JP2012119236A - Battery manufacturing method, battery, motor vehicle, rf-id tag, and electronic device - Google Patents

Abstract

PROBLEM TO BE SOLVED: To provide: a battery arranged so that the short circuit of positive and negative electrodes can be prevented with reliability, and having excellent battery characteristics; a battery manufacturing method by which such battery can be manufactured with a high productivity; and a device having the battery.SOLUTION: The battery manufacturing method comprises the steps of: applying, by a nozzle dispensing method, a solid electrolytic material-containing coating liquid to an electrolytic region 11 which is a gap between negative and positive electrode current collectors 121 and 131 provided on a surface of an insulative base material 10 to be opposed to each other thereby to form an electrolytic partition wall 111 made of solid electrolyte in the electrolytic region 11 in contact with the surface of the base material 10; after that, applying a negative electrode active material-containing coating liquid to a surface of the negative electrode current collector 121 thereby to form a negative electrode active material layer 122; and applying a positive electrode active material-containing coating liquid to a surface of the positive electrode current collector 131 thereby to form a positive electrode active material layer 132. Since the negative and positive electrode active material layers 122 and 132 are formed after formation of the electrolytic partition wall 111, the short circuit thereof can be prevented with reliability.

Description

  The present invention relates to a method for manufacturing a battery such as a lithium ion secondary battery in which a solid electrolyte layer is interposed between active material layers, a battery manufactured by the manufacturing method, and a device on which the battery is mounted.

  Conventionally, as a method of manufacturing a chemical battery such as a lithium ion battery, a metal foil as a current collector and a positive electrode active material and a negative electrode active material, which are attached to each other, are overlapped via a separator such as a nonwoven fabric. A technique for impregnating a separator with an electrolytic solution is known. However, since batteries that contain highly volatile organic solvents as electrolytes need to be handled with care, and further downsizing and higher output are required, in recent years solid electrolytes have been used instead of electrolytes. Techniques to use have been proposed.

  For example, in the technique disclosed in Patent Document 1, a positive electrode current collector and a negative electrode current collector made of a conductor such as a metal are formed on an insulating substrate so as to be close to each other, and on these current collectors, Positive and negative active material layers are formed by applying a slurry containing a positive electrode active material and a negative electrode active material, respectively. Then, by filling the gap between the positive and negative electrodes formed in this manner with a material containing a solid electrolyte, a secondary battery having a structure in which the positive and negative electrodes face each other through the solid electrolyte in the direction along the substrate surface is manufactured. ing.

JP 2006-147210 A

  Solid electrolytes that have been put to practical use so far generally have lower ionic conductivity than liquid electrolytes. Therefore, in order to obtain good charge / discharge characteristics in a battery using a solid electrolyte, it is necessary to reduce the thickness of the solid electrolyte layer interposed between the positive and negative active material layers. For this purpose, it is required to make the distance between the positive and negative active material layers as narrow as possible.

  Further, in order to obtain a high energy density in a battery using a solid electrolyte, it is necessary to increase the battery capacity per unit area. For that purpose, it is required to increase the height of the active material layer in the direction orthogonal to the substrate surface. In other words, in order to improve the characteristics of a battery using a solid electrolyte, it is necessary to reduce the thickness of the solid electrolyte layer and increase the height, that is, to increase the aspect ratio of the solid electrolyte layer. It becomes.

  However, in the technique disclosed in Patent Document 1, a battery is formed by a method in which a space between a positive electrode and a negative electrode formed so as to face each other is filled with a solid electrolyte material. Therefore, there is a possibility that the positive electrode and the negative electrode may be short-circuited in the battery manufacturing process, and particularly when the solid electrolyte layer is made as thin and high as possible as described above, the positive electrode active material and the negative electrode active material immediately after application are likely to contact each other. Therefore, it is difficult to reliably prevent a short circuit.

  The present invention has been made in view of the above problems, and a battery having excellent battery characteristics while reliably preventing a short circuit between positive and negative electrodes, a manufacturing method capable of manufacturing the battery with high productivity, and the battery It aims at providing the apparatus provided with.

  In order to solve the above-described problems, the invention of claim 1 is directed to an electrolyte between a negative electrode current collector and a positive electrode current collector provided to face the surface of an insulating base material in a battery manufacturing method. Applying a coating solution containing a solid electrolyte material in the region, and forming an electrolyte partition wall in the electrolyte region on the surface of the substrate; and after the electrolyte partition wall forming step, on the surface of the negative electrode current collector After the negative electrode active material layer forming step of forming a negative electrode active material layer by applying a coating solution containing a negative electrode active material and the electrolyte partition wall forming step, a coating liquid containing a positive electrode active material is applied to the surface of the positive electrode current collector. And a positive electrode active material layer forming step of forming a positive electrode active material layer by coating.

  The invention according to claim 2 is the battery manufacturing method according to claim 1, wherein the negative electrode current collector and the positive electrode current collector are arranged to face each other at a predetermined interval in a plan view. It is characterized by having a comb-like pattern.

  According to a third aspect of the present invention, in the battery manufacturing method according to the second aspect of the present invention, the height of the electrolyte partition is at least twice the width.

  According to a fourth aspect of the present invention, in the battery manufacturing method according to the third aspect of the present invention, in the electrolyte partition wall forming step, a coating solution to which a thermosetting agent or a photocuring agent is added is applied to the electrolyte region. Features.

  According to a fifth aspect of the present invention, in the battery manufacturing method according to any one of the first to fourth aspects, the negative electrode current collector and the positive electrode current collector are formed by a photolithography method. It is characterized by.

  Further, the invention of claim 6 is the battery manufacturing method according to any one of claims 1 to 5, wherein, in the electrolyte partition wall forming step, a nozzle for discharging a coating liquid containing a solid electrolyte material is provided on the base. The coating liquid is applied to the electrolyte region by moving relative to the surface of the material.

  The invention of claim 7 is the battery manufacturing method according to the invention of claim 6, wherein in the electrolyte partition wall forming step, a coating solution containing a solid electrolyte material is provided from a plurality of discharge ports arranged in a row on the nozzle. The nozzle is moved relative to the surface of the substrate while being discharged.

  According to an eighth aspect of the present invention, in the battery manufacturing method according to any one of the first to seventh aspects, a protective layer that continuously covers the negative electrode active material layer and the positive electrode active material layer is formed. It further comprises a protective layer forming step.

  The invention of claim 9 is a battery, and is manufactured by the battery manufacturing method according to any one of claims 1 to 8.

  The invention of claim 10 is a vehicle, and is equipped with a battery according to the invention of claim 9.

  The invention of claim 11 is an RF-ID tag, characterized in that it comprises a battery according to the invention of claim 9.

  A twelfth aspect of the invention is an electronic device comprising the battery according to the ninth aspect of the invention and a circuit unit that operates using the battery as a power source.

  According to the first to seventh aspects of the present invention, the solid electrolyte material is included in the electrolyte region between the negative electrode current collector and the positive electrode current collector provided to face the surface of the insulating base material. A coating solution is applied to form an electrolyte partition in the electrolyte region, and then a coating solution containing a negative electrode active material is applied to the surface of the negative electrode current collector to form a negative electrode active material layer, and the surface of the positive electrode current collector Since a positive electrode active material layer is formed by applying a coating solution containing a positive electrode active material to the positive electrode, it is possible to reliably prevent a short circuit between the positive and negative electrodes, and to face a positive and negative active material across a wide area through a thin electrolyte partition Therefore, a battery having excellent battery characteristics capable of high-speed charge / discharge can be manufactured. In addition, since the electrolyte partition, the negative electrode active material layer, and the positive electrode active material layer are formed by applying the coating liquid, the number of steps is small, and the battery can be manufactured with high productivity.

  In particular, according to the second aspect of the present invention, the negative electrode current collector and the positive electrode current collector are formed in a comb-teeth pattern that is opposed to be meshed with each other at a predetermined interval in plan view. The contact area between the positive and negative active material layers per unit area on the material surface and the electrolyte partition can be increased, and the reaction efficiency of the battery can be improved.

  In particular, according to the invention of claim 3, since the height of the electrolyte partition is twice or more the width, the electrolyte partition is thin and high, and the height of the active material layer of the positive and negative electrodes can be increased. As a result, the battery capacity per unit area of the substrate surface can be increased and a high energy density can be obtained.

  In particular, according to the invention of claim 4, since the coating solution to which the thermosetting agent or the photo-curing agent is added is applied to the electrolyte region, it is possible to easily form a thin and high electrolyte partition wall by preventing dripping after application. Can do.

  In particular, according to the invention of claim 5, since the negative electrode current collector and the positive electrode current collector are formed by a photolithography method, the negative electrode current collector and the positive electrode current collector are formed facing each other with high positional accuracy. It is possible to prevent positive and negative current collectors from contacting each other. Further, the negative electrode current collector and the positive electrode current collector can be made difficult to peel off from the base material.

  In particular, according to the invention of claim 6, since the nozzle for discharging the coating liquid containing the solid electrolyte material is moved relative to the surface of the base material and the coating liquid is applied to the electrolyte region, the electrolyte region is accurately applied. In addition, the electrolyte partition can be formed by applying the coating liquid at a high throughput.

  In particular, according to the invention of claim 7, in order to move the nozzle relative to the surface of the substrate while discharging the coating liquid containing the solid electrolyte material from the plurality of discharge ports arranged in a row on the nozzle, For the electrolyte regions parallel to each other, the time required for the coating process can be remarkably shortened.

  According to the ninth aspect of the invention, since the battery is manufactured by the method for manufacturing a battery according to any one of the first to eighth aspects, the battery characteristics can be prevented while reliably preventing a short circuit between the positive and negative electrodes. It can be excellent.

  According to the invention of claim 10, the battery according to the invention of claim 9 can be suitably used as a power source for driving the vehicle.

  According to the invention of claim 11, the battery according to the invention of claim 9 can be suitably used as a power source for the RF-ID tag.

  According to the invention of claim 12, the battery according to the invention of claim 9 can be suitably used as the power source of the circuit portion of the electronic device.

It is a top view of the lithium ion secondary battery manufactured by the manufacturing method of the battery which concerns on this invention. It is sectional drawing which shows the AA cut surface of the lithium ion secondary battery of FIG. It is a flowchart which shows the manufacture procedure of a lithium ion secondary battery. It is a perspective view of the laminated body in which the negative electrode collector and the positive electrode collector were formed on the surface of the base material. It is a figure which shows the structure of the coating unit used for the nozzle dispensing method. It is sectional drawing which shows the internal structure of a discharge nozzle. It is a perspective view of the stage in which the electrolyte partition of the solid electrolyte was formed in the surface of a base material. It is sectional drawing which shows the BB cut surface of the laminated body of FIG. It is a perspective view in the stage where the negative electrode active material layer was formed on the surface of the negative electrode current collector. It is sectional drawing which shows CC cut surface of the laminated body of FIG. It is a perspective view in the stage where the positive electrode active material layer was formed on the surface of the positive electrode current collector. It is sectional drawing which shows the DD cut surface of the laminated body of FIG. It is a figure which shows typically the electric vehicle carrying the lithium ion secondary battery which concerns on this invention. It is a figure which shows typically the RF-ID tag carrying the lithium ion secondary battery which concerns on this invention. It is a figure which shows the other example of the pattern of a negative electrode collector and a positive electrode collector. It is a figure which shows the other example of the pattern of a negative electrode collector and a positive electrode collector.

  Hereinafter, embodiments of the present invention will be described in detail with reference to the drawings.

<1. Lithium-ion battery structure>
FIG. 1 is a top view of a lithium ion secondary battery 1 manufactured by the battery manufacturing method according to the present invention. 2 is a cross-sectional view showing an AA cut surface of the lithium ion secondary battery 1 of FIG. In each drawing after FIG. 1, the dimensions and number of each part are exaggerated or simplified as necessary for easy understanding. A lithium ion secondary battery is a secondary battery (storage battery) in which lithium ions are responsible for electrical conduction, has a high energy density, a small memory effect, and a low deterioration due to repeated charge and discharge. Have. The lithium ion secondary battery 1 has a structure in which negative electrode regions 12 and positive electrode regions 13 that are separated from each other by an electrolyte partition wall 111 of a solid electrolyte are alternately arranged on the surface of an insulating base material 10. . That is, the electrolyte partition 111 is provided between the negative electrode region 12 and the positive electrode region 13.

  As shown in FIG. 2, in the negative electrode region 12, a negative electrode current collector 121 is formed on the surface of the substrate 10, and a negative electrode active material layer 122 is laminated on the surface of the negative electrode current collector 121. As shown in FIG. 1, the tip of the negative electrode current collector 121 is formed in a comb-like shape having a plurality of teeth at predetermined intervals, and each tooth is located in the negative electrode region 12. The entire negative electrode current collector 121 is a single metal film, and the negative electrode current collectors 121 formed in the plurality of negative electrode regions 12 are electrically connected to each other. The end of the negative electrode current collector 121 opposite to the comb teeth is a negative electrode tab 123.

  Similarly, in the positive electrode region 13 separated from the negative electrode region 12 and the electrolyte partition wall 111, the positive electrode current collector 131 is formed on the surface of the base material 10, and the positive electrode active material layer 132 is laminated on the surface of the positive electrode current collector 131. Has been. The tip of the positive electrode current collector 131 is formed in a comb shape having a plurality of teeth at predetermined intervals, and each tooth is located in the positive electrode region 13. The pitch of the comb teeth of the negative electrode current collector 121 and the positive electrode current collector 131 is equal, and the negative electrode current collector 121 and the positive electrode current collector 131 are provided to face each other so that both the comb teeth mesh with each other. Further, the positive electrode current collector 131 is also a single metal film, and the positive electrode current collectors 131 formed in the plurality of positive electrode regions 13 are electrically connected to each other, and are opposite to the comb teeth of the positive electrode current collector 131. The part is a positive electrode tab 133.

  A gap between the comb teeth of the negative electrode current collector 121 and the comb teeth of the positive electrode current collector 131 in the surface of the substrate 10 is an electrolyte region 11. A coating solution containing a solid electrolyte material is applied to the electrolyte region 11 by a nozzle dispensing method to form a solid electrolyte electrolyte partition 111.

  The protective layer 14 is formed so as to continuously cover the surfaces of the negative electrode active material layer 122 formed in the negative electrode region 12 and the positive electrode active material layer 132 formed in the positive electrode region 13. As the protective layer 14, for example, the same solid electrolyte that forms the electrolyte partition wall 111 can be used.

  In such a structure, the negative electrode structure 120 including the negative electrode current collector 121 and the negative electrode active material layer 122 stacked in the negative electrode region 12, and the positive electrode current collector 131 and the positive electrode active material layer stacked in the positive electrode region 13. The positive electrode structure 130 made of 132 is disposed so as to face a thin and high electrolyte partition wall 111 formed of a solid electrolyte. For this reason, the charge and lithium ions move between the negative electrode active material layer 122 and the positive electrode active material layer 132 through the solid electrolyte, thereby functioning as the lithium ion secondary battery 1. Such a lithium ion secondary battery 1 is accommodated in a casing to form a secondary battery as a final product.

<2. Manufacturing method of lithium ion battery>
Next, a method for manufacturing the lithium ion secondary battery 1 having the above configuration will be described. FIG. 3 is a flowchart showing a manufacturing procedure of the lithium ion secondary battery. First, the insulating base material 10 is prepared (step S1). The base material 10 is a flat plate member formed of an insulating material, and for example, a resin substrate such as a flexible substrate, a glass substrate, a ceramic substrate, or the like can be used. If the lithium ion secondary battery 1 is incorporated in an RF-ID tag as will be described later, it is preferable to use a flexible substrate having flexibility.

  Next, the negative electrode current collector 121 and the positive electrode current collector 131 are formed on the surface of the insulating base material 10 (step S2). In the present embodiment, the negative electrode current collector 121 and the positive electrode current collector 131 are formed using a so-called photolithography method. Specifically, first, a metal (copper in this embodiment) film that forms the negative electrode current collector 121 is formed on the surface of the base material 10 by vacuum deposition or sputtering. Then, a photoresist (photosensitive organic substance) is applied thereon to form a resist film, and the surface of the resist film is exposed to the shape of the negative electrode current collector 121 having a comb-like pattern. Subsequently, the exposed portion (or non-exposed portion) of the resist film is removed by development processing, and the metal film is etched using the remaining resist film as a mask. Thereafter, by removing all the resist films, the negative electrode current collector 121 having a comb-like pattern is formed on the surface of the substrate 10.

  Similarly, a positive electrode current collector 131 having a comb-like pattern is also formed. At this time, it is preferable to form a film of metal (aluminum in this embodiment) constituting the positive electrode current collector 131 by masking the previously formed negative electrode current collector 121. As a mask for the negative electrode current collector 121, the resist film remaining after the above development processing may be used as it is.

  FIG. 4 is a perspective view of a laminate in which the negative electrode current collector 121 and the positive electrode current collector 131 are formed on the surface of the base material 10. As shown in the figure, the negative electrode current collector 121 and the positive electrode current collector 131 are formed in a comb-like pattern that is arranged to face each other at a predetermined interval in plan view. That is, both of the negative electrode current collector 121 and the positive electrode current collector 131 are formed in a comb-like shape having a plurality of teeth, and the arrangement pitch of these teeth (the interval between adjacent teeth) is equal to each other. The teeth of the negative electrode current collector 121 enter between adjacent teeth of the positive electrode current collector 131 and the teeth of the positive electrode current collector 131 enter between adjacent teeth of the negative electrode current collector 121. The electric body is arranged. However, the negative electrode current collector 121 and the positive electrode current collector 131 are not in contact with each other, and a gap with a predetermined interval is formed between the teeth of the negative electrode current collector 121 and the teeth of the positive electrode current collector 131. The two current collectors are arranged to face each other. Note that portions other than the comb-like pattern of the negative electrode current collector 121 and the positive electrode current collector 131 (for example, the negative electrode tab 123 and the positive electrode tab 133) are also formed by photolithography.

  The formation technique of the negative electrode current collector 121 and the positive electrode current collector 131 is not limited to the photolithography method, and various known techniques that can form a metal film having a predetermined pattern can be used. . For example, the negative electrode current collector 121 and the positive electrode current collector 131 may be formed by printing a comb-like pattern of metal particle dispersion droplets as a current collector material using an inkjet printer or an imprint technique. . Alternatively, the negative electrode current collector 121 and the positive electrode current collector 131 may be formed by patterning a material containing metal fine particles as a current collector material by an electrophotographic method such as a laser printer. Alternatively, the negative electrode current collector 121 and the positive electrode current collector 131 may be formed directly by vacuum deposition or sputtering after applying an appropriate mask. Furthermore, the current collectors 121 and 131 of both electrodes may be formed by applying a conductive paste containing metal particles to the surface of the substrate 10 by a nozzle dispensing method as described later.

  As the metal constituting the negative electrode current collector 121 and the positive electrode current collector 131, copper, aluminum, stainless steel, or the like can be used. However, as in the present embodiment, the negative electrode current collector 121 is formed of copper, and the positive electrode current collector 121 is formed. The electric body 131 is preferably formed of aluminum. The thicknesses of the negative electrode current collector 121 and the positive electrode current collector 131 are not particularly limited, but may be 5 μm to 20 μm, for example.

  Next, an electrolyte partition 11 is formed by applying a coating solution containing a solid electrolyte material to the base material 10 on which the negative electrode current collector 121 and the positive electrode current collector 131 are formed (step S3). The negative electrode current collector 121 and the positive electrode current collector 131 are pattern-formed in a comb-teeth shape so as to face each other so as to mesh with each other at a predetermined interval. The gap of a predetermined interval between the comb-like pattern of the negative electrode current collector 121 and the comb-like pattern of the positive electrode current collector 131 exposes the surface of the base material 10, and the gap serves as the electrolyte region 11. . In step S3, a coating solution containing a solid electrolyte material is applied to the electrolyte region 11 using a nozzle dispensing method.

  FIG. 5 is a diagram showing the configuration of the coating unit 2 used in the nozzle dispensing method. 5 and 6 are appropriately attached with an XYZ orthogonal coordinate system in which the Z-axis direction is a vertical direction and the XY plane is a horizontal plane in order to clarify the directional relationship.

  In the coating unit 2, the stage moving mechanism 20 is provided on the base 210, and the stage 30 that holds the substrate 10 can be moved in the horizontal plane (in the XY plane) by the stage moving mechanism 20. A discharge nozzle 40 is fixedly installed above the stage 30. That is, in the present embodiment, the stage 30 that holds the substrate 10 moves in a horizontal plane with respect to the discharge nozzle 40 that is fixedly installed, so that the discharge nozzle 40 moves relative to the surface of the substrate 10. It will be.

  The stage moving mechanism 20 includes an X direction moving mechanism 21 that moves the stage 30 in the X direction from the lower stage, a Y direction moving mechanism 22 that moves in the Y direction perpendicular to the X direction, and an axis along the vertical direction (Z direction). Is provided with a θ rotation mechanism 23 that rotates around the center. The X-direction moving mechanism 21 has a structure in which a ball screw 212 is connected to a motor 211 and a nut 213 fixed to the Y-direction moving mechanism 22 is screwed into the ball screw 212. When the guide rail 214 is fixed above the ball screw 212 and the motor 211 rotates, the Y-direction moving mechanism 22 moves smoothly along the guide rail 214 in the X direction along with the nut 213.

  The Y-direction moving mechanism 22 includes a motor 221, a ball screw mechanism, and a guide rail 224. When the motor 221 rotates, the θ rotation mechanism 23 moves in the Y direction along the guide rail 224 by the ball screw mechanism. The θ rotation mechanism 23 rotates the stage 30 about the axis along the Z direction by the motor 231. With the above configuration, the discharge nozzle 40 is relatively moved in the X direction and the Y direction relative to the surface of the substrate 10 by the stage moving mechanism 20, and the posture with respect to the substrate 10 can also be changed.

  One end of a supply pipe 422 is connected to the discharge nozzle 40 that is fixedly installed. A check valve 421 is inserted in the supply pipe 422. The other end of the supply pipe 422 is bifurcated, one of which is connected to a pump 423 and the other is connected to a tank 425 for storing a coating solution containing a solid electrolyte material via a control valve 424.

As a coating solution containing a solid electrolyte material, a polymer electrolyte material functioning as a solid electrolyte, for example, a resin such as polyethylene oxide and / or polystyrene, as a supporting salt, for example, lithium hexafluorophosphate (LiPF ₆ ) and a solvent For example, a mixture of diethylene carbonate and the like can be used. As the supporting salt, lithium perchlorate (LiClO ₄ ) or lithium bistrifluoromethanesulfonylimide (LiTFSI) may be used instead of lithium hexafluorophosphate.

  In particular, when the aspect ratio of the electrolyte partition 111 of the solid electrolyte is increased as described later, it is preferable to add a thermosetting agent that is cured by heating to a predetermined temperature or higher to the coating solution. As such a thermosetting agent, for example, methyl methacrylate as a monomer solution and 2,2′-azobis (isobutyronitrile) as a polymerization initiator and ethylene glycol dimethacrylate as a crosslinking agent are added. Can be used. Instead of the thermosetting agent, a photocuring agent that is cured by irradiation with light such as ultraviolet light may be added to the coating solution.

  FIG. 6 is a cross-sectional view showing the internal structure of the discharge nozzle 40. 6A shows a cross section of the discharge nozzle 40 cut along the YZ plane, and FIG. 6B shows a cross section cut along the XZ plane. As shown in FIG. 6, a cavity functioning as a buffer space BF is formed inside the discharge nozzle 40, and a coating solution of the solid electrolyte material fed to the buffer space BF via the supply pipe 422 is formed. It is sent. The discharge nozzle 40 is formed with a plurality of flow paths 41 extending downward from the buffer space BF. The plurality of flow paths 41 are provided in a row at equal intervals along the Y direction. The lower end opening of each flow path 41 forms a discharge port 44. Therefore, a plurality of discharge ports 44 are arranged in the Y direction on the lower end surface of the discharge nozzle 40. The arrangement interval of the plurality of discharge ports 44 is equal to the arrangement interval of the electrolyte region 11 formed by meshing the comb teeth of the negative electrode current collector 121 and the positive electrode current collector 131. Further, the opening shape of each discharge port 44 is substantially square, and the length of one side thereof is substantially the same as the width of the electrolyte region 11. The number of discharge ports 44 provided in the discharge nozzle 40 is not particularly limited, and may be an appropriate number according to the number of comb teeth.

  Each motor of the stage moving mechanism 20, the pump 423, and the control valve 424 are electrically connected to the control unit 38. The configuration of the control unit 38 as hardware is the same as that of a general computer. That is, the control unit 38 stores a CPU that performs various arithmetic processes, a ROM that is a read-only memory that stores basic programs, a RAM that is a readable and writable memory that stores various information, control software, data, and the like. It is configured with a magnetic disk to be placed. When the CPU of the control unit 38 executes a predetermined processing program, the above-described components of the coating unit 2 are controlled by the control unit 38, and the coating process including the solid electrolyte material on the electrolyte region 11 proceeds.

  When the coating liquid containing the solid electrolyte material is applied by the coating unit 2 having such a configuration, the base material 10 on which the comb-like negative electrode current collector 121 and the positive electrode current collector 131 are formed is placed on the upper surface of the stage 30. Place. The substrate 10 is fixed to the upper surface of the stage 30 by a clamp mechanism (not shown).

  Thereafter, the control unit 38 drives and controls each motor of the stage moving mechanism 20 to move the substrate 10 held on the stage 30 to the application start position. The application start position is a position where the discharge port 44 of the discharge nozzle 40 is directly above the electrolyte region 11. And after the base material 10 reaches | attains the application | coating start position, discharge of the coating liquid containing a solid electrolyte material from the discharge nozzle 40 is started.

  The discharge of the coating liquid from the discharge nozzle 40 is performed by the check valve 421, the pump 423, and the control valve 424 shown in FIG. First, the pump 423 performs a suction operation with the control valve 424 opened under the control of the control unit 38. At this time, since the check valve 421 prevents the backflow of the coating liquid from the discharge nozzle 40, the coating liquid containing the solid electrolyte material is sucked from the tank 425 to the pump 423. Next, the control valve 424 is closed under the control of the control unit 38, and the pump 423 performs an extrusion operation. Thereby, the coating liquid containing the solid electrolyte material is fed from the pump 423 to the discharge nozzle 40. The supplied coating liquid is once sent into the buffer space BF in the discharge nozzle 40 and then discharged downward from the plurality of discharge ports 44. Thus, since the discharge nozzle 40 discharges the coating liquid through the buffer space BF, the coating liquid containing the negative electrode active material at a uniform flow rate from the plurality of discharge ports 44 arranged in the Y direction. Can be discharged. In addition, when the viscosity of the coating liquid containing the solid electrolyte material is high and only the extrusion pressure of the pump 423 is not sufficient, the discharge nozzle 40 is also provided with a syringe pump or the like, and is stored in the buffer space BF by the syringe pump. The coating liquid may be pushed out from the plurality of discharge ports 44.

  At the same time as the discharge of the coating liquid from the discharge port 44 is started, the control unit 38 controls the stage moving mechanism 20 to start the movement of the stage 30. In the present embodiment, the stage 30 moves in one direction while the coating liquid containing the solid electrolyte material is continuously discharged from the plurality of discharge ports 44 of the discharge nozzle 40, and the coating liquid is linearly applied to the electrolyte region 11. Apply. At this time, since the coating liquid containing the solid electrolyte material is simultaneously ejected from the plurality of ejection ports 44, the coating liquid can be applied to a plurality of linear patterns parallel to each other by one nozzle scan.

  Thus, the nozzle dispensing method in which the discharge nozzle 40 is moved relative to the surface of the substrate 10 in one direction while discharging the coating liquid containing the solid electrolyte material from the plurality of discharge ports 44 arranged in a row. Thus, the coating liquid containing the solid electrolyte material is applied to the plurality of electrolyte regions 11 parallel to each other. By drying and curing this coating solution, electrolyte partition walls 111 are formed in the electrolyte region 11 on the surface of the substrate 10.

  FIG. 7 is a perspective view of a stage where the solid electrolyte electrolyte partition 111 is formed on the surface of the substrate 10. FIG. 8 is a cross-sectional view showing a BB cut surface of the laminate of FIG. A solid electrolyte electrolyte partition 111 is formed in the electrolyte region 11 in the gap between the comb-shaped pattern of the negative electrode current collector 121 and the comb-shaped pattern of the positive electrode current collector 131, and as a result, the electrolyte partition walls 111 are adjacent to each other. The teeth of the negative electrode current collector 121 and the teeth of the positive electrode current collector 131 are partitioned. The negative electrode current collector 121 and the positive electrode current collector 131 in contact with the electrolyte partition wall 111 become the negative electrode region 12 and the positive electrode region 13, respectively.

  The width EW of the electrolyte partition 111 of the solid electrolyte is 10 μm to 100 μm. As described above, the solid electrolyte generally has a lower ionic conductivity than the liquid electrolyte, and the width EW of the electrolyte partition 111 needs to be reduced in order to obtain good charge / discharge characteristics. From such a viewpoint, the width EW of the electrolyte partition wall 111 is set to 100 μm or less, and the width Ew is preferably set to 50 μm or less in order to obtain better charge / discharge characteristics. On the other hand, when the width EW of the electrolyte partition wall 111 is less than 10 μm, the electrolyte partition wall 111 becomes too thin and may cause a short circuit between the negative electrode structure 120 and the positive electrode structure 130. For this reason, the width Ew of the electrolyte partition 111 is set to 10 μm to 100 μm.

  The height EH of the electrolyte partition wall 111 is set to 10 μm to 100 μm. As described above, in order to obtain a high energy density in a battery using a solid electrolyte, it is necessary to increase the battery capacity per unit area. For this purpose, the height EH of the electrolyte partition 111 needs to be increased. From this point of view, the height EH of the electrolyte partition wall 111 is at least 10 μm, and the higher the better. But when the height EH of the electrolyte partition 111 exceeds 100 micrometers, there exists a possibility that productivity may fall.

  Thus, in the lithium ion secondary battery 1 using a solid electrolyte, in order to obtain good charge / discharge characteristics and high energy density, the width EW of the electrolyte partition 111 of the solid electrolyte is reduced and the height EH is increased. It is required to do. In other words, it is required to increase the aspect ratio (height EH / width EW) of the electrolyte partition 111, and is preferably set to 2 or more (that is, the height EH of the electrolyte partition 111 is at least twice the width EW). Preferably). For this reason, in this embodiment, the height EH of the electrolyte partition 111 of the solid electrolyte is 100 μm, and the width EW is 50 μm.

In order to increase the aspect ratio of the electrolyte partition 111, it is preferable to apply to the electrolyte region 11 a solution obtained by adding a thermosetting agent or a photocuring agent to the coating solution of the solid electrolyte material. A coating solution to which a photo-curing agent or a thermo-curing agent is added is applied to the electrolyte region 11, and immediately after the application, light irradiation with ultraviolet light or the like is performed, or heating with a heater or the like is performed to quickly cure while maintaining a high aspect. A partition wall 111 can be formed. Further, the viscosity is increased by increasing the solid components of the coating liquid itself containing the solid electrolyte material (the shear rate is 1 s ⁻¹ (1 / second) to about 20 Pa · s (pascal second) to about 2000 Pa · s). An electrolyte partition wall 111 having an aspect ratio may be formed.

After the formation of the solid electrolyte electrolyte partition 111, a negative electrode active material layer 122 is formed by applying a coating liquid containing a negative electrode active material on the surface of the negative electrode current collector 121 in the negative electrode region 12 (step S4). Examples of the coating liquid containing a negative electrode active material include lithium titanate (Li ₄ Ti ₅ O ₁₂ ) as a negative electrode active material, acetylene black or ketjen black as a conductive additive, and polyvinylidene fluoride as a binder. (PVDF), styrene butadiene rubber (SBR), polyvinyl pyrrolidone (PVP), polyvinyl alcohol (PVA) or polytetrafluoroethylene (PTFE), a mixture of N-methyl-2-pyrrolidone (NMP) as a solvent, etc. Can be used. The viscosity of the coating solution is preferably about 1 mPa · s to 100 Pa · s at a shear rate of 1 s ⁻¹ , for example. As the negative electrode active material, it is possible to use, for example, graphite, metallic lithium, SnO ₂ , an alloy system, etc. in addition to the above lithium titanate.

  Various known coating methods can be applied as the coating method of the coating liquid containing the negative electrode active material. For example, the same nozzle dispensing method as that of the coating liquid containing the solid electrolyte material described above can be used. Further, an ink jet method or a screen printing method may be used. In the manufacturing method of the present embodiment, since the electrolyte partition 111 formed in advance prevents the coating liquid from flowing out, by using a low-viscosity coating liquid, the entire negative electrode region 12 can be efficiently and efficiently activated in the short time. A coating solution containing a substance can be distributed.

  FIG. 9 is a perspective view of a stage where the negative electrode active material layer 122 is formed on the surface of the negative electrode current collector 121 in the negative electrode region 12. FIG. 10 is a cross-sectional view showing a cut surface of the laminate of FIG. A negative electrode active material layer 122 is laminated on the surface of a negative electrode current collector 121 that covers the negative electrode region 12. The height position of the upper surface of the negative electrode active material layer 122 should not exceed the upper surface of the electrolyte partition wall 111 and is preferably slightly lower. That is, it is preferable to apply the coating liquid containing the negative electrode active material so that the sum of the thickness of the negative electrode current collector 121 and the thickness of the negative electrode active material layer 122 is slightly smaller than the height EH of the electrolyte partition wall 111.

  By doing so, the negative electrode active material layer 122 can be brought into contact with almost the entire side wall surface on one side of the electrolyte partition wall 111, and the battery capacity per unit area of the base material 10 is increased to increase the lithium ion secondary battery 1. The energy density can be increased. Note that when the coating liquid containing the negative electrode active material is applied to such an extent that the height position of the upper surface of the negative electrode active material layer 122 exceeds the upper surface of the electrolyte partition wall 111, the negative electrode active material and the positive electrode active material come into contact with each other to cause a short circuit. There is a fear.

Similarly, after forming the electrolyte partition wall 111 of the solid electrolyte, a coating liquid containing a positive electrode active material is applied to the surface of the positive electrode current collector 131 in the positive electrode region 13 to form the positive electrode active material layer 132 (step S5). . Examples of the coating liquid containing the positive electrode active material include lithium cobaltate (LiCoO ₂ ) as the positive electrode active material, acetylene black as the conductive additive, polyvinylidene fluoride (PVDF) as the binder, and N as the solvent. A mixture of methyl-2-pyrrolidone (NMP) and the like can be used. In this embodiment, lithium hexafluorophosphate (LiPF ₆ ) used as a supporting salt for the electrolyte partition 111 of the solid electrolyte has a property of reacting with water and decomposing. Therefore, if water is contained as a solvent for the coating solution containing the positive electrode and the negative electrode active material that are in direct contact with the electrolyte partition 111, the water in the solvent and lithium hexafluorophosphate may react and decompose. For this reason, as a solvent of the coating liquid containing the active material of positive and negative electrodes, what does not contain water is preferable, and NMP which is an organic solvent is used in this embodiment, for example. As the positive electrode active material, in addition to LiCoO ₂ , LiNiO ₂ or LiFePO ₄ , LiMnPO ₄ , LiMn ₂ O ₄ , and LiMeO ₂ (Me = MxMyMz; Me and M are transition metals, x + y + z = 1) are representative. For example, LiNi _1/3 Mn _1/3 Co _1/3 O ₂ or LiNi _0.8 Co _0.15 Al _0.05 O ₂ can be used. The viscosity of the coating liquid containing the positive electrode active material is preferably about 1 mPa · s to 100 Pa · s at a shear rate of 1 s ⁻¹ , for example, as in the case of the negative electrode active material coating liquid.

  Various known coating methods can be applied as a coating method of the coating liquid containing the positive electrode active material. For example, the above-described nozzle dispensing method, inkjet method, screen printing method, or the like can be used. In the manufacturing method of the present embodiment, since the electrolyte partition 111 formed in advance prevents the coating liquid from flowing out, by using a low-viscosity coating liquid, the entire positive electrode region 13 can be efficiently activated in a short time. A coating solution containing a substance can be distributed. Note that the order of the formation of the negative electrode active material layer 122 in step S4 and the formation of the positive electrode active material layer 132 in step S5 may be reversed.

  FIG. 11 is a perspective view of a stage where the positive electrode active material layer 132 is formed on the surface of the positive electrode current collector 131. 12 is a cross-sectional view showing a cut surface of the laminate shown in FIG. A positive electrode active material layer 132 is laminated on the surface of the positive electrode current collector 131 that covers the positive electrode region 13. As a result, the negative electrode active material layer 122 and the positive electrode active material layer 132 are alternately arranged along the surface of the substrate 10 with the electrolyte partition wall 111 interposed therebetween.

  As with the negative electrode active material layer 122, the height position of the upper surface of the positive electrode active material layer 132 should not exceed the upper surface of the electrolyte partition wall 111 and is preferably slightly lower to prevent a short circuit. That is, it is preferable to apply the coating liquid containing the negative electrode active material so that the sum of the thickness of the positive electrode current collector 131 and the thickness of the positive electrode active material layer 132 is slightly smaller than the height EH of the electrolyte partition wall 111. More preferably, the upper surface height position of the positive electrode active material layer 132 and the upper surface height position of the negative electrode active material layer 122 are approximately the same.

  By doing so, the positive electrode active material layer 132 can be brought into contact with almost the entire side wall surface on the other side of the electrolyte partition wall 111, and the contact area between the solid electrolyte and the positive electrode active material can be increased. The reaction efficiency of the lithium ion secondary battery 1 can be increased by increasing the contact area between both the negative electrode active material and the positive electrode active material and the solid electrolyte.

  And the coating liquid containing a solid electrolyte material is apply | coated so that the negative electrode active material layer 122 and the positive electrode active material layer 132 which were formed in this way may be covered, and the protective layer 14 which protects the surface of an active material layer is formed (step) S6). The coating liquid for forming the protective layer 14 may be the same as that for forming the electrolyte partition 111 described above, but a coating having a lower viscosity is preferable for the purpose of forming a thin and uniform film. As a coating method for forming the protective layer 14, a nozzle dispensing method, an inkjet method, screen printing, or the like can be used. Further, the protective layer 14 may be formed by spin coating after masking the negative electrode tab 123 and the positive electrode tab 133. The lithium ion secondary battery 1 shown in FIGS. 1 and 2 is the one after the protective layer 14 is formed.

<3. Advantages of Manufacturing Method of Present Embodiment>
In the manufacturing method of the lithium ion secondary battery 1 of the present embodiment, the gap between the negative electrode current collector 121 and the positive electrode current collector 131 provided so as to face each other on the surface of the insulating base material 10. A coating solution containing a solid electrolyte material is applied to a certain electrolyte region 11 using a nozzle dispensing method, and an electrolyte partition wall 111 of a solid electrolyte is formed in the electrolyte region 11 on the surface of the substrate 10. And since the negative electrode active material layer 122 and the positive electrode active material layer 132 are formed after forming the electrolyte partition 111 first, it is possible to reliably prevent short circuit between them. In particular, even if the electrolyte partition 111 is made thin and high to improve battery characteristics, the electrolyte partition 111 that functions as a partition wall is formed prior to the formation of the negative electrode active material layer 122 and the positive electrode active material layer 132. A short circuit between the positive electrode and the negative electrode can be reliably prevented.

  This indicates that the charge / discharge characteristics and high energy density can be obtained by increasing the aspect ratio of the electrolyte partition wall 111. That is, by forming the electrolyte partition 111 in advance, it is possible to reliably prevent the positive and negative electrodes from being short-circuited. Therefore, the height EH of the electrolyte partition 111 can be made twice or more the width EW. As a result, the charge and discharge characteristics are improved by the thin electrolyte partition 111, and the energy density can be increased by increasing the battery capacity per unit area of the substrate 10, and the battery characteristics of the lithium ion secondary battery 1 can be improved. It can be excellent.

  In order to increase the aspect ratio of the electrolyte partition 111, it is preferable to add a thermosetting agent or a photocuring agent to the coating solution of the solid electrolyte material. By applying such a coating solution to the electrolyte region 11 and quickly curing it by light irradiation or heating, it is possible to easily form the electrolyte partition wall 111 having a high aspect ratio while preventing dripping after coating.

  Further, a coating solution containing a solid electrolyte material is applied to the electrolyte region 11 using a nozzle dispensing method to form an electrolyte partition 111, and then a negative electrode active material layer 122 and a positive electrode active material layer 132 are formed by a coating method. Therefore, the lithium ion secondary battery 1 can be manufactured with high productivity with a small number of steps.

  Further, in the present embodiment, the negative electrode current collector 121 and the positive electrode current collector 131 are formed in a comb-like pattern in which the negative electrode current collector 121 and the positive electrode current collector 131 are arranged to face each other at a predetermined interval using a photolithography method. . For this reason, the contact area of the negative electrode active material layer 122 and the positive electrode active material layer 132 per unit area on the surface of the base material 10 and the electrolyte partition 111 can be increased, and the reaction efficiency of the lithium ion secondary battery 1 is improved. be able to. In particular, since the negative electrode current collector 121 and the positive electrode current collector 131 are formed on the surface of the insulating base material 10 by a photolithography method, their adhesion is good, and the negative electrode current collector 121 and the positive electrode current collector 131 are good. The problem that the electric body 131 is peeled off from the base material 10 is less likely to occur. Further, when the areas of the teeth of the comb-like pattern are increased when the negative electrode current collector 121 and the positive electrode current collector 131 are formed, the negative electrode active material layer 122 and the positive electrode active material layer 132 formed thereafter are formed. Thus, the lithium ion secondary battery 1 can be a high capacity battery.

  In the present embodiment, the negative electrode current collector 121 and the positive electrode current collector 131 are elements that are formed before the electrolyte partition wall 111 of the solid electrolyte. However, if a photolithography method is used, the negative electrode current collector 121 is formed with very high positional accuracy. A comb-like pattern of the electric body 121 and the positive electrode current collector 131 can be formed. For this reason, even if the electrolyte partition 111 as a partition wall does not exist, contact (short circuit) between the negative electrode current collector 121 and the positive electrode current collector 131 can be reliably prevented.

  Further, since the coating liquid is applied to the electrolyte region 11 by using the nozzle dispensing method in which the discharge nozzle 40 that discharges the coating liquid containing the solid electrolyte material is moved relative to the surface of the base material 10, the opposing negative electrode The electrolyte partition wall 111 can be formed by applying a coating solution containing a solid electrolyte material accurately and with high throughput to the electrolyte region 11 which is a gap between the current collector 121 and the positive electrode current collector 131. In particular, since the plurality of discharge ports 44 are collectively moved relative to each other while the coating liquid containing the solid electrolyte material is continuously discharged from the plurality of discharge ports 44 arranged in the discharge nozzle 40, this embodiment is performed. For the electrolyte regions 11 parallel to each other as in the form, the time required for the coating process can be remarkably shortened.

<4. Application examples of lithium-ion batteries>
The lithium ion secondary battery 1 manufactured by the manufacturing method of the present embodiment is thin and has excellent battery characteristics. The lithium ion secondary battery 1 is an all-solid battery that does not contain an organic solvent, is easy to handle, and has a small size and excellent performance. Such a lithium ion secondary battery 1 includes, for example, electric vehicles (including hybrid electric vehicles), electric assist bicycles, electric tools, robots, and other machines, personal computers (including notebook computers), mobile phones and mobile phones. Type music players, mobile devices such as digital cameras and video cameras, RF-ID (Radio Frequency Identification) tags including non-contact IC cards, game machines, portable measuring devices, communication devices, toys, etc. It can be used for various electronic devices.

  Below, although the example of the apparatus which mounts the lithium ion secondary battery 1 which concerns on this invention is demonstrated, these are some examples of the apparatus which can apply the lithium ion secondary battery 1 of this embodiment. The application range of the lithium ion secondary battery 1 according to the present invention is not limited to these.

  FIG. 13 is a diagram schematically showing a vehicle, specifically an electric vehicle, as an example of a device equipped with the lithium ion secondary battery 1 according to the present invention. The electric vehicle 70 includes a wheel 71, a motor 72 that drives the wheel 71, and a battery 73 that supplies power to the motor 72. As the battery 73, a battery in which a plurality of lithium ion secondary batteries 1 of the above embodiment are connected in series and in parallel can be mounted on the electric vehicle 70. Since the lithium ion secondary battery 1 of this embodiment has a high energy density and good charge / discharge characteristics, it can obtain a high output even in a small size and can be charged in a short time. It is suitable as a power source for driving a vehicle such as 70.

  FIG. 14 is a diagram schematically showing an electronic device, specifically, an RF-ID tag as another example of a device on which the lithium ion secondary battery 1 according to the present invention is mounted. The RF-ID tag 80 serves as a power source for the pair of housings 81 and 82 that form a card-type package by being overlaid on each other, the circuit module 83 housed in the housing, and the circuit module 83. A battery 84 is provided. The circuit module 83 includes a loop-shaped antenna 831 for communication with the outside, and a circuit unit 832 including an integrated circuit (IC) that performs data exchange with the external device via the antenna 831 and various arithmetic / storage processes. And. As the battery 84, a battery including one set or a plurality of sets of the lithium ion secondary battery 1 of the present embodiment can be used, and the circuit unit 832 operates using the battery 84 as a power source.

  According to such a configuration, a communicable distance with an external device can be extended and more complicated processing can be performed as compared with a tag that itself does not have a power supply (so-called passive tag). It becomes possible. The lithium ion secondary battery 1 according to the present invention has a structure in which the negative electrode structures 120 and the positive electrode structures 130 are alternately arranged along the surface of the base material 10 with the electrolyte partition walls 111 interposed therebetween. Even if the number of constituents of the negative electrode structure 120 and the positive electrode structure 130 is increased, the thin structure can be easily realized. Further, as described above, the lithium ion secondary battery 1 is also excellent in battery characteristics. Therefore, it is also suitable as a power source for a card-type RF-ID tag.

  Even in devices other than the electric vehicle 70 and the RF-ID tag 80, for example, the lithium ion secondary battery 1 according to the present invention is mounted on an electronic device such as a laptop computer, and a circuit unit (CPU, liquid crystal) of the laptop computer is mounted. A circuit included in a display, a hard disk, or the like) may be operated using the lithium ion secondary battery 1 as a power source.

<5. Modification>
While the embodiments of the present invention have been described above, the present invention can be modified in various ways other than those described above without departing from the spirit of the present invention. For example, in the above embodiment, the negative electrode current collector 121 and the positive electrode current collector 131 are formed in a comb-like pattern having straight teeth, but the shape of the comb teeth is limited to a straight line. It may not be a thing but other shapes may be sufficient. For example, as shown in FIG. 15, the teeth of the comb-like pattern may have a curved shape. Also in the pattern example shown in the figure, the negative electrode current collector 121 and the positive electrode current collector 131 are formed in a comb-like pattern that is opposed to each other so as to mesh with each other at a predetermined interval in plan view. That is, the “comb-tooth shape” is a shape having a plurality of teeth, and both the electrode current collector 121 and the cathode current collector 131 are formed in a comb-teeth shape having a plurality of teeth, and one tooth is The arrangement is such that it enters between the other adjacent teeth. However, the tooth shape of the comb-like pattern in the example shown in FIG. 15 is a sine curve.

  The negative electrode current collector 121 and the positive electrode current collector 131 having such a comb-like pattern may be formed by photolithography as in the above embodiment. The gap between the curved comb teeth of both the negative electrode current collector 121 and the positive electrode current collector 131 becomes the electrolyte region 11, and the coating liquid containing the solid electrolyte material in a sinusoidal shape along the electrolyte region 11 by a nozzle dispensing method. Is applied. Even in the pattern shown in FIG. 15, since the electrolyte region 11 has a sinusoidal shape parallel to each other, the discharge nozzle 40 is sine while continuously discharging the coating liquid containing the solid electrolyte material from the plurality of discharge ports 44. By performing relative movement so as to draw a locus of a curve, it is possible to apply the plurality of electrolyte regions 11 at once. By drying and curing the coating solution, a solid electrolyte electrolyte partition 111 is formed in a sinusoidal shape between the negative electrode current collector 121 and the positive electrode current collector 131. The negative electrode current collector 121 and the positive electrode current collector 131 in contact with the electrolyte partition wall 111 become the negative electrode region 12 and the positive electrode region 13, respectively. Thereafter, as in the above embodiment, a negative electrode active material layer 122 is formed by applying a coating liquid containing a negative electrode active material to the surface of the negative electrode current collector 121 in the negative electrode region 12, and the positive electrode current collector in the positive electrode region 13. A positive electrode active material layer 132 is formed by applying a coating liquid containing a positive electrode active material to the surface of 131. Even in this case, as in the above embodiment, since the negative electrode active material layer 122 and the positive electrode active material layer 132 are formed after the electrolyte partition wall 111 is formed first, the short circuit between the positive and negative electrodes can be reliably prevented. A battery having excellent battery characteristics can be produced with high productivity.

  Further, the sinusoidal pattern shown in FIG. 15 may be a zigzag polygonal line pattern. That is, the tooth shape of the comb-like pattern may be a zigzag polygonal line shape. Even in this case, since the electrolyte region 11 has a polygonal line shape parallel to each other, the discharge nozzle 40 has a polygonal line locus while continuously discharging the coating liquid containing the solid electrolyte material from the plurality of discharge ports 44. By performing relative movement as depicted, it is possible to apply to a plurality of electrolyte regions 11 at once.

  Further, the electrolyte region 11 that is the gap between the comb teeth of the negative electrode current collector 121 and the positive electrode current collector 131 is not limited to being parallel to each other. For example, as shown in FIG. May not be parallel to each other. However, in this case, the coating solution containing the solid electrolyte material is applied to the electrolyte region 11 by moving the nozzle having a single discharge port relative to the surface of the substrate 10. Specifically, while continuously discharging the coating liquid containing the solid electrolyte material from a single discharge port, the nozzle is moved relative to the base material 10, so that the electrolyte regions 11 are not parallel to each other. The electrolyte partition 111 is formed by applying a coating solution containing a solid electrolyte material. At this time, a plurality of nozzles each having a single discharge port may be individually moved relative to each other, or one nozzle having a single discharge port may be relatively moved repeatedly. Also in the example shown in FIG. 16, the negative electrode current collector 121 and the positive electrode current collector 131 that are in contact with the electrolyte partition wall 111 become the negative electrode region 12 and the positive electrode region 13, respectively.

  Then, after the electrolyte partition 111 is formed, a negative electrode active material layer 122 is formed by applying a coating liquid containing a negative electrode active material to the surface of the negative electrode current collector 121 in the negative electrode region 12, and the positive electrode current collector in the positive electrode region 13. A positive electrode active material layer 132 is formed by applying a coating liquid containing a positive electrode active material to the surface of the electric body 131. Even in this case, since the negative electrode active material layer 122 and the positive electrode active material layer 132 are formed after the electrolyte partition wall 111 is formed first, the positive and negative electrodes are reliably prevented from being short-circuited, and the battery characteristics are excellent. The battery can be manufactured with high productivity. However, as in the above-described embodiment, higher productivity is obtained when the discharge nozzle 40 having the plurality of discharge ports 44 is relatively moved so that the coating liquid is applied to the plurality of electrolyte regions 11 at once. be able to.

  You may make it apply | coat the coating liquid containing a solid electrolyte material from the nozzle which has a single discharge outlet with respect to the mutually parallel electrolyte area | region 11 as shown in FIG. In the case of a nozzle having a single discharge port, a coating liquid containing a solid electrolyte material is applied to the entire gap between the negative electrode current collector 121 and the positive electrode current collector 131 to form the electrolyte partition wall 111. Also good. The negative electrode region 12 that functions as the negative electrode (that is, the region in which the negative electrode active material layer 122 is formed) can be any region of the negative electrode current collector 121 that is in contact with the electrolyte partition wall 111. Similarly, the positive electrode region 13 that functions as the positive electrode (that is, the region in which the positive electrode active material layer 132 is formed) can be any region of the positive electrode current collector 131 that is in contact with the electrolyte partition wall 111.

  The shapes of the negative electrode current collector 121 and the positive electrode current collector 131 are not necessarily limited to having a comb-like pattern. Even if it does not have a comb-like pattern, the negative electrode current collector 121 and the positive electrode current collector 131 are provided so as to face the surface of the substrate 10, and the electrolyte region 11 in the gap includes a solid electrolyte material. If the coating liquid is applied, a battery structure can be realized. However, from the viewpoint of increasing the battery reaction efficiency per unit area of the substrate 10, it is preferable to pattern the negative electrode current collector 121 and the positive electrode current collector 131 in a comb-teeth shape so as to face each other.

  In the above embodiment, the electrolyte partition 111 is formed by applying the coating solution containing the solid electrolyte material to the electrolyte region 11 using the nozzle dispensing method. However, the electrolyte partition 111 of the solid electrolyte is formed by other methods. 111 may be formed. For example, the electrolyte partition 111 may be formed by an inkjet method or a screen printing method. However, when these methods are adopted, in order to increase the height EH of the electrolyte partition wall 111, a plurality of times of overcoating are required. Therefore, the nozzle dispensing method can quickly increase the aspect ratio. The electrolyte partition wall 111 can be formed.

  In the above embodiment, the protective layer 14 is formed as the final step. However, the formation of the protective layer 14 is not an essential requirement for realizing a structure that functions as a battery, and is omitted. You may do it.

  In the above embodiment, the negative electrode current collector 121 is formed of copper and the positive electrode current collector 131 is formed of aluminum. However, other metal materials may be used, and further, the negative electrode current collector may be used. The body 121 and the positive electrode current collector 131 may be formed of the same metal material (for example, gold). If the positive and negative current collectors 121 and 131 are formed of the same metal material, the negative electrode current collector 121 and the positive electrode current collector 131 can be formed simultaneously by photolithography.

  The materials such as the current collector, the active material, and the electrolyte exemplified in the above embodiment are only examples, and are not limited thereto, and may be used as a constituent material of a lithium ion secondary battery. Even in the case of manufacturing a lithium ion secondary battery using this material, the manufacturing method according to the present invention can be preferably applied. Moreover, you may make it apply the manufacturing method based on this invention not only to a lithium ion secondary battery but to manufacture of other types of chemical batteries, such as a lithium ion primary battery and an alkaline battery.

  INDUSTRIAL APPLICABILITY The present invention can be suitably applied to an all-solid battery manufacturing technology using a solid electrolyte such as a polymer electrolyte as an electrolyte, and is particularly suitable for manufacturing a thin battery having excellent battery characteristics with high productivity. ing.

DESCRIPTION OF SYMBOLS 1 Lithium ion secondary battery 2 Application | coating unit 10 Base material 11 Electrolyte area | region 12 Negative electrode area | region 13 Positive electrode area | region 14 Protective layer 20 Stage moving mechanism 30 Stage 40 Discharge nozzle 44 Discharge port 70 Electric vehicle 80 RF-ID tag 111 Electrolyte partition 120 Negative electrode structure Body 121 Negative electrode current collector 122 Negative electrode active material layer 130 Positive electrode structure 131 Positive electrode current collector 132 Positive electrode active material layer 832 Circuit portion

Claims (12)

A coating solution containing a solid electrolyte material is applied to the electrolyte region between the negative electrode current collector and the positive electrode current collector provided to face the surface of the insulating base material, and the surface of the base material An electrolyte partition wall forming step of forming an electrolyte partition wall in the electrolyte region;
After the electrolyte partition wall forming step, a negative electrode active material layer forming step of forming a negative electrode active material layer by applying a coating liquid containing a negative electrode active material on the surface of the negative electrode current collector,
A positive electrode active material layer forming step of forming a positive electrode active material layer by applying a coating liquid containing a positive electrode active material on the surface of the positive electrode current collector after the electrolyte partition wall forming step;
A method for producing a battery, comprising: In the manufacturing method of the battery of Claim 1,
The method of manufacturing a battery, wherein the negative electrode current collector and the positive electrode current collector are patterned in a comb-teeth shape so as to face each other at a predetermined interval in a plan view. In the manufacturing method of the battery of Claim 2,
The method for manufacturing a battery, wherein the height of the electrolyte partition is at least twice the width. In the manufacturing method of the battery of Claim 3,
In the electrolyte partition wall forming step, a coating solution to which a thermosetting agent or a photocuring agent is added is applied to the electrolyte region. In the manufacturing method of the battery in any one of Claims 1-4,
The method for manufacturing a battery, wherein the negative electrode current collector and the positive electrode current collector are formed by a photolithography method. In the manufacturing method of the battery in any one of Claims 1-5,
In the electrolyte partition wall forming step, a nozzle for discharging a coating liquid containing a solid electrolyte material is moved relative to the surface of the substrate to apply the coating liquid to the electrolyte region. . In the manufacturing method of the battery according to claim 6,
In the electrolyte partition wall forming step, the nozzle is relatively moved with respect to the surface of the substrate while discharging a coating liquid containing a solid electrolyte material from a plurality of discharge ports arranged in a row on the nozzle. Battery manufacturing method. In the manufacturing method of the battery in any one of Claims 1-7,
The manufacturing method of the battery characterized by further providing the protective layer formation process which forms the protective layer which covers the said negative electrode active material layer and the said positive electrode active material layer continuously.   The battery manufactured by the manufacturing method of the battery in any one of Claims 1-8.   A vehicle comprising the battery according to claim 9.   An RF-ID tag comprising the battery according to claim 9. A battery according to claim 9;
A circuit unit that operates using the battery as a power source;
An electronic device comprising:

Images