WO2023277100A1 - 蓄電デバイス、及び、蓄電デバイスの製造方法 - Google Patents

蓄電デバイス、及び、蓄電デバイスの製造方法 Download PDF

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Publication number
WO2023277100A1
WO2023277100A1 PCT/JP2022/026084 JP2022026084W WO2023277100A1 WO 2023277100 A1 WO2023277100 A1 WO 2023277100A1 JP 2022026084 W JP2022026084 W JP 2022026084W WO 2023277100 A1 WO2023277100 A1 WO 2023277100A1
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WIPO (PCT)
Prior art keywords
storage device
mass
aluminum alloy
electricity storage
exterior member
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2022/026084
Other languages
English (en)
French (fr)
Japanese (ja)
Inventor
敦子 高萩
慎二 林
健太 平木
美帆 佐々木
昌保 山崎
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Dai Nippon Printing Co Ltd
Original Assignee
Dai Nippon Printing Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Dai Nippon Printing Co Ltd filed Critical Dai Nippon Printing Co Ltd
Priority to US18/572,896 priority Critical patent/US20240304904A1/en
Priority to EP22833246.6A priority patent/EP4366045A4/en
Priority to KR1020247001370A priority patent/KR20240026486A/ko
Priority to JP2023501913A priority patent/JP7279872B1/ja
Priority to CN202280045802.7A priority patent/CN117616621A/zh
Publication of WO2023277100A1 publication Critical patent/WO2023277100A1/ja
Priority to JP2023076690A priority patent/JP7444315B2/ja
Anticipated expiration legal-status Critical
Priority to JP2024023944A priority patent/JP2024052801A/ja
Ceased legal-status Critical Current

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
    • H01M50/103—Primary casings; Jackets or wrappings characterised by their shape or physical structure prismatic or rectangular
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/116—Primary casings; Jackets or wrappings characterised by the material
    • H01M50/124—Primary casings; Jackets or wrappings characterised by the material having a layered structure
    • H01M50/126—Primary casings; Jackets or wrappings characterised by the material having a layered structure comprising three or more layers
    • H01M50/129—Primary casings; Jackets or wrappings characterised by the material having a layered structure comprising three or more layers with two or more layers of only organic material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
    • B32B15/085—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin comprising polyolefins
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/04—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • B32B15/08—Layered products comprising a layer of metal comprising metal as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
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    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B32B7/04—Interconnection of layers
    • B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
    • C—CHEMISTRY; METALLURGY
    • C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22C—ALLOYS
    • C22C21/00—Alloys based on aluminium
    • C22C21/06—Alloys based on aluminium with magnesium as the next major constituent
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    • 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
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    • H01G11/84—Processes for the manufacture of hybrid or EDL capacitors, or components thereof
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    • H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
    • H01M50/105—Pouches or flexible bags
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    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present invention relates to an electricity storage device and a method for manufacturing an electricity storage device.
  • Patent Document 1 discloses a secondary battery.
  • an electrode body is sealed in a bag made of an exterior member (laminate film) (see Patent Document 1).
  • the sealing portion of the exterior member is provided on the surface with the large area. Since the seal portion is a region where the exterior members are overlapped, it is thicker than other regions. When another secondary battery is stacked on the surface provided with the seal portion, the upper secondary battery may tilt with the seal portion as a fulcrum. As a result, uneven distribution of pressure applied to the lower secondary battery becomes large.
  • the present invention has been made to solve such problems, and an object of the present invention is to suppress uneven distribution of pressure applied to adjacent power storage devices when a plurality of power storage devices are stacked, Another object of the present invention is to provide an electricity storage device having corrosion resistance and a method for manufacturing the electricity storage device.
  • a power storage device includes an electrode body and an exterior body.
  • the outer body seals the electrode body.
  • the exterior body is configured by a film-like exterior member.
  • the exterior body includes a first sealing portion, a first surface, and a second surface, which are sealed by bonding surfaces facing each other while the exterior member is wrapped around the electrode body.
  • the area of the first surface is larger than the area of the second surface.
  • the first sealing portion does not overlap the first surface in plan view.
  • the exterior member is composed of a laminate including at least a substrate layer, a barrier layer, and a heat-fusible resin layer in this order.
  • the barrier layer contains an aluminum alloy foil satisfying a composition of Fe: 0.2% by mass or more and 2.0% by mass or less and Mg: 0.1% by mass or more and 5.0% by mass or less.
  • the first sealing portion does not overlap the large first surface in plan view. That is, the first sealing portion does not exist on the large first surface. Therefore, even if another power storage device is arranged side by side on the first surface, the other power storage device does not tilt. As a result, according to this power storage device, when a plurality of power storage devices are stacked, uneven distribution of pressure applied to adjacent power storage devices can be suppressed. Moreover, since the aluminum alloy foil of the exterior member has the above structure, the aluminum alloy foil is less likely to corrode.
  • the first sealing portion may be bent so as to be in contact with the second surface.
  • the first sealing portion may cover substantially the entire second surface while being bent so as to be in contact with the second surface.
  • the first sealing portion covers substantially the entire second surface, so that a wide bonding width can be secured in the first sealing portion.
  • the electricity storage device further includes an electrode terminal electrically connected to the electrode body, the exterior body further includes a second sealing portion that is sealed with the electrode terminal sandwiched therebetween, and a portion of the electrode terminal includes:
  • the root portion of the portion outside the exterior body may be located at approximately half the thickness of the power storage device in the thickness direction of the power storage device.
  • a portion of the electrode terminal outside the exterior body is located at a position approximately half the thickness of the electricity storage device in the thickness direction of the electricity storage device. Therefore, according to this electricity storage device, each of the plurality of electrodes included in the electrode body and the electrode terminal are more likely to be connected to each other than, for example, the case where the portion is located at substantially the same position as the first surface in the thickness direction of the electricity storage device. It is possible to reduce the difference between the longest distance and the shortest distance among the distances between
  • the region where the bonding strength between the surfaces is strong and the region where the bonding strength between the surfaces is weak are arranged along the boundary between the first surface and the second surface.
  • a thin region and a thick region may be arranged along the boundary between the first surface and the second surface.
  • the electric storage device may further include an electrode terminal electrically connected to the electrode body, and the first sealing portion may be sealed while sandwiching the electrode terminal.
  • the above electricity storage device further includes an electrode terminal electrically connected to the electrode body, and a lid body to which the electrode terminal is attached, wherein the exterior body is sealed in a state of being joined to the lid body. It may further include a sealing portion.
  • the lid body includes a first surface facing the electrode body and a second surface opposite to the first surface, and the second sealing portion joins the exterior body and the second surface. It may contain a part that
  • the power storage device further includes a lid
  • the exterior body further includes a second sealing portion that is sealed in a state of being joined to the lid, and the lid is a portion where the metal layer is exposed on the surface, or , a metal portion that is a portion made of a metal material, and the metal portion and the electrode body may be welded together.
  • the electricity storage device further includes an electrode terminal electrically connected to the electrode body, and the exterior body is sealed in a state in which the electrode terminal is sandwiched between the protruding portion protruding outward and the protruding portion.
  • a second seal may be further included.
  • the direction along the boundary between the first surface and the second surface may be a direction orthogonal to the flow direction of the exterior member.
  • the direction along the boundary between the first surface and the second surface is the flow direction of the exterior member. It is the orthogonal direction. Therefore, according to this electric storage device, even if a fold line is formed in the direction perpendicular to the flow direction of the exterior member, the exterior member is unlikely to break, so that the first sealing portion is broken when the first sealing portion is bent. can reduce the likelihood of
  • An electricity storage device includes an electrode body, electrode terminals electrically connected to the electrode body, and an exterior body that seals the electrode body.
  • the exterior body is configured by a film-like exterior member, and includes long sides and short sides in a plan view.
  • the electrode terminals are arranged along the long sides.
  • a power storage device includes an electrode body and an exterior body.
  • the outer body seals the electrode body.
  • the exterior member is configured by a film-shaped exterior member.
  • the outer body includes a piece portion in which peripheral edges of surfaces facing each other are joined together while being wrapped around the electrode body. A space is formed in the piece portion in which the surfaces facing each other are not joined to each other. In the piece portion, a region where the surfaces facing each other are joined and a region where the surfaces facing each other are not joined are arranged in the vicinity of the boundary between the surfaces.
  • the exterior member is composed of a laminate including at least a substrate layer, a barrier layer, and a heat-fusible resin layer in this order.
  • the barrier layer contains an aluminum alloy foil satisfying a composition of Fe: 0.2% by mass or more and 2.0% by mass or less and Mg: 0.1% by mass or more and 5.0% by mass or less.
  • Gas can be generated inside the exterior body.
  • this electricity storage device a space is formed in the piece, and a region where the surfaces facing each other are joined and a region where the surfaces facing each other are not joined are arranged in the vicinity of the boundary between the surfaces. I'm in. Therefore, according to this electric storage device, by releasing the sealed state of the exterior body at the piece portion, the gas in the exterior body can be discharged through the piece portion. Then, by sealing the exterior body again, the electricity storage device after degassing can be manufactured. Moreover, since the aluminum alloy foil of the exterior member has the above structure, the aluminum alloy foil is less likely to corrode.
  • the composition of the aluminum alloy foil may satisfy Si: 0.5% by mass or less.
  • the composition of the aluminum alloy foil satisfies Mg: 0.1% by mass or more and 1.5% by mass or less, and at least one surface of the aluminum alloy foil contains 5.0 atomic percent or more of Mg, and At least one surface of the aluminum alloy foil may have an oxide film having a thickness of 80 ⁇ or more.
  • the composition of the aluminum alloy foil satisfies Mg: 0.1% by mass or more and 1.5% by mass or less, and the aluminum alloy foil has a tensile strength of 110 MPa or more and 180 MPa or less and a breaking elongation of 10% or more. There may be.
  • the composition of the aluminum alloy foil satisfies Mg: more than 1.5% by mass and 5.0% by mass or less, and at least one surface of the aluminum alloy foil contains 15.0 atomic percent or more Mg, and , an oxide film having a thickness of 120 ⁇ or more may be formed on at least one surface of the aluminum alloy foil.
  • the composition of the aluminum alloy foil satisfies Mg: more than 1.5% by mass and 5.0% by mass or less, and the aluminum alloy foil has a tensile strength of 180 MPa or more and a breaking elongation of 15% or more. good too.
  • the aluminum alloy foil may have an orientation density of 15 or less in each of the Copper orientation and the R orientation of the texture.
  • the aluminum alloy foil may have an average grain size of 25 ⁇ m or less.
  • the aluminum alloy foil contains Al and unavoidable impurities as the balance, and the ratio of the length L1 of the large-angle grain boundary per unit area and the length L2 of the small-angle grain boundary measured by a backscattered electron diffraction method. may satisfy the relationship L1/L2>3.0.
  • the aluminum alloy foil may contain Mn: 0.1% by mass or less as an unavoidable impurity.
  • a method of manufacturing an electricity storage device is a method of manufacturing an electricity storage device from an unfinished product.
  • the unfinished product includes an electrode body and an exterior body.
  • the outer body seals the electrode body.
  • the exterior body is configured by a film-like exterior member.
  • the outer body includes a piece portion in which peripheral edges of surfaces facing each other are joined in a state in which the outer member is wound around the electrode body.
  • a space is formed in the piece portion in which the surfaces facing each other are not joined to each other. In the piece portion, a region where the surfaces facing each other are joined and a region where the surfaces facing each other are not joined are arranged in the vicinity of the boundary between the surfaces.
  • the exterior member is composed of a laminate including at least a substrate layer, a barrier layer, and a heat-fusible resin layer in this order.
  • the barrier layer contains an aluminum alloy foil satisfying a composition of Fe: 0.2% by mass or more and 2.0% by mass or less and Mg: 0.1% by mass or more and 5.0% by mass or less.
  • the manufacturing method includes the step of releasing the sealed state of the exterior body at the piece to discharge the gas to the outside of the exterior body, and resealing the body.
  • the electricity storage device after gas removal can be manufactured by discharging the gas through the piece and sealing the exterior body again.
  • ADVANTAGE OF THE INVENTION when a plurality of power storage devices are stacked, uneven distribution of pressure applied to the lower power storage devices can be suppressed, and corrosion resistance is provided, and a method for manufacturing the power storage device is provided. can do.
  • FIG. 1 is a perspective view schematically showing an electricity storage device according to Embodiment 1; FIG. It is a top view which shows an electrical storage device typically. It is a side view which shows an electrical storage device typically. Sectional drawing which shows an example of the layer structure of an exterior member. Sectional drawing which shows an example of the layer structure of an exterior member. Sectional drawing which shows an example of the layer structure of an exterior member. Sectional drawing which shows an example of the layer structure of an exterior member. Sectional drawing which shows an example of the layer structure of an exterior member. 1 is a micrograph showing the surface of an aluminum alloy foil used for corrosion resistance evaluation, showing a surface without corrosion. 1 is a micrograph showing the surface of an aluminum alloy foil used for corrosion resistance evaluation, showing a corroded surface. FIG.
  • FIG. 4 is a side view showing a state in which an exterior member is wound around an electrode assembly during manufacture of the electricity storage device according to Embodiment 1;
  • FIG. 4 is a view showing from below a state in which an exterior member is wound around an electrode assembly during manufacture of the electricity storage device according to Embodiment 1;
  • FIG. 3 is a diagram schematically showing a part of the VI-VI cross section of FIG. 2; It is a figure for demonstrating the formation method of a 2nd sealing part.
  • 4 is a flow chart showing a procedure for manufacturing an electricity storage device according to Embodiment 1.
  • FIG. FIG. 4 is a plan view schematically showing an electricity storage device according to Embodiment 2; It is a side view which shows an electrical storage device typically.
  • FIG. 10 is a diagram showing a first example in which a lid body and electrode terminals are integrally formed;
  • FIG. 10 is a diagram showing a second example in which a lid and electrode terminals are integrally formed;
  • 7 is a flow chart showing a procedure for manufacturing an electricity storage device according to Embodiment 2.
  • FIG. 10 is a flow chart showing another manufacturing procedure of the electricity storage device according to Embodiment 2.
  • FIG. 11 is a side view showing a state in which an exterior member is wound around an electrode body in Embodiment 3;
  • FIG. 11 is a diagram showing from below a state in which an exterior member is wound around an electrode body and a lid is attached to the exterior member in Embodiment 3; 10 is a flow chart showing a procedure for manufacturing an electricity storage device according to Embodiment 3.
  • FIG. FIG. 11 is a plan view schematically showing an electricity storage device according to Embodiment 4;
  • FIG. 11 is a side view schematically showing an electricity storage device according to Embodiment 4;
  • FIG. 11 is a side view showing a state in which an exterior member is wound around an electrode body in a modification; It is a perspective view which shows the electrical storage device of a modification typically.
  • FIG. 11 is a perspective view schematically showing a lid body of a modified example and electrode terminals attached to the lid body.
  • FIG. 24 is a perspective view schematically showing an electricity storage device to which the lid of FIG. 23 is attached; It is a front view which shows typically the cover of another modification. It is a front view which shows typically the cover of another modification.
  • FIG. 11 is a plan view schematically showing an electricity storage device of another modified example;
  • FIG. 1 is a perspective view schematically showing power storage device 10 according to the first embodiment.
  • FIG. 2 is a plan view schematically showing the electricity storage device 10.
  • FIG. 3A is a side view schematically showing the electricity storage device 10.
  • FIG. 3B to 3E are cross-sectional views showing the layer structure of the exterior member 101 of the electricity storage device 10.
  • the arrow UD direction indicates the thickness direction of the electricity storage device 10
  • the arrow LR direction indicates the width direction of the electricity storage device 10.
  • the arrow FB direction indicates the depth direction of the power storage device 10 .
  • the directions indicated by the arrows UDLRFB are also common in the subsequent drawings.
  • the electricity storage device 10 includes an electrode body 200, an exterior body 100, and a plurality (two) of electrode terminals 300.
  • the electrode body 200 includes electrodes (a positive electrode and a negative electrode), a separator, and the like, which constitute a power storage member such as a lithium ion battery, a capacitor, or an all-solid-state battery.
  • the shape of the electrode body 200 is a substantially rectangular parallelepiped.
  • substantially rectangular parallelepiped is meant to include not only perfect rectangular parallelepipeds, but also solids that can be regarded as rectangular parallelepipeds by, for example, modifying the shape of a part of the outer surface.
  • the electrode terminal 300 is a metal terminal used for power input/output in the electrode body 200 .
  • One end of the electrode terminal 300 is electrically connected to the electrode (positive electrode or negative electrode) included in the electrode body 200 , and the other end protrudes outward from the edge of the exterior body 100 .
  • the metal material forming the electrode terminal 300 is, for example, aluminum, nickel, copper, or the like.
  • the electrode terminal 300 connected to the positive electrode is usually made of aluminum or the like
  • the electrode terminal 300 connected to the negative electrode is usually made of copper, nickel or the like. be.
  • the exterior body 100 is composed of a film-like exterior member 101 (FIG. 4, etc.) and seals the electrode body 200 .
  • the exterior body 100 is formed by winding the exterior member 101 around the electrode body 200 and sealing the open portion.
  • a housing portion for housing the electrode body 200 in the exterior member 101 through cold forming.
  • the exterior body 100 seals the electrode body 200 by winding the exterior member 101 around the electrode body 200 , the electrode body 200 can be easily sealed regardless of the thickness of the electrode body 200 .
  • the exterior member 101 was wound so as to be in contact with the outer surface of the electrode assembly 200. condition is preferred.
  • the exterior member 101 is composed of a laminate including at least a base layer 101A, a barrier layer 101C, and a heat-fusible resin layer 101D in this order.
  • the substrate layer 101A is the outermost layer
  • the heat-fusible resin layer 101D is the innermost layer.
  • the barrier layer 101C contains an aluminum alloy foil. That is, the barrier layer 101C can be made of an aluminum alloy foil.
  • the exterior member 101 of the present embodiment using an aluminum alloy foil that satisfies the predetermined composition and characteristics described later has excellent followability of the exterior member at corners and the like, effectively suppresses corrosion of the aluminum alloy foil, and furthermore Excellent mechanical strength.
  • the exterior member 101 has an adhesive layer between the base layer 101A and the barrier layer 101C for the purpose of increasing the adhesion between these layers, if necessary.
  • 101B For example, as shown in FIGS. 3D and 3E, between the barrier layer 101C and the heat-fusible resin layer 101D, an adhesive layer 101E may be optionally provided for the purpose of improving the adhesion between these layers.
  • a surface coating layer 101F or the like may be provided on the outside of the base material layer 101A (the side opposite to the heat-fusible resin layer 101D side), if necessary.
  • the thickness of the laminate constituting the exterior member 101 is not particularly limited, but from the viewpoint of cost reduction, improvement of energy density, etc., it is, for example, 190 ⁇ m or less, preferably about 180 ⁇ m or less, about 155 ⁇ m or less, and about 120 ⁇ m or less. .
  • the thickness of the laminate constituting the exterior member 101 is preferably about 35 ⁇ m or more, about 45 ⁇ m or more, or about 60 ⁇ m or more from the viewpoint of maintaining the function of the exterior member 101 to protect the electrode body 200 . .
  • the preferred range of the laminate constituting the exterior member 101 is, for example, about 35 to 190 ⁇ m, about 35 to 180 ⁇ m, about 35 to 155 ⁇ m, about 35 to 120 ⁇ m, about 45 to 190 ⁇ m, about 45 to 180 ⁇ m, 45 to 180 ⁇ m, About 155 ⁇ m, about 45 to 120 ⁇ m, about 60 to 190 ⁇ m, about 60 to 180 ⁇ m, about 60 to 155 ⁇ m, and about 60 to 120 ⁇ m can be mentioned, and about 60 to 155 ⁇ m is particularly preferable.
  • the base material layer 101A, the adhesive layer 101B provided as necessary, the barrier layer 101C, and the adhesive layer 101E provided as necessary with respect to the thickness (total thickness) of the laminate constituting the exterior member 101 The heat-fusible resin layer 101D, and the optionally provided surface coating layer 101F preferably have a total thickness ratio of 90% or more, more preferably 95% or more, and even more preferably 98%. That's it.
  • the thickness of the laminate constituting the exterior member 101 is preferably 90% or more, more preferably 95% or more, and still more preferably 98% or more.
  • a barrier layer 101C which will be described later, can usually be distinguished between MD (Machine Direction) and TD (Transverse Direction) in the manufacturing process.
  • MD Machine Direction
  • TD Transverse Direction
  • the barrier layer 101C is made of an aluminum alloy foil
  • linear streaks called rolling marks are formed on the surface of the metal foil in the rolling direction (RD) of the metal foil. Since the rolling marks extend along the rolling direction, the rolling direction of the metal foil can be grasped by observing the surface of the metal foil.
  • the MD of the laminate usually matches the RD of the metal foil, so the surface of the metal foil of the laminate is observed to identify the rolling direction (RD) of the metal foil.
  • the MD of the laminate can be specified.
  • the TD of the laminate is perpendicular to the MD of the laminate, the TD of the laminate can also be specified.
  • the MD of the exterior member 101 cannot be specified due to the rolling marks of the aluminum alloy foil, it can be specified by the following method.
  • a method of confirming the MD of the exterior member 101 there is a method of observing the cross section of the heat-fusible resin layer of the exterior member 101 with an electron microscope to confirm the sea-island structure.
  • the MD can be determined as the direction parallel to the cross section in which the average diameter of the island shape in the direction perpendicular to the thickness direction of the heat-fusible resin layer is maximum.
  • the cross section in the length direction of the heat-fusible resin layer is changed by 10 degrees from a direction parallel to the cross section in the length direction, and the direction is perpendicular to the cross section in the length direction.
  • each cross section the shape of each individual island is observed.
  • the linear distance connecting the leftmost end in the direction perpendicular to the thickness direction of the heat-sealable resin layer and the rightmost end in the perpendicular direction is defined as the diameter y.
  • the average of the top 20 diameters y of the island shape is calculated in descending order of diameter y. The direction parallel to the cross section in which the average diameter y of the island shape is the largest is determined as the MD.
  • Base material layer> 101 A of base materials layers are layers provided for the purpose of exhibiting the function as a base material of the exterior member 101, etc.
  • FIG. 101 A of base materials layers are located in the outer layer side of the exterior member 101. As shown in FIG.
  • the material forming the base layer 101A is not particularly limited as long as it functions as a base material, that is, at least has insulating properties.
  • 101 A of base materials layers can be formed, for example using resin, and the resin may contain the below-mentioned additive agent.
  • the base layer 101A may be, for example, a resin film made of resin, or may be formed by applying resin.
  • the resin film may be an unstretched film or a stretched film.
  • stretched films include uniaxially stretched films and biaxially stretched films, with biaxially stretched films being preferred.
  • stretching methods for forming a biaxially stretched film include successive biaxial stretching, inflation, and simultaneous biaxial stretching.
  • Methods for applying the resin include a roll coating method, a gravure coating method, an extrusion coating method, and the like.
  • Examples of resins forming the base material layer 101A include resins such as polyester, polyamide, polyolefin, epoxy resin, acrylic resin, fluororesin, polyurethane, silicon resin, phenol resin, and modified products of these resins. Further, the resin forming the base material layer 101A may be a copolymer of these resins or a modified copolymer thereof. Furthermore, it may be a mixture of these resins.
  • polyester and polyamide are preferably used as the resin forming the base material layer 101A.
  • polyester examples include polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polybutylene naphthalate, polyethylene isophthalate, and copolymerized polyester.
  • copolyester examples include copolyester having ethylene terephthalate as a main repeating unit.
  • copolymer polyester polymerized with ethylene isophthalate with ethylene terephthalate as the main repeating unit hereinafter abbreviated after polyethylene (terephthalate / isophthalate)
  • polyethylene (terephthalate / adipate) polyethylene (terephthalate / sodium sulfoisophthalate)
  • polyethylene (terephthalate/sodium isophthalate) polyethylene (terephthalate/phenyl-dicarboxylate), polyethylene (terephthalate/decanedicarboxylate), and the like.
  • These polyesters may be used singly or in combination of two or more.
  • polyamide specifically, aliphatic polyamide such as nylon 6, nylon 66, nylon 610, nylon 12, nylon 46, copolymer of nylon 6 and nylon 66; terephthalic acid and / or isophthalic acid Hexamethylenediamine-isophthalic acid-terephthalic acid copolymer polyamide such as nylon 6I, nylon 6T, nylon 6IT, nylon 6I6T (I represents isophthalic acid, T represents terephthalic acid) containing structural units derived from, polyamide MXD6 (polymetallic Polyamides containing aromatics such as silylene adipamide); alicyclic polyamides such as polyamide PACM6 (polybis(4-aminocyclohexyl)methane adipamide); Copolymerized polyamides, polyesteramide copolymers and polyetheresteramide copolymers which are copolymers of copolymerized polyamides with polyesters or polyalkylene ether glycols; and polyamides such
  • the base layer 101A preferably includes at least one of a polyester film, a polyamide film, and a polyolefin film, and preferably includes at least one of a stretched polyester film, a stretched polyamide film, and a stretched polyolefin film. More preferably, at least one of an oriented polyethylene terephthalate film, an oriented polybutylene terephthalate film, an oriented nylon film, and an oriented polypropylene film is included, and the biaxially oriented polyethylene terephthalate film, biaxially oriented polybutylene terephthalate film, and biaxially oriented nylon film , biaxially oriented polypropylene film.
  • the base layer 101A may be a single layer, or may be composed of two or more layers.
  • the substrate layer 101A may be a laminate obtained by laminating resin films with an adhesive or the like, or may be formed by co-extrusion of resin to form two or more layers. It may also be a laminate of resin films. A laminate of two or more resin films formed by coextrusion of resin may be used as the base layer 101A without being stretched, or may be uniaxially stretched or biaxially stretched to form the base layer 101A.
  • a laminate of two or more layers of resin films include a laminate of a polyester film and a nylon film, a laminate of nylon films of two or more layers, and a laminate of polyester films of two or more layers. etc., preferably a laminate of a stretched nylon film and a stretched polyester film, a laminate of two or more layers of stretched nylon films, and a laminate of two or more layers of stretched polyester films.
  • the substrate layer 101A is a laminate of two layers of resin films, a laminate of polyester resin films and polyester resin films, a laminate of polyamide resin films and polyamide resin films, or a laminate of polyester resin films and polyamide resin films.
  • a laminate is preferred, and a laminate of polyethylene terephthalate film and polyethylene terephthalate film, a laminate of nylon film and nylon film, or a laminate of polyethylene terephthalate film and nylon film is more preferred.
  • the polyester resin is resistant to discoloration when, for example, an electrolytic solution adheres to its surface. Therefore, when the base layer 101A is a laminate of two or more resin films, the polyester resin film is used as the base layer 101A. It is preferably located in the outermost layer.
  • the two or more layers of resin films may be laminated via an adhesive.
  • Preferred adhesives are the same as those exemplified for the adhesive layer 101B described later.
  • the method for laminating two or more layers of resin films is not particularly limited, and known methods can be employed. Examples thereof include dry lamination, sandwich lamination, extrusion lamination, thermal lamination, and the like. A lamination method is mentioned.
  • the thickness of the adhesive is, for example, about 2 to 5 ⁇ m.
  • an anchor coat layer may be formed on the resin film and laminated.
  • the anchor coat layer the same adhesives as those exemplified for the adhesive layer 101B described later can be used. At this time, the thickness of the anchor coat layer is, for example, about 0.01 to 1.0 ⁇ m.
  • At least one of the surface and the inside of the base layer 101A may contain additives such as lubricants, flame retardants, antiblocking agents, antioxidants, light stabilizers, tackifiers, and antistatic agents. good. Only one type of additive may be used, or two or more types may be mixed and used.
  • a lubricant exists on the surface of the base material layer 101A.
  • the lubricant is not particularly limited, but preferably includes an amide-based lubricant.
  • Specific examples of amide lubricants include saturated fatty acid amides, unsaturated fatty acid amides, substituted amides, methylolamides, saturated fatty acid bisamides, unsaturated fatty acid bisamides, fatty acid ester amides, and aromatic bisamides.
  • saturated fatty acid amides include lauric acid amide, palmitic acid amide, stearic acid amide, behenic acid amide, and hydroxystearic acid amide.
  • unsaturated fatty acid amides include oleic acid amide and erucic acid amide.
  • substituted amides include N-oleyl palmitic acid amide, N-stearyl stearic acid amide, N-stearyl oleic acid amide, N-oleyl stearic acid amide, N-stearyl erucic acid amide and the like.
  • methylolamide include methylol stearamide.
  • saturated fatty acid bisamides include methylenebisstearic acid amide, ethylenebiscapric acid amide, ethylenebislauric acid amide, ethylenebisstearic acid amide, ethylenebishydroxystearic acid amide, ethylenebisbehenic acid amide, hexamethylenebisstearin. acid amide, hexamethylenebisbehenamide, hexamethylenehydroxystearic acid amide, N,N'-distearyladipic acid amide, N,N'-distearylsebacic acid amide and the like.
  • unsaturated fatty acid bisamides include ethylenebisoleic acid amide, ethylenebiserucic acid amide, hexamethylenebisoleic acid amide, N,N'-dioleyladipic acid amide, and N,N'-dioleylsebacic acid amide. etc.
  • fatty acid ester amides include stearamide ethyl stearate.
  • aromatic bisamide include m-xylylenebisstearic acid amide, m-xylylenebishydroxystearic acid amide, N,N'-distearyl isophthalic acid amide and the like.
  • Lubricants may be used singly or in combination of two or more.
  • a lubricant exists on the surface of the base material layer 101A, its amount is not particularly limited, but is preferably about 3 mg/m 2 or more, more preferably about 4 to 15 mg/m 2 , still more preferably 5 to 14 mg. / m 2 degree.
  • the lubricant present on the surface of the base layer 101A may be obtained by exuding the lubricant contained in the resin constituting the base layer 101A, or by applying the lubricant to the surface of the base layer 101A.
  • the thickness of the base material layer 101A is not particularly limited as long as it functions as a base material.
  • the thickness of each resin film constituting each layer is preferably about 2 to 25 ⁇ m.
  • the adhesive layer 101B is a layer provided between the base material layer 101A and the barrier layer 101C, if necessary, for the purpose of enhancing the adhesiveness between them.
  • the adhesive layer 101B is formed of an adhesive capable of bonding the base layer 101A and the barrier layer 101C.
  • the adhesive used to form the adhesive layer 101B is not limited, but may be any of a chemical reaction type, a solvent volatilization type, a heat melting type, a heat pressure type, and the like. Further, it may be a two-liquid curing adhesive (two-liquid adhesive), a one-liquid curing adhesive (one-liquid adhesive), or a resin that does not involve a curing reaction. Further, the adhesive layer 101B may be a single layer or multiple layers.
  • the adhesive component contained in the adhesive include polyesters such as polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polybutylene naphthalate, polyethylene isophthalate, and copolymerized polyester; polyether; polyurethane; epoxy resin; Phenolic resins; polyamides such as nylon 6, nylon 66, nylon 12, and copolymerized polyamides; polyolefin resins such as polyolefins, cyclic polyolefins, acid-modified polyolefins, and acid-modified cyclic polyolefins; polyvinyl acetate; cellulose; (meth)acrylic resins; polyimide; polycarbonate; amino resin such as urea resin and melamine resin; rubber such as chloroprene rubber, nitrile rubber and styrene-butadiene rubber; These adhesive components may be used singly or in combination of two or more.
  • polyurethane adhesives are preferred.
  • an appropriate curing agent can be used in combination with these adhesive component resins to increase the adhesive strength.
  • the curing agent is selected from among polyisocyanates, polyfunctional epoxy resins, oxazoline group-containing polymers, polyamine resins, acid anhydrides, etc., depending on the functional groups of the adhesive component.
  • polyurethane adhesives examples include polyurethane adhesives containing a main agent containing a polyol compound and a curing agent containing an isocyanate compound.
  • Two-component curing type polyurethane adhesives using polyols such as polyester polyols, polyether polyols, and acrylic polyols as main agents and aromatic or aliphatic polyisocyanates as curing agents are preferred.
  • the polyol compound it is preferable to use a polyester polyol having a hydroxyl group in a side chain in addition to the terminal hydroxyl group of the repeating unit. Since the adhesive layer 101B is made of a polyurethane adhesive, the exterior member 101 is endowed with excellent electrolytic solution resistance, and peeling of the base layer 101A is suppressed even if the electrolytic solution adheres to the side surface.
  • the adhesive layer 101B may contain other components as long as they do not interfere with adhesion, and may contain colorants, thermoplastic elastomers, tackifiers, fillers, and the like. Since the adhesive layer 101B contains a coloring agent, the exterior member 101 can be colored. Known substances such as pigments and dyes can be used as the colorant. In addition, only one type of colorant may be used, or two or more types may be mixed and used.
  • the type of pigment is not particularly limited as long as it does not impair the adhesiveness of the adhesive layer 101B.
  • organic pigments include azo-based, phthalocyanine-based, quinacridone-based, anthraquinone-based, dioxazine-based, indigothioindigo-based, perinone-perylene-based, isoindolenine-based, and benzimidazolone-based pigments.
  • pigments include carbon black, titanium oxide, cadmium, lead, chromium oxide, and iron pigments, as well as fine powder of mica and fish scale foil.
  • coloring agents for example, carbon black is preferable in order to make the outer appearance of the exterior member 101 black.
  • the average particle size of the pigment is not particularly limited, and is, for example, about 0.05 to 5 ⁇ m, preferably about 0.08 to 2 ⁇ m.
  • the average particle size of the pigment is the median size measured with a laser diffraction/scattering particle size distribution analyzer.
  • the content of the pigment in the adhesive layer 101B is not particularly limited as long as the exterior member 101 is colored.
  • the thickness of the adhesive layer 101B is not particularly limited as long as the substrate layer 101A and the barrier layer 101C can be adhered to each other. , about 5 ⁇ m or less, and preferable ranges include about 1 to 10 ⁇ m, about 1 to 5 ⁇ m, about 2 to 10 ⁇ m, and about 2 to 5 ⁇ m.
  • the colored layer is a layer provided as necessary between the base layer 101A and the barrier layer 101C (not shown).
  • a colored layer may be provided between the base layer 101A and the adhesive layer 101B and between the adhesive layer 101B and the barrier layer 101C.
  • a colored layer may be provided outside the base layer 101A. By providing the colored layer, the exterior member 101 can be colored.
  • the colored layer can be formed, for example, by applying ink containing a coloring agent to the surface of the base layer 101A, the adhesive layer 101B, or the barrier layer 101C.
  • a coloring agent such as pigments and dyes can be used as the colorant.
  • only one type of colorant may be used, or two or more types may be mixed and used.
  • colorant contained in the colored layer are the same as those exemplified for the adhesive layer 101B.
  • the barrier layer 101C is a layer that prevents at least moisture from entering.
  • the barrier layer 101C of the exterior member 101 contains aluminum alloy foil. The features of the aluminum alloy foil are described below.
  • ⁇ Fe 0.2% by mass or more and 2.0% by mass or less Fe crystallizes as an Al-Fe intermetallic compound during casting, and if the size of the compound is large, it becomes a recrystallization site during annealing. It has the effect of refining crystal grains.
  • the content of Fe is set within the above range.
  • the lower limit of the Fe content is preferably 0.5% by mass, and for the same reason, the lower limit of the Fe content is preferably 1.0% by mass and the upper limit is 1.8% by mass. .
  • Mg dissolves in aluminum and can increase the strength of the soft foil by solid-solution strengthening.
  • Mg since Mg is easily dissolved in aluminum, even if it is contained together with Fe, there is little risk that the intermetallic compound will coarsen and the conformability and rollability of the exterior member at corners and the like will deteriorate. If the Mg content is below the lower limit, the strength will not be sufficiently improved, and if the Mg content is above the upper limit, the aluminum alloy foil will become hard, resulting in reduced rollability and formability.
  • a particularly preferable range for the Mg content is 0.5% by mass or more and 5.0% by mass or less.
  • Mg improves the corrosion resistance of the lithium-ion secondary battery to the electrolyte solution.
  • the details of the mechanism are not clear, the greater the amount of Mg added, the more difficult it is for the aluminum alloy foil to react with lithium in the electrolytic solution, which can suppress the pulverization of the aluminum alloy foil and the formation of through holes.
  • the conformability of the exterior member at corners and the like is slightly reduced, it is desirable to set the lower limit of the Mg content to 0.5% by mass even when a particularly clear improvement in corrosion resistance is expected.
  • Si 0.5% by mass or less Si may be added for the purpose of increasing the strength of the foil if the amount is very small.
  • the composition of the aluminum alloy foil has a Si content of 0.5% by mass or less. Therefore, the size of the Al--Fe--Si based intermetallic compound produced during casting is reduced, and the elongation of the foil and the followability of the exterior member at corners and the like are enhanced. In addition, even when the thickness of the foil is thin, breakage originating from the intermetallic compound is less likely to occur, and rollability is improved.
  • the amount of Mg—Si based precipitates formed is reduced, so that the reduction in rollability and the amount of Mg in solid solution are less likely to occur, and the strength is less likely to be reduced.
  • the aluminum alloy foil can contain unavoidable impurities such as Cu and Mn.
  • the amount of each element in these unavoidable pure substances is desirably 0.1% by mass or less.
  • the upper limit of the content of the unavoidable impurities is not limited to the above numerical value.
  • Mn is difficult to dissolve in aluminum, unlike Mg, solid solution strengthening cannot be expected to significantly increase the strength of the soft foil. Also, if a large amount of Mn is added to an alloy with a high Fe content, there is a high risk of coarsening of intermetallic compounds and the formation of Al-Fe-Mn-based giant intermetallic compounds. There is a possibility that the followability of the member may be deteriorated. Therefore, the Mn content is desirably 0.1% by mass or less.
  • Each orientation density of Copper orientation and R orientation of the texture is 15 or less
  • the texture has a great influence on the mechanical properties of the foil and the followability of the exterior member at corners and the like. If either of the densities of the Copper orientation and the R orientation exceeds 15, uniform deformation cannot be achieved during molding, and there is a concern that the followability of the exterior member at corners and the like will be reduced. In order to obtain the followability of the exterior member at corners and the like, it is desirable to keep the density in each of the Copper orientation and the R orientation at 15 or less. More preferably, each orientation density is 10 or less.
  • the surface Mg concentration is 5.0 atomic percent or more, and the oxide film thickness is 80 ⁇ or more (Mg: 0.1% by mass or more and 1.5% by mass or less)
  • Mg 0.1% by mass or more and 1.5% by mass or less
  • the details of the mechanism are not clear, it has been confirmed that the Mg concentration on the foil surface and the thickness of the oxide film contribute to the corrosion resistance of the lithium ion secondary battery to the electrolyte. Corrosion resistance is improved due to the high Mg concentration on the foil surface and the formation of a thick oxide film. Therefore, when Mg is 0.1% by mass or more and 1.5% by mass or less, it is desirable to set the Mg concentration on the aluminum foil surface to 5.0 atomic percent or more and the oxide film thickness to be 80 ⁇ or more.
  • the surface Mg concentration is 15.0 atomic percent or more and the oxide film thickness is 200 ⁇ or more. More desirably, the surface Mg concentration is 20.0 atomic percent or more.
  • the surface Mg concentration is the Mg concentration in the surface portion from the outermost surface to a depth of 8 nm, and the Mg concentration is the amount with respect to the total of 100 atomic % of all elements.
  • the surface Mg concentration is 15.0 atomic percent or more and the oxide film thickness is 120 ⁇ or more (when Mg: more than 1.5% by mass and 5.0% by mass or less)
  • the Mg concentration on the foil surface and the thickness of the oxide film contribute to the corrosion resistance of the lithium ion secondary battery to the electrolytic solution. Corrosion resistance is improved due to the high Mg concentration on the foil surface and the formation of a thick oxide film. Therefore, when the Mg content is more than 1.5% by mass and 5.0% by mass or less, it is desirable to set the Mg concentration on the aluminum foil surface to 15.0 atomic percent or more and the oxide film thickness to be 120 ⁇ or more. More preferably, the surface Mg concentration is 20.0 atomic percent or more and the oxide film thickness is 220 ⁇ or more. More desirably, the surface Mg concentration is 25.0 atomic percent or more.
  • L1 is the length of the large-angle grain boundary per unit area
  • L2 is the length of the small-angle grain boundary measured by the backscattered electron diffraction method.
  • the ratio of High-Angle Grain Boundary (HAGB) and Low-Angle Grain Boundary (LAGB) in the recrystallized grain structure after annealing affects the elongation of the foil and the followability of the exterior material at the corners. affect. If the LAGB ratio is high in the recrystallized grain structure after the final annealing, localization of deformation tends to occur, and the followability of the exterior member at elongation, corners, and the like decreases. For this reason, by increasing the ratio of HAGB with L1/L2>3.0, high elongation and favorable followability of the exterior member at corners and the like can be expected. More preferably, L1/L2>5.0.
  • ⁇ Tensile strength 110 MPa or more and 180 MPa or less (when Mg: 0.1 mass% or more and 1.5 mass% or less) Mg: When it is 0.1% by mass or more and 1.5% by mass or less, a tensile strength of 110 MPa or more is required to dramatically improve the impact resistance and puncture strength of existing foils such as JIS A8079 and 8021. Saga is necessary.
  • the tensile strength is preferably 180 MPa or less in order to improve the followability of the exterior member at corners and the like. Tensile strength can be achieved by selection of composition and optimization of grain size.
  • Tensile strength 180 MPa or more (when Mg: more than 1.5% by mass and 5.0% by mass or less) Mg: When more than 1.5% by mass and 5.0% by mass or less, a tensile strength of 180 MPa or more is required to dramatically improve the impact resistance and puncture strength of existing foils such as JIS A8079 and 8021. is preferred. For the same reason, the tensile strength is desirably 200 MPa or more. However, the higher the tensile strength, the lower the conformability of the exterior member at corners and the like. As noted above, tensile strength can be achieved through composition selection and grain size optimization.
  • ⁇ Breaking elongation 10% or more (when Mg: 0.1% by mass or more and 1.5% by mass or less)
  • Mg 0.1% by mass or more and 1.5% by mass or less
  • Elongation properties can be achieved by composition selection and grain size refinement.
  • ⁇ Elongation 15% or more (when Mg: more than 1.5% by mass and 5.0% by mass or less)
  • the influence of elongation on the followability of the exterior member at corners etc. varies greatly depending on the molding method, and the followability of the exterior member at corners etc. is not determined solely by elongation, but aluminum packaging materials In the stretching process often used in , the higher the elongation of the aluminum alloy foil, the more advantageous the followability. is desirable.
  • elongation properties can be achieved through composition selection and grain size refinement.
  • ⁇ Average crystal grain size 25 ⁇ m or less
  • the average crystal grain size can be achieved by selecting the composition and manufacturing conditions that optimize the homogenization treatment and cold rolling rate.
  • An aluminum alloy ingot is cast by a conventional method such as a semi-continuous casting method.
  • the aluminum alloy ingot contains Fe: 0.2% by mass or more and 2.0% by mass or less, Mg: 0.1% by mass or more and 5.0% by mass or less, and the balance contains Al and unavoidable impurities. It has a composition of Mn: 0.1% by mass or less.
  • the obtained ingot is homogenized at 480-550° C. for 6-12 hours.
  • Homogenization treatment 450 to 550 ° C
  • the purpose of the homogenization treatment is to eliminate micro-segregation in the ingot and to adjust the distribution of intermetallic compounds.
  • the homogenization treatment of aluminum materials is performed at 400 to 600° C. for a long time, but in the present invention, it is necessary to consider grain refinement by adding Fe.
  • the temperature is less than 450° C., precipitation of Fe becomes insufficient, and there is concern about coarsening of crystal grains during the final annealing.
  • the ratio of in-situ recrystallization increases, the ratio of LAGB increases, and there is concern about a decrease in L1/L2.
  • the followability of the exterior member at corners or the like may be reduced due to an increase in the density of each orientation of the Copper orientation and the R orientation.
  • crystallized substances grow significantly, leading to coarsening of crystal grains during the final annealing and deterioration of followability of the exterior member at corners and the like. It is necessary to secure at least 3 hours or more for the homogenization treatment. If the time is less than 3 hours, precipitation is not sufficient and the density of the fine intermetallic compounds is lowered. Desirably, the temperature is 480-520° C. and the time is 5 hours or longer.
  • Hot rolling is performed to obtain an aluminum alloy plate with the desired thickness.
  • Hot rolling can be performed by a conventional method, and the coiling temperature for hot rolling is desirably higher than the recrystallization temperature, specifically 300° C. or higher. If the temperature is less than 300° C., fine Al—Fe intermetallic compounds of 0.3 ⁇ m or less are deposited.
  • recrystallized grains and fiber grains are mixed after hot rolling, and there is a concern that the grain size after intermediate annealing and final annealing will be non-uniform and the elongation characteristics will deteriorate, which is not desirable.
  • intermediate annealing After hot rolling, cold rolling, intermediate annealing, and final cold rolling are performed to obtain the aluminum alloy foil of the present invention with a thickness of 5 to 100 ⁇ m.
  • intermediate annealing There are two types of intermediate annealing: batch annealing, in which coils are placed in a furnace and held for a certain period of time, and rapid heating and rapid cooling in a continuous annealing line (hereinafter referred to as CAL annealing). Any method may be used when the intermediate annealing is applied, but CAL annealing is preferable for refining the crystal grains and increasing the strength.
  • Final cold rolling reduction 84.0% or more and 97.0% or less
  • the ratio of L1/L2 also decreases, so it is desirable to set the final cold rolling reduction to 97.0% or less.
  • the final cold rolling reduction is low, there is a concern that the followability of the exterior member at corners and the like may deteriorate due to coarsening of crystal grains and a decrease in L1/L2.
  • the more desirable final cold rolling reduction range is 90.0% or more and 93.0% or less.
  • final annealing is performed to obtain a soft foil.
  • Final annealing after foil rolling may generally be performed at 250°C to 400°C.
  • the temperature is more preferably 350°C to 400°C. If the final annealing temperature is low, the softening is insufficient, and there is concern that the L1/L2 ratio will decrease and the densities of each orientation of the Copper orientation and the R orientation will increase.
  • the concentration of Mg on the foil surface and the growth of the oxide film will be insufficient, resulting in a decrease in corrosion resistance.
  • the temperature exceeds 400° C., there is a concern that Mg will be excessively concentrated on the foil surface, discoloring the foil, or that the properties of the oxide film will change and microcracks will occur, resulting in a decrease in corrosion resistance. If the final annealing time is less than 5 hours, the effect of the final annealing is insufficient.
  • the obtained aluminum alloy foil has, for example, a tensile strength of 110 MPa to 180 MPa and an elongation of 10% or more at room temperature when Mg: 0.1 mass % to 1.5 mass %.
  • Mg more than 1.5% by mass and 5.0% by mass or less
  • the tensile strength is 180 MPa or more and the elongation is 15% or more.
  • the average crystal grain size is 25 ⁇ m or less. The average grain size can be determined by the cutting method specified in JIS G0551.
  • the thickness of the aluminum alloy foil in the exterior member 101 should exhibit at least a function as a barrier layer that suppresses the infiltration of moisture.
  • the upper limit of the thickness of the aluminum alloy foil is, for example, preferably about 85 ⁇ m or less, more preferably about 50 ⁇ m or less, even more preferably about 45 ⁇ m or less, and particularly preferably about 40 ⁇ m or less.
  • the lower limit is preferably about 10 ⁇ m or more, more preferably about 20 ⁇ m or more, and more preferably about 25 ⁇ m or more.
  • the aluminum alloy foil is provided with a corrosion-resistant film in order to prevent dissolution and corrosion of the aluminum alloy foil.
  • the aluminum alloy foil may be provided with a corrosion resistant coating on both sides.
  • the corrosion-resistant film includes, for example, hydrothermal transformation treatment such as boehmite treatment, chemical conversion treatment, anodizing treatment, plating treatment such as nickel and chromium, and corrosion prevention treatment such as coating with a coating agent on aluminum alloy foil.
  • the treatment for forming the corrosion-resistant film one type may be performed, or two or more types may be used in combination. Also, not only one layer but also multiple layers can be used.
  • the hydrothermal transformation treatment and the anodizing treatment are treatments in which the surface of the metal foil is dissolved with a treating agent to form a metal compound having excellent corrosion resistance. These treatments are sometimes included in the definition of chemical conversion treatment.
  • the aluminum alloy foil has a corrosion-resistant film
  • the aluminum alloy foil includes the corrosion-resistant film.
  • the corrosion-resistant coating prevents delamination between the aluminum alloy foil and the base material layer during molding of the exterior member 101, and dissolves the surface of the aluminum alloy foil by hydrogen fluoride generated by the reaction between the electrolyte and moisture. Prevents corrosion, dissolution and corrosion of aluminum oxide present on the surface of the aluminum alloy foil, improves the adhesion (wettability) of the surface of the aluminum alloy foil, and prevents the base layer and the aluminum alloy foil from heat-sealing. and the effect of preventing delamination between the base material layer and the aluminum alloy foil during molding.
  • corrosion-resistant coatings formed by chemical conversion treatment are known, and are mainly composed of at least one of phosphates, chromates, fluorides, triazinethiol compounds, and rare earth oxides. and corrosion-resistant coatings containing.
  • Examples of chemical conversion treatments using phosphate and chromate include chromic acid chromate treatment, phosphoric acid chromate treatment, phosphoric acid-chromate treatment, and chromate treatment.
  • Examples of compounds include chromium nitrate, chromium fluoride, chromium sulfate, chromium acetate, chromium oxalate, chromium biphosphate, chromium acetyl acetate, chromium chloride, potassium chromium sulfate, and the like.
  • Phosphorus compounds used for these treatments include sodium phosphate, potassium phosphate, ammonium phosphate, polyphosphoric acid, and the like.
  • Examples of the chromate treatment include etching chromate treatment, electrolytic chromate treatment, coating-type chromate treatment, etc., and coating-type chromate treatment is preferred.
  • the inner layer side surface of the barrier layer (for example, aluminum alloy foil) is first subjected to a well-known method such as an alkali immersion method, an electrolytic cleaning method, an acid cleaning method, an electrolytic acid cleaning method, an acid activation method, or the like.
  • metal phosphate such as Cr (chromium) phosphate, Ti (titanium) phosphate, Zr (zirconium) phosphate, Zn (zinc) phosphate is applied to the degreased surface.
  • a processing solution mainly composed of a salt and a mixture of these metal salts a processing solution mainly composed of a non-metal phosphate salt and a mixture of these non-metal salts, or a mixture of these and a synthetic resin.
  • This is a treatment in which a treatment liquid composed of a mixture is applied by a well-known coating method such as a roll coating method, a gravure printing method, or an immersion method, and then dried.
  • Various solvents such as water, alcohol-based solvents, hydrocarbon-based solvents, ketone-based solvents, ester-based solvents, and ether-based solvents can be used as the treatment liquid, and water is preferred.
  • the resin component used at this time includes polymers such as phenolic resins and acrylic resins. and the chromate treatment used.
  • the repeating units represented by the following general formulas (1) to (4) may be contained singly or in any combination of two or more. good too.
  • the acrylic resin is polyacrylic acid, acrylic acid methacrylic acid ester copolymer, acrylic acid maleic acid copolymer, acrylic acid styrene copolymer, or derivatives thereof such as sodium salts, ammonium salts, and amine salts. is preferred.
  • derivatives of polyacrylic acid such as ammonium salt, sodium salt or amine salt of polyacrylic acid are preferred.
  • polyacrylic acid means a polymer of acrylic acid.
  • the acrylic resin is preferably a copolymer of acrylic acid and dicarboxylic acid or dicarboxylic anhydride, and the ammonium salt, sodium salt, Alternatively, it is also preferably an amine salt. Only one type of acrylic resin may be used, or two or more types may be mixed and used.
  • X represents a hydrogen atom, hydroxy group, alkyl group, hydroxyalkyl group, allyl group or benzyl group.
  • R 1 and R 2 are the same or different and represent a hydroxy group, an alkyl group or a hydroxyalkyl group.
  • alkyl groups represented by X, R 1 and R 2 in general formulas (1) to (4) include methyl group, ethyl group, n-propyl group, isopropyl group, n-butyl group, isobutyl group, A linear or branched alkyl group having 1 to 4 carbon atoms such as a tert-butyl group can be mentioned.
  • hydroxyalkyl groups represented by X, R 1 and R 2 include hydroxymethyl group, 1-hydroxyethyl group, 2-hydroxyethyl group, 1-hydroxypropyl group, 2-hydroxypropyl group, 3- A straight or branched chain having 1 to 4 carbon atoms substituted with one hydroxy group such as hydroxypropyl group, 1-hydroxybutyl group, 2-hydroxybutyl group, 3-hydroxybutyl group and 4-hydroxybutyl group An alkyl group is mentioned.
  • the alkyl groups and hydroxyalkyl groups represented by X, R 1 and R 2 may be the same or different.
  • X is preferably a hydrogen atom, a hydroxy group or a hydroxyalkyl group.
  • the number average molecular weight of the aminated phenol polymer having repeating units represented by formulas (1) to (4) is, for example, preferably about 500 to 1,000,000, more preferably about 1,000 to 20,000. more preferred.
  • the aminated phenol polymer is produced, for example, by polycondensing a phenol compound or naphthol compound and formaldehyde to produce a polymer comprising repeating units represented by the general formula (1) or general formula (3), followed by formaldehyde. and an amine (R 1 R 2 NH) to introduce a functional group (--CH 2 NR 1 R 2 ) into the polymer obtained above.
  • An aminated phenol polymer is used individually by 1 type or in mixture of 2 or more types.
  • the corrosion-resistant film is formed by a coating-type corrosion prevention treatment in which a coating agent containing at least one selected from the group consisting of rare earth element oxide sol, anionic polymer, and cationic polymer is applied.
  • a coating agent containing at least one selected from the group consisting of rare earth element oxide sol, anionic polymer, and cationic polymer is applied.
  • the coating agent may further contain phosphoric acid or a phosphate, a cross-linking agent for cross-linking the polymer.
  • rare earth element oxide sol rare earth element oxide fine particles (for example, particles having an average particle size of 100 nm or less) are dispersed in a liquid dispersion medium.
  • rare earth element oxides include cerium oxide, yttrium oxide, neodymium oxide, and lanthanum oxide, and cerium oxide is preferable from the viewpoint of further improving adhesion.
  • the rare earth element oxides contained in the corrosion-resistant coating can be used singly or in combination of two or more.
  • various solvents such as water, alcohol solvents, hydrocarbon solvents, ketone solvents, ester solvents, and ether solvents can be used, with water being preferred.
  • the cationic polymer include polyethyleneimine, an ionic polymer complex composed of a polymer containing polyethyleneimine and carboxylic acid, a primary amine-grafted acrylic resin obtained by graft-polymerizing a primary amine to an acrylic backbone, polyallylamine, or a derivative thereof. , aminated phenols and the like are preferred.
  • the anionic polymer is preferably poly(meth)acrylic acid or a salt thereof, or a copolymer containing (meth)acrylic acid or a salt thereof as a main component.
  • the cross-linking agent is preferably at least one selected from the group consisting of a compound having a functional group such as an isocyanate group, a glycidyl group, a carboxyl group, or an oxazoline group, and a silane coupling agent.
  • the phosphoric acid or phosphate is preferably condensed phosphoric acid or condensed phosphate.
  • fine particles of metal oxides such as aluminum oxide, titanium oxide, cerium oxide, and tin oxide, and barium sulfate are dispersed in phosphoric acid, which is applied to the surface of the barrier layer. C. or more, and those formed by performing baking processing are mentioned.
  • the corrosion-resistant film may, if necessary, have a laminated structure in which at least one of a cationic polymer and an anionic polymer is further laminated.
  • a cationic polymer and anionic polymers include those described above.
  • the analysis of the composition of the corrosion-resistant coating can be performed using, for example, time-of-flight secondary ion mass spectrometry.
  • the amount of the corrosion - resistant film formed on the surface of the aluminum alloy foil in the chemical conversion treatment is not particularly limited. is about 0.5 to 50 mg, preferably about 1.0 to 40 mg in terms of chromium, the phosphorus compound is about 0.5 to 50 mg, preferably about 1.0 to 40 mg in terms of phosphorus, and aminated phenol polymer is contained in a ratio of, for example, about 1.0 to 200 mg, preferably about 5.0 to 150 mg.
  • the thickness of the corrosion-resistant coating is not particularly limited, but is preferably about 1 nm to 20 ⁇ m, more preferably 1 nm to 100 nm, from the viewpoint of cohesion of the coating and adhesion to the barrier layer and the heat-sealable resin layer. about 1 nm to 50 nm, more preferably about 1 nm to 50 nm.
  • the thickness of the corrosion-resistant film can be measured by observation with a transmission electron microscope, or by a combination of observation with a transmission electron microscope and energy dispersive X-ray spectroscopy or electron beam energy loss spectroscopy.
  • secondary ions composed of Ce, P and O for example, at least one of Ce 2 PO 4 + and CePO 4 ⁇ species
  • secondary ions composed of Cr, P, and O eg, at least one of CrPO 2 + and CrPO 4 ⁇
  • a solution containing a compound used for forming a corrosion-resistant film is applied to the surface of the aluminum alloy foil by a bar coating method, a roll coating method, a gravure coating method, an immersion method, or the like. is carried out by heating so that the temperature of is about 70 to 200°C.
  • the aluminum alloy foil may be previously subjected to degreasing treatment by an alkali immersion method, an electrolytic cleaning method, an acid cleaning method, an electrolytic acid cleaning method, or the like. By performing the degreasing treatment in this way, it becomes possible to perform the chemical conversion treatment on the surface of the aluminum alloy foil more efficiently.
  • an acid degreasing agent obtained by dissolving a fluorine-containing compound in an inorganic acid for degreasing treatment it is possible to form not only the degreasing effect of the metal foil but also the passive metal fluoride. In such cases, only degreasing treatment may be performed.
  • the heat-fusible resin layer 101D corresponds to the innermost layer, and exhibits a function of sealing the electrode body 200 by heat-fusifying the heat-fusible resin layers 101D to each other when the electricity storage device 10 is assembled. layer (sealant layer).
  • the resin forming the heat-fusible resin layer 101D is not particularly limited as long as it is heat-fusible, but resins containing a polyolefin skeleton such as polyolefin and acid-modified polyolefin are preferable.
  • the fact that the resin forming the heat-fusible resin layer 101D contains a polyolefin skeleton can be analyzed by, for example, infrared spectroscopy, gas chromatography-mass spectrometry, or the like. Further, when the resin forming the heat-fusible resin layer 101D is analyzed by infrared spectroscopy, it is preferable that a peak derived from maleic anhydride is detected.
  • peaks derived from maleic anhydride are detected near wavenumbers of 1760 cm@-1 and 1780 cm@-1.
  • the heat-sealable resin layer 101D is a layer composed of maleic anhydride-modified polyolefin, a peak derived from maleic anhydride is detected by infrared spectroscopy.
  • the degree of acid denaturation is low, the peak may be too small to be detected. In that case, it can be analyzed by nuclear magnetic resonance spectroscopy.
  • polyolefins include polyethylenes such as low-density polyethylene, medium-density polyethylene, high-density polyethylene, and linear low-density polyethylene; ethylene- ⁇ -olefin copolymers; block copolymers of ethylene), random copolymers of polypropylene (for example, random copolymers of propylene and ethylene); propylene- ⁇ -olefin copolymers; ethylene-butene-propylene terpolymers; Among these, polypropylene is preferred.
  • the polyolefin resin is a copolymer, it may be a block copolymer or a random copolymer. These polyolefin-based resins may be used alone or in combination of two or more.
  • the polyolefin may be a cyclic polyolefin.
  • a cyclic polyolefin is a copolymer of an olefin and a cyclic monomer.
  • the olefin which is a constituent monomer of the cyclic polyolefin, include ethylene, propylene, 4-methyl-1-pentene, styrene, butadiene, and isoprene. be done.
  • Examples of cyclic monomers constituting cyclic polyolefins include cyclic alkenes such as norbornene; cyclic dienes such as cyclopentadiene, dicyclopentadiene, cyclohexadiene and norbornadiene. Among these, cyclic alkenes are preferred, and norbornene is more preferred.
  • Acid-modified polyolefin is a polymer modified by block polymerization or graft polymerization of polyolefin with an acid component.
  • the acid-modified polyolefin the above polyolefin, a copolymer obtained by copolymerizing the above polyolefin with a polar molecule such as acrylic acid or methacrylic acid, or a polymer such as crosslinked polyolefin can be used.
  • acid components used for acid modification include carboxylic acids such as maleic acid, acrylic acid, itaconic acid, crotonic acid, maleic anhydride and itaconic anhydride, and anhydrides thereof.
  • the acid-modified polyolefin may be an acid-modified cyclic polyolefin.
  • Acid-modified cyclic polyolefin is a polymer obtained by copolymerizing a part of the monomers constituting the cyclic polyolefin in place of the acid component, or by block-polymerizing or graft-polymerizing the acid component to the cyclic polyolefin. be.
  • the acid-modified cyclic polyolefin is the same as described above.
  • the acid component used for acid modification is the same as the acid component used for modification of polyolefin.
  • Preferable acid-modified polyolefins include polyolefins modified with carboxylic acid or its anhydride, polypropylene modified with carboxylic acid or its anhydride, maleic anhydride-modified polyolefin, and maleic anhydride-modified polypropylene.
  • the heat-fusible resin layer 101D may be formed of one type of resin alone, or may be formed of a blend polymer in which two or more types of resin are combined. Furthermore, the heat-fusible resin layer 101D may be formed of only one layer, or may be formed of two or more layers of the same or different resins.
  • the heat-fusible resin layer 101D may contain a lubricant or the like as necessary.
  • a lubricant is not particularly limited, and known lubricants can be used. Lubricants may be used singly or in combination of two or more.
  • the lubricant is not particularly limited, but preferably includes an amide-based lubricant. Specific examples of the lubricant include those exemplified for the base material layer 101A. Lubricants may be used singly or in combination of two or more.
  • the amount of the lubricant is not particularly limited, but from the viewpoint of enhancing the conformability of the exterior member to the corners of the exterior member 101, it is preferably 10 to 10. About 50 mg/m2, more preferably about 15 to 40 mg/m2.
  • the lubricant present on the surface of the heat-fusible resin layer 101D may be obtained by exuding the lubricant contained in the resin constituting the heat-fusible resin layer 101D.
  • the surface may be coated with a lubricant.
  • the thickness of the heat-fusible resin layer 101D is not particularly limited as long as the heat-fusible resin layers are heat-sealed to each other to exhibit the function of sealing the electricity storage device element. About 85 ⁇ m or less, more preferably about 15 to 85 ⁇ m. For example, when the thickness of the adhesive layer 101E described later is 10 ⁇ m or more, the thickness of the heat-fusible resin layer 101D is preferably about 85 ⁇ m or less, more preferably about 15 to 45 ⁇ m. When the thickness of the adhesive layer 101E described later is less than 10 ⁇ m or when the adhesive layer 101E is not provided, the thickness of the heat-fusible resin layer 101D is preferably about 20 ⁇ m or more, more preferably 35 to 85 ⁇ m. degree.
  • the adhesive layer 101E is a layer provided between the barrier layer 101C (or acid-resistant film) and the heat-fusible resin layer 101D as necessary in order to firmly bond them.
  • the adhesive layer 101E is made of a resin capable of bonding the barrier layer 101C and the heat-fusible resin layer 101D.
  • the adhesive layer 101E is preferably formed of a cured product of a resin composition containing a curable resin.
  • a curable resin means a curable resin such as a thermosetting resin or an ionizing radiation curable resin, and does not have a distinct melting peak temperature after curing, for example.
  • the resin used for forming the adhesive layer 101E for example, the same adhesives as those exemplified for the adhesive layer 101B can be used.
  • the resin used to form the adhesive layer 101E preferably contains a polyolefin skeleton, and includes the polyolefins and acid-modified polyolefins exemplified for the heat-fusible resin layer 101D.
  • Whether the resin forming the adhesive layer 101E contains a polyolefin skeleton can be analyzed by, for example, infrared spectroscopy, gas chromatography mass spectrometry, or the like, and the analysis method is not particularly limited. Further, when the resin forming the adhesive layer 101E is analyzed by infrared spectroscopy, it is preferable that a peak derived from maleic anhydride is detected.
  • peaks derived from maleic anhydride are detected near wavenumbers of 1760 cm ⁇ 1 and 1780 cm ⁇ 1 .
  • the peak may be too small to be detected. In that case, it can be analyzed by nuclear magnetic resonance spectroscopy.
  • the adhesive layer 101E preferably contains acid-modified polyolefin.
  • acid-modified polyolefins are polyolefins modified with carboxylic acid or its anhydride, polypropylene modified with carboxylic acid or its anhydride, maleic anhydride-modified polyolefin, and maleic anhydride-modified polypropylene.
  • the adhesive layer 101E is a cured product of a resin composition containing an acid-modified polyolefin and a curing agent. It is more preferable to have In this case, the acid-modified polyolefin and the curing agent constitute the curable resin.
  • Preferred examples of the acid-modified polyolefin include those mentioned above.
  • the adhesive layer 101E is a cured product of a resin composition containing acid-modified polyolefin and at least one selected from the group consisting of compounds having an isocyanate group, compounds having an oxazoline group, and compounds having an epoxy group.
  • a cured product of a resin composition containing an acid-modified polyolefin and at least one selected from the group consisting of a compound having an isocyanate group and a compound having an epoxy group is particularly preferred.
  • the adhesive layer 101E preferably contains at least one selected from the group consisting of polyurethane, polyester, and epoxy resin, and more preferably contains polyurethane and epoxy resin.
  • the polyester for example, an amide ester resin is preferable.
  • Amide ester resins are generally produced by the reaction of carboxyl groups and oxazoline groups.
  • the adhesive layer 101E is more preferably a cured product of a resin composition containing at least one of these resins and the acid-modified polyolefin.
  • the adhesive layer 101E contains an isocyanate group-containing compound, an oxazoline group-containing compound, or an unreacted product of a curing agent such as an epoxy resin
  • the presence of the unreacted product can be detected by, for example, infrared spectroscopy, It can be confirmed by a method selected from Raman spectroscopy, time-of-flight secondary ion mass spectrometry (TOF-SIMS), and the like.
  • the adhesive layer 101E contains at least one selected from the group consisting of oxygen atoms, heterocycles, C ⁇ N bonds, and C—O—C bonds It is preferably a cured product of a resin composition containing one curing agent.
  • the curing agent having a heterocyclic ring includes, for example, a curing agent having an oxazoline group, a curing agent having an epoxy group, and the like.
  • the curing agent having a C ⁇ N bond includes a curing agent having an oxazoline group, a curing agent having an isocyanate group, and the like.
  • curing agents having a C—O—C bond examples include curing agents having an oxazoline group, curing agents having an epoxy group, and polyurethanes.
  • the fact that the adhesive layer 101E is a cured product of a resin composition containing these curing agents can be achieved by, for example, gas chromatography mass spectrometry (GCMS), infrared spectroscopy (IR), time-of-flight secondary ion mass spectrometry (TOF). -SIMS) and X-ray photoelectron spectroscopy (XPS).
  • GCMS gas chromatography mass spectrometry
  • IR infrared spectroscopy
  • TOF time-of-flight secondary ion mass spectrometry
  • -SIMS X-ray photoelectron spectroscopy
  • the compound having an isocyanate group is not particularly limited, but from the viewpoint of effectively increasing the adhesion between the barrier layer 101C and the adhesive layer 101E, polyfunctional isocyanate compounds are preferred.
  • the polyfunctional isocyanate compound is not particularly limited as long as it is a compound having two or more isocyanate groups.
  • Specific examples of polyfunctional isocyanate curing agents include pentane diisocyanate (PDI), isophorone diisocyanate (IPDI), hexamethylene diisocyanate (HDI), tolylene diisocyanate (TDI), diphenylmethane diisocyanate (MDI), polymerization and nurate compounds, mixtures thereof, copolymers with other polymers, and the like.
  • adducts, burettes, isocyanurates and the like are included.
  • the content of the compound having an isocyanate group in the adhesive layer 101E is preferably in the range of 0.1 to 50% by mass, more preferably 0.5 to 40% by mass, in the resin composition constituting the adhesive layer 101E. A range is more preferred. This can effectively improve the adhesion between the barrier layer 101C and the adhesive layer 101E.
  • the compound having an oxazoline group is not particularly limited as long as it is a compound having an oxazoline skeleton.
  • Specific examples of compounds having an oxazoline group include those having a polystyrene main chain and those having an acrylic main chain.
  • the Epocross series by Nippon Shokubai Co., Ltd. etc. are mentioned, for example.
  • the ratio of the compound having an oxazoline group in the adhesive layer 101E is preferably in the range of 0.1 to 50% by mass, more preferably 0.5 to 40% by mass, in the resin composition constituting the adhesive layer 101E. is more preferable. This can effectively improve the adhesion between the barrier layer 101C and the adhesive layer 101E.
  • Examples of compounds having an epoxy group include epoxy resins.
  • the epoxy resin is not particularly limited as long as it is a resin capable of forming a crosslinked structure with epoxy groups present in the molecule, and known epoxy resins can be used.
  • the weight average molecular weight of the epoxy resin is preferably about 50 to 2000, more preferably about 100 to 1000, still more preferably about 200 to 800.
  • the weight average molecular weight of the epoxy resin is a value measured by gel permeation chromatography (GPC) under conditions using polystyrene as a standard sample.
  • epoxy resins include glycidyl ether derivatives of trimethylolpropane, bisphenol A diglycidyl ether, modified bisphenol A diglycidyl ether, novolac glycidyl ether, glycerin polyglycidyl ether, and polyglycerin polyglycidyl ether.
  • An epoxy resin may be used individually by 1 type, and may be used in combination of 2 or more types.
  • the proportion of the epoxy resin in the adhesive layer 101E is preferably in the range of 0.1 to 50% by mass, more preferably in the range of 0.5 to 40% by mass, in the resin composition constituting the adhesive layer 101E. is more preferred. This can effectively improve the adhesion between the barrier layer 101C and the adhesive layer 101E.
  • the polyurethane is not particularly limited, and known polyurethanes can be used.
  • the adhesive layer 101E may be, for example, a cured product of two-component curing type polyurethane.
  • the proportion of polyurethane in the adhesive layer 101E is preferably in the range of 0.1 to 50% by mass, more preferably in the range of 0.5 to 40% by mass, in the resin composition constituting the adhesive layer 101E. more preferred.
  • the adhesion between the barrier layer 101C and the adhesive layer 101E can be effectively increased in an atmosphere containing a component that induces corrosion of the barrier layer, such as an electrolytic solution.
  • the adhesive layer 101E is a cured product of a resin composition containing at least one selected from the group consisting of a compound having an isocyanate group, a compound having an oxazoline group, and an epoxy resin, and the acid-modified polyolefin.
  • the acid-modified polyolefin functions as a main agent, and the compound having an isocyanate group, the compound having an oxazoline group, and the compound having an epoxy group each function as a curing agent.
  • the upper limit of the thickness of the adhesive layer 101E is preferably about 50 ⁇ m or less, about 40 ⁇ m or less, about 30 ⁇ m or less, about 20 ⁇ m or less, or about 5 ⁇ m or less, and the lower limit is preferably about 0.1 ⁇ m or more.
  • the thickness range is preferably about 0.1 to 50 ⁇ m, about 0.1 to 40 ⁇ m, about 0.1 to 30 ⁇ m, about 0.1 to 20 ⁇ m, 0 .1 to 5 ⁇ m, 0.5 to 50 ⁇ m, 0.5 to 40 ⁇ m, 0.5 to 30 ⁇ m, 0.5 to 20 ⁇ m, and 0.5 to 5 ⁇ m.
  • the thickness is preferably about 1 to 10 ⁇ m, more preferably about 1 to 5 ⁇ m. In the case of using the resin exemplified for the heat-fusible resin layer 101D, the thickness is preferably about 2 to 50 ⁇ m, more preferably about 10 to 40 ⁇ m.
  • the adhesive layer 101E is the adhesive exemplified for the adhesive layer 101B or a cured product of a resin composition containing an acid-modified polyolefin and a curing agent, for example, the resin composition is applied and cured by heating or the like. Thereby, the adhesive layer 101E can be formed. Further, when using the resin exemplified for the heat-fusible resin layer 101D, for example, the heat-fusible resin layer 101D and the adhesive layer 101E can be formed by extrusion molding.
  • the exterior member 101 is provided on the substrate layer 101A (substrate A surface coating layer 101F may be provided on the layer 101A opposite the barrier layer 101C.
  • the surface coating layer 101F is a layer positioned on the outermost layer side of the exterior member 101 when the power storage device is assembled using the exterior member 101 .
  • the surface coating layer 101F can be made of resin such as polyvinylidene chloride, polyester, polyurethane, acrylic resin, and epoxy resin, for example.
  • the resin forming the surface coating layer 101F is a curable resin
  • the resin may be either a one-liquid curable type or a two-liquid curable type, preferably the two-liquid curable type.
  • the two-liquid curing resin include two-liquid curing polyurethane, two-liquid curing polyester, and two-liquid curing epoxy resin. Among these, two-liquid curable polyurethane is preferred.
  • two-liquid curable polyurethanes examples include polyurethanes containing a main agent containing a polyol compound and a curing agent containing an isocyanate compound.
  • Preferable examples include two-component curing type polyurethanes using polyols such as polyester polyols, polyether polyols, and acrylic polyols as main agents and aromatic or aliphatic polyisocyanates as curing agents.
  • the polyol compound it is preferable to use a polyester polyol having a hydroxyl group in a side chain in addition to the terminal hydroxyl group of the repeating unit. Since the surface coating layer 101F is made of polyurethane, the exterior member 101 is endowed with excellent electrolyte resistance.
  • the surface coating layer 101F may be coated with at least one of the surface and the inside of the surface coating layer 101F according to the functionality to be provided on the surface coating layer 101F and the surface thereof, and if necessary, the above-described lubricant or anti-rust agent.
  • Additives such as blocking agents, matting agents, flame retardants, antioxidants, tackifiers and antistatic agents may be included.
  • the additive include fine particles having an average particle size of about 0.5 nm to 5 ⁇ m. The average particle size of the additive is the median size measured with a laser diffraction/scattering particle size distribution analyzer.
  • the shape of the additive is not particularly limited, and examples thereof include spherical, fibrous, plate-like, amorphous, scale-like, and the like.
  • additives include talc, silica, graphite, kaolin, montmorillonite, mica, hydrotalcite, silica gel, zeolite, aluminum hydroxide, magnesium hydroxide, zinc oxide, magnesium oxide, aluminum oxide, neodymium oxide, and antimony oxide.
  • Additives may be used singly or in combination of two or more.
  • silica, barium sulfate, and titanium oxide are preferred from the viewpoint of dispersion stability and cost.
  • the additive may be subjected to various surface treatments such as insulation treatment and high-dispersion treatment.
  • a method for forming the surface covering layer 101F is not particularly limited, and an example thereof includes a method of applying a resin for forming the surface covering layer 101F.
  • a resin mixed with the additives may be applied.
  • the thickness of the surface coating layer 101F is not particularly limited as long as the above functions of the surface coating layer 101F are exhibited.
  • the method for manufacturing the exterior member 101 is not particularly limited as long as a laminate obtained by laminating the layers included in the exterior member 101 of the present embodiment is obtained. A method including a step of laminating the adhesive resin layers 101D in this order may be mentioned. As described above, as the barrier layer 101C, an aluminum alloy foil that satisfies the predetermined composition described above can be used.
  • a laminate (hereinafter also referred to as "laminate A") is formed by sequentially laminating a base layer 101A, an adhesive layer 101B, and a barrier layer 101C.
  • the laminate A is formed by applying an adhesive used for forming the adhesive layer 101B on the base layer 101A or on the barrier layer 101C whose surface is chemically treated as necessary, by gravure coating, After coating and drying by a coating method such as a roll coating method, the barrier layer 101C or base layer 101A is laminated and the adhesive layer 101B is cured by a dry lamination method.
  • a heat-fusible resin layer 101D is laminated.
  • the heat-fusible resin layer 101D is directly laminated on the barrier layer 101C
  • the heat-fusible resin layer 101D is laminated on the barrier layer 101C of the laminate A by a method such as thermal lamination or extrusion lamination. do it.
  • the adhesive layer 101E is provided between the barrier layer 101C and the heat-fusible resin layer 101D, for example, (1) the adhesive layer 101E and the heat-fusible resin layer are placed on the barrier layer 101C of the laminate A.
  • the barrier layer 101C of the laminate A with an adhesive for forming the adhesive layer 101E in solution,
  • an adhesive for forming the adhesive layer 101E for example, a drying method, a baking method, or the like is used to laminate the adhesive layer 101E, and a heat-fusible resin layer 101D that has been formed in a sheet form in advance is laminated on the adhesive layer 101E.
  • the surface covering layer 101F is laminated on the surface of the base material layer 101A opposite to the barrier layer 101C.
  • the surface covering layer 101F can be formed, for example, by coating the surface of the base material layer 101A with the above-described resin that forms the surface covering layer 101F.
  • the order of the step of laminating the barrier layer 101C on the surface of the base layer 101A and the step of laminating the surface coating layer 101F on the surface of the base layer 101A is not particularly limited.
  • the barrier layer 101C may be formed on the surface of the base layer 101A opposite to the surface coating layer 101F.
  • each layer constituting the laminate may be subjected to surface activation treatment such as corona treatment, blast treatment, oxidation treatment, ozone treatment, etc., as necessary to improve workability.
  • surface activation treatment such as corona treatment, blast treatment, oxidation treatment, ozone treatment, etc.
  • the printability of the ink onto the surface of the substrate layer 101A can be improved.
  • the exterior member 101 has one or more layers having a buffer function (hereinafter referred to as "buffer layers”) outside the heat-fusible resin layer 101D, more preferably outside the barrier layer 101C. preferably.
  • the buffer layer may be laminated on the outside of the base layer 101A, and the base layer 101A may also function as a buffer layer.
  • the plurality of buffer layers may be adjacent to each other, or may be laminated via the base layer 101A or the barrier layer 101C.
  • the material that constitutes the cushioning layer can be arbitrarily selected from materials that have cushioning properties.
  • Materials with cushioning properties are, for example, rubber, non-woven fabrics, or foam sheets.
  • Rubber is, for example, natural rubber, fluororubber, or silicone rubber.
  • the rubber hardness is preferably about 20-90.
  • the material constituting the nonwoven fabric is preferably a material having excellent heat resistance.
  • the lower limit of the thickness of the buffer layer is preferably 100 ⁇ m, more preferably 200 ⁇ m, and even more preferably 1000 ⁇ m.
  • the upper limit of the thickness of the buffer layer is preferably 5000 ⁇ m, more preferably 3000 ⁇ m.
  • Preferred ranges for the thickness of the buffer layer are 100 ⁇ m to 5000 ⁇ m, 100 ⁇ m to 3000 ⁇ m, 200 ⁇ m to 3000 ⁇ m, 1000 ⁇ m to 5000 ⁇ m, or 1000 ⁇ m to 3000 ⁇ m.
  • the thickness range of the buffer layer is most preferably 1000 ⁇ m to 3000 ⁇ m.
  • the lower limit of the thickness of the buffer layer is preferably 0.5 mm.
  • the upper limit of the thickness of the buffer layer is preferably 10 mm, more preferably 5 mm, still more preferably 2 mm.
  • the preferred range of thickness of the buffer layer is 0.5 mm to 10 mm, 0.5 mm to 5 mm, or 0.5 mm to 2 mm.
  • the cushioning layer functions as a cushion, thereby suppressing damage to the exterior member 101 due to impact when the power storage device 10 is dropped or handling during manufacturing of the power storage device 10 . be done.
  • FIG. 4 is a side view showing a state in which the exterior member 101 is wrapped around the electrode body 200 during the manufacture of the electricity storage device 10.
  • an exterior member 101 is wound around the electrode assembly 200 .
  • the outermost layer of electrode body 200 does not necessarily have to be an electrode, and may be, for example, a protective tape or a separator.
  • the facing surfaces (the heat-fusible resin layers) of the exterior member 101 are heat-sealed to form the first sealing portion 110.
  • the root portion of the first sealing portion 110 is on the side 135 of the exterior body 100 .
  • Side 135 is formed at the boundary between first surface 130 and second surface 140 having a smaller area than first surface 130 . That is, it can be said that the root portion of the first sealing portion 110 is formed at the boundary between the first surface 130 and the second surface 140, and does not exist on either the first surface 130 or the second surface 140. It can be said.
  • the root portion of the first sealing portion 110 may exist on the second surface 140 .
  • first sealing portion 110 is bent toward second surface 140 about side 135 .
  • the first sealing portion 110 is in contact with the second surface 140 and covers substantially the entire second surface 140 . Note that “substantially the entire second surface 140 ” means a region that occupies 75% or more of the area of the second surface 140 .
  • the first sealing portion 110 is not formed on the first surface 130 having a large area.
  • the first surface 130 is flat compared to when a sealing portion such as the first sealing portion 110 is in contact with the first surface 130 . Therefore, even if another power storage device 10 is placed on the first surface 130, the other power storage device 10 does not tilt.
  • the power storage device 10 when a plurality of power storage devices 10 are stacked, uneven distribution of pressure applied to the power storage device 10 below can be suppressed.
  • the first sealing portion 110 is not arranged on the surface (first surface 130) adjacent to the adjacent power storage devices 10. .
  • such a configuration is preferable from the viewpoint that it is necessary to uniformly apply a high pressure from the outer surface of the battery in order to exhibit the battery performance.
  • the root portion of the first sealing portion 110 is on the side 135 of the exterior body 100 . Therefore, according to power storage device 10, compared to when the base portion of first sealing portion 110 is on second surface 140 (for example, the central portion of second surface 140 in the direction of arrow UD), A wide bonding area can be secured in the sealing portion 110 . It should be noted that the bonding region of the first sealing portion 110 does not necessarily have to be the entire region of the first sealing portion 110. may be part of
  • substantially the entire second surface 140 is covered with the first sealing portion 110 . That is, in power storage device 10, the length of first sealing portion 110 in the direction of arrow UD is longer than, for example, when first sealing portion 110 covers only half or less of second surface 140. (See Figure 3). Therefore, according to the power storage device 10 , a wide bonding area can be secured in the first sealing portion 110 .
  • substantially the entire second surface 140 is covered with the first sealing portion 110, even if the electricity storage device 10 is placed upright so that the second surface 140 is in contact with the mounting surface, the electricity storage device 10 does not stabilizes. That is, the power storage device 10 is less likely to tilt with respect to the mounting surface. Therefore, such a configuration is effective, for example, when a plurality of power storage devices 10 are arranged side by side to form a module.
  • FIG. 5 is a view from below showing a state in which the exterior member 101 is wound around the electrode body 200 during the manufacture of the electricity storage device 10 .
  • the direction along the side 135 is the TD (Transverse Direction) of the exterior member 101
  • the direction orthogonal to the side 135 is the MD (Machine Direction) of the exterior member 101.
  • the direction along the side 135 is the direction (TD) orthogonal to the flow direction (MD) of the exterior member 101 .
  • the first sealing portion 110 is bent along the side 135 , and the direction along the side 135 is perpendicular to the flow direction of the exterior member 101 . Therefore, according to the electric storage device 10, the exterior member 101 is less likely to break even if a fold is formed in the direction orthogonal to the flow direction of the exterior member 101. It is possible to reduce the possibility that the portion 110 will break.
  • the flow direction (MD) of the exterior member 101 corresponds to the rolling direction (RD) of the metal foil (aluminum alloy foil, etc.) of the barrier layer included in the exterior member 101 .
  • the TD of the exterior member 101 corresponds to the TD of the metal foil.
  • the rolling direction (RD) of the metal foil can be determined by the rolling pattern.
  • heat-fusible resin layer of the exterior member 101 were observed with an electron microscope to confirm a sea-island structure, and a direction perpendicular to the thickness direction of the heat-fusible resin layer (hereinafter referred to as "heat-fusible The direction parallel to the cross section in which the average diameter of the islands was maximum can be determined as the MD.
  • the MD of the exterior member 101 cannot be specified by the rolling grain of the metal foil, the MD can be specified by this method.
  • the angle is changed by 10 degrees from the cross section in the length direction of the heat-fusible resin layer and the direction parallel to the cross section in the length direction, and each direction up to the direction perpendicular to the cross section in the length direction
  • the sea-island structure is confirmed by observing each cross section (10 cross sections in total) with electron micrographs.
  • the diameter d of the island is measured by the linear distance connecting both ends in the direction perpendicular to the thickness direction of the heat-fusible resin layer.
  • the average diameter d of the 20 largest islands is calculated.
  • the MD is determined as the direction parallel to the cross section where the average diameter d of the islands is the largest.
  • FIG. 6 is a diagram schematically showing part of the VI-VI cross section of FIG. As shown in FIG. 6 , the second sealing portion 120 is sealed with the electrode terminal 300 sandwiched between the exterior body 100 and the electrode terminal 300 .
  • FIG. 7A and 7B are diagrams for explaining a method of forming the second sealing portion 120.
  • FIG. 7 As shown in FIG. 7, the exterior member 101 is folded, and the facing surfaces (heat-fusible resin layers) of the exterior member 101 are heat-sealed to form the second sealing portion 120 .
  • the electrode terminals 300 are positioned between the facing surfaces of the exterior member 101 .
  • An adhesive film that adheres to both metal and resin may be arranged between the electrode terminal 300 and the exterior member 101 .
  • the electrode body 200 includes a plurality of electrodes 210 (positive and negative electrodes).
  • a current collector 215 extending from each electrode 210 is connected to an electrode terminal 300 .
  • a portion of the electrode terminal 300 outside the exterior body 100 is located at approximately half the thickness of the electricity storage device 10 in the thickness direction of the electricity storage device 10 . That is, the length L2 is approximately half the length L1. Note that “substantially half the thickness of the electricity storage device 10 ” means 35% to 65% of the thickness of the electricity storage device 10 .
  • each of the plurality of electrodes 210 and the electrode terminal 300 It is possible to reduce the difference between the longest distance and the shortest distance among the distances between the two.
  • FIG. 8 is a flowchart showing the procedure for manufacturing the electricity storage device 10. As shown in FIG. The process shown in FIG. 8 is performed, for example, by a manufacturing apparatus for power storage device 10 .
  • the manufacturing apparatus winds the exterior member 101 around the electrode body 200 (step S100).
  • the manufacturing apparatus forms the first sealing portion 110 by heat-sealing the mutually facing surfaces (heat-fusible resin layers) of the exterior member 101 (step S110).
  • the unfinished product shown in FIGS. 4 and 5 is completed.
  • the manufacturing apparatus bends the first sealing portion 110 so that the first sealing portion 110 is in contact with the second surface 140 (step S120).
  • the manufacturing apparatus forms the second sealing portion 120 by folding the exterior member 101 with the electrode body 200 stored therein and heat-sealing the facing surfaces (heat-fusible resin layers) of the exterior member 101 (step S130). Thereby, the electric storage device 10 is completed.
  • first sealing portion 110 is bent toward second surface 140 having a smaller area. That is, the first sealing portion 110 does not exist on the first surface 130 having a large area. Therefore, even if another power storage device 10 is placed on the first surface 130, the other power storage device 10 does not tilt. As a result, according to the power storage device 10, when a plurality of power storage devices 10 are stacked, uneven distribution of pressure applied to the power storage device 10 below can be suppressed. Moreover, when used in an all-solid-state battery, it is necessary to uniformly apply a high pressure from the outer surface of the battery in order to exhibit the battery performance, so the packaging form of the present invention is preferable.
  • the root portion of the first sealing portion 110 is on the side 135 of the exterior body 100 . Therefore, according to the power storage device 10, when the first sealing portion 110 is accommodated on the second surface 140, compared to when the root portion of the first sealing portion 110 is on the second surface 140, A wide bonding width can be ensured in the first sealing portion 110 .
  • second sealing portion 120 is formed by folding exterior member 101 and heat-sealing the facing surfaces of exterior member 101 .
  • shape and formation method of the second sealing part 120 are not limited to this. Note that the following description will focus on the parts that are different from the first embodiment, and will omit the description of the parts that are common to the first embodiment.
  • FIG. 9 is a plan view schematically showing power storage device 10X according to the second embodiment.
  • FIG. 10 is a side view schematically showing the power storage device 10X.
  • FIG. 11 is a perspective view schematically showing the lid body 400.
  • the exterior member 100X is configured by fitting lids 400 into openings at both ends of the exterior member 101 wound around the electrode body 200. As shown in FIG.
  • the second sealing portion 120X is formed by heat-sealing the exterior member 101 and the lid 400 with the lid 400 fitted therein.
  • the lid 400 is a bottomed tray-shaped member that is rectangular in plan view, and is formed by, for example, cold forming the exterior member 101 .
  • the lid 400 does not necessarily have to be composed of the exterior member 101, and may be a metal molded product or a resin molded product.
  • lid body 400 is arranged such that the bottom side of lid body 400 is located inside exterior body 100X.
  • the bottom surface side of the lid 400 does not necessarily have to be positioned inside the exterior body 100X.
  • the bottom side of lid 400 may be located outside exterior body 100X.
  • the electrode terminal 300 protrudes outside the exterior body 100X through the space between the lid body 400 and the exterior member 101 when the electrode body 200 is housed. That is, the lid 400 and the exterior member 101 are heat-sealed with the electrode terminals 300 sandwiched therebetween.
  • the position where the electrode terminal 300 protrudes to the outside does not necessarily have to be between the lid 400 and the exterior member 101 .
  • the electrode terminal 300 may protrude from a hole formed in one of the six surfaces of the exterior body 100X. In this case, a slight gap between the exterior body 100X and the electrode terminal 300 is filled with resin, for example.
  • the lid 400 and the electrode terminal 300 are provided separately.
  • the lid 400 and the electrode terminals 300 do not necessarily have to be provided separately.
  • the lid 400 and the electrode terminal 300 may be integrally formed.
  • FIG. 12 is a diagram showing a first example in which the lid body 400 and the electrode terminal 300 are integrally formed. As shown in FIG. 12, in the first example, the electrode terminal 300 is heat-sealed in advance to the side surface of the lid 400 .
  • an adhesive film that adheres to both metal and resin may be arranged between the cover 400 and the electrode terminals 300 .
  • FIG. 13 is a diagram showing a second example in which the lid body 400 and the electrode terminal 300 are integrally formed. As shown in FIG. 13, in the second example, electrode terminals 300 pass through holes formed in the bottom surface of lid 400 . A slight gap in the hole in the bottom surface of lid 400 is filled with resin, for example.
  • a gas valve may be attached to a hole formed in one of the second sealing portion 120X or the six surfaces of the exterior body 100X.
  • the gas valve is configured by, for example, a check valve or a break valve, and is configured to reduce the pressure when the pressure inside the exterior body 100X rises due to the gas generated inside the power storage device 10X. ing.
  • FIG. 14 is a flow chart showing the manufacturing procedure of the power storage device 10X. The process shown in FIG. 14 is performed, for example, by a manufacturing apparatus for power storage device 10X.
  • the manufacturing apparatus winds the exterior member 101 around the electrode body 200 (step S200).
  • the manufacturing apparatus forms the first sealing portion 110 by heat-sealing the mutually facing surfaces (heat-fusible resin layers) of the exterior member 101 (step S210).
  • the unfinished product shown in FIGS. 4 and 5 is completed.
  • the manufacturing apparatus bends the first sealing portion 110 so that the first sealing portion 110 is in contact with the second surface 140 (step S220).
  • the manufacturing apparatus accommodates the electrode body 200 in the unfinished product produced in step S220, and attaches the lid body 400 to each of the openings at both ends (step S230).
  • the manufacturing apparatus forms the second sealing portion 120X by heat-sealing the exterior member 101 and the lid 400 (step S240). This completes the power storage device 10X.
  • first sealing portion 110 is bent toward second surface 140 having a smaller area. Therefore, according to the power storage device 10X, when a plurality of power storage devices 10X are stacked, uneven distribution of pressure applied to the lower power storage devices 10X can be suppressed.
  • first sealing portion 110 does not necessarily have to be bent toward second surface 140 having a smaller area.
  • first sealing portion 110 may be bent toward the first surface 130 having a large area.
  • the root portion of the first sealing portion 110 does not necessarily have to be on the side 135 of the exterior body 100X.
  • the root portion of first sealing portion 110 may be positioned, for example, on a surface of exterior body 100X other than lid body 400 .
  • power storage device 10X according to the second embodiment includes, for example, the following features.
  • the power storage device 10X includes an electrode body (electrode body 200) and an exterior body ( exterior body 100X) that seals the electrode body (electrode body 200). 200), and includes an exterior member (exterior member 101) having openings at both ends thereof, and a lid body (lid body 400) that seals the opening.
  • the second sealing portion 120X is not formed by heat-sealing the facing surfaces of the exterior member 101 as in the first embodiment (see FIG. 7).
  • the opening of the exterior member 101 wound around the electrode body 200 is sealed by the lid body 400.
  • a second sealing portion 120X is formed in a portion where the lid body 400 and the exterior member 101 overlap (see FIGS. 9 and 10). According to such a configuration, by adjusting the depth L3 (FIG. 11) of the lid 400, the region of the second sealing portion 120X can be easily narrowed.
  • the corner C1 (FIGS. 9 and 10) of the exterior member 101 that covers the corner C1 of the electrode body 200 does not impinge on the exterior member 101, causing an excessive load.
  • the second sealing portion 120X is not formed by heat-sealing the mutually facing surfaces of the exterior member 101 as in the first embodiment. .
  • the procedure for manufacturing the power storage device 10X is not limited to the procedure shown in the flowchart of FIG.
  • the power storage device 10X may be manufactured according to the procedure shown in the flowchart of FIG.
  • FIG. 15 is a flowchart showing another manufacturing procedure for power storage device 10X according to the second embodiment.
  • the process shown in FIG. 15 is performed, for example, by a manufacturing apparatus for power storage device 10X.
  • the manufacturing apparatus attaches a member (for example, the member shown in FIGS. 12 and 13) in which the electrode terminal 300 and the lid body 400 are integrated to the electrode body 200 (step S250).
  • electrode terminal 300 is welded to electrode body 200 .
  • the manufacturing apparatus winds the exterior member 101 around the electrode body 200 (step S260).
  • the manufacturing apparatus forms the first sealing portion 110 by heat-sealing the mutually facing surfaces (heat-fusible resin layers) of the exterior member 101 and heat-sealing the exterior member 101 and the lid 400 . to form the second sealing portion 120X (step S270).
  • the power storage device 10X may be manufactured by such procedures.
  • Embodiment 3 It is common to undergo a process (hereinafter referred to as an aging process) of aging the temporarily sealed power storage device in a predetermined temperature environment for a predetermined time for the purpose of permeating the electrolyte into the electrode assembly in the battery manufacturing process. Gas is generated from the electrode body 200 in the process, and it is necessary to discharge the gas to the outside of the battery. Electricity storage device 10X according to the second embodiment is not provided with a mechanism for extracting gas generated in the aging process at the final stage of manufacturing electricity storage device 10X. Electricity storage device 10Y according to the third embodiment is provided with a mechanism for extracting gas generated from electrode body 200 at the final stage of manufacturing electricity storage device 10Y. In addition, below, it demonstrates centering on a different part from Embodiment 2, and abbreviate
  • FIG. 16 is a side view showing a state in which the exterior member 101Y is wound around the electrode body 200 during the manufacture of the electricity storage device 10Y.
  • FIG. 17 is a view from below showing a state in which the electrode body 200 is wrapped with the exterior member 101Y and the lid member 400 is attached to the exterior member 101Y during the manufacturing of the electricity storage device 10Y.
  • the piece 150 is formed in a state in which the exterior member 101Y is wound around the electrode body 200.
  • the piece 150 is formed by joining the facing surfaces of the exterior member 101Y in a state in which the exterior member 101Y is wound around the electrode body 200 . More specifically, the piece 150 is formed by joining (heat-sealing) the peripheral edges of the surfaces facing each other in a state where the exterior member 101Y is wound around the electrode body 200 . That is, a first sealing portion 154 is formed on the peripheral edge of the piece portion 150 .
  • a space 152 is formed in which the facing surfaces of the exterior member 101Y are not joined.
  • joined regions 151 where the facing surfaces of the exterior member 101Y are joined and unjoined regions 153 where the facing surfaces of the exterior member 101Y are not joined are arranged alternately. That is, a pattern of bonding regions 151 is formed along the sides 135 of the piece 150 .
  • the gas generated from the electrode body 200 is discharged to the outside of the exterior body 100Y by cutting off a portion of the piece 150 or otherwise releasing the sealed state of the exterior body 100Y.
  • the gas discharged to the outside of the exterior body 100Y is not necessarily limited to the gas generated from the electrode body 200, and may be any gas other than the gas generated from the electrode body 200, such as air, water vapor, or hydrogen sulfide. good too.
  • the portion including the vicinity of the side 135 is heat-sealed in a belt shape, so that the exterior body 100Y is sealed again.
  • regions with strong bonding strength between the facing surfaces of the exterior member 101Y and regions with weak bonding strength between the surfaces are alternately arranged along the side 135. .
  • thin portions and thick portions alternate along side 135 . This is because the non-bonded area 153 is single-sealed by heat-sealing the vicinity of the side 135 again, but the bonded area 151 is double-sealed.
  • FIG. 18 is a flow chart showing the manufacturing procedure of the electricity storage device 10Y. The process shown in FIG. 18 is performed, for example, by a manufacturing apparatus for power storage device 10Y.
  • the manufacturing apparatus winds the exterior member 101Y around the electrode body 200 (step S300).
  • the manufacturing apparatus forms the first sealing portion 154 by heat-sealing the peripheral edges of the mutually facing surfaces (heat-fusible resin layers) of the exterior member 101Y (step S310).
  • the manufacturing apparatus forms a pattern of the joint region 151 by heat-sealing the facing surfaces of the exterior member 101Y in the vicinity of the side 135 (step S320).
  • the manufacturing apparatus attaches the lids 400 to the openings at both ends with the electrode bodies 200 housed in the unfinished product produced in step S320 (step S330).
  • the manufacturing apparatus forms the second sealing portion 120X by heat-sealing the exterior member 101Y and the lid 400 (step S340). After that, it undergoes an aging process.
  • the manufacturing apparatus removes the gas generated in the aging process by, for example, cutting off the piece 150 (step S350).
  • the manufacturing apparatus heat seals the portion including the joint region 151 of the piece 150 in a band shape and removes the edge portion to reseal the exterior body 100Y (step S360). After that, the electrical storage device 10Y is completed by bending the piece portion 150 toward the second surface 140 side.
  • piece portion 150 including first sealing portion 154 is bent toward second surface 140 having a smaller area. Therefore, according to the power storage device 10Y, when a plurality of power storage devices 10Y are stacked, uneven distribution of pressure applied to the power storage device 10Y below can be suppressed. When used in an all-solid-state battery, it is necessary to uniformly apply a high pressure from the outer surface of the battery in order to exhibit battery performance, so the packaging form of the present invention is preferred.
  • Embodiment 4 In power storage device 10X according to the second embodiment, the position at which electrode terminal 300 protrudes to the outside is between lid 400 and exterior member 101 . However, the position where the electrode terminal 300 protrudes to the outside is not limited to this. In addition, below, it demonstrates centering on a different part from Embodiment 2, and abbreviate
  • FIG. 19 is a plan view schematically showing power storage device 10XA according to the fourth embodiment.
  • FIG. 20 is a side view schematically showing the power storage device 10XA.
  • the exterior body 100X of the power storage device 10XA includes a pair of long sides 100XA and a pair of short sides 100XB in plan view.
  • the exterior body 100X is configured by fitting the lid body 400 into each opening along the long side 100XA of the exterior member 101 wound around the electrode body 200 .
  • the second sealing portion 120X is formed by heat-sealing the exterior member 101 and the lid 400 with the lid 400 fitted therein.
  • a through hole (not shown) is formed in the lid 400 .
  • the two electrode terminals 300 protrude from the through holes of the lid 400 to the outside of the exterior body 100X.
  • the two electrode terminals 300 are shaped along the long side 100XA of the exterior body 100X.
  • a slight gap between the through hole and the electrode terminal 300 is filled with resin, for example.
  • the first sealing portion 110 is formed on one side of the pair of short sides 100XB.
  • the position in the lid 400 where the electrode terminals 300 protrude in the thickness direction (arrow UD direction) of the power storage device 10XA can be arbitrarily selected.
  • electrode terminal 300 protrudes from approximately the center of lid body 400 to the outside of exterior body 100X in the thickness direction of power storage device 10XA.
  • the length of electrode terminal 300 in the depth direction (direction of arrow FB) of power storage device 10XA can be arbitrarily selected.
  • the length of electrode terminal 300 in the depth direction (direction of arrow FB) of power storage device 10XA is substantially the same as the length of electrode body 200 .
  • power storage device 10XA since electrode terminals 300 are arranged along long side 100XA having a long length in the depth direction, larger electrode terminals 300 can be used. Therefore, the high-output power storage device 10XA can be provided.
  • An aluminum alloy ingot having each composition shown in Tables 1 and 2 (the balance being Al and other unavoidable impurities) was prepared.
  • a homogenization treatment was performed under the conditions shown in Tables 1 and 2, and then hot rolling was performed at a finish temperature of 330°C to obtain a plate material having a thickness of 3 mm.
  • hot rolling was performed at a finish temperature of 330°C to obtain a plate material having a thickness of 3 mm.
  • an aluminum alloy foil sample having a thickness of 40 ⁇ m and a width of 1200 mm was produced.
  • the conditions for intermediate annealing and final annealing are shown in Tables 1 and 2.
  • CAL annealing was performed as intermediate annealing.
  • CAL was performed under the following conditions: heating rate: 70°C/sec, heating temperature: 420°C, holding time: 0 sec, cooling rate: 50°C/sec.
  • the item of cold rolling in Tables 1 and 2 shows the plate thickness immediately before intermediate annealing and the cold rolling reduction up to the plate thickness. The following tests or measurements were performed on the prepared exterior member containing the aluminum alloy foil, and the results are shown in Tables 1 to 4.
  • the elongation is the elongation at break and was calculated by the following method. First, two lines were marked in the vertical direction of the test piece at intervals of 50 mm, which is the gauge length, in the longitudinal center of the test piece before the test. After the test, the fracture surfaces of the aluminum alloy foil were brought together to measure the distance between the marks. The gauge length (50 mm) was subtracted from the distance between the marks to calculate the elongation (mm), and the elongation (%) was obtained by dividing the elongation by the gauge length (50 mm).
  • the surface of the aluminum alloy foil was electropolished at a voltage of 20 V using a mixed solution of 20% by volume perchloric acid and 80% by volume ethanol. Then, it was anodized in Barker's solution at a voltage of 30V. Crystal grains of the treated specimens were observed with an optical microscope. The average crystal grain size was calculated from the photographs taken by the cutting method specified in JIS G0551.
  • the Mg concentration on the foil surface was estimated by XPS (X-ray Photoelectron Spectroscopy). Waveform separation was performed on the narrow spectrum obtained by narrow scan measurement in the surface portion from the outermost surface to a depth of 8 nm, and the atomic concentration of each element was quantified. Incidentally, the Mg2p spectrum was used for quantifying the Mg amount. The details of the analysis conditions are as follows.
  • the oxide film thickness was measured with an FE-EPMA (Electron Probe Micro Analyzer) device.
  • the oxide film thickness of the sample was calculated using the calibration curve of the X-ray intensity obtained from the oxide film sample whose thickness was known from the beginning.
  • the FE-EPMA apparatus used was JXA-8530F manufactured by JEOL. Analysis conditions were an acceleration voltage of 10 kV, an irradiation current of 100 nA, and a beam diameter of 50 ⁇ m.
  • ⁇ Penetration strength of aluminum alloy foil A needle with a diameter of 1.0 mm and a tip shape radius of 0.5 mm is pierced at a speed of 50 mm / min into an exterior member containing an aluminum alloy foil with a thickness of 40 ⁇ m, and the needle penetrates the foil.
  • the maximum load (N) up to was measured as the puncture strength.
  • the puncture strength was 9.0 N or more, the puncture resistance was judged to be good, and indicated as "A” in Tables 3 and 4.
  • the puncture strength was less than 9.0 N, it was determined to be poor in puncture resistance, and indicated as "C” in Tables 3 and 4.
  • the test sample AL was set as the working electrode, metallic lithium Li (disk-shaped with a diameter of 15 mm and a thickness of 0.35 mm) was set as the counter electrode, and an electrolytic solution (1 mol/l LiPF6 , ethylene carbonate, diethyl carbonate and dimethyl carbonate (consisting of a mixed solution with a volume ratio of 1:1:1).
  • an electrolytic solution (1 mol/l LiPF6 , ethylene carbonate, diethyl carbonate and dimethyl carbonate (consisting of a mixed solution with a volume ratio of 1:1:1).
  • a voltage of 0.1 V was applied in an environment of 20° C. for 1 hour, and then the surface of the aluminum alloy foil was observed.
  • FIG. 3F(B) the surface corroded was evaluated as C, and as shown in FIG. A compound with lithium is formed on the corroded aluminum alloy foil surface, and the surface is observed to swell due to volume expansion.
  • the pierce strength was measured from the substrate layer side by a method conforming to JIS Z1707:1997. Specifically, in a measurement environment of 23 ⁇ 2 ° C. and relative humidity (50 ⁇ 5)%, the test piece is fixed with a table with a diameter of 115 mm having an opening of 15 mm in the center and a pressing plate. A semicircular needle with a tip shape radius of 0.5 mm was pierced at a speed of 50 ⁇ 5 mm per minute, and the maximum stress until the needle penetrated was measured. The number of test pieces was 5, and the average value was obtained.
  • an acid-resistant film a film formed by chromate treatment and having a chromium content of 30 mg/m 2
  • a two-component curable urethane adhesive polyol compound and an aromatic isocyanate compound
  • aging treatment was performed to prepare a laminate of base layer/adhesive layer/barrier layer.
  • a maleic anhydride-modified polypropylene (40 ⁇ m thick) as an adhesive layer and a polypropylene (40 ⁇ m thick) as a heat-fusible resin layer are co-extruded on the barrier layer of the resulting laminate.
  • the adhesive layer/heat-fusible resin layer was laminated on the barrier layer.
  • polyethylene terephthalate film (12 ⁇ m)/adhesive layer (3 ⁇ m)/biaxially oriented nylon film (15 ⁇ m)/adhesive layer (3 ⁇ m)/barrier layer ( 40 ⁇ m)/adhesive layer (40 ⁇ m)/heat-fusible resin layer (40 ⁇ m) were laminated in this order to obtain an exterior member.
  • a lubricant layer was formed on each of both surfaces of the exterior member by allowing erucamide to exist as a lubricant.
  • Each of the exterior members of the electricity storage devices of Examples 1 to 15 and 22 to 40 is composed of a laminate comprising at least a substrate layer, a barrier layer, and a heat-fusible resin layer in this order. includes an aluminum alloy foil that satisfies the composition of Fe: 0.2% by mass or more and 2.0% by mass or less and Mg: 0.1% by mass or more and 5.0% by mass or less.
  • 40 are excellent in followability of the exterior members at corners and the like, and corrosion of the aluminum alloy foil when electricity is generated in a state where the electrolytic solution is adhered is effectively prevented. inhibited and have higher mechanical strength.
  • Embodiments 1 to 4 have been described above, the present invention is not limited to the above Embodiments 1 to 4, and various modifications are possible without departing from the gist thereof. Modifications will be described below.
  • the electrode assembly 200 is wound with one sheet of exterior member.
  • the number of exterior members wound around the electrode body 200 does not necessarily have to be one.
  • electrode assembly 200 may be wound with two or more exterior members.
  • FIG. 21 is a side view showing a state in which exterior members 101Z1 and 101Z2 are wound around the electrode assembly 200 during manufacture of the electricity storage device in the modification.
  • the electrode body 200 is surrounded by exterior members 101Z1 and 101Z2.
  • a first sealing portion 110Z is formed by joining the facing surfaces of the exterior members 101Z1 and 101Z2.
  • each first sealing portion 110Z is bent toward the second surface 140Z, not toward the first surface 130Z. Even with such a configuration, when a plurality of power storage devices are stacked, uneven distribution of pressure applied to the lower power storage devices can be suppressed.
  • each first sealing portion 110Z does not necessarily have to be bent. Further, in this modification, each sealing portion 110Z may be sealed with a part of the electrode terminal 300 sandwiched therebetween. Furthermore, in this modification, each first sealing portion 110Z does not need to be formed on the side 135Z, and may protrude outward from approximately the center of the second surface 140Z in the thickness direction of the power storage device.
  • the electrode body 200 is a so-called stack type configured by stacking a plurality of electrodes 210, but the form of the electrode body 200 is not limited to this.
  • the electrode body 200 may be, for example, a so-called wound type configured by winding a positive electrode and a negative electrode with a separator interposed therebetween.
  • the electrode body 200 may be configured by stacking a plurality of so-called wound electrode bodies.
  • the second surface 140 is a flat surface extending downward from the first surface 130 at a substantially right angle.
  • the form of the second surface 140 is not limited to this.
  • the electrode body 200 is a wound electrode body and has a flat surface and a curved surface on its outer circumference.
  • the planar area is larger than the curved surface area
  • the first surface 130 covers the planar surface of the electrode body
  • the second surface 140 covers the curved surface of the electrode body.
  • the second surface 140 may be curved.
  • the boundary portion where the second surface 140 extends downward from the first surface 130 is the side 135 .
  • the bonding regions 151 are formed at four locations.
  • the number of locations where the bonding regions 151 are formed is not limited to this.
  • the joint regions 151 may be formed only at two locations near both ends along the side 135, only at one location near the center of the side 135, or may be formed at five or more locations.
  • the electrode terminal 300 is arranged in the second sealing portion 120 , but the position where the electrode terminal 300 is arranged in the exterior body 100 is not limited to this.
  • the electrode terminal 300 can also be arranged on the first sealing portion 110.
  • the first sealing portion 110 is sealed with the electrode terminal 300 sandwiched therebetween.
  • at least one of the two electrode terminals 300 may be bent toward the second surface 140 , bent toward the side opposite to the second surface 140 , or projected outward from the side 135 .
  • the electrode terminal 300 and the first sealing portion 110 can be easily sealed, so the sealing performance of the exterior body 100 is enhanced. Moreover, the electrode body 200 can be easily accommodated in the exterior body 100 .
  • lids 400 are fitted into the respective openings at both ends of exterior member 101 as in the second embodiment.
  • the second sealing portion 120 is formed by heat-sealing the exterior member 101 and the lid 400 with the lid 400 fitted therein.
  • FIG. 23 is a perspective view showing a lid body 500 that is a modification of the lid body 400.
  • FIG. Lid 500 is plate-shaped, for example, and includes a first surface 500A facing electrode body 200 (see FIG. 9) and a surface 500B opposite to first surface 500A.
  • a hole 500C passing through the first surface 500A and the second surface 500B is formed in the center of the lid 500.
  • the material forming the lid 500 is, for example, resin.
  • an adhesive film 530 that adheres to both the electrode terminal 300 and the lid 500 is attached to a predetermined range including a portion of the electrode terminal 300 that is bonded to the lid 500 .
  • the lid body 500 is composed of a member divided into a first portion 510 and a second portion 520. The first portion 510 and the second portion 520 are joined so as to sandwich the electrode terminal 300 and the adhesive film 530. may be manufactured. Alternatively, the lid 500 may be manufactured by insert-molding the lid 500 onto the electrode terminal 300 to which the adhesive film 530 is attached. Moreover, in this modified example, a barrier layer is preferably laminated on at least part of the surface of the lid 500 .
  • the barrier layer may be formed on any layer.
  • a material forming the barrier layer is, for example, aluminum.
  • the gap is preferably filled with, for example, a resin material such as hot melt.
  • the exterior member 100X is the second surface by joining the exterior member 101 and the second surface 500B of the lid member 500 with the lid member 500 fitted therein.
  • a sealing portion 120X is formed.
  • a means for joining exterior member 101 and second surface 500B of lid 500 is, for example, heat sealing.
  • the exterior member 101 is joined to a wider area of the lid 500, so that the sealing performance of the exterior 100X is enhanced.
  • FIG. 25 is a front view of a lid body 600 that is another modification of the lid body 400 in the second embodiment.
  • Lid body 600 includes metal part 610, which is a part where metal is exposed on the surface, and metal part 610 and electrode 210 of electrode body 200 are welded.
  • the lid body 600 may be entirely composed of the metal portion 610 only, or the metal portion 610 may be partially formed.
  • the lid body 600 is made of a multi-layered material including a metal layer.
  • the metal part 610 is a part where the layers other than the metal layer are partially removed so that the metal layer is exposed.
  • the power storage device 10X see FIG. 9) can be made small.
  • FIG. 26 is a front view of a lid body 700 that is another modification of the lid body 400 in the second embodiment.
  • the lid 700 includes a metal portion 710 made of a metal material, and a non-metal portion 720 connected to the metal portion 710 and made of a resin material.
  • Metal portion 710 is welded to electrode 210 of electrode assembly 200 .
  • the power storage device 10X see FIG. 9) can be made small.
  • the second sealing portion 120 is formed by folding the exterior member 101 and heat-sealing the heat-fusible resin layers of the exterior member 101 to each other.
  • the method for forming the second sealing portion 120 is not limited to this.
  • FIG. 27 is a plan view schematically showing an electricity storage device 10 having a second sealing portion 120Y of a modification.
  • the exterior member 101 has an overhanging portion 101X extending outward from the exterior body 100, and the heat-sealing resin layers of the overhanging portion 101X are heat-sealed to form a second sealing portion 120Y. It is formed.
  • the heat-sealable resin layer of the projecting portion 101X and the electrode terminal 300 are heat-sealed at the portion of the projecting portion 101X where the electrode terminal 300 is arranged.
  • the second sealing portion 120Y can be heat-sealed more firmly, so that the sealing performance of the exterior body 100 is improved. Note that, in this modification, portions of the overhanging portion 101X other than the portion heat-sealed with the electrode terminal 300 may be cut off as necessary. This modification can also be applied to the modification shown in FIG.
  • 10, 10X, 10XA, 10Y, 10Z power storage device 100, 100X, 100Y exterior body, 101, 101Y, 101Z1, 101Z2 exterior member, 101A base layer, 101C barrier layer, 101D heat-fusible resin layer, 101X extension Part, 110, 110Z, 154 First sealing part, 120, 120X, 120Y Second sealing part, 130, 130Z First surface, 135, 135Z Side, 140, 140Z Second surface, 150 Piece, 151 Joining area , 152 space, 153 unbonded region, 200 electrode body, 210 electrode, 215 current collector, 300 electrode terminal, 500A first surface, 500B second surface, 400,500,700 lid, 610,710 metal part, C1 corner.

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PCT/JP2022/026084 2021-06-29 2022-06-29 蓄電デバイス、及び、蓄電デバイスの製造方法 Ceased WO2023277100A1 (ja)

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US18/572,896 US20240304904A1 (en) 2021-06-29 2022-06-29 Power storage device and method for manufacturing power storage device
EP22833246.6A EP4366045A4 (en) 2021-06-29 2022-06-29 ENERGY STORAGE DEVICE AND METHOD FOR MANUFACTURING ENERGY STORAGE DEVICE
KR1020247001370A KR20240026486A (ko) 2021-06-29 2022-06-29 축전 디바이스, 및 축전 디바이스의 제조 방법
JP2023501913A JP7279872B1 (ja) 2021-06-29 2022-06-29 蓄電デバイス、及び、蓄電デバイスの製造方法
CN202280045802.7A CN117616621A (zh) 2021-06-29 2022-06-29 蓄电器件和蓄电器件的制造方法
JP2023076690A JP7444315B2 (ja) 2021-06-29 2023-05-08 蓄電デバイス、及び、蓄電デバイスの製造方法
JP2024023944A JP2024052801A (ja) 2021-06-29 2024-02-20 蓄電デバイス、及び、蓄電デバイスの製造方法

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