WO2011155060A1 - リチウム二次電池およびその製造方法 - Google Patents
リチウム二次電池およびその製造方法 Download PDFInfo
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- WO2011155060A1 WO2011155060A1 PCT/JP2010/059933 JP2010059933W WO2011155060A1 WO 2011155060 A1 WO2011155060 A1 WO 2011155060A1 JP 2010059933 W JP2010059933 W JP 2010059933W WO 2011155060 A1 WO2011155060 A1 WO 2011155060A1
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- porous layer
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- secondary battery
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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
- 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
- H01M10/058—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
- H01M4/13—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
- H01M4/36—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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/449—Separators, membranes or diaphragms characterised by the material having a layered structure
- H01M50/451—Separators, membranes or diaphragms characterised by the material having a layered structure comprising layers of only organic material and layers containing inorganic material
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/449—Separators, membranes or diaphragms characterised by the material having a layered structure
- H01M50/457—Separators, membranes or diaphragms characterised by the material having a layered structure comprising three or more layers
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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
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
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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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y02T10/00—Road transport of goods or passengers
- Y02T10/60—Other road transportation technologies with climate change mitigation effect
- Y02T10/70—Energy storage systems for electromobility, e.g. 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
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T29/00—Metal working
- Y10T29/49—Method of mechanical manufacture
- Y10T29/49002—Electrical device making
- Y10T29/49108—Electric battery cell making
- Y10T29/49115—Electric battery cell making including coating or impregnating
Definitions
- the present invention relates to a lithium secondary battery, and more particularly to a lithium secondary battery with improved durability against charge / discharge cycles and a method for manufacturing the same.
- lithium ion batteries In recent years, lithium ion batteries, nickel metal hydride batteries, and other secondary batteries have become increasingly important as on-vehicle power supplies or personal computers and portable terminals.
- a lithium ion battery that is lightweight and obtains a high energy density is expected to be preferably used as a high-output power source mounted on a vehicle.
- charging and discharging are performed by lithium ions traveling between the positive electrode and the negative electrode.
- Patent Documents 1 to 4 are known as conventional techniques related to this type of secondary battery.
- lithium ion batteries are assumed to be used in such a manner that charging / discharging (rapid charging / discharging) at a high rate is repeated.
- a lithium ion battery used as a power source for a vehicle for example, a lithium ion battery mounted on a hybrid vehicle that uses a lithium ion battery and another power source having different operating principles such as an internal combustion engine as a power source
- the present invention has been made in view of such a point, and a main object thereof is to provide a lithium secondary battery with improved cycle durability against charge and discharge.
- the inventor of the present application focused on the fact that in a lithium secondary battery provided with a wound electrode body, when discharging and charging are repeated continuously, an event in which the battery capacity is significantly reduced is observed. Then, the influence which the repetition of this charging / discharging has on the lithium secondary battery was analyzed in detail.
- the amount of the electrolyte in the electrode is insufficient at the time of charging / discharging in the winding center, so that the charge / discharge performance of the entire battery is lowered.
- the battery reaction concentrates on the portion where the amount of the electrolytic solution is relatively large (that is, the outer portion of the winding), the deterioration of the portion is promoted. Any of these events can be a factor of reducing the durability (deteriorating battery capacity) of the lithium secondary battery with respect to the charge / discharge cycle.
- the present invention improves the durability of the lithium secondary battery against charge / discharge cycles by an approach of eliminating or mitigating the electrolyte withering at the winding center of the wound electrode body.
- the lithium secondary battery provided by the present invention is a lithium secondary battery including a wound electrode body in which a positive electrode sheet and a negative electrode sheet are wound through a separator sheet.
- a porous layer is formed on the surface of at least one of the positive electrode sheet, the negative electrode sheet, and the separator sheet constituting the wound electrode body over the longitudinal direction of the sheet.
- the wound center part site located on the wound center side
- the wound outer side part site located on the wound outside
- a porous layer is formed on the surface of at least one of the positive electrode sheet, the negative electrode sheet, and the separator sheet, and the winding center portion of the porous layer is thicker than the winding outer portion. .
- the amount of the electrolytic solution penetrating into the winding center portion of the wound electrode body is increased, and the liquid retaining property of the winding center portion is improved.
- the amount of electrolyte at the center of rotation can be kept appropriate. As a result, durability against charge / discharge cycles (for example, capacity retention after charge / discharge cycles) can be improved.
- the sheet formed with the porous layer in the winding direction of the wound electrode body, is formed up to 20% from the end portion on the winding center side of the wound electrode body.
- the average thickness of the formed porous layer may be larger than the average thickness of the porous layer formed up to 20% from the end portion on the wound outer side of the wound electrode body.
- the porous layer is formed so as to gradually become thicker from the winding outer side of the wound electrode body toward the winding center side. Thereby, it can suppress more reliably that electrolyte solution withering by a non-aqueous electrolyte being extruded from the winding center part.
- the porous layer has a thickest thickest part and a thinnest thinnest part.
- the difference in thickness between the thickest part and the thinnest part is 2 ⁇ m to 4 ⁇ m. If it is smaller than this range (typically less than 2 ⁇ m), the liquid retention effect at the center of winding is reduced, and the cycle durability improvement effect as described above may not be obtained. If it is larger than this range (typically over 4 ⁇ m), the difference in distance between the electrode plates is too large between the winding center and the winding outer side, resulting in non-uniform battery reaction and cycle durability. It can be a downward trend.
- the porosity of the porous layer is 45% to 65%. If it is smaller than this range (typically below 45%), the porous layer itself acts as a resistance component, so that the cycle durability may tend to be lower than when there is no porous layer. If it is larger than this range (typically more than 65%), it may be impossible to sufficiently suppress heat generation during an internal short circuit.
- the porous layer is formed on the surface of the separator sheet.
- the porous layer is formed on the surface of the separator sheet on the negative electrode sheet side. In this case, compared with the case where it forms on the surface of a negative electrode sheet, while manufacturing cost becomes cheap, a porous layer can be formed, without affecting input-output characteristics.
- the present invention also provides a method for manufacturing any of the lithium secondary batteries disclosed herein.
- This manufacturing method includes a step of forming a porous layer by applying a coating material for forming a porous layer on the surface of at least one of a traveling positive electrode sheet, negative electrode sheet, and separator sheet by an application means and drying.
- the coating material for forming a porous layer is applied while changing the traveling speed of the sheet.
- seat can be formed easily.
- the application means is a gravure roll.
- the said coating material for porous layer formation is apply
- seat can be formed easily.
- any of the lithium secondary batteries disclosed herein has performance suitable for a battery mounted on a vehicle (for example, high output can be obtained), and can be particularly excellent in durability against high-rate charge / discharge. . Therefore, according to this invention, the vehicle provided with one of the lithium secondary batteries disclosed here is provided.
- a vehicle for example, an automobile
- the lithium secondary battery as a power source (typically, a power source of a hybrid vehicle or an electric vehicle) is provided.
- lithium that can be used in a charge / discharge cycle including a high rate charge / discharge of 50 A or more (for example, 50 A to 250 A), or even 100 A or more (for example, 100 A to 200 A) is envisaged.
- Secondary battery; a large capacity type having a theoretical capacity of 1 Ah or more (more than 3 Ah), and a charge / discharge cycle including high rate charge / discharge of 2C or more (for example, 2C to 50C) or even 10C or more (for example, 10C to 40C) Examples are lithium secondary batteries that are supposed to be used.
- FIG. 1 is a side view schematically showing a lithium secondary battery according to an embodiment of the present invention.
- 2 is a cross-sectional view taken along line II-II in FIG.
- FIG. 3 is a diagram schematically showing a wound electrode body of a lithium secondary battery according to an embodiment of the present invention.
- FIG. 4 is an enlarged cross-sectional view showing the main part of the sheet-like electrode body of the lithium secondary battery according to one embodiment of the present invention.
- FIG. 5 is a diagram schematically showing a coating apparatus according to an embodiment of the present invention.
- FIG. 6 is a diagram schematically showing a porous layer forming step according to an embodiment of the present invention.
- FIG. 7 is a side view schematically showing a vehicle including a lithium secondary battery according to an embodiment of the present invention.
- lithium secondary battery lithium ion battery
- a wound electrode body wound electrode body
- a non-aqueous electrolyte are contained in a cylindrical container
- FIG. 1 to 3 show a schematic configuration of a lithium ion battery according to an embodiment of the present invention. *
- the lithium secondary battery 100 includes an electrode body 80 (winding electrode body) 80 in which a long positive electrode sheet 10 and a long negative electrode sheet 20 are wound through a long separator 40. It has the structure accommodated in the container 50 of the shape (cylindrical type) which can accommodate this winding electrode body 80 with the nonaqueous electrolyte solution which is not shown in figure.
- the container 50 includes a bottomed cylindrical container main body 52 having an open upper end and a lid 54 that closes the opening.
- a metal material such as aluminum, steel, or Ni-plated SUS is preferably used (Ni-plated SUS in the present embodiment).
- a positive electrode terminal 70 that is electrically connected to the positive electrode 10 of the wound electrode body 80 is provided on the upper surface (that is, the lid body 54) of the container 50.
- a negative electrode terminal 72 (in this embodiment also serves as the container main body 52) that is electrically connected to the negative electrode 20 of the wound electrode body 80 is provided.
- a wound electrode body 80 is accommodated together with a non-aqueous electrolyte (not shown).
- the wound electrode body 80 according to the present embodiment is the same as the wound electrode body of a normal lithium ion battery except for the configuration of the separator 40 described later, and as shown in FIG. A long sheet structure (sheet-like electrode body) 88 is provided at the stage before assembly.
- the positive electrode sheet 10 has a structure in which a positive electrode active material layer 14 containing a positive electrode active material is held on both surfaces of a long sheet-like foil-shaped positive electrode current collector 12. However, the positive electrode active material layer 14 is not attached to one side edge (the lower side edge portion in the figure) along the edge in the width direction of the positive electrode sheet 10, and the positive electrode current collector 12 has a constant width. An exposed positive electrode active material layer non-forming portion is formed.
- the negative electrode sheet 20 has a structure in which a negative electrode active material layer 24 containing a negative electrode active material is held on both surfaces of a long sheet-like foil-shaped negative electrode current collector 22.
- the negative electrode active material layer 24 is not attached to one side edge (the upper side edge portion in the figure) along the edge in the width direction of the negative electrode sheet 20, and the negative electrode current collector 22 is exposed with a certain width.
- a negative electrode active material layer non-formed portion is formed.
- the positive electrode sheet 10 and the negative electrode sheet 20 are laminated via two separator sheets 40 to produce a sheet-like electrode body 88.
- the positive electrode sheet 10 and the negative electrode sheet 20 are formed such that the positive electrode active material layer non-formed portion of the positive electrode sheet 10 and the negative electrode active material layer non-formed portion of the negative electrode sheet 20 protrude from both sides in the width direction of the separator sheet 40. Are overlapped slightly in the width direction.
- the wound electrode body 80 can be produced by winding the sheet-like electrode body 88 produced by overlapping in this way.
- a wound core portion 82 (that is, the positive electrode active material layer 14 of the positive electrode sheet 10, the negative electrode active material layer 24 of the negative electrode sheet 20, and the separator sheet 40) is densely arranged in the central portion of the wound electrode body 80 in the winding axis direction. Laminated portions) are formed. In addition, the electrode active material layer non-formed portions of the positive electrode sheet 10 and the negative electrode sheet 20 protrude outward from the wound core portion 82 at both ends in the winding axis direction of the wound electrode body 80.
- a positive electrode lead terminal 74 and a negative electrode lead terminal 76 are respectively provided on the protruding portion 84 (that is, a portion where the positive electrode active material layer 14 is not formed) 84 and the protruding portion 86 (that is, a portion where the negative electrode active material layer 24 is not formed) 86. Attached and electrically connected to the above-described positive electrode terminal 70 and negative electrode terminal 72 (here, the container body 52 also serves).
- the components constituting the wound electrode body 80 may be the same as those of the conventional wound electrode body of the lithium ion battery except for the separator sheet 40, and are not particularly limited.
- the positive electrode sheet 10 can be formed by applying a positive electrode active material layer 14 mainly composed of a positive electrode active material for a lithium ion battery on a long positive electrode current collector 12.
- a positive electrode active material layer 14 mainly composed of a positive electrode active material for a lithium ion battery on a long positive electrode current collector 12.
- an aluminum foil or other metal foil suitable for the positive electrode is preferably used.
- the positive electrode active material one type or two or more types of materials conventionally used in lithium ion batteries can be used without any particular limitation.
- lithium and a transition metal element such as lithium nickel oxide (LiMn 2 O 4 ), lithium cobalt oxide (LiCoO 2 ), and lithium manganese oxide (LiNiO 2 ) are used.
- a positive electrode active material mainly containing an oxide (lithium transition metal oxide) containing as a constituent metal element.
- the negative electrode sheet 20 can be formed by applying a negative electrode active material layer 24 mainly composed of a negative electrode active material for a lithium ion battery on a long negative electrode current collector 22.
- a negative electrode active material layer 24 mainly composed of a negative electrode active material for a lithium ion battery on a long negative electrode current collector 22.
- a copper foil or other metal foil suitable for the negative electrode is preferably used.
- the negative electrode active material one or more of materials conventionally used in lithium ion batteries can be used without any particular limitation.
- Preferable examples include carbon-based materials such as graphite carbon and amorphous carbon, lithium-containing transition metal oxides and transition metal nitrides.
- separator sheet 40 suitable for use between the positive and negative electrode sheets 10 and 20 examples include those made of a porous polyolefin resin.
- a porous separator sheet made of synthetic resin for example, made of polyolefin such as polyethylene
- synthetic resin for example, made of polyolefin such as polyethylene
- the porous layer 60 is formed on the surface of the separator sheet 40 constituting the wound electrode body.
- the porous layer 60 is formed over the longitudinal direction of the separator sheet.
- the porous layer 60 is formed on the surface 46 on the negative electrode sheet side of the separator sheet, which is an interface between the separator sheet and the negative electrode sheet.
- the porous layer 60 includes metal compound particles and a binder (binder), and the metal compound particles and the metal compound particles and the separator sheet are bonded to each other by the binder.
- the metal compound particles constituting the porous layer those having heat resistance and electrochemically stable within the battery use range are preferable.
- Preferred examples include alumina (Al 2 O 3 ), alumina hydrate (eg boehmite (Al 2 O 3 .H 2 O)), magnesium hydroxide (Mg (OH) 2 ), magnesium carbonate (MgCO 3 ), and the like. Is exemplified.
- alumina or alumina hydrate is preferable because it has high Mohs hardness and can improve the durability of the porous layer.
- the binder used in the porous layer is for bonding metal compound particles, and the material constituting the binder is not particularly limited, and various materials can be widely used.
- Preferable examples include acrylic resins.
- acrylic resin monomers such as acrylic acid, methacrylic acid, acrylamide, methacrylamide, 2-hydroxyethyl acrylate, 2-hydroxyethyl methacrylate, methacrylate, methyl methacrylate, ethylhexyl acrylate, butyl acrylate, etc. were polymerized in one kind.
- a homopolymer is preferably used.
- the acrylic resin may be a copolymer obtained by polymerizing two or more of the above monomers.
- polyvinylidene fluoride polytetrafluoroethylene (PTFE)
- PTFE polytetrafluoroethylene
- polyacrylonitrile polymethyl methacrylate
- the ratio of the metal compound particles in the entire porous layer is preferably about 90% by mass or more (typically 90 to 98% by mass), preferably about 92 to 96% by mass. Preferably there is. Further, the ratio of the binder in the entire porous layer can be, for example, 2 to 10% by mass, and is preferably about 4 to 8% by mass.
- FIG. 4 is a schematic cross-sectional view showing a part of a cross section along the longitudinal direction of the sheet-like electrode body 88, which is a stage before constructing the wound electrode body, and includes a separator sheet 40 and the separator sheet.
- the porous layer 60 provided on the surface of 40 is shown.
- the left side in the figure is the winding center side (winding start side), and the right side is the winding outside (winding end side).
- the porous layer 60 is formed over the longitudinal direction of the separator sheet 40.
- the porous layer 60 includes metal compound particles 61 and a binder (not shown), and the metal compound particles 61 and the metal compound particles 61 and the separator sheet 40 are bonded to each other by the binder.
- a large number of pores 63 are formed between the adjacent metal compound particles 61 at sites not bound by the binder, and the nonaqueous electrolyte can be held in the pores 63 (that is, in the porous layer). Can be infused with non-aqueous electrolyte).
- the winding center portion (portion located on the winding center side) 62 in the winding direction of the winding electrode body (longitudinal direction of the sheet 40) is the winding outer portion (positioned on the winding outer side). Thicker than 64).
- the porous layer 60 is formed so as to gradually increase in thickness from the winding outer side of the wound electrode body toward the winding center side.
- the thickness (D1) of the winding center part 62 provided at one end in the winding direction (longitudinal direction) of the porous layer is the winding provided at the other end in the winding direction (longitudinal direction) of the porous layer. It is thicker than the thickness (D2) of the outer portion 64 (D1> D2). According to this configuration, the amount of the electrolytic solution penetrating into the winding center portion of the wound electrode body is increased, and the liquid retaining property of the winding center portion is improved.
- the winding center of the wound electrode body is caused by the expansion and contraction of the wound electrode body accompanying the charge / discharge.
- Part of the non-aqueous electrolyte that has permeated the portion is pushed out of the wound electrode body. For this reason, the amount of the non-aqueous electrolyte at the center of winding is less than the required amount, and the electrolyte may wither.
- the amount of the electrolytic solution in the electrode is insufficient at the time of charging / discharging in the winding center portion, so that the charge / discharge performance as a whole battery is deteriorated.
- the battery reaction concentrates on the portion where the amount of the electrolytic solution is relatively large (that is, the outer portion of the winding), the deterioration of the portion is promoted. Any of these events can be a factor of reducing the durability (deteriorating battery capacity) of the lithium secondary battery with respect to the charge / discharge cycle.
- a porous layer (a layer having pores 63 capable of holding a non-aqueous electrolyte) 60 is formed on the surface of the separator sheet 40, and the winding center portion 62 of the porous layer 60 is formed. Is thicker than the wound outer portion 64. For this reason, the amount of the electrolytic solution penetrating into the winding center portion of the wound electrode body is increased, and the liquid retaining property of the winding center portion is improved. According to this configuration, even when the wound electrode body repeatedly expands and contracts due to charge and discharge, it is possible to suppress the occurrence of electrolyte erosion due to the nonaqueous electrolyte being pushed out from the center of the wound. The amount of electrolyte at the center of rotation can be kept appropriate. This can improve durability against charge / discharge cycles (for example, capacity retention after charge / discharge cycles).
- the configuration in which the winding center portion 62 of the porous layer is thicker than the winding outer portion 64 is, for example, in the winding direction of the winding electrode body in the winding electrode body of the sheet 40 on which the porous layer 60 is formed.
- the average thickness of the porous layer 60 formed up to 20% from the end 42 on the winding center side is the average thickness of the porous layer 60 formed up to 20% from the end 44 outside the winding electrode body. It may be realized by making it thicker. Thereby, it can suppress more reliably that electrolyte solution withering by a non-aqueous electrolyte being extruded from the winding center part.
- the porous layer in which the winding center part 62 is thicker than the winding outer part 64 is formed, for example, so that the porous layer 60 gradually becomes thicker from the winding outer side of the winding electrode body toward the winding center side. Should be realized. Thereby, it can suppress more reliably that electrolyte solution withering by a non-aqueous electrolyte being extruded from the winding center part.
- the porous layer 60 has the thickest thickest portion 66 and the thinnest thinnest portion 68.
- the porous layer 60 has the thickest thickest portion 66 at the winding center portion 62 provided at one end in the winding direction (longitudinal direction) of the porous layer, and the winding direction of the porous layer
- the thinnest thinnest portion 68 is provided on the wound outer side portion 64 provided at the other end in the (longitudinal direction).
- the difference in thickness between the thickest part and the thinnest part is 2 ⁇ m to 4 ⁇ m. If it is smaller than this range (typically less than 2 ⁇ m), the liquid retention effect at the center of winding is reduced, and the cycle durability improvement effect as described above may not be obtained. On the other hand, if it is larger than this range (typically over 4 ⁇ m), the difference in the distance between the electrode plates at the winding center and the outside of the winding is too large, resulting in non-uniform battery reaction and cycle durability. May tend to decline.
- the thickness difference between the thickest part and the thinnest part is generally 2 ⁇ m to 4 ⁇ m, more preferably 2.5 ⁇ m to 4 ⁇ m, and particularly preferably 3 ⁇ m to 4 ⁇ m.
- the thickness (D2) of the thinnest portion 68 is not particularly limited, but may be approximately 2 ⁇ m or more (typically 2 ⁇ m to 10 ⁇ m, for example, about 4 ⁇ m).
- the porosity of the porous layer is 45% to 65%. If it is smaller than this range (typically below 45%), the porous layer itself acts as a resistance component, so that the cycle durability may tend to be lower than when there is no porous layer. Moreover, if it is larger than this range (typically more than 65%), there may be a case where heat generation during an internal short circuit cannot be sufficiently suppressed.
- the porosity is preferably about 45% to 65%, more preferably 50% to 65%, and particularly preferably 50% to 60%.
- the said porosity is good to calculate by following formula (1) from the true volume V1 which does not contain the void
- Porosity (%) [(V2 ⁇ V1) / V2] ⁇ 100 (1)
- the true volume V1 can be calculated from the true density of the metal compound particles and the binder and the blending ratio thereof.
- the apparent volume V2 can be obtained from the outer dimensions (thickness and area) of the porous layer.
- the separator sheet 40 is not opposed to the negative electrode sheet 20 from the end 42 on the winding center side of the wound electrode body to the predetermined position 48 (that is, the end on the winding center side of the negative electrode sheet 20).
- a portion L of the unwrapped portion protruding from the portion).
- This unwinding part L is good also as an extra winding part for winding around a winding core, for example.
- the thickness of the porous layer 60 formed in the discarded portion L is not particularly limited.
- the thickest portion 66 is disposed so as to be closest to the winding center of the wound electrode body, and the porous layer formed in the winding portion L has the thickest thickness. It is formed so as to gradually become thinner from the portion 66 toward the end portion 65 on the winding center side.
- the porous layer 60 disclosed herein includes, for example, a separator for forming a porous layer in which metal compound particles, a binder, and other porous layer forming components are dispersed in a suitable solvent (preferably an organic solvent). It can be formed by applying a belt shape (here one side) and drying.
- a suitable solvent preferably an organic solvent
- Examples of the solvent used in the coating material for forming the porous layer include organic solvents such as N-methylpyrrolidone (NMP), pyrrolidone, methyl ethyl ketone, methyl isobutyl ketone, ixahexanone, toluene, dimethylformamide, dimethylacetamide, and the like.
- organic solvents such as N-methylpyrrolidone (NMP), pyrrolidone, methyl ethyl ketone, methyl isobutyl ketone, ixahexanone, toluene, dimethylformamide, dimethylacetamide, and the like.
- NMP N-methylpyrrolidone
- pyrrolidone pyrrolidone
- methyl ethyl ketone methyl isobutyl ketone
- ixahexanone ixahexanone
- toluene dimethylformamide
- dimethylacetamide dimethylace
- the operation (process) for applying such a coating material for forming a porous layer to the surface of the separator sheet is not particularly limited, and various types can be used widely. For example, it can be formed by applying a predetermined amount of a coating material for forming a porous layer to the separator sheet using an appropriate coating apparatus.
- a coating apparatus 200 As an apparatus for applying the porous layer forming paint to the separator sheet, for example, a coating apparatus 200 as shown in FIG.
- this coating apparatus 200 while the separator sheet 40 is conveyed by the rotation of the backup roll 220, the gap between the backup roll 220 and the application unit 230 is passed, and from the application unit 230 over the longitudinal direction of the separator sheet being conveyed.
- the porous layer forming paint 240 is applied.
- the solvent (for example, NMP) in the coating material 240 for porous layer formation is volatilized through the drying furnace 250, and the porous layer 60 is formed.
- the coating apparatus 200 is a gravure coating apparatus, and the coating means 230 is a gravure roll.
- the porous layer forming coating material 240 adhering to the surface irregularities of the gravure roll 230 is scraped off by a blade (not shown) and then travels with the backup roll 220 that rotates in the same direction as the rotation of the gravure roll 230. It is transferred to the surface of 40 and applied.
- the porous layer 60 having different thicknesses in the longitudinal direction of the sheet it is important to form the porous layer 60 having different thicknesses in the longitudinal direction of the sheet.
- a porous layer 60 can be formed, for example, by applying a porous layer forming paint to the surface of the separator sheet 40 that is running while changing the running speed of the sheet 40.
- the porous layer forming paint becomes thicker as the traveling speed of the sheet relatively decreases. Therefore, by applying the coating material for forming a porous layer while changing the traveling speed of the sheet, porous layers having different thicknesses in the longitudinal direction of the sheet can be formed.
- the coating material for forming a porous layer is applied while gradually changing the traveling speed of the sheet. Thereby, the porous layer from which thickness differs continuously in the longitudinal direction of a sheet
- a gravure roll 230 is used as a coating means.
- the porous layer forming coating material may be applied while changing the rotation speed of the gravure roll 230.
- the coating for forming the porous layer becomes thicker as the rotational speed of the gravure roll 230 is relatively increased. Therefore, by applying the coating material for forming a porous layer while changing the rotation speed of the gravure roll, porous layers having different thicknesses in the longitudinal direction of the sheet can be formed.
- the coating material for forming a porous layer is applied while gradually changing the rotation speed of the gravure roll. Thereby, the porous layer from which thickness differs continuously in the longitudinal direction of a sheet
- a porous layer 60 corresponding to a plurality of batteries is continuously formed on the surface of the traveling sheet 40.
- the porous layer forming paint is applied while changing the traveling speed of the sheet (and the rotational speed of the gravure roll)
- the porous layer 60 having a thickness different in the longitudinal direction of the sheet is applied to the traveling sheet 40. It can be formed continuously on the surface.
- the separator sheet 40 is then cut into a length corresponding to one battery. Then, the wound electrode body 80 is constructed by winding the positive electrode sheet 10 and the negative electrode sheet 20 through the two separator sheets 40.
- a positive electrode sheet 10 and a negative electrode sheet 20 are laminated via two separator sheets 40 to produce a sheet-like electrode body 88 (FIG. 3).
- the wound electrode body 80 is constructed by winding the sheet electrode body 88.
- FIG. In this way, the construction of the wound electrode body 80 according to the present embodiment is completed.
- the wound electrode body 80 having such a configuration is accommodated in the container body 52, and an appropriate nonaqueous electrolytic solution is disposed (injected) into the container body 52.
- an appropriate nonaqueous electrolytic solution is disposed (injected) into the container body 52.
- the same non-aqueous electrolyte as that used in a conventional lithium secondary battery can be used without any particular limitation.
- Such a nonaqueous electrolytic solution typically has a composition in which a supporting salt is contained in a suitable nonaqueous solvent.
- non-aqueous solvent examples include ethylene carbonate (EC), ethyl methyl carbonate (EMC), dimethyl carbonate (DMC), diethyl carbonate (DEC), propylene carbonate (PC), and the like.
- the supporting salt for example, LiPF 6, LiBF 4, LiAsF 6, LiCF 3 SO 3, can be preferably used a lithium salt of LiClO 4 and the like.
- a nonaqueous electrolytic solution in which LiPF 6 as a supporting salt is contained in a mixed solvent containing EC, EMC, and DMC in a volume ratio of 3: 4: 3 at a concentration of about 1 mol / liter can be preferably used.
- the non-aqueous electrolyte is housed in the container main body 52 together with the wound electrode body 80, and the opening of the container main body 52 is sealed with the lid body 54, thereby constructing (assembling) the lithium secondary battery 100 according to the present embodiment. ) Is completed.
- positioning (injection) process of electrolyte solution can be performed similarly to the method currently performed by manufacture of the conventional lithium secondary battery. Thereafter, the battery is conditioned (initial charge / discharge). You may perform processes, such as degassing and a quality inspection, as needed.
- test examples relating to the present invention will be described, but the present invention is not intended to be limited to those shown in the following test examples.
- ⁇ Test Example 1 Production of porous layer-forming coating material> Using an alumina powder having an average particle size of 0.7 ⁇ m as metal compound particles and a binder solution containing an acrylic resin as a binder, the mass ratio of the alumina powder to the binder is 95: 5, and the solid content concentration is about 40 mass. % In NMP. The mixture was pre-kneaded at 15000 rpm for 5 minutes with a high-speed stirring disperser (CLEAMIX: manufactured by M Technique Co., Ltd.), and then kneaded at 20000 rpm for 15 minutes to prepare a coating material for forming a porous layer.
- a high-speed stirring disperser (CLEAMIX: manufactured by M Technique Co., Ltd.)
- Test Example 2 Formation of porous layer>
- the various porous layer forming coating materials prepared in Test Example 1 were used for the long separator sheet 40 (thickness 20 ⁇ m, and a three-layer structure of polypropylene (PP) -polyethylene (PE) -polypropylene (PP) was used).
- the porous layer 60 was formed by apply
- ⁇ Test Example 3 Production of lithium secondary battery> A lithium secondary battery was produced using the separator sheet 40 provided with various porous layers 60 produced in Test Example 2 above. The production of the lithium secondary battery was performed as follows.
- Nickel cobalt lithium manganate (LiNi 1/3 Co 1/3 Mn 1/3 O 2 ) powder having an average particle diameter of 5 ⁇ m as a positive electrode active material, acetylene black (AB) as a conductive material, and polyfluorination as a binder Vinylidene (PVdF) was mixed in NMP so that the mass ratio of these materials was 85: 10: 5 to prepare a positive electrode active material layer forming paste.
- the positive electrode active material layer forming paste is applied to both surfaces of a 15 ⁇ m-thick long sheet-like aluminum foil (positive electrode current collector 12) in a strip shape and dried, whereby the positive electrode active material is formed on both surfaces of the positive electrode current collector 12
- the positive electrode sheet 10 provided with the layer 14 was produced.
- the coating amount of the positive electrode active material layer forming paste was adjusted so as to be about 16.8 mg / cm 2 (solid content basis) for both surfaces.
- graphite powder having an average particle diameter of 10 ⁇ m as a negative electrode active material, styrene butadiene rubber (SBR) as a binder, and carboxymethyl cellulose (CMC) as a thickener have a mass ratio of 98: 1: 1 was mixed in water to prepare a negative electrode active material layer forming paste.
- the negative electrode active material layer forming paste is applied to both sides of a long sheet-like copper foil (negative electrode current collector 22) having a thickness of 10 ⁇ m in a strip shape and dried to thereby form a negative electrode active material on both sides of the negative electrode current collector 22
- the negative electrode sheet 20 provided with the layer 24 was produced.
- the coating amount of the negative electrode active material layer forming paste was adjusted so that the total amount on both sides was about 9.2 mg / cm 2 (based on solid content).
- the wound electrode body 80 was produced by winding the positive electrode sheet 10 and the negative electrode sheet 20 through the two separator sheets 40. At that time, the separator layer was disposed so that the porous layer 60 on the surface of the separator sheet and the negative electrode sheet 20 face each other, and wound so that the thickest portion 66 of the porous layer 60 was located on the winding center side of the wound electrode body.
- the wound electrode body 80 obtained in this way was housed in a cylindrical battery container 50 together with a non-aqueous electrolyte, and the opening of the battery container 50 was hermetically sealed.
- a mixed solvent containing ethylene carbonate (EC), ethyl methyl carbonate (EMC), and dimethyl carbonate (DMC) in a volume ratio of 1: 1: 1 is about 1 mol / liter of LiPF 6 as a supporting salt.
- the non-aqueous electrolyte solution contained at a concentration of was used.
- the lithium secondary battery 100 was assembled. Thereafter, an initial charge / discharge treatment (conditioning) was performed by a conventional method to obtain a test lithium secondary battery.
- a lithium secondary battery was constructed using a separator sheet having no porous layer formed on the surface (Sample 14).
- ⁇ Test Example 4 Charge / Discharge Cycle Test> A charge / discharge cycle test was performed on each of the various lithium secondary batteries prepared in Test Example 3. Specifically, at 25 ° C., the battery is charged with a constant current method up to 4.1 V with a current of 2 C, further charged with a constant voltage method of 4.1 V with a current of 1/20 C, and after 2 minutes of rest, The charging / discharging cycle which discharges by a constant current system until it became 3V with the electric current of 1000 was repeated 1000 times continuously.
- the lithium secondary batteries of Samples 1 to 12 having a thickness difference in the porous layer are the battery of Sample 13 in which the thickness difference is 0 ⁇ m, and the battery of Sample 14 in which the porous layer is not formed.
- the capacity retention rate showed an increasing tendency, and it was confirmed that the battery had excellent cycle durability.
- it is 80% or more when the thickness difference d between the thickest part and the thinnest part is 2 ⁇ m to 4 ⁇ m based on the comparison of samples 1 to 5. An extremely high capacity retention rate was achieved.
- ⁇ Test Example 5 Foreign object internal short circuit test> Five lithium secondary batteries prepared in Test Example 3 were prepared, and a foreign substance internal short-circuit test was performed on each of the batteries. The foreign matter internal short-circuit test was performed according to JISC8714 using L-shaped nickel pieces having a height of 0.2 mm ⁇ width of 0.1 mm and sides of 1 mm. Then, the number of NG products that resulted in abnormal heat generation was evaluated. The results are shown in the corresponding places in Table 1.
- the lithium secondary batteries of Samples 1 to 13 in which the porous layer is formed have significantly fewer batteries that cause abnormal heat generation than the battery of Sample 14 in which the porous layer is not formed. It was confirmed that the battery was excellent. Although not particularly limited, in the case of the battery used here, a battery with higher safety can be obtained by comparing the samples 3 and 6 to 9 with the porosity of the porous layer being 65% or less. It was confirmed that can be realized.
- porous layer disclosed here is an interface between the separator sheet and the negative electrode sheet and is formed on the surface of the separator sheet on the negative electrode sheet side, it is not limited to this.
- the porous layer may be formed on the surface of the separator sheet on the positive electrode sheet side, may be formed on the surface of the positive electrode sheet, or may be formed on the surface of the negative electrode sheet.
- the porous layer disclosed herein is formed so as to gradually increase in thickness from the winding outer side of the wound electrode body toward the winding center side, but is not limited thereto. For example, it is possible to form step-like porous layers having thicknesses that differ in stages.
- the shape (outer shape and size) of the lithium secondary battery to be constructed is not particularly limited.
- the outer package may be a thin sheet type constituted by a laminate film or the like, and the battery outer case may be a cylindrical or cuboid battery, or may be a small button shape.
- any of the lithium secondary batteries 100 disclosed herein has a performance suitable for a battery mounted on a vehicle (for example, high output can be obtained), and is particularly excellent in durability against high-rate charge / discharge. It can be. Therefore, according to the present invention, as shown in FIG. 7, a vehicle 1 including any of the lithium secondary batteries 100 disclosed herein is provided.
- a vehicle 1 for example, an automobile
- the lithium secondary battery 100 as a power source (typically, a power source of a hybrid vehicle or an electric vehicle) is provided.
- Lithium secondary battery 100 charge / discharge including high capacity charge / discharge with a theoretical capacity of 1Ah or more (more than 3Ah), 2C or more (for example, 2C-50C) and even 10C or more (for example, 10C-40C) Examples include lithium secondary batteries that are supposed to be used in cycles.
Abstract
Description
空孔率(%)=[(V2-V1)/V2]×100 (1)
ここで、真体積V1は金属化合物粒子およびバインダの真密度とその配合比とから算出することができる。また、見掛け体積V2は多孔層の外寸(厚みと面積)から求めることができる。
金属化合物粒子としての平均粒径0.7μmのアルミナ粉末と、バインダとしてのアクリル樹脂を含むバインダ溶液とを使用し、アルミナ粉末とバインダとの質量比が95:5となり固形分濃度が約40質量%となるようにNMP中で混合した。該混合物を高速攪拌分散機(クレアミックス:Mテクニック社製)で15000rpm、5分間、予備混練し、次いで、20000rpm、15分間、本混練することにより、多孔層形成用塗料を調製した。
上記試験例1で作製した各種の多孔層形成用塗料を長尺状のセパレータシート40(厚み20μm、ポリプロピレン(PP)-ポリエチレン(PE)-ポリプロピレン(PP)の3層構造を使用した。)の片面にグラビアロール(キスリバース方式)により帯状に塗布して乾燥することにより、多孔層60を形成した。その際、セパレータシートの走行速度Aに対するグラビアロールの回転速度Bの比率(速比=A/B)を1.1~1.5で漸次変化させながら多孔層形成用塗料を塗布することによって、シートの長手方向に厚みが異なる5種類の多孔層60を形成した(サンプル1~5)。最厚部の厚みD1、最薄部の厚みD2、厚み差dをそれぞれ表1に示す。
上記試験例2で作製した各種の多孔層60が設けられたセパレータシート40を用いてリチウム二次電池を作製した。リチウム二次電池の作製は、以下のようにして行った。
上記試験例3で作製した各種のリチウム二次電池のそれぞれに対し、充放電サイクル試験を行った。具体的には、25℃において、2Cの電流で4.1Vまで定電流方式で充電を行い、さらに1/20Cの電流で4.1Vの定電圧方式で充電し、1分間の休止後、2Cの電流で3Vになるまで定電流方式で放電を行う充放電サイクルを1000回連続して繰り返した。そして、上記充放電サイクル試験前における初期の容量と、上記充放電サイクル試験後における放電容量とから、充放電サイクル試験後の容量維持率(=[充放電サイクル試験後の放電容量/充放電サイクル試験前の初期容量]×100)を算出した。その結果を表1の該当箇所に示す。
特に限定されるものではないが、ここで供試した電池の場合、サンプル1~5の比較から、最厚部と最薄部の厚み差dを2μm~4μmにすることによって、80%以上という極めて高い容量維持率を達成できた。また、サンプル3及び6~9の比較から、多孔層の空孔率を45%以上にすることによって、80%以上という極めて高い容量維持率を達成できた。さらに、サンプル2~4及び10~12の比較から、セパレータシートの材質に関係なく、サイクル耐久性を向上できることが確認できた。
上記試験例3で作製した各種のリチウム二次電池を5個ずつ作製し、それぞれの電池に対し、異物内部短絡試験を実施した。異物内部短絡試験は、高さ0.2mm×幅0.1mmで各辺1mmのL字形のニッケル小片を用いてJISC8714に準じて行った。そして、異常発熱に至ったNG品の数を評価した。結果を表1の該当箇所に示す。
Claims (12)
- 正極シートと負極シートとがセパレータシートを介して捲回された捲回電極体を備えたリチウム二次電池であって、
前記捲回電極体を構成する正極シート、負極シート及びセパレータシートの少なくともいずれかのシート表面には、該シートの長手方向に亘って多孔層が形成されており、
前記捲回電極体の捲回方向において、前記多孔層は、捲回中心部が捲回外側部よりも厚い、リチウム二次電池。 - 前記捲回電極体の捲回方向において、前記多孔層が形成された前記シートのうち前記捲回電極体の捲回中心側の端部から20%までに形成された多孔層の平均厚みが、前記捲回電極体の捲回外側の端部から20%までに形成された多孔層の平均厚みよりも厚い、請求項1に記載のリチウム二次電池。
- 前記多孔層は、前記捲回電極体の捲回外側から捲回中心側に向けて漸次厚くなるように形成されている、請求項1または2に記載のリチウム二次電池。
- 前記多孔層は、最も厚い最厚部と最も薄い最薄部とを有し、
前記最厚部と前記最薄部との厚みの差が2μm~4μmである、請求項1から3の何れか一つに記載のリチウム二次電池。 - 前記多孔層の空孔率が45%~65%である、請求項1から4の何れか一つに記載のリチウム二次電池。
- 前記多孔層は、金属化合物粒子から構成されている、請求項1から5の何れか一つに記載のリチウム二次電池。
- 前記多孔層は、前記セパレータシートの表面に形成されている、請求項1から6の何れか一つに記載のリチウム二次電池。
- 前記多孔層は、前記セパレータシートの負極シート側の表面に形成されている、請求項7に記載のリチウム二次電池。
- 請求項1から8の何れかに記載のリチウム二次電池を製造する方法であって、
走行中の正極シート、負極シート及びセパレータシートの少なくともいずれかのシートの表面に、塗布手段により多孔層形成用塗料を塗布し、乾燥することにより多孔層を形成する工程を有し、
前記多孔層形成用塗料を前記シートの走行速度を変化させながら塗布することを特徴とする、リチウム二次電池の製造方法。 - 前記塗布手段は、グラビアロールであり、
前記多孔層形成用塗料を前記グラビアロールの回転速度を変化させながら塗布する、請求項9に記載の製造方法。 - 前記走行中のシート表面に複数の電池分に相当する多孔層を連続して形成する、請求項9または10に記載の製造方法。
- 請求項1から8の何れかに記載のリチウム二次電池もしくは請求項9から11の何れか一つに記載の製造方法により製造されたリチウム二次電池を搭載した車両。
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JPWO2011155060A1 (ja) | 2013-08-01 |
JP5218873B2 (ja) | 2013-06-26 |
US8771860B2 (en) | 2014-07-08 |
CN102405552A (zh) | 2012-04-04 |
US20130101876A1 (en) | 2013-04-25 |
CN102405552B (zh) | 2015-08-19 |
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