WO2023189693A1 - 電池およびその製造方法 - Google Patents

電池およびその製造方法 Download PDF

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Publication number
WO2023189693A1
WO2023189693A1 PCT/JP2023/010502 JP2023010502W WO2023189693A1 WO 2023189693 A1 WO2023189693 A1 WO 2023189693A1 JP 2023010502 W JP2023010502 W JP 2023010502W WO 2023189693 A1 WO2023189693 A1 WO 2023189693A1
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Prior art keywords
solid electrolyte
battery
negative electrode
positive electrode
resin sheet
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English (en)
French (fr)
Japanese (ja)
Inventor
拓海 大塚
優太 佐藤
雄介 川端
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Maxell Ltd
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Maxell Ltd
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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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
    • H01M10/0562—Solid materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00—Primary cells; Manufacture thereof
    • H01M6/14—Cells with non-aqueous electrolyte
    • H01M6/18—Cells with non-aqueous electrolyte with solid electrolyte
    • 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 battery that has a solid electrolyte layer and has excellent reliability and productivity, and a method for manufacturing the same.
  • lithium batteries particularly lithium ion batteries, that can meet this demand use an organic electrolyte solution containing an organic solvent and a lithium salt as a non-aqueous electrolyte.
  • lithium ion batteries With the further development of equipment to which lithium ion batteries can be applied, there is a need for lithium ion batteries to have a longer lifespan, higher capacity, and higher energy density. The reliability of lithium-ion batteries is also in high demand.
  • the organic electrolyte used in lithium-ion batteries contains an organic solvent, which is a flammable substance, there is a possibility that the organic electrolyte will generate abnormal heat if an abnormal situation such as a short circuit occurs in the battery. There is.
  • the recent trend towards higher energy densities in lithium ion batteries and an increase in the amount of organic solvents in organic electrolytes there is a demand for even greater reliability in lithium ion batteries.
  • solid electrolyte batteries such as all-solid batteries that use solid electrolytes (molded bodies thereof) instead of organic electrolytes are attracting attention.
  • Solid electrolyte batteries are highly safe because there is no risk of abnormal heat generation of the solid electrolyte.
  • Goal 3 of the 17 Sustainable Development Goals (SDGs) established by the United Nations, ensuring healthy lives for all people of all ages.
  • Goal 7 (ensure access to affordable, reliable, sustainable and modern energy for all)
  • Goal 11 (ensure inclusive, safe, resilient and sustainable cities and 12 (ensure sustainable production and consumption patterns).
  • Patent Document 1 discloses that in a coin-shaped all-solid-state battery, a conductive layer made of porous metal is placed between the metal case or sealing plate and the electrode, thereby reducing internal resistance and increasing efficiency. Techniques have been proposed to improve charge/discharge characteristics and active material utilization.
  • Patent Document 2 discloses that the side surface of a battery stack in which unit cells having a positive electrode current collector layer, a positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer are stacked in series is insulated.
  • the unit battery is coated with a film, and the insulating film is further provided with an extension extending beyond the end face of the battery laminate in the stacking direction, thereby covering the peripheral edge of the end face of the battery laminate.
  • Techniques have been proposed for suppressing materials from falling off from the edges of each layer constituting the device, thereby preventing the occurrence of short circuits that may be caused by these materials.
  • the present invention has been made in view of the above circumstances, and its purpose is to provide a battery having a solid electrolyte layer and excellent reliability and productivity, and a method for manufacturing the same.
  • the battery of the present invention has a laminated electrode body in which a positive electrode, a negative electrode, and a solid electrolyte layer interposed between the positive electrode and the negative electrode are laminated, and the side surface of the laminated electrode body is at least the side surface of the solid electrolyte layer.
  • the end portion is covered with a resin sheet that is in direct contact with the side surface end portion, and the resin sheet does not extend from the side surface of the laminated electrode body.
  • the battery of the present invention includes a step of laminating a positive electrode, a negative electrode, and a solid electrolyte layer to form a laminated electrode body, placing the laminated electrode body in a tube made of a heat-shrinkable resin sheet, and heating the tube. a step of shrinking and covering at least a side surface end portion of the solid electrolyte layer on the side surface of the laminated electrode body with a heat-shrinkable material of the heat-shrinkable resin sheet, and using the laminated electrode body with the side surface covered
  • the battery can be manufactured by the manufacturing method of the present invention, which is characterized by comprising a step of assembling the battery.
  • the present invention it is possible to provide a battery that has a solid electrolyte layer and has excellent reliability and productivity, and a method for manufacturing the same.
  • FIG. 1 is a cross-sectional view schematically showing an example of a battery of the present invention.
  • a molded body (such as a pellet) of a positive electrode mixture containing a positive electrode active material, a conductive agent, a solid electrolyte, etc., containing the positive electrode active material, a conductive agent, a solid electrolyte, etc. may be used as it is, or this molded body may be used as a positive electrode mixture. It is common to use it by forming it on a current collector as a material layer, and as for the negative electrode, a molded negative electrode mixture containing negative electrode active material, solid electrolyte, etc. can be used as is. This molded body may be used by forming it on a current collector as a negative electrode mixture layer.
  • the mixture components may peel off from the positive electrode mixture molded body or the negative electrode mixture molded body, and the negative electrode mixture may peel off from the negative electrode mixture molded body. Touching may cause a short circuit. Such peeling of the mixture component from the electrode is likely to occur, for example, at the outermost corner of the electrode disposed at the outermost side in the lamination direction of the laminated electrode body.
  • Patent Document 2 an insulating film that covers the side surface of the battery laminate (stacked electrode body) covers up to the peripheral edge of the end face of the battery laminate (the corner of the stacked electrode body), It is intended to suppress the occurrence of short circuits that may occur due to the causes described above.
  • the outermost surface of the laminated electrode body is usually used for collecting current to extract electricity, and if an insulating film is placed on this surface, it will impede current collection. It becomes impossible to exhibit the battery characteristics well.
  • the battery of the present invention at least the entire end portion of the solid electrolyte layer on the side surface of the laminated electrode body formed by laminating the positive electrode, the negative electrode, and the solid electrolyte layer interposed between the positive electrode and the negative electrode is made of resin.
  • the short circuit due to peeling as described above occurs when a part of the peeled mixture component reaches the opposite electrode beyond the side edge of the solid electrolyte layer. Therefore, by covering the side edges of the solid electrolyte layer with the resin sheet, the peeled mixture component cannot come into contact with the counter electrode, so it is possible to highly suppress the occurrence of short circuits.
  • the resin sheet disposed on the side surface of the laminated electrode body is brought into direct contact with the side surface of the laminated electrode body, and preferably, the side surface of the laminated electrode body is directed toward the inside of the laminated electrode body. Make sure to press it. Thereby, the resin sheet can be fixed at a predetermined position on the side surface of the laminated electrode body without using an adhesive or the like. Further, in the battery of the present invention, the resin sheet disposed on the side surface of the laminated electrode body is prevented from extending from the side surface (that is, from protruding from the upper and lower ends of the side surface). This can prevent current collection from being obstructed by the resin sheet. Therefore, in the battery of the present invention, it is possible to suppress the occurrence of short circuits without causing a deterioration in battery characteristics.
  • the battery of the present invention can suppress the occurrence of short circuits during manufacturing and increase its productivity, and can also suppress the occurrence of short circuits during use and increase its reliability. .
  • a laminated electrode body it is sufficient that at least the side edges of the solid electrolyte layer are covered with a resin sheet. Preferably, it is covered with a sheet.
  • the positive electrode, the negative electrode, and the solid electrolyte layer interposed between the positive electrode and the negative electrode that constitute the laminated electrode body preferably have the same shape in plan view. That is, the areas of the positive electrode, negative electrode, and solid electrolyte layer are the same, and on the side surface of the laminated electrode body, the side edge of the positive electrode, the side edge of the negative electrode, and the side edge of the solid electrolyte layer are flat (positive electrode, It is desirable that the negative electrode and the solid electrolyte layer have a polygonal shape in plan view) or a curved surface (in the case that the positive electrode, negative electrode and solid electrolyte layer have a circular or elliptical shape in plan view). In this case, it becomes easier to cover all the side surfaces of the laminated electrode body with the resin sheet.
  • the resin sheet covering the side surface of the laminated electrode body is composed of one sheet, thereby making it easier to manufacture the laminated electrode body.
  • a tube formed of a heat-shrinkable resin sheet as the resin sheet covering the side surface of the laminated electrode body, and to heat-shrink the tube to cover a predetermined location on the side surface of the laminated electrode body.
  • the side surface of the laminated electrode body is covered with the heat-shrinkable material of the heat-shrinkable resin sheet while being pressed toward the inside of the laminated electrode body.
  • Resin sheets used to cover the side surfaces of the laminated electrode body include polyester resins, polystyrene resins, polyolefin resins, polyvinyl chloride resins, polyphenylene sulfide resins, polyether ether ketone resins, fluoride resins, etc. Examples include sheets of known heat-shrinkable resins.
  • the shrinkage temperature of the heat-shrinkable resin sheet is preferably 70°C or higher, more preferably 80°C or higher, preferably 200°C or lower, and 160°C. It is more preferable that it is below.
  • the shrinkage temperature of a heat-shrinkable resin sheet as used herein means the lowest temperature at which the sheet can be heat-shrinked.
  • the thickness of the heat-shrinkable resin sheet is preferably 10 ⁇ m or more, more preferably 20 ⁇ m or more.
  • a heat-shrinkable resin sheet When a heat-shrinkable resin sheet is heat-shrinked, its thickness increases, but if it is as thick as described above before heat-shrinking, even if it is heat-shrinked to cover the sides of the laminated electrode body, it will not break due to the pressing force. It is possible to ensure strength to the extent that such problems do not occur, and it is possible to better suppress short circuits of the battery.
  • the thickness of the heat-shrinkable resin sheet is increased, the effect will be saturated and the amount of components that are not involved in power generation within the battery will increase, so the thickness is preferably 200 ⁇ m or less.
  • the thickness of the sheet after heat-shrinking is about 12 to 300 ⁇ m.
  • the battery of the present invention includes a primary battery and a secondary battery. Moreover, in addition to having a solid electrolyte layer, the battery of the present invention has at least a positive electrode having a positive electrode mixture containing a solid electrolyte, and further, a negative electrode having a negative electrode mixture containing a solid electrolyte, or a negative electrode having a negative electrode mixture containing a solid electrolyte. Preferably, it is an all-solid-state battery with a sheet of metal or alloy acting as the active material.
  • the positive electrode for a battery may be one consisting only of a molded body of a positive electrode mixture containing a positive electrode active material and a solid electrolyte, or a layer (positive electrode mixture layer) consisting of a molded body of the positive electrode mixture. Examples include structures formed on the body.
  • the same positive electrode active material used in conventionally known non-aqueous electrolyte primary batteries can be used.
  • manganese dioxide, lithium-containing manganese oxide for example, LiMn 3 O 6 , or a crystal structure that has the same crystal structure as manganese dioxide ( ⁇ type, ⁇ type, or a structure in which ⁇ type and ⁇ type are mixed)] and a Li content of 3.5% by mass or less, preferably 2% by mass or less, more preferably 1.5% by mass or less, particularly preferably 1% by mass or less
  • Li a Ti Lithium-containing composite oxide such as 5/3 O 4 (4/3 ⁇ a ⁇ 7/3)
  • the battery is a secondary battery
  • the same active material as the positive electrode active material used in conventionally known non-aqueous electrolyte secondary batteries, that is, the active material that can absorb and release Li (lithium) ions. Things can be used.
  • Li 1-x M r Mn 2-r O 4 (where M is Li, Na, K, B, Mg, Ca, Sr, Ba, Ti, V, Cr, Zr, Fe, Co , Ni, Cu, Zn, Al, Sn, Sb, In, Nb, Ta, Mo, W, Y, Ru and Rh, and 0 ⁇ x ⁇ 1,0 ⁇ r ⁇ 1), a spinel-type lithium manganese composite oxide, Li r Mn (1-s-t) Ni s M t O (2-u) F v (where M is Co, Mg, Al , B, Ti, V, Cr, Fe, Cu, Zn, Zr, Mo, Sn, Ca, Sr and W, and 0 ⁇ r ⁇ 1.2, 0 ⁇ s ⁇ 0.5, 0 ⁇ t ⁇ 0.5, u+v ⁇ 1, -0.1 ⁇ u ⁇ 0.2, 0 ⁇ v ⁇ 0.1), Li 1-x Co 1-r M r O 2 (where M is from the group consisting of Al, Mg, Ti, V, Cr, Z
  • Olivine type composite oxide Li 2-x M 1-r N r P 2 O 7 (However, M is at least one element selected from the group consisting of Fe, Mn and Co, and N is Al, Mg, Ti, Zr, Ni, Cu, Zn, Ga, Ge, Nb, Mo , Sn, Sb, V and Ba, and pyrophosphoric acid compounds represented by 0 ⁇ x ⁇ 2, 0 ⁇ r ⁇ 0.5). Only one type of these may be used, or two or more types may be used in combination.
  • the average particle diameter of the positive electrode active material is preferably 1 ⁇ m or more, more preferably 2 ⁇ m or more, and preferably 10 ⁇ m or less, and 8 ⁇ m or less. It is more preferable.
  • the positive electrode active material may be primary particles or secondary particles obtained by agglomerating primary particles. When a positive electrode active material having an average particle diameter in the above range is used, a large number of interfaces with the solid electrolyte contained in the positive electrode can be obtained, thereby further improving the load characteristics of the battery.
  • the average particle diameter of various particles (positive electrode active material, solid electrolyte, etc.) referred to in this specification is measured using a particle size distribution measuring device (such as Microtrac particle size distribution measuring device "HRA9320" manufactured by Nikkiso Co., Ltd.). It means the value of the 50% diameter (D 50 ) of the volume-based integrated fraction when calculating the integrated volume from .
  • a particle size distribution measuring device such as Microtrac particle size distribution measuring device "HRA9320” manufactured by Nikkiso Co., Ltd.
  • the positive electrode active material preferably has a reaction suppression layer on its surface for suppressing reaction with the solid electrolyte contained in the positive electrode.
  • the solid electrolyte may oxidize and form a resistance layer, which may reduce the ionic conductivity within the molded body.
  • a reaction suppression layer is provided on the surface of the positive electrode active material to suppress the reaction with the solid electrolyte, and by preventing direct contact between the positive electrode active material and the solid electrolyte, the ionic conductivity inside the molded body due to oxidation of the solid electrolyte is reduced. The decrease can be suppressed.
  • the reaction suppression layer may be made of a material that has ionic conductivity and can suppress the reaction between the positive electrode active material and the solid electrolyte.
  • materials that can constitute the reaction suppression layer include, for example, oxides containing Li and at least one element selected from the group consisting of Nb, P, B, Si, Ge, Ti, and Zr;
  • Nb-containing oxides such as LiNbO 3 , Li 3 PO 4 , Li 3 BO 3 , Li 4 SiO 4 , Li 4 GeO 4 , LiTiO 3 , LiZrO 3 , Li 2 WO 4 and the like.
  • the reaction suppression layer may contain only one type of these oxides, or may contain two or more types of these oxides, and may further contain multiple types of these oxides in a composite compound. may be formed.
  • these oxides it is preferable to use Nb-containing oxides, and it is more preferable to use LiNbO 3 .
  • the reaction suppression layer is preferably present on the surface in an amount of 0.1 to 1.0 parts by mass based on 100 parts by mass of the positive electrode active material. Within this range, the reaction between the positive electrode active material and the solid electrolyte can be suppressed well.
  • Examples of methods for forming a reaction suppression layer on the surface of the positive electrode active material include a sol-gel method, a mechanofusion method, a CVD method, a PVD method, and an ALD method.
  • the content of the positive electrode active material in the positive electrode mixture is preferably 60 to 98% by mass.
  • the positive electrode mixture can contain a conductive additive.
  • a conductive additive include carbon materials such as graphite (natural graphite, artificial graphite), graphene, carbon black, carbon nanofibers, and carbon nanotubes. Note that, for example, when Ag 2 S is used as the active material, conductive Ag is generated during the discharge reaction, so it is not necessary to include a conductive aid.
  • the content is preferably 1 to 10% by mass.
  • the positive electrode mixture can contain a binder.
  • a binder include fluororesins such as PVDF.
  • PVDF fluororesins
  • good moldability can be achieved in forming a molded body of the positive electrode mixture without using a binder. If it can be ensured, the positive electrode mixture does not need to contain a binder.
  • the content is preferably 15% by mass or less, and preferably 0.5% by mass or more.
  • the content is preferably 0.5% by mass or less, and preferably 0.3% by mass or less. More preferably, the content is 0% by mass (that is, no binder is contained).
  • the solid electrolyte contained in the positive electrode mixture is not particularly limited as long as it has lithium ion conductivity, and includes, for example, a sulfide solid electrolyte, a hydride solid electrolyte, a halide solid electrolyte, and an oxide solid electrolyte. etc. can be used.
  • sulfide-based solid electrolytes include particles such as Li 2 S-P 2 S 5 , Li 2 S-SiS 2 , Li 2 S-P 2 S 5 -GeS 2 , and Li 2 S-B 2 S 3 -based glass.
  • Examples of the hydride solid electrolyte include LiBH 4 , a solid solution of LiBH 4 and the following alkali metal compound (for example, one in which the molar ratio of LiBH 4 and the alkali metal compound is 1:1 to 20:1), and the like. Can be mentioned.
  • Examples of the alkali metal compounds in the solid solution include lithium halides (LiI, LiBr, LiF, LiCl, etc.), rubidium halides (RbI, RbBr, RbF, RbCl, etc.), and cesium halides (CsI, CsBr, CsF, CsCl, etc.). , lithium amide, rubidium amide, and cesium amide.
  • oxide-based solid electrolytes examples include garnet type Li 7 La 3 Zr 2 O 12 , NASICON type Li 1+O Al 1+O Ti 2-O (PO 4 ) 3 , Li 1+p Al 1+p Ge 2-p (PO 4 ) 3 , perovskite-type Li 3q La 2/3-q TiO 3 and the like.
  • sulfide-based solid electrolytes are preferred because they have high lithium ion conductivity, and sulfide-based solid electrolytes containing Li and P are more preferred, particularly those that have high lithium ion conductivity and are chemically stable.
  • An argyrodite-type sulfide-based solid electrolyte having high properties is more preferred.
  • the average particle diameter of the solid electrolyte is preferably 0.1 ⁇ m or more, more preferably 0.2 ⁇ m or more from the viewpoint of reducing grain boundary resistance. From the viewpoint of forming a sufficient contact interface, the thickness is preferably 10 ⁇ m or less, more preferably 5 ⁇ m or less.
  • the content of the solid electrolyte in the positive electrode mixture is preferably 4 to 40% by mass.
  • metal foil such as aluminum or stainless steel, punched metal, net, expanded metal, foamed metal, carbon sheet, etc. can be used as the current collector.
  • the positive electrode mixture molded body is produced by, for example, compressing a positive electrode mixture prepared by mixing a positive electrode active material with a conductive additive, a binder, a solid electrolyte, etc. added as necessary, by pressure molding or the like. can be formed with.
  • a positive electrode having a current collector it can be manufactured by bonding a molded product of the positive electrode mixture formed by the method described above to the current collector by pressing or the like.
  • a positive electrode mixture-containing composition is prepared by mixing the above-mentioned positive electrode mixture and a solvent, and this is applied onto a base material such as a current collector or a solid electrolyte layer facing the positive electrode, and after drying, press processing is performed. By performing this step, a molded body of the positive electrode mixture may be formed.
  • An organic solvent such as water or N-methyl-2-pyrrolidone (NMP) can be used as the solvent for the positive electrode mixture-containing composition.
  • NMP N-methyl-2-pyrrolidone
  • sulfide-based solid electrolytes and hydride-based solid electrolytes cause chemical reactions with minute amounts of water, so hydrocarbon solvents such as hexane, heptane, octane, nonane, decane, decalin, toluene, and xylene are typical.
  • non-polar aprotic solvents are used.
  • a super dehydrated solvent with a water content of 0.001% by mass (10 ppm) or less.
  • fluorinated solvents such as “Vertrell (registered trademark)” manufactured by Mitsui-DuPont Fluorochemicals, “Zeorolla (registered trademark)” manufactured by Nippon Zeon, and “Novec (registered trademark)” manufactured by Sumitomo 3M
  • Non-aqueous organic solvents such as , dichloromethane and diethyl ether can also be used.
  • the molded body of the positive electrode mixture is preferably formed by compressing the positive electrode mixture using pressure molding or the like. , more preferred.
  • the thickness of the molded body of the positive electrode mixture is usually 50 ⁇ m or more, but from the viewpoint of increasing the capacity of the battery, it is preferably 200 ⁇ m or more. Further, the thickness of the molded body of the positive electrode mixture is usually 3000 ⁇ m or less, and preferably 2000 ⁇ m or less from the viewpoint of increasing the output of the battery.
  • the positive electrode mixture layer is preferably 50 to 1000 ⁇ m, and more preferably 500 ⁇ m or less from the viewpoint of increasing the output of the battery.
  • the negative electrode of the battery has, for example, a molded body of a negative electrode mixture containing a negative electrode active material, a lithium sheet, or a lithium alloy sheet.
  • the negative electrode has a molded body of a negative electrode mixture containing a negative electrode active material, a molded body formed by molding the negative electrode mixture (pellet, etc.) or a layer formed from a molded body of the negative electrode mixture (negative electrode mixture layer)
  • a molded body formed by molding the negative electrode mixture pellet, etc.
  • a layer formed from a molded body of the negative electrode mixture negative electrode mixture layer
  • Examples include those having a structure in which the electrode is formed on a current collector.
  • examples of the negative electrode active material include carbon materials such as graphite, simple substances containing elements such as Si and Sn, compounds (such as oxides), and alloys thereof. It will be done. Furthermore, lithium metal and lithium alloys (lithium-aluminum alloy, lithium-indium alloy, etc.) can also be used as the negative electrode active material.
  • the content of the negative electrode active material in the negative electrode mixture is preferably 10 to 99% by mass.
  • a conductive additive can be contained in the negative electrode mixture. Specific examples thereof include the same conductive additives as those exemplified above as those that can be included in the positive electrode mixture.
  • the content of the conductive additive in the negative electrode mixture is preferably 1 to 10% by mass.
  • the negative electrode mixture can contain a binder.
  • a binder Specific examples thereof include the same binders as those exemplified above as those that can be included in the positive electrode mixture. Note that, for example, when a sulfide-based solid electrolyte is contained in the negative electrode mixture (details will be described later), good moldability can be achieved in forming a molded body of the negative electrode mixture without using a binder. If it can be ensured, the negative electrode mixture does not need to contain a binder.
  • a binder When a binder is required in the negative electrode mixture, its content is preferably 15% by mass or less, and preferably 0.5% by mass or more. On the other hand, in the case where moldability can be obtained without the need for a binder in the negative electrode mixture, the content thereof is preferably 0.5% by mass or less, and preferably 0.3% by mass or less. More preferably, the content is 0% by mass (that is, no binder is contained).
  • the negative electrode mixture contains a solid electrolyte.
  • a solid electrolyte include the same solid electrolytes as those exemplified above as those that can be included in the positive electrode mixture.
  • solid electrolytes mentioned above it is more preferable to use a sulfide-based solid electrolyte because it has high lithium ion conductivity and also has a function of improving the moldability of the negative electrode mixture.
  • the content of the solid electrolyte in the negative electrode mixture is preferably 4 to 49% by mass.
  • a current collector When a current collector is used for a negative electrode having a molded body of negative electrode mixture, copper or nickel foil, punched metal, net, expanded metal, foamed metal, carbon sheet, etc. can be used as the current collector. can.
  • a negative electrode mixture molded body is produced by, for example, compressing a negative electrode mixture prepared by mixing a negative electrode active material, a conductive additive, a solid electrolyte, a binder, etc. added as necessary, by pressure molding or the like. It can be formed by In the case of a negative electrode composed only of a molded body of negative electrode mixture, it can be manufactured by the method described above.
  • a negative electrode having a current collector it can be manufactured by bonding a molded body of the negative electrode mixture formed by the method described above to the current collector by pressing or the like.
  • a negative electrode mixture-containing composition in which a negative electrode active material, a conductive additive, a solid electrolyte, a binder, etc. added as necessary, are dispersed in a solvent.
  • a negative electrode mixture-containing composition in which a negative electrode active material, a conductive additive, a solid electrolyte, a binder, etc. added as necessary, are dispersed in a solvent.
  • pressure molding such as calendering as necessary to form a negative electrode mixture molded body (negative electrode mixture layer) on the surface of the current collector. It can also be manufactured by other methods.
  • Organic solvents such as water and NMP can be used as the solvent for the negative electrode mixture-containing composition, but when the negative electrode mixture-containing composition also contains a solid electrolyte, the solvent should be one that does not easily deteriorate the solid electrolyte. It is desirable to select the following, and it is preferable to use the same solvent as the various solvents exemplified above as the solvent for the positive electrode mixture containing composition containing the solid electrolyte.
  • the molded body of the negative electrode mixture is preferably formed by compressing the negative electrode mixture by pressure molding or the like. , more preferred.
  • the thickness of the molded body of the negative electrode mixture is usually 50 ⁇ m or more, but preferably 200 ⁇ m or more from the viewpoint of increasing the capacity of the battery. Further, the thickness of the molded body of the negative electrode mixture is usually 3000 ⁇ m or less, and preferably 2000 ⁇ m or less from the viewpoint of increasing the output of the battery.
  • the negative electrode mixture layer is preferably 50 to 1000 ⁇ m, and more preferably 500 ⁇ m or less from the viewpoint of increasing the output of the battery.
  • alloying elements for lithium alloys include aluminum, lead, bismuth, indium, and gallium, with aluminum and indium being preferred.
  • the proportion of alloying elements in the lithium alloy is preferably 50 atomic % or less (in this case, the remainder is lithium and unavoidable impurities).
  • a layer containing an alloying element to form a lithium alloy is laminated on the surface of a lithium layer (layer containing lithium) made of metal lithium foil, etc.
  • a lithium alloy can be formed on the surface of the lithium layer to form a negative electrode by using the laminate and bringing the laminate into contact with a solid electrolyte in a battery.
  • a laminate having a layer containing an alloying element on only one side of the lithium layer may be used, or a laminate having a layer containing an alloying element on both sides of the lithium layer may be used.
  • the laminate can be formed, for example, by press-bonding a metal lithium foil and a foil made of an alloy element.
  • a current collector can be used when a lithium alloy is formed in a battery to form a negative electrode.
  • a negative electrode current collector has a lithium layer on one side of the negative electrode current collector, and a lithium layer negative electrode current collector
  • a laminate having a layer containing an alloy element on the side opposite to the negative electrode current collector may be used, and has a lithium layer on both sides of the negative electrode current collector, and the side of each lithium layer opposite to the negative electrode current collector.
  • a laminate having a layer containing an alloying element may also be used.
  • the negative electrode current collector and the lithium layer may be laminated by pressure bonding or the like.
  • the layer containing the alloying element of the laminate to be used as the negative electrode for example, a foil made of these alloying elements can be used.
  • the thickness of the layer containing the alloying element is preferably 1 ⁇ m or more, more preferably 3 ⁇ m or more, preferably 20 ⁇ m or less, and more preferably 12 ⁇ m or less.
  • a metal lithium foil or the like can be used for the lithium layer of the laminate to serve as the negative electrode.
  • the thickness of the lithium layer is preferably 0.1 to 1.5 mm.
  • the thickness of the negative electrode sheet having a lithium or lithium alloy sheet is preferably 0.1 to 1.5 mm.
  • the current collector may be one of the current collectors that can be used for a negative electrode having a negative electrode mixture molded body. The same one can be used.
  • the solid electrolytes constituting the solid electrolyte layer interposed between the positive electrode and the negative electrode include the various sulfide-based solid electrolytes, hydride-based solid electrolytes, and halide-based solid electrolytes listed above as those that can be used for the positive electrode. and oxide-based solid electrolytes, or one or more of them can be used.
  • both the positive electrode and the solid electrolyte layer contain a sulfide-based solid electrolyte, and it is particularly desirable that an argyrodite-type sulfide-based solid electrolyte be included.
  • the solid electrolyte layer may have a porous material such as a resin nonwoven fabric as a support.
  • a solid electrolyte layer is formed by compressing a solid electrolyte by pressure molding or the like; a solid electrolyte layer-forming composition prepared by dispersing a solid electrolyte in a solvent is applied onto a base material, a positive electrode, and a negative electrode, and dried. If necessary, it can be formed by a method of performing pressure molding such as press treatment; however, it is more preferable to employ the method of compressing the solid electrolyte described above.
  • the solvent used in the composition for forming a solid electrolyte layer is preferably one that does not easily deteriorate the solid electrolyte, and it is preferable to select a solvent that does not easily deteriorate the solid electrolyte. It is preferable to use the same one.
  • the thickness of the solid electrolyte layer is preferably 10 to 400 ⁇ m.
  • FIG. 1 shows a vertical cross-sectional view schematically showing an example of the battery of the present invention.
  • the battery 1 shown in FIG. A laminated electrode body having two negative electrodes 3, 3 and two solid electrolyte layers 4, 4 is enclosed.
  • a solid electrolyte layer 4 is interposed between the positive electrode 2 on the upper side of the figure and the negative electrode 3 on the upper side of the figure, and between the positive electrode on the lower side of the figure and the negative electrode on the lower side of the figure. ing.
  • a current collector 7 is arranged between the positive electrode 2 on the upper side in the figure of the two positive electrodes constituting the laminated electrode body, and the negative electrode 3 on the lower side in the figure among the two negative electrodes, These positive electrodes 2 and negative electrodes 3 are connected in series. That is, the positive electrode 2 on the upper side in the figure and the negative electrode 3 on the lower side in the figure of the laminated electrode body constitute a bipolar electrode.
  • the side surfaces of the laminated electrode body are covered with a resin sheet 5 that is pressed toward the inside of the laminated electrode body.
  • a resin sheet 5 that is pressed toward the inside of the laminated electrode body.
  • the sealed can 9 also serves as a negative electrode terminal by being electrically connected to the negative electrode 3 on the upper side in the figure via the current collector 6 on its inner surface, and the outer can 8 However, by being electrically connected to the positive electrode 2 on the lower side in the figure via the current collector 6 on its inner surface, it also serves as a positive electrode terminal.
  • the outer can may also serve as the negative electrode terminal, and the sealed can may also serve as the positive electrode terminal.
  • a laminated electrode body related to a battery has one positive electrode, one negative electrode, and one solid electrolyte layer interposed between these positive and negative electrodes, and may be configured by stacking these, Moreover, it may have a plurality of positive electrodes, a plurality of negative electrodes, and a solid electrolyte interposed between these positive electrodes and negative electrodes, and may be configured by stacking these.
  • a laminated electrode body having a plurality of positive electrodes and a plurality of negative electrodes for example, as shown in FIG. 1, some of the positive electrodes and some of the negative electrodes are connected in series with a current collector in between.
  • a bipolar electrode can be constructed in which a solid electrolyte layer is disposed between the other positive electrode and negative electrode.
  • a battery having a laminated electrode body having a plurality of positive electrodes and a plurality of negative electrodes there is no particular restriction on the number of layers of positive electrodes and negative electrodes in the laminated electrode body, and the number of layers of positive electrodes and negative electrodes in the laminated electrode body may be 2, 3, 4, or more as necessary. It can be done.
  • a battery container consisting of an exterior can and a sealed can as shown in FIG. 1 is used. That is, an all-solid-state battery having such a battery container as an exterior body is a coin-shaped (button-shaped) battery.
  • FIG. 1 In the case of a battery container in which the outer body of the battery has an outer can and a sealed can, as shown in FIG. An example is one in which these are bonded together with a resin.
  • Stainless steel can be used for the outer can and sealing can.
  • polypropylene, nylon, etc. can be used as the material for the gasket, and if heat resistance is required due to battery usage, materials such as tetrafluoroethylene-perfluoroalkoxyethylene copolymer (PFA) can be used.
  • Heat-resistant materials with melting points exceeding 240°C such as fluororesin, polyphenylene ether (PPE), polysulfone (PSF), polyarylate (PAR), polyether sulfone (PES), polyphenylene sulfide (PPS), and polyether ether ketone (PEEK) Resins can also be used.
  • a glass hermetic seal can also be used to seal the battery.
  • the shape of the exterior body made of a battery container having an exterior can and a sealing can may be circular or polygonal such as a quadrilateral (square or rectangle) in plan view. Moreover, in the case of a polygon, the corners may be curved.
  • a laminate film exterior body made of a metal laminate film such as an aluminum laminate film or a ceramic container can also be used as the exterior body of the battery.
  • current collectors 6, 6 are arranged on the outermost surface of the stacked electrode body in the stacking direction. Regardless of the type of exterior body used, the current collector can be disposed on at least one of the outermost surfaces of the stacked electrode body in the stacking direction.
  • a molded body of conductive particles (metal particles, carbon particles, etc.) or a foamed metal porous body for the current collector disposed on the outermost surface in the lamination direction of the laminated electrode body.
  • the current collection efficiency is better than, for example, when a current collector made of metal foil (metal plate) with a relatively smooth surface is used.
  • the molded body of the positive electrode mixture and the molded body of the negative electrode mixture have relatively rough surfaces, but the molded bodies of the conductive particles Current collectors made of metal bodies or foam-like porous metal bodies also have relatively rough surfaces, so some of the surface may penetrate inside from the surface of the positive electrode mixture molded body or the negative electrode mixture molded body. This is presumably due to the larger contact area.
  • conductive particles are likely to fall off from a current collector made of a molded body of conductive particles or a foamed metal porous body, and this may cause a short circuit in the battery.
  • a resin sheet preferably pressed toward the inside of the laminated electrode body
  • the current collector is coated with a resin sheet (resin sheet)
  • the occurrence of short circuits can be highly suppressed even when using the current collector in the form described above. Therefore, when the battery of the present invention has a current collector made of a molded body of conductive particles or a foamed metal porous body, the effect becomes particularly remarkable.
  • Metals that do not react with Li can be used as the metal for the molded body of conductive particles and the foamed metal porous body.
  • the molded body of conductive particles include a sintered body of metal particles, a dried coating film formed using carbon paste, and the like.
  • the foamed metal porous body include "Celmet (registered trademark)" manufactured by Sumitomo Electric Industries, Ltd.
  • the current collector disposed on the outermost surface of the laminated electrode body in the lamination direction may be bonded to the outermost electrode (positive electrode or negative electrode) of the laminated electrode body to form the laminated electrode body. It may be overlapped with the laminated electrode body within the battery without being integrated with the electrode body.
  • the thickness of the current collector disposed on the outermost surface of the laminated electrode body in the lamination direction is preferably, for example, 20 to 1000 ⁇ m.
  • the current collector disposed on the outermost surface of the laminated electrode body in the stacking direction.
  • the area area in plan view
  • the area can be made larger than the area of the outermost surface of the laminated electrode body in the lamination direction.
  • the current collector for this bipolar electrode (the current collector disposed between the positive electrode and the negative electrode) also has the above-mentioned conductivity.
  • a molded body of particles, a foamed metal porous body, etc. can be used.
  • the thickness of the current collector related to the bipolar electrode is preferably 50 to 300 ⁇ m, for example.
  • the method for manufacturing a battery of the present invention includes a step of laminating a positive electrode, a negative electrode, and a solid electrolyte layer to form a laminated electrode body (a laminated electrode body forming step), and a step of forming a laminated electrode body from a heat-shrinkable resin sheet. a step of heat-shrinking the tube to cover at least a side end of the solid electrolyte layer on the side surface of the laminated electrode body with a heat-shrinkable material of the heat-shrinkable resin sheet (laminated and a step of assembling a battery using the laminated electrode body whose side surfaces are coated (battery assembly step).
  • the positive electrode, negative electrode, and solid electrolyte layer manufactured by the method described above may be laminated according to a conventional method to form a laminated electrode body.
  • the constituent materials of the solid electrolyte layer solid electrolyte, etc.
  • the positive electrode mixture is formed on one side of the temporary molded body.
  • One of the agent and the negative electrode mixture is placed and pressed at low pressure to form a temporary molded body of the positive electrode mixture or the negative electrode mixture, and then the other mixture is placed on the other side of the temporary molded body of the solid electrolyte layer.
  • a laminated electrode body in which a part of the positive electrode and the negative electrode constitute a bipolar electrode for example, a plurality of unit electrode bodies are formed by laminating the positive electrode, solid electrolyte layer, and negative electrode, and these units A method can be adopted in which electrode bodies are laminated with a current collector interposed therebetween.
  • a method of heat-shrinking a tube formed of a heat-shrinkable resin sheet in order to cover a predetermined part of the side surface of the laminated electrode body there is no particular restriction as long as the sides of the body can be well covered.
  • a method can be adopted in which the tube containing the laminated electrode body is heated by placing it in a general heating furnace.
  • a step of heating and drying is sometimes performed to remove internal moisture, but this step is performed with the laminated electrode body placed in the tube. By subjecting it to water, moisture can be removed and the side surfaces of the laminated electrode body can be covered at the same time.
  • a laminated electrode body whose side surfaces are covered with a heat-shrinkable material made of heat-shrinkable resin sheet is housed inside the exterior body using a method normally adopted depending on the exterior body used, and then the battery is assembled. can be completed.
  • Example 1 ⁇ Preparation of laminated electrode body> Lithium titanate (Li 4 Ti 5 O 12 , negative electrode active material) with an average particle diameter of 2 ⁇ m, sulfide-based solid electrolyte (Li 7.0 PS 6 Cl) with an average particle diameter of 0.7 ⁇ m, and graphene (conductive material) (auxiliary agent) at a mass ratio of 50:41:9 to prepare a negative electrode mixture.
  • Lithium titanate Li 4 Ti 5 O 12 , negative electrode active material
  • sulfide-based solid electrolyte Li 7.0 PS 6 Cl
  • graphene conductive material
  • LiCoO 2 positive electrode active material
  • LiNbO 3 a coating layer of LiNbO 3 formed on the surface
  • Li 7.0 PS 6 Cl a sulfide-based solid electrolyte with an average particle diameter of 3 ⁇ m
  • a positive electrode mixture was prepared by mixing carbon black and vapor grown carbon fiber (VGCF) at a mass ratio of 70:26.8:1.1:2.1.
  • powder of sulfide-based solid electrolyte (Li 7.0 PS 6 Cl) with an average particle size of 0.7 ⁇ m is placed in a powder molding mold, and pressure molded at low pressure using a press machine to form the solid electrolyte. A preformed layer of the layer was formed. Further, the negative electrode mixture was placed on the upper surface of the temporary molded layer of the solid electrolyte layer, and pressure molding was performed at low pressure to further form a temporary formed layer of the negative electrode on the temporary molded layer of the solid electrolyte layer.
  • the positive electrode mixture was placed on the upper surface of the temporary molding layer of the solid electrolyte layer in the mold (the side opposite to the surface with the temporary molding layer of the negative electrode), and the entire pressure was increased to 1300 MPa.
  • pressure molding with a surface pressure of (13 tf/cm 2 )
  • two unit electrode bodies having a thickness of 0.75 mm in which the negative electrode, the solid electrolyte layer, and the positive electrode were integrated were fabricated.
  • a nickel foam metal porous body (“Celmet (registered trademark)" manufactured by Sumitomo Electric Industries, Ltd. was punched out to a size of 10 mm ⁇ .
  • the surface of the positive electrode of one of the two unit electrode bodies and one side of the foamed metal porous body are bonded together, and the surface of the negative electrode of the other unit electrode body and the surface of the foamed metal porous body are bonded together. It has two positive electrodes and two negative electrodes, with one positive electrode and negative electrode forming a bipolar electrode with a current collector in between, and the remaining positive electrode and negative electrode forming a bipolar electrode. obtained a laminated electrode body in which a solid electrolyte layer was interposed.
  • the laminated electrode body was placed in a polyetheretherketone resin sheet tube (thickness 100 ⁇ m, tube opening diameter 9 mm) so that its side surface faced the resin sheet constituting the tube, and heated at 150°C. By doing so, the tube was heat-shrinked, and the side surface of the laminated electrode body was covered with the heat-shrinkable resin sheet. ). Thereafter, the portions of the resin sheet (heat-shrinkable material) protruding from the upper and lower ends of the side surface of the laminated electrode body were cut to prevent the resin sheet from extending from the side surface of the laminated electrode body.
  • ⁇ Battery assembly> Two 10 mm diameter pieces of the same nickel foam metal porous material used for the laminated electrode body were punched out, and one of them was made of stainless steel and fitted with an annular gasket made of polyphenylene sulfide. It was placed on the inner bottom surface of a sealed can. On top of that, the laminated electrode body whose side surfaces are covered with a resin sheet (heat-shrinkable material) is placed so that the side whose outermost surface is the negative electrode is in contact with the foamed metal porous body (current collector). did.
  • a resin sheet heat-shrinkable material
  • an all-solid-state secondary battery (coin-shaped all-solid-state secondary battery) having the structure shown in FIG. 1 was produced.
  • Example 2 An all-solid-state secondary battery was produced in the same manner as in Example 1, except that the current collectors placed between two unit electrode bodies and on both outermost surfaces of the laminated electrode body were changed to aluminum foam metal porous bodies. Created.
  • Example 3 An all-solid-state secondary battery was produced in the same manner as in Example 1, except that the current collectors disposed between two unit electrode bodies and on both outermost surfaces of the laminated electrode body were changed to nickel powder sintered bodies.
  • Example 4 The entire solid state was prepared in the same manner as in Example 1, except that the resin sheet covering the side surface of the laminated electrode body was changed to a polyphenylene sulfide resin sheet tube (thickness 100 ⁇ m, tube opening diameter 9 mm), and the heating temperature was changed to 120°C. A secondary battery was produced.
  • Example 5 The current collectors placed between the two unit electrode bodies and on both outermost surfaces of the laminated electrode body were changed to aluminum foam metal porous bodies, and the resin sheet covering the sides of the laminated electrode body was replaced with tetrafluoroethylene hexane.
  • An all-solid-state secondary battery was produced in the same manner as in Example 1, except that the tube was changed to a fluoropropylene copolymer resin sheet tube (thickness: 100 ⁇ m, tube opening diameter: 9 mm), and the heating temperature was changed to 100° C.
  • Example 6 The current collectors placed between the two unit electrode bodies and on both outermost surfaces of the laminated electrode body were changed to sintered nickel powder, and the resin sheet covering the sides of the laminated electrode body was replaced with a polyphenylene sulfide resin sheet tube (thickness: An all-solid-state secondary battery was produced in the same manner as in Example 1, except that the tube opening diameter was changed to 100 ⁇ m and the tube opening diameter was 9 mm) and the heating temperature was changed to 120° C.
  • Comparative example 1 An all-solid-state secondary battery was produced in the same manner as in Example 1, except that the side surfaces of the laminated electrode body were not covered with a resin sheet.
  • Comparative example 2 An all-solid-state secondary battery was produced in the same manner as in Example 3, except that the side surfaces of the laminated electrode body were not covered with a resin sheet.
  • the presence or absence of short circuits in all-solid-state secondary batteries immediately after manufacture was determined by measuring the battery voltage of 100 all-solid-state secondary batteries of Examples 1 to 6 and Comparative Examples 1 and 2 immediately after manufacture. The evaluation was made by determining that a short circuit had occurred if there was a short circuit.
  • vibration tests for all-solid-state secondary batteries were performed on batteries that were determined to have no short circuits immediately after manufacture, after being firmly fixed on a vibration table of a vibration device, using a logarithmic sweep of a sinusoidal waveform, with a frequency of 7 Hz ⁇ An operation of sweeping from 200 Hz to 7 Hz in 15 minutes was repeated 12 times in each of the three mutually perpendicular directions of the battery.
  • the conditions for logarithmic sweep are as follows.
  • the peak acceleration is maintained at 1 g n from 7 Hz until reaching 18 Hz.
  • g n is the standard gravitational acceleration.
  • the vibration is kept at 0.8 mm (total amplitude 1.6 mm) and increased until the peak acceleration is 8 g n .
  • the all-solid-state secondary batteries of Examples 1 to 6 each having a laminated electrode body whose side surface was covered with a resin sheet in direct contact (pressed inward), were free from short circuits immediately after manufacture. No short circuit was observed, and the productivity was good. Also, no short circuit occurred even after the vibration test, and the reliability was excellent.
  • the battery of the present invention can be applied to the same uses as conventionally known primary batteries and secondary batteries, but it has excellent heat resistance because it has a solid electrolyte instead of an organic electrolyte. It can be preferably used in applications that are exposed to high temperatures.

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2025142958A1 (ja) * 2023-12-28 2025-07-03 マクセル株式会社 電気化学素子の組立方法及び組立装置

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Publication number Priority date Publication date Assignee Title
JPS57172662A (en) * 1981-04-17 1982-10-23 Toshiba Corp Lithium solid-electrolyte battery
JPH07220754A (ja) * 1994-02-07 1995-08-18 Tdk Corp 積層型リチウム二次電池
JP2000311717A (ja) * 1999-02-25 2000-11-07 Mitsubishi Chemicals Corp 電池要素及び電池
JP2002245998A (ja) * 2001-02-13 2002-08-30 Toshiba Corp 電池パック及び電池

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS57172662A (en) * 1981-04-17 1982-10-23 Toshiba Corp Lithium solid-electrolyte battery
JPH07220754A (ja) * 1994-02-07 1995-08-18 Tdk Corp 積層型リチウム二次電池
JP2000311717A (ja) * 1999-02-25 2000-11-07 Mitsubishi Chemicals Corp 電池要素及び電池
JP2002245998A (ja) * 2001-02-13 2002-08-30 Toshiba Corp 電池パック及び電池

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2025142958A1 (ja) * 2023-12-28 2025-07-03 マクセル株式会社 電気化学素子の組立方法及び組立装置

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