WO2018135545A1 - Film protecteur, batterie, et procédé de fabrication de batterie - Google Patents

Film protecteur, batterie, et procédé de fabrication de batterie Download PDF

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Publication number
WO2018135545A1
WO2018135545A1 PCT/JP2018/001269 JP2018001269W WO2018135545A1 WO 2018135545 A1 WO2018135545 A1 WO 2018135545A1 JP 2018001269 W JP2018001269 W JP 2018001269W WO 2018135545 A1 WO2018135545 A1 WO 2018135545A1
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WO
WIPO (PCT)
Prior art keywords
heat
resin layer
protective film
metal foil
electrode
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2018/001269
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English (en)
Japanese (ja)
Inventor
亮 藤原
高萩　敦子
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Dai Nippon Printing Co Ltd
Original Assignee
Dai Nippon Printing Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Dai Nippon Printing Co Ltd filed Critical Dai Nippon Printing Co Ltd
Priority to CN201880007219.0A priority Critical patent/CN110178248B/zh
Priority to JP2018563373A priority patent/JP7024734B2/ja
Publication of WO2018135545A1 publication Critical patent/WO2018135545A1/fr
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
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/531—Electrode connections inside a battery casing
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/78—Cases; Housings; Encapsulations; Mountings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/78—Cases; Housings; Encapsulations; Mountings
    • H01G11/80—Gaskets; Sealings
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
    • H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
    • H01G11/84—Processes for the manufacture of hybrid or EDL capacitors, or components thereof
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/04—Construction or manufacture in general
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a protective film, a battery, and a method for manufacturing the battery.
  • a metal material has been conventionally used, but in recent years, various shapes are required for the battery, and a reduction in thickness and weight is also required. With metal packaging materials, it is difficult to follow the diversification of shapes, and there is a limit to weight reduction. Therefore, as a packaging material that can be easily processed into various shapes and can be made thinner and lighter, a film-like laminate in which a base material layer / barrier layer / heat-sealable resin layer are sequentially laminated has also been proposed. (For example, refer to Patent Document 1).
  • a positive electrode obtained by applying a positive electrode active material on both sides of a positive electrode foil and a negative electrode obtained by applying a negative electrode active material on both sides of a negative electrode foil are wound through a separator, and the wound body (electrode) The group) is widely known in a battery case.
  • a metal foil exposed portion in which the positive and negative metal foils are exposed is formed at both ends in the winding axis direction of the wound body (electrode group), and an electrode is formed on the exposed metal foil. Terminals and current collectors are connected by welding or the like (see Patent Document 2).
  • Patent Document 2 when a metal foil exposed portion and a current collector are joined by ultrasonic welding, laser welding, friction stir welding, or the like, a minute amount is obtained from the metal foil exposed portion or current collector to be joined. It is known that a large piece of metal is scattered. When such a minute metal piece is mixed in the electrode group, there may be a problem that a micro short circuit occurs inside the battery.
  • Patent Document 2 discloses that at least a part of a joint portion constituted by a metal foil exposed portion and a connection plate is made of a resin adhesive tape, a resin adhesive, or a hot melt resin agent. A technique for coating with is disclosed.
  • the conventional method using resin adhesive tape, etc. causes the resin adhesive tape to thermally shrink due to high temperatures, so that the shape cannot be maintained and the periphery of the welded part cannot be protected. There is also. Furthermore, the conventional resin adhesive tape has a problem of insufficient insulation.
  • the present invention can be suitably fixed in the battery around the portion where the exposed portion of the metal foil of the electrode is welded. Furthermore, the main purpose is to provide an excellent protective film. Another object of the present invention is to provide a battery using the protective film and a method for producing the battery.
  • the present inventors have intensively studied to solve the above problems.
  • a protective film used for a battery including an electrode having a metal foil and an active material layer located on the surface of the metal foil, and the electrode is provided with a metal foil exposed portion where the metal foil is exposed.
  • the protective film is used to protect at least part of the periphery of the portion where the exposed portion of the metal foil of the electrode and the metal terminal are welded, and the protective film contains at least an adhesive component (adhesive property).
  • a first heat-welding resin layer, a heat-resistant intermediate layer, and a second heat-welding resin layer in this order, and the first heat-welding resin layer constitutes one surface of the protective film.
  • the protective film can be suitably fixed around the portion where the exposed portion of the metal foil of the electrode is welded in the battery, and further, heat shrinkage due to high temperature during welding is small, and the insulating property is also excellent. I found out.
  • the present invention has been completed by further studies based on such knowledge.
  • a protective film used in a battery comprising an electrode having a metal foil and an active material layer located on the surface of the metal foil, The electrode is provided with a metal foil exposed portion where the metal foil is exposed, The protective film is used to protect at least part of the periphery of a portion where the metal foil exposed portion of the electrode and the metal terminal are welded, The protective film includes at least a first heat-welding resin layer having adhesiveness, a heat-resistant intermediate layer, and a second heat-welding resin layer in this order, The first heat-welding resin layer is a protective film that constitutes one surface of the protective film.
  • the protective film according to Item 1 wherein the thermal shrinkage measured under conditions of a test temperature of 200 ° C and a heating time of 10 seconds is 10% or less.
  • Item 3. Item 3. The protective film according to Item 1 or 2, wherein the resin constituting the first heat-weldable resin layer has a polyolefin skeleton.
  • Item 4. Item 4. The protective film according to any one of Items 1 to 3, wherein the first heat-welding resin layer contains a modified polyolefin.
  • Item 6. Item 6.
  • Item 7. Item 7. The protective film according to any one of Items 1 to 6, wherein the second heat-weldable resin layer constitutes a surface opposite to the first heat-weldable resin layer.
  • Item 8. Item 8. The protective film according to any one of Items 1 to 7, wherein at least one of the first heat-weldable resin layer, the intermediate layer, and the second heat-weldable resin layer is colored.
  • At least a battery element including an electrode and an electrolyte is a battery accommodated in a package formed of a battery packaging material,
  • the electrode includes a metal foil and an active material layer located on the surface of the metal foil,
  • the electrode is provided with a metal foil exposed portion where the metal foil is exposed, Item 10.
  • the battery, wherein at least a part of the periphery of a portion where the metal foil exposed portion and the metal terminal of the electrode are welded is covered with the protective film according to any one of Items 1-9.
  • a method for producing a battery comprising an electrode having a metal foil and an active material layer located on the surface of the metal foil, The electrode is provided with a metal foil exposed portion where the metal foil is exposed, The step of covering at least part of the periphery of the portion where the metal foil exposed portion and the metal terminal of the electrode are to be welded with the protective film according to any one of Items 1 to 9, And subsequently welding the exposed metal foil portion to the metal terminal; A method for producing a battery.
  • the exposed portion of the metal foil of the electrode can be suitably fixed around the portion to be welded, and further, thermal contraction due to high temperature during welding is small, and the insulating property is also excellent.
  • a protective film can be provided.
  • the battery using the said protective film and the manufacturing method of the said battery can also be provided.
  • FIG. 1 It is a schematic diagram of an example of the part by which the metal foil exposed part of an electrode is welded. It is a schematic sectional drawing of an example of the protective film of this invention. It is a schematic sectional drawing of an example of the protective film of this invention. It is a schematic sectional drawing of an example of the protective film of this invention. It is a schematic sectional drawing of an example of the protective film of this invention. It is a schematic diagram for demonstrating the method of insulation evaluation. It is a schematic diagram for demonstrating the structure of the battery of this invention. It is a conceptual diagram of a change in the position of the probe in measuring the displacement of the probe using an atomic force microscope to which a cantilever (probe) with a heating mechanism is attached.
  • FIG. 1 It is a schematic diagram of a change in the position of the probe in measuring the displacement of the probe using an atomic force microscope to which a cantilever (probe) with a heating mechanism is attached.
  • FIG. 5 is a schematic diagram showing the position of the surface of the heat-resistant intermediate layer in the cross section of a laminated film where the probe is installed in measuring the displacement of the probe using an atomic force microscope to which a cantilever (probe) with a heating mechanism can be attached.
  • a cantilever probe
  • FIG. 5 is a schematic diagram showing the position of the surface of the heat-resistant intermediate layer in the cross section of a laminated film where the probe is installed in measuring the displacement of the probe using an atomic force microscope to which a cantilever (probe) with a heating mechanism can be attached.
  • a cantilever probe
  • the protective film of the present invention is a protective film used for a battery including an electrode having a metal foil and an active material layer positioned on the surface of the metal foil, and the electrode is exposed to a metal foil exposed metal foil.
  • the protective film is used to protect at least part of the periphery of the portion where the exposed portion of the metal foil of the electrode and the metal terminal are welded, and the protective film has at least a first adhesive property. 1 heat-weldable resin layer, heat-resistant intermediate layer, and second heat-weldable resin layer are provided in this order, and the first heat-weldable resin layer constitutes one surface of the protective film. It is characterized by that.
  • the protective film of the present invention, the battery using the protective film, and the production methods thereof will be described in detail.
  • the numerical range indicated by “to” means “above” or “below”.
  • the notation of 2 to 15 mm means 2 mm or more and 15 mm or less.
  • the protective film of the present invention protects at least a part of the periphery of a portion where the exposed portion of the metal foil of the electrode is welded (hereinafter, also referred to as “welded portion” or “part to be welded”) in the battery. Used to do.
  • the battery includes electrodes (positive electrode and negative electrode) in which an active material layer is formed on the surface of a metal foil. Further, the electrode is provided with a metal foil exposed portion where the metal foil of the electrode is exposed. Specifically, the electrode is provided with a metal foil exposed portion where the active material layer is not present and the metal foil of the electrode is exposed. Further, the exposed portion of the metal foil is welded to a conductive member such as a metal terminal so that the inside and the outside of the battery are electrically connected.
  • FIG. 1 a plurality of metal foils 20 of an electrode are stacked at a metal foil exposed portion 21, and a schematic diagram when welding the metal foil exposed portions 21 and the metal terminals 30 of the plurality of metal foils 20 by a welding head 40 is illustrated. The figure is shown.
  • the metal foil exposed portion 21 of the metal foil 20 adjacent to the metal terminal 30 is welded to the metal terminal 30, and the plurality of metal foils 20 adjacent to each other is also included. It shows a state of being welded.
  • FIG. 1 is a schematic view of an example of a portion where the metal foil exposed portion 21 of the metal foil 20 of the electrode is welded, and the structure of the right end portion of the metal foil exposed portion 21 is omitted.
  • FIG. 1 illustrates a case where a region R surrounded by a broken line is covered with the protective film 10 of the present invention.
  • the region R scatters.
  • the periphery of the weld P can be effectively protected from the fine metal pieces.
  • the at least part of the periphery of the welded portion (welded portion P) means, for example, the vicinity of the welded portion P, the vicinity thereof, a range in which fine metal pieces are likely to be scattered, or the like.
  • the protective film 10 When covering at least a part of the periphery of the welded portion P with the protective film 10 of the present invention, the protective film 10 has the surface of the first heat-welding resin layer 1 on the metal foil exposed portion 21 side, and the second heat It arrange
  • the protective film 10 of the present invention By disposing the protective film 10 of the present invention in this way, the surface of the first heat-welding resin layer 1 having adhesiveness can be suitably fixed around the welded portion P. That is, the protective film of the present invention is used so that the first heat-welding resin layer 1 side of the protective film is in contact with a part of the periphery of the portion where the metal foil exposed portion 21 and the metal terminal 30 are welded. .
  • the second heat-weldable resin layer 2 constitutes a surface opposite to the first heat-weldable resin layer 1
  • the generated high-temperature metal piece can be captured by being thermally welded to the surface of the second heat-weldable resin layer 2. Since the heat-welded metal piece is not easily detached from the surface of the second heat-weldable resin layer 2, the periphery of the welded portion P can be more effectively protected.
  • the welding method is not particularly limited, and conventionally known welding methods such as ultrasonic welding and laser welding can be used.
  • the battery in which the protective film of the present invention is used is, for example, as shown in the schematic diagram of FIG. 7, at least an electrode having a metal foil 20 and an active material layer 22 on the surface of the metal foil 20,
  • the battery element including the electrolyte and the like has a structure accommodated in the package formed by the packaging material 50.
  • the electrode includes a positive electrode and a negative electrode, and a separator 23 is disposed between the positive electrode and the negative electrode.
  • the inside 50 a of the battery means a region where the battery element is accommodated by the packaging material 50
  • the outside 50 b of the battery means the outside of the packaging material 50.
  • the inside 50a and the outside 50b of the battery are isolated from each other through a package.
  • the protective film 10 of the present invention includes, for example, at least a first heat-welding resin layer 1 having adhesiveness, a heat-resistant intermediate layer 3, and a second heat as shown in the schematic diagrams of FIGS. It is comprised by the laminated body provided with the weldable resin layer 2 in this order.
  • the first heat weldable resin layer 1 constitutes one surface of the protective film 10.
  • a laminated body provided with a first heat-welding resin layer 1 / heat-resistant intermediate layer 3 / second heat-welding resin layer 2 in this order as shown in FIG.
  • Structure Laminated structure including first heat-welding resin layer 1 / heat-resistant intermediate layer 3 / thermoplastic resin layer 4 / second heat-welding resin layer 2 in this order as shown in FIG. 3; shown in FIG.
  • a laminated structure comprising the first heat-welding resin layer 1 / thermoplastic resin layer 4 / heat-resistant intermediate layer 3 / second heat-welding resin layer 2 in this order; first heat-welding property as shown in FIG.
  • Examples include a laminated structure including resin layer 1 / thermoplastic resin layer 4 / heat-resistant intermediate layer 3 / thermoplastic resin layer 4 / second heat-weldable resin layer 2 in this order.
  • the second heat-weldable resin layer 2 may include a pressure-sensitive adhesive component and be sticky like the first heat-weldable resin layer 1.
  • the thermoplastic resin layer 4 may have a heat-weldability like the first heat-weld resin layer 1 and the second heat-weld resin layer 2. Other layers different from these layers may be further laminated on the protective film of the present invention.
  • the protective film of the present invention has a first heat-welding resin layer 1 / heat-resistant intermediate layer 3 / as shown in FIG. It is preferable to have a three-layer structure including the second heat-weldable resin layer 2 in this order. Moreover, it is preferable to thicken a protective film from a viewpoint of followable
  • a four-layer laminated structure including a first heat-welding resin layer 1 / heat-resistant intermediate layer 3 / thermoplastic resin layer 4 / second heat-welding resin layer 2 in this order.
  • a laminated structure of four layers comprising the first heat-welding resin layer 1 / thermoplastic resin layer 4 / heat-resistant intermediate layer 3 / second heat-welding resin layer 2 in this order as shown in FIG. 4;
  • a first heat-weldable resin layer 1 / thermoplastic resin layer 4 / heat-resistant intermediate layer 3 / thermoplastic resin layer 4 / second heat-weldable resin layer 2 having a five-layer laminated structure in this order are provided. It is preferable.
  • the first heat-welding resin layer 1 having adhesiveness (containing an adhesive component) is laminated on the heat-resistant intermediate layer 3 via the thermoplastic resin layer 4, thereby improving the adhesive strength between the layers.
  • the protective film of the present invention is preferably a laminated structure of 5 layers having adhesiveness on both sides (including an adhesive component) (specifically, the first heat having adhesiveness).
  • the protective film of the present invention may be colored. Specifically, at least one of the first heat-weldable resin layer 1, the heat-resistant intermediate layer 3, and the second heat-weldable resin layer 2 may be colored. When at least one layer of the protective film of the present invention is colored, it is visually confirmed that at least a part of the periphery of the portion where the exposed portion of the metal foil of the electrode is welded is protected by the protective film of the present invention. It can be easily confirmed.
  • the colorant is not particularly limited, and known pigments, dyes and the like can be used. Specific examples of the colorant include carbon black.
  • the thickness of the protective film of the present invention is preferably about 50 to 200 ⁇ m, more preferably about 80 to 150 ⁇ m, from the viewpoint of reducing the thermal shrinkage in a high temperature environment during welding and further exhibiting excellent insulation. Can be mentioned.
  • the protective film of the present invention preferably has a smaller number of layers, with the lower limit being 3 or more and the preferred upper limit being 5 or less. From the viewpoint of reducing the heat shrinkage rate in a high temperature environment during welding and exhibiting excellent insulating properties, the number of layers of the protective film of the present invention is preferably about 3 to 5, more preferably 3 to 4. Degree.
  • the battery packaging material is, for example, a film-like laminate (laminated film) in which a base layer / barrier layer (generally composed of a metal such as aluminum) / a heat-fusible resin layer is laminated in order.
  • a base layer / barrier layer generally composed of a metal such as aluminum
  • a heat-fusible resin layer is laminated in order.
  • the peripheral portion of the packaging material is heat sealed, so that the battery element such as an electrode is sealed with the packaging material.
  • a protective film is disposed around the portion where the exposed portion of the metal foil of the electrode is welded, and a metal piece scattered by welding adheres to the surface of the protective film. Sealed.
  • the metal foil 20 of the electrode, the protective film 10, the metal piece, and the packaging material are positioned in this order, and when these are sealed in this state, the metal piece becomes the protective film 10 and the packaging material.
  • the metal foil 20 and the barrier layer of the packaging material are electrically connected through the metal piece and a short circuit is caused.
  • the protective film of the present invention having excellent insulating properties can be preferably used.
  • the area of one surface of the protective film of the present invention can be appropriately set according to the size of the portion to be coated.
  • the heat shrinkage of the protective film of the present invention measured under conditions of a test temperature of 200 ° C. and a heating time of 10 seconds.
  • the upper limit is preferably about 10% or less, more preferably about 5% or less, and still more preferably about 4% or less.
  • the lower limit is about 0% or more and about 0.1% or more. It is done.
  • the range of the heat shrinkage rate is preferably about 0 to 10%, about 0 to 5%, about 0 to 4%, about 0.1 to 10%, about 0.1 to 5%, About 1 to 4% can be mentioned.
  • the heat shrinkage rate can be measured by a method based on JIS K 7133: 1999.
  • JIS K 7133 stipulates that the test piece size is 120 mm x 120 mm, but it is possible if the heat shrinkage rate can be measured only with a test piece having a size smaller than the test piece size. For the square test piece close to the test piece size, the heat shrinkage rate is measured in the same manner.
  • the 1st heat weldable resin layer 1 is a layer which comprises the surface of the one side of a protective film. That is, the 1st heat weldable resin layer 1 comprises the outermost layer of the one side of the protective film 10 of this invention.
  • the first heat-welding resin layer 1 has adhesiveness (specifically, it contains an adhesive component). More specifically, the 1st heat weldable resin layer 1 is comprised by the heat weldable resin composition containing the adhesion component.
  • the adhesive component is not particularly limited as long as it can impart adhesiveness to the first heat-weldable resin layer 1, and for example, rosin or hydrogenated rosin, polymerized rosin, rosin ester such as rosin or derivatives thereof; ⁇ - Examples include terpene resins such as pinene, ⁇ -pinene, and limonene; terpene phenol resins, coumarone / indene resins, styrene resins, xylene resins, phenol resins, petroleum resins, hydrogenated petroleum resins, and the like.
  • hydrogenated terpene resin, rosin resin, and petroleum resin are compatible with the elastomer phase of the styrene block copolymer, and are highly effective in improving the adhesion to nonpolar members such as polyolefin.
  • Phenol resins, styrene resins, and the like are compatible with the styrene phase and have the effect of increasing the cohesive force.
  • hydrogenated terpene resin, rosin resin, petroleum resin and xylene-based resin, phenol-based resin, styrene-based resin or the like can be combined to form an adhesive component.
  • amorphous polyolefin can be used as the adhesive component.
  • Amorphous polyolefins include, for example, amorphous polypropylene or copolymers of amorphous propylene and other ⁇ -olefins.
  • Specific examples include propylene / ethylene copolymers, propylene / butene-1 copolymers, propylene. ⁇ Butene-1, ethylene, terpolymer, propylene, hexene-1, octene-1, terpolymer, propylene, hexene-1, 4-methylpentene-1, terpolymer, propylene, hexene -1,4-methylpentene-1, ternary copolymer, polybutene-1, and the like.
  • target amorphous alpha polyolefins those having a number average molecular weight of 20000 or less and a glass transition point of ⁇ 20 ° C. or less having a high content of low molecular weight components are preferred.
  • amorphous polyolefin As the adhesive component, amorphous polyolefin is preferable.
  • amorphous polyolefin examples include REXtac2280 (manufactured by REXtac. LLC).
  • REXtac2280 manufactured by REXtac. LLC
  • the content of REXtac2280 is about 10 parts per 100 parts by weight of the modified polyolefin. It is preferable to set it as about a mass part or about 20 mass parts.
  • the adhesive component may be used alone or in combination of two or more.
  • the proportion of the adhesive component contained in the first heat-welding resin layer 1 is not particularly limited, but the lower limit is preferably about 1% by mass or more, more preferably about 5% by mass or more, and the upper limit is , Preferably about 30% by mass or less, more preferably about 25% by mass or less. Further, the range of the ratio of the adhesive component is preferably about 1 to 30% by mass, about 1 to 25% by mass, about 5 to 30% by mass, and about 5 to 25% by mass. Since the ratio of the pressure-sensitive adhesive component contained in the first heat-welding resin layer 1 has such a value, the protective film of the present invention can exhibit excellent pressure-sensitive adhesive properties, The protective film 10 of the present invention can be suitably fixed.
  • the heat-weldable resin contained in the first heat-weldable resin layer 1 is not particularly limited, but reduces heat shrinkage in a high-temperature environment during welding and exhibits excellent insulation while exhibiting excellent adhesiveness. From the viewpoint of exhibiting the properties, a modified polyolefin (that is, having a polyolefin skeleton) is preferable. A heat-welding resin having a polyolefin skeleton is preferable as a heat-welding resin contained in the first heat-welding resin layer 1 because it has excellent solvent resistance to an electrolytic solution and the like.
  • the resin constituting the first heat-weldable resin layer 1 may or may not include a polyolefin skeleton, but from the above viewpoint, it preferably includes a polyolefin skeleton.
  • the fact that the resin constituting the first heat-welding resin layer 1 contains a polyolefin skeleton can be analyzed by, for example, infrared spectroscopy, gas chromatography mass spectrometry, etc., and the analysis method is not particularly limited. For example, when measuring the infrared spectroscopy at a maleic anhydride-modified polyolefin, a peak derived from maleic acid is detected in the vicinity of the wave number of 1760 cm -1 and near the wave number 1780 cm -1.
  • the modified polyolefin is preferably an acid-modified polyolefin.
  • the acid-modified polyolefin include a polyolefin modified with an unsaturated carboxylic acid or an anhydride thereof.
  • the unsaturated carboxylic acid or anhydride thereof used for acid modification include maleic acid, acrylic acid, itaconic acid, crotonic acid, maleic anhydride, itaconic anhydride and the like.
  • the polyolefin to be modified is not particularly limited, but from the viewpoint of reducing the heat shrinkage in a high temperature environment during welding and exhibiting excellent insulating properties while exhibiting excellent adhesiveness, Low density polyethylene, medium density polyethylene, high density polyethylene, polyethylene such as linear low density polyethylene; homopolypropylene, polypropylene block copolymer (eg, propylene and ethylene block copolymer), polypropylene random copolymer (eg, propylene and ethylene Random copolymers) and other crystalline or amorphous polypropylenes; ethylene-butene-propylene terpolymers.
  • polypropylene is preferable as the polyolefin to be modified.
  • the heat-welding resin contained in the first heat-welding resin layer 1 Among these, modified polyolefins such as maleic anhydride-modified polypropylene and maleic anhydride-modified polyethylene are particularly preferable.
  • the number of the heat-welding resins contained in the first heat-welding resin layer 1 may be one or two or more.
  • the ratio of the heat-welding resin contained in the first heat-welding resin layer 1 is not particularly limited, but the lower limit is preferably about 70% by mass or more, more preferably about 80% by mass or more, and the upper limit. Is preferably about 95% by mass or less, more preferably about 90% by mass or less.
  • the range of the ratio of the heat-welding resin is preferably about 70 to 95% by mass, about 70 to 90% by mass, about 80 to 95% by mass, or about 80 to 90% by mass.
  • the softening point of the first heat-weldable resin layer 1 is preferable. Is about 90 ° C. or lower, more preferably about 80 ° C. or lower. Moreover, as a minimum of the softening point of the 1st heat weldable resin layer 1, about 40 degreeC or more, for example, Preferably 50 degreeC or more is mentioned. Preferable ranges of the softening point of the heat-welding resin layer 1 include about 40 to 90 ° C, about 40 to 80 ° C, about 50 to 90 ° C, and about 50 to 80 ° C. In the present invention, the softening point of the heat-welding resin layer 1 is a value measured in the same manner as the softening point of the heat-resistant intermediate layer described later.
  • the thickness of the first heat-welding resin layer 1 is not particularly limited, but the viewpoint of reducing the heat shrinkage rate in a high-temperature environment during welding and exhibiting excellent insulating properties while exhibiting excellent adhesiveness. Therefore, the lower limit is preferably about 5 ⁇ m or more, more preferably about 10 ⁇ m or more, further preferably about 20 ⁇ m or more, and the upper limit is preferably about 200 ⁇ m or less, more preferably about 100 ⁇ m or less, still more preferably about 50 micrometers or less are mentioned.
  • the thickness range of the first heat-welding resin layer 1 is preferably about 5 to 200 ⁇ m, about 5 to 100 ⁇ m, about 5 to 50 ⁇ m, about 10 to 200 ⁇ m, about 10 to 100 ⁇ m, about 10 to 50 ⁇ m. 20 to 200 ⁇ m, 20 to 100 ⁇ m, and 20 to 50 ⁇ m.
  • the heat resistant intermediate layer 3 is located between the 1st heat weldable resin layer 1 and the 2nd heat weldable resin layer 2, and has ensured the outstanding heat resistance of a protective film.
  • the material constituting the heat-resistant intermediate layer 3 is not particularly limited as long as it has excellent heat resistance.
  • polyester, polyimide, polyamide, epoxy resin, polyvinyl alcohol, polyphenylene sulfide, polyarylate, polycarbonate, acrylic resin, Fluorine resin, silicone resin, phenol resin, polyetherimide, and mixtures and copolymers thereof can be used.
  • polyesters include polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, polybutylene naphthalate, polyethylene isophthalate, copolymerized polyester mainly composed of ethylene terephthalate, and butylene terephthalate mainly composed of repeating units. And the like copolyester.
  • the copolymer polyester mainly composed of ethylene terephthalate is a copolymer polyester that polymerizes with ethylene isophthalate mainly composed of ethylene terephthalate (hereinafter, polyethylene (terephthalate / isophthalate)). ) And polyethylene (terephthalate / decane dicarboxylate).
  • a copolymer polyester mainly composed of butylene terephthalate as a repeating unit specifically, a copolymer polyester that polymerizes with butylene isophthalate having butylene terephthalate as a repeating unit (hereinafter referred to as polybutylene (terephthalate / isophthalate)).
  • polybutylene (terephthalate / adipate) polybutylene (terephthalate / sebacate), polybutylene (terephthalate / decanedicarboxylate), polybutylene naphthalate, and the like.
  • These polyesters may be used individually by 1 type, and may be used in combination of 2 or more type.
  • the material of the heat-resistant intermediate layer 3 polyethylene terephthalate, polyethylene naphthalate, polyimide, polyphenylene sulfide, Examples include aramid, vinylon (polyvinyl alcohol), or polyarylate.
  • middle layer 3 a film, a fiber nonwoven fabric, etc. are mentioned.
  • the heat-resistant intermediate layer 3 is composed of a polyethylene terephthalate film, a polyethylene naphthalate film, a polyimide film, a polyphenylene sulfide fiber nonwoven fabric, an aramid fiber nonwoven fabric, a vinylon (polyvinyl alcohol) fiber nonwoven fabric, or a polyarylate fiber nonwoven fabric. It is preferable.
  • the heat resistant intermediate layer 3 has a probe installed on the surface of the heat resistant intermediate layer 3 in the cross section of the protective film 10 in measuring the displacement of the probe using an atomic force microscope to which a cantilever (probe) with a heating mechanism can be attached.
  • a cantilever probe
  • the probe position should not be lower than the initial value. Is desirable. Since the heat resistant intermediate layer 3 has such characteristics, the heat shrinkage rate in a high temperature environment during welding can be further reduced, and the appearance after heat welding can be made better.
  • the probe 90 is installed at the position Q in the case of the protective film 10 in FIG. 9 (measurement start A in FIG. 8).
  • the cross section at this time is a portion where the cross section of the heat resistant intermediate layer obtained by cutting in the thickness direction so as to pass through the central portion of the protective film is exposed. Cutting can be performed using a commercially available rotary microtome or the like.
  • a cantilever probe
  • a heating mechanism for example, an afm plus system manufactured by ANASIS INSTRUMENTS is used, and a cantilever ThermoLever AN2-200 (spring constant 0.5 to 3 N / m) is used as a probe.
  • the probe tip radius is 30 nm or less
  • the probe deflection setting is ⁇ 4 V
  • the temperature rise rate is 5 ° C./min.
  • the protective film to be measured is in a room temperature (25 ° C.) environment, and the probe 90 heated to 40 ° C. is placed on the surface of the heat resistant intermediate layer in the cross section of the protective film. To start measurement.
  • the protective film of the present invention when the probe was heated from 40 ° C. to 220 ° C. under the conditions that the deflection setting of the probe at the start of measurement was ⁇ 4 V and the temperature rising rate was 5 ° C./min, The position of the probe placed on the surface of the heat-resistant intermediate layer in the cross section does not fall below the initial value (position when the probe temperature is 40 ° C), and further, when heated from 160 ° C to 200 ° C, protection More preferably, the position of the probe placed on the surface of the heat resistant intermediate layer in the cross section of the film does not decrease.
  • the member's heat welding step using the protective film is usually performed by heating to about 160 ° C to 200 ° C. For this reason, when the probe is heated from 160 ° C.
  • the protective film in which the position of the probe placed on the surface of the heat resistant intermediate layer in the cross section of the protective film does not decrease can exhibit particularly high heat resistance.
  • the position of the probe placed on the surface of the heat resistant intermediate layer in the cross section of the protective film does not decrease from the initial value, More preferably, the position of the probe placed on the surface of the heat resistant intermediate layer in the cross section of the protective film does not decrease when heated from 160 ° C. to 200 ° C.
  • the softening point of the heat-resistant intermediate layer 3 is, for example, 90 ° C. or higher, preferably about 160 ° C. or higher, more preferably about 200 ° C. or higher.
  • the upper limit of the softening point of the heat-resistant intermediate layer 3 is not particularly present, and examples thereof include about 250 ° C. or less.
  • Preferable ranges of the softening point of the heat resistant intermediate layer 3 include about 90 to 250 ° C, about 160 to 250 ° C, and about 200 to 250 ° C.
  • the softening point of the heat resistant intermediate layer 3 is a temperature at which the deflection of the probe becomes maximum in the above-described probe displacement measurement.
  • the temperature at which the deflection of the probe is maximized is read for five samples of the heat resistant intermediate layer to be measured.
  • the average value of the three temperatures excluding the minimum value is taken as the softening point.
  • the softening point of the heat-resistant intermediate layer 3 is preferably higher than the softening point of the first heat-welding resin layer 1. Furthermore, the softening point of the heat-resistant intermediate layer 3 is preferably higher than the softening point of the first heat-welding resin layer 1 and the softening point of the second heat-welding resin layer 2.
  • the softening point of the heat-resistant intermediate layer 3 is preferably 30 ° C. or higher, more preferably 60 ° C. or higher, and even more preferably 90 ° C. or higher than the softening point of the first heat-welding resin layer 1. Further, the softening point of the heat-resistant intermediate layer 3 is preferably 8 ° C. or higher, more preferably 30 ° C. or higher, more preferably 90 ° C. or higher than the softening point of the second heat-weldable resin layer 2. .
  • the thickness of the heat-resistant intermediate layer 3 is not particularly limited, but from the viewpoint of reducing the heat shrinkage rate in a high-temperature environment during welding and further exhibiting excellent insulating properties, the lower limit is preferably about 5 ⁇ m or more, More preferably, it is about 10 ⁇ m or more, and the upper limit is preferably about 200 ⁇ m or less, more preferably about 100 ⁇ m or less.
  • the thickness range of the heat resistant intermediate layer 3 is preferably about 5 to 200 ⁇ m, about 5 to 100 ⁇ m, about 10 to 200 ⁇ m, and about 10 to 100 ⁇ m.
  • the basis weight of the nonwoven fabric is not particularly limited, but is a layer adjacent to the heat resistant intermediate layer 3 (for example, the first heat-welding resin layer 1 and the second From the viewpoint of sufficiently impregnating the nonwoven fabric with the heat-welding resin layer 2, the thermoplastic resin layer 4, etc.) and stabilizing the adhesive strength between the layers, the basis weight is preferably small, and the lower limit is preferably about 5 g / m. 2 or more. Further, from the viewpoint of reducing the heat shrinkage rate in a high temperature environment during welding, it is preferable that the basis weight is large, and the upper limit is 30 g / m 2 or less.
  • the weight per unit area is preferably about 5 to 30 g / m 2 , more preferably 7 to 25 g / m 2. There are about two .
  • the second heat weldable resin layer 2 is a layer located on the opposite side of the heat resistant intermediate layer 3 from the first heat weldable resin layer 1.
  • the second heat weldable resin layer 2 is composed of a heat weldable resin composition.
  • the second heat-weldable resin layer 2 constitutes the surface opposite to the first heat-weldable resin layer 1, the high temperature generated during welding.
  • These metal pieces can be supplemented by thermally welding to the surface of the second heat-weldable resin layer 2. Since the heat-welded metal piece is not easily detached from the surface of the second heat-weldable resin layer 2, the periphery of the welded portion can be more effectively protected.
  • the 2nd heat weldable resin layer 2 comprises the surface on the opposite side to the 1st heat weldable resin layer 1.
  • the heat-weldable resin contained in the second heat-weldable resin layer 2 is not particularly limited, but reduces the heat shrinkage rate in a high-temperature environment during welding, exhibits excellent insulating properties, and further generates high temperatures during welding.
  • a modified polyolefin that is, having a polyolefin skeleton
  • the resin constituting the second heat-weldable resin layer 2 may or may not include a polyolefin skeleton, but from the above viewpoint, it preferably includes a polyolefin skeleton.
  • a heat-welding resin having a polyolefin skeleton is preferable as a heat-welding resin contained in the second heat-welding resin layer 2 because it has excellent solvent resistance to an electrolytic solution and the like.
  • the fact that the resin constituting the second heat-weldable resin layer 2 contains a polyolefin skeleton can be analyzed by, for example, infrared spectroscopy, gas chromatography mass spectrometry, etc., and the analysis method is not particularly limited. For example, when measuring the infrared spectroscopy at a maleic anhydride-modified polyolefin, a peak derived from maleic acid is detected in the vicinity of the wave number of 1760 cm -1 and near the wave number 1780 cm -1.
  • the modified polyolefin is preferably an acid-modified polyolefin.
  • the acid-modified polyolefin include a polyolefin modified with an unsaturated carboxylic acid or an anhydride thereof.
  • the unsaturated carboxylic acid or anhydride thereof used for acid modification include maleic acid, acrylic acid, itaconic acid, crotonic acid, maleic anhydride, itaconic anhydride and the like.
  • the polyolefin to be modified is not particularly limited, but reduces the heat shrinkage rate in a high temperature environment during welding, exhibits excellent insulating properties, and further converts a high temperature metal piece generated during welding into a second heat welding resin.
  • polyethylene such as low density polyethylene, medium density polyethylene, high density polyethylene, linear low density polyethylene; homopolypropylene, block copolymer of polypropylene (for example, propylene and ethylene) Block copolymers), random copolymers of polypropylene (eg, random copolymers of propylene and ethylene) and the like; and polypropylene-terpolymers of ethylene-butene-propylene.
  • polypropylene is preferable as the polyolefin to be modified.
  • the heat-weldable resin contained in the second heat-weldable resin layer 2 may be one type or two or more types.
  • the ratio of the heat-weldable resin contained in the second heat-weldable resin layer 2 is not particularly limited, but the lower limit is preferably about 70% by weight or more, more preferably about 80% by weight or more. Is preferably about 95% by mass or less, more preferably about 90% by mass or less.
  • the range of the ratio of the heat-welding resin is preferably about 70 to 95% by mass, about 70 to 90% by mass, about 80 to 95% by mass, or about 80 to 90% by mass.
  • the second heat-weldable resin layer 2 may have adhesiveness as necessary (specifically, an adhesive component may be included).
  • an adhesive component may be included.
  • the 2nd heat weldable resin layer 2 can exhibit adhesiveness similarly to the 1st heat weldable resin layer 1.
  • FIG. When the second heat weldable resin layer 2 constitutes the surface opposite to the first heat weldable resin layer 1, the second heat weldable resin layer 2 contains an adhesive component.
  • the adhesiveness to the periphery of the part where the metal foil exposed part of the electrode is welded can be imparted to both surfaces of the first heat-weldable resin layer 1 and the second heat-weldable resin layer 2 of the protective film 10.
  • the high-temperature metal pieces generated during welding can be suitably adhered and thermally welded and captured by the adhesive force of the second heat-weldable resin layer 2.
  • the adhesive component When the adhesive component is contained in the 2nd heat weldable resin layer 2, it does not restrict
  • the softening point of the second heat-weldable resin layer 2 is preferably about 90 ° C. or less, more preferably about 80 ° C. or less. Moreover, as a minimum of the softening point of the 2nd heat weldable resin layer 2, about 40 degreeC or more, for example, Preferably 50 degreeC or more is mentioned.
  • Preferable ranges of the softening point of the heat-welding resin layer 2 include about 40 to 90 ° C, about 40 to 80 ° C, about 50 to 90 ° C, and about 50 to 80 ° C.
  • the softening point of the heat-welding resin layer 2 is a value measured in the same manner as the softening point of the heat-resistant intermediate layer described above.
  • the thickness of the second heat-weldable resin layer 2 is not particularly limited, but the lower limit is preferably about 5 ⁇ m or more from the viewpoint of reducing the heat shrinkage rate in a high temperature environment during welding and exhibiting excellent insulating properties. More preferably, it is about 10 ⁇ m or more, more preferably about 20 ⁇ m or more, and the upper limit is preferably about 200 ⁇ m or less, more preferably about 100 ⁇ m or less, still more preferably about 50 ⁇ m or less.
  • the thickness range of the second heat-weldable resin layer 2 is preferably about 5 to 200 ⁇ m, about 5 to 100 ⁇ m, about 5 to 50 ⁇ m, about 10 to 200 ⁇ m, about 10 to 100 ⁇ m, about 10 to 50 ⁇ m. 20 to 200 ⁇ m, 20 to 100 ⁇ m, and 20 to 50 ⁇ m.
  • thermoplastic resin layer 4 is a layer laminated
  • the thermoplastic resin layer 4 is preferably laminated between the first heat-welding resin layer 1 and the heat-resistant intermediate layer 3 and between the heat-resistant intermediate layer 3 and the second heat-welding resin layer 2. .
  • One layer of the thermoplastic resin layer 4 may be laminated on the protective film 10, or two or more layers may be laminated.
  • the number of the thermoplastic resin layers 4 in the protective film 10 is preferably about 0 to 2, more preferably about 0 to 1.
  • the thermoplastic resin constituting the thermoplastic resin layer 4 is not particularly limited as long as it has thermoplasticity.
  • the thermoplastic resin include polyolefin, polyester, polyamide, acrylic resin, fluororesin, and silicone resin.
  • the thermoplastic resin layer 4 is preferably made of polyolefin, and more preferably made of modified polyolefin (that is, having a polyolefin skeleton).
  • modified polyolefin the same ones as exemplified in the second heat-weldable resin layer 2 are preferably exemplified. That is, the resin constituting the thermoplastic resin layer 4 may or may not contain a polyolefin skeleton, but from the above viewpoint, it preferably contains a polyolefin skeleton.
  • thermoplastic resin having a polyolefin skeleton is preferable as a thermoplastic resin contained in the thermoplastic resin layer 4 because it has excellent solvent resistance to an electrolytic solution and the like.
  • the fact that the resin constituting the thermoplastic resin layer 4 contains a polyolefin skeleton can be analyzed by, for example, infrared spectroscopy, gas chromatography mass spectrometry, etc., and the analysis method is not particularly limited. For example, when measuring the infrared spectroscopy at a maleic anhydride-modified polyolefin, a peak derived from maleic acid is detected in the vicinity of the wave number of 1760 cm -1 and near the wave number 1780 cm -1.
  • thermoplastic resin layer 4 may have adhesiveness as necessary (specifically, an adhesive component may be included).
  • an adhesive component may be included.
  • the thermoplastic resin layer 4 can exhibit adhesiveness similarly to the 1st heat weldable resin layer 1.
  • FIG. When the adhesive component is contained in the thermoplastic resin layer 4, it does not restrict
  • the softening point of the thermoplastic resin layer 4 is preferably about 90 ° C. or less, more preferably about 80 ° C. or less. Moreover, as a minimum of the softening point of the thermoplastic resin layer 4, about 40 degreeC or more, for example, Preferably about 50 degreeC or more is mentioned. Preferable ranges of the softening point of the thermoplastic resin layer 4 include about 40 to 90 ° C, about 40 to 80 ° C, about 50 to 90 ° C, and about 50 to 80 ° C. In the present invention, the softening point of the thermoplastic resin layer 4 is a value measured in the same manner as the softening point of the heat-resistant intermediate layer described above.
  • the thickness of the thermoplastic resin layer 4 is not particularly limited, but the lower limit is preferably about 5 ⁇ m or more from the viewpoint of reducing the heat shrinkage rate in a high temperature environment during welding and further exhibiting excellent insulating properties. More preferably, it is about 10 ⁇ m or more, more preferably about 20 ⁇ m or more, and the upper limit is preferably about 200 ⁇ m or less, more preferably about 100 ⁇ m or less, and further preferably about 50 ⁇ m or less.
  • the thickness range of the thermoplastic resin layer 4 is preferably about 5 to 200 ⁇ m, about 5 to 100 ⁇ m, about 5 to 50 ⁇ m, about 10 to 200 ⁇ m, about 10 to 100 ⁇ m, about 10 to 50 ⁇ m, about 20 to Examples thereof include about 200 ⁇ m, about 20 to 100 ⁇ m, and about 20 to 50 ⁇ m.
  • these thicknesses mean the thickness of one layer of the thermoplastic resin layer 4.
  • the protective film 10 of the present invention is further laminated with other layers different from the first heat weldable resin layer 1, the second heat weldable resin layer 2, the heat resistant intermediate layer 3, and the thermoplastic resin layer 4. May be.
  • the protective film 10 of the present invention may contain various additives such as a lubricant, an antioxidant, an ultraviolet absorber, and a light stabilizer as necessary.
  • the protective film 10 may be discolored depending on the type and content of the additive.
  • the protective film 10 of the present invention comprises at least a first heat-welding resin layer 1, a heat-resistant intermediate layer 3, a second heat-welding resin layer 2, and a thermoplastic resin layer 4 provided as necessary. It can be manufactured by laminating.
  • a method for laminating these layers is not particularly limited, and for example, a thermal lamination method, a sandwich lamination method, an extrusion lamination method, or the like can be used.
  • middle layer 3 when the heat resistant intermediate
  • the adhesion strength with adjacent layers for example, the first heat-weldable resin layer 1, the second heat-weldable resin layer 2, the thermoplastic resin layer 4, etc.
  • the surface of the heat-resistant intermediate layer 3 can be provided with well-known easy adhesion means such as corona discharge treatment, ozone treatment, plasma treatment, etc., if necessary.
  • adhesion promoter for forming the adhesion promoter layer
  • known adhesion promoters such as isocyanate, polyethyleneimine, polyester, polyurethane, and polybutadiene can be used.
  • the adhesion promoter layer can also be formed using a known adhesive such as a two-component curable adhesive or a one-component curable adhesive.
  • a known adhesive such as a two-component curable adhesive or a one-component curable adhesive.
  • the isocyanate-based adhesion promoter those composed of an isocyanate component selected from a triisocyanate monomer and polymeric MDI are excellent in laminate strength and have a small decrease in laminate strength after being immersed in an electrolytic solution.
  • triphenylmethane-4,4 ′, 4 ′′ -triisocyanate which is a triisocyanate monomer
  • polymethylene polyphenyl polyisocyanate which is a polymeric MDI (with an NCO content of about 30% and a viscosity of 200 to 700 mPa ⁇ s).
  • tri-isocyanate monomer such as tris (p-isocyanate phenyl) thiophosphate or a polyethyleneimine-based adhesive and a polycarbodiimide as a crosslinking agent. It is also preferable to form with an accelerator.
  • the adhesion promoter layer can be provided on one side or both sides of the heat resistant intermediate layer 3.
  • the adhesion promoter layer can be formed by coating and drying by a known coating method such as a bar coating method, a roll coating method, or a gravure coating method.
  • the application amount of the adhesion promoter is 20 to 100 mg / m 2 , preferably 40 to 60 mg / m 2 in the case of the adhesion promoter made of triisocyanate, and 40 in the case of the adhesion promoter made of polymeric MDI.
  • the upper limit of the coating amount is preferably about 10 g / m 2 or less, and the lower limit is preferably about 1 g / m 2 .
  • the triisocyanate monomer is a monomer having three isocyanate groups in one molecule, and the polymeric MDI is a mixture of MDI and MDI oligomer obtained by polymerizing MDI, and is represented by the following formula.
  • the battery of the present invention includes a battery element including at least a metal foil 20, an electrode having an active material layer 22 on the surface of the metal foil 20, and an electrolyte.
  • 50 has a structure housed in a package formed by the The electrode includes a positive electrode and a negative electrode, and a separator 23 is disposed between the positive electrode and the negative electrode.
  • the inside 50 a of the battery means a region where the battery element is accommodated by the packaging material 50
  • the outside 50 b of the battery means the outside of the packaging material 50.
  • the inside 50a and the outside 50b of the battery are isolated from each other through a package.
  • the electrode is provided with a metal foil exposed portion where the metal foil is exposed, and at least part of the periphery of the portion where the metal foil exposed portion of the electrode and the metal terminal are welded is covered with the protective film 10 of the present invention.
  • the battery of the present invention includes electrodes (positive electrode and negative electrode) in which an active material layer is formed on the surface of a metal foil.
  • the electrode is provided with a metal foil exposed portion 21 (the active material layer 22 is not present) from which the metal foil 20 of the electrode is exposed.
  • the metal foil 20 and the conductive member such as the metal terminal 30 are welded (welded portion P). Thereby, the inside and the outside of the battery are electrically connected.
  • the positive electrode and the negative electrode are disposed via a separator.
  • the electrode is usually wound or laminated and accommodated in the packaging material.
  • the battery of the present invention usually includes a plurality of laminates in which a positive electrode and a negative electrode are laminated via a separator, and each of the metal foil exposed portions 21 of the positive electrode or the negative electrode has a plurality of metal foils 20. Are stacked.
  • a conductive member such as a metal terminal 30 is welded to the metal foil 20 at a portion where a plurality of metal foils 20 of the electrode are laminated.
  • the portion of the present invention At least part of the periphery of the portion (corresponding to the welded portion P) where the metal foil exposed portion 21 provided on the electrode and the conductive member such as the metal terminal 30 are welded is the portion of the present invention. It is covered with a protective film 10 (region R).
  • the packaging material that accommodates battery elements such as electrodes and electrolytes may be made of metal or a laminated film in which a base material layer / barrier layer / heat-fusible resin layer are sequentially laminated.
  • the battery of the present invention includes a step of covering at least a part of the periphery of a portion where the metal foil exposed portion 21 of the electrode and the metal terminal 30 are welded with the protective film 10 of the present invention, and the metal foil exposed portion 21 is made of metal. It can manufacture by the method provided with the process of welding with the terminal 30.
  • FIG. Examples of the method of covering with the protective film 10 of the present invention include a method of attaching the surface of the first heat-weldable resin layer 1 of the protective film 10 of the present invention to at least a part around the welded portion as described above. .
  • the protective film 10 of this invention can be suitably fixed to the circumference
  • the welding method is not particularly limited, and ultrasonic welding, laser welding, or the like can be employed.
  • the portion covered with the protective film 10 of the present invention may be a part of the periphery of the portion where the exposed metal foil portion of the electrode is welded, or the entire portion. What is necessary is just to select suitably the place which can suppress that the fine metal piece which generate
  • the active material layer of the battery can be composed of a known material such as an active material, a conductive aid, and a binder, and various combinations are known.
  • the active material used for the positive electrode include LiCoO 2 , LiMn 2 O 4 , LiNiO 2 , LiFeO 2 , Li 4 Ti 5 O 12 , LiFePO 4 , LiNi 1/3 Mn 1/3 Co 1 /
  • positive electrode active materials such as lithium transition metal composite oxides such as 3 O 2 and LiNi 0.80 Co 0.15 Al 0.05 O 2 . Only one type of positive electrode active material may be used, or two or more types may be mixed and used.
  • active materials used in the negative electrode include natural graphite, artificial graphite, amorphous carbon, carbon black, carbon materials obtained by adding different elements to these components, metallic lithium and its alloys, tin, silicon And materials that can occlude and release alkali metal ions, such as alloys thereof, oxides of tin, silicon, and titanium. Only one type of negative electrode active material may be used, or two or more types may be mixed and used.
  • the conductive assistant include conductive carbon black such as graphite, furnace black, acetylene black, and ketjen black, carbon fiber such as carbon nanotube, or metal powder. Only one type of conductive assistant may be used, or two or more types may be used in combination.
  • binder examples include polyvinylidene fluoride, styrene / butadiene rubber, polyamide, polyimide, and polyacrylic acid. Only one type of binder may be used, or two or more types may be mixed and used.
  • the battery of the present invention may be either a primary battery or a secondary battery, but is preferably a secondary battery.
  • the type of secondary battery is not particularly limited.
  • lithium ion battery, lithium ion polymer battery, lead storage battery, nickel / hydrogen storage battery, nickel / cadmium storage battery, nickel / iron storage battery, nickel / zinc storage battery, silver oxide / A zinc storage battery, a metal air battery, a polyvalent cation battery, a capacitor, a capacitor, etc. are mentioned.
  • a lithium ion battery and a lithium ion polymer battery are preferable.
  • the softening point of the resin is a value measured by the following method.
  • the softening point was measured by measuring the displacement of the probe using an atomic force microscope to which a cantilever (probe) with a heating mechanism can be attached.
  • a probe was placed on the surface of the heat resistant intermediate layer in the cross section of the protective film.
  • the cross section at this time is a portion where the cross section of the heat resistant intermediate layer obtained by cutting in the thickness direction so as to pass through the central portion of the protective film is exposed. Cutting was performed using a commercially available rotary microtome or the like.
  • a cantilever probe
  • ANASIS INSTRUMENTS As an atomic force microscope to which a cantilever (probe) with a heating mechanism can be attached, an afm plus system manufactured by ANASIS INSTRUMENTS is used, and a cantilever ThermoLever AN2-200 (spring constant 0.5 to 3 N / m) is used as a probe. did.
  • the probe tip radius was 30 nm or less, the probe deflection setting was -4 V, and the temperature elevation rate was 5 ° C./min.
  • the probe is heated in this state, the surface of the heat-resistant intermediate layer is expanded by the heat from the probe, the probe is pushed up, and the probe position is the initial value (when the probe temperature is 40 ° C.). Position).
  • the protective film to be measured was in a room temperature (25 ° C.) environment, and the measurement was started by placing the probe heated to 40 ° C. on the surface of the heat resistant intermediate layer.
  • the softening point of the heat resistant intermediate layer was the temperature at which the deflection of the probe was maximized in measuring the displacement of the probe.
  • the temperature when the deflection of the probe is maximized is read, and the maximum and minimum values of the five temperatures are read. The average value of the three temperatures excluding was used as the softening point.
  • the main surface 1a of the first heat-weldable resin layer of the protective film (specifically, the heat-resistant intermediate layer side of the first heat-weldable resin layer) A probe was placed on the surface on the opposite side (see FIG. 10), and the measurement was performed in the same manner as the measurement of the softening point of the heat-resistant intermediate layer.
  • a probe is set on the surface of the second heat-welding resin layer in the cross section of the protective film, and the measurement is performed in the same manner as the softening point of the heat-resistant intermediate layer. Went.
  • Example 1 A heat-welding resin containing an adhesive component and a maleic anhydride-modified polyethylene resin on one surface of a nonwoven fabric (weight per unit area: 14 g / m 2 , thickness: 60 ⁇ m, softening point: 160 ° C. or higher) as a heat-resistant intermediate layer
  • the composition was extruded and applied to a thickness of 30 ⁇ m with a T-die extruder to form a first heat-weldable resin layer (adhesive PEa, softening point 54 ° C.).
  • maleic anhydride-modified polypropylene resin is extruded and applied to a thickness of 30 ⁇ m with a T-die extruder on the other surface of the heat-resistant intermediate layer, and a second heat-welding resin layer (PPa, softening point 75 ° C.) is applied.
  • a protective film in which the second heat-weldable resin layer (PPa, thickness 30 ⁇ m) was laminated in this order was obtained.
  • Example 2 Except that a polyethylene naphthalate (PEN) film (thickness 12 ⁇ m, softening point 160 ° C. or higher) was used as the heat-resistant intermediate layer, the adhesive layer (including the adhesive component) was used in the same manner as in Example 1. A protective film in which 1 heat-weldable resin layer (adhesive PEa, 30 ⁇ m) / heat-resistant intermediate layer (PEN, thickness 12 ⁇ m) / second heat-weldable resin layer (PPa, thickness 30 ⁇ m) is laminated in this order is obtained. It was.
  • PEN polyethylene naphthalate
  • Example 3 On one side of a polyethylene naphthalate (PEN) film (thickness 12 ⁇ m, softening point 160 ° C. or higher) as a heat-resistant intermediate layer, maleic anhydride-modified polypropylene resin is extruded and applied to a thickness of 30 ⁇ m with a T-die extruder. A thermoplastic resin layer (PPa, softening point 75 ° C.) was formed.
  • PEN polyethylene naphthalate
  • thermoplastic resin layer a heat-welding resin composition containing an adhesive component and maleic anhydride-modified polyethylene is extruded and applied to a thickness of 30 ⁇ m with a T-die extruder, and the first heat-welding resin layer ( Adhesive PEa, softening point 54 ° C.) was formed.
  • Adhesive PEa softening point 54 ° C.
  • maleic anhydride-modified polypropylene resin is extruded and applied to a thickness of 30 ⁇ m with a T-die extruder on the other surface of the heat-resistant intermediate layer, and a second heat-welding resin layer (PPa, softening point 75 ° C.) is applied.
  • PPa softening point 75 ° C.
  • First heat-weldable resin layer (adhesive PEa, thickness 30 ⁇ m) / thermoplastic resin layer (PPa, thickness 30 ⁇ m) / heat-resistant intermediate layer (PEN, thickness) 12 ⁇ m) / second heat-weldable resin layer (PPa, thickness 30 ⁇ m) was obtained in this order.
  • Example 4 Adhesiveness was the same as in Example 1 except that a non-woven fabric (weight per unit area 15 g / m 2 , thickness 25 ⁇ m, softening point 160 ° C. or higher) made of polyphenylene sulfide (PPS) resin was used as the heat resistant intermediate layer.
  • First heat-welding resin layer (adhesive PEa, 30 ⁇ m) / heat-resistant intermediate layer (PPS nonwoven fabric, basis weight 15 g / m 2 , thickness 25 ⁇ m) / second heat-welding resin layer ( A protective film in which PPa and a thickness of 30 ⁇ m were laminated in this order was obtained.
  • Example 5 In Example 3, except that the maleic anhydride-modified polypropylene resin forming the second heat-weldable resin layer (PPa, softening point 75 ° C.) was colored black by blending a colorant (carbon black),
  • the first heat-welding resin layer (adhesive PEa, thickness 30 ⁇ m) having adhesiveness (including an adhesive component) / thermoplastic resin layer (PPa, thickness 30 ⁇ m) / heat-resistant intermediate A protective film in which a layer (PEN, thickness 12 ⁇ m) / second heat-weldable resin layer (PPa, black, thickness 30 ⁇ m) was laminated in this order was obtained.
  • Adhesiveness in the same manner as in Example 1 except that a nonwoven fabric made of polyethylene fibers (PE nonwoven fabric, basis weight 10 g / m 2 , thickness 25 ⁇ m, softening point 50 ° C.) was used as the intermediate layer.
  • First heat-weldable resin layer (adhesive PEa, thickness 30 ⁇ m) / intermediate layer (PE nonwoven fabric, basis weight 10 g / m 2 , thickness 25 ⁇ m) / second heat-weldable resin layer (PPa, thickness 30 ⁇ m) ) was obtained in this order.
  • Comparative Example 2 A commercially available acrylic adhesive tape (Nichiban manufactured by Nichiban Co., Ltd., thickness: 90 ⁇ m) was used as a protective film.
  • a packaging material composed of a laminated film was produced by the following procedure.
  • One surface of an aluminum foil (thickness 40 ⁇ m) and a biaxially stretched nylon film (thickness 25 ⁇ m) were laminated via a urethane adhesive (thickness 4 ⁇ m).
  • the other side of the aluminum foil and an unstretched polypropylene film (thickness 30 ⁇ m) are sandwich-laminated with an acid-modified polypropylene resin (thickness 15 ⁇ m, polypropylene graft-modified with an unsaturated carboxylic acid), and acid is applied with hot air.
  • the obtained packaging material was cut into a size of 150 mm in length (MD) ⁇ 60 mm in width (TD).
  • one protective film cut to a size of length 150 mm (MD) ⁇ width 60 mm (TD) was prepared.
  • a nickel terminal having a length of 100 mm, a width of 5 mm, and a thickness of 0.1 mm and a nickel wire having a length of 100 mm and ⁇ 24 ⁇ m were prepared.
  • the method for evaluating the insulating property will be described with reference to the schematic diagram of FIG.
  • the first heat-welding resin layer side of the protective film 10 was overlapped on the surface of the packaging material 50 on the unstretched polypropylene film side so that the length direction and the width direction coincided.
  • the surface opposite to the adhesive surface of the acrylic adhesive tape was overlapped.
  • this was folded in half so that the protective film 10 was inside at the center in the length direction.
  • the wires 70 were placed on the nickel terminals 60 so that the respective length directions coincided, and the ends were fixed with tape so that the wires 70 would not move.
  • the nickel terminal 60 on which the wire 70 was placed was inserted between the protective film 10 folded in half.
  • a tester HOKI 3154 DIGITAL M ⁇ HiTESTER
  • the positive electrode was connected to the nickel terminal 60
  • the negative electrode was connected to the aluminum foil of the packaging material 50.
  • the negative electrode was connected to the aluminum foil of the packaging material 50 by sandwiching the packaging material 50 with the alligator clip and penetrating the alligator clip to the aluminum foil.
  • adhesive PEa means a first heat-weldable resin layer composed of a maleic anhydride-modified polyethylene resin composition containing an adhesive component
  • PPa is a maleic anhydride-modified polypropylene resin. It means the second heat-weldable resin layer formed.
  • PEN means polyethylene naphthalate
  • PPS nonwoven fabric means a nonwoven fabric made of polyphenylene sulfide (PPS) resin
  • PE nonwoven fabric means a nonwoven fabric made of polyethylene.
  • a first heat-welding resin layer having adhesiveness (containing an adhesive component), a heat-resistant intermediate layer, and a second heat-welding resin layer are provided in this order.
  • the protective films of Examples 1 to 4 in which the first heat-welding resin layer constitutes one surface of the protective film have low thermal shrinkage in a high temperature environment and excellent insulation properties.
  • the thermal contraction rate and insulation evaluation of the protective film of Example 5 were the same as those of Example 3.
  • middle layer has a high heat shrinkage rate, and its insulation property is also low.
  • the comparative example 2 using an acrylic adhesive tape has low insulation.
  • SYMBOLS 1 1st heat-welding resin layer 1a which has adhesiveness (it contains an adhesion component) 2 Main surface of 1st heat-welding resin layer 2 2nd heat-welding resin layer 3 Heat resistant intermediate
  • middle layer 4 Thermoplastic resin layer 10 Protective film 20 Metal foil 21 Metal foil exposed part 22 Active material layer 23 Separator 30 Metal terminal 40 Welding head 50 Packaging material 50a Battery inside 50b Battery outside 60 Nickel terminal 70 Wire 80 Metal bar 90 Probe P Welding part Q Cross section of laminated film Position R of the surface of the heat-resistant intermediate layer of R

Landscapes

  • Engineering & Computer Science (AREA)
  • Power Engineering (AREA)
  • General Chemical & Material Sciences (AREA)
  • Chemical & Material Sciences (AREA)
  • Electrochemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Manufacturing & Machinery (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Secondary Cells (AREA)
  • Laminated Bodies (AREA)
  • Electric Double-Layer Capacitors Or The Like (AREA)
  • Connection Of Batteries Or Terminals (AREA)
  • Sealing Battery Cases Or Jackets (AREA)

Abstract

L'invention fournit un film protecteur qui permet d'être fixé de manière adéquate à la périphérie d'une portion sur laquelle une partie exposition de feuille métallique d'une électrode est soudée, à l'intérieur d'une batterie, et qui en outre présente une faible contraction thermique sous l'effet de hautes températures lors du soudage, et d'excellentes propriétés d'isolation. Plus précisément, l'invention concerne un film protecteur qui est mis en œuvre dans une batterie équipée d'une électrode possédant une feuille métallique, et une couche de matière active positionnée à la surface de ladite feuille métallique. La partie exposition de feuille métallique telle que ladite feuille métallique est exposée, est agencée sur ladite électrode. Ledit film protecteur est mis en œuvre afin de protéger au moins partiellement la périphérie de la portion soudure d'une borne métallique et de ladite partie exposition de feuille métallique de ladite électrode. Ledit film protecteur est équipé dans l'ordre, au moins d'une première couche de résine thermocollante dotée de propriétés adhésives, d'une couche intermédiaire résistante à la chaleur, et d'une seconde couche de résine thermocollante. La première couche de résine thermocollante configure une surface d'un côté dudit film protecteur.
PCT/JP2018/001269 2017-01-17 2018-01-17 Film protecteur, batterie, et procédé de fabrication de batterie Ceased WO2018135545A1 (fr)

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JP2018563373A JP7024734B2 (ja) 2017-01-17 2018-01-17 保護フィルム、電池、及び電池の製造方法

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