WO2012111815A1 - 電極の製造方法及び電池の製造方法 - Google Patents
電極の製造方法及び電池の製造方法 Download PDFInfo
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- WO2012111815A1 WO2012111815A1 PCT/JP2012/053844 JP2012053844W WO2012111815A1 WO 2012111815 A1 WO2012111815 A1 WO 2012111815A1 JP 2012053844 W JP2012053844 W JP 2012053844W WO 2012111815 A1 WO2012111815 A1 WO 2012111815A1
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- electrode
- current collector
- strip
- active material
- containing layer
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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
- H01M4/04—Processes of manufacture in general
- H01M4/043—Processes of manufacture in general involving compressing or compaction
- H01M4/0435—Rolling or calendering
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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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
- H01M4/04—Processes of manufacture in general
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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
- H01M4/04—Processes of manufacture in general
- H01M4/043—Processes of manufacture in general involving compressing or compaction
- H01M4/0433—Molding
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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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
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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
- H01M4/64—Carriers or collectors
- H01M4/66—Selection of materials
- H01M4/661—Metal or alloys, e.g. alloy coatings
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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
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/04—Construction or manufacture in general
- H01M10/0431—Cells with wound or folded electrodes
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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
- 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
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- 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
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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
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- 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
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T29/00—Metal working
- Y10T29/49—Method of mechanical manufacture
- Y10T29/49002—Electrical device making
- Y10T29/49108—Electric battery cell making
Definitions
- Embodiments of the present invention relate to an electrode manufacturing method and a battery manufacturing method.
- Batteries have recently been used for power sources for hybrid electric vehicles in addition to conventional small electronic devices. Accordingly, there is a demand for a battery having high capacity, long cycle life, quick chargeability, and the like. In order to fill a limited battery with as much active material as possible, the electrodes are also compressed to a higher density.
- an active material-containing slurry is applied to a current collector made of a metal foil, dried, and then the application portion is compressed by a roll press device or the like.
- the ground current collector of the compressed coated portion also expands due to plastic deformation, but the uncoated portion where the active material-containing slurry is not coated does not apply press pressure to the current collector, and therefore does not stretch as much as the ground current collector.
- the residual stress acts on the boundary between the coated portion and the uncoated portion due to the difference in elongation of the current collector, and the electrode is distorted and warped.
- the electrodes When laminating such electrodes on a separator and winding them, the electrodes may be damaged due to distortion or warpage, or the electrodes may be damaged or cracked when correcting the displacement. Waking up occurs. In addition, the distortion and warpage of the electrodes are a factor that deteriorates quality and yield and hinders high-speed production line operation.
- the cause of the distortion and warping of the electrode is the difference in elongation of the base current collector between the slurry-applied portion after compression and the uncoated portion.
- a method of forming a groove in a press roll and compressing and extending an uncoated portion current collector simultaneously with the coated portion, and a method of extending the current collector by plastic deformation by tensile stress are proposed. ing.
- the groove shape of the press roll Managing is not technically or economically efficient. Further, when the uncoated portion current collector is removed from the groove formed by, for example, meandering of the electrode, there is a problem that uneven compression density of the electrode or electrode breakage occurs.
- An object of the present invention is to provide a method for manufacturing an electrode with a small amount of distortion and a method for manufacturing a battery using this method.
- an electrode manufacturing method including a compression molding step and a tension applying step can be provided.
- compression molding is performed on the active material-containing layer of the strip electrode plate.
- the strip-shaped electrode plate is formed on at least one long side of the strip-shaped current collector and the strip-shaped current collector, and the current collector exposed portion where the active material-containing layer does not exist on both sides, and the current collector exposure of the strip-shaped current collector And an active material-containing layer formed on at least a part other than the part.
- the strip electrode plate is disposed on the roller having the step protruding from the circumferential surface and the recess adjacent to the step, and the current collector exposed portion is positioned at the step, and the active material containing layer Is placed in the recess, and tension is applied in the long side direction of the strip electrode plate.
- an electrode manufacturing method including a step of applying tension.
- the electrode is formed on the long side of at least one of the strip-shaped current collector and the strip-shaped current collector, and the current collector exposed portion where the active material-containing layer does not exist on both sides, and the current collector exposed portion of the strip-shaped current collector And an active material-containing layer formed on at least a part thereof.
- the current collector exposed portion is located in the step portion and the active material-containing layer is located in the recess portion on the roller having the step portion protruding from the circumferential surface and the recess portion adjacent to the step portion. And tension is applied in the long side direction of the belt-like current collector.
- FIG. 1 is a schematic diagram showing one step of the method according to the first embodiment.
- FIG. 2 is a schematic diagram showing the positional relationship between the guide roller and the strip electrode plate in FIG.
- FIG. 3 is a cross-sectional view showing the positional relationship between the guide roller and the strip electrode plate used in the first embodiment.
- FIG. 4 is a cross-sectional view showing the positional relationship between the guide roller and the strip electrode plate used in the first embodiment.
- FIG. 5 is an exploded perspective view of a battery manufactured by the method according to the second embodiment. 6 is a partially developed perspective view of an electrode group used in the battery shown in FIG.
- FIG. 7 is a schematic diagram illustrating a method of measuring the amount of strain of the electrode of the example.
- FIG. 8 is a schematic diagram showing one step of the method according to the third embodiment.
- FIG. 9 is a schematic diagram showing the positional relationship between the guide roller and the strip electrode plate in FIG.
- FIG. 10 is a cross-sectional view showing the positional relationship between the guide roller and the strip electrode plate used in the third embodiment.
- FIG. 11 is a cross-sectional view showing the positional relationship between a guide roller and a strip electrode plate used in the third embodiment.
- FIG. 12 is a schematic diagram showing one step of the method according to the third embodiment.
- FIG. 13 is a schematic diagram showing one step of the method according to the fourth embodiment.
- FIG. 14 is an exploded perspective view of a battery manufactured by the method according to the fifth embodiment.
- 15 is a partially developed perspective view of an electrode group used in the battery shown in FIG.
- FIG. 1 is a schematic diagram showing a press device, a guide roller device, and a winding device used for manufacturing an electrode.
- FIG. 2 is a schematic diagram showing the positional relationship between the guide roller and the strip electrode plate in the curvature correction process.
- FIG. 2A is a plan view of the strip electrode plate running on the guide roller as viewed from the guide roller side, and FIG. 2B is obtained by cutting the guide roller parallel to the rotation axis. It is sectional drawing obtained.
- 3A is a cross-sectional view obtained when a guide roller having a taper formed at the corner of the step portion is cut in parallel to the rotation axis.
- FIG. 3B is a cross-sectional view of FIG.
- FIG. 4A is a plan view of the strip electrode plate running on the guide roller as viewed from the guide roller side
- FIG. 4B is a view of cutting the guide roller parallel to the rotation axis. It is sectional drawing obtained.
- a pressing device 21, a guide roller device 22, and a winding device 23 are arranged from the front side to the rear side of the manufacturing process.
- the press device 21 has a pair of press rolls 21a and 21b.
- the press rolls 21a and 21b are compression-molded by rotating a belt-like electrode plate 25 inserted between the press rolls 21a and 21 by being rotated in the direction of the arrow shown in FIG.
- the winding device 23 is configured such that the belt-like electrode plate 25 is wound in a hoop shape by rotating a rotating shaft 23a in the direction of the arrow shown in FIG. 1 by a drive unit (not shown).
- the guide roller device 22 is for conveying the belt-like electrode plate 25 from the press device 21 to the winding device 23, and has a plurality of metal guide rollers 24 1 to 24 5 (driven rollers). Tension (winding tension) is applied in the longitudinal direction to the strip-shaped electrode plate 25 conveyed from the press rolls 21a and 21b to the winding device 23.
- the guide rollers 24 1 to 24 5 are alternately arranged on the upper and lower surfaces of the strip electrode plate 25 so that the tension applied to the strip electrode plate 25 falls within a desired range suitable for winding.
- Guide rollers 24 3 also serves as a bending straightening device.
- Guide roller 24 3 as shown in FIG. 2 (b), it has a stepped portion 26 protruding from the circumferential surface on one end of the rotation axis direction. In the guide roller 24 3 , the remaining portion adjacent to the step portion 26 is a recess 27.
- the strip electrode plate 25 is produced. As shown in FIG. 2A and FIG. 3B, the strip electrode plate 25 is formed on one long side of the strip current collector and the strip current collector. It includes a current collector exposed portion 25a that does not exist, and an active material-containing layer 25b that is formed on both sides of the strip-shaped current collector other than the current collector exposed portion 25a.
- the active material-containing layer 25b is continuously formed in the long side direction of the strip-shaped current collector. The width in the short side direction of the active material containing layer 25b is wider than that of the current collector exposed portion 25a.
- the strip electrode plate 25 is obtained, for example, by applying an active material-containing slurry to a strip collector on both sides except for one long side, and drying. Or after apply
- the active material-containing slurry is prepared, for example, by adding a conductive agent and a binder as necessary to the active material and kneading them in the presence of a solvent.
- a conductive agent and a binder as necessary to the active material and kneading them in the presence of a solvent.
- the active material either a positive electrode or a negative electrode may be used.
- the active material of the positive electrode is not particularly limited, and various oxides such as lithium-containing cobalt oxide (for example, LiCoO 2 ), manganese dioxide, lithium manganese composite oxide (for example, LiMn 2 O 4 , LiMnO) 2 ), lithium-containing nickel oxide (eg, LiNiO 2 ), lithium-containing nickel cobalt oxide (eg, LiNi 0.8 Co 0.2 O 2 ), lithium-containing iron oxide, vanadium oxide containing lithium, Examples thereof include chalcogen compounds such as titanium disulfide and molybdenum disulfide.
- the active material of the negative electrode is not particularly limited, and for example, a graphite material or a carbonaceous material (for example, graphite, coke, carbon fiber, spherical carbon, pyrolytic vapor carbonaceous material, resin fired body, etc.), chalcogen Compound (eg, titanium disulfide, molybdenum disulfide, niobium selenide, etc.), light metal (eg, aluminum, aluminum alloy, magnesium alloy, lithium, lithium alloy, etc.), lithium titanium oxide (eg, spinel type lithium titanate) And the like.
- a graphite material or a carbonaceous material for example, graphite, coke, carbon fiber, spherical carbon, pyrolytic vapor carbonaceous material, resin fired body, etc.
- chalcogen Compound eg, titanium disulfide, molybdenum disulfide, niobium selenide, etc.
- light metal eg, aluminum, aluminum alloy, magnesium alloy, lithium
- the conductive agent is not particularly limited, and examples thereof include graphite, carbonaceous material, acetylene black, and carbon black.
- the binder is not particularly limited, and for example, polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVdF), or fluorine-based rubber can be used.
- Metal foil can be used for the strip current collector.
- the metal foil include an aluminum foil, an aluminum alloy foil, and a copper foil.
- the thickness of the strip-shaped current collector can be 50 ⁇ m or less.
- the obtained strip electrode plate 25 is inserted between press rolls 21a and 21b rotating in the direction of the arrow shown in FIG. Since the insertion direction of the strip electrode plate 25 is parallel to the longitudinal direction of the strip electrode plate 25, the pressing pressure is mainly applied to the active material-containing layer 25b, and the active material-containing layer 25b is compression-molded to increase the density. Since almost no pressing pressure is applied to the current collector exposed portion 25a, the elongation is smaller than that of the base current collector of the active material-containing layer 25b. As a result, the belt-like electrode plate 25 is distorted or warped.
- the strip electrode plate 25 that has passed between the press rolls 21a and 21b is conveyed to the winding device 23 via the guide rollers 24 1 to 24 5 .
- the guide roller 24 3 which also serves as a bending straightening device, as shown in FIGS. 2 and 3, the boundary X between the stepped portion 26 and the recess 27, the boundary between the current collector exposed portion 25a and the active material-containing layer 25b Only the current collector exposed portion 25 a is located on the stepped portion 26.
- the active material containing layer 25 b is disposed in the recess 27. Thereby, the winding tension applied in the conveying direction (longitudinal direction) of the strip electrode plate 25 can be concentrated on the current collector exposed portion 25a.
- the current collector exposed portion 25a can be sufficiently extended by the winding tension, so that the distortion and warpage generated in the strip electrode plate 25 can be corrected.
- the strip electrode plate 25 that has passed through the guide roller 24 3 is wound around the winding device 23 via the guide rollers 24 4 , 24 5 . Subsequently, the electrode is obtained by cutting the hoop-shaped strip electrode plate 25 into a desired size as necessary.
- the strip electrode plate 25 can be used as an electrode as it is.
- the entire strip-shaped current collector is not stretched. Therefore, when the strip-shaped electrode plate 25 before compression molding is brought into contact with the guide roller 24 3 , the current collector exposed portion 25a on the step portion 26 is obtained.
- the winding tension (stress) is dispersed in the active material-containing layer 25b.
- the base current collector of the active material-containing layer 25b is stretched and loosened, so that the winding current (stress) is hardly applied to the base current collector of the active material-containing layer 25b and is not stretched.
- the winding tension can be concentrated on the exposed portion 25a. At this time, the amount of distortion of the electrode can be reduced by about 10% after the electrode is wound around the winding device 23 with the same tension as the winding tension at the time of compression.
- the winding tension is to distribute to the active material-containing layer 25b, the winding tension of the collector-exposed portion 25a Concentration becomes insufficient, and the base current collector of the active material-containing layer 25b that has already been stretched may be further extended, so that the distortion and warping of the electrode are not corrected.
- the thickness per one side strip collector of the active material-containing layer upon 100%.
- the thickness per side of the strip-shaped current collector of the active material-containing layer is the thickness per side of the strip-shaped current collector of the active material-containing layer in the manufactured electrode.
- the stress can be sufficiently concentrated on the exposed portion of the current collector and extended.
- the level difference H 600% or less it is possible to suppress wrinkles and cracks from occurring near the boundary between the active material-containing layer 25b and the current collector exposed portion 25a. These wrinkles and cracks may cause electrode breakage or welding failure in a later process. Therefore, by setting the level difference H to 150% or more and 600% or less, it is possible to suppress the occurrence of wrinkles and cracks in the vicinity of the boundary between the active material containing layer 25b and the current collector exposed portion 25a, and stress on the current collector exposed portion. Can be stretched with sufficient concentration. In order to enhance the effect of preventing wrinkles and cracks, the range of 200 ⁇ H ⁇ 400 is more preferable.
- the taper is desirably formed at a portion where the boundary X between the step portion 26 and the recess 27 intersects with the upper surface of the step portion 26.
- the taper R (mm) is preferably R ⁇ 15.
- the taper R is calculated by coordinate plotting several points on the R surface of the R portion of the step portion 26 with a three-dimensional measuring instrument.
- a three-dimensional measuring instrument for example, a three-dimensional measuring machine (model: WMM550) manufactured by Carl Zeiss Co., Ltd. can be used.
- the tensile stress F (N / mm 2 ) in the cross section parallel to the short side direction of the strip-shaped electrode plate 25 is in the range of 20 ⁇ F ⁇ 100.
- the tensile stress F is set to 20 (N / mm 2 ) or more, the current collector exposed portion can be sufficiently extended while satisfying the stress necessary for winding the electrode with high accuracy.
- the tensile stress F is 100 (N / mm 2 ) or less, the current collector exposed portion can be sufficiently extended without causing problems of electrode breakage and winding accuracy reduction.
- the current collector exposed portion can be sufficiently extended without breaking the electrode and accurately winding the electrode. Can do.
- the range of 20 ⁇ F ⁇ 40 is more preferable in order to enhance the effect of preventing the electrode from breaking and winding accuracy.
- the heat treatment temperature T is set to 60 ° C. or more, the effect of reducing the stress required for plastic deformation can be enhanced. Further, when the stress applied to the strip electrode plate is the same, the effect of correcting the distortion and warpage of the electrode can be enhanced by heating. These effects are more easily obtained when the heat treatment temperature T is higher, but the heat treatment temperature T is preferably in the range of 60 ° C. or higher and 150 ° C. or lower in order to avoid alteration of the active material-containing layer due to heat.
- a press roll is used as the press device 21, but any press material that can increase the density of the active material-containing layer can be used instead of the press roll.
- a flat plate press can be used instead of the press roll.
- the pressing process may be performed by changing the pressing pressure in multiple stages.
- one guide roller among the plurality of guide rollers is used as the curvature correcting device, but the number of guide rollers used as the curvature correcting device is not limited to one, and a plurality of all or all of the guide rollers are used. be able to. Further, the position of the guide roller used as the curvature correcting device is not limited to the third guide roller 243 from the front stage side, and a guide roller at an arbitrary position can be used.
- the step portion 26 protruding from the circumferential surface is provided at one end portion in the rotation axis direction of the guide roller 24 3 , but the method of forming the step portion is not limited to this, and the current collector exposed portion is Any material can be used as long as the effect of stretching can be obtained.
- an annular step portion 26 protruding from the circumferential surface can be provided near the center in the rotation axis direction, and the circumferential surfaces on both sides adjacent to the step portion 26 can be formed as the recesses 27. .
- the current collector exposed portion is provided only on the long side of one side of the strip electrode plate, but the current collector exposed portion may be provided on both long sides of the strip plate. Providing current collector exposed portions on both long sides of the strip electrode plate can further enhance the effect of preventing warping and distortion of the electrode. On the other hand, when the current collector exposed portion is provided only on the long side of one side of the strip electrode plate as shown in FIG. 2, a high battery capacity and energy density can be obtained.
- the active material-containing layer is provided on both sides of the strip electrode, but the active material-containing layer may be provided only on one side of the strip electrode.
- the active material-containing layer is continuously formed in the long-side direction of the strip-shaped current collector.
- the active material-containing layer is intermittently formed in the long-side direction of the strip-shaped current collector. You may provide an active material content layer non-formation part between content layers.
- the strip-shaped electrode plate subjected to compression molding is arranged such that the current collector exposed portion is located in the stepped portion of the roller and the active material-containing layer is located in the recessed portion of the roller. Since the tension is applied in the long side direction of the belt-like electrode plate, the tension can be concentrated on the current collector exposed portion, and the current collector exposed portion can be sufficiently stretched by plastic deformation. Thereby, the distortion and the curvature which arose in the electrode by compression molding can be corrected. In addition, the electrode can be prevented from being broken when the electrode group is manufactured. As a result, an electrode with excellent quality can be manufactured with high production efficiency.
- FIG. 5 is an exploded perspective view of a nonaqueous electrolyte battery manufactured by the method according to the second embodiment.
- 6 is a partially developed perspective view of an electrode group used in the battery shown in FIG.
- the battery shown in FIG. 5 is a sealed prismatic non-aqueous electrolyte secondary battery.
- the nonaqueous electrolyte secondary battery includes an outer can 1, a lid 2, a positive electrode output terminal 3, a negative electrode output terminal 4, and an electrode group 5.
- the outer can 1 has a bottomed rectangular tube shape, and is formed of a metal such as aluminum, an aluminum alloy, iron, or stainless steel, for example.
- the flat electrode group 5 has a positive electrode 6 and a negative electrode 7 wound in a flat shape with a separator 8 therebetween.
- the positive electrode 6 is a positive electrode current collector except for a strip-shaped positive electrode current collector made of, for example, a metal foil, a positive electrode current collector tab 6a formed of a current collector exposed portion of the positive electrode current collector, and at least a portion of the positive electrode current collector tab 6a.
- the negative electrode 7 is a negative electrode except for a strip-shaped negative electrode current collector made of, for example, a metal foil, a negative electrode current collector tab 7a formed of a current collector exposed portion of the negative electrode current collector, and at least a portion of the negative electrode current collector tab 7a. And a negative electrode active material layer 7b formed on the current collector.
- the positive electrode current collecting tab 6 a protrudes from the separator 8 in the winding axis direction of the electrode group, and the negative electrode current collecting tab 7 a protrudes from the separator 8 in the opposite direction.
- the positive electrode 6 and the negative electrode 7 are wound while being shifted in position.
- the electrode group 5 has the positive electrode current collecting tab 6a wound spirally from one end face and is wound spirally from the other end face.
- the negative electrode current collection tab 7a protrudes.
- Electrolytic solution (not shown) is impregnated in the electrode group 5.
- the rectangular plate-like lid 2 is seam welded to the opening of the outer can 1 by, for example, a laser.
- the lid 2 is made of a metal such as aluminum, aluminum alloy, iron or stainless steel, for example.
- the lid 2 and the outer can 1 are preferably formed from the same type of metal.
- a safety valve 9 is provided near the center of the outer surface of the lid 2.
- the safety valve 9 has a rectangular recess 9a provided on the outer surface of the lid 2 and an X-shaped groove 9b provided in the recess 9a.
- the groove 9b is formed, for example, by press-molding the lid 2 in the plate thickness direction.
- the liquid injection port 10 is opened in the lid 2 and sealed after the electrolytic solution is injected.
- the positive and negative output terminals 3 and 4 are caulked and fixed to the outer surface of the lid 2 via insulating gaskets (not shown) on both sides of the safety valve 9 therebetween.
- a lithium ion secondary battery using a carbon-based material for the negative electrode active material for example, aluminum or an aluminum alloy is used for the positive electrode output terminal 3, and copper, nickel, nickel plating is used for the negative electrode output terminal 4, for example. Used metals such as iron are used.
- lithium titanate is used as the negative electrode active material, in addition to the above, aluminum or an aluminum alloy may be used for the negative electrode output terminal 4.
- One end of the positive electrode lead 11 is electrically connected to the positive electrode output terminal 3 by caulking or welding, and the other end is electrically connected to the positive electrode current collecting tab 6a.
- One end of the negative electrode lead 12 is electrically connected to the negative electrode output terminal 4 by caulking or welding, and the other end is electrically connected to the negative electrode current collecting tab 7a.
- a method of electrically connecting the positive and negative electrode leads 11 and 12 to the positive and negative electrode current collecting tabs 6a and 7a is not particularly limited, and examples thereof include welding such as ultrasonic welding and laser welding.
- the positive electrode output terminal 3 and the positive electrode current collecting tab 6 a are electrically connected via the positive electrode lead 11, and the negative electrode output terminal 4 and the negative electrode current collecting tab 7 a are electrically connected via the negative electrode lead 12.
- current can be taken out from the positive and negative output terminals 3 and 4.
- the material of the positive and negative electrode leads 11 and 12 is not particularly specified, it is desirable to use the same material as that of the positive and negative electrode output terminals 3 and 4.
- the material of the output terminal is aluminum or an aluminum alloy
- the material of the lead is aluminum or an aluminum alloy.
- the output terminal is copper
- the material of the lead is copper.
- the separator is not particularly limited, and for example, a microporous film, a woven fabric, a non-woven fabric, or a laminate of the same material or different materials among these can be used.
- the material for forming the separator include polyethylene, polypropylene, ethylene-propylene copolymer, ethylene-butene copolymer, and cellulose.
- Non-aqueous electrolyte a non-aqueous electrolyte solution in which an electrolyte (for example, a lithium salt) is dissolved in a non-aqueous solvent
- Nonaqueous solvents include, for example, ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), dimethyl carbonate (DMC), diethyl carbonate (DEC), ethyl methyl carbonate (EMC), ⁇ -butyrolactone ( ⁇ - BL), sulfolane, acetonitrile, 1,2-dimethoxyethane, 1,3-dimethoxypropane, dimethyl ether, tetrahydrofuran (THF), 2-methyltetrahydrofuran and the like.
- EC ethylene carbonate
- PC propylene carbonate
- BC butylene carbonate
- DMC dimethyl carbonate
- DEC diethyl carbonate
- EMC ethyl methyl carbonate
- Nonaqueous solvents may be used alone or in combination of two or more.
- the electrolyte include lithium perchlorate (LiClO 4 ), lithium hexafluorophosphate (LiPF 6 ), lithium tetrafluoroborate (LiBF 4 ), lithium hexafluoroarsenate (LiAsF 6 ), and trifluoromethanesulfonic acid.
- a lithium salt such as lithium (LiCF 3 SO 3 ) can be given.
- the electrolyte may be used alone or in combination of two or more.
- the amount of electrolyte dissolved in the non-aqueous solvent is preferably 0.2 mol / L to 3 mol / L. If the electrolyte concentration is too low, sufficient ionic conductivity may not be obtained. On the other hand, if it is too high, it may not be completely dissolved in the electrolyte.
- the strip-shaped electrode plate that has been subjected to compression molding is arranged such that the current collector exposed portion is located at the stepped portion of the roller and the active material-containing layer is located at the recessed portion of the roller. Since the tension is applied in the long side direction of the belt-like electrode plate, the tension can be concentrated on the current collector exposed portion, and the current collector exposed portion can be sufficiently stretched by plastic deformation. Thereby, the distortion and the curvature which arose in the electrode by compression molding can be corrected. In addition, it is possible to eliminate problems such as electrode breakage, winding misalignment, wrinkles, cracks, etc. that have occurred in the process of producing a wound electrode group, so that it is possible to manufacture electrodes with excellent quality and production efficiency. Can do.
- FIG. 8 is a schematic diagram showing a press device, a guide roller device, and a first winding device used for manufacturing an electrode.
- FIG. 9 is a schematic diagram showing the positional relationship between the guide roller and the strip electrode plate in the curvature correction process.
- FIG. 9A is a plan view of the belt-like electrode plate running on the guide roller as viewed from the guide roller side
- FIG. 9B is a view of cutting the guide roller parallel to the rotation axis. It is sectional drawing obtained.
- 10A is a cross-sectional view obtained when a guide roller having a taper formed at a corner of a step portion is cut in parallel to the rotation axis
- FIG. 10B is a cross-sectional view of FIG.
- FIG. 11A is a plan view of the belt-like electrode plate running on the guide roller as viewed from the guide roller side
- FIG. 11B is a view of cutting the guide roller parallel to the rotation axis. It is sectional drawing obtained.
- FIG. 12 is a schematic diagram showing a feeding device and a second winding device used for manufacturing an electrode.
- the pressing device 21 from the first-stage of the manufacturing process towards the subsequent stage, the guide roller device 22, the first winding device 23 1 is disposed.
- the press device 21 has a pair of press rolls 21a and 21b.
- the press rolls 21a and 21b are compression-molded by rotating the belt-like electrode plate 25 inserted between the press rolls 21a and 21 by rotating in the direction of the arrow shown in FIG.
- the belt-like electrode plate 25 is wound up in a reel shape by rotating the rotating shaft 23 a in the direction of the arrow shown in FIG. 8 by a drive unit (not shown). .
- the guide roller device 22 is for conveying the strip electrode plate 25 from the press device 21 to the first winding device 23 1 , and has a plurality of metal guide rollers 24 1 to 24 5 (driven rollers). Tension (winding tension) is applied in the longitudinal direction to the strip-shaped electrode plate 25 conveyed from the press rolls 21a and 21b to the first winding device 23 1 .
- the guide rollers 24 1 to 24 5 are alternately arranged on the upper and lower surfaces of the strip electrode plate 25 so that the tension applied to the strip electrode plate 25 falls within a desired range suitable for winding.
- Guide rollers 24 3 also serves as a bending straightening device.
- the strip electrode plate 25 is produced. As shown in FIG. 9A and FIG. 10B, the strip electrode plate 25 is formed on one long side of the strip collector and the strip collector, and has an active material containing layer on both sides. It includes a current collector exposed portion 25a that does not exist, and an active material-containing layer 25b that is formed on both sides of the strip-shaped current collector other than the current collector exposed portion 25a. The active material-containing layer 25b is continuously formed in the long side direction of the strip-shaped current collector. The width in the short side direction of the active material containing layer 25b is wider than that of the current collector exposed portion 25a.
- the strip electrode plate 25 is obtained, for example, by applying an active material-containing slurry to a strip collector on both sides except for one long side, and drying. Or after apply
- the active material-containing slurry is prepared, for example, by adding a conductive agent and a binder as necessary to the active material and kneading them in the presence of a solvent.
- a conductive agent and a binder as necessary to the active material and kneading them in the presence of a solvent.
- the active material either a positive electrode or a negative electrode may be used.
- the active material of the positive electrode is not particularly limited, and various oxides such as lithium-containing cobalt oxide (for example, LiCoO 2 ), manganese dioxide, lithium manganese composite oxide (for example, LiMn 2 O 4 , LiMnO) 2 ), lithium-containing nickel oxide (eg, LiNiO 2 ), lithium-containing nickel cobalt oxide (eg, LiNi 0.8 Co 0.2 O 2 ), lithium-containing iron oxide, vanadium oxide containing lithium, Examples thereof include chalcogen compounds such as titanium disulfide and molybdenum disulfide.
- the active material of the negative electrode is not particularly limited, and for example, a graphite material or a carbonaceous material (for example, graphite, coke, carbon fiber, spherical carbon, pyrolytic vapor carbonaceous material, resin fired body, etc.), chalcogen Compound (eg, titanium disulfide, molybdenum disulfide, niobium selenide, etc.), light metal (eg, aluminum, aluminum alloy, magnesium alloy, lithium, lithium alloy, etc.), lithium titanium oxide (eg, spinel type lithium titanate) And the like.
- a graphite material or a carbonaceous material for example, graphite, coke, carbon fiber, spherical carbon, pyrolytic vapor carbonaceous material, resin fired body, etc.
- chalcogen Compound eg, titanium disulfide, molybdenum disulfide, niobium selenide, etc.
- light metal eg, aluminum, aluminum alloy, magnesium alloy, lithium
- the conductive agent is not particularly limited, and examples thereof include graphite, carbonaceous material, acetylene black, and carbon black.
- the binder is not particularly limited, and for example, polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVdF), or fluorine-based rubber can be used.
- Metal foil can be used for the strip current collector.
- the metal foil include an aluminum foil, an aluminum alloy foil, and a copper foil.
- the thickness of the strip-shaped current collector can be 50 ⁇ m or less.
- the obtained belt-like electrode plate 25 is inserted between press rolls 21a and 21b rotating in the direction of the arrow shown in FIG. Since the insertion direction of the strip electrode plate 25 is parallel to the longitudinal direction of the strip electrode plate 25, the pressing pressure is mainly applied to the active material-containing layer 25b, and the active material-containing layer 25b is compression-molded to increase the density. Since almost no pressing pressure is applied to the current collector exposed portion 25a, the elongation is smaller than that of the base current collector of the active material-containing layer 25b. As a result, the belt-like electrode plate 25 is distorted or warped.
- the strip electrode plate 25 that has passed between the press rolls 21a and 21b is conveyed to the first winding device 23 1 via the guide rollers 24 1 to 24 5 .
- the guide roller 24 3 which also serves as a bending straightening device, as shown in FIGS. 9 and 10, the boundary X between the stepped portion 26 and the recess 27, the boundary between the current collector exposed portion 25a and the active material-containing layer 25b Only the current collector exposed portion 25 a is located on the stepped portion 26.
- the active material containing layer 25 b is disposed in the recess 27. Thereby, the winding tension applied in the conveying direction (longitudinal direction) of the strip electrode plate 25 can be concentrated on the current collector exposed portion 25a.
- the current collector exposed portion 25a can be sufficiently extended by the winding tension, so that the distortion and warpage generated in the strip electrode plate 25 can be corrected.
- the strip electrode plate 25 that has passed through the guide roller 24 3 is wound around the first winding device 23 1 via the guide rollers 24 4 and 24 5 .
- the entire strip-shaped current collector is not stretched. Therefore, when the strip-shaped electrode plate 25 before compression molding is brought into contact with the guide roller 24 3 , the current collector exposed portion 25a on the step portion 26 is obtained.
- the winding tension (stress) is dispersed in the active material-containing layer 25b.
- the base current collector of the active material-containing layer 25b is stretched and loosened, so that the winding current (stress) is hardly applied to the base current collector of the active material-containing layer 25b and is not stretched.
- the winding tension can be concentrated on the exposed portion 25a. At this time, the amount of distortion of the electrodes, the distortion amount of compressed hand, be reduced to about 10% after recombinant winding the electrode to the first winding device 23 1 in the same tension as the winding tension at the time of compression it can.
- the winding tension is to distribute to the active material-containing layer 25b, the winding tension of the collector-exposed portion 25a Concentration becomes insufficient, and the base current collector of the active material-containing layer 25b that has already been stretched may be further extended, so that the distortion and warping of the electrode are not corrected.
- the thickness per one side strip collector of the active material-containing layer upon 100%.
- the thickness per side of the strip-shaped current collector of the active material-containing layer is the thickness per side of the strip-shaped current collector of the active material-containing layer in the manufactured electrode.
- the stress can be sufficiently concentrated on the exposed portion of the current collector and extended.
- the level difference H 600% or less it is possible to suppress wrinkles and cracks from occurring near the boundary between the active material-containing layer 25b and the current collector exposed portion 25a. These wrinkles and cracks may cause electrode breakage or welding failure in a later process. Therefore, by setting the level difference H to 150% or more and 600% or less, it is possible to suppress the occurrence of wrinkles and cracks in the vicinity of the boundary between the active material containing layer 25b and the current collector exposed portion 25a, and stress on the current collector exposed portion. Can be stretched with sufficient concentration. In order to enhance the effect of preventing wrinkles and cracks, the range of 200 ⁇ H ⁇ 400 is more preferable.
- Corner of the stepped portion 26 provided on the guide roller 24 3, may be a right angle or substantially a right angle as illustrated in (b) of FIG. 9 may be provided a taper.
- the taper is desirably formed at a portion where the boundary X between the step portion 26 and the recess 27 intersects with the upper surface of the step portion 26.
- the taper R (mm) is preferably R ⁇ 15.
- the taper R is calculated by coordinate plotting several points on the R surface of the R portion of the step portion 26 with a three-dimensional measuring instrument.
- a three-dimensional measuring instrument for example, a three-dimensional measuring machine (model: WMM550) manufactured by Carl Zeiss Co., Ltd. can be used.
- the tensile stress F (N / mm 2 ) in the cross section parallel to the short side direction of the strip-shaped electrode plate 25 is in the range of 20 ⁇ F ⁇ 100.
- the tensile stress F is set to 20 (N / mm 2 ) or more, the current collector exposed portion can be sufficiently extended while satisfying the stress necessary for winding the electrode with high accuracy.
- the tensile stress F is 100 (N / mm 2 ) or less, the current collector exposed portion can be sufficiently extended without causing problems of electrode breakage and winding accuracy reduction.
- the current collector exposed portion can be sufficiently extended without breaking the electrode and accurately winding the electrode. Can do.
- the range of 20 ⁇ F ⁇ 40 is more preferable in order to enhance the effect of preventing the electrode from breaking and winding accuracy.
- the heat treatment temperature T is set to 60 ° C. or more, the effect of reducing the stress required for plastic deformation can be enhanced. Further, when the stress applied to the strip electrode plate is the same, the effect of correcting the distortion and warpage of the electrode can be enhanced by heating. These effects are more easily obtained when the heat treatment temperature T is higher, but the heat treatment temperature T is preferably in the range of 60 ° C. or higher and 150 ° C. or lower in order to avoid alteration of the active material-containing layer due to heat.
- the strip-shaped electrode plate 25 wound in a reel shape by the first winding device 23 1 is dried.
- the drying process is desirably performed in a vacuum of 100 ° C. or higher and 180 ° C. or lower, reduced pressure, or atmospheric pressure.
- the temperature of the atmosphere By setting the temperature of the atmosphere to 100 ° C. or higher, moisture removal from the strip electrode plate 25 can be promoted.
- the heat deterioration of the material contained in an active material content layer can be prevented by setting it as 180 degrees C or less. Therefore, by setting the temperature of the atmosphere to a range of 100 ° C. or higher and 180 ° C. or lower, moisture removal from the strip electrode plate 25 can be promoted while preventing thermal deterioration of the material contained in the active material-containing layer.
- the drying time is desirably 10 hours or more.
- the strip electrode plate 25 Since the strip electrode plate 25 is wound in a reel shape, tension due to winding is applied.
- the base current collector of the active material-containing layer 25b is deformed following the winding of the active material-containing layer 25b, so that it is more susceptible to tension than the current collector exposed portion 25a.
- plastic deformation is promoted by heat, so that the base current collector of the active material-containing layer 25b extends more than the current collector exposed portion 25a, and as a result, Warpage or distortion occurs again in the strip electrode plate 25.
- the second curvature correction is performed using the apparatus shown in FIG. As shown in FIG. 12, a feeding device 28, a plurality of metal guide rollers 24 1 to 24 4 , and a second winding device 29 are arranged from the front side to the rear side of the manufacturing process.
- the feeding device 28 is configured so that the belt-like electrode plate 25 wound in a reel shape is fed out in the transport direction by rotating the rotating shaft 28a in the direction of the arrow shown in FIG. 12 by a drive unit (not shown).
- the second winding device 29 is configured such that the belt-like electrode plate 25 is wound in a reel shape by rotating a rotating shaft 29a in the direction of the arrow shown in FIG. 12 by a drive unit (not shown).
- the plurality of guide rollers 24 1 to 24 4 are alternately arranged on the upper and lower surfaces of the belt-like electrode plate 25 so that the belt-like electrode plate 25 is tensioned for winding.
- the guide rollers 24 1 to 24 4 are the same as those described in the first curvature correction, and the guide roller 24 3 also serves as a curvature correction device.
- the strip electrode plate 25 fed out from the feeding device 28 passes through the guide rollers 24 1 to 24 2 and is then conveyed to the guide roller 24 3 .
- the boundary between the current collector exposed portion 25 a and the active material containing layer 25 b is located at the boundary X between the step portion 26 and the concave portion 27. Only the exposed portion 25 a is disposed on the stepped portion 26.
- the active material containing layer 25 b is disposed in the recess 27. Thereby, the winding tension applied in the conveying direction (longitudinal direction) of the strip electrode plate 25 can be concentrated on the current collector exposed portion 25a.
- the current collector exposed portion 25a can be sufficiently extended by the winding tension, so that the distortion and warpage generated in the strip electrode plate 25 can be corrected again.
- the strip-shaped electrode plate 25 that has passed through the guide roller 24 3 is wound around the second winding device 29 via the guide roller 24 4 .
- the electrode is obtained by cutting the strip-shaped electrode plate 25 wound in a reel shape by the second winding device 29 into a desired size as necessary.
- the strip electrode plate 25 can be used as an electrode as it is.
- a press roll is used as the press device 21, but it can be used instead of the press roll as long as the active material-containing layer can be densified.
- a flat plate press can be used instead of the press roll.
- one guide roller among the plurality of guide rollers is used as the curvature correcting device, but the number of guide rollers used as the curvature correcting device is not limited to one, and a plurality of all or all of the guide rollers are used. Can be individual. Further, the position of the guide roller used as the curvature correcting device is not limited to the third guide roller 243 from the front stage side, and a guide roller at an arbitrary position can be used.
- the method of forming the stepped portion is not limited to this, the collector-exposed portion Any material can be used as long as the effect of stretching can be obtained.
- an annular stepped portion 26 protruding from the circumferential surface can be provided near the center in the rotation axis direction, and the circumferential surfaces on both sides adjacent to the stepped portion 26 can be recessed portions 27. .
- the current collector exposed portion is provided only on the long side of one side of the strip electrode plate, but the current collector exposed portion may be provided on both long sides of the strip electrode plate. Providing current collector exposed portions on both long sides of the strip electrode plate can further enhance the effect of preventing warping and distortion of the electrode. On the other hand, when the current collector exposed portion is provided only on the long side of one side of the strip electrode plate as shown in FIG. 9, a high battery capacity and energy density can be obtained.
- the active material-containing layer is provided on both sides of the strip electrode plate, but the active material-containing layer may be provided only on one side of the strip electrode plate.
- the active material-containing layer is continuously formed in the long side direction of the strip-shaped current collector. However, the active material-containing layer is intermittently formed in the long side direction of the strip-shaped current collector, and the active material is formed. You may provide an active material content layer non-formation part between content layers.
- curvature correction is performed after each step of compression molding and drying.
- the strip electrode is arranged so that the current collector exposed portion is located at the step portion of the roller and the active material containing layer is located at the concave portion of the roller, and tension is applied in the long side direction of the strip electrode plate. Therefore, the tension can be concentrated on the current collector exposed portion, and the current collector exposed portion can be sufficiently deformed by plastic deformation. Thereby, the distortion and the curvature which arose in the electrode by the compression molding and the drying process can be corrected. As a result, an electrode with excellent quality can be manufactured with high production efficiency.
- Compressive molding may be performed once as in the third embodiment, but can also be performed in multiple stages.
- the required load (pressure) is reduced at each stage, so that warpage and distortion generated in the electrode at each stage are reduced.
- the distortion of the electrode that occurs when compressed to the desired thickness (or density) at once and the distortion of the electrode that occurs when compressed to the desired thickness (or density) divided into multiple times (divided into multiple times) The sum of the generated electrode strains), the latter strain becomes smaller. Therefore, after performing compression molding in a plurality of times and then performing curvature correction, it is possible to efficiently manufacture a high-density electrode without warping or distortion.
- FIG. 13 is a schematic diagram showing a pressing device and a guide roller used for manufacturing an electrode.
- a first press device 21 1 a plurality of metal guide rollers 24 1 to 24 4 , and a second press device 21 2 are arranged from the front side to the rear side of the manufacturing process.
- the first and second press devices 21 1 and 21 2 each have a pair of press rolls 21a and 21b.
- the press rolls 21a and 21b are compression-molded by rotating a belt-like electrode plate 25 inserted between the press rolls 21a and 21 by being rotated in the direction of the arrow shown in FIG.
- the plurality of guide rollers 24 1 to 24 4 are alternately arranged on the upper and lower surfaces of the belt-like electrode plate 25 so that the belt-like electrode plate 25 is tensioned for conveyance.
- the guide rollers 24 1 to 24 4 are the same as those described in the first curvature correction, and the guide roller 24 3 also serves as a curvature correction device.
- the strip-shaped electrode plate that has passed through the second pressing device 21 2 is wound in a reel shape by a winding device via a guide roll device. As the guide roll device and the winding device, those shown in FIG. 8 can be used.
- the third strip electrode plate 25 obtained in the same manner as described in embodiments, the first press device 21 1 of the press rolls 21a, inserted between the 21b, subjected to compression molding. Since the insertion direction of the strip electrode plate 25 is parallel to the longitudinal direction of the strip electrode plate 25, the pressing pressure is mainly applied to the active material-containing layer 25b, and the active material-containing layer 25b is compression-molded to increase the density. Since almost no pressing pressure is applied to the current collector exposed portion 25a, the elongation is smaller than that of the base current collector of the active material-containing layer 25b. As a result, the belt-like electrode plate 25 is distorted or warped.
- the strip electrode plate 25 that has passed between the press rolls 21a and 21b of the first pressing device 21 1 is conveyed to the guide roller 24 3 via the guide rollers 24 1 to 24 2 .
- the boundary between the current collector exposed portion 25 a and the active material containing layer 25 b is located at the boundary X between the step portion 26 and the concave portion 27. Only the exposed portion 25 a is disposed on the stepped portion 26.
- the active material containing layer 25 b is disposed in the recess 27. Thereby, the winding tension applied in the conveying direction (longitudinal direction) of the strip electrode plate 25 can be concentrated on the current collector exposed portion 25a.
- the current collector exposed portion 25a can be sufficiently extended by the winding tension, so that the distortion and warpage generated in the strip electrode plate 25 can be corrected.
- the strip-shaped electrode plate 25 that has passed through the guide roller 24 3 is conveyed to the second press device 21 2 via the guide roller 24 4 .
- the strip-shaped electrode plate 25 is inserted between the press rolls 21a and 21b of the second press device 21 2 and subjected to compression molding. Since the insertion direction of the strip electrode plate 25 is parallel to the longitudinal direction of the strip electrode plate 25, the pressing pressure is mainly applied to the active material-containing layer 25b, and the active material-containing layer 25b is compression-molded to increase the density. Since almost no pressing pressure is applied to the current collector exposed portion 25a, the elongation is smaller than that of the base current collector of the active material-containing layer 25b. As a result, the belt-like electrode plate 25 is distorted or warped.
- the strip electrode plate 25 that has passed through the second press device 21 2 is conveyed to the winding device via a plurality of guide rollers. Since one of the plurality of guide rollers also serves as a curvature correction device, the distortion and warpage generated in the strip electrode plate 25 can be corrected.
- An electrode is obtained by cutting the strip-shaped electrode plate wound in a reel shape by a winding device into a desired size as necessary. Note that a strip electrode plate can be used as an electrode as it is.
- the compression molding is performed in two stages, but is not limited to this, and can be performed in three or more stages.
- the curvature is corrected each time compression molding is performed, and then the electrode is obtained by cutting to a desired size as necessary.
- a press roll is used as the press device 21, but any press material that can increase the density of the active material-containing layer can be used instead of the press roll.
- a flat plate press can be used instead of the press roll.
- one guide roller among the plurality of guide rollers is used as the curvature correcting device, but the number of guide rollers used as the curvature correcting device is not limited to one, and a plurality of all or all of the guide rollers are used. be able to. Further, the position of the guide roller used as the curvature correcting device is not limited to the third guide roller 243 from the front stage side, and a guide roller at an arbitrary position can be used. Furthermore, the position and number of guide rollers used as the curvature correcting device may be the same in all the steps, or may be different for each step.
- an electrode manufacturing method including multistage compression molding and curvature correction is provided.
- the strip electrode plate is arranged so that the current collector exposed portion is located at the step portion of the roller and the active material-containing layer is located at the concave portion of the roller, and the strip electrode plate is arranged in the long side direction of the strip electrode plate. Since tension is applied, the tension can be concentrated on the current collector exposed portion, and the current collector exposed portion can be sufficiently deformed by plastic deformation. Therefore, by combining multi-stage compression molding and curvature correction, it is possible to sufficiently correct the distortion and warpage generated in the electrode. As a result, an electrode with excellent quality can be manufactured with high production efficiency.
- FIG. 14 is an exploded perspective view of a nonaqueous electrolyte battery manufactured by the method according to the third embodiment.
- 15 is a partially developed perspective view of an electrode group used in the battery shown in FIG.
- the battery shown in FIG. 14 is a sealed prismatic non-aqueous electrolyte secondary battery.
- the nonaqueous electrolyte secondary battery includes an outer can 1, a lid 2, a positive electrode output terminal 3, a negative electrode output terminal 4, and an electrode group 5.
- the outer can 1 has a bottomed rectangular tube shape, and is formed of a metal such as aluminum, an aluminum alloy, iron, or stainless steel, for example.
- the flat electrode group 5 has a positive electrode 6 and a negative electrode 7 wound in a flat shape with a separator 8 therebetween.
- the positive electrode 6 is a positive electrode current collector except for a strip-shaped positive electrode current collector made of, for example, a metal foil, a positive electrode current collector tab 6a formed of a current collector exposed portion of the positive electrode current collector, and at least a portion of the positive electrode current collector tab 6a.
- the negative electrode 7 is a negative electrode except for a strip-shaped negative electrode current collector made of, for example, a metal foil, a negative electrode current collector tab 7a formed of a current collector exposed portion of the negative electrode current collector, and at least a portion of the negative electrode current collector tab 7a. And a negative electrode active material layer 7b formed on the current collector.
- the positive electrode current collecting tab 6 a protrudes from the separator 8 in the winding axis direction of the electrode group, and the negative electrode current collecting tab 7 a protrudes from the separator 8 in the opposite direction.
- the positive electrode 6 and the negative electrode 7 are wound while being shifted in position.
- the electrode group 5 has the positive electrode current collecting tab 6a wound spirally from one end face and is wound spirally from the other end face.
- the negative electrode current collection tab 7a protrudes.
- Electrolytic solution (not shown) is impregnated in the electrode group 5.
- the rectangular plate-like lid 2 is seam welded to the opening of the outer can 1 by, for example, a laser.
- the lid 2 is made of a metal such as aluminum, aluminum alloy, iron or stainless steel, for example.
- the lid 2 and the outer can 1 are preferably formed from the same type of metal.
- a safety valve 9 is provided near the center of the outer surface of the lid 2.
- the safety valve 9 has a rectangular recess 9a provided on the outer surface of the lid 2 and an X-shaped groove 9b provided in the recess 9a.
- the groove 9b is formed, for example, by press-molding the lid 2 in the plate thickness direction.
- the liquid injection port 10 is opened in the lid 2 and sealed after the electrolytic solution is injected.
- the positive and negative output terminals 3 and 4 are caulked and fixed to the outer surface of the lid 2 via insulating gaskets (not shown) on both sides of the safety valve 9 therebetween.
- a lithium ion secondary battery using a carbon-based material for the negative electrode active material for example, aluminum or an aluminum alloy is used for the positive electrode output terminal 3, and copper, nickel, nickel plating is used for the negative electrode output terminal 4, for example. Used metals such as iron are used.
- lithium titanate is used as the negative electrode active material, in addition to the above, aluminum or an aluminum alloy may be used for the negative electrode output terminal 4.
- One end of the positive electrode lead 11 is electrically connected to the positive electrode output terminal 3 by caulking or welding, and the other end is electrically connected to the positive electrode current collecting tab 6a.
- One end of the negative electrode lead 12 is electrically connected to the negative electrode output terminal 4 by caulking or welding, and the other end is electrically connected to the negative electrode current collecting tab 7a.
- a method of electrically connecting the positive and negative electrode leads 11 and 12 to the positive and negative electrode current collecting tabs 6a and 7a is not particularly limited, and examples thereof include welding such as ultrasonic welding and laser welding.
- the positive electrode output terminal 3 and the positive electrode current collecting tab 6 a are electrically connected via the positive electrode lead 11, and the negative electrode output terminal 4 and the negative electrode current collecting tab 7 a are electrically connected via the negative electrode lead 12.
- current can be taken out from the positive and negative output terminals 3 and 4.
- the material of the positive and negative electrode leads 11 and 12 is not particularly specified, it is desirable to use the same material as that of the positive and negative electrode output terminals 3 and 4.
- the material of the output terminal is aluminum or an aluminum alloy
- the material of the lead is aluminum or an aluminum alloy.
- the output terminal is copper
- the material of the lead is copper.
- the separator is not particularly limited, and for example, a microporous film, a woven fabric, a non-woven fabric, or a laminate of the same material or different materials among these can be used.
- the material for forming the separator include polyethylene, polypropylene, ethylene-propylene copolymer, ethylene-butene copolymer, and cellulose.
- Non-aqueous electrolyte a non-aqueous electrolyte solution in which an electrolyte (for example, a lithium salt) is dissolved in a non-aqueous solvent
- Nonaqueous solvents include, for example, ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), dimethyl carbonate (DMC), diethyl carbonate (DEC), ethyl methyl carbonate (EMC), ⁇ -butyrolactone ( ⁇ - BL), sulfolane, acetonitrile, 1,2-dimethoxyethane, 1,3-dimethoxypropane, dimethyl ether, tetrahydrofuran (THF), 2-methyltetrahydrofuran and the like.
- EC ethylene carbonate
- PC propylene carbonate
- BC butylene carbonate
- DMC dimethyl carbonate
- DEC diethyl carbonate
- EMC ethyl methyl carbonate
- Nonaqueous solvents may be used alone or in combination of two or more.
- the electrolyte include lithium perchlorate (LiClO 4 ), lithium hexafluorophosphate (LiPF 6 ), lithium tetrafluoroborate (LiBF 4 ), lithium hexafluoroarsenate (LiAsF 6 ), and trifluoromethanesulfonic acid.
- a lithium salt such as lithium (LiCF 3 SO 3 ) can be given.
- the electrolyte may be used alone or in combination of two or more.
- the amount of electrolyte dissolved in the non-aqueous solvent is preferably 0.2 mol / L to 3 mol / L. If the electrolyte concentration is too low, sufficient ionic conductivity may not be obtained. On the other hand, if it is too high, it may not be completely dissolved in the electrolyte.
- the strip electrode plate is disposed such that the current collector exposed portion is located in the step portion of the roller and the active material-containing layer is located in the recess portion of the roller. Since the tension is applied in the long side direction, the tension can be concentrated on the current collector exposed portion, and the current collector exposed portion can be sufficiently stretched by plastic deformation. Thereby, the distortion and the curvature which arose in the electrode in manufacturing processes, such as a compression molding and a drying process, can be corrected. In addition, it is possible to eliminate problems such as electrode breakage, winding misalignment, wrinkles, cracks, etc. that have occurred in the process of producing a wound electrode group, so that it is possible to manufacture electrodes with excellent quality and production efficiency. Can do.
- the curving correction is not limited to the strip electrode plate that has been compression molded or dried, but is caused by the difference in elongation between the base current collector and the current collector exposed portion of the active material-containing layer. This is effective when warping or distortion occurs.
- the first and second curvature corrections in the third embodiment and the curvature correction in the fourth embodiment can be performed by the same method as the curvature correction according to the first embodiment.
- Example 1 Examples of positive and negative electrodes for lithium ion secondary batteries are shown below.
- LiCoO 2 as a positive electrode active material, graphite powder as a conductive agent, and polyvinylidene fluoride (PVdF) as a binder were mixed and dispersed in an organic solvent to prepare a slurry.
- the obtained slurry was applied to a strip-shaped aluminum foil as a current collector except for both sides of the long side, and then dried to prepare a strip-shaped positive electrode plate.
- Li 4 Ti 5 O 12 as a negative electrode active material, carbon powder as a conductive agent, and polyvinylidene fluoride (PVdF) as a binder were mixed and dispersed in an organic solvent to prepare a slurry.
- the obtained slurry was applied to a strip-shaped aluminum foil as a current collector, excluding both sides of the long side, and then dried to prepare a strip-shaped negative electrode plate.
- Each of the belt-like positive electrode plate and the belt-like negative electrode plate was compressed into a hoop shape by the winding device 23 via the guide roller device 22 after compressing the active material-containing layer with the press device 21 shown in FIG.
- the guide roller 24 3 which also serves as a bending straightening device, the boundary X between the stepped portion 26 and the recess 27, to position the boundary between the current collector exposed portion 25a and the active material-containing layer 25b, and collector-exposed portion 25a
- the active material-containing layer 25 b was disposed in the recess 27 on the stepped portion 26.
- Table 1 shows a step H and a taper R of the step portion 26.
- a tensile tension (winding tension) was applied in the longitudinal direction of each of the belt-like positive electrode plate and the belt-like negative electrode plate from the compression molding step by the press device 21 to the winding device 23 winding the hoop shape.
- Table 1 shows the tensile stress F in the cross section parallel to the short side direction of each of the belt-like positive electrode plate and the belt-like negative electrode plate.
- the heat treatment was not performed in the curvature correction step, and the curvature correction was performed in a room temperature (RT) atmosphere.
- each of the positive electrode plate and the negative electrode plate wound in a hoop shape by the winding device 23 was cut into a length of 1 m, and the amount of distortion was measured.
- the amount of strain is the shortest distance Y 1 between a point parallel to the length L (1 m) of the positive electrode 6 and the most curved portion of the positive electrode 6, as shown in FIG.
- the shortest distance Y 2 between a point parallel to the length L (1 m) of the negative electrode 7 and the most curved portion of the negative electrode 7 is defined as the strain amount. Table 1 shows the measurement results of the strain amount.
- a separator is disposed between the positive electrode and the negative electrode, and a positive electrode current collecting tab made of a current collector exposed portion is protruded from the separator in the winding axis direction of the electrode group, and a current collector exposed portion is formed.
- the negative electrode current collection tab was protruded from the separator in the opposite direction, and wound into a flat shape to produce the electrode group shown in FIG.
- the presence or absence of electrode breakage at the time of winding in the electrode group production process, and further, the produced electrode group was disassembled to investigate whether or not there were electrode misalignment, wrinkles or cracks. The results are shown in Table 2.
- Example 2 to 18 and Comparative Example 1 Similar to Example 1, except that the step H of the step provided on the guide roller, the taper R, the tensile stress F of the strip-like positive and negative plates, and the heating temperature T of the electrode are as shown in Table 1. did. The results are shown in Tables 1 and 2.
- Comparative Example 1 the guide roller was not provided with a step portion, and no electrode distortion or warpage was corrected.
- the heating temperature T is displayed as “RT”, the curvature was corrected in a room temperature (RT) atmosphere.
- Example 13 in which the heating temperature T is 140 ° C., the straightening was performed while heating the positive and negative electrode plates at 140 ° C.
- Example 19 to 21 Similar to Example 1, except that the step H of the step provided on the guide roller, the taper R, the tensile stress F of the strip-like positive and negative plates, and the heating temperature T of the electrode are as shown in Table 1. did. The results are shown in Tables 1 and 2.
- both the positive electrode strain amount and the negative electrode strain amount are smaller than those of Comparative Example 1. Further, according to Examples 1 to 18, there is no electrode breakage during electrode production. On the other hand, in Comparative Example 2, since the active material-containing layer is disposed on the stepped portion, the stress to be concentrated only on the current collector exposed portion is dispersed in the active material-containing layer, and compared with the current collector exposed portion. As a result, the stress was concentrated by the thicker active material containing layer. For this reason, according to Comparative Example 2, the electrode breaks during winding, and there is a winding slip in the electrode group that can be produced without electrode breakage, and the positive and negative electrodes in the electrode group are wrinkled and cracked. It was.
- Example 15 where the level difference H exceeds 600%, the distortion of the positive and negative electrodes is reduced, but when the positive and negative electrodes are wound to produce an electrode group, wrinkles and cracks may occur.
- Example 19 to 21 even when the level difference H exceeds 600%, if the level difference H is less than 750%, the distortion of the positive and negative electrodes is reduced, and there is a problem when winding the positive and negative electrodes. It was also found that no cracks occurred.
- Example 16 From the comparison between Examples 1, 5 to 8, and 16, the positive and negative electrode distortions of Examples 1 and 5 to 8 having a taper R of 15 mm or less are greatly corrected as compared with Example 16 in which the taper R exceeds 15 mm. I understand that In Example 5 in which the taper R is 0.5 mm, the smaller the taper R, the smaller the amount of distortion. However, when the positive and negative electrodes were wound to produce an electrode group, wrinkles and cracks might occur.
- Example 18 From the comparison of Examples 1, 9 to 12, 17, and 18, the positive and negative strains of Examples 1, 9 to 12, and 18 having a tensile stress F of 20 (N / mm 2 ) or more showed a tensile stress F of 20 ( It can be seen that it is greatly corrected as compared with Example 17 of less than N / mm 2 ). In Example 18 where the tensile stress F exceeds 100 in the case where the tensile stress F is larger, in Example 18 where the tensile stress F exceeds 100, wrinkles and cracks may occur when the positive and negative electrodes are wound.
- Example 13 By comparing Example 1 and Example 13, the distortion of the positive and negative electrodes of Example 13 having a heating temperature of 60 ° C. or more and 150 ° C. or less was greatly corrected as compared with Example 1 in which no heat treatment was performed. I understand that.
- the step H (%) of the step provided on the guide roller preferably satisfies the following formula (A) when the thickness of the active material-containing layer per side of the belt-like current collector is 100%.
- step H By setting the step H to be 150% or more and 750% or less, stress can be sufficiently concentrated and extended on the exposed portion of the current collector, so that the warpage and distortion amount of the electrode can be reduced. Therefore, it is possible to prevent the electrode from being broken when the electrode is wound. Further, by setting the step H to 150% or more and less than 750%, it is possible to reduce distortion and warpage generated in the electrode by compression molding, and to prevent the electrode from being wrinkled and cracked when the electrode is wound. Can be suppressed.
- the strip-shaped electrode plate subjected to compression molding has a current collector exposed portion located at a step portion of the roller, and an active material-containing layer at the concave portion of the roller. Since it is placed so that it is positioned and tension is applied in the long side direction of the strip electrode plate, the tension can be concentrated on the current collector exposed portion, and the current collector exposed portion can be sufficiently stretched by plastic deformation. . Thereby, the distortion and the curvature which arose in the electrode by compression molding can be corrected, without increasing the tension
- Example 22 Examples of positive and negative electrodes for lithium ion secondary batteries are shown below.
- LiCoO 2 as a positive electrode active material, graphite powder as a conductive agent, and polyvinylidene fluoride (PVdF) as a binder were mixed and dispersed in an organic solvent to prepare a slurry.
- the obtained slurry was applied to a strip-shaped aluminum foil as a current collector except for both sides of the long side, and then dried.
- the positive electrode plate is cut with a slitting device in the longitudinal direction so that the ratio of the width of the coated part (active material-containing layer) to the uncoated part (current collector exposed part) is 9: 1. I got a plate.
- Li 4 Ti 5 O 12 as a negative electrode active material, carbon powder as a conductive agent, and polyvinylidene fluoride (PVdF) as a binder were mixed and dispersed in an organic solvent to prepare a slurry.
- the obtained slurry was applied to a strip-shaped aluminum foil as a current collector except for both sides of the long side, and then dried.
- the negative electrode plate is cut with a slitting device in the longitudinal direction so that the ratio of the width of the coated part (active material-containing layer) to the non-coated part (current collector exposed part) is 9: 1. I got a plate.
- the active material-containing layer is compressed by the press device 21 shown in FIG. 8 and then wound in a reel shape by the first winding device 23 1 via the guide roller device 22. I took it.
- the guide roller 24 3 which also serves as a bending straightening device, the boundary X between the stepped portion 26 and the recess 27, to position the boundary between the current collector exposed portion 25a and the active material-containing layer 25b, and collector-exposed portion 25a
- the active material-containing layer 25 b was disposed in the recess 27 on the stepped portion 26.
- the step H of the step portion 26 was 300%, and the taper R was 6.5 mm.
- a tensile tension (winding tension) is applied in the longitudinal direction of each of the belt-like positive electrode plate and the belt-like negative electrode plate from the compression molding process by the press device 21 to the reel winding by the first winding device 23 1. It was.
- the tensile stress F in the cross section parallel to the short side direction of each of the belt-like positive electrode plate and the belt-like negative electrode plate was 40 (N / mm 2 ).
- the heat treatment was not performed in the curvature correction step, and the curvature correction was performed in a room temperature (RT) atmosphere.
- each positive electrode plate and negative electrode plate wound on a reel were measured strain.
- the amount of strain is the shortest distance Y 1 between a point parallel to the length L (1 m) of the positive electrode 6 and the most curved portion of the positive electrode 6, as shown in FIG.
- the shortest distance Y 2 between a point parallel to the length L (1 m) of the negative electrode 7 and the most curved portion of the negative electrode 7 is defined as the strain amount.
- a separator is disposed between the positive electrode and the negative electrode for which the strain amount was measured in the third step, and the positive electrode current collecting tab formed of the current collector exposed portion is projected from the separator in the winding axis direction of the electrode group, and The negative electrode current collection tab which consists of an electric-conductor exposed part was protruded from the separator in the opposite direction, and the electrode group shown in FIG. 15 was produced by winding in a flat shape. The frequency of electrode breakage during winding in the electrode group production process was investigated. Further, in the electrode group production process, positive and negative meandering correction was performed by detecting the ends of the positive and negative electrodes with a sensor during winding. The correction amount at that time was defined as the amount of meandering of the electrode.
- Example 3 A positive and negative electrode and an electrode group are manufactured in the same manner as in Example 22 except that no step is provided on the guide roller and no electrode distortion or warpage is corrected, and the amount of distortion, the amount of meander and the frequency of fracture are measured. did.
- the guide roller 24 3 which also serves as a bending straightening device was placed a boundary between the current collector exposed portion 25a and the active material-containing layer 25b. Further, on the stepped portion 26, the entire width of the current collector exposed portion 25a in the short side direction and the active material containing layer 25b having a width equal to the width in the short side direction of the current collector exposed portion 25a were disposed.
- the level difference H, taper R, and tensile stress F of the stepped portion 26 were the same as in Example 22. Further, curvature correction was performed in a room temperature (RT) atmosphere as in Example 22.
- Table 3 shows the results of displaying the strain amount and meandering amount of Example 22 and Comparative Example 4 with the measured value of Comparative Example 3 as 100%, and the fracture frequency of the electrode plates of Example 22 and Comparative Examples 3 and 4. It shows.
- the amount of distortion and meandering amount of both the positive and negative electrodes after the third step are smaller than those of Comparative Example 3, and compared with Example 22 and Comparative Example 4.
- the strain amount of both the positive and negative electrodes is smaller than that of Comparative Example 4 in any of the first to third steps, and the meandering amount at the time of manufacturing the electrode group is smaller than that of Comparative Example 4.
- the frequency of breakage of the positive and negative electrodes when producing the wound electrode group was not found in Example 1 but occasionally occurred in Comparative Examples 3 and 4.
- Example 23 The positive and negative electrodes and the electrode group were produced in the same manner as in Example 22 except that the drying condition in the second step was 10 hours in an atmospheric pressure atmosphere at 150 ° C., and the amount of strain, the amount of meander and the frequency of fracture were measured. .
- Example 5 A positive and negative electrode and an electrode group are manufactured in the same manner as in Example 23 except that no step is provided on the guide roller and no electrode distortion or warpage is corrected, and the amount of distortion, the amount of meander and the frequency of fracture are measured. did.
- Table 4 shows the results of displaying the strain amount and meandering amount of Example 23 and Comparative Example 6 with the measured value of Comparative Example 5 as 100%, and the fracture frequency of the electrode plates of Example 23 and Comparative Examples 5 and 6. It shows.
- Example 23 the amount of strain and meandering of both the positive and negative electrodes after the third step are smaller than those of Comparative Example 5, and also compared with Example 23 and Comparative Example 6.
- the distortion amount of both the positive and negative electrodes is smaller than that of Comparative Example 6 in any of the first to third steps, and the meandering amount when the electrode group is produced is smaller than that of Comparative Example 6.
- the frequency of fracture of the positive and negative electrodes when producing the wound electrode group was none in Example 23, but occasionally occurred in Comparative Examples 5 and 6.
- Example 24 (First step) The first step strip prepared in the same manner as described in the positive electrode plate of Example 22, for each negative electrode plate of the strip, before compression the active material-containing layer in the first press apparatus 211 shown in FIG. 12 After compressing to 90% of the thickness (100% after coating and drying), it was conveyed by guide rollers 24 1 to 24 4 . In the guide roller 24 3 , curvature correction was performed in the same manner as described in Example 22. Thereafter, the amount of strain was measured in the same manner as in Example 22.
- a separator is disposed between the positive electrode and the negative electrode for which the strain amount was measured in the third step, and the positive electrode current collecting tab formed of the current collector exposed portion is projected from the separator in the winding axis direction of the electrode group, and The negative electrode current collection tab which consists of an electric-conductor exposed part was protruded from the separator in the opposite direction, and the electrode group shown in FIG. 15 was produced by winding in a flat shape. The frequency of electrode breakage during winding in the electrode group production process and the amount of meandering of the electrode plate were investigated.
- Example 7 A positive and negative electrode and an electrode group are produced in the same manner as in Example 24 except that no step is provided on the guide roller and no electrode distortion or warpage is corrected, and the amount of distortion, the amount of meander and the frequency of fracture are measured. did.
- Comparative Example 8 Except that the curvature correction performed in the first to third steps is the same as in Comparative Example 4, positive and negative electrodes and an electrode group are manufactured in the same manner as in Example 24, and the amount of distortion, the amount of meander and the frequency of fracture are measured. did.
- Table 5 shows the results of displaying the strain amount and meandering amount of Example 24 and Comparative Example 8 with the measured value of Comparative Example 7 as 100%, and the fracture frequency of the electrode plates of Example 24 and Comparative Examples 7 and 8. It shows.
- the amount of distortion and meandering amount of both positive and negative electrodes after the third step are smaller than those of Comparative Example 7, and compared with Example 24 and Comparative Example 8.
- the distortion amount of both the positive and negative electrodes is smaller than that of Comparative Example 8 in any of the first to third steps, and the meandering amount at the time of preparing the electrode group is smaller than that of Comparative Example 8.
- the frequency of breakage of the positive and negative electrodes in producing the wound electrode group was none in Example 24, but occasionally occurred in Comparative Examples 7 and 8.
- Example 25 Except for setting the step H of the step portion 26 to 600%, positive and negative electrodes and an electrode group were produced in the same manner as in Example 22, and the amount of strain, the amount of meandering, and the frequency of fracture were measured. The results are also shown in Table 3.
- Example 26 Except for setting the step H of the step portion 26 to 740%, positive and negative electrodes and an electrode group were produced in the same manner as in Example 22, and the amount of strain, the amount of meandering, and the frequency of fracture were measured. The results are also shown in Table 3.
- the step H (%) of the step provided on the guide roller preferably satisfies the following formula (A) when the thickness of the active material-containing layer per side of the belt-like current collector is 100%.
- step H By setting the step H to be 150% or more and 750% or less, stress can be sufficiently concentrated and extended on the exposed portion of the current collector, so that the warpage and distortion amount of the electrode can be reduced. Therefore, it is possible to prevent the electrode from being broken when the electrode is wound. In addition, by setting the step H to 150% or more and less than 750%, it is possible to reduce the distortion and warpage generated in the electrode by compression molding, and to suppress the breakage of the electrode when the electrode is wound. Can do.
- the embodiments and examples have been described above, but are not limited to those described.
- the ratio between the coated part and the uncoated part, the compression density of the electrode plate, or the influence of the second process The same effect can be obtained by appropriately changing the shape, tensile stress, and the like.
- the active material paste can be applied continuously or intermittently, and the same effect can be obtained.
- the current collecting base material of the electrode is not limited to the aluminum foil, and its material, thickness, tension, etc. The same effect can also be obtained by appropriately changing the height and shape of the step, the tensile stress, etc. according to the strength and hardness.
- the current collector exposed portion is positioned at the stepped portion of the roller and the active material containing layer is positioned at the concave portion of the roller,
- tension in the long side direction distortion and curvature generated in the electrode are corrected.
- tension can be concentrated on the current collector exposed portion, and the current collector exposed portion can be sufficiently deformed by plastic deformation.
- SYMBOLS 1 ... Exterior can, 2 ... Cover, 3 ... Positive electrode output terminal, 4 ... Negative electrode output terminal, 5 ... Electrode group, 6 ... Positive electrode, 6a ... Positive electrode current collection tab, 6b ... Positive electrode active material containing layer, 7 ... Negative electrode, 7a DESCRIPTION OF SYMBOLS ... Negative electrode current collection tab, 7b ... Negative electrode active material containing layer, 8 ... Separator, 9 ... Safety valve, 9a ... Recessed part, 9b ... Groove part, 10 ... Injection hole, 11 ... Positive electrode lead, 12 ... Negative electrode lead, 21 ... Press apparatus , 21 1, 21 2 ... first, second press device, 21a, 21b ...
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Abstract
Description
図1は、電極の製造に用いるプレス装置、ガイドローラ装置、及び、巻取り装置を示す模式図である。図2は、湾曲矯正工程におけるガイドローラと帯状極板との位置関係を示す模式図である。図2の(a)は、ガイドローラ上を走行している帯状極板をガイドローラ側から見た平面図であり、図2の(b)はガイドローラを回転軸に平行に裁断することにより得られる断面図である。図3の(a)は、段部のコーナーにテーパーが形成されたガイドローラを回転軸に平行に切断した際に得られる断面図で、図3の(b)は、図3の(a)に示すガイドローラに帯状極板を配置した状態を示す断面図である。図4の(a)は、ガイドローラ上を走行している帯状極板をガイドローラ側から見た平面図であり、図4の(b)はガイドローラを回転軸に平行に裁断することにより得られる断面図である。
段差Hを150%以上にすることによって、集電体露出部に応力を十分に集中させて伸ばすことができる。また、段差Hを600%以下にすることによって、活物質含有層25bと集電体露出部25aとの境界付近に皺及び亀裂が生じるのを抑えることができる。これらの皺や亀裂は、後工程において電極破断や溶接不良の原因になる恐れがある。従って、段差Hを150%以上600%以下にすることによって、活物質含有層25bと集電体露出部25aとの境界付近に皺及び亀裂が生じるのを抑えつつ、集電体露出部に応力を十分に集中させて伸ばすことができる。皺や亀裂を防止する効果を高めるには、200≦H≦400の範囲がより好ましい。
第2の実施形態によれば、正極と、負極と、非水電解質とを備える電池の製造方法が提供される。正極及び負極のうち少なくとも一方の電極は、第1の実施形態に係る方法で製造される。図5は、第2の実施形態に係る方法で製造される非水電解質電池の展開斜視図である。図6は、図5示す電池で用いられる電極群の部分展開斜視図である。
第3の実施形態によれば、帯状極板の作製、圧縮成形、第1の湾曲矯正、乾燥、及び第2の湾曲矯正を含む電極の製造方法を提供することができる。
まず、帯状極板25を作製する。帯状極板25は、図9の(a)及び図10の(b)に示すように、帯状集電体と、帯状集電体の一方の長辺に形成され、両面共に活物質含有層が存在しない集電体露出部25aと、帯状集電体の集電体露出部25a以外の箇所に両面とも形成された活物質含有層25bとを含む。活物質含有層25bは、帯状集電体の長辺方向に連続的に形成されている。短辺方向の幅は、活物質含有層25bの方が集電体露出部25aよりも広くなっている。帯状極板25は、例えば、活物質含有スラリーを帯状集電体に一方の長辺を除いて両面に塗布し、乾燥することにより得られる。あるいは、活物質含有スラリーを集電体の両面に部分的に塗布し、乾燥した後、集電体露出部となる未塗布部が長辺に位置するように裁断することにより帯状極板25を得る。
次いで、得られた帯状極板25を、図8に示す矢印方向に回転しているプレスロール21a,21b間に挿入し、圧縮成形を施す。帯状極板25の挿入方向が帯状極板25の長手方向に平行であるため、プレス圧力は、活物質含有層25bに主に加わり、活物質含有層25bが圧縮成形され、密度が高められる。集電体露出部25aには、プレス圧力がほとんど加わらないため、活物質含有層25bの下地集電体に比して伸びが小さくなる。その結果、帯状極板25に歪みや反りが生じる。
プレスロール21a,21b間を通過した帯状極板25は、ガイドローラ241~245を経由して第1の巻取り装置231まで搬送される。湾曲矯正装置を兼ねたガイドローラ243では、図9及び図10に示すように、段部26と凹部27との境界Xに、集電体露出部25aと活物質含有層25bとの境界が位置し、集電体露出部25aのみが段部26上に配置される。活物質含有層25bは、凹部27に配置される。これにより、帯状極板25の搬送方向(長手方向)に加わる巻取り張力を、集電体露出部25aに集中させることができる。その結果、集電体露出部25aを巻取り張力によって十分に伸ばすことができるため、帯状極板25に生じた歪み及び反りを矯正することができる。ガイドローラ243を通過した帯状極板25は、ガイドローラ244,245を経由して第1の巻取り装置231に巻き取られる。
段差Hを150%以上にすることによって、集電体露出部に応力を十分に集中させて伸ばすことができる。また、段差Hを600%以下にすることによって、活物質含有層25bと集電体露出部25aとの境界付近に皺及び亀裂が生じるのを抑えることができる。これらの皺や亀裂は、後工程において電極破断や溶接不良の原因になる恐れがある。従って、段差Hを150%以上600%以下にすることによって、活物質含有層25bと集電体露出部25aとの境界付近に皺及び亀裂が生じるのを抑えつつ、集電体露出部に応力を十分に集中させて伸ばすことができる。皺や亀裂を防止する効果を高めるには、200≦H≦400の範囲がより好ましい。
第1の巻取り装置231によりリール状に巻き取られた帯状極板25に乾燥処理が施される。乾燥処理は、100℃以上180℃以下の真空、減圧もしくは大気圧雰囲気で行うことが望ましい。雰囲気の温度を100℃以上にすることにより、帯状極板25からの水分除去を促進することができる。また、180℃以下とすることによって、活物質含有層に含まれる材料の熱劣化を防止することができる。よって、雰囲気の温度を100℃以上180℃以下の範囲にすることによって、活物質含有層に含まれる材料の熱劣化を防止しつつ、帯状極板25からの水分除去を促進することができる。
第2の湾曲矯正は、図12に示す装置を用いて行われる。図12に示すように、製造工程の前段側から後段に向かって繰出し装置28、複数の金属製ガイドローラ241~244、第2の巻取り装置29が配置されている。繰出し装置28は、駆動部(図示しない)によって回転軸28aが図12に示す矢印の方向に回転することで、リール状に巻かれた帯状極板25が搬送方向に繰り出されるようになっている。第2の巻取り装置29は、駆動部(図示しない)によって回転軸29aが図12に示す矢印の方向に回転することで、帯状極板25がリール状に巻き取られるようになっている。複数のガイドローラ241~244は、帯状極板25に巻き取りに必要な張力が掛かるように、帯状極板25の上下面に交互に配置されている。ガイドローラ241~244には、第1の湾曲矯正で説明したのと同様なものが用いられ、ガイドローラ243が湾曲矯正装置を兼ねている。
第4の実施形態によれば、帯状極板の圧縮成形と、湾曲矯正とを含む電極の製造方法を提供することができる。
第5の実施形態によれば、正極と、負極と、非水電解質とを備える電池の製造方法が提供される。正極及び負極のうち少なくとも一方の電極は、第3~第4の実施形態に係るいずれかの方法で製造される。図14は、第3の実施形態に係る方法で製造される非水電解質電池の展開斜視図である。図15は、図14に示す電池で用いられる電極群の部分展開斜視図である。
以下に、リチウムイオン二次電池用の正極および負極の実施例を示す。
ガイドローラに設ける段部の段差H、テーパーR、帯状の正負極板の引張応力F、さらに電極の加熱温度Tの条件を表1に示した様にすること以外は、実施例1と同様にした。結果を表1、2に示す。なお、比較例1では、ガイドローラに段部を設けず、電極の歪み、反りの矯正を一切行わなかった。また、加熱温度Tが「RT」と表示されているものは、室温(RT)雰囲気で湾曲矯正を行った。加熱温度Tに140℃と記載されている実施例13では、正負極板に140℃の加熱処理を施しながら湾曲矯正を行った。
湾曲矯正装置を兼ねたガイドローラ243の段部26上に集電体露出部25aと活物質含有層25bとの境界を位置させ、かつ段部26上に、集電体露出部25aの短辺方向の幅分全てと、集電体露出部25aの短辺方向幅と等しい幅分の活物質含有層25bとを配置すること以外は、実施例1と同様にした。結果を表1、2に示す。
ガイドローラに設ける段部の段差H、テーパーR、帯状の正負極板の引張応力F、さらに電極の加熱温度Tの条件を表1に示した様にすること以外は、実施例1と同様にした。結果を表1、2に示す。
段差Hを150%以上750%以下にすることによって、集電体露出部に応力を十分に集中させて伸ばすことができるため、電極の反り及び歪み量を少なくすることができる。従って、電極を捲回した際の電極の破断を防止することができる。また、段差Hを150%以上750%未満にすることによって、圧縮成形で電極に生じた歪み及び反りを少なくすることができると共に、電極を捲回した際に電極に皺及び亀裂が生じるのを抑えることができる。
以下に、リチウムイオン二次電池用の正極および負極の実施例を示す。
正極活物質としてLiCoO2と、導電剤として黒鉛粉末と、結着剤としてポリフッ化ビニリデン(PVdF)とを混合し、これらを有機溶媒に分散させ、スラリーを調製した。得られたスラリーを集電体としての帯状アルミニウム箔に長辺一辺の両面を除いて塗布した後、乾燥した。ひきつづき、スリット装置で正極板をその長手方向に塗布部(活物質含有層)と未塗布部(集電体露出部)との幅の比率が9:1になるように裁断し、帯状の正極板を得た。
第1の工程後のリール状の正極板及び負極板に乾燥処理をそれぞれ施した。乾燥条件は、150℃の真空雰囲気で10時間とした。その後、リール状の正極板及び負極板それぞれから、1mの長さ分を切り出し、第1の工程で説明したのと同様にして歪み量を計測した。
リール状の正極板及び負極板それぞれについて、図12に示す繰出し装置28を用いて繰り出し、ガイドローラ241~242を経由してガイドローラ243に搬送した。ガイドローラ243では、第1の工程で説明したのと同様にして湾曲矯正を行った。その後、リール状の正極板及び負極板それぞれから、1mの長さ分を切り出し、第1の工程で説明したのと同様にして歪み量を計測した。
ガイドローラに段部を設けず、電極の歪み、反りの矯正を一切行わないこと以外は、実施例22と同様にして正負極及び電極群を製造し、歪み量、蛇行量及び破断頻度を測定した。
第1の工程と第3の工程で行われる湾曲矯正を下記のように変更すること以外は、実施例22と同様にして正負極及び電極群を製造し、歪み量、蛇行量及び破断頻度を測定した。
第二の工程における乾燥条件を150℃の大気圧雰囲気で10時間とすること以外は、実施例22と同様にして正負極及び電極群を製造し、歪み量、蛇行量及び破断頻度を測定した。
ガイドローラに段部を設けず、電極の歪み、反りの矯正を一切行わないこと以外は、実施例23と同様にして正負極及び電極群を製造し、歪み量、蛇行量及び破断頻度を測定した。
第1の工程と第3の工程で行われる湾曲矯正を比較例4と同様にすること以外は、実施例23と同様にして正負極及び電極群を製造し、歪み量、蛇行量及び破断頻度を測定した。
(第1の工程)
実施例22の第1の工程で説明したのと同様にして作製した帯状の正極板、帯状の負極板それぞれについて、図12に示す第1のプレス装置211で活物質含有層を圧縮前の厚さ(塗布・乾燥後を100%とする)の90%になるまで圧縮した後、ガイドローラ241~244により搬送した。ガイドローラ243では、実施例22で説明したのと同様にして湾曲矯正を行った。その後、実施例22と同様にして歪み量を測定した。
第1の工程で歪み量を測定した後、第2のプレス装置212で活物質含有層を圧縮前の厚さ(塗布・乾燥後を100%とする)の80%になるまで圧縮した。第2のプレス装置212を通過した帯状極板25に実施例22で説明したのと同様にして湾曲矯正を行った。その後、実施例22と同様にして歪み量を測定した。
第2の工程で歪み量を測定した後、第1、第2のプレス装置と同様な構成の第3のプレス装置で活物質含有層を圧縮前の厚さ(塗布・乾燥後を100%とする)の75%になるまで圧縮した。第3のプレス装置を通過した帯状極板に実施例22で説明したのと同様にして湾曲矯正を行った。その後、実施例22と同様にして歪み量を測定した。
ガイドローラに段部を設けず、電極の歪み、反りの矯正を一切行わないこと以外は、実施例24と同様にして正負極及び電極群を製造し、歪み量、蛇行量及び破断頻度を測定した。
第1~第3の工程で行われる湾曲矯正を比較例4と同様にすること以外は、実施例24と同様にして正負極及び電極群を製造し、歪み量、蛇行量及び破断頻度を測定した。
段部26の段差Hを600%にすること以外は、実施例22と同様にして正負極及び電極群を製造し、歪み量、蛇行量及び破断頻度を測定した。その結果を表3に併記する。
段部26の段差Hを740%にすること以外は、実施例22と同様にして正負極及び電極群を製造し、歪み量、蛇行量及び破断頻度を測定した。その結果を表3に併記する。
段差Hを150%以上750%以下にすることによって、集電体露出部に応力を十分に集中させて伸ばすことができるため、電極の反り及び歪み量を少なくすることができる。従って、電極を捲回した際の電極の破断を防止することができる。また、段差Hを150%以上750%未満にすることによって、圧縮成形で電極に生じた歪み及び反りを少なくすることができると共に、電極を捲回した際に電極に破断が生じるのを抑えることができる。
Claims (16)
- 帯状集電体と、前記帯状集電体の少なくとも一方の長辺に形成され、両面共に活物質含有層が存在しない集電体露出部と、前記帯状集電体の前記集電体露出部以外の少なくとも一部に形成された活物質含有層とを含む帯状極板の前記活物質含有層に、圧縮成形を施す工程と、
円周面から突出した段部と、前記段部に隣接する凹部とを有するローラ上に、前記帯状極板を、前記集電体露出部が前記段部に位置し、かつ前記活物質含有層が前記凹部に位置するように配置し、前記帯状極板の長辺方向に張力を加える工程と
を含むことを特徴とする電極の製造方法。 - 前記段部の段差が下記(A)式を満たすことを特徴とする請求項1記載の電極の製造方法。
150≦H≦750 (A)
但し、Hは、前記電極の前記活物質含有層の帯状集電体片面当たりの厚さを100%とした際の前記段差の大きさ(%)である。 - 前記段部の段差が下記(1)式を満たすことを特徴とする請求項1記載の電極の製造方法。
150≦H≦600 (1)
但し、Hは、前記電極の前記活物質含有層の帯状集電体片面当たりの厚さを100%とした際の前記段差の大きさ(%)である。 - 前記段部のテーパーR(mm)を、R≦15とすることを特徴とする請求項2または3いずれか1項記載の電極の製造方法。
- 前記張力を加える工程での前記帯状極板の引張応力F(N/mm2)が、20≦F≦100を満たすことを特徴とする請求項2または3いずれか1項記載の電極の製造方法。
- 前記張力を加える工程では、前記帯状極板に60℃以上150℃以下の温度で加熱処理が施されることを特徴とする請求項5記載の電極の製造方法。
- 前記活物質含有層は、前記帯状集電体の長手方向に連続的もしくは間欠的に形成されていることを特徴とする請求項2または3いずれか1項記載の電極の製造方法。
- 前記帯状集電体は、アルミニウム箔、アルミニウム合金箔または銅箔であることを特徴とする請求項2または3いずれか1項記載の電極の製造方法。
- 正極と、負極と、非水電解質とを備える電池の製造方法であって、
前記正極及び前記負極のうち少なくとも一方の電極が、請求項1~8いずれか1項記載の方法で製造されることを特徴とする電池の製造方法。 - 帯状集電体と、前記帯状集電体の少なくとも一方の長辺に形成され、両面共に活物質含有層が存在しない集電体露出部と、前記帯状集電体の前記集電体露出部以外の少なくとも一部に形成された活物質含有層とを含む電極の製造方法であって、
円周面から突出した段部と、前記段部に隣接する凹部とを有するローラ上に、前記集電体露出部が前記段部に位置し、かつ前記活物質含有層が前記凹部に位置するように配置し、前記帯状集電体の長辺方向に張力を加える工程
を含むことを特徴とする電極の製造方法。 - 前記張力を加える工程は、活物質含有層を圧縮成形する工程の後に行われることを特徴とする請求項10記載の電極の製造方法。
- 前記張力を加える工程の後に乾燥工程が行われ、前記乾燥工程の後、前記張力を加える工程が再度行われることを特徴とする請求項11記載の電極の製造方法。
- 前記張力を加える工程と、前記活物質含有層を圧縮成形する工程とが交互に行われることを特徴とする請求項11記載の電極の製造方法。
- 前記活物質含有層は、前記帯状集電体の長手方向に連続的もしくは間欠的に形成されていることを特徴とする請求項12または13いずれか1項記載の電極の製造方法。
- 前記帯状集電体は、アルミニウム箔、アルミニウム合金箔または銅箔であることを特徴とする請求項12または13いずれか1項記載の電極の製造方法。
- 正極と、負極と、非水電解質とを備える電池の製造方法であって、
前記正極及び前記負極のうち少なくとも一方の電極が、請求項10~15いずれか1項記載の方法で製造されることを特徴とする電池の製造方法。
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- 2012-02-17 CN CN201280004055.9A patent/CN103250277B/zh active Active
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2013
- 2013-08-16 US US13/969,047 patent/US10038179B2/en active Active
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2018
- 2018-06-22 US US16/016,314 patent/US20180301688A1/en not_active Abandoned
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Cited By (11)
Publication number | Priority date | Publication date | Assignee | Title |
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JP2013069637A (ja) * | 2011-09-26 | 2013-04-18 | Nissan Motor Co Ltd | 帯状電極の製造装置および製造方法 |
JP2013073690A (ja) * | 2011-09-26 | 2013-04-22 | Toshiba Corp | 電極のプレス装置、電極の製造装置及び電極の製造方法 |
JP2014116141A (ja) * | 2012-12-07 | 2014-06-26 | Toyota Motor Corp | 帯状電極の製造方法 |
JP2014167859A (ja) * | 2013-02-28 | 2014-09-11 | Toyota Industries Corp | 電極の製造装置、及び電極の製造方法 |
CN103258997A (zh) * | 2013-04-08 | 2013-08-21 | 内蒙古稀奥科镍氢动力电池有限公司 | 一种消除电池极板应力的方法 |
CN103258997B (zh) * | 2013-04-08 | 2015-02-25 | 内蒙古稀奥科镍氢动力电池有限公司 | 一种消除电池极板应力的方法 |
JP2017084697A (ja) * | 2015-10-30 | 2017-05-18 | 三洋電機株式会社 | 電極板の製造方法及び二次電池の製造方法 |
US10553852B2 (en) | 2015-10-30 | 2020-02-04 | Sanyo Electric Co., Ltd. | Method for manufacturing electrode and method for manufacturing secondary battery |
JP2017142915A (ja) * | 2016-02-08 | 2017-08-17 | トヨタ自動車株式会社 | 捲回電極体の製造方法 |
JP2021163688A (ja) * | 2020-04-02 | 2021-10-11 | トヨタ自動車株式会社 | 電極板の製造方法 |
JP7413900B2 (ja) | 2020-04-02 | 2024-01-16 | トヨタ自動車株式会社 | 電極板の製造方法 |
Also Published As
Publication number | Publication date |
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US20130326865A1 (en) | 2013-12-12 |
CN103250277B (zh) | 2016-02-17 |
US20180301688A1 (en) | 2018-10-18 |
EP2677567A4 (en) | 2014-11-05 |
EP2677567A1 (en) | 2013-12-25 |
JPWO2012111815A1 (ja) | 2014-07-07 |
JP5596183B2 (ja) | 2014-09-24 |
CN103250277A (zh) | 2013-08-14 |
US10038179B2 (en) | 2018-07-31 |
EP2677567B1 (en) | 2018-06-13 |
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