接着層１５ａ、１５ｂ内に浸入すると、第１及び第２の電解質層１３ａ、１３ｂ内の電解液量が減少する。このため、蓄電デバイス１の蓄電特性が劣化する。 The first and second insulating adhesive layers 15a and 15b are made of a resin composition containing a resin. For this reason, the electrolytic solution contained in the first and second electrolyte layers 13a and 13b permeates into the first and second insulating adhesive layers 15a and 15b, and the first and second insulating adhesive layers 15a and 15b, There is a possibility that 15b may swell. When the electrolyte solution contained in the first and second electrolyte layers 13a and 13b penetrates into the first and second insulating adhesive layers 15a and 15b, the electrolyte solution in the first and second electrolyte layers 13a and 13b The amount decreases. Therefore, the storage characteristic of the storage device 1 is degraded.
　蓄電デバイス１では、第１及び第２の絶縁性接着層１５ａ、１５ｂのうちの少なくとも第１及び第３の部分１５ａ１，１５ｂ１に無機フィラーが添加されている。このため、第１及び第２の電解質層１３ａ、１３ｂに含まれる電解液が第１及び第２の絶縁性接着層１５ａ、１５ｂ内に浸入することが抑制されている。電解液の第１及び第２の絶縁性接着層１５ａ、１５ｂ内への浸入を抑制する観点からは、第１及び第２の絶縁性接着層１５ａ、１５ｂの全体に多くの無機フィラーを添加することが好ましい。但し、第２及び第４の部分１５ａ２，１５ｂ２における無機フィラーの含有量を多くしすぎると、第２の部分１５ａ２と第４の部分１５ｂ２との間の接着強度が低くなる虞がある。第２の部分１５ａ２と第４の部分１５ｂ２との間の接着強度が低くなると、第２の部分１５ａ２と第４の部分１５ｂ２との間から電解液が漏洩し、第１及び第２の電解質層１３ａ、１３ｂにおける電解液量が少なくなる虞がある。 In the electric storage device 1, an inorganic filler is added to at least first and third portions 15a1 and 15b1 of the first and second insulating adhesive layers 15a and 15b. For this reason, it is suppressed that the electrolyte solution contained in 1st and 2nd electrolyte layer 13a, 13b infiltrates in the 1st and 2nd insulating contact bonding layer 15a, 15b. From the viewpoint of suppressing the permeation of the electrolytic solution into the first and second insulating adhesive layers 15a and 15b, many inorganic fillers are added to the entire first and second insulating adhesive layers 15a and 15b. Is preferred. However, if the content of the inorganic filler in the second and fourth portions 15a2 and 15b2 is too large, the adhesive strength between the second portion 15a2 and the fourth portion 15b2 may be reduced. When the adhesive strength between the second portion 15a2 and the fourth portion 15b2 decreases, the electrolyte leaks from between the second portion 15a2 and the fourth portion 15b2, and the first and second electrolyte layers are produced. There is a possibility that the amount of electrolytic solution in 13a and 13b may decrease.
　そこで、蓄電デバイス１では、第２の部分１５ａ２における無機フィラーの含有量を、第１の部分１５ａ１における無機フィラーの含有量よりも少なくし、第４の部分１５ｂ２における無機フィラーの含有量を、第３の部分１５ｂ１における無機フィラーの含有量よりも少なくされている。このため、第１及び第２の絶縁性接着層１５ａ、１５ｂに無機フィラーを添加することによる第１及び第２の絶縁性接着層１５ａ、１５ｂへ電解液が浸入することが効果的に抑制されていると共に、第２の部分１５ａ２と第４の部分１５ｂ２との接着強度を高め、第２の部分１５ａ２と第４の部分１５ｂ２との間からの電解液の漏洩が効果的に抑制されている。よって、第１及び第２の電解質層１３ａ、１３ｂにおける電解液の減少を抑制することができる。その結果、蓄電特性が劣化しにくい蓄電デバイス１を実現することができる。 Therefore, in the electric storage device 1, the content of the inorganic filler in the second portion 15a2 is smaller than the content of the inorganic filler in the first portion 15a1, and the content of the inorganic filler in the fourth portion 15b2 is It is less than the content of the inorganic filler in the portion 15 b 1 of 3. Therefore, it is effectively suppressed that the electrolytic solution infiltrates into the first and second insulating adhesive layers 15a and 15b by adding the inorganic filler to the first and second insulating adhesive layers 15a and 15b. While the adhesive strength between the second portion 15a2 and the fourth portion 15b2 is increased, and the leakage of the electrolyte from between the second portion 15a2 and the fourth portion 15b2 is effectively suppressed. . Therefore, the reduction of the electrolytic solution in the first and second electrolyte layers 13a and 13b can be suppressed. As a result, it is possible to realize the storage device 1 in which storage characteristics are not easily deteriorated.
　第１及び第２の電解質層１３ａ、１３ｂにおける電解液の減少をより効果的に抑制する観点からは、第１の部分１５ａ１における無機フィラーの含有量を５質量％以上４０質量％以下とすることが好ましく、１０質量％以上３０質量％以下とすることがより好ましい。また、第２の部分１５ａ２と第４の部分１５ｂ２との間からの電解液の漏洩をより効果的に抑制することにより第１及び第２の電解質層１３ａ、１３ｂにおける電解液の減少をより効果的に抑制する観点からは、第２及び第４の部分１５ａ２，１５ｂ２における無機フィラーの含有量を３０質量％以下とすることが好ましく、第２及び第４の部分１５ａ２，１５ｂ２が無機フィラーを実質的に含まないことがより好ましく、第２及び第４の部分１５ａ２，１５ｂ２が無機フィラーを含まないことがさらに好ましい。一方、第１及び第２の絶縁性接着層１５ａ、１５ｂへ電解液が浸入することをより効果的に抑制する観点からは、第２及び第４の部分１５ａ２，１５ｂ２における無機フィラーの含有量を５質量％以上とすることが好ましく、１０質量％以上とすることがより好ましい。 From the viewpoint of more effectively suppressing the decrease in the electrolyte solution in the first and second electrolyte layers 13a and 13b, the content of the inorganic filler in the first portion 15a1 is 5% by mass or more and 40% by mass or less Is preferable, and 10% by mass or more and 30% by mass or less is more preferable. Further, the electrolytic solution leakage from the second portion 15a2 and the fourth portion 15b2 can be more effectively suppressed to further reduce the electrolytic solution in the first and second electrolyte layers 13a and 13b. It is preferable to make content of the inorganic filler in 2nd and 4th part 15a2 and 15b2 into 30 mass% or less from a viewpoint of suppressing actively, and 2nd and 4th part 15a2 and 15b2 make an inorganic filler substantial It is more preferable that the second and fourth portions 15a2 and 15b2 do not contain the inorganic filler. On the other hand, the content of the inorganic filler in the second and fourth portions 15a2 and 15b2 is set from the viewpoint of more effectively suppressing the electrolyte solution from invading the first and second insulating adhesive layers 15a and 15b. The content is preferably 5% by mass or more, and more preferably 10% by mass or more.
　第２の部分１５ａ２と第４の部分１５ｂ２との間からの電解液の漏洩をより効果的に抑制すると共に、１及び第２の絶縁性接着層１５ａ、１５ｂへ電解液が浸入することをより効果的に抑制する観点からは、ｔ２／ｔ１及びｔ４／ｔ３のそれぞれが、１．０以下であることが好ましく、０．５５以下であることがより好ましい。但し、ｔ２／ｔ１及びｔ４／ｔ３が小さすぎると、第２の部分１５ａ２と第４の部分１５ｂ２との接着強度が低くなりすぎる虞がある。従って、ｔ２／ｔ１及びｔ４／ｔ３のそれぞれが、０．１以上であることが好ましく、０．２５以上であることがより好ましい。 While effectively suppressing the leakage of the electrolytic solution from between the second portion 15a2 and the fourth portion 15b2, it is more likely that the electrolytic solution intrudes into the first and second insulating adhesive layers 15a and 15b. From the viewpoint of effectively suppressing, each of t2 / t1 and t4 / t3 is preferably 1.0 or less, and more preferably 0.55 or less. However, if t2 / t1 and t4 / t3 are too small, the adhesive strength between the second portion 15a2 and the fourth portion 15b2 may be too low. Therefore, each of t2 / t1 and t4 / t3 is preferably 0.1 or more, and more preferably 0.25 or more.
　但し、
　ｔ１：第１の部分１５ａ１の厚み、１８～２２μｍ
　ｔ２：第２の部分１５ａ２の厚み、６～８μｍ
　ｔ３：第３の部分１５ｂ１の厚み、１８～２２μｍ
　ｔ４：第２の部分１５ｂ２の厚み、６～８μｍ
　である。 However,
t1: thickness of first portion 15a1, 18 to 22 μm
t2: Thickness of second portion 15a2, 6 to 8 μm
t3: Thickness of third portion 15b1, 18 to 22 μm
t4: Thickness of second portion 15b2, 6 to 8 μm
It is.
　ｔ１～ｔ４は、超音波厚さ計等を用いて測定することができる。 T1 to t4 can be measured using an ultrasonic thickness gauge or the like.
　なお、第１及び第２の絶縁性接着層１５ａ、１５ｂにおける無機フィラーの好ましい平均粒子径は、０．２μｍ以上０．９μｍ以下であることが好ましく、０．５μｍ以上３．０μｍ以下であることがより好ましい。なお、無機フィラーの平均粒子径は、堀場製作所製ＬＡ－９６０（レーザ回折／散乱式粒子径分布測定装置）を用いて、粒度分布を測定することにより求めることができる。 The preferable average particle diameter of the inorganic filler in the first and second insulating adhesive layers 15a and 15b is preferably 0.2 μm to 0.9 μm, and more preferably 0.5 μm to 3.0 μm. Is more preferred. The average particle size of the inorganic filler can be determined by measuring the particle size distribution using LA-960 (laser diffraction / scattering type particle size distribution measuring device) manufactured by Horiba, Ltd.
　例えば、蓄電デバイス１をリフロー実装する際などに蓄電デバイス１に熱が加わり、温度が上昇すると、蓄電デバイス１内の内圧が上昇する。蓄電デバイス１の内圧は、蓄電デバイス１の内部に存在する不純物及び水分のガス化量に依存する。そして、蓄電デバイス１の内部応力が高くなるほど、蓄電デバイス１の変形量（特に外装体１０Ｂの変形量）が大きくなる。従って、蓄電デバイス１の内部応力が高くなるほど、蓄電デバイス１の温度が上昇したときに破損しやすくなる。 For example, when the storage device 1 is reflow-mounted, heat is applied to the storage device 1, and when the temperature rises, the internal pressure in the storage device 1 rises. The internal pressure of the storage device 1 depends on the amount of gasification of impurities and water present inside the storage device 1. Then, as the internal stress of the storage device 1 becomes higher, the amount of deformation of the storage device 1 (in particular, the amount of deformation of the exterior body 10B) becomes larger. Therefore, the higher the internal stress of the storage device 1, the easier it is to be damaged when the temperature of the storage device 1 rises.
　蓄電デバイス１では、第１の絶縁性接着層１５ａが第１の電解質層１３ａの長さ方向Ｌにおける両側及び幅方向Ｗにおける両側を覆っている。かつ、第２の絶縁性接着層１５ｂが、第２の電解質層１３ｂの長さ方向Ｌにおける両側及び幅方向Ｗにおける両側を覆っている。そして、第１及び第２の絶縁性接着層１５ａ、１５ｂが無機フィラーを含んでいる。このため、第１及び第２の絶縁性接着層１５ａ、１５ｂに長さ方向Ｌにおける両側と、幅方向Ｗにおける両側とを覆われた第１及び第２の活物質層１１ｂ、１２ｂに外部から水分や不純物等が浸入しにくい。よって、蓄電デバイス１の内部の水分量が増加しにくい。従って、蓄電デバイス１内への水分や不純物等の侵入がより効果的に抑制されている。よって、蓄電デバイス１の温度が上昇した際に蓄電デバイス１の内圧が上昇することに伴う蓄電デバイス１の破損がより効果的に抑制されている。換言すれば、蓄電デバイス１は、蓄電デバイスの温度が上昇した際にも破損しにくい。すなわち、蓄電デバイス１は、優れた温度耐久性を有している。 In the storage device 1, the first insulating adhesive layer 15 a covers both sides in the length direction L of the first electrolyte layer 13 a and both sides in the width direction W. And, the second insulating adhesive layer 15 b covers both sides in the length direction L of the second electrolyte layer 13 b and both sides in the width direction W. The first and second insulating adhesive layers 15a and 15b contain an inorganic filler. Therefore, the first and second active material layers 11b and 12b are covered with the first and second insulating adhesive layers 15a and 15b at both sides in the length direction L and at both sides in the width direction W from the outside. Moisture and impurities do not easily enter. Thus, the amount of water in the storage device 1 is difficult to increase. Therefore, the entry of moisture, impurities and the like into the storage device 1 is more effectively suppressed. Therefore, when the temperature of the storage device 1 rises, damage to the storage device 1 caused by the increase in the internal pressure of the storage device 1 is more effectively suppressed. In other words, the storage device 1 is unlikely to be damaged even when the temperature of the storage device rises. That is, the storage device 1 has excellent temperature durability.
　さらに、蓄電デバイス１では、第１及び第２の絶縁性接着層１５ａ、１５ｂに含まれる無機フィラーが、活物質層１１ｂ、１２ｂに含まれる活物質（活物質粒子）の吸油量よりも低い給油量を有している。よって、蓄電デバイス１内への水分や不純物等の侵入がより効果的に抑制されている。従って、蓄電デバイス１の温度が上昇した際に蓄電デバイス１が破損することがより効果的に抑制されている。 Furthermore, in the electricity storage device 1, the inorganic filler contained in the first and second insulating adhesive layers 15 a and 15 b is less than the oil absorption of the active material (active material particles) contained in the active material layers 11 b and 12 b. Have a quantity. Therefore, the penetration of moisture, impurities and the like into the storage device 1 is more effectively suppressed. Therefore, it is more effectively suppressed that the storage device 1 is damaged when the temperature of the storage device 1 rises.
　なお、吸油量は、ＪＩＳ　Ｋ５１０１－１３－２に規定された試験方法に準拠して測定することができる。 The oil absorption can be measured in accordance with the test method defined in JIS K5101-13-2.
　蓄電デバイス１の温度が上昇した際に蓄電デバイス１が破損することをより効果的に抑制する観点からは、無機フィラーの吸油量を、５質量％以下とすることが好ましく、４質量％以下とすることがより好ましい。無機フィラーの吸油量が活物質層１１ｂ、１２ｂに含まれる活物質（活物質粒子）の吸油量の０．５倍以下であることが好ましく、０．１倍以下であることがより好ましい。 From the viewpoint of more effectively suppressing breakage of the storage device 1 when the temperature of the storage device 1 rises, the oil absorption of the inorganic filler is preferably 5% by mass or less, and 4% by mass or less It is more preferable to do. The oil absorption of the inorganic filler is preferably 0.5 times or less of the oil absorption of the active material (active material particles) contained in the active material layers 11b and 12b, and more preferably 0.1 times or less.
　同様の観点から、第１及び第２の絶縁性接着層１５ａ、１５ｂの厚みは、それぞれ、２０μｍ以上２５μｍ以下であることが好ましい。 From the same viewpoint, the thickness of each of the first and second insulating adhesive layers 15a and 15b is preferably 20 μm or more and 25 μm or less.
　蓄電デバイス１のように、第１及び第２の絶縁性接着層１５ａ、１５ｂに無機フィラーを含有させることにより、第１及び第２の絶縁性接着層１５ａ、１５ｂの強度を向上することができる。よって、蓄電デバイス１の強度が向上する。従って、蓄電デバイス１の製造工程や実装工程等において、蓄電デバイス１が破損することがより効果的に抑制されている。 By incorporating an inorganic filler in the first and second insulating adhesive layers 15a and 15b as in the storage device 1, the strength of the first and second insulating adhesive layers 15a and 15b can be improved. . Thus, the strength of the power storage device 1 is improved. Therefore, breakage of the storage device 1 is more effectively suppressed in the manufacturing process, mounting process, and the like of the storage device 1.
　なお、本実施形態では、第１の部分１５ａ１と第２の部分１５ａ２とが別体である例について説明した。但し、本発明において、第１の部分と第２の部分とが一体に設けられていてもよい。その場合、第１の絶縁性接着層における無機フィラーの含有量が第２の絶縁性接着層側に向かって段階的に減少していてもよいし、漸減していてもよい。同様に、本発明において、第３の部分と第４の部分とが一体に設けられていてもよい。その場合、第２の絶縁性接着層における無機フィラーの含有量が第１の絶縁性接着層側に向かって段階的に減少していてもよいし、漸減していてもよい。 In the present embodiment, an example in which the first portion 15a1 and the second portion 15a2 are separate bodies has been described. However, in the present invention, the first part and the second part may be integrally provided. In that case, the content of the inorganic filler in the first insulating adhesive layer may be decreased stepwise or gradually toward the second insulating adhesive layer side. Similarly, in the present invention, the third part and the fourth part may be integrally provided. In that case, the content of the inorganic filler in the second insulating adhesive layer may be decreased stepwise or gradually toward the first insulating adhesive layer side.
　（蓄電デバイス１の製造方法）
　以下、蓄電デバイス１の製造方法の一例について説明する。もっとも、本発明に係る蓄電デバイスの製造方法は、以下の製造方法に限定されない。 (Method of Manufacturing Storage Device 1)
Hereinafter, an example of the manufacturing method of the electrical storage device 1 will be described. However, the method of manufacturing the electricity storage device according to the present invention is not limited to the following manufacturing method.
　まず、例えば、アルミニウム箔等により構成された集電体の上に、スクリーン印刷法等の印刷法を用いて活物質粒子や導電材等を含むペーストを印刷し、乾燥させることにより、電極を形成する。 First, for example, a paste containing active material particles, a conductive material, and the like is printed on a current collector made of aluminum foil or the like using a printing method such as screen printing, and the electrode is formed by drying. Do.
　次に、形成した電極の上に、活物質層の外周を覆うように、無機フィラー及び樹脂を含むペーストを、スクリーン印刷法等の印刷法を用いて印刷し、乾燥させることにより、絶縁性接着層の第１又は第３の部分を形成する。 Next, on the formed electrode, a paste containing an inorganic filler and a resin is printed using a printing method such as a screen printing method so as to cover the outer periphery of the active material layer, and then dried. Form a first or third part of the layer.
　次に、無機フィラー及び樹脂を含むペーストを、スクリーン印刷法等の印刷法を用いて印刷し、乾燥させることにより、絶縁性接着層の第２又は第４の部分を形成する。この第２又は第４の部分の形成に用いるペーストとしては、第１又は第３の部分を形成するために用いたペーストよりも無機フィラーの含有量が少ないペーストを用いる。 Next, a paste containing an inorganic filler and a resin is printed using a printing method such as screen printing and dried to form a second or fourth portion of the insulating adhesive layer. As a paste used for formation of this 2nd or 4th part, the paste in which content of an inorganic filler is smaller than the paste used in order to form a 1st or 3rd part is used.
　次に、例えば、スクリーン印刷法等の印刷法を用いて電解液を含むペーストを印刷し、活物質層の上に電解質層を形成する。 Next, for example, a paste containing an electrolytic solution is printed using a printing method such as a screen printing method to form an electrolyte layer on the active material layer.
　上述のようにして作製した２つの積層体を、各々の活物質層が接触し、かつ、一方の積層体の集電体が長さ方向の一方側端面に露出し、他方の積層体の集電体が長さ方向の他方側端面に露出するように重ね合わせ、プレスすることにより一体化し、蓄電ユニットを作製する。 The active material layers of the two laminates produced as described above are in contact with each other, and the current collector of one laminate is exposed at one end face in the lengthwise direction, and the collection of the other laminate is performed. The electricity storage unit is manufactured by stacking and pressing so that the current collector is exposed on the other end surface in the lengthwise direction.
　次に、複数の蓄電ユニットを接着剤を介在させて積層し、接着剤を硬化することにより、機能部を作製する。 Next, a plurality of power storage units are stacked with an adhesive interposed, and the adhesive is cured to produce a functional unit.
　次に、機能部の周囲に外装体を設ける。外装体は、例えば、樹脂モールドや樹脂ケースにより設けることができる。 Next, an exterior body is provided around the functional part. The exterior body can be provided, for example, by a resin mold or a resin case.
　次に、集電体が露出した各端面に溶射や、スパッタリング法等の薄膜形成法を用いて電極膜を形成する。 Next, an electrode film is formed on each end face where the current collector is exposed, using a thin film forming method such as thermal spraying or sputtering.
　次に、各電極膜の上に導電性接着剤を塗布した後に金属キャップを被せ、導電性接着剤を硬化させることにより、蓄電デバイス１を完成させることができる。 Next, a conductive adhesive is applied on each electrode film and then covered with a metal cap, and the conductive adhesive is cured, whereby the storage device 1 can be completed.
　１　　　　：蓄電デバイス
１０　　　：デバイス本体
１０Ａ　　：機能部
１０Ｂ　　：外装体
１０ａ　　：第１の主面
１０ｂ　　：第２の主面
１０ｃ　　：第１の側面
１０ｄ　　：第２の側面
１０ｅ　　：第１の端面
１０ｆ　　：第２の端面
１１　　　：第１の内部電極
１１ａ　　：第１の集電体
１１ｂ　　：第１の活物質層
１２　　　：第２の内部電極
１２ａ　　：第２の集電体
１２ｂ　　：第２の活物質層
１３　　　：電解質層
１３ａ　　：第１の電解質層
１３ｂ　　：第２の電解質層
１５ａ　　：第１の絶縁性接着層
１５ａ１　：第１の部分
１５ａ２　：第２の部分
１５ｂ　　：第２の絶縁性接着層
１５ｂ１　：第３の部分
１５ｂ２　：第４の部分
１６　　　：接着層
１７　　　：蓄電ユニット
１８　　　：第１の外部電極
１８ａ　　：第１の電極膜
１８ｂ　　：第１の導電性接着層
１８ｃ　　：第１の金属キャップ
１９　　　：第２の外部電極
１９ａ　　：第２の電極膜
１９ｂ　　：第２の導電性接着層
１９ｃ　　：第２の金属キャップ 1: storage device 10: device body 10A: functional unit 10B: exterior body 10a: first main surface 10b: second main surface 10c: first side 10d: second side 10e: first end 10f: Second end face 11: first inner electrode 11a: first current collector 11b: first active material layer 12: second inner electrode 12a: second current collector 12b: second active material layer 13: electrolyte layer 13a: first electrolyte layer 13b: second electrolyte layer 15a: first insulating adhesive layer 15a1: first portion 15a2: second portion 15b: second insulating adhesive layer 15b1: Third portion 15b2: fourth portion 16: adhesive layer 17: storage unit 18: first external electrode 18a: first electrode film 18b: first conductive adhesive layer 18c: first metal cap 19: Second outside Part electrode 19a: second electrode film 19b: second conductive adhesive layer 19c: second metal cap

Claims (6)

  1. 　長さ方向及び幅方向に沿って延び、第１の集電体と、前記第１の集電体の上に設けられた第１の活物質層とを有する第１の内部電極と、
    　前記第１の活物質層の上に配された第１の電解質層と、
    　前記第１の活物質層及び前記第１の電解質層の周囲を覆っており、無機フィラーが分散した樹脂組成物からなる第１の絶縁性接着層と、
    　前記第１の内部電極に対して厚み方向に積層されており、第２の集電体と、前記第２の集電体の上に設けられた第２の活物質層とを有する第２の内部電極と、
    　前記第２の活物質層の上に配されており、前記第１の電解質層と接触している第２の電解質層と、
    　前記第２の活物質層及び前記第２の電解質層の周囲を覆っており、無機フィラーが分散した樹脂組成物からなり、前記第１の絶縁性接着層と接着されている第２の絶縁性接着層と、
    　を備え、
    　前記第１の絶縁性接着層は、
    　前記第１の活物質層の周囲を覆っている第１の部分と、
    　前記第１の電解質層の周囲を覆っており、前記第２の絶縁性接着層と接着されている第２の部分と、
    　を有し、
    　前記第２の絶縁性接着層は、
    　前記第２の活物質層の周囲を覆っている第３の部分と、
    　前記第２の電解質層の周囲を覆っており、前記第２の部分と接着されている第４の部分と、
    　を有し、
    　前記第２の部分における前記無機フィラーの含有量が前記第１の部分における前記無機フィラーの含有量よりも少なく、
    　前記第４の部分における前記無機フィラーの含有量が前記第３の部分における前記無機フィラーの含有量よりも少ない、蓄電デバイス。     A first inner electrode extending along the length direction and the width direction and having a first current collector and a first active material layer provided on the first current collector;
    A first electrolyte layer disposed on the first active material layer,
    A first insulating adhesive layer covering a periphery of the first active material layer and the first electrolyte layer, and made of a resin composition in which an inorganic filler is dispersed;
    A second current collector, and a second active material layer provided on the second current collector, the second current collector being stacked in the thickness direction with respect to the first internal electrode; Internal electrode,
    A second electrolyte layer disposed on the second active material layer and in contact with the first electrolyte layer;
    A second insulating property which covers the periphery of the second active material layer and the second electrolyte layer, is made of a resin composition in which an inorganic filler is dispersed, and is bonded to the first insulating adhesive layer. Adhesive layer,
    Equipped with
    The first insulating adhesive layer is
    A first portion covering the periphery of the first active material layer,
    A second portion covering the periphery of the first electrolyte layer and bonded to the second insulating adhesive layer;
    Have
    The second insulating adhesive layer is
    A third portion covering the periphery of the second active material layer,
    A fourth portion covering the periphery of the second electrolyte layer and bonded to the second portion;
    Have
    The content of the inorganic filler in the second portion is less than the content of the inorganic filler in the first portion,
    The electrical storage device, wherein a content of the inorganic filler in the fourth portion is smaller than a content of the inorganic filler in the third portion.
  2. 　前記第２及び第４の部分が前記無機フィラーを含まない、請求項１に記載の蓄電デバイス。 The power storage device according to claim 1, wherein the second and fourth portions do not include the inorganic filler.
  3. 　前記第１及び第２の電解質層は、それぞれ、電解液を含み、
    　前記第１及び第２の絶縁性接着層に含まれる樹脂が前記電解液により膨潤する樹脂である、請求項１又は２に記載の蓄電デバイス。     The first and second electrolyte layers each contain an electrolyte,
    The power storage device according to claim 1, wherein a resin contained in the first and second insulating adhesive layers is a resin that swells with the electrolytic solution.
  4. 　前記第１の部分の厚みをｔ１とし、
    　前記第２の部分の厚みをｔ２とし、
    　前記第３の部分の厚みをｔ３とし、
    　前記第４の部分の厚みをｔ４としたときに、
    　ｔ２／ｔ１及びｔ４／ｔ３が、それぞれ０．５５以下である、請求項１～３のいずれか一項に記載の蓄電デバイス。     Let t1 be the thickness of the first portion,
    Let t2 be the thickness of the second portion,
    Let t3 be the thickness of the third portion,
    When the thickness of the fourth portion is t4
    The power storage device according to any one of claims 1 to 3, wherein t2 / t1 and t4 / t3 are each 0.55 or less.
  5. 　前記第１及び第２の活物質層は、それぞれ、活物質を含み、
    　前記無機フィラーの吸油量が前記活物質の吸油量よりも低い、請求項１～４のいずれか一項に記載の蓄電デバイス。     The first and second active material layers each include an active material,
    The electricity storage device according to any one of claims 1 to 4, wherein an oil absorption amount of the inorganic filler is lower than an oil absorption amount of the active material.
  6. 　前記無機フィラーが、酸化アルミニウム、酸化ケイ素、酸化チタン、酸化マグネシウム酸化ジルコニウム、ジルコン、炭化ケイ素、リン酸アルミニウム、窒化アルミニウム、窒化ケイ素、ステアタイト、コージライト、ムライト及びサイアロンからなる群から選ばれた少なくとも一種を含む、請求項１～５のいずれか一項に記載の蓄電デバイス。  The inorganic filler is selected from the group consisting of aluminum oxide, silicon oxide, titanium oxide, magnesium zirconium oxide, zircon, silicon carbide, aluminum phosphate, aluminum nitride, silicon nitride, steatite, cordierite, mullite and sialon The power storage device according to any one of claims 1 to 5, including at least one.
PCT/JP2018/015494 2017-06-19 2018-04-13 Electricity storage device WO2018235408A1 (en)

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