WO2022195926A1 - 固体電解質シート、及びこれを使用した固体電解質二次電池 - Google Patents

固体電解質シート、及びこれを使用した固体電解質二次電池 Download PDF

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Publication number
WO2022195926A1
WO2022195926A1 PCT/JP2021/034429 JP2021034429W WO2022195926A1 WO 2022195926 A1 WO2022195926 A1 WO 2022195926A1 JP 2021034429 W JP2021034429 W JP 2021034429W WO 2022195926 A1 WO2022195926 A1 WO 2022195926A1
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Prior art keywords
solid electrolyte
electrolyte sheet
sheet
electrode layer
negative electrode
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Ceased
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PCT/JP2021/034429
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English (en)
French (fr)
Japanese (ja)
Inventor
祐輝 山本
幸雄 山川
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Vehicle Energy Japan Inc
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Vehicle Energy Japan Inc
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Filing date
Publication date
Application filed by Vehicle Energy Japan Inc filed Critical Vehicle Energy Japan Inc
Priority to CN202180048018.7A priority Critical patent/CN115769408A/zh
Priority to US18/021,903 priority patent/US20240006663A1/en
Priority to EP25223336.6A priority patent/EP4685976A3/en
Priority to EP21930609.9A priority patent/EP4310969B1/en
Priority to JP2023506719A priority patent/JP7477714B2/ja
Publication of WO2022195926A1 publication Critical patent/WO2022195926A1/ja
Anticipated expiration legal-status Critical
Priority to JP2024066668A priority patent/JP2024086926A/ja
Ceased legal-status Critical Current

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • 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
    • 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
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • 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
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/431—Inorganic material
    • H01M50/434—Ceramics
    • 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
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/44—Fibrous material
    • 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
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/443—Particulate material
    • 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
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/446—Composite material consisting of a mixture of organic and inorganic materials
    • 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
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/463—Separators, membranes or diaphragms characterised by their shape
    • 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
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H01M2300/0071—Oxides
    • 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 secondary battery used in various industrial equipment, and more particularly to a solid electrolyte sheet, which is a battery element, and a solid electrolyte secondary battery using the same.
  • Electrolyte batteries containing positive and negative electrodes that can absorb/desorb lithium ions are widely used in various fields such as electric vehicles, power storage, and information equipment as high energy density batteries.
  • the use of this electrolyte battery in electric vehicle power applications requires high energy density, that is, high discharge capacity per unit weight or unit volume.
  • solid electrolyte secondary batteries have been developed.
  • a solid electrolyte secondary battery is a secondary battery that uses a solid electrolyte instead of the conventional organic electrolyte. Since the solid electrolyte secondary battery does not use an organic electrolytic solution, it is a highly safe secondary battery with a low possibility of ignition even if the discharge capacity per unit weight or unit volume is increased.
  • Patent Document 1 Such a solid electrolyte secondary battery is described, for example, in Japanese Patent Application Laid-Open No. 2019-057399 (Patent Document 1).
  • Patent Document 1 a solid electrolyte secondary battery is composed of a solid electrolyte sheet containing solid electrolyte particles. is in contact with the positive electrode layer. Power can be extracted by connecting the positive electrode layer and the negative electrode layer to a load.
  • the rigidity of the solid electrolyte sheet is low.
  • damage may occur in the vicinity of the periphery of the solid electrolyte sheet, causing a short circuit between the positive electrode layer and the negative electrode layer.
  • the rigidity of the solid electrolyte sheet is low, the size of the solid electrolyte sheet is naturally restricted, and there is a problem that it is difficult to secure a large ion conducting region.
  • An object of the present invention is to provide a solid electrolyte sheet capable of increasing the rigidity of the solid electrolyte sheet, and a solid electrolyte secondary battery using this solid electrolyte sheet.
  • the present invention The solid electrolyte sheet is formed of a plate-shaped base containing a solid electrolyte and a plate-shaped reinforcing portion formed outside the base,
  • the reinforcing portion is formed by combining two electrically insulating members made of different materials, and is characterized by being a composite material having high rigidity with respect to the base portion.
  • the present invention it is possible to increase the rigidity of the solid electrolyte sheet, particularly in the vicinity of the periphery, so that the possibility of damage to the vicinity of the periphery of the solid electrolyte sheet can be reduced.
  • the solid electrolyte sheet since the rigidity of the solid electrolyte sheet as a whole can be increased, the solid electrolyte sheet can be made large, and a large ion conduction area can be secured.
  • FIG. 1 is a plan view of a solid electrolyte sheet according to a first embodiment of the invention
  • FIG. FIG. 2 is a sectional view showing the AA section of the solid electrolyte sheet of FIG. 1
  • FIG. 4 is an explanatory diagram illustrating a method for manufacturing a solid electrolyte sheet according to the first embodiment
  • FIG. 5 is a plan view of a solid electrolyte sheet that is a first modification of the first embodiment of the present invention
  • FIG. 5 is a plan view of a solid electrolyte sheet that is a second modification of the first embodiment of the present invention
  • FIG. 11 is a plan view of a solid electrolyte sheet that is a third modification of the first embodiment of the present invention
  • FIG. 5 is a cross-sectional view of a solid electrolyte sheet according to a second embodiment of the present invention
  • FIG. 5 is a cross-sectional view of a solid electrolyte sheet that is a modification of the second embodiment of the present invention
  • FIG. 1 shows a plan view of the solid electrolyte sheet viewed from the side of the first surface (surface), and FIG. 2 shows a cross section of the solid electrolyte sheet of FIG. 1 taken along the line AA.
  • the solid electrolyte sheet 10 includes a rectangular central region 11 (corresponding to a base in the claims) having a first side (front side) and a second side (back side), and this It is composed of a peripheral reinforcing region 12 (corresponding to a reinforcing portion in the claims) along the outer peripheral shape of the central region 11 .
  • the central region 11 and the peripheral reinforcing region 12 are formed in a plate shape, and the peripheral reinforcing region 12 is formed outside the central region 11 so as to surround the rectangular central region 11 from four sides.
  • the peripheral edge reinforcing region 12 can be formed only on the peripheral edges of two or three sides facing each other.
  • the peripheral reinforcement region 12 is formed in a frame shape surrounding the central region 11 from the four outer sides, and is configured to have greater rigidity than the central region 11 .
  • the configuration and method for increasing this rigidity will be described later.
  • peripheral edge reinforcing region 12 By providing the peripheral edge reinforcing region 12 in this manner, not only the rigidity of the peripheral edge portion of the solid electrolyte sheet 10 can be increased, but also the rigidity of the solid electrolyte sheet 10 as a whole can be increased.
  • the rigidity of the solid electrolyte sheet 10 as a whole can be increased, the area of the solid electrolyte sheet 10 can be increased, and a large ion conduction region can be secured.
  • a configuration in which the area of the solid electrolyte sheet 10 is increased will be described in a second embodiment.
  • the periphery of the solid electrolyte sheet is often gripped. At this time, the periphery of the solid electrolyte sheet may be damaged, and the solid electrolyte sheet may become a defective product and become unusable. .
  • the rigidity of the solid electrolyte sheet 10 is increased by providing the peripheral edge reinforcing region 12, the peripheral edge portion of the solid electrolyte sheet is not damaged, and the solid electrolyte sheet becomes a defective product and cannot be used. can be avoided.
  • the central region 11 is the central region in the in-plane direction of the solid electrolyte sheet 10
  • the peripheral reinforcing region 12 is the peripheral reinforcing region in the in-plane direction of the solid electrolyte sheet 10
  • the central region 11 of the solid electrolyte sheet 10 is composed only of the solid electrolyte
  • the peripheral reinforcement region 12 is composed of the first electrical insulating member, the electrically insulating solid electrolyte (powder), or the inorganic oxide (powder).
  • the thickness of the solid electrolyte sheet 10 is about 15 ⁇ m to 100 ⁇ m, and considering the energy density of the battery, the thickness is preferably 15 ⁇ m to 30 ⁇ m. In this embodiment, the thickness of the solid electrolyte sheet 10 is set to 30 ⁇ m.
  • the lithium ion conductivity at 25° C. is, for example, 1 ⁇ 10 ⁇ 7 S/cm or more, preferably 1 ⁇ 10 ⁇ 3 S/cm. / cm or more.
  • the central region 11 is configured to contain powder of an oxide-based solid electrolyte or a sulfide-based solid electrolyte.
  • the central region 11 may contain one type of solid electrolyte (powder) alone, or may contain a mixture of two or more types of solid electrolyte (powder).
  • the central region 11 may contain fibers or powder of an inorganic compound such as a filler as a reinforcing member, and the central region 11 may further contain other components such as a binder.
  • these materials are collectively referred to as solid electrolytes.
  • the solid electrolyte made of these powders and fibers is held in a central region 11 by being held by a holding body made of an inorganic material or an organic material and having voids.
  • a nonwoven fabric sheet made of an organic material is used as the support.
  • the holder is not limited to the non-woven fabric sheet, but may be a lattice-like sheet in which the warp and weft are woven. Then, the solid electrolyte described above is kneaded into a slurry, applied to the support forming the central region 11, and dried.
  • the central region 11 of the solid electrolyte sheet 10 described above can be formed.
  • the solid electrolyte may be present also in the peripheral reinforcing region 12 other than the central region 11 . Since the nonwoven fabric sheet is used, the solid electrolyte can be filled up to the inside of the nonwoven fabric sheet by pressure molding.
  • peripheral reinforcing region 12 which is a feature of the present embodiment, is provided in a frame shape on the four outer sides of the solid electrolyte sheet 10, as described above.
  • the peripheral reinforcing region 12 may be provided only on the sides of the solid electrolyte sheet 10 on which the positive electrode current collector foil and the negative electrode current collector foil are located.
  • the width of the peripheral reinforcement region 12 in the plane direction is set to a length of about 2 mm. Since the peripheral reinforcing region 12 is outside the active area of the secondary battery, there is no substantial problem even if the lithium ion conductivity is low. may be composed of a material of 1 ⁇ 10 ⁇ 4 S/cm or less, or a material that does not have lithium ion conductivity. Of course, the same solid electrolyte as the central region 11 may be used with the same lithium ion conductivity in consideration of ease of manufacture.
  • the peripheral reinforcing region 12 includes the first electrical insulation member and the second electrical insulation member, as described above.
  • a composite member composed of a first electrical insulating member made of a powdered electrical insulating material and a second electrical insulating member made of an electrically insulating holder that holds the powdered electrical insulating material.
  • the first electrical insulating member it is possible to use an electrically insulating solid electrolyte containing lithium ions, or an electrically insulating material such as aluminum oxide that has electrical insulation but does not contain lithium ions. These are processed into powder, and in this embodiment, a solid electrolyte is used as the first insulating member.
  • a sulfide-based solid electrolyte or an oxide-based solid electrolyte can be used for this solid electrolyte.
  • the second insulating member is made of an electrically insulating inorganic material, an organic material, or the like, and has the function of a holding member that holds the first electrical insulating member.
  • a non-woven fabric made from an organic material is used for the second electrical insulation member.
  • it is not limited to the non-woven fabric, and a lattice-like one in which the warp and the weft are woven can also be used.
  • the peripheral reinforcing region 12 is made of a combination of an inorganic material for the first electrical insulation member and an organic material for the second electrical insulation member.
  • the solid electrolyte sheet 10 of the present embodiment is formed by laminating a peripheral edge reinforcing sheet 13 forming a peripheral edge reinforcing region 12 and a solid electrolyte base sheet 14 having the same outer shape as the peripheral edge reinforcing sheet 13 and pressure-molding them. there is This superimposed lamination area becomes the peripheral reinforcement area 12 with increased rigidity.
  • FIG. 3A a rectangular non-woven fabric (second electrical insulating member) made of polypropylene is prepared, and as shown in FIG. Cut out to produce the peripheral edge reinforcing sheet 13 . Thereby, a region for exposing the peripheral reinforcing region 12 and the central region 11 of the solid electrolyte sheet 10 can be formed.
  • second electrical insulating member made of polypropylene
  • a solid electrolyte base sheet 14 is prepared by applying a solid electrolyte to a base 15 made of polyethylene terephthalate (PET) and drying it.
  • PET polyethylene terephthalate
  • the solid electrolyte base sheets 14 are overlapped so as to sandwich the peripheral edge reinforcing sheets 13 from both sides to form a laminated shape.
  • the solid electrolyte base sheet 14 is placed on a base 15 made of polyethylene terephthalate (PET). Using the base 15 as a support, the solid electrolyte base sheet 14 is pressed against the peripheral edge reinforcing sheet 13 by a press machine. to mold.
  • PET polyethylene terephthalate
  • the peripheral edge portion (corresponding to the peripheral edge reinforcing region 12) of the solid electrolyte base sheet 14 and the peripheral edge reinforcing sheet 13 are overlapped and pressed, whereby the solid electrolyte of the solid electrolyte base sheet 14 and the peripheral edge reinforcing sheet are pressed together. Thirteen solid electrolytes are integrally formed in an intermixed state.
  • the peripheral edge portion of the solid electrolyte sheet 10 is can sufficiently increase the rigidity of By removing the base 15 after this pressing, the solid electrolyte sheet 10 as shown in FIG. 3(D) is obtained.
  • a slurry-like solid electrolyte is applied to the peripheral edge reinforcing sheet 13 and the solid electrolyte base sheet 14 and pre-pressurized to fill the peripheral edge reinforcing sheet 13 and the solid electrolyte base sheet 14 with the solid electrolyte in advance, It is also possible to integrate both by laminating and pressing both before drying.
  • a slurry-like solid electrolyte is applied on the peripheral edge reinforcing sheet 13 laid on the base 15 and dried. After pressing the dried sheet, the solid electrolyte sheet 10 may be produced by peeling off the base 15 .
  • the present embodiment is characterized by forming the peripheral edge reinforcing region 12 on the outer peripheral edge of the solid electrolyte sheet 10, and various methods such as the filling method of the solid electrolyte may be appropriately adopted. be.
  • the central region 11 is composed of a solid electrolyte having lithium ion conductivity
  • the peripheral reinforcement region 12 on the outer periphery thereof is made of a composite material with increased rigidity.
  • the lithium ion conductivity of the central region 11, which is the active area where the positive electrode layer and the negative electrode layer face each other can be sufficiently maintained.
  • the solid electrolyte sheet 10 has a high rigidity in the vicinity of the peripheral portion, it is possible to reduce the risk of damage to this portion.
  • the rigidity of the solid electrolyte sheet 10 as a whole can be improved by increasing the rigidity in the vicinity of the peripheral portion.
  • the electrolyte sheet 10 has high rigidity in the vicinity of the periphery. This will also be explained in the second embodiment.
  • the periphery of the solid electrolyte sheet 10 is often gripped, and at this time the periphery of the solid electrolyte sheet 10 may be damaged. For this reason, there is a risk that the solid electrolyte sheet 10 will become a defective product and cannot be used.
  • the solid electrolyte sheet 10 since the solid electrolyte sheet 10 has high rigidity in the vicinity of the periphery, such a problem can be solved. .
  • the solid electrolyte sheet 10 Since the solid electrolyte sheet 10 has a large rigidity in the vicinity of the periphery, the rigidity of the solid electrolyte sheet 10 as a whole is improved, so that the handleability is further improved. In addition, since the rigidity of the whole is improved, the size of the solid electrolyte sheet 10 can be increased, and a large ion conduction area can be secured.
  • a solid electrolyte or aluminum oxide can be used for the first electrical insulating member of the peripheral reinforcing region 12 . According to this, by using the same solid electrolyte as the central region 11, production efficiency can be improved, and by using an inorganic material such as aluminum oxide that does not have lithium ion conductivity, material costs can be reduced. can be achieved.
  • the outer shape of the solid electrolyte base sheet 14 and the outer shape of the peripheral edge reinforcing sheet 13 are formed in the same rectangular shape, and the dimensions are also determined to be the same. As a result, the peripheral edges of the solid electrolyte base sheet 14 and the peripheral edge reinforcing sheet 13 are matched in shape.
  • the nonwoven fabric using an organic material is used as the second insulating member of the peripheral reinforcing region 12, the solid electrolyte or inorganic oxide powder (first electrical insulating member) is pressurized into the voids of the nonwoven fabric. It is possible to form a thin solid electrolyte sheet having a thickness of about 30 ⁇ m and a high rigidity.
  • the peripheral edge reinforcing region 12 by forming the peripheral edge reinforcing region 12, not only the peripheral edge portion of the electrolyte sheet 10, but also the rigidity of the electrolyte sheet as a whole can be increased.
  • the rigidity of the solid electrolyte sheet particularly in the vicinity of the peripheral edge, so that the risk of damage to the solid electrolyte sheet in the vicinity of the peripheral edge can be reduced.
  • the rigidity of the solid electrolyte sheet 10 as a whole can be increased, the area of the solid electrolyte sheet 10 can be increased, and a large ion conduction region can be secured.
  • FIG. 4 shows the plane of the solid electrolyte sheet, and the same reference numerals are given to the same functional elements as in the first embodiment.
  • the solid electrolyte sheet 20 is composed of a rectangular central region 11 having a first surface (front surface) and a second surface (back surface), and a peripheral reinforcing region 12 along the outer peripheral shape of the central region 11. .
  • the central region 11 and the peripheral reinforcing region 12 are formed in a plate shape, and the peripheral reinforcing region 12 is formed outside the central region 11 so as to surround the rectangular central region 11 from four sides.
  • the peripheral reinforcing region 12 is formed in a frame shape surrounding the central region 11 from four sides, and is configured to have greater rigidity with respect to the central region 11 .
  • the configuration and method for increasing this rigidity are as described above.
  • the central region 11 of the solid electrolyte sheet 20 is provided with an auxiliary reinforcing region 21 .
  • the auxiliary reinforcing region 21 is formed in an elongated shape connecting the vicinity of the centers of the short sides of the solid electrolyte sheet 20 facing each other, and is integrally formed with the peripheral reinforcing region 12 .
  • the peripheral edge reinforcing sheet 13 shown in FIG. 3 can be cut into the shape shown in FIG. It is considered as a composite material consisting of members.
  • the opposing short sides are connected by the auxiliary reinforcing regions 21, but the opposing long sides may be connected by the auxiliary reinforcing regions 21.
  • the reason for providing such an auxiliary reinforcing region 21 is as follows.
  • the area of the central region 11 of the solid electrolyte sheet 20 is large, for example, when the area of the central region 11 is 10 cm 2 or more, if the central region 11 is accidentally touched while handling the solid electrolyte sheet 20, this region Since the rigidity is lower than that of the peripheral reinforcing region 12 and the area is larger, the central region 11 may be damaged.
  • an auxiliary reinforcing region 21 connected to the peripheral reinforcing region 12 is provided.
  • the rigidity of the central region 11 can be further improved, and even if the central region 11 is accidentally touched while the solid electrolyte sheet 20 is being handled, the central region 11 can be prevented from being damaged.
  • the auxiliary reinforcing region 21 exists in the central region 11, which is the active area, the lithium ion conductivity is preferably close to the central region 11. Thereby, good battery performance can be obtained, and the rigidity of the central region 11 can also be improved.
  • the solid electrolyte sheet 20 has the auxiliary reinforcing region 21 described above. It is possible to reduce the risk of damaging the solid electrolyte sheet 20 during such handling work.
  • the first electrical insulation member of the auxiliary reinforcing region 21 is composed of a solid electrolyte having lithium ion conductivity, and the lithium ion conductivity is It preferably has a value as close as possible to the lithium ion conductivity of region 11 .
  • the rigidity of the central region 11, which is the active area of the solid electrolyte sheet 20, can be further improved, and the auxiliary reinforcing region 21 can also be used as the active area.
  • FIG. 5 shows the plane of the solid electrolyte sheet, and the same reference numerals are given to the same functional elements as in the first embodiment.
  • the solid electrolyte sheet 30 is composed of a rectangular central region 11 having a first surface (front surface) and a second surface (back surface), and a peripheral reinforcing region 12 along the outer peripheral shape of the central region 11. .
  • the central region 11 and the peripheral reinforcing region 12 are formed in a plate shape, and the peripheral reinforcing region 12 is formed outside the central region 11 so as to surround the rectangular central region 11 from four sides.
  • the peripheral reinforcing region 12 is formed in a frame shape surrounding the central region 11 from four sides, and is configured to have greater rigidity with respect to the central region 11 .
  • the configuration and method for increasing this rigidity are as described above.
  • the central region 11 of the solid electrolyte sheet 30 is provided with a horizontal auxiliary reinforcing region 31 and a vertical auxiliary reinforcing region 32 which are formed in a grid pattern.
  • the lateral auxiliary reinforcing region 31 is formed in an elongated shape connecting positions (here, three positions) obtained by equally dividing the mutually opposing short sides of the solid electrolyte sheet 30, and is formed integrally with the peripheral edge reinforcing region 12. .
  • the vertical auxiliary reinforcing region 32 is formed in a long shape by connecting equally divided positions (here, five positions) of the mutually opposing long sides of the solid electrolyte sheet 30, and is integrally formed with the peripheral reinforcing region 12. ing.
  • the horizontal auxiliary reinforcing region 31, the vertical auxiliary reinforcing region 32, and the peripheral reinforcing region 12 can be formed by cutting out the peripheral reinforcing sheet 13 shown in FIG. 3 into the shape shown in FIG.
  • the peripheral reinforcement region 12 of the first embodiment it is a composite member made up of a first electrical insulation member and a second electrical insulation member.
  • auxiliary reinforcing regions 31 and 32 are the same as in Modification 1. For this reason, in this modified example, grid-like auxiliary reinforcing regions 31 and 32 connected to the peripheral reinforcing region 12 are provided. As a result, the rigidity of the central region 11 can be further improved, and damage to the central region 11 can be avoided even if the central region 11 is accidentally touched while the solid electrolyte sheet 30 is being handled.
  • the auxiliary reinforcing regions 31 and 32 are present in the central region 11, which is the active area, it is preferable that the lithium ion conductivity is close to the central region 11. Thereby, good battery performance can be obtained, and the rigidity of the central region 11 can also be improved.
  • the solid electrolyte sheet 30 has the above-described lattice-shaped auxiliary reinforcing regions 31 and 32, so that the process of forming the solid electrolyte sheet 30 and the It is possible to reduce the risk of damaging the solid electrolyte sheet 30 during handling operations such as lamination after formation.
  • the first insulating members of the auxiliary reinforcing regions 31 and 32 are made of a solid electrolyte having lithium ion conductivity, and the lithium The ionic conductivity preferably has a value as close as possible to the lithium ion conductivity of the central region 11 .
  • the rigidity of the central region 11, which is the active area of the solid electrolyte sheet 30, can be improved, and the lattice-shaped auxiliary reinforcing regions 31 and 32 can also be used as active areas.
  • the lattice-shaped auxiliary reinforcing regions 31 and 32 allow the aspect ratio of each surface of the central region 11 composed only of the solid electrolyte to be arbitrarily set. As a result, it is possible to obtain the effect of being able to select an appropriate rigidity while ensuring the lithium ion conductivity.
  • FIG. 6 shows the plane of the solid electrolyte sheet, and the same reference numerals are given to the same functional elements as in the first embodiment.
  • the solid electrolyte sheet 40 is composed of a rectangular central region 11 having a first surface (front surface) and a second surface (back surface), and a peripheral reinforcing region 12 along the outer peripheral shape of the central region 11. .
  • the central region 11 and the peripheral reinforcing region 12 are formed in a plate shape, and the peripheral reinforcing region 12 is formed outside the central region 11 so as to surround the rectangular central region 11 from four sides.
  • the peripheral reinforcing region 12 is formed in a frame shape surrounding the central region 11 from four sides, and is configured to have greater rigidity with respect to the central region 11 .
  • the configuration and method for increasing this rigidity are as described above.
  • the central region 11 of the solid electrolyte sheet 40 is provided with a first oblique auxiliary reinforcing region 41 and a second oblique auxiliary reinforcing region 42 formed in a diagonal line.
  • the first oblique auxiliary reinforcing region 41 and the second oblique auxiliary reinforcing region 42 are formed in an elongated shape along the diagonal line of the rectangular central region 11 of the solid electrolyte sheet 40, and are integrally formed with the peripheral edge reinforcing region 12.
  • the peripheral edge reinforcing sheet 13 shown in FIG. 3 can be cut out into the shape shown in FIG. and a second electrical insulating member.
  • oblique auxiliary reinforcing regions 41 and 42 are provided along the diagonal lines connected to the peripheral edge reinforcing region 12 .
  • the rigidity of the central region 11 can be improved, and damage to the central region 11 can be avoided even if the central region 11 is accidentally touched while the solid electrolyte sheet 40 is being handled.
  • the lithium ion conductivity is preferably close to the central region 11. Thereby, good battery performance can be obtained, and the rigidity of the central region 11 can also be improved.
  • the solid electrolyte sheet 40 has the oblique auxiliary reinforcing regions 41 and 42 along the diagonal lines described above. It is possible to reduce the risk of damaging the solid electrolyte sheet 40 during handling such as the step of laminating after the formation of the solid electrolyte sheet 40 .
  • the first insulating member of the diagonal auxiliary reinforcing regions 41 and 42 is composed of a solid electrolyte having lithium ion conductivity.
  • the lithium ion conductivity preferably has a value as close as possible to the lithium ion conductivity of the central region 11 .
  • the rigidity of the central region 11, which is the active area of the solid electrolyte sheet 40 can be improved, and the oblique auxiliary reinforcement regions 41 and 42 can also be used as active areas.
  • the solid electrolyte sheet 10 used in the solid electrolyte secondary battery described below is the solid electrolyte sheet 10 according to the first embodiment.
  • the solid electrolyte sheet 10 is formed with a thickness of, for example, 30 ⁇ m, it does not have the peripheral reinforcing region 12 and is composed only of the solid electrolyte like the central region 11 .
  • the edge reinforcing region 12 does not exist, the rigidity of the end surface of the solid electrolyte sheet 10 is small.
  • this portion collapses, causing a phenomenon in which the positive electrode layer 53 and the negative electrode layer 54 are short-circuited.
  • ensuring safety is the most important issue, and it is necessary to take all possible measures to prevent accidents.
  • the area of the negative electrode layer is larger than the area of the positive electrode layer.
  • the area of the solid electrolyte sheet 10 cannot be made larger than the area of the negative electrode layer, and the current collector foils or terminals of the positive electrode layer and the negative electrode are not subjected to insulation treatment. This is a hindrance to deriving a large amount of electric power.
  • the area of the solid electrolyte sheet 10 cannot be increased, it is difficult to secure a large ion-conducting region.
  • the present embodiment proposes a solid electrolyte secondary battery as shown in FIG.
  • the unit battery shown in FIG. 7 is actually a secondary battery formed by stacking a plurality of solid electrolyte batteries.
  • FIG. 7 is a cross section of the solid electrolyte secondary battery 50 along the lead-out direction of the positive current collector foil 51 and the negative current collector foil 52 .
  • the positive collector foil 51 has a positive terminal 51T
  • the negative collector foil 52 has a negative terminal 52T.
  • the solid electrolyte secondary battery 50 has a positive electrode layer 53 formed of a positive electrode active material on one side of the solid electrolyte sheet 10, and a negative electrode active material on the other side of the solid electrolyte sheet 10.
  • a negative electrode layer 54 is formed.
  • a positive current collector foil 51 is attached so as to be electrically conductive. is attached so that the negative electrode current collector foil 52 is electrically conductive.
  • the characteristic configuration of this embodiment is as follows. First, when viewed in the terminal lead-out direction (longitudinal direction), the length (L0) of the positive electrode layer 53 is the same as the length (L1) of the central region 11 of the solid electrolyte sheet 10 . Therefore, the end surface of the positive electrode layer 53 on the opposite side of the positive electrode terminal 51T of the positive electrode current collector foil 51 and the corresponding end surface of the central region 11 of the solid electrolyte sheet 10 are aligned when viewed in the terminal lead-out direction. (So-called flush relationship).
  • the projected image of the positive electrode layer 53 in the direction orthogonal to the terminal lead-out direction is determined to have dimensions that match and overlap the central region 11 of the solid electrolyte sheet 10 .
  • the end surface of the positive electrode terminal 51T side of the positive electrode current collector foil 51 and the edge reinforcing region 12 of the solid electrolyte sheet 10 on the side opposite to the positive electrode terminal 51T have a length (L2), and the end surface of the positive electrode layer 53 has a length (L2). protruding from Therefore, since the positive electrode layer 53 and the central region 11 of the solid electrolyte sheet 10, which is the active area, are in full contact with each other, lithium ions can efficiently move, and the input/output characteristics of the secondary battery can be improved. can be improved.
  • the length (L3) of the negative electrode layer 54 is longer than the length (L1) of the central region 11 of the solid electrolyte sheet 10 . Therefore, the negative terminal 52T side of the negative electrode current collector foil 52 and the end surface of the negative electrode layer 54 opposite to the negative electrode terminal 52T have a length (L4) from the end surface of the central region 11 of the solid electrolyte sheet 10. protruding. Therefore, since the negative electrode layer 54 and the central region 11 of the solid electrolyte sheet 10, which is the active area, are in full contact, lithium ions can efficiently move.
  • the end face of the peripheral reinforcing region 12 of the solid electrolyte sheet 10 protrudes from the end face of the negative electrode layer 54 by the length (L5). Therefore, the peripheral reinforcing region 12 is configured to support the end surface of the negative electrode layer 54 . Therefore, even if some external mechanical force acts on the end surface of the negative electrode layer 54, the peripheral reinforcing region 12 can receive the external force from the negative electrode layer 54, so damage to the solid electrolyte sheet 10 can be suppressed. As a result, it becomes possible to prevent a short circuit between the positive electrode layer 53 and the negative electrode layer 54 .
  • the solid electrolyte sheet 10 is reinforced in its overall rigidity by the peripheral reinforcement region 12, even if the solid electrolyte sheet 10 is as thin as about 30 ⁇ m in thickness, the area can be made larger than that of the negative electrode layer 54. As a result, it is possible to prevent short-circuiting of the battery due to contact between the positive current collector foil 51 and the negative current collector foil 52 .
  • the solid electrolyte sheet 10 as a whole is reinforced in rigidity, even if the thickness of the solid electrolyte sheet 10 is as thin as about 30 ⁇ m, the area of the solid electrolyte sheet 10 can be made larger than the area of the negative electrode layer 54, A large ion conduction region can be secured, and an impediment to deriving a large amount of power can be eliminated.
  • the battery performance can be improved by using the solid electrolyte sheet 10 described in the first embodiment.
  • the end face of the positive electrode layer 53 is flush with the end face of the central region 11 of the solid electrolyte sheet 10 , and the end face of the negative electrode layer 54 overlaps with the peripheral reinforcement region 12 of the solid electrolyte sheet 10 . According to such a configuration, the main reaction of the battery takes place in the central region 11 where the lithium ion conductivity is relatively high, so high battery performance can be obtained.
  • the pressing process is performed in a state in which the positive electrode layer 53, the negative electrode layer 54, and the solid electrolyte sheet 10 are laminated.
  • the solid electrolyte sheet 10 is not damaged, and the short circuit of the battery can be prevented.
  • the peripheral edge reinforcing region 12 by using a solid electrolyte for the first electrical insulating member of the peripheral reinforcing region 12, it can be used as an active area. Furthermore, by setting the ionic conductivity of the peripheral edge reinforcing region 12 to be low, it is possible to suppress current concentration in the peripheral edge reinforcing region 12, and effects such as suppression of lithium electrodeposition and improvement of cycle characteristics can be expected.
  • the surface area of the solid electrolyte sheet 10 including the peripheral reinforcing region 12 can be made larger than the surface area of the positive electrode layer 53 and the negative electrode layer 54 . Therefore, it is possible to prevent current collector foils between the positive current collector foil 51 of the positive electrode layer 53 and the negative current collector foil 52 of the negative electrode layer 54 from coming into contact with each other and causing a short circuit.
  • the modification shown in FIG. 8 has basically the same shape and the same dimensional relationship as the second embodiment, and the lengths (L1) to (L5) are the same. However, the difference is that the length of the positive electrode layer 53 is determined to be longer than that of the second embodiment, and the length of the positive electrode layer 53 is determined to be (L7) in this modified example. This point will be described below.
  • the length (L6) of the positive electrode layer 53 is set longer than the length (L1) of the central region 11 of the solid electrolyte sheet 10.
  • the end surface of the positive electrode layer 53 on the side extends beyond the central region 11 to the peripheral reinforcing region 12 by a length (L7).
  • the peripheral reinforcing region 12 is configured to support the end surface of the positive electrode layer 53 . Therefore, even if some mechanical external force acts on the end surface of the positive electrode layer 53, the peripheral edge reinforcing region 12 can receive the load from the positive electrode layer 53, so damage to the solid electrolyte sheet 10 can be suppressed. As a result, it becomes possible to prevent a short circuit between the positive electrode layer 53 and the negative electrode layer 54 . Moreover, it goes without saying that this modified example also has the same functions and effects as those of the above-described second embodiment.
  • the solid electrolyte sheet is formed from a plate-shaped base containing a solid electrolyte and a plate-shaped reinforcing portion formed outside the base, and the reinforcing portion is made of a material
  • the composite member is formed by combining two electrically insulating members with different values, and is a composite member having a large rigidity with respect to the base.
  • the solid electrolyte sheet since the rigidity of the solid electrolyte sheet as a whole can be increased, the solid electrolyte sheet can be made large, and a large ion conduction area can be secured.
  • the present invention is not limited to the above-described embodiments, and includes various modifications.
  • the above-described embodiments have been described in detail in order to explain the present invention in an easy-to-understand manner, and are not necessarily limited to those having all the described configurations.
  • it is possible to replace part of the configuration of one embodiment with the configuration of another embodiment and it is also possible to add the configuration of another embodiment to the configuration of one embodiment.
  • Solid electrolyte sheet 11... Central area, 12... Peripheral reinforcing area, 13... Peripheral edge reinforcing sheet, 14... Solid electrolyte base sheet, 15... Base, 20... Solid electrolyte sheet, 21... Auxiliary reinforcing area, 30... Solid Electrolyte sheet 31 Horizontal auxiliary reinforcing region 32 Vertical auxiliary reinforcing region 40 Solid electrolyte sheet 41 First oblique auxiliary reinforcing region 42 Second oblique auxiliary reinforcing region 50 Solid electrolyte secondary battery 51 Positive electrode current collector foil, 51T Positive electrode terminal, 52 Negative electrode current collector foil, 52T Negative electrode terminal, 53 Positive electrode layer, 54 Negative electrode layer.

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PCT/JP2021/034429 2021-03-16 2021-09-17 固体電解質シート、及びこれを使用した固体電解質二次電池 Ceased WO2022195926A1 (ja)

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CN202180048018.7A CN115769408A (zh) 2021-03-16 2021-09-17 固体电解质片和使用它的固体电解质二次电池
US18/021,903 US20240006663A1 (en) 2021-03-16 2021-09-17 Solid electrolyte sheet, and solid electrolyte secondary battery using said solid electrolyte sheet
EP25223336.6A EP4685976A3 (en) 2021-03-16 2021-09-17 Solid electrolyte sheet, and solid electrolyte secondary battery using said solid electrolyte sheet
EP21930609.9A EP4310969B1 (en) 2021-03-16 2021-09-17 Solid electrolyte sheet, and solid electrolyte secondary battery using said solid electrolyte sheet
JP2023506719A JP7477714B2 (ja) 2021-03-16 2021-09-17 固体電解質シート、及びこれを使用した固体電解質二次電池
JP2024066668A JP2024086926A (ja) 2021-03-16 2024-04-17 固体電解質シート、及びこれを使用した固体電解質二次電池

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WO2025022640A1 (ja) * 2023-07-27 2025-01-30 日産自動車株式会社 全固体電池用電解質複合体及び全固体電池

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EP4310969B1 (en) 2026-01-21
EP4685976A2 (en) 2026-01-28
JPWO2022195926A1 (https=) 2022-09-22
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EP4310969A1 (en) 2024-01-24
EP4685976A3 (en) 2026-04-22

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