WO2012124108A1 - 固体電池、及び固体電池の製造方法 - Google Patents
固体電池、及び固体電池の製造方法 Download PDFInfo
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- WO2012124108A1 WO2012124108A1 PCT/JP2011/056427 JP2011056427W WO2012124108A1 WO 2012124108 A1 WO2012124108 A1 WO 2012124108A1 JP 2011056427 W JP2011056427 W JP 2011056427W WO 2012124108 A1 WO2012124108 A1 WO 2012124108A1
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/30—Arrangements for facilitating escape of gases
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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
- H01M6/00—Primary cells; Manufacture thereof
- H01M6/42—Grouping of primary cells into batteries
- H01M6/46—Grouping of primary cells into batteries of flat cells
- H01M6/48—Grouping of primary cells into batteries of flat cells with bipolar electrodes
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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
- H01M10/04—Construction or manufacture in general
- H01M10/0436—Small-sized flat cells or batteries for portable equipment
- H01M10/044—Small-sized flat cells or batteries for portable equipment with bipolar electrodes
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
- H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
- H01M10/0562—Solid materials
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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
- H01M10/058—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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- 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
- H01M10/34—Gastight accumulators
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/471—Spacing elements inside cells other than separators, membranes or diaphragms; Manufacturing processes thereof
- H01M50/474—Spacing elements inside cells other than separators, membranes or diaphragms; Manufacturing processes thereof characterised by their position inside the cells
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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
- 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
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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
- 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
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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
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T29/00—Metal working
- Y10T29/49—Method of mechanical manufacture
- Y10T29/49002—Electrical device making
- Y10T29/49108—Electric battery cell making
- Y10T29/4911—Electric battery cell making including sealing
Definitions
- the present invention relates to a solid battery sealed under reduced pressure in an exterior material, and a method for manufacturing the solid battery.
- Lithium ion secondary batteries are characterized by higher energy density than other secondary batteries and capable of operating at high voltages. For this reason, it is used as a secondary battery that can be easily reduced in size and weight in information equipment such as a mobile phone, and in recent years, there is an increasing demand for large motive power such as for electric vehicles and hybrid vehicles.
- the lithium ion secondary battery includes a positive electrode layer and a negative electrode layer, and an electrolyte layer disposed therebetween. Further, as the electrolyte provided in the electrolyte layer, for example, a non-aqueous liquid or solid is used. When a liquid (hereinafter referred to as “electrolytic solution”) is used as the electrolyte, the electrolytic solution easily penetrates into the positive electrode layer and the negative electrode layer. Therefore, an interface between the active material contained in the positive electrode layer or the negative electrode layer and the electrolytic solution is easily formed, and the performance is easily improved. However, since the widely used electrolyte is flammable, it is necessary to mount a system for ensuring safety.
- solid electrolyte (hereinafter referred to as “solid electrolyte”) is nonflammable, the above system can be simplified. Therefore, a lithium ion secondary battery in a form provided with a layer containing a solid electrolyte that is nonflammable has been proposed.
- a bipolar electrode in which a positive electrode is formed on one surface of a current collector and a negative electrode is formed on the other surface is sandwiched with an electrolyte layer.
- the bipolar secondary battery element is disposed between the bipolar secondary battery element and the outer packaging material more than the outer packaging material.
- Patent Document 1 discloses a unit cell in which a positive electrode layer, an electrolyte layer, and a negative electrode layer are stacked, and a seal portion disposed around the unit cell in a cross-sectional view perpendicular to the stacking direction of the unit cells.
- a battery having a configuration including the unit cell and a pair of current collectors sandwiching the seal portion is disclosed. By providing the seal portion in this manner, adjacent current collectors can be insulated.
- an exterior material as disclosed in Patent Document 1
- the space surrounded by the exterior material hereinafter referred to as “inside the exterior material”
- the seal portion disposed at the outer edge portion of the unit cell prevents the gas from flowing, so that the gas in the space surrounded by the seal portion cannot escape.
- the gas in the exterior material may expand during heat generation, or the gas in the exterior material may react with the constituent members of the battery. .
- the present invention relates to a solid state battery that is sealed under reduced pressure in an exterior material, the solid battery capable of exhausting the gas in the exterior material when the inside of the exterior material is decompressed, and a method for producing the solid battery.
- the issue is to provide.
- a first aspect of the present invention includes a laminate including a positive electrode layer, a negative electrode layer, and an electrolyte layer disposed between the positive electrode layer and the negative electrode layer, and a cross section in a direction perpendicular to the stacking direction of the laminate.
- a single cell comprising an insulating portion disposed on the outer periphery of the laminated body and a pair of current collectors sandwiching the laminated body and the insulating portion as viewed, and the single cell is decompressed in an exterior material. It is a solid state battery characterized in that it is sealed and the insulating part has a vent hole.
- vent hole means a hole through which a gas in the exterior material can pass when the interior of the exterior material is depressurized in the manufacturing process of the solid battery of the present invention.
- the air hole of the insulating portion is crushed.
- vent hole is crushed means that the vent hole that had air permeability before the production of the solid battery of the present invention was crushed in the production process of the solid battery of the present invention, It means that the air permeability of the vent is lost.
- breathability means the property of allowing gas to pass from one space partitioned by an insulating portion to the other space. Usually, even if a member having such a vent hole is crushed by pressurization or heating, it is possible to find a trace of the vent hole.
- the solid state battery according to the first aspect of the present invention may have a form in which a plurality of unit cells are sealed under reduced pressure in an exterior material.
- a laminate including a positive electrode layer, a negative electrode layer, and an electrolyte layer disposed between the positive electrode layer and the negative electrode layer, and a cross-sectional view in a direction perpendicular to the lamination direction of the laminate.
- Manufacturing a unit cell comprising an insulating part having a vent and a pair of current collectors sandwiching the layered body and the insulating unit, disposed on the outer periphery of the laminate, and the unit cell as an exterior material
- a method for producing a solid state battery comprising: a step of sealing under reduced pressure inside, and a step of crushing a vent hole of an insulating portion.
- crushing the air vent means that the air permeability of the air vent is lost.
- a solid state battery sealed under reduced pressure in an exterior material the solid state battery capable of extracting gas in the exterior material when decompressing the interior of the exterior material, and a method for producing the solid battery Can be provided.
- FIG. 1 is a cross-sectional view schematically showing a solid state battery 10 of the present invention according to one embodiment.
- 2A to 2E are diagrams for explaining the manufacturing process of the solid state battery 10.
- FIG. 3A is a view taken in the direction of arrows IIIA-IIIA in FIG.
- FIG. 3B is a view taken along the arrow IIIB-IIIB in FIG. It is sectional drawing which shows schematically the solid battery 20 of this invention concerning other embodiment.
- the solid battery of the present invention is a lithium ion secondary battery having a solid electrolyte layer.
- FIG. 1 is a cross-sectional view schematically showing a solid state battery 10 of the present invention according to one embodiment.
- the vertical direction of the drawing in FIG. 1 is the stacking direction.
- a solid battery 10 includes a laminated body 4 including a positive electrode layer 1, a negative electrode layer 2, and an electrolyte layer 3 disposed between the positive electrode layer 1 and the negative electrode layer 2, and a laminated body 4.
- a cell comprising: an insulating portion 6 disposed on the outer periphery of the laminated body 4 in a cross-sectional view in a direction orthogonal to the laminating direction; and a pair of current collectors 5 and 5 sandwiching the laminated body 4 and the insulating portion 6. 8 is provided.
- the unit cell 8 is hermetically sealed in the exterior material 7.
- the current collector 5 in contact with the positive electrode layer 1 is referred to as a positive electrode current collector 5a
- the current collector 5 in contact with the negative electrode layer 2 is referred to as a negative electrode current collector 5b.
- the insulating part 6 is composed of the first insulating layer 6a and the second insulating layer 6b, and a part of the insulating part 6 on the positive electrode current collector 5a side is referred to as a first insulating layer 6a.
- a part of the insulating portion 6 on the negative electrode current collector 5b side may be referred to as a second insulating layer 6b.
- the solid battery 10 also includes a positive electrode terminal 8a (see FIG. 3A) connected to the positive electrode current collector 5a and a negative electrode terminal 8b (see FIG. 3B) connected to the negative electrode current collector 5b. I have.
- the positive electrode current collector 5 a and the negative electrode current collector 5 b can be made of a known conductive material that can be used as a positive electrode current collector or a negative electrode current collector of a lithium ion secondary battery.
- a conductive material include one or more elements selected from the group consisting of Cu, Ni, Al, V, Au, Pt, Mg, Fe, Ti, Co, Cr, Zn, Ge, and In. Examples of the metal material to be included are illustrated.
- the form of the positive electrode current collector 5a and the negative electrode current collector 5b can be, for example, a metal foil or a metal mesh.
- the insulating part 6 includes a first insulating layer 6a and a second insulating layer 6b. Moreover, the 1st insulating layer 6a and the 2nd insulating layer 6b are provided with the crushed ventilation hole.
- the “crushed vent” is a hole having air permeability before the solid battery 10 is manufactured, and is a hole that has lost air permeability by being crushed in the manufacturing process of the solid battery 10 as will be described later. Means. Note that “breathability” means a property that allows gas to pass from one space partitioned by the insulating portion 6 to the other space as will be described later.
- the air holes provided in the members used for the first insulating layer 6a and the second insulating layer 6b are formed in the exterior material 7 (enclosed by the insulation portion 6) when the interior of the exterior material 7 is decompressed in the manufacturing process of the solid battery 10 described later. It is sufficient that the gas can be passed through the space and can be crushed by pressurization and / or heating.
- a form of such a vent hole there are a hole configured by connecting a plurality of bubbles, a straight through hole, and the like.
- the first insulating layer 6a and the second insulating layer 6b have air permeability and can be lost by pressurization and / or heating, etc., when the solid battery 10 is used. It can be made of a known insulating material that can withstand this environment. Examples of such an insulating material include a polyurethane sponge having open cells, a polyamideimide resin, an epoxy resin, and a fluorine resin.
- Positive electrode layer 1 As the positive electrode active material contained in the positive electrode layer 1, a known active material that can be contained in the positive electrode layer of the lithium ion secondary battery can be appropriately used. Examples of such a positive electrode active material include lithium cobaltate (LiCoO 2 ). Moreover, as the electrolyte contained in the positive electrode layer 1, a known electrolyte that can be contained in the positive electrode layer of the battery can be appropriately used.
- organic solid electrolytes such as polyethylene oxide can be exemplified.
- the positive electrode layer 1 may contain a binder that binds the positive electrode active material and the electrolyte and a conductive material that improves conductivity.
- Examples of the binder that can be contained in the positive electrode layer 1 include butylene rubber, and examples of the conductive material that can be contained in the positive electrode layer 1 include carbon black.
- a solvent used when manufacturing the positive electrode layer 1 the well-known solvent which can be used when adjusting the slurry used at the time of positive electrode layer preparation of a lithium ion secondary battery can be used suitably. As such a solvent, heptane and the like can be exemplified.
- the negative electrode active material contained in the negative electrode layer 2 As the negative electrode active material contained in the negative electrode layer 2, a known active material that can be contained in the negative electrode layer of the lithium ion secondary battery can be appropriately used. Examples of such an active material include graphite.
- the electrolyte contained in the negative electrode layer 5 As the electrolyte contained in the negative electrode layer 5, a known electrolyte that can be contained in the negative electrode layer of the lithium ion secondary battery can be appropriately used.
- the said inorganic solid electrolyte, organic solid electrolyte, etc. which can be contained in the positive electrode layer 1 can be illustrated.
- the negative electrode layer 2 may contain a binder for binding the negative electrode active material and the electrolyte and a conductive material for improving conductivity.
- binder and conductive material that can be contained in the negative electrode layer 2 examples include the binder and conductive material that can be contained in the positive electrode layer 1.
- the binder and conductive material that can be contained in the positive electrode layer 1 examples include the binder and conductive material that can be contained in the positive electrode layer 1.
- the said solvent etc. which can be used when producing the positive electrode layer 1 can be illustrated.
- Solid electrolyte layer 3 Examples of the solid electrolyte contained in the solid electrolyte layer 3 include the inorganic solid electrolyte and the organic solid electrolyte that can be contained in the positive electrode layer 1. Moreover, as a solvent used when producing the solid electrolyte layer 3, the said solvent etc. which can be used when producing the positive electrode layer 1 can be illustrated.
- the packaging material 7 can withstand the environment during use of the lithium ion secondary battery, has a property of not allowing gas or liquid to permeate, and can be sealed without particular limitation. Can do.
- Examples of the material constituting the exterior material 7 include known metal foils typified by aluminum foils, films made of resins typified by polyethylene, polyvinyl fluoride, polyvinylidene chloride, and the like. Examples thereof include a metal-deposited film in which a metal such as aluminum is deposited on the surface thereof.
- FIG. 1 illustrates a form in which the exterior material 7 is composed of a single bag-like member. However, the exterior material 7 has a form in which the cell 8 is sandwiched between two films. Further, it may be composed of a plurality of members.
- the positive electrode terminal 8a and the negative electrode terminal 8b can be made of a material having good electrical conductivity that can withstand the environment when the solid battery 10 is used, and can cope with the force applied when the solid battery 10 is used. It is preferable to comprise by the material which has intensity
- the positive electrode current collector 5a can be formed so as to partially protrude, and the protruding portion can be used as the positive electrode terminal 8a, and the negative electrode current collector 5b can be partially protruded.
- the protruding portion can be used as the negative electrode terminal 8b.
- the manufacturing method of such a solid battery 10 is not particularly limited, for example, it can be manufactured through the following steps.
- FIG. 2 (A) to 2 (E) are diagrams for explaining a manufacturing process of the solid state battery 10.
- 3A is a view taken in the direction of arrows IIIA-IIIA in FIG. 2A
- FIG. 3B is a view taken in the direction of arrows IIIB-IIIB in FIG. 2A to 2E and the back / front direction of FIG. 3A and FIG. 3B are stacking directions.
- the first insulating layer 6a is formed on the outer edge of the positive electrode current collector 5a to which the positive electrode terminal 8a is connected by a known method such as thermocompression bonding. .
- a masking material is disposed on the surface of the first insulating layer 6a, and the positive electrode layer 1 is formed on the surface of the positive electrode current collector 5a surrounded by the first insulating layer 6a.
- the positive electrode layer 1 is, for example, a well-known method such as a doctor blade method in which a positive electrode slurry prepared by dispersing at least a positive electrode active material and a solid electrolyte in a solvent is applied to the entire surface of the positive electrode current collector 5a surrounded by the first insulating layer 6a. It can be formed by applying the method and evaporating the solvent. In this way, as shown in FIGS. 2A and 3A, the first stacked body 4a including the positive electrode layer 1, the positive electrode current collector 5a, and the first insulating layer 6a can be manufactured. it can.
- the second insulating layer 6b is formed by a known method similar to that for the first insulating layer 6a, as shown in FIGS. 2A and 3B. Form on the outer edge.
- a masking material is disposed on the surface of the second insulating layer 6b, and the negative electrode layer 2 is formed on the surface of the negative electrode current collector 5b surrounded by the second insulating layer 6b.
- the negative electrode layer 2 is, for example, a well-known method such as a doctor blade method in which a negative electrode slurry prepared by dispersing at least a negative electrode active material and a solid electrolyte in a solvent is applied to the entire surface of the negative electrode current collector 5b surrounded by the second insulating layer 6b. It can be formed by applying the method and evaporating the solvent.
- a known method such as a doctor blade method
- the solid electrolyte layer 3 can be formed on the negative electrode layer 2 through a process of volatilizing the solvent.
- the second stacked body 4b including the negative electrode layer 2, the negative electrode current collector 5b, and the second insulating layer 6b can be manufactured. it can.
- the masking material of the first laminate 4a and the second laminate 4b produced as described above is removed, and the positive electrode layer 1 and the solid electrolyte layer 3 face each other as shown in FIG. In this manner, the first stacked body 4a and the second stacked body 4b are stacked.
- the first laminated body 4a and the second laminated body 4b are accommodated in an exterior material 7 having an exhaust port 7a for vacuuming.
- an exterior material 7 having an exhaust port 7a for vacuuming.
- at least a part of the positive electrode terminal 8 a and the negative electrode terminal 8 b is not accommodated in the exterior material 7.
- the exterior material 7 is evacuated (depressurized).
- the vacuuming pressure is not particularly limited, and can be, for example, about 0.1 MPa.
- the inner side is the outer side (outer peripheral side, the end in the left-right direction in FIG. 2B) viewed from the stacking direction of the first stack 4a and the second stack 4b. B) the central portion in the left-right direction. Therefore, the first insulating layer 6 a and the second insulating layer 6 b are more easily pressed by the exterior material 7 than the positive electrode layer 1 and the solid electrolyte layer 3. As a result, as shown in FIG. 2C, a space S defined by the first insulating layer 6a, the second insulating layer 6b, the positive electrode layer 1, and the solid electrolyte layer 3 is formed.
- the conventional solid battery may cause problems such as expansion of the gas in the exterior material during heat generation, and reaction of the gas in the exterior material and the constituent members of the battery. Further, if the gas in the space S remains, there is a possibility that the battery performance may be deteriorated due to the insufficient interface formed between the solid electrolyte layer and the positive electrode layer or the negative electrode layer.
- the first insulating layer 6a and the second insulating layer 6b have vent holes, so that the gas in the space S is exhausted as shown in FIG. be able to.
- the exhaust port 7a of the exterior material 7 can be sealed by, for example, heat welding.
- the solid battery 10 can be manufactured as shown in FIG. 2 (E) by applying pressure in the stacking direction using appropriate pressure members 20 and 20.
- the pressure applied in this pressurizing step can be appropriately determined according to the form of the solid battery to be produced.
- the pressure can be set to 1 MPa or more and 500 MPa or less, for example.
- the method of crushing the air holes of the first insulating layer 6a and the second insulating layer 6b is not limited to pressurization, and the air holes of the first insulating layer 6a and the second insulating layer 6b can be formed by applying pressure while heating or heating. May be crushed.
- the solid state battery of the present invention by forming the insulating portion with the insulating member having the air hole, the gas in the exterior material can be exhausted during the manufacturing process as described above. Therefore, the solid state battery of the present invention can prevent the gas in the exterior material from expanding during heat generation or the like, and the reaction of the gas in the exterior material and the members constituting the battery. Further, the solid electrolyte layer and the positive electrode layer or the negative electrode layer can be brought into close contact with each other to improve battery performance. Further, as described above, the solid battery of the present invention can insulate the current collectors by crushing the ventilation holes of the insulating portion in the manufacturing process.
- the insulating part 6 is constituted by the first insulating layer 6a formed on the positive electrode current collector 5a and the second insulating layer 6b formed on the negative electrode current collector 5b.
- the solid battery of the present invention is not limited to this form.
- the insulating part may be composed of one member. In this case, the insulating part may be formed only on one of the positive electrode current collector and the negative electrode current collector in the manufacturing process.
- the first insulating layer 6a is formed prior to the positive electrode layer 1 and the second insulating layer 6b is formed prior to the negative electrode layer 2 in the manufacturing process.
- the solid battery is not limited to this form.
- an insulating layer may be formed on the outer periphery thereof, and after forming the negative electrode layer on the current collector, the insulating layer may be formed on the outer periphery thereof.
- an insulating layer may be formed on the outer periphery thereof.
- the negative electrode layer and the solid electrolyte layer on the current collector the insulating layer may be formed on the outer periphery thereof. Good.
- FIG. 4 is a cross-sectional view schematically showing a solid state battery 20 according to another embodiment of the present invention.
- a plurality of bipolar electrodes in which the positive electrode layer 1 is formed on one surface of the current collector 5 and the negative electrode layer 2 is formed on the other surface of the current collector 5 are prepared.
- a solid battery 20 in which a plurality of single cells are accommodated in the exterior member 17 can be obtained.
- a method for forming the insulating portion 6, a method for sealing under reduced pressure in the exterior material 17, and the like can be the same as those for the solid battery 10 described above.
- the substantially rectangular parallelepiped unit cell 8 is illustrated, but the unit cell used in the present invention is not limited to this shape.
- the unit cell may have other shapes such as a cylindrical shape or a hexagonal column shape.
- the single battery 8 that is a lithium ion secondary battery is provided, but a battery to which the present invention is applicable is not limited to this mode.
- the unit cell according to the present invention may be configured such that ions other than lithium ions move between the positive electrode layer and the negative electrode layer. Examples of such ions include sodium ions and potassium ions.
- the positive electrode active material, the solid electrolyte, and the negative electrode active material may be appropriately selected according to the moving ions.
- the single battery in the present invention can be a primary battery.
- the solid state battery of the present invention can be used as a power source for portable devices, electric vehicles, hybrid vehicles, and the like.
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Abstract
Description
本発明の第1の態様は、正極層、負極層、並びに、正極層及び負極層の間に配設された電解質層を備えた積層体と、該積層体の積層方向に直交する方向の断面視において積層体の外周に配設された絶縁部と、該積層体及び該絶縁部を挟持する一対の集電体と、を備える単電池を備えており、該単電池が外装材内に減圧密封されており、絶縁部が通気孔を備えていることを特徴とする、固体電池である。
固体電池10において、正極集電体5aや負極集電体5bは、リチウムイオン二次電池の正極集電体や負極集電体として使用可能な公知の導電性材料によって構成することができる。そのような導電性材料としては、Cu、Ni、Al、V、Au、Pt、Mg、Fe、Ti、Co、Cr、Zn、Ge、Inからなる群から選択される一又は二以上の元素を含む金属材料を例示することができる。また、正極集電体5a及び負極集電体5bの形態は、例えば、金属箔や金属メッシュ等とすることができる。
絶縁部6は、第1絶縁層6a及び第2絶縁層6bから構成されている。また、第1絶縁層6a及び第2絶縁層6bは、潰された通気孔を備えている。「潰された通気孔」とは、固体電池10を製造する前には通気性を有する孔であり、後に説明するように固体電池10の製造過程において潰されることにより、通気性を失った孔を意味する。なお、「通気性」とは、後に説明するように絶縁部6で区切られた一方の空間から他方の空間へと気体を通すことができる性質を意味する。通常、このような通気孔を有していた部材は、加圧や加熱等して該通気孔を潰したとしても、該通気孔が存在していた痕跡を見つけることが可能である。第1絶縁層6a及び第2絶縁層6bに用いられる部材が備える通気孔は、後に説明する固体電池10の製造過程で外装材7内を減圧する際に外装材7内(絶縁部6で囲まれた空間)の気体を通すことができ、加圧及び/又は加熱することによって潰せる程度の大きさであればよい。このような通気孔の形態としては、複数の気泡が一繋がりになることによって構成される孔や、直線状の貫通孔等がある。このような第1絶縁層6a及び第2絶縁層6bは、通気性を有するとともに、加圧及び/又は加熱する等して該通気性を失わせることが可能であり、固体電池10の使用時の環境に耐え得る公知の絶縁性材料によって構成することができる。そのような絶縁性材料としては、例えば、連続気泡を有するポリウレタンスポンジ、ポリアミドイミド樹脂、エポキシ樹脂、フッ素樹脂等を挙げることができる。
正極層1に含有させる正極活物質としては、リチウムイオン二次電池の正極層に含有させることが可能な公知の活物質を適宜用いることができる。そのような正極活物質としては、コバルト酸リチウム(LiCoO2)等を例示することができる。また、正極層1に含有させる電解質としては、電池の正極層に含有させることが可能な公知の電解質を適宜用いることができる。そのような電解質としては、Li3PO4等の酸化物系固体電解質、Li3PS4や、Li2S:P2S5=50:50~100:0となるようにLi2S及びP2S5を混合して作製した硫化物系固体電解質(例えば、質量比で、Li2S:P2S5=75:25となるようにLi2S及びP2S5を混合して作製した硫化物固体電解質)等の無機固体電解質のほか、ポリエチレンオキサイド等の有機固体電解質を例示することができる。このほか、正極層1には、正極活物質や電解質を結着させるバインダーや導電性を向上させる導電材が含有されていてもよい。正極層1に含有させることが可能なバインダーとしては、ブチレンゴム等を例示することができ、正極層1に含有させることが可能な導電材としては、カーボンブラック等を例示することができる。また、正極層1を作製する際に用いる溶媒としては、リチウムイオン二次電池の正極層作製時に用いるスラリーを調整する際に使用可能な公知の溶媒を適宜用いることができる。そのような溶媒としては、ヘプタン等を例示することができる。
負極層2に含有させる負極活物質としては、リチウムイオン二次電池の負極層に含有させることが可能な公知の活物質を適宜用いることができる。そのような活物質としては、グラファイト等を例示することができる。また、負極層5に含有させる電解質としては、リチウムイオン二次電池の負極層に含有させることが可能な公知の電解質を適宜用いることができる。そのような電解質としては、正極層1に含有させることが可能な上記無機固体電解質や有機固体電解質等を例示することができる。このほか、負極層2には、負極活物質や電解質を結着させるバインダーや導電性を向上させる導電材が含有されていてもよい。負極層2に含有させることが可能なバインダーや導電材としては、正極層1に含有させることが可能な上記バインダーや導電材等を例示することができる。また、負極層3を作製する際に用いる溶媒としては、正極層1を作製する際に使用可能な上記溶媒等を例示することができる。
固体電解質層3に含有させる固体電解質としては、正極層1に含有させることが可能な上記無機固体電解質や有機固体電解質等を例示することができる。また、固体電解質層3を作製する際に用いる溶媒としては、正極層1を作製する際に使用可能な上記溶媒等を例示することができる。
外装材7は、リチウムイオン二次電池の使用時の環境に耐えることができ、気体や液体を透過させない性質を有し、且つ、密封することができるものを、特に限定されることなく用いることができる。このような外装材7を構成するものとしては、アルミニウム箔等に代表される公知の金属箔や、ポリエチレン、ポリフッ化ビニルやポリ塩化ビニリデン等に代表される樹脂からなるフィルムのほか、これらのフィルムの表面にアルミニウム等の金属を蒸着させた金属蒸着フィルム等を例示することができる。なお、図1には外装材7が一つの袋状の部材で構成される形態を例示しているが、外装材7は2枚のフィルムで単電池8を挟んで包むような形態であってもよく、さらに複数の部材で構成されていてもよい。
正極端子8a及び負極端子8bは、固体電池10の使用時の環境に耐え得る良好な電気伝導性を有する材料によって構成することができ、固体電池10の使用時に付与される力にも対応可能な強度及び柔軟性を有する材料によって構成することが好ましい。例えば、図3に示したように、正極集電体5aを一部が突出するように形成し、該突出部分を正極端子8aとすることができ、負極集電体5bを一部が突出するように形成し、該突出部分を負極端子8bとすることができる。
2 負極層
3 固体電解質層
4a 第1積層体
4b 第2積層体
4 積層体
5 集電体
6 絶縁部
6a 第1絶縁層
6b 第2絶縁層
7 外装材
8 素電池
10 固体電池
17 外装材
20 固体電池
Claims (4)
- 正極層、負極層、並びに、前記正極層及び前記負極層の間に配設された電解質層を備えた積層体と、
前記積層体の積層方向に直交する方向の断面視において前記積層体の外周に配設された絶縁部と、
前記積層体及び前記絶縁部を挟持する一対の集電体と、
を備える単電池を備えており、
前記単電池が外装材内に減圧密封されており、
前記絶縁部が通気孔を備えていることを特徴とする、固体電池。 - 前記通気孔が潰されていることを特徴とする、請求項1に記載の固体電池。
- 前記外装材内に複数の前記単電池が減圧密封されていることを特徴とする、請求項1又は2に記載の固体電池。
- 正極層、負極層、並びに、前記正極層及び前記負極層の間に配設された電解質層を備えた積層体と、前記積層体の積層方向に直交する方向の断面視において前記積層体の外周に配設された、通気孔を有する絶縁部と、前記積層体及び前記絶縁部を挟持する一対の集電体と、を備える単電池を作製する工程と、
前記単電池を外装材内に減圧密封する工程と、
前記絶縁部の前記通気孔を潰す工程と、
を備えていることを特徴とする、固体電池の製造方法。
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