WO2013031938A1 - Secondary battery - Google Patents

Secondary battery Download PDF

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Publication number
WO2013031938A1
WO2013031938A1 PCT/JP2012/072128 JP2012072128W WO2013031938A1 WO 2013031938 A1 WO2013031938 A1 WO 2013031938A1 JP 2012072128 W JP2012072128 W JP 2012072128W WO 2013031938 A1 WO2013031938 A1 WO 2013031938A1
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WO
WIPO (PCT)
Prior art keywords
positive electrode
outer peripheral
electrode
secondary battery
negative electrode
Prior art date
Application number
PCT/JP2012/072128
Other languages
French (fr)
Japanese (ja)
Inventor
孝夫 大道寺
Original Assignee
Ｎｅｃエナジーデバイス株式会社
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Filing date
Publication date
Application filed by Ｎｅｃエナジーデバイス株式会社 filed Critical Ｎｅｃエナジーデバイス株式会社
Publication of WO2013031938A1 publication Critical patent/WO2013031938A1/en

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H01M4/0402—Methods of deposition of the material
    • H01M4/0404—Methods of deposition of the material by coating on electrode collectors
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • the present invention relates to a stacked secondary battery in which a battery element in which a positive electrode and a negative electrode are stacked via a separator is sealed with an exterior material.
  • a stacked secondary battery such as a lithium ion battery in which a positive electrode and a negative electrode are stacked with a separator interposed therebetween increases the area of the positive electrode and the negative electrode or increases the number of stacked positive and negative electrodes per unit cell. Therefore, it is suitable for a battery having a large charge / discharge capacity.
  • the positive electrode is coated with a slurry for a positive electrode in which a particulate positive electrode active material, a conductive material, a binder, etc. are mixed on the surface of a strip-shaped aluminum foil of a current collector. It is manufactured by cutting it.
  • apply negative electrode slurry in which particulate negative electrode active material, conductive material, binder, etc.
  • the corner portion of the cut electrode It is possible to use a cutting tool that pushes with a cutting blade such that becomes a quadrant.
  • the electrode by blanking by punching with a cutting tool that has a cutting blade that matches the electrode shape, but this is not applicable to large shapes that cannot be punched at once. Therefore, there is a problem that it is not industrially suitable, such as the need for a cutting blade. Therefore, the width direction and the length direction of the electrode are cut separately, and after cutting one of the width direction or the length direction by an arbitrary method, the corner of the electrode is cut when the other is pushed off. A cutting tool having a cutting blade that is a quadrant is used. However, in this case, when the edge of the cutting blade does not match the side of the electrode that has been cut in advance, the positive electrode cutting body 106 cut from the positive electrode substrate as shown in FIG.
  • the negative electrode has a larger area than the positive electrode. Things are needed. For this reason, those that are not cut into a predetermined shape, or that have a chamfered portion that does not coincide with the outer peripheral line of the positive electrode or the negative electrode and have a stepped portion, etc., can not be used for manufacturing a lithium ion battery. There wasn't.
  • the present invention has a high production yield rate even when a slight positioning error or the like occurs between the positive electrode base material or negative electrode base material and the cutting tool during the manufacture of the laminated secondary battery. It is an object of the present invention to provide a stable stacked secondary battery.
  • This invention solves the said subject, Comprising: The 1st chamfering part by which at least one place of the intersection of two adjacent sides of the outer periphery of the positive electrode electrical power collector with which the positive electrode active material was apply
  • a separator is provided between the negative electrode and at least a part of an outer peripheral line of the first or second chamfered portion has a curved portion and two outer peripheral connection portions connected to the curved portion, and the curved portion And at least one of the angles formed by the tangent line at the intersection of the outer peripheral connection part and the line of the outer peripheral connection part.
  • the tangent means a straight line.
  • the obtuse angle is 120 ° or more and less than 180 °. More preferably, the secondary battery has an obtuse angle of 135 ° or more and less than 180 °.
  • the present invention is a stacked secondary battery in which the positive electrode and the negative electrode have a positive electrode collector tab, a positive electrode extraction tab formed integrally with the negative electrode collector, and a negative electrode extraction tab, respectively.
  • the present invention is the above secondary battery in which the curved portion is an arc.
  • This invention is the said secondary battery which is a lithium ion secondary battery.
  • the present invention is the above-described stacked secondary battery in which the positive electrode and the negative electrode have a rectangular outer shape.
  • the two outer peripheral connection portions connected to the end portion of the curved portion, and the intersection of the curved portion and the outer peripheral connection portion are all projected by projecting the positive electrode onto a plane parallel to the positive electrode current collector. It means what is represented on the plane figure formed on the figure.
  • the angle formed between the tangent line and the line of the outer peripheral connection portion is the tangent line of the portion where the two tangent lines intersect at two intersections of the curved portion and the outer peripheral connection portion and the line of the outer peripheral connection portion. It means the angle to make.
  • the chamfered portion having a specific shape is formed at the corner of at least one of the positive electrode and the negative electrode.
  • a chamfered portion having a desired shape is formed even when a mutual misalignment or the like occurs when cutting with a cutting tool, so that a secondary battery with improved productivity and stable quality can be provided.
  • the chamfered portion of the present invention is formed at least on the positive electrode or the negative electrode located closest to the battery container, the electrode and the container are pierced through the insulating film disposed between the battery container and the like. The possibility of short-circuiting can be reduced, and a lithium ion battery excellent in productivity can be provided.
  • the negative electrode current collector When applied to a lithium ion battery, in order to prevent generation of lithium dendrites on the negative electrode current collector, the negative electrode current collector must be disposed on the negative electrode current collector facing the surface on which the positive electrode active material is formed. Therefore, the positive electrode tends to have a smaller outer dimension than the negative electrode. That is, the area of the positive electrode is one of the factors that govern the size of the battery capacity. Therefore, if the chamfered portion of the present invention is formed at least on the positive electrode, it is possible to obtain an effect of increasing the battery capacity by the amount of the electrode active material to be removed.
  • FIG. 1 is a diagram illustrating a manufacturing process of a positive electrode and a negative electrode.
  • FIG. 2 is a diagram for explaining an embodiment of the laminated secondary battery of the present invention.
  • 2A is a front view
  • FIG. 2B is a cross-sectional view taken along the line A-A ′ in FIG. 1A and showing an enlarged view of the stacking direction.
  • FIG. 3 is a plan view illustrating the chamfered portion of the positive electrode according to one embodiment of the present invention.
  • FIG. 3A is a plan view illustrating a positive electrode having a chamfered portion.
  • FIG. 3B is an enlarged view of the chamfered portion.
  • FIG. 4 is a view for explaining an example of a cutting tool used for forming the chamfered portion of the present invention and the conventional one.
  • FIG. 4A is a diagram for explaining an example of a conventional cutting tool
  • FIG. 4B is a diagram for explaining an example of a cutting tool used for manufacturing the positive electrode of the present invention.
  • FIG. 5 is a diagram for explaining another embodiment of the present invention.
  • FIG. 6 is a diagram for explaining the positive electrode in which the positioning of the positive electrode base material and the cutting tool has shifted.
  • FIG. 1 is a diagram illustrating a manufacturing process of a positive electrode and a negative electrode. Since the positive electrode and the negative electrode are produced by the same method except for the constituent materials, the positive electrode is described in the following description.
  • the positive electrode base material is a positive electrode base material in which a slurry-like positive electrode mixture is intermittently applied to both surfaces on a positive electrode current collector made of a strip-shaped aluminum foil, dried and then compressed by a roller press or the like to be molded. It is produced by cutting to a predetermined size.
  • lithium-containing composite oxides such as lithium manganese composite oxide and lithium cobalt composite oxide, conductive materials such as carbon black, binders such as polyvinylidene fluoride, and the like are used.
  • a slurry dispersed in 2-pyrrolidone can be used.
  • a positive electrode active material layer 103 is intermittently formed on the positive electrode base material 102 at a portion shown by a shaded portion.
  • the positive electrode active material layer is formed by intermittently forming the positive electrode active material layer 103 in an area larger than the positive electrode part outline 104 indicating the size of the positive electrode to be manufactured. Yes.
  • both side surface portions 105a and 105b in the length direction of the strip-like positive electrode base material 102 are cut along a predetermined positive electrode outer shape line.
  • the positive electrode active material layer 103 applied intermittently in the length direction is cut along a first cutting line 110 formed of a curved portion at a straight portion and both ends.
  • the positive electrode extraction tab forming part 113 is cut integrally with the second cutting line 112 for taking out the positive electrode extraction tab, and the positive electrode cut body 106 is produced. Since the positive electrode active material application part 114 remains at the tip of the positive electrode extraction tab formation part 113, the positive electrode active material application part 114 is cut to form the positive electrode extraction tab 115 as shown in FIG. 1D.
  • the electrode 100 is completed.
  • the positive electrode 100 has a chamfered portion 150 whose corners are chamfered in a curved shape.
  • FIGS. 1A to 1D the example in which the positive electrode extraction tab is located on one side of the center line in the width direction has been described. However, the center line may coincide with the center line of the positive electrode extraction tab.
  • the negative electrode comprises a strip-shaped copper foil on a negative electrode current collector, a carbon material that absorbs and releases lithium ions, a conductive material such as carbon black, a binder such as polyvinylidene fluoride, and the like. Disperse in pyrrolidone to form a slurry, and apply this slurry-like negative electrode mixture on both sides of the negative electrode current collector intermittently, and after drying, compress it with a roller press or the like to perform molding.
  • a negative electrode can be produced in the same manner as the positive electrode by manufacturing the material and cutting it into a predetermined size.
  • FIG. 2 is a diagram for explaining an embodiment of the laminated secondary battery of the present invention.
  • 2A is a front view
  • FIG. 2B is a cross-sectional view taken along the line AA ′ in FIG. 2A and showing an enlarged view of the stacking direction.
  • the stacked secondary battery 1 forms a stacked body 400 in which a positive electrode 100 and a negative electrode 200 are stacked via a separator 300, and a positive electrode extraction tab 115 and a negative electrode extraction tab 215 are provided in the same direction from the stacked body 400. It has been taken out.
  • the positive electrode extraction tab 115 and the negative electrode extraction tab 215 connected to the negative electrode 200 are taken out from the sealing portion 510 of the film-shaped packaging material 500.
  • the film-like exterior material a material having strength and heat resistance such as nylon or polyethylene terephthalate is used on the outer surface side of the aluminum foil, and a material having good heat fusion such as polypropylene or polyethylene is used on the inner surface side.
  • a material having strength and heat resistance such as nylon or polyethylene terephthalate is used on the outer surface side of the aluminum foil, and a material having good heat fusion such as polypropylene or polyethylene is used on the inner surface side.
  • Each layer can be used.
  • the exterior material of the stacked secondary battery is not limited to the film-like exterior material as described above, and a metal exterior container or the like may be used.
  • FIG. 3 is a plan view for explaining a chamfered portion of the positive electrode.
  • FIG. 3A is a plan view illustrating a positive electrode having a chamfered portion.
  • FIG. 3B is an enlarged view of the chamfered portion.
  • a chamfered portion 150 in which at least one corner of an intersection of adjacent peripheral lines of the projection portion on the surface parallel to the positive electrode current collector, that is, a corner portion is chamfered in a curved shape.
  • the curved portion 152 of the chamfered portion 150 has a shape different from the quadrant 151 shown by a broken line in FIG. 3A, and both end portions are connected to the two outer peripheral connection portions 153 and 154.
  • All the chamfers of the outer peripheral portion of the positive electrode including the corners 159 and 160 formed by the tangents 157 and 158 and the outer peripheral connection portions 153 and 154 at the intersections 155 and 156 of the curved portion 152 and the outer peripheral connection portions 153 and 154. It is characterized in that at least one or more of the angles formed by the tangent at the part and the outer peripheral connection part is an obtuse angle. In the present invention, the angle formed between the tangent at the intersection of the curved portion and the outer peripheral connection portion and the line of the outer peripheral connection portion is the two tangent lines extending in both directions at the two intersections of the curved portion and the outer peripheral connection portion.
  • the angle formed by the tangent line on the side that intersects each other from the intersection and the line of the outer peripheral connection portion means the angle on the side where the electrode exists, that is, the inner angle side in the case of a polygon. If the outer peripheral connection portion is a straight line, the tangent here means the direction of the straight line itself.
  • the positive electrode is caused by a slight deviation between the end of the quadrant and the outer peripheral connection portion.
  • step difference is produced in a cut part can be prevented.
  • the chamfered portion is formed with a connecting portion between the tangent at the intersection of the curved portion and the outer peripheral connecting portion and the curved portion where the angle formed by the line of the outer peripheral connecting portion is an obtuse angle.
  • the positive electrode has been described, but the negative electrode can also be manufactured in the same manner as the positive electrode.
  • the battery electrode of the present invention has a larger outer shape than the chamfered portion indicated by the quadrant 151, and therefore the battery electrode is more battery-operated than the case where the chamfered portion formed by the quadrant is formed. The effect that the effective area of an electrode becomes large and battery capacity becomes large can also be acquired.
  • the positive electrode extraction tab formation part 113 and the negative electrode extraction tab formation part 115 used as the unformed part of an active material are moved to the one side of the width direction of strip
  • the same chamfered portion can be formed even by a method in which the active material is continuously formed from the electrode and punched into a predetermined shape.
  • the outer peripheral lines of at least some of the corners of the positive electrode and the negative electrode have a curved shape as described above. It is more preferable to use the same shape when chamfering the corner.
  • FIG. 4 is a view for explaining an example of a cutting tool used for forming the chamfered portion of the present invention and the conventional one.
  • a cutting tool 600 shown in FIG. 4A is a diagram for explaining an example of a conventional cutting tool, and is a diagram showing a cross section cut along a plane parallel to the current collector surface at the time of cutting.
  • the cutting tool 600 includes a cutting blade 601.
  • the cutting blade 601 has a flat surface portion 602 and curved surface portions 603a and 603b connected to the flat surface portion 602.
  • the length between both ends of the cutting blade 601 is the same as the width of the positive electrode width PW cut from the positive electrode base material, and the cross section formed in the curved surface portions 603a and 603b is a quadrant-shaped cutting blade.
  • the end portion can be cut to coincide with the end face of the positive electrode base material, and a quadrant connected to the outer peripheral portion can be formed.
  • a quadrant is formed in the chamfered portion when the end of the cutting tool coincides with the end surface of the positive electrode base material.
  • the end portion of the cutting blade does not coincide with the end surface of the positive electrode base material, there is a problem that a part of the cutting blade is not cut or a curved chamfer is not performed.
  • a cutting tool 610 shown in FIG. 4B is a view for explaining an example of a cutting tool used for manufacturing the positive electrode of the present invention, and is a view showing a cross section cut along a plane parallel to the current collector surface at the time of cutting. is there.
  • the cutting tool 610 used for manufacturing the positive electrode of the present invention includes a cutting blade 611, and the cutting blade 611 has a flat surface portion 612 and curved surface portions 613a and 613b connected thereto.
  • the length of the flat portion of the cutting blade 611 is shorter than the width of the positive electrode width PW produced from the positive electrode base material, and the length of the curved surface portions 613a and 613b is compared with the conventional quadrant provided at both ends. Long.
  • the length between the both ends of the width direction of the positive electrode base material of a cutting tool is characterized by being longer than the length of the positive electrode width PW produced from a positive electrode base material.
  • the length between both ends in the width direction of the positive electrode base material of the cutting blade 611 is slightly longer than the positive electrode width PW.
  • the length is preferably 1 to 1.06 times considering the tolerance of each member.
  • the curved surface shape of the cutting blade can be an arc shape that is easy to manufacture, but any curved line, such as an elliptical arc, can be used as long as the linear distance from the end of the flat surface to the tip of the curved surface increases.
  • the curved shape can be used.
  • Example 1 Lithium manganate (LiMn 2 O 4 ), carbon black, and polyvinylidene fluoride were blended and dispersed in N-methyl-2-pyrrolidone to prepare a positive electrode mixture.
  • the obtained positive electrode mixture was applied to both surfaces of an aluminum foil having a thickness of 20 ⁇ m, dried, and then subjected to compression molding with a roller press machine to obtain positive electrodes having a positive electrode layer having a thickness of 80 ⁇ m on both surfaces.
  • the prepared positive electrode is attached to a cutting device, and at least a part of the chamfered portion has a curved portion and at least one outer peripheral connection portion connected to the curved portion, and the curved portion and the outer peripheral connection portion Cutting was performed by changing the angle formed between the tangent line at the intersection and the line of the outer peripheral connection portion. The same tendency was observed when cutting at two or more locations to obtain the desired shape, or when cutting only one location to obtain the desired shape. The results are shown below. Evaluation at each cutting point was performed according to the following evaluation criteria. Active material drop-off rate: When the current collector of the active material application part was exposed by visual observation, it was regarded as defective.
  • Burr generation rate Visual confirmation with a magnifying glass was performed, and those having a burr size of 60 ⁇ m or more were regarded as defective.
  • Punching defect rate If a step difference in punching deviation was confirmed by visual inspection, it was determined as defective.
  • FIG. 5 is a diagram for explaining another embodiment of the present invention.
  • FIG. 5A is a plan view for explaining the positive electrode
  • FIG. 5B is an enlarged view for explaining the chamfered portion.
  • the positive electrode 100 has a chamfered portion 150 in which at least one corner of an intersection of adjacent outer sides of the projection portion on the surface parallel to the positive electrode current collector, that is, a corner portion is chamfered in a curved shape.
  • the curved portion 152 of the chamfered portion 150 is connected to the two outer peripheral connection portions 153 and 154 at both ends.
  • At least one of the angles 159 and 160 formed by the tangents 157 and 158 at the intersections 155 and 156 between the curved portion 152 and the outer peripheral connection portions 153 and 154 and the outer peripheral connection portions 153 and 154 is an obtuse angle. It is said. Further, the outer peripheral connection portions 153 and 154 are inclined so that the outer peripheral connection portions 153 and 154 form an acute angle from the outer peripheral lines 165 and 167 of the positive electrode toward the curved surface portion 150. As a result, each corner portion forms a curved outer peripheral line formed by the curved surface and the outer peripheral connection portion, so that the effect of preventing the active material from falling off can be enhanced.
  • the chamfered portion is chamfered at the time of chamfering at least some of the corners in the insertion direction of the positive electrode and the negative electrode on the bag separator or the battery outer container.
  • the battery element is packaged with a film-like packaging material.
  • a battery can be produced by storing the battery in a metal battery can and sealing the electrolyte solution after injection.
  • the laminated secondary battery of the present invention has chamfered portions formed from curved surfaces of a specific shape at the corners of the positive electrode and the negative electrode, the positive electrode base material, the negative electrode base material to the positive electrode, Even when a positional shift occurs when the negative electrode is manufactured by cutting, a stacked secondary battery in which the positive electrode active material and the negative electrode active material are not dropped from the corners can be provided.
  • DESCRIPTION OF SYMBOLS 100 ... Positive electrode, 102 ... Positive electrode base material, 103 ... Positive electrode active material layer, 104 ... Positive electrode part outline, 105a, 105b ... Both side part, 106 ... Positive electrode 110 ... first cutting line, 112 ... second cutting line, 113 ... positive electrode extraction tab forming part, 114 ... positive electrode active material application part, 115 ... positive electrode extraction tab, 150 ... chamfered portion, 165, 167 ... positive electrode outer peripheral line, 200 ... negative electrode, 300 ... separator, 400 ... laminate, 115 ...

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Secondary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

This stacked secondary battery in which a positive-electrode active material layer and a negative-electrode active material layer are prevented from falling off from the corners comprises: a positive electrode having a first beveled part formed by beveling at least one of intersection points each formed between two adjacent sides of outer peripheral lines of a projection of a positive-electrode charge collector, which is coated with a positive-electrode active material, onto a plane parallel to the positive-electrode charge collector; a negative electrode having a second beveled part formed by beveling at least one of intersection points each formed between two adjacent sides of outer peripheral lines of a projection of a negative-electrode charge collector, which is coated with a negative-electrode active material, onto a plane parallel to the negative-electrode charge collector; and a separator between the positive electrode and the negative electrode. At least a portion of the first or the second beveled part has a curvilinear part and two outer peripheral connection parts connected to the curvilinear part. At least one angle formed between a tangential line at the intersection point between the curvilinear part and the outer peripheral connection part and a line along said outer peripheral connection part is an obtuse angle.

Description

二次電池Secondary battery
　本発明は、正極電極と負極電極とをセパレータを介して積層した電池要素を外装材で封口した積層型二次電池に関する。 The present invention relates to a stacked secondary battery in which a battery element in which a positive electrode and a negative electrode are stacked via a separator is sealed with an exterior material.
　正極電極と負極電極とをセパレータを介して積層したリチウムイオン電池等の積層型二次電池は、正極、負極の面積を大きくしたり、積層する正極、負極の枚数を増加することによって単位電池当たりの容量を大きくすることが容易であるので、充放電容量が大きな電池として好適である。
　リチウムイオン電池では、正極電極は、集電体の帯状のアルミニウム箔面に、粒子状の正極活物質、導電性材料、結着剤等を混合した正極用スラリーを塗布、乾燥後，所定の大きさに切断することによって製造されている。負極電極も同様に、集電体の帯状の銅箔面に、粒子状の負極活物質、導電性材料、結着剤等を混合した負極用スラリーを塗布、乾燥後、所定の大きさに切断して製造されている。
　正極電極、負極電極の角部が直角になるように切断されていると、角部が角形電池容器に接触し、正極及び負極活物質が脱落したり、電極が折れ曲がったりする不都合が生じ、このため電池の内部ショートによる不良率が増加し、生産性の低いものとなってしまう。この問題点を解決するために、正極電極、負極電極のそれぞれの少なくとも角形電池容器への挿入側のコーナー部を円弧形状とすることが提案されている（特許文献１参照）。 A stacked secondary battery such as a lithium ion battery in which a positive electrode and a negative electrode are stacked with a separator interposed therebetween increases the area of the positive electrode and the negative electrode or increases the number of stacked positive and negative electrodes per unit cell. Therefore, it is suitable for a battery having a large charge / discharge capacity.
In a lithium ion battery, the positive electrode is coated with a slurry for a positive electrode in which a particulate positive electrode active material, a conductive material, a binder, etc. are mixed on the surface of a strip-shaped aluminum foil of a current collector. It is manufactured by cutting it. Similarly, apply negative electrode slurry in which particulate negative electrode active material, conductive material, binder, etc. are mixed on the surface of the strip-shaped copper foil of the current collector, and then cut to a predetermined size. Manufactured.
If the corners of the positive electrode and the negative electrode are cut so that they are at right angles, the corners may come into contact with the rectangular battery container, causing the inconvenience that the positive electrode and the negative electrode active material may fall off or the electrode may be bent. Therefore, the defect rate due to the internal short circuit of the battery increases, resulting in low productivity. In order to solve this problem, it has been proposed that at least the corners on the insertion side of each of the positive electrode and the negative electrode into the rectangular battery container have an arc shape (see Patent Document 1).
　電極の角部を円弧状に加工するためには、帯状の部材にスラリーを塗布して形成した正極電極基材、負極電極基材を所定の寸法に切断する場合、切断された電極の角部が４分円になるような切断刃で押し切る切断工具を使用することができる。 In order to process the corner of the electrode into an arc shape, when the positive electrode base material formed by applying slurry to the band-shaped member and the negative electrode base material are cut into predetermined dimensions, the corner portion of the cut electrode It is possible to use a cutting tool that pushes with a cutting blade such that becomes a quadrant.
特開平９－８２３６１号公報Japanese Patent Laid-Open No. 9-82361
　電極形状に合致した切断刃が閉じた切断工具によって打ち抜くブランキングによって電極を製造することも可能であるが、１度に打ちぬけない大きな形状には適用できないことはもちろん、電極形状が大きくなると大型の切断刃が必要となるなど、工業的には適さないという問題がある。そこで、電極の幅方向と長さ方向とは別々に切断することになり、幅方向または長さ方向のいずれか一方を任意の方法で切断したのち、他方を押し切りする際に電極の角部が４分円になるような切断刃をもった切断工具を用いることになる。しかしこの場合、切断刃の端部と、あらかじめ切断された電極の辺とが一致しない場合には、図６に示すように正極電極基材から切断された正極電極用切断体１０６には、面取部の端部が正極電極基材１０２の外周部と一致しないために、所定の切断ができなくなる。その結果、切断残渣部１１８を生じる等の問題が起きるために、電池には使用することができるものが得られないことがあった。 It is possible to manufacture the electrode by blanking by punching with a cutting tool that has a cutting blade that matches the electrode shape, but this is not applicable to large shapes that cannot be punched at once. Therefore, there is a problem that it is not industrially suitable, such as the need for a cutting blade. Therefore, the width direction and the length direction of the electrode are cut separately, and after cutting one of the width direction or the length direction by an arbitrary method, the corner of the electrode is cut when the other is pushed off. A cutting tool having a cutting blade that is a quadrant is used. However, in this case, when the edge of the cutting blade does not match the side of the electrode that has been cut in advance, the positive electrode cutting body 106 cut from the positive electrode substrate as shown in FIG. Since the end portion of the take-up portion does not coincide with the outer peripheral portion of the positive electrode base material 102, predetermined cutting cannot be performed. As a result, problems such as the generation of the cutting residue portion 118 occur, so that there are cases where a battery that can be used cannot be obtained.
　特にリチウムイオン電池の場合には、セパレータを介して対向する正極電極の対向面には負極電極が必ず存在するように配置することが不可欠であるために、負極電極は正極電極よりも面積が大きなものが必要である。このため、所定の形状に切断されていないものや、面取部が正極電極あるいは負極電極の外周線と一致せずに段差部等を生じたものはリチウムイオン電池の製造に利用することはできなかった。
　本発明は、積層型二次電池の製造時に、正極電極基材あるいは負極電極基材と、切断工具との間に多少の位置決め誤差等が生じた場合であっても製造歩留まり率が高く、特性が安定した積層型二次電池を提供することを課題とするものである。 In particular, in the case of a lithium ion battery, it is indispensable to dispose the negative electrode on the opposite surface of the positive electrode facing each other with the separator interposed therebetween. Therefore, the negative electrode has a larger area than the positive electrode. Things are needed. For this reason, those that are not cut into a predetermined shape, or that have a chamfered portion that does not coincide with the outer peripheral line of the positive electrode or the negative electrode and have a stepped portion, etc., can not be used for manufacturing a lithium ion battery. There wasn't.
The present invention has a high production yield rate even when a slight positioning error or the like occurs between the positive electrode base material or negative electrode base material and the cutting tool during the manufacture of the laminated secondary battery. It is an object of the present invention to provide a stable stacked secondary battery.
　発明者が鋭意検討した結果、電極の角部は必ずしも全体が完全に曲線になっていなくとも、所定の形状にすることで電極の脱落や折れを防ぐことが可能であることを見出した。
　本発明は、上記課題を解決するものであって、正極活物質が塗布された正極集電体の外周線の隣り合う２辺の交点の少なくとも一箇所が面取りされた第一の面取部を有する正極電極と、負極活物質が塗布された負極集電体の外周線の隣り合う２辺の交点の少なくとも一箇所が面取りされた第二の面取部を有する負極電極と、前記正極電極と前記負極電極との間にセパレータを備え、前記第一または第二の面取部の外周線の少なくとも一部が曲線部と前記曲線部に接続する二つの外周接続部を有し、前記曲線部と前記外周接続部との交点における接線と前記外周接続部の線とのなす角の少なくとも１つ以上が鈍角である積層型二次電池である。
　ここで、前記外周接続部が直線の場合には、前記接線とは直線を意味する。 As a result of intensive studies by the inventors, it has been found that the electrode corners can be prevented from falling off or breaking even if the corners of the electrode are not necessarily completely curved.
This invention solves the said subject, Comprising: The 1st chamfering part by which at least one place of the intersection of two adjacent sides of the outer periphery of the positive electrode electrical power collector with which the positive electrode active material was apply | coated was chamfered is provided. A negative electrode having a second chamfered portion where at least one of the intersections of two adjacent sides of the outer peripheral line of the negative electrode current collector coated with the negative electrode active material is chamfered, and the positive electrode A separator is provided between the negative electrode and at least a part of an outer peripheral line of the first or second chamfered portion has a curved portion and two outer peripheral connection portions connected to the curved portion, and the curved portion And at least one of the angles formed by the tangent line at the intersection of the outer peripheral connection part and the line of the outer peripheral connection part.
Here, when the outer peripheral connection portion is a straight line, the tangent means a straight line.
　前記鈍角が、１２０°以上１８０°未満である二次電池である。
　さらに好ましくは、前記鈍角が１３５°以上１８０°未満である二次電池である。
　本発明は、前記正極電極、前記負極電極は、それぞれ前記正極集電体、前記負極集電体と一体に形成された正極引出タブ、負極引出タブを有する積層型二次電池である。
　本発明は、前記曲線部が円弧である前記の二次電池である。
　本発明は、リチウムイオン二次電池である前記の二次電池である。
　本発明は、前記正極電極、前記負極電極の外形が矩形状である前記の積層型の二次電池である。 In the secondary battery, the obtuse angle is 120 ° or more and less than 180 °.
More preferably, the secondary battery has an obtuse angle of 135 ° or more and less than 180 °.
The present invention is a stacked secondary battery in which the positive electrode and the negative electrode have a positive electrode collector tab, a positive electrode extraction tab formed integrally with the negative electrode collector, and a negative electrode extraction tab, respectively.
The present invention is the above secondary battery in which the curved portion is an arc.
This invention is the said secondary battery which is a lithium ion secondary battery.
The present invention is the above-described stacked secondary battery in which the positive electrode and the negative electrode have a rectangular outer shape.
　本発明において、前記曲線部の端部に接続する二つの外周接続部、前記曲線部と前記外周接続部との交点とは、いずれも正極電極を正極集電体に平行な面に投影した投影図上に形成される平面図形上で表されるものを意味する。
　また、前記接線と前記外周接続部の線とのなす角度とは、前記曲線部と前記外周接続部との二つの交点における二つの接線が交わる方向の部分の接線と外周接続部の線とのなす角度を意味する。 In the present invention, the two outer peripheral connection portions connected to the end portion of the curved portion, and the intersection of the curved portion and the outer peripheral connection portion are all projected by projecting the positive electrode onto a plane parallel to the positive electrode current collector. It means what is represented on the plane figure formed on the figure.
Further, the angle formed between the tangent line and the line of the outer peripheral connection portion is the tangent line of the portion where the two tangent lines intersect at two intersections of the curved portion and the outer peripheral connection portion and the line of the outer peripheral connection portion. It means the angle to make.
　本発明に係る積層型二次電池によれば、正極電極、負極電極の少なくとも一方の電極の角部には特定の形状を有する面取り部を形成したので、正極電極基材、負極電極基材から切断工具によって切断する際に、相互の位置ずれ等が生じても、所望の形状の面取部が形成されるので、生産性が向上し、品質が安定した二次電池を提供することができる。
　ここで、少なくとも最も電池容器の近くに位置する正極電極または負極電極に本発明の面取部を形成しておけば、電池容器と間とに配置される絶縁膜等を突き破って電極と容器とがショートする可能性を低減することができ、生産性にも優れたリチウムイオン電池を提供することができる。
　リチウムイオン電池に適用する場合、負極集電体上にリチウムのデンドライトが発生しないようにするために、正極電極活物質が形成された面と対向する負極集電体上には、必ず負極活物質が形成されるように配置されるので、相対的に正極電極は負極電極よりも外形寸法が小さくなる傾向がある。すなわち、正極電極の面積は電池容量の大きさを支配する要素の一つになっている。そこで本発明の面取部を少なくとも正極電極に形成すれば、取り除かれる電極活物質の量が少ない分だけ電池容量を増加させる効果を得ることもできる。 According to the multilayer secondary battery according to the present invention, the chamfered portion having a specific shape is formed at the corner of at least one of the positive electrode and the negative electrode. A chamfered portion having a desired shape is formed even when a mutual misalignment or the like occurs when cutting with a cutting tool, so that a secondary battery with improved productivity and stable quality can be provided. .
Here, if the chamfered portion of the present invention is formed at least on the positive electrode or the negative electrode located closest to the battery container, the electrode and the container are pierced through the insulating film disposed between the battery container and the like. The possibility of short-circuiting can be reduced, and a lithium ion battery excellent in productivity can be provided.
When applied to a lithium ion battery, in order to prevent generation of lithium dendrites on the negative electrode current collector, the negative electrode current collector must be disposed on the negative electrode current collector facing the surface on which the positive electrode active material is formed. Therefore, the positive electrode tends to have a smaller outer dimension than the negative electrode. That is, the area of the positive electrode is one of the factors that govern the size of the battery capacity. Therefore, if the chamfered portion of the present invention is formed at least on the positive electrode, it is possible to obtain an effect of increasing the battery capacity by the amount of the electrode active material to be removed.
図１は、正極電極、負極電極の製造工程を説明する図である。FIG. 1 is a diagram illustrating a manufacturing process of a positive electrode and a negative electrode. 図２は、本発明の積層型二次電池の一実施形態を説明する図である。図２Ａは、正面図を示し、図２Ｂは、図１ＡのＡ－Ａ’の位置における断面図であって積層方向を拡大した図を示す。FIG. 2 is a diagram for explaining an embodiment of the laminated secondary battery of the present invention. 2A is a front view, and FIG. 2B is a cross-sectional view taken along the line A-A ′ in FIG. 1A and showing an enlarged view of the stacking direction. 図３は、本発明の一実施態様の正極電極の面取部を説明する平面図である。図３Ａは、面取部を形成した正極電極を説明する平面図である。また、図３Ｂは面取部を拡大した図である。FIG. 3 is a plan view illustrating the chamfered portion of the positive electrode according to one embodiment of the present invention. FIG. 3A is a plan view illustrating a positive electrode having a chamfered portion. FIG. 3B is an enlarged view of the chamfered portion. 図４は、本発明および従来の面取部の形成に用いる切断工具の一例を説明する図である。図４Ａは、従来の切断工具の一例を説明する図であり、図４Ｂは、本発明の正極電極を製造するために使用する切断工具の一例を説明する図である。FIG. 4 is a view for explaining an example of a cutting tool used for forming the chamfered portion of the present invention and the conventional one. FIG. 4A is a diagram for explaining an example of a conventional cutting tool, and FIG. 4B is a diagram for explaining an example of a cutting tool used for manufacturing the positive electrode of the present invention. 図５は、本発明の他の実施態様を説明する図である。FIG. 5 is a diagram for explaining another embodiment of the present invention. 図６は、正極電極基材と切断工具との位置決めにずれが生じた正極電極を説明する図である。FIG. 6 is a diagram for explaining the positive electrode in which the positioning of the positive electrode base material and the cutting tool has shifted.
　以下に、図面を参照して本発明を説明する。
 リチウムイオン二次電池を例に挙げて本発明を説明する。
　図１は、正極電極、負極電極の製造工程を説明する図である。
　正極電極、負極電極は、その構成材料が相違するのみで同様の方法によって作製されているので、以下の説明においては正極電極について説明する。
　正極電極は、帯状のアルミニウム箔からなる正極集電体上に、スラリー状の正極合剤を間欠的に両面に塗布し、乾燥後、ローラープレス機等によって圧縮して成型を行い正極電極基材から所定の大きさに切断することによって作製する。
　正極合剤としては、リチウムマンガン複合酸化物、リチウムコバルト複合酸化物等のリチウムを含有する複合酸化物と、カーボンブラック等の導電性材料、ポリフッ化ビニリデン等の結着剤等をＮ－メチル－２－ピロリドンに分散させてスラリー状としたものを用いることができる。 The present invention will be described below with reference to the drawings.
The present invention will be described by taking a lithium ion secondary battery as an example.
FIG. 1 is a diagram illustrating a manufacturing process of a positive electrode and a negative electrode.
Since the positive electrode and the negative electrode are produced by the same method except for the constituent materials, the positive electrode is described in the following description.
The positive electrode base material is a positive electrode base material in which a slurry-like positive electrode mixture is intermittently applied to both surfaces on a positive electrode current collector made of a strip-shaped aluminum foil, dried and then compressed by a roller press or the like to be molded. It is produced by cutting to a predetermined size.
As the positive electrode mixture, lithium-containing composite oxides such as lithium manganese composite oxide and lithium cobalt composite oxide, conductive materials such as carbon black, binders such as polyvinylidene fluoride, and the like are used. A slurry dispersed in 2-pyrrolidone can be used.
　図１Ａで示すように、正極電極基材１０２には、網掛け部で示すよう部分に正極活物質層１０３が間欠的に形成されている。また、図１Ａにおいて破線で示すように正極活物質層は、製造する正極電極の外形の大きさを示す正極電極部外形線１０４よりも大きな面積で正極活物質層１０３が間欠的に形成されている。
　次に、図１Ｂに示すように、帯状の正極電極基材１０２の長さ方向の両側面部１０５ａ、１０５ｂを所定の正極電極外形線に沿って切断する。次いで、図１Ｃに示すように長さ方向に間欠的に塗布した正極活物質層１０３を、直線部と両端部に曲面状部からなる第一切断線１１０に沿って切断する。また、正極引出タブを取り出す第二切断線１１２によって正極引出タブ形成部１１３と一体に切断して正極電極用切断体１０６を作製する。
　正極引出タブ形成部１１３の先端部には正極活物質塗布部１１４が残っているので、図１Ｄに示すように、正極活物質塗布部１１４を切断して正極引出タブ１１５を形成することによって正極電極１００が完成する。正極電極１００には、その角部の外周が曲線状に面取された面取部１５０を有している。
　図１Ａ～図１Ｄでは、正極引出タブが幅方向の中心線の一方の側に位置する例について説明したが、前記中心線と正極引出タブの中心線が一致するものであっても良い。 As shown in FIG. 1A, a positive electrode active material layer 103 is intermittently formed on the positive electrode base material 102 at a portion shown by a shaded portion. In addition, as shown by a broken line in FIG. 1A, the positive electrode active material layer is formed by intermittently forming the positive electrode active material layer 103 in an area larger than the positive electrode part outline 104 indicating the size of the positive electrode to be manufactured. Yes.
Next, as shown in FIG. 1B, both side surface portions 105a and 105b in the length direction of the strip-like positive electrode base material 102 are cut along a predetermined positive electrode outer shape line. Next, as shown in FIG. 1C, the positive electrode active material layer 103 applied intermittently in the length direction is cut along a first cutting line 110 formed of a curved portion at a straight portion and both ends. Moreover, the positive electrode extraction tab forming part 113 is cut integrally with the second cutting line 112 for taking out the positive electrode extraction tab, and the positive electrode cut body 106 is produced.
Since the positive electrode active material application part 114 remains at the tip of the positive electrode extraction tab formation part 113, the positive electrode active material application part 114 is cut to form the positive electrode extraction tab 115 as shown in FIG. 1D. The electrode 100 is completed. The positive electrode 100 has a chamfered portion 150 whose corners are chamfered in a curved shape.
In FIGS. 1A to 1D, the example in which the positive electrode extraction tab is located on one side of the center line in the width direction has been described. However, the center line may coincide with the center line of the positive electrode extraction tab.
　負極電極は、帯状の銅箔を負極集電体上に、リチウムイオンを吸蔵、放出する炭素材料、カーボンブラック等の導電性材料、ポリフッ化ビニリデン等の結着剤等をＮ－メチル－２－ピロリドンに分散させてスラリー状とし、このスラリー状の負極合剤を負極集電体上に間欠的に両面に塗布し、乾燥後、ローラープレス機等によって圧縮して成型を行って、負極電極基材を製造して所定の大きさに切断することによって正極電極と同様の方法で負極電極を作製することができる。 The negative electrode comprises a strip-shaped copper foil on a negative electrode current collector, a carbon material that absorbs and releases lithium ions, a conductive material such as carbon black, a binder such as polyvinylidene fluoride, and the like. Disperse in pyrrolidone to form a slurry, and apply this slurry-like negative electrode mixture on both sides of the negative electrode current collector intermittently, and after drying, compress it with a roller press or the like to perform molding. A negative electrode can be produced in the same manner as the positive electrode by manufacturing the material and cutting it into a predetermined size.
　図２は、本発明の積層型二次電池の一実施形態を説明する図である。図２Ａは、正面図を示し、図２Ｂは、図２ＡのＡ－Ａ’の位置における断面図であって積層方向を拡大した図を示す。
　積層型二次電池１は、正極電極１００と負極電極２００がセパレータ３００を介して積層された積層体４００を形成しており、積層体４００から同一方向に正極引出タブ１１５および負極引出タブ２１５が取り出されている。フィルム状外装材５００の封口部５１０から正極引出タブ１１５と負極電極２００に接続した負極引出タブ２１５から取り出されている。また、フィルム状外装材には、アルミニウム箔の外面側にはナイロン、ポリエチレンテレフタレート等の強度および耐熱性を有する部材を、内面側には、ポリプロピレン、ポリエチレン等の熱融着製が良好な材料をそれぞれ積層したものを用いることができる。積層型二次電池の外装材には、上記したようなフィルム状外装材に限らず金属製の外装容器等を用いたものであってもよい。 FIG. 2 is a diagram for explaining an embodiment of the laminated secondary battery of the present invention. 2A is a front view, and FIG. 2B is a cross-sectional view taken along the line AA ′ in FIG. 2A and showing an enlarged view of the stacking direction.
The stacked secondary battery 1 forms a stacked body 400 in which a positive electrode 100 and a negative electrode 200 are stacked via a separator 300, and a positive electrode extraction tab 115 and a negative electrode extraction tab 215 are provided in the same direction from the stacked body 400. It has been taken out. The positive electrode extraction tab 115 and the negative electrode extraction tab 215 connected to the negative electrode 200 are taken out from the sealing portion 510 of the film-shaped packaging material 500. In addition, for the film-like exterior material, a material having strength and heat resistance such as nylon or polyethylene terephthalate is used on the outer surface side of the aluminum foil, and a material having good heat fusion such as polypropylene or polyethylene is used on the inner surface side. Each layer can be used. The exterior material of the stacked secondary battery is not limited to the film-like exterior material as described above, and a metal exterior container or the like may be used.
　次に、本発明の正極電極、負極電極の面取部について説明する。
　図３は、正極電極の面取部を説明する平面図である。図３Ａは、面取部を形成した正極電極を説明する平面図である。また、図３Ｂは面取部を拡大した図である。
　正極電極の外周部には、正極集電体に平行な面への投影部の外周線の隣り合う２辺の交点、すなわち角部の少なくとも一箇所が曲線状に面取りされた面取部１５０を有しており、前記面取部１５０の曲線部１５２は図３Ａにおいて破線で示す４分円１５１とは異なる形状を有し、両端部が二つの外周接続部１５３、１５４と接続している。 Next, the chamfered portions of the positive electrode and the negative electrode of the present invention will be described.
FIG. 3 is a plan view for explaining a chamfered portion of the positive electrode. FIG. 3A is a plan view illustrating a positive electrode having a chamfered portion. FIG. 3B is an enlarged view of the chamfered portion.
On the outer peripheral portion of the positive electrode, a chamfered portion 150 in which at least one corner of an intersection of adjacent peripheral lines of the projection portion on the surface parallel to the positive electrode current collector, that is, a corner portion is chamfered in a curved shape. The curved portion 152 of the chamfered portion 150 has a shape different from the quadrant 151 shown by a broken line in FIG. 3A, and both end portions are connected to the two outer peripheral connection portions 153 and 154.
　前記曲線部１５２と前記外周接続部１５３、１５４との交点１５５、１５６における接線１５７、１５８と前記外周接続部１５３、１５４とがなす角１５９、１６０を含む正極電極の外周部のすべての面取部での前記接線と前記外周接続部とのなす角のうちの少なくとも１つ以上が鈍角であることを特徴としている。
　　本発明において、曲線部と外周接続部との交点における接線と外周接続部の線とのなす角とは、前記曲線部と前記外周接続部との二つの交点において両方向に延びる二つの接線の前記交点から互いに交わる側に位置する側の接線と前記外周接続部の線とのなす角度で、電極が存在する側の角度、すなわち多角形でいうなら内角側を意味する。なお、外周接続部が直線であれば、ここでの接線は直線そのものの方向を意味するものとする。 All the chamfers of the outer peripheral portion of the positive electrode including the corners 159 and 160 formed by the tangents 157 and 158 and the outer peripheral connection portions 153 and 154 at the intersections 155 and 156 of the curved portion 152 and the outer peripheral connection portions 153 and 154. It is characterized in that at least one or more of the angles formed by the tangent at the part and the outer peripheral connection part is an obtuse angle.
In the present invention, the angle formed between the tangent at the intersection of the curved portion and the outer peripheral connection portion and the line of the outer peripheral connection portion is the two tangent lines extending in both directions at the two intersections of the curved portion and the outer peripheral connection portion. The angle formed by the tangent line on the side that intersects each other from the intersection and the line of the outer peripheral connection portion means the angle on the side where the electrode exists, that is, the inner angle side in the case of a polygon. If the outer peripheral connection portion is a straight line, the tangent here means the direction of the straight line itself.
　面取部を以上のような形状とすることによって、図３Ａにおいて、破線で示す４分円による面取の場合のように、４分円の端部と外周接続部とのわずかなずれによって正極電極基材から正極電極が切断されないという問題や、あるいは切断部に段差を生じるという問題の発生を防止することができる。その結果、面取部には曲線部と外周接続部との交点における接線と外周接続部の線とのなす角が鈍角である曲線部との接続部が形成されるので、角部からの正極活物質の脱落を防止した、特性が優れた積層型二次電池を提供することができる。以上の説明では正極電極について説明をしたが、負極電極についても正極電極と同様に作製することができる。
　また、本発明の電池電極は、図３Ａで説明したように、４分円１５１で示す面取部よりも外形が大きくなるので、４分円からなる面取部を形成した場合に比べて電池電極の有効面積が大きくなり、電池容量が大きくなるという効果も得ることができる。
　なお、ここでは間欠的に塗布した電極を用いて説明したが、活物質の未形成部となる正極引出タブ形成部１１３や負極引出タブ形成部１１５を帯状の箔の幅方向の一方側に寄せて連続して活物質を形成した電極から、所定の形状に打ちぬく方法であっても同様の面取り部を形成することができる。 By making the chamfered portion into the shape as described above, in FIG. 3A, as in the case of chamfering with a quadrant shown by a broken line, the positive electrode is caused by a slight deviation between the end of the quadrant and the outer peripheral connection portion. Generation | occurrence | production of the problem that a positive electrode is not cut | disconnected from an electrode base material, or the problem that a level | step difference is produced in a cut part can be prevented. As a result, the chamfered portion is formed with a connecting portion between the tangent at the intersection of the curved portion and the outer peripheral connecting portion and the curved portion where the angle formed by the line of the outer peripheral connecting portion is an obtuse angle. It is possible to provide a stacked secondary battery with excellent characteristics in which the active material is prevented from falling off. In the above description, the positive electrode has been described, but the negative electrode can also be manufactured in the same manner as the positive electrode.
In addition, as described with reference to FIG. 3A, the battery electrode of the present invention has a larger outer shape than the chamfered portion indicated by the quadrant 151, and therefore the battery electrode is more battery-operated than the case where the chamfered portion formed by the quadrant is formed. The effect that the effective area of an electrode becomes large and battery capacity becomes large can also be acquired.
In addition, although it demonstrated using the electrode apply | coated intermittently here, the positive electrode extraction tab formation part 113 and the negative electrode extraction tab formation part 115 used as the unformed part of an active material are moved to the one side of the width direction of strip | belt-shaped foil. The same chamfered portion can be formed even by a method in which the active material is continuously formed from the electrode and punched into a predetermined shape.
　また、本発明の積層型二次電池においては、正極電極、負極電極の角部の少なくとも一部の角部の外周線を上記のような曲線状となるようにすることが好ましいが、すべての角部の面取加工時に同様の形状とすることがより好ましい。 In the multilayer secondary battery of the present invention, it is preferable that the outer peripheral lines of at least some of the corners of the positive electrode and the negative electrode have a curved shape as described above. It is more preferable to use the same shape when chamfering the corner.
　本発明の積層型二次電池の正極電極、負極電極の面取部の形成方法の一例について説明する。
　図４は、本発明および従来の面取部の形成に用いる切断工具の一例を説明する図である。　図４Ａに示す切断工具６００は、従来の切断工具の一例を説明する図であり、切断時の集電体面に平行な面で切断した断面を示す図である。
　切断工具６００は、切断刃６０１を備えており、切断刃６０１には平面部６０２とそれに接続する曲面部６０３ａ、６０３ｂを有している。
　切断刃６０１の両端部間の長さは、正極電極基材から切断する正極電極幅ＰＷの幅と同じであって、曲面部６０３ａ、６０３ｂに形成された断面が４分円状の切断刃の端部を正極電極基材の端面に一致させて切断し、外周部に接続した４分円を形成することができる。　このような切断刃を有する切断工具を用いた場合には、切断工具の端部が正極電極基材の端面に一致している場合には面取部には４分円が形成される。しかしながら、切断刃の端部が正極電極基材の端面に一致しない場合には一部が切断されなかったり、曲面状の面取が行われないという問題が生じていた。 An example of a method for forming the chamfered portions of the positive electrode and the negative electrode of the multilayer secondary battery of the present invention will be described.
FIG. 4 is a view for explaining an example of a cutting tool used for forming the chamfered portion of the present invention and the conventional one. A cutting tool 600 shown in FIG. 4A is a diagram for explaining an example of a conventional cutting tool, and is a diagram showing a cross section cut along a plane parallel to the current collector surface at the time of cutting.
The cutting tool 600 includes a cutting blade 601. The cutting blade 601 has a flat surface portion 602 and curved surface portions 603a and 603b connected to the flat surface portion 602.
The length between both ends of the cutting blade 601 is the same as the width of the positive electrode width PW cut from the positive electrode base material, and the cross section formed in the curved surface portions 603a and 603b is a quadrant-shaped cutting blade. The end portion can be cut to coincide with the end face of the positive electrode base material, and a quadrant connected to the outer peripheral portion can be formed. When a cutting tool having such a cutting blade is used, a quadrant is formed in the chamfered portion when the end of the cutting tool coincides with the end surface of the positive electrode base material. However, when the end portion of the cutting blade does not coincide with the end surface of the positive electrode base material, there is a problem that a part of the cutting blade is not cut or a curved chamfer is not performed.
　図４Ｂに示す切断工具６１０は、本発明の正極電極を製造するために使用する切断工具の一例を説明する図であり、切断時の集電体面に平行な面で切断した断面を示す図である。
　本発明の正極電極の製造に使用する切断工具６１０は、切断刃６１１を備えており、切断刃６１１には平面部６１２とそれに接続する曲面部６１３ａ、６１３ｂを有している。
　切断刃６１１の平面部の長さは、正極電極基材から作製する正極電極幅ＰＷの幅よりも短く、曲面部６１３ａ、６１３ｂの長さは、従来の両端部に設けた４分円に比べて長い。また、切断工具の正極電極基材の幅方向の両端部間の長さは、正極電極基材から作製する正極電極幅ＰＷの長さよりも長いことを特徴としている。 A cutting tool 610 shown in FIG. 4B is a view for explaining an example of a cutting tool used for manufacturing the positive electrode of the present invention, and is a view showing a cross section cut along a plane parallel to the current collector surface at the time of cutting. is there.
The cutting tool 610 used for manufacturing the positive electrode of the present invention includes a cutting blade 611, and the cutting blade 611 has a flat surface portion 612 and curved surface portions 613a and 613b connected thereto.
The length of the flat portion of the cutting blade 611 is shorter than the width of the positive electrode width PW produced from the positive electrode base material, and the length of the curved surface portions 613a and 613b is compared with the conventional quadrant provided at both ends. Long. Moreover, the length between the both ends of the width direction of the positive electrode base material of a cutting tool is characterized by being longer than the length of the positive electrode width PW produced from a positive electrode base material.
　例えば、切断刃６１１の正極電極基材の幅方向の両端部間の長さは、正極電極幅ＰＷに比べてわずかに長くすることが好ましい。具体的には、各部材の公差を考慮して１～１．０６倍の長さとすることが好ましい。
　切断工具の切断刃の長さを正極電極このような長さとすることによって、切断工程において正極電極基材と切断工具との間に位置ずれが生じた場合であっても電極の面取部に曲面部を形成することができる。
　以上の説明では、正極電極基材の正極引出タブを取り出していない側を切断する工具について述べたが、正極引出タブを取り出す側を切断する側の切断工具には、正極引出タブ形成部を切断可能な切断工具を用いることができる。 For example, it is preferable that the length between both ends in the width direction of the positive electrode base material of the cutting blade 611 is slightly longer than the positive electrode width PW. Specifically, the length is preferably 1 to 1.06 times considering the tolerance of each member.
By setting the length of the cutting blade of the cutting tool to such a length as the positive electrode, even in the case where a positional deviation occurs between the positive electrode base material and the cutting tool in the cutting process, the chamfered portion of the electrode A curved surface portion can be formed.
In the above description, the tool that cuts the side of the positive electrode base material from which the positive electrode extraction tab is not taken out has been described. However, the cutting tool that cuts the side from which the positive electrode extraction tab is taken out is cut into the positive electrode extraction tab forming portion. Possible cutting tools can be used.
　切断刃の曲面部形状は、製作加工が容易な円弧形状とすることができるが、平面部の端部から曲面の先端部までの直線距離が増加する曲線であれば，楕円弧をはじめとする任意の曲面形状のものを使用することができる。 The curved surface shape of the cutting blade can be an arc shape that is easy to manufacture, but any curved line, such as an elliptical arc, can be used as long as the linear distance from the end of the flat surface to the tip of the curved surface increases. The curved shape can be used.
　実施例１
　リチウムマンガン酸（ＬｉＭｎ2Ｏ4）、カーボンブラック、ポリフッ化ビニリデンを配合して、Ｎ－メチル－２－ピロリドンに分散してさせて正極合剤を調製した。
　得られた正極合剤を厚さ２０μｍのアルミニウム箔の両面に塗布し、乾燥後、ローラープレス機で圧縮成型を行なって、両面にそれぞれ８０μｍ厚さの正極電極層を有する正極電極を得た。 Example 1
Lithium manganate (LiMn 2 O 4 ), carbon black, and polyvinylidene fluoride were blended and dispersed in N-methyl-2-pyrrolidone to prepare a positive electrode mixture.
The obtained positive electrode mixture was applied to both surfaces of an aluminum foil having a thickness of 20 μm, dried, and then subjected to compression molding with a roller press machine to obtain positive electrodes having a positive electrode layer having a thickness of 80 μm on both surfaces.
　作製した正極電極を切断装置に取り付けて、面取部の少なくとも一部が曲線部と前記曲線部に接続する少なくとも一つ以上の外周接続部を有し、前記曲線部と前記外周接続部との交点における接線と前記外周接続部の線とのなす角を変えて切断を行った。
　二個所以上の切断を行って所望の形状とした場合も、一個所のみの切断によって所望の形状とした場合も同様の傾向が見られたので、１個所の切断を行った場合について評価を行い、その結果を以下に示す。　
　各切断個所における評価は、以下の評価基準によって行った。
　活物質脱落率：目視により活物質塗布部の集電体が露出している場合は不良とした。
　バリ発生率：拡大鏡による目視で確認を行い、バリ寸法が６０μｍ以上のものとを不良とした。　打ち抜き加工不良率：目視により打ち抜きズレの段差が確認された場合は不良とした。
これらの結果を表１に示す。 The prepared positive electrode is attached to a cutting device, and at least a part of the chamfered portion has a curved portion and at least one outer peripheral connection portion connected to the curved portion, and the curved portion and the outer peripheral connection portion Cutting was performed by changing the angle formed between the tangent line at the intersection and the line of the outer peripheral connection portion.
The same tendency was observed when cutting at two or more locations to obtain the desired shape, or when cutting only one location to obtain the desired shape. The results are shown below.
Evaluation at each cutting point was performed according to the following evaluation criteria.
Active material drop-off rate: When the current collector of the active material application part was exposed by visual observation, it was regarded as defective.
Burr generation rate: Visual confirmation with a magnifying glass was performed, and those having a burr size of 60 μm or more were regarded as defective. Punching defect rate: If a step difference in punching deviation was confirmed by visual inspection, it was determined as defective.
These results are shown in Table 1.
表１
鈍角　　　活物質剥離率(％) バリ発生率(％)　打ち抜き加工不良率(％)　
４分円で切断　　　　６　　　　　　１１　　　　　　 １０
１０５°　　　　　　３　　　　　　　１　　　　　　　 ０
１２０°　　　　　　１　　　　　　　０　　　　　　　 ０
１３５°　　　　　　０　　　　　　　０　　　　　　　 ０
１５０°　　　　　　０　　　　　　　０　　　　　　　 ０
１６５°　　　　　　０　　　　　　　０　　　　　　　 ０
１８０°　　　　　　０　　　　　　　０　　　　　　　 ０ Table 1
Obtuse angle Active material peeling rate (%) Burr generation rate (%) Punching defect rate (%)
Cut into quarter circles 6 11 10
105 ° 3 1 0
120 ° 1 0 0
135 ° 0 0 0
150 ° 0 0 0
165 ° 0 0 0
180 ° 0 0 0
　図５は、本発明の他の実施態様を説明する図である。
　図５Ａは、正極電極を説明する平面図であり、図５Ｂは、面取部を拡大して説明する図である。
　正極電極１００は、正極集電体に平行な面への投影部の外周線の隣り合う２辺の交点、すなわち角部の少なくとも一箇所が曲線状に面取りされた面取部１５０を有しており、前記面取部１５０の曲線部１５２は両端部が二つの外周接続部１５３、１５４と接続している。
　前記曲線部１５２と前記外周接続部１５３、１５４との交点１５５、１５６における接線１５７、１５８と前記外周接続部１５３、１５４とのなす角１５９、１６０の少なくとも１つ以上が鈍角であることを特徴としている。
　また、外周接続部１５３、１５４は、正極電極の外周線１６５、１６７から曲面部１５０に向けて外周接続部１５３、１５４が鋭角をなすように傾斜している。その結果、それぞれの角部は曲面と外周接続部によって形成される曲線状外周線を形成するので、活物質の脱落の防止効果を高めることができる。 FIG. 5 is a diagram for explaining another embodiment of the present invention.
FIG. 5A is a plan view for explaining the positive electrode, and FIG. 5B is an enlarged view for explaining the chamfered portion.
The positive electrode 100 has a chamfered portion 150 in which at least one corner of an intersection of adjacent outer sides of the projection portion on the surface parallel to the positive electrode current collector, that is, a corner portion is chamfered in a curved shape. The curved portion 152 of the chamfered portion 150 is connected to the two outer peripheral connection portions 153 and 154 at both ends.
At least one of the angles 159 and 160 formed by the tangents 157 and 158 at the intersections 155 and 156 between the curved portion 152 and the outer peripheral connection portions 153 and 154 and the outer peripheral connection portions 153 and 154 is an obtuse angle. It is said.
Further, the outer peripheral connection portions 153 and 154 are inclined so that the outer peripheral connection portions 153 and 154 form an acute angle from the outer peripheral lines 165 and 167 of the positive electrode toward the curved surface portion 150. As a result, each corner portion forms a curved outer peripheral line formed by the curved surface and the outer peripheral connection portion, so that the effect of preventing the active material from falling off can be enhanced.
　このような形状とすることによって、図２Ａにおいて破線で示す４分円によって面取する場合に、４分円の端部と外周接続部とのずれによって切断されなかったり、あるいは段差を生じるという問題の発生を防止することができる。その結果、面取部には所望の曲面を形成することができるので、角部からの正極活物質の脱落を防止した特性が優れたリチウムイオン二次電池を提供することができる。 By adopting such a shape, when chamfering with a quadrant shown by a broken line in FIG. 2A, there is a problem that the cut is not caused by the deviation between the end of the quadrant and the outer peripheral connection portion, or a step is generated. Can be prevented. As a result, since a desired curved surface can be formed in the chamfered portion, it is possible to provide a lithium ion secondary battery having excellent characteristics in which the positive electrode active material is prevented from falling off from the corner portion.
　また、本発明の積層型二次電池においては、正極電極、負極電極を袋上セパレータ、あるいは電池外装容器に挿入方向の角部の少なくとも一部の角部の面取加工時において面取部を本発明のようなとすることが好ましいが、すべての角部の面取加工時に本発明のような曲面形状に加工することがより好ましい。 Further, in the laminated secondary battery of the present invention, the chamfered portion is chamfered at the time of chamfering at least some of the corners in the insertion direction of the positive electrode and the negative electrode on the bag separator or the battery outer container. Although it is preferable to be as in the present invention, it is more preferable to process into a curved surface shape as in the present invention when chamfering all corners.
　以上の様にして作製した正極電極、負極電極をセパレータを介して積層して、充放電電流を取り出す各電極の引出タブを接合した電池要素を作製したの後、フィルム状外装材によって外装したり、金属製の電池缶に収納し、電解液を注入の後に封口することによって電池を作製することができる。 After the positive electrode and the negative electrode prepared as described above are laminated via a separator to produce a battery element in which the extraction tab of each electrode for taking out the charge / discharge current is joined, the battery element is packaged with a film-like packaging material. A battery can be produced by storing the battery in a metal battery can and sealing the electrolyte solution after injection.
　本発明の積層型二次電池は、正極電極、負極電極の角部に、特定の形状の曲面から形成された面取部を設けたので、正極電極基材、負極電極基材から正極電極、負極電極を切断によって製造する際に位置ずれが生じた場合であっても、角部からの正極活物質、負極活物質の脱落がない積層型二次電池を提供することができる。 Since the laminated secondary battery of the present invention has chamfered portions formed from curved surfaces of a specific shape at the corners of the positive electrode and the negative electrode, the positive electrode base material, the negative electrode base material to the positive electrode, Even when a positional shift occurs when the negative electrode is manufactured by cutting, a stacked secondary battery in which the positive electrode active material and the negative electrode active material are not dropped from the corners can be provided.
　１００・・・正極電極、１０２・・・正極電極基材、１０３・・・正極活物質層、１０４・・・正極電極部外形線、１０５ａ，１０５ｂ・・・両側面部、１０６・・・正極電極用切断体、１１０・・・第一切断線、１１２・・・第二切断線、１１３・・・正極引出タブ形成部、１１４・・・正極活物質塗布部、１１５・・・正極引出タブ、１５０・・・面取部、１６５，１６７・・・正極電極の外周線、２００・・・負極電極、３００・・・セパレータ、４００・・・積層体、１１５・・・正極引出タブ、１１８・・・切断残渣部、２１５・・・負極引出タブ、５００・・・フィルム状外装材、５１０・・・封口部、１５１・・・４分円、１５２・・・曲線部、１５３，１５４・・・外周接続部、１５５，１５６・・・交点、１５７，１５８・・・接線、１５９、１６０・・・接線と前記外周接続部とがなす角、６００・・・切断工具、６０１・・・切断刃、６０２・・・平面部、６０３ａ，６０３ｂ・・・曲面部、６１０・・・切断工具、６１１・・・切断刃、６１２・・・平面部、６１３ａ，６１３ｂ・・・曲面部、ＰＷ・・・正極電極幅 DESCRIPTION OF SYMBOLS 100 ... Positive electrode, 102 ... Positive electrode base material, 103 ... Positive electrode active material layer, 104 ... Positive electrode part outline, 105a, 105b ... Both side part, 106 ... Positive electrode 110 ... first cutting line, 112 ... second cutting line, 113 ... positive electrode extraction tab forming part, 114 ... positive electrode active material application part, 115 ... positive electrode extraction tab, 150 ... chamfered portion, 165, 167 ... positive electrode outer peripheral line, 200 ... negative electrode, 300 ... separator, 400 ... laminate, 115 ... positive electrode extraction tab, 118 ··· Cutting residue portion, 215 ··· Negative electrode extraction tab, ····························································································································· -Outer peripheral connection part, 155, 156 ... intersection, 157, 15 ... Tangential line, 159, 160 ... An angle formed by the tangent line and the outer peripheral connection part, 600 ... Cutting tool, 601 ... Cutting blade, 602 ... Plane part, 603a, 603b ... Curved surface Part, 610 ... cutting tool, 611 ... cutting blade, 612 ... plane part, 613a, 613b ... curved surface part, PW ... positive electrode width

Claims (8)

  1. 　活物質が塗布された集電体を集電体に平行な面への投影部の外周線の隣り合う２辺の交点の少なくとも一箇所が面取りされた面取部であって、
    　前記面取部の少なくとも一部が曲線部と前記曲線部に接続する少なくとも一つ以上の外周接続部を有し、
    　前記曲線部と前記外周接続部との交点における接線と前記外周接続部の線とのなす角の少なくとも１つ以上が鈍角であること
    を特徴とする電極。
    ここで、前記外周接続部が直線の場合には、前記接線とは直線を意味する。     A chamfered portion in which at least one intersection of two adjacent sides of the outer peripheral line of the projected portion of the current collector coated with the active material on a plane parallel to the current collector is chamfered,
    At least a part of the chamfered portion has a curved portion and at least one outer peripheral connecting portion connected to the curved portion,
    The electrode characterized in that at least one or more of the angles formed by the tangent line at the intersection of the curved portion and the outer peripheral connection portion and the line of the outer peripheral connection portion is an obtuse angle.
    Here, when the outer peripheral connection portion is a straight line, the tangent means a straight line.
  2. 　前記鈍角が、１０５°以上１８０°未満であることを特徴とする請求項１に記載の二次電池。 The secondary battery according to claim 1, wherein the obtuse angle is 105 ° or more and less than 180 °.
  3. 　前記鈍角が１２０°以上１８０°未満であることを特徴とする請求項１に記載の二次電池。 The secondary battery according to claim 1, wherein the obtuse angle is 120 ° or more and less than 180 °.
  4. 　前記鈍角が１３５°以上１８０°未満であることを特徴とする請求項１に記載の二次電池。 The secondary battery according to claim 1, wherein the obtuse angle is not less than 135 ° and less than 180 °.
  5. 　前記正極電極、前記負極電極は、それぞれ前記正極集電体、前記負極集電体と一体に形成された正極引出タブ、負極引出タブを有することを特徴とする請求項１から４のいずれか１項に記載の二次電池。 The said positive electrode and the said negative electrode have the positive electrode extraction tab and the negative electrode extraction tab which were respectively formed integrally with the said positive electrode collector and the said negative electrode collector, The any one of Claim 1 to 4 characterized by the above-mentioned. A secondary battery according to item.
  6. 　前記曲線部が円弧であることを特徴とする請求項１から５のいずれか１項記載の二次電池。 The secondary battery according to any one of claims 1 to 5, wherein the curved portion is an arc.
  7. 　リチウムイオン二次電池であることを特徴とする請求項１から６のいずれか１項記載の二次電池。 The secondary battery according to claim 1, wherein the secondary battery is a lithium ion secondary battery.
  8. 　前記正極電極、前記負極電極の外形が矩形状である請求項１から７のいずれか１項記載の二次電池。 The secondary battery according to any one of claims 1 to 7, wherein an outer shape of the positive electrode and the negative electrode is rectangular.
PCT/JP2012/072128 2011-08-31 2012-08-31 Secondary battery WO2013031938A1 (en)

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