WO2014122847A1 - 非水電解液二次電池,非水電解液二次電池の正極板の製造方法,および非水電解液二次電池の製造方法 - Google Patents
非水電解液二次電池,非水電解液二次電池の正極板の製造方法,および非水電解液二次電池の製造方法 Download PDFInfo
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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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- 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
- H01M10/052—Li-accumulators
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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
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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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
- H01M10/0587—Construction or manufacture of accumulators having only wound construction elements, i.e. wound positive electrodes, wound negative electrodes and wound separators
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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
- H01M4/0411—Methods of deposition of the material by extrusion
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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
- H01M4/0471—Processes of manufacture in general involving thermal treatment, e.g. firing, sintering, backing particulate active material, thermal decomposition, pyrolysis
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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
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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
- H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M4/139—Processes of manufacture
- H01M4/1391—Processes of manufacture of electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
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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
- H01M4/1393—Processes of manufacture of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
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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
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/362—Composites
- H01M4/366—Composites as layered products
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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
- H01M2004/021—Physical characteristics, e.g. porosity, surface area
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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
- Y10T29/49117—Conductor or circuit manufacturing
Definitions
- the present invention relates to a non-aqueous electrolyte secondary battery having an electrode winding body and a method for manufacturing the same, particularly a method for manufacturing the positive electrode plate. More specifically, the non-aqueous electrolyte secondary battery and the non-aqueous electrolyte secondary battery are designed to prevent elution of metal components at the width direction end of the mixture layer in the outermost peripheral portion of the electrode winding body.
- the present invention relates to a method for manufacturing a positive electrode plate and a method for manufacturing a non-aqueous electrolyte secondary battery.
- an electrode winding body in which a positive electrode plate and a negative electrode plate are wound with a separator interposed therebetween has been used.
- the electrode plate in this type of non-aqueous electrolyte secondary battery is obtained by forming a mixture layer of an electrode active material on a current collector plate (metal foil).
- a mixture paste obtained by kneading a powder of an electrode active material and other components of the mixture layer together with a solvent is generally used. That is, a mixture paste, which is a fluid, is applied to a current collector plate and dried to form a mixture layer.
- the conventional techniques described above have the following problems. That is, at the end portion of the resulting mixture layer, a thin layer region in which the surface is inclined and the layer thickness is inevitably formed due to the fluidity and surface tension of the mixture paste is formed. This thin layer region causes a problem that the battery capacity of the nonaqueous electrolyte secondary battery cannot be obtained sufficiently. In this thin layer region, the metal element is further eluted by a local potential increase during charging. The elution of metal elements becomes a problem particularly at the end of the positive electrode mixture layer. As shown in the schematic cross-sectional view of FIG. 1, the negative electrode mixture layer 21 is usually formed wider than the positive electrode mixture layer 31 in the electrode winding body of this type of non-aqueous electrolyte secondary battery.
- lithium ions diffuse into the negative electrode mixture layer 21 formed wider than the positive electrode mixture layer 31 (arrow A). This is because the amount of lithium ions released per unit active material amount increases in the thin layer region 31R at the end.
- the separator is indicated by the number “4”.
- the present invention has been made in order to solve the problems of the conventional techniques described above.
- the problem is to manufacture a non-aqueous electrolyte secondary battery and a positive electrode plate for a non-aqueous electrolyte secondary battery that can effectively prevent problems due to the thin layer region at the end of the mixture layer.
- the present invention provides a method and a method for manufacturing a non-aqueous electrolyte secondary battery.
- a nonaqueous electrolyte secondary battery is a nonaqueous electrolyte secondary battery having an electrode winding body in which a positive electrode plate and a negative electrode plate are wound with a separator interposed therebetween,
- the outermost electrode plate of the wound body is a negative electrode plate
- the cross-sectional shape of the end portion in the width direction of the mixture layer on the outer surface side of the outermost periphery portion of the positive electrode plate is the flat portion at the center in the width direction of the mixture layer.
- the width of the portion having a thickness of 50% or less of the thickness is a steep sectional shape having a width of 100 ⁇ m or less.
- the manufacturing method of the positive electrode plate of the non-aqueous electrolyte secondary battery which concerns on the 2nd aspect of this invention is a non-aqueous electrolyte solution which has an electrode winding body formed by winding up a positive electrode plate and a negative electrode plate through a separator.
- a method for producing a positive electrode plate of a secondary battery comprising: a coating step of applying a positive electrode mixture paste to a current collector plate to form a mixture layer;
- the cross-sectional shape of the end portion in the width direction is at least 50% of the thickness of the flat portion at the center in the width direction of the mixture layer in at least the outermost peripheral region on the surface side that is the outer surface side of the electrode winding body.
- a method of applying a steep cross-sectional shape in which a width of a certain portion is 100 ⁇ m or less is an application target.
- the coating process prior to the coating process, at least the electrode winding body in the longitudinal direction of the current collector plate on the outer surface side of the outermost peripheral region, which is the outermost peripheral range, the ratio NA / wetability value NA of the widthwise end portion that becomes the non-coated portion and the wettability value NB of the widthwise central portion that becomes the coated portion NB 0.5 ⁇ NA / NB ⁇ 1
- a wettability adjustment process is performed to adjust so as to be.
- the steep cross-sectional shape of the end portion in the width direction of the mixture layer is realized. This is because the positive electrode mixture paste is uniformly applied to the coated portion having high wettability, while the positive electrode mixture paste is repelled in the non-coated portion having low wettability.
- the process of reducing the wettability of the current collector plate in the width direction and the process of improving the wettability of the current collector plate in the width direction is performed.
- the process for reducing wettability include an oil application process or a water repellent application process.
- the treatment for improving the wettability include corona discharge treatment, surface roughening treatment, and solvent washing treatment.
- the wettability adjustment process may be performed over the entire longitudinal direction of the current collector plate, or may be performed only on the outermost periphery of the electrode winding body in the entire longitudinal direction of the current collector plate.
- a positive electrode mixture paste having a TI value, which is a ratio to the viscosity at 1 is in the range of 1.7 to 4.6.
- the steep cross-sectional shape of the width direction edge part of the above-mentioned mixture layer is implement
- the method for manufacturing the positive electrode plate of the nonaqueous electrolyte secondary battery it is desirable to perform a drying step of drying the mixture layer formed in the coating step. And in the entrance side of a drying process, it is desirable to make the width direction edge part of a mixture layer temperature lower than the width direction center part. This is because drying can proceed while suppressing a decrease in viscosity due to a temperature rise at the end in the width direction of the mixture layer.
- the back side of the current collector plate after the coating process is supported by a supporting roller, and as the supporting roller, an end cooling roller having a cooling section at the end in the width direction and a non-cooling section therebetween is used. be able to.
- a central heating roller having a heating section at the center in the width direction and both ends being non-heating sections can be used as the carrying roller.
- the positive electrode plate produced by any one of the production methods described above is used together with the negative electrode plate and the separator, and the positive electrode plate and the negative electrode plate are wound through the separator.
- a winding step for forming an electrode winding body is performed.
- the electrode plate on the outermost periphery of the electrode winding body is used as a negative electrode plate, and a portion having a steep cross-sectional shape at the end in the width direction of the mixture layer is disposed on at least the outer peripheral side of the positive electrode plate.
- a method for manufacturing a non-aqueous electrolyte secondary battery is provided.
- the battery 1 is a lithium ion secondary battery.
- the battery 1 of FIG. 2 is a battery container 2 in which an electrode winding body 3 is accommodated.
- the battery container 2 is a member that forms the outer shape of the battery 1.
- the battery container 2 includes a container body 24 and a lid member 5.
- External terminal plates 6 and 7 are attached to the lid member 5.
- Bolts 8 and 9 are fixed by external terminal plates 6 and 7.
- Insulating members 10 and 15 are disposed between the external terminal plates 6 and 7 and the lid member 5.
- the lid member 5 in the battery 1 is provided with a liquid injection port 23.
- the electrode winding body 3 is obtained by winding a positive electrode plate, a negative electrode plate, and a separator. Further, the electrode winding body 3 is impregnated with an electrolytic solution.
- the electrode winding body 3 is a power generation element in the battery 1.
- a region 20 where only the negative electrode plate exists and a region 30 where only the positive electrode plate exists are provided at both ends of the electrode winding body 3 in the direction parallel to the winding axis direction.
- the region 20 and the external terminal board 6 are connected by the current collecting member 13. Further, the region 30 and the external terminal plate 7 are connected by the current collecting member 12.
- the electrode winding body 3 will be further described.
- the electrode winding body 3 is obtained by winding a negative electrode plate 22 and a positive electrode plate 32 as shown in the schematic cross-sectional view of FIG.
- the separator is wound together with the positive electrode plate 32 and the negative electrode plate 22, but in FIG. 3, the separator is omitted and the electrode winding body 3 is drawn.
- the separator 4 shown in FIG. 1 is always interposed between the negative electrode plate 22 and the positive electrode plate 32, and the positive electrode plate 32 and the negative electrode plate 22 are not in direct contact with each other. Absent.
- the negative electrode plate 22 is located on the outermost periphery of the electrode winding body 3.
- the actual outermost layer in the electrode winding body 3 is a separator, but when referring to the “outermost periphery”, only the positive electrode plate 32 and the negative electrode plate 22 are considered without considering the separator.
- a portion from the outermost end 32 ⁇ / b> A to a portion 32 ⁇ / b> B that is one circumference inside the outermost end 32 ⁇ / b> A is referred to as an outermost peripheral portion 32 ⁇ / b> C of the positive electrode plate 32. This is because the positive electrode plate 32 does not exist further outside the outermost peripheral portion 32C.
- the outermost peripheral portion 32 ⁇ / b> C of the positive electrode plate 32 exists immediately inside the portion of the outermost peripheral portion of the negative electrode plate 22.
- each of the positive electrode plate 32 and the negative electrode plate 22 is obtained by forming a mixture layer of an electrode active material on a current collector plate (metal foil) by applying a paste.
- the electrode winding body 3 of the present embodiment is the same as in FIG. 1 in that the mixture layer of the negative electrode plate 22 is wider than the mixture layer of the positive electrode plate 32. However, the difference in width is slight.
- the width of the mixture layer in the electrode winding body 3 is the size of the mixture layer in the left-right direction in FIG.
- FIG. 4 shows a cross-sectional view of the positive electrode plate 32 of this embodiment.
- 4 is a cross-sectional view of the positive electrode plate 32 in the CC direction in FIG.
- the left-right direction in FIG. 4 corresponds to the left-right direction in FIG.
- the positive electrode plate 32 is obtained by forming a positive electrode mixture layer 31 on the surface of a current collector plate 33 made of aluminum.
- the positive electrode mixture layer 31 is drawn only on one side of the current collector plate 33, but actually the positive electrode mixture layer 31 exists on both sides of the current collector plate 33.
- the positive electrode mixture layer 31 is not formed on the entire surface of the current collector plate 33. In the vicinity of the right end in FIG. 4, there is an uncoated portion 34 where the positive electrode mixture layer 31 is not formed. In the non-coating portion 34, the positive electrode mixture layer 31 is not formed on both the front and back surfaces, and the surface of the current collector plate 33 is exposed. There is no non-coated portion 34 on the left end side in FIG. Therefore, the positive electrode mixture layer 31 is formed on the entire surface and both surfaces of the positive electrode plate 32 except for the non-coated portion 34 on the right end side in FIG. The portion where the positive electrode mixture layer 31 is formed is located in a region between the region 20 and the region 30 in the electrode winding body 3 in FIG. On the other hand, the part of the non-coating part 34 is located in the area
- a thin layer region 31 ⁇ / b> R whose surface is inclined and the layer thickness is thin is present in the vicinity of the boundary with the non-coated portion 34 in the positive electrode mixture layer 31.
- a portion having a flat surface and a uniform thickness other than the thin layer region 31R in the positive electrode mixture layer 31 is referred to as a flat region 31F.
- the layer thickness of the flat region 31F in the positive electrode mixture layer 31 is represented by “T”.
- a portion where the layer thickness is less than half the layer thickness T of the flat region 31F is referred to as a tip region 31S.
- the width is represented by “L”.
- the width L of the tip region 31S is suppressed to a very small value of 100 ⁇ m or less at least on the outer surface side of the outermost peripheral portion 32C.
- the cross-sectional shape of the end portion in the width direction of the positive electrode mixture layer 31 is a steep cross-sectional shape with a small width of the tip region 31S.
- the negative electrode plate 22 of this embodiment also has substantially the same configuration as the positive electrode plate 32 shown in FIG.
- the current collector is made of copper instead of aluminum.
- the material of the mixture layer is also different.
- the non-coated portion of the negative electrode plate 22 is disposed in the electrode winding body 3 in the direction opposite to the non-coated portion 34 of the positive electrode plate 32 and is located in the region 20 in FIG. Further, the negative electrode mixture layer does not need to satisfy the condition of the width of the tip region as in the positive electrode mixture layer 31.
- the positive electrode plate 32 is manufactured by applying the positive electrode active material mixture paste to the aluminum foil as the current collector plate 33 to form the positive electrode mixture layer 31.
- the positive electrode plate 32 is manufactured by applying the positive electrode active material mixture paste to the aluminum foil as the current collector plate 33 to form the positive electrode mixture layer 31.
- the method of performing surface treatment on the current collector plate 33 in advance will be described as a first embodiment and will be described below.
- the aluminum foil current collector plate 33 has wettability between the portion where the positive electrode mixture layer 31 is to be formed and the portion where the non-coated portion 34 is to be formed prior to the coating treatment. Process to make a difference.
- the wettability of the portion where the positive electrode mixture layer 31 is to be formed is increased, and the wettability of the portion which is to be the non-coated portion 34 is decreased. This prevents the mixture paste applied on the portion where the positive electrode mixture layer 31 is to be formed from flowing and moving onto the portion where the non-coated portion 34 is to be formed.
- the width L of the tip region 31S of the positive electrode mixture layer 31 to be formed becomes large. Even if the mixture paste is applied only on the portion where the positive electrode mixture layer 31 is to be formed, the coated mixture paste flows on the portion where the non-coated portion 34 should flow. Will move to. For this reason, the amount of the mixture per area is small in the vicinity of the edge of the positive electrode mixture layer 31. On the other hand, if the wettability of the portion where the positive electrode mixture layer 31 is to be formed is low, there is an adverse effect that pinholes are easily generated in the positive electrode mixture layer 31. By adding a difference in wettability to the surface of the current collector plate 33 as described above, the positive electrode material mixture layer 31 having a good tip shape and no pinholes is formed.
- regions 134 with low wettability are provided at both ends in the width direction (left-right direction in FIG. 5) of the long strip-shaped aluminum foil 133 to be the current collector plate 33.
- a portion between the region 134 and the region 134, that is, a central portion in the width direction of the aluminum foil 133 is defined as a region 135 having high wettability.
- the positive electrode mixture layer 31 is formed on the region 135, and the region 134 becomes the non-coated portion 34.
- Such a division between the region 134 and the region 135 may be performed on both the front and back surfaces of the aluminum foil 133 serving as the current collector plate 33, or may be performed only on one surface. In the case where it is performed only on one side, the surface on the side of the division is set to be an outward surface in the electrode winding body 3. Although it is advantageous in terms of cost to perform the sorting process on only one side, it is necessary to manage the front and back of the positive electrode plate 32 in the winding process. If the separation processing is performed on both the front and back surfaces, the cost increases, but it is not necessary to manage the front and back surfaces of the positive electrode plate 32 in the winding process.
- the specific method of giving a difference in wettability between the region 134 and the region 135 is roughly classified into two types. These are a method of reducing the wettability of the region 134 and a method of improving the wettability of the region 135. Either one of both methods may be performed, or both may be performed.
- a method for reducing the wettability of the region 134 a low wettability component may be applied to the corresponding part. Examples of the low wettability component include various oils and fats and water repellents (fluorine resin, silicone, etc.). Examples of methods for improving the wettability of the region 135 include corona discharge treatment, surface roughening treatment, and cleaning treatment with a solvent.
- the degree of wettability difference between the region 134 and the region 135 will be described.
- the wettability is expressed as a numerical value that is so low that it is difficult to get wet and so high that it is easy to get wet.
- the ratio of wettability NA to wettability NB (NA / NB) 0.5 ⁇ NA / NB ⁇ 1 Within the range of The wettability may be measured by any known method. In the examples described later, the evaluation was performed based on the repellent state of the wettability evaluation reagent. As the evaluation reagent, a liquid mixture for wet tension evaluation manufactured by Wako Pure Chemical Industries, Ltd. was used. Another method is to measure the contact angle.
- FIG. 6 shows a state in which the positive electrode mixture layer 31 is formed on the aluminum foil 133 shown in FIG.
- the region 134 in FIG. 5 is the non-coated portion 34.
- the positive electrode mixture layer 31 is formed on the entire region 135 in FIG.
- both edge portions 31E of the positive electrode mixture layer 31 have a cross-sectional shape with the width L of the tip region 31S shown in FIG.
- the slit position where the positive electrode plate 32 is cut is indicated by a one-dot chain line. That is, the positive electrode plate 32 is cut into two in the width direction by the line 136 at the center in the width direction. Moreover, it cut
- the length Y corresponds to the length of the positive electrode plate 32 necessary for producing one electrode winding body 3.
- a width W that is half of the entire width of the positive electrode plate 32 shown in FIG. 6 corresponds to the full width of the positive electrode plate 32 shown in FIG.
- the partition between the region 134 and the region 135 in the aluminum foil 133 is not limited to that shown in FIG. 5, but may be that shown in FIG.
- the low wettability area 134 is formed over the entire length of the aluminum foil 133 (vertical direction in FIG. 5), but the area 134 in the section of FIG. Is formed. All areas except for the area where the area 134 is formed are the areas 135.
- the section shown in FIG. 7 has good original wettability on the surface of the aluminum foil 133 to be used, and is suitable for the case where a method of partially reducing the wettability to form the region 134 is used.
- the region 134 does not exist, may be the same as the front surface (that is, FIG. 7), or the region 134 may continuously exist in the longitudinal direction (that is, the same as FIG. 5). .
- FIG. 8 shows a state in which the positive electrode mixture layer 31 is formed on the aluminum foil 133 of FIG.
- the positive electrode plate 32 in FIG. 8 not only the region 134 in FIG. 7 but also the edge portion in the region 135 is the non-coated portion 34.
- the arrangement itself of the positive electrode mixture layer 31 and the non-coated part 34 is the same in FIGS.
- both edge portions 31 ⁇ / b> E of the positive electrode mixture layer 31 have the cross-sectional shape shown in FIG. 4.
- the slit position where the positive electrode plate 32 is cut is indicated by an alternate long and short dash line as in FIG. That is, the positive electrode plate 32 is cut into two in the width direction by the line 136 (width W), and is cut by the line 137 in the longitudinal direction for each length Y.
- width W and length Y are the same as in the case of FIG.
- FIG. 9 shows a plan view of one positive electrode plate 32 of the electrode winding body 3 in which the positive electrode plate 32 of FIG. 8 is cut by a line 136 and a line 137.
- the vertical dimension Z of the region 134 corresponds to the winding length of the outermost peripheral portion 32 ⁇ / b> C of the positive electrode plate 32 in FIG. 3 in the electrode winding body 3. That is, the length from the outermost end 32A of the positive electrode plate 32 in FIG. 3 to the portion 32B on the inner side of the circumference is equal to the dimension Z in FIG.
- the end without the region 134 that is, the lower end is the winding start end in the winding process, and the end with the region 134 is present.
- the upper part is the winding end. Note that the surface shown in FIG. 9 faces outward in the electrode winding body 3.
- the partition between the region 134 and the region 135 in the aluminum foil 133 may be as shown in FIG. 10 in addition to those shown in FIGS.
- the region 134 is intermittently formed in the longitudinal direction, and all the remaining regions are regions 135, but conversely in FIG. 10, the region 135 is intermittently formed in the longitudinal direction. , All remaining areas are designated as areas 134.
- the section shown in FIG. 10 is suitable for the case where the original wettability of the surface of the aluminum foil 133 to be used is low, and a method for partially improving the wettability to form the region 135 is used.
- the region 135 is not present, may be any of the front surface (that is, FIG. 10), and the region 135 may be continuously present in the longitudinal direction (that is, the same as FIG. 5). .
- FIG. 11 shows a state in which the positive electrode mixture layer 31 is formed on the aluminum foil 133 of FIG.
- the positive electrode mixture layer 31 is formed not only on the region 135 in FIG. 10 but also on portions of the region 134 other than both end portions in the width direction.
- the arrangement itself of the positive electrode mixture layer 31 and the non-coated part 34 is the same in any of FIGS. 6, 8, and 11.
- both edge portions 31 ⁇ / b> E of the positive electrode mixture layer 31 have the cross-sectional shape shown in FIG. 4.
- the slit position where the positive electrode plate 32 is cut is indicated by an alternate long and short dash line as in FIGS.
- the cutting method is the same as in the case of FIGS.
- the meanings of width W and length Y are the same. Therefore, even in the case of FIG. 11, there are one location of the region 135 in the length Y range.
- the region 135 is located at the end of the range of the length Y, and is the winding end on the outer surface side when winding.
- the process of dividing the end portion and the center portion may be performed intermittently, which may be advantageous in terms of processing cost. However, it is necessary to manage the direction of the start and end of winding of the positive electrode plate 32 in the winding process. If continuous processing as shown in FIG. 5 is performed, it may be costly, but it is not necessary to manage the orientation of the positive electrode plate 32 in the winding process.
- FIG. 12 shows an apparatus configuration for performing partitioning by corona discharge treatment.
- the apparatus shown in FIG. 12 includes an unwinding roll 201, a first roller 202, a corona discharge processing unit 203, a second roller 204, a die coating unit 205, a drying furnace 206, and a winding roll 207.
- the unprocessed aluminum foil is wound around the unwinding roll 201.
- the unprocessed aluminum foil unwound from the unwinding roll 201 reaches the winding roll 207 through the path stretched by the first roller 202 and the second roller 204 and is wound up.
- it is subjected to discharge treatment by the corona discharge treatment unit 203, coating by the die coating unit 205, and drying by the drying furnace 206.
- the corona discharge treatment unit 203 the aluminum foil is partially subjected to corona discharge treatment.
- the wettability of the surface of the aluminum foil that has been subjected to corona discharge treatment is improved. For this reason, a portion where the corona discharge treatment is performed becomes a region 135 and a portion where the corona discharge treatment is not performed becomes a region 134.
- the corona discharge processing unit 203 for example, “Corona Master” manufactured by Shinko Electric Instrumentation Co., Ltd. or a device having the same function can be used. In Examples described later, “Corona Master PS-1” was used.
- the corona discharge processing unit 203 has a mask 213 shown in FIG.
- a window 212 is formed in the mask 213.
- the corona discharge treatment is performed on the aluminum foil within the range of the window 212, but the corona discharge treatment is shielded by the mask 213 outside the range of the window 212.
- the mask 213 is arranged so that the window 212 faces the width direction range to be the region 135 of the aluminum foil and covers the remaining portion.
- the surface of the aluminum foil 133 that has passed through the corona discharge treatment unit 203 is divided into regions 134 and 135 as shown in FIG.
- the division as shown in FIG. 10 can be performed.
- the division as shown in FIG. 7 can be performed by the configuration of the corona discharge processing unit 203.
- a movable portion may be provided on the mask 213, or a plurality of corona discharge treatment portions 203 themselves may be provided in the width direction.
- the aluminum foil 133 whose surface is divided into regions 134 and 135 by the corona discharge treatment unit 203 is applied with an active material mixture paste by the die coating unit 205.
- the mixture paste is applied to the surface on the side subjected to the corona discharge treatment by the corona discharge treatment unit 203.
- the mixture paste is dried in the drying furnace 206.
- the positive electrode mixture layer 31 is formed.
- the aluminum foil 133 on which the positive electrode mixture layer 31 is formed is temporarily wound around the winding roll 207.
- the positive electrode mixture layer 31 is formed in the same manner on the back surface. Thereafter, pressing of the positive electrode mixture layer 31 and cutting along lines 136 and 137 shown in FIGS. 6, 8, and 11 are performed, and then the electrode winding body 3 is prepared.
- FIG. 14 shows an apparatus configuration for performing division by roughening processing.
- the configuration of the apparatus of FIG. 14 is the same as that of the apparatus of FIG. 12 except for the following points. That is, in the apparatus of FIG. 14, a roughening processing unit 223 is provided instead of the corona discharge processing unit 203 in the apparatus of FIG. 12.
- the roughening processing section 223 has a roughening roller 221 shown in FIG.
- the roughening roller 221 in FIG. 15 has a rough surface region 225 at the center in the width direction and smooth surface regions 224 on both sides thereof.
- the rough surface region 225 is a region formed with a material having fine irregularities on the surface and higher hardness than the aluminum foil.
- the width of the rough surface region 225 matches the width of the region 135 to be formed on the aluminum foil.
- the smooth surface region 224 is a region whose surface is a smooth surface.
- the smooth surface region 224 is preferably formed of a flexible material such as rubber.
- the roughening roller 221 is arranged so that the rough surface region 225 contacts the range in the width direction that should become the region 135 of the aluminum foil.
- the aluminum foil 133 shown in FIG. 5 can also be obtained by the apparatus of FIG. 14 having such a roughening processing section 223. Further, the aluminum foil 133 of FIG. 11 can be obtained by making the roughening roller 221 movable. Moreover, the aluminum foil 133 of FIG. 7 can also be obtained by providing a plurality of roughening rollers and making some of them movable.
- the apparatus of FIG. 12 and FIG. 14 can also be made into a multi-strand coating type. That is, a wide aluminum foil having a width corresponding to a plurality of aluminum foils shown in FIG. 5 or the like is targeted, and a plurality of positive electrode mixture layers 31 are formed at a time.
- the partitioning of the region 134 and the region 135 is also adapted to that.
- it can also be set as the apparatus structure which performs division by methods (refer to [0031]) other than a corona discharge process and a roughening process.
- an application roller, a cleaning device, or the like may be provided as appropriate in place of the corona discharge processing unit 203 and the roughening processing unit 223 in FIGS.
- the coating method is not limited to die coating.
- Electrolyte LiPF 6
- Electrolyte Mixed liquid of the following three components: Ethylene carbonate (EC) 3 parts by weight Dimethyl carbonate (DMC) 4 parts by weight Ethyl methyl carbonate (EMC) 3 parts by weight
- EC Ethylene carbonate
- DMC Dimethyl carbonate
- EMC Ethyl methyl carbonate
- the aluminum foil serving as the positive electrode current collector plate was subjected to the continuous sorting process shown in FIG. 5 by a corona discharge process (processing apparatus of FIG. 12). Corona discharge treatment was performed on the portion corresponding to the region 135 in FIG.
- the wettability of the aluminum foil on the current collector plate was as follows before and after the corona discharge treatment. Before treatment: 32 dyne / cm (corresponding to wettability NA of region 134) After treatment: 54 dyne / cm (corresponding to the wettability NB of the region 135) That is, in Example 1, the wettability ratio “NA / NB” is about 0.59.
- the aluminum foil serving as the positive electrode current collector plate was subjected to the continuous sorting process shown in FIG. 5 by roughening instead of the corona discharge process. A portion corresponding to the region 135 in FIG. 5 was roughened with a roughening roller having fine irregularities on the surface.
- the wettability of the aluminum foil on the current collector plate was as follows with or without roughening treatment. No roughening: 32 dyne / cm (corresponding to wettability NA of region 134) With roughening: 36 dyne / cm (corresponding to wettability NB of region 135) That is, in Example 2, the wettability ratio “NA / NB” is about 0.89.
- the aluminum foil serving as the positive electrode current collector plate was subjected to the continuous sorting process shown in FIG. 5 by oil application instead of the corona discharge process. Oil was applied to a portion corresponding to the region 134 in FIG. Aqua oil B-2S manufactured by Aqua Chemical Co., Ltd. was used as the oil to be applied.
- the wettability of the aluminum foil on the current collector plate was as follows with and without oil application. Application: 28 dyne / cm (corresponding to wettability NA of region 134) No application: 32 dyne / cm (corresponding to wettability NB of region 135) That is, in Example 3, the wettability ratio “NA / NB” is about 0.88.
- the aluminum foil serving as the positive electrode current collector was subjected to the continuous sorting process shown in FIG. 5 by applying a water repellent agent instead of the corona discharge process.
- a water repellent was applied to a portion corresponding to the region 134 in FIG.
- a fluororesin type was used as the water repellent to be applied.
- the wettability of the aluminum foil on the current collector plate was as follows depending on whether or not the water repellent was applied. With application: 22.6 dyne / cm (corresponding to wettability NA of region 134) No application: 32 dyne / cm (corresponding to wettability NB of region 135) That is, in Example 4, the wettability ratio “NA / NB” is about 0.71.
- the aluminum foil used as the positive electrode current collector plate was subjected to the continuous sorting process shown in FIG. 5 by the combined use of corona discharge treatment and oil coating. Corona discharge treatment was performed on the portion corresponding to the region 135 in FIG. 5, and oil was applied to the portion corresponding to the region 134. The same oil as that used in Example 3 was used as the oil to be applied.
- the wettability of the aluminum foil on the current collector plate was as follows between the corona discharge treated part and the oiled part.
- the aluminum foil used as the current collector for the positive electrode was subjected to the continuous sorting process shown in FIG. 5 by the combined use of corona discharge treatment and water repellent coating.
- a corona discharge treatment was performed on a portion corresponding to the region 135 in FIG. 5, and a water repellent was applied to a portion corresponding to the region 134.
- the same water repellent as applied in Example 4 was used.
- the wettability of the aluminum foil on the current collector plate was as follows between the part subjected to the corona discharge treatment and the part coated with the water repellent.
- Water repellent coating 22.6 dyne / cm (corresponding to wettability NA of region 134)
- Corona discharge treatment 54 dyne / cm (corresponding to wettability NB of region 135) That is, in Example 6, the wettability ratio “NA / NB” is about 0.42.
- Corona discharge treatment was intermittently performed by corona discharge treatment on the aluminum foil serving as the positive electrode current collector, and the sorting treatment shown in FIG. 10 was performed. Corona discharge treatment was performed on the portion corresponding to the region 135 in FIG. Corona discharge treatment was applied to the same part on the front and back. And as demonstrated in FIG. 11, the location which performed the corona discharge process was made to be located in the outermost periphery in an electrode winding body.
- the wettability of the aluminum foil of the current collector was the same as in Example 1. That is, in Example 7, the wettability ratio “NA / NB” is about 0.59.
- the aluminum foil serving as the positive electrode current collector plate was subjected to the coating of the positive electrode mixture layer as it was without any corona discharge treatment or other wettability adjustment treatment.
- the wettability of the aluminum foil of the current collector plate was the same as the value before the corona discharge treatment in Example 1. That is, in Comparative Example 1, the difference in wettability is not divided, and the ratio “NA / NB” is 1.0.
- a corona discharge treatment was applied to the entire surface of the aluminum foil serving as the positive electrode current collector.
- the wettability of the current collector plate after the treatment of the aluminum foil was the same as the value after the corona discharge treatment in Example 1. That is, even in Comparative Example 2, the difference in wettability is not divided, and the ratio “NA / NB” is 1.0.
- the voltage failure occurrence rate was measured by the following method. That is, for each example and comparative example, 200 batteries were prepared and tested according to the following procedure. -It charged to 4.0V with a constant current (4A) at 25 degreeC. ⁇ -It stored for 48 hours in a 75 degreeC thermostat in the open circuit state. ⁇ • The battery voltage was measured at 25 ° C.
- the stability check of the coating width was performed as follows. That is, the width direction end part of the mixture layer of the produced electrode plate was observed using a microscope over a length of 1 m in the longitudinal direction. As a result, it was confirmed whether or not there was a portion where the end portion of the mixture layer was recessed larger than 0.6 mm in the width direction. That is, the edge linearity was checked for quality.
- Example 6 is indicated only in Example 6, and “ ⁇ ” is indicated for all others. This is because in Example 6, one location where the end portion of the mixture layer was recessed slightly larger than 0.6 mm was found. Except Example 6, the recessed part exceeding 0.6 mm was not seen. From this, it is understood that Example 6 is inferior in the stability of the coating width as compared with the other examples. This is considered to be because the value of the wettability ratio “NA / NB” between the region 134 and the region 135 is 0.42, which is much lower than the other. That is, it is understood that the difference in wettability between the region 134 and the region 135 is slightly excessive.
- the overall evaluation in Table 1 was not “x” but “ ⁇ ”.
- the overall evaluation in Table 1 was not “x” but “ ⁇ ”.
- the overall evaluation was “ ⁇ ”. From the above, the value of the ratio “NA / NB” must be less than 1.
- the value of the ratio “NA / NB” is preferably larger than 0.5.
- Example 1 shows that the same results as in Example 1 were obtained in Example 7 in which the corona discharge treatment was intermittently performed.
- Example 1 is the same as Example 7 except that the corona discharge treatment is continuously performed. From this, it was confirmed that the partitioning of the region 134 and the region 135 may be performed only on the outermost part of the electrode winding body as described with reference to FIGS.
- the thin layer region is formed at the end portion of the mixture layer because the mixture paste is a fluid.
- the lower the viscosity of the mixture paste the more easily the thin layer region is formed. This is because a mixture paste having a low viscosity tends to flow. In that sense, it is desirable that the mixture paste has a high viscosity in order not to form a large thin layer region at the end of the mixture layer.
- the high viscosity of the mixture paste is a factor that makes the process of applying the mixture paste to the aluminum foil (the process of the above-described die coat part 205) itself difficult. This is because a certain amount of fluidity is required for the mixture paste in order to apply the mixture paste flat on the aluminum foil.
- the positive electrode active material mixture paste used for forming the positive electrode mixture layer 31 in the positive electrode plate 32 generally has viscosity characteristics as shown in the graph of FIG. In FIG. 16, the horizontal axis indicates the shear rate and the vertical axis indicates the viscosity, and the thixotropy in which the viscosity decreases as the shear rate increases.
- the mixture paste used for forming the positive electrode mixture layer 31 is equivalent to being stirred at a shear rate of about 100 seconds- 1 at the time of coating. It is in a state equivalent to being stirred at a shear rate of about 2 seconds -1 . Therefore, in order to carry out the coating process without difficulty, it is desired that the viscosity at a shear rate of 100 seconds- 1 (star P in FIG. 16, hereinafter referred to as “100 s- 1 viscosity”) is low. On the other hand, in order not to form a large thin layer region at the end of the mixture layer after coating, the viscosity at a shear rate of 2 seconds ⁇ 1 (star sign Q in FIG. 16, hereinafter referred to as “2s ⁇ 1 viscosity”). ) Is desired to be high.
- the mixture paste used for forming the positive electrode mixture layer 31 has a remarkable difference in height between the stars P and Q in FIG.
- a parameter of a ratio of 100 s ⁇ 1 viscosity (V100) to 2 s ⁇ 1 viscosity (V2), V2 / V100 is introduced. This parameter is referred to as a TI (thixotropy index) value.
- a positive electrode mixture paste prepared so that the TI value is increased to some extent is used.
- the viscosity of the mixture paste is low during coating and is easy to apply, and is somewhat high and difficult to flow on the aluminum foil after coating. For this reason, the thin layer region is not formed largely at the end portion of the mixture layer.
- the TI value is too high, the flatness of the flat region 31 ⁇ / b> F of the positive electrode mixture layer 31 is poor. This is because the fluidity of the coated mixture paste on the current collector plate is low. Accordingly, there is a preferable range for the TI value of the mixture paste. As will be described later, it is in the range of 1.7 to 4.6.
- a special heat treatment is performed so as not to form a large thin layer region at the end of the mixture layer even in the drying step after coating. This is because in the drying process, the temperature of the just-applied mixture paste increases, but the viscosity of the mixture paste decreases due to this temperature increase.
- the graph of FIG. 17 shows the relationship between the temperature and viscosity of the mixture paste. From this graph, it can be seen that the viscosity decreases as the temperature of the mixture paste increases. For this reason, in the drying process, if the temperature rises excessively before the mixture paste is dried and solidified, flow occurs at the end portion and the thin layer region becomes large.
- the coated aluminum foil can be supported using a special support roller in order to realize the temperature difference between the end and the center.
- the special carrying roller is as shown in FIG. 18 or FIG.
- a water channel 141 is provided inside the carrying roller 140 of FIG.
- the water channels 141 are provided at both ends of the carrying roller 140 in the width direction. That is, there is a cooling section at the width direction end of the carrying roller 140, and there is a non-cooling area 142 without the water channel 141 between them.
- the biting width 144 of the water channel 141 with respect to the portion of the aluminum foil carrying the region 135 (the region where the positive electrode mixture layer 31 is present) is about 10 mm on both the left and right sides.
- the supporting roller 140 supports the aluminum foil while passing cooling water (or a coolant other than water) through the water channel 141.
- a temperature difference in the width direction can be generated in the conveyed aluminum foil as follows. That is, in a certain range of the water channel 141 at both ends in the width direction, the temperature becomes relatively low due to the cooling action by the cooling water. As a result, the portion 144 having a width of about 10 mm at the end in the width direction of the mixture paste coated on the aluminum foil is also relatively low in temperature and maintained in a high viscosity state.
- the non-cooling region 142 between the two water channels 141 has a relatively high temperature because there is no cooling action of the cooling water, and the evaporation of the solvent component from the mixture paste is promoted. That is, in the width direction of the carrying roller 140, the region with the water channel 141 is a low temperature region, and the non-cooling region 142 without the water channel 141 is a high temperature region.
- the bearing roller 150 in FIG. 19 does not have the water channel 141 unlike the one in FIG. Instead, the carrier roller 150 has a heater 151 built therein. Unlike the water channels 141 arranged at both ends in the width direction, the heater 151 is located at the center in the width direction. That is, the carrier roller 150 has a heating section in the center in the width direction, and both ends are non-heating sections. Of course, the supporting roller 150 supports the aluminum foil while heating by the heater 151. Then, in the carrier roller 150, depending on the presence or absence of heating by the heater 151, the central portion in the width direction becomes a high temperature region and both end portions become low temperature regions.
- the protrusion width 154 of the coating region 135 from the width of the heater 151 is approximately the same as the width 144 in FIG.
- an apparatus having a configuration obtained by removing the corona discharge processing unit 203 or the roughening processing unit 223 from the apparatus configuration shown in FIG. 12 or FIG. 14 is used.
- the part after the die coat part 205 is shown in the upper half of FIG. In this configuration, the carrying roller 140 or 150 comes into contact with the back surface side of the positive electrode plate 32 at a location after the die coat portion 205 and before the drying furnace 206.
- the positive electrode plate 32 enters the drying furnace 206 with the temperature difference in the width direction as described above. Therefore, particularly at the initial stage of the drying process in the drying furnace 206, as described in [0083], the expansion of the thin layer region at the end of the mixture layer is prevented.
- the temperature difference in the width direction gradually attenuates after the middle stage of the drying process, but at that time, the amount of solvent in the mixture paste has decreased to some extent. For this reason, even if the temperature of the mixture paste rises at the end in the width direction, it does not lead to the expansion of the thin layer region. This is because the mixture paste has already begun to harden.
- the lower half of FIG. 20 shows a graph of changes in temperature and residual solvent amount in the mixture layer 31 of the positive electrode plate 32 conveyed in the drying furnace 206.
- the temperature shown here is the temperature at the flat portion at the center in the width direction. Further, an example in which the end cooling type support roller 140 shown in FIG. 18 is used as the support roller in front of the drying furnace 206 is shown.
- the temperature rises rapidly, but the amount of solvent does not decrease much. This is because the temperature itself is not so high during this period.
- the temperature difference due to the carrying roller 140 is in the mixture layer 31, the thin layer region does not expand.
- the constant rate drying period 226 is entered after the preheating period 216, the temperature becomes substantially saturated and constant. And the amount of solvent decreases almost linearly.
- the temperature difference due to the carrying roller 140 is considerably weak, but the mixture paste becomes difficult to flow due to the decrease in the amount of solvent. For this reason, the thin layer region is not enlarged.
- the speed of the decrease in the amount of solvent decreases. This is because the residual solvent amount itself approaches zero. And with it, the temperature rises slightly again. This is because the heat of vaporization caused by the evaporated solvent is reduced. At this point, the temperature difference due to the carrier roller 140 has almost disappeared, but almost no fluidity remains in the mixture layer 31 itself. For this reason, the thin layer region is not enlarged. Thus, in the second embodiment, it is possible to prevent the thin layer region from being enlarged at the end portion of the mixture layer 31.
- the supporting roller 140 or 150 is provided in the region of the preheating period 216 in the drying furnace 206 (1/6 to 1/4 of the entire length of the drying furnace 206). May be. However, it does not make much sense to provide the carrying rollers 140 or 150 at locations corresponding to the constant rate drying period 226 or the reduced rate drying period 236. Further, instead of providing the supporting roller 140 or 150, the heater 217 (or hot air outlet) in the region of the preheating period 216 in the drying furnace 206 is faced only at the center of the mixture layer 31 as shown in FIG. May be provided.
- the TI value described in [0080] was adjusted according to the kneading time for the positive electrode mixture paste. That is, the longer the kneading time, the lower the TI value is obtained, and the shorter the kneading time, the higher the TI value is obtained.
- a planetary mixer was used for kneading. Then, the viscosity of the positive electrode mixture paste after kneading was measured at 20 ° C. at two levels of shear rates of about 100 seconds- 1 and about 2 seconds- 1, and the TI value was calculated from the measurement results. For the viscosity measurement, “Physica MCR301” manufactured by Anton Paar was used.
- the kneading time of the positive electrode mixture paste was 90 minutes, and a mixture paste having a TI value of 1.8 was obtained. Further, as the supporting roller before the drying furnace 206, a normal roller which is not the special one shown in FIGS. 18 and 19 was used. The hot air temperature in the drying furnace 206 was set to 150 ° C.
- the kneading time of the positive electrode mixture paste was 60 minutes, and a mixture paste having a TI value of 2.7 was obtained. Others were the same as in Example 8.
- the kneading time of the positive electrode mixture paste was 40 minutes, and a mixture paste having a TI value of 3.6 was obtained. Others were the same as in Example 8.
- the kneading time of the positive electrode mixture paste was 30 minutes, and a mixture paste having a TI value of 4.5 was obtained. Others were the same as in Example 8.
- the central heating type supporting roller 150 shown in FIG. 19 was used as the supporting roller before the drying furnace 206.
- the hot air temperature in the drying furnace 206 was 140 ° C. Others were the same as in Example 9.
- the kneading time of the positive electrode mixture paste was 120 minutes, and a mixture paste having a TI value of 1.3 was obtained. Others were the same as in Example 8.
- the kneading time of the positive electrode mixture paste was 20 minutes, and a mixture paste having a TI value of 5.5 was obtained. Others were the same as in Example 8.
- the cycle characteristics were tested as follows. First, the following charge / discharge was performed at 25 ° C., and the initial battery capacity was calculated by this charge / discharge. -The battery was charged to 4.1 V with a constant current (4 A). ⁇ -Paused for 10 minutes. ⁇ -Discharged to 3.0 V with a constant current (4A).
- Capacity maintenance rate Battery capacity after cycle / Initial battery capacity
- the measurement results are shown in Table 2 together with the TI value of the mixture paste.
- the relationship between the TI value of the mixture paste in Table 2 and the L dimension of the end cross-sectional shape is shown in the graph of FIG. In FIG. 22, the TI value is on the horizontal axis and the L dimension is on the vertical axis. According to FIG. 22, it can be seen that the higher the TI value of the mixture paste, the smaller the width of the “L” portion at the end of the mixture layer. This is consistent with the description in [0080].
- the width of the “L” portion needs to be 100 ⁇ m or less as described in [0024]. Since the L dimension of Comparative Example 3 exceeds 115 ⁇ m, it is not good. For this reason, for Comparative Example 3 (TI value 1.3), the overall evaluation in Table 2 was “x”.
- Example 8 In all cases other than Comparative Example 3 (Examples 8 to 13, Comparative Example 4, TI value 1.8 to 5.5), the L dimension was less than 100 ⁇ m. Among them, Example 8 (TI value 1.8, L dimension 73 ⁇ m) has the lowest TI value and the largest L dimension. Since the L dimension in Example 8 and Comparative Example 3 are considerably different, the allowable lower limit value of the TI value is considered to be about 1.7, which is slightly lower than the TI value in Example 8.
- Example 11 (TI value 4.5, capacity retention rate 88%) has the highest TI value and the lowest capacity retention rate. Since the capacity retention rates of Example 11 and Comparative Example 4 are considerably different, the allowable upper limit value of the TI value is considered to be about 4.6, which is slightly higher than the TI value of Example 11.
- the overall evaluation in Table 2 was “ ⁇ ” for Examples 8 to 13 except Comparative Example 3 in which the L dimension of the end shape was bad and Comparative Example 4 in which the capacity retention rate was bad. Accordingly, the preferable range of the TI value of the mixture paste is in the range of 1.7 to 4.6.
- Examples 12 and 13 using a special roller as a supporting roller before the drying furnace 206 will be further discussed. These Examples 12 and 13 are the same as Example 9 regarding the TI value of the used mixture paste. However, in Examples 12 and 13, an L dimension superior to that of Example 9 is obtained. That is, in Examples 12 and 13, an L dimension comparable to Examples 10 and 11 using a mixture paste having a higher TI value was obtained. Nevertheless, Examples 12 and 13 are superior to Examples 10 and 11 in terms of capacity retention. In particular, in Example 13 using the central heating type support roller, the capacity retention rate surpassed that of Example 8 using a mixture paste having a lower TI value.
- Examples 12 and 13 are considered to be due to the use of the end-cooling support roller in FIG. 18 or the central heating support roller in FIG. That is, in these examples, the drying process is started after a temperature difference is given to the coated mixture paste layer between the end and the center. As a result, the compatibility between the small L dimension and the high capacity retention ratio is realized at a higher level.
- the portion that should be the coating portion and the non-coating portion of the aluminum foil serving as the positive electrode current collector plate there is a difference in wettability with the part that should be.
- a positive electrode mixture paste used for coating is adjusted so that the TI value is within a predetermined range.
- region of the width direction edge part of the positive mix layer 31 is 100 micrometers or less.
- a non-aqueous electrolyte secondary battery a method for manufacturing a positive electrode plate of a non-aqueous electrolyte secondary battery, and a method for manufacturing a non-aqueous electrolyte secondary battery, which eliminates the problem of current concentration at the outermost peripheral portion of the positive electrode, are realized. Has been.
- the present invention can naturally be improved and modified in various ways without departing from the gist thereof.
- the specific material of each part and the outer shape of the battery may be anything as long as they function as a nonaqueous electrolyte secondary battery.
- the first form and the second form may be used in combination.
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Abstract
Description
0.5 < NA/NB< 1
となるように調整する濡れ性調整処理を行う。この濡れ性調整処理により,前述の合剤層の幅方向端部の急峻断面形状が実現される。濡れ性の高い塗工部には正極合剤ペーストが均一に塗工される一方で,濡れ性の低い非塗工部では正極合剤ペーストがはじかれるからである。
このうち,集電板33にあらかじめ表面処理を施しておく手法を第1の形態とし,以下に説明する。第1の形態では,アルミ箔の集電板33について,塗工処理に先立ち,正極合剤層31が形成されるべき部分と非塗工部34となるべき部分との間に,濡れ性の差を付ける処理を行う。むろん,正極合剤層31が形成されるべき部分の濡れ性を高くして,非塗工部34となるべき部分の濡れ性を低くする。これにより,正極合剤層31が形成されるべき部分の上に塗工された合剤ペーストが,流動して非塗工部34となるべき部分の上に移動してしまうことを防ぐ。
NA < NB
となる。本形態ではさらに,濡れ性NAと濡れ性NBとの比(NA/NB)について,
0.5 < NA/NB< 1
の範囲内としている。濡れ性の測定については,公知のいかなる方法で行っても良い。後述する実施例では,濡れ性評価試薬のはじき具合で評価した。その評価試薬として,和光純薬工業製の濡れ張力評価用混合液を使用した。別の手法としては,接触角の測定による方法もある。
集電板:15μm厚のアルミ箔
合剤固形分:以下の3成分の混合物
・ニッケルマンガンコバルト酸リチウム(※) 90重量部
・アセチレンブラック 8重量部
・ポリフッ化ビニリデン(PVDF) 2重量部
※はNi:Mn:Co=1:1:1モル比のもの
混練溶媒:N-メチル-2-ピロリドン(NMP)
塗工方法:ダイ塗工
プレス,スリット後の電極板の寸法:
集電板幅115mm
長さ3000mm
合剤層幅95mm
合剤層厚0.065mm
集電板:10μm厚の銅箔
合剤固形分:以下の3成分の混合物
黒鉛 98.6重量部
カルボキシメチルセルロース(CMC,BSH-12) 0.7重量部
スチレンブタジエンゴム(SBR) 0.7重量部
混練溶媒:水
塗工方法:ダイ塗工
セパレータ:PP/PE/PPの3層 総厚20μm
電解液:
電解質:LiPF6
電解液:以下の3成分の混合液
エチレンカーボネート(EC) 3重量部
ジメチルカーボネート(DMC) 4重量部
エチルメチルカーボネート(EMC)3重量部
濃度:1.0M
電池構成:
電極捲回体の形状:楕円捲回体
電池容器の形状:角形
定格容量:4.0Ah
処理前:32dyne/cm(領域134の濡れ性NAに相当)
処理後:54dyne/cm(領域135の濡れ性NBに相当)
つまり実施例1では,濡れ性の比「NA/NB」は約0.59である。
粗面化無:32dyne/cm(領域134の濡れ性NAに相当)
粗面化有:36dyne/cm(領域135の濡れ性NBに相当)
つまり実施例2では,濡れ性の比「NA/NB」は約0.89である。
塗布有:28dyne/cm(領域134の濡れ性NAに相当)
塗布無:32dyne/cm(領域135の濡れ性NBに相当)
つまり実施例3では,濡れ性の比「NA/NB」は約0.88である。
塗布有:22.6dyne/cm(領域134の濡れ性NAに相当)
塗布無:32dyne/cm(領域135の濡れ性NBに相当)
つまり実施例4では,濡れ性の比「NA/NB」は約0.71である。
オイル塗布:28dyne/cm(領域134の濡れ性NAに相当)
コロナ放電処理:54dyne/cm(領域135の濡れ性NBに相当)
つまり実施例5では,濡れ性の比「NA/NB」は約0.52である。
撥水剤塗布:22.6dyne/cm(領域134の濡れ性NAに相当)
コロナ放電処理:54dyne/cm(領域135の濡れ性NBに相当)
つまり実施例6では,濡れ性の比「NA/NB」は約0.42である。
・完成した電池における電圧不良発生率の測定
・正極用の集電板における合剤層の塗工幅の安定性検査
・正極用の集電板における合剤層の幅方向端部の断面形状評価
・25℃にて,定電流(4A)で4.0Vまで充電した。
↓
・開回路状態で75℃の恒温槽に48時間保管した。
↓
・25℃にして,電池電圧を測定した。
判定基準電圧 = Vave - 3σ
かかる判定基準電圧より低い電圧を示すものを不良とし,各実施例および比較例ごとに不良率を算出した。
次に第2の形態,すなわち合剤ペーストとして特別に調製したものを用いる手法を説明する。合剤層の端部に薄層領域ができてしまうのは要するに,合剤ペーストが流動物であることによる。むろん,合剤ペーストの粘度が低いほど,薄層領域が顕著にできやすい。粘度の低い合剤ペーストは流動しやすいからである。その意味では,合剤層の端部に薄層領域を大きく形成させないためには,合剤ペーストの粘度が高いことが望ましい。
・完成した電池における電圧不良発生率の測定
・正極用の集電板における合剤層の幅方向端部の断面形状評価
・完成した電池のサイクル特性の試験
このうちの電圧不良発生率と断面形状評価については,前述の第1の形態の実施例で行った試験と同様である。
・定電流(4A)で4.1Vまで充電した。
↓
・10分間休止させた。
↓
・定電流(4A)で3.0Vまで放電させた。
・定電流(8A)で4.1Vまで充電する。
↓
・10分間休止させる。
↓
・定電流(8A)で3.0Vまで放電させる。
↓
・10分間休止させる。
容量維持率 = サイクル後の電池容量/初期の電池容量
3 電極捲回体
4 セパレータ
22 負極板
31 正極合剤層
31F 平坦領域
31S 先端領域
32 正極板
32C 最外周部分
34 非塗工部
140 端部冷却式の加熱ローラ
150 中央部加熱式の加熱ローラ
203 コロナ放電処理部
205 ダイコート部
206 乾燥炉
223 粗面化処理部
Claims (10)
- 正極板および負極板をセパレータを介して巻き重ねてなる電極捲回体を有する非水電解液二次電池において,
前記電極捲回体における最外周の電極板は負極板であり,
前記正極板における最外周部分の外面側の合剤層の幅方向の端部の断面形状は,前記合剤層の幅方向中央の平坦部の厚さの50%以下の厚さである部分の幅が100μm以下である急峻断面形状とされていることを特徴とする非水電解液二次電池。 - 正極板および負極板をセパレータを介して巻き重ねてなる電極捲回体を有する非水電解液二次電池の正極板の製造方法において,
集電板に正極合剤ペーストを塗工して合剤層を形成する塗工工程を有し,
前記塗工工程に先立ち,集電板の長手方向における,少なくとも電極捲回体にて最外周となる範囲である最外周領域の外面側に,非塗工部となる幅方向端部の濡れ性値NAと塗工部となる幅方向中央部の濡れ性値NBとの比NA/NBが,
0.5 < NA/NB< 1
となるように調整する濡れ性調整処理を行うことにより,
前記塗工工程で形成される合剤層の幅方向の端部の断面形状を,少なくとも電極捲回体にて外面側となる面側の前記最外周領域では,前記合剤層の幅方向中央の平坦部の厚さの50%以下の厚さである部分の幅が100μm以下である急峻断面形状とすることを特徴とする非水電解液二次電池の正極板の製造方法。 - 請求項2に記載の非水電解液二次電池の正極板の製造方法において,
前記濡れ性調整処理では,
集電板の幅方向端部の濡れ性を低下させる処理と,集電板の幅方向中央部の濡れ性を向上させる処理との少なくとも一方を行うとともに,
前記濡れ性を低下させる処理を行う場合の当該低下させる処理が,オイル塗布処理もしくは撥水剤塗布処理であり,
前記濡れ性を向上させる処理を行う場合の当該向上させる処理が,コロナ放電処理,粗面化処理,溶剤による洗浄処理のいずれか1つであることを特徴とする非水電解液二次電池の正極板の製造方法。 - 請求項2または請求項3に記載の非水電解液二次電池の正極板の製造方法において,
前記濡れ性調整処理を,集電板の長手方向全体にわたって行うことを特徴とする非水電解液二次電池の正極板の製造方法。 - 請求項2または請求項3に記載の非水電解液二次電池の正極板の製造方法において,
前記濡れ性調整処理を,集電板の長手方向全体のうち,電極捲回体にて最外周となる範囲に対してのみ行うことを特徴とする非水電解液二次電池の正極板の製造方法。 - 正極板および負極板をセパレータを介して巻き重ねてなる電極捲回体を有する非水電解液二次電池の正極板の製造方法において,
集電板に正極合剤ペーストを塗工して合剤層を形成する塗工工程を有し,
前記塗工工程では,20℃における,せん断速度2s-1での粘度とせん断速度100s-1での粘度との比であるTI値が,1.7~4.6の範囲内にある正極合剤ペーストを使用することにより,
前記塗工工程で形成される合剤層の幅方向の端部の断面形状を,前記合剤層の幅方向中央の平坦部の厚さの50%以下の厚さである部分の幅が100μm以下である急峻断面形状とすることを特徴とする非水電解液二次電池の正極板の製造方法。 - 請求項6に記載の非水電解液二次電池の正極板の製造方法において,
前記塗工工程で形成した合剤層を乾燥させる乾燥工程を有し,
前記乾燥工程の入り側では,合剤層の幅方向端部を幅方向中央部より低温とすることを特徴とする非水電解液二次電池の正極板の製造方法。 - 請求項7に記載の非水電解液二次電池の正極板の製造方法において,
前記塗工工程後の集電板の裏面側を担持ローラで担持するとともに,
前記担持ローラとして,幅方向端部に冷却区間を有しその間が非冷却区間である端部冷却ローラを用いることを特徴とする非水電解液二次電池の正極板の製造方法。 - 請求項7に記載の非水電解液二次電池の正極板の製造方法において,
前記塗工工程後の集電板の裏面側を担持ローラで担持するとともに,
前記担持ローラとして,幅方向中央部に加熱区間を有し両端が非加熱区間である中央部加熱ローラを用いることを特徴とする非水電解液二次電池の電極板の製造方法。 - 請求項2から請求項9までのいずれか1つに記載の製造方法で製造された正極板を,負極板およびセパレータとともに用い,
正極板および負極板をセパレータを介して巻き重ねて電極捲回体とする捲回工程を有し,
前記捲回工程では,
前記電極捲回体の最外周の電極板を負極板とし,
前記正極板における少なくとも最外周部分の外面側に,合剤層の幅方向の端部を前記急峻断面形状とした部分を配置することを特徴とする非水電解液二次電池の製造方法。
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CN201380072418.7A CN104981935A (zh) | 2013-02-08 | 2013-12-09 | 非水电解液二次电池、非水电解液二次电池的正极板的制造方法、和非水电解液二次电池的制造方法 |
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KR102613891B1 (ko) * | 2015-11-27 | 2023-12-13 | 니폰 제온 가부시키가이샤 | 비수계 2차 전지 접착층용 조성물, 비수계 2차 전지용 접착층, 및 비수계 2차 전지 |
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