Manufacturing apparatus of all-solid battery cell and manufacturing method

Abstract

To provide a manufacturing apparatus of an all-solid battery cell and a manufacturing method, capable of easily confirming an operation during powder pressing at the time of a cell manufacturing.SOLUTION: A manufacturing apparatus 1 of an all-solid battery cell 23, using a press machine, comprises a cylinder-shape electrode guide 11 covering a sample 21. In the electrode guide 11, at least one part of a peripheral direction (one of half split bodies 12 and 13, and a split body 113) is an another split body against a remaining portion (the other one of half split bodies 12 and 13, and the remaining portion 112), and the split body can be detached to the remaining portion before and after pressing. In a manufacturing method of the all-solid battery cell 23, the all-solid battery cell 23 is pressed in each of a plurality of steps, and the split body is detached from and attached to the remaining portion each time pressing is performed.SELECTED DRAWING: Figure 5

Description

[Technical field]

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

[0002] The establishment of a three-electrode cell for an all-solid-state lithium-ion battery is a challenge for practical use. An all-solid-state three-electrode cell equipped with a reference electrode is described in, for example, Patent Document 1. The shape of the cell used in the conventional technology has a structure in which the electrode guide portion is divided horizontally in advance, and when the cell is produced, the solid electrolyte is poured in two stages and the reference electrode is placed between them. The electrode guide is cylindrical and made of a tough material such as zirconia or alumina to ensure the strength to withstand a molding pressure equivalent to 1000 MPa. [Prior art documents] [Patent documents]

[0003] [Patent Document 1] JP 2022-007408 A Summary of the Invention [Problem to be solved by the invention]

[0004] However, in the above-mentioned conventional technology, the powder inside receives a pressure of up to 1000 MPa during compaction, which can cause misalignment between the divided electrode guides, resulting in powder leakage or unevenness in the applied pressure. In addition, once the powder is compressed, it is not possible to access the cross section of the internal sample, making it difficult to insert the reference electrode, and it is not possible to check whether the reference electrode is maintained in the intended position after the powder is compressed without twisting, etc. For this reason, the performance of the cell with the reference electrode cannot be judged without performing electrochemical measurements, which means that there is a lot of rework required in case of failure. In addition, electrode guides that require strength (zirconia, alumina, etc.) are made of opaque materials, so the position where the reference electrode can be inserted cannot be confirmed visually. Also, electrode guides made of zirconia and other materials have low X-ray transparency, so the internal condition cannot be observed non-destructively using CT or other methods.

[0005] The present invention has been made in consideration of the above circumstances, and provides an apparatus and method for manufacturing an all-solid-state battery cell that allows easy confirmation of the powder pressing operation during cell production. [Means for solving the problem]

[0006] As a means for solving the above problems, a first aspect of the present invention is a manufacturing apparatus for an all-solid-state battery cell using a press machine, comprising a cylindrical electrode guide that covers a sample, at least a portion of the electrode guide in a circumferential direction is a divided body that is separate from a remaining portion, and the divided body is detachable from the remaining portion before and after pressing. According to this configuration, the divided bodies of the electrode guide can be attached and detached before and after pressing, so that the divided bodies are attached before pressing to form a cylindrical electrode guide which functions as the outer wall during pressing, and the divided bodies can be removed after pressing to check whether the samples are stacked normally. By making the electrode guide into a split structure, even pressed specimens that are difficult to remove due to adhesion can be easily removed. It is possible to insert a reference electrode into the pressed body through the opening when the divided body is removed and measure whether it is electrically connected, which shortens the manufacturing time and also makes it possible to attach the divided body again and press it. In addition, when changing the pressing pressure and pressing multiple times, it is easy to add additional samples.

[0007] In a second aspect of the present invention, in the first aspect, the joint between the divided body and the remaining portion is a recessed / protruding fitting portion having a recess and a protrusion that fit together. According to this configuration, the joint between the divided body and the remaining portion is a concave-convex fitting portion, so that the divided body is less likely to come off and the sample can be pressed while minimizing misalignment of the divided body. For example, in the case of a split electrode guide (made of zirconia), misalignment may occur if the outer periphery is not positioned, but by providing a concave-convex fitting portion at the joint, misalignment of the split body can be prevented.

[0008] In a third aspect of the present invention, in the first aspect, the electrode guide is divided into segments over a range of less than half the circumference in the circumferential direction and over a range through which the pressed body of the sample can be removed. With this configuration, compared to when the electrode guide is split in half, the range of the split body is narrowed to reduce the opening of the electrode guide, and the minimum opening through which the sample press body can be removed can be set.

[0009] A fourth aspect of the present invention is the third aspect, wherein the remaining portion of the electrode guide excluding the divided bodies forms an opening having an opening width equal to or larger than the diameter of the pressed body of the sample. According to this configuration, the remaining portion excluding the divided body has an opening width greater than or equal to the diameter of the sample press body, so that the sample press body can be reliably removed even when the divided body extends over a range of less than half the circumference in the circumferential direction.

[0010] A fifth aspect of the present invention is the electrode guide according to any one of the first to fourth aspects, wherein the electrode guide is made of zirconia. According to this configuration, by forming the electrode guide from zirconia, which is one of the ceramics with high strength, it is possible to form an electrode guide that is suppressed from deforming and can withstand pressure even if it has a divided structure.

[0011] A sixth aspect of the present invention is any one of the first to fifth aspects, further comprising a restraining device for restraining the electrode guide from an outer periphery side. According to this configuration, the electrode guide having a split structure is restrained by the restraining device, and pressing is performed in this state, so that the electrode guide can withstand the internal pressure caused by pressing.

[0012] A seventh aspect of the present invention is a manufacturing method for an all-solid-state battery cell using a press, comprising: a cylindrical electrode guide covering a sample; at least a portion of the electrode guide in a circumferential direction is a divided body separate from a remaining portion; the all-solid-state battery cell is pressed in a plurality of stages; and the divided body is attached to and detached from the remaining portion each time the all-solid-state battery cell is pressed. According to this configuration, when pressing is performed in multiple stages to mold a pressed body such as compressed lithium, it is possible to attach and detach the divided bodies after each pressing to check whether the sample is stacked normally, making it easy to form a high-quality laminate.

[0013] In an eighth aspect of the present invention, in the seventh aspect, a sample is introduced into the electrode guide and pressurized to form a temporary shape, and then a reference electrode is inserted into the sample in the temporary shape. According to this configuration, since the solid electrolyte can be managed to a certain extent as a solid by pressing once, the pressing pressure can be weakened to form a solid electrolyte of a temporary shape into which the reference electrode can be easily inserted, which facilitates the production of an all-solid-state battery cell.

[0014] In a ninth aspect of the present invention, in the seventh or eighth aspect, the sample is covered with a covering material made of a polyimide film on the inside of the electrode guide. According to this configuration, it is possible to prevent other materials from being mixed inside the electrode guide. The covering material can be made of a commonly available material such as Kapton (registered trademark).

[0015] A tenth aspect of the present invention is the above-mentioned ninth aspect, wherein the polyimide film covering material is cut and peeled off to expose the pressed body. With this configuration, the press body can be easily exposed for inspection and the reference electrode can be easily inserted.

[0016] In an eleventh aspect of the present invention, in the ninth or tenth aspect, the sample introduced into the coating material is pressed in the axial direction while the divided body and the remaining portion of the electrode guide are restrained from the outer circumferential side. According to this configuration, by pressing the sample inside the covering material while the electrode guide having a split structure is restrained, it is possible to press the sample while enduring the internal pressure caused by the press. Effect of the Invention

[0017] According to the present invention, it is possible to provide an apparatus and method for manufacturing an all-solid-state battery cell that allows easy confirmation of the powder pressing work during cell production. [Brief description of the drawings]

[0018] [Figure 1] FIG. 2 is an explanatory diagram showing a first stage of an overall manufacturing flow of an all-solid-state battery cell in an embodiment of the present invention. [Diagram 2] FIG. 2 is an explanatory diagram showing a second stage of the overall manufacturing process. [Diagram 3] FIG. 11 is an explanatory diagram showing a third stage of the overall manufacturing flow. [Figure 4] FIG. 11 is an explanatory diagram showing a fourth stage of the overall manufacturing flow. [Diagram 5] 5A is a horizontal cross-sectional view of the sample position in FIG. 4, (b) is a cross-sectional view showing a first modified example of the electrode guide, and (c) is a cross-sectional view showing a second modified example of the electrode guide. [Figure 6] FIG. 2 is an explanatory diagram showing a first detail of a process for producing an all-solid-state battery cell according to an embodiment of the present invention. [Figure 7] FIG. 11 is an explanatory diagram showing a second detail of the manufacturing process. [Figure 8] FIG. 11 is an explanatory diagram showing a third detail of the manufacturing process. [Figure 9] FIG. 11 is an explanatory diagram showing a fourth detail of the manufacturing process. [Figure 10] FIG. 11 is an explanatory diagram showing a fifth detail of the above manufacturing process. [Figure 11] FIG. 11 is an explanatory diagram showing a sixth detail of the manufacturing process. [Figure 12] FIG. 11 is an explanatory diagram showing a seventh detail of the manufacturing process. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0019] Hereinafter, an embodiment of the present invention will be described with reference to the drawings. 4 and 5, in the manufacturing apparatus 1 and manufacturing method for the all-solid-state battery cell 23 in this embodiment, the electrode guide 11 is formed into a vertically divided shape when manufacturing the all-solid-state battery cell (basic evaluation cell) 23, so that the electrode guide 11 can be removed even after the pellet is manufactured, and the cross section of the pellet can be exposed, making it possible to insert the reference electrode 22. In addition, by inserting a Kapton (registered trademark) tube between the short and long axes 5, 9 of the current collecting blocks 3, 7 of the manufacturing apparatus 1 and the electrode guide 11, the structure is maintained even if the zirconia tube (electrode guide 11) is removed after the pellet is manufactured, and the internal state can be visually inspected to confirm the position where the reference electrode 22 can be inserted.

[0020] In addition, by inserting a polyimide tube between the short and long axes 5, 9 of the current collecting guide that presses the basic evaluation cell 23 and the electrode guide 11, the zirconia tube can be moved up and down, making it possible to align the position where the reference electrode 22 can be inserted. Furthermore, by making the electrode guide 11 of the basic evaluation cell 23 into a divided shape and restraining it with the restraining device 18, it is possible to realize a strength capable of withstanding a pressure equivalent to 1000 MPa. Furthermore, by making the electrode guide 11, which is opaque to X-rays, removable without manipulating the current collecting blocks 3 and 7, non-destructive synchrotron radiation measurement and in situ measurement at each manufacturing stage can be performed.

[0021] The manufacturing apparatus 1 and the manufacturing method for the all-solid-state battery cell 23 will be described below. As shown in Fig. 4, the manufacturing apparatus 1 includes a first jig (short-axis current collecting block 3) fixed to a movable die of the press machine, and a second jig (long-axis current collecting block 7) fixed to a fixed die of the press machine. In Fig. 4, the movable die is disposed on the top and the fixed die is disposed on the bottom, and the up-down direction in the figure is the pressing direction.

[0022] 5(a), the short-axis current collecting block 3 has a cylindrical first convex portion (short-axis convex portion 5) that is inserted from one axial end side into the cylindrical covering material 16. The short-axis current collecting block 3 has the short-axis convex portion 5 protruding downward from a substantially horizontal base portion 4. The long-axis current collecting block 7 has a columnar second convex portion (long-axis convex portion 9) that is inserted from the other axial end side into the cylindrical covering material 16. The long-axis current collecting block 7 has the long-axis convex portion 9 protruding upward from a substantially horizontal base portion 8. The minor axis protrusion 5 is shorter in the press direction than the major axis protrusion 9. The tip face of the minor axis protrusion 5 and the tip face of the major axis protrusion 9 face each other in the press direction within the covering material 16.

[0023] The covering material 16 is a cylindrical member with its axis oriented in the pressing direction. The covering material 16 is detachably arranged on the inner periphery side of the electrode guide 11 to cover the sample 21. The covering material 16 is formed by rolling a polyimide film such as Kapton (registered trademark), which is commonly available, into a cylindrical shape. The covering material 16 has an inner periphery surface that matches the outer periphery surfaces of the short and long axis protrusions 5 and 9.

[0024] The electrode guide 11 is a cylindrical member that is disposed on the outer periphery of the coating material 16 to cover the coating material 16 and receives the internal pressure caused by pressing the sample 21. The electrode guide 11 is a cylindrical member that is disposed coaxially with the coating material 16 and has a greater wall thickness than the coating material 16. The electrode guide 11 has an inner peripheral surface that matches the outer peripheral surface of the coating material 16 into which the short and long axis protrusions 5, 9 are inserted. For example, the electrode guide 11 is made of zirconia to ensure strength.

[0025] When the electrode guide 11 is formed from zirconia, the electrode guide 11 alone can ensure the strength to withstand the internal pressure caused by the press; however, when a restraining device 18 for restraining the electrode guide 11 is provided, the electrode guide 11 may be formed from a material having a lower strength than zirconia (Macol (registered trademark), alumina, etc.).

[0026] For example, the electrode guide 11 is divided along the axial direction into a pair of half bodies 12, 13. The electrode guide 11 is attached to an object such as a coating material 16 so that the pair of half bodies 12, 13 sandwich the electrode guide 11 in the radial direction. In FIG. 5(a), the joint between the pair of half bodies 12, 13 is such that flat surfaces extending in the radial direction are in contact with each other. 5(b), the joint between the pair of half bodies 12, 13 may be a concave-convex fitting portion 115 having concaves and convexes. In this case, the half bodies 12, 13 are less likely to be misaligned with each other, and are less likely to peel off from each other, so that the sample 21 can be pressed well. By using a strong electrode guide 11, the sample 21 and the covering material 16 are prevented from expanding outward even when the sample 21 is pressed, and a pressed body with a uniform diameter is formed.

[0027] One of the pair of half bodies 12, 13 can be seen as a separate divided body from the other. In this case, the divided body is formed in a range of 1 / 2 of the circumference of the electrode guide 11 in the circumferential direction. 5(c), for example, about 1 / 4 of the circumferential range of the electrode guide 11 may be a divided body 113, and this divided body 113 may be detachable from the remaining portion 112. In this case, the range in which the divided body 113 is provided may be the minimum range in which the pressed body of the sample 21 can be removed.

[0028] In the embodiment, the size of the divided body 113 (the size of the opening of the electrode guide 11) is based on the circumferential length of the outer peripheral surface of the electrode guide 11. "The divided body 113 is in a range of about 1 / 4 of the circumference of the electrode guide 11" means that the divided body 113 is cut out along a straight line (or a tangent line extended to the inner peripheral surface) extending from both ends t1 of the 1 / 4 arc of the outer peripheral surface of the electrode guide 11 to both ends t2 of the 1 / 2 arc of the inner peripheral surface of the electrode guide 11 in the cross-sectional view of FIG. 5. At this time, the remaining portion 112 excluding the divided body 113 forms an opening having an opening width h1 equal to or larger than the diameter of the inner peripheral surface of the electrode guide 11 (equal to or larger than the diameter of the cylindrical pressed body formed in the electrode guide 11). This makes it possible to take out the pressed body of the sample 21 even when the divided body 113 is in a range of less than half the circumference of the electrode guide 11.

[0029] In other words, at least a portion of the electrode guide 11 in the circumferential direction is formed as a separate divided body from the remaining portion, and this divided body can be attached and detached from the remaining portion before and after pressing to form an open portion through which the pressed body of sample 21 can be removed. In the embodiment, an example is shown in which the divided bodies are arranged over a range of 1 / 2 or 1 / 4 of the circumference of the electrode guide 11, but this is not limited to the configuration. For example, the divided bodies may be made small to about 1 / 8 of the circumference of the electrode guide 11 (provided that they can withstand the internal pressure of the press). In this case, the open portion of the remaining portion 112 has an opening width h1 that is equal to or larger than the diameter of the inner surface of the electrode guide 11. Furthermore, the electrode guide 11 is not limited to being divided into two in the circumferential direction, but may be divided into three or more in the circumferential direction. In this case, if the circumferential length of the inner surface of each divided body is less than 1 / 2 the circumference of the electrode guide 11, the pressed body of the sample 21 can be taken out.

[0030] First, the overall flow of manufacturing the all-solid-state battery cell (basic evaluation cell) 23 will be described. 1 shows a state in which a powder sample 21 (SE (solid electrolyte)) is sandwiched between the short axis convex portion 5 and the long axis convex portion 9, the short axis convex portion 5, the long axis convex portion 9 and the outer periphery of the sample 21 are covered with a covering material 16, and the outer periphery of the covering material 16 is covered with an electrode guide 11. In this state, a load of about human force is applied in the pressing direction to the short axis current collecting block 3 and the long axis current collecting block 7 without using a press machine, and pressure is applied to the extent that the sample 21 hardens into a temporary shape.

[0031] Thereafter, as shown in Fig. 2, the electrode guide 11 is removed, and the position of the semi-transparent covering material 16 that covers the sample 21 is visually confirmed. Then, a cut is made with a cutter or the like at the position of the covering material 16 that covers the sample 21, and the reference electrode 22 is inserted radially. Since the sample 21 is in a hardened state with a light load, it is easy to insert the reference electrode 22. The gap between the electrode guide 11 and the reference electrode 22 is sealed with insulating putty, epoxy resin bond, dental cement, or the like. By preventing the reference electrode 22 from moving, it is possible to suppress the occurrence of unexpected changes in potential, etc.

[0032] 3 and 4, the electrode guide 11 is attached again, a metal reference device is attached to the electrode guide 11, and the electrode guide 11 is fixed into a cylindrical shape. One half 13 of the electrode guide 11 has a through hole 14 through which the wiring side of the reference electrode 22 is inserted. In this state, the short-axis current collecting block 3 and the long-axis current collecting block 7 are attached to the movable and fixed dies of a press, respectively, and pressed with the press at a specified pressure.

[0033] Next, the manufacture of the all-solid-state battery cell (basic evaluation cell) 23 in this embodiment will be described in more detail. In the embodiment, as shown in FIG. 6, the short-axis current collecting block 3 is placed upside down, and the short-axis protrusion 5 is covered with a covering material 16 (polyimide tube) from above. A powder sample 21 (SE powder) is placed in the covering material 16, and the sample 21 is deposited on the tip of the short-axis protrusion 5. After that, the long-axis protrusion 9 of the long-axis current collecting block 7 is inserted into the covering material 16 from above, and the sample 21 is sandwiched between the short-axis protrusion 5. At this time, the outer periphery of the covering material 16 is covered with an electrode guide 11. In this state, a load of about human force is applied to the short-axis current collecting block 3 and the long-axis current collecting block 7, and pressure is applied to the extent that the sample 21 hardens into a temporary shape. The hardness of the sample 21 at this time is determined by the extent to which the powder does not fall off even if the long-axis protrusion 9 is removed from the covering material 16 and the covering material 16 is turned upside down.

[0034] Thereafter, the electrode guide 11 is removed, and the sample 21 portion is visually confirmed from the polyimide tube (coating material 16) (see FIG. 2). Then, a cut is made in the sample 21 portion of the covering material 16 using a cutter or the like, and the reference electrode 22 is inserted radially. Alternatively, the reference electrode 22 may be placed in the polyimide tube (coating material 16) before the sample 21 is introduced, and then the sample 21 may be introduced. The insertion location may be sealed with polyimide tape or the like.

[0035] The reference electrode 22 here is assumed to be an LTO or LFP used in general lithium ion batteries, etc., electrically connected with a platinum or Ni wire, etc., but there are no particular limitations on the material or structure as long as it is possible to obtain a reference potential with respect to the electrode and insulation is maintained between the reference electrode 22 and the measuring device.

[0036] As shown in FIG. 7, at this stage, either the short axis convex portion 5 or the long axis convex portion 9 is removed, and the positive electrode 21a is placed on the sample 21 in the temporary shape. In this embodiment, the short axis convex portion 5 is removed. The positive electrode 21a may be of either a dry or wet type, but when a current collecting foil is placed, the current collecting foil is placed on the current collecting block side, not on the sample 21 side. In this embodiment, an example is shown in which the positive electrode 21a is placed on the short axis convex portion 5 side. When introducing the sample 21 or the like into the covering material 16, the sample 21 is allowed to flow along the covering material 16, particularly when the sample 21 has a sol-like temporary shape.

[0037] The effects of the configuration thus far are that, first, the electrode guide 11 can be removed, so that the position of the sample 21 can be visually confirmed, making it easier to confirm the position for inserting the reference electrode 22. In addition, even after the reference electrode 22 is inserted, the insertion state can be visually confirmed. In addition, by using a polyimide tube for the covering material 16, the powder does not spill out even if a cut is made in the cross section of the sample 21.

[0038] As shown in FIG. 8, one half 13 of the electrode guide 11 has a through hole 14 for inserting the reference electrode 22. After inserting the short-axis protrusion 5 into the covering material 16 again, insert the wiring side of the reference electrode 22 into the through hole 14 of the half 13, and move the half 13 close to the covering material 16 until it comes into contact with the covering material 16. The other half 12 is brought into contact with the covering material 16 from the opposite side. This causes the covering material 16, its inner short-axis protrusions 5 and 9, and the sample 21 to be sandwiched between the pair of half halves 12 and 13. If there is a gap between the through hole 14 for inserting the reference electrode 22 and the reference electrode 22, use epoxy resin bond or dental cement to fill the gap. At this time, be careful not to interfere with the reference electrode 22.

[0039] 9, a restraining device 18 is attached to the electrode guide 11 to fix it into a cylindrical shape. In this state, the short-axis current collecting block 3 and the long-axis current collecting block 7 are attached to the movable and fixed dies of a press, respectively, and the powder compaction press is performed by the press at a specified pressure (maximum equivalent to 1000 MPa).

[0040] The electrode guide 11 is fixed using polyimide tape or the like to hold the electrode guide 11 in a position that does not interfere with the reference electrode 22. A through-hole (not shown) for inserting the reference electrode 22 is also formed in the restraining device 18, and the reference electrode 22 is inserted into the through-hole of the restraining device 18, and the electrode guide 11 is restrained while being careful not to interfere with it. In this state, powder compaction (maximum equivalent to 1000 MPa) is performed using a press.

[0041] The effects of the configuration thus far include, firstly, being able to visually check the state of the reference electrode 22 at each stage of molding by being able to remove the electrode guide 11. Also, in addition to being able to remove the electrode guide 11, by using the polyimide tube covering material 16, it becomes possible to perform in situ analysis on the all-solid-state battery cell (basic evaluation cell) 23 while keeping it in a state where it is not exposed to the atmosphere.

[0042] As shown in Fig. 10, after the powder compaction, the restraining device 18 is removed once, the current collecting block opposite the positive electrode 21a is removed, and then the negative electrode 21b (Li, etc.) is placed on the sample 21. When placing a current collecting foil, the current collecting foil is placed on the current collecting block side, not on the sample 21 side. In order to hold the electrode guide 11 in a position where it does not interfere with the reference electrode 22, the electrode guide 11 is fixed using polyimide tape or the like.

[0043] 11, the reference electrode 22 is inserted into the through hole formed in the restraining device 18 for inserting the reference electrode 22, and the electrode guide 11 is restrained while being careful not to interfere with the electrode guide 11. In this state, a pressure bonding press is performed to bond the negative electrode 21b to the sample 21. (In the case of Li, the pressure is equivalent to 150 MPa. In the case of either material, the pressure is lower than that of the previous powder compacting press.)

[0044] Thereafter, as shown in Fig. 12, the restraining device 18 and the electrode guide 11 are removed. In order to maintain the restraining pressure (equivalent to 1 to 5 MPa) in the pressing direction of the fabricated all-solid-state battery cell (basic evaluation cell) 23, the current collecting blocks 3, 7 are fastened together using bolts 19 or the like. Since the pressure at this time is much lower than that during molding, if it is confirmed that the shape of the sample can be maintained, it is not necessary to attach the restraining parts and electrode guide 11. Depending on the situation, only the electrode guide 11 may be attached.

[0045] The effects of the configuration thus far include, firstly, being able to visually check the state of the reference electrode 22 at each stage of molding by being able to remove the electrode guide 11. Also, in addition to being able to remove the electrode guide 11, by using the polyimide tube covering material 16, it becomes possible to perform in situ analysis on the all-solid-state battery cell (basic evaluation cell) 23 while keeping it in a state where it is not exposed to the atmosphere.

[0046] In order to keep the covering material 16 from being exposed to the atmosphere, after pressing is completed, both ends of the covering material 16 are sealed by, for example, bonding with a heat sealer. Alternatively, after pressing is completed, both ends of the covering material 16 are sealed by, for example, bonding with epoxy resin. These sealing methods may use a heat sealer on one side and an adhesive on the other. If the covering material 16 has excess length, it may be sealed by rolling or twisting it without bonding it, or by using a tool such as a clip.

[0047] For example, an information-bearing section for recording identifying information of the sample 21 may be provided on the outer surface of the covering material 16. This allows the sample 21 to be identified at its destination. The paint or ink used for printing or writing on the information-bearing section is transparent to X-rays. This makes it possible to reduce the influence of the X-ray inspection of the sample 21 on the inspection.

[0048] As described above, the configuration of the above embodiment is a manufacturing apparatus 1 for an all-solid-state battery cell 23 using a press machine, and includes a cylindrical electrode guide 11 that covers the sample 21, and a cylindrical covering material 16 that is disposed between the electrode guide 11 and the sample 21 and is detachable from the electrode guide 11. According to this configuration, by covering the sample 21 with the cylindrical covering material 16 inside the electrode guide 11, it is possible to easily remove the sample 21 that is difficult to remove due to adhesion. Since the sample 21 is contained inside the covering material 16, cleaning of the electrode guide 11 is not necessary, and the next work can be performed inside the glove box, thereby improving manufacturing efficiency. By removing the electrode guide 11, it is possible to check whether the sample 21 is stacked normally before and after pressing.

[0049] In the manufacturing apparatus 1 for the all-solid-state battery cell 23, the covering material 16 is made of polyimide. Specifically, the covering material 16 is made of a polyimide film. According to this configuration, by forming the covering material 16 from polyimide, the influence of the pressed body in the covering material 16 on the X-ray inspection is suppressed, and the pressed body can be removed from the electrode guide 11 without being exposed to the atmosphere. The covering material 16 can be formed from a commonly available material such as Kapton (registered trademark).

[0050] Moreover, the configuration of the embodiment is a manufacturing apparatus 1 for an all-solid-state battery cell 23 using a press machine, and includes a cylindrical electrode guide 11 that covers the sample 21, and at least a portion of the electrode guide 11 in the circumferential direction (one of the half bodies 12, 13, the divided body 113) is a divided body that is separate from the remaining portion (the other half body 12, 13, the remaining portion 112), and the divided body is detachable from the remaining portion before and after pressing. According to this configuration, the divided bodies of the electrode guide 11 can be attached and detached before and after pressing, so that the divided bodies are attached before pressing to form a cylindrical electrode guide 11 which functions as an outer wall during pressing, and the divided bodies can be removed after pressing to check whether the sample 21 is stacked normally. By making the electrode guide 11 into a split structure, even a pressed body of the sample 21 that is difficult to remove due to adhesion can be easily removed. It is possible to insert a reference electrode 22 into the pressed body through the opening when the divided body is removed and measure whether it is electrically connected, which shortens the manufacturing time and also makes it possible to attach the divided body again and press it. In addition, this configuration makes it easy to add additional samples 21 when changing the pressing pressure and pressing multiple times.

[0051] In the manufacturing apparatus 1 for the all-solid-state battery cell 23, the joint between the divided body and the remaining portion may be a concave-convex fitting portion 115 having a convex portion that fits into each other. According to this configuration, the joint between the divided body and the remaining part is the concave-convex fitting part 115, so the divided body is unlikely to peel off, and positional deviation of the divided body is suppressed, and then the sample 21 can be pressed. For example, in the case of a halved electrode guide 11 (made of zirconia), deviation may occur if the outer periphery is not positioned, but by having the concave-convex fitting part 115 at the joint, positional deviation of the divided body can be suppressed.

[0052] In the manufacturing apparatus 1 for the all-solid-state battery cell 23, the electrode guide 11 may have a divided body 113 in a range less than halfway around the circumference and from which the pressed body of the sample 21 can be removed. In this case, the remaining portion 112 of the electrode guide 11 excluding the divided body 113 forms an opening having an opening width h1 equal to or larger than the diameter of the pressed body of the sample 21. With this configuration, compared to when the electrode guide 11 is divided in half, the range of the divided body 113 is narrowed to reduce the opening of the electrode guide 11, and the minimum opening through which the pressed body of the sample 21 can be set is set so that the pressed body of the sample 21 can be removed. Since the remaining portion 112 excluding the divided body 113 has an opening width h1 that is equal to or larger than the diameter of the pressed body of the sample 21, the pressed body of the sample 21 can be reliably removed even when the divided body 113 is set to a range less than halfway around the circumference.

[0053] In the manufacturing apparatus 1 for the all-solid-state battery cell 23, the electrode guide 11 may be made of zirconia. According to this configuration, by forming the electrode guide 11 from zirconia, which is one of the ceramics with high strength, it is possible to form an electrode guide 11 that is suppressed from deforming and can withstand pressure even if it has a divided structure.

[0054] The manufacturing apparatus 1 for the all-solid-state battery cell 23 includes a restraining device 18 for restraining the electrode guide 11 from the outer periphery side. According to this configuration, the electrode guide 11 having a split structure is restrained by the restraining device 18, and pressing is performed in this state, so that the electrode guide 11 can withstand the internal pressure caused by pressing.

[0055] Moreover, the configuration of the above embodiment is a manufacturing method for an all-solid-state battery cell 23 using a press, and includes a cylindrical electrode guide 11 that covers the sample 21, and a cylindrical covering material 16 that is disposed between the electrode guide 11 and the sample 21 and is detachable from the electrode guide 11, and the sample 21 is poured along the covering material 16. According to this configuration, by pouring the sample 21 along the covering material 16, even if the powder of the sample 21 is in a temporary sol-like shape, the sample 21 can be guided by the covering material 16, making it easy to introduce the sample 21 into the stacking position.

[0056] In the above-described method for manufacturing the all-solid-state battery cell 23, after pressing is completed, at least one of both ends of the covering material 16 may be fixed and sealed with a heat sealer. According to this configuration, by fixing and sealing the ends of the covering material 16, the pressed sample 21 can be taken out of the glove box without being exposed to the atmosphere.

[0057] In the above-described method for manufacturing the all-solid-state battery cell 23, after pressing is completed, at least one of both ends of the covering material 16 may be adhered and sealed with an epoxy resin. According to this configuration, by gluing and sealing the ends of the covering material 16, the pressed sample 21 can be taken out of the glove box without being exposed to the atmosphere.

[0058] In the method for manufacturing the all-solid-state battery cell 23, specific information about the sample 21 may be written on the surface of the covering material 16. According to this configuration, by writing specific information of the sample 21 in the information-writing section, it is possible to prevent misassembly and make the sample 21 easier to identify.

[0059] In the manufacturing method of the all-solid-state battery cell 23, the specific information is written using paint that transmits X-rays. According to this configuration, by using a material that transmits X-rays for writing on the covering material 16, it is possible to prevent the information written on the covering material 16 from affecting the X-ray inspection.

[0060] In the manufacturing method of the all-solid-state battery cell 23, a short-axis current collecting block 3 and a long-axis current collecting block 7 are fixed to the movable side and fixed side of a press machine, respectively, and the short-axis current collecting block 3 and the long-axis current collecting block 7 each have a short-axis convex portion 5 and a long-axis convex portion 9 that are inserted into the interior from the end of a covering material 16, the short-axis convex portion 5 is shorter than the long-axis convex portion 9, the short-axis convex portion 5 is inserted into the covering material 16 from one end side, an electrode guide 11 is arranged on the outer periphery of the covering material 16, a sample 21 is introduced onto the tip of the short-axis convex portion 5 in the covering material 16, and the long-axis convex portion 9 is inserted into the covering material 16 from the other end side to press the sample 21. According to this configuration, by pressing the sample 21 inside the cylindrical covering material 16, the covering material 16 can be used to press the laminate.

[0061] In the method for producing the all-solid-state battery cell 23, the long axis protrusion 9 is once removed, and an additional laminate (negative electrode 21b) is laminated on the pressed sample 21, and then the long axis protrusion 9 is inserted again and pressed. According to this configuration, pressing can be performed that is suitable for stacking additional laminates that are sensitive to pressure, and the additional laminates can be easily introduced even when pressing multiple times with different pressures.

[0062] Moreover, the configuration of the above embodiment is a manufacturing method for an all-solid-state battery cell 23 using a press machine, and includes a cylindrical electrode guide 11 that covers a sample 21, at least a portion of the electrode guide 11 in the circumferential direction is a divided body that is separate from the remaining portion, the all-solid-state battery cell 23 is pressed in a plurality of stages, and the divided body is attached to and detached from the remaining portion each time pressing is performed. According to this configuration, when pressing is performed in multiple stages to mold a pressed body such as compressed lithium, it is possible to attach and detach the divided bodies after each pressing to check whether the sample 21 is stacked normally, and a high-quality laminate can be easily formed.

[0063] In the manufacturing method of the all-solid-state battery cell 23, the sample 21 is introduced into the electrode guide 11 and pressurized to form a temporary shape, and then the reference electrode 22 is inserted into the sample 21 in the temporary shape. According to this configuration, once pressing, the solid electrolyte can be managed to a certain extent as a solid, and by reducing the pressing pressure to form a solid electrolyte having a temporary shape into which the reference electrode 22 can be easily inserted, the production of the all-solid-state battery cell 23 can be facilitated.

[0064] In the manufacturing method of the all-solid-state battery cell 23, the sample 21 is covered on the inside of the electrode guide 11 with a covering material 16 made of a polyimide film. This configuration can prevent other materials from being mixed inside the electrode guide 11. The covering material 16 can be made of a commonly available material such as Kapton (registered trademark).

[0065] In the manufacturing method of the all-solid-state battery cell 23, the polyimide film covering material 16 is cut and peeled off to expose the pressed body of the sample 21. According to this configuration, the pressed body of the sample 21 can be easily exposed and checked, and the reference electrode 22 can be easily inserted.

[0066] In the manufacturing method of the all-solid-state battery cell 23, the sample 21 introduced into the covering material 16 is pressed in the axial direction while the divided body 113 and the remaining portion 112 of the electrode guide 11 are restrained from the outer periphery side. According to this configuration, by pressing the sample 21 in the covering material 16 while the electrode guide 11 having a split structure is restrained, the sample 21 can be pressed while enduring the internal pressure caused by the press.

[0067] The configuration of the embodiment described above is one example of the present invention, and various modifications are possible without departing from the gist of the present invention, such as replacing the components of the embodiment with well-known components. [Explanation of symbols]

[0068] 1 Manufacturing equipment 3 Short-axis collector block (first fixture) 5 Short axis convex part (first convex part) 7 Long-axis current collecting block (second jig) 9 Long axis convex part (second convex part) 11 Electrode Guide 12,13 Half body 16 Covering material 18 Restraint Devices 21 Sample 22 Reference electrode 23 All-solid-state battery cell (basic evaluation cell) 112 Remaining parts 113 Split body 115 Concave-convex fitting part

Claims

1. An apparatus for manufacturing an all-solid-state battery cell using a press machine, A cylindrical electrode guide is provided to cover the sample. At least a portion of the electrode guide in a circumferential direction is a separate divided body from the remaining portion, The divided body is detachable from the remaining portion before and after pressing.

2. The manufacturing apparatus for an all-solid-state battery cell according to claim 1 , wherein a joint between the divided body and the remaining portion is a concave-convex fitting portion having a convex portion and a concave portion that fit together.

3. The manufacturing apparatus for an all-solid-state battery cell according to claim 1 , wherein the electrode guide has a divided body in a range of less than halfway around the circumference and from which the pressed body of the sample can be removed.

4. The manufacturing apparatus for an all-solid-state battery cell according to claim 3 , wherein a remaining portion of the electrode guide excluding the divided body forms an opening having an opening width equal to or larger than a diameter of the pressed body.

5. The apparatus for manufacturing an all-solid-state battery cell according to claim 1 , wherein the electrode guide is made of zirconia.

6. The manufacturing apparatus for an all-solid-state battery cell according to claim 1 , further comprising a restraining device that restrains the electrode guide from an outer periphery side.

7. A method for manufacturing an all-solid-state battery cell using a press, comprising: A cylindrical electrode guide is provided to cover the sample. At least a portion of the electrode guide in a circumferential direction is a separate divided body from the remaining portion, The all-solid-state battery cell is pressed in multiple stages, The divided body is attached to and detached from the remaining portion each time the divided body is pressed.

8. The method for manufacturing an all-solid-state battery cell according to claim 7 , further comprising the steps of: introducing the sample into the electrode guide and applying pressure to form a temporary shape; and then inserting a reference electrode into the sample in the temporary shape.

9. The method for manufacturing an all-solid-state battery cell according to claim 7 or 8, wherein the sample is covered on the inside of the electrode guide with a covering material made of a polyimide film.

10. The method for producing an all-solid-state battery cell according to claim 9 , wherein the covering material made of a polyimide film is peeled off by cutting to expose the pressed body.

11. The method for manufacturing an all-solid-state battery cell according to claim 9 , wherein the sample introduced into the covering material is pressed in an axial direction in a state in which the divided body and the remaining portion of the electrode guide are constrained from an outer periphery side.

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