JP2020013711A - Manufacturing method of series-stacked all-solid-state battery - Google Patents

Abstract

To provide a manufacturing method of a series-stacked all-solid-state battery that can suppress a material from falling off from the end of a battery stack during manufacturing.SOLUTION: A manufacturing method of a series-stacked all-solid-state battery includes (a) preparing an exterior body having an accommodation portion for accommodating a battery stack, (b) inserting a unit battery or one or more layers constituting the unit battery into a housing portion of one partial exterior body in order within a direction ±60° perpendicular to the stacking direction, (c) combining all the partial exterior bodies to form an exterior body, thereby accommodating the battery stack in the exterior body, and (d) connecting electrode terminals to both end surfaces in the stacking direction of the battery stack via through holes at both ends of the battery stack.SELECTED DRAWING: Figure 1

Description

  The present disclosure relates to a method for manufacturing a series-stacked all-solid-state battery.

  2. Description of the Related Art In recent years, with the rapid spread of information-related devices such as personal computers, video cameras, and mobile phones, communication devices, and the like, development of a stacked battery used as a power source thereof has been regarded as important. In addition, the automobile industry and the like have been developing high-output and high-capacity stacked all-solid-state batteries for electric vehicles or hybrid vehicles.

  For example, in Patent Literature 1, a housing for housing a charging / discharging unit has a positioning protrusion, a component of the charging / discharging unit has a hole into which the positioning protrusion can be inserted, and charging / discharging is performed along the positioning protrusion. A method for manufacturing an all-solid-state battery including a laminating step of laminating the components of a part is disclosed.

  Further, in Patent Document 2, an electrode body held by a support structure having a clip mechanism is placed on a pedestal, and the electrodes are stacked in a direction perpendicular to the plane direction of the bipolar electrode. Disclosed is a method for manufacturing a bipolar battery including a step of eliminating.

  Patent Literature 3 discloses a fuel cell stack in which unit cells are stacked using a positioning guide.

JP 2011-103279 A JP 2012-190809 A JP 2003-086232 A

  The stacked all-solid-state battery, in which the electrolyte is replaced with a solid electrolyte layer and the battery is solidified, does not use a flammable organic solvent in the battery, thereby simplifying the safety device, reducing manufacturing costs and Because of its excellent productivity, it is attracting attention.

  When manufacturing such a stacked all-solid-state battery, usually, a positive electrode current collector layer, a positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer are laminated, and a unit battery To form Then, the unit batteries are stacked in series or in parallel to form a battery stack. Thereafter, the battery stack is connected to the electrode terminals and housed in an exterior body or the like to manufacture an all-solid-state battery.

  However, when the battery stack is accommodated from the opening of the outer package, the positive electrode current collector layer, the positive electrode active material layer, the solid electrolyte layer, the negative electrode active material layer, or the negative electrode current collector layer included in the battery stack Material from the edges may fall off. In particular, the longer the distance in which the battery stack is moved in the direction perpendicular to the surface direction in the outer package, the longer the distance between the inner wall of the outer package and the end of the battery stack. Material from the end portion is likely to fall off. If the material falls off in this manner, the dropped material may adhere to the edge of another layer, thereby causing a short circuit.

  Accordingly, the present disclosure has been made in view of the above circumstances, and when a battery stack is accommodated in an exterior body, a series stack type all-solid battery that can prevent the material from falling off from the end of the battery stack. It is intended to provide a manufacturing method.

The present inventor of the present disclosure has found that the above-mentioned problems can be solved by a method for manufacturing a series-stacked all-solid-state battery including the following steps:
(A) Preparing an exterior body having an accommodation portion for accommodating a battery stack, wherein the exterior body has through holes at both ends in a stacking direction of the battery stack, and is divided. The battery stack comprises at least two unit batteries stacked in series, and the unit battery comprises a positive electrode current collector layer and a positive electrode active material layer. , A solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer in this order;
(B) The unit battery or one or a plurality of layers constituting the unit battery are sequentially inserted into the accommodating portion of the one partial exterior body within a direction ± 60 ° perpendicular to the stacking direction. thing;
(C) combining all of the partial exterior bodies to form the exterior body, thereby accommodating the battery stack in the exterior body;
(D) connecting electrode terminals to both end faces in the stacking direction of the battery stack through the through holes at both ends of the package;

  According to the manufacturing method of the series-stacked all-solid-state battery of the present disclosure, when the battery stack is housed in the exterior body, it is possible to prevent the material from falling off from the end of the battery stack.

FIG. 1 is a schematic cross-sectional view illustrating one embodiment of each step included in the method of manufacturing a series-stacked all-solid-state battery of the present disclosure. FIG. 2 is a schematic view showing one mode in which the pressing step is included in the middle of the step (d).

  Hereinafter, embodiments for carrying out the present disclosure will be described in detail with reference to the drawings. Note that, for convenience of description, the same or corresponding portions are denoted by the same reference numerals in each drawing, and redundant description will be omitted. All of the components of the embodiment are not necessarily essential, and some components may be omitted in some cases. However, the embodiments shown in the following drawings are examples of the present disclosure, and do not limit the present disclosure.

<< Manufacturing method of series stacked type all solid state battery >>
The method for manufacturing the series-stacked all-solid-state battery of the present disclosure includes the following steps:
(A) Preparing an exterior body having an accommodation portion for accommodating the battery stack, wherein the exterior body has through holes at both ends and is divided in the stacking direction of the battery stack. The battery stack comprises at least two unit batteries stacked in series, and the unit battery includes a positive electrode current collector layer, a positive electrode active material layer, and a solid electrolyte layer. , A negative electrode active material layer, and a negative electrode current collector layer in this order;
(B) Inserting the unit battery or one or more layers constituting the unit battery into the accommodation portion of one partial exterior body in order within a direction ± 60 ° perpendicular to the stacking direction;
(C) combining all of the partial exterior bodies to form an exterior body, thereby accommodating the battery stack within the exterior body;
(D) connecting electrode terminals to both end surfaces in the stacking direction of the battery stack through the through holes at both ends of the outer package;

  In the present disclosure, the “series-stacked all-solid-state battery” is an all-solid-state battery having a battery stack in which two or more unit cells are stacked in series, and is located at both end faces in the stacking direction of the battery stack. This is an all-solid-state battery that can be charged and discharged from a current collector layer. An example of a series-stacked all-solid-state battery includes, but is not limited to, a bipolar-type all-solid-state battery.

  The “stacking direction of the battery stack” refers to the direction in which the unit cells constituting the battery stack or the respective layers constituting the unit battery are stacked, that is, the surface direction of the unit battery or the respective layers constituting the unit battery. Refers to the direction of the axis perpendicular to. In addition, in the case where the exterior body does not accommodate the battery stack, it indicates the stacking direction of the battery stack to be accommodated by the exterior body.

<Step (a)>
In the step (a), an exterior body having an accommodation portion for accommodating the battery stack is prepared.

  Here, in the stacking direction of the battery stack, the outer package has at least two partial outer packages having through holes at both ends and having a divided shape, and the battery stack includes a unit battery. Two or more are stacked in series, and the unit battery is formed by stacking a positive electrode current collector layer, a positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer in this order. I have.

  For example, FIG. 1A is a schematic cross-sectional view illustrating an aspect in which an exterior body 11 having an accommodation portion 11a for accommodating the battery stack 10 is prepared. Here, in the stacking direction of the battery stack 10, the exterior body 11 has through holes 11b and 11c at both ends. The exterior body 11 is composed of two partial exterior bodies 11x and 11y having divided shapes. Since the details of the battery stack 10 are shown in the right diagram of FIG. 1B, the description is omitted here.

  The shape of the exterior body is not particularly limited, and can be appropriately set according to the shape of the battery stack to be housed. For example, when the battery stack is a columnar type, the exterior body may be a columnar type having a size that can accommodate the battery stack.

  The accommodation part in the exterior body is a space for accommodating the battery stack. For this reason, as long as the battery stack can be housed after all the partial exterior bodies having the divided shape are combined, any one of the partial exterior bodies having the divided shape may have an accommodation portion. Well, you don't have to.

  The number of partial exterior bodies constituting the exterior body is not particularly limited as long as it is two or more. That is, the exterior body is divided into two, three, four, or the like in the stacking direction of the battery stack. Although it may be composed of a partial exterior body having a bent shape, it is preferable that the partial exterior body has a shape divided into two from the viewpoint of operability. Further, the shape (or size) of each partial exterior body is not particularly limited, and may be the same or different.

  Further, in the stacking direction of the battery stack, the exterior body has through holes at both ends. The through-holes are openings for connecting electrode terminals to both end faces in the stacking direction of a battery stack described later. For example, as shown in FIG. 1A, in the stacking direction of the battery stack, the outer package 11 has through holes 11b and 11c at both ends. In a step (d) described later, the electrode terminals 31 and 30 can be connected to both end faces in the stacking direction of the battery stack 10 through the through-holes 11b.

  The sizes of the through-holes at both ends of the exterior body may be the same or different. The upper limit of each size may be the same as the surface area of the inner surface of the exterior body, and the lower limit of each size may be such that an electrode terminal can be connected.

  The size of the through-hole portion of the outer package is, for example, 100% or less, 95% or less, 90% or less, 85% or less, 80% or less, 75% or less, 70% or less, of the area of the end face of the battery laminate. It may be 65% or less, 60% or less, 55% or less, 50% or less, 40% or less, or 30% or less.

  In the case where the battery laminate is pressed in the package described below, the battery laminate can be pressed through the through-holes of the package. Further, from the viewpoint of operability in the case of including the step of pressing the battery laminate, the size of the through-hole portion of the exterior body on the side where the battery laminate contacts the pressing means is in contact with the pressing means of the battery laminate. It is preferable that the size is the same as the size of the end face on the side to be formed.

  The material constituting the exterior body is not particularly limited, and may be, for example, metal or fiber-reinforced plastic. As the metal, for example, a material having appropriate rigidity such as aluminum, an aluminum alloy, and stainless steel is used, but is not limited thereto. Examples of the fiber reinforced plastic include, but are not limited to, carbon fiber reinforced plastic, boron fiber reinforced plastic, aramid fiber reinforced plastic, polyethylene fiber reinforced plastic, and Zylon reinforced plastic.

  The exterior body may further have an insulating layer on the inner wall. The insulating layer is not particularly limited, and may be, for example, an insulating film layer or an insulating resin layer. In particular, when a metal is used as the exterior body, an embodiment further including an insulating layer on the inner wall of the exterior body is preferable because a short circuit between the exterior body and the current collector layer can be prevented. In addition, it is also possible to prevent a short circuit by performing insulation treatment on the end of each layer of the battery stack instead of the insulation layer.

<Step (b)>
In the step (b), the unit battery or one or a plurality of layers constituting the unit battery are sequentially inserted into the accommodating portion of one partial exterior body from a direction ± 60 ° perpendicular to the stacking direction.

  As in the step (b), the unit battery or one or more layers constituting the unit battery are sequentially inserted into the accommodating portion of one partial exterior body within a direction perpendicular to the stacking direction ± 60 °. By doing so, the partial exterior body directly serves as a guide for one or more layers constituting the unit battery or the unit battery, and facilitates alignment of each layer constituting the unit battery (or the battery laminate). As a result, misalignment of each layer can be prevented.

  In addition, the unit battery or one or a plurality of layers constituting the unit battery are sequentially arranged with respect to the accommodating portion of one partial exterior body, within a direction of ± 45 ° perpendicular to the lamination direction, within a direction of ± 30 °, Within the direction of ± 15 °, may be inserted from ± 0 ° (ie, the direction perpendicular to the laminating direction), preferably from the direction ± 0 ° perpendicular to the laminating direction (ie, the direction perpendicular to the laminating direction). insert.

  For example, FIG. 1B is a schematic cross-sectional view illustrating one mode of the step (b). As shown in the left drawing of FIG. 1B, the layers constituting the unit battery 6c: the positive / negative current collector layer 5c, the positive electrode active material layers 4c, 5c, 4c,. The battery stack 10 is inserted into the 11x storage section from a direction perpendicular to the stacking direction of the battery stack 10. As a result, as shown in the right diagram of FIG. 1B, the battery stack 10 formed by stacking the unit batteries 6a, 6b, and 6c in series is inserted into the accommodating portion of the partial exterior body 11x. I have.

  Further, the active material layer and the solid electrolyte layer constituting the unit battery can be formed by compacting (press molding) each constituent material.

For example, a positive electrode active material, and a solid electrolyte used as needed, a conductive auxiliary, and a constituent material containing an additive used for the positive electrode active material layer of an all solid state battery such as a binder, by compacting the positive electrode, An active material layer can be formed. In addition, the negative electrode active material, and a solid electrolyte used as necessary, a conductive auxiliary, and a constituent material containing an additive used in the negative electrode active material layer of the all-solid battery such as a binder, by compacting, the negative electrode An active material layer can be formed. In addition, the solid electrolyte layer and the constituent materials containing the additives used for the solid electrolyte layer of the all-solid battery such as the conductive auxiliary agent and the binder used as needed are formed by compacting the solid electrolyte layer to form the solid electrolyte layer. Can be.
<Step (c)>
In the step (c), all the partial exterior bodies are joined to form an exterior body, and thereby the battery stack is accommodated in the exterior body.

  For example, FIG. 1C is a schematic cross-sectional view illustrating one mode of the step (c). As shown in FIG. 1C, in order to accommodate the battery stack 10 arranged in the accommodating portion of the partial exterior body 11x, the partial exterior body 11x and the other partial exterior body 11y are combined. The exterior body 11 is formed, and thereby, the battery stack 10 is accommodated in the exterior body 11.

<Step (d)>
In the step (d), electrode terminals are connected to both end surfaces in the stacking direction of the battery stack through the through holes at both ends of the package.

  By connecting the electrode terminals, electric power generated in the battery stack can be taken out.

  For example, FIG. 1D shows a mode in which the electrode terminals 30 and 31 are connected to both end surfaces in the stacking direction of the battery stack 10 through the through holes 11c and 11b at both ends of the outer package.

  Further, as the electrode terminals, those having a function as a current collector layer can be used. In this case, not the current collector layer but the positive electrode active material layer or the negative electrode active material layer located at the end face in the stacking direction of the battery laminate, and these active material layers function as a current collector layer. May be connected.

  Further, it is preferable to further include a pressing step before, during, or after the step (d). The pressing step is a step of pressing the battery stack in the stacking direction of the battery stack.

  For example, FIG. 2 is a schematic view showing an embodiment in which this pressing step is included in the middle of the step (d). As shown in FIG. 2A, an electrode terminal 32 is connected to the lower end surface of the battery stack 20 in the stacking direction. Thereafter, as shown in FIG. 2B, the battery stack 20 is pressed along the stacking direction of the battery stack 20 and toward the end face to which the electrode terminals 32 are connected. Then, as shown in FIG. 2C, the electrode terminal 33 is connected to the upper end surface of the battery stack 20 in the stacking direction. As described above, by performing the pressing step in the middle of the step (d), the battery stack 20 can be restrained in the stacking direction. Note that the exterior body 21 has an insulating layer 22 on the inner wall thereof.

  As described above, according to the method of the present disclosure, it is possible to manufacture a series-stacked all-solid-state battery that can prevent the material from falling off during manufacturing.

  《Series-stacked all-solid-state battery》

  The all solid state battery of the present disclosure manufactured by the above-described method has a battery stack in which two or more unit cells are stacked in series.

  Here, the unit battery is configured by stacking a positive electrode current collector layer, a positive electrode active material layer, a solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer in this order.

  For example, the battery stack 10 shown in the right diagram of FIG. 1B is formed by stacking three unit batteries 6a, 6b, and 6c in series. Further, the unit battery 6a is configured by stacking a positive / negative electrode current collector layer 1a, a negative electrode active material layer 2a, a solid electrolyte layer 3a, a positive electrode active material layer 4a, and a positive / negative electrode current collector layer 5a in this order. Have been. The unit battery 6b is configured by stacking a positive / negative current collector layer 1b, a negative electrode active material layer 2b, a solid electrolyte layer 3b, a positive electrode active material layer 4b, and a positive / negative electrode current collector layer 5b in this order. I have. The unit battery 6c is configured by stacking a positive / negative current collector layer 1c, a negative electrode active material layer 2c, a solid electrolyte layer 3c, a positive electrode active material layer 4c, and a positive / negative electrode current collector layer 5c in this order. I have.

  When two or more unit batteries are stacked in series, two unit batteries adjacent in the stacking direction may share a positive electrode / negative electrode current collector layer used as both a positive electrode and a negative electrode current collector layer.

  That is, in the battery stack, in the stacking direction, a negative electrode current collector layer (or a positive electrode / negative electrode current collector layer), a negative electrode active material layer, a solid electrolyte layer, a positive electrode active material layer, a positive electrode / negative electrode current collector layer, and a negative electrode An active material layer, a solid electrolyte layer, a positive electrode active material layer, and a positive electrode current collector layer (or a positive electrode / negative electrode current collector layer) can be laminated in this order to form a battery laminate. In this case, since the “positive electrode / negative electrode current collector layer” is used as both the positive electrode and the negative electrode current collector layer, any of the “positive electrode current collector layer” or the “negative electrode current collector layer” in the present disclosure is used. This is also true.

  For example, as shown in the right diagram of FIG. 1B, the unit battery 6a and the unit battery 6b share the positive / negative current collector layer 5a (1b), and the unit battery 6b and the unit battery 6b. 6c shares the positive electrode / negative electrode current collector layer 5b (1c).

  Note that such a positive / negative current collector may not be shared between the unit batteries, in which case a positive current collector layer and a negative current collector layer are provided in accordance with the adjacent active material layer. , May be in electrical contact with each other (not shown).

  In the present disclosure, the battery stack may be constrained in the stacking direction. Thereby, at the time of charge and discharge, the conductivity of ions and electrons between each layer and between each layer of the all-solid-state battery stack can be improved, and the battery reaction can be further promoted.

  The shape of the battery stack is not particularly limited, and may be, for example, a coin type, a laminate type, a columnar type, a square type, or the like.

  Specific examples of the constituent materials of each layer constituting the unit battery will be described as follows. In addition, in order to easily understand the present disclosure, a unit battery used for an all-solid lithium-ion secondary battery will be described as an example.However, the all-solid battery of the present disclosure is not limited to a lithium-ion secondary battery, and is widely used. Applicable.

(Positive electrode current collector layer)
The conductive material used for the positive electrode current collector layer is not particularly limited, and a material that can be used for an all-solid-state battery can be appropriately used. For example, the conductive material used for the positive electrode current collector layer may be, but is not limited to, SUS, aluminum, copper, nickel, iron, titanium, carbon, or the like.

  The shape of the positive electrode current collector layer is not particularly limited, and examples thereof include a foil shape, a plate shape, and a mesh shape. Among these, a foil shape is preferred.

(Positive electrode active material layer)
The positive electrode active material layer contains at least a positive electrode active material, and preferably further contains a solid electrolyte described later. In addition, additives used in the positive electrode active material layer of the all solid state battery, such as a conductive additive or a binder, can be included in accordance with the intended use or intended purpose.

The material of the positive electrode active material is not particularly limited. For example, the positive electrode active material is lithium cobaltate (LiCoO ₂ ), lithium nickelate (LiNiO ₂ ), lithium manganate (LiMn ₂ O ₄ ), LiCo _1/3 Ni _1/3 Mn _1/3 O ₂ , Li _{1 + x} Li-Mn spinel or the like with a composition represented by Mn _{2- xy My} O ₄ (M is one or more metal elements selected from Al, Mg, Co, Fe, Ni, and Zn) , But is not limited thereto.

  The conductive assistant is not particularly limited. For example, the conductive assistant may be, but is not limited to, a carbon material such as VGCF (vapor grown carbon fiber, vapor grown carbon fiber) and carbon nanofiber, and a metal material.

  The binder is not particularly limited. For example, the binder may be a material such as, but not limited to, polyvinylidene fluoride (PVdF), carboxymethyl cellulose (CMC), butadiene rubber (BR), or styrene butadiene rubber (SBR).

(Solid electrolyte layer)
The solid electrolyte layer contains at least a solid electrolyte. The solid electrolyte is not particularly limited, and a material that can be used as a solid electrolyte for an all-solid battery can be used. For example, the solid electrolyte may be, but is not limited to, a sulfide solid electrolyte, an oxide solid electrolyte, a polymer electrolyte, or the like.

Examples of the sulfide solid electrolyte include, but are not limited to, a sulfide-based amorphous solid electrolyte, a sulfide-based crystalline solid electrolyte, and an aldirodite-type solid electrolyte. Examples of specific sulfide solid electrolytes include Li ₂ S—P ₂ S ₅ (Li ₇ P ₃ S ₁₁ , Li ₃ PS ₄ , Li ₈ P ₂ S _{9 and the} like), Li ₂ S—SiS ₂ , and LiI. _{-Li 2 S-SiS 2, LiI} -Li 2 S-P 2 S 5, LiI-LiBr-Li 2 S-P 2 S 5, Li 2 S-P 2 S 5 -GeS 2 (Li 13 GeP 3 S 16 , _Li 10 _GeP 2 _{S 12, etc.), LiI-Li 2 S-} P 2 O 5, LiI-Li 3 PO 4 -P 2 S 5, Li 7-x PS 6-x Cl x , and the like; or combinations thereof But not limited thereto.

Examples of the oxide solid _{electrolyte, Li 7 La 3 Zr 2 O} 12, Li 7-x La 3 Zr 1-x Nb x O 12, Li 7-3x La 3 Zr 2 Al x O 12, Li 3x La 2 / _{3-x TiO 3, Li 1} + x Al x Ti 2-x (PO 4) 3, Li 1 + x Al x Ge 2-x (PO 4) 3, Li 3 PO 4, or _{Li 3 + x PO 4-x} N x (LiPON ) And the like, but are not limited thereto.

(Polymer electrolyte)
Polymer electrolytes include, but are not limited to, polyethylene oxide (PEO), polypropylene oxide (PPO), and copolymers thereof.

  The solid electrolyte may be glass or crystallized glass (glass ceramic). Further, the solid electrolyte layer may contain a binder or the like as necessary, in addition to the solid electrolyte described above. As a specific example, it is the same as the “binder” listed in the above “positive electrode active material layer”, and the description is omitted here.

(Negative electrode active material layer)
The negative electrode active material layer contains at least a negative electrode active material, and preferably further contains the solid electrolyte described above. In addition, additives used in the negative electrode active material layer of the all-solid-state battery, such as a conductive assistant or a binder, can be included in accordance with the intended use or intended purpose.

  The material of the negative electrode active material is not particularly limited, and is preferably capable of inserting and extracting metal ions such as lithium ions. For example, the negative electrode active material may be an alloy-based negative electrode active material or a carbon material, but is not limited thereto.

  The alloy-based negative electrode active material is not particularly limited, and examples thereof include a Si alloy-based negative electrode active material and a Sn alloy-based negative electrode active material. Examples of the Si alloy-based negative electrode active material include silicon, silicon oxide, silicon carbide, silicon nitride, and solid solutions thereof. Further, the Si alloy-based negative electrode active material can include elements other than silicon, for example, Fe, Co, Sb, Bi, Pb, Ni, Cu, Zn, Ge, In, Sn, Ti, and the like. Examples of the Sn alloy-based negative electrode active material include tin, tin oxide, tin nitride, and solid solutions thereof. In addition, the Sn alloy-based negative electrode active material can include elements other than tin, for example, Fe, Co, Sb, Bi, Pb, Ni, Cu, Zn, Ge, In, Ti, Si, and the like. Among these, a Si alloy-based negative electrode active material is preferable.

  The carbon material is not particularly limited, and examples thereof include hard carbon, soft carbon, and graphite.

  For the solid electrolyte, conductive auxiliary agent, binder, and other additives used in the negative electrode active material layer, those described in the above-mentioned items of the “positive electrode active material layer” and “solid electrolyte layer” can be appropriately adopted. .

(Negative electrode current collector layer)
The conductive material used for the negative electrode current collector layer is not particularly limited, and a material that can be used for an all-solid battery can be appropriately used. For example, the conductive material used for the negative electrode current collector layer may be, but is not limited to, SUS, aluminum, copper, nickel, iron, titanium, or carbon.

  The shape of the negative electrode current collector layer is not particularly limited, and examples thereof include a foil shape, a plate shape, and a mesh shape. Among these, a foil shape is preferred.

  Note that the size of the negative electrode active material layer may be the same as or different from the size of the positive electrode active material layer, but metal ions released from the positive electrode active material layer during charging may be added to the negative electrode active material layer. From the viewpoint of reliable and smooth movement, the size of the negative electrode active material layer is preferably set to be larger than the size of the positive electrode active material layer.

  Further, the size of the positive electrode current collector layer, the negative electrode current collector layer, or the size of the positive electrode / negative electrode current collector layer may be set to be the same as the size of the solid electrolyte layer (not shown).

1a, 5a, 1b, 5b, 1c, 5c Positive electrode / negative electrode current collector layer 2a, 2b, 2c, 2d, 2e Negative electrode active material layer 3a, 3b, 3c, 3d, 3e Solid electrolyte layer 4a, 4b, 4c, 4d 4e Positive electrode active material layer 6a, 6b, 6c Unit battery 10, 20 Battery stack 11, 21 Outer case 11a Outer case accommodating part 11x, 11y Partial outer case 11b, 11c Through hole 22 Insulating layer 30, 31, 32 , 33 electrode terminals

Claims (1)

A method for manufacturing a series-stacked all-solid-state battery including the following steps:
(A) preparing an exterior body having an accommodating portion for accommodating the battery stack, wherein the exterior body has through holes at both ends in the stacking direction of the battery stack, and is divided; The battery stack comprises at least two unit batteries stacked in series, and the unit battery comprises a positive electrode current collector layer and a positive electrode active material layer. , A solid electrolyte layer, a negative electrode active material layer, and a negative electrode current collector layer in this order;
(B) The unit battery or one or a plurality of layers constituting the unit battery are sequentially inserted into the accommodating portion of the one partial exterior body within a direction ± 60 ° perpendicular to the stacking direction. thing;
(C) combining all of the partial exterior bodies to form the exterior body, thereby accommodating the battery stack in the exterior body;
(D) connecting electrode terminals to both end faces in the stacking direction of the battery stack through the through holes at both ends of the package;

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