WO2011128963A1 - 電池用電極の製造方法 - Google Patents
電池用電極の製造方法 Download PDFInfo
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- WO2011128963A1 WO2011128963A1 PCT/JP2010/056533 JP2010056533W WO2011128963A1 WO 2011128963 A1 WO2011128963 A1 WO 2011128963A1 JP 2010056533 W JP2010056533 W JP 2010056533W WO 2011128963 A1 WO2011128963 A1 WO 2011128963A1
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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
- H01M4/70—Carriers or collectors characterised by shape or form
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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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/04—Processes of manufacture in general
- H01M4/0473—Filling tube-or pockets type electrodes; Applying active mass in cup-shaped terminals
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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
- H01M4/36—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
- H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M4/621—Binders
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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
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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
- H01M4/665—Composites
- H01M4/667—Composites in the form of layers, e.g. coatings
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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
Definitions
- the present invention relates to a method of manufacturing a battery electrode, and more particularly to a method of manufacturing a battery electrode having a configuration in which an electrode mixture layer containing an electrode active material is held by a current collector.
- a lithium secondary battery that is lightweight and has a high energy density is expected to be preferably used as a high-output power source for mounting on a vehicle.
- an electrode having a configuration in which a material (electrode active material) capable of reversibly occluding and releasing lithium ions is held in a conductive member (electrode current collector) is used.
- the electrode active material (negative electrode active material) used for the negative electrode carbon-based materials such as graphite carbon and amorphous carbon are exemplified.
- a typical example of the electrode current collector (negative electrode current collector) used for the negative electrode is a sheet-like or foil-like member mainly composed of copper or a copper alloy.
- a composite of a negative electrode active material powder and a binder (binder) dispersed in a suitable medium As one of the typical methods for holding a negative electrode active material on a negative electrode current collector, a composite of a negative electrode active material powder and a binder (binder) dispersed in a suitable medium.
- the binder in the negative electrode mixture layer has a role of binding the negative electrode active materials to each other and binding between the negative electrode mixture layer and the negative electrode current collector. Further, the binder in the negative electrode mixture layer also has a role of binding the negative electrode mixture layer to the negative electrode current collector.
- Patent document 1 is mentioned as technical literature regarding manufacture of this kind of electrode.
- the main objective is to provide the manufacturing method of the electrode for batteries which can improve the adhesive strength (adhesiveness) of a collector and a composite material layer. It is.
- the composite material layer is formed by applying a composite paste containing the active material to a current collector and drying it.
- the formation of the composite material layer includes a step of forming a projection made of a polymer on the surface of the current collector.
- the method includes a step of forming a binder solution layer by applying a binder solution containing a binder onto the current collector from above the polymer protrusion.
- the method includes a step of depositing the binder solution layer and the composite paste layer on the current collector by applying a composite paste containing an active material from above the binder solution layer.
- the method includes a step of obtaining an electrode in which the composite material layer is formed on the current collector by drying the deposited binder solution layer and the composite material paste layer together.
- the binder solution layer is formed between the current collector and the composite paste layer, and the binder solution layer and the composite paste layer are dried together to form the composite layer.
- Many binders derived from the binder solution layer are arranged at the interface between the current collector and the composite material layer. As a result, the amount of the binder near the current collector is increased, and an electrode having a composite layer having good adhesion (adhesive strength) to the current collector can be obtained.
- the mixture paste layer can be prevented from slipping. That is, when the composite paste is applied from above the binder solution layer, the composite paste is repelled by the binder solution layer, causing slippage, and unevenness may occur on the surface (coating surface) of the composite layer obtained after drying.
- a polymer protrusion is formed on the surface of the current collector, and a binder solution layer and a composite paste layer are sequentially deposited thereon, so that the composite paste layer is a polymer protrusion. Get caught in. As a result, slippage of the composite paste layer is prevented, and an electrode having a flat composite layer with few irregularities on the surface can be produced.
- the height of the polymer projection is preferably larger than the thickness of the binder solution layer. In this case, since the tip of the polymer projection protrudes above the upper surface of the binder solution layer, the slip of the composite paste layer can be appropriately suppressed.
- the height of the polymer protrusion is larger than the total thickness of the binder solution layer and the composite paste layer combined.
- the tip of the polymer projection protrudes upward from the upper surface of the composite paste layer, the slip of the composite paste layer can be more reliably suppressed.
- the polymer protrusion is formed into a plurality of independent dots (spots).
- the slip of the composite paste layer can be appropriately suppressed by a large number of independent dot-like projections.
- the polymer protrusion is formed into a patterned convex shape.
- the slippage of the composite paste layer can be appropriately suppressed by the patterned uneven projection.
- the polymer protrusion is formed by applying a polymer solution containing a polymer to a current collector and then drying.
- the polymer protrusion can be easily formed.
- a dot-shaped polymer projection can be easily formed by applying the polymer solution by spraying.
- a patterned convex polymer projection can be easily formed.
- static electricity is imparted to the polymer solution coating.
- the drying rate of the polymer solution coating is increased by electrostatic energy. Therefore, the polymer protrusion can be formed efficiently (preferably without a drying furnace).
- the polymer protrusion functions as a binder in the composite layer.
- the polymer protrusion since the polymer protrusion functions as a binder, it is possible to further improve the adhesion between the composite material layer and the current collector.
- the polymer protrusion can be made of the same material (common polymer) as the binder contained in the binder solution.
- a battery for example, a lithium secondary battery constructed using the electrode obtained by any one of the methods disclosed herein.
- a battery exhibits excellent battery performance because it is constructed using at least one of the electrodes.
- a battery satisfying at least one (preferably all) of high cycle durability, excellent output characteristics, and good productivity can be provided. .
- Such a battery is suitable as a battery mounted on a vehicle such as an automobile. Therefore, according to the present invention, there is provided a vehicle including any of the batteries disclosed herein (which may be in the form of an assembled battery in which a plurality of batteries are connected).
- the battery is a lithium secondary battery (typically a lithium ion battery), and the lithium secondary battery is used as a power source (typically a hybrid vehicle or an electric vehicle).
- a vehicle for example, an automobile
- a power source of the vehicle is preferable.
- FIG. 1 is a cross-sectional view schematically showing an electrode according to an embodiment of the present invention.
- FIG. 2 is a cross-sectional view schematically showing an electrode manufacturing process according to an embodiment of the present invention.
- FIG. 3 is a cross-sectional view schematically showing an electrode manufacturing process according to an embodiment of the present invention.
- FIG. 4 is a cross-sectional view schematically showing an electrode manufacturing process according to an embodiment of the present invention.
- FIG. 5 is a cross-sectional view schematically showing an electrode manufacturing process according to an embodiment of the present invention.
- FIG. 6 is a cross-sectional view schematically showing an electrode manufacturing process according to an embodiment of the present invention.
- FIG. 7 is a cross-sectional view schematically showing an electrode manufacturing apparatus according to an embodiment of the present invention.
- FIG. 8 is a diagram illustrating a film thickness profile of the composite material layer according to the example and the comparative example.
- FIG. 9 is a diagram schematically showing a battery according to an embodiment of the present invention.
- FIG. 10A is a cross-sectional view schematically showing a manufacturing process of the electrode according to one embodiment of the present invention.
- FIG. 10B is a top view schematically showing a manufacturing process of the electrode according to one embodiment of the present invention.
- FIG. 11 is a side view of a vehicle equipped with a battery according to an embodiment of the present invention.
- the electrode manufacturing method disclosed herein is a method for manufacturing an electrode 30 having a configuration in which a mixture layer 20 including an active material 22 and a first binder 54 is held by a current collector 10 as shown in FIG. .
- the composite material layer 20 is formed by applying a composite paste containing an active material 22 to the current collector 10 and drying it.
- a protrusion 64 made of a polymer is formed on the surface of the current collector 10.
- a binder solution 50 including a binder (first binder) 54 is applied to the current collector 10 from above the polymer protrusions 64 to form a binder solution layer 56.
- the binder solution layer 56 and the mixture paste layer 46 are deposited on the current collector 10 by applying the mixture paste 40 containing the active material 22 from above the binder solution layer 56. To do.
- the deposited binder solution layer 56 and the composite paste layer 46 are dried together to obtain the electrode 30 in which the composite layer 20 is formed on the current collector 10.
- the binder solution layer 56 is formed between the current collector 10 and the composite paste layer 46, and the binder solution layer 56 and the composite paste layer are formed. 46 is dried together, the composite material layer 20 is formed. Therefore, a large amount of the first binder 54 derived from the binder solution layer 56 is arranged at the interface between the current collector 10 and the composite material layer 20. As a result, the amount of binder in the vicinity of the current collector 10 is increased, and the electrode 30 including the mixture layer 20 having good adhesion (bonding strength) to the current collector 10 is obtained.
- the mixture paste layer 46 can be prevented from slipping. That is, when the composite paste 40 is applied from above the binder solution layer 56, the composite paste 40 is repelled by the binder solution layer 56 to cause slipping, and the surface of the composite layer 20 obtained after drying has unevenness.
- the polymer protrusion 64 is formed on the surface of the current collector 10, and the binder solution layer 56 and the mixture paste layer 46 are sequentially deposited thereon. The paste layer 46 is caught on the polymer protrusion 64. As a result, slippage of the composite paste layer 46 is prevented, and the electrode 30 provided with the flat composite layer 20 with less unevenness on the surface can be manufactured.
- the height (h) of the polymer protrusion is preferably larger than the thickness (d) of the binder solution layer 56 as shown in FIG.
- the tip 64a of the polymer protrusion protrudes upward from the upper surface 56a of the binder solution layer, the slip of the composite paste layer 46 can be appropriately suppressed.
- the height of the polymer protrusion 64 is larger than the total thickness of the thickness of the binder solution layer 56 and the thickness of the composite paste layer 46. In this case, since the tip 64a of the polymer projection protrudes upward from the upper surface of the composite paste layer 46, the slip of the composite paste layer 46 can be reliably suppressed.
- the height of the polymer protrusion is preferably 2 ⁇ m to 45 ⁇ m or more, For example, it is more preferably 47 ⁇ m or more.
- the polymer protrusion is provided in at least a range (region) where the composite paste 40 is applied on the surface of the current collector 10.
- the composite paste 40 is applied only to one side of the current collector 10 (which may be part of the single side or the entire range)
- the single-sided composite paste 40 is applied.
- the polymer protrusion is provided within the range to be applied, and when the composite paste 40 is applied to both surfaces of the current collector 10, the polymer protrusion is within the range in which the double-sided composite paste 40 is applied.
- the polymer protrusion is formed in a plurality of independent dots (spots).
- the slip of the composite paste layer 46 can be appropriately prevented by a large number of independent dot-like projections.
- the size of the dot is not particularly limited, but is, for example, about 10 ⁇ m to 100 ⁇ m in diameter.
- Such dot-like projection is preferably formed so as to be 5000 / cm 2 ⁇ distribution number of 150,000 / cm 2 per unit area of the collector.
- the polymer protrusions can be formed by applying a polymer solution 60 containing a polymer 66 to the current collector 10 and then drying it.
- the dot-shaped polymer protrusion can be formed by applying the polymer solution 60 containing the polymer 66 to the current collector 10 by spraying and then drying.
- the polymer constituting the polymer protrusion is not particularly limited as long as it is an adhesive polymer that can adhere to the surface of the current collector, but it preferably functions as a binder in the composite layer.
- the polymer protrusion is preferably made of the same material as the binder used for a typical lithium secondary battery electrode.
- the polymer protrusion 64 functions as a binder in the composite material layer, the adhesion between the composite material layer 20 and the current collector 10 can be further enhanced.
- the polymer constituting the polymer protrusion and the binder contained in the binder solution can be made of the same material.
- examples of the polymer constituting the polymer projection include styrene butadiene rubber (SBR), carboxymethyl cellulose (CMC), polytetrafluoroethylene (PTFE), polyethylene (PE), polyacrylic acid (PAA), and the like.
- SBR styrene butadiene rubber
- CMC carboxymethyl cellulose
- PTFE polytetrafluoroethylene
- PE polyethylene
- PAA polyacrylic acid
- organic solvent polymers such as polyvinylidene fluoride (PVDF) and polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-HFP) are exemplified.
- the solvent 62 constituting the polymer solution may be any solvent that can disperse or dissolve the polymer.
- a water-soluble or water-dispersible polymer water or a mixed solvent mainly composed of water is preferably used.
- a solvent component other than water constituting such a mixed solvent one or more organic solvents (lower alcohol, lower ketone, etc.) that can be uniformly mixed with water can be appropriately selected and used.
- a particularly preferred example is an aqueous solvent substantially consisting of water.
- a non-aqueous solvent for example, N-methylpyrrolidone (NMP) can be used.
- NMP N-methylpyrrolidone
- the polymer concentration (solid content concentration) in the polymer solution is suitably about 5% to 35% by mass, and preferably about 10% to 20% by mass. If the polymer concentration is too high, the applicability of the polymer solution is deteriorated. On the other hand, if the polymer concentration is too low, the drying rate is slow and productivity may be reduced.
- Such an operation of applying the polymer solution 60 to the current collector 10 can be easily performed using a general fluid application technique such as a printing method (inkjet, letterpress, gravure, screen, etc.) or spray spraying. it can.
- a suitable spraying device such as a spray gun
- a predetermined amount of the polymer solution is sprayed on the surface of the current collector 10 to form a dot-like coating material (droplet).
- the solvent 62 in the polymer solution is removed by drying (typically 70 to 160 ° C.) the applied material by an appropriate drying means.
- drying typically 70 to 160 ° C.
- the drying rate of the coating solution (droplet) of the polymer solution is increased by electrostatic energy. Therefore, the polymer protrusion 64 can be formed efficiently (preferably without a drying furnace).
- the method of applying static electricity to the polymer solution coating (droplets) is not particularly limited, and examples thereof include a method of applying a voltage (high-frequency voltage) to the polymer 66 mixed in the polymer solution. By mixing the polymer to which the voltage is applied in this way into the polymer solution, static electricity can be efficiently imparted to the coating solution (droplet) of the polymer solution.
- the amount of voltage applied varies depending on the selection of the polymer and other polymer solution composition, coating conditions, etc., but is appropriately about 5 kV ⁇ ⁇ A or more, usually 40 kV ⁇ ⁇ A or more (for example, 40 kV ⁇ ⁇ A to 200 kV ⁇ ⁇ A). (Range).
- the binder solution 50 containing the binder 54 from above the polymer projections 64. is applied onto the current collector 10 to form a binder solution layer 56.
- a preferred example of the solvent 52 used in the binder solution is an aqueous solvent.
- the aqueous solvent water or a mixed solvent mainly composed of water is preferably used.
- a solvent component other than water constituting such a mixed solvent one or more organic solvents (lower alcohol, lower ketone, etc.) that can be uniformly mixed with water can be appropriately selected and used.
- a particularly preferred example is an aqueous solvent substantially consisting of water.
- the binder solution is not limited to an aqueous solvent, and may be a non-aqueous solvent (a binder dispersion medium is mainly an organic solvent).
- a binder dispersion medium is mainly an organic solvent.
- NMP N-methylpyrrolidone
- the binder (first binder) 54 used in the binder solution is not particularly limited as long as it is the same as that used for a typical lithium secondary battery electrode.
- the binder solution layer is formed using an aqueous solvent (a solution using water or a mixed solvent containing water as a main component as a binder dispersion medium)
- the binder is dispersed or dissolved in water as the binder.
- a polymer can be preferably employed.
- the polymer dispersed or dissolved in water include styrene butadiene rubber (SBR), carboxymethyl cellulose (CMC), polytetrafluoroethylene (PTFE), polyethylene (PE), polyacrylic acid (PAA), and the like.
- SBR styrene butadiene rubber
- CMC carboxymethyl cellulose
- PTFE polytetrafluoroethylene
- PE polyethylene
- PAA polyacrylic acid
- the binder solution layer is formed using a solvent-based solvent (a solution in which the binder dispersion medium is mainly an organic solvent)
- a polymer that is dispersed or dissolved in the solvent-based solvent can be used.
- the polymer that is dispersed or dissolved in the solvent-based solvent include polyvinylidene fluoride (PVDF), polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-HFP), and the like.
- the operation of applying the binder solution to the current collector can be performed using a general fluid application technique such as printing (inkjet, letterpress, gravure, screen, etc.), dispenser, spray spray, nanowire coating, and the like.
- a method of applying the binder solution on the current collector includes a method of applying the binder solution on the current collector using a dispenser.
- the binder solution layer 56 having a uniform thickness can be formed.
- the thickness of the binder solution layer is not particularly limited, but can usually be 1.5 ⁇ m to 6 ⁇ m, for example, about 2 ⁇ m to 4 ⁇ m is appropriate.
- the coating amount of the binder solution (coating amount per unit area) is not particularly limited. However, if the coating amount of the binder solution is too small, the amount of the binder in the binder solution layer is excessively reduced and the current collector and the composite layer The effect of increasing the adhesive strength may not be obtained. On the other hand, if the amount of the binder solution applied is too large, the amount of the binder in the binder solution layer may increase so that the interface resistance between the current collector and the composite material layer may increase. Therefore, the coating amount of the binder solution is approximately 0.01 mg / cm 2 to 0.05 mg / cm 2 , usually 0.02 mg in terms of solid content (that is, in terms of the mass of the binder after drying). / Cm 2 to 0.03 mg / cm 2 is preferably adjusted.
- the binder solution layer 56 and the mixture paste layer 46 are applied by applying the mixture paste 40 from above the binder solution layer 56. Is deposited on the current collector 10.
- the composite paste is prepared by mixing an active material (typically powder) 22 and other composite material layer forming components (for example, a binder 44) used as necessary in a suitable solvent 42. Can be prepared.
- an active material typically powder
- other composite material layer forming components for example, a binder 44
- the active material (typically powder) 22 is not particularly limited as long as it is the same as that used for a typical lithium ion secondary battery.
- Representative examples of the negative electrode active material 22 used for the negative electrode include carbon-based materials such as graphite carbon and amorphous carbon, lithium transition metal composite oxides (lithium titanium composite oxides, etc.), lithium transition metal composite nitrides, and the like.
- the above-mentioned composite paste can contain a material used for a composite paste for forming a composite layer in the production of a general electrode, if necessary.
- a representative example of such a material is a conductive material and a binder (second binder) 44.
- the conductive material carbon powder such as carbon black (acetylene black or the like), conductive metal powder such as nickel powder, or the like can be used.
- the binder 44 plays a role of binding the active material particles.
- the binder 44 may be the same material as the binder 54 included in the binder solution layer 56 or a different material.
- the solvent 42 used in the composite paste include water or a mixed solvent mainly composed of water (aqueous solvent).
- a solvent other than water constituting such a mixed solvent one or more organic solvents (lower alcohol, lower ketone, etc.) that can be uniformly mixed with water can be appropriately selected and used.
- the solvent 42 is not limited to an aqueous solvent, and may be a non-aqueous solvent.
- the non-aqueous solvent for example, N-methylpyrrolidone (NMP) can be used.
- the operation of applying the composite paste 40 to the current collector 10 is the same as that of the conventional method except that the current collector is formed with the polymer protrusion 64 and the binder solution layer 56 formed on the surface as described above. This can be carried out in the same manner as the production of a general lithium secondary battery electrode.
- the composite paste layer 46 is formed by applying a predetermined amount of the composite paste 40 onto the current collector 10 from above the binder solution layer 56 using an appropriate application device (a die coater or the like). obtain.
- the composite paste 40 when the composite paste 40 is applied from above the binder solution layer 56, the composite paste 40 is repelled by the binder solution layer 56, causing slippage, and unevenness may occur on the surface of the composite paste layer 46.
- the polymer protrusion 64 is formed on the surface of the current collector 10, and the binder solution layer 56 and the composite paste layer 46 are sequentially deposited thereon. It catches on the protrusion 64. As a result, slippage of the composite paste layer 46 can be prevented and the application can be performed stably.
- the binder solution layer 56 and the composite paste layer 46 are deposited on the current collector 10 in this manner, the deposited binder solution layer 56 and the composite paste layer 46 are then dried together as shown in FIG. By doing so, the electrode 30 in which the composite material layer 20 is formed on the current collector 10 is obtained.
- the drying temperature may be a temperature range in which both the solvent 52 of the binder solution layer and the solvent 42 of the composite paste layer can be volatilized.
- the drying temperature can be about 70 ° C. to 160 ° C., and is usually preferably 80 ° C. to 150 ° C.
- the manufacture of the electrode 30 according to this embodiment is completed.
- the thickness and density of the composite layer 20 can be adjusted by performing an appropriate press process (for example, roll press process) as needed.
- FIG. 5 schematically shows a cross-sectional structure of an electrode 30 for a lithium secondary battery that is preferably manufactured by applying the electrode manufacturing method disclosed herein.
- the electrode 30 has a configuration in which the composite material layer 20 including the active material 22 is held by the current collector 10.
- the composite material layer 20 has a polymer protrusion 64 formed on the surface of the current collector, and a binder solution layer 56 and a composite paste layer 46 are sequentially deposited thereon, and then a binder solution. It is formed by drying the layer 56 and the composite paste layer 46 together.
- the binder solution layer 56 is formed between the current collector 10 and the mixture paste layer 46, and the binder solution layer 56 and the mixture paste layer 46 are dried together to thereby form the mixture layer. 20 is formed, a large amount of the binder 54 derived from the binder solution layer 56 is arranged at the interface between the current collector 10 and the composite material layer 20. As a result, the amount of binder in the vicinity of the current collector 10 is increased, and the electrode 30 including the mixture layer 20 having good adhesion (adhesive strength) to the current collector 10 is obtained.
- the polymer protrusion 64 is formed on the surface of the current collector 10, and the binder solution layer 56 and the composite paste layer 46 are sequentially deposited thereon. The polymer projection 64 is caught. This prevents slipping of the composite paste layer 46, and an electrode 30 provided with the flat composite layer 20 with less unevenness on the surface is obtained. Furthermore, according to this embodiment, since the polymer protrusion 64 functions as a binder, the adhesion between the composite material layer 20 and the current collector 10 can be further enhanced.
- the binder solution 50 is configured to maintain a state separated from the composite paste 40 for at least a certain time. Specifically, as shown in FIG. 4, at least a period from the time when the composite paste 40 is applied onto the binder solution layer 56 to the time of drying (approximately 0.1 seconds or more, for example, about 1 second to 90 seconds or more) As described above, usually two seconds to 10 seconds or more are formed) to form a state in which two liquid layers of the binder solution layer 56 and the composite paste layer 46 are deposited (liquid phase two-layer state). It is configured to be able to.
- the composite paste layer 46 is at least approximately ( For example, the configuration of the drying furnace, the drying conditions (temperature, time, air volume, etc.), the current carrying speed of the current collector, and the like are adjusted so that the solvent is dried (so that 50% by volume of the solvent is volatilized and removed). This suppresses the mixing of the binder solution layer 56 and the composite paste layer 46 at least during the period from the application of the composite paste 40 onto the binder solution layer 56 to the drying, and therefore the vicinity of the current collector 10. In addition, the first binder 54 can be properly retained.
- the formation of the liquid phase two-layer state can be realized, for example, by increasing the viscosity of at least one of the binder solution and the composite paste.
- the viscosity of at least one of the binder solution and the composite paste may be adjusted to 1000 mPa ⁇ s (B-type viscometer rotor, 20 rpm, 20 ° C.) or more.
- the viscosity on the high-viscosity side is suitably about 1000 mPa ⁇ s or more, usually preferably 2000 mPa ⁇ s or more, and more preferably 3000 mPa ⁇ s or more, for example.
- the upper limit of the viscosity on the high-viscosity side is not particularly limited, but from the viewpoint of applicability, it is generally about 20000 mPa ⁇ s, and is preferably 10000 mPa ⁇ s or less (for example, 8000 mPa ⁇ s or less).
- the viscosity of one of the binder solution and the composite paste is adjusted to 2000 mPa ⁇ s or more (preferably 3000 mPa ⁇ s or more), and the other viscosity (viscosity on the low viscosity side) is adjusted.
- the viscosity difference between the binder solution and the composite paste is appropriately about 1000 mPa ⁇ s or more, and is usually preferably 2000 mPa ⁇ s or more, for example, 2500 Pa ⁇ s or more (eg, about 2500 Pa or more). More preferably, it is in the range of s to 8000 Pa ⁇ s, for example 2600 Pa ⁇ s or more, and further 2900 Pa ⁇ s or more.
- the high viscosity side is a composite paste
- the low viscosity side is a binder solution.
- the viscosity of the binder solution and the composite paste can be adjusted, for example, by appropriately adjusting the solid content ratio in the liquid.
- the viscosity of the composite paste can be adjusted by appropriately adjusting the solid content concentration of the active material, the binder, and other composite layer forming components (for example, a conductive material) in the composite paste.
- the viscosity of the binder solution can be adjusted by appropriately adjusting the binder concentration in the binder solution. Or you may adjust so that the said viscosity may become a suitable range by adding a thickener (typically polymer material).
- a thickener typically polymer material
- the same solvent for example, a common aqueous solvent
- Other methods for realizing the liquid phase two-layer state include a method of providing an SP value difference.
- the SP value difference between the binder solution and the composite paste is adjusted to be 2.0 or more.
- the above SP value difference is suitably about 2 or more, and is usually preferably 2 to 25, more preferably 5 to 20, for example.
- the SP value difference in the preferred range can be realized, for example, by appropriately selecting the solvent of the composite paste and the solvent of the binder solution.
- the solvent of the composite paste is water (SP value 23.4) or N-methylpyrrolidone (SP value 11.3)
- the solvent of the binder solution is carbon tetrachloride (SP value 8.6) or fluorine type.
- a liquid can be preferably used.
- other material components active material, binder, other composite material layer forming components constituting the composite material paste and the binder solution are appropriately selected. As a result, the SP difference in the preferred range can be realized.
- mixing suppression include a method of imparting a specific gravity difference.
- the specific gravity of the binder solution is adjusted to be larger than the specific gravity of the composite paste. By providing such a specific gravity difference, the mixing can be appropriately suppressed.
- the methods for realizing the liquid phase two-layer state described above can be used alone or in combination.
- the long sheet-shaped current collector 10 is unwound from an unillustrated unwinding portion, and is conveyed through the apparatus 90 by the rotation of rollers 91 and 92.
- a spraying device 95, a drying furnace 97, a dispenser device 94, a die coater 96, and a drying furnace 98 are arranged in order from the upstream side in the conveyance path of the current collector 10.
- the spray spraying device 95 contains the polymer solution 60 and sprays the polymer solution 60 onto the surface of the current collector 10 being conveyed. Thereafter, the polymer solution 60 is dried by passing through a drying furnace 97, whereby dot-like polymer projections are formed on the current collector.
- the dispenser device 94 accommodates the binder solution 50, and the binder solution 50 is applied on the current collector 10 being transported from above the polymer protrusions in a strip shape.
- the die coater 96 accommodates the composite paste 40, and the composite paste 40 is applied in a strip shape on the current collector 10 being conveyed (from above the binder solution layer). Then, the negative electrode sheet 30 in which the composite material layer 20 is formed on the current collector is obtained by passing the drying furnace 98 and drying the binder solution and the composite material paste. The negative electrode sheet 30 is taken up by the take-up unit 99 and then subjected to the next step.
- styrene butadiene rubber (SBR) as the polymer material 66 is dispersed in water to prepare a polymer solution 60 (solid content concentration 12 wt%), which is formed into a long sheet-like copper foil (current collector).
- the copper foil 10 with the dot-like polymer projections 64 provided on the surface was obtained by applying and drying on the surface of the body 10 with a spray gun (manufactured by Nordson).
- the polymer solution is applied by moving the discharge port of the spray gun at a distance of 200 mm from the surface of the current collector (copper foil) at a speed of 60 m / min and spraying the polymer solution from the discharge port at a rate of 100 g / min. Was done.
- styrene butadiene rubber (SBR) as the binder 54 was dispersed in water to prepare a binder solution 50 (solid content concentration 10%) having a viscosity of 80 mPa ⁇ s.
- carbon powder as the negative electrode active material 22 and carboxymethyl cellulose (CMC) as the thickener are dispersed in water so that the mass ratio of these materials is 99: 1, and the viscosity is 3000 mPa ⁇ s.
- a material paste was prepared. The binder solution is applied onto the current collector (copper foil) from above the polymer protrusion 64 to deposit the binder solution layer 56, and the composite paste 40 is applied from above the binder solution layer 56 to form the composite paste layer. 46 was deposited.
- a negative electrode sheet 30 in which the composite material layer 20 was provided on the current collector (copper foil) 10 was obtained.
- the viscosity of the binder solution and the composite paste was measured using a B-type viscometer after adjusting the liquid temperature to 20 ° C. and rotating the rotor at 20 rpm.
- a negative electrode sheet was prepared without forming the polymer protrusion 64 on the surface of the current collector (copper foil).
- a negative electrode sheet was obtained in the same manner as in Example except that the polymer protrusion 64 was not formed.
- a negative electrode sheet (normal electrode) was prepared in the same manner as in the past (without applying the binder solution to the copper foil). Specifically, carbon powder as a negative electrode active material, SBR as a binder, and CMC as a thickener are dispersed in water so that the mass ratio of these materials is 98: 1: 1. A paste was prepared, applied to a current collector (copper foil) and dried to obtain a negative electrode sheet having a negative electrode mixture layer provided on the surface of the current collector.
- the surface shape (film thickness profile) of the composite layer according to each example obtained in this way was measured and evaluated.
- the surface shape (film thickness profile) of the composite material layer was measured using a laser displacement meter manufactured by Lasertec. The result is shown in FIG.
- a negative electrode (negative electrode sheet) 30 manufactured using a current collector having a polymer protrusion formed on the surface is used as the negative electrode (negative electrode sheet) 30.
- the electrode manufacturing method disclosed here can be applied to manufacture of both the positive electrode and the negative electrode.
- the lithium secondary battery 100 includes a case 82 made of metal (a resin or a laminate film is also suitable).
- the case (outer container) 82 includes a flat cuboid case main body 84 having an open upper end, and a lid 86 that closes the opening.
- a long sheet-like positive electrode (positive electrode sheet) 70 and a long sheet-like negative electrode (negative electrode sheet) 30 are laminated together with a total of two long sheet-like separators (separator sheets) 76.
- a flat wound electrode body 80 produced by winding and then crushing the resulting wound body from the side direction and kidnapping is housed.
- the negative electrode sheet 30 has a configuration in which a negative electrode mixture layer 20 mainly composed of a negative electrode active material is provided on both surfaces of a long sheet-like negative electrode current collector 10.
- the positive electrode sheet 70 has a configuration in which a positive electrode mixture layer mainly composed of a positive electrode active material is provided on both surfaces of a long sheet-like positive electrode current collector. At one end in the width direction of these electrode sheets 30 and 70, an electrode mixture layer non-formed portion in which the electrode mixture layer is not provided on any surface is formed.
- the positive electrode sheet 70 and the negative electrode mixture layer non-formed portion of the positive electrode sheet 70 and the negative electrode mixture layer non-formed portion of the negative electrode sheet 30 protrude from both sides of the separator sheet 76 in the width direction.
- the negative electrode sheet 30 is overlaid with a slight shift in the width direction.
- the electrode composite material layer non-forming portions of the positive electrode sheet 70 and the negative electrode sheet 30 are respectively wound core portions (that is, the positive electrode composite material layer forming portion of the positive electrode sheet 70). And a portion where the negative electrode active material layer forming portion of the negative electrode sheet 30 and the two separator sheets 76 are wound tightly).
- a positive electrode lead terminal 78 and a negative electrode lead terminal 79 are respectively attached to the protruding portion (that is, the non-formed portion of the positive electrode mixture layer) 70A and the protruding portion (that is, the non-formed portion of the negative electrode active material layer) 30A. Are electrically connected to the positive terminal 72 and the negative terminal 74 described above.
- the constituent elements other than the negative electrode sheet 30 constituting the wound electrode body 80 may be the same as those of the electrode body of the conventional lithium secondary battery, and are not particularly limited.
- the positive electrode sheet 70 can be formed by providing a positive electrode mixture layer mainly composed of a positive electrode active material for a lithium secondary battery on a long positive electrode current collector.
- a positive electrode current collector an aluminum foil or other metal foil suitable for the positive electrode is preferably used.
- the positive electrode active material one kind or two or more kinds of substances conventionally used in lithium secondary batteries can be used without any particular limitation.
- Preferable examples include lithium transition metal composite oxides containing lithium and one or more transition metal elements as constituent metal elements such as LiMn 2 O 4 , LiCoO 2 , and LiNiO 2 as main components. .
- separator sheet 76 used between the positive and negative electrode sheets 70 and 30 is a sheet made of a porous polyolefin resin.
- a separator may not be necessary (that is, in this case, the electrolyte itself can function as a separator).
- the wound electrode body 80 is accommodated in the main body 84 from the upper end opening of the case main body 84 and an electrolytic solution containing an appropriate electrolyte is disposed (injected) in the case main body 84.
- the electrolyte is lithium salt such as LiPF 6, for example.
- a nonaqueous electrolytic solution obtained by dissolving a suitable amount (for example, concentration 1M) of a lithium salt such as LiPF 6 in a mixed solvent of diethyl carbonate and ethylene carbonate (for example, a mass ratio of 1: 1) can be used.
- the opening is sealed by welding or the like with the lid 86, and the assembly of the lithium secondary battery 100 according to the present embodiment is completed.
- the sealing process of the case 82 and the process of placing (injecting) the electrolyte may be the same as those used in the production of a conventional lithium secondary battery, and do not characterize the present invention. In this way, the construction of the lithium secondary battery 100 according to this embodiment is completed.
- the lithium secondary battery 100 constructed in this manner is constructed using at least one of the electrodes manufactured using the current collector having the anti-slip protrusion formed on the surface described above, It shows excellent battery performance. For example, providing the lithium secondary battery 100 satisfying at least one (preferably all) of high cycle durability, excellent output characteristics, and good productivity by constructing a battery using the above electrodes. can do.
- the shape of the polymer protrusion is not limited to the dot shape.
- the polymer protrusion 64 can be formed in a patterned convex shape. Even in this case, slipping of the composite paste layer can be appropriately suppressed by the patterned uneven projection 64.
- Such polymer protrusions 64 can be formed, for example, by pattern-printing a polymer solution containing a polymer on a current collector and then drying.
- a method for manufacturing a battery electrode including a composite layer having good adhesion to a current collector and good surface flatness it is possible to provide a method for manufacturing a battery electrode including a composite layer having good adhesion to a current collector and good surface flatness.
- the battery according to the present invention (for example, a lithium secondary battery) has excellent battery performance as described above, it can be suitably used as a power source for a motor (electric motor) mounted on a vehicle such as an automobile. Therefore, the present invention, as schematically shown in FIG. 11, is a vehicle (typically an automobile, particularly a hybrid automobile, an electric automobile, a fuel cell automobile) provided with such a battery (which may be in the form of an assembled battery) 100 as a power source. An automobile equipped with an electric motor such as 1) is provided.
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Abstract
Description
Claims (12)
- 活物質とバインダを含む合材層が集電体に保持された構成の電池用電極を製造する方法であって、
集電体の表面にポリマーからなる突起物を形成する工程と、
前記ポリマー突起物の上からバインダを含むバインダ溶液を集電体上に塗布してバインダ溶液層を形成する工程と、
前記バインダ溶液層の上から活物質を含む合材ペーストを塗布することによって、前記バインダ溶液層と合材ペースト層とを集電体上に堆積する工程と、
前記堆積したバインダ溶液層と合材ペースト層とを共に乾燥させることによって、前記集電体上に合材層が形成された電極を得る工程と
を包含する、電池用電極の製造方法。 - 前記ポリマー突起物の高さは、前記バインダ溶液層の厚みよりも大きい、請求項1に記載の製造方法。
- 前記ポリマー突起物の高さは、前記バインダ溶液層の厚みと前記合材ペースト層の厚みとを合わせた合計厚みよりも大きい、請求項1または2に記載の製造方法。
- 前記ポリマー突起物をドット状に形成する、請求項1から3の何れか一つに記載の製造方法。
- 前記ポリマー突起物をパターニングされた凸状に形成する、請求項1から3の何れか一つに記載の製造方法。
- 前記ポリマー突起物を、ポリマーを含むポリマー溶液を集電体に塗布した後、乾燥することにより形成する、請求項1から5の何れか一つに記載の製造方法。
- 前記ポリマー溶液の塗布をスプレー噴霧により行う、請求項6に記載の製造方法。
- 前記ポリマー溶液の塗布物に対して静電気を付与する、請求項6または7に記載の製造方法。
- 前記ポリマー突起物は、前記合材層においてバインダとして機能する、請求項1から8の何れか一つに記載の製造方法。
- 前記ポリマー突起物は、前記バインダ溶液に含まれるバインダと同じ材料で構成されている、請求項1から9の何れか一つに記載の製造方法。
- 請求項1から10のいずれか一つに記載の方法により製造された電極を用いて構築された電池。
- 請求項11に記載の電池を搭載した車両。
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PCT/JP2010/056533 WO2011128963A1 (ja) | 2010-04-12 | 2010-04-12 | 電池用電極の製造方法 |
CN2010800044955A CN102292850B (zh) | 2010-04-12 | 2010-04-12 | 电池用电极的制造方法 |
US13/130,767 US8911900B2 (en) | 2010-04-12 | 2010-04-12 | Battery electrode production method |
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