WO2021145344A1 - 非水電解質二次電池、集電体、及び非水電解質二次電池の製造方法 - Google Patents

非水電解質二次電池、集電体、及び非水電解質二次電池の製造方法 Download PDF

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Publication number
WO2021145344A1
WO2021145344A1 PCT/JP2021/000882 JP2021000882W WO2021145344A1 WO 2021145344 A1 WO2021145344 A1 WO 2021145344A1 JP 2021000882 W JP2021000882 W JP 2021000882W WO 2021145344 A1 WO2021145344 A1 WO 2021145344A1
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WIPO (PCT)
Prior art keywords
current collector
layer
negative electrode
secondary battery
electrolyte secondary
Prior art date
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Ceased
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PCT/JP2021/000882
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English (en)
French (fr)
Japanese (ja)
Inventor
高央 溝口
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Fujifilm Corp
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Fujifilm Corp
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Application filed by Fujifilm Corp filed Critical Fujifilm Corp
Priority to EP21741905.0A priority Critical patent/EP4092788A4/en
Priority to JP2021571209A priority patent/JPWO2021145344A1/ja
Priority to KR1020227021036A priority patent/KR20220104781A/ko
Priority to CN202180007255.9A priority patent/CN114830383A/zh
Publication of WO2021145344A1 publication Critical patent/WO2021145344A1/ja
Priority to US17/857,048 priority patent/US12418030B2/en
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/665—Composites
    • H01M4/667—Composites in the form of layers, e.g. coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/661—Metal or alloys, e.g. alloy coatings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/663—Selection of materials containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/021—Physical characteristics, e.g. porosity, surface area
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/027—Negative electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/028—Positive electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/029—Bipolar electrodes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a non-aqueous electrolyte secondary battery, a current collector, and a method for manufacturing a non-aqueous electrolyte secondary battery.
  • Non-aqueous electrolyte secondary batteries represented by lithium ion secondary batteries have high energy density, excellent storage performance, low temperature operability, etc., and are widely used in portable electronic devices such as mobile phones and laptop computers. ..
  • the size of batteries has been increased so that they can be used in transportation equipment such as automobiles, and they are also being used as storage devices for nighttime electric power and electric power generated by natural energy power generation.
  • Patent Document 1 In order to increase the energy density of a lithium ion secondary battery, it has been proposed to use a hard polymer film having metal films formed on both sides as a current collector (Patent Document 1). According to the technique described in Patent Document 1, the battery life can be increased by 10% to 99% by adjusting the thickness of the metal film formed on the hard polymer film.
  • Patent Document 2 describes a lithium ion secondary battery using a current collector having a multi-layer structure.
  • a current collector in which metal layers are formed on both sides of the low melting point resin film, the low melting point resin film melts when abnormal heat generation occurs, and the electrode is damaged. It is said that the generated current is cut, the temperature rise inside the battery is suppressed, and ignition is prevented.
  • the energy density of the lithium ion secondary battery can be increased by using a current collector having metal layers on both sides of the resin film as the current collector of the lithium ion secondary battery. It is said that it can be enhanced and safety can be enhanced.
  • a current collector having metal layers on both sides of the resin film as the current collector of the lithium ion secondary battery. It is said that it can be enhanced and safety can be enhanced.
  • an oxide film is formed on the surface of the metal layer constituting the current collector, or a side reaction between the metal layer and the electrolyte occurs, and these phenomena occur in the metal layer. It causes a decrease in adhesion or electron conductivity between the electrode active material layer and the electrode active material layer. Therefore, there is room for further improvement in improving battery life (cycle characteristics).
  • An object of the present invention is to provide a non-aqueous electrolyte secondary battery having excellent cycle characteristics and excellent safety. Another object of the present invention is to provide a current collector suitable for use in the non-aqueous electrolyte secondary battery and a method for producing the non-aqueous electrolyte secondary battery.
  • the present inventors have made extensive studies in view of the above problems.
  • the non-aqueous electrolyte secondary battery obtained by using a resin film as a support and a laminated body having a laminated structure of a conductive layer and a contact resistance reducing layer formed on one side thereof as a current collector has a cycle characteristic. It was found that it is sufficiently enhanced, and that it is less likely to ignite or smoke when an internal short circuit occurs, and that it is also excellent in safety. Based on these findings, the present invention has been further studied and completed.
  • a non-aqueous electrolyte secondary battery having a separator arranged in the. At least one of the positive electrode current collector and the negative electrode current collector With resin film A non-aqueous electrolyte secondary battery which is a laminated body having a laminated structure of a conductive layer and a contact resistance reducing layer arranged on one side or both sides of the resin film.
  • the positive electrode current collector is composed of the laminated body
  • the conductive layer of the laminated body is in contact with the resin film
  • the contact resistance reducing layer of the laminated body is in contact with the positive electrode active material layer.
  • the negative electrode current collector is composed of the laminated body
  • the conductive layer of the laminated body is in contact with the resin film
  • the contact resistance reducing layer of the laminated body is in contact with the negative electrode active material layer [1].
  • the positive electrode current collector is composed of the laminated body
  • the conductive layer of the laminated body contains aluminum
  • the contact resistance reducing layer of the laminated body contains conductive carbon, [1] or [2].
  • the conductive layer of the laminate contains at least one of copper and nickel, and the contact resistance reducing layer of the laminate is conductive carbon, nickel, and titanium.
  • At least one of the positive electrode current collector and the negative electrode current collector is a laminate having a resin film and a conductive layer arranged on one side of the resin film, and the surface roughness of at least one surface of the conductive layer is rough.
  • the resin film contains at least one of a polyester resin and a polyolefin resin.
  • a current collector having a laminated structure of a conductive layer and a contact resistance reducing layer arranged on one side or both sides of the resin film.
  • the current collector is a negative electrode current collector, the conductive layer contains at least one of copper and nickel, and the contact resistance reducing layer contains at least one of conductive carbon, nickel, titanium, tantalum and tungsten.
  • a non-aqueous electrolyte comprising arranging the current collector according to any one of [13] to [23] as at least one of a positive electrode current collector, a negative electrode current collector, and a bipolar current collector. How to manufacture a secondary battery.
  • a positive electrode having a positive electrode current collector and a positive electrode active material layer in contact with the positive electrode current collector, a negative electrode having a negative electrode current collector and a negative electrode active material layer in contact with the negative electrode current collector, and a bipolar current collector and the bipolar current collector. It has a bipolar electrode having a positive electrode active material layer in contact with one side of the bipolar current collector and a negative electrode active material layer in contact with the other surface, the positive electrode is on the negative electrode active material layer side of the bipolar electrode, and the negative electrode is on the negative electrode active material layer side.
  • a non-aqueous electrolyte secondary battery having a structure in which a separator is sandwiched between the positive electrode active material layers of the bipolar electrode.
  • a non-aqueous electrolyte secondary battery which is a laminated body having a laminated structure of a conductive layer and a contact resistance reducing layer arranged on one side or both sides of the resin film.
  • the numerical range represented by using “-” means a range including the numerical values before and after "-" as the lower limit value and the upper limit value.
  • the “non-aqueous electrolyte” means an electrolyte that is substantially free of water. That is, the “non-aqueous electrolyte” may contain a small amount of water as long as it does not interfere with the effects of the present invention.
  • the “non-aqueous electrolyte” has a water concentration of 200 ppm (mass basis) or less, preferably 100 ppm or less, and more preferably 20 ppm or less.
  • the non-aqueous electrolyte in the present invention includes a non-aqueous electrolyte solution having ionic conductivity such as lithium ion, a solid electrolyte, and the like.
  • the "non-aqueous electrolyte secondary battery” broadly includes a secondary battery using a non-aqueous electrolyte.
  • the non-aqueous electrolyte secondary battery of the present invention has excellent cycle characteristics and safety. Further, the current collector of the present invention is suitable as a current collector of the non-aqueous electrolyte secondary battery of the present invention. Further, according to the method for producing a non-aqueous electrolyte secondary battery of the present invention, it is possible to obtain a non-aqueous electrolyte secondary battery having excellent cycle characteristics and excellent safety.
  • FIG. 1 is a vertical cross-sectional view schematically showing a basic laminated structure of a sheet-type non-aqueous electrolyte secondary battery.
  • FIG. 2 is a vertical cross-sectional view schematically showing an embodiment of a laminated structure of a current collector of the present invention.
  • FIG. 3 is a vertical cross-sectional view schematically showing a basic laminated structure of a monopolar non-aqueous electrolyte secondary battery.
  • FIG. 4 is a vertical cross-sectional view schematically showing a basic laminated structure of a monopolar non-aqueous electrolyte secondary battery.
  • FIG. 5 is a vertical cross-sectional view schematically showing a basic laminated structure of a bipolar non-aqueous electrolyte secondary battery.
  • FIG. 6 is a vertical cross-sectional view schematically showing an embodiment of the laminated structure of the current collector of the present invention.
  • the non-aqueous electrolyte secondary battery is arranged between a positive electrode, a negative electrode, and a positive electrode and a negative electrode. It has a separator.
  • the positive electrode has a positive electrode current collector and a positive electrode active material layer in contact with the positive electrode current collector
  • the negative electrode has a negative electrode current collector and a negative electrode active material layer in contact with the negative electrode current collector.
  • the positive electrode active material layer and the negative electrode active material layer are arranged toward the separator side, respectively, and are arranged so as to face each other via the separator.
  • the current collector included in the non-aqueous electrolyte secondary battery in the first embodiment is two types, a positive electrode current collector and a negative electrode current collector. That is, it does not have a bipolar current collector, which will be described later.
  • at least one of the positive electrode current collector and the negative electrode current collector has a resin film and a laminated structure of a conductive layer and a contact resistance reducing layer arranged on one side or both sides of the resin film. It is a laminated body.
  • the conductive layer side may face the resin film side, or the contact resistance reducing layer side may face the resin film side.
  • the current collector (Z1) is preferably in a form in which the resin film and the conductive layer are in contact with each other. That is, when the positive electrode current collector is the current collector (Z1), it is preferable that the contact resistance reducing layer of the current collector (Z1) and the positive electrode active material layer are in contact with each other, and the negative electrode current collector is the current collector (Z1).
  • the contact resistance reducing layer of the current collector (Z1) and the negative electrode active material layer are in contact with each other.
  • the non-aqueous secondary battery of the first embodiment is the sheet type shown in FIG. 1, it is preferable that at least the positive electrode current collector is a current collector (Z1), and the positive electrode current collector and the negative electrode current collector It is also preferable that both are current collectors (Z1).
  • the current collector (Z1) preferably has a laminated structure of a conductive layer and a contact resistance reducing layer on one side on which the positive electrode active material layer or the negative electrode initial material layer is arranged.
  • a current collector having positive electrode active material layers arranged on both sides or a negative electrode active material layer arranged on both sides is arranged.
  • the current collector is preferably a current collector (Z1), and the current collector (Z1) preferably has a laminated structure of a conductive layer and a contact resistance reducing layer on both sides.
  • the current collector in which the positive electrode active material layer or the negative electrode initial material layer is arranged on only one side may be a current collector (Z1), not a current collector (Z1). May be good.
  • the resin film layer constituting the "current collector (Z1)" may have a single-layer structure or a multi-layer structure.
  • the conductive layer may also have a single-layer structure or a multi-layer structure.
  • the contact resistance reducing layer can also have a single-layer structure or a multi-layer structure.
  • FIG. 1 is a cross-sectional view schematically showing a laminated structure of a general sheet-type non-aqueous electrolyte secondary battery 10, including an operating electrode when operating as a battery.
  • the non-aqueous electrolyte secondary battery 10 has a laminated structure having a negative electrode current collector 1, a negative electrode active material layer 2, a separator 3, a positive electrode active material layer 4, and a positive electrode current collector 5 in this order when viewed from the negative electrode side. ing.
  • the negative electrode active material layer and the positive electrode active material layer are filled with a non-aqueous electrolyte (not shown) and separated by a separator 3.
  • the separator 3 has holes and functions as a positive / negative electrode separation membrane that insulates between the positive and negative electrodes while allowing electrolytes and ions to pass through in a normal battery use state.
  • the lithium ions (Li + ) accumulated in the negative electrode are returned to the positive electrode side via the electrolyte, and electrons are supplied to the operating portion 6.
  • a light bulb is used for the operating portion 6, and the light bulb is turned on by electric discharge.
  • the separator 3 may be formed of a solid electrolyte.
  • the negative electrode current collector 1 and the negative electrode active material layer 2 are collectively referred to as a negative electrode
  • the positive electrode active material layer 4 and the positive electrode current collector 5 are collectively referred to as a positive electrode.
  • the non-aqueous electrolyte secondary battery of the first embodiment has a monopolar type laminated form schematically shown in FIG. 3 or FIG.
  • FIGS. 3 and 4 show a laminated structure of a monopolar non-aqueous electrolyte secondary battery.
  • the monopolar type laminate 30 shown in FIG. 3 includes a negative electrode current collector 31, a negative electrode active material layer 32, a separator 33, a positive electrode active material layer 34, a positive electrode current collector 35, a positive electrode active material layer 34, a separator 33, and a negative electrode active material.
  • the material layer 32 and the negative electrode current collector 31 are laminated in this order.
  • the 4 includes a positive electrode current collector 35, a positive electrode active material layer 34, a separator 33, a negative electrode active material layer 32, a negative electrode current collector 31, a negative electrode active material layer 32, a separator 33, and a positive electrode activity.
  • the material layer 34 and the positive electrode current collector 35 are laminated in this order.
  • the materials, electrolytes, members, and the like used in the non-aqueous electrolyte secondary battery of the first embodiment are not particularly limited except for the configuration of the current collector (Z1). As these materials, members and the like, those used for ordinary non-aqueous electrolyte secondary batteries can be appropriately applied. Further, as for the method for producing the non-aqueous electrolyte secondary battery of the present invention, a normal method can be appropriately adopted except for the configuration of the current collector. For example, Japanese Patent Application Laid-Open No. 2016-201308, Japanese Patent Application Laid-Open No. 2005-108835, Japanese Patent Application Laid-Open No. 2012-185938, and the like can be appropriately referred to.
  • the current collector (Z1) which is a characteristic configuration of the non-aqueous electrolyte secondary battery of the first embodiment, will be described below.
  • a current collector (Z1) is adopted for at least one of the positive electrode current collector and the negative electrode current collector.
  • the current collector (Z1) is a laminated body having a resin film and a laminated structure of a conductive layer and a contact resistance reducing layer arranged on one side or both sides of the resin film.
  • FIG. 2 shows a preferred form of the current collector (Z1), in which the current collector (Z1) has the above-mentioned laminated structure on one side of the resin film and the resin film and the conductive layer are in contact with each other.
  • FIG. 2 is a preferred embodiment as a current collector (Z1) in which a positive electrode active material layer or a negative electrode active material layer is arranged on only one side.
  • the current collector (Z1) is not limited to the form shown in FIG. 2 except as specified in the present invention. Further, the laminated structure of the conductive layer and the contact resistance reducing layer shown in FIG. 2 may be arranged on both sides of the resin film.
  • the current collector (Z1) of such a form is a monopolar non-aqueous electrolyte secondary battery in which a positive electrode active material layer is arranged on both sides or a negative electrode active material layer is arranged on both sides. Is preferably used as.
  • the current collector (Z1) 20 shown in FIG. 2 has a resin film 21 as a support, and a conductive layer 22 and a contact resistance reducing layer 23 on the resin film 21 in this order.
  • the configurations of the resin film, the conductive layer, and the contact resistance reducing layer constituting the current collector (Z1) in the first embodiment will be described with reference to FIG. 2, but the first embodiment other than the configurations shown in FIG.
  • the configurations of the resin film, the conductive layer, and the contact resistance reducing layer described below are preferably applied.
  • the constituent material (resin) of the resin film 21 is not particularly limited, and an electronically insulating resin can be preferably used.
  • an electronically insulating resin can be preferably used.
  • polyester resin, polyolefin resin, polyimide resin, polytetrafluoroethylene resin, polyvinylidene fluoride resin and the like can be mentioned, and it is preferable to use one or more of polyester resin and polyolefin resin.
  • the polyester resin include polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polybutylene naphthalate, and polyethylene isophthalate. Of these, polyethylene terephthalate is preferable.
  • polystyrene resin examples include low-density polyethylene, linear low-density polyethylene, medium-density polyethylene, high-density polyethylene, ultra-low-density polyethylene, random copolymerized polypropylene, block copolymerized polypropylene, homopolyprolene, polybutene, and polymethylpentene.
  • Ethylene-vinyl acetate copolymer, ionomer resin ethylene- (meth) acrylic acid copolymer, ethylene- (meth) acrylic acid ester copolymer, ethylene-butene copolymer, ethylene-hexene copolymer, etc.
  • polyethylene or polypropylene is preferable, and polyethylene is more preferable.
  • the resin film 21 may have a single-layer structure or a multi-layer structure.
  • the electrode active material layer side positive electrode active material layer side or negative electrode active material layer side, and the conductive layer side
  • the layer located in the synonym can also be a heat-sealing layer (a layer having a heat-sealing property).
  • the layer located on the electrode active material layer side may be a layer having adhesiveness.
  • the resin film 21 may be composed of three or more layers, and the layers other than the surface layer may be a metal layer such as an aluminum layer. Such a form is also included in the "resin film" used in the present invention.
  • the resin film 21 has a resin layer containing at least one of elemental carbon, gold, nickel and silver.
  • a current collector (Z1) has a positive electrode active material layer arranged on both sides or a negative electrode active material layer arranged on both sides.
  • the resin film 21 constituting the current collector (Z1) may have a resin layer containing at least one of carbon, gold, nickel and silver.
  • the resin film 21 is composed of one resin layer containing at least one of carbon, gold, nickel and silver. It is more preferable to be done.
  • Examples of the form of the resin layer containing single carbon constituting the resin film 21 include a resin film 21 formed of a resin in which single carbon is kneaded into the resin (single carbon is dispersed in the resin).
  • Examples of elemental carbon include acetylene black, ketjen black, carbon fiber, carbon nanofiber, graphene and the like.
  • Examples of the type of resin to be combined with the single carbon include polypropylene resin, epoxy resin, polystyrene resin, polyethylene resin, ABS resin, polycarbonate resin, polyethylene terephthalate resin, and the like, and polypropylene resin or epoxy resin is preferable. Resins in which single carbon is kneaded into the resin can also be obtained from the market.
  • Leopound (trade name, manufactured by Lion Specialty Chemicals), S-Dash PP (trade name, Nittetsu Chemical & Materials Co., Ltd.) Is commercially available.
  • the content of elemental carbon in the resin film is preferably 1 to 80% by mass, more preferably 3 to 50% by mass.
  • the resin layer containing gold constituting the resin film 21 it is preferable that gold-coated particles (resin particles coated with gold) are dispersed in the resin.
  • the particle size of the gold-coated particles is preferably 0.1 to 500 ⁇ m, more preferably 1 to 100 ⁇ m. In the present invention, the particle size means a volume-based median diameter.
  • the type of resin to be combined with the gold-coated particles include polypropylene resin, epoxy resin, polystyrene resin, polyethylene resin, ABS resin, polycarbonate resin, and polyethylene terephthalate resin, and polypropylene resin or epoxy resin is preferable.
  • Gold-coated particles can be obtained from the market, and are commercially available, for example, as Micropearl AU (trade name, manufactured by Sekisui Chemical Co., Ltd.) and Bright GNR-MX (trade name, manufactured by Nippon Kagaku Co., Ltd.).
  • the form of the nickel-containing resin layer constituting the resin film 21 is preferably one in which nickel particles are dispersed in the resin.
  • the particle size of the nickel particles is preferably 0.1 to 500 ⁇ m, more preferably 0.5 to 100 ⁇ m.
  • Examples of the type of resin to be combined with the nickel particles include polypropylene resin, epoxy resin, polystyrene resin, polyethylene resin, ABS resin, polycarbonate resin, polyethylene terephthalate resin, and the like, and polypropylene resin or epoxy resin is preferable.
  • Pastes in which nickel particles are dispersed in a resin can also be obtained from the market, and are commercially available, for example, as ECA202 (trade name, manufactured by Nihon Handa Co., Ltd.) and EMTech NI41 (trade name, manufactured by Elminet Co., Ltd.).
  • the form of the silver-containing resin layer constituting the resin film 21 is preferably one in which silver particles are dispersed in the resin.
  • the particle size of the silver particles is preferably 0.05 to 500 ⁇ m, more preferably 0.1 to 100 ⁇ m.
  • Examples of the type of resin to be combined with the silver particles include polypropylene resin, epoxy resin, polystyrene resin, polyethylene resin, ABS resin, polycarbonate resin, polyethylene terephthalate resin, and the like, and among them, polypropylene resin and epoxy resin are preferable.
  • Pastes in which silver particles are dispersed in a resin can also be obtained from the market, for example, LS-453-1 (trade name, manufactured by Asahi Chemical Laboratory Co., Ltd.), ECA-100 (trade name, manufactured by Nihon Handa Co., Ltd.), SCP. It is commercially available as -101 (trade name, manufactured by Shinetsu Silicone Co., Ltd.).
  • the resin film 21 is a coating film. That is, it is also preferable that the film is obtained by applying a paste in which the constituent materials of the resin film are dissolved on the metal foil using a metal foil as the conductive layer and drying the paste.
  • the current collector (Z1) Since the current collector (Z1) has a resin film, the safety of the battery, particularly the safety at the time of an internal short circuit, can be effectively enhanced.
  • the reason is considered as follows.
  • the conductive layer In the case of a form having no resin film (support), the conductive layer is inevitably formed to be thick to some extent (for example, a metal foil is used).
  • a metal foil is used.
  • a large amount of electrons are instantly supplied to the internal short circuit portion through the conductive layer (metal layer) of the current collector, which is considered to cause thermal runaway. ..
  • the current collector (Z1) having a resin film as a support since the metal layer is formed into a thin film by vapor deposition or the like, even if an internal short circuit occurs, the amount of electrons supplied to the internal short circuit portion is restricted. It is thought that the heat runaway can be suppressed. This is common to the action of the resin film on the bipolar current collector (Z2) in the second embodiment described later.
  • the thickness of the resin film can be appropriately set as long as the effect of the present invention is not impaired.
  • it can be 1 to 50 ⁇ m, more preferably 2 to 40 ⁇ m, and even more preferably 3 to 35 ⁇ m.
  • the thickness of each layer such as the constituent layer of the non-aqueous electrolyte secondary battery and the constituent layer of the current collector is randomly set at 100 points in the cross-sectional observation (electron microscope observation) of each layer in the stacking direction. Is measured and used as the arithmetic mean of those 100 measurements.
  • the conductive layer 22 is a layer exhibiting electronic conductivity, and is usually made of a metal material.
  • the conductive layer 22 preferably contains aluminum, and more preferably is made of aluminum or an aluminum alloy.
  • the conductive layer 22 may be configured to include a metal material such as titanium, stainless steel, or nickel, or an alloy thereof.
  • the conductive layer 22 preferably contains at least one of copper and nickel, and is composed of copper or a copper alloy, or nickel or a nickel alloy. More preferred.
  • the conductive layer 22 more preferably contains copper.
  • the conductive layer 22 is preferably formed into a thin layer by vapor deposition (preferably physical vapor deposition), sputtering, plating (preferably electroless plating) or the like. It can also be formed by arranging a metal foil such as a copper foil.
  • the thickness of the conductive layer 22 is preferably 10 to 5000 nm. From the viewpoint of improving the cycle characteristics, the thickness of the conductive layer 22 is more preferably 20 to 3000 nm, further preferably 70 to 2000 nm, further preferably 100 to 1000 nm, further preferably 150 to 900 nm, further preferably 200 to 800 nm.
  • the conductive layer 22 is formed of a metal foil, its thickness is preferably 500 to 5000 nm, and preferably 1000 to 3000 nm.
  • the conductive layer 22 is formed into a thin layer by vapor deposition (preferably physical vapor deposition), sputtering, plating (preferably electroless plating) or the like, if the thickness of the conductive layer of the negative electrode current collector is constant, the positive electrode collection
  • the thickness of the conductive layer 22 of the electric body By setting the thickness of the conductive layer 22 of the electric body to 150 to 900 nm (preferably 200 to 800 nm, more preferably 250 to 750 nm), the cycle characteristics can be further enhanced.
  • the thickness of the conductive layer of the positive electrode current collector is constant, the thickness of the conductive layer 22 of the negative electrode current collector is set to 150 to 900 nm (preferably 200 to 800 nm, more preferably 250 to 750 nm). Thereby, the cycle characteristics can be further improved.
  • At least one surface of the conductive layer 22 can be roughened.
  • at least one surface of the conductive layer 22 can have a surface roughness Ra of 0.3 ⁇ m or more (in this case, the thickness of the conductive layer 22 is preferably 100 nm or more, more preferably 150 nm or more. Yes, more preferably 200 nm or more).
  • the roughening method is not particularly limited, and for example, it can be formed by embossing or sandblasting the surface of the resin film and providing the conductive layer 22 in a thin layer by vapor deposition.
  • the surface of the conductive layer 22 opposite to the resin film also has a shape that reflects the unevenness of the sandblasting treatment, so that both sides of the conductive layer 22 are roughened as desired.
  • the surface roughness Ra of this surface is usually 5.0 ⁇ m or less, more preferably 3.0 ⁇ m or less, and preferably 2.0 ⁇ m or less. It is also preferable that the thickness is 1.5 ⁇ m or less.
  • the surface roughness Ra is an arithmetic mean roughness, and is determined with a reference length of 2.5 mm in accordance with JIS B0601 2001.
  • the contact resistance reducing layer 23 plays a role of increasing electron conductivity.
  • the conductive layer 22 constituting the current collector (Z1) 20 is usually formed of a metal material, and an oxide film is formed on the surface thereof, or a side reaction between the metal and the electrolyte occurs.
  • the adhesion or electron conductivity between the conductive layer 22 and the electrode active material layer or the like tends to decrease.
  • the layer contains a conductive substance.
  • a layer containing at least one of conductive carbon, nickel, titanium, tantalum and tungsten is preferable, and a layer containing at least one of conductive carbon and nickel is preferable, and the layer contains conductive carbon. It is preferably a layer.
  • the contact resistance reducing layer 23 is a conductive carbon-containing layer
  • the contact resistance reducing layer 23 may be formed by using a mixture of graphite and a binder, and it is also preferable to add conductive carbon such as acetylene black.
  • the content of the conductive carbon in the contact resistance reducing layer 23 is preferably 30% by mass or more, more preferably 40% by mass or more, and further 50% by mass or more. It is preferably 70% by mass or more.
  • the rest other than the conductive carbon is composed of the above binder and the like.
  • the contact resistance reducing layer 23 By forming the contact resistance reducing layer 23 as a titanium-containing layer, corrosion can be effectively prevented due to its high oxidation resistance.
  • a titanium-containing layer can be formed by depositing a titanium metal or the like. Further, the contact resistance reducing layer 23 may be formed by using an alloy containing titanium or a mixture of titanium and a binder.
  • the titanium content in the contact resistance reducing layer 23 is preferably 30% by mass or more, more preferably 40% by mass or more, further preferably 50% by mass or more, and 70% by mass. It is also preferable to set it to% or more.
  • the rest other than titanium is composed of the above binder and the like.
  • a tantalum-containing layer can be formed by depositing a tantalum metal or the like. Further, the contact resistance reducing layer 23 may be formed by using an alloy containing tantalum or a mixture of tantalum and a binder.
  • the tantalum content in the contact resistance reducing layer 23 is preferably 30% by mass or more, more preferably 40% by mass or more, further preferably 50% by mass or more, and 70% by mass. It is also preferable to set it to% or more.
  • the rest other than tantalum is composed of the above binder and the like.
  • the contact resistance reducing layer 23 By forming the contact resistance reducing layer 23 as a tungsten-containing layer, corrosion can be effectively prevented due to its high oxidation resistance.
  • a tungsten-containing layer can be formed by depositing a tungsten metal or the like. Further, the contact resistance reducing layer 23 may be formed by using a mixture of tungsten and a binder.
  • the content of tungsten in the contact resistance reducing layer 23 is preferably 30% by mass or more, more preferably 40% by mass or more, further preferably 50% by mass or more, and 70% by mass. It is also preferable to set it to% or more.
  • the rest other than tungsten is composed of the above binder and the like.
  • a nickel-containing layer can be formed by depositing a nickel metal or the like. Further, the contact resistance reducing layer 23 may be formed by using a mixture of nickel and a binder.
  • the nickel content in the contact resistance reducing layer 23 is preferably 30% by mass or more, more preferably 40% by mass or more, further preferably 50% by mass or more, and 70% by mass. It is also preferable to set it to% or more.
  • the rest other than nickel is composed of the above binder and the like.
  • the contact resistance reducing layer 23 has a configuration including conductive carbon. It is preferable to do so.
  • the contact resistance reducing layer 23 preferably contains at least one of conductive carbon, nickel, titanium, tantalum, and tungsten, and the conductive carbon. It is preferable that the configuration includes. It is also preferable that the contact resistance reducing layer contains at least one of conductive carbon and nickel.
  • the contact resistance reducing layer 23 there is a form in which a layer (also referred to as a rust preventive material-containing layer or a rust preventive layer) containing a rust preventive material (a material having a rust preventive action) is used.
  • a layer also referred to as a rust preventive material-containing layer or a rust preventive layer
  • a rust preventive material a material having a rust preventive action
  • 1,2,3-benzotriazole 1- [N, N-bis (2-ethylhexyl) aminomethyl] benzotriazole, carboxybenzotriazole, 1- [N, N-bis (2-ethylhexyl) ) Aminomethyl] methylbenzotriazole, 2,2'-[[(methyl-1H-benzotriazole-1-yl) methyl] imino] bisethanol, benzotriazole compounds such as 1,2,3-benzotriazole sodium salts; Phosphate compounds such as polyphosphates; silicate compounds such as metasilicates; nitrite compounds such as calcium nitrite can be mentioned.
  • the current collector in which the contact resistance reducing layer 23 contains a rust preventive material is preferable as a positive electrode current collector and also as a negative electrode current collector.
  • the contact resistance reducing layer 23 of the positive electrode current collector and the negative electrode current collector are used. It may be the same as or different from the contact resistance reducing layer 23 of the above.
  • the contact resistance reducing layer 23 of the positive electrode current collector and the contact resistance reducing layer 23 of the negative electrode current collector can both be a conductive carbon layer, or both can be a rust preventive material-containing layer.
  • the contact resistance reducing layer 23 of the positive electrode current collector is used as a conductive carbon layer
  • the contact resistance reducing layer 23 of the negative electrode current collector is used as a rust preventive material-containing layer
  • the contact resistance reducing layer 23 of the negative electrode current collector is conductive.
  • the carbon layer it is also preferable that the contact resistance reducing layer 23 of the positive electrode current collector is used as a rust preventive material-containing layer.
  • the method for forming the contact resistance reducing layer 23 is not particularly limited.
  • a coating liquid in which a target component is dissolved or dispersed in a solvent is prepared, a coating film using this coating liquid is formed, and then dried. Can be formed.
  • the contact resistance reducing layer 23 is formed of metal, it can be formed by vapor deposition or plating as described above.
  • the thickness of the contact resistance reducing layer 23 is preferably 10 to 3000 nm, more preferably 20 to 2000 nm, further preferably 30 to 1000 nm, further preferably 40 to 800 nm, still more preferably 50 to 700 nm.
  • the thickness of the contact resistance reducing layer 23 is preferably 60 nm or more, more preferably 80 nm or more, further preferably 100 nm or more, from the viewpoint of improving cycle characteristics. 120 nm or more is further preferable, 150 nm or more is further preferable, and 180 nm or more is further preferable.
  • the thickness of the contact resistance reducing layer 23, which is the conductive carbon-containing layer, is preferably 800 nm or less, more preferably 700 nm or less, preferably 600 nm or less, and preferably 550 nm or less.
  • the contact resistance reducing layer 23 is a rust preventive layer
  • a sufficient effect tends to be obtained even if the thickness of the contact resistance reducing layer 23 is 50 nm or less.
  • the thickness of the contact resistance reducing layer 23, which is a rust preventive layer is preferably 10 to 100 nm, more preferably 20 to 80 nm, and preferably 30 to 70 nm.
  • the non-aqueous electrolyte secondary battery of the first embodiment can be manufactured by arranging the above-mentioned current collector (Z1) as at least one of the positive electrode current collector and the negative electrode current collector, and the others by a conventional method.
  • the positive electrode current collector or the negative electrode current collector is not composed of the current collector (Z1)
  • the configuration of the current collector is not particularly limited, and those usually used as a current collector for a non-aqueous electrolyte secondary battery can be widely applied.
  • the positive electrode current collector or the negative electrode current collector which is not the current collector (Z1), has a resin film as a support. More preferably, the positive electrode current collector or the negative electrode current collector, which is not the current collector (Z1), has a configuration in which the contact resistance reducing layer is removed from the current collector (Z1). That is, it is preferable to use a resin film as a support and to form the conductive layer into a thin layer (for example, a thickness of 5000 nm or less, preferably a thickness of 2000 nm or less, more preferably a thickness of 1500 nm or less) by vapor deposition or the like.
  • a resin film for example, a thickness of 5000 nm or less, preferably a thickness of 2000 nm or less, more preferably a thickness of 1500 nm or less
  • the preferred form of this resin film is the same as the preferred form of the resin film described in the current collector (Z1). .. Further, the preferred form of the conductive layer in the positive electrode current collector or the negative electrode current collector other than the current collector (Z1) is the same as the preferable form of the conductive layer described in the current collector (Z1).
  • the positive electrode current collector or the negative electrode current collector which is not the current collector (Z1), has a configuration in which the contact resistance reduction layer is removed from the current collector (Z1), at least one surface of the conductive layer is roughened. It is preferable to do so.
  • at least one surface of the conductive layer can have a surface roughness Ra of 0.3 ⁇ m or more (in this case, the thickness of the conductive layer is preferably 100 nm or more, more preferably 150 nm or more. More preferably, it is 200 nm or more).
  • the contact area between the conductive layer and the layer in contact with the conductive layer can be increased, and the adhesion, electron conductivity, and the like can be further improved.
  • the roughening method is not particularly limited, and for example, it can be formed by sandblasting the surface of the resin film and providing a conductive layer on the surface of the resin film by thin film deposition.
  • the surface of the conductive layer opposite to the resin film also has a shape that reflects the unevenness of the sandblasting treatment, so that both sides of the conductive layer are roughened as desired.
  • the surface roughness Ra of this surface is usually 5.0 ⁇ m or less, more preferably 3.0 ⁇ m or less, and preferably 2.0 ⁇ m or less. It is also preferable that the thickness is 5.5 ⁇ m or less.
  • the non-aqueous electrolyte secondary battery has a positive electrode, a negative electrode, and a bipolar electrode.
  • the positive electrode has a positive electrode current collector and a positive electrode active material layer in contact with the positive electrode current collector
  • the negative electrode has a negative electrode current collector and a negative electrode active material layer in contact with the negative electrode current collector.
  • the bipolar electrode has a bipolar current collector (Z2), a positive electrode active material layer in contact with one surface of the bipolar current collector (Z2), and a negative electrode active material layer in contact with the other surface.
  • the non-aqueous electrolyte secondary battery of the second embodiment has a structure in which the positive electrode is arranged on the negative electrode active material layer side of the bipolar electrode and the negative electrode is arranged on the positive electrode active material layer side of the bipolar electrode with a separator interposed therebetween.
  • the positive electrode active material layer and the negative electrode active material layer are arranged toward the separator side, respectively, and are arranged so as to face each other via the separator.
  • the bipolar current collector (Z2) is a laminated body having a resin film and a laminated structure of a conductive layer and a contact resistance reducing layer arranged on one side or both sides of the resin film. More preferably, it is a laminate having a resin film and a laminated structure of a conductive layer and a contact resistance reducing layer arranged on both sides of the resin film.
  • FIG. 5 shows a laminated structure of a bipolar non-aqueous electrolyte secondary battery.
  • the bipolar type laminate 40 shown in FIG. 5 includes a negative electrode current collector 41, a negative electrode active material layer 42, a separator 43, a positive electrode active material layer 44, a bipolar current collector 45, a negative electrode active material layer 42, a separator 43, and a positive electrode activity.
  • the material layer 44 and the positive electrode current collector 46 are laminated in this order.
  • the configuration of a normal bipolar non-aqueous electrolyte secondary battery can be adopted.
  • the materials, electrolytes, members, and the like used in the non-aqueous electrolyte secondary battery of the second embodiment are not particularly limited except for the configuration of the bipolar current collector (Z2). As these materials, members and the like, those used for ordinary non-aqueous electrolyte secondary batteries can be appropriately applied. Further, it is also preferable that at least one of the positive electrode current collector and the negative electrode current collector used in the second embodiment is the current collector (Z1) described in the first embodiment.
  • the usual method as described in the first embodiment may be appropriately adopted except for the configuration of the bipolar current collector (Z2).
  • the technique of the bipolar non-aqueous electrolyte secondary battery for example, Japanese Patent Application Laid-Open No. 2013-110081 can be appropriately referred to.
  • the bipolar current collector (Z2) which is a characteristic configuration of the non-aqueous electrolyte secondary battery of the second embodiment, will be described below.
  • the bipolar current collector (Z2) is a laminated body having a resin film and a laminated structure of a conductive layer and a contact resistance reducing layer arranged on one side or both sides of the resin film. In this respect, it has the same structure as the current collector (Z1) in the first embodiment. That is, in the present invention, in the case of "a current collector having a resin film and a laminated structure of a conductive layer and a contact resistance reducing layer arranged on one side or both sides of the resin film", the current collector (Z1) and It is meant to include both bipolar current collectors (Z2).
  • FIG. 6 shows a preferred form of the bipolar current collector (Z2), in which the bipolar current collector (Z2) has the above-mentioned laminated structure on both sides of the resin film and the resin film and the conductive layer are in contact with each other.
  • FIG. 6 shows a preferred embodiment of the bipolar current collector (Z2), and the bipolar current collector (Z2) is limited to the embodiment shown in the drawings except as specified in the present invention. is not it.
  • the laminated structure of the conductive layer and the contact resistance reducing layer shown in FIG. 6 may be arranged on only one side of the resin film.
  • the structure of the resin film and the conductive layer in the second embodiment will be described with reference to FIG. 6, but the structure of the resin film and the conductive layer described below is preferably applied to the second embodiment other than FIG. Will be done.
  • the configuration of the bipolar current collector (Z2) 50 other than that described below the embodiment described in the current collector (Z1) in the first embodiment is preferably applied.
  • the form of the contact resistance reducing layer of the bipolar current collector (Z2) 50 the form of the contact resistance reducing layer described in the current collector (Z1) is preferably applied.
  • the contact resistance reducing layer of the bipolar current collector (Z2) 50 preferably contains the above-mentioned rust preventive material or conductive carbon.
  • the constituent material (resin) of the resin film 51 is not particularly limited, and the form (constituent material, layer structure, thickness, etc.) of the resin film 21 constituting the current collector (Z1) of the first embodiment is the resin film 51.
  • a film containing a conductive material is preferable.
  • the resin film 51 preferably has a resin layer containing at least one of elemental carbon, gold, nickel and silver.
  • the resin film 51 is composed of one resin layer containing at least one of carbon, gold, nickel and silver. It is more preferable to be done.
  • the conductive layer 52 is a layer exhibiting electronic conductivity, and is usually made of a metal material.
  • the conductive layer 52 is arranged on the positive electrode active material layer side constituting the bipolar electrode, it preferably contains at least one of aluminum and nickel from the viewpoint of oxidation resistance. These aluminum and nickel can be fixed to the surface of the resin film 52 by vapor deposition or the like.
  • the conductive layer 52 arranged on the negative electrode active material layer side constituting the bipolar electrode is preferably a copper foil from the viewpoint of reduction resistance. Therefore, it is preferable that the conductive layer 52 arranged on the positive electrode active material layer side constituting the bipolar electrode is thick to some extent.
  • the bipolar current collector (Z2) has a laminated structure of a conductive layer and a contact resistance reducing layer on both sides, it is preferable that the conductive layers constituting both laminated structures are made of different materials.
  • the non-aqueous electrolyte secondary battery of the present invention is, for example, a laptop computer, a pen input computer, a mobile computer, an electronic book player, a mobile phone, a cordless phone slave unit, a pager, a handy terminal, a mobile fax, a mobile copy, a mobile printer, a headphone.
  • Can be installed in electronic devices such as stereos, video movies, LCD TVs, handy cleaners, portable CDs, mini discs, electric shavers, transceivers, electronic notebooks, calculators, memory cards, portable tape recorders, radios, backup power supplies, memory cards, etc. can.
  • Example 1 ⁇ Preparation of non-aqueous electrolyte solution> A non-aqueous electrolyte solution was prepared by dissolving LiPF 6 as a lithium salt at a concentration of 1 M in a non-aqueous solvent consisting of 40 parts by mass of ethylene carbonate and 60 parts by mass of ethyl methyl carbonate.
  • ⁇ Preparation of slurry for forming positive electrode active material layer 85 parts by mass of LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523) as the positive electrode active material, 7 parts by mass of acetylene black as the conductive auxiliary agent, PVDF (polyvinylidene fluoride) as the binder.
  • NCM523 LiNi 0.5 Co 0.2 Mn 0.3 O 2
  • acetylene black as the conductive auxiliary agent
  • PVDF polyvinylidene fluoride
  • ⁇ Separator> A polypropylene separator (porosity 35%, film thickness 20 ⁇ m) was used.
  • slurry for forming conductive carbon layer A slurry containing 10 parts by mass of natural graphite, 2 parts by mass of acetylene black, and 2 parts by mass of PVDF (mesitylene as a medium) was prepared and used as a slurry for forming a conductive carbon layer.
  • a sheet-type non-aqueous electrolyte secondary battery having a laminated structure shown in FIG. 1 was produced as follows. -Preparation of positive electrode current collector- A polyethylene terephthalate (PET) film having a thickness of 12 ⁇ m was used as the resin film, and aluminum was vapor-deposited on the film to form a conductive layer having a thickness of 300 nm. The slurry for forming a conductive carbon layer was applied onto the aluminum conductive layer and dried to form a conductive carbon layer (contact resistance reducing layer) having a thickness of 200 nm. In this way, a positive electrode current collector was obtained.
  • PET polyethylene terephthalate
  • the slurry for forming the positive electrode active material layer is applied onto the conductive carbon layer of the positive electrode current collector obtained above and dried to form a positive electrode active material layer having a thickness of 80 ⁇ m to obtain a positive electrode. rice field.
  • the slurry for forming the negative electrode active material layer was applied onto the conductive layer of the negative electrode current collector obtained above and dried to form a negative electrode active material layer having a thickness of 80 ⁇ m to obtain a negative electrode.
  • non-aqueous electrolyte secondary batteries The obtained positive electrode and negative electrode were laminated with the positive electrode active material layer and the negative electrode active material layer on the separator side, respectively, via the separator. Wiring (tabs) was connected to the conductive layer of each current collector, and these wirings were pulled out to the outside, and then the above electrolytic solution was sealed using a resin film to obtain a non-aqueous electrolyte secondary battery.
  • the obtained non-aqueous electrolyte secondary battery was charged at 25 ° C. at a current value of 30 mA and a final voltage of 4.2 V, and then charged and discharged three times at a current value of 30 mA and a final voltage of 3.0 V. In this way, a sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained.
  • Example 2 In the production of the negative electrode current collector of Example 1, the above-mentioned slurry for forming a conductive carbon layer was applied onto the conductive layer (copper vapor deposition layer) and dried to form a conductive carbon layer having a thickness of 200 nm. A sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained in the same manner as in Example 1.
  • Example 3 In the preparation of the negative electrode current collector of Example 1, an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass was applied onto the conductive layer (copper vapor deposition layer) and dried. A sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained in the same manner as in Example 1 except that a rust-preventive layer having a thickness of 50 nm was formed.
  • Example 4 In the preparation of the negative electrode current collector of Example 1, an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass was applied onto the conductive layer (copper vapor deposition layer) and dried. A sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained in the same manner as in Example 1 except that a rust-preventive layer having a thickness of 150 nm was formed.
  • Example 5 In the production of the positive electrode current collector of Example 1, instead of the slurry for forming the conductive carbon layer, an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass was used to obtain a thickness. A sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained in the same manner as in Example 1 except that a rust preventive layer having a diameter of 50 nm was formed.
  • Example 6 In the production of the negative electrode current collector of Example 5, the same as in Example 5 except that the surface of the PET film was sandblasted and copper was vapor-deposited on the treated surface to form a conductive layer having a thickness of 300 nm. A sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained. Ra was 0.4 ⁇ m on both sides of the conductive layer.
  • Example 7 In the production of the negative electrode current collector of Example 5, the same as in Example 5 except that the surface of the PET film was sandblasted and copper was vapor-deposited on the treated surface to form a conductive layer having a thickness of 300 nm. A sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained. Ra was 1.0 ⁇ m on both sides of the conductive layer.
  • Example 8 Example 9, Example 10, Example 11
  • a sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained in the same manner as in Example 1 except that the thickness of the conductive carbon layer was as shown in the table below. rice field.
  • Example 12 Example 13, Example 14, Example 15
  • a sheet-type non-aqueous electrolyte secondary having a capacity of 300 mAh is the same as in Example 1 except that the thickness of the conductive layer (aluminum-deposited layer) is as shown in the table below. I got a battery.
  • Example 16 In the preparation of the positive electrode current collector of Example 1, a sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained in the same manner as in Example 1 except that the thickness of the PET film was as shown in the table below.
  • Example 18 In the production of the positive electrode current collector of Example 1, a sheet type having a capacity of 300 mAh was used in the same manner as in Example 1 except that a polyethylene (PE) film having a thickness of 20 ⁇ m was used instead of the PET film having a thickness of 12 ⁇ m. A non-aqueous electrolyte secondary battery was obtained.
  • PE polyethylene
  • Example 1 A sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained in the same manner as in Example 1 except that the conductive carbon layer was not formed in the production of the positive electrode current collector of Example 1.
  • Example 2 In the production of the positive electrode current collector of Example 1, the above-mentioned slurry for forming a conductive carbon layer was applied onto an aluminum foil having a thickness of 20 ⁇ m without using a resin film, dried, and made conductive with a thickness of 300 nm. A sheet-type non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained in the same manner as in Example 1 except that the sex carbon layer was formed.
  • Discharge capacity retention rate (%) 100 x [Discharge capacity in the 100th cycle] / [Discharge capacity in the 1st cycle] -Evaluation criteria for cycle characteristics- S: Discharge capacity retention rate is 95% or more A: Discharge capacity retention rate is 93% or more and less than 95% B: Discharge capacity retention rate is 90% or more and less than 93% C: Discharge capacity retention rate is 85% or more and less than 90% D : Discharge capacity retention rate is less than 85% The results are shown in the table below.
  • the obtained non-aqueous electrolyte secondary battery results in significantly inferior cycle characteristics.
  • Comparative example 1 when the positive electrode current collector does not have a resin film and therefore the conductive layer is formed thickly, the obtained non-aqueous electrolyte secondary battery can sufficiently suppress thermal runaway when an internal short circuit occurs. It could not be done (Comparative Example 2).
  • the non-aqueous electrolyte secondary batteries having the current collector specified in the present invention were all excellent in cycle characteristics and safety (Examples 1 to 18).
  • Example 19 A non-aqueous electrolytic solution, a slurry for forming a positive electrode active material layer, a slurry for forming a negative electrode active material layer, and a separator were prepared in the same manner as in Example 1.
  • a monopolar non-aqueous electrolyte secondary battery having a laminated structure shown in FIG. 3 was produced as follows.
  • a PET film having a thickness of 12 ⁇ m was used as the resin film, and aluminum was vapor-deposited on both sides of the film to form conductive layers having a thickness of 300 nm on both sides of the PET film.
  • a rust preventive layer having a thickness of 50 nm was formed on the aluminum conductive layers on both sides by using an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass, respectively. In this way, a positive electrode current collector having a laminated structure of a conductive layer and a contact resistance reducing layer (rust preventive layer) was obtained on both sides of the resin film.
  • Example 20 A non-aqueous electrolytic solution, a slurry for forming a positive electrode active material layer, a slurry for forming a negative electrode active material layer, and a separator were prepared in the same manner as in Example 1.
  • a monopolar non-aqueous electrolyte secondary battery having a laminated structure shown in FIG. 4 was produced as follows.
  • a PET film having a thickness of 12 ⁇ m was used as the resin film, and copper was vapor-deposited on both sides of the film to form conductive layers having a thickness of 300 nm on both sides of the film.
  • a rust preventive layer having a thickness of 50 nm was formed on the copper conductive layers on both sides by using an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass, respectively. In this way, a negative electrode current collector having a laminated structure of a conductive layer and a contact resistance reducing layer (rust preventive layer) was obtained on both sides of the resin film.
  • Example 21 Example 19 except that a carbon resin (C resin) film (molded product) having a thickness of 85 ⁇ m was used instead of the PET film having a thickness of 12 ⁇ m as the resin film constituting the positive electrode current collector. In the same manner as above, a monopolar non-aqueous electrolyte secondary battery was obtained.
  • the above “carbon resin film (molded product)” was produced as follows.
  • polypropylene (trade name "SunAllomer PL500A”, manufactured by SunAllomer Ltd.) 75% by mass
  • acetylene black (AB) (trade name "Denka Black HS-100", manufactured by Denka Co., Ltd.) 20
  • a material for a current collector was obtained by melt-kneading 5% by mass and 5% by mass of a dispersant (trade name "Admer QE800” manufactured by Mitsui Chemicals Ltd.) at 180 ° C., 100 rpm and a residence time of 10 minutes.
  • the obtained current collector material was rolled by a hot press to obtain a carbon-containing resin film having a thickness of 85 ⁇ m.
  • Example 22 A monopolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 21 except that the production of the positive electrode current collector was changed as follows in Example 21. (Preparation of positive electrode current collector) A carbon-containing resin film having a thickness of 85 ⁇ m was obtained in the same manner as in Example 21. Further, an aluminum foil having a thickness of 10 ⁇ m was laminated and treated by a hot roll press to obtain a carbon-containing resin film / aluminum foil laminate. Further, aluminum was vapor-deposited on the other surface of the carbon-containing resin film to form a conductive layer having a thickness of 300 nm.
  • an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass was used to form a rust preventive layer having a thickness of 50 nm, respectively, to form a positive electrode current collector.
  • Example 23 A monopolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 22 except that the production of the positive electrode current collector was changed as follows in Example 22.
  • Liquid epoxy resin [Selokiside 2021P (oil ring type epoxy resin; manufactured by Daicel)] 7 parts by mass, polyfunctional epoxy resin [Marproof G2050M (manufactured by Nichiyu)] 15 parts by mass, acetylene black 5 parts by mass and curing agent [Sun Aid SI -60 (manufactured by Sanshin Chemical Industry Co., Ltd.)] 0.5 parts by mass was mixed to prepare a paste containing a carbon resin (mesticylene as a medium).
  • the paste containing this carbon resin was applied onto the aluminum foil and dried to form a carbon resin film (coating film) having a thickness of 85 ⁇ m.
  • aluminum was vapor-deposited on the side of the carbon resin film opposite to the side having the aluminum foil to form a conductive layer having a thickness of 300 nm.
  • a rust preventive layer having a thickness of 50 nm was formed on the aluminum conductive layers (foil and vapor-deposited film) on both sides by using an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass, respectively. .. In this way, a positive electrode current collector having a laminated structure of a conductive layer and a contact resistance reducing layer (rust preventive layer) was obtained on both sides of the resin film.
  • Example 24 a monopolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 23, except that the thickness of the carbon resin film (coating film) constituting the positive electrode current collector was 20 ⁇ m.
  • Example 25 In Example 20, except that the resin film constituting the negative electrode current collector was a carbon resin film (molded product) having a thickness of 85 ⁇ m in Example 21 instead of the PET film having a thickness of 12 ⁇ m. In the same manner as above, a monopolar non-aqueous electrolyte secondary battery was obtained.
  • Example 26 A monopolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 25, except that the fabrication of the negative electrode current collector was changed as follows in Example 25.
  • a carbon resin film / copper foil laminate was obtained by stacking a carbon resin film (molded product) having a thickness of 85 ⁇ m and a copper foil having a thickness of 10 ⁇ m of Example 21 and treating them with a hot roll press. Further, copper was vapor-deposited on the other surface of the carbon resin film to form a conductive layer having a thickness of 300 nm.
  • an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass was used to form a rust preventive layer having a thickness of 50 nm, respectively, to form a negative electrode current collector.
  • Example 27 A monopolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 26, except that the fabrication of the negative electrode current collector was changed as follows in Example 26.
  • a carbon resin film (molded product) having a thickness of 85 ⁇ m of Example 21 and a copper foil MT18FL (manufactured by Mitsui Kinzoku Co., Ltd.) with a carrier of copper foil (2 ⁇ m) / carrier copper foil (18 ⁇ m) are laminated and processed by a thermal roll press. As a result, a laminate of a carbon resin film (85 ⁇ m) / copper foil (2 ⁇ m) / carrier copper foil (18 ⁇ m) was obtained.
  • Example 28 A monopolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 27, except that the preparation of the negative electrode current collector was changed as follows in Example 27.
  • copper was vapor-deposited on the side of the carbon resin film opposite to the side having the copper foil to form a conductive layer having a thickness of 300 nm.
  • the carrier copper foil was peeled off to obtain a laminated body of a copper vapor deposition film (300 nm) / carbon resin film (85 ⁇ m) / copper foil (2 ⁇ m).
  • a rust preventive layer having a thickness of 50 nm was formed on the copper conductive layers (foil and vapor-deposited film) on both sides by using an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass, respectively. ..
  • a negative electrode current collector having a laminated structure of a conductive layer and a contact resistance reducing layer (rust preventive layer) was obtained on both sides of the resin film.
  • Example 29 a monopolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 28, except that the thickness of the carbon resin film (coating film) constituting the negative electrode current collector was 20 ⁇ m.
  • Example 3 In the production of the positive electrode current collector of Example 19, the same conductive carbon layer forming slurry as used in Example 1 was applied to both sides of an aluminum foil having a thickness of 20 ⁇ m without using a resin film. A monopolar non-aqueous electrolyte secondary battery having a capacity of 600 mAh was obtained in the same manner as in Example 19 except that it was dried to form a conductive carbon layer having a thickness of 200 nm.
  • the column of Comparative Example 3 in Table 2 describes Al foil and 20000 nm in both the front and back columns of the positive electrode current collector, but only one aluminum foil was used as described above. ..
  • Discharge capacity retention rate (%) 100 x [Discharge capacity in the 100th cycle] / [Discharge capacity in the 1st cycle] -Evaluation criteria for cycle characteristics- S: Discharge capacity retention rate is 95% or more A: Discharge capacity retention rate is 93% or more and less than 95% B: Discharge capacity retention rate is 90% or more and less than 93% C: Discharge capacity retention rate is 85% or more and less than 90% D : Discharge capacity retention rate is less than 85% The results are shown in the table below.
  • Example 30 A non-aqueous electrolytic solution, a slurry for forming a positive electrode active material layer, a slurry for forming a negative electrode active material layer, and a separator were prepared in the same manner as in Example 1.
  • a bipolar non-aqueous electrolyte secondary battery having a laminated structure shown in FIG. 5 was produced as follows.
  • bipolar current collector- Using the carbon resin film (molded product) having a thickness of 85 ⁇ m of Example 21 as a resin film, aluminum is vapor-deposited on one side (positive electrode surface) of this film, and copper is vapor-deposited on the other side (negative electrode surface). A conductive layer having a thickness of 300 ⁇ m was formed on both sides. A rust preventive layer having a thickness of 50 nm was formed on the conductive layers on both sides by using an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass, respectively. In this way, a bipolar current collector having a laminated structure of a conductive layer and a contact resistance reducing layer (rust preventive layer) was obtained on both sides of the resin film.
  • rust preventive layer a bipolar current collector having a laminated structure of a conductive layer and a contact resistance reducing layer
  • the slurry for forming the positive electrode active material layer is coated on the aluminum vapor deposition layer side and dried to form a positive electrode active material layer having a thickness of 80 ⁇ m.
  • the above-mentioned slurry for forming a negative electrode active material layer was applied to the copper vapor deposition layer side and dried to form a negative electrode active material layer having a thickness of 80 ⁇ m. In this way, a bipolar electrode having a positive electrode active material layer on one surface (positive electrode surface) and a negative electrode active material layer on the other surface (negative electrode surface) of the bipolar current collector was obtained.
  • the slurry for forming the positive electrode active material layer was applied onto the conductive layer of the positive electrode current collector obtained above and dried to form a positive electrode active material layer having a thickness of 80 ⁇ m to obtain a positive electrode.
  • the slurry for forming the negative electrode active material layer was applied onto the conductive layer of the negative electrode current collector obtained above and dried to form a negative electrode active material layer having a thickness of 80 ⁇ m to obtain a negative electrode.
  • the separator is overlaid on the negative electrode surface of the bipolar electrode, the silicone insulating film on the frame is placed around the bipolar electrode and the separator, the positive electrode is overlaid so as to be in contact with the separator, and the electrolytic solution is injected into the insulating layer. Sealed. Wiring (tabs) were connected to the conductive layers of the positive electrode and the negative electrode, and these wirings were pulled out to the outside, and then the aluminum laminate film was sealed to obtain a non-aqueous electrolyte secondary battery. The obtained non-aqueous electrolyte secondary battery was charged at 25 ° C.
  • Example 31 A bipolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 30 except that the preparation of the bipolar current collector was changed as follows in Example 30.
  • a carbon resin film (molded product) having a thickness of 85 ⁇ m of Example 21 and a copper foil MT18FL (manufactured by Mitsui Kinzoku Co., Ltd.) with a carrier of copper foil (2 ⁇ m) / carrier copper foil (18 ⁇ m) are laminated and processed by a thermal roll press. As a result, a laminate of a carbon resin film (85 ⁇ m) / copper foil (2 ⁇ m) / carrier copper foil (18 ⁇ m) was obtained.
  • Example 32 A bipolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 31 except that the preparation of the bipolar current collector was changed as follows in Example 31.
  • aluminum was vapor-deposited on the side of the carbon resin film opposite to the side having the copper foil to form a conductive layer having a thickness of 300 nm.
  • the carrier copper foil was peeled off to obtain a laminate of a conductive layer (300 nm) / carbon resin film (85 ⁇ m) / copper foil (2 ⁇ m).
  • a rust preventive layer having a thickness of 50 nm was formed on the conductive layers (foil and vapor-deposited film) on both sides by using an ethanol solution prepared by dissolving 1,2,3-benzotriazole at a concentration of 2% by mass, respectively.
  • a bipolar current collector having a laminated structure of a conductive layer and a contact resistance reducing layer (rust preventive layer) was obtained on both sides of the resin film.
  • Example 33 A bipolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 32, except that the thickness of the carbon resin film (coating film) constituting the bipolar current collector was set to 20 ⁇ m in Example 32.
  • Example 34 A bipolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 33, except that the aluminum vapor deposition layer constituting the bipolar current collector was replaced with a nickel vapor deposition layer in Example 33.
  • Example 35 In the production of the bipolar current collector of Example 34, instead of applying a paste containing a carbon resin on the copper foil, 7 parts by mass of a liquid epoxy resin [Selokiside 2021P (aliphatic epoxy resin; manufactured by Daicel)], Polyfunctional epoxy resin [Marproof G2050M (manufactured by Nichiyu)] 15 parts by mass, gold coated particles [Micropearl AU (manufactured by Sekisui Chemical Co., Ltd.)] 10 parts by mass and curing agent [Sun Aid SI-60 (manufactured by Sanshin Chemical Industry Co., Ltd.) ]
  • a bipolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 34, except that a paste (the medium was mesitylene) mixed with 0.5 parts by mass was applied.
  • Example 36 In the production of the bipolar current collector of Example 34, instead of applying a paste containing a carbon resin on the copper foil, 7 parts by mass of a liquid epoxy resin [Ceroxide 2021P (alicyclic epoxy resin; manufactured by Daicel)], Polyfunctional epoxy resin [Marproof G2050M (manufactured by Nichiyu)] 15 parts by mass, nickel powder [NIE02PB (manufactured by high-purity chemicals)] 10 parts by mass and curing agent [Sun Aid SI-60 (manufactured by Sanshin Chemical Industries)] 0.
  • a bipolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 34, except that a paste (the medium was mesitylene) mixed with 5 parts by mass was applied.
  • Example 37 In the production of the bipolar current collector of Example 34, instead of applying a paste in which a carbon resin is dissolved on a copper foil, 7 parts by mass of a liquid epoxy resin [Selokiside 2021P (alicyclic epoxy resin; manufactured by Daicel)] , Polyfunctional epoxy resin [Marproof G2050M (manufactured by Nichiyu)] 15 parts by mass, silver powder [AgC-2011 (manufactured by Fukuda Metal Foil Powder Industry)] 10 parts by mass and curing agent [Sun Aid SI-60 (Sanshin Kagaku Kogyo) (Manufactured)] A bipolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 34, except that a paste (the medium was mesitylene) mixed with 0.5 parts by mass was applied.
  • a paste the medium was mesitylene
  • Example 38 A bipolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 30 except that a rust preventive layer was provided on the negative electrode surface of the bipolar current collector in Example 30.
  • Example 39 A bipolar non-aqueous electrolyte secondary battery was obtained in the same manner as in Example 30 except that both the conductive layer and the rust preventive layer were provided on the negative electrode surface of the bipolar current collector in Example 30.
  • Example 30 the same conductive carbon layer forming slurry used in Example 1 was applied to one side of an aluminum foil having a thickness of 10 ⁇ m as a bipolar current collector, dried, and dried to a thickness of 200 nm.
  • a bipolar non-aqueous electrolyte secondary having a capacity of 300 mAh is the same as in Example 30, except that the aluminum foil side of the laminate on which the conductive carbon layer is formed and the copper foil having a thickness of 2 ⁇ m are laminated. I got a battery.
  • Example 30 a carbon resin film (molded product) having a thickness of 85 ⁇ m of Example 21 was used as a resin film as a bipolar current collector, and aluminum was vapor-deposited on one side of this film to form a conductive layer having a thickness of 300 ⁇ m.
  • a bipolar non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained in the same manner as in Example 30 except that the formed one was used.
  • Example 30 a bipolar non-aqueous electrolyte secondary battery having a capacity of 300 mAh was obtained in the same manner as in Example 30 except that the carbon resin film (molded product) of Example 21 was used as the bipolar current collector. ..
  • Discharge capacity retention rate (%) 100 x [Discharge capacity in the 100th cycle] / [Discharge capacity in the 1st cycle] -Evaluation criteria for cycle characteristics- S: Discharge capacity retention rate is 90% or more A +: Discharge capacity retention rate is 85% or more and less than 90% A: Discharge capacity retention rate is 80% or more and less than 85% B +: Discharge capacity retention rate is 75% or more and less than 80% B : Discharge capacity retention rate is 70% or more and less than 75% C: Discharge capacity retention rate is 60% or more and less than 70% D: Discharge capacity retention rate is less than 60% The results are shown in the table below.
  • the bipolar non-aqueous electrolyte secondary batteries having the bipolar current collector specified in the present invention are all excellent in cycle characteristics and safety (Examples 30 to 39). ..

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