Method for manufacturing solid-state battery

Through a multi-stage pressing process and pressure control, the densification and cracking problems of the electrode stack during the manufacturing process of all-solid-state batteries were solved, and a low-resistance and crack-free battery manufacturing method was achieved.

CN120728017APending Publication Date: 2025-09-30HONDA MOTOR CO LTD
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Patent Information

Application Number
CN202510233911.7
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Priority Date
2024-03-30
Filing Date
2025-02-28
Publication Date
2025-09-30

AI Technical Summary

Technical Problem

In existing all-solid-state battery manufacturing methods, the electrode stack is prone to cracking and increased resistance during the pressing process, making it difficult to achieve densification and crack prevention at the same time.

Method used

A multi-stage pressing process is adopted. By adjusting the pressing pressure and temperature of each stage, especially the pressing pressure of the second A step and the third step is greater than 600 MPa and less than 1000 MPa, and greater than 800 MPa and less than 1200 MPa, the first and second solid electrolyte layers are densified respectively, and a gel electrolyte layer is introduced in the fourth step to suppress cracks.

Benefits of technology

It effectively reduces the resistance of solid batteries, inhibits the generation of cracks in electrodes, and improves the overall performance of batteries.

✦ Generated by Eureka AI based on patent content.

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Abstract

The problem addressed by the present invention is to provide a method for manufacturing a solid-state battery provided with an electrode laminate in which a negative electrode, an intermediate layer, an electrolyte layer, and a positive electrode are laminated in this order, the electrolyte layer is formed by laminating a first solid electrolyte layer, a gel electrolyte layer, and a second solid electrolyte layer in this order in the lamination direction of the electrode laminate, and the method for manufacturing the solid-state battery comprises: a first A step for pressing the negative electrode in a state in which a material constituting the intermediate layer is disposed on the negative electrode, and a second A step for pressing the negative electrode in a state in which the material constituting the intermediate layer is disposed on the negative electrode; obtaining an intermediate layer-negative electrode laminate; a second A step for obtaining a first solid electrolyte layer-intermediate layer-negative electrode laminate by pressing the intermediate layer-negative electrode laminate in a state in which a material constituting the first solid electrolyte layer is disposed on the surface of the intermediate layer-negative electrode laminate on which the intermediate layer is disposed; a third step for obtaining a second solid electrolyte layer-positive electrode laminate by pressing the positive electrode in a state in which a material constituting the second solid electrolyte layer is disposed on the positive electrode; and a fourth A step, a material constituting the gel electrolyte layer is disposed between the surface of the first solid electrolyte layer-intermediate layer-negative electrode laminate on which the first solid electrolyte layer is disposed and the surface of the second solid electrolyte layer-positive electrode laminate on which the second solid electrolyte layer is disposed. And obtaining the electrode laminate.
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Description

Technical Field

[0001] The present invention relates to a method for manufacturing a solid battery. Background Art

[0002] In recent years, research and development of solid-state batteries that contribute to improving energy efficiency have been underway to ensure that more people have access to affordable, reliable, sustainable, and advanced energy.

[0003] As a solid-state battery, an all-solid-state battery having a solid electrolyte layer disposed between a positive electrode and a negative electrode is known.

[0004] Patent Document 1 describes a method for manufacturing an all-solid-state battery in which a positive electrode stack, an intermediate solid electrolyte layer, and a negative electrode stack are stacked in sequence. The positive electrode stack comprises a positive electrode current collector layer, a positive electrode active material layer, and a first solid electrolyte layer, and the negative electrode stack comprises a second solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer containing copper. The method for manufacturing an all-solid-state battery includes a first pressing step for pressing the positive electrode stack, a second pressing step for pressing the negative electrode stack, and a third pressing step for pressing the positive electrode stack, the intermediate solid electrolyte layer, and the negative electrode stack. At this time, the pressing pressure of the first pressing step is higher than the pressing pressure of the third pressing step, and the pressing temperature of the first pressing step is above 150°C and below 175°C. Furthermore, the pressing pressure of the second pressing step is higher than the pressing pressure of the third pressing step, and the pressing temperature of the second pressing step is below 125°C. Furthermore, the pressing temperature of the third pressing step is 125° C. or lower, and the intermediate solid electrolyte layer is not pressed at a pressure exceeding the pressing pressure of the third pressing step before the pressing in the third pressing step.

[0005] [Prior Art Literature]

[0006] (Patent Document)

[0007] Patent Document 1: Japanese Patent Application Laid-Open No. 2017-10816 Summary of the Invention

[0008] [Problems to be solved by the invention]

[0009] However, in the all-solid-state battery manufacturing method described in Patent Document 1, if the pressing pressure in the first and second pressing steps is high, the first and second solid electrolyte layers become denser, and cracks may form in the electrode during pressing in the third pressing step. On the other hand, if the pressing pressure in the first and second pressing steps is low, the first and second solid electrolyte layers do not become denser, and the resistance of the all-solid-state battery increases.

[0010] An object of the present invention is to provide a method for manufacturing a solid battery that can reduce the resistance of the solid battery and suppress cracking of the electrode.

[0011] [Technical means to solve the problem]

[0012] (1) A method for manufacturing a solid battery, wherein the solid battery comprises an electrode stack in which a negative electrode, an intermediate layer, an electrolyte layer, and a positive electrode are stacked in sequence, and the electrolyte layer comprises a first solid electrolyte layer, a gel electrolyte layer, and a second solid electrolyte layer stacked in sequence in the stacking direction of the electrode stack, and the method for manufacturing the solid battery comprises the following steps: a first step A, in which a material constituting the intermediate layer is arranged on the negative electrode and pressed to obtain an intermediate layer-negative electrode stack; a second step A, in which a material constituting the first solid electrolyte layer is arranged on a side of the intermediate layer-negative electrode stack on which the intermediate layer is arranged The first step is to press the material constituting the second solid electrolyte layer on the positive electrode to obtain a first solid electrolyte layer-intermediate layer-negative electrode stack; the third step is to press the material constituting the second solid electrolyte layer on the positive electrode to obtain a second solid electrolyte layer-positive electrode stack; and the fourth step is to press the material constituting the gel electrolyte layer between the surface of the first solid electrolyte layer-intermediate layer-negative electrode stack on the side where the first solid electrolyte layer is arranged and the surface of the second solid electrolyte layer-positive electrode stack on the side where the second solid electrolyte layer is arranged to obtain the electrode stack.

[0013] (2) The method for manufacturing a solid battery according to (1), wherein the pressing pressure in the second A step is higher than the pressing pressure in the fourth A step.

[0014] (3) The method for manufacturing a solid battery according to (2), wherein the pressing pressure in the second step A is 600 MPa or more and 1000 MPa or less.

[0015] (4) The method for producing a solid battery according to any one of (1) to (3), wherein the pressing pressure in the third step is higher than the pressing pressure in the fourth A step.

[0016] (5) The method for producing a solid battery according to (4), wherein the pressing pressure in the third step is 800 MPa or more and 1200 MPa or less.

[0017] (6) A method for manufacturing a solid battery, wherein the solid battery comprises an electrode stack in which a negative electrode, an electrolyte layer, and a positive electrode are stacked in sequence, and the electrolyte layer comprises a first solid electrolyte layer, a gel electrolyte layer, and a second solid electrolyte layer stacked in sequence in the stacking direction of the electrode stack, the method comprising the following steps: a second step B of pressing the negative electrode with a material constituting the first solid electrolyte layer disposed on the negative electrode to obtain a first solid electrolyte layer-negative electrode stack; a third step of pressing the positive electrode with a material constituting the second solid electrolyte layer disposed on the positive electrode to obtain a second solid electrolyte layer-positive electrode stack; and a fourth step B of pressing the electrode stack with a material constituting the gel electrolyte layer disposed between a surface of the first solid electrolyte layer-negative electrode stack on which the first solid electrolyte layer is disposed and a surface of the second solid electrolyte layer-positive electrode stack on which the second solid electrolyte layer is disposed.

[0018] (7) The method for producing a solid battery according to any one of (1) to (6), wherein the solid battery is a solid lithium metal battery.

[0019] (Effects of the Invention)

[0020] According to the present invention, a method for manufacturing a solid battery capable of reducing the resistance of the solid battery and suppressing the occurrence of cracks in the electrode can be provided. BRIEF DESCRIPTION OF THE DRAWINGS

[0021] Figure 1 is a cross-sectional view illustrating a solid state battery according to one embodiment of the present invention.

[0022] Figure 2 It is a cross-sectional view illustrating a method for producing an intermediate layer-negative electrode stack.

[0023] Figure 3 It is a cross-sectional view illustrating a method for producing a first solid electrolyte layer-intermediate layer-negative electrode stack.

[0024] Figure 4 It is a cross-sectional view illustrating a method for producing the second solid electrolyte layer-positive electrode stack.

[0025] Figure 5 It is a cross-sectional view explaining the method of manufacturing the electrode stack.

[0026] Figure 6 It is a cross-sectional view illustrating a method for producing a first solid electrolyte layer-negative electrode stack.

[0027] Figure 7 It is a cross-sectional view explaining the method of manufacturing the electrode stack. DETAILED DESCRIPTION

[0028] Hereinafter, embodiments of the present invention will be described with reference to the accompanying drawings.

[0029] [Solid-state battery]

[0030] exist Figure 1 FIG. 2 shows a solid-state battery according to one embodiment of the present invention.

[0031] The solid-state battery 1 includes an electrode stack in which a negative electrode 2, an intermediate layer 5, an electrolyte layer 4, a positive electrode 3, an electrolyte layer 4, an intermediate layer 5, and a negative electrode 2 are stacked in this order. The electrolyte layer 4 includes a first solid electrolyte layer 41, a gel electrolyte layer 42, and a second solid electrolyte layer 43 stacked in this order in the stacking direction of the electrode stack. In this case, a portion of the gel electrolyte constituting the gel electrolyte layer 42 may permeate into the first solid electrolyte layer 41 and / or the second solid electrolyte layer 43.

[0032] The negative electrode 2 includes a negative electrode composite material layer 21 and a negative electrode current collector 22 stacked in this order in the stacking direction of the electrode stack. A negative electrode collector tab 22 a extends from one end of the negative electrode current collector 22 .

[0033] The positive electrode 3 is stacked in the order of a positive electrode composite material layer 31, a positive electrode current collector 32, and a positive electrode composite material layer 31. When the positive electrode 3 is viewed from above in the direction of the electrode stack, the outer periphery of the positive electrode composite material layer 31 is located further inward than the outer periphery of the positive electrode current collector 32. An insulating frame 6 is provided around the outer periphery of the positive electrode composite material layer 31. When the insulating frame 6 is viewed from above in the direction of the electrode stack, the outer periphery of the insulating frame 6 is located at approximately the same position as the outer periphery of the positive electrode current collector 32. The positive electrode collector tab 32a extends from the end of the positive electrode current collector 32 on the opposite side of the side from which the negative electrode collector tab 22a extends.

[0034] Furthermore, the solid battery 1 is not particularly limited as long as it includes an electrode stack in which a negative electrode 2, an intermediate layer 5, an electrolyte layer 4, and a positive electrode 3 are stacked in this order. For example, the solid battery 1 may include multiple positive electrodes 3. Alternatively, the solid battery 1 may include a single negative electrode 2, a single intermediate layer 5, and a single electrolyte layer 4. In this case, the positive electrode 3 includes a positive electrode composite material layer 31 and a positive electrode current collector 32 stacked in this order in the stacking direction of the electrode stack. Furthermore, the solid battery 1 may not include an intermediate layer 5.

[0035] [Method for manufacturing solid-state batteries]

[0036] Next, use Figures 2 to 5 A method for manufacturing the solid state battery 1 will be described.

[0037] (Intermediate layer-negative electrode stack)

[0038] The negative electrode 2 is pressed with the material constituting the intermediate layer 5 disposed on the surface thereof where the negative electrode composite material layer 21 is disposed, thereby obtaining an intermediate layer-negative electrode laminate L1 (first step A; see Figure 2 、 3 ). There is no particular limitation on the method of configuring the material constituting the intermediate layer 5 on the surface of the negative electrode 2 on the side where the negative electrode composite material layer 21 is configured, and an example thereof is a method of transferring the intermediate layer 5 onto the negative electrode composite material layer 21 using an intermediate layer transfer sheet. The intermediate layer transfer sheet is obtained, for example, by dispersing the material constituting the intermediate layer 5 in a solvent, coating the obtained slurry on a support sheet, and then drying it. The pressing pressure in the first A step is not particularly limited, and for example, it is greater than 400 MPa and less than 1000 MPa. The pressing temperature in the first A step is not particularly limited, and for example, it is greater than 25°C and less than 150°C.

[0039] (First solid electrolyte layer-intermediate layer-negative electrode stack)

[0040] The intermediate layer-negative electrode stack L1 is pressed with the material constituting the first solid electrolyte layer 41 disposed on the surface thereof on which the intermediate layer 5 is disposed, thereby obtaining the first solid electrolyte layer-intermediate layer-negative electrode stack L2 (second A step; see Figure 3 、 5 ). There is no particular limitation on the method of configuring the material constituting the first solid electrolyte layer 41 on the surface of the intermediate layer-negative electrode stack L1 on the side where the intermediate layer 5 is configured, and examples thereof include a method of transferring the first solid electrolyte layer 41 to the intermediate layer 5 using a first solid electrolyte layer transfer sheet. The first solid electrolyte layer transfer sheet is obtained, for example, by dispersing a solid electrolyte having a median particle size of less than 1 μm in a solvent, coating the obtained slurry on a support sheet, and then drying it. At this time, the pressing pressure in the second A process is preferably higher than the pressing pressure in the fourth A process described later. As a result, the first solid electrolyte layer 41 is densified, while the breakage and deformation of each layer are suppressed. The pressing pressure in the second A process is not particularly limited as long as it can densify the first solid electrolyte layer 41, and is, for example, greater than 600 MPa and less than 1000 MPa. The pressing temperature in the second A process is not particularly limited, and is, for example, greater than 25°C and less than 150°C.

[0041] The density of the first solid electrolyte layer 41 is not particularly limited, for example, 1.65 g / cm 3 Above and 2.00 g / cm 3The porosity of the first solid electrolyte layer 41 is not particularly limited, and is, for example, 1% to 7%. The thickness of the first solid electrolyte layer 41 is not particularly limited, and is, for example, 1 μm to 7 μm.

[0042] (Second solid electrolyte layer-positive electrode stack)

[0043] The second solid electrolyte layer 43 is formed on both sides of the positive electrode 3 where the positive electrode composite material layer 31 and the insulating frame 6 are formed, and the second solid electrolyte layer-positive electrode laminate L3 is obtained by pressing (third step; see Figure 4 、 5 ). There is no particular limitation on the method of configuring the material constituting the second solid electrolyte layer 43 on the surfaces on both sides of the positive electrode 3 where the positive electrode composite material layer 31 and the insulating frame 6 are arranged. For example, a method of transferring the second solid electrolyte layer 43 to the positive electrode composite material layer 31 and the insulating frame 6 using a second solid electrolyte layer transfer sheet can be cited. The second solid electrolyte layer transfer sheet is obtained, for example, by dispersing a solid electrolyte having a median particle size of less than 1 μm in a solvent, coating the obtained slurry on a support sheet, and then drying it. At this time, the pressing pressure in the third process is preferably higher than the pressing pressure in the fourth A process described later. As a result, the second solid electrolyte layer 43 is densified, while the breakage and deformation of each layer are suppressed. The pressing pressure in the third process is not particularly limited as long as it can densify the second solid electrolyte layer 43, for example, it is greater than 800 MPa and less than 1200 MPa. The pressing temperature in the third process is not particularly limited, for example, it is greater than 25°C and less than 1000°C.

[0044] The density of the second solid electrolyte layer 43 is not particularly limited, for example, 1.65 g / cm 3 Above and 2.00 g / cm 3 The porosity of the second solid electrolyte layer 43 is not particularly limited, and is, for example, 1% to 7%. The thickness of the second solid electrolyte layer 43 is not particularly limited, and is, for example, 1 μm to 7 μm.

[0045] (Electrode stack)

[0046] The electrode stack is obtained by pressing with the material constituting the gel electrolyte layer 42 disposed between the surface of the first solid electrolyte layer-intermediate layer-negative electrode stack L2 on which the first solid electrolyte layer 41 is disposed and the surface of the second solid electrolyte layer-positive electrode stack L3 on which the second solid electrolyte layer 43 is disposed (Step 4A; see Figure 5). Therefore, even if the first solid electrolyte layer 41 and the second solid electrolyte layer 43 are densified, cracks in the negative electrode 2 and / or the positive electrode 3 can be suppressed during pressing. There is no particular limitation on the method of configuring the material constituting the gel electrolyte layer 42, and examples include a method of transferring the gel electrolyte layer 42 onto the first solid electrolyte layer 41 or the second solid electrolyte layer 43 using a gel electrolyte layer transfer sheet. The gel electrolyte layer transfer sheet can be obtained, for example, by dispersing the material constituting the gel electrolyte layer 42 in a solvent, applying the obtained slurry on a support sheet, and then drying it. The pressing pressure in the fourth A step is not particularly limited as long as it can integrate the electrolyte layer 4, and is, for example, 500 MPa or less.

[0047] The apparatus used when manufacturing the solid battery 1 is not particularly limited, and examples thereof include a roller press apparatus and a plate press apparatus.

[0048] Next, use Figure 4 、 6 7 will now describe a method for manufacturing the solid battery 1 when the intermediate layer 5 is not provided.

[0049] (First solid electrolyte layer-negative electrode stack)

[0050] The negative electrode 2 is pressed with the material constituting the first solid electrolyte layer 41 disposed on the surface thereof where the negative electrode composite material layer 21 is disposed, thereby obtaining a first solid electrolyte layer-negative electrode laminate L2A (second B step; see Figure 6 、 7 The method for arranging the material constituting the first solid electrolyte layer 41 on the surface of the negative electrode 2 on the side where the negative electrode composite material layer 21 is arranged is not particularly limited. For example, a method of transferring the first solid electrolyte layer 41 onto the negative electrode composite material layer 21 using a first solid electrolyte layer transfer sheet can be used. The first solid electrolyte layer transfer sheet can be obtained, for example, by dispersing a solid electrolyte having a median particle size of 1 μm or less in a solvent, applying the obtained slurry on a support sheet, and then drying. The pressing pressure is not particularly limited as long as it can densify the first solid electrolyte layer 41.

[0051] (Second solid electrolyte layer-positive electrode stack)

[0052] The second solid electrolyte layer-positive electrode stack L3 is obtained by the above-mentioned method (third step; refer to Figure 4 ).

[0053] (Electrode stack)

[0054] The electrode stack is obtained by pressing with the material constituting the gel electrolyte layer 42 disposed between the surface of the first solid electrolyte layer-negative electrode stack L2A on which the first solid electrolyte layer 41 is disposed and the surface of the second solid electrolyte layer-positive electrode stack L3 on which the second solid electrolyte layer 43 is disposed (step 4B; see Figure 7 ). Therefore, even if the first solid electrolyte layer 41 and the second solid electrolyte layer 43 are densified, cracks in the negative electrode 2 and / or the positive electrode 3 are suppressed during pressing. There is no particular limitation on the method of configuring the material constituting the gel electrolyte layer 42, and an example thereof is a method of transferring the gel electrolyte layer 42 onto the first solid electrolyte layer 41 or the second solid electrolyte layer 43 using a gel electrolyte layer transfer sheet. The gel electrolyte layer transfer sheet is obtained, for example, by dispersing the material constituting the gel electrolyte layer 42 in a solvent, applying the obtained slurry on a support sheet, and then drying it. There is no particular limitation on the pressing pressure as long as the electrolyte layer 4 can be integrated.

[0055] Furthermore, the apparatus used when producing the solid battery 1 without the intermediate layer 5 is not particularly limited, and examples thereof include a roller press apparatus and a plate press apparatus.

[0056] The solid battery 1 is not particularly limited, and examples thereof include solid lithium metal batteries. Hereinafter, a case where the solid battery 1 is a solid lithium metal battery will be described.

[0057] The negative electrode mixture layer 21 is a lithium metal layer. The negative electrode current collector 22 is not particularly limited, and examples thereof include copper foil.

[0058] The positive electrode composite material layer 31 contains a positive electrode active material and may further contain a solid electrolyte, a conductive aid, a binder, and the like. As the positive electrode active material, there is no particular limitation as long as it can embed and deintercalate lithium ions, and examples thereof include lithium nickel cobalt manganese composite oxides. As the solid electrolyte, there is no particular limitation as long as it has lithium ion conductivity, and examples thereof include oxide-based electrolytes and sulfide-based electrolytes. As the conductive aid, there is no particular limitation as long as it has electronic conductivity, and examples thereof include carbon black. As the binder, there is no particular limitation as long as it can improve the bonding properties, and examples thereof include styrene-butadiene rubber.

[0059] The positive electrode current collector 32 is not particularly limited, and an example thereof is aluminum foil.

[0060] The first solid electrolyte layer 41 and the second solid electrolyte layer 43 include a solid electrolyte. The solid electrolyte is not particularly limited as long as it has lithium ion conductivity, and examples thereof include inorganic solid electrolytes such as oxide-based electrolytes and sulfide-based electrolytes. Furthermore, the solid electrolytes constituting the first solid electrolyte layer 41 and the second solid electrolyte layer 43 may be the same or different.

[0061] Gel electrolyte layer 42 comprises a matrix resin, an electrolyte, and a solvent. The matrix resin is not particularly limited as long as it can gel and integrate electrolyte layer 4; examples include polyethylene oxide. The electrolyte is not particularly limited as long as it has lithium ion conductivity; examples include lithium salts. The solvent is not particularly limited as long as it can dissolve the electrolyte; examples include carbonate-based solvents.

[0062] The intermediate layer 5 includes a metal capable of alloying with lithium and amorphous carbon, and may further include a binder. The metal capable of alloying with lithium and the amorphous carbon are preferably nanoparticles. Examples of metals capable of alloying with lithium include tin (Sn), silicon (Si), zinc (Zn), magnesium (Mg), gold (Au), platinum (Pt), palladium (Pd), silver (Ag), aluminum (Al), bismuth (Bi), and antimony (Sb). Examples of amorphous carbon include carbon blacks such as acetylene black, furnace black, and Ketjen black, coke, and activated carbon. Amorphous carbon may be easily graphitized carbon (soft carbon), or difficult to graphitize carbon (hard carbon), carbon nanotubes (CNTs), fullerenes, and graphene. As a binder, there is no particular limitation as long as it can improve adhesion, and examples include polyvinylidene difluoride (PVDF).

[0063] Because the intermediate layer 5 has the function of uniformly depositing lithium metal, the interface between the intermediate layer 5 and the first solid electrolyte layer 41 becomes stable. When the solid battery 1 includes the intermediate layer 5, the solid battery 1 can be an anode-less battery that does not form a lithium metal layer as the negative electrode composite material layer 21 during the initial charge. An anode-less battery forms a lithium metal layer as the negative electrode composite material layer 21 after the initial charge and discharge.

[0064] The thickness of the intermediate layer 5 is not particularly limited, and may be, for example, 4 μm or more and 10 μm or less.

[0065] The material constituting the insulating frame 6 is not particularly limited, and examples thereof include insulating oxides such as alumina, resins such as polyvinylidene fluoride (PVDF), and rubbers such as styrene butadiene rubber (SBR).

[0066] While the embodiments of the present invention have been described above, the present invention is not limited to the above embodiments and may be appropriately modified within the scope of the present invention. For example, the solid battery 1 may further include an outer casing (e.g., a laminate film) that surrounds the electrode stack.

[0067] Reference numerals

[0068] 1 Solid-state battery

[0069] 2 Negative electrode

[0070] 21. Negative electrode composite material layer

[0071] 22 Negative electrode collector

[0072] 22a Negative collector lug

[0073] 3. Positive electrode

[0074] 31. Positive electrode composite material layer

[0075] 32 positive electrode collector

[0076] 32a Positive collector lug

[0077] 4 Electrolyte layer

[0078] 41 First solid electrolyte layer

[0079] 42 Gel electrolyte layer

[0080] 43 Second solid electrolyte layer

[0081] 5 Middle Layer

[0082] 6 Insulation frame

[0083] L1 Intermediate layer-negative electrode stack

[0084] L2 First solid electrolyte layer-intermediate layer-negative electrode stack

[0085] L2A First solid electrolyte layer-negative electrode stack

[0086] L3 Second solid electrolyte layer-positive electrode stack

Claims

1. A method for manufacturing a solid battery, comprising an electrode stack in which a negative electrode, an intermediate layer, an electrolyte layer, and a positive electrode are stacked in this order, and The electrolyte layer includes a first solid electrolyte layer, a gel electrolyte layer, and a second solid electrolyte layer stacked in this order in the stacking direction of the electrode stack. The solid battery manufacturing method includes the following steps: a first step A, in which a material constituting the intermediate layer is placed on the negative electrode and pressed to obtain an intermediate layer-negative electrode laminate; The second step A comprises pressing the intermediate layer-negative electrode stack with the material constituting the first solid electrolyte layer disposed on the surface of the intermediate layer-negative electrode stack, thereby obtaining a first solid electrolyte layer-intermediate layer-negative electrode stack; The third step is to press the material constituting the second solid electrolyte layer on the positive electrode to obtain a second solid electrolyte layer-positive electrode laminate; and In the fourth A step, the electrode stack is obtained by pressing the material constituting the gel electrolyte layer between the surface of the first solid electrolyte layer-intermediate layer-negative electrode stack on the side where the first solid electrolyte layer is arranged and the surface of the second solid electrolyte layer-positive electrode stack on the side where the second solid electrolyte layer is arranged.

2. The method for manufacturing a solid battery according to claim 1, wherein: The pressing pressure in the aforementioned second A step is higher than the pressing pressure in the aforementioned fourth A step.

3. The method for manufacturing a solid battery according to claim 2, wherein: The pressing pressure in the aforementioned second A step is 600 MPa or more and 1000 MPa or less.

4. The method for manufacturing a solid battery according to any one of claims 1 to 3, wherein: The pressing pressure in the aforementioned third step is higher than the pressing pressure in the aforementioned fourth A step.

5. The method for manufacturing a solid battery according to claim 4, wherein: The pressing pressure in the third step is 800 MPa or more and 1200 MPa or less.

6. A method for manufacturing a solid battery, comprising an electrode stack in which a negative electrode, an electrolyte layer, and a positive electrode are stacked in this order, and The electrolyte layer includes a first solid electrolyte layer, a gel electrolyte layer, and a second solid electrolyte layer stacked in this order in the stacking direction of the electrode stack. The solid battery manufacturing method includes the following steps: a second step B of pressing the negative electrode with the material constituting the first solid electrolyte layer disposed thereon to obtain a first solid electrolyte layer-negative electrode laminate; The third step is to press the material constituting the second solid electrolyte layer on the positive electrode to obtain a second solid electrolyte layer-positive electrode laminate; and The fourth step B is to obtain the electrode stack by pressing the material constituting the gel electrolyte layer between the surface of the first solid electrolyte layer-negative electrode stack on the side where the first solid electrolyte layer is arranged and the surface of the second solid electrolyte layer-positive electrode stack on the side where the second solid electrolyte layer is arranged.

7. The method for manufacturing a solid battery according to claim 1 or 6, wherein: The aforementioned solid battery is a solid lithium metal battery.

Citation Information

Patent Citations

  • Method of manufacturing all-solid battery

    JP2017010816A