WO2011070918A1 - Electrical storage device and method for manufacturing same - Google Patents

Electrical storage device and method for manufacturing same Download PDF

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Publication number
WO2011070918A1
WO2011070918A1 PCT/JP2010/071074 JP2010071074W WO2011070918A1 WO 2011070918 A1 WO2011070918 A1 WO 2011070918A1 JP 2010071074 W JP2010071074 W JP 2010071074W WO 2011070918 A1 WO2011070918 A1 WO 2011070918A1
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Prior art keywords
negative electrode
positive electrode
current collector
storage device
overlapping region
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PCT/JP2010/071074
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French (fr)
Japanese (ja)
Inventor
真治 山本
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株式会社 村田製作所
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Publication of WO2011070918A1 publication Critical patent/WO2011070918A1/en

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    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10Primary casings; Jackets or wrappings
    • H01M50/116Primary casings; Jackets or wrappings characterised by the material
    • H01M50/124Primary casings; Jackets or wrappings characterised by the material having a layered structure
    • H01M50/1243Primary casings; Jackets or wrappings characterised by the material having a layered structure characterised by the internal coating on the casing
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50Current conducting connections for cells or batteries
    • H01M50/572Means for preventing undesired use or discharge
    • H01M50/584Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries
    • H01M50/586Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries inside the batteries, e.g. incorrect connections of electrodes
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10Primary casings; Jackets or wrappings
    • H01M50/116Primary casings; Jackets or wrappings characterised by the material
    • H01M50/117Inorganic material
    • H01M50/119Metals
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10Primary casings; Jackets or wrappings
    • H01M50/116Primary casings; Jackets or wrappings characterised by the material
    • H01M50/121Organic material
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10Primary casings; Jackets or wrappings
    • H01M50/116Primary casings; Jackets or wrappings characterised by the material
    • H01M50/124Primary casings; Jackets or wrappings characterised by the material having a layered structure
    • H01M50/126Primary casings; Jackets or wrappings characterised by the material having a layered structure comprising three or more layers
    • H01M50/129Primary 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
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10Primary casings; Jackets or wrappings
    • H01M50/131Primary casings; Jackets or wrappings characterised by physical properties, e.g. gas permeability, size or heat resistance
    • H01M50/133Thickness
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10Primary casings; Jackets or wrappings
    • H01M50/131Primary casings; Jackets or wrappings characterised by physical properties, e.g. gas permeability, size or heat resistance
    • H01M50/136Flexibility or foldability
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10Primary casings; Jackets or wrappings
    • H01M50/172Arrangements of electric connectors penetrating the casing
    • H01M50/174Arrangements of electric connectors penetrating the casing adapted for the shape of the cells
    • H01M50/178Arrangements of electric connectors penetrating the casing adapted for the shape of the cells for pouch or flexible bag cells
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50Current conducting connections for cells or batteries
    • H01M50/531Electrode connections inside a battery casing
    • H01M50/536Electrode connections inside a battery casing characterised by the method of fixing the leads to the electrodes, e.g. by welding
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50Current conducting connections for cells or batteries
    • H01M50/531Electrode connections inside a battery casing
    • H01M50/54Connection of several leads or tabs of plate-like electrode stacks, e.g. electrode pole straps or bridges
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50Current conducting connections for cells or batteries
    • H01M50/543Terminals
    • H01M50/547Terminals characterised by the disposition of the terminals on the cells
    • H01M50/548Terminals characterised by the disposition of the terminals on the cells on opposite sides of the cell
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50Current conducting connections for cells or batteries
    • H01M50/543Terminals
    • H01M50/552Terminals characterised by their shape
    • H01M50/553Terminals adapted for prismatic, pouch or rectangular cells
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50Current conducting connections for cells or batteries
    • H01M50/543Terminals
    • H01M50/564Terminals characterised by their manufacturing process
    • H01M50/566Terminals characterised by their manufacturing process by welding, soldering or brazing
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50Current conducting connections for cells or batteries
    • H01M50/572Means for preventing undesired use or discharge
    • H01M50/574Devices or arrangements for the interruption of current
    • H01M50/578Devices or arrangements for the interruption of current in response to pressure
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50Current conducting connections for cells or batteries
    • H01M50/572Means for preventing undesired use or discharge
    • H01M50/584Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries
    • H01M50/59Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries characterised by the protection means
    • H01M50/593Spacers; Insulating plates
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00Secondary cells; Manufacture thereof
    • H01M10/05Accumulators with non-aqueous electrolyte
    • H01M10/058Construction or manufacture
    • H01M10/0585Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10Energy storage using batteries

Definitions

  • the present invention generally relates to an electricity storage device and a method for manufacturing the same, and specifically, a lithium ion secondary battery, a lithium secondary battery, a polymer secondary battery, an organic radical battery, an all-solid battery, an electric double layer capacitor, and the like.
  • the electrical storage element which accommodates this electrical storage element using the outer packaging member which has flexibility, and its manufacturing method are related.
  • a lithium ion secondary battery containing a storage element using a flexible laminate film (also referred to as a laminated sheet) is used.
  • the laminate film is positioned on the inner surface side facing the power storage element, and is positioned on the outer surface of the synthetic resin, the outer surface of the lithium ion secondary battery, the outer surface layer of the synthetic resin, and the inner surface layer and the outer surface layer. It consists of an intermediate layer placed between them.
  • the inner surface layer is made of, for example, a thermoplastic resin excellent in electrolytic solution resistance and heat sealability, such as polyethylene and polypropylene.
  • middle layer consists of a metal layer excellent in flexibility and intensity
  • the outer surface layer is made of, for example, an insulating resin excellent in electrical insulation, such as nylon or polyamide.
  • the power storage element is formed by winding or alternately stacking a positive electrode plate and a negative electrode plate via a separator.
  • Patent Document 1 in Japanese Unexamined Patent Publication No. 2000-58011 (hereinafter referred to as Patent Document 1), an external terminal foil (positive electrode or negative electrode connection terminal) and a current collector It has been proposed that the terminal connection portion is covered with a thermosetting resin to suppress a short circuit between the connection portion and the outer packaging member and deterioration of the sealing reliability of the outer case (outer packaging member).
  • Patent Document 2 Japanese Patent No. 4065915 (hereinafter referred to as Patent Document 2), in a lithium secondary battery, a welded portion of a grid (electrode current collector) and a tab member (positive electrode or negative electrode connection terminal) is covered with an insulating tape. Therefore, it has been proposed to prevent a short circuit caused by damage to the packaging material (outer packaging member) due to the welded portion or the tab member.
  • Patent Document 3 Japanese Patent Application Laid-Open No. 2005-149938 (hereinafter referred to as Patent Document 3), without removing the burrs at the ends of the positive electrode tab (positive electrode connection terminal) and the negative electrode tab (negative electrode connection terminal) in the film-covered battery, In order to prevent defects due to burrs, protective tape is applied to the joints between the positive and negative current collectors and the positive and negative tabs to cover the positive and negative tabs Has been proposed.
  • Patent Document 4 in a flat battery, a current collector and positive electrode lead (positive electrode connection terminal) of a positive electrode plate, and a current collector and negative electrode lead (negative electrode connection) of a negative electrode plate. A terminal), and an electrode group in which the positive electrode plate and the negative electrode plate are insulated via a separator by covering the connection portion with an adhesive resin insoluble in the electrolyte, and an outer case (outer packaging member) It has been proposed to integrate.
  • Patent Document 4 the space surrounded by the seal part of the outer case and the end face of the electrode group facing the seal part is filled with an adhesive resin that is insoluble in the electrolytic solution, and each lead is used as an adhesive resin. It has been proposed to coat them.
  • Patent Documents 1 to 4 have the following problems. That is, since an insulating layer is formed at the ends of the positive electrode current collector and the negative electrode current collector before injecting the electrolytic solution in the manufacturing process, the electrolytic solution is used with the ends of the current collector sealed with the insulating layer. Will be injected. Then, the electrolyte solution cannot be impregnated from the end side of the current collector toward the center portion of the electrode laminate, and the impregnation time of the electrolyte solution deteriorates or the impregnation time becomes insufficient. There is a problem of becoming longer.
  • an object of the present invention is to provide a power storage device using a flexible outer packaging member, which can prevent a short circuit due to damage of the outer packaging member, and can improve productivity by improving the impregnation property of the electrolytic solution. It is to provide a device and its manufacturing method.
  • An electricity storage device includes an electrode laminate formed by alternately laminating a plurality of positive plates and a plurality of negative plates with a separator interposed therebetween, an inner surface layer made of at least a thermoplastic resin, and an outer side thereof And a flexible outer packaging member that accommodates the electrode stack, and ends of the positive electrode current collectors of the plurality of positive electrode plates and the negative electrode current collectors of the plurality of negative electrode plates, respectively. And a positive electrode connection terminal and a negative electrode connection terminal led out from the outer peripheral edge of the outer packaging member. An overlapping region where each end of the positive electrode current collector and the negative electrode current collector overlaps with each of the positive electrode connecting terminal and the negative electrode connecting terminal and a non-overlapping region where they do not overlap are formed.
  • the overlapping region includes a connection portion between each end of the positive electrode current collector and the negative electrode current collector and each of the positive electrode connection terminal and the negative electrode connection terminal.
  • a coating layer is formed on the inner surface layer of the outer packaging member so as to cover at least one of the overlapping region and the non-overlapping region.
  • the coating layer is formed on the inner surface layer of the outer packaging member so as to cover at least one of the overlapping region and the non-overlapping region, at least the positive electrode current collector and the negative electrode current collector A covering layer is formed so as to cover each end of the body. For this reason, it is possible to prevent the covering member from damaging the outer packaging member when the end portion of the current collector or the connection portion between the end portion of the current collector and the positive electrode or the negative electrode connecting terminal contacts the outer packaging member. it can. Thereby, it can prevent that each edge part of a positive electrode collector and a negative electrode collector and the metal layer of an outer packaging member short-circuit (prevention function).
  • the coating layer can be easily formed in advance on the inner surface layer of the outer packaging member. Therefore, the coating layer having the above-described prevention function can be formed without reducing productivity.
  • the coating layer is formed in advance on the inner surface layer of the outer packaging member, and then the electrode laminate is accommodated in the outer packaging member.
  • the electrolyte can be injected from the opening of the outer packaging member. For this reason, when the electrolytic solution is injected, since the coating layer is not disposed so as to seal the end of the current collector, the electrolytic solution can be sufficiently impregnated into the electrode laminate. Therefore, the coating layer having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate.
  • a coating layer is formed on the inner surface layer of the outer packaging member so as to cover the overlapping region and the non-overlapping region, that is, to cover the entire end of the current collector.
  • the connecting portion is formed by ultrasonic welding.
  • the coating layer preferably contains a tape material.
  • the coating layer is preferably formed by applying a thermoplastic resin.
  • the covering layer may be any of an insulating layer, a conductive layer, and a conductive resin layer as long as the above-described prevention function is achieved.
  • a coating layer can be formed by intermittently applying a thermoplastic resin so as to cover only the resin. Moreover, if the coating layer is remelted at the temperature at which the outer packaging member is thermally welded, the outer packaging member and the electrode laminate can be integrated.
  • the electrode laminate is formed by alternately laminating a plurality of positive plates and a plurality of negative plates with a ninety-fold folded long separator interposed therebetween. Preferably it is.
  • the separator can be handled as a strip-shaped continuous body, so that it is possible to prevent positional deviation between the electrode plate and the separator when the electrode stack is stacked.
  • the bent portion of the separator covers one of the electrode plates, so that the electrolyte impregnation performance is reduced when the electrolyte is injected in the manufacturing process.
  • the coating layer is not disposed so as to seal the end portion of the current collector, the electrode laminate can be impregnated with the electrolyte from the end side. Therefore, the coating layer having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate.
  • the method for manufacturing an electricity storage device according to the present invention is applied to an electricity storage device having the following preconditions.
  • the electricity storage device is disposed on an outer side of an electrode laminate formed by alternately laminating a plurality of positive plates and a plurality of negative plates with a separator interposed therebetween, at least an inner layer made of a thermoplastic resin.
  • a flexible outer packaging member that accommodates the electrode laminate, and electrically connected to each end of the positive electrode current collector of the plurality of positive electrode plates and the negative electrode current collector of the plurality of negative electrode plates.
  • a positive connection terminal and a negative connection terminal led out from the outer peripheral edge of the outer packaging member are provided.
  • An overlapping region where each end of the positive electrode current collector and the negative electrode current collector overlaps with each of the positive electrode connecting terminal and the negative electrode connecting terminal and a non-overlapping region where they do not overlap are formed.
  • the overlapping region includes a connection portion between each end of the positive electrode current collector and the negative electrode current collector and each of the positive electrode connection terminal and the negative electrode connection terminal.
  • a coating layer is formed in advance on the inner surface layer of the outer packaging member so as to cover at least one of the overlapping region and the non-overlapping region. To do.
  • the coating layer can be easily formed on the inner surface layer of the outer packaging member in advance. Therefore, the coating layer having the above-described prevention function can be formed without reducing productivity.
  • an insulating layer is formed in advance on the inner surface layer of the outer packaging member, and then the electrode stack is accommodated in the outer packaging member.
  • the electrolyte can be injected from the opening of the outer packaging member. For this reason, when the electrolytic solution is injected, since the coating layer is not disposed so as to seal the end of the current collector, the electrolytic solution can be sufficiently impregnated into the electrode laminate. Therefore, the coating layer having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate.
  • a covering layer may be formed in advance on the inner surface layer of the outer packaging member so as to cover the overlapping region and the non-overlapping region, that is, to cover the entire end of the current collector. preferable.
  • the connecting portion is formed by ultrasonic welding.
  • the coating layer preferably contains a tape material.
  • the coating layer is preferably formed by applying a thermoplastic resin.
  • a coating layer can be formed by intermittently applying a thermoplastic resin so as to cover only the resin. Moreover, if the coating layer is remelted at the temperature at which the outer packaging member is thermally welded, the outer packaging member and the electrode laminate can be integrated.
  • the electrode laminate is formed by alternately laminating a plurality of positive plates and a plurality of negative plates with a ninety-fold long separator interposed therebetween. Preferably it is formed.
  • the separator can be handled as a strip-shaped continuous body, so that it is possible to prevent positional deviation between the electrode plate and the separator when the electrode stack is stacked.
  • the bent portion of the separator covers one of the electrode plates, so that the electrolyte impregnation performance is reduced when the electrolyte is injected in the manufacturing process.
  • the coating layer is not disposed so as to seal the end portion of the current collector, the electrode laminate can be impregnated with the electrolyte from the end side. Therefore, the insulating layer having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate.
  • an electricity storage device using a flexible outer packaging member it is possible to prevent a short circuit due to damage of the outer packaging member and to improve productivity by improving the impregnation property of the electrolytic solution.
  • FIG. 1 is a schematic plan view showing an example of a laminated lithium ion secondary battery that is an embodiment of an electricity storage device of the present invention.
  • FIG. 2 is a partial cross-sectional view showing, in an enlarged manner, a cross section viewed from a direction along line II-II in FIG. 1 in a laminated lithium ion secondary battery before sealing.
  • FIG. 3 is a partial cross-sectional view showing, in an enlarged manner, a cross section viewed from a direction along line III-III in FIG. 1 in a laminated lithium ion secondary battery before sealing.
  • FIG. 1 is a schematic plan view showing an example of a laminated lithium ion secondary battery that is an embodiment of an electricity storage device of the present invention.
  • FIG. 2 is a partial cross-sectional view showing, in an enlarged manner, a cross section viewed from a direction along line II-II in FIG. 1 in a laminated lithium ion secondary battery before sealing.
  • FIG. 3 is a partial cross-
  • FIG. 4 is a partial cross-sectional view showing, in an enlarged manner, a cross section viewed from a direction along the line IV-IV in FIG. 1 as one embodiment of the electrode laminate in the laminated lithium ion secondary battery of the present invention.
  • FIG. 2 is a partial cross-sectional view showing, in an enlarged manner, a cross section viewed from a direction along line II-II in FIG. 1 in a laminated lithium ion secondary battery after sealing.
  • FIG. 3 is a plan view schematically showing a positional relationship between a negative electrode connection terminal and a current collector in a laminated lithium ion secondary battery as one embodiment of the present invention.
  • a laminate-type lithium ion secondary battery 100 includes an electrode laminate 10 and two upper and lower flexible outer packaging members that have a rectangular shape and accommodate and seal the electrode laminate 10. 20, and a positive electrode connection terminal 30 and a negative electrode connection terminal 40 which are electrically connected to the electrode laminate 10 and led out from the outer peripheral edge of the outer packaging member 20 in a direction facing each other.
  • the sealing part 21 is formed in the outer periphery part of the four directions of the outer packaging member 20 by heat welding (heat sealing).
  • the electrode laminate 10 includes a plurality of positive plates 11, a plurality of negative plates 12, and a separator 13 disposed so as to be interposed between the positive plates 11 and the negative plates 12. And a non-aqueous electrolyte (not shown).
  • the plurality of positive electrode plates 11 and the plurality of negative electrode plates 12 have a strip shape, the separator 13 has a long shape, and the separator 13 is formed into a ninety-nine fold (zigzag shape). 12 are alternately laminated. Further, the outermost periphery of the separator 13 is circulated so as to surround the electrode stack 10. Note that the number of rounds of the outer periphery of the separator 13 is not particularly limited.
  • the negative electrode plate 12 includes a negative electrode current collector 121, and is connected to the negative electrode connection terminal 40 through an end portion where the plurality of negative electrode current collectors 121 of the plurality of negative electrode plates 12 are integrated.
  • the positive electrode plate 11 includes a positive electrode current collector, and is connected to the positive electrode connection terminal 30 (FIG. 1) via an end portion where a plurality of positive electrode current collectors of the plurality of positive electrode plates 11 are integrated. It is connected.
  • the outer packaging member 20 is positioned on the inner surface side facing the electrode laminate 10, and is positioned on the outer surface of the laminated lithium ion secondary battery 100, the inner surface layer made of synthetic resin, It is formed of a single film composed of a metal layer disposed between a layer and an outer surface layer, that is, a laminate film having a three-layer structure (the three-layer structure is omitted in FIGS. 2 and 3).
  • the inner surface layer is made of polypropylene which is a heat-sealable thermoplastic resin and has a thickness of 30 to 120 ⁇ m.
  • the metal layer is made of an aluminum foil or an aluminum alloy foil and has a thickness of 30 to 50 ⁇ m.
  • the outer surface layer is made of nylon (registered trademark) and has a thickness of 20 to 40 ⁇ m.
  • the outer packaging member 20 configured in this manner is a material that is easily deformed and has flexibility.
  • the laminate film should just have an inner surface layer and the metal layer arrange
  • the outer peripheral edge portions of two laminate films are overlapped and heat-welded so that the sealing portion 21 is formed on the outer peripheral edge portions of the four sides.
  • the overlapping region P includes connection portions 121a and non-connection portions 121b between the end portions of the plurality of negative electrode current collectors 121 and the negative electrode connection terminals 40.
  • the connection part 121a is formed by, for example, ultrasonic welding, and is arranged at a plurality of places with the non-connection part 121b interposed therebetween (in FIG. 3, three connection parts 121a and four non-connection parts 121b).
  • the connecting portion 121a may be formed by resistance welding or laser welding.
  • the surface of the inner surface layer of the outer packet member 20 is opposed to at least one of the overlapping region P and the non-overlapping region Q.
  • the covering layer 50 is formed in advance.
  • the covering layer 50 is disposed so as to face the overlapping region P and the non-overlapping region Q, that is, to face the entire end portion R of the negative electrode current collector 121. It is formed in a band shape.
  • the coating layer 50 when forming the coating layer 50 only in the overlapping region P, it is formed intermittently so as not to face the non-overlapping region Q.
  • the coating layer 50 is formed so as to cover the end of the negative electrode current collector 121 on the negative electrode connection terminal 40, but the portion led to the negative electrode connection terminal 40 of the negative electrode current collector 121 (FIG. 2 of the curved negative electrode current collector 121) may be formed.
  • an insulating tape is used in which a silicon-based, acrylic-based, or urethane-based adhesive is adhered to both sides of a base material made of a thermoplastic resin such as polypropylene or polyimide. It is affixed on the surface of the inner surface layer of the outer packaging member 20.
  • the manufacturing process a step of injecting an electrolyte into the outer packaging member 20 in which the electrode laminate 10 is accommodated and a step of vacuum sealing (vacuum sealing) the outer packaging member 20 will be described.
  • the three sides one of the two sides from which the positive electrode connection terminal 30 and the negative electrode connection terminal 40 are led out and the two sides from which the connection terminal is not led out
  • the electrolytic solution is injected into the outer packet member 20 through an opening formed in the other of the outer peripheral edge portions that are not sealed (the other of the two sides from which the connection terminals are not led out).
  • the sides forming the opening may be any of the four sides.
  • the coating layer 50 is disposed on the inner surface layer of the outer packaging member 20 before sealing, and is not disposed so as to seal the ends of both current collectors.
  • the laminate 10 can be sufficiently impregnated.
  • the outer periphery of the outer packaging member 20 is sealed by thermal welding by vacuum-sealing the sides forming the opening.
  • the covering layer 50 formed on the inner surface layer of the outer packaging member 20 is in close contact with the negative electrode current collector 121 so as to cover the entire end of the negative electrode current collector 121. It is formed. In this way, the electrode laminate 10 is vacuum-sealed in the outer packaging member 20 as shown in FIG.
  • the inner layer of the outer packaging member 20 has a coating layer so as to cover at least one of the overlapping region P and the non-overlapping region Q. 50 is formed, the covering layer 50 is formed so as to cover at least the respective ends of the positive electrode current collector and the negative electrode current collector 121.
  • the outer packaging member 20 is damaged when the end portion of the current collector or the connecting portion 121a between the current collector end portion and the positive electrode connection terminal 30 or the negative electrode connection terminal 40 contacts the outer packaging member 20. This can be prevented by the covering layer 50. Thereby, it can prevent that each edge part of the positive electrode collector and the negative electrode collector 121 and the metal layer of the outer packaging member 20 short-circuit (prevention function).
  • the coating layer 50 can be easily formed in advance on the inner surface layer of the outer packaging member 20. Therefore, the coating layer 50 having the above prevention function can be formed without reducing productivity.
  • the coating layer 50 is formed in advance on the inner surface layer of the outer packaging member 20, and then the electrode stack 10 is formed.
  • the electrolytic solution can be injected from the opening of the outer packaging member 20 by being housed in the outer packaging member 20. For this reason, when the electrolytic solution is injected, since the coating layer 50 is not disposed so as to seal the end portion of the current collector, the electrode laminate 10 can be sufficiently impregnated with the electrolytic solution. Therefore, the coating layer 50 having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate 10.
  • the inner surface layer of the outer packaging member 20 covers the overlapping region P and the non-overlapping region Q, that is, the entire end portion of the current collector.
  • a covering layer 50 is formed so as to cover R.
  • the connecting portion 121a is formed by ultrasonic welding, burrs or the like generated by ultrasonic welding are in contact with the outer packaging member 20.
  • the outer cover member 20 can be prevented from being damaged by the covering layer 50. Thereby, it can prevent that the burr
  • the covering layer 50 includes the tape material, so that the covering layer 50 specifically disposed on the inner surface layer of the outer packaging member 20 can be easily formed. Can be formed (pasted). Therefore, the coating layer 50 having the above prevention function can be formed without reducing productivity.
  • the coating layer 50 is configured to include a tape material, but the coating layer 50 is formed by applying a thermoplastic resin. You may do it. By being configured in this manner, the overlapping is further performed so as to cover only the overlapping region P where the respective ends of the positive electrode current collector and the negative electrode current collector 121 overlap with each of the positive electrode connection terminal 30 and the negative electrode connection terminal 40.
  • the coating layer 50 can be formed by intermittently applying a thermoplastic resin so as to cover only the connection portion 121a in the region P. Moreover, if the coating layer 50 is remelted at the temperature at which the outer packaging member 20 is thermally welded, the outer packaging member 20 and the electrode laminate 10 can be integrated.
  • the covering layer 50 may be any of an insulating layer, a conductive layer, and a conductive resin as long as it performs the above-described prevention function.
  • the electrode laminate 10 includes a plurality of positive electrode plates 11 with the long separator 13 folded in ninety-nine folds. It is formed by alternately laminating a plurality of negative electrode plates 12.
  • the separator 13 can be handled as a belt-like continuous body, so that it is possible to prevent positional deviation between the electrode plate and the separator 13 when the electrode laminate 10 is stacked.
  • the bent portion of the separator 13 covers one of the electrode plates, so that the electrolyte solution is impregnated when the electrolyte solution is injected in the manufacturing process.
  • the coating layer 50 is not disposed so as to seal the end portion of the current collector, the electrode laminate 10 is impregnated with the electrolyte from the end side. Can do. Therefore, the coating layer 50 having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate 10.
  • the negative electrode connection terminal 40 is connected by ultrasonic welding on the lower surface of the portion where the ends of the current collector are integrated, but the negative electrode connection terminal 40 may be connected by ultrasonic welding on the upper surface of the location where the current collector is integrated, or arranged so as to be inserted into the location where the current collector is integrated, and by ultrasonic welding. They may be connected (the same applies to the positive electrode side).
  • one separator 13 is interposed between the positive electrode plate 11 and the negative electrode plate 12 as a configuration of the electrode laminate 10. May be interposed.
  • the material of the plurality of separators may be the same or different.
  • a strip-shaped separator may be interposed between the positive electrode plate and the negative electrode plate.
  • polyolefin resins such as polypropylene and polyethylene, or a combination thereof, those obtained by adding ceramics such as silica and alumina to polyolefin resins, polyethylene terephthalate, cellulose, nonwoven fabric, and the like are used.
  • the positive electrode plate 11 is configured by forming a positive electrode mixture layer containing a positive electrode active material on both surfaces of the positive electrode current collector, except for an end portion on the side connected to the positive electrode connection terminal 30.
  • the negative electrode plate 12 is configured by forming a negative electrode mixture layer containing a negative electrode active material on both surfaces of the negative electrode current collector, except for an end portion on the side connected to the negative electrode connection terminal 40.
  • the positive electrode plate 11 has a positive electrode slurry obtained by kneading a positive electrode active material, a binder, and optionally a conductive additive in an organic solvent, on both surfaces of a positive electrode current collector made of aluminum foil. It is produced by applying to the substrate and drying to form a positive electrode mixture layer on both surfaces of the positive electrode current collector.
  • the positive electrode active material a metal oxide, a metal sulfide, or a specific polymer can be used depending on the type of the target battery.
  • a metal sulfide or oxide such as TiS 2 , MoS 2 , NbSe 2 , or V 2 O 5 can be used as the positive electrode active material.
  • LiM x O 2 in the chemical formula, M represents one or more transition metals, x varies depending on the charge / discharge state of the battery, and is usually 0.05 or more and 1.10 or less as a positive electrode active material of the lithium ion secondary battery.
  • Lithium composite oxide mainly composed of As the transition metal M constituting this lithium composite oxide, Co, Ni, Mn and the like are preferable.
  • These lithium composite oxides can generate a high voltage and become a positive electrode active material having an excellent energy density.
  • a plurality of these positive electrode active materials may be used in combination.
  • the well-known binder currently normally used for the positive electrode compound material of a lithium ion secondary battery can be used, and said positive electrode compound material is used.
  • the negative electrode plate 12 is made of a negative electrode slurry formed by kneading a negative electrode active material, a binder, and optionally a conductive additive in an organic solvent, on both sides of a negative electrode current collector made of copper foil or aluminum foil. It is produced by coating uniformly on the top and drying to form a negative electrode mixture layer on both sides of the negative electrode current collector.
  • a carbon material such as a non-graphitizable carbon material or a graphite material can be used as the negative electrode active material.
  • carbon materials such as pyrolytic carbons, cokes, graphites, glassy carbon fibers, organic polymer compound fired bodies, carbon fibers, and activated carbon can be used.
  • the cokes include pitch coke, needle coke, and petroleum coke.
  • said organic polymer compound fired body means what carbonized by baking a phenol resin, furan resin, etc. at a suitable temperature.
  • materials that can be doped and dedoped with lithium include polymers such as polyacetylene and polypyrrole, Sn oxides such as SnO 2 , Sn alloys such as Sn 5 Cu 6 , and SiMg 2.
  • Si alloy system such as Li 4 Ti 5 O 12 (lithium titanate) can also be used.
  • the well-known binder currently normally used for the negative electrode compound material of a lithium ion secondary battery can be used, and said negative electrode compound material is used.
  • the nonaqueous electrolytic solution is prepared by dissolving an electrolyte in a nonaqueous solvent.
  • the electrolyte for example, a solution obtained by dissolving LiPF 6 at a concentration of 1.0 mol / L in a non-aqueous solvent is used.
  • an electrolyte other than LiPF 6 lithium salts such as LiBF 4 , LiAsF 6 , LiClO 4 , LiCF 3 SO 3 , LiN (SO 2 CF 3 ) 2 , LiC (SO 2 CF 3 ) 3 , LiAlCl 4 , LiSiF 6 are used. Can be mentioned.
  • LiPF 6 or LiBF 4 is particularly used as the electrolyte.
  • Such an electrolyte is preferably used by being dissolved in a non-aqueous solvent at a concentration of 0.1 mol / L to 3.0 mol / L, and is preferably dissolved at a concentration of 0.5 mol / L to 2.0 mol / L. More preferably, it is used.
  • the non-aqueous solvent for example, a mixture of propylene carbonate, ethylene carbonate and diethyl carbonate in a volume ratio of 5 to 20:20 to 30:60 to 70 is used.
  • non-aqueous solvents include: cyclic carbonates such as propylene carbonate and ethylene carbonate; chain carbonates such as diethyl carbonate and dimethyl carbonate; carboxylic acid esters such as methyl propionate and methyl butyrate; ⁇ -butyllactone, sulfolane, Ethers such as 2-methyltetrahydrofuran and dimethoxyethane can be used.
  • cyclic carbonates such as propylene carbonate and ethylene carbonate
  • chain carbonates such as diethyl carbonate and dimethyl carbonate
  • carboxylic acid esters such as methyl propionate and methyl butyrate
  • ⁇ -butyllactone sulfolane
  • Ethers such as 2-methyltetrahydrofuran and dimethoxyethane can be used.
  • carbonate ester it is preferable from the point of oxidation stability to use carbonate ester as a non-aqueous solvent.
  • the present invention is applied to the lithium ion secondary battery 100 as an example of an electricity storage device.
  • an electricity storage device using a flexible outer packaging member to accommodate at least the electrode stack If so, the present invention can be applied.
  • the present invention can be applied to a lithium secondary battery, a polymer secondary battery, an electric double layer capacitor, and the like.
  • the electricity storage device of the present invention in an electricity storage device that houses an electricity storage element using a flexible outer packaging member, prevents a short circuit due to damage to the outer packaging member, and improves productivity by improving the impregnation property of the electrolytic solution. Therefore, an electricity storage device in which a flexible outer packaging member can be used, for example, a lithium secondary battery, a polymer secondary battery, an organic radical battery, an all solid state battery in addition to a lithium ion secondary battery as an electricity storage element This contributes to improving the productivity of an electricity storage device that accommodates various electricity storage elements such as electric double layer capacitors.
  • SYMBOLS 10 Electrode laminated body, 11: Positive electrode plate, 12: Negative electrode plate, 13: Separator, 20: Outer packaging member, 50: Coating layer, 100: Laminate type lithium ion secondary battery, 121: Negative electrode collector, 121a: Connection Part, 121b: non-connection part, P: overlapping area, Q: non-overlapping area.

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Abstract

Disclosed is an electrical storage device using a flexible outer package member, wherein a short-circuit due to breakage of the outer package member is eliminated, and productivity is improved by improving impregnation of an electrolytic solution. Also disclosed is a method for manufacturing the electrical storage device. In the electrical storage device, overlapping regions (P) where the end portion of a positive electrode collector and that of a negative electrode collector (121) overlap a positive electrode connecting terminal (30) and a negative electrode connecting terminal (40), respectively, and a non-overlapping region (Q) where the end portions and the terminals do not overlap are formed. The overlapping regions (P) include, connecting sections (121a) where the end portions of respective positive electrode collector and the negative electrode collector (121) are respectively connected to the positive electrode connecting terminal (30) and the negative electrode connecting terminal (40). On the inner surface layer of the outer packaging member (20), a coat layer (50) is formed such that the coat layer covers the overlapping regions (P) and/or the non-overlapping region (Q).

Description

蓄電デバイスとその製造方法Electric storage device and manufacturing method thereof
 本発明は、一般的には蓄電デバイスとその製造方法に関し、特定的には、リチウムイオン二次電池、リチウム二次電池、ポリマー二次電池、有機ラジカル電池、全固体電池、電気二重層キャパシタなどの蓄電要素を、可撓性を有する外包部材を用いて収容する蓄電デバイスおよびその製造方法に関するものである。 The present invention generally relates to an electricity storage device and a method for manufacturing the same, and specifically, a lithium ion secondary battery, a lithium secondary battery, a polymer secondary battery, an organic radical battery, an all-solid battery, an electric double layer capacitor, and the like. The electrical storage element which accommodates this electrical storage element using the outer packaging member which has flexibility, and its manufacturing method are related.
 従来から、たとえば、リチウムイオン二次電池等の蓄電デバイスに関しては、多様な用途の拡大に伴って、軽量化、薄型化、形状の自由度等の要求が高まっている。 2. Description of the Related Art Conventionally, with respect to power storage devices such as lithium ion secondary batteries, there are increasing demands for weight reduction, thickness reduction, shape flexibility, and the like with the expansion of various applications.
 そこで、軽量化、薄型化に優れたリチウムイオン二次電池として、可撓性のラミネートフィルム(積層シートともいう)を用いて蓄電要素を収容したリチウムイオン二次電池が用いられている。ラミネートフィルムは、蓄電要素に面する内面側に位置付けられ、合成樹脂からなる内面層と、リチウムイオン二次電池の外表面に位置付けられ、合成樹脂からなる外面層と、内面層と外面層との間に配置される中間層から構成される。内面層は、たとえば、ポリエチレン、ポリプロピレン等の耐電解液性とヒートシール性に優れた熱可塑性樹脂からなる。中間層は、たとえば、アルミニウム箔等の可撓性と強度に優れた金属層からなる。外面層は、たとえば、ナイロン、ポリアミド等の電気絶縁性に優れた絶縁樹脂からなる。蓄電要素は、セパレータを介して正極板と負極板とを巻回または交互に積層させてなる。 Therefore, as a lithium ion secondary battery excellent in weight reduction and thickness reduction, a lithium ion secondary battery containing a storage element using a flexible laminate film (also referred to as a laminated sheet) is used. The laminate film is positioned on the inner surface side facing the power storage element, and is positioned on the outer surface of the synthetic resin, the outer surface of the lithium ion secondary battery, the outer surface layer of the synthetic resin, and the inner surface layer and the outer surface layer. It consists of an intermediate layer placed between them. The inner surface layer is made of, for example, a thermoplastic resin excellent in electrolytic solution resistance and heat sealability, such as polyethylene and polypropylene. An intermediate | middle layer consists of a metal layer excellent in flexibility and intensity | strength, such as aluminum foil, for example. The outer surface layer is made of, for example, an insulating resin excellent in electrical insulation, such as nylon or polyamide. The power storage element is formed by winding or alternately stacking a positive electrode plate and a negative electrode plate via a separator.
 一方、このようなラミネートフィルムを用いたリチウムイオン二次電池の電池特性においても、高入出力特性、高エネルギー密度、高サイクル特性等が求められている。そこで、蓄電要素として、セパレータを介在して複数の正極板と複数の負極板とを交互に積層させることにより形成された電極積層体を用いることで、高入出力特性、高エネルギー密度、高サイクル特性等を満足させることが検討されている。しかしながら、電極積層体は、長尺状の電極板を用いる電極巻回体と異なり、複数の短冊状の正極板および負極板を用いるため、製造工程において長尺状の正極板および負極板を個々の短冊状にカットする必要がある。このとき、正極板の正極集電体の端部および負極板の負極集電体の端部にバリや突起などが形成されてしまうと、ラミネートフィルムの内面層が損傷し、集電体の端部とラミネートフィルムの中間層を構成する金属層とが接触して短絡してしまう恐れがある。 On the other hand, in the battery characteristics of a lithium ion secondary battery using such a laminate film, high input / output characteristics, high energy density, high cycle characteristics, and the like are required. Therefore, by using an electrode laminate formed by alternately laminating a plurality of positive plates and a plurality of negative plates with separators interposed as power storage elements, high input / output characteristics, high energy density, and high cycle Satisfying characteristics and the like is being studied. However, since the electrode laminate uses a plurality of strip-like positive and negative plates unlike an electrode winding body that uses a long electrode plate, the long positive and negative plates are individually used in the manufacturing process. It is necessary to cut it into strips. At this time, if burrs or protrusions are formed at the end of the positive electrode current collector of the positive electrode plate and the end of the negative electrode current collector of the negative electrode plate, the inner surface layer of the laminate film is damaged, and the end of the current collector There is a possibility that the metal layer constituting the intermediate layer of the laminate film and the laminate film may come into contact with each other and short-circuit.
 そこで、これらの問題を解決するために、たとえば、特開2000-58011号公報(以下、特許文献1という)では、扁平型電池において、外部端子箔(正極または負極接続端子)と集電体の端子接続部を熱硬化性樹脂で被覆し、結線部分と外包部材の短絡と、外装ケース(外包部材)の封止信頼性の劣化を抑制することが提案されている。 In order to solve these problems, for example, in Japanese Unexamined Patent Publication No. 2000-58011 (hereinafter referred to as Patent Document 1), in a flat battery, an external terminal foil (positive electrode or negative electrode connection terminal) and a current collector It has been proposed that the terminal connection portion is covered with a thermosetting resin to suppress a short circuit between the connection portion and the outer packaging member and deterioration of the sealing reliability of the outer case (outer packaging member).
 また、特許第4065915号公報(以下、特許文献2という)では、リチウム二次電池において、グリッド(電極の集電体)とタブ部材(正極または負極接続端子)の溶接部を絶縁テープで被覆することにより、溶接部またはタブ部材によって包装材(外包部材)が損傷することによって短絡する現象を防止することが提案されている。 Further, in Japanese Patent No. 4065915 (hereinafter referred to as Patent Document 2), in a lithium secondary battery, a welded portion of a grid (electrode current collector) and a tab member (positive electrode or negative electrode connection terminal) is covered with an insulating tape. Therefore, it has been proposed to prevent a short circuit caused by damage to the packaging material (outer packaging member) due to the welded portion or the tab member.
 また、特開2005-149938号公報(以下、特許文献3という)では、フィルム外装電池において、正極タブ(正極接続端子)および負極タブ(負極接続端子)の端部のカエリ除去を行うことなく、カエリによる不具合を防止するために、正極集電部および負極集電部と正極タブおよび負極タブとの接合部分に、正極タブおよび負極タブのカエリを被覆するように保護テープが貼り付けられたものが提案されている。 Further, in Japanese Patent Application Laid-Open No. 2005-149938 (hereinafter referred to as Patent Document 3), without removing the burrs at the ends of the positive electrode tab (positive electrode connection terminal) and the negative electrode tab (negative electrode connection terminal) in the film-covered battery, In order to prevent defects due to burrs, protective tape is applied to the joints between the positive and negative current collectors and the positive and negative tabs to cover the positive and negative tabs Has been proposed.
 さらに、特開2002-175790号公報(以下、特許文献4という)では、扁平電池において、正極板の集電体と正極リード(正極接続端子)、負極板の集電体と負極リード(負極接続端子)、および、これらの接続部を、電解液に不溶性の接着性樹脂で被覆することによって、正極板と負極板とがセパレータを介して絶縁された電極群と、外装ケース(外包部材)とを一体化することが提案されている。また、特許文献4では、外装ケースのシール部と、シール部を臨む電極群の端面とに取り囲まれた空間部に、電解液に不溶性の接着性樹脂を充填し、各リードを接着性樹脂にて被覆することが提案されている。 Further, in Japanese Patent Application Laid-Open No. 2002-175790 (hereinafter referred to as Patent Document 4), in a flat battery, a current collector and positive electrode lead (positive electrode connection terminal) of a positive electrode plate, and a current collector and negative electrode lead (negative electrode connection) of a negative electrode plate. A terminal), and an electrode group in which the positive electrode plate and the negative electrode plate are insulated via a separator by covering the connection portion with an adhesive resin insoluble in the electrolyte, and an outer case (outer packaging member) It has been proposed to integrate. In Patent Document 4, the space surrounded by the seal part of the outer case and the end face of the electrode group facing the seal part is filled with an adhesive resin that is insoluble in the electrolytic solution, and each lead is used as an adhesive resin. It has been proposed to coat them.
特開2000-58011号公報JP 2000-58011 A 特許第4065915号Patent No. 4065915 特開2005-149938号公報JP 2005-149938 A 特開2002-175790号公報JP 2002-175790 A
 しかしながら、特許文献1~4では、次のような問題がある。すなわち、製造工程において電解液を注入する前に正極集電体および負極集電体の端部に絶縁層を形成するので、集電体の端部が絶縁層で封じられた状態で電解液を注入することになる。そうすると、集電体の端部側から電極積層体の中央部に向かって電解液を含浸させていくことができず、電解液の含浸性が悪くなったり、十分に含浸させるために含浸時間が長くなるといった問題がある。 However, Patent Documents 1 to 4 have the following problems. That is, since an insulating layer is formed at the ends of the positive electrode current collector and the negative electrode current collector before injecting the electrolytic solution in the manufacturing process, the electrolytic solution is used with the ends of the current collector sealed with the insulating layer. Will be injected. Then, the electrolyte solution cannot be impregnated from the end side of the current collector toward the center portion of the electrode laminate, and the impregnation time of the electrolyte solution deteriorates or the impregnation time becomes insufficient. There is a problem of becoming longer.
 そこで、本発明の目的は、可撓性の外包部材を用いた蓄電デバイスにおいて、外包部材の損傷による短絡を防止するとともに、電解液の含浸性の向上によって生産性を向上させることが可能な蓄電デバイスとその製造方法を提供することである。 SUMMARY OF THE INVENTION Accordingly, an object of the present invention is to provide a power storage device using a flexible outer packaging member, which can prevent a short circuit due to damage of the outer packaging member, and can improve productivity by improving the impregnation property of the electrolytic solution. It is to provide a device and its manufacturing method.
 本発明に従った蓄電デバイスは、セパレータを介在して複数の正極板と複数の負極板とを交互に積層させることにより形成された電極積層体と、少なくとも熱可塑性樹脂からなる内面層とその外側に配置される金属層とを有し、この電極積層体を収容する可撓性の外包部材と、複数の正極板の正極集電体および複数の負極板の負極集電体のそれぞれの端部に電気的に接続されるとともに、外包部材の外周縁部から導出された正極接続端子及び負極接続端子とを備える。正極集電体および負極集電体のそれぞれの端部と正極接続端子および負極接続端子のそれぞれとが重なる重複領域と、重ならない非重複領域とが形成されている。重複領域が、正極集電体および負極集電体のそれぞれの端部と正極接続端子および負極接続端子のそれぞれとの接続部を含む。外包部材の内面層には、重複領域および非重複領域の少なくともいずれかの領域を覆うように被覆層が形成されている。 An electricity storage device according to the present invention includes an electrode laminate formed by alternately laminating a plurality of positive plates and a plurality of negative plates with a separator interposed therebetween, an inner surface layer made of at least a thermoplastic resin, and an outer side thereof And a flexible outer packaging member that accommodates the electrode stack, and ends of the positive electrode current collectors of the plurality of positive electrode plates and the negative electrode current collectors of the plurality of negative electrode plates, respectively. And a positive electrode connection terminal and a negative electrode connection terminal led out from the outer peripheral edge of the outer packaging member. An overlapping region where each end of the positive electrode current collector and the negative electrode current collector overlaps with each of the positive electrode connecting terminal and the negative electrode connecting terminal and a non-overlapping region where they do not overlap are formed. The overlapping region includes a connection portion between each end of the positive electrode current collector and the negative electrode current collector and each of the positive electrode connection terminal and the negative electrode connection terminal. A coating layer is formed on the inner surface layer of the outer packaging member so as to cover at least one of the overlapping region and the non-overlapping region.
 本発明の蓄電デバイスにおいては、外包部材の内面層には、重複領域および非重複領域の少なくともいずれかの領域を覆うように被覆層が形成されているので、少なくとも正極集電体および負極集電体のそれぞれの端部を覆うように被覆層が形成されている。このため、集電体の端部、または、集電体の端部と正極もしくは負極接続端子との接続部が外包部材に接触することによって外包部材が損傷することを被覆層によって防止することができる。これにより、正極集電体および負極集電体のそれぞれの端部と外包部材の金属層とが短絡することを防止することができる(防止機能)。 In the electricity storage device of the present invention, since the coating layer is formed on the inner surface layer of the outer packaging member so as to cover at least one of the overlapping region and the non-overlapping region, at least the positive electrode current collector and the negative electrode current collector A covering layer is formed so as to cover each end of the body. For this reason, it is possible to prevent the covering member from damaging the outer packaging member when the end portion of the current collector or the connection portion between the end portion of the current collector and the positive electrode or the negative electrode connecting terminal contacts the outer packaging member. it can. Thereby, it can prevent that each edge part of a positive electrode collector and a negative electrode collector and the metal layer of an outer packaging member short-circuit (prevention function).
 また、外包部材の内面層は熱可塑性樹脂といった樹脂材料からなるので、予め被覆層を外包部材の内面層に容易に形成することができる。したがって、生産性を低下させることがなく、上記の防止機能を有する被覆層を形成することができる。 Further, since the inner surface layer of the outer packaging member is made of a resin material such as a thermoplastic resin, the coating layer can be easily formed in advance on the inner surface layer of the outer packaging member. Therefore, the coating layer having the above-described prevention function can be formed without reducing productivity.
 さらに、正極集電体および負極集電体のそれぞれの端部の上に直接被覆層を形成しないで、外包部材の内面層に被覆層を予め形成した後、電極積層体を外包部材に収納し、外包部材の開口部より電解液を注入することができる。このため、電解液が注入される際には、集電体の端部を封じるように被覆層が配置されていないので、電解液を電極積層体に十分に含浸することができる。したがって、電解液の電極積層体への含浸性を低下させることがなく、上記の防止機能を有する被覆層を形成することができる。 Furthermore, without forming the coating layer directly on the respective end portions of the positive electrode current collector and the negative electrode current collector, the coating layer is formed in advance on the inner surface layer of the outer packaging member, and then the electrode laminate is accommodated in the outer packaging member. The electrolyte can be injected from the opening of the outer packaging member. For this reason, when the electrolytic solution is injected, since the coating layer is not disposed so as to seal the end of the current collector, the electrolytic solution can be sufficiently impregnated into the electrode laminate. Therefore, the coating layer having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate.
 本発明の蓄電デバイスにおいて、外包部材の内面層には、重複領域および非重複領域を覆うように、すなわち、集電体の端部全体を覆うように被覆層が形成されていることが好ましい。 In the electricity storage device of the present invention, it is preferable that a coating layer is formed on the inner surface layer of the outer packaging member so as to cover the overlapping region and the non-overlapping region, that is, to cover the entire end of the current collector.
 このように構成することにより、集電体の端部のいずれの箇所が外包部材に接触しても、集電体の端部が外包部材に接触することによって外包部材が損傷することを被覆層によって防止することができる。これにより、集電体の端部と外包部材の金属層とが短絡することを防止することができる。 By configuring in this way, even if any part of the end portion of the current collector contacts the outer packaging member, the outer packaging member is damaged by the end portion of the current collector contacting the outer packaging member. Can be prevented. Thereby, it can prevent that the edge part of an electrical power collector and the metal layer of an outer packaging member short-circuit.
 また、本発明の蓄電デバイスにおいて、接続部は、超音波溶着によって形成されていることが好ましい。 In the electricity storage device of the present invention, it is preferable that the connecting portion is formed by ultrasonic welding.
 この場合、超音波溶着によって生じるバリ等が外包部材に接触することによって外包部材が損傷することを被覆層によって防止することができる。これにより、超音波溶着によって生じるバリ等と外包部材の金属層とが短絡することを防止することができる。 In this case, it is possible to prevent the covering member from damaging the outer packaging member due to the burr or the like generated by ultrasonic welding contacting the outer packaging member. Thereby, it can prevent that the burr | flash etc. which arise by ultrasonic welding, and the metal layer of an outer packaging member short-circuit.
 さらに、本発明の蓄電デバイスにおいて、被覆層がテープ材を含むことが好ましい。 Furthermore, in the electricity storage device of the present invention, the coating layer preferably contains a tape material.
 このように構成することにより、外包部材の内面層に特定的に配置された被覆層を容易に形成する(貼り付ける)ことができる。したがって、生産性を低下させることがなく、上記の防止機能を有する被覆層を形成することができる。 By configuring in this way, it is possible to easily form (paste) a coating layer specifically disposed on the inner surface layer of the outer packaging member. Therefore, the coating layer having the above-described prevention function can be formed without reducing productivity.
 あるいは、本発明の蓄電デバイスにおいて、被覆層が熱可塑性樹脂を塗布して形成してなることが好ましい。また、被覆層は上述の防止機能を果たす限り、絶縁層、導電層、導電性樹脂層のいずれであってもかまわない。 Alternatively, in the electricity storage device of the present invention, the coating layer is preferably formed by applying a thermoplastic resin. Further, the covering layer may be any of an insulating layer, a conductive layer, and a conductive resin layer as long as the above-described prevention function is achieved.
 このように構成することにより、正極集電体および負極集電体のそれぞれの端部と正極接続端子および負極接続端子のそれぞれとが重なる重複領域のみを覆うように、さらには重複領域の接続部のみを覆うように、熱可塑性樹脂を間欠的に塗布することによって被覆層を形成することができる。また、外包部材の熱溶着時の温度で被覆層が再溶融すれば、外包部材と電極積層体との一体化が可能である。 By configuring in this way, only the overlapping region where the respective end portions of the positive electrode current collector and the negative electrode current collector overlap with each of the positive electrode connection terminal and the negative electrode connection terminal is further covered. A coating layer can be formed by intermittently applying a thermoplastic resin so as to cover only the resin. Moreover, if the coating layer is remelted at the temperature at which the outer packaging member is thermally welded, the outer packaging member and the electrode laminate can be integrated.
 また、本発明の蓄電デバイスにおいて、電極積層体は、九十九折りにした長尺状のセパレータを介在して、複数の正極板と複数の負極板とを交互に積層させることにより形成されていることが好ましい。 Further, in the electricity storage device of the present invention, the electrode laminate is formed by alternately laminating a plurality of positive plates and a plurality of negative plates with a ninety-fold folded long separator interposed therebetween. Preferably it is.
 このように構成することにより、セパレータを帯状の連続体で取り扱うことができるので、電極積層体の積み重ね時の電極板とセパレータとの位置ずれ等を防止することができる。ここで、九十九折りにした長尺状のセパレータを用いると、セパレータの折り曲げ部が一方の電極板を覆うことになり、製造工程において電解液を注入する際に電解液の含浸性が低下するという問題があるが、本発明においては、集電体の端部を封じるように被覆層が配置されていないので、端部側からも電解液を電極積層体に含浸することができる。したがって、電解液の電極積層体への含浸性を低下させることがなく、上記の防止機能を有する被覆層を形成することができる。 By configuring in this way, the separator can be handled as a strip-shaped continuous body, so that it is possible to prevent positional deviation between the electrode plate and the separator when the electrode stack is stacked. Here, when a long and narrow separator is used, the bent portion of the separator covers one of the electrode plates, so that the electrolyte impregnation performance is reduced when the electrolyte is injected in the manufacturing process. However, in the present invention, since the coating layer is not disposed so as to seal the end portion of the current collector, the electrode laminate can be impregnated with the electrolyte from the end side. Therefore, the coating layer having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate.
 本発明に従った蓄電デバイスの製造方法は、以下の前提となる構成を有する蓄電デバイスに適用される。 The method for manufacturing an electricity storage device according to the present invention is applied to an electricity storage device having the following preconditions.
 その蓄電デバイスは、セパレータを介在して複数の正極板と複数の負極板とを交互に積層させることにより形成された電極積層体と、少なくとも熱可塑性樹脂からなる内面層とその外側に配置される金属層とを有し、この電極積層体を収容する可撓性の外包部材と、複数の正極板の正極集電体および複数の負極板の負極集電体のそれぞれの端部に電気的に接続されるとともに、外包部材の外周縁部から導出された正極接続端子および負極接続端子とを備える。正極集電体および負極集電体のそれぞれの端部と正極接続端子および負極接続端子のそれぞれとが重なる重複領域と、重ならない非重複領域とが形成されている。重複領域が、正極集電体および負極集電体のそれぞれの端部と正極接続端子および負極接続端子のそれぞれとの接続部を含む。 The electricity storage device is disposed on an outer side of an electrode laminate formed by alternately laminating a plurality of positive plates and a plurality of negative plates with a separator interposed therebetween, at least an inner layer made of a thermoplastic resin. A flexible outer packaging member that accommodates the electrode laminate, and electrically connected to each end of the positive electrode current collector of the plurality of positive electrode plates and the negative electrode current collector of the plurality of negative electrode plates. A positive connection terminal and a negative connection terminal led out from the outer peripheral edge of the outer packaging member are provided. An overlapping region where each end of the positive electrode current collector and the negative electrode current collector overlaps with each of the positive electrode connecting terminal and the negative electrode connecting terminal and a non-overlapping region where they do not overlap are formed. The overlapping region includes a connection portion between each end of the positive electrode current collector and the negative electrode current collector and each of the positive electrode connection terminal and the negative electrode connection terminal.
 本発明の蓄電デバイスの製造方法では、上記の前提となる構成を有する蓄電デバイスにおいて、外包部材の内面層に、重複領域および非重複領域の少なくともいずれかの領域を覆うように被覆層を予め形成する。 In the power storage device manufacturing method of the present invention, in the power storage device having the above-described configuration, a coating layer is formed in advance on the inner surface layer of the outer packaging member so as to cover at least one of the overlapping region and the non-overlapping region. To do.
 本発明の蓄電デバイスの製造方法においては、外包部材の内面層は熱可塑性樹脂といった樹脂材料からなるので、予め被覆層を外包部材の内面層に容易に形成することができる。したがって、生産性を低下させることがなく、上記の防止機能を有する被覆層を形成することができる。 In the method for manufacturing an electricity storage device of the present invention, since the inner surface layer of the outer packaging member is made of a resin material such as a thermoplastic resin, the coating layer can be easily formed on the inner surface layer of the outer packaging member in advance. Therefore, the coating layer having the above-described prevention function can be formed without reducing productivity.
 また、正極集電体および負極集電体のそれぞれの端部の上に直接被覆層を形成しないで、外包部材の内面層に絶縁層を予め形成した後、電極積層体を外包部材に収納し、外包部材の開口部より電解液を注入することができる。このため、電解液が注入される際には、集電体の端部を封じるように被覆層が配置されていないので、電解液を電極積層体に十分に含浸することができる。したがって、電解液の電極積層体への含浸性を低下させることがなく、上記の防止機能を有する被覆層を形成することができる。 In addition, without forming a coating layer directly on the respective end portions of the positive electrode current collector and the negative electrode current collector, an insulating layer is formed in advance on the inner surface layer of the outer packaging member, and then the electrode stack is accommodated in the outer packaging member. The electrolyte can be injected from the opening of the outer packaging member. For this reason, when the electrolytic solution is injected, since the coating layer is not disposed so as to seal the end of the current collector, the electrolytic solution can be sufficiently impregnated into the electrode laminate. Therefore, the coating layer having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate.
 本発明の蓄電デバイスの製造方法において、外包部材の内面層には、重複領域および非重複領域を覆うように、すなわち、集電体の端部全体を覆うように被覆層を予め形成することが好ましい。 In the method for manufacturing an electricity storage device of the present invention, a covering layer may be formed in advance on the inner surface layer of the outer packaging member so as to cover the overlapping region and the non-overlapping region, that is, to cover the entire end of the current collector. preferable.
 このように構成することにより、集電体の端部のいずれの箇所が外包部材に接触しても、集電体の端部が外包部材に接触することによって外包部材が損傷することを被覆層によって防止することができる。これにより、集電体の端部と外包部材の金属層とが短絡することを防止することができる。 By configuring in this way, even if any part of the end portion of the current collector contacts the outer packaging member, the outer packaging member is damaged by the end portion of the current collector contacting the outer packaging member. Can be prevented. Thereby, it can prevent that the edge part of an electrical power collector and the metal layer of an outer packaging member short-circuit.
 また、本発明の蓄電デバイスの製造方法において、接続部は、超音波溶着によって形成されていることが好ましい。 In the method for manufacturing an electricity storage device of the present invention, it is preferable that the connecting portion is formed by ultrasonic welding.
 この場合、超音波溶着によって生じるバリ等が外包部材に接触することによって外包部材が損傷することを被覆層によって防止することができる。これにより、超音波溶着によって生じるバリ等と外包部材の金属層とが短絡することを防止することができる。 In this case, it is possible to prevent the covering member from damaging the outer packaging member due to the burr or the like generated by ultrasonic welding contacting the outer packaging member. Thereby, it can prevent that the burr | flash etc. which arise by ultrasonic welding, and the metal layer of an outer packaging member short-circuit.
 さらに、本発明の蓄電デバイスの製造方法において、被覆層がテープ材を含むことが好ましい。 Furthermore, in the method for manufacturing an electricity storage device of the present invention, the coating layer preferably contains a tape material.
 このように構成することにより、外包部材の内面層に特定的に配置された被覆層を容易に形成する(貼り付ける)ことができる。したがって、生産性を低下させることがなく、上記の防止機能を有する被覆層を形成することができる。 By configuring in this way, it is possible to easily form (paste) a coating layer specifically disposed on the inner surface layer of the outer packaging member. Therefore, the coating layer having the above-described prevention function can be formed without reducing productivity.
 さらにまた、本発明の蓄電デバイスの製造方法において、被覆層が熱可塑性樹脂を塗布して形成してなることが好ましい。 Furthermore, in the method for manufacturing an electricity storage device of the present invention, the coating layer is preferably formed by applying a thermoplastic resin.
 このように構成することにより、正極集電体および負極集電体のそれぞれの端部と正極接続端子および負極接続端子のそれぞれとが重なる重複領域のみを覆うように、さらには重複領域の接続部のみを覆うように、熱可塑性樹脂を間欠的に塗布することによって被覆層を形成することができる。また、外包部材の熱溶着時の温度で被覆層が再溶融すれば、外包部材と電極積層体との一体化が可能である。 By configuring in this way, only the overlapping region where the respective end portions of the positive electrode current collector and the negative electrode current collector overlap with each of the positive electrode connection terminal and the negative electrode connection terminal is further covered. A coating layer can be formed by intermittently applying a thermoplastic resin so as to cover only the resin. Moreover, if the coating layer is remelted at the temperature at which the outer packaging member is thermally welded, the outer packaging member and the electrode laminate can be integrated.
 また、本発明の蓄電デバイスの製造方法において、電極積層体は、九十九折りにした長尺状のセパレータを介在して、複数の正極板と複数の負極板とを交互に積層させることにより形成されていることが好ましい。 Further, in the method for manufacturing an electricity storage device of the present invention, the electrode laminate is formed by alternately laminating a plurality of positive plates and a plurality of negative plates with a ninety-fold long separator interposed therebetween. Preferably it is formed.
 このように構成することにより、セパレータを帯状の連続体で取り扱うことができるので、電極積層体の積み重ね時の電極板とセパレータとの位置ずれ等を防止することができる。ここで、九十九折りにした長尺状のセパレータを用いると、セパレータの折り曲げ部が一方の電極板を覆うことになり、製造工程において電解液を注入する際に電解液の含浸性が低下するという問題があるが、本発明においては、集電体の端部を封じるように被覆層が配置されていないので、端部側からも電解液を電極積層体に含浸することができる。したがって、電解液の電極積層体への含浸性を低下させることがなく、上記の防止機能を有する絶縁層を形成することができる。 By configuring in this way, the separator can be handled as a strip-shaped continuous body, so that it is possible to prevent positional deviation between the electrode plate and the separator when the electrode stack is stacked. Here, when a long and narrow separator is used, the bent portion of the separator covers one of the electrode plates, so that the electrolyte impregnation performance is reduced when the electrolyte is injected in the manufacturing process. However, in the present invention, since the coating layer is not disposed so as to seal the end portion of the current collector, the electrode laminate can be impregnated with the electrolyte from the end side. Therefore, the insulating layer having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate.
 本発明によれば、可撓性の外包部材を用いた蓄電デバイスにおいて、外包部材の損傷による短絡を防止するとともに、電解液の含浸性の向上によって生産性を向上させることが可能となる。 According to the present invention, in an electricity storage device using a flexible outer packaging member, it is possible to prevent a short circuit due to damage of the outer packaging member and to improve productivity by improving the impregnation property of the electrolytic solution.
本発明の蓄電デバイスの一つの実施の形態であるラミネート型リチウムイオン二次電池の一例を示す概略的な平面図である。BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1 is a schematic plan view showing an example of a laminated lithium ion secondary battery that is an embodiment of an electricity storage device of the present invention. 封止前のラミネート型リチウムイオン二次電池において図1のII-II線に沿った方向から見た断面を拡大して示す部分断面図である。FIG. 2 is a partial cross-sectional view showing, in an enlarged manner, a cross section viewed from a direction along line II-II in FIG. 1 in a laminated lithium ion secondary battery before sealing. 封止前のラミネート型リチウムイオン二次電池において図1のIII-III線に沿った方向から見た断面を拡大して示す部分断面図である。FIG. 3 is a partial cross-sectional view showing, in an enlarged manner, a cross section viewed from a direction along line III-III in FIG. 1 in a laminated lithium ion secondary battery before sealing. 本発明のラミネート型リチウムイオン二次電池の内部において、電極積層体の一つの実施の形態として、図1のIV-IV線に沿った方向から見た断面を拡大して示す部分断面図である。FIG. 4 is a partial cross-sectional view showing, in an enlarged manner, a cross section viewed from a direction along the line IV-IV in FIG. 1 as one embodiment of the electrode laminate in the laminated lithium ion secondary battery of the present invention. . 封止後のラミネート型リチウムイオン二次電池において図1のII-II線に沿った方向から見た断面を拡大して示す部分断面図である。FIG. 2 is a partial cross-sectional view showing, in an enlarged manner, a cross section viewed from a direction along line II-II in FIG. 1 in a laminated lithium ion secondary battery after sealing. 本発明の一つの実施の形態としてラミネート型リチウムイオン二次電池の内部において、負極接続端子と集電体との位置関係を模式的に示す平面図である。FIG. 3 is a plan view schematically showing a positional relationship between a negative electrode connection terminal and a current collector in a laminated lithium ion secondary battery as one embodiment of the present invention.
 以下、本発明の一つの実施の形態を図面に基づいて説明する。 Hereinafter, an embodiment of the present invention will be described with reference to the drawings.
 図1に示すように、ラミネート型リチウムイオン二次電池100は、電極積層体10と、矩形状を有し、電極積層体10を収容して封止する上下二枚の可撓性の外包部材20と、電極積層体10に電気的に接続されるとともに外包部材20の外周縁部から互いに対向する方向に導出された正極接続端子30および負極接続端子40とから構成される。なお、外包部材20の四方の外周縁部には熱溶着(ヒートシール)によって封着部21が形成されている。 As shown in FIG. 1, a laminate-type lithium ion secondary battery 100 includes an electrode laminate 10 and two upper and lower flexible outer packaging members that have a rectangular shape and accommodate and seal the electrode laminate 10. 20, and a positive electrode connection terminal 30 and a negative electrode connection terminal 40 which are electrically connected to the electrode laminate 10 and led out from the outer peripheral edge of the outer packaging member 20 in a direction facing each other. In addition, the sealing part 21 is formed in the outer periphery part of the four directions of the outer packaging member 20 by heat welding (heat sealing).
 図2と図4に示すように、電極積層体10は、複数の正極板11と、複数の負極板12と、正極板11と負極板12との間に介在するように配置されたセパレータ13と、図示しない非水電解液とを含む。複数の正極板11および複数の負極板12は短冊状を有し、セパレータ13は長尺状を有し、セパレータ13を九十九折り(ジグザグ状)にして、複数の正極板11および負極板12が交互に積層されている。また、セパレータ13の最外周は電極積層体10を包囲するように周回されている。なお、セパレータ13の外周の周回数は特に限定されない。負極板12は負極集電体121を含み、複数の負極板12の複数の負極集電体121を集積した端部を介して負極接続端子40に接続されている。図示されていないが、同様にして、正極板11は正極集電体を含み、複数の正極板11の複数の正極集電体を集積した端部を介して正極接続端子30(図1)に接続されている。 As shown in FIGS. 2 and 4, the electrode laminate 10 includes a plurality of positive plates 11, a plurality of negative plates 12, and a separator 13 disposed so as to be interposed between the positive plates 11 and the negative plates 12. And a non-aqueous electrolyte (not shown). The plurality of positive electrode plates 11 and the plurality of negative electrode plates 12 have a strip shape, the separator 13 has a long shape, and the separator 13 is formed into a ninety-nine fold (zigzag shape). 12 are alternately laminated. Further, the outermost periphery of the separator 13 is circulated so as to surround the electrode stack 10. Note that the number of rounds of the outer periphery of the separator 13 is not particularly limited. The negative electrode plate 12 includes a negative electrode current collector 121, and is connected to the negative electrode connection terminal 40 through an end portion where the plurality of negative electrode current collectors 121 of the plurality of negative electrode plates 12 are integrated. Although not shown, in the same manner, the positive electrode plate 11 includes a positive electrode current collector, and is connected to the positive electrode connection terminal 30 (FIG. 1) via an end portion where a plurality of positive electrode current collectors of the plurality of positive electrode plates 11 are integrated. It is connected.
 外包部材20は、電極積層体10に面する内面側に位置づけられ、合成樹脂からなる内面層と、ラミネート型リチウムイオン二次電池100の外表面に位置づけられ、合成樹脂からなる外面層と、内面層と外面層との間に配置される金属層とから構成される単一のフィルム、すなわち、三層構造のラミネートフィルムで形成されている(図2、図3では三層構造は省略している)。内面層は、一例として、ヒートシール可能な熱可塑性樹脂であるポリプロピレンからなり、厚みが30~120μmである。金属層は、一例として、アルミニウム箔またはアルミニウム合金箔からなり、厚みが30~50μmである。外面層は、一例として、ナイロン(登録商標)からなり、厚みが20~40μmである。このように構成された外包部材20は、容易に変形しやすい材料であり、可撓性を有する。なお、ラミネートフィルムは、少なくとも内面層とその外側に配置される金属層とを有するものであればよく、必要に応じて外面層を設ければよい。また、必要に応じて層間にウレタン樹脂等の接着層や他の合成樹脂層を設けてもよい。図1に示すように、外包部材20は、たとえば、2枚のラミネートフィルムの外周縁部を重ね合わせて熱溶着することによって、封着部21が四辺の外周縁部に形成される。なお、1枚のラミネートフィルムを二つ折りして折り曲げた辺以外の三方を熱溶着してもよい。 The outer packaging member 20 is positioned on the inner surface side facing the electrode laminate 10, and is positioned on the outer surface of the laminated lithium ion secondary battery 100, the inner surface layer made of synthetic resin, It is formed of a single film composed of a metal layer disposed between a layer and an outer surface layer, that is, a laminate film having a three-layer structure (the three-layer structure is omitted in FIGS. 2 and 3). ) For example, the inner surface layer is made of polypropylene which is a heat-sealable thermoplastic resin and has a thickness of 30 to 120 μm. For example, the metal layer is made of an aluminum foil or an aluminum alloy foil and has a thickness of 30 to 50 μm. For example, the outer surface layer is made of nylon (registered trademark) and has a thickness of 20 to 40 μm. The outer packaging member 20 configured in this manner is a material that is easily deformed and has flexibility. In addition, the laminate film should just have an inner surface layer and the metal layer arrange | positioned on the outer side at least, and should just provide an outer surface layer as needed. Moreover, you may provide adhesive layers, such as a urethane resin, and another synthetic resin layer between layers as needed. As shown in FIG. 1, in the outer packet member 20, for example, the outer peripheral edge portions of two laminate films are overlapped and heat-welded so that the sealing portion 21 is formed on the outer peripheral edge portions of the four sides. In addition, you may heat-weld three sides other than the side which folded and folded one laminated film.
 図3と図6に示すように、複数の負極集電体121の端部が負極接続端子40に重なる重複領域Pと、複数の負極集電体121の端部が負極接続端子40に重ならない非重複領域Qとが形成されている(図示されていないが、以下正極側も同様である)。重複領域Pが、複数の負極集電体121の端部と負極接続端子40との接続部121aと非接続部121bとを含む。接続部121aは、たとえば、超音波溶着によって形成され、非接続部121bを間に挟んで複数箇所、配置されている(図3では接続部121aが3箇所、非接続部121bが4箇所)。なお、接続部121aは抵抗溶接やレーザー溶接で形成されてもよい。 As shown in FIGS. 3 and 6, the overlapping region P where the ends of the plurality of negative electrode current collectors 121 overlap the negative electrode connection terminal 40 and the end portions of the plurality of negative electrode current collectors 121 do not overlap the negative electrode connection terminal 40. A non-overlapping region Q is formed (not shown, but the same applies to the positive electrode side hereinafter). The overlapping region P includes connection portions 121a and non-connection portions 121b between the end portions of the plurality of negative electrode current collectors 121 and the negative electrode connection terminals 40. The connection part 121a is formed by, for example, ultrasonic welding, and is arranged at a plurality of places with the non-connection part 121b interposed therebetween (in FIG. 3, three connection parts 121a and four non-connection parts 121b). The connecting portion 121a may be formed by resistance welding or laser welding.
 図2と図3に示すように、外包部材20の封止前においては、外包部材20の内面層の表面には、重複領域Pおよび非重複領域Qの少なくともいずれかの領域に対向するように被覆層50が予め形成されている。この実施形態では、図3と図6に示すように、重複領域Pおよび非重複領域Qに対向するように、すなわち、負極集電体121の端部全体Rに対向するように被覆層50が帯状に形成されている。なお、被覆層50を重複領域Pのみに形成する場合は、非重複領域Qには対向しないように間欠的に形成されている。重複領域Pの接続部121aのみに形成する場合は、接続部121a以外には対向しないように間欠的に形成されている。また、図2において被覆層50は負極接続端子40上の負極集電体121の端部を覆うように形成されているが、負極集電体121の負極接続端子40まで導出される部分(図2の湾曲している負極集電体121の部分)まで覆うように形成されていてもよい。また、この実施形態では、被覆層50として、ポリプロピレン、ポリイミドなどの熱可塑性樹脂からなる基材にシリコン系、アクリル系、ウレタン系の接着剤を両面に付着した絶縁テープが用いられ、絶縁テープが外包部材20の内面層の表面に貼り付けられている。 As shown in FIGS. 2 and 3, before sealing the outer packet member 20, the surface of the inner surface layer of the outer packet member 20 is opposed to at least one of the overlapping region P and the non-overlapping region Q. The covering layer 50 is formed in advance. In this embodiment, as shown in FIGS. 3 and 6, the covering layer 50 is disposed so as to face the overlapping region P and the non-overlapping region Q, that is, to face the entire end portion R of the negative electrode current collector 121. It is formed in a band shape. In addition, when forming the coating layer 50 only in the overlapping region P, it is formed intermittently so as not to face the non-overlapping region Q. When forming only in the connection part 121a of the duplication area | region P, it forms intermittently so that it may not oppose except the connection part 121a. Further, in FIG. 2, the coating layer 50 is formed so as to cover the end of the negative electrode current collector 121 on the negative electrode connection terminal 40, but the portion led to the negative electrode connection terminal 40 of the negative electrode current collector 121 (FIG. 2 of the curved negative electrode current collector 121) may be formed. In this embodiment, as the coating layer 50, an insulating tape is used in which a silicon-based, acrylic-based, or urethane-based adhesive is adhered to both sides of a base material made of a thermoplastic resin such as polypropylene or polyimide. It is affixed on the surface of the inner surface layer of the outer packaging member 20.
 ここで、製造工程において、電極積層体10が収容された外包部材20の内部に電解液を注入する工程および外包部材20を真空シール(真空封着)する工程について説明する。まず、外包部材20の外周縁部の三方(正極接続端子30および負極接続端子40の導出されている二辺と接続端子の導出されていない二辺のうちの一方)を封着し、残りの封着されていない外周縁部の他方(接続端子が導出されていない二辺のうちの他方)に形成された開口部を通じて外包部材20の内部に電解液を注入する。なお、開口部を形成する辺は四辺のいずれでも構わない。このとき、図2に示すように被覆層50は封着前の外包部材20の内面層に配置されており、両集電体の端部を封じるように配置されていないので、電解液を電極積層体10に十分に含浸させることができる。次に初充電を行い、発生したガスを排出した後、開口部を形成する辺を真空シールすることで、外包部材20の四方の外周縁部が熱溶着により封着される。このとき、図2の二点鎖線で示すように、外包部材20の内面層に形成された被覆層50が負極集電体121と密着して負極集電体121の端部全体を覆うように形成される。このようにして、図5に示すように電極積層体10が外包部材20内に真空封止される。 Here, in the manufacturing process, a step of injecting an electrolyte into the outer packaging member 20 in which the electrode laminate 10 is accommodated and a step of vacuum sealing (vacuum sealing) the outer packaging member 20 will be described. First, the three sides (one of the two sides from which the positive electrode connection terminal 30 and the negative electrode connection terminal 40 are led out and the two sides from which the connection terminal is not led out) of the outer peripheral edge of the outer packaging member 20 are sealed. The electrolytic solution is injected into the outer packet member 20 through an opening formed in the other of the outer peripheral edge portions that are not sealed (the other of the two sides from which the connection terminals are not led out). Note that the sides forming the opening may be any of the four sides. At this time, as shown in FIG. 2, the coating layer 50 is disposed on the inner surface layer of the outer packaging member 20 before sealing, and is not disposed so as to seal the ends of both current collectors. The laminate 10 can be sufficiently impregnated. Next, after the initial charge is performed and the generated gas is discharged, the outer periphery of the outer packaging member 20 is sealed by thermal welding by vacuum-sealing the sides forming the opening. At this time, as shown by a two-dot chain line in FIG. 2, the covering layer 50 formed on the inner surface layer of the outer packaging member 20 is in close contact with the negative electrode current collector 121 so as to cover the entire end of the negative electrode current collector 121. It is formed. In this way, the electrode laminate 10 is vacuum-sealed in the outer packaging member 20 as shown in FIG.
 以上のように構成された本発明のラミネート型リチウムイオン二次電池100においては、外包部材20の内面層には、重複領域Pおよび非重複領域Qの少なくともいずれかの領域を覆うように被覆層50が形成されているので、少なくとも正極集電体および負極集電体121のそれぞれの端部を覆うように被覆層50が形成されている。このため、集電体の端部、または、集電体の端部と正極接続端子30もしくは負極接続端子40との接続部121aが外包部材20に接触することによって外包部材20が損傷することを被覆層50によって防止することができる。これにより、正極集電体および負極集電体121のそれぞれの端部と外包部材20の金属層とが短絡することを防止することができる(防止機能)。 In the laminate type lithium ion secondary battery 100 of the present invention configured as described above, the inner layer of the outer packaging member 20 has a coating layer so as to cover at least one of the overlapping region P and the non-overlapping region Q. 50 is formed, the covering layer 50 is formed so as to cover at least the respective ends of the positive electrode current collector and the negative electrode current collector 121. For this reason, the outer packaging member 20 is damaged when the end portion of the current collector or the connecting portion 121a between the current collector end portion and the positive electrode connection terminal 30 or the negative electrode connection terminal 40 contacts the outer packaging member 20. This can be prevented by the covering layer 50. Thereby, it can prevent that each edge part of the positive electrode collector and the negative electrode collector 121 and the metal layer of the outer packaging member 20 short-circuit (prevention function).
 また、外包部材20の内面層は熱可塑性樹脂といった樹脂材料からなるので、予め被覆層50を外包部材20の内面層に容易に形成することができる。したがって、生産性を低下させることがなく、上記の防止機能を有する被覆層50を形成することができる。 Moreover, since the inner surface layer of the outer packaging member 20 is made of a resin material such as a thermoplastic resin, the coating layer 50 can be easily formed in advance on the inner surface layer of the outer packaging member 20. Therefore, the coating layer 50 having the above prevention function can be formed without reducing productivity.
 さらに、正極集電体および負極集電体121のそれぞれの端部の上に直接被覆層50を形成しないで、外包部材20の内面層に被覆層50を予め形成した後、電極積層体10を外包部材20に収納し、外包部材20の開口部より電解液を注入することができる。このため、電解液が注入される際には、集電体の端部を封じるように被覆層50が配置されていないので、電解液を電極積層体10に十分に含浸することができる。したがって、電解液の電極積層体10への含浸性を低下させることがなく、上記の防止機能を有する被覆層50を形成することができる。 Furthermore, without forming the coating layer 50 directly on the respective ends of the positive electrode current collector and the negative electrode current collector 121, the coating layer 50 is formed in advance on the inner surface layer of the outer packaging member 20, and then the electrode stack 10 is formed. The electrolytic solution can be injected from the opening of the outer packaging member 20 by being housed in the outer packaging member 20. For this reason, when the electrolytic solution is injected, since the coating layer 50 is not disposed so as to seal the end portion of the current collector, the electrode laminate 10 can be sufficiently impregnated with the electrolytic solution. Therefore, the coating layer 50 having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate 10.
 上記の実施形態では、本発明のラミネート型リチウムイオン二次電池100において、外包部材20の内面層には、重複領域Pおよび非重複領域Qを覆うように、すなわち、集電体の端部全体Rを覆うように被覆層50が形成されている。このように構成することにより、集電体の端部のいずれの箇所が外包部材20に接触しても、集電体の端部が外包部材20に接触することによって外包部材20が損傷することを被覆層50によって防止することができる。これにより、集電体の端部と外包部材20の金属層とが短絡することを防止することができる。 In the above embodiment, in the laminated lithium ion secondary battery 100 of the present invention, the inner surface layer of the outer packaging member 20 covers the overlapping region P and the non-overlapping region Q, that is, the entire end portion of the current collector. A covering layer 50 is formed so as to cover R. By comprising in this way, even if any location of the edge part of an electrical power collector contacts the outer packaging member 20, the outer packaging member 20 will be damaged because the edge part of an electrical power collector contacts the outer packaging member 20 Can be prevented by the coating layer 50. Thereby, it can prevent that the edge part of an electrical power collector and the metal layer of the outer packaging member 20 short-circuit.
 また、上記の実施形態では、本発明のラミネート型リチウムイオン二次電池100において、接続部121aが超音波溶着によって形成されているので、超音波溶着によって生じるバリ等が外包部材20に接触することによって外包部材20が損傷することを被覆層50によって防止することができる。これにより、超音波溶着によって生じるバリ等と外包部材20の金属層とが短絡することを防止することができる。 Further, in the above embodiment, in the laminated lithium ion secondary battery 100 of the present invention, since the connecting portion 121a is formed by ultrasonic welding, burrs or the like generated by ultrasonic welding are in contact with the outer packaging member 20. The outer cover member 20 can be prevented from being damaged by the covering layer 50. Thereby, it can prevent that the burr | flash etc. which arise by ultrasonic welding, and the metal layer of the outer packaging member 20 short-circuit.
 さらに、上記の実施形態では、本発明のラミネート型リチウムイオン二次電池100において、被覆層50がテープ材を含むことにより、外包部材20の内面層に特定的に配置された被覆層50を容易に形成する(貼り付ける)ことができる。したがって、生産性を低下させることがなく、上記の防止機能を有する被覆層50を形成することができる。 Furthermore, in the above embodiment, in the laminated lithium ion secondary battery 100 of the present invention, the covering layer 50 includes the tape material, so that the covering layer 50 specifically disposed on the inner surface layer of the outer packaging member 20 can be easily formed. Can be formed (pasted). Therefore, the coating layer 50 having the above prevention function can be formed without reducing productivity.
 上記の実施形態では、本発明のラミネート型リチウムイオン二次電池100において、被覆層50がテープ材を含むように構成されているが、被覆層50が熱可塑性樹脂を塗布して形成してなるようにしてもよい。このように構成することにより、正極集電体および負極集電体121のそれぞれの端部と正極接続端子30および負極接続端子40のそれぞれとが重なる重複領域Pのみを覆うように、さらには重複領域Pの接続部121aのみを覆うように、熱可塑性樹脂を間欠的に塗布することによって被覆層50を形成することができる。また、外包部材20の熱溶着時の温度で被覆層50が再溶融すれば、外包部材20と電極積層体10との一体化が可能である。 In the above embodiment, in the laminated lithium ion secondary battery 100 of the present invention, the coating layer 50 is configured to include a tape material, but the coating layer 50 is formed by applying a thermoplastic resin. You may do it. By being configured in this manner, the overlapping is further performed so as to cover only the overlapping region P where the respective ends of the positive electrode current collector and the negative electrode current collector 121 overlap with each of the positive electrode connection terminal 30 and the negative electrode connection terminal 40. The coating layer 50 can be formed by intermittently applying a thermoplastic resin so as to cover only the connection portion 121a in the region P. Moreover, if the coating layer 50 is remelted at the temperature at which the outer packaging member 20 is thermally welded, the outer packaging member 20 and the electrode laminate 10 can be integrated.
 なお、被覆層50は上述の防止機能を果たす限り、絶縁層、導電層、導電性樹脂のいずれであってもかまわない。 The covering layer 50 may be any of an insulating layer, a conductive layer, and a conductive resin as long as it performs the above-described prevention function.
 また、上記の実施形態では、本発明のラミネート型リチウムイオン二次電池100において、電極積層体10は、九十九折りにした長尺状のセパレータ13を介在して、複数の正極板11と複数の負極板12とを交互に積層させることにより形成されている。このように構成することにより、セパレータ13を帯状の連続体で取り扱うことができるので、電極積層体10の積み重ね時の電極板とセパレータ13との位置ずれ等を防止することができる。ここで、九十九折りにした長尺状のセパレータ13を用いると、セパレータ13の折り曲げ部が一方の電極板を覆うことになり、製造工程において電解液を注入する際に電解液の含浸性が低下するという問題があるが、本発明においては、集電体の端部を封じるように被覆層50が配置されていないので、端部側からも電解液を電極積層体10に含浸することができる。したがって、電解液の電極積層体10への含浸性を低下させることがなく、上記の防止機能を有する被覆層50を形成することができる。 Further, in the above embodiment, in the laminated lithium ion secondary battery 100 of the present invention, the electrode laminate 10 includes a plurality of positive electrode plates 11 with the long separator 13 folded in ninety-nine folds. It is formed by alternately laminating a plurality of negative electrode plates 12. By configuring in this way, the separator 13 can be handled as a belt-like continuous body, so that it is possible to prevent positional deviation between the electrode plate and the separator 13 when the electrode laminate 10 is stacked. Here, when the long separator 13 having a ninety-nine fold shape is used, the bent portion of the separator 13 covers one of the electrode plates, so that the electrolyte solution is impregnated when the electrolyte solution is injected in the manufacturing process. In the present invention, since the coating layer 50 is not disposed so as to seal the end portion of the current collector, the electrode laminate 10 is impregnated with the electrolyte from the end side. Can do. Therefore, the coating layer 50 having the above-described prevention function can be formed without reducing the impregnation property of the electrolytic solution into the electrode laminate 10.
 上記の実施形態では、図2と図6に示されるように、負極接続端子40は、集電体の端部が集積された箇所の下面にて超音波溶着により接続されるが、負極接続端子40は、集電体が集積された箇所の上面にて超音波溶着により接続されてもよく、あるいは、集電体が集積された箇所の内部に挿入されるように配置して超音波溶着により接続されてもよい(正極側も同様)。 In the above embodiment, as shown in FIGS. 2 and 6, the negative electrode connection terminal 40 is connected by ultrasonic welding on the lower surface of the portion where the ends of the current collector are integrated, but the negative electrode connection terminal 40 may be connected by ultrasonic welding on the upper surface of the location where the current collector is integrated, or arranged so as to be inserted into the location where the current collector is integrated, and by ultrasonic welding. They may be connected (the same applies to the positive electrode side).
 なお、上記のラミネート型リチウムイオン二次電池100の例では、電極積層体10の構成として正極板11と負極板12との間に一枚のセパレータ13を介在させているが、複数枚のセパレータを介在させてもよい。複数枚のセパレータの材質は同種でも異種でもよい。また、正極板と負極板との間に短冊状のセパレータを介在させてもよい。セパレータの材質としては、ポリプロピレン、ポリエチレンなどのポリオレフィン系樹脂の単独またはその組み合わせや、ポリオレフィン系樹脂にシリカやアルミナなどのセラミックを添加したものや、ポリエチレンテレフタレートや、セルロース、不織布等が用いられる。 In the example of the laminate-type lithium ion secondary battery 100 described above, one separator 13 is interposed between the positive electrode plate 11 and the negative electrode plate 12 as a configuration of the electrode laminate 10. May be interposed. The material of the plurality of separators may be the same or different. Further, a strip-shaped separator may be interposed between the positive electrode plate and the negative electrode plate. As the material of the separator, polyolefin resins such as polypropylene and polyethylene, or a combination thereof, those obtained by adding ceramics such as silica and alumina to polyolefin resins, polyethylene terephthalate, cellulose, nonwoven fabric, and the like are used.
 正極板11は、正極接続端子30に接続される側の端部を除いて、正極活物質を含む正極合材層が正極集電体の両面上に形成されることによって構成される。負極板12は、負極接続端子40に接続される側の端部を除いて、負極活物質を含む負極合材層が負極集電体の両面上に形成されることによって構成される。 The positive electrode plate 11 is configured by forming a positive electrode mixture layer containing a positive electrode active material on both surfaces of the positive electrode current collector, except for an end portion on the side connected to the positive electrode connection terminal 30. The negative electrode plate 12 is configured by forming a negative electrode mixture layer containing a negative electrode active material on both surfaces of the negative electrode current collector, except for an end portion on the side connected to the negative electrode connection terminal 40.
 たとえば、正極板11は、正極活物質と結着剤と必要に応じて導電助剤とを有機溶媒中で混錬してなる正極スラリーを、アルミニウム箔からなる正極集電体の両面上に均一に塗布し、乾燥して、正極合材層を正極集電体の両面上に形成することにより作製される。 For example, the positive electrode plate 11 has a positive electrode slurry obtained by kneading a positive electrode active material, a binder, and optionally a conductive additive in an organic solvent, on both surfaces of a positive electrode current collector made of aluminum foil. It is produced by applying to the substrate and drying to form a positive electrode mixture layer on both surfaces of the positive electrode current collector.
 一般的に正極活物質としては、目的とする電池の種類に応じて金属酸化物、金属硫化物または特定の高分子を用いることができる。 Generally, as the positive electrode active material, a metal oxide, a metal sulfide, or a specific polymer can be used depending on the type of the target battery.
 リチウムイオン二次電池を構成する場合、正極活物質としては、TiS、MoS、NbSe、V等の金属硫化物または酸化物を使用することができる。また、リチウムイオン二次電池の正極活物質としてLiM(化学式中、Mは一種以上の遷移金属を表し、xは電池の充放電状態によって異なり、通常0.05以上、1.10以下である)を主体とするリチウム複合酸化物等を使用することができる。このリチウム複合酸化物を構成する遷移金属Mとしては、Co、Ni、Mn等が好ましい。このようなリチウム複合酸化物の具体例としてはLiCoO、LiNiO、LiNiCo1-y(化学式中、0<y<1である)、Li1+a(NiCoMn)O2-b(化学式中、-0.1<a<0.2、x+y+z=1、-0.1<b<0.1)、LiMn等を挙げることができる。これらのリチウム複合酸化物は、高電圧を発生でき、エネルギー密度が優れた正極活物質となる。正極板11を作製するために、これらの正極活物質の複数種をあわせて使用してもよい。 When a lithium ion secondary battery is configured, a metal sulfide or oxide such as TiS 2 , MoS 2 , NbSe 2 , or V 2 O 5 can be used as the positive electrode active material. In addition, LiM x O 2 (in the chemical formula, M represents one or more transition metals, x varies depending on the charge / discharge state of the battery, and is usually 0.05 or more and 1.10 or less as a positive electrode active material of the lithium ion secondary battery. Lithium composite oxide mainly composed of As the transition metal M constituting this lithium composite oxide, Co, Ni, Mn and the like are preferable. Specific examples of such a lithium composite oxide include LiCoO 2 , LiNiO 2 , LiNi y Co 1-y O 2 (where 0 <y <1), and Li 1 + a (Ni x Co y Mn z ) O. 2-b (in the chemical formula, −0.1 <a <0.2, x + y + z = 1, −0.1 <b <0.1), LiMn 2 O 4 and the like. These lithium composite oxides can generate a high voltage and become a positive electrode active material having an excellent energy density. In order to produce the positive electrode plate 11, a plurality of these positive electrode active materials may be used in combination.
 また、上記の正極合材に含有される結着剤としては、通常、リチウムイオン二次電池の正極合材に用いられている公知の結着剤を用いることができ、上記の正極合材には、導電助剤や酸化物等、公知の添加剤を添加することができる。 Moreover, as a binder contained in said positive electrode compound material, the well-known binder currently normally used for the positive electrode compound material of a lithium ion secondary battery can be used, and said positive electrode compound material is used. Can be added with known additives such as a conductive additive and an oxide.
 たとえば、負極板12は、負極活物質と結着剤と必要に応じて導電助剤とを有機溶媒中で混錬してなる負極スラリーを、銅箔またはアルミニウム箔からなる負極集電体の両面上に均一に塗布し、乾燥して、負極合材層を負極集電体の両面上に形成することにより作製される。 For example, the negative electrode plate 12 is made of a negative electrode slurry formed by kneading a negative electrode active material, a binder, and optionally a conductive additive in an organic solvent, on both sides of a negative electrode current collector made of copper foil or aluminum foil. It is produced by coating uniformly on the top and drying to form a negative electrode mixture layer on both sides of the negative electrode current collector.
 リチウムイオン二次電池を構成する場合、負極活物質としては、難黒鉛化炭素系材料やグラファイト系材料等の炭素材料を使用することができる。具体的には、熱分解炭素類、コークス類、黒鉛類、ガラス状炭素繊維、有機高分子化合物焼成体、炭素繊維、活性炭等の炭素材料を使用することができる。上記のコークス類には、ピッチコークス、ニードルコークス、石油コークス等がある。また、上記の有機高分子化合物焼成体とは、フェノール樹脂、フラン樹脂等を適当な温度で焼成して炭素化したものをいう。上述した炭素材料のほか、リチウムをドープ、脱ドープできる材料としては、ポリアセチレン、ポリピロール等の高分子や、SnO等のSn酸化物系や、SnCu等のSn合金系や、SiMg等のSi合金系や、LiTi12(チタン酸リチウム)等の酸化物を使用することもできる。 When a lithium ion secondary battery is configured, a carbon material such as a non-graphitizable carbon material or a graphite material can be used as the negative electrode active material. Specifically, carbon materials such as pyrolytic carbons, cokes, graphites, glassy carbon fibers, organic polymer compound fired bodies, carbon fibers, and activated carbon can be used. Examples of the cokes include pitch coke, needle coke, and petroleum coke. Moreover, said organic polymer compound fired body means what carbonized by baking a phenol resin, furan resin, etc. at a suitable temperature. In addition to the carbon material described above, materials that can be doped and dedoped with lithium include polymers such as polyacetylene and polypyrrole, Sn oxides such as SnO 2 , Sn alloys such as Sn 5 Cu 6 , and SiMg 2. Si alloy system such as Li 4 Ti 5 O 12 (lithium titanate) can also be used.
 また、上記の負極合材に含有される結着剤としては、通常、リチウムイオン二次電池の負極合材に用いられている公知の結着剤を用いることができ、上記の負極合材には、導電助剤や酸化物等、公知の添加剤を添加することができる。 Moreover, as a binder contained in said negative electrode compound material, the well-known binder currently normally used for the negative electrode compound material of a lithium ion secondary battery can be used, and said negative electrode compound material is used. Can be added with known additives such as a conductive additive and an oxide.
 非水電解液は、電解質を非水溶媒に溶解して調製される。電解質としては、たとえば、非水溶媒中にLiPFを1.0mol/Lの濃度で溶解したものが使用される。LiPF以外の電解質としては、LiBF、LiAsF、LiClO、LiCFSO、LiN(SOCF、LiC(SOCF、LiAlCl、LiSiF等のリチウム塩を挙げることができる。これらの中でも、電解質として特にLiPF、LiBFを用いることが酸化安定性の点から望ましい。このような電解質は、非水溶媒中に、0.1mol/L~3.0mol/Lの濃度で溶解されて用いられることが好ましく、0.5mol/L~2.0mol/Lの濃度で溶解されて用いられることがさらに好ましい。非水溶媒としては、たとえば、炭酸プロピレンと炭酸エチレンと炭酸ジエチルとを体積比で5~20:20~30:60~70の割合で混合したものが使用される。その他の非水溶媒としては、炭酸プロピレン、炭酸エチレン等の環状炭酸エステル;炭酸ジエチル、炭酸ジメチル等の鎖状炭酸エステル;プロピオン酸メチル、酪酸メチル等のカルボン酸エステル;γ-ブチルラクトン、スルホラン、2-メチルテトラヒドロフラン、ジメトキシエタン等のエーテル類等を使用することができる。これらの非水溶媒は単独で使用してもよく、複数種を混合して使用してもよい。これらの中でも、非水溶媒として特に炭酸エステルを用いることが酸化安定性の点から好ましい。 The nonaqueous electrolytic solution is prepared by dissolving an electrolyte in a nonaqueous solvent. As the electrolyte, for example, a solution obtained by dissolving LiPF 6 at a concentration of 1.0 mol / L in a non-aqueous solvent is used. As an electrolyte other than LiPF 6 , lithium salts such as LiBF 4 , LiAsF 6 , LiClO 4 , LiCF 3 SO 3 , LiN (SO 2 CF 3 ) 2 , LiC (SO 2 CF 3 ) 3 , LiAlCl 4 , LiSiF 6 are used. Can be mentioned. Among these, it is desirable from the viewpoint of oxidation stability that LiPF 6 or LiBF 4 is particularly used as the electrolyte. Such an electrolyte is preferably used by being dissolved in a non-aqueous solvent at a concentration of 0.1 mol / L to 3.0 mol / L, and is preferably dissolved at a concentration of 0.5 mol / L to 2.0 mol / L. More preferably, it is used. As the non-aqueous solvent, for example, a mixture of propylene carbonate, ethylene carbonate and diethyl carbonate in a volume ratio of 5 to 20:20 to 30:60 to 70 is used. Other non-aqueous solvents include: cyclic carbonates such as propylene carbonate and ethylene carbonate; chain carbonates such as diethyl carbonate and dimethyl carbonate; carboxylic acid esters such as methyl propionate and methyl butyrate; γ-butyllactone, sulfolane, Ethers such as 2-methyltetrahydrofuran and dimethoxyethane can be used. These non-aqueous solvents may be used alone or in combination of two or more. Among these, it is preferable from the point of oxidation stability to use carbonate ester as a non-aqueous solvent.
 上記の実施の形態では、本発明を蓄電デバイスの一例としてリチウムイオン二次電池100に適用した例について説明したが、少なくとも電極積層体を収容するために可撓性の外包部材を用いた蓄電デバイスであれば、本発明を適用することができ、たとえば、リチウムイオン二次電池の他に、リチウム二次電池、ポリマー二次電池、電気二重層キャパシタなどに本発明を適用することができる。 In the above embodiment, the example in which the present invention is applied to the lithium ion secondary battery 100 as an example of an electricity storage device has been described. However, an electricity storage device using a flexible outer packaging member to accommodate at least the electrode stack. If so, the present invention can be applied. For example, in addition to a lithium ion secondary battery, the present invention can be applied to a lithium secondary battery, a polymer secondary battery, an electric double layer capacitor, and the like.
 今回開示された実施の形態はすべての点で例示であって制限的なものではないと考慮されるべきである。本発明の範囲は以上の実施の形態ではなく、請求の範囲によって示され、請求の範囲と均等の意味および範囲内でのすべての修正と変形を含むものであることが意図される。 The embodiment disclosed this time should be considered as illustrative in all points and not restrictive. The scope of the present invention is shown not by the above embodiment but by the scope of claims, and is intended to include all modifications and variations within the meaning and scope equivalent to the scope of claims.
 本発明の蓄電デバイスは、可撓性を有する外包部材を用いて蓄電要素を収容する蓄電デバイスにおいて、外包部材の損傷による短絡を防止するとともに、電解液の含浸性の向上によって生産性を向上させるものであるから、可撓性を有する外包部材が使用可能な蓄電デバイス、例えば、蓄電要素としてリチウムイオン二次電池の他に、リチウム二次電池、ポリマー二次電池、有機ラジカル電池、全固体電池、電気二重層キャパシタ等の種々の蓄電要素を収容する蓄電デバイスの生産性向上に寄与するものである。 The electricity storage device of the present invention, in an electricity storage device that houses an electricity storage element using a flexible outer packaging member, prevents a short circuit due to damage to the outer packaging member, and improves productivity by improving the impregnation property of the electrolytic solution. Therefore, an electricity storage device in which a flexible outer packaging member can be used, for example, a lithium secondary battery, a polymer secondary battery, an organic radical battery, an all solid state battery in addition to a lithium ion secondary battery as an electricity storage element This contributes to improving the productivity of an electricity storage device that accommodates various electricity storage elements such as electric double layer capacitors.
 10:電極積層体、11:正極板、12:負極板、13:セパレータ、20:外包部材、50:被覆層、100:ラミネート型リチウムイオン二次電池、121:負極集電体、121a:接続部、121b:非接続部、P:重複領域、Q:非重複領域。
 
DESCRIPTION OF SYMBOLS 10: Electrode laminated body, 11: Positive electrode plate, 12: Negative electrode plate, 13: Separator, 20: Outer packaging member, 50: Coating layer, 100: Laminate type lithium ion secondary battery, 121: Negative electrode collector, 121a: Connection Part, 121b: non-connection part, P: overlapping area, Q: non-overlapping area.

Claims (12)

  1.  セパレータを介在して複数の正極板と複数の負極板とを交互に積層させることにより形成された電極積層体と、
     少なくとも熱可塑性樹脂からなる内面層と、前記内面層の外側に配置される金属層とを有し、前記電極積層体を収容する可撓性の外包部材と、
     前記複数の正極板の正極集電体および前記複数の負極板の負極集電体のそれぞれの端部に電気的に接続されるとともに、前記外包部材の外周縁部から導出された正極接続端子および負極接続端子とを備え、
     前記正極集電体および前記負極集電体のそれぞれの端部と前記正極接続端子および前記負極接続端子のそれぞれとが重なる重複領域と、重ならない非重複領域とが形成され、
     前記重複領域が、前記正極集電体および前記負極集電体のそれぞれの端部と前記正極接続端子および前記負極接続端子のそれぞれとの接続部を含み、
     前記外包部材の内面層には、前記重複領域および前記非重複領域の少なくともいずれかの領域を覆うように被覆層が形成されている、蓄電デバイス。
    An electrode laminate formed by alternately laminating a plurality of positive electrode plates and a plurality of negative electrode plates with a separator interposed therebetween;
    A flexible outer packaging member that has an inner surface layer made of at least a thermoplastic resin and a metal layer disposed outside the inner surface layer and accommodates the electrode laminate;
    A positive electrode connection terminal electrically connected to each end of the positive electrode current collector of the plurality of positive electrode plates and a negative electrode current collector of the plurality of negative electrode plates; A negative connection terminal,
    An overlapping region where each of the positive electrode current collector and the negative electrode current collector overlaps with each of the positive electrode connection terminal and the negative electrode connection terminal, and a non-overlapping region which does not overlap, are formed,
    The overlapping region includes a connection portion between each end portion of the positive electrode current collector and the negative electrode current collector and each of the positive electrode connection terminal and the negative electrode connection terminal;
    The electricity storage device, wherein a coating layer is formed on an inner surface layer of the outer packaging member so as to cover at least one of the overlapping region and the non-overlapping region.
  2.  前記外包部材の内面層には、前記重複領域および前記非重複領域を覆うように前記被覆層が形成されている、請求項1に記載の蓄電デバイス。 The electricity storage device according to claim 1, wherein the coating layer is formed on an inner surface layer of the outer packaging member so as to cover the overlapping region and the non-overlapping region.
  3.  前記接続部は、超音波溶着によって形成されている、請求項1または請求項2に記載の蓄電デバイス。 The electric storage device according to claim 1 or 2, wherein the connection portion is formed by ultrasonic welding.
  4.  前記被覆層がテープ材を含む、請求項1から請求項3までのいずれか1項に記載の蓄電デバイス。 The electric storage device according to any one of claims 1 to 3, wherein the coating layer includes a tape material.
  5.  前記被覆層が熱可塑性樹脂を塗布して形成してなる、請求項1から請求項4までのいずれか1項に記載の蓄電デバイス。 The electricity storage device according to any one of claims 1 to 4, wherein the coating layer is formed by applying a thermoplastic resin.
  6.  前記電極積層体は、九十九折りにした長尺状のセパレータを介在して、前記複数の正極板と前記複数の負極板とを交互に積層させることにより形成されている、請求項1から請求項5までのいずれか1項に記載の蓄電デバイス。 The electrode laminate is formed by alternately laminating the plurality of positive plates and the plurality of negative plates with a long separator folded into ninety-nine folds. The electricity storage device according to any one of claims 5 to 6.
  7.  セパレータを介在して複数の正極板と複数の負極板とを交互に積層させることにより形成された電極積層体と、少なくとも熱可塑性樹脂からなる内面層と、前記内面層の外側に配置される金属層とを有し、前記電極積層体を収容する可撓性の外包部材と、前記複数の正極板の正極集電体および前記複数の負極板の負極集電体のそれぞれの端部に電気的に接続されるとともに、前記外包部材の外周縁部から導出された正極接続端子および負極接続端子とを備え、前記正極集電体および前記負極集電体のそれぞれの端部と前記正極接続端子および前記負極接続端子のそれぞれとが重なる重複領域と、重ならない非重複領域とが形成され、前記重複領域が、前記正極集電体および前記負極集電体のそれぞれの端部と前記正極接続端子および前記負極接続端子のそれぞれとの接続部を含む蓄電デバイスの製造方法であって、
     前記外包部材の内面層に、前記重複領域および前記非重複領域の少なくともいずれかの領域を覆うように被覆層を予め形成する、蓄電デバイスの製造方法。
    An electrode laminate formed by alternately laminating a plurality of positive plates and a plurality of negative plates with a separator interposed therebetween, an inner surface layer made of at least a thermoplastic resin, and a metal disposed outside the inner surface layer A flexible outer packaging member that accommodates the electrode laminate, and electrically connected to respective ends of the positive electrode current collector of the plurality of positive electrode plates and the negative electrode current collector of the plurality of negative electrode plates And a positive electrode connection terminal and a negative electrode connection terminal led out from the outer peripheral edge of the outer packaging member, and each end of the positive electrode current collector and the negative electrode current collector, the positive electrode connection terminal, and An overlapping region that overlaps with each of the negative electrode connection terminals and a non-overlapping region that does not overlap with each other are formed, and the overlapping regions include the respective ends of the positive electrode current collector and the negative electrode current collector, the positive electrode connection terminals, and Negative electrode A method of manufacturing a power storage device including a connecting portion between each of the connection terminals,
    A method for manufacturing an electricity storage device, wherein a covering layer is formed in advance on an inner surface layer of the outer packaging member so as to cover at least one of the overlapping region and the non-overlapping region.
  8.  前記外包部材の内面層には、前記重複領域および前記非重複領域を覆うように前記被覆層を予め形成する、請求項7に記載の蓄電デバイスの製造方法。 The method for manufacturing an electricity storage device according to claim 7, wherein the covering layer is formed in advance on the inner surface layer of the outer packaging member so as to cover the overlapping region and the non-overlapping region.
  9.  前記接続部は、超音波溶着によって形成されている、請求項7または請求項8に記載の蓄電デバイスの製造方法。 The method for manufacturing an electricity storage device according to claim 7 or 8, wherein the connection portion is formed by ultrasonic welding.
  10.  前記被覆層が絶縁テープを含む、請求項7から請求項9までのいずれか1項に記載の蓄電デバイスの製造方法。 The method for manufacturing an electricity storage device according to any one of claims 7 to 9, wherein the coating layer includes an insulating tape.
  11.  前記被覆層が熱可塑性樹脂を塗布して形成してなる、請求項7から請求項10までのいずれか1項に記載の蓄電デバイスの製造方法。 The method for manufacturing an electricity storage device according to any one of claims 7 to 10, wherein the coating layer is formed by applying a thermoplastic resin.
  12.  前記電極積層体は、九十九折りにした長尺状のセパレータを介在して、前記複数の正極板と前記複数の負極板とを交互に積層させることにより形成されている、請求項7から請求項11までのいずれか1項に記載の蓄電デバイスの製造方法。
     
    The electrode laminate is formed by alternately laminating the plurality of positive plates and the plurality of negative plates with a ninety-fold folded long separator interposed therebetween. The manufacturing method of the electrical storage device of any one of Claim 11.
PCT/JP2010/071074 2009-12-07 2010-11-26 Electrical storage device and method for manufacturing same WO2011070918A1 (en)

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JP2019179673A (en) * 2018-03-30 2019-10-17 株式会社エンビジョンAescエナジーデバイス Electrochemical device and manufacturing method thereof
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