WO2022102639A1 - 全固体電池 - Google Patents
全固体電池 Download PDFInfo
- Publication number
- WO2022102639A1 WO2022102639A1 PCT/JP2021/041276 JP2021041276W WO2022102639A1 WO 2022102639 A1 WO2022102639 A1 WO 2022102639A1 JP 2021041276 W JP2021041276 W JP 2021041276W WO 2022102639 A1 WO2022102639 A1 WO 2022102639A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- solid
- power generation
- generation element
- sealing
- state battery
- Prior art date
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- 238000010248 power generation Methods 0.000 claims abstract description 87
- 238000007789 sealing Methods 0.000 claims abstract description 79
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 53
- 229910002804 graphite Inorganic materials 0.000 claims description 50
- 239000010439 graphite Substances 0.000 claims description 50
- 230000002093 peripheral effect Effects 0.000 claims description 32
- 239000007784 solid electrolyte Substances 0.000 claims description 21
- 230000000994 depressogenic effect Effects 0.000 abstract 1
- 239000000463 material Substances 0.000 description 13
- 238000003825 pressing Methods 0.000 description 8
- 230000006866 deterioration Effects 0.000 description 7
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 6
- 229910001416 lithium ion Inorganic materials 0.000 description 6
- 239000007774 positive electrode material Substances 0.000 description 6
- 239000002253 acid Substances 0.000 description 5
- 238000004519 manufacturing process Methods 0.000 description 5
- 239000011255 nonaqueous electrolyte Substances 0.000 description 5
- 238000000034 method Methods 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 3
- 239000004020 conductor Substances 0.000 description 3
- 229910052744 lithium Inorganic materials 0.000 description 3
- 239000002203 sulfidic glass Substances 0.000 description 3
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 2
- 239000002041 carbon nanotube Substances 0.000 description 2
- 229910021393 carbon nanotube Inorganic materials 0.000 description 2
- 239000002131 composite material Substances 0.000 description 2
- 230000006835 compression Effects 0.000 description 2
- 238000007906 compression Methods 0.000 description 2
- 238000002788 crimping Methods 0.000 description 2
- 238000007599 discharging Methods 0.000 description 2
- 238000005187 foaming Methods 0.000 description 2
- 239000007769 metal material Substances 0.000 description 2
- 238000000465 moulding Methods 0.000 description 2
- 239000007773 negative electrode material Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 239000008188 pellet Substances 0.000 description 2
- 238000011084 recovery Methods 0.000 description 2
- 238000005096 rolling process Methods 0.000 description 2
- 239000010935 stainless steel Substances 0.000 description 2
- 229910001220 stainless steel Inorganic materials 0.000 description 2
- 229910052717 sulfur Inorganic materials 0.000 description 2
- 239000011593 sulfur Substances 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 1
- 229910000733 Li alloy Inorganic materials 0.000 description 1
- 229910013641 LiNbO 3 Inorganic materials 0.000 description 1
- 229910011328 LiNi0.6Co0.2Mn0.2O2 Inorganic materials 0.000 description 1
- SOXUFMZTHZXOGC-UHFFFAOYSA-N [Li].[Mn].[Co].[Ni] Chemical compound [Li].[Mn].[Co].[Ni] SOXUFMZTHZXOGC-UHFFFAOYSA-N 0.000 description 1
- 238000010306 acid treatment Methods 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- 239000003575 carbonaceous material Substances 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
- 239000010949 copper Substances 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- QHGJSLXSVXVKHZ-UHFFFAOYSA-N dilithium;dioxido(dioxo)manganese Chemical compound [Li+].[Li+].[O-][Mn]([O-])(=O)=O QHGJSLXSVXVKHZ-UHFFFAOYSA-N 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000001704 evaporation Methods 0.000 description 1
- 150000004678 hydrides Chemical class 0.000 description 1
- 238000001746 injection moulding Methods 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 239000001989 lithium alloy Substances 0.000 description 1
- 229910000625 lithium cobalt oxide Inorganic materials 0.000 description 1
- BFZPBUKRYWOWDV-UHFFFAOYSA-N lithium;oxido(oxo)cobalt Chemical compound [Li+].[O-][Co]=O BFZPBUKRYWOWDV-UHFFFAOYSA-N 0.000 description 1
- URIIGZKXFBNRAU-UHFFFAOYSA-N lithium;oxonickel Chemical compound [Li].[Ni]=O URIIGZKXFBNRAU-UHFFFAOYSA-N 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 239000006262 metallic foam Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 229910021382 natural graphite Inorganic materials 0.000 description 1
- 229910000484 niobium oxide Inorganic materials 0.000 description 1
- URLJKFSTXLNXLG-UHFFFAOYSA-N niobium(5+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[Nb+5].[Nb+5] URLJKFSTXLNXLG-UHFFFAOYSA-N 0.000 description 1
- 239000010450 olivine Substances 0.000 description 1
- 229910052609 olivine Inorganic materials 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 238000009751 slip forming Methods 0.000 description 1
- 230000008016 vaporization Effects 0.000 description 1
Images
Classifications
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- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/50—Current conducting connections for cells or batteries
- H01M50/531—Electrode connections inside a battery casing
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- H01M50/10—Primary casings; Jackets or wrappings
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- 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
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- 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
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- 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
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- H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
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- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
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- H01M50/166—Lids or covers characterised by the methods of assembling casings with lids
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- 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
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- 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
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Definitions
- This disclosure relates to all-solid-state batteries.
- the positive electrode and the negative electrode are arranged facing each other via a separator, and this is housed in a battery case composed of a positive electrode can and a negative electrode can, and the positive electrode can and the negative electrode can are gaskets.
- a lithium ion secondary battery caulked via the above Patent Document 1
- an elastic body coated with a conductor is arranged between the positive electrode and the positive electrode can and between the negative electrode and the negative electrode can.
- the lithium ion secondary battery can secure a sufficient contact area between the positive electrode and the positive electrode can and the negative electrode and the negative electrode can, alleviates the stress when caulking the positive electrode can and the negative electrode can, and cracks the positive electrode and the negative electrode. Can be prevented.
- Japanese Patent Application Laid-Open No. 2003-151511 includes a positive electrode can and a negative electrode can, and a positive electrode material, a negative electrode material and a separator accommodated in both cans, and a gasket is arranged between the peripheral edge of the positive electrode can and the peripheral edge of the negative electrode can.
- a flat non-aqueous electrolyte battery is disclosed (Patent Document 2).
- a sealing wall in contact with the gasket is provided on the peripheral edge of the bottom wall of the positive electrode can, and the positive electrode material is housed in a recess provided radially inside the sealing wall.
- the lithium ion secondary battery of Patent Document 1 uses an elastic body whose surface is coated with a conductor. That is, a conductor having electrical conductivity is arranged only around the elastic body. Therefore, the elastic body of Patent Document 1 becomes a resistance component that inhibits electrical conductivity, and thus increases the internal resistance of the battery.
- the flat non-aqueous electrolyte battery of Patent Document 2 has improved sealing performance by providing a recess in the radial direction from the sealing wall of the bottom wall of the positive electrode can.
- the flat non-aqueous electrolyte battery of Patent Document 2 is not supposed to accommodate a power generation element in which a positive electrode layer, a solid electrolyte layer, and a negative electrode layer are laminated, instead of an all-solid-state battery. Therefore, there is no cushioning material for the pressing force generated when crimping the positive electrode can and the sealing can, and if the power generation element is housed in the battery, the power generation element may be damaged such as cracked. be.
- the present disclosure provides an all-solid-state battery capable of sufficiently ensuring electrical contact between the outer can and the power generation element and electrical contact between the sealing can and the power generation element, and preventing damage to the positive electrode layer or the negative electrode layer.
- the challenge is to provide.
- the all-solid-state battery according to the present disclosure may include an outer can having a bottom including a recess recessed outward and a cylindrical side wall.
- the all-solid-state battery may have a flat surface portion and a peripheral wall portion, and may include a sealing can that covers the opening of the outer can.
- the all-solid-state battery has a positive electrode layer, a negative electrode layer, and a solid electrolyte layer arranged between the positive electrode layer and the negative electrode layer, which is arranged between the inner bottom surface of the concave portion of the outer can and the flat surface portion of the sealing can. May have elements.
- the all-solid-state battery may include a gasket that is crimped between the cylindrical side wall portion of the outer can and the peripheral wall portion of the sealing can.
- the all-solid-state battery is of a first restorative conductive sheet arranged between the inner bottom surface of the recess and the power generation element, and a second restorable conductive sheet arranged between the flat surface portion of the sealing can and the power generation element. At least one of them may be provided.
- the all-solid-state battery it is possible to sufficiently secure the electrical contact between the outer can and the power generation element and the electrical contact between the sealing can and the power generation element, and prevent damage to the positive electrode layer or the negative electrode layer. can.
- FIG. 1 is a cross-sectional view showing the structure of the all-solid-state battery according to the present embodiment.
- FIG. 2 is a cross-sectional view showing a manufacturing process of the all-solid-state battery shown in FIG.
- FIG. 3 is a cross-sectional view showing a manufacturing process of the all-solid-state battery shown in FIG.
- FIG. 4 is a cross-sectional view showing a manufacturing process of the all-solid-state battery shown in FIG.
- FIG. 5 is a cross-sectional view showing the structure of the all-solid-state battery according to the modified example.
- the all-solid-state battery according to the present embodiment may include an outer can having a bottom including a recess recessed outward and a cylindrical side wall.
- the all-solid-state battery may have a flat surface portion and a peripheral wall portion, and may include a sealing can that covers the opening of the outer can.
- the all-solid-state battery has a positive electrode layer, a negative electrode layer, and a solid electrolyte layer arranged between the positive electrode layer and the negative electrode layer, which is arranged between the inner bottom surface of the concave portion of the outer can and the flat surface portion of the sealing can. May have elements.
- the all-solid-state battery may include a gasket that is crimped between the cylindrical side wall portion of the outer can and the peripheral wall portion of the sealing can.
- the all-solid-state battery may include a first resilient conductive sheet disposed between the power generation element and at least one of the inner bottom surface of the recess and the flat surface of the sealing can.
- the first recoverable conductive sheet can maintain good continuity of the outer can and the power generation element and the continuity of the sealing can and the power generation element due to its resilience, and also acts as a cushioning material. It is possible to alleviate the pressing force generated when crimping the outer can and the sealing can to prevent damage to the positive electrode layer and the negative electrode layer. Further, when the first restorative conductive sheet is arranged between the inner bottom surface of the recess and the power generation element, it is positioned in the recess, so that the first restorability when caulking the outer can and the sealing can. It is possible to prevent the conductive sheet from being misaligned and being pinched between the bottom of the outer can and the gasket. As a result, it is possible to suppress the deterioration of the sealing property in the all-solid-state battery.
- the first restorative conductive sheet may be arranged between the inner bottom surface of the recess and the power generation element.
- the depth of the recess may be greater than the thickness of the first restorative conductive sheet. That is, the first restorative conductive sheet has a thickness smaller than the depth of the recess.
- the first restorative conductive sheet may be arranged between the inner bottom surface of the recess and the power generation element.
- the all-solid-state battery may further include a second resilient conductive sheet disposed between the flat surface of the sealing can and the power generation element.
- the first recoverable conductive sheet is arranged between the inner bottom surface of the recess and the power generation element, the first recoverable conductive sheet is misaligned when caulking the outer can and the sealing can. Therefore, it is possible to prevent the outer can from being pinched between the bottom of the outer can and the gasket. As a result, it is possible to suppress the deterioration of the sealing property in the all-solid-state battery.
- the depth of the recess may be smaller than the height from the inner bottom surface of the recess to the upper end of the outer peripheral surface of the solid electrolyte layer. This makes it possible to prevent the bottom of the outer can from coming into contact with the negative electrode layer and causing a short circuit.
- the first and second recoverable conductive sheets may be graphite sheets.
- the all-solid-state battery 1 includes an outer can 2, a sealing can 3, a power generation element 4, and a restoring conductive sheet 5 arranged between the outer can 2 and the power generation element 4. It is composed of a restoring conductive sheet 5 arranged between the sealing can 3 and the power generation element 4, and a gasket 6.
- the all-solid-state battery 1 is a flat battery.
- the outer can 2 includes a circular bottom portion 21 and a cylindrical cylindrical side wall portion 22 continuously formed from the outer periphery of the bottom portion 21.
- the tubular side wall portion 22 is provided so as to extend substantially perpendicular to the bottom portion 21 in a vertical cross-sectional view.
- the outer can 2 is made of a metal material such as stainless steel.
- the bottom portion 21 of the outer can 2 has a recess 211.
- the recess 211 is formed integrally with the outer can 2 by press working.
- the recess 211 is recessed in the axial direction toward the outside (lower part of the figure) of the all-solid-state battery 1 from the bottom 21.
- the recess 211 accommodates the restorative conductive sheet 5.
- the recess 211 has a depth d. As shown in FIG. 1, the depth d of the recess 211 is the depth from the inner surface of the bottom portion 21 to the inner bottom surface of the recess 211.
- the depth d and the inner diameter d1 of the recess 211 will be described in detail later.
- the sealing can 3 includes a circular flat surface portion 31 and a cylindrical peripheral wall portion 32 formed continuously from the outer periphery of the flat surface portion 31.
- the opening of the sealing can 3 faces the opening of the outer can 2.
- the sealing can 3 is made of a metal material such as stainless steel.
- the outer can 2 and the sealing can 3 have a gasket between the cylindrical side wall portion 22 of the outer can 2 and the peripheral wall portion 32 of the sealing can 3 after accommodating the power generation element 4 and the restorable conductive sheet 5 in the internal space. It is crimped through 6. Specifically, the outer can 2 and the sealing can 3 face each other with the openings of the outer can 2 and the sealing can 3 facing each other, and the peripheral wall portion 32 of the sealing can 3 is provided inside the tubular side wall portion 22 of the outer can 2. After being inserted, it is crimped between the tubular side wall portion 22 and the peripheral wall portion 32 via the gasket 6. As a result, the internal space formed by the outer can 2 and the sealing can 3 is sealed.
- the material, shape, and the like of the outer can 2, the sealing can 3, and the gasket 6 are not particularly limited.
- the power generation element 4 includes a positive electrode layer 41, a negative electrode layer 42, and a solid electrolyte layer 43.
- the solid electrolyte layer 43 is arranged between the positive electrode layer 41 and the negative electrode layer 42.
- the power generation element 4 is laminated in the order of the positive electrode layer 41, the solid electrolyte layer 43, and the negative electrode layer 42 from the bottom 21 side (lower part in the drawing) of the outer can 2.
- the power generation element 4 is formed in a cylindrical shape.
- the power generation element 4 is arranged on the inner bottom surface of the recess 211 of the outer can 2 via the restorative conductive sheet 5. Therefore, the outer can 2 functions as a positive electrode can.
- the power generation element 4 is in contact with the inner surface of the flat surface portion 31 of the sealing can 3 via the restorative conductive sheet 5. Therefore, the sealing can 3 functions as a negative electrode can.
- the power generation element 4 is not limited to the cylindrical shape, but can be variously changed according to the shape of the all-solid-state battery 1, such as a rectangular parallelepiped shape or a polygonal prism shape.
- the positive electrode layer 41 contains LiNi 0.6 Co 0.2 Mn 0.2 O 2 having an average particle size of 3 ⁇ m and a sulfide solid electrolyte (Li 6 PS 5 Cl) as the positive electrode active material used in the lithium ion secondary battery.
- This is a positive electrode pellet formed into a columnar shape by putting a 180 mg positive electrode mixture containing carbon nanotubes, which are conductive aids, in a mass ratio of 55:40: 5 into a mold having a diameter of 10 mm.
- the positive electrode layer 41 is not particularly limited as long as it can function as the positive electrode layer of the power generation element 4, and is, for example, lithium cobalt oxide, lithium nickel oxide, lithium manganate, lithium nickel cobalt manganese composite oxide, and the like.
- the size and shape of the positive electrode layer 41 are not limited to the cylindrical shape, and can be variously changed according to the size and shape of the all-solid-state battery 1.
- the negative electrode layer 42 contains LTO (Li 4 Ti 5 O 12 , lithium titanate), a sulfide solid electrolyte (Li 6 PS 5 Cl), and carbon nanotubes as the negative electrode active material used for the lithium ion secondary battery. It is a negative electrode pellet obtained by molding a negative electrode mixture of 300 mg contained in a weight ratio of 50:45: 5 into a cylindrical shape.
- the negative electrode layer 42 is not particularly limited as long as it can function as the negative electrode layer of the power generation element 4, and is, for example, a carbon material such as metallic lithium, a lithium alloy, graphite, or low crystalline carbon, SiO, or LTO.
- the size and shape of the negative electrode layer 42 are not limited to the cylindrical shape, and can be variously changed according to the size and shape of the all-solid-state battery 1.
- the solid electrolyte layer 43 is formed by molding 60 mg of a sulfide solid electrolyte (Li 6 PS 5 Cl) into a cylindrical shape.
- the solid electrolyte layer 43 is not particularly limited, but may be another sulfur-based solid electrolyte such as an algyrodite type from the viewpoint of ion conductivity.
- a sulfur-based solid electrolyte it is preferable to coat the surface of the positive electrode active material with a niobium oxide (LiNbO 3 , etc.) in order to prevent the reaction with the positive electrode active material.
- the solid electrolyte layer 43 may be a hydride-based solid electrolyte, an oxide-based solid electrolyte, or the like.
- the size and shape of the solid electrolyte layer 43 are not limited to the cylindrical shape, and can be variously changed according to the size and shape of the all-solid-state battery 1.
- the restorative conductive sheet 5 is a sheet made of a material that has conductivity and generates a certain repulsive force in an attempt to restore the shape when compressed to reduce the thickness.
- the sheet constituting the recoverable conductive sheet 5 has elasticity, and in addition to elastically deformable materials such as carbon black and conductive rubber which is made conductive by uniformly mixing metal powder and rubber, for example, graphite.
- the restorable conductive sheet 5 is arranged between the recess 211 of the outer can 2 and the positive electrode layer 41 of the power generation element 4, and between the flat surface portion 31 of the sealing can 3 and the negative electrode layer 42 of the power generation element 4, respectively. .. That is, the restorative conductive sheet 5 is arranged on both the upper surface and the lower surface of the power generation element 4.
- the plan view shape of the restorable conductive sheet 5 is formed to be substantially similar to the plan view shape of the internal space of the all-solid-state battery 1. Therefore, the restorative conductive sheet 5 is formed in a substantially circular shape in a plan view.
- the area of the upper surface of the resilient conductive sheet 5 on the outer can 2 side may be the same as the area of the lower surface of the positive electrode layer 41 of the power generation element 4, or slightly different from the area of the lower surface of the positive electrode layer 41 of the power generation element 4. There may be a difference. Further, the area of the lower surface of the restorable conductive sheet 5 on the sealing can 3 side may be the same as the area of the upper surface of the negative electrode layer 42 of the power generation element 4, or the area of the upper surface of the negative electrode layer 42 of the power generation element 4. There may be a slight difference.
- the upper surface of the restorative conductive sheet 5 on the outer can 2 side preferably covers the lower surface of the positive electrode layer 41, and the lower surface of the restorative conductive sheet 5 on the sealing can 3 side is the upper surface of the negative electrode layer 42. It is preferable to cover the.
- the restoring conductive sheet 5 is pressed together with the power generation element 4 by caulking at the time of battery assembly, and the restoring conductive sheet 5 is compressed in the thickness direction (vertical direction in FIG. 1), and the battery assembly is completed and collected. Functions as an electric sheet.
- the power generation element 4 When the assembled all-solid-state battery 1 is charged and discharged, the power generation element 4 repeatedly expands and contracts, but the restoring conductive sheet 5 is maintained in a compressed state, so that the power generation element 4 is continuously pressed by the repulsive force. As a result, the continuity of the outer can 2 and the power generation element 4 and the continuity of the sealing can 3 and the power generation element 4 can be maintained satisfactorily. Further, by arranging the recoverable conductive sheet 5 between the concave portion 211 of the outer can 2 and the positive electrode layer 41 of the power generation element 4, the recoverable conductive sheet is formed when the outer can 2 and the sealing can 3 are crimped.
- the restoring conductive sheet 5 is not limited to a substantially circular shape in a plan view, and can be variously changed according to the plan view shape of the all-solid-state battery 1, such as an elliptical shape and a substantially polygonal shape in a plan view. Further, the restoring conductive sheet 5 may not be arranged between the power generation element 4 and both the inner bottom surface of the recess 211 of the outer can 2 and the flat surface portion 31 of the sealing can 3, and the power generation element 4 and the exterior may not be arranged.
- the power generation element 4 may be arranged only between the inner bottom surface of the concave portion 211 of the can 2 or only between the power generation element 4 and the flat surface portion 31 of the sealing can 3, and the power generation element 4 is continuously pressed by the repulsive force to the exterior.
- the continuity of the can 2 and the power generation element 4 and the continuity of the sealed can 3 and the power generation element 4 can be maintained satisfactorily.
- the peripheral edge of the flat surface portion 31 of the sealing can 3 is easily deformed by receiving a force during caulking, if the restorative conductive sheet 5 is arranged at least on the side of the flat surface portion 31 of the sealing can 3, this can be achieved. It acts as a cushioning material and can prevent the negative electrode layer 42 from being damaged.
- the restorable conductive sheet 5 may be a graphite sheet as described above.
- the graphite sheet is formed by rolling expanded graphite, and more specifically, it is manufactured as follows. First, the particles of acid-treated graphite obtained by subjecting natural graphite to acid treatment are heated. Then, the acid-treated graphite expands by vaporizing and foaming the acid between the layers.
- the expanded graphite (expanded graphite) is molded into a felt shape and further rolled using a roll rolling mill to form a sheet body.
- the graphite sheet is manufactured by hollowing out the expanded graphite sheet body into a circular shape. As described above, expanded graphite is formed by evaporating the acid and foaming the acid-treated graphite.
- the graphite sheet is formed into a porous sheet. Therefore, the graphite sheet has excellent flexibility and resilience due to the porosity as well as the conductivity of graphite itself. As a result, the graphite sheet functions as a current collector and can suppress damage to the power generation element 4 that expands and contracts during charging and discharging and deterioration of conductivity.
- the method for producing the graphite sheet is not limited to this, and the graphite sheet may be produced by any method.
- the restorative conductive sheet 5 is not limited to the graphite sheet, and may be made of a conductive tape.
- the depth d and the inner diameter d1 of the recess 211 will be described in detail.
- the depth d of the recess 211 is larger than the thickness t of the restorable conductive sheet 5.
- the inner diameter of the recess 211 is larger than the outer diameter of the restorable conductive sheet 5. That is, the entire restorable conductive sheet 5 is housed in the internal space of the recess 211. This makes it possible to prevent the restorative conductive sheet 5 from being sandwiched between the bottom portion 21 of the outer can 2 and the gasket 6 when the outer can 2 and the sealing can 3 are crimped. As a result, the current collecting efficiency of the restorative conductive sheet 5 can be improved.
- the ratio A (t / d) between the depth d of the recess 211 and the restorable conductive sheet 5 is preferably less than 1.0, preferably 0.9 or less, and more preferably 0.9 or less. , 0.8 or less is recommended.
- the restorative conductive sheet 5 is made too thin, the effects of preventing damage and preventing deterioration of conductivity when the power generation element 4 expands and contracts are reduced.
- the ratio A (t / d) between the depth d of the recess 211 and the restorable conductive sheet 5 is preferably 0.5 or more, preferably 0.6 or more, and more preferably 0.6 or more. It should be 0.7 or more.
- the thickness t of the restoring conductive sheet 5 improves the ratio of the power generation element 4 to the internal space of the all-solid-state battery 1, that is, From the viewpoint of improving the battery capacity of the power generation element 4, preventing damage when the power generation element 4 expands and contracts, and preventing deterioration of conductivity, 0.05 mm or more is preferable, and 0.07 mm or more is more preferable. It is preferably 0.5 mm or less, more preferably 0.2 mm or less.
- the thickness t of the restorative conductive sheet 5 (graphite sheet) is not limited to the graphite sheet, and can be applied to the restorative conductive sheet 5 formed of another material such as a conductive tape.
- the apparent density of the recoverable conductive sheet 5 is preferably 0.3 g / cm 3 or more, more preferably 0.7 g / cm 3 or more, and more preferably 1.5 g / cm 3 or less. It is preferably 1.3 g / cm 3 or less. This is because if the apparent density is too low, the restorative conductive sheet 5 (graphite sheet) is easily damaged, and if the apparent density is too high, the flexibility is lowered.
- the apparent density of the restorative conductive sheet 5 (graphite sheet) is not limited to the graphite sheet, and can be applied to the restorative conductive sheet 5 formed of another material such as a conductive tape.
- the restoration rate of the recoverable conductive sheet 5 is preferably 7% or more. Since the restorative conductive sheet 5 (graphite sheet) has such an appropriate stability, the restorative conductive sheet 5 (graphite sheet) moderately presses the power generation element 4. As a result, the continuity between the inner bottom surface of the recess 211 of the outer can 2 and the power generation element 4 can be well maintained, and the continuity between the inner surface of the flat surface portion 31 of the sealing can 3 and the power generation element 4 can be well maintained. Can be done.
- the restoration rate is more preferably 10% or more from the viewpoint of maintaining good continuity.
- the restoration rate is preferably 80% or less, and more preferably 50% or less. , 30% or less is particularly preferable.
- the stability is defined as the thickness of the restoring conductive sheet 5 (graphite sheet) being t, the thickness of the restoring conductive sheet 5 (graphite sheet) when compressed by a predetermined pressing force is t1, and the pressing force is excluded. Restorability at the time When the thickness of the conductive sheet 5 (graphite sheet) is t2, it is expressed by the following formula.
- the recoverable conductive sheet 5 (graphite sheet) has resilience when the recovery rate is equal to or higher than a certain level.
- the restoration rate can be measured by the method described in Japanese Industrial Standards JIS R3453 2001 (joint sheet).
- the restoration rate of the recoverable conductive sheet 5 (graphite sheet) is not limited to the graphite sheet, and can be applied to the recoverable conductive sheet 5 formed of another material such as a conductive tape.
- the apparent density or thickness of the recoverable conductive sheet 5 is determined in a well-balanced manner in consideration of flexibility, resilience, and effective use of the space of the internal space. ..
- the restorable conductive sheet 5 (graphite sheet) has excellent conductivity and flexibility as described above. Therefore, the restorable conductive sheet 5 (graphite sheet) can function as a current collector, expands and contracts due to charging and discharging of the power generation element 4, or crimps the outer can 2 and the sealing can 3. It can absorb the pressing force. As a result, the all-solid-state battery 1 can suppress deterioration of battery performance due to damage to the power generation element 4 and formation of gaps.
- the resilient conductive sheet 5 (graphite sheet) having excellent flexibility is described above with respect to expansion due to charging of the power generation element 4 or compression due to pressing force when caulking the outer can 2 and the sealing can 3. As you can see, it has moderate resilience. As a result, the all-solid-state battery 1 can maintain good continuity between the inner surface of the bottom portion 21 of the outer can 2 and the power generation element 4, and conducts the conduction between the inner surface of the flat surface portion 31 of the sealing can 3 and the power generation element 4. It can be maintained well and the battery performance can be maintained.
- the depth d of the recess 211 is smaller than the height h.
- the height h is the height from the inner bottom surface of the recess 211 to the upper end of the outer peripheral surface of the solid electrolyte layer 43.
- the height h is the total height of the positive electrode layer 41 and the solid electrolyte layer 43. This makes it possible to prevent the bottom portion 21 of the outer can 2 from coming into contact with the negative electrode layer 42 and short-circuiting.
- the height h is the total height of the negative electrode layer 42 and the solid electrolyte layer 43.
- the outer diameter d2 of the restorable conductive sheet 5 is smaller than the inner diameter d1 of the recess 211 in order to accommodate the restorable conductive sheet 5 in the recess 211. If the outer diameter d2 of the restorable conductive sheet 5 is too large with respect to the inner diameter d1 of the recess 211, it becomes difficult to accommodate the restorable conductive sheet 5 in the recess 211. Therefore, the ratio C (d1 / d2) between the inner diameter d1 of the recess 211 and the outer diameter d2 of the restorable conductive sheet 5 is preferably 1.02 or more, preferably 1.05 or more. More preferably, it is 1.08 or more.
- the ratio C (d1 / d2) is preferably 1.15 or less, preferably 1.12 or less, and more preferably 1.09 or less.
- the inner diameter d1 of the recess 211 is smaller than the outer diameter of the positive electrode layer 41 of the power generation element 4. This is because, as shown in FIG. 1, the end portion of the power generation element 4 on the positive electrode layer 41 side is housed in the recess 211.
- the restorative conductive sheet 5 is housed in the recess 211 of the outer can 2. Then, after the power generation element 4 is placed on the upper surface of the restoring conductive sheet 5, the restoring conductive sheet 5 is further placed on the upper surface of the power generation element 4.
- a gasket 6 is formed at the peripheral end of the peripheral wall portion 32 of the sealing can 3.
- the gasket 6 is formed from the inner surface of the peripheral wall portion 32 to the outer surface of the peripheral wall portion 32 through the peripheral end of the peripheral wall portion 32.
- the method for forming the gasket 6 is not particularly limited, but an injection molding method or the like is adopted.
- the sealing can 3 is placed so as to cover the opening of the outer can 2.
- the gasket 6 comes into contact with the inner surface of the bottom portion 21 of the outer can 2, it does not enter the inside of the recess 211.
- the restorable conductive sheet 5 is housed in the recess 211 of the outer can 2, it is possible to prevent the restorable conductive sheet 5 from being sandwiched between the inner surface of the bottom portion 21 of the outer can 2 and the gasket 6. can.
- the tip of the gasket 6 formed on the outside of the peripheral wall portion 32 is pushed together with the tubular side wall portion 22 of the outer can 2 toward the outer peripheral surface of the peripheral wall portion 32 of the sealing can 3.
- the outer can 2 and the sealing can 3 are crimped to complete the all-solid-state battery 1 shown in FIG.
- the all-solid-state battery 1 shown in FIG. 1 assembled using the graphite sheet (restorable conductive sheet 5) can prevent damage to the positive electrode layer 41 and the negative electrode layer 42 due to the resilience of the graphite sheet. Further, the all-solid-state battery 1 is excellent in sealing property because it can prevent the graphite sheet from being sandwiched between the inner surface of the bottom portion 21 of the outer can 2 and the gasket 6. Therefore, when the all-solid-state battery 1 is charged and discharged, a predetermined discharge capacity can be obtained.
- a cycle test was carried out for each of the all-solid-state batteries having the same configuration as that of the battery 1.
- the restorative conductive sheet 5 a graphite sheet having a thickness of 0.1 mm, an apparent density of 1.2 g / cm 3 and a recovery rate of 12% was used.
- the former all-solid-state battery 1 can maintain good continuity between the outer can 2 and the sealing can 3 and the power generation element 4 when the charge / discharge cycle is repeated, so that the battery 1 can be charged even after 100 cycles. It was possible to maintain a discharge capacity of 95% or more compared to before repeating the discharge cycle.
- a metal foam base material (exterior can side: aluminum, sealing can side: copper) having a thickness of 1 mm and a porosity of 97% was used.
- the same cycle test as above was also performed on the all-solid-state battery having the same configuration as the all-solid-state battery 1 shown in FIG. Since the foamed base material of this all-solid-state battery is a current collector having substantially no resilience, it is not possible to maintain good continuity between the outer can and the sealing can and the power generation element. Therefore, the discharge capacity of this all-solid-state battery decreased to about 10% after 100 cycles as compared with that before repeating the charge / discharge cycle.
- the restoring conductive sheet 5 is provided between the power generation element 4 and the inner bottom surface of the recess 211 of the outer can 2, and the power generation element 4 and the inner surface of the flat surface portion 31 of the sealing can 3 are provided.
- the restoring conductive sheet 5 is provided between them, the restoring conductive sheet 5 may be provided only between the power generation element 4 and the inner surface of the flat surface portion 31 of the sealing can 3.
- the peripheral wall portion 32 of the sealing can 3 may be composed of a base end portion 32a, a diameter expansion portion 32b, and a step portion 32c.
- the base end portion 32a is provided so as to extend substantially perpendicular to the flat surface portion 31 in a vertical cross-sectional view.
- the enlarged diameter portion 32b is provided stepwise via a stepped portion 32c so that the diameter is larger than that of the base end portion 32a. That is, the step portion 32c is provided between the base end portion 32a and the diameter-expanded portion 32b.
- the open end of the cylindrical side wall portion 22 of the outer can 2 is bent and crimped toward the step portion 22c.
- the outer can 2 and the sealing can 3 can be sufficiently crimped, and the diameter of the flat surface portion 31 of the sealing can 3 can be made larger than that of the all-solid-state battery 1 of the above-described embodiment.
- the all-solid-state battery 1 shown in FIG. 5 has the same diameter as the all-solid-state battery 1 of the above-described embodiment, the internal space of the all-solid-state battery 1 can be effectively used, or the above-mentioned implementation.
- the all-solid-state battery 1 can be miniaturized. In the all-solid-state battery 1 shown in FIG.
- the peripheral wall portion 32 of the sealing can 3 is bent at the opening end and the enlarged diameter portion 32b is a double wall, but the enlarged diameter portion 32b is not bent and is linear. It is also possible to form the peripheral wall portion 32 so as to face the bottom portion 21 of the outer can 2.
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Abstract
Description
(t2-t1)/(t-t1)×100(%)
復元率は、日本産業規格JIS R3453 2001(ジョイントシート)に記載された方法で測定することができる。なお、復元性導電シート5(黒鉛シート)の復元率は、黒鉛シートに限られるものではなく、導電性テープなど他の素材によって形成された復元性導電シート5においても適用可能である。
上記実施形態の全固体電池1では、発電要素4と外装缶2の凹部211の内底面との間に復元性導電シート5を設け、発電要素4と封口缶3の平面部31の内面との間に復元性導電シート5を設けたが、復元性導電シート5を発電要素4と封口缶3の平面部31の内面との間にのみ設けることもできる。
2 外装缶、21 底部、211 凹部、22 筒状側壁部
3 封口缶、31 平面部、32 周壁部
4 発電要素、41 正極層、42 負極層、43 固体電解質層
5 復元性導電シート
6 ガスケット
Claims (5)
- 外方に窪む凹部を含む底部及び筒状側壁部を有する外装缶と、
平面部及び周壁部を有し、前記外装缶の開口を覆う封口缶と、
前記外装缶の凹部の内底面と前記封口缶の平面部との間に配置され、正極層と負極層と前記正極層及び前記負極層の間に配置される固体電解質層とを有する発電要素と、
前記外装缶の筒状側壁部と前記封口缶の周壁部との間でカシメられるガスケットと、
前記発電要素と前記凹部の内底面及び前記封口缶の平面部の少なくとも一方との間に配置される第1の復元性導電シートとを備える、全固体電池。 - 請求項1に記載の全固体電池であって、
前記第1の復元性導電シートは、前記凹部の内底面と前記発電要素との間に配置され、
前記凹部の深さは、前記第1の復元性導電シートの厚みよりも大きい、全固体電池。 - 請求項1又は2に記載の全固体電池であって、
前記第1の復元性導電シートは、前記凹部の内底面と前記発電要素との間に配置され、
前記全固体電池はさらに、
前記封口缶の平面部と前記発電要素との間に配置される第2の復元性導電シートを備える、全固体電池。 - 請求項1~3のいずれか1項に記載の全固体電池であって、
前記凹部の深さは、前記凹部の内底面から前記固体電解質層の外周面の上端までの高さよりも小さい、全固体電池。 - 請求項1~4のいずれか1項に記載の全固体電池であって、
前記第1及び第2の復元性導電シートは、黒鉛シートである、全固体電池。
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JP2022519526A JPWO2022102639A1 (ja) | 2020-11-13 | 2021-11-10 | |
US18/036,746 US20230411802A1 (en) | 2020-11-13 | 2021-11-10 | All-solid-state battery |
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JPH11144761A (ja) | 1997-11-10 | 1999-05-28 | Toyota Motor Corp | リチウムイオン2次電池 |
JP2003151511A (ja) | 2001-11-16 | 2003-05-23 | Hitachi Maxell Ltd | 扁平形非水電解質電池 |
JP2004146127A (ja) * | 2002-10-22 | 2004-05-20 | Matsushita Electric Ind Co Ltd | エネルギー蓄積デバイス |
JP2005056827A (ja) * | 2003-07-23 | 2005-03-03 | Matsushita Electric Ind Co Ltd | コイン型全固体電池 |
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JP2016171169A (ja) * | 2015-03-12 | 2016-09-23 | セイコーインスツル株式会社 | 電気化学セル、及び端子付電気化学セル |
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2021
- 2021-11-10 WO PCT/JP2021/041276 patent/WO2022102639A1/ja active Application Filing
- 2021-11-10 JP JP2022519526A patent/JPWO2022102639A1/ja active Pending
- 2021-11-10 CN CN202180075878.XA patent/CN116457972A/zh active Pending
- 2021-11-10 EP EP21891885.2A patent/EP4246644A1/en active Pending
- 2021-11-10 US US18/036,746 patent/US20230411802A1/en active Pending
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JPH11144761A (ja) | 1997-11-10 | 1999-05-28 | Toyota Motor Corp | リチウムイオン2次電池 |
JP2003151511A (ja) | 2001-11-16 | 2003-05-23 | Hitachi Maxell Ltd | 扁平形非水電解質電池 |
JP2004146127A (ja) * | 2002-10-22 | 2004-05-20 | Matsushita Electric Ind Co Ltd | エネルギー蓄積デバイス |
JP2005056827A (ja) * | 2003-07-23 | 2005-03-03 | Matsushita Electric Ind Co Ltd | コイン型全固体電池 |
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WO2024018982A1 (ja) * | 2022-07-19 | 2024-01-25 | マクセル株式会社 | 全固体電池 |
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EP4246644A1 (en) | 2023-09-20 |
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