All-solid-state battery manufacturing method and all-solid-state battery manufacturing device

Abstract

To provide an all-solid-state battery manufacturing method and an all-solid-state battery manufacturing device that can stabilize the amount of powder supplied to a substrate in an electrode laminate formation step.SOLUTION: A manufacturing method of an all-solid-state battery 1 includes a block formation step of solidifying a powder material to form a block B, an electrode laminate formation step of depositing the powder generated by removing and processing the block B on a first substrate F1 to form the electrode laminate 2, and a lamination step of laminating the electrode laminate 2 and a current collector 3.SELECTED DRAWING: Figure 8

Description

Technical Field

[0001] The present invention relates to a method for manufacturing an all-solid-state battery and an apparatus for manufacturing an all-solid-state battery.

Background Art

[0002] Conventionally, a method of forming a film of functional powder (powder film) using an electrostatic screen printing apparatus has been known (see Patent Document 1 below).

Prior Art Document

Patent Document

[0003]

Patent Document 1

Summary of the Invention

Problems to be Solved by the Invention

[0004] In an electrostatic screen printing apparatus as described in Patent Document 1, when the fluidity of the powder is low, the powder may be blocked before being supplied to the screen, or the screen may be clogged, resulting in an unstable supply amount of the powder to the substrate and a possibility of uneven film thickness (poor film thickness accuracy) in the powder film.

[0005] If the supply amount of the powder to the substrate becomes unstable, it may not be possible to obtain a powder layer having a desired thickness. Further, if there is uneven film thickness in the powder film, it may have an adverse effect on battery performance such as a decrease in charge / discharge efficiency and a decrease in lifespan.

[0006] The present invention provides a method for manufacturing an all-solid-state battery capable of stabilizing the amount of powder supplied onto a substrate in an electrode laminate forming step and forming a powder layer having a uniform film thickness, and an apparatus for manufacturing an all-solid-state battery.

Means for Solving the Problems

[0007] The present invention [1] includes a block forming step of solidifying a powder material to form a block, an electrode laminate forming step of depositing the powder generated by removing the block on a substrate to form an electrode laminate, and a lamination step of laminating the electrode laminate and a current collector, and includes a method for manufacturing an all-solid-state battery.

[0008] According to such a method, in the electrode laminate forming step, the block of the powder material is removed and the generated powder is deposited on the substrate.

[0009] Therefore, the influence of powder physical properties such as fluidity can be reduced, and the amount of powder supplied onto the substrate can be controlled according to the amount of block cut.

[0010] As a result, the amount of powder supplied onto the substrate can be stabilized, and a powder layer with a uniform film thickness can be formed.

[0011] The present invention [2] includes the method for manufacturing an all-solid-state battery according to [1] above, in which the powder material is pressure-molded in the block forming step.

[0012] According to such a method, the density of the block can be made uniform, the amount of powder supplied onto the substrate can be stabilized, and the film thickness of the powder layer can be made uniform.

[0013] The present invention [3] includes the method for manufacturing an all-solid-state battery according to [2] above, in which the powder material is pressure-molded by a vibration press in the block forming step.

[0014] According to such a method, the density of the block can be made more uniform, the amount of powder supplied onto the substrate can be made more stable, and the film thickness of the powder layer can be made more uniform.

[0015] The present invention [4] includes the method for manufacturing an all-solid-state battery according to [2] or [3] above, in which the powder material is pressure-molded at 100 MPa or less in the block forming step.

[0016] According to such a method, it is possible to suppress the block from becoming overly hard and solidified, and in the electrode laminate forming step, the block can be easily removed by machining.

[0017] The present invention [5] includes a method for manufacturing an all-solid-state battery according to any one of [1] to [4] above, in which the powder generated by removing the block in the electrode laminate forming step is moved onto the substrate by electrostatic force.

[0018] According to such a method, the powder generated by removing the block can be induced onto the substrate by electrostatic force.

[0019] The present invention [6] is a manufacturing apparatus used in the method for manufacturing an all-solid-state battery according to any one of [1] to [5] above, including a block support member that supports the block, a support base that is disposed apart from the block support member and supports the substrate, and a removal processing member that removes the block supported by the block support member.

[0020] According to such a configuration, it is possible to remove the block of the powder material and deposit the generated powder on the substrate.

[0021] Therefore, the amount of powder supplied onto the substrate can be controlled according to the amount of the block shaved.

[0022] As a result, the amount of powder supplied onto the substrate can be stabilized.

[0023] The present invention [7] includes the manufacturing apparatus for an all-solid-state battery according to [6] above, further including a pressing member that presses the block supported by the block support member toward the removal processing member.

[0024] According to such a configuration, the block can be stably brought into contact with the removal processing member.

[0025] The present invention [8] further includes a mask member disposed between the block support member and the base material and having an opening through which the powder generated by machining the block can pass, and includes the manufacturing apparatus for all-solid-state batteries of the above [6] or [7].

[0026] According to such a configuration, the powder can be deposited on the base material in a shape corresponding to the opening of the mask member.

[0027] The present invention [9] includes the manufacturing apparatus for all-solid-state batteries of any one of the above [6] to [8], wherein the block support member is fixed to the support table, and the machining member is slidable, rotatable or vibratable with respect to the block support member.

[0028] The present invention

[10] includes the manufacturing apparatus for all-solid-state batteries of any one of the above [6] to [8], wherein the machining member is fixed to the support table, and the block support member is slidable, rotatable or vibratable with respect to the machining member.

[0029] The present invention

[11] includes the manufacturing apparatus for all-solid-state batteries of any one of the above [6] to

[10] , wherein the manufacturing apparatus includes a plurality of the machining members having different shapes from each other.

[0030] According to such a configuration, by switching a plurality of machining members, the speed of cutting the block and the uniformity of the thickness of the powder layer can be optimized.

[0031] The present invention

[12] further includes a measuring member for measuring the thickness of the block supported by the block support member, and includes the manufacturing apparatus for all-solid-state batteries of any one of the above [6] to

[11] .

[0032] According to such a configuration, by measuring the thickness of the block supported by the block support member, the amount of the block cut can be calculated.

[0033] Furthermore, the amount of deposited powder and the thickness of the powder layer can be calculated from the amount of the removed block.

[0034] The present invention

[13] includes a manufacturing apparatus for an all-solid-state battery according to any one of [6] to

[12] above, wherein the support table is slidable or rotatable while supporting the base material.

[0035] According to such a configuration, by sliding or rotating the support table while supporting the base material, powder can be deposited on the base material over a large area.

Advantages of the Invention

[0036] According to the method for manufacturing an all-solid-state battery and the manufacturing apparatus for an all-solid-state battery of the present invention, the amount of powder supplied onto the base material in the electrode laminate forming step can be stabilized, and a powder layer with a uniform film thickness can be formed.

Brief Description of the Drawings

[0037]

Figure 1

Figure 2

Figure 3

Figure 4

Figure 5

Figure 6

Figure 7

Figure 8

Figure 9

Figure 10

Figure 11

MODE FOR CARRYING OUT THE INVENTION

[0038] 1. All-solid-state battery An example of the all-solid-state battery 1 will be described. Note that the shape of the all-solid-state battery 1 is not limited as long as it is an all-solid-state battery manufactured according to the present invention [1].

[0039] As shown in FIGS. 1A and 1B, the all-solid-state battery 1 includes a plurality of electrode laminates 2, a plurality of current collectors 3, a positive electrode lead 4, a negative electrode lead 5, and an exterior member 6.

[0040] (1) Electrode laminate In the present embodiment, the electrode laminate 2 has a sheet shape. The electrode laminate 2 is substantially rectangular when viewed from the thickness direction of the electrode laminate 2. Note that the shape of the electrode laminate 2 is not limited. The electrode laminate 2 may have a plate shape or a film shape. Also, the electrode laminate 2 may be substantially circular when viewed from the thickness direction of the electrode laminate 2.

[0041] The thickness of the electrode laminate 2 is, for example, 100 μm or more, preferably 200 μm or more, and, for example, 1000 μm or less, preferably 800 μm or less.

[0042] As shown in FIG. 2A, the electrode laminate 2 includes a positive electrode layer 21, a negative electrode layer 22, and a solid electrolyte layer 23. The electrode laminate 2 is composed of the positive electrode layer 21, the negative electrode layer 22, and the solid electrolyte layer 23. The electrode laminate 2 has the solid electrolyte layer 23 between the positive electrode layer 21 and the negative electrode layer 22.

[0043] (1-1) Positive electrode layer The positive electrode layer 21 is arranged away from the negative electrode layer 22 in the thickness direction of the electrode laminate 2. The positive electrode layer 21 is arranged on the opposite side of the negative electrode layer 22 with respect to the solid electrolyte layer 23 in the thickness direction of the electrode laminate 2. The positive electrode layer 21 contacts the solid electrolyte layer 23 and does not contact the negative electrode layer 22.

[0044] The positive electrode layer 21 is made of a powder containing a positive electrode active material. The positive electrode layer 21 may contain a resin such as a binder. In the present embodiment, the positive electrode layer 21 is made of a mixture (positive electrode composite material) of a powder of a positive electrode active material and a powder of a solid electrolyte. The positive electrode layer 21 may contain a conductive assistant. Note that the positive electrode layer 21 does not necessarily contain a solid electrolyte. The positive electrode layer 21 may consist only of a positive electrode active material.

[0045] Examples of the positive electrode active material include lithium-containing oxides. Examples of the lithium-containing oxides include lithium-nickel composite oxides (LiNi X M 1-X O2), lithium cobalt oxide (LiCoO2), lithium nickel oxide (LiNiO2), lithium-nickel-cobalt-aluminum composite oxides (LiNi 0.8 Co 0.15 Al 0.05 O2, NCA-based layered oxides), lithium manganese oxide (spinel-type lithium manganese oxide (LiMn2O4)), and Li-excess composite oxides (Li2MnO3-LiMO2).

[0046] The cathode active material is not limited to lithium-containing oxides as long as insertion and extraction of lithium ions are possible. Examples of the cathode active material include olivine-based compounds (LiMPO4) and sulfur-containing compounds (Li2S).

[0047] In the above chemical formula, M represents a transition metal.

[0048] From the viewpoint of easily obtaining high capacity, the cathode active material preferably includes a lithium-containing oxide containing at least one selected from the group consisting of Co, Ni, and Mn.

[0049] Also, from the viewpoint of improving rate characteristics, the surface of the cathode active material may be coated with a coating material.

[0050] Examples of the coating material include Li4Ti5O 12 , LiTaO3, Li4NbO3, LiAlO2, Li2ZrO3, Li2WO4, Li2TiO3, Li2B4O7, Li3PO4, Li2MoO4, LiBO2, alumina (Al2O3), and carbon (C).

[0051] The cathode active material can be used alone or in combination of two or more.

[0052] The solid electrolyte exhibits lithium ion conductivity. Examples of the solid electrolyte include organic solid electrolytes and inorganic solid electrolytes.

[0053] Examples of the inorganic solid electrolyte include sulfides, oxides, nitrides, and hydrides.

[0054] Examples of the sulfide include those containing Li2S and another sulfide containing at least one element selected from the group consisting of Group 13 elements, Group 14 elements, and Group 15 elements of the periodic table.

[0055] Examples of Group 13 elements, Group 14 elements, and Group 15 elements of the periodic table include P, Si, Ge, As, Sb, and Al. Preferably, P, Si, and Ge are included. More preferably, P is included.

[0056] Specifically, examples of sulfides include Li2S-SiS2, Li2S-P2S5, Li2S-GeS2, Li2S-B2S3, Li2S-Ga2S3, Li2S-Al2S3, Li2S-GeS2-P2S5, Li2S-Al2S3-P2S5, Li2S-P2S3, Li2S-P2S3-P2S5, LiX-Li2S-P2S5, LiX-Li2S-SiS2, and LiX-Li2S-B2S3 (X: I, Br, or Cl).

[0057] As the solid electrolyte, preferably, an inorganic solid electrolyte is included. More preferably, a sulfide is included. The solid electrolyte can be used alone or in combination of two or more. The ratio of the positive electrode active material to the solid electrolyte is not limited.

[0058] The thickness of the positive electrode layer 21 is, for example, 50 μm or more, preferably 100 μm or more. The thickness of the positive electrode layer 21 is, for example, 500 μm or less, preferably 300 μm or less.

[0059] (1-2) Negative electrode layer The negative electrode layer 22 is disposed away from the positive electrode layer 21 in the thickness direction of the electrode laminate 2. The negative electrode layer 22 is disposed on the opposite side of the positive electrode layer 21 with respect to the solid electrolyte layer 23 in the thickness direction of the electrode laminate 2. The negative electrode layer 22 is in contact with the solid electrolyte layer 23 and not in contact with the positive electrode layer 21.

[0060] The negative electrode layer 22 is made of a powder containing a negative electrode active material. The negative electrode layer 22 may contain a resin such as a binder. In the present embodiment, the negative electrode layer 22 is made of a mixture (negative electrode composite material) of a powder of a negative electrode active material and a powder of a solid electrolyte. The negative electrode layer 22 may contain a conductive assistant. Note that the negative electrode layer 22 does not necessarily contain a solid electrolyte. The negative electrode layer 22 may consist only of a negative electrode active material.

[0061] The negative electrode active material is not limited as long as it is a material capable of inserting and extracting lithium ions. Examples of the negative electrode active material include carbon materials, metals and their alloys, semimetals, and compounds of metals or semimetals.

[0062] Examples of the carbon material include graphite (natural graphite, artificial graphite), hard carbon, and amorphous carbon. Examples of the metal and its alloy include lithium and its alloy. Examples of the semimetal include silicon. Examples of the compound of the metal or semimetal include oxides, sulfides, nitrides, hydrides, and silicides (lithium silicide) of the metal or semimetal. Examples of the oxide of the metal or semimetal include titanium oxide and silicon oxide.

[0063] The negative electrode active material can be used alone or in combination of two or more. For example, silicon oxide and a carbon material can be used in combination as the negative electrode active material.

[0064] Examples of the solid electrolyte contained in the negative electrode layer 22 include the above-mentioned solid electrolytes. Preferably, the solid electrolyte contained in the negative electrode layer 22 is the same as the solid electrolyte contained in the positive electrode layer 21. The ratio of the negative electrode active material to the solid electrolyte is not limited.

[0065] The thickness of the negative electrode layer 22 is substantially the same as the thickness of the positive electrode layer 21. The thickness of the negative electrode layer 22 is, for example, 50 μm or more, preferably 100 μm or more. The thickness of the negative electrode layer 22 is, for example, 500 μm or less, preferably 300 μm or less.

[0066] (1-3) Solid electrolyte layer The solid electrolyte layer 23 is disposed between the positive electrode layer 21 and the negative electrode layer 22 in the thickness direction of the electrode laminate 2. The solid electrolyte layer 23 is made from a powder of the solid electrolyte. The solid electrolyte layer 23 may contain a resin such as a binder.

[0067] Examples of the solid electrolyte include the above-described solid electrolyte. Preferably, the solid electrolyte is the same as the solid electrolyte contained in the positive electrode layer 21.

[0068] The solid electrolyte layer 23 is thinner than the positive electrode layer 21 and the negative electrode layer 22. The thickness of the solid electrolyte layer 23 is, for example, 10 μm or more, preferably 30 μm or more. The thickness of the solid electrolyte layer 23 is, for example, 300 μm or less, preferably 100 μm or less.

[0069] (2) Current collector As shown in FIG. 2B, in the case of parallel connection, each of the plurality of current collectors 3 is alternately laminated with each of the plurality of electrode laminate bodies 2. The plurality of current collectors 3 includes a positive electrode current collector 3A and a negative electrode current collector 3B. The positive electrode current collector 3A is in contact with the positive electrode layer 21 of the electrode laminate body 2. The negative electrode current collector 3B is in contact with the negative electrode layer 22 of the electrode laminate body 2.

[0070] Specifically, in the present embodiment, in the lamination direction of the electrode laminate body 2 and the current collector 3, from one side to the other side, the positive electrode current collector 3A, the first electrode laminate body 2A, the negative electrode current collector 3B, the second electrode laminate body 2B, and the positive electrode current collector 3A are laminated in this order. In the lamination direction, one negative electrode current collector 3B is disposed between the negative electrode layer 22 of the first electrode laminate body 2A and the negative electrode layer 22 of the second electrode laminate body 2B. That is, in the lamination direction, one current collector 3 is disposed between two electrode laminate bodies 2. In the case of series connection, the plurality of electrode laminate bodies 2 are stacked so that the lamination order of the positive electrode layer 21, the solid electrolyte layer 23, and the negative electrode layer 22 is the same, and the current collector 3 is disposed only on the uppermost layer and the lowermost layer.

[0071] As shown in FIGS. 3A and 3B, the current collector 3 includes a conductor 31, an insulating member 32, and an adhesive layer 33.

[0072] (2-1) Conductor The conductor 31 is made of, for example, metal. The conductor 31 has a laminated portion 311 and a tab 312.

[0073] The laminated portion 311 extends in the first direction and the second direction. The first direction is orthogonal to the lamination direction. The second direction is orthogonal to both the first direction and the lamination direction. The laminated portion 311 has a sheet shape. The laminated portion 311 has one surface S1 and the other surface S2 in the thickness direction. In other words, the conductor 31 has one surface S1 and the other surface S2 in the thickness direction. The laminated portion 311 is in contact with the electrode laminate 2. When the current collector 3 is the positive current collector 3A, the laminated portion 311 is in contact with the positive electrode layer 21 of the electrode laminate 2. When the current collector 3 is the negative current collector 3B, the laminated portion 311 is in contact with the negative electrode layer 22 of the electrode laminate 2.

[0074] The tab 312 is disposed at the edge of the laminated portion 311. In the present embodiment, the tab 312 is disposed at one edge of the laminated portion 311 in the second direction. The tab 312 protrudes from the edge of the laminated portion 311. The tab 312 is a member different from the laminated portion 311 and may be joined to the laminated portion 311. The tab 312 has a belt shape. The tab 312 does not contact the electrode laminate 2. When the current collector 3 is the positive current collector 3A, the conductor 31 has the positive tab 312A as the tab 312. When the current collector 3 is the negative current collector 3B, the conductor 31 has the negative tab 312B as the tab 312. In a state where the electrode laminate 2, the positive current collector 3A, and the negative current collector 3B are laminated, the negative tab 312B is disposed away from the positive tab 312A. In the lamination direction, in a state where the electrode laminate 2, the positive current collector 3A, and the negative current collector 3B are laminated, the negative tab 312B does not overlap the positive tab 312A.

[0075] The thickness of the conductor 31 is, for example, 1 μm or more, preferably 5 μm or more, and, for example, 100 μm or less, preferably 50 μm or less.

[0076] Examples of the material of the conductor 31 include copper (Cu), magnesium (Mg), stainless steel, titanium (Ti), iron (Fe), cobalt (Co), nickel (Ni), zinc (Zn), aluminum (Al), germanium (Ge), indium (In), lithium (Li), tin (Sn), and alloys thereof.

[0077] (2-2) Insulating member As shown in FIG. 3B, the insulating member 32 is laminated on one surface S1 of the conductor 31. As shown in FIG. 3A, the insulating member 32 is disposed on the laminated portion 311 of the conductor 31. The insulating member 32 is laminated on the peripheral edge of the laminated portion 311 of the conductor 31. The insulating member 32 has a substantially rectangular frame shape when viewed from the lamination direction. The insulating member 32 is not disposed on the tab 312 of the conductor 31.

[0078] In a state where the electrode laminate 2, the positive current collector 3A, and the negative current collector 3B are laminated, the insulating member 32 is disposed around the electrode laminate 2. As shown in FIG. 1B, in a state where the electrode laminate 2, the positive current collector 3A, and the negative current collector 3B are laminated, the insulating member 32 is disposed between the positive current collector 3A and the negative current collector 3B in the lamination direction. In a state where the electrode laminate 2, the positive current collector 3A, and the negative current collector 3B are laminated, the insulating member 32 insulates the positive current collector 3A from the negative current collector 3B.

[0079] In the lamination direction, the thickness of the insulating member 32 is thinner than the thickness of the electrode laminate 2. When the current collector 3 does not have the adhesive layer 33, the thickness of the insulating member 32 may be the same as the thickness of the electrode laminate 2. The thickness of the insulating member 32 is, for example, 50 μm or more, preferably 75 μm or more, and, for example, 500 μm or less, preferably 400 μm or less.

[0080] Examples of the material of the insulating member 32 include polyethylene terephthalate and polyimide.

[0081] (2-3) Adhesive layer As shown in FIG. 3B, the adhesive layer 33 is laminated on the other surface S2 of the conductor 31 at the peripheral edge of the conductor 31. The current collector 3 may not have the adhesive layer 33. As shown in FIG. 1B, in a state where one electrode laminate 2 is laminated between two current collectors 3, the adhesive layer 33 of the current collector 3 disposed on the other side of the electrode laminate 2 in the lamination direction is adhered to the insulating member 32 of the current collector 3 disposed on one side of the electrode laminate 2 in the lamination direction.

[0082] The sum of the thickness of the adhesive layer 33 and the thickness of the insulating member 32 is equal to or less than the thickness of the electrode laminate 2. The thickness of the adhesive layer 33 is, for example, 30 μm or more, preferably 50 μm or more, and, for example, 300 μm or less, preferably 200 μm or less.

[0083] The adhesive layer 33 is preferably insulating. Examples of the material of the adhesive layer 33 include resins such as acrylic, polyimide, and silicone, and non-woven fabrics impregnated with these resins.

[0084] (3) Positive electrode lead and negative electrode lead As shown in FIG. 1A, a part of the positive electrode lead 4 is exposed from the exterior member 6. As shown in FIG. 4, the positive electrode lead 4 is joined to the positive electrode tab 312A within the exterior member 6. Thereby, the positive electrode lead 4 is electrically connected to the positive electrode current collector 3A. The positive electrode lead 4 is not connected to the negative electrode current collector 3B.

[0085] As shown in FIG. 1A, a part of the negative electrode lead 5 is exposed from the exterior member 6. The negative electrode lead 5 is joined to the negative electrode tab 312B (see FIG. 3A) within the exterior member 6. Thereby, the negative electrode lead 5 is electrically connected to the negative electrode current collector 3B (see FIG. 1B). The negative electrode lead 5 is not connected to the positive electrode current collector 3A.

[0086] Each of the positive electrode lead 4 and the negative electrode lead 5 has, for example, a substantially rectangular flat plate shape. Examples of the material of the positive electrode lead 4 and the negative electrode lead 5 include pure metals and alloys. Examples of the pure metal include copper, nickel, aluminum, gold, and platinum. Examples of the alloy include alloys of the above pure metals, stainless steel, and titanium. The positive electrode lead 4 and the negative electrode lead 5 may be plated. For example, the positive electrode lead 4 and the negative electrode lead 5 may be copper plates having a nickel plating layer and a gold plating layer.

[0087] (4) Exterior member As shown in FIGS. 1A and 1B, the exterior material 6 covers the laminate of the electrode laminate 2 and the current collector 3. Examples of the exterior material 6 include a metal laminate film in which resin films are laminated on both sides of a metal foil.

[0088] 2. Method for manufacturing all-solid-state battery Next, a method for manufacturing the above-described all-solid-state battery 1 will be described.

[0089] The method for manufacturing the all-solid-state battery 1 includes a block forming step, an electrode laminate forming step (see FIGS. 5A to 6A), a pressing step (see FIG. 6B), a cutting step, a peeling step (see FIG. 6C), and a lamination step.

[0090] (1) Block forming step In the block forming step, a powder material is solidified to form a block. Examples of the powder material include a powder of a solid electrolyte, a positive electrode composite material, and a negative electrode composite material.

[0091] In the block forming step, the powder material is preferably solidified by a dry method. Specifically, in the block forming step, the powder material is pressure-molded. Alternatively, a solvent in which the powder material is dispersed is poured into a mold and dried to remove the solvent to solidify it, or the powder material packed in a mold is baked and solidified (sintered).

[0092] Examples of the pressure molding method include a uniaxial molding method, a biaxial molding method, and a cold isostatic pressing method (CIP pressing method). Preferably, the biaxial molding method is used as the pressure molding method.

[0093] Examples of the pressing method include a mechanical press, a hydraulic press, and a vibration press. Preferably, the vibration press is used as the pressing method.

[0094] In the block forming step, the powder material is preferably pressure-molded by a vibration press for biaxial molding. When using a vibration press for biaxial molding, it is possible to suppress non-uniform density of the obtained block.

[0095] The pressure in the pressure forming is, for example, 100 MPa or less, preferably 50 MPa or less, more preferably 20 MPa or less. Further, the pressure in the pressure forming is, for example, 1 MPa or more, preferably 5 MPa or more. The range of the pressure in the pressure forming may be 1 MPa to 100 MPa, 5 MPa to 50 MPa, or 5 MPa to 20 MPa.

[0096] When the pressure in the pressure forming is equal to or less than the above upper limit value, it is possible to suppress the block from becoming overly hard and solidifying, and in the electrode laminate forming step, the block of the powder material can be easily removed by machining. When the pressure in the pressure forming is equal to or more than the above lower limit value, it is possible to suppress the block from easily collapsing, and the handleability of the block can be ensured.

[0097] (2) Electrode laminate forming step As shown in FIGS. 5A to 6A, in the electrode laminate forming step, the powder generated by removing the block obtained in the block forming step is preferably deposited on the first base material F1 in a dry manner to form the electrode laminate 2.

[0098] Specifically, as shown in FIG. 5A, the powder P1 generated by removing the block of the positive electrode composite material is deposited on the first base material F1 to form the positive electrode layer 21 on the first base material F1. Examples of the removal process include cutting, grinding, and polishing. In addition, the removal process is not limited to grinding and cutting, and any process that generates powder by removing the block is not limited.

[0099] In the electrode laminate forming step, the powder P1 generated by removing the block may be moved onto the first base material F1 by electrostatic force.

[0100] Next, as shown in FIG. 5B, the powder P2 generated by removing the block of the solid electrolyte is deposited on the positive electrode layer 21 to form the solid electrolyte layer 23 on the positive electrode layer 21.

[0101] Next, the powder generated by removing the block of the negative electrode composite material is deposited on the solid electrolyte layer 23, and a negative electrode layer 22 (see FIG. 6A) is formed on the solid electrolyte layer 23.

[0102] Thereby, as shown in FIG. 6A, the electrode laminate 2 is formed on the first base material F1.

[0103] The material of the first base material F1 is not limited. Examples of the material of the first base material F1 include a metal foil. Examples of the metal foil include an aluminum foil.

[0104] Also, as long as the electrode laminate 2 can be formed, the formation order of the positive electrode layer 21, the negative electrode layer 22, and the solid electrolyte layer 23 is not limited. The negative electrode layer 22 may be formed on the first base material F1, the solid electrolyte layer 23 may be formed on the negative electrode layer 22, and the positive electrode layer 21 may be formed on the solid electrolyte layer 23.

[0105] (2) Pressing step The pressing step is carried out after the electrode laminate forming step. As shown in FIG. 6B, in the pressing step, the second base material F2 is laminated on the electrode laminate 2, and the obtained laminate L is pressed. The obtained laminate L is a laminate of the first base material F1, the electrode laminate 2, and the second base material F2.

[0106] The material of the second base material F2 may be the same as or different from the material of the first base material F1.

[0107] The pressure applied to the laminate L is not limited as long as the electrode laminate 2 can be formed. The pressure applied to the laminate L is, for example, 100 MPa or more, preferably 500 MPa or more, and for example, 5000 MPa or less, preferably 3000 MPa or less. Note that the laminate L may be charged and discharged for performance confirmation after the pressing step.

[0108] (3) Cutting step The cutting process is carried out after the pressing process. In the cutting process, the electrode laminate 2 is cut into a desired shape. In the present embodiment, the electrode laminate 2 is cut into a substantially rectangular shape as viewed from the thickness direction of the electrode laminate 2. Note that the cutting process may not be carried out.

[0109] (4) Peeling process The peeling process is carried out after the cutting process. Note that the peeling process may be carried out before the cutting process. In the peeling process, as shown in FIG. 6C, at least one of the first base material F1 and the second base material F2 is peeled off from the electrode laminate 2. In the present embodiment, both the first base material F1 and the second base material F2 are peeled off from the electrode laminate 2. Note that, in order to prevent the electrode laminate 2 from collapsing, only one of the first base material F1 and the second base material F2 may be peeled off from the electrode laminate 2. Note that the peeling process may not be carried out. In that case, in the laminating process, the first base material F1 and the second base material F2 may be used as the current collector 3.

[0110] (5) Laminating process In the laminating process, as shown in FIG. 1B, the electrode laminate 2 and the current collector 3 (see FIG. 3B) are alternately laminated. By laminating each of the electrode laminate 2 and the current collector 3 in a desired number, the laminating process is completed.

[0111] After the laminating process, as shown in FIG. 4, the positive electrode tab 312A is joined to the positive electrode lead 4, and the negative electrode tab 312B is joined to the negative electrode lead 5, and the laminate of the electrode laminate 2 and the current collector 3 is vacuum-packed with the exterior material 6.

[0112] Thus, the manufacturing of the above-described all-solid-state battery 1 is completed.

[0113] 3. Manufacturing apparatus for all-solid-state battery Next, with reference to FIGS. 7 and 8, the manufacturing apparatus 10 used in the electrode laminate forming process of the manufacturing method of the above-described all-solid-state battery 1 will be described.

[0114] The manufacturing apparatus 10 includes a block support member 11, a support base 12 (see FIG. 8), a removal processing member 13, a pressing member 14, and a mask member 15 (see FIG. 8).

[0115] (1) Block support member As shown in FIG. 8, the block support member 11 supports the block B. In the present embodiment, the block support member 11 has a cylindrical shape capable of accommodating the block B. The block support member 11 extends in the vertical direction. The block support member 11 has an inlet 111 and an outlet 112. The inlet 111 is disposed at the upper end of the block support member 11. The block B is set into the block support member 11 through the inlet 111. The outlet 112 is disposed at the lower end of the block support member 11. The block B within the block support member 11 faces the removal processing member 13 through the outlet 112. Note that the shape of the block support member 11 is not limited as long as the block B can be positioned with respect to the removal processing member 13. In the present embodiment, the block support member 11 is fixed to the support base 12.

[0116] (2) Support base As shown in FIG. 8, the support base 12 is disposed apart from the block support member 11 in the vertical direction. The support base 12 supports the first base material F1. The support base 12 is made of metal. A predetermined voltage is applied to the support base 12.

[0117] (3) Removal processing member As shown in FIG. 8, the removal processing member 13 faces the outlet 112 of the block support member 11. The removal processing member 13 is disposed between the block support member 11 and the support base 12 in the vertical direction. With the block B set in the block support member 11 and the first base material F1 set on the support base 12, the removal processing member 13 is disposed between the block B and the first base material F1 in the vertical direction. The removal processing member 13 is movable horizontally or vibratable with respect to the block support member 11. The horizontal movement may be a slide (linear movement) or a rotation. That is, the removal processing member 13 is slidable, rotatable or vibratable with respect to the block support member 11. The direction in which the removal processing member 13 slides is defined as the slide direction. With the block B set in the block support member 11, the removal processing member 13 contacts the block B. With the block B in the block support member 11 in contact with the removal processing member 13, when the removal processing member 13 moves with respect to the block support member 11, the removal processing member 13 processes the block B supported by the block support member 11. A predetermined voltage is applied to the removal processing member 13 so that an electric field is generated between the removal processing member 13 and the support base 12. Examples of the removal processing member 13 include a cutting member, a grinding member, and a polishing member.

[0118] In the present embodiment, as shown in FIG. 7, the removal processing member 13 has a frame 131 and a mesh 132.

[0119] The frame 131 has a substantially rectangular flat plate shape. The frame 131 is made of metal. The frame 131 has an opening 130.

[0120] In this embodiment, the mesh 132 is a metal mesh. The mesh 132 covers the opening 130 of the frame 131. With the block B in the block support member 11 in contact with the mesh 132, as the removal member 13 moves relative to the block support member 11, the mesh 132 removes the block B supported by the block support member 11. As shown in FIG. 8, the powder generated by removing the block B is deposited on the first substrate F1 through the mesh of the mesh 132.

[0121] (4) Pressing member The pressing member 14 is disposed on the side opposite to the removal member 13 with respect to the block B. The pressing member 14 presses the block B supported by the block support member 11 toward the removal member 13. In this embodiment, the pressing member 14 is a metal weight. As long as the block B can be pressed toward the removal member 13, the pressing member 14 is not limited. The pressing member 14 does not have to be a weight. The pressing member 14 may be a piston pressed against the block B by an air cylinder.

[0122] (5) Mask member The mask member 15 is disposed between the block support member 11 and the first substrate F1 if necessary. The mask member 15 is disposed between the removal member 13 and the first substrate F1. The mask member 15 has an opening 150. The powder generated by removing the block B can pass through the opening 150. The opening 150 is smaller than the opening 130 of the frame 131 of the removal member 13. The shape of the opening 150 is not limited as long as the desired-shaped electrode laminate 2 can be obtained. In this embodiment, the shape of the opening 150 is rectangular so that a rectangular electrode laminate 2 can be obtained.

[0123] 4. Operational effects (1) According to the method for manufacturing the all-solid-state battery 1 and the manufacturing apparatus 10 for the all-solid-state battery 1, as shown in FIG. 8, in the block formation step, the density of the powder material is made uniform, and in the electrode laminate formation step, the block B of the powder material is removed, and the generated powder is deposited on the first substrate F1.

[0124] Therefore, the influence of powder physical properties such as fluidity can be reduced, and the amount of powder supplied onto the first substrate F1 can be controlled according to the amount of the block B to be scraped off.

[0125] As a result, the amount of powder supplied onto the first substrate F1 can be stabilized, and a powder layer (positive electrode layer 21, negative electrode layer 22, or solid electrolyte layer 23) with a uniform film thickness can be formed.

[0126] (2) In the method for manufacturing the all-solid-state battery 1, in the block forming step, the powder material is pressure-molded.

[0127] Thereby, the density of the block B can be made uniform, the amount of powder supplied onto the first substrate F1 can be stabilized, and the film thickness of the powder layer can be made uniform.

[0128] (3) According to the method for manufacturing the all-solid-state battery 1, in the block forming step, the powder material is pressure-molded by a vibration press.

[0129] Thereby, the density of the block B can be made more uniform, the amount of powder supplied onto the first substrate F1 can be made more stable, and the film thickness of the powder layer can be made more uniform.

[0130] (4) According to the method for manufacturing the all-solid-state battery 1, in the block forming step, the powder material is pressure-molded at 100 MPa or less.

[0131] Thereby, it is possible to prevent the block B from becoming overly hard and solidified, and in the electrode laminate forming step, the block B can be easily removed by machining.

[0132] (5) According to the method for manufacturing the all-solid-state battery 1 and the manufacturing apparatus 10 for the all-solid-state battery 1, in the electrode laminate forming step, the powder generated by removing the block B is moved onto the first substrate F1 by electrostatic force.

[0133] As a result, the powder generated by machining the block B can be induced onto the first substrate F1 by electrostatic force.

[0134] (6) According to the manufacturing apparatus 10 of the all-solid-state battery 1, as shown in FIG. 8, the block B supported by the block support member 11 can be pressed by the pressing member 14 toward the machining member 13.

[0135] Therefore, the block B can be stably brought into contact with the machining member 13.

[0136] (7) According to the manufacturing apparatus 10 of the all-solid-state battery 1, as shown in FIG. 8, the mask member 15 is disposed between the block support member 11 and the first substrate F1.

[0137] Therefore, the powder can be deposited on the first substrate F1 in a shape corresponding to the opening 15 of the mask member 15.

[0138] 5. Modification Hereinafter, the modification will be described. In the modification, the same members as those in the above-described embodiment are denoted by the same reference numerals, and the description thereof will be omitted.

[0139] (1) The support base 12 may be horizontally movable together with the mask member 15 while supporting the first substrate F1. The horizontal movement may be a slide (linear movement) or a rotation.

[0140] According to this modification, by horizontally moving the support base 12 while supporting the first substrate F1, the powder can be deposited on the first substrate F1 over a large area.

[0141] (2) In the above-described embodiment, the block support member 11 is fixed to the support base 12, and the machining member 13 slides, rotates, or vibrates with respect to the block support member 11. In this regard, the machining member 13 may be fixed to the support base 12, and the block support member 11 may be slidable, rotatable, or vibratable with respect to the machining member 13.

[0142] Even in this modified example, the same operational effects as those of the above-described embodiment can be obtained.

[0143] (3) The structure of the removal processing member 13 is not limited as long as the block B can be removed by processing.

[0144] For example, as shown in FIG. 9, the removal processing member 13 may include a frame 161 having a slit 160 and a blade 162. The slit 160 extends in a direction intersecting the sliding direction of the removal processing member 13. The blade 162 is attached to the edge of the slit 160. The blade 162 extends in a direction intersecting the sliding direction of the removal processing member 13. In this modified example, the powder cut out from the block B by the blade 162 accumulates on the first base material F1 through the slit.

[0145] Also, for example, as shown in FIGS. 10A and 10B, the removal member 13 may include a base frame 170, a support plate 171, a blade 172, and a spacer 173. That is, the removal member 13 may have a blade 172 instead of the mesh 132. The base frame 170 has a frame shape. The support plate 171 is attached to one half of the base frame 170 in the sliding direction of the removal member 13. The support plate 171 supports the block B (see FIG. 10B). The blade 172 is disposed at a distance from the support plate 171 in the sliding direction of the removal member 13. The blade 172 is attached to the other half of the base frame 170 in the sliding direction of the removal member 13. The blade 172 extends in a direction intersecting the sliding direction of the removal member 13. The spacer 173 is disposed between the blade 172 and the base frame 170 in the vertical direction. The spacer 173 positions the cutting edge of the blade 172 above the upper surface of the support plate 171. Thus, as shown in FIG. 10B, when the removal member 13 is slid with the block B in contact with the upper surface of the support plate 171, the cutting edge of the blade 172 can shave the block B. In this modification, the thickness of the spacer 173 can adjust the vertical distance between the cutting edge of the blade 172 and the upper surface of the support plate 171. By adjusting the vertical distance between the cutting edge of the blade 172 and the upper surface of the support plate 171, the shaving amount can be adjusted. Note that if the vertical distance between the cutting edge of the blade 172 and the upper surface of the support plate 171 can be adjusted, the removal member 13 may not have the spacer 173. For example, the shaving amount may be adjusted by the difference between the thickness of the support plate 171 and the thickness of the blade 172, or the shaving amount may be adjusted by adjusting the angle of the blade 172 with respect to the support plate 171.

[0146] As shown in FIG. 11, the removal processing member 13 may have a punching metal 180 instead of the mesh 132. The punching metal 180 includes a plurality of through holes 181 and a plurality of blades 182 disposed around each through hole 181. In this modification, the powder cut out from the block B by the blade 182 accumulates on the first base material F1 through the through holes 181.

[0147] (4) The manufacturing apparatus 10 may include a plurality of removal processing members 13 having different shapes from each other. As the plurality of removal processing members 13, for example, the removal processing member 13 having the above-described mesh 132 (see FIG. 7), the removal processing member 13 having the above-described blade 162 or blade 172 (see FIGS. 9 and 10A), and the removal processing member 13 having the above-described punching metal 180 (see FIG. 11) can be mentioned. Further, the removal processing member 13 having a plurality of meshes 132 with different openings or linear shapes may be used, or the removal processing member 13 having a plurality of blades with different blade angles may be used.

[0148] According to this modification, by switching the plurality of removal processing members 13, the speed of cutting the block and the uniformity of the thickness of the powder layer can be optimized.

[0149] (5) The manufacturing apparatus 10 may further include a measuring member for measuring the thickness of the block B supported by the block support member 11. The measuring member is not limited. The measuring member may be, for example, a scale provided on the inner surface of the block support member 11, or a sensor for measuring the stroke amount of the air cylinder used for the pressing member 14.

[0150] According to this modification, by measuring the thickness of the block B supported by the block support member 11, the amount of the block B that has been cut can be calculated.

[0151] Furthermore, from the amount of the block B that has been cut, the amount of the deposited powder and the thickness of the powder layer can be calculated.

[0152] (6) The positive electrode layer 21, the negative electrode layer 22, and the solid electrolyte layer 23 may be formed by different methods. For example, on the positive electrode layer 21 formed by electrostatic screen printing, the powder generated by removing the block B of the solid electrolyte is laminated to form the solid electrolyte layer 23, and the negative electrode layer 22 may be formed by electrostatic screen printing on the solid electrolyte layer 23.

[0153] Alternatively, the positive electrode layer 21 is coated on the first base material F1 by a coater or the like, the powder generated by removing the block B of the solid electrolyte is laminated on the positive electrode layer 21 to form the solid electrolyte layer 23, and the one in which the negative electrode layer 22 is coated on the second base material F2 by a coater or the like may be disposed on the solid electrolyte layer 23.

[0154] Alternatively, the powder generated by removing the block B of the positive electrode composite material is laminated to form the positive electrode layer 21, the powder generated by removing the block B of the solid electrolyte is laminated on the positive electrode layer 21 to form the solid electrolyte layer 23, and a sheet of silicone or lithium metal may be disposed as the negative electrode layer 22 on the solid electrolyte layer 23.

[0155] (7) In the block forming step, the powder material may be aggregated to form the first granule, and the first granule may be solidified to form a block. Further, in the block forming step, the first granule formed by aggregating the powder material may be crushed to form a second granule smaller than the first granule, and the second granule may be solidified to form a block.

Explanation of Reference Numerals

[0156] 1 All-solid-state battery 2 Electrode laminate 3 Current collector 10 Manufacturing apparatus 11 Block support member 12 Support base 13 Removal processing member 14 Pressing member 15 Mask member

Claims

1. A block forming step of solidifying a powder material to form a block, An electrode laminate forming step of depositing the powder generated by removing the block on a substrate to form an electrode laminate, A lamination step of laminating the electrode laminate and a current collector, A method for manufacturing an all-solid-state battery, comprising:

2. The method for manufacturing an all-solid-state battery according to claim 1, wherein in the block forming step, the powder material is pressure-molded.

3. The method for manufacturing an all-solid-state battery according to claim 2, wherein in the block forming step, the powder material is pressure-molded by a vibration press.

4. The method for manufacturing an all-solid-state battery according to claim 2, wherein in the block forming step, the powder material is pressure-molded at 100 MPa or less.

5. The method for manufacturing an all-solid-state battery according to claim 1, wherein in the electrode laminate forming step, the powder generated by removing the block is moved onto the substrate by electrostatic force.

6. A manufacturing apparatus used in the method for manufacturing an all-solid-state battery according to any one of claims 1 to 5, A block support member for supporting the block, A support base arranged away from the block support member and supporting the substrate, A machining member for removing the block supported by the block support member, A manufacturing apparatus for an all-solid-state battery, comprising:

7. The manufacturing apparatus for an all-solid-state battery according to claim 6, further comprising a pressing member for pressing the block supported by the block support member toward the machining member.

8. The manufacturing apparatus for an all-solid-state battery according to claim 6, further comprising a mask member arranged between the block support member and the substrate and having an opening through which the powder generated by removing the block can pass.

9. The block support member is fixed to the support base, The machining member is slidable, rotatable or vibratable with respect to the block support member. The manufacturing apparatus for an all-solid-state battery according to claim 6.

10. The machining member is fixed to the support base, The block support member is slidable, rotatable or vibratable with respect to the machining member. The manufacturing apparatus for an all-solid-state battery according to claim 6.

11. The manufacturing apparatus according to claim 6, comprising a plurality of the machining members having different shapes from each other.

12. The manufacturing apparatus for an all-solid-state battery according to claim 6, further comprising a measuring member for measuring the thickness of the block supported by the block support member.

13. The manufacturing apparatus for an all-solid-state battery according to claim 6, wherein the support table is slidable or rotatable while supporting the base material.

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