WO2010089855A1 - 全固体電池及びその製造方法 - Google Patents
全固体電池及びその製造方法 Download PDFInfo
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- WO2010089855A1 WO2010089855A1 PCT/JP2009/051851 JP2009051851W WO2010089855A1 WO 2010089855 A1 WO2010089855 A1 WO 2010089855A1 JP 2009051851 W JP2009051851 W JP 2009051851W WO 2010089855 A1 WO2010089855 A1 WO 2010089855A1
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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
- H01M10/0413—Large-sized flat cells or batteries for motive or stationary systems with plate-like 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
- H01M10/058—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
- H01M10/05—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
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- 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
- H01M10/04—Construction or manufacture in general
- H01M10/0459—Cells or batteries with folded separator between plate-like 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
- H01M10/0468—Compression means for stacks of electrodes and 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
- H01M2220/00—Batteries for particular applications
- H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
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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 an all-solid battery and a method for manufacturing the same.
- 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-sized power such as for hybrid vehicles.
- the lithium ion secondary battery includes a positive electrode layer and a negative electrode layer, and an electrolyte disposed therebetween, and the electrolyte is composed of a non-aqueous liquid or solid.
- electrolytic solution a non-aqueous liquid
- the electrolytic solution penetrates into the positive electrode layer. Therefore, the interface between the positive electrode active material constituting the positive electrode layer and the electrolyte is easily formed, and the performance is easily improved.
- the widely used electrolyte is flammable, it is necessary to mount a system for ensuring safety.
- the solid electrolyte is nonflammable, the above system can be simplified. Therefore, a lithium ion secondary battery in a form provided with a solid electrolyte that is nonflammable (hereinafter sometimes referred to as a “solid electrolyte layer”) has been proposed.
- a lithium ion secondary battery in which a solid electrolyte layer is disposed between a positive electrode layer and a negative electrode layer (hereinafter sometimes referred to as a “compact all-solid battery”), the positive electrode active material and the electrolyte are solid.
- the electrolyte hardly penetrates into the positive electrode active material, and the interface between the positive electrode active material and the electrolyte is likely to be reduced. Therefore, in the powder all-solid battery, the area of the interface is increased by using, as the positive electrode layer, a positive electrode mixture layer containing a mixed powder obtained by mixing a positive electrode active material powder and a solid electrolyte powder.
- Patent Document 1 discloses an electrode in which one electrode is disposed in a concave portion on one surface of a battery separator bent in a pleat shape and the other electrode is disposed in a concave portion on the other surface.
- a battery having a group is disclosed.
- Patent Document 2 discloses a plurality of positive electrode sheets obtained by applying a positive electrode active material to a sheet-like positive electrode current collector, and a plurality of negative electrode sheets obtained by applying a negative electrode active material to a sheet-like negative electrode current collector.
- Patent Document 3 a plurality of sheet-like positive electrode plates and negative electrode plates are alternately stacked opposite to each other through a separator, and at least the positive electrode plate or the negative electrode plate is continuous by a tape-shaped separator. In this state, a rectangular battery is disclosed that is packed in a bag and folded at a separator fusion portion between each electrode plate.
- an object of the present invention is to provide an all-solid-state battery and a method for manufacturing the same that can suppress an increase in fastening load while increasing a power density.
- the first aspect of the present invention includes a plurality of laminates each including a positive electrode layer and a negative electrode layer, and a solid electrolyte layer disposed between the positive electrode layer and the negative electrode layer, and is selected from the plurality of laminates.
- any two adjacent laminated bodies are the first laminated body and the second laminated body
- the positive electrode layer of the first laminated body and the positive electrode layer of the second laminated body are in contact with each other, or the first laminated body
- a plurality of laminates are laminated such that the negative electrode layer of the body and the negative electrode layer of the second laminate are in contact with each other, and the solid electrolyte layer of the first laminate and the solid electrolyte layer of the second laminate are
- a first current collector that is connected to the positive electrode layer and not connected to the negative electrode layer and a second current collector that is connected to the negative electrode layer and not connected to the positive electrode layer are formed on a pair of side surfaces of the plurality of stacked layers that are connected and stacked.
- the connected insulating layer solution electrolyte layer is arranged, which is all-solid-state battery.
- An electrolyte layer forming step for forming each layer, and a plurality of positive electrodes at intervals on one side of a substrate including the surface of the solid electrolyte layer formed between the plurality of insulating layers after the electrolyte layer forming step Forming an electrode layer forming step, forming a plurality of negative electrode layers at intervals on the other surface side of the substrate including the surface of the solid electrolyte layer formed between the plurality of insulating layers;
- a folding step of folding the substrate as a crease, a first current collector disposed so as to be in contact with the positive electrode layer and not in contact with the negative electrode layer, and a second current collector so as to be in contact with the negative electrode layer and not in contact with the positive electrode layer A current collector arranging step for arranging It is a method of manufacture.
- the “base material” is a material that can maintain a solid state in the manufacturing process of an all-solid-state battery, can withstand the environment during use of the all-solid-state battery, and can transmit ions. If it is comprised by this, the form will not be specifically limited. Examples of the form of the substrate include a woven or fibrous sheet provided with slit-like or lattice-like holes.
- the all solid state battery of the present invention a plurality of laminates are laminated so that the negative electrode layers of adjacent laminates or the positive electrode layers of adjacent laminates are in contact with each other. Therefore, even if the number of stacked bodies is increased to increase the electrode area, the area to which the fastening load is applied can be kept constant. Therefore, according to the present invention, an increase in the fastening load can be suppressed by making the area to which the fastening load is applied constant. In addition, according to the present invention, by increasing the number of stacked bodies, it is possible to increase the electrode area and increase the output density. Therefore, according to the present invention, it is possible to provide an all solid state battery capable of suppressing an increase in fastening load while increasing a power density.
- the all solid state battery of the present invention can be produced through a process of folding a base material on which a plurality of laminated bodies are formed at intervals.
- the manufacturing method of an all-solid-state battery which can manufacture the all-solid-state battery which can suppress the increase in a fastening load, increasing a power density can be provided.
- FIG. 1 is a cross-sectional view showing an example of a configuration of an all-solid battery 10. It is a flowchart which shows the flow of the process included in the manufacturing method of an all-solid-state battery. It is a figure which simplifies and shows the manufacturing method of an all-solid-state battery.
- FIG. 1 is a cross-sectional view showing an embodiment of an all solid state battery 10 of the present invention.
- FIG. 1 only a part of the all solid state battery 10 is extracted and enlarged. Further, in FIG. 1, some reference numerals are omitted.
- the all solid state battery 10 includes stacked bodies 4, 4,.
- the laminate 4 includes a positive electrode layer 1 having a positive electrode active material through which lithium ions enter and exit, a negative electrode layer 2 having a negative electrode active material through which lithium ions enter and exit, and a positive electrode layer 1 and a negative electrode layer 2.
- a solid electrolyte layer 3 disposed between them is provided, and the solid electrolyte layers 3 and 3 of two adjacent stacked bodies 4 and 4 are connected by an insulating layer 5.
- the two adjacent laminated bodies 4 and 4 are in contact with the negative electrode layers 2 and 2 constituting the respective laminated bodies 4 and 4 or the positive electrode layers 1 and 1 constituting the respective laminated bodies 4 and 4. So that they are stacked.
- a first current collector 6 and a second current collector 7 are disposed on a pair of side surfaces (upper side surface and lower side surface in FIG. 1) of the stacked layers 4, 4,. Are arranged respectively.
- the first current collector 6 is in contact with the positive electrode layers 1, 1,..., While the first current collector 6 is not in contact with the negative electrode layers 2, 2,. Are separated by insulating layers 5, 5,.
- the second current collector 7 is in contact with the negative electrode layers 2, 2,..., But is not in contact with the positive electrode layers 1, 1,. Are separated by insulating layers 5, 5,.
- terminal portions 8, 8 are disposed at the left and right ends of the sheet of FIG.
- the positive electrode layer 1 contains a positive electrode active material, a solid electrolyte, and a conductive material, and these are uniformly mixed through a binder.
- the thickness of the positive electrode layer 1 is t1
- the positive electrode layers 1, 1 of the adjacent laminates 4, 4 or the negative electrode layers 2, 2 Since the layers are laminated so that they are in contact with each other, the total thickness of the positive electrode layers 1 and 1 sandwiched between the pair of solid electrolyte layers 3 and 3 is apparently 2 ⁇ t1.
- the solid electrolyte layers 3 and 3 are disposed on both sides of the two positive electrode layers 1 and 1.
- lithium ions present in each positive electrode layer 1, 1 can go back and forth between the solid electrolyte layers 3, 3 constituting the laminates 4, 4 together with the respective positive electrode layers 1, 1. That is, the lithium ions in the positive electrode layer 1 located on the right side of the contact interface between the two positive electrode layers 1 and 1 can travel to and from the solid electrolyte layer 3 existing on the right side of the contact interface. Lithium ions in the positive electrode layer 1 located on the left side of the interface can travel to and from the solid electrolyte layer 3 existing on the left side of the contact interface. Therefore, in the all solid state battery 10, it is possible to keep the maximum value of the movement distance of lithium ions moving inside the positive electrode layers 1 and 1 at t1.
- the negative electrode layer 2 contains a negative electrode active material, a solid electrolyte, and a conductive material, and these are uniformly mixed through a binder.
- the thickness of the negative electrode layer 2 is t2
- the positive electrode layers 1, 1 of the adjacent laminates 4, 4 or the negative electrode layers 2, 2 Since the layers are laminated so that they are in contact with each other, the total thickness of the negative electrode layers 2 and 2 sandwiched between the pair of solid electrolyte layers 3 and 3 is apparently 2 ⁇ t2.
- the solid electrolyte layers 3 and 3 are disposed on both sides of the two negative electrode layers 2 and 2.
- lithium ions present in each negative electrode layer 2, 2 can go back and forth between the solid electrolyte layers 3, 3 constituting the laminates 4, 4 together with the respective negative electrode layers 2, 2. That is, lithium ions in the negative electrode layer 2 located on the right side of the contact interface between the two negative electrode layers 2 and 2 can go back and forth between the solid electrolyte layer 3 existing on the right side of the contact interface. Lithium ions in the negative electrode layer 2 located on the left side of the interface can travel to and from the solid electrolyte layer 3 existing on the left side of the contact interface. Therefore, in the all solid state battery 10, it is possible to keep the maximum value of the movement distance of lithium ions moving inside the negative electrode layers 2 and 2 at t2.
- the solid electrolyte layer 3 contains a solid electrolyte that has lithium ion conductivity and does not have conductivity. Except for the left and right ends of the all solid state battery 10, the solid electrolyte layer 3 is not in contact with the first current collector 6 and the second current collector 7. In addition, since the solid electrolyte layer 3 does not have conductivity, there is no problem even if it contacts the first current collector 6 and / or the second current collector 7 at the left and right ends of the all-solid battery 10.
- the laminate 4 has a positive electrode layer 1, a negative electrode layer 2, and a solid electrolyte layer 3 disposed between the positive electrode layer 1 and the negative electrode layer 2.
- the all-solid-state battery 10 has a plurality of stacked bodies 4, 4,... And is folded with insulating layers 5, 5,. Or it laminates
- the insulating layer 5 is connected to the solid electrolyte layer 3.
- the insulating layer 5 in the all solid state battery 10 is made of a dense insulating material having flexibility. Because of the flexibility, the insulating layers 5, 5,... Can be folded as folds. Further, since the insulating layers 5, 5,... Are made of a dense material, the contact between the first current collector 6 and the negative electrode layers 2, 2,. Contact with the layers 1, 1,... Can be prevented.
- the first current collector 6 has conductive powder. By having the conductive powder, contact with the positive electrode layers 1, 1,... Can be ensured even if the end surfaces of the positive electrode layers 1, 1,. In the all solid state battery 10, the first current collector 6 is in contact with the positive electrode layers 1, 1,... And is not in contact with the negative electrode layers 2, 2,. Between the negative electrode layers 2, 2,... And the first current collector 6, insulating layers 5, 5,.
- the second current collector 7 has conductive powder. By having the conductive powder, even if the end surfaces of the negative electrode layers 2, 2,... Are curved, contact with the negative electrode layers 2, 2,. In the all solid state battery 10, the second current collector 7 is in contact with the negative electrode layers 2, 2,..., And is not in contact with the positive electrode layers 1, 1,. Between the positive electrode layers 1, 1,... And the second current collector 7, insulating layers 5, 5,.
- the terminal part 8 is comprised by the solid electrolyte layer 3 and the layers 8a and 8a which do not have lithium ion conductivity and electroconductivity.
- it is necessary to reduce the interface resistance at the contact interface between the positive electrode active material and the solid electrolyte and the interface resistance at the contact interface between the negative electrode active material and the solid electrolyte.
- it is effective to apply a predetermined pressure or more to the contact interface so that the positive electrode active material and the solid electrolyte and the negative electrode active material and the solid electrolyte are in close contact with each other.
- Terminal portions 8 and 8 are arranged at the ends, respectively, and a fastening load is applied via the terminal portions 8 and 8.
- the pressure (surface pressure) applied to the contact interface has a correlation with the magnitude of the fastening load and the area of the surface to which the fastening load is applied. That is, when a surface pressure of a certain level or more is secured, the larger the area of the surface to which the fastening load is applied, the larger the fastening load needs to be applied.
- the all-solid-state battery 10 includes a plurality of positive electrode layers 1, 1,... And negative electrode layers 2, 2,..., Which are folded with the insulating layers 5, 5,. The area of the surface to which the fastening load is applied is kept constant even if the number of the positive electrode layers 1, 1,...
- the all-solid-state battery 10 the number of the stacked bodies 4, 4,... (The number of the positive electrode layers 1, 1,... And the negative electrode layers 2, 2,. Even in such a case, it is not necessary to increase the fastening load. Therefore, according to the all-solid-state battery 10, it becomes possible to ensure a fixed surface pressure by giving a fixed fastening load irrespective of the number of the laminated bodies 4, 4,.
- the current collector 9 is in contact with the first current collector 6 or the second current collector 7.
- the current collector 9 in contact with the first current collector 6 functions as a positive electrode
- the current collector 9 in contact with the second current collector 7 functions as a negative electrode. That is, in the all solid state battery 10, the current collectors 9 and 9 function as external output terminals.
- the current collection parts 9 and 9 when the structure pinched
- the positive electrode active material contained in the positive electrode layer 1 a known positive electrode active material that can be used in a lithium ion secondary battery having a solid electrolyte layer can be used.
- Specific examples of the positive electrode active material contained in the positive electrode layer 1 include an active material containing 50% by mass or more of LiCoO 2 .
- the well-known solid electrolyte which can be used with the lithium ion secondary battery which has a solid electrolyte layer can be used as a solid electrolyte contained in the positive electrode layer 1 and the negative electrode layer 2.
- FIG. Specific examples of the solid electrolyte contained in the positive electrode layer 1 and the negative electrode layer 2 include LiPF 6 and Li 7 P 3 S 11 .
- a conductive material contained in the positive electrode layer 1 and the negative electrode layer 2 a known conductive material that can be used in the positive electrode layer of a lithium ion secondary battery having a solid electrolyte layer can be used.
- the conductive material contained in the positive electrode layer 1 and the negative electrode layer 2 include a fibrous carbon material typified by carbon nanotubes, a green compact of carbon black, and the like.
- this invention is not limited to the said form, The positive electrode layer and negative electrode layer of a form which do not have a conductive material are used. It is also possible. However, from the standpoint of securing a conduction path for electrons moving up and down in FIG. 1 and reducing the electron conduction resistance, it is necessary to use a positive electrode layer and a negative electrode layer containing a conductive material. preferable.
- the lithium ion conductivity of the solid electrolyte contained in the positive electrode layer 1 is ⁇ Li [S / cm]
- the volume fraction of the positive electrode active material contained in the positive electrode layer 1 is CLi [%]
- the volume fraction of the conductive material contained in the positive electrode layer 1 is Ce ⁇ [%]
- the thickness of the positive electrode layer 1 is t1 [mm]
- the width of the layer 1 (the length in the vertical direction of the paper in FIG. 1; the same applies hereinafter) is defined as W1 [mm].
- the relationship of the following formula 1 assumes that the electron conductivity is sufficiently higher than the lithium ion conductivity.
- the relationship of the following formula 1 is that lithium ions that are less likely to be conducted than electrons are conducted in the horizontal direction of the paper in FIG. 1, and electrons that are more likely to be conducted than lithium ions are conducted in the vertical direction of the paper in FIG. It can be said that there is no increase in resistance, the charge / discharge speed can be increased, and the all solid state battery 10 capable of increasing the capacity should be satisfied.
- the contact interface between the pair of positive electrode layers 1 and 1 stacked It is preferable that the current collector foil or the like is not inserted into the contact interface between the pair of negative electrode layers 2 and 2 to be formed.
- the negative electrode active material contained in the negative electrode layer 2 a known negative electrode active material that can be used in a lithium ion secondary battery having a solid electrolyte layer can be used.
- Specific examples of the negative electrode active material contained in the negative electrode layer 2 include graphitizable coke and non-graphitizable carbon material.
- the solid electrolyte contained in the solid electrolyte layer 3 a known solid electrolyte that can be used in a lithium ion secondary battery having a solid electrolyte layer can be used.
- Specific examples of the solid electrolyte contained in the solid electrolyte layer 3 include Li 2 S—P 2 S 5 .
- the insulating material contained in the insulating layer 5 is a flexible dense insulating material and has a property that can withstand the environment when the all solid state battery 10 is used. If there is, it will not be specifically limited.
- Specific examples of the insulating material contained in the insulating layer 5 include polyolefin materials (polypropylene (PP) and polyethylene (PE)), polyethylene terephthalate (PET) materials, and the like.
- specific examples of the conductive powder constituting the first current collector 6 and the second current collector 7 include carbon powder.
- the layer 8 a constituting the terminal unit 8 may be composed of a material that can withstand the environment during use of the all solid state battery 10 and does not have lithium ion conductivity and conductivity. it can.
- the material include polyolefin materials (polypropylene (PP), polyethylene (PE)), polyethylene terephthalate (PET) materials, and the like.
- the current collector 9 can be made of a known material that can form an external output terminal in a lithium ion secondary battery having a solid electrolyte layer.
- the form of the current collection part 9 is not specifically limited, It can be set as the form of current collection foil or a current collection sheet.
- FIG. 2 is a flowchart showing a flow of steps included in the method for producing an all solid state battery of the present invention.
- FIG. 3 is a simplified diagram showing the method for manufacturing an all-solid battery according to the present invention. In FIG. 3, the description of some symbols is omitted. In FIG. 3, the same reference numerals as those used in FIG. 1 are given to those having the same configuration as that of the all solid state battery 10, and the description thereof will be omitted as appropriate.
- the manufacturing method of the all-solid battery of the present invention will be described below with reference to FIGS.
- the manufacturing method of the all-solid-state battery of this invention has an insulating layer formation process (process S1), an electrolyte layer formation process (process S2), an electrode layer formation process (process S3), The folding step (step S4) and the current collector arrangement step (step S5) are included, and the all solid state battery 10 of the present invention is manufactured through the steps S1 to S5.
- process S1 an insulating layer formation process
- process S2 an electrolyte layer formation process
- process S3 an electrode layer formation process
- the folding step S4 and the current collector arrangement step (step S5) are included, and the all solid state battery 10 of the present invention is manufactured through the steps S1 to S5.
- Step S1 is a step of forming a plurality of insulating layers 5, 5,... In a mesh sheet base material 11 having a plurality of holes with a plurality of intervals 12, 12,.
- Step S1 for example, a solution in which an insulating material constituting the insulating layers 5, 5,... Is dissolved is applied to the mesh sheet base material 11 in a regular pattern, and the solvent is volatilized, whereby a plurality of intervals 12 are obtained.
- 12,... Are formed to form a plurality of insulating layers 5, 5,.
- Step S2 is a step of forming solid electrolyte layers 3, 3,... At least between the plurality of insulating layers 5, 5,.
- step S2 for example, a solution in which the solid electrolyte constituting the solid electrolyte layers 3, 3,... Is dispersed is applied to the portion of the mesh sheet base material 11 where the insulating layers 5, 5,. By volatilizing the solvent, a plurality of mesh sheet base material 11 in the longitudinal direction at both ends (both ends located on the left and right sides in FIG. 3), and between the insulating layers 5, 5,.
- the step of forming solid electrolyte layers 3, 3, When the solid electrolyte layers 3, 3,... Are formed in this manner, a member in which the insulating layers 5, 5,... And the solid electrolyte layers 3, 3,.
- Step S3 In the step S3, after the step S2, an interval is formed on one surface side of the mesh sheet substrate 11 including the surfaces of the solid electrolyte layers 3, 3,... Formed between the plurality of insulating layers 5, 5,.
- the other side of the mesh sheet substrate 11 that includes the surfaces of the solid electrolyte layers 3, 3,... Formed between the plurality of insulating layers 5, 5,. Are a plurality of negative electrode layers 2, 2,... Formed at intervals.
- Step S3 includes, for example, all the solid electrolyte layers 3 except the solid electrolyte layers 3 and 3 formed at both ends in the longitudinal direction of the mesh sheet base material 11 among the solid electrolyte layers 3 and 3 formed in the step S2.
- step S2 if the solid electrolyte layers 3, 3,... Are formed only in places where the insulating layers 5, 5,... Are not formed, the solid electrolyte layers 3, 3,. Become. Therefore, by forming positive electrode layers 1, 1,... On one surface side of the solid electrolyte layers 3, 3,... And negative electrode layers 2, 2,. The layers 1, 1,... And the plurality of negative electrode layers 2, 2,. In step S3, for example, the plurality of positive electrode layers 1, 1,...
- the plurality of negative electrode layers 2, 2,... Are, for example, a solution in which the negative electrode active material, the solid electrolyte, the conductive material, and the binder constituting the negative electrode layers 2, 2,. It can form by apply
- Step S4 is a step of folding the mesh sheet base material 11 with the insulating layers 5, 5,... Formed in the step S1 as folds.
- Step S4 is, for example, after the step S3, by folding the mesh sheet substrate 11 with the insulating layers 5, 5,... As folds, the positive electrode layers 1, 1 of the adjacent laminates 4, 4, or It can be set as the process of laminating
- Step S5 the first current collector 6 is disposed so as to be in contact with the positive electrode layers 1, 1,... Formed in the step S3 and not in contact with the negative electrode layers 2, 2,.
- the second current collector 7 is disposed so as to be in contact with the negative electrode layers 2, 2,... Formed in the step S3 and not in contact with the positive electrode layers 1, 1,. .
- the second current collector 7 is disposed in a casing (not shown; the same applies hereinafter) in which the current collector 9 is disposed at the bottom, and then the structure manufactured in step S4 is encased.
- a step of disposing the current collector 9 on the first current collector 6 after the first current collector 6 is disposed on the upper surface of the structure that is inserted into the body and then inserted into the housing. be able to.
- the method for producing an all-solid battery of the present invention having the steps S1 to S5, for example, the solid electrolyte layers formed at both ends in the longitudinal direction of the mesh sheet substrate 11 between the step S3 and the step S4.
- the all-solid-state battery 10 can be manufactured by interposing the step of forming the layer 8a on the upper and lower surfaces of the layers 3 and 3.
- An all-solid-state battery manufacturing method capable of manufacturing the all-solid-state battery 10 that can be suppressed can be provided.
- the mesh sheet substrate 11 used in the method for producing an all-solid battery of the present invention has a function of complementing the tensile strength of the solid electrolyte layers 3, 3,... To which tension is applied when folded in a bellows shape in step S 4. Bear. Further, since lithium ions pass through the solid electrolyte layers 3, 3,... Formed on the mesh sheet substrate 11, the mesh sheet substrate 11 has holes through which lithium ions can pass. Specific examples of the constituent material of the mesh sheet substrate 11 include polypropylene (PP), polyethylene (PE), polyethylene terephthalate (PET), and the like.
- the form in which the mesh sheet base material 11 was used was illustrated, this invention is not limited to the said form.
- the base material on which the insulating layers 5, 5,..., The solid electrolyte layers 3, 3,... And the negative electrode layers 2, 2, It has only to be configured by a member that can maintain a solid state in the manufacturing process of the all solid state battery 10 and can withstand the environment when the all solid state battery 10 is used.
- Examples of other forms of the substrate used in the method for producing an all solid state battery of the present invention include a sheet-like substrate and a long roll-like substrate having a plurality of slit-like holes. Can do.
- the mode in which the step S2 of forming the solid electrolyte layers 3, 3,... Is provided only in the places where the insulating layers 5, 5,.
- the method for producing an all solid state battery of the present invention is not limited to this form.
- the solid electrolyte layer 3 may be formed on the entire surface including the surfaces of the insulating layers 5, 5,.
- Step S3 in the method for producing an all-solid-state battery of the present invention includes a positive electrode on the surface of the insulating layer 5 (a portion indicated by X in FIG. 3) to be in contact with the pair of positive electrode layers 1 and 1 when folded in step S4. It is possible to form the layers 1, 1,...
- Step S3 in the method for producing an all-solid-state battery of the present invention includes a negative electrode on the surface of the insulating layer 5 to be brought into contact with the pair of negative electrode layers 2 and 2 (location indicated by Y in FIG. 3) when folded in step S4. It is also possible to form the layers 2, 2,.
- the present invention is not limited to this form.
- a negative electrode layer constituted by an In foil may be provided.
- the all-solid-state battery of the present invention having a solid electrolyte layer and the manufacturing method thereof have been described.
- the technical idea relating to the structure of the all solid state battery of the present invention and the method of manufacturing the all solid state battery of the present invention can be applied to a secondary battery including a non-aqueous electrolyte by making necessary changes. Is possible.
- the all-solid-state battery 10 when a structure sandwiched between a pair of current collectors 9 and 9 is stacked, it is not essential to interpose the current collector 9 between adjacent structures.
- the all-solid-state battery of the present invention can be used as a power source for electric vehicles and information equipment.
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Abstract
Description
本発明の第1の態様は、正極層及び負極層、並びに、正極層と負極層との間に配設された固体電解質層を有する積層体、を複数具備し、複数の積層体から選択された任意の隣り合う2つの積層体を第1積層体及び第2積層体とするとき、第1積層体の正極層と第2積層体の正極層とが接触するように、又は、第1積層体の負極層と第2積層体の負極層とが接触するように、複数の積層体が積層され、第1積層体の固体電解質層と第2積層体の固体電解質層とが、絶縁層によって接続され、積層された複数の積層体の一対の側面に、正極層と接続され且つ負極層と接続されない第1集電体及び負極層と接続され且つ正極層と接続されない第2集電体が、それぞれ配設され、正極層と第2集電体との間、及び、負極層と第1集電体との間に、固体電解質層に接続された絶縁層がそれぞれ配置されていることを特徴とする、全固体電池である。
図1は、本発明の全固体電池10の形態例を示す断面図である。図1では、全固体電池10の一部のみを抽出し、拡大して示している。また、図1では、一部符号の記載を省略している。
正極層1は、正極活物質、固体電解質、及び、導電材を含有し、結着材を介してこれらが均一に混合されている。正極層1の厚さをt1とするとき、図1の左右端部を除いて、全固体電池10では、隣り合う積層体4、4の正極層1、1同士、又は、負極層2、2同士が接触するように積層されるため、一対の固体電解質層3、3によって挟まれた正極層1、1の全体の厚さは、見かけ上、2×t1となる。ところが、全固体電池10では、2つの正極層1、1の両側に固体電解質層3、3が配置されている。そのため、各正極層1、1に存在するリチウムイオンは、それぞれの正極層1、1と共に積層体4、4を構成する固体電解質層3、3との間で行き来することができる。すなわち、2つの正極層1、1の接触界面の右側に位置する正極層1内のリチウムイオンは、当該接触界面の右側に存在する固体電解質層3との間で行き来することができ、当該接触界面の左側に位置する正極層1内のリチウムイオンは、当該接触界面の左側に存在する固体電解質層3との間で行き来することができる。したがって、全固体電池10では、各正極層1、1の内部を移動するリチウムイオンの移動距離の最大値をt1に留めることが可能になる。
負極層2は、負極活物質、固体電解質、及び、導電材を含有し、結着材を介してこれらが均一に混合されている。負極層2の厚さをt2とするとき、図1の左右端部を除いて、全固体電池10では、隣り合う積層体4、4の正極層1、1同士、又は、負極層2、2同士が接触するように積層されるため、一対の固体電解質層3、3によって挟まれた負極層2、2の全体の厚さは、見かけ上、2×t2となる。ところが、全固体電池10では、2つの負極層2、2の両側に固体電解質層3、3が配置されている。そのため、各負極層2、2に存在するリチウムイオンは、それぞれの負極層2、2と共に積層体4、4を構成する固体電解質層3、3との間で行き来することができる。すなわち、2つの負極層2、2の接触界面の右側に位置する負極層2内のリチウムイオンは、当該接触界面の右側に存在する固体電解質層3との間で行き来することができ、当該接触界面の左側に位置する負極層2内のリチウムイオンは、当該接触界面の左側に存在する固体電解質層3との間で行き来することができる。したがって、全固体電池10では、各負極層2、2の内部を移動するリチウムイオンの移動距離の最大値をt2に留めることが可能になる。
固体電解質層3は、リチウムイオン伝導性を有し、且つ、導電性を有しない固体電解質を含有している。全固体電池10の左右端部を除いて、固体電解質層3は、第1集電体6及び第2集電体7と接触していない。なお、固体電解質層3は導電性を有しないため、全固体電池10の左右端部において第1集電体6及び/又は第2集電体7と接触しても問題はない。
積層体4は、正極層1、負極層2、及び、正極層1と負極層2との間に配設された固体電解質層3を有している。全固体電池10は、複数の積層体4、4、…を有し、後述する絶縁層5、5、…を折り目として折り畳むことにより、隣り合う積層体4、4の正極層1、1同士、又は、負極層2、2同士が接触する形態で積層される。
絶縁層5は、固体電解質層3に接続されている。全固体電池10における絶縁層5は、可撓性を有する緻密な絶縁材料によって構成されている。可撓性を有するため、絶縁層5、5、…を折り目として折り畳むことができる。また、緻密な材料によって構成されるため、絶縁層5、5、…は、後述する第1集電体6と負極層2、2、…との接触、及び、第2集電体7と正極層1、1、…との接触を防ぐことができる。
第1集電体6は、導電性粉体を有している。導電性粉体を有することで、正極層1、1、…の端面が湾曲していても、正極層1、1、…との接触を確保することができる。全固体電池10において、第1集電体6は、正極層1、1、…と接触し、負極層2、2、…とは接触しない。負極層2、2、…と第1集電体6との間には、絶縁層5、5、…が配置される。
第2集電体7は、導電性粉体を有している。導電性粉体を有することで、負極層2、2、…の端面が湾曲していても、負極層2、2、…との接触を確保することができる。全固体電池10において、第2集電体7は、負極層2、2、…と接触し、正極層1、1、…とは接触しない。正極層1、1、…と第2集電体7との間には、絶縁層5、5、…が配置される。
端末部8は、固体電解質層3と、リチウムイオン伝導性及び導電性を有しない層8a、8aによって構成されている。全固体電池10の性能を向上させるためには、正極活物質と固体電解質との接触界面における界面抵抗、及び、負極活物質と固体電解質との接触界面における界面抵抗を低減する必要がある。界面抵抗の低減には、接触界面に所定以上の圧力を付与し、正極活物質と固体電解質、及び、負極活物質と固体電解質を密着させることが有効であるため、全固体電池10では、左右端に端末部8、8をそれぞれ配置し、当該端末部8、8を介して締結荷重を付与している。ここで、接触界面へと付与される圧力(面圧)は、締結荷重の大きさ、及び、締結荷重が付与される面の面積と相関がある。すなわち、一定以上の面圧を確保する場合、締結荷重が付与される面の面積が大きければ大きいほど、大きな締結荷重を付与する必要がある。全固体電池10には、複数の正極層1、1、…、及び、負極層2、2、…が備えられているが、これらは絶縁層5、5、…を折り目として折り畳まれているため、締結荷重が付与される面の面積は、正極層1、1、…及び負極層2、2、…の数を増やしても一定に保たれる。それゆえ、全固体電池10によれば、出力密度を増大させるために積層体4、4、…の数(正極層1、1、…、及び、負極層2、2、…の数)を増大させた場合であっても、締結荷重を増大させる必要がない。したがって、全固体電池10によれば、積層体4、4、…の数によらず、一定の締結荷重を付与することによって、一定の面圧を確保することが可能になる。
集電部9は、第1集電体6又は第2集電体7と接触している。全固体電池10では、第1集電体6と接触している集電部9が+極として機能し、第2集電体7と接触している集電部9が-極として機能する。すなわち、全固体電池10では、集電部9、9が外部出力端子として機能する。なお、本発明において、一対の集電部9、9によって挟まれた構成物を図1の紙面上下方向へと積層する場合、積層された複数の構成物の上下端に集電部9、9がそれぞれ配置されていれば良く、積層された構成物と構成物との間には集電部9を配置しなくても良い。
(W1/t1)2≦(Ce-×σe-)/(CLi×σLi) (式1)
同様に、負極層2の厚さt2、及び、負極層2の幅W2を用いると、下記式2が導かれる。
(W2/t2)2≦(Ce-×σe-)/(CLi×σLi) (式2)
例えば、σe-=50[S/cm]、Ce-=10[%]、σLi=0.01[S/cm]、CLi=30[%]、t1=t2=0.1[mm]とすると、W1≦4.08mm、W2≦4.08mmとなる。なお、積層される一対の正極層1、1の接触界面、及び/又は、積層される一対の負極層2、2の接触界面に集電箔等を挿入すれば、電子伝導抵抗を低減することが可能になる。そのため、この場合には、正極層1及び負極層2の幅を上記関係式の上限値よりも大きくしても、内部抵抗の増大が無く、充放電を速く行うことが可能な、全固体電池を提供することができる。しかし、接触界面に集電箔を挿入すると、全固体電池全体の体積及び質量が増大するため、出力密度の増大効果が損なわれやすい。したがって、締結荷重の増加抑制効果のみならず、出力密度の増大効果をも奏することが可能な形態にする等の観点からは、積層される一対の正極層1、1の接触界面、及び、積層される一対の負極層2、2の接触界面に集電箔等が挿入されない形態とすることが好ましい。
図2は、本発明の全固体電池の製造方法に含まれる工程の流れを示すフローチャートである。図3は、本発明の全固体電池の製造方法を簡略化して示す図である。図3では、一部符号の記載を省略する。また、図3において、全固体電池10と同様の構成を採るものには、図1で使用した符号と同一の符号を付し、その説明を適宜省略する。図1~図3を参照しつつ、本発明の全固体電池の製造方法について、以下に説明する。
工程S1は、複数の孔を有する網目シート基材11に、複数の間隔12、12、…を開けて、複数の絶縁層5、5、…を形成する工程である。工程S1は、例えば、絶縁層5、5、…を構成する絶縁材料を溶解させた溶液を、網目シート基材11へ規則的なパターンで塗布し、溶媒を揮発させることにより、複数の間隔12、12、…を開けて、複数の絶縁層5、5、…を形成する工程、とすることができる。
工程S2は、上記工程S1の後に、少なくとも複数の絶縁層5、5、…の間に、固体電解質層3、3、…を形成する工程である。工程S2は、例えば、固体電解質層3、3、…を構成する固体電解質を分散させた溶液を、絶縁層5、5、…が形成されていない網目シート基材11の箇所へと塗布し、溶媒を揮発させることにより、網目シート基材11の長手方向両端(図3の紙面左右側に位置する両端部。以下において同じ。)、及び、絶縁層5、5、…の間に、複数の固体電解質層3、3、…を形成する工程、とすることができる。固体電解質層3、3、…をこのように形成すると、絶縁層5、5、…と固体電解質層3、3、…とが交互に隙間無く形成された部材を作製することができる。
工程S3は、上記工程S2の後に、複数の絶縁層5、5、…の間に形成された固体電解質層3、3、…の表面を含む網目シート基材11の一面側に、間隔を開けて複数の正極層1、1、…を形成し、複数の絶縁層5、5、…の間に形成された固体電解質層3、3、…の表面を含む網目シート基材11の他面側に、間隔を開けて複数の負極層2、2、…を形成する工程である。工程S3は、例えば、上記工程S2で形成した固体電解質層3、3、…のうち、網目シート基材11の長手方向両端に形成した固体電解質層3、3を除くすべての固体電解質層3、3、…の一面側(図3の紙面上側)にのみ正極層1、1、…を形成し、正極層1、1、…が形成される固体電解質層3、3、…の他面側(図3の紙面下側)にのみ負極層2、2、…を形成することにより、複数の積層体4、4、…を形成する工程とすることができる。上記工程S2において、絶縁層5、5、…が形成されていない箇所にのみ固体電解質層3、3、…を形成すると、固体電解質層3、3、…は間隔を開けて形成されることになる。そのため、当該固体電解質層3、3、…の一面側に正極層1、1、…を、他面側に負極層2、2、…をそれぞれ形成することにより、間隔を開けて、複数の正極層1、1、…、及び、複数の負極層2、2、…を形成することができる。工程S3において、複数の正極層1、1、…は、例えば、正極層1、1、…を構成する正極活物質、固体電解質、導電材、及び、結着材を分散させた溶液を固体電解質層3、3、…の一面側に塗布し、溶媒を揮発させることにより形成することができる。また、工程S3において、複数の負極層2、2、…は、例えば、負極層2、2、…を構成する負極活物質、固体電解質、導電材、及び、結着材を分散させた溶液を固体電解質層3、3、…の他面側に塗布し、溶媒を揮発させることにより形成することができる。
工程S4は、上記工程S1で形成された絶縁層5、5、…を折り目として、網目シート基材11を折り畳む工程である。工程S4は、例えば、上記工程S3の後に、絶縁層5、5、…を折り目として、網目シート基材11を折り畳むことにより、隣り合う積層体4、4の正極層1、1同士、又は、負極層2、2同士を接触させる形態で、複数の積層体4、4、…を積層する工程、とすることができる。
工程S5は、上記工程S3で形成された正極層1、1、…と接触し且つ上記工程S3で形成された負極層2、2、…と接触しないように第1集電体6を配置し、上記工程S3で形成された負極層2、2、…と接触し且つ上記工程S3で形成された正極層1、1、…と接触しないように第2集電体7を配置する工程である。工程S5は、例えば、底に集電部9が配置された筐体(不図示。以下において同じ。)に第2集電体7を配置した後、上記工程S4で作製された構造体を筐体へ挿入し、次いで、筐体へと挿入された構造体の上面に第1集電体6を配置した後、第1集電体6の上に集電部9を配置する工程、とすることができる。
S2…電解質層形成工程
S3…電極層形成工程
S4…折り畳み工程
S5…集電体配置工程
1…正極層
2…負極層
3…固体電解質層
4…積層体
5…絶縁層
6…第1集電体
7…第2集電体
8…端末部
8a…層
9…集電箔
10…全固体電池
11…網目シート基材(基材)
12…間隔
Claims (2)
- 正極層及び負極層、並びに、前記正極層と前記負極層との間に配設された固体電解質層を有する積層体、を複数具備し、
複数の前記積層体から選択された任意の隣り合う2つの前記積層体を第1積層体及び第2積層体とするとき、前記第1積層体の前記正極層と前記第2積層体の前記正極層とが接触するように、又は、前記第1積層体の前記負極層と前記第2積層体の前記負極層とが接触するように、複数の前記積層体が積層され、
前記第1積層体の前記固体電解質層と前記第2積層体の前記固体電解質層とが、絶縁層によって接続され、
積層された複数の前記積層体の一対の側面に、前記正極層と接続され且つ前記負極層と接続されない第1集電体、及び、前記負極層と接続され且つ前記正極層と接続されない第2集電体が、それぞれ配設され、
前記正極層と前記第2集電体との間、及び、前記負極層と前記第1集電体との間に、前記固体電解質層に接続された絶縁層がそれぞれ配置されていることを特徴とする、全固体電池。 - 基材に、複数の間隔を開けて複数の絶縁層を形成する、絶縁層形成工程と、
前記絶縁層形成工程の後に、少なくとも複数の前記絶縁層の間に固体電解質層をそれぞれ形成する、電解質層形成工程と、
前記電解質層形成工程の後に、複数の前記絶縁層の間に形成された前記固体電解質層の表面を含む前記基材の一面側に、間隔を開けて複数の正極層を形成し、複数の前記絶縁層の間に形成された前記固体電解質層の表面を含む前記基材の他面側に、間隔を開けて複数の負極層を形成する、電極層形成工程と、
前記絶縁層を折り目として前記基材を折り畳む、折り畳み工程と、
前記正極層と接触し且つ前記負極層と接触しないように第1集電体を配置し、前記負極層と接触し且つ前記正極層と接触しないように第2集電体を配置する、集電体配置工程と、
を有することを特徴とする、全固体電池の製造方法。
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PCT/JP2009/051851 WO2010089855A1 (ja) | 2009-02-04 | 2009-02-04 | 全固体電池及びその製造方法 |
JP2009550180A JP5152200B2 (ja) | 2009-02-04 | 2009-02-04 | 全固体電池及びその製造方法 |
KR1020107004655A KR101155808B1 (ko) | 2009-02-04 | 2009-02-04 | 전고체 전지 및 그 제조 방법 |
CN200980100243XA CN101861675B (zh) | 2009-02-04 | 2009-02-04 | 全固体电池及其制造方法 |
US12/673,782 US8338036B2 (en) | 2009-02-04 | 2009-02-04 | All-solid-state battery and manufacturing method thereof |
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EP2395588A1 (en) | 2011-12-14 |
KR20100113473A (ko) | 2010-10-21 |
KR101155808B1 (ko) | 2012-06-12 |
US20110281160A1 (en) | 2011-11-17 |
JPWO2010089855A1 (ja) | 2012-08-09 |
CN101861675A (zh) | 2010-10-13 |
CN101861675B (zh) | 2013-03-27 |
EP2395588B1 (en) | 2015-03-25 |
EP2395588A4 (en) | 2013-11-06 |
US8338036B2 (en) | 2012-12-25 |
JP5152200B2 (ja) | 2013-02-27 |
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