WO2015037560A1 - 二次電池 - Google Patents

二次電池 Download PDF

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Publication number
WO2015037560A1
WO2015037560A1 PCT/JP2014/073706 JP2014073706W WO2015037560A1 WO 2015037560 A1 WO2015037560 A1 WO 2015037560A1 JP 2014073706 W JP2014073706 W JP 2014073706W WO 2015037560 A1 WO2015037560 A1 WO 2015037560A1
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WIPO (PCT)
Prior art keywords
positive electrode
negative electrode
tab
current collector
plate
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PCT/JP2014/073706
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English (en)
French (fr)
Japanese (ja)
Inventor
田中　明
雄輔 内田
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新神戸電機株式会社
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Priority to JP2015536572A priority Critical patent/JPWO2015037560A1/ja
Priority to KR1020167004814A priority patent/KR20160055137A/ko
Publication of WO2015037560A1 publication Critical patent/WO2015037560A1/ja

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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
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/531—Electrode connections inside a battery casing
    • H01M50/533—Electrode connections inside a battery casing characterised by the shape of the leads or tabs
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • 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
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • 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
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • 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
    • 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
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/543—Terminals
    • 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
    • H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
    • H01M2010/4292—Aspects relating to capacity ratio of electrodes/electrolyte or anode/cathode
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2220/00—Batteries for particular applications
    • H01M2220/10—Batteries in stationary systems, e.g. emergency power source in plant
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2220/00—Batteries for particular applications
    • H01M2220/20—Batteries in motive systems, e.g. vehicle, ship, plane
    • 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
    • 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
    • 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

Definitions

  • the present invention relates to a secondary battery.
  • Secondary batteries include nickel cadmium batteries, nickel metal hydride batteries, lithium ion batteries, and the like.
  • Nickel cadmium batteries are being converted to nickel metal hydride batteries and lithium ion batteries because cadmium is toxic.
  • the lithium ion secondary battery is particularly suitable for increasing the energy density, and its development is being actively promoted.
  • the main components of the nickel metal hydride battery and the lithium ion secondary battery are a negative electrode plate having a negative electrode active material layer formed on the surface of the negative electrode current collector plate, a separator for holding an electrolyte, and a positive electrode on the surface of the positive electrode current collector plate. It is a positive electrode plate on which an active material layer is formed.
  • the nickel metal hydride battery employs nickel oxide as the positive electrode active material and a hydrogen storage alloy as the negative electrode active material.
  • the lithium ion secondary battery employs a lithium metal oxide as the positive electrode active material and a carbon material such as graphite as the negative electrode active material.
  • Battery structures are broadly divided into a cylindrical structure in which strip-shaped negative plates, separators, and positive plates are stacked in a spiral shape, and a stacked structure in which strip-shaped negative plates, separators, and positive plates are alternately arranged.
  • the Laminate type in which strip-like negative plates, separators, and positive plates are arranged alternately, rather than a cylindrical structure with many volume parts not involved in power generation, such as a strip-like negative plate, separator, and positive electrode core.
  • the structure is generally suitable for high volume energy density. This is because the laminated type does not require an axis for winding, and the positive electrode terminal and the negative electrode terminal for external output are easily formed on the same surface, so the volume other than the part that contributes to power generation is reduced. Because it can.
  • a current collecting tab for electrically connecting to an external terminal of the battery is formed on one side of a metal current collector (current collector plate) having an active material layer formed on the surface.
  • current collecting tabs are formed on a strip-shaped plate at regular intervals and wound.
  • the stacked type has a current collecting tab formed on one side of a strip-shaped electrode plate.
  • a predetermined number of current collecting tabs are bundled and connected to an electrical wiring member (current collector) that is electrically connected to an external terminal of the battery. As the capacity and current of the battery increase, it is necessary to reduce the electrical resistance of the electrical wiring member and the current collecting tab in order to prevent heat generation by the electrical wiring member and the current collecting tab.
  • the cited document 1 has no description regarding the temperature rise inside the lithium ion secondary battery.
  • the capacity of a lithium ion secondary battery (a large capacity, large current stacked battery) is increased, there is a problem that the heat dissipation within the battery is lowered and the life is reduced.
  • the battery temperature exceeds about 60 ° C. due to temperature rise, the life of the lithium battery is greatly reduced.
  • the temperature increase ( ⁇ T) of the positive electrode active material due to a decrease in heat dissipation is preferably 35 ° C. or less. More preferably, the temperature rise ( ⁇ T) of the positive electrode active material is preferably lower than 30 ° C.
  • the current collecting tab is formed by cutting a strip-shaped electrode roll with a predetermined-shaped blade or the like. In the winding process after the current collecting tab is formed, the length of the current collecting tab is longer than the width. Then, there is a concern that the current collecting tab hangs down due to its own weight and is bent and wound. For this reason, the relationship between the length and width of the current collecting tab is important.
  • An object of the present invention is to provide a secondary battery capable of suppressing a decrease in workability of the negative electrode tab and the positive electrode tab and suppressing an increase in temperature inside the battery.
  • a more specific object of the present invention is to provide a lithium ion secondary battery capable of suppressing a decrease in workability of the negative electrode tab and the positive electrode tab in the lithium ion secondary battery and suppressing an increase in temperature inside the battery.
  • the present invention provides a negative electrode plate comprising a negative electrode tab in which a negative electrode active material layer is formed on a negative electrode current collector plate and a part of the negative electrode current collector plate extends, a separator, and a positive electrode
  • a positive electrode group in which a positive electrode active material layer is formed on a current collector plate and a positive electrode plate having a positive electrode tab formed by extending a part of the positive electrode current collector plate, a negative electrode terminal, and a positive electrode terminal I have.
  • the width dimension of the negative electrode tab is W ′
  • the width dimension of the positive electrode tab is W
  • the width dimension of the negative electrode current collector plate is L ′
  • the width dimension of the positive electrode current collector plate is L.
  • the secondary battery having the above relationship desirably has the following relationship where the length of the negative electrode tab is T ′ and the length of the positive electrode tab is T.
  • the area where the negative electrode current collector and the negative electrode tab of the negative electrode terminal are in contact with each other, and the area where the positive electrode current collector and the positive electrode tab of the positive electrode terminal are in electrical contact are 1/3 or more of the area of the negative electrode tab and the positive electrode tab. It is desirable to be. If it does in this way, the electrical resistance in a junction part can be reduced and the emitted-heat amount from a junction part can be reduced.
  • a positive electrode plate having a positive electrode tab formed by extending a part of the positive electrode current collector plate, a negative electrode terminal, a positive electrode terminal, and a lithium manganate as a positive electrode active material
  • the width dimension of the negative electrode tab is W ′
  • the length method of the negative electrode tab is T ′
  • the width dimension of the positive electrode tab is W
  • the positive electrode When the length dimension of the tab is T, the width dimension of the negative electrode current collector plate is L ′, and the width dimension of the positive electrode current collector plate is L, 45> [(W / L) ⁇ 100]> 28 45> [(W ′ / L ′) ⁇ 100]> 28 4 ⁇ W / T> 1.8 4 ⁇ W ′ / T ′> 1.8
  • the width dimension of the negative electrode tab is W ′
  • the length method of the negative electrode tab is T ′
  • the positive electrode When the width dimension of the tab is W, the length dimension of the positive electrode tab is T, the width dimension of the negative electrode current collector plate is L ′, and the width dimension of the positive electrode current collector plate is L, 45> [(W / L) ⁇ 100]> 33 45> [(W ′ / L ′) ⁇ 100]> 33 4 ⁇ W / T ⁇ 3 4 ⁇ W ′ / T ′ ⁇ 3 If the relationship is satisfied, the active material temperature rise ⁇ T can be made lower than 30 ° C. In particular, when the present invention is applied to a lithium ion secondary battery in which the number of negative electrode plates and positive electrode plates is determined such that the capacity of the electrode plate group is 100 Ah to 500 Ah, an excellent effect can be obtained. .
  • the present invention it is possible to provide a secondary battery and a lithium ion secondary battery that can suppress deterioration in workability at the time of tab processing and can suppress temperature rise inside the battery.
  • a secondary battery and a lithium ion secondary battery having a large capacity and a large current with a high volumetric energy density, in which the current collecting part inside the battery is compact.
  • a positive electrode plate is produced by forming a positive electrode active material layer containing a positive electrode active material and a binder on a positive electrode current collector plate. Specifically, a positive electrode active material and a binder, and if necessary, a conductive material and a thickener mixed in a dry form into a sheet form are pressure-bonded to the positive electrode current collector plate, or these The material is dissolved and dispersed in a liquid medium, applied as a slurry to the positive electrode current collector plate, and dried to form a positive electrode active material layer on the positive electrode current collector plate.
  • a known lithium and transition metal composite oxide capable of inserting, desorbing and dissolving lithium can be used alone or in combination of two or more.
  • the composite oxide of lithium metal and transition metal include lithium manganate, lithium nickelate, lithium cobaltate, and lithium iron phosphate. These composite oxides may be of a single phase, a transition metal partially substituted with a different element, or a surface coated with an oxide or carbon.
  • the positive electrode conductive material a known conductive material can be arbitrarily used. Specific examples include metal materials such as copper and nickel; graphite such as natural graphite and artificial graphite (graphite); carbon black such as acetylene black; and carbonaceous materials such as amorphous carbon such as needle coke. In addition, these may be used individually by 1 type and may use 2 or more types together by arbitrary combinations and arbitrary ratios.
  • the binder used for manufacturing the positive electrode active material layer is not particularly limited, and in the case of a coating method, any material that dissolves or disperses in the liquid medium used during electrode manufacturing may be used.
  • the binder include resin polymers such as polyethylene, polypropylene, polyethylene terephthalate, polymethyl methacrylate, polyimide, aromatic polyamide, cellulose, and nitrocellulose; SBR (styrene-butadiene rubber), NBR (acrylonitrile-butadiene) Rubber), fluoropolymer, isoprene rubber, butadiene rubber, ethylene-propylene rubber, and other rubbery polymers; styrene / butadiene / styrene block copolymers or hydrogenated products thereof, EPDM (ethylene / propylene / diene terpolymers) ), Thermoplastic elastomeric polymers such as styrene / ethylene / butadiene / ethylene copoly
  • these substances may be used individually by 1 type, and may use 2 or more types together by arbitrary combinations and arbitrary ratios.
  • a fluorine-based polymer such as polyvinylidene fluoride (PVdF) or polytetrafluoroethylene / vinylidene fluoride copolymer is preferable.
  • the positive electrode active material layer obtained by coating and drying is preferably consolidated by a hand press, a roller press or the like in order to increase the packing density of the positive electrode active material.
  • the material for the positive electrode current collector plate is not particularly limited, and any known material can be used.
  • metal materials such as aluminum, stainless steel, nickel plating, titanium, and tantalum
  • carbonaceous materials such as carbon cloth and carbon paper.
  • metal materials particularly aluminum foil, are preferred.
  • the form of the positive electrode current collector plate is not particularly limited, and a known form can be arbitrarily used.
  • the metal material include metal foil, metal cylinder, metal coil, metal plate, metal thin film, expanded metal, punch metal, and foam metal.
  • metal foil is preferred.
  • the metal foil may be appropriately formed in a mesh shape.
  • the thickness of the metal foil is arbitrary, but is usually 1 ⁇ m or more, preferably 3 ⁇ m or more, more preferably 5 ⁇ m or more, and usually 1 mm or less, preferably 100 ⁇ m or less, more preferably 50 ⁇ m or less. If the metal foil is thinner than this range, the strength required for the current collector may be insufficient. Conversely, if the metal foil is thicker than this range, the handleability may be impaired.
  • Negative electrode plate As for the negative electrode plate, the negative electrode compound material containing the negative electrode active material which can occlude / release lithium ion electrochemically is apply
  • negative electrode active materials include carbonaceous materials, inorganic oxides such as tin oxide and silicon oxide, metal composite oxides, lithium alloys such as lithium alone and lithium aluminum alloys, and inorganic materials that can form alloys with lithium such as tin and silicon. Is mentioned. These may be used individually by 1 type, or may use 2 or more types together by arbitrary combinations and a ratio. Among these, it is preferable from the viewpoint of safety to use a carbonaceous material or a lithium composite oxide.
  • the metal composite oxide is not particularly limited as long as it can occlude and release lithium, but it contains titanium and / or lithium as a constituent component in view of high current density charge / discharge characteristics. To preferred.
  • Carbonaceous materials include amorphous carbon, natural graphite, composite carbonaceous materials in which a film formed by dry CVD (Chemical Vapor Deposition) method or wet spray method is formed on natural graphite, resins such as epoxy and phenol Carbonaceous materials such as artificial graphite and amorphous carbon materials produced by firing raw materials or pitch-based materials obtained from petroleum and coal, or lithium that can occlude and release lithium by forming a compound with lithium
  • An oxide or nitride of a group 14 element such as silicon, germanium, tin, or the like, which forms a compound with metal, lithium, and is inserted into a crystal gap to absorb and release lithium, can be used.
  • the negative electrode mixture may contain two or more carbonaceous materials having different properties as a conductive material.
  • the negative electrode current collector plate As the negative electrode current collector plate, a known one can be arbitrarily used.
  • the negative electrode current collector plate include metal materials such as copper, nickel, stainless steel, and nickel-plated steel. Among these, copper is preferable from the viewpoint of ease of processing and cost.
  • the shape of the negative electrode current collector plate include metal foil, metal cylinder, metal coil, metal plate, metal thin film, expanded metal, punching metal, and foam metal when the current collector plate is a metal material.
  • a copper foil is preferable, and a rolled copper foil obtained by a rolling method and an electrolytic copper foil obtained by an electrolytic method can be more preferably used as a negative electrode current collector.
  • a copper alloy phosphor bronze, titanium copper, Corson alloy, Cu—Cr—Zr alloy, etc.
  • the binder for binding the negative electrode active material is not particularly limited as long as it is a material that is stable with respect to the non-aqueous electrolyte solution and the solvent used during electrode production.
  • resin-based polymers such as polyethylene, polypropylene, polyethylene terephthalate, polymethyl methacrylate, aromatic polyamide, cellulose, nitrocellulose; SBR (styrene-butadiene rubber), isoprene rubber, butadiene rubber, fluorine rubber, NBR ( Acrylonitrile-butadiene rubber), rubber-like polymers such as ethylene-propylene rubber; styrene / butadiene / styrene block copolymer or hydrogenated product thereof; EPDM (ethylene / propylene / diene terpolymer), styrene / ethylene ⁇ Thermoplastic elastomeric polymers such as butadiene / styrene copolymers, styrene /
  • the resin separator has a predetermined mechanical strength that electrically insulates both electrodes, has a high ion permeability, and is resistant to oxidation on the side in contact with the positive electrode and reducibility on the negative electrode side.
  • a resin having both is used.
  • An olefin polymer is used as such a resin.
  • a porous sheet containing at least one of polypropylene and polyethylene as a material. .
  • the resin separator As the form of the resin separator, a microporous film having a thin film shape, a pore diameter of 0.01 to 1 ⁇ m, and a thickness of 15 to 50 ⁇ m is preferably used. Further, the porosity of the resin separator is preferably 30 to 50%, more preferably 35 to 45%. Note that the resin separator of this example (a resin separator having a thickness of 15 to 50 ⁇ m) may be constituted by a single separator or may be constituted by stacking two or more separators.
  • the electrolytic solution used in the lithium ion secondary battery of this example is composed of a lithium salt and a non-aqueous solvent that dissolves the lithium salt, and may further contain an additive.
  • a known lithium salt is used as an electrolyte of a non-aqueous electrolyte for a lithium ion secondary battery, and examples thereof include the following.
  • Inorganic lithium salts inorganic fluoride salts such as LiPF 6 , LiBF 4 , LiAsF 6 , LiSbF 6 ; perhalogenates such as LiClO 4 , LiBrO 4 , LiIO 4 ; inorganic chloride salts such as LiAlCl 4 .
  • Fluorine-containing organic lithium salt perfluoroalkane sulfonate such as F 3 SO 3 ; LiN (CF 3 SO 2 ) 2 , LiN (CF 3 CF 2 SO 2 ) 2 , LiN (CF 3 SO 2 ) (C 4 Perfluoroalkanesulfonylimide salts such as F 9 SO 2 ); perfluoroalkanesulfonylmethide salts such as LiC (CF 3 SO 2 ) 3 ; Li [PF 5 (CF 2 CF 2 CF 3 )], Li [PF 4 (CF 2 CF 2 CF 3 ) 2 ], Li [PF 3 (CF 2 CF 2 CF 3 ) 3 ], Li [PF 5 (CF 2 CF 2 CF 2 CF 3 )], Li [PF 4 (CF 2 CF 2 CF 3 ) 2 ], Li [PF 3 (CF 2 CF 2 CF 3 ) 3 ], Li [PF 3 (CF 2 CF 2 CF 3 )], Li [PF 4 (CF 2
  • Oxalatoborate salts lithium bis (oxalato) borate, lithium difluorooxalatoborate, etc. These may be used individually by 1 type, or may use 2 or more types together by arbitrary combinations and ratios. Among these, lithium hexafluorophosphate (LiPF 6 ) is preferable when comprehensively judging the solubility in a solvent, charge / discharge characteristics when used in a secondary battery, output characteristics, cycle characteristics, and the like.
  • LiPF 6 lithium hexafluorophosphate
  • the concentration of these electrolytes in the nonaqueous electrolytic solution is not particularly limited, but is usually 0.5 mol / L or more, preferably 0.6 mol / L or more, more preferably 0.7 mol / L or more. Moreover, the upper limit is 2 mol / L or less normally, Preferably it is 1.8 mol / L or less, More preferably, it is 1.7 mol / L or less. If the concentration is too low, the electrical conductivity of the electrolyte solution may be insufficient. On the other hand, if the concentration is too high, the electrical conductivity may decrease due to an increase in viscosity, and the performance of the lithium ion secondary battery may be reduced. May decrease.
  • non-aqueous solvent a known non-aqueous solvent is used as an electrolyte of a non-aqueous electrolyte for a lithium ion secondary battery, and examples thereof include the following.
  • Cyclic carbonate The alkylene group constituting the cyclic carbonate preferably has 2 to 6 carbon atoms, particularly preferably 2 to 4 carbon atoms. Specific examples include ethylene carbonate, propylene carbonate, butylene carbonate, and the like. Of these, ethylene carbonate and propylene carbonate are preferable.
  • ⁇ Chain carbonate As the chain carbonate, dialkyl carbonate is preferable, and the number of carbon atoms of the alkyl group is preferably 1 to 5, and particularly preferably 1 to 4. Specifically, for example, symmetrical chain carbonates such as dimethyl carbonate, diethyl carbonate, and di-n-propyl carbonate; asymmetric chain carbonates such as ethyl methyl carbonate, methyl-n-propyl carbonate, and ethyl-n-propyl carbonate And dialkyl carbonates. Of these, dimethyl carbonate, diethyl carbonate, and ethyl methyl carbonate are preferable.
  • Chain ester methyl acetate, ethyl acetate, propyl acetate, methyl propionate, etc. are mentioned.
  • Cyclic ether Tetrahydrofuran, 2-methyltetrahydrofuran, tetrahydropyran and the like.
  • the additive is not particularly limited as long as it is known to be used as an additive for a non-aqueous electrolyte solution for a lithium ion secondary battery, and examples thereof include the following.
  • a heterocyclic compound containing nitrogen and / or sulfur is not particularly limited, but includes 1-methyl-2-pyrrolidinone, 1,3-dimethyl-2-pyrrolidinone, Pyrrolidinones such as 1,5-dimethyl-2-pyrrolidinone, 1-ethyl-2-pyrrolidinone, 1-cyclohexyl-2-pyrrolidinone; 3-methyl-2-oxazolidinone, 3-ethyl-2-oxazolidinone, 3-cyclohexyl- Oxazolidinones such as 2-oxazolidinone; piperidones such as 1-methyl-2-piperidone and 1-ethyl-2-piperidone; 1,3-dimethyl-2-imidazolidinone, 1,3-diethyl-2-imidazolidi Imidazolidinones such as non-sulfones; sulfolane, 2-methylsulfolane, 3-methylsulfolane, etc.
  • Sulfolanes Sulfolenes; sulfites such as ethylene sulfite and propylene sulfite; 1,3-propane sultone, 1-methyl-1,3-propane sultone, 3-methyl-1,3-propane sultone, 1,4 -Sultone such as butane sultone, 1,3-propene sultone, 1,4-butene sultone, and the like.
  • Cyclic carboxylic acid ester is not particularly limited, but ⁇ -butyrolactone, ⁇ -valerolactone, ⁇ -hexalactone, ⁇ -heptalactone, ⁇ -octalactone, ⁇ -nonalactone, ⁇ -decalactone , ⁇ -undecalactone, ⁇ -dodecalactone, ⁇ -methyl- ⁇ -butyrolactone, ⁇ -ethyl- ⁇ -butyrolactone, ⁇ -propyl- ⁇ -butyrolactone, ⁇ -methyl- ⁇ -valerolactone, ⁇ -ethyl- ⁇ -Valerolactone, ⁇ , ⁇ -dimethyl- ⁇ -butyrolactone, ⁇ , ⁇ -dimethyl- ⁇ -valerolactone, ⁇ -valerolactone, ⁇ -hexalactone, ⁇ -octalactone, ⁇ -nonalactone, ⁇ -nonalactone, ⁇ -buty
  • Fluorine-containing cyclic carbonate is not particularly limited, and examples thereof include fluoroethylene carbonate, difluoroethylene carbonate, trifluoroethylene carbonate, tetrafluoroethylene carbonate, and trifluoropropylene carbonate.
  • aromatic compounds such as biphenyl, alkylbiphenyl, terphenyl, partially hydrogenated terphenyl, cyclohexylbenzene, t-butylbenzene, t-amylbenzene, diphenyl ether, dibenzofuran, etc .; 2-fluoro Partially fluorinated products of the above aromatic compounds such as biphenyl, o-cyclohexylfluorobenzene, p-cyclohexylfluorobenzene; 2,4-difluoroanisole, 2,5-difluoroanisole, 2,6-difluoroanisole, 3,5-difluoro Examples thereof include fluorine-containing anisole compounds such as anisole.
  • examples of the negative electrode film forming material include succinic anhydride, glutaric anhydride, maleic anhydride, citraconic anhydride, glutaconic anhydride, itaconic anhydride, cyclohexanedicarboxylic anhydride, and the like.
  • succinic anhydride and maleic anhydride are used. Two or more of these may be used in combination.
  • methyl methanesulfonate, busulfan, and dimethylsulfone are used. Two or more of these may be used in combination.
  • FIG. 1 is a partially cutaway perspective view of a lithium ion secondary battery according to an embodiment of the present invention.
  • FIG. 2A shows a positive electrode plate 10 having a positive electrode current plate (copper foil) 12 with a positive electrode tab 3 coated with a positive electrode active material, a terminal portion 4A, and a positive electrode current collector 4B.
  • 4 is a schematic plan view showing a relationship 4.
  • FIG. 2B shows a negative electrode plate 10 ′ obtained by applying a negative electrode active material to a negative electrode current collector plate (aluminum foil) 12 ′ with a negative electrode tab 3 ′, a terminal portion 4′A, and a negative electrode current collector 4 ′.
  • FIG. 1 It is a schematic plan view which shows the relationship of negative electrode terminal 4 'provided with B.
  • a plurality of positive electrode plates 10 in an electrode plate group 2 housed in a battery can 1 are electrically and mechanically connected to a positive electrode current collector 4 ⁇ / b> B of a positive electrode terminal 4 via a plurality of positive electrode tabs 3.
  • the plurality of negative electrode plates 10 ′ are electrically and mechanically connected to the positive electrode current collector 4 ′ B of the negative electrode terminal 4 ′ via the plurality of negative electrode tabs 3 ′.
  • the positive electrode terminal 4 is fixed to the lid plate 8 with a fastening component 5 such as a nut.
  • the negative fictitious terminal 4 ′ is also fixed to the lid plate 8 with a fastening part 5 ′ such as a nut.
  • a fastening part 5 ′ such as a nut.
  • the lid plate 8 is provided with a liquid injection hole plug 6 that seals a liquid injection hole for injecting an electrolytic solution, and a safety valve 7 for releasing the internal pressure of the battery can at an unsteady time such as overcharge. Yes.
  • the electrode plate group 2 includes a plurality of negative electrode plates 10 ′, a plurality of separators (not shown) for holding an electrolyte, and a plurality of positive electrode plates 10, a negative electrode plate 10 ′, a separator, and a negative electrode plate 10 ′. It is the structure which piled up alternately in this order. The dimensions such as the thickness of the electrode plate group 2 and the number of stacked layers are determined by the required battery capacity.
  • the battery can 1 has a rectangular shape in order to include the rectangular electrode plate group 2.
  • a rectangular battery has a shaft core for winding, etc., compared to a case where a laminated body of a strip-shaped positive electrode plate, a strip-shaped separator, and a strip-shaped negative electrode plate is rolled into a cylindrical battery can. Therefore, there is an advantage that the volume energy density can be increased.
  • the battery can 1 is formed of an aluminum alloy by impact press molding. When the material of the battery can 1 is an aluminum metal, it may be produced by die casting. The material of the battery can 1 may be stainless steel.
  • the material of the battery can 1 is preferably a metal material such as aluminum or stainless steel from the viewpoint of mechanical strength, but is not limited to a metal material, and is not limited to a resin that is not eroded by the electrolyte, such as fluorine, polyethylene, polypropylene, and epoxy.
  • a resin such as POM, PEEK, or BT resin may be used.
  • Resin-based battery cans have the advantage of being lighter than metal-based battery cans because of the lower material density. On the other hand, resin systems are weak in strength and have disadvantages such as poor heat dissipation due to low thermal conductivity.
  • the battery can 1 may be mainly composed of a metal material, and the surface thereof may be coated with the resin.
  • the number of positive electrode tabs 3 and negative electrode tabs 3 ′ in the electrode plate group 2 is determined by the capacity, and batteries having a capacity of several tens Ah to several hundreds Ah range from several tens to several hundreds of tabs.
  • batteries having a capacity of several tens Ah to several hundreds Ah range from several tens to several hundreds of tabs.
  • both the positive electrode terminal 4 and the negative electrode terminal 4 ′ protrude from the same surface (lid 8) of the battery. Thereby, since the wiring to the positive electrode terminal 4 and the negative electrode terminal 4 ′ can be accommodated in one plane, the wiring space can be reduced.
  • the positive electrode plate 10 has an uncoated portion in which the positive electrode active material layer 9 is not formed on a part of the positive electrode current collector plate 12 having the positive electrode active material layer 9 formed on the surface thereof. 11 is formed. A part of the uncoated portion 11 is extended to form the positive electrode tab 3.
  • the length dimension T of the positive electrode tab 3 is shorter than the width dimension W of the positive electrode tab 3 in consideration of the bending of the positive electrode tab.
  • the plurality of positive electrode tabs 3 are electrically and mechanically connected to the positive electrode current collector 4B of the positive electrode terminal 4 in a stacked state. Further, as shown in FIG.
  • the negative electrode plate 10 ′ has a negative electrode active material layer 9 ′ formed on a part of a negative electrode current collector plate 12 ′ having a negative electrode active material layer 9 ′ formed on the surface thereof.
  • An uncoated part 11 ′ is formed.
  • a part of the uncoated portion 11 ′ is extended to form a negative electrode tab 3 ′.
  • the length dimension T ′ of the negative electrode tab 3 ′ is shorter than the width dimension W ′ of the negative electrode tab 3 ′ in consideration of bending of the negative electrode tab.
  • the plurality of negative electrode tabs 3 ′ are electrically and mechanically connected to the negative electrode current collector 4 ′ B of the negative electrode terminal 4 ′ in a stacked state.
  • the area where the negative electrode current collector 4′B and the positive electrode current collector 4B are in contact with or joined to the negative electrode tab 3 ′ and the positive electrode tab 3 is 1/3 or more of the area of the negative electrode tab 3 ′ and the positive electrode tab 3.
  • the positive electrode plate 10 on which the positive electrode active material layer 9 is formed is produced, for example, as follows.
  • a lithium-containing oxide (positive electrode active material) lithium manganate powder, carbon powder as a conductive material, and polyvinylidene fluoride (hereinafter abbreviated as PVDF) as a binder are mixed, and N-methylpyrrolidone (dispersing solvent) is mixed therewith.
  • an appropriate amount of NMP is added and sufficiently kneaded and dispersed to obtain a slurry.
  • This slurry is applied to both surfaces of a 20 ⁇ m-thick strip-shaped aluminum foil to be the positive electrode current collector plate 12 by transfer and dried.
  • the aluminum foil coated with the positive-electrode active material having a length of several hundred meters is rolled. It is wound up as an electrode plate.
  • a strip-shaped electrode plate is pulled out from the roll-shaped electrode plate, and a tab 3 is formed by a tab-forming cutting machine, and is wound into a roll as a tab-shaped electrode plate.
  • a roll-shaped positive electrode is obtained by compressing with a predetermined press pressure by a roll press machine having a heated roll and winding it into a roll shape.
  • a strip-shaped positive electrode is drawn out from the roll-shaped positive electrode and cut into a predetermined width by a cutting device to obtain a rectangular positive plate 10 with a positive electrode tab 3 on which a positive electrode active material layer is formed.
  • the negative electrode plate 10 ′ is made by mixing a carbon material (negative electrode active material) and PVDF as a binder, adding an appropriate amount of NMP, sufficiently kneading, and dispersing to make a slurry.
  • This slurry is applied to both sides of a 10 ⁇ m thick copper foil to be a negative electrode current collector by transfer, dried, and wound up as a rolled electrode plate.
  • the subsequent tab forming process and subsequent steps are the same as the manufacturing process of the positive electrode plate 10.
  • the positive electrode plate 10 and the negative electrode plate 10 ′ with tabs cut to a predetermined width and the separator are stacked to form the electrode plate group 2.
  • each device is equipped with various rotary rolls for feeding, guiding, direction changing, tension adjustment, etc., and the strip-shaped metal current collector plate passes while contacting the rotary rolls. . Since the band-shaped metal current collector is produced while being in contact with the roll as described above, the metal current collector plate (12 or 12 ′) is applied to the electrode plate as it is a thin foil of 10 ⁇ m to 20 ⁇ m when passing through the roll portion. If the tab length dimension T, T 'is large due to tension balance, conveyance deviation, temperature distribution in the electrode plate, etc., it will bend by its own weight, cannot follow the roll diameter, will warp, There is a possibility of cracking.
  • Ultrasonic bonding was used for the bonding of the positive electrode current collector 4B of the positive electrode terminal 4 and the plurality of positive electrode tabs 3 and the bonding of the negative electrode current collector 4′B of the negative electrode plate 4 ′ and the plurality of negative electrode tabs 3 ′.
  • the welded portion of the plurality of positive electrode tabs 3 is joined to the positive electrode current collector 4B of the positive electrode terminal 4
  • the welded portion of the plurality of negative electrode tabs 3 ′ is joined to the negative electrode current collector 4′B of the negative electrode terminal. It is joined.
  • the tab corners are formed at right angles, but the base of the tabs are not formed at right angles but curved so that cracks do not occur due to the tensile stress generated in the winding process. It is preferred that
  • the positive electrode tab 3 and the negative electrode tab 3 ′ were changed from 30 mm to 80 mm as shown in Table 1 to produce a positive electrode plate 10 and a negative electrode plate 10 ′.
  • the width dimensions L and L ′ of the positive electrode current collector plate 12 and the negative electrode current collector plate 12 ′ were 178 mm in both the examples and the comparative examples.
  • the length h of the active material applied to the positive electrode current collector plate 12 and the negative electrode current collector plate 12 ′ was 130 mm.
  • lithium ion batteries having a capacity of 100 Ah were produced. This battery is usually capable of a large discharge current of 100A to 500A.
  • the quality of processing was evaluated as x when 20% or more of tabs were cut out of the total number of tabs during the manufacturing process of the positive electrode plate 10 and the negative electrode plate 10 '. .
  • the tab breakage was 20% or less when the tab width dimensions W and W ′ were larger than the tab length dimensions T and T ′.
  • the tab widths W and W ′ are smaller than the tab lengths T and T ′, tab breakage occurs more than 20%, and the yield is low. Therefore, it is difficult to substantially manufacture the battery.
  • the active material temperature rise value in Table 1 is the maximum surface temperature of the active material layer when measuring the discharge characteristics of the batteries having the tab shape of the produced examples and comparative examples. Even if the tab width dimensions W and W ′ are the same, if the tab length dimensions T and T ′ are long, the temperature rise of the active material tends to increase due to heat generation in the tab portion. Further, it was found that even if the tab length dimension T is the same, if the tab width dimensions W and W ′ are large, the temperature rise of the active material can be suppressed small.
  • the active material temperature rise ⁇ T is 35 ° C. or less, the temperature of the active material is 55 ° C. or less, so that elution of manganese from the positive electrode plate can be suppressed and battery deterioration can be suppressed.
  • the active material temperature rise ⁇ T can be made lower than 30 ° C.
  • Comparative Example 1 to Comparative Example 6 in which the tab width dimensions W and W ′ were 30 mm and 40 mm were not suitable for large current discharge because the temperature increase in the active material was larger than 35 ° C.
  • the tab width dimensions W and W ′ were 50 mm
  • the tab length dimensions T and T ′ were 20 mm or less
  • the temperature was 35 ° C. or less.
  • Comparative Example 7 and Comparative Example 8 were found to be larger than 35 ° C. because the tab length T was long, and the dimensions were inappropriate for use as a battery.
  • the tab width W was increased to 60 mm, the tab length T was 29 mm or less and 35 ° C.
  • Comparative Example 9 having the same tab width had good workability, but the temperature increase was larger than 35 ° C., and Comparative Example 10 was unsatisfactory in both workability and temperature increase.
  • the tab width dimensions W and W ′ were 70 mm, as shown in Example 4 and Example 5, the temperature increase was suppressed to 35 ° C. or less up to a tab length of 38 mm.
  • Comparative Example 11 in which the same tab width dimensions W and W ′ are 70 mm, the workability is good, but since the tab length is long, the temperature rise is higher than 35 ° C., and Comparative Example 12 is unsatisfactory in workability and temperature rise. there were.
  • the temperature rise can be suppressed to 35 ° C. or less in Examples 6 and 7 where the tab length dimensions T and T ′ are 42 mm or less.
  • the temperature rise increased more than 35 ° C.
  • the tab width dimensions W and W ′ are 1.82 times or more of the tab length dimensions T and T ′
  • the temperature rise can be suppressed to 35 ° C. or less.
  • the tab width dimensions W and W ′ were 28% or more of the width dimension L of the positive electrode current collector plate 12 and the negative electrode current collector plate 12 ′, the temperature increase could be suppressed to 35 ° C. or less.
  • the width dimension of the negative electrode tab is W ′
  • the length method of the negative electrode tab is T ′
  • the width dimension of the positive electrode tab is W
  • the width dimension of the negative electrode current collector plate is L
  • the width dimension of the positive electrode current collector plate is L
  • the width of the negative electrode tab is W ′
  • the width of the positive electrode tab is W
  • the negative electrode current collector When the width dimension of the plate is L ′ and the width dimension of the positive electrode current collector plate is L, 45> [(W / L) ⁇ 100]> 28 (1) 45> [(W ′ / L ′) ⁇ 100]> 28 (2) If the above relationship is satisfied, deterioration in workability of the negative electrode tab and the positive electrode tab can be suppressed, and heat generation at the junction between the negative electrode tab and the negative electrode collector and between the positive electrode tab and the positive electrode collector is caused.

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JP2018156901A (ja) * 2017-03-21 2018-10-04 株式会社東芝 二次電池、電池パック、及び車両
JP2019096591A (ja) * 2017-11-22 2019-06-20 寧徳時代新能源科技股▲分▼有限公司Ｃｏｎｔｅｍｐｏｒａｒｙ Ａｍｐｅｒｅｘ Ｔｅｃｈｎｏｌｏｇｙ Ｃｏ．， Ｌｉｍｉｔｅｄ 電極部材、電極ユニット及び充電電池
CN114975864A (zh) * 2021-02-23 2022-08-30 北京小米移动软件有限公司 极片、电芯结构、锂电池以及电子设备

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JP2018156901A (ja) * 2017-03-21 2018-10-04 株式会社東芝 二次電池、電池パック、及び車両
JP2019096591A (ja) * 2017-11-22 2019-06-20 寧徳時代新能源科技股▲分▼有限公司Ｃｏｎｔｅｍｐｏｒａｒｙ Ａｍｐｅｒｅｘ Ｔｅｃｈｎｏｌｏｇｙ Ｃｏ．， Ｌｉｍｉｔｅｄ 電極部材、電極ユニット及び充電電池
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CN114975864A (zh) * 2021-02-23 2022-08-30 北京小米移动软件有限公司 极片、电芯结构、锂电池以及电子设备

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