Peeling mechanism and peeling method

Abstract

The present invention provides a peeling mechanism and peeling method that can improve the accuracy of peeling a substrate from a solid electrolyte layer. [Solution] A peeling mechanism 132 for peeling a base sheet 123 from a first solid electrolyte layer SE1 transferred to a positive electrode side sheet member 200, comprising a peeling roller 130 for peeling the base sheet 123 from the first solid electrolyte layer SE1, and a base roll body 131 for winding up the base sheet 123 peeled off by the peeling roller 130, wherein the peeling roller 130 peels the base sheet 123 in the opposite direction to the transport direction of the positive electrode side sheet member 200.

Description

Technical Field

[0001] The present invention relates to a peeling mechanism and a peeling method.

Background Art

[0002] In recent years, in order to enable more people to access affordable, reliable, sustainable, and advanced energy, research and development on secondary batteries that contribute to energy efficiency have been carried out.

[0003] Conventionally, as a method for manufacturing a solid battery, a method of manufacturing by pressing a positive electrode layer, a solid electrolyte layer, and a negative electrode layer with a roll is known (for example, Patent Document 1).

Prior Art Documents

Patent Documents

[0004]

Patent Document 1

Summary of the Invention

Problems to be Solved by the Invention

[0005] In the transfer of the solid electrolyte layer to the positive electrode layer, after transferring the solid electrolyte layer provided on the base material to the positive electrode layer by roll pressing, the base material is peeled off from the solid electrolyte layer, but there is a risk that the accuracy of peeling the base material may decrease.

[0006] The present invention provides a peeling mechanism and a peeling method capable of improving the accuracy when peeling the base material from the solid electrolyte layer. And, by extension, it contributes to energy efficiency.

Means for Solving the Problems

[0007] One aspect of the present invention is a peeling mechanism for peeling a base material from a transfer body transferred to a base material sheet, A peeling roller for peeling the substrate from the transfer body, The system comprises a base material roll body for winding up the base material peeled off by the peeling roller, The aforementioned peeling roller is The base material is peeled off in the direction opposite to the transport direction of the base material sheet.

[0008] Furthermore, other embodiments of the present invention include: A peeling method for peeling a substrate from a transfer body transferred to a base material sheet, A recognition step of recognizing the peeling initiation point where the substrate peels off, A peeling initiation point control step that controls the peeling initiation point to be at a predetermined position, The system includes a peeling step of peeling the substrate in the opposite direction to the transport direction of the base material sheet, based on a peeling initiation point controlled to a predetermined position. [Effects of the Invention]

[0009] According to the present invention, it is possible to improve the accuracy of peeling the substrate sheet from the solid electrolyte layer. This, in turn, can contribute to energy efficiency. [Brief explanation of the drawing]

[0010] [Figure 1] Figure 1 is a cross-sectional view showing an example of a solid-state battery 1. [Figure 2] Figure 2 shows an example of a press machine 100 used to manufacture a solid-state battery 1. [Figure 3] Figure 3 is a diagram showing a part of the press apparatus 100, and in particular, it is a diagram illustrating an example of a configuration in which the base sheet 123 is peeled off after the first solid electrolyte layer SE1 has been transferred. [Figure 4] Figure 4 is a diagram illustrating an example of the peeling mechanism 132. [Figure 5] Figure 5 shows a part of the press apparatus 100, and in particular, it shows an example of the transfer of the intermediate layer transfer roller 150 and the negative electrode side transfer roller 160. [Figure 6]FIG. 6 is a flowchart showing an example of the pressing method of the pressing device 100 including the peeling method. [Figure 7] FIG. 7 is a diagram for explaining another example of the peeling mechanism 132. [Figure 8] FIG. 8 is a diagram showing a comparative example of the peeling mechanism 132a.

Mode for Carrying Out the Invention

[0011] Hereinafter, an embodiment will be described with reference to the drawings. The peeling mechanism 132 in the embodiment is a part of the pressing device 100 for manufacturing the solid-state battery 1. Further, the peeling method is a part of the pressing method using the pressing device 100. In the following description, the solid-state battery 1, the pressing device 100 including the peeling mechanism 132, and the pressing method including the peeling method will be described in this order.

[0012] [Solid-State Battery] FIG. 1 is a schematic diagram showing an example of the solid-state battery 1. The solid-state battery 1 is an all-solid-state battery having an electrode 10 in which a negative electrode layer 2, a solid electrolyte layer 3, and a positive electrode layer 4 are laminated. In the embodiment, as shown in FIG. 1, the structure in which the negative electrode layer 2, the solid electrolyte layer 3, the positive electrode layer 4, the solid electrolyte layer 3, and the negative electrode layer 2 are laminated in this order will be described as the laminated structure of the solid-state battery 1. Note that the structure of the solid-state battery 1 is not limited to the above. The solid-state battery 1 may have a configuration that can be used for a solid-state battery such as an exterior body in addition to the electrode 10 shown in FIG. 1.

[0013] The solid electrolyte layer 3 in the solid-state battery 1 has at least a first solid electrolyte layer SE1 disposed on the positive electrode layer 4 side and a negative electrode side solid electrolyte layer SE3 disposed on the negative electrode layer 2 side. The solid electrolyte layer 3 may have a second solid electrolyte layer SE2 disposed adjacent to the first solid electrolyte layer SE1. In the embodiment, the solid electrolyte layer 3 will be described as being composed of the above three layers. An intermediate layer 5 may be arbitrarily disposed between the negative electrode layer 2 and the solid electrolyte layer 3.

[0014] The solid-state battery 1 is not particularly limited and may be a lithium-ion solid-state secondary battery or a lithium metal secondary battery.

[0015] (Negative electrode layer) The negative electrode layer 2 includes a negative electrode active material layer 21 and a negative electrode current collector layer 22. The negative electrode active material layer 21 is not particularly limited and can be composed of a material that can be used as the negative electrode active material of the solid-state battery 1. Examples of the negative electrode active material constituting the negative electrode active material layer 21 include lithium metal, lithium alloy, silicon-based active materials such as Si and Si alloy, lithium transition metal oxides such as lithium titanate (Li4Ti5O 12 ), etc., transition metal oxides such as TiO2, Nb2O3, and WO3, metal sulfides, metal nitrides, carbon materials such as graphite, soft carbon, and hard carbon, and metal indium, etc.

[0016] The negative electrode active material layer 21 may contain materials other than those described above that can be contained in the negative electrode active material layer 21 of the solid-state battery 1. Examples of such materials include, for example, solid electrolytes, conductive aids, binders, etc. Examples of the solid electrolyte include the same ones as those contained in the solid electrolyte layer 3 described later. Examples of the conductive aid include carbon black, natural graphite, carbon fiber, carbon nanotube, etc. Examples of the binder include nitrile-based polymers, polyester-based polymers, acrylic acid-based polymers, cellulose-based polymers, styrene-based polymers, styrene-butadiene-based polymers, vinyl acetate-based polymers, urethane-based polymers, fluoroethylene-based polymers, etc.

[0017] The negative electrode current collector layer 22 is not particularly limited and can be composed of copper, nickel, stainless steel, etc. Examples of the shape of the negative electrode current collector layer 22 include, for example, foil shape, plate shape, mesh shape, non-woven fabric shape, foamed shape, etc. In an embodiment, the negative electrode current collector layer 22 is composed of a negative electrode current collector foil 22a.

[0018] (Solid electrolyte layer) The solid electrolyte layer 3 is formed between the negative electrode layer 2 and the positive electrode layer 4. In this embodiment, the solid electrolyte layer 3 has a structure in which a first solid electrolyte layer SE1, which is placed in contact with the positive electrode layer, a second solid electrolyte layer SE2, and a negative electrode side solid electrolyte layer SE3, which is placed on the negative electrode side, are stacked in this order.

[0019] The first solid electrolyte layer SE1 is positioned in contact with the positive electrode active material layer 41 in the positive electrode layer 4. The solid electrolyte constituting the first solid electrolyte layer SE1 is not particularly limited and can be any material that can be used as an electrolyte in a solid-state battery. Examples include inorganic solid electrolytes such as sulfide solid electrolytes, oxide solid electrolytes, halide solid electrolytes, and lithium-containing salts, as well as polymer-based solid electrolytes such as polyethylene oxide. One type of the above solid electrolyte may be used, or two or more types may be used in combination.

[0020] Furthermore, the first solid electrolyte layer SE1 contains a binder in addition to the solid electrolyte material. The binder can be the same material as the binder that can be contained in the negative electrode active material layer 21. The binder content in the first solid electrolyte layer SE1 relative to the total mass of the first solid electrolyte layer SE1 is equal to or greater than the binder content in the second solid electrolyte layer SE2 relative to the total mass of the second solid electrolyte layer SE2. The upper limit of the binder content in the first solid electrolyte layer SE1 is, for example, 25% by mass. Preferably, the binder content in the first solid electrolyte layer SE1 is 10 to 30% by mass. This makes it easier for the first solid electrolyte layer SE1 to stretch in accordance with the positive electrode layer 4 when the positive electrode layer 4 is pressed.

[0021] In addition to the solid electrolyte material and binder, the first solid electrolyte layer SE1 may also contain materials that can be used in the solid electrolyte layer of a solid-state battery.

[0022] Furthermore, the thickness of the first solid electrolyte layer SE1 (length in the stacking direction of each layer) is preferably thinner than the thickness of the second solid electrolyte layer SE2. The thickness of the first solid electrolyte layer SE1 is preferably, for example, 3 to 15 μm.

[0023] The second solid electrolyte layer SE2 is an arbitrarily placed layer and is positioned adjacent to the first solid electrolyte layer SE1. The solid electrolyte material constituting the second solid electrolyte layer SE2 is not particularly limited and can be the same as the solid electrolyte material constituting the first solid electrolyte layer SE1. The second solid electrolyte layer SE2 may contain a binder or the like in addition to the solid electrolyte material, similar to the first solid electrolyte layer SE1. The binder content of the second solid electrolyte layer SE2 is less than or equal to the binder content of the first solid electrolyte layer SE1. The binder content of the second solid electrolyte layer SE2 is preferably, for example, 10 to 30 mass%. This can improve the energy density of the solid battery 1. The second solid electrolyte layer SE2 may contain a support. The support may be a three-dimensional structure such as a mesh, woven fabric, nonwoven fabric, embossed body, punched body, expanded, or foam. The second solid electrolyte layer SE2 does not need to contain the support.

[0024] The thickness of the second solid electrolyte layer SE2 (length in the stacking direction of each layer) is preferably greater than the thickness of the first solid electrolyte layer SE1. Furthermore, the thickness of the second solid electrolyte layer SE2 is preferably greater than the thickness of the negative electrode side solid electrolyte layer SE3, which will be described later. The thickness of the second solid electrolyte layer SE2 is preferably, for example, 10 to 50 μm.

[0025] The negative electrode solid electrolyte layer SE3 is located on the negative electrode layer side. The negative electrode solid electrolyte layer SE3 is located adjacent to the negative electrode layer 2. If the solid battery 1 has an intermediate layer 5 as shown in Figure 1, the negative electrode solid electrolyte layer SE3 may be located adjacent to the intermediate layer 5.

[0026] The solid electrolyte material constituting the negative electrode solid electrolyte layer SE3 is not particularly limited and can be the same as the solid electrolyte material constituting the first solid electrolyte layer SE1. The binder content of the negative electrode solid electrolyte layer SE3 is preferably, for example, 1.3 to 8.7 mass%. In terms of volume%, the binder content of the negative electrode solid electrolyte layer SE3 is preferably, for example, 2.7 volume% to 10 volume%. The binder content of the negative electrode solid electrolyte layer SE3 is less than the binder content of the first solid electrolyte layer SE1.

[0027] The thickness of the negative electrode solid electrolyte layer SE3 (length in the stacking direction of each layer) is preferably thinner than the thickness of the second solid electrolyte layer SE2. The thickness of the negative electrode solid electrolyte layer SE3 is preferably, for example, 3 to 8.5 μm.

[0028] (Positive electrode layer) The positive electrode layer 4 comprises a positive electrode active material layer 41 and a positive electrode current collector layer 42. In one embodiment, the positive electrode layer 4 has a configuration in which two positive electrode active material layers 41 are laminated on both sides of one positive electrode current collector layer 42. However, the configuration of the positive electrode layer 4 is not limited to the above, and it may have a configuration in which one positive electrode active material layer 41 is laminated on one side of one positive electrode current collector layer 42.

[0029] The positive electrode active material layer 41 is not particularly limited and can be composed of a material that can be used as a positive electrode active material in a solid-state battery. Examples of positive electrode active materials that make up the positive electrode active material layer 41 include LiCoO2, LiNiO2, and LiCo x Ni y Mn z Layered cathode active material particles such as O2(x+y+z=1), LiVO2, LiCrO2, LiMn2O4, Li(Ni 0.25 Mn 0.75Examples of positive electrode active materials include spinel-type positive electrode active materials such as 2O4, LiCoMnO4, and Li2NiMn3O8; olivine-type positive electrode active materials such as LiCoPO4, LiMnPO4, and LiFePO4; conductive polymers such as solid solution oxides (Li2MnO3-LiMO2 (M=Co, Ni, etc.)), polyaniline, and polypyrrole; sulfides such as Li2S, CuS, Li-Cu-S compounds, TiS2, FeS, MoS2, and Li-Mo-S compounds; and mixtures of sulfur and carbon. The positive electrode active material may consist of one of the above materials or a composition of two or more of the above materials.

[0030] The positive electrode active material layer 41 may contain a binder or the like. The binder content of the positive electrode active material layer 41 is preferably 0.5 to 5% by mass. Preferably, it may be 2.56% by mass. The thickness of the positive electrode active material layer 41 (length in the stacking direction of each layer) is preferably, for example, 80 to 100 μm. This improves the battery capacity of the solid-state battery 1.

[0031] The positive electrode current collector layer 42 is not particularly limited, but can be made of, for example, aluminum, stainless steel, conductive carbon (e.g., graphite, carbon nanotubes, etc.). The shape of the positive electrode current collector layer 42 can be, for example, foil, plate, mesh, nonwoven fabric, or foam. In this embodiment, the positive electrode current collector layer 42 is made of a positive electrode current collector foil 42a.

[0032] (Middle class) The intermediate layer 5 is positioned between the negative electrode layer 2 and the solid electrolyte layer 3. The intermediate layer 5 has the function of uniformly depositing lithium metal, for example, when the solid battery 1 is a lithium metal battery. Therefore, the interface between the intermediate layer 5 and the solid electrolyte layer 3 is stabilized. When the solid battery 1 is a lithium metal secondary battery having the intermediate layer 5, the solid battery 1 may be an anode-free battery in which the negative electrode active material layer 21 does not exist at the time of the first charge. In this case, the lithium metal layer as the negative electrode active material layer 21 is formed after the first charge and discharge.

[0033] The materials constituting the intermediate layer 5 are not particularly limited, but examples include metals that can be alloyed with lithium, and amorphous carbon. Examples of metals that can be alloyed 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). The metals that can be alloyed with lithium may also be nanoparticles. Examples of amorphous carbon include carbon blacks such as acetylene black, furnace black, and Ketjen black, as well as coke and activated carbon. The amorphous carbon may be easily graphitizable carbon (soft carbon), difficult-to-graphitize carbon (hard carbon), CNTs (carbon nanotubes), fullerenes, and graphene. The intermediate layer may also contain a binder in addition to the above materials.

[0034] [Pressing device] Next, the configuration of the press apparatus 100 for manufacturing the solid-state battery 1 configured as described above will be explained. Figure 2 shows an example of the press apparatus 100 in the embodiment. The press apparatus 100 has as its main components a first positive electrode side transfer roller 120, a peeling roller 130 (see Figure 3), a second positive electrode side transfer roller 140, an intermediate layer transfer roller 150 (see Figure 5), a negative electrode side transfer roller 160 (see Figure 5), a negative electrode side sheet member lamination roller 170, a positive electrode press roll 180, and an integrated press roll 190. The peeling roller 130 is a component of the peeling mechanism 132, which will be described later. The press apparatus 100 continuously manufactures the solid-state battery 1 by feeding the positive electrode side sheet member 200 in one direction using these rollers.

[0035] In Figure 2, the direction in which the positive electrode sheet member 200 is fed is defined as the "conveying direction," and the direction perpendicular to that conveying direction is defined as the "width direction." Figure 1 also shows the range that is pressed or transferred during the positive electrode press step S4, the second solid electrolyte layer transfer step S5, the intermediate layer transfer step S6, the negative electrode solid electrolyte layer transfer step S7, and the integration press step S9, which will be described later.

[0036] The positive electrode side sheet member 200 is an example of a "base sheet," and is a sheet-like member obtained by laminating a positive electrode active material layer 41 on a positive electrode current collector foil 42a that constitutes the positive electrode current collector layer 42. The positive electrode side sheet member 200 is fed out by a roller (not shown) and transported so as to extend continuously from the base end to the end in the manufacturing line of the solid-state battery 1.

[0037] The first positive electrode side transfer roller 120, the peeling roller 130, the second positive electrode side transfer roller 140, the intermediate layer transfer roller 150, the negative electrode side transfer roller 160, and the negative electrode side sheet member lamination roller 170 are each composed of a pair of rotating bodies having a predetermined length in the width direction.

[0038] These rotating bodies are arranged in the order of the first positive electrode side transfer roller 120, peeling roller 130, positive electrode press roll 180, second positive electrode side transfer roller 140, negative electrode side sheet member lamination roller 170, and integrated press roll 190, from upstream to downstream, along the conveying direction of the positive electrode side sheet member 200.

[0039] The intermediate layer transfer roller 150 and the negative electrode side transfer roller 160 are positioned away from the transport line (hereinafter simply referred to as the "transport line") on which the positive electrode side sheet member 200 is transported in the transport direction, and perform transfer pressing of the intermediate layer 5 or the negative electrode side solid electrolyte layer SE3. Subsequently, as will be described later, the intermediate layer 5 and the negative electrode layer 2 on which the negative electrode side solid electrolyte layer SE3 has been transferred are transported to the upper or lower side of the positive electrode side sheet member 200, join the transport line of the positive electrode side sheet member 200, and are laminated by the negative electrode side sheet member lamination roller 170.

[0040] The first positive electrode side transfer roller 120, the second positive electrode side transfer roller 140, the intermediate layer transfer roller 150, and the negative electrode side transfer roller 160 perform a transfer press by passing a sheet of the substrate to be transferred and a sheet on which the solid electrolyte layer to be transferred is provided between a pair of rollers while applying pressure.

[0041] Figure 3 shows a more detailed enlarged view of the area enclosed by the dashed line in Figure 2. As shown here, the first positive electrode side transfer roller 120 pressurizes the transfer sheet 121, which has been unwound from the transfer sheet roll body 122 around which the transfer sheet 121 is wound, by sandwiching it between a pair of rollers. This allows the first solid electrolyte layer SE1 provided on the transfer sheet 121 to be transferred to the positive electrode side sheet member 200. The first solid electrolyte layer SE1 is an example of a "transfer body".

[0042] As shown in Figure 3, the transfer sheet 121 comprises a first solid electrolyte layer SE1 and a base sheet 123 on which the first solid electrolyte layer SE1 is provided. The base sheet 123 is peeled off from the transferred first solid electrolyte layer SE1 by a peeling mechanism 132 and is made of, for example, PET (polyethylene terephthalate).

[0043] Here, the peeling mechanism 132 in the embodiment will be described. The peeling mechanism 132 includes the peeling roller 130 described above for peeling the base sheet 123 from the first solid electrolyte layer SE1 transferred to the positive electrode side sheet member 200, and a base roll body 131 for winding up the base sheet 123 peeled off by the peeling roller 130. As shown in Figure 3, the peeling mechanism 132 is provided downstream of the first positive electrode side transfer roller 120 and peels the base sheet 123 from the transferred first solid electrolyte layer SE1. In Figure 3, the first solid electrolyte layer SE1 is shown by a solid line and the base sheet 123 to be peeled off is shown by a dashed line among the transfer sheet 121 unwound from the transfer sheet roll body 122. The arrows shown for each roller and each roll body in Figure 3 indicate the rotation direction of each roller and each roll body.

[0044] As described above, the peeling roller 130 peels the base sheet 123 from the first solid electrolyte layer SE1 transferred to the positive electrode side sheet member 200. However, the peelability of the base sheet 123 may differ depending on the direction in which the base sheet 123 is peeled (hereinafter referred to as the "peeling direction"). For example, as shown in the comparative example in Figure 8, if the peeling direction of the base sheet 123a is 90° or less, with the transport direction of the positive electrode side sheet member 200a to which the first solid electrolyte layer SE1a is transferred being 0°, the base sheet 123a will be pulled up by the peeling roller 130 in a direction of 90° or less. In such a case, the peeling direction of the base sheet 123a and the transport direction of the positive electrode side sheet member 200a are in the same direction, and it may not be possible to generate an appropriate shear force between the first solid electrolyte layer SE1a and the base sheet 123a, which may reduce the peelability of the base sheet 123a. For example, the positive electrode side sheet member 200a may bend, or this bending may cause the positive electrode side sheet member 200a to break. Therefore, in the embodiment shown in Figure 3, an appropriate shear force is generated between the first solid electrolyte layer SE1 and the base sheet 123 to improve the peelability of the base sheet 123. The above-mentioned "peeling direction and transport direction are in the same direction" means that the base sheet 123 is peeled at an angle within the range of 0° to 90° or less. In addition, in the comparative example in Figure 8, a reference numeral followed by "a" is used to distinguish it from the same components in the embodiment.

[0045] In this embodiment, the peeling roller 130 is configured to peel the base sheet 123 in the opposite direction to the transport direction of the positive electrode side sheet member 200. Here, "peeling in the opposite direction to the transport direction" means that, if the transport direction is set to 0°, the base sheet 123 is peeled at an angle greater than 90° and less than 180°. As an example of realizing such a configuration, the peeling roller 130 is positioned upstream of the peeling initiation point P, which is the starting point for peeling the base sheet 123 from the transferred first solid electrolyte layer SE1, in the transport direction of the positive electrode side sheet member 200. By positioning the peeling roller 130 upstream of the peeling initiation point P, the base sheet 123 is peeled in the opposite direction to the transport direction starting from the peeling initiation point P; in other words, the base sheet 123 is pulled in a direction against the transport direction. This improves the peelability of the base sheet 123 compared to the case where the transport direction and the peeling direction are the same, as in the comparative example in Figure 8 above.

[0046] In this embodiment, the peeling angle α of the base sheet 123 is greater than 90° and less than 180° when the transport direction is set to 0°, as described above. However, in order to improve the peelability of the base sheet 123, it is preferable that the base sheet 123 is peeled at a peeling angle that is closer to parallel to the opposite direction of the transport direction. Therefore, it is more preferable that the peeling angle α of the base sheet 123 is an angle closer to 180°.

[0047] In this way, by peeling the base sheet 123 in the opposite direction to the transport direction of the positive electrode side sheet member 200, the base sheet 123 is pulled in a direction against the transport direction, so that an appropriate shear force can be generated between the first solid electrolyte layer SE1 and the base sheet 123, and bending of the positive electrode side sheet member 200 or fracture starting from this bending can be suppressed. As a result, the peelability when peeling the base sheet 123 from the first solid electrolyte layer SE1 can be improved.

[0048] On the other hand, as described above, since the positive electrode side sheet member 200 is moving at a predetermined speed in the transport direction, if the winding speed of the base sheet 123 by the base roll body 131 does not match the transport speed of the positive electrode side sheet member 200, the peeling start point P may shift from the predetermined position. Also, theoretically, if the winding speed of the base sheet 123 and the transport speed of the positive electrode side sheet member 200 match, the peeling start point P should not shift from the predetermined position. However, in reality, even if the winding speed of the base sheet 123 and the transport speed of the positive electrode side sheet member 200 match, the peeling start point P may shift from the predetermined position. Here, "predetermined position" refers to the ideal position of the peeling start point P, which is set to, for example, a position where the base sheet 123 can be stably peeled off. In the embodiment, in order to stably peel off the base sheet 123, the peeling start point P is constantly recognized and the recognized peeling start point P is controlled to a predetermined position.

[0049] Specifically, as shown in Figure 4, the peeling mechanism 132 further comprises a recognition unit 300 that recognizes the peeling starting point P, and a control unit 400 that controls the peeling starting point P recognized by the recognition unit 300 to a predetermined position. The recognition unit 300 may be a camera or the like capable of recognizing the peeling starting point P. The information recognized by the recognition unit 300 is output to the control unit 400. The control unit 400 may be a known computer including, for example, a control unit that performs various calculations, a storage unit having a storage medium, and an input / output interface (not shown) that controls the input and output of data to and from the inside and outside of the control unit 400. In the example shown in Figure 4, only the upper side of the configuration of the peeling mechanism 132 and the transfer sheet 121 is shown with respect to the positive electrode side sheet member 200, and the lower side configuration is omitted.

[0050] The control unit 400 controls the position of the peeling initiation point P to a predetermined position by controlling the rotational speed of the base material roll 131. More specifically, the control unit 400 increases the rotational speed of the base material roll 131 when the peeling initiation point P is located downstream of the predetermined position. In other words, when the peeling initiation point P is located downstream of the predetermined position, the rotational speed of the base material roll 131 is relatively slow compared to the transport speed of the positive electrode side sheet member 200, so the control unit 400 controls the peeling initiation point P to the predetermined position by increasing the rotational speed of the base material roll 131. Conversely, when the peeling initiation point P is located upstream of the predetermined position, the control unit 400 decreases the rotational speed of the base material roll 131. In other words, if the peeling initiation point P is located upstream of a predetermined position, the rotational speed of the base material roll 131 will be relatively faster than the transport speed of the positive electrode side sheet member 200. Therefore, the control unit 400 controls the peeling initiation point P to a predetermined position by reducing the rotational speed of the base material roll 131.

[0051] Furthermore, it is preferable to control the peeling initiation point P, which is the starting point for peeling the base sheet 123 from the first solid electrolyte layer SE1, in the width direction of the positive electrode side sheet member 200. For example, it is preferable to configure the peeling roller 130 in advance so that one side is inclined with respect to the other side in the width direction. This allows the base sheet 123 to be peeled off from the first solid electrolyte layer SE1 while being inclined from one side to the other in the width direction. In such a case, the peeling initiation line connecting the peeling initiation points P in the width direction is configured to be inclined with respect to that width direction.

[0052] This allows control of the peeling starting line in addition to the position of the peeling starting point P, thereby improving the accuracy of peeling the base sheet 123 compared to when the peeling roller 130 is not tilted in the width direction.

[0053] As shown in Figure 3, the transfer sheet 121 is provided on both sides of the positive electrode sheet member 200 so as to be vertically symmetrical, and is configured to transfer the first solid electrolyte layer SE1 to both sides of the positive electrode sheet member 200. This allows the first solid electrolyte layer SE1 to be transferred to both sides of the positive electrode sheet member 200 simultaneously.

[0054] As shown in Figure 2, the second positive electrode side transfer roller 140 transfers the second solid electrolyte layer SE2 onto the positive electrode side sheet member 200, which has been pressed with the first solid electrolyte layer SE1 transferred onto it.

[0055] As shown in Figure 5, the intermediate layer transfer roller 150 transfers the intermediate layer 5 onto the negative electrode active material layer 21, which is laminated on the negative electrode current collector foil 22a. As a result, the intermediate layer 5 is positioned between the negative electrode active material layer 21 and the negative electrode side solid electrolyte layer SE3.

[0056] As shown in Figure 5, the negative electrode side transfer roller 160 transfers the negative electrode side solid electrolyte layer SE3 onto the intermediate layer 5 to form the negative electrode side sheet member 210.

[0057] As shown in Figure 2, the negative electrode side sheet member lamination roller 170 transports and laminates the negative electrode side sheet member 210, on which the negative electrode side solid electrolyte layer SE3 has been transferred, onto the positive electrode side sheet member 200, on which the first solid electrolyte layer SE1 and the second solid electrolyte layer SE2 have been transferred.

[0058] As shown in Figure 2, the positive electrode press roll 180 and the integrated press roll 190, like each transfer roller, are each composed of a pair of rotating rollers. The positive electrode side sheet member 200, on which solid electrolyte layers and the like are laminated according to each process, is passed through the pair of rollers under pressure to increase its density. The positive electrode press roll 180 presses the positive electrode side sheet member 200 on which the first solid electrolyte layer SE1 has been transferred. The integrated press roll 190 presses the electrode 10 so that the positive electrode side sheet member 200 and the negative electrode side sheet member 210 are laminated together and the electrode 10 is integrated. As a result, the positive electrode side sheet member 200 and the negative electrode side sheet member 210 are integrated, and at the same time, the first solid electrolyte layer SE1, the second solid electrolyte layer SE2, and the negative electrode side solid electrolyte layer SE3 are increased in density.

[0059] [Pressing method] Next, a pressing method using the press device 100 configured as described above for the solid-state battery 1 will be explained. Figure 6 is a flowchart showing an example of the pressing method. The pressing method includes, as a process, a positive electrode side sheet member feeding step S1, a first solid electrolyte layer transfer step S2, a base sheet peeling step S3, a positive electrode pressing step S4, a second solid electrolyte layer transfer step S5, an intermediate layer transfer step S6, a negative electrode side solid electrolyte layer transfer step S7, a negative electrode side sheet member lamination step S8, and an integrated pressing step S9.

[0060] The positive electrode side sheet member feeding step S1 is a step in which the positive electrode side sheet member 200 is conveyed and fed out by a conveying roller (not shown). That is, the positive electrode side sheet member 200, which is laminated by coating the positive electrode active material onto the positive electrode current collector foil 42a that constitutes the positive electrode current collector layer 42, is fed out.

[0061] The first solid electrolyte layer transfer step S2 is a step in which the first solid electrolyte layer SE1 is transferred to the positive electrode side sheet member 200 by the first positive electrode side transfer roller 120. Specifically, the first solid electrolyte layer transfer step S2 aligns the first solid electrolyte layer SE1 so that it is placed within a range guided by a guide roller (not shown). Then, the slurry constituting the first solid electrolyte layer SE1 is passed over the positive electrode side sheet member 200 under pressure by a pair of first positive electrode side transfer rollers 120 to perform a transfer press. The pressure at this time is, for example, 50 to 500 MPa at room temperature (for example, 10 to 35°C). Preferably, it is 100 MPa at 25°C.

[0062] The substrate sheet peeling step S3 is a step in which the substrate sheet 123 is peeled off from the first solid electrolyte layer SE1 that has been transferred and pressed using a peeling roller 130. Specifically, the substrate sheet peeling step S3 includes a recognition step S30, a peeling start point control step S31, and a peeling step S32.

[0063] The recognition step S30 is a step in which the peeling initiation point P of the base sheet 123 is recognized. That is, as described above, the recognition unit 300 that recognizes the peeling initiation point P continuously monitors the peeling initiation point P. The information of the peeling initiation point P recognized by the recognition unit 300 is output to the control unit 400.

[0064] Step S31, the peeling initiation point control step, is a step to control the peeling initiation point P to a predetermined position. As described above, the predetermined position is the ideal position for the peeling initiation point P, and the control unit 400 provides feedback control to the rotation speed of the substrate roll body 131 so that the peeling initiation point P recognized by the recognition unit 300 is at that predetermined position. The specific control details are as described above, so their explanation is omitted here.

[0065] The peeling step S32 is a step in which the base sheet 123 is peeled in the opposite direction to the transport direction of the positive electrode side sheet member 200, based on a peeling starting point P controlled to a predetermined position. In other words, the control unit 400 controls the rotation speed of the base roll body 131 so that the peeling starting point P is in a predetermined position, and using that position as a reference, the peeling roller 130, which is positioned upstream of the peeling starting point P, peels the base sheet 123 in the opposite direction to the transport direction.

[0066] The positive electrode pressing step S4 is a step in which the positive electrode side sheet member 200, onto which the first solid electrolyte layer SE1 has been transferred, is pressed by the positive electrode pressing roll 180. This positive electrode pressing step S4 increases the density of the positive electrode. The pressing pressure for increasing density is, for example, about 800 to 1200 MPa at 25 to 100°C. The laminate of the densified positive electrode side sheet member 200 and the first solid electrolyte layer SE1 is conveyed downstream on the conveyor line.

[0067] The second solid electrolyte layer transfer step S5 is a step in which, after the positive electrode press step S4, the second solid electrolyte layer SE2 is transferred onto the positive electrode side sheet member 200, which has been pressed with the first solid electrolyte layer SE1 transferred onto it, by the second positive electrode side transfer roller 140. Specifically, in the second solid electrolyte layer transfer step S5, the second solid electrolyte layer SE2 is positioned on the positive electrode side sheet member 200, to which the first solid electrolyte layer SE1 has been transferred, within a range guided by a guide roller (not shown). Then, the slurry constituting the second solid electrolyte layer SE2 is passed over the positive electrode side sheet member 200 under pressure by the second positive electrode side transfer roller 140, which acts as a transfer roller, and a transfer press is performed. The pressure at this time is, for example, 50 to 500 MPa at room temperature (e.g., 10 to 35°C). In this way, the positive electrode side sheet member 200 is pressed two or more times. Preferably, it is 150 MPa at 25°C.

[0068] Meanwhile, the negative electrode side sheet member 210 is prepared at a location separate from the transport line. First, as shown in the upper part of Figure 5, the intermediate layer 5 is transferred to the negative electrode active material layer 21 laminated on the negative electrode current collector foil 22a by the intermediate layer transfer roller 150 (intermediate layer transfer step S6). Then, as shown in the lower part of Figure 5, the negative electrode side solid electrolyte layer SE3 is transferred onto the intermediate layer 5 by the negative electrode side transfer roller 160 to form the negative electrode side sheet member 210 (negative electrode side solid electrolyte layer transfer step S7). As a result, the intermediate layer 5 is positioned between the negative electrode active material layer 21 and the negative electrode side solid electrolyte layer SE3. In this embodiment, the negative electrode side sheet member 210 includes a laminated negative electrode current collector foil 22a, negative electrode active material layer 21, intermediate layer 5, and negative electrode side solid electrolyte layer SE3, but the negative electrode active material layer 21 and intermediate layer 5 may be omitted.

[0069] In the intermediate layer transfer step S6, the slurry constituting the intermediate layer 5 is positioned on the negative electrode active material layer 21 within a range guided by a guide roller (not shown). Then, the intermediate layer 5 is passed over the negative electrode active material layer 21 under pressure by an intermediate layer transfer roller 150, which acts as a transfer roller, to perform an intermediate layer transfer press, transferring the intermediate layer 5 to the negative electrode active material layer 21. The pressure at this time is, for example, 50 to 800 MPa at room temperature (e.g., 10 to 35°C). More preferably, it is in the range of 300 MPa or more and 800 MPa or less at 25°C.

[0070] In the negative electrode solid electrolyte layer transfer step S7, the slurry constituting the negative electrode solid electrolyte layer SE3 is positioned on the intermediate layer 5 within a range guided by a guide roller (not shown). Then, the negative electrode solid electrolyte layer SE3 is passed over the intermediate layer 5 under pressure by the negative electrode transfer roller 160, which acts as a transfer roller, and the negative electrode active material layer transfer press is performed to transfer the negative electrode solid electrolyte layer SE3 to the intermediate layer 5. The pressure at this time is, for example, 600 to 800 MPa at room temperature (for example, 10 to 35°C).

[0071] Regarding pressure, the pressing pressure in the positive electrode pressing step S4 is not only the maximum pressure applied to the positive electrode side sheet member 200, but also the maximum pressing pressure in the entire pressing apparatus method. The positive electrode side sheet member 200 is pressed at high pressure to increase its energy density and densify the electrodes. The maximum pressing pressure in the positive electrode pressing step S4 is greater than or equal to the maximum pressing pressure applied to the negative electrode side sheet member 210.

[0072] Furthermore, the pressure during the transfer of the first solid electrolyte layer in step S2 and the second solid electrolyte layer in step S5 is less than the pressing pressure in the positive electrode pressing step S4. Also, the pressure during the transfer of the first solid electrolyte layer in step S2 and the second solid electrolyte layer in step S5 is less than the pressing pressure in the negative electrode solid electrolyte layer in step S7.

[0073] Since the first solid electrolyte layer SE1 and the second solid electrolyte layer SE2 contain a relatively large amount of binder, the press pressure during transfer can be reduced. Furthermore, by setting the transfer press pressure as low as possible, the amount of stretching of the first solid electrolyte layer SE1 and the second solid electrolyte layer SE2 due to the transfer press can be reduced. Therefore, in the subsequent integration press step S9, etc., room is left for the first solid electrolyte layer SE1 and the second solid electrolyte layer SE2 to stretch, and the first solid electrolyte layer SE1 can be stretched to follow the positive electrode layer 4. This improves the bonding of the first solid electrolyte layer SE1 with the positive electrode active material layer 41.

[0074] After the negative electrode solid electrolyte layer transfer step S7, the formed negative electrode sheet member 210 is cut with a cutter while being supported by the feed roll that feeds out the material to be transferred in the negative electrode solid electrolyte layer transfer step S7. The negative electrode sheet member 210 is cut to the design dimensions of the negative electrode layer 2 of the solid battery 1.

[0075] The negative electrode sheet member 210, cut to the design dimensions, is transported to the positive electrode sheet member 200 so as to merge with the positive electrode sheet member 200's transport line, as shown in Figures 2 and 6, and is stacked on the positive electrode sheet member 200. At this time, prior to the integration press step S9 described later, a first solid electrolyte layer SE1 is provided on the lower side of the positive electrode sheet member 200 facing the negative electrode solid electrolyte layer SE3, and a second solid electrolyte layer SE2 is provided on top of it. Then, in its cut state, the negative electrode sheet member 210 is placed on the positive electrode sheet member 200.

[0076] Specifically, in the negative electrode side sheet member lamination step S8, the negative electrode side sheet member 210, on which the negative electrode side solid electrolyte layer SE3 has been transferred, is transported and laminated onto the positive electrode side sheet member 200, on which the first solid electrolyte layer SE1 and the second solid electrolyte layer SE2 have been transferred, by the negative electrode side sheet member lamination roller 170. In the negative electrode side sheet member lamination step S8, the negative electrode side sheet member 210, cut to the design dimensions, is positioned on the positive electrode side sheet member 200, on which the first solid electrolyte layer SE1 and the second solid electrolyte layer SE2 have been transferred, within a range guided by a guide roller (not shown).

[0077] Thus, with the positive electrode sheet member 200 and the negative electrode sheet member 210 stacked, the electrodes 10 are pressed together by the integrating press roll 190 (integrating press step S9). Immediately before the integrating press step S9, the thickness of the positive electrode sheet member 200 is greater than that of the negative electrode sheet member 210 in the stacking direction. The pressure at this time is, for example, about 500 to 900 MPa at 25 to 100°C. The integrating press step S9 integrates the positive electrode sheet member 200 and the negative electrode sheet member 210, and at the same time, the first solid electrolyte layer SE1, the second solid electrolyte layer SE2, and the negative electrode solid electrolyte layer SE3 become denser. Comparing the pressing pressure of the integrating press step S9 and the positive electrode press step S4, the pressing pressure of the positive electrode press step S4 is greater than that of the integrating press step S9.

[0078] After the integration press step S9, the formed electrode 10 is cut with a rotary cutter.

[0079] Furthermore, the following processes—transfer of the first solid electrolyte layer SE1 in the first solid electrolyte layer transfer step S2, pressing of the positive electrode side sheet member 200 in the positive electrode press step S4, transfer of the second solid electrolyte layer SE2 in the second solid electrolyte layer transfer step S5, lamination of the negative electrode side sheet member 210 before integration in the negative electrode side sheet member lamination step S8, and integration pressing in the integration press step S9—are performed on both sides of the positive electrode side sheet member 200 that was fed out in the positive electrode side sheet member feeding step S1. As a result, a solid-state battery 1 is obtained in which each layer is symmetrically laminated on both the upper and lower surfaces, sandwiching the positive electrode side sheet member 200, as shown in Figure 1.

[0080] Thus, in this embodiment, by peeling the base sheet 123 in the opposite direction to the transport direction of the positive electrode side sheet member 200, the base sheet 123 is pulled in a direction against the transport direction. Compared to, for example, a case where the transport direction and the peeling direction are the same, an appropriate shear force can be generated between the first solid electrolyte layer SE1 and the base sheet 123, thereby suppressing bending of the positive electrode side sheet member 200 and fracture of the positive electrode side sheet member 200 starting from this bending. As a result, the peelability when peeling the base sheet 123 from the first solid electrolyte layer SE1 can be improved.

[0081] While embodiments have been described above with reference to the drawings, it goes without saying that the present invention is not limited to these embodiments. It is clear to those skilled in the art that various modifications and alterations can be conceived within the scope of the claims, and these are also understood to naturally fall within the technical scope of the present invention. Furthermore, the components of the above embodiments may be combined in any way without departing from the spirit of the invention.

[0082] For example, in the above-described embodiment, as an example of peeling the base sheet 123 in the opposite direction to the transport direction of the positive electrode side sheet member 200, the peeling starting point P was controlled to a predetermined position by feedback control by the recognition unit 300 and the control unit 400 to peel the base sheet 123. However, other configurations are also possible as long as the base sheet 123 is peeled in the opposite direction to the transport direction. For example, as shown in Figure 7, a guide mechanism 500 may be provided for peeling the base sheet 123 in the opposite direction to the transport direction, starting from the peeling starting point P. With such a configuration, for example, peeling the base sheet 123 in the opposite direction to the transport direction can be achieved without providing the recognition unit 300 and other components described above.

[0083] Furthermore, in the above-described embodiment, various solid electrolyte layers were laminated on both sides of the positive electrode sheet member 200, but this lamination may be configured to be laminated on only one side.

[0084] This specification contains at least the following information. The components indicated in parentheses in the embodiments described above are, but are not limited thereto.

[0085] (1) A peeling mechanism (peeling mechanism 132) for peeling the substrate (substrate sheet 123) from the transfer body (first solid electrolyte layer SE1) transferred to the base material sheet (positive electrode side sheet member 200), A peeling roller (peeling roller 130) for peeling the substrate from the transfer body, The system includes a base material roll body (base material roll body 131) for winding up the base material peeled off by the peeling roller, The aforementioned peeling roller is The substrate is peeled off in the direction opposite to the conveying direction of the base material sheet. Peeling mechanism.

[0086] According to (1), by peeling the substrate in the opposite direction to the conveying direction of the base sheet, the substrate is pulled in a direction against the conveying direction of the base sheet. Therefore, compared to peeling the substrate in the same direction as the conveying direction, for example, an appropriate shear force can be generated between the base sheet and the transfer body. As a result, bending of the base sheet and fracture caused by this bending can be suppressed. In other words, the peelability of the substrate when peeling it from the transfer body can be improved.

[0087] (2) The peeling mechanism described in (1), The aforementioned peeling roller is In the aforementioned transport direction, the following is positioned upstream of the peeling initiation point (peeling initiation point P) where the substrate peels off: Peeling mechanism.

[0088] According to (2), in the transport direction, the peeling roller is positioned upstream of the peeling starting point where the substrate is peeled off, so that the substrate can be reliably pulled in the opposite direction to the transport direction, thereby generating an appropriate shear force between the base material sheet and the transfer body.

[0089] (3) The peeling mechanism described in (2), A recognition unit (recognition unit 300) that recognizes the peeling initiation point, The system includes a control unit (control unit 400) that controls the rotational speed of the base material roll body, The control unit, The rotational speed of the substrate roll body is controlled so that the peeling initiation point recognized by the recognition unit is at a predetermined position. Peeling mechanism.

[0090] According to (3), stable peeling of the substrate can be achieved by performing feedback control based on the recognition of the recognition unit so that the peeling starting point is at a predetermined position.

[0091] (4) The peeling mechanism described in (3), The control unit, When the peeling initiation point is located downstream of the predetermined position, the rotational speed of the base material roll body is increased. When the peeling initiation point is located upstream of the predetermined position, the rotational speed of the base material roll is reduced. Peeling mechanism.

[0092] According to (4), the winding speed of the substrate on the substrate roll and the transport speed with respect to the base sheet may not coincide. In such cases, the peeling point will shift from a predetermined position. However, by controlling the rotation speed of the substrate roll according to the shift from the predetermined position, it is possible to control the peeling point to a predetermined position. This enables stable peeling of the substrate.

[0093] (5) The peeling mechanism described in (2), On the base material sheet onto which the transfer body has been transferred, the peeling initiation line connecting the peeling initiation points is configured to be inclined with respect to the width direction perpendicular to the transport direction. Peeling mechanism.

[0094] According to (5), the substrate can be peeled along a peeling initiation line configured to be inclined in the width direction, for example, stress concentration at a predetermined peeling initiation point can be suppressed, and as a result, the peelability of the substrate can be improved.

[0095] (6) The peeling mechanism described in (5), The aforementioned peeling roller is In the width direction, one side of the peeling roller is inclined relative to the other side. Peeling mechanism.

[0096] According to (6), in the width direction, one side of the peeling roller is inclined relative to the other side, which enables the peeling of the substrate along the peeling starting line.

[0097] (7) A peeling mechanism as described in (1) or (2), The aforementioned transfer material is a solid electrolyte layer (first solid electrolyte layer SE1), The aforementioned base sheet is the positive electrode side sheet member (positive electrode side sheet member 200). Peeling mechanism.

[0098] According to (7), the substrate can be properly peeled off from the solid electrolyte layer transferred to the positive electrode sheet member.

[0099] (8) A peeling method for peeling a substrate (substrate sheet 123) from a transfer body (first solid electrolyte layer SE1) transferred to a base material sheet (positive electrode side sheet member 200), A recognition step (recognition step S30) recognizes the peeling initiation point (peeling initiation point P) where the substrate peels off, A peeling initiation point control step (peeling initiation point control step S31) controls the peeling initiation point to be at a predetermined position, The system includes a peeling step (peeling step S32) in which the substrate is peeled in the opposite direction to the transport direction of the base material sheet based on the peeling starting point controlled to the predetermined position, Method of removal.

[0100] According to (8), by controlling the peeling starting point to a predetermined position and peeling the substrate in the opposite direction to the transport direction starting from that controlled position, stable peeling of the substrate can be achieved. This suppresses bending and tearing of the base sheet and improves the peelability of the substrate. [Explanation of symbols]

[0101] 123 Base sheet (base material) 130 peeling roller 131 Base material roll 132 Peeling mechanism 200 Positive electrode side sheet material (base sheet) 300 Recognition part 400 Control Unit P Delamination starting point SE1 First solid electrolyte layer (transfer material) S30 Recognition Step S31 Detachment Initiation Point Control Step S32 Peeling step

Claims

1. A peeling mechanism for peeling a substrate from a transfer body transferred to a base material sheet, A peeling roller for peeling the substrate from the transfer body, The system comprises a base material roll body for winding up the base material peeled off by the peeling roller, The aforementioned peeling roller is The substrate is peeled off in the direction opposite to the conveying direction of the base material sheet. Peeling mechanism.

2. A peeling mechanism according to claim 1, The aforementioned peeling roller is In the aforementioned transport direction, the following is positioned upstream of the peeling initiation point where the substrate peels off: Peeling mechanism.

3. The peeling mechanism according to claim 2, A recognition unit that recognizes the peeling point, The system includes a control unit for controlling the rotational speed of the base material roll, The control unit, The rotational speed of the substrate roll body is controlled so that the peeling initiation point recognized by the recognition unit is at a predetermined position. Peeling mechanism.

4. The peeling mechanism according to claim 3, The control unit, When the peeling initiation point is located downstream of the predetermined position, the rotational speed of the base material roll body is increased. When the peeling initiation point is located upstream of the predetermined position, the rotational speed of the base material roll is reduced. Peeling mechanism.

5. The peeling mechanism according to claim 2, On the base material sheet onto which the transfer body has been transferred, the peeling initiation line connecting the peeling initiation points is configured to be inclined with respect to the width direction perpendicular to the transport direction. Peeling mechanism.

6. The peeling mechanism according to claim 5, The aforementioned peeling roller is In the width direction, one side of the peeling roller is inclined relative to the other side. Peeling mechanism.

7. A peeling mechanism according to claim 1 or 2, The aforementioned transfer material is a solid electrolyte layer, The aforementioned base sheet is the positive electrode side sheet member. Peeling mechanism.

8. A peeling method for peeling a substrate from a transfer body transferred to a base material sheet, A recognition step of recognizing the peeling initiation point where the substrate peels off, A peeling initiation point control step that controls the peeling initiation point to be at a predetermined position, The system includes a peeling step in which the substrate is peeled in the opposite direction to the transport direction of the base material sheet based on the peeling starting point controlled to the predetermined position, Method of removal.

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