WO2020013295A1 - 全固体二次電池の製造設備 - Google Patents
全固体二次電池の製造設備 Download PDFInfo
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- WO2020013295A1 WO2020013295A1 PCT/JP2019/027585 JP2019027585W WO2020013295A1 WO 2020013295 A1 WO2020013295 A1 WO 2020013295A1 JP 2019027585 W JP2019027585 W JP 2019027585W WO 2020013295 A1 WO2020013295 A1 WO 2020013295A1
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0402—Methods of deposition of the material
- H01M4/0404—Methods of deposition of the material by coating on electrode collectors
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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
- H01M10/0404—Machines for assembling batteries
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
- B05B—SPRAYING APPARATUS; ATOMISING APPARATUS; NOZZLES
- B05B5/00—Electrostatic spraying apparatus; Spraying apparatus with means for charging the spray electrically; Apparatus for spraying liquids or other fluent materials by other electric means
- B05B5/025—Discharge apparatus, e.g. electrostatic spray guns
- B05B5/03—Discharge apparatus, e.g. electrostatic spray guns characterised by the use of gas, e.g. electrostatically assisted pneumatic spraying
- B05B5/032—Discharge apparatus, e.g. electrostatic spray guns characterised by the use of gas, e.g. electrostatically assisted pneumatic spraying for spraying particulate materials
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B05—SPRAYING OR ATOMISING IN GENERAL; APPLYING FLUENT MATERIALS TO SURFACES, IN GENERAL
- B05B—SPRAYING APPARATUS; ATOMISING APPARATUS; NOZZLES
- B05B5/00—Electrostatic spraying apparatus; Spraying apparatus with means for charging the spray electrically; Apparatus for spraying liquids or other fluent materials by other electric means
- B05B5/16—Arrangements for supplying liquids or other fluent material
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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
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/043—Processes of manufacture in general involving compressing or compaction
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/049—Manufacturing of an active layer by chemical means
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
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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
- H01M2300/00—Electrolytes
- H01M2300/0017—Non-aqueous electrolytes
- H01M2300/0065—Solid electrolytes
- H01M2300/0068—Solid electrolytes inorganic
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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
Definitions
- the present invention relates to a facility for manufacturing an all-solid secondary battery.
- All-solid secondary batteries are known as safe secondary batteries because they do not require the use of flammable organic solvents. Instead of using a flammable organic solvent, the all-solid-state secondary battery mainly has a powder laminate made of a powder material. For this reason, the all-solid-state secondary battery has improved safety, but also has a problem derived from a powder material.
- the powder material of each layer may be mixed between adjacent layers.
- a method has been proposed in which a slurry serving as a material for another layer is sprayed onto a dried layer by a spray method so that the powder material is not mixed and the other layer is formed.
- Such a method is disclosed, for example, in Japanese Patent Application Laid-Open No. 2012-252833 (hereinafter referred to as patent document).
- the method described in the above-mentioned patent document employs a wet method in which a powder material is dissolved in a solvent to form a slurry.
- the wet method if impurities such as a solvent cannot be completely removed from the powder laminate, the impurities will remain in the powder laminate. Further, the portion from which the impurities have been removed may remain in the powder laminate as voids. Since such impurities and voids do not function as a battery, if the impurities and / or voids remain in the powder laminate, the battery performance of the all-solid-state secondary battery including the powder laminate decreases. .
- an object of the present invention is to provide an all-solid-state secondary battery manufacturing facility capable of improving battery performance.
- an all-solid-state secondary battery manufacturing facility is an all-solid-state secondary battery manufacturing facility having a powder stack formed by stacking powder films.
- a mixing device for mixing a plurality of types of powder materials A conveying device for conveying the powder material mixed by the mixing device, From the powder material transported by the transport device, comprising an electrostatic film forming apparatus that forms the powder film using at least electrostatic force, The process of forming the powder laminate from the plurality of types of powder materials is a dry process.
- the powder laminate in the manufacturing equipment for the all-solid secondary battery according to the first invention has a positive electrode layer, a solid electrolyte layer, and a negative electrode layer.
- An electrostatic film forming apparatus includes: a positive electrode electrostatic film forming machine for forming a positive electrode layer; an electrolyte electrostatic film forming machine for forming a solid electrolyte layer; and a negative electrode static film forming machine for forming a negative electrode layer. And an electro-deposition machine.
- the transport device in the manufacturing equipment for the all-solid secondary battery according to the second invention uses a powder material for forming a positive electrode layer for a positive electrode.
- the apparatus further includes an electrolyte transporter that transports the powder material for forming the solid electrolyte layer to the electrolyte electrostatic film forming machine.
- the solid electrolyte layer in the manufacturing equipment for the all-solid secondary battery according to the second or third invention is formed of a sulfide-based solid electrolyte. Layer.
- the electrostatic film forming apparatus in the manufacturing equipment for an all solid state secondary battery according to the first or second invention is filled with a powder material. It has a powder filling member and a DC power supply that drops the powder material filled in the powder filling member by electrostatic force to form a powder film.
- the all-solid-state secondary battery manufacturing facility according to the sixth invention is the all-solid-state secondary battery manufacturing facility according to the first or second aspect, wherein the powder film formed by the electrostatic film-forming apparatus is used.
- a pressurizing device for pressurizing The apparatus further comprises a cutting and removing device for cutting and removing an outer peripheral end of the powder film pressed by the pressing device.
- the manufacturing equipment for an all-solid secondary battery according to the seventh invention is the manufacturing equipment for an all-solid secondary battery according to the sixth invention, wherein the object to be pressurized by the pressing device is an electrostatic film forming apparatus. And a current collector on which the powder film is placed, The current collector has at least a roughened surface on which the powder film is placed, It further comprises a pressure charging / discharging device for charging / discharging while pressing the electrode body constituted by sandwiching the powder laminate between the two current collectors.
- the manufacturing equipment for the all-solid-state secondary battery according to the eighth invention is the manufacturing equipment for an all-solid-state secondary battery according to the sixth invention, wherein the cutting and removing device removes the outer peripheral end of the laminated powder film.
- the cutting and removing apparatus forms the powder laminate so that the area of the interface between the negative electrode layer or the positive electrode layer and the solid electrolyte layer is larger than the area of the interface between the positive electrode layer or the negative electrode layer and the solid electrolyte layer.
- the cutting is performed so that the side surface that is the cut surface is inclined.
- the cutting and removing device is provided at a position where the powder film is cut.
- the cutting is performed in a state where the rigidity inside from the position is higher than the rigidity outside from the position.
- the all-solid-state secondary battery manufacturing facility is the all-solid-state secondary battery manufacturing facility according to the sixth or eighth aspect, wherein the cutting and removing device includes a die for holding a powder film.
- the die has a flank on an inner peripheral wall where the punch is inserted,
- the die holds the powder film such that deformation of the powder film punched by the punch is allowed.
- the formed powder laminate does not contain impurities such as a solvent in a wet method, nor does a void remain after the removal of the impurities.
- the battery performance of the all-solid secondary battery manufactured from the powder laminate can be improved.
- FIG. 2 is a cross-sectional view of the all-solid-state secondary battery according to Embodiments 1 and 2 of the present invention.
- FIG. 2 is a block diagram for explaining facilities for manufacturing the all-solid-state secondary battery according to Embodiment 1 of the present invention.
- FIG. 9 is a block diagram for explaining a manufacturing facility for an all solid state secondary battery according to Embodiment 2 of the present invention. It is the schematic for demonstrating the specific example 1 of the electrostatic film-forming apparatus in the manufacturing equipment. It is a schematic diagram for explaining especially a screen version as example 2 of the same electrostatic film forming device. It is a schematic diagram for explaining example 1 of the cutting removal device in the manufacturing equipment. It is the schematic for demonstrating the specific example 2 of the cutting removal apparatus in the manufacturing equipment.
- the all-solid-state secondary battery 1 has a powder laminate 3 formed by laminating powder films. More specifically, the powder laminate 3 includes a positive electrode layer 5 and a negative electrode layer 7, and a solid electrolyte layer 6 disposed between the positive electrode layer 5 and the negative electrode layer 7. Each of the positive electrode layer 5, the negative electrode layer 7, and the solid electrolyte layer 6 may be formed of one powder film, or may be formed by stacking a plurality of powder films. Further, the all-solid secondary battery 1 has a positive electrode current collector 2 and a negative electrode current collector 4 arranged so as to sandwich the powder laminate 3 from the thickness direction thereof.
- the positive electrode current collector 2 and the negative electrode current collector 4 and the powder laminate 3 sandwiched between the positive electrode current collector 2 and the negative electrode current collector 4 are referred to as electrode bodies 2 to 4.
- the electrode bodies 2 to 4 may include an insulating member disposed between the positive electrode current collector 2 and the negative electrode current collector 4 and outside the powder laminate 3.
- the all-solid-state secondary battery 1 has an exterior 8 such as a laminate pack 8 or a can, which encloses the electrode bodies 2 to 4 as necessary. When the electrode bodies 2 to 4 are sealed in the exterior, the positive electrode current collector 2 and the negative electrode current collector 4 are electrically connected to the outside of the exterior 8.
- Examples of the positive electrode current collector 2 and the negative electrode current collector 4 include copper (Cu), magnesium (Mg), stainless steel, titanium (Ti), iron (Fe), cobalt (Co), nickel (Ni), and zinc (Zn). ), Aluminum (Al), germanium (Ge), indium (In), lithium (Li), tin (Sn), thin plates and foils made of alloys of these, or films formed of various materials. Used. Here, the thin plate and the foil have a thickness in the range of 5 ⁇ m to 100 ⁇ m. Furthermore, the positive electrode current collector 2 and the negative electrode current collector 4 may be those whose surfaces have been subjected to a roughening treatment from the viewpoint of improving the adhesion to the powder laminate 3 composed of powder. preferable. The roughening process is a process for increasing the surface roughness by etching or the like. Also, an insulating sheet made of a polymer material such as a PET film is used as the insulating member.
- the positive electrode layer 5 and the negative electrode layer 7 were prepared by mixing a positive electrode active material and a negative electrode active material for securing an electron conduction path between particles and a solid electrolyte having ionic conductivity at a predetermined ratio in order to transfer electrons. It is a layer made of a mixed material. By mixing the solid electrolyte having lithium ion conductivity with the positive electrode active material and the negative electrode active material in this manner, ion conductivity is imparted in addition to electron conductivity, and an ion conduction path can be secured between particles. .
- the positive electrode active material suitable for the positive electrode layer 5 is not particularly limited as long as it is capable of inserting and removing lithium ions.
- lithium-nickel composite oxide LiNi x M 1-x O 2
- lithium cobaltate LiCoO 2
- lithium nickelate LiNiO 2
- lithium-nickel-cobalt-aluminum composite oxide LiNi 0.8 Co 0.15 Al 0.05 O 2 , NCA-based layered oxide
- lithium manganate eg, spinel-type lithium manganate LiMn 2 O 4
- composite oxide containing excess Li Li 2 MnO 3 -LiMO 2
- compounds other than oxides etc.
- Examples of the compound other than the oxide include an olivine-based compound (LiMPO 4 ), a sulfur-containing compound (Li 2 S, and the like).
- M represents a transition metal.
- the positive electrode active material one kind can be used alone, or two or more kinds can be used in combination. From the viewpoint of easily obtaining a high capacity, a lithium-containing oxide containing at least one selected from the group consisting of Co, Ni and Mn is preferable.
- the lithium-containing oxide may further include a typical metal element such as Al.
- the positive electrode active material may be coated with a coating material on the surface of the active material from the viewpoint of improving rate characteristics.
- a coating material specifically, Li 4 Ti 5 O 12 , LiTaO 3 , Li 4 NbO 3 , LiAlO 2 , Li 2 ZrO 3 , Li 2 WO 4 , Li 2 TiO 3 , Li 2 B 4 O 7 , Li 3 PO 4 , Li 2 MoO 4 , LiBO 2 , alumina (Al 2 O 3 ), carbon (C), and the like can be given.
- the negative electrode active material suitable for the negative electrode layer 7 a mixed material of the negative electrode active material and the lithium ion conductive solid electrolyte or the negative electrode active material is used alone.
- the negative electrode active material is not particularly limited as long as lithium ions can be inserted and desorbed, and a known negative electrode active material used in an all-solid-state battery can be used.
- the negative electrode active material include a carbonaceous material capable of inserting and removing lithium ions, and a simple substance, alloy, or compound of a metal or metalloid capable of inserting and removing lithium ions.
- the carbonaceous material include graphite (natural graphite, artificial graphite, etc.), hard carbon, amorphous carbon, and the like.
- Examples of the simple substance or alloy of metal or semimetal include lithium metal, alloy, and simple substance of Si.
- Examples of the compound include an oxide, a sulfide, a nitride, a hydrate, and a silicide (such as lithium silicide).
- Examples of the oxide include titanium oxide and silicon oxide.
- As the negative electrode active material one kind may be used alone, or two or more kinds may be used in combination. For example, a silicon oxide and a carbonaceous material may be used in combination.
- Solid electrolytes are roughly classified into organic polymer electrolytes (also referred to as organic solid electrolytes), inorganic inorganic solid electrolytes, and the like, and any of them may be used as the solid electrolyte. Further, inorganic solid electrolytes are roughly classified into oxide-based materials and sulfide-based materials, and any of them may be used. Further, the inorganic solid electrolyte can be appropriately selected from crystalline or amorphous ones. That is, the solid electrolyte can be appropriately selected from materials composed of an organic compound, an inorganic compound, or a mixture thereof.
- the solid electrolyte for example, a lithium ion conductive solid electrolyte or a sulfide-based inorganic solid electrolyte that is known to have a higher ion conductivity than other inorganic compounds. is there.
- lithium-containing metal oxides such as Li 2 —SiO 2 , Li 2 —SiO 2 —P 2 O 5 , and Li x PyO 1 Lithium-containing metal nitrides such as -z N 2 , Li 2 SP 2 S 5 system, Li 2 S-SiS 2 system, Li 2 SB 2 S 3 system, Li 2 S-GeS 2 system, Li 2 S-SiS 2 -LiI system, Li 2 S-SiS 2 -Li 3 PO 4 based, Li 2 S-Ge 2 S 2 system, Li 2 S-GeS 2 -P 2 S 5 based, Li 2 S-GeS 2 lithium-containing sulfide-based glass such -ZnS-based, and PEO (polyethylene oxide), PVDF (polyvinylidene fluoride), lithium phosphate (Li 3 PO 4), lithium-containing transition metal oxide such as lithium titanium oxide Thing,
- a sulfide (a sulfide-based inorganic solid electrolyte) is preferable.
- the sulfide include one or two or more sulfides containing Li 2 S and at least one element selected from the group consisting of an element belonging to Group 13 of the periodic table, an element belonging to Group 14 and an element belonging to Group 15 of the periodic table. Is preferable.
- the elements belonging to Groups 13 to 15 of the periodic table are not particularly limited, but include, for example, P, Si, Ge, As, Sb, and Al. P, Si, and Ge are preferable, and P is particularly preferable. Is preferred.
- the solid electrolyte suitable for the solid electrolyte layer 6 may be the same as or different from the solid electrolyte used for the positive electrode layer 5 and the negative electrode layer 7.
- the positive electrode active material, the negative electrode active material, and the solid electrolyte are not limited to the above-mentioned materials, and those generally used in the field of batteries can be used.
- the manufacturing equipment 100 includes a mixing device 10 for mixing a plurality of types (two types in FIG. 2 as an example) of powder materials A and S, and a powder material mixed by the mixing device 10.
- the apparatus includes a transfer device 20 for transferring the AS, and an electrostatic film forming device 30 for forming the powder film from the powder material AS transferred by the transfer device 20.
- the electrostatic film forming apparatus 30 also forms the powder laminate 3 by laminating the formed powder films, that is, by forming additional powder films on the formed powder films.
- the manufacturing facility 100 is a dry process up to at least the step of forming the powder laminate 3 from the plurality of types of powder materials A and S.
- the powder materials A and S mixed by the mixing device 10 are, for example, a first powder material A which is a powder material such as a positive electrode active material or a negative electrode active material, and a solid electrolyte.
- the second powder material S is a powder material such as Since it is preferable that the plurality of types of powder materials A and S have a small variation in the particle size, those having a predetermined particle size range may be extracted and used by a classification operation after treatment with a ball mill or the like.
- the mixing device 10 mixes the plurality of types of powder materials A and S until they become uniform by, for example, a process using a ball mill.
- the degree of uniform mixing is determined by the degree of mixing.
- the degree of mixing is determined by, for example, measuring the color density of the mixed powder material AS at a plurality of locations, and determining the variance or standard deviation of the measured color density at the plurality of locations. Since the plurality of types of powder materials A and S have different color densities for each type, a specific powder in the mixed powder material AS is measured by measuring the color density of the mixed powder material AS. It is possible to know the ratio of the materials A and S.
- the mixing device 10 mixes a plurality of types of powder materials A and S until the degree of mixing becomes equal to or less than a predetermined value. Since it is preferable that the mixed powder material AS also has a small variation in particle size, a powder having a predetermined particle size range may be extracted and used by a classification operation.
- the transporting device 20 transports the mixed powder material AS without giving any vibration to the powder material AS.
- a mixture of a plurality of types of powder materials A and S having different particle sizes or densities may be separated into powder materials A and S for each type when vibration is applied.
- the conveying device 20 can stably convey the powder material AS (in a state of being uniformly mixed) by not giving vibration to the mixed powder material AS. is there.
- the transfer device 20 is provided with a powder material necessary for one powder film formed by the electrostatic film forming device 30. It has a container for subdivision, which is transported for each AS.
- the electrostatic film forming apparatus 30 uses at least an electrostatic force to form the powder film.
- the electrostatic film forming apparatus 30 may use another force (such as gravity, vibration force, and / or pressing force) in addition to electrostatic force to form the powder film.
- the electrostatic film forming apparatus 30 can form a powder film having a flat and uniform thickness by using at least an electrostatic force.
- such an electrostatic film forming apparatus 30 is, for example, dropped by an electrostatic force to a powder filling member filled with the powder material AS and a powder filling member filled with the powder material AS. And a DC power supply for converting the powder film.
- the electrostatic film forming apparatus 30 includes a cleaning tool for cleaning a tool used for forming the powder film every time a predetermined number of powder films are formed.
- the electrostatic film forming apparatus 30 shown in FIG. 2 also forms the powder laminate 3 by laminating the formed powder film, that is, by forming a further powder film on the formed powder film.
- the manufacturing facility 100 also includes a separate device for stacking a plurality of powder films formed by the electrostatic film forming device 30 to form the powder laminate 3.
- the manufacturing facility 100 for the all-solid-state secondary battery 1 may have a configuration other than those described above. Regardless of the configuration, at least the powder material A, S All processes up to the process of forming the laminate 3 are dry. In other words, from the place where the plurality of types of powder materials A and S are stored, at least the powder laminate 3 included in the manufacturing facility 100 including the mixing device 10, the transport device 20 and the electrostatic film forming device 30 is provided. All the components up to the process of forming are dry type.
- the dry method is a method that does not use a liquid. Since the manufacturing facility 100 is of a dry type, unlike the case of a wet type, it does not use a liquid such as a solvent, so that there is no problem caused by using a solvent.
- the manufacturing facility 100 does not require a device for drying the powder laminate 3.
- a plurality of types of powder materials A and S are mixed by the mixing device 10. That is, the mixing apparatus 10 provides a mixing step of mixing a plurality of types of powder materials A and S.
- the powder material AS mixed by the mixing device 10 is transferred from the mixing device 10 to the electrostatic film forming device 30 by the transfer device 20. That is, the transport device 20 provides a transport process of transporting the mixed powder material AS from the mixing device 10 to the electrostatic film forming device 30.
- the electrostatic film forming apparatus 30 forms a powder film from the mixed powder material AS using at least electrostatic force. That is, the electrostatic film forming apparatus 30 provides an electrostatic film forming step of forming a powder film from the mixed powder material AS using at least electrostatic force.
- the formed powder film is laminated by the electrostatic film forming apparatus 30 or a separate apparatus to form the powder laminate 3. That is, the electrostatic film forming apparatus 30 or a separate apparatus provides a powder laminate forming step of forming the powder laminate 3 by laminating the powder films.
- the above-described mixing step, transport step, electrostatic film forming step and powder laminate forming step are all dry. Therefore, no impurities remain in the powder laminate 3 formed by these steps, and no void remains after the removal of the impurities.
- the powder laminate 3 is sandwiched between the positive electrode current collector 2 and the negative electrode current collector 4 shown in FIG.
- the electrode bodies 2 to 4 are stacked as a single layer or a large number of them, and are sealed in an outer case 8 such as a laminate pack 8 or a can, as required, to form the all-solid secondary battery 1.
- the manufacturing facility 100 of the all-solid-state secondary battery 1 impurities such as a solvent in a wet method do not remain in the formed powder laminate 3, and traces of the impurities are removed. Since no voids remain, the battery performance of the all-solid secondary battery 1 manufactured from the powder laminate 3 can be improved. Furthermore, according to the manufacturing equipment 100 for the all-solid secondary battery 1, since a device for drying the powder laminate 3 is not required, the configuration can be simplified as a whole, and the all-solid secondary battery 1 can be simplified. The cost required for the manufacture of the device can be reduced.
- the first powder material A is a powder material of a positive electrode active material or a negative electrode active material
- the body material S is a sulfide-based solid electrolyte powder material.
- the transport device 20 that transports the powder material AS mixed by the mixing device 10 includes a positive transport device 25 that transports the powder material AS for forming the positive electrode layer 5, and a powder for forming the negative electrode layer 7.
- the manufacturing equipment 100 includes an electrolyte transporter 60 that transports the powder material S of the sulfide-based solid electrolyte, which is the second powder material S, for transporting the powder material in addition to the transport device 20. I do.
- the positive electrode transporter 25, the electrolyte transporter 60, and the negative electrode transporter 27 may all have the same configuration or different configurations.
- the electrostatic film forming apparatus 30 forms a positive electrode electrostatic film forming machine 35 for forming the positive electrode layer 5, an electrolyte electrostatic film forming machine 36 for forming the solid electrolyte layer 6, and forms a negative electrode layer 7. And an electrostatic film forming machine 37 for negative electrode.
- an electrostatic film forming machine for positive electrode 35, an electrostatic film forming machine for electrolyte 36, and an electrostatic film forming machine for negative electrode 37 are arranged in this order. That is, the electrostatic film forming apparatus 30 forms the positive electrode layer 5 with the positive electrode electrostatic film forming machine 35 and forms the solid electrolyte layer 6 on the positive electrode layer 5 with the electrolyte electrostatic film forming machine 36.
- the negative electrode layer 7 is formed on the solid electrolyte layer 6 by the negative electrode electrostatic film forming machine 37 (that is, the powder laminate 3 is formed).
- the positive electrode electrostatic film forming machine 35, the electrolyte electrostatic film forming machine 36, and the negative electrode electrostatic film forming machine 37 may all have the same configuration or different configurations.
- the solid electrolyte layer 6 formed by the electrolyte film forming machine 36 is a layer composed of a sulfide-based solid electrolyte because the material to be used is a sulfide-based solid electrolyte powder material S.
- the manufacturing facility 100 for the all-solid-state secondary battery 1 according to Embodiment 2 includes the current collector supply device 40 that supplies the positive electrode current collector 2 and the negative electrode current collector 4.
- the current collector supply device 40 supplies the positive electrode current collector 2 to the positive electrode electrostatic film forming machine 35 to form the positive electrode layer 5 on the positive electrode current collector 2.
- the current collector supply device 40 supplies the negative electrode current collector 4 to a pressure device 50 described below, so that the object to be pressed by the pressure device 50 is not the powder laminate 3 but the electrode body 2. Up to 4. Before forming all of the positive electrode layer 5, the solid electrolyte layer 6, and the negative electrode layer 3, these powder films may be pressed with a small pressure at an arbitrary timing to level the powder films.
- the positive electrode current collector 2 and / or the negative electrode current collector 4 supplied by the current collector supply device 40 have a roughened surface in contact with the positive electrode layer 5 and / or the negative electrode layer 7.
- the surface of the positive electrode current collector 2 and / or the negative electrode current collector 4 is roughened, so that the positive electrode layer 5 and / or the negative electrode layer 7 in contact with the surface are also roughened. In other words, the roughness on the surface of the positive electrode current collector 2 and / or the negative electrode current collector 4 is transferred to the positive electrode layer 5 and / or the negative electrode layer 7.
- the manufacturing equipment 100 for the all-solid-state secondary battery 1 according to Embodiment 2 further includes a pressurizing device 50 for pressing the electrode bodies 2 to 4 and a pressurizing device 50 for the electrode bodies 2 to 4 pressurized by the pressurizing device 50.
- the apparatus includes a cutting and removing device 70 for cutting and removing the outer peripheral end, and a laminating device 80 for enclosing the electrode bodies 2 to 4 whose outer peripheral end has been cut and removed in the laminate pack 8. In some cases, a laminating apparatus or a laminating apparatus is required.
- the pressure device 50 presses the electrode bodies 2 to 4 in the thickness direction.
- main pressurization the powders of the powder laminate 3 of the electrode bodies 2 to 4 become denser with each other, which leads to an improvement in battery performance.
- the pressing device 50 has a pressing body for pressing the electrode bodies 2 to 4.
- the pressurizing device 50 may perform pressurization at a lower pressure than the main pressurization in a low vacuum environment before the main pressurization is performed. If the pressurization of the electrode bodies 2 to 4 is only the main pressurization, the gas contained in the powder laminate 3 of the electrode bodies 2 to 4 is rapidly pushed out by the main pressurization, so that the powder laminate 3 is easily destroyed.
- the control device 50 for the temporary pressurization and the main pressurization may be performed manually, or may be performed by a separate control device (not shown).
- the control device includes a vacuum temporary pressurizing unit that causes the pressurizing device 50 to perform a temporary vacuum pressurization, and a main pressurizing unit that causes the pressurizing device 50 to perform a full pressurization. Is provided.
- the cutting and removing device 70 cuts and removes the outer peripheral end portion of the electrode bodies 2 to 4 which is a portion where the battery performance is likely to deteriorate, and only the central portion which is the other portion is the solid-state secondary battery 1. It is intended to be used for Since the powder laminate 3 of the electrode bodies 2 to 4 is formed by pressing the powder material, collapse and / or short-circuit is likely to occur at the outer peripheral end. Even if collapse and / or short-circuit occurs at the outer peripheral end of the powder laminate 3, the outer peripheral end is cut and removed by the cutting and removing device 70, so that the battery performance due to the collapse and / or short-circuit is generated. Is prevented from decreasing.
- the cutting and removing apparatus 70 employs, for example, a method of punching out the center of the electrode bodies 2 to 4 or a method of cutting off the outer peripheral end of the electrode bodies 2 to 4 (such as a chocolate break method).
- the cutting and removing apparatus 70 employing a method of punching out the center of the electrode bodies 2 to 4 includes a die for holding the outer peripheral end of the electrode bodies 2 to 4 and an electrode body for which the outer peripheral end is held by the die. And a punch for punching 2 to 4 central portions.
- the cutting and removing apparatus 70 adopting a method of cutting off the outer peripheral end portions of the electrode bodies 2 to 4 (specifically, the chocolate break method) provides a split groove along the inner edge of the portion of the electrode bodies 2 to 4 to be cut off.
- a holding plate for holding the center of the electrode bodies 2 to 4 on which the divided grooves are formed, and an outer peripheral end of the electrode bodies 2 to 4 held by the holding plate are bent by the bending moment.
- a dividing tool for dividing along the dividing groove.
- the laminating device 80 is for laminating the electrode bodies 2 to 4 whose outer peripheral ends have been cut and removed and leaving them in a single layer or by laminating them in a large number, and enclosing them in the laminate pack 8. When a large number of layers are stacked, a current collector for electrically connecting the layers is provided as necessary.
- the laminating apparatus 80 may include a vacuum pump for enclosing the electrode bodies 2 to 4 in the laminate pack 8 under a high vacuum atmosphere.
- the electrode bodies 2 to 4 When the electrode bodies 2 to 4 are sealed in the laminate pack 8 in a high vacuum atmosphere, the electrode bodies 2 to 4 of the manufactured all solid secondary battery 1 are Since the atmospheric pressure is constantly received from the outside due to the pressure difference from the outside, the powders in the powder laminate 3 of the electrode bodies 2 to 4 are kept dense.
- the pressure device 50, the cutting and removing device 70, and the laminating device 80 are all of a dry type, and are arranged, for example, in a dry room.
- the powder material of the positive electrode active material (first powder material A) and the powder material of the sulfide solid electrolyte (second powder material S) are mixed by the mixing device 10.
- the mixed powder material AS is transported to the positive electrode electrostatic film forming device 35 by the positive electrode transport device 25.
- the sulfide-based solid electrolyte powder material (second powder material S) is transported by the electrolyte transport device 60 to the electrolyte electrostatic film forming device 36.
- the mixing device 10 mixes the powder material of the negative electrode active material (first powder material A) and the powder material of the sulfide-based solid electrolyte (second powder material S).
- the mixed powder material AS is transported to the negative electrode electrostatic film forming device 37 by the negative electrode transport device 27.
- the positive electrode layer 5 is formed on the positive electrode current collector 2 supplied from the current collector supply device 40 by the positive electrode electrostatic film forming machine 35.
- the solid electrolyte layer 6 is formed on the positive electrode layer 5 by the electrolyte electrostatic film forming machine 36.
- the negative electrode layer 7 is formed on the solid electrolyte layer 6 by the negative electrode electrostatic film forming machine 37, whereby the powder laminate 3 is formed.
- the negative electrode current collector 4 supplied from the current collector supply device 40 is placed on the negative electrode layer 7 of the powder laminate 3 by the pressurizing device 50, whereby the electrode bodies 2 to 4 are formed. Then, the pressurizing device 50 performs the main pressurization on the electrode bodies 2 to 4 or the temporary vacuum pressurization before the main pressurization. That is, the pressurizing device 50 provides a main pressurizing step of performing a main pressurization on the electrode bodies 2 to 4, or a vacuum temporary pressurizing step and a main pressurizing step.
- the cutting and removing apparatus 70 provides a cutting and removing step of cutting and removing the outer peripheral end portions of the electrode bodies 2 to 4.
- the lamination device 80 cuts and removes the outer peripheral end portions of the electrode bodies 2 to 4 as they are, or a large number of them are laminated, and sealed in the laminate pack 8 under a high vacuum atmosphere. When a large number of layers are stacked, a current collector for electrically connecting the layers is provided as necessary. That is, the laminating apparatus 80 provides a laminating step of enclosing the electrode bodies 2 to 4 in the laminating pack 8 under a high vacuum atmosphere.
- the powder stack By making the powders 3 dense, the battery performance can be further improved.
- the powder laminate 3 is less likely to collapse, so that the battery performance can be further improved.
- the cutting and removing device 70 cuts and removes the outer peripheral end portion of the electrode bodies 2 to 4 which is likely to deteriorate the battery performance, and removes the central part of the electrode bodies 2 to 4 where the battery performance is high to the all-solid secondary battery. Since it is used, the battery performance can be further improved.
- the electrode bodies 2 to 4 since the electrode bodies 2 to 4 always receive the atmospheric pressure from the outside by the laminating device 80, the powder in the powder laminate 3 of the electrode bodies 2 to 4 is maintained densely, so that the battery performance is improved. Can be further improved.
- the positive electrode layer 5 is formed first, and the negative electrode layer 7 is formed later.
- the negative electrode layer 7 is formed first, and the positive electrode layer 5 is formed later. Is also good. That is, in FIGS. 1 and 3, the positive electrode layer 5, the positive electrode transporter 25, and the positive electrode electrostatic film forming machine 35 are replaced with the negative electrode layer 7, the negative electrode transporter 27, and the negative electrode electrostatic film forming machine 37. May be adopted.
- the configuration of the all-solid secondary battery 1 has been described with reference to FIG. 1.
- the configuration is not limited to the configuration illustrated in FIG. 1.
- the production facility 100 performs charge and discharge while applying pressure to the electrode bodies 2 to 4 (hereinafter, referred to as pressurized charge and discharge).
- An apparatus may be provided.
- the powder laminate 3 of the electrode bodies 2 to 4 is pressed against the positive electrode current collector 2 and the negative electrode current collector 4. Since the powder laminate 3 expands and contracts as it is, the powder laminate 3 sufficiently bites into the roughened surfaces of the positive electrode current collector 2 and the negative electrode current collector 4, and as a result, the battery performance under no pressure is improved. It can be further improved.
- the specific configurations of the electrostatic film forming apparatus 30 and the powder laminate forming step have not been described. However, for example, the following configurations may be used.
- the electrostatic film forming apparatus 30 includes a screen plate 31 which is electrically neutral without contacting a target O on which a powder film is formed, and a negatively (or positively) charged powder material. It has a rubbing body 32 for rubbing the AS against the screen plate 31 and dropping it on the object O, a pedestal 33 on which the object O is placed, and a DC power supply 34 for positively charging the pedestal 33.
- the screen plate 31 has a mesh portion 38 into which the powder material AS is rubbed by the rubbing body 32.
- the material of the mesh portion 38 polyester, nylon, stainless steel, polyethylene, or the like may be adopted, or another material may be adopted according to the powder material AS used.
- the screen plate 31 is configured such that the powder material AS is not positively charged due to friction caused by the rubbing of the rubbing body 32. It is preferable to use a material (e.g., nylon or rayon) or a metal in which the charging line is on the positive side.
- the screen plate 31 prevents the powder material AS from being negatively charged due to friction caused by the rubbing of the rubbing body 32. It is preferable to employ a material (eg, polyethylene or polyester) having a negative charging line or a metal.
- a material eg, polyethylene or polyester having a negative charging line or a metal.
- the rubbing body 32 is a squeegee or a sponge. Instead of the rubbing body 32, an air nozzle that drops the powder material AS from the screen plate 31 to the target O by blowing gas may be used.
- the powder material AS is brought into contact with a negative electrode plate (or positive electrode plate) to which a voltage is applied, though not shown.
- the individual powder constituting the powder material AS is charged by vibrating the negative electrode plate (or the positive electrode plate).
- the powder material AS may be charged by friction or corona discharge.
- the powder material AS placed on the screen plate 31 is negatively (or positively) charged before being placed on the screen plate 31. In comparison, it is more reliably negatively (or positively) charged.
- the pedestal 33 is connected to the positive electrode of the DC power supply 34 so as to be positively charged.
- the base 33 is connected to the negative electrode of the DC power supply 34 so as to be negatively charged.
- the powder material AS placed on the screen plate 31 is positively (or positively) charged positively. ) Uniformly falls from the screen plate 31 onto the charged object O, so that a powder film having a uniform thickness can be formed.
- Experimental Examples 1 to 3 and a comparative example for verifying that a powder film having a uniform thickness is formed by the electrostatic film forming apparatus 30 are as follows.
- Example 1 the electrostatic film forming apparatus 30 shown in FIG. 4 was used.
- a mesh portion 38 (opening) having a square shape, a mesh number of 300 / inch, a wire diameter of 30 ⁇ m, and an opening of 55 ⁇ m was used.
- 17 types of heavy calcium carbonate were used for experiments.
- the powder material was brought into contact with the positive electrode plate to which a voltage of about -200 to -100 V was applied while vibrating.
- Experimental Example 2 the polarity of charging in Experimental Example 1 was reversed. That is, the powder material was positively charged, and the pedestal 33 was negatively charged. Except for this, Experimental Example 2 is the same as Experimental Example 1.
- Experimental Example 3 an air nozzle was used instead of the rubbing body 32 of Experimental Example 1. Except for this, Experimental Example 3 is the same as Experimental Example 1.
- the powder material is not charged before being placed on the screen plate 31 as shown in FIG. 4, and the powder material is rubbed with the rubbing body 32 into the negatively charged screen plate 31.
- a powder film was formed on the object O.
- Table 1 shows the data on the thickness of the powder film thus formed. Table 1 shows the results in each of Experimental Examples 1 to 3 and Comparative Example, aiming at the thickness of the formed powder film to be 100 ⁇ m.
- the electrostatic film forming apparatus 30 has a screen plate 31 shown in FIG. 5 and other known structures required for electrostatic film forming. Of course, other than this known configuration, the configuration shown in FIG. 4 may be used.
- the screen plate 31 shown in FIG. 5 has a mesh portion 38 (opening) having different openings and / or opening ratios depending on locations.
- the mesh portion 38 is not limited to a square, but may be another polygon or a circle.
- the screen plate 31 is not limited to being arranged in parallel with the object O on which the powder film is formed, but may be arranged at an inclination (10 to 40 °). In the example shown in FIG.
- the mesh portion 38 has a large aperture and an opening ratio at an outer peripheral portion (hereinafter, a first mesh portion 38A), and a portion surrounded by the first mesh portion 38A (hereinafter, a first mesh portion 38A).
- the openings and the aperture ratio are small in the two mesh portions 38B).
- the screen plate 31 has an opening of 104 ⁇ m, an aperture ratio of 61.1%, a mesh number of 190 / inch, a wire diameter of 29 ⁇ m in the first mesh portion 38A, and an opening in the second mesh portion 38B. 55 ⁇ m, aperture ratio: 42.9%, number of meshes: 302 / inch, wire diameter: 29 ⁇ m.
- the screen plate 31 was arranged in parallel with the object O at a distance of 10 mm, and the applied voltage was 5 kV.
- a powder film was formed by dropping the powder material from the screen plate 31 onto the target O with the rubbing body 32 with the voltage applied.
- the thickness of the powder film was 600 to 700 ⁇ m at the portion corresponding to the first mesh portion 38A, and was 300 to 400 ⁇ m at the portion corresponding to the second mesh portion 38B.
- the use of the screen plate 31 having the mesh portions 38 having different apertures and / or opening ratios depending on locations allows a desired thickness to be obtained at an arbitrary location in the powder film.
- the boundary between the positive electrode layer 5 and the solid electrolyte layer 6 and / or the boundary between the negative electrode layer 7 and the solid electrolyte layer 6 are shown in FIG. Instead of being flat as shown, it may have undulations as shown in FIGS. 10 to 12, for example. However, it is preferable that the entire powder laminate 3 be laminated so as to be flat. In addition, the thickness of the solid electrolyte layer 6 is increased at the end of the powder laminate 3. Thereby, even when the end of the stacked body 3 collapses, a short circuit at the end is less likely to occur.
- the outer surfaces of the positive electrode layer 5 and the negative electrode layer 7 are shown in FIGS. It is flat as shown in (omitted).
- the thickness of the positive electrode layer 5 and the thickness of the negative electrode layer 7 are small and the thickness of the solid electrolyte layer 6 is large at the end portion as shown in FIGS.
- the thickness of the solid electrolyte layer 6 be significantly larger than the thickness of the positive electrode layer 5 and the negative electrode layer 7 at each corner. . This makes it difficult for a short circuit to occur at the end between the positive electrode layer 5 and the negative electrode layer 7. Is prevented.
- the thickness of the negative electrode layer 7 is larger than the thickness of the positive electrode layer 5 in any part of the powder laminate 3 as shown in FIGS.
- the thickness of the negative electrode layer 7 be in the range of 1.05 to 2.00 with respect to the thickness of the positive electrode layer 5. This prevents a short circuit due to the inhibition of the deposition of Li in the negative electrode layer 7 and the growth toward the positive electrode layer 5, and improves the cycle characteristics of the all-solid secondary battery 1.
- the powder laminate forming step may be any method as long as it forms the powder laminate 3 having the undulations.
- the mesh portion 38 opening
- the powder lamination having the undulation is provided.
- a method of forming the body 3 may be used.
- each layer may be pressurized.
- a material having elasticity is preferably used for the pressing body of the pressurizing device 50 for pressurizing so as to pressurize the respective layers as a whole while leaving the undulation of each layer to some extent.
- the thickness of the solid electrolyte layer 6 becomes larger and the thickness of the positive electrode layer 5 and the thickness of the negative electrode layer 7 become smaller as approaching the end portion. Only the layer 6 may be used. It is preferable that the entire powder laminate 3 be laminated so as to be flat.
- the cutting and removing apparatus 70 is an apparatus for using the above-described method of punching out the central part of the electrode bodies 2 to 4 (at least the powder laminate 3). This is a device for inclining the side surface 3s in the central part of 2 to 4. More specifically, the cutting and removing apparatus 70 includes a die 71s for forming an inclined side surface that holds the outer peripheral ends of the electrode bodies 2 to 4, and an electrode body that has the outer peripheral end held by the inclined side forming die 71s. And a punch 75s for forming an inclined side surface, which punches out 2 to 4 central portions.
- the inclined side forming die 71s has a pedestal surface 72 on which the electrode bodies 2 to 4 are placed, and a space 73 through which the inclined side forming punch 75s passes. Further, the inclined side surface forming die 71s does not need to press down the electrode bodies 2 to 4 placed on the pedestal surface 72 from above. The reason is that the powder laminate 3 which is a main component of the electrode bodies 2 to 4 is a brittle material composed of one powder film or a plurality of laminated powder films, and when punched, it is greatly damaged. This is because it breaks before it is deformed.
- the inclined side surface forming die 71s does not use a pressing plate for holding down the electrode bodies 2 to 4, the electrode bodies 2 to 4 are deformed so that the punched electrode bodies 2 to 4 can be deformed. It can be said to hold.
- the press plate may be used for the inclined side surface forming die 71 s, the press plate to be used is pressed with such a force that deformation of the electrode bodies 2 to 4 by punching is allowed. Hold bodies 2-4.
- the inclined side surface forming punch 75s has a blade 78 extending from the tip end 76 to the inner peripheral surface 77I.
- the blade 78 cuts the electrode bodies 2 to 4 by punching.
- the blade 78 has a sharp tip 76 and is thicker as it approaches the inner peripheral surface 77I.
- the blade 78 is not limited to the inner blade 78 extending from the distal end 76 to the inner peripheral surface 77I, and may be a double blade extending from the distal end 76 to both the inner peripheral surface 77I and the outer peripheral surface 770.
- a Thomson method using a Thomson blade may be used instead of the method using the inclined side surface forming die 71s and the inclined side surface forming punch 75s.
- the electrode bodies 2 to 4 are mounted (an example of holding) on the inclined side surface forming die 71s so as to cover the space 73 thereof.
- the electrode bodies 2 to 4 are punched out by the punch 75s for forming the inclined side surface.
- the side surfaces 3s of the electrode bodies 2 to 4 are cut so as to be inclined.
- the area of the interface between the negative electrode layer 7 and the solid electrolyte layer 6 is larger than the area of the interface between the positive electrode layer 5 and the solid electrolyte layer 6.
- a battery using lithium ions such as a lithium ion secondary battery
- when there is an excess positive electrode layer not facing the negative electrode layer floating metallic lithium is deposited from an end of the negative electrode layer located near the excess positive electrode layer.
- this tends to cause a short circuit.
- a battery using lithium ions is generally configured so that the area of the negative electrode layer is larger than that of the positive electrode layer.
- portions of the negative electrode layer that do not overlap with the positive electrode layer are wasted. Even when the area of the negative electrode layer is larger than the area of the positive electrode layer, a short circuit is likely to occur if the position of the positive electrode layer is shifted and a portion of the positive electrode layer that does not face the negative electrode layer is generated. For this reason, the area of the negative electrode layer is determined in consideration of the arrangement (alignment) error of the positive electrode layer. This leads to a problem that the size of the negative electrode layer is unnecessarily large, which leads to an increase in the size of the battery.
- the side surface 3s is inclined, and the area of the interface between the negative electrode layer 7 and the solid electrolyte layer 6 is larger than the area of the interface between the positive electrode layer 5 and the solid electrolyte layer 6.
- the electrodes 2 to 4 do not cause such a problem.
- the side surfaces 3s of the electrode bodies 2 to 4 are inclined, a short circuit which may occur in the conventional all-solid secondary battery due to the collapse of the protruding portions of the positive electrode layer 5 and the negative electrode layer 7 can be prevented. .
- the inclined side surfaces 3s of the electrode bodies 2 to 4 need only be continuously inclined, they are not limited to flat surfaces, and may be curved surfaces such as convex or concave surfaces. In particular, if the inclined side surfaces 3s of the electrode bodies 2 to 4 are curved convex surfaces, the electrode bodies 2 to 4 are less likely to collapse at the ends. When the electrode bodies 2 to 4 have a large number of side faces such as a polygon in a plan view, the number of the inclined side faces 3s may be any number.
- the cutting and removing apparatus 70 has been described as performing cutting so that the area of the interface between the negative electrode layer 7 and the solid electrolyte layer 6 is larger than the area of the interface between the positive electrode layer 5 and the solid electrolyte layer 6,
- the cutting may be performed so that the area of the interface between the anode and the solid electrolyte layer 6 is larger than the area of the interface between the anode layer 7 and the solid electrolyte layer 6.
- the cutting and removing apparatus 70 includes a pressing plate 79 for pressing the electrode bodies 2 to 4 from above and below, and a dividing groove for breaking (an example of cutting) the outer peripheral ends of the electrode bodies 2 to 4. It has a dividing groove forming tool (not shown) for forming 3g, and a load applying part (not shown) for applying a load F to the ends of the electrode bodies 2 to 4 in which the dividing grooves 3g are formed.
- the pressing plate 79 holds the electrode bodies 2 to 4 with such a force that deformation of the electrode bodies 2 to 4 due to breakage is allowed.
- the dividing groove forming tool forms a dividing groove 3g as a cut, which is a starting point of fracture when a load F is applied to the ends of the electrode bodies 2 to 4. For this reason, the dividing groove 3g is formed in such a shape that the side surface 3s of the electrode body 2 to 4 formed by breaking is inclined. Further, the dividing groove 3g may be formed on the positive electrode current collector 2 side or may be formed on the negative electrode current collector 4 side.
- the division groove forming tool is not limited as long as it forms the division groove 3g. For example, a cutter blade, a rotary blade (a roller is provided with a blade), or a protrusion matching the shape of the division groove 3g. And a pressing die having a portion.
- the load applying section applies a load F such that a fracture starts from the divided groove 3g by generating a bending moment and / or a shear stress in the divided groove 3g.
- the electrode bodies 2 to 4 are pressed by the pressing plate 79 from above and below.
- a dividing groove 3g for breaking (an example of cutting) the outer peripheral ends of the electrode bodies 2 to 4 is formed by a dividing groove forming tool.
- a load is applied to the ends of the electrode bodies 2 to 4 on which the division grooves 3g are formed by the load application unit, so that the side surfaces 3s of the electrode bodies 2 to 4 are inclined from the division grooves 3g to the outer peripheral ends. The part is broken.
- the formation of the dividing groove 3g by the dividing groove forming tool includes, for example, the following two pattern procedures in addition to the procedure described above.
- the first pattern is a procedure in which a division groove 3g is formed in the positive electrode current collector 2 or the negative electrode current collector 4 before the powder laminate 3 is formed.
- the second pattern is that after forming the powder laminate 3 (or the electrode bodies 2 to 4), the powder laminate 3 (or the electrode bodies 2 to 4) is This is a procedure for forming a division groove 3g in the laminated body 3 (or the electrode bodies 2 to 4).
- this cutting and removing apparatus 70 is an apparatus for using the method of punching out the central portion of the above-mentioned electrode bodies 2 to 4 (at least the powder laminate 3). It is not a device for inclining the side surface 3s at the center of the bodies 2 to 4.
- the cutting and removing device 70 is a device that also prevents roughness of the side surface 3s formed by punching. More specifically, the cutting and removing apparatus 70 punches out a die 71 holding the outer peripheral end of the electrode bodies 2 to 4 and a central part of the electrode bodies 2 to 4 having the outer peripheral end held by the die 71. And a punch 75.
- the die 71 has a pedestal surface 72 on which the electrode bodies 2 to 4 are placed, and a space 73 through which the punch 75 passes.
- the die 71 has an inner peripheral wall 74 facing the space 73.
- a blade 74a for cutting the outer peripheral ends of the electrode bodies 2 to 4 by punching with the punch 75 is formed.
- the inner peripheral wall 74 is vertical when the height is equal to or more than the predetermined height 74h, but is inclined at an angle ⁇ 1 in a direction in which the space 73 expands downward as the height decreases below the predetermined height 74h.
- the inner peripheral wall 74 having a height less than the predetermined height 74h is a flank 74e.
- the flank 74e prevents the side surface 3s punched by the punch 75 and formed on the electrode bodies 2 to 4 from being roughened.
- the flank 74e is preferably formed below the intermediate portion of the inner peripheral wall 74 in order to extend the life of the die 71.
- the punch 75 preferably has a shear angle in order to reduce the thrust for punching.
- the shear angle also improves the accuracy of punching depending on the angle.
- the shear angle may be included in the punch 75, may be included in the die 71, or may be included in both the punch 75 and the die 71.
- the clearance 75 between the punch 75 and the inner peripheral wall 74 of the die 71 is set to about several to several tens ⁇ m.
- the punching speed V of the punch 75 is set to 100 mm / sec or less.
- the punching speed V is low, the impact on the electrode bodies 2 to 4 due to the punching of the electrode bodies 2 to 4 which is a fragile material is small, so that the collapse of the electrode bodies 2 to 4 due to the punching is prevented.
- the punching speed is more preferably 50 mm / sec or less, and even more preferably 25 mm / sec or less.
- the punch 75 and the die 71 also the inclined side surface forming punch 75 s and the inclined side surface forming die 71 s have at least portions that touch the electrode units 2 to 4 so that a short circuit does not occur by punching out the electrode units 2 to 4. Is preferably coated with an insulating material.
- the electrode bodies 2 to 4 are placed on the die 71 so as to cover the space 73.
- the electrode bodies 2 to 4 are punched out by the punch 75.
- the outer peripheral end of the electrode bodies 2 to 4 is cut by the blade 74a, and the center of the electrode bodies 2 to 4 descends the space 73.
- the flank 74e prevents the side surface 3s formed on the electrode bodies 2 to 4 from being roughened.
- cutting can be performed in a state where the rigidity inside the electrode bodies 2 to 4 from the cutting position is higher than the rigidity outside the position from the cutting position.
- all of the specific examples 1 to 3 of the cutting and removing apparatus 70 remove the electrode bodies 2 to 4 in a state where the rigidity of the central part of the electrode bodies 2 to 4 is higher than the rigidity of the outer peripheral end to be cut.
- Cutting is preferred. This is because the distortion due to the cutting is absorbed by the outer peripheral end portion having low rigidity, so that damage or failure to the central portion which is a product is prevented.
- the cutting and removing apparatus 70 is different from the cutting and removing apparatus 70 described as the third embodiment only in the inner peripheral wall 74 of the die 71.
- the specific example 3 of the cutting and removing device 70 punches out the electrode bodies 2 to 4 once by the single downward movement of the punch 75
- the specific example 4 of the cutting and removing device 70 includes By having a plurality of blades 74a having different inner diameters on the peripheral wall 74, the electrode bodies 2 to 4 are punched out a plurality of times by a single downward movement of the punch 75. More specifically, as shown in FIG.
- the die 71 in the cutting and removing device 70 has an upper blade 74a formed at the upper end of the inner peripheral wall 74 and a lower portion and an inner portion below the upper blade 74a. It has a middle blade 74b and a lower blade 74c formed below and inside the middle blade 74b.
- the inner peripheral wall 74 is slightly inclined from the upper blade 74a to the middle blade 74b in a direction in which the space 73 is widened downward, and is horizontal at the height of the middle blade 74b.
- the inner peripheral wall 74 is slightly inclined from the middle blade 74b to the lower blade 74c in a direction in which the space 73 is widened downward, and is horizontal at the height of the lower blade 74c.
- the upper blade 74a, the middle blade 74b, and the lower blade 74c have similar shapes as necessary. While the lower blade 74c determines the outer shape of the product, it is shaped according to the desired outer shape of the product, whereas the upper blade 74a and the middle blade 74b need not be shaped as such.
- the inner peripheral wall 74 is vertical from the lower blade 74c to a predetermined height 74h, but is inclined at an angle ⁇ 2 in a direction of expanding the space 73 downward as the height is less than the predetermined height 74h.
- the inner peripheral wall 74 having a height less than the predetermined height 74h is a flank 74e. The flank 74e prevents the side surface 3s punched by the punch 75 and formed on the electrode bodies 2 to 4 from being roughened.
- the electrode bodies 2 to 4 are placed on the die 71 so as to cover the space 73.
- the electrode bodies 2 to 4 are punched three times by the inclined side surface forming punch 75s. More specifically, as the punch 75 descends after passing through the upper blade 74a, the electrode bodies 2 to 4 are punched in a size two steps larger than the desired size. Then, as the punch 75 passes through the middle blade 74b and descends, the electrode bodies 2 to 4 having a size two steps larger than the desired size are punched out in a size one step larger than the desired size.
- the electrode bodies 2 to 4 having a size one step larger than the desired size are punched in the desired size.
- the electrode bodies 2 to 4 of a desired size descend in the space 73 below the lower blade 74c, but the flank 74e prevents the formed side surface 3s from being roughened.
- the cutting and removing device 70 is not limited to the above-described specific examples 1 to 4, but may be any as long as it cuts and removes the outer peripheral end portions of the electrode bodies 2 to 4 (at least the powder laminate 3).
- the cutting of the electrode bodies 2 to 4 is not limited to those described in the specific examples 1 to 4, but may be any device that cuts, such as a laser, a Thomson blade, a shearing, and a cutting machine.
- the all-solid secondary battery 1 according to the present invention only needs to have at least the powder laminated body 3.
- the hydrogen sulfide can be discharged to the outside even if moisture flows into the inside without lowering the basic performance. You may make it the structure which does not leak.
- a specific example of the all-solid secondary battery 1 having such a structure will be described with reference to FIGS.
- This all-solid-state secondary battery 1 has a hydrogen sulfide adsorbent 9 as shown in, for example, FIGS.
- a hydrogen sulfide adsorbent 9 activated carbon, zeolite, a catalyst (zinc oxide), and / or a dehydrating agent (such as diphosphorus pentoxide or silica gel) are used.
- a dehydrating agent such as diphosphorus pentoxide or silica gel
- the hydrogen sulfide adsorbent 9 one obtained by disposing the catalyst and / or the dehydrating agent on a porous body such as nonwoven fabric, glass paper, or foamed resin may be used.
- the hydrogen sulfide adsorbent 9 preferably has a thickness of 10 to several 100 ⁇ m.
- the hydrogen sulfide adsorbent 9 is thicker than several hundred ⁇ m, the external dimensions and weight of the electrode bodies 2 to 4 and the all-solid secondary battery 1 become too large, causing waste.
- the hydrogen sulfide adsorbent 9 is thinner than 10 ⁇ m, it absorbs hydrogen sulfide. The effect of hydrogen sulfide is reduced, which may cause leakage of hydrogen sulfide to the outside.
- the amount of hydrogen sulfide that can be adsorbed by the hydrogen sulfide adsorbent 9 for example, when a catalyst (zinc oxide) is used as the hydrogen sulfide adsorbent 9, the oxidization by the reaction formula (H 2 S + ZnO ⁇ ZnS + H 2 O) is performed. If zinc is 81.4 g, the amount of hydrogen sulfide adsorbed is theoretically 34.1 g (32.1 g of sulfur).
- the all-solid-state secondary battery 1 generally has the hydrogen sulfide adsorbent 9 inside the electrode bodies 2 to 4.
- the hydrogen sulfide adsorbent 9 has a shape of a square in a plan view, is mostly located on the outer periphery of the positive electrode layer 5 and inside the solid electrolyte layer 6, and is disposed on the positive electrode current collector 2.
- the area of the negative electrode layer 7 exceeds the area of the positive electrode layer 5. Is thinner than the central part due to the absence of.
- the force applied to the end of the powder laminate 3 in the pressing step is smaller than that of the center. Structure collapse easily occurs. Further, even if the area of the negative electrode layer 7 is equal to the area of the positive electrode layer 5, if the area of the solid electrolyte layer 6 exceeds the area of the negative electrode layer 7 and the area of the positive electrode layer 5, the end of the powder laminate 3 is located closer to the center. Similarly, the structure is likely to collapse at the end. However, with the arrangement of the hydrogen sulfide adsorbent 9 as shown in FIG. 13, the end of the powder laminate 3 is prevented from being thinner than the center, so that the structural collapse at the end is prevented. You.
- the hydrogen sulfide adsorbent 9 is not limited to the position shown in FIG. 13 and may be arranged between the positive electrode layer 5 and the solid electrolyte layer 6 or between the solid electrolyte layer 6 and the negative electrode layer 7. Further, in the pressing step, when the end portion of the powder laminate 3 is structurally destroyed, for example, the force applied to the end portion is too large as compared with the center portion, or the thickness of the central portion of the powder laminate 3 is increased. When the thickness is smaller than the end, the hydrogen sulfide adsorbent 9 may be arranged at the center of the powder laminate 3.
- the all-solid-state secondary battery 1 schematically has a structure in which a plurality of electrode bodies 2 to 4 are stacked, and the current collectors 2 and 4 of the adjacent electrode bodies 2 to 4 Through the hydrogen sulfide adsorbent 9 having the same polarity. If the hydrogen sulfide adsorbent 9 is not provided in the structure shown in FIG. 14, a plurality of electrodes may be displaced due to the displacement of the electrodes 2 to 4 and / or the deformation and / or bending of the electrodes 2 to 4 due to the pressing step. It may not be possible to precisely stack the bodies 2 to 4 with the same poles facing each other.
- the all-solid secondary battery 1 is not limited to the example shown in FIG. 14, and the current collectors 2 and 4 of the adjacent electrode bodies 2 to 4 may have different polarities.
- the hydrogen sulfide adsorbent 9 may be made of a material having an insulating property (a nonwoven fabric, glass paper, or a foamed resin as a main material). Further, the hydrogen sulfide adsorbent 9 is not limited to the shape of ⁇ in plan view as shown in FIG. 14, but may be a sheet-like material in its entirety. It may be arranged.
- the all-solid-state rechargeable battery 1 schematically includes a plurality of electrode bodies 2 to 4 stacked and sealed in an exterior 8, and current collection of adjacent electrode bodies 2 to 4 is performed.
- the body has the same polarity, and a hydrogen sulfide adsorbent 9 is disposed between the uppermost and lowermost current collectors 2 and 4 and the exterior 8. Since there is a surplus space between the uppermost and lowermost current collectors 2 and 4 and the outer package 8, the hydrogen sulfide adsorbent 9 is arranged using the space in FIG.
- the hydrogen sulfide adsorbent 9 may have a ⁇ shape in plan view shown in FIG. It may be arranged so as to compensate for a dent caused by unevenness in thickness of 2 to 4.
- the all-solid-state secondary battery 1 shown in FIGS. 13 to 15 is merely an example.
- a separate current collector may be provided, and the hydrogen sulfide adsorbent 9 is not essential.
- the ends of 3 may be aligned, or the electrodes connected and stacked on one exterior 8 may be sealed.
- This all-solid-state secondary battery 1 does not require charging and discharging when discharging and charging.
- it is essential to satisfy the following requirements (1) and (2), and it is preferable that the following requirements (3) and / or (4) are also satisfied.
- (1) The surface of the positive electrode layer 5 and / or the negative electrode layer 7 is roughened.
- (2) Pressure charging and discharging are performed in a state where the positive electrode layer 5 and / or the negative electrode layer 7 and the positive electrode current collector 2 and / or the negative electrode current collector 4 are in contact with each other.
- first and second embodiments are illustrative in all aspects and are not restrictive.
- the scope of the present invention is defined by the terms of the claims, rather than the description above, and is intended to include any modifications within the scope and meaning equivalent to the terms of the claims.
- configurations other than the configuration described as the first invention in “Means for Solving the Problems” are arbitrary configurations, and can be deleted and changed as appropriate. It is.
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Abstract
Description
複数種の粉体材料を混合する混合装置と、
混合装置で混合された粉体材料を搬送する搬送装置と、
搬送装置で搬送された粉体材料から、少なくとも静電力を用いて前記粉体膜を形成する静電成膜装置とを具備し、
前記複数種の粉体材料から前記粉体積層体を形成する過程が乾式であるものである。
静電成膜装置が、正極層を形成するための正極用静電成膜機と、固体電解質層を形成するための電解質用静電成膜機と、負極層を形成するための負極用静電成膜機とを有するものである。
固体電解質層を形成するための粉体材料を電解質用静電成膜機に搬送する電解質用搬送機をさらに具備するものである。
前記加圧装置で加圧された粉体膜の外周端部を切断して除去する切断除去装置とをさらに具備するものである。
前記集電体が、少なくとも前記粉体膜が載置される面を粗化したものであり、
粉体積層体を2つの前記集電体で挟んで構成される電極体に、加圧しながら充放電を行う加圧充放電装置をさらに具備するものである。
前記切断除去装置が、形成する粉体積層体を、その負極層または正極層と固体電解質層との界面の面積が正極層または負極層と固体電解質層との界面の面積よりも大きくなるように、且つ、切断された面である側面が傾斜するように、切断するものである。
前記ダイが、前記パンチの挿入される内周壁に逃げ面を有し、
前記ダイが、前記パンチにより打ち抜かれる粉体膜の変形が許容されるように当該粉体膜を保持するものである。
以下、本発明の実施の形態1に係る全固体二次電池の製造設備について、図面に基づき説明する。
以下、前記実施の形態1をより具体的に示した実施の形態2に係る全固体二次電池1の製造設備100について図面に基づき説明する。以下、前記実施の形態1で省略した構成に着目して説明するとともに、前記実施の形態1と同一の構成については、同一の符号を付してその説明を省略する。
図4に示すように、この静電成膜装置30は、粉体膜を形成する対象Oに非接触で電気的に中立のスクリーン版31と、負(または正)に帯電された粉体材料ASを当該スクリーン版31に擦り込んで前記対象Oに落とす擦込体32と、前記対象Oを載置する台座33と、この台座33を正に帯電する直流電源34とを有する。
この静電成膜装置30は、図5に示すスクリーン版31と、その他に静電成膜に必要な公知の構成とを有する。勿論、この公知の構成以外にも、図4に示す構成であってもよい。図5に示す前記スクリーン版31は、箇所によって目開きおよび/または開口率が異なるメッシュ部38(開口部)を有する。このメッシュ部38は、四角形に限られず、他の多角形または円形にしてもよい。前記スクリーン版31は、粉体膜を形成する対象Oに対して、平行に配置されることに限られず、傾斜(10~40°)して配置されてもよい。前記メッシュ部38は、図5に示す例だと、外周の箇所(以下、第1メッシュ部38A)で目開きおよび開口率が大きく、この第1メッシュ部38Aに囲われた箇所(以下、第2メッシュ部38B)で目開きおよび開口率が小さい。このようなメッシュ部38を有するスクリーン版31を使用することで、形成される粉体膜は、目開きおよび開口率が大きい第1メッシュ部38Aに相当する箇所で厚く、目開きおよび開口率が小さい第2メッシュ部38Bに相当する箇所で薄くなる。
この粉体積層体形成工程で形成される粉体積層体3は、正極層5と固体電解質層6との境界、および/または、負極層7と固体電解質層6との境界が、図1に示すような平坦ではなく、例えば図10~図12に示すようなうねりを有するものとしてよい。ただし、粉体積層体3全体としては平坦になるように積層することが好ましい。また、粉体積層体3の端部において、固体電解質層6の厚さが大きくなるようにしておく。これにより、積層体3の端部が崩れた場合でも、端部での短絡が発生しにくくなる。なお、前記粉体積層体3は、正極層5および負極層7の外面(正極集電体2および負極集電体4に接する面)が、図10~図12(負極集電体4を図示省略)に示すように、平坦である。前記うねりは、短波長の粗さ成分ではなく、長波長のうねり成分によるものであり、粗さ成分とうねり成分とを区分するカットオフ値が0.08~2.50mmであることが好ましい。さらに、前記うねりは、正極層5、固体電解質層6および負極層7のそれぞれが、
(最大厚さ-最小厚さ)/平均厚さ=0.1~2.0
を満たすことが好ましい。
図6に示すように、この切断除去装置70は、前述の電極体2~4(少なくとも粉体積層体3)の中央部を打ち抜く方法を使用するための装置であり、且つ、打ち抜きにより電極体2~4の中央部における側面3sを傾斜させる装置である。具体的に説明すると、前記切断除去装置70は、電極体2~4の外周端部を保持する傾斜側面形成用ダイ71sと、この傾斜側面形成用ダイ71sに外周端部が保持された電極体2~4の中央部を打ち抜く傾斜側面形成用パンチ75sとを有する。
この切断除去装置70は、形成する電極体2~4の形状は前述の具体例1と同様であるが、打ち抜きではなく、チョコレートブレイク法を採用するものである。
[切断除去装置70の具体例3]
[切断除去装置70の具体例4]
この全固体二次電池1は、例えば図13~図15に示すように、硫化水素吸着剤9を有する。当該硫化水素吸着剤9としては、活性炭、ゼオライト、触媒(酸化亜鉛)および/または脱水剤(五酸化二リンまたはシリカゲルなど)などが用いられる。また、前記硫化水素吸着剤9としては、不織布、ガラスペーパまたは発泡樹脂などの多孔質体に、前記触媒および/または前記脱水剤を配したものが用いられてもよい。ここで、前記硫化水素吸着剤9は、厚さが10~数100μmであることが好ましい。前記硫化水素吸着剤9は、数100μmより厚いと、電極体2~4および全固体二次電池1の外形寸法および重量が大きくなり過ぎることで無駄が生じ、10μmより薄いと、硫化水素を吸着する効果が小さくなることで硫化水素が外部に漏出するおそれを生じさせる。前記硫化水素吸着剤9が吸着し得る硫化水素の量については、例えば当該硫化水素吸着剤9として触媒(酸化亜鉛)が用いられる場合、反応式(H2S+ZnO→ZnS+H2O)により、当該酸化亜鉛が81.4gであれば、理論上、吸着される硫化水素は34.1g(硫黄は32.1g)となる。
この全固体二次電池1は、放電および充電の際に充電および放電が不要である。このような全固体二次電池1では、次の(1)および(2)の要件を満たすことが必須であり、次の(3)および/または(4)の要件も満たすことが好ましい。
(1)正極層5および/または負極層7の表面が粗化されている。
(2)正極層5および/または負極層7と正極集電体2および/または負極集電体4とを接触させた状態で、加圧充放電を行う。
(3)正極集電体2および/または負極集電体4の表面を粗化しておき、正極層5および/または負極層7を加圧成形する際に、正極集電体2および/または負極集電体4ごと加圧することで、正極集電体2および/または負極集電体4の粗化を正極層5および/または負極層7の表面に転写する。
(4)正極層5および/または負極層7の表面の粗化は、Rz=0.5~10.0μmであり、好ましくはRz=1.0~5.0μmである。
Claims (10)
- 粉体膜を積層して構成される粉体積層体を有する全固体二次電池の製造設備であって、
複数種の粉体材料を混合する混合装置と、
混合装置で混合された粉体材料を搬送する搬送装置と、
搬送装置で搬送された粉体材料から、少なくとも静電力を用いて前記粉体膜を形成する静電成膜装置とを具備し、
前記複数種の粉体材料から前記粉体積層体を形成する過程が乾式であることを特徴とする全固体二次電池の製造設備。 - 粉体積層体が、正極層、固体電解質層および負極層を有するものであり、
静電成膜装置が、正極層を形成するための正極用静電成膜機と、固体電解質層を形成するための電解質用静電成膜機と、負極層を形成するための負極用静電成膜機とを有することを特徴とする請求項1に記載の全固体二次電池の製造設備。 - 搬送装置が、正極層を形成するための粉体材料を正極用静電成膜機に搬送する正極用搬送機と、負極層を形成するための粉体材料を負極用静電成膜機に搬送する負極用搬送機とを有し、
固体電解質層を形成するための粉体材料を電解質用静電成膜機に搬送する電解質用搬送機をさらに具備することを特徴とする請求項2に記載の全固体二次電池の製造設備。 - 固体電解質層が、硫化物系固体電解質で構成される層であることを特徴とする請求項2または3に記載の全固体二次電池の製造設備。
- 静電成膜装置が、粉体材料が充填される粉体充填部材と、この粉体充填部材に充填された粉体材料を静電力により落下させて粉体膜にする直流電源とを有することを特徴とする請求項1または2に記載の全固体二次電池の製造設備。
- 静電成膜装置で形成された粉体膜を加圧する加圧装置と、
前記加圧装置で加圧された粉体膜の外周端部を切断して除去する切断除去装置とをさらに具備することを特徴とする請求項1または2に記載の全固体二次電池の製造設備。 - 加圧装置で加圧される対象が、静電成膜装置で形成された粉体膜と、この粉体膜を載置した集電体とであり、
前記集電体が、少なくとも前記粉体膜が載置される面を粗化したものであり、
粉体積層体を2つの前記集電体で挟んで構成される電極体に、加圧しながら充放電を行う加圧充放電装置をさらに具備することを特徴とする請求項6に記載の全固体二次電池の製造設備。 - 切断除去装置が、積層された粉体膜の外周端部を切断して除去することで、粉体積層体を形成するものであり、
前記切断除去装置が、形成する粉体積層体を、その負極層または正極層と固体電解質層との界面の面積が正極層または負極層と固体電解質層との界面の面積よりも大きくなるように、且つ、切断された面である側面が傾斜するように、切断するものであることを特徴とする請求項6に記載の全固体二次電池の製造設備。 - 切断除去装置が、粉体膜の切断される位置から内側の剛性が当該位置から外側の剛性よりも高い状態で、切断するものであることを特徴とする請求項6または8に記載の全固体二次電池の製造設備。
- 切断除去装置が、粉体膜を保持するダイと、このダイに保持された粉体膜を100mm/sec以下の速度で打ち抜くパンチとを有し、
前記ダイが、前記パンチの挿入される内周壁に逃げ面を有し、
前記ダイが、前記パンチにより打ち抜かれる粉体膜の変形が許容されるように当該粉体膜を保持するものであることを特徴とする請求項6または8に記載の全固体二次電池の製造設備。
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EP3823075A1 (en) | 2021-05-19 |
EP3823075A4 (en) | 2022-06-29 |
KR20210028657A (ko) | 2021-03-12 |
JPWO2020013295A1 (ja) | 2021-07-15 |
CN112385069A (zh) | 2021-02-19 |
US20210280843A1 (en) | 2021-09-09 |
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