JP6524457B2 - Method of manufacturing all solid storage device - Google Patents

Description

  The present invention relates to a method of manufacturing an all-solid storage device having a configuration in which a solid electrolyte layer is disposed between a positive electrode layer and a negative electrode layer.

  In Patent Document 1, an electronic circuit is formed on a first surface of a first insulating substrate, and a positive electrode current collector, a positive electrode layer, and an electrolyte layer are sequentially formed on a second surface of the first insulating substrate, A battery integrated circuit device in which a negative electrode current collector, a negative electrode layer, and an electrolyte layer are sequentially formed on an insulating substrate of No. 2 and their electrolyte layers are bonded together so that the positive electrode layer and the negative electrode layer face each other. Is disclosed. In this battery integrated circuit device, a polymer electrolyte layer as a solid polymer electrolyte layer membrane is used for the electrolyte layer. The polymer electrolyte layer includes polyethylene oxide as a main component of the polymer, and may contain a lithium salt.

JP 2005-339825 A

  However, when using, for example, a solid electrolyte of lithium-containing metal oxide type for the electrolyte layer, unevenness due to the fine particles of the solid electrolyte is formed on the surface of the electrolyte layer, so two electrolyte layers on the positive electrode side and the negative electrode side are There is a problem that the contact area when pasted together becomes small. Furthermore, there is also a problem that the adhesion is insufficient. For this reason, since the ion conduction between the bonded electrolyte layers becomes inadequate, it was difficult to exhibit the high charging / discharging performance as a secondary battery.

  Then, an object of this invention is to provide the manufacturing method of the all-solid-state electricity storage device which can ensure the contact area between two electrolyte layers by the side of a positive electrode layer and a negative electrode layer, and can improve charge / discharge performance.

In order to solve the above problems, the method for producing an all solid storage device of the present invention comprises the steps of: forming a positive electrode current collector on a first insulating substrate; forming a positive electrode layer on the positive electrode current collector; The steps of forming a first solid electrolyte layer on the positive electrode layer, forming the negative electrode current collector on the second insulating substrate, forming the negative electrode layer on the negative electrode current collector, and A step of forming a solid electrolyte layer, a step of forming an adhesive layer on at least one of the first solid electrolyte layer and the second solid electrolyte layer, a first solid electrolyte layer and a second solid electrolyte layer by the adhesive layer and a bonding step of bonding together, the adhesive layer is observed containing a polymer solid electrolyte and a solvent, the first solid electrolyte layer and the second solid electrolyte layer are respectively made of a solid electrolyte and a binder, the binder polymer solid electrolyte It is characterized by including .

  Thereby, the contact area between the two electrolyte layers on the positive electrode layer side and the negative electrode layer side can be secured to enhance the charge / discharge performance.

In addition , the first solid electrolyte layer, the adhesive layer, and the second solid electrolyte layer, which are adjacent to each other, include a solid polymer electrolyte, which can contribute to the improvement of charge and discharge characteristics.

  In the method of manufacturing an all-solid storage device of the present invention, the polymer solid electrolyte preferably contains lithium bis (trifluoromethanesulfonyl) imide.

In the method for manufacturing all-solid energy storage device of the present invention, it is preferred solid electrolyte is Li-Al-Ti-PO ₄ based solid electrolyte.

In the method of manufacturing an all-solid storage device of the present invention, the solid electrolyte is preferably Li _1.3 Al _0.3 Ti _1.7 (PO ₄ ) ₃ .

  In the method for producing an all solid storage device of the present invention, the solvent is preferably γ-butyrolactone or acetonitrile.

  In the method of manufacturing an all-solid storage device of the present invention, the binder preferably contains an ethylene propylene / polypropylene copolymer and γ-butyrolactone or acetonitrile.

  In the method for producing an all-solid storage device of the present invention, the binder preferably contains polyethylene oxide or ethylene oxide / propylene oxide copolymer, and γ-butyrolactone or acetonitrile.

  In the method of manufacturing an all solid storage device of the present invention, it is preferable that the first solid electrolyte layer and the second solid electrolyte layer be bonded by thermocompression bonding in the bonding step.

  According to the present invention, the contact area between the two electrolyte layers on the positive electrode layer side and the negative electrode layer side can be secured to enhance charge and discharge performance.

It is a sectional view showing the composition of the all-solid-state storage device concerning the embodiment of the present invention, and is a figure showing the state before bonding the 1st solid electrolyte layer and the 2nd solid electrolyte layer. It is a sectional view showing the composition of the all-solid storage device concerning the embodiment of the present invention, and is a figure showing the state after joining the 1st solid electrolyte layer and the 2nd solid electrolyte layer. It is a graph which shows the charge / discharge characteristic about one sample of Example 3 of Table 1. It is a graph which shows the charge / discharge characteristic about the sample different from FIG. 3 among Example 3 of Table 1. FIG. It is a graph which shows the charge / discharge characteristic about one sample of Example 4 of Table 1. It is a graph which shows the charge / discharge characteristic about the sample different from FIG. 5 among Example 4 of Table 1. FIG. It is a graph which shows the charge / discharge characteristic about one sample of Example 5 of Table 1. It is a graph which shows the charge / discharge characteristic about the sample different from FIG. 7 among Example 5 of Table 1. FIG. It is a graph which shows the charge / discharge characteristic about one sample of Example 6 of Table 1. It is a graph which shows the charge / discharge characteristic about the sample different from FIG. 9 among Example 6 of Table 1. FIG. It is a graph which shows the charge / discharge characteristic about one sample of Example 7 of Table 1. It is a graph which shows the charge / discharge characteristic about one sample of Example 9 of Table 1. It is a graph which shows the charging / discharging characteristic about one sample of Example 10 of Table 1. FIG. It is a graph which shows the charge / discharge characteristic about the sample different from FIG. 13 among Example 10 of Table 1. FIG. It is a graph which shows the charging / discharging characteristic about one sample of Example 11 of Table 1. FIG.

  Hereinafter, the manufacturing method of the all-solid-state storage device concerning the embodiment of the present invention is explained in detail, referring to drawings.

  1 and 2 are cross-sectional views showing the configuration of the all-solid-state storage device 10 according to the present embodiment, and FIG. 1 is a state before the first solid electrolyte layer 24 and the second solid electrolyte layer 34 are joined. FIG. 2 shows the state after the first solid electrolyte layer 24 and the second solid electrolyte layer 34 are joined. The Z direction shown in FIGS. 1 and 2 is the stacking direction (thickness direction), and the XY plane is a plane orthogonal to the Z direction. In the following description, the Z direction may be referred to as the upward direction.

  As shown in FIG. 1 and FIG. 2, the all solid storage device 10 includes a positive electrode structure 20, a negative electrode structure 30, and an adhesive layer 40. The positive electrode structure 20 includes a first insulating substrate 21, a positive electrode current collector 22 formed on the first insulating substrate 21, a positive electrode layer 23 formed on the positive electrode current collector 22, and a positive electrode layer 23. And the formed first solid electrolyte layer 24. The negative electrode structure 30 includes a second insulating substrate 31, a negative electrode current collector 32 formed on the second insulating substrate 31, a negative electrode layer 33 formed on the negative electrode current collector 32, and a negative electrode layer 33. And the formed second solid electrolyte layer 34.

  As the first insulating substrate 21 and the second insulating substrate 31, for example, a glass substrate or a resin substrate of epoxy, phenol or the like can be used, and in the case where it is preferable to have flexibility, polyimide, polyester or polyamide It is also possible to use a flexible substrate by the like.

  The positive electrode current collector 22 uses, for example, aluminum foil or stainless steel foil, and the negative electrode current collector 32 uses, for example, copper foil or stainless steel foil.

The positive electrode layer 23 is formed by screen printing an ink-like positive electrode paste. The components contained in the positive electrode paste include a positive electrode active material, a conductive material, a solid electrolyte, a binder, and a solvent, and at least the positive electrode active material and the solvent are contained. As the positive electrode active material, for example, a Li-Mn based composite oxide such as lithium manganate (LiMn ₂ O ₄ ) or a Li-Ni based composite oxide such as lithium nickelate (LiNiO ₂ ) is used. Examples of the solvent include acetoanilyl and γ-butyrolactone. It is preferable to use acetylene black as the conductive material. As the solid electrolyte, it is preferable to use powdery Li ₂ O-Al ₂ O ₃ -Ti ₂ O-P ₂ O ₅ based solid electrolyte (LATP), and as LATP, for example, Li _{1 + x} Al _x Ti _2-x What is represented by (PO ₄ ) ₃ (x is 0 <x ≦ 0.5) is used. An ion conductive resin is used as the binder, and examples thereof include polyethylene oxide, ethylene oxide / propylene oxide copolymer, polyvinylidene fluoride, and may contain lithium bis (trifluoromethanesulfonyl) imide as a lithium salt. In the following description, the baking conditions after printing are preferably set according to the type of solvent, and when γ-butyrolactone is used, for example, 100 ° C. for 60 minutes.

The negative electrode layer 33 is formed by screen printing an ink-like negative electrode paste. The components contained in the negative electrode paste include a negative electrode active material, a conductive material, a solid electrolyte powder, a binder, and a solvent, and at least the negative electrode active material and the solvent are contained. Examples of the negative electrode active material include crystalline carbon materials and non-crystalline carbon materials. For example, one or more of natural graphite, artificial graphite, carbon black, activated carbon, carbon fiber, coke, soft carbon and hard carbon Use It is preferable to use acetylene black as the conductive material. As the solid electrolyte, it is preferable to use powdery Li ₂ O-Al ₂ O ₃ -Ti ₂ O-P ₂ O ₅ based solid electrolyte (LATP), and as LATP, for example, Li _{1 + x} Al _x Ti _2-x What is represented by (PO ₄ ) ₃ (x is 0 <x ≦ 0.5) is used. An ion conductive resin is used as the binder, and examples thereof include polyethylene oxide, ethylene oxide / propylene oxide copolymer, polyvinylidene fluoride, and may contain lithium bis (trifluoromethanesulfonyl) imide as a lithium salt. Examples of the solvent include acetoanilyl and γ-butyrolactone.

  The positive electrode paste and the negative electrode paste preferably have adjusted physical property values, particularly the viscosity, so that the positive electrode layer 23 or the negative electrode layer 33 is formed to have a desired film thickness. The viscosity may be performed by changing the ratio of the solvent contained in each paste and the contained components other than the solvent.

  The first solid electrolyte layer 24 and the second solid electrolyte layer 34 are formed by screen printing an electrolyte paste and baking the paste at a predetermined temperature for a predetermined time. The electrolyte paste contains a powdery solid electrolyte and a binder.

As the solid electrolyte, it is preferable to use a Li-Al-Ti-PO ₄ -based solid electrolyte (LATP), and as LATP, for example, _one represented by Li _{1 + x} Al _x Ti _2-x (PO ₄ ) ₃ (x Uses 0 <x ≦ 0.5).

  As the binder, a polymer solid electrolyte is preferably used, and a lithium salt such as lithium bis (trifluoromethanesulfonyl) imide (LiTFSI), ethylene oxide / propylene oxide copolymer (EO / PO copolymer) or polyethylene oxide (PEO), polymers such as polyvinylidene fluoride (PVdF), solvents such as acetoanilyl, or gamma-butyrolactone.

  In the preparation of the binder of the electrolyte paste, the lithium salt is preferably first dissolved in the solvent, but alternatively, the polymer may be first dissolved in the solvent and then the lithium salt may be dissolved. In addition, it is preferable to adjust the physical property value, particularly the viscosity, of the electrolyte paste so that the first solid electrolyte layer 24 or the second solid electrolyte layer 34 is formed to have a desired film thickness.

  The adhesive layer 40 is obtained by dropping an adhesive on at least one of the first solid electrolyte layer 24 and the second solid electrolyte layer 34 and performing thermocompression bonding while applying pressure between the positive electrode structure 20 and the negative electrode structure 30. It is formed. The adhesive contains a lithium salt, a polymer, and a solvent. Similar to the first solid electrolyte layer 24 and the second solid electrolyte layer 34, lithium bis (trifluoromethanesulfonyl) imide (LiTFSI) is used as the lithium salt. As the polymer, for example, ethylene oxide / propylene oxide copolymer (EO / PO copolymer), polyethylene oxide (PEO), polyvinylidene fluoride (PVdF) or the like is used. As a solvent, for example, γ-butyrolactone or acetonitrile is used.

Next, a method of manufacturing the all-solid storage device 10 will be described.
The all solid storage device 10 first forms the positive electrode structure 20 and the negative electrode structure 30 respectively, and then uses the adhesive layer 40 to form the first solid electrolyte layer 24 of the positive electrode structure 20 and the second solid electrolyte layer of the negative electrode structure 30. The positive electrode structure 20 and the negative electrode structure 30 are integrated by joining the electrodes 34 together. Each step will be described below.

  As the formation of the positive electrode structure 20, first, the first surface 21a (the upper surface in the Z direction in FIG. 1 and FIG. 2) of the first insulating substrate 21 is disposed upward to a predetermined range of the first surface 21a. An aluminum foil or the like as the positive electrode current collector 22 is disposed and attached by adhesion. Next, the positive electrode paste is screen-printed on the first surface 22 a (the upper surface in the Z direction) of the positive electrode current collector 22 and baked to form the positive electrode layer 23. Subsequently, the electrolyte paste is screen-printed on the first surface 23 a (surface on the upper side in the Z direction) of the positive electrode layer 23 and fired to form the first solid electrolyte layer 24.

  In forming the negative electrode structure 30, first, the first surface 31a (the surface on the lower side in the Z direction of FIGS. 1 and 2) of the second insulating substrate 31 is disposed upward, and the negative electrode structure 30 is formed in a predetermined range of the first surface 31a. A copper foil or the like as the negative electrode current collector 32 is disposed and attached by adhesion. Next, the negative electrode paste is screen-printed on the first surface 32 a (the lower surface in the Z direction) of the negative electrode current collector 32 and baked to form the negative electrode layer 33. Subsequently, the electrolyte paste is screen-printed on the first surface (surface on the lower side in the Z direction) of the negative electrode layer 33 and baked to form the second solid electrolyte layer 34.

Next, as shown in FIG. 1, after a predetermined amount of adhesive is dropped on the first surface 24 a of the first solid electrolyte layer 24, the first surface 34 a of the second solid electrolyte layer 34 is made the first solid electrolyte layer 24. The adhesive layer 40 is formed between the first surface 24 a and the first surface 34 a by opposing the first surface 24 a and sandwiching the first surface 24 a with a predetermined pressure. In this state, thermocompression bonding is performed under a predetermined temperature, time, pressure and atmosphere. The conditions for thermocompression bonding are, for example, a pressure of about 10 kg / cm ² or less for 1 minute at 150 ° C. in a nitrogen atmosphere. By this thermocompression bonding, as shown in FIG. 2, the adhesive spreads over the entire surface of the first surface 24a of the first solid electrolyte layer 24 and the first surface 34a of the second solid electrolyte layer 34, and solidifies to a predetermined thickness. Thereby, the first solid electrolyte layer 24 of the positive electrode structure 20 and the second solid electrolyte layer 34 of the negative electrode structure 30 are bonded to each other, and the positive electrode structure 20 and the negative electrode structure 30 are integrated. The solvent in the adhesive layer of the integrated all solid storage device is removed by vacuum heat drying at 80 ° C.

Next, an example of the present embodiment will be described.
Table 1 is a table showing manufacturing conditions and evaluation results of Examples 1 to 11 of the present embodiment. FIGS. 4-15 is a graph which shows the charging / discharging characteristic about the sample of an Example, and the relationship of each figure and an Example is as follows.

  Fig. 3 · Fig. 4: Example 3 of Table 1, Fig. 5 · Fig. 6: Example 4, Fig. 7 · Fig. 8: Example 5, Fig. 9 · Fig. 10: Example 6, Fig. 11: Example 7, 12: Example 9, FIG. 13 and FIG. 14: Example 10, FIG. 15: Example 11.

For each example shown in Table 1, two samples were prepared and evaluated.
(A) The constitution of each layer of the embodiment shown in Table 1 is as follows.

<Insulating substrate>
The first insulating substrate 21 and the second insulating substrate 31 are glass substrates having a thickness of 0.5 mm.

<Current collector>
(1) Examples 1 to 6
As a positive electrode current collector 22 ("commercially available positive electrode" in Table 1) on which the positive electrode layer 23 was formed, a positive electrode (model number: EQ-Lib-LMO) manufactured by MTI Corporation was used. Moreover, the electrode for negative electrodes (model number: EQ-Lib-CMSG) of MTI company was used as a negative electrode collector 32 ("commercially available negative electrode" of Table 1) in which the negative electrode layer 33 was formed.
The positive electrode current collector 22 is an aluminum foil having a thickness of 25 μm, and is attached by pressure bonding to the first insulating substrate 21.
The negative electrode current collector 32 is a copper foil having a thickness of 25 μm, and is attached by pressure bonding to the second insulating substrate 31.

(2) Examples 7 to 11
The positive electrode current collector 22 and the negative electrode current collector 32 are stainless steel foils each having a thickness of 0.1 mm, and are attached by pressure bonding to the first insulating substrate 21 or the second insulating substrate 31. .

<Electrode layer>
(1) Examples 1 to 6
The positive electrode layer 23 is formed with a 140 μm-thick positive electrode layer using lithium manganate as a positive electrode active material.
In the negative electrode layer 33, a 100 μm-thick negative electrode layer is formed using mesocarbon microbeads (spherical artificial graphite) as a negative electrode active material.

(2) Examples 7 to 11
The positive electrode layer 23 formed a positive electrode layer with a thickness of about 50 μm using lithium manganate as a positive electrode active material. In Examples 7 to 8, lithium manganate was not crushed, and in Examples 9 to 11, lithium manganate was crushed. Lithium manganate has a particle size of about 5 to 20 [mu] m in an uncrushed form and a particle size of about 0.5 [mu] m in a crushed form.
The negative electrode layer 33 used hard carbon as a negative electrode active material, and formed the negative electrode layer about 50 micrometers thick.

<Solid electrolyte layer>
The electrolyte paste used to form the first solid electrolyte layer 24 and the second solid electrolyte layer 34 is common, and the composition of the material of the electrolyte paste shown in Table 1 is as follows.

(1) LP-1
LATP01 (solid electrolyte): 95 wt% (wt%)
Binder: 5 wt%
Here, the binder is an ethylene oxide-propylene oxide copolymer, and LiTFSI is not added.

(2) LP-2
LATP01 (solid electrolyte): 95 wt%
Binder: 5 wt%
Here, the binder is a polymer solid obtained by dissolving 15 wt% of ethylene oxide-propylene oxide copolymer in γ-butyrolactone and then adding 0.25 mol (0.25 M) of LiTFSI under a low humidity of about 2% RH. It is solid content of electrolyte.

(3) LP-3:
LATP01 (solid electrolyte): 95 wt%
Binder: 5 wt%
Here, the binder is the solid content of a solid polymer electrolyte in which 15 wt% of ethylene oxide-propylene oxide copolymer is dissolved after 0.25 mol of LiTFSI is added to γ-butyrolactone.

  The number of printed layers of the electrolyte paste was once or twice, and was fired at 100 ° C. for 60 minutes each time of printing. The thickness of the solid electrolyte layer formed by this was 50 to 80 μm in the case of one printed layer, and was 80 to 120 μm in the case of two layers.

<Adhesive layer>
The composition of the adhesive used to form the adhesive layer 40 is
It is a polymer electrolyte in which 15 wt% of ethylene oxide / propylene oxide copolymer is dissolved after adding 5 mol of LiTFSI to γ-butyrolactone or acetonitrile as a solvent.

The adhesive is dropped on the first surface 24a of the first solid electrolyte layer 24 by 1.5 to 7.5 microliters per square centimeter of the battery effective area, and then the first surface 34a of the second solid electrolyte layer 34 is formed. The adhesive layer 40 is sandwiched between the first surface 24 a and the first surface 34 a at a pressure of about 10 kg / cm ² or less while facing the first surface 24 a of the first solid electrolyte layer 24. In this state, thermocompression bonding is performed at 150 ° C. for 1 minute in a nitrogen atmosphere (relative humidity 2% RH or less). The solvent of the adhesive layer after thermocompression bonding is removed by vacuum heating and drying at 80.degree.

(B) The evaluation results of the example will be described.
The evaluation column of Table 1 has shown the evaluation result of the charge / discharge characteristic about two samples with respect to each manufacturing condition of Examples 1-11. This evaluation is carried out with a current load of 1 mA in a nitrogen-purged glove box with a humidity of 2% or less, a cutoff voltage of 4.1 V-0.1 V, and basically one charge / discharge cycle. And

  In Table 1, "(circle)" has shown the case where charge / discharge characteristics were favorable by two samples. In the case of “Δ”, one sample has good charge / discharge characteristics but the other sample can not be charged / discharge or has low charge / discharge characteristics. Here, that the charge and discharge characteristics are good means that the discharge time is long in the constant current charge and discharge test.

  In Example 3 shown in FIG. 3 and FIG. 4, charging exceeding 3 V is possible in the charging shown by the solid line, and discharging continues for 1300 seconds or more in the discharging shown by the broken line, and the charge / discharge characteristics become good. ing. In Example 4 shown in FIG. 5 and FIG. 6, charging exceeding 3 V is possible, and the discharge is sustained for about 600 seconds or more, and the charge / discharge characteristics are good. In Example 5 shown in FIG. 7 and FIG. 8, charging exceeding 3 V is possible, and discharge is continued for 2000 seconds or more, and charge / discharge characteristics are good. In Example 6 shown in FIG. 9 and FIG. 10, charging exceeding 3 V is possible, and the discharge is sustained for about 800 seconds or more, and the charge / discharge characteristics are good. In Example 7 shown in FIG. 11, charging exceeding 3 V is possible, and discharge is continued for 2000 seconds or more, and charge / discharge characteristics are good. In Example 9 shown in FIG. 12, charging of over 3 V is possible with respect to a current load of 0.1 mA, and the discharge is maintained for about 2000 seconds, and the charge and discharge characteristics are good. In Example 10 shown in FIG. 13 and FIG. 14, charging exceeding 3 V is possible, and discharge is sustained for 1000 seconds or more, and charge / discharge characteristics are good. In Example 11 shown in FIG. 15, charging exceeding 3 V is possible, and discharging is continued for 1000 seconds or more, and charge / discharge characteristics are good.

  Although the present invention has been described with reference to the above embodiment, the present invention is not limited to the above embodiment, and can be improved or changed within the scope of the improvement purpose or the spirit of the present invention.

  As mentioned above, the manufacturing method of the all-solid-state storage device concerning the present invention is useful to improvement of charge-and-discharge characteristic of a device of composition of which electrolyte layers were pasted together so that a positive electrode layer and a negative electrode layer may face.

10 all-solid storage device 20 positive electrode structure 21 first insulating substrate 22 positive electrode current collector 23 positive electrode layer 24 first solid electrolyte layer 30 negative electrode structure 31 second insulating substrate 32 negative electrode current collector 33 negative electrode layer 34 second solid electrolyte Layer 40 Adhesive Layer

Claims (8)

Forming a positive electrode current collector on the first insulating substrate;
Forming a positive electrode layer on the positive electrode current collector;
Forming a first solid electrolyte layer on the positive electrode layer;
Forming a negative electrode current collector on the second insulating substrate;
Forming a negative electrode layer on the negative electrode current collector;
Forming a second solid electrolyte layer on the negative electrode layer;
Forming an adhesive layer on at least one of the first solid electrolyte layer and the second solid electrolyte layer;
And a bonding step of bonding the first solid electrolyte layer and the second solid electrolyte layer to each other by the adhesive layer,
The adhesive layer viewing contains a polymer solid electrolyte and a solvent,
The first solid electrolyte layer and the second solid electrolyte layer each comprise a solid electrolyte and a binder,
The method of manufacturing an all-solid storage device, wherein the binder comprises the solid polymer electrolyte . The method for producing an all-solid storage device according to claim 1 , wherein the solid polymer electrolyte contains lithium bis (trifluoromethanesulfonyl) imide. Method for manufacturing an all-solid battery device according to claim 1 or claim 2, wherein the solid electrolyte is Li-Al-Ti-PO ₄ based solid electrolyte. Method for manufacturing an all-solid battery device according to claim 3 wherein the solid electrolyte which is a _{Li 1.3 Al 0.3 Ti 1.7 (PO} 4) 3. The said solvent is (gamma) -butyrolactone or acetonitrile, The manufacturing method of the all-solid-state electrical storage device of any one of the Claims 1-4 characterized by the above-mentioned. The said binder contains an ethylene propylene / polypropylene copolymer, (gamma) -butyrolactone, or acetonitrile, The manufacturing method of the all-solid-state electrical storage device of any one of the Claims 1-5 characterized by the above-mentioned. The said binder contains a polyethylene oxide or ethylene oxide propylene oxide copolymer, (gamma) -butyrolactone or acetonitrile, The manufacturing of the all-solid-state electrical storage device of any one of the Claims 1-5 characterized by the above-mentioned. Method. The all-solid storage device according to any one of claims 1 to 7 , wherein in the bonding step, the first solid electrolyte layer and the second solid electrolyte layer are bonded by thermocompression bonding. Production method.