WO2018135011A1 - Wound-type battery - Google Patents

Wound-type battery Download PDF

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Publication number
WO2018135011A1
WO2018135011A1 PCT/JP2017/010543 JP2017010543W WO2018135011A1 WO 2018135011 A1 WO2018135011 A1 WO 2018135011A1 JP 2017010543 W JP2017010543 W JP 2017010543W WO 2018135011 A1 WO2018135011 A1 WO 2018135011A1
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WO
WIPO (PCT)
Prior art keywords
negative electrode
electrode
positive electrode
wound
battery
Prior art date
Application number
PCT/JP2017/010543
Other languages
French (fr)
Japanese (ja)
Inventor
阿部　敏浩
山中　英明
拓磨 森下
Original Assignee
マクセルホールディングス株式会社
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Priority to JP2017517145A priority Critical patent/JPWO2018135011A1/en
Publication of WO2018135011A1 publication Critical patent/WO2018135011A1/en

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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
    • H01M50/572—Means for preventing undesired use or discharge
    • H01M50/584—Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries
    • H01M50/59—Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries characterised by the protection means
    • H01M50/595—Tapes
    • 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
    • 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
    • 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
    • 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
    • H01M4/134—Electrodes based on metals, Si or alloys
    • 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
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/46—Alloys based on magnesium or aluminium
    • 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
    • H01M50/572—Means for preventing undesired use or discharge
    • H01M50/584—Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries
    • H01M50/586—Means for preventing undesired use or discharge for preventing incorrect connections inside or outside the batteries inside the batteries, e.g. incorrect connections of electrodes
    • 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

Definitions

  • the present invention relates to a wound battery having an electrode body formed by winding a positive electrode, a negative electrode, and a separator, each formed in a strip shape, in an overlapped state.
  • Patent Document 1 discloses a cylindrical type by winding a positive electrode plate, a negative electrode plate, and a separator interposed between the electrode plates using a winding core. A method of obtaining a flat spiral electrode body by producing an electrode body and pressing the electrode body is disclosed.
  • Patent Document 2 discloses that an alloy of lithium and aluminum, lead, zinc, tin or the like is used as the negative electrode active material. Patent Document 2 also discloses that when such a lithium alloy is used as a negative electrode active material, dendrites are generated in the lithium alloy and become fine powder as the battery is charged and discharged. .
  • Patent Document 2 when a lithium alloy is used as the negative electrode active material, there is a possibility that the lithium alloy of the negative electrode is pulverized by charging and discharging of the battery. If it does so, a part of micronized lithium alloy may fall out from a negative electrode within a battery.
  • the end of the negative electrode winding end of the negative electrode in the electrode body means the end of the negative electrode in the longitudinal direction and the portion located on the outermost periphery of the negative electrode in the electrode body.
  • the dropped part affects the electrical characteristics of the negative electrode. Therefore, the battery characteristics of the wound battery may be deteriorated.
  • An object of the present invention is to provide a wound battery including an electrode body formed by winding a positive electrode, a negative electrode, and a separator, each formed in a strip shape, and the negative electrode contains a metal alloyed with Li. It is to prevent the end portion of the negative electrode from being wound down and falling off due to charge / discharge.
  • a positive electrode, a negative electrode, and a separator each formed in a strip shape are wound so that the separator is positioned between the positive electrode and the negative electrode,
  • An extending columnar electrode body is provided.
  • the negative electrode includes an element that can be alloyed with Li.
  • the end of winding of the negative electrode in the electrode body is covered with a protective member.
  • the electrode body has a columnar shape wound so that the separator is positioned between the positive electrode and the negative electrode.
  • the negative electrode includes an element that can be alloyed with Li, and a winding end portion of the negative electrode in the electrode body is covered with a protective member.
  • FIG. 1 is a perspective view illustrating a schematic configuration of the wound battery according to the embodiment.
  • FIG. 2 is a cross-sectional view showing the configuration of the wound battery along the line II-II in FIG.
  • FIG. 3 is a diagram schematically showing the arrangement of the positive electrode, the negative electrode, and the separator.
  • FIG. 4 is a diagram schematically illustrating a state where the positive electrode, the negative electrode, and the separator are wound in a state where they are stacked in the thickness direction.
  • FIG. 7 is a perspective view showing a schematic configuration of a wound battery according to another embodiment.
  • a positive electrode, a negative electrode, and a separator each formed in a strip shape are wound so that the separator is positioned between the positive electrode and the negative electrode,
  • An extending columnar electrode body is provided.
  • the negative electrode includes an element that can be alloyed with Li.
  • the end of winding of the negative electrode in the electrode body is covered with a protective member (first configuration).
  • the negative electrode containing an element that can be alloyed with Li an alloy with Li is generated when the battery is charged. Therefore, in the said negative electrode, micronization may arise by charging / discharging of a battery.
  • the end of winding of the negative electrode in the electrode body is covered with a protective member, so that an alloy with Li is not generated in the portion covered with the protective member. Therefore, in the part covered with the said protection member, pulverization does not arise by charging / discharging of a battery.
  • the end of winding end of the negative electrode in the electrode body means the end of the negative electrode in the longitudinal direction and the portion located on the outermost periphery of the negative electrode in the electrode body.
  • the end of the negative electrode in the electrode body is covered with a protective member, so that the separator can be prevented from being damaged by the end.
  • the protective member is provided so as to cover the end of winding of the negative electrode from one end to the other end in the short direction of the negative electrode (second). Configuration).
  • the above configuration can more reliably prevent the separator from being damaged by the winding end portion of the negative electrode.
  • the protective member is provided so as to cover a winding end end portion of the negative electrode and a portion within a predetermined range from the winding end end portion in the short-side end portion of the negative electrode. (Third configuration).
  • the separator can be prevented from being damaged by the winding end side of the negative electrode. Therefore, it is possible to more reliably prevent the separator from being damaged by the negative electrode.
  • the positive electrode includes a positive electrode active material layer.
  • the protective member is provided in a portion of the winding end portion of the negative electrode that overlaps the positive electrode active material layer with the separator interposed therebetween in a radial direction of the electrode body (fourth configuration).
  • the negative electrode and the positive electrode active material layer may come into contact with each other to cause a short circuit.
  • a protective member in the portion as described above it is possible to prevent the negative electrode and the positive electrode active material layer from being short-circuited due to damage to the separator by the negative electrode.
  • the protective member is provided so as to cover both surfaces of the winding end portion of the negative electrode (fifth configuration). Thereby, it can prevent more reliably that the winding end part of the negative electrode in an electrode body pulverizes and a part falls off by charging / discharging of a battery.
  • the protective member is provided so as to partially cover an end surface extending in the thickness direction of the negative electrode (sixth configuration). As a result, when burrs, protrusions, etc. are formed on the end surface extending in the thickness direction at the end of winding of the negative electrode in the electrode body, the end surface is in direct contact with the separator and the separator is damaged. Can be prevented.
  • the protection member is made of an electrically insulating material that does not contribute to the battery reaction (seventh configuration).
  • the protective member provided on the negative electrode can prevent a short circuit from occurring inside the battery and can also prevent the battery characteristics from being affected.
  • the negative electrode includes a Li—Al alloy as a negative electrode active material after charging the battery (eighth configuration).
  • the negative electrode is pulverized by charging and discharging of the battery. Even in the case where the Li—Al alloy is generated in the negative electrode in this way, by applying the first to seventh configurations described above, the winding end portion of the negative electrode in the electrode body is pulverized and partly falls off. This can be effectively suppressed.
  • the negative electrode is a laminate having a metal base layer that is not alloyed with Li and a metal surface layer joined to at least one of the metal base layers in the thickness direction. At least the surface side of the metal surface layer contains the Li—Al alloy after charging the battery (ninth configuration).
  • the negative electrode has a metal base layer and a metal surface layer as in the above-described configuration, the negative electrode has high rigidity. Therefore, in an electrode body wound with the positive electrode, the negative electrode, and the separator being stacked, a force that is displaced in the radial direction of the electrode body is more likely to be generated at the end of winding of the negative electrode. Therefore, there is a high possibility that the winding end portion of the negative electrode in the electrode body will damage the separator.
  • the first to seventh configurations described above are more effective in preventing the separator from being damaged in the electrode body wound using the negative electrode having the configuration described above.
  • FIG. 1 is a perspective view showing a schematic configuration of a wound battery 1 according to an embodiment of the present invention.
  • the wound battery 1 includes a bottomed cylindrical outer can 10, a cover plate 20 that covers an opening of the outer can 10, and an electrode body 30 that is accommodated in the outer can 10.
  • a rectangular parallelepiped battery case 2 (exterior body) having a rectangular parallelepiped space is formed.
  • a non-aqueous electrolyte is also enclosed in the battery case 2.
  • the outer can 10 is a bottomed cylindrical member made of an aluminum alloy, and constitutes the battery case 2 together with the cover plate 20.
  • the outer can 10 is a bottomed cylindrical member having a rectangular bottom surface 11 in a top view.
  • the outer can 10 includes a bottom surface 11 and a flat cylindrical side wall 12. That is, the outer can 10 is formed in a flat shape such that the dimension in the thickness direction corresponding to the short side direction of the bottom surface 11 is smaller than the width direction corresponding to the long side direction of the bottom surface 11.
  • the outer can 10 is joined to a lid plate 20 connected to a positive electrode lead (not shown), it also serves as a positive electrode terminal of the wound battery 1.
  • a positive electrode 31 described later of the electrode body 30 is connected to the lid plate 20 by a positive electrode lead (not shown).
  • the lid plate 20 is joined to the opening of the outer can 10 by welding so as to cover the opening of the outer can 10. Thereby, the upper surface of the battery case 2 is formed by the cover plate 20. Similar to the outer can 10, the lid plate 20 is made of a member made of an aluminum alloy and is formed in a rectangular shape so as to be fitted inside the opening of the outer can 10. Moreover, the through-hole 20a is formed in the center part of the longitudinal direction at the cover board 20 (refer FIG. 2).
  • an insulating packing 21 made of polypropylene and a negative electrode terminal 22 made of stainless steel are inserted into the through hole 20 a of the cover plate 20.
  • a substantially cylindrical insulating packing 21 into which a substantially columnar negative electrode terminal 22 is inserted is fitted to the peripheral edge of the through hole 20a.
  • the negative electrode terminal 22 has a configuration in which flat portions are integrally formed at both ends of a cylindrical shaft portion.
  • the negative electrode terminal 22 is arranged with respect to the insulating packing 21 so that the flat surface portion is exposed to the outside and the shaft portion is positioned in the insulating packing 21.
  • a stainless steel lead plate 27 is connected to the negative terminal 22. Thereby, the negative electrode terminal 22 is electrically connected to the negative electrode 32 of the electrode body 30 via the lead plate 27 and the negative electrode lead 35 described later.
  • An insulator 26 is disposed between the lead plate 27 and the lid plate 20.
  • a resin insulating plate 36 is disposed between the negative electrode terminal 22 attached to the cover plate 20 and the electrode body 30 between the negative electrode terminal 22 attached to the cover plate 20 and the electrode body 30, a resin insulating plate 36 is disposed.
  • a negative electrode lead 35 penetrates the insulating plate 36.
  • a positive electrode lead (not shown) extends to the lid plate 20 through the insulating plate 36 or through the side of the insulating plate 36.
  • a non-aqueous electrolyte inlet 24 is formed in the lid plate 20 along with the negative electrode terminal 22.
  • the injection port 24 is formed in a substantially circular shape in plan view.
  • the injection port 24 has a small diameter portion and a large diameter portion so that the diameter changes in two steps in the thickness direction of the lid plate 20.
  • the injection port 24 is sealed by a sealing plug 25 formed in a step shape corresponding to a change in the diameter of the injection port 24.
  • the outer peripheral portion on the large diameter side of the sealing plug 25 and the peripheral portion of the injection port 24 are joined by laser welding so that no gap is generated between the sealing plug 25 and the peripheral portion of the injection port 24.
  • the inlet 24 and the sealing plug 25 are not limited to the above-described configuration, and may have any configuration as long as it can be sealed after injecting the nonaqueous electrolytic solution into the battery case 2. .
  • the electrode body 30 is formed in a state in which the positive electrode 31 and the negative electrode 32 formed in a strip shape are overlapped with each other so that the separators 33 are positioned between them and below the positive electrode 31 (see FIG. 3).
  • the wound electrode body is formed by winding the positive electrode 31, the negative electrode 32, and the separator 33 in the direction of the white arrow in FIG.
  • a state in which the electrode body 30 is configured by winding the positive electrode 31, the negative electrode 32, and the separator 33 is schematically shown in FIG.
  • the electrode body 30 is formed in a flat shape after being wound in a state where the positive electrode 31, the negative electrode 32, and the separator 33 are overlapped (see FIG. 5). That is, the electrode body 30 is obtained by crushing a cylindrical wound body extending along the axis L to make it flat. As shown in FIG. 2, the flat electrode body 30 is accommodated in the battery case 2.
  • the electrode body 30 formed flat as described above has a pair of bent portions 30a bent so that the positive electrode 31, the negative electrode 32, and the separator 33 are folded back in the thickness direction.
  • the pair of bent portions 30a are located at the ends in the width direction when the electrode body 30 is viewed from the side.
  • the electrode body 30 shown in FIG. 2 is only shown for several layers on the outer peripheral side. However, in FIG. 2, the illustration of the inner peripheral side portion of the electrode body 30 is omitted, and naturally, the positive electrode 31, the negative electrode 32, and the separator 33 are also present on the inner peripheral side of the electrode body 30. .
  • FIG. 3 the positions of the positive electrode 31, the negative electrode 32, and the separator 33 are moved from the actual arrangement and shown in perspective in order to illustrate a state in which the positive electrode 31, the negative electrode 32, and the separator 33 are overlapped.
  • the positive electrode current collector 41, the positive electrode active material layer 42, and the negative electrode 32 of the positive electrode 31 are hatched, although not in cross section.
  • the axial direction of the electrode body 30 means a direction along the axis L.
  • the radial direction of the electrode body 30 means a direction along the thickness direction of the positive electrode 31, the negative electrode 32, and the separator 33 constituting the electrode body 30.
  • the positive electrode 31 has a positive electrode active material layer 42 containing a positive electrode active material provided on one or both sides of a positive electrode current collector 41 made of a metal foil such as aluminum (see FIG. 6).
  • the positive electrode active material layer 42 is provided on both surfaces of the positive electrode current collector 41).
  • the positive electrode 31 has a positive electrode active material that is a lithium-containing oxide capable of occluding and releasing lithium ions, a positive electrode mixture containing a conductive additive and a binder on a positive electrode current collector 41 made of aluminum foil or the like. It is formed by applying and drying.
  • the positive electrode active material layer 42 is formed on the positive electrode current collector 41 other than one end in the longitudinal direction.
  • lithium-containing oxide that is a positive electrode active material examples include Li 1 + x M 1 O 2 ( ⁇ 0.1 ⁇ x ⁇ 0.1, M 1 : Co, Ni, Mn, Al, Mg, Ti, Zr, and the like.
  • Lithium-containing composite oxide having a layered structure represented by one or more selected elements LiMn 2 O 4 or a lithium manganese composite oxide having a spinel structure in which a part of the element is substituted with another element, Li 4 / 3 Ti 5/3 O 4 and a lithium manganese composite oxide synthesized at a low temperature represented by a composition such as a lithium titanium composite oxide having a spinel structure in which part of the element is substituted with another element, LiMn 3 O 6
  • an olivine type compound represented by LiM 2 PO 4 M 2 : one or more elements selected from Co, Ni, Mn, Fe, etc.
  • lithium-containing composite oxide having a layered structure examples include lithium cobalt oxide such as LiCoO 2 and LiNi 1-a Co ab Al b O 2 (0.1 ⁇ a ⁇ 0.3, 0.01 ⁇ b ⁇ 0.2), an oxide containing at least Co, Ni and Mn (LiMn 1/3 Ni 1/3 Co 1/3 O 2 , LiMn 5/12 Ni 5/12 Co 1/6 O 2 , LiNi 3/5 Examples thereof include lithium-containing nickel composite oxides such as Mn 1/5 Co 1/5 O 2 . Note that only one type of material may be used as the positive electrode active material, or two or more types of materials may be used. Further, the positive electrode active material is not limited to the above-described materials.
  • the battery is assembled using a laminate of the negative electrode current collector and the Al layer as the negative electrode precursor, and the assembled battery is charged to form the negative electrode It is preferable to produce this Li—Al alloy because part or all of the irreversible capacity of the positive electrode can be offset by the negative electrode.
  • binders for the positive electrode mixture examples include polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), styrene butadiene rubber (SBR), carboxymethyl cellulose (CMC), and imide binders (polyamideimide, polyimide, etc.), An amide binder (polyamide, aramid, etc.) can be used.
  • PVDF polyvinylidene fluoride
  • PTFE polytetrafluoroethylene
  • SBR styrene butadiene rubber
  • CMC carboxymethyl cellulose
  • imide binders polyamideimide, polyimide, etc.
  • An amide binder polyamide, aramid, etc.
  • conductive assistants related to the positive electrode mixture include graphite (graphite carbon material) such as natural graphite (flaky graphite), artificial graphite; acetylene black, ketjen black, channel black, furnace black, lamp black, Carbon materials such as carbon black such as thermal black; carbon fiber; and the like can be used.
  • graphite carbon material such as natural graphite (flaky graphite), artificial graphite; acetylene black, ketjen black, channel black, furnace black, lamp black, Carbon materials such as carbon black such as thermal black; carbon fiber; and the like can be used.
  • the positive electrode 31 having the positive electrode active material layer 42 and the positive electrode current collector 41 includes, for example, a positive electrode active material, a conductive additive, a binder, and the like in water or an organic solvent such as N-methyl-2-pyrrolidone (NMP). Disperse to prepare a positive electrode mixture-containing composition (slurry, paste, etc.) (the binder may be dissolved in a solvent), which is applied onto the positive electrode current collector 41 and dried, and if necessary It can manufacture by passing through the process of performing press processes, such as a calendar process.
  • NMP N-methyl-2-pyrrolidone
  • the content of the positive electrode active material in the positive electrode mixture is preferably 80 to 98.8% by mass.
  • the content of the conductive auxiliary in the positive electrode mixture is preferably 1.5 to 10% by mass.
  • the binder content in the positive electrode mixture is preferably 0.3 to 10% by mass.
  • the thickness of the positive electrode active material layer 42 is preferably 30 to 300 ⁇ m.
  • the positive electrode current collector 41 a metal foil such as Al and Al alloy, a punching metal, a net, an expanded metal, or the like can be used, but an Al foil is usually preferably used.
  • the thickness of the positive electrode current collector 41 is preferably 10 to 30 ⁇ m.
  • the positive electrode lead is connected to a portion of the positive electrode current collector 41 where the positive electrode mixture is not applied, that is, a portion where the positive electrode current collector 41 is exposed.
  • the negative electrode 32 has a metal base layer 45 containing a copper alloy, and a metal surface layer 46 located on both surfaces of the metal base layer 45 and containing an aluminum alloy.
  • the negative electrode 32 is made of, for example, a clad material composed of a layer containing a copper alloy and a layer containing an aluminum alloy positioned on both surfaces of the layer.
  • the negative electrode 32 has a longer dimension and a shorter dimension in the plan view than the positive electrode active material layer 42 of the positive electrode 31.
  • the negative electrode 32 contains a Li—Al alloy on at least the surface side of the portion of the metal surface layer 46 that overlaps the positive electrode active material layer 42 of the positive electrode 31 in the thickness direction with the separator 33 interposed therebetween after charging of the wound battery 1. . That is, the negative electrode 32 having the metal base layer 45 and the metal surface layer 46 is used as a precursor to charge the wound battery 1 assembled together with the positive electrode 31 described above, thereby sandwiching the separator 33 in the metal surface layer 46. The portion of the positive electrode 31 that overlaps the positive electrode active material layer 42 in the thickness direction is electrochemically reacted with Li ions in the non-aqueous electrolyte. As a result, a Li—Al alloy is formed on at least the surface side of the metal surface layer 46 of the negative electrode 32 that overlaps the positive electrode active material layer 42 of the positive electrode 31 in the thickness direction with the separator 33 interposed therebetween.
  • the metal base layer 45 may be made of nickel or the like.
  • the metal substrate layer 45 may be laminated with the metal surface layer 46 by pressure bonding or the like.
  • the metal surface layer 46 may be provided only on one side of the metal base layer 45.
  • a metal layer containing an element that can be alloyed with Li (for example, Si or Sn) may be provided on one side or both sides of the metal base layer 45.
  • the thickness of the metal surface layer 46 provided on one surface of the metal base layer 45 is preferably 5 ⁇ m or more, more preferably 10 ⁇ m or more, and further preferably 15 ⁇ m or more.
  • the metal surface layer 46 has a thickness of 150 ⁇ m or less, more preferably 70 ⁇ m or less, and more preferably 50 ⁇ m or less, on the one surface of the metal base layer 45. preferable.
  • the negative electrode 32 has an electrical insulating property at the end of the negative electrode 32 in the longitudinal direction and at the outermost periphery of the negative electrode 32 in the electrode body 30, that is, at the end of the winding end, and does not contribute to the battery reaction.
  • a resin protection member 55 is provided.
  • the protective member 55 is provided at the end of the negative electrode 32 at the end of winding, thereby preventing the negative electrode 32 from being pulverized and partially falling off during charging and discharging of the battery.
  • the protective member 55 is provided at an end portion on the winding end side in the longitudinal direction of the negative electrode 32 and a portion within a predetermined range from the end portion in the longitudinal direction. A detailed configuration of the protection member 55 will be described later.
  • the separator 33 preferably has a property (that is, a shutdown function) that closes the pores at 80 ° C. or higher (more preferably 100 ° C. or higher) and 170 ° C. or lower (more preferably 150 ° C. or lower).
  • the separator 33 can use the separator used for the normal nonaqueous electrolyte secondary battery etc., for example, the microporous film made from polyolefin, such as polyethylene (PE) and polypropylene (PP).
  • the microporous membrane constituting the separator 33 may be, for example, one using only PE or one using only PP, or a laminate of a PE microporous membrane and a PP microporous membrane. It may be.
  • the thickness of the separator 33 is preferably 10 to 30 ⁇ m, for example.
  • a laminated separator in which a heat-resistant porous layer containing an inorganic filler or the like is provided on the surface of a polyolefin microporous film as described above, or tetrafluoroethylene-perfluoro Fluorine resins such as alkoxyethylene copolymers (PFA), polyphenylene sulfide (PPS), polyether ether ketone (PEEK), polybutylene terephthalate (PBT), polymethylpentene, cellulose, aramid, polyimide, polyamideimide, and other heat resistant resins
  • PFA alkoxyethylene copolymers
  • PPS polyphenylene sulfide
  • PEEK polyether ether ketone
  • PBT polybutylene terephthalate
  • a non-woven fabric separator or the like can also be used.
  • Nonaqueous electrolyte solvents include, for example, ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), dimethyl carbonate (DMC), diethyl carbonate (DEC), methyl ethyl carbonate (MEC), and lactone rings.
  • EC ethylene carbonate
  • PC propylene carbonate
  • BC butylene carbonate
  • DMC dimethyl carbonate
  • DEC diethyl carbonate
  • MEC methyl ethyl carbonate
  • lactone rings lactone rings
  • aprotic organic solvent such as phosphoric acid triester (trimethyl phosphate, triethyl phosphate, etc.), trimethoxymethane, sulfolane, 3-methyl-2-oxazolidinone, diethyl ether, etc. Rahidorofuran etc.) and the like can be used as alone in a mixed solvent or a mixture of two or more.
  • the lithium salt according to the non-aqueous electrolyte for example, LiClO 4, LiPF 6, LiBF4 , LiAsF 6, LiSbF 6, LiCF 3 SO 3, LiCF 3 CO 2, Li 2 C 2 F 4 (SO 3) 2, LiN ( FSO 2 ) 2 , LiN (CF 3 SO 2 ) 2 , LiC (CF 3 SO 2 ) 3 , LiC n F 2n + 1 SO 3 (n ⁇ 2), LiN (RfOSO 2 ) 2 [where Rf is a fluoroalkyl group] And at least one selected from the above.
  • LiClO 4 LiPF 6, LiBF4 , LiAsF 6, LiSbF 6, LiCF 3 SO 3, LiCF 3 CO 2, Li 2 C 2 F 4 (SO 3) 2, LiN ( FSO 2 ) 2 , LiN (CF 3 SO 2 ) 2 , LiC (CF 3 SO 2 ) 3 , LiC n F 2n + 1 SO 3 (n ⁇ 2), LiN (RfOSO
  • the concentration of the non-aqueous electrolyte of these lithium salts is preferably 0.6 to 1.8 mol / l, more preferably 0.9 to 1.6 mol / l.
  • Two or more lithium salts may be used in combination, and in that case, the total concentration of the lithium salts may be adjusted to fall within the above range.
  • vinylene carbonates for the purpose of further improving various characteristics of the battery, vinylene carbonates, cyclic sultone compounds such as 1,3-propane sultone and 1,3-propene sultone, disulfide compounds such as diphenyl disulfide, Benzene compounds such as cyclohexylbenzene, biphenyl, fluorobenzene, t-butylbenzene, fluorine-substituted cyclic carbonates such as 4-fluoro-1,3-dioxolan-2-one (FEC), lithium tetrakis (acetate) borate, Additives such as lithium organic borate such as lithium bis (oxalate) borate (LiBOB) can be added as appropriate.
  • cyclic sultone compounds such as 1,3-propane sultone and 1,3-propene sultone
  • disulfide compounds such as diphenyl disulfide
  • Benzene compounds such as
  • non-aqueous electrolyte the above-mentioned solution (non-aqueous electrolyte) may be used in the form of a gel (gel electrolyte) using a known polymer or other gelling agent.
  • the winding end end portion of the electrode body 30 (the end portion in the longitudinal direction of the negative electrode 32 and the outermost periphery of the negative electrode 32 in the electrode body 30).
  • the protective member 55 is provided on the portion to be protected. In the longitudinal direction of the negative electrode 32, the protective member 55 is provided with a first protective portion 55 a provided from one end portion in the short direction of the negative electrode 32 to the other end portion at the winding end end portion of the electrode body 30.
  • the protection member 55 has second protection portions 55 b provided in a predetermined range from the end portion on the winding end side in the longitudinal direction of the negative electrode 32 at both ends in the short direction of the negative electrode 32. That is, the protection member 55 is provided in a U shape on the winding end side of the negative electrode 32 when viewed from the thickness direction.
  • the protection member 55 may have only the first protection part 55 a provided at the end of the negative electrode 32 on the winding end side in the longitudinal direction of the negative electrode 32, or the second protection part 55 b may be the negative electrode 32. It may be provided only at one end in the short direction.
  • the predetermined range is a range in which pulverization occurs in the negative electrode 32 by charging the wound battery 1.
  • the range in which pulverization occurs in the negative electrode 32 is a range in which a Li—Al alloy is generated in the metal surface layer 46 of the negative electrode 32.
  • the range in which the Li—Al alloy is generated includes the range in which the negative electrode 32 overlaps the positive electrode active material layer 42 when the negative electrode 32 is viewed in the thickness direction, and the repeated charging and discharging of the battery when the Li—Al alloy is generated. And the range in which Li—Al alloying proceeds.
  • the predetermined range may be from one end in the longitudinal direction of the negative electrode 32 to the other end.
  • the first protection part 55 a of the protection member 55 may be provided only at a part of the negative electrode 32 in the short direction at the winding end end of the negative electrode 32 in the electrode body 30.
  • the protective member 55 is preferably provided in a portion of the end portion on the winding end side of the negative electrode 32 that overlaps the positive electrode active material layer 42 in the thickness direction in the electrode body 30.
  • a protective member 55 can be provided. Accordingly, it is possible to more reliably prevent the pulverization of the negative electrode 32 at the end of the negative electrode 32 on the winding end side.
  • the protective member 55 is provided on both surfaces of the end portion of the negative electrode 32 on the winding end side so as to straddle the end surface of the end portion. That is, the protection member 55 is provided in a U-shape when viewed in a cross section perpendicular to the longitudinal direction of the negative electrode 32 (see FIG. 6). In this way, by providing the protective member 55 on the end surface extending in the thickness direction of the negative electrode 32, when the burr or the projection is formed on the end surface, the separator 33 is damaged by the burr or the projection. Can be prevented.
  • the protective member 55 may be provided only on both surfaces of the negative electrode 32 on the winding end side. That is, the protection member 55 may not be provided on the end surface of the end portion on the winding end side of the negative electrode 32.
  • the protective member 55 is formed of tape or resin as will be described later, and is a member different from the negative electrode 32. Thereby, the thickness of the protection member 55 can be adjusted easily.
  • the protective member 55 is made of resin tape (polyethylene terephthalate (PET) tape, polypropylene (PP) tape, polyphenylene sulfide resin (PPS) tape, polyimide tape, etc.), or various resins or ultraviolet curable resins that are cured by ultraviolet rays. It is made of an electrically insulating material that does not contribute to the battery reaction, such as a molded member or an adhesive made of various resins.
  • resin tape polyethylene terephthalate (PET) tape, polypropylene (PP) tape, polyphenylene sulfide resin (PPS) tape, polyimide tape, etc.
  • various resins or ultraviolet curable resins that are cured by ultraviolet rays.
  • It is made of an electrically insulating material that does not contribute to the battery reaction, such as a molded member or an adhesive made of various resins.
  • the wound battery 1 by charging the battery, on the surface side of the metal surface layer 46 of the negative electrode 32 and at least a portion overlapping the positive electrode active material layer 42 when viewed from the thickness direction of the negative electrode 32, A layer containing a Li—Al alloy can be formed. Thereby, the winding type battery 1 with high heat resistance is obtained.
  • the end of winding of the negative electrode 32 in the electrode body 30 is covered with a protective member 55.
  • a protective member 55 it can prevent that pulverization arises in the winding end part of the negative electrode 32 by charging / discharging of the winding type battery 1.
  • FIG. Therefore, it is possible to prevent a part of the negative electrode 32 from falling off due to pulverization at the winding end end of the negative electrode 32. Therefore, it is possible to prevent the battery characteristics of the wound battery 1 from being deteriorated.
  • the protective member 55 is provided at the winding end of the negative electrode 32 so as to cover from one end of the negative electrode 32 in the short direction to the other end, so that the negative electrode 32 is provided at the winding end. Can be more reliably prevented from being pulverized and partly falling off.
  • the protective member 55 so as to cover the end of winding of the negative electrode 32 and the end of the negative electrode 32 in a short direction, the end of winding of the negative electrode 32 is covered. It can prevent more reliably that pulverization and partial drop-off occur at the portion located on the side.
  • the protective member 55 is provided in a portion of the winding end end of the negative electrode 32 that overlaps the positive electrode active material layer 42 across the separator 33 in the radial direction of the electrode body 30. It can prevent more reliably that pulverization arises by charging / discharging of the winding type battery 1.
  • the electrode body 30 is accommodated in the rectangular battery case 2.
  • the electrode body 30 may be accommodated in an exterior body having another configuration.
  • the electrode body 30 may be accommodated in the laminate film exterior body, or may be accommodated in a battery case having another can structure.
  • FIG. 7 shows an example of a wound battery 101 in which the electrode body 30 is accommodated in a laminate film exterior body 110 (exterior body).
  • the wound battery 101 is a secondary battery having a rectangular shape in a plan view in which the electrode body 30 is covered with the laminate film exterior body 110.
  • the wound battery 101 includes an electrode body 30 and a laminate film exterior body 110 that covers the electrode body 30.
  • the wound battery 101 includes a positive electrode connection terminal 121 and a negative electrode connection terminal 122 that are electrically connected to the positive electrode 31 and the negative electrode 32 of the electrode body 30, respectively.
  • a non-aqueous electrolyte similar to that in the above-described embodiment is also enclosed in the wound battery 1.
  • the laminate film exterior body 110 is made of a material in which one side of an aluminum metal foil is covered with nylon and the other side is covered with polypropylene. That is, the laminate film exterior body 110 is made of a material obtained by laminating aluminum with nylon and polypropylene. Thereby, the laminate film exterior body 110 is welded by applying pressure while heating in a state where the laminate film exterior bodies 110 are overlapped.
  • the metal foil is not limited to aluminum but may be formed of other metal materials such as stainless steel.
  • the laminate film outer package 110 is formed in a substantially rectangular shape.
  • the outer peripheral sides of the laminate film exterior body 110 are welded together to form a bulging portion 101a and a seal portion 101b as shown in FIG.
  • the bulging portion 101a is formed by covering the electrode body 30 with the laminate film exterior body 110, and the bulging portion 101a is surrounded by welding the laminate film exterior body 110 to each other around the bulging portion 101a.
  • the seal portion 101b is formed.
  • the positive electrode connection terminal 121 and the negative electrode connection terminal 122 are laminated with the pair of laminate film exterior bodies 110 sandwiched therebetween.
  • the film exterior bodies 110 are fixed by welding.
  • the positive electrode connection terminal 121 and the negative electrode connection terminal 122 are respectively connected to a positive electrode lead and a negative electrode lead 35 attached to the electrode body 30.
  • the electrode body 30 covered with the laminate film exterior body 110 can be electrically connected to the outside.
  • the present invention is not limited to this, and one laminate film exterior body is folded back so as to sandwich the electrode body 30 therebetween. It may be welded.
  • the direction in which the laminate film exterior body is folded back may be the extending direction of the positive electrode connection terminal 121 and the negative electrode connection terminal 122 with respect to the electrode body 30 or the width direction.
  • the electrode body 30 has a flat cross section.
  • the electrode body may have a cylindrical shape having a circular cross section.
  • the negative electrode 32 is constituted by a clad material composed of the metal base layer 45 and the metal surface layer 46.
  • the negative electrode 32 may have a configuration other than the clad material as long as it has a metal base layer and a metal surface layer.
  • the negative electrode 32 is formed by combining a powder containing an element that can be alloyed with Li with a binder or the like, and applying the mixture onto the surface of a metal foil (metal substrate layer) that serves as a current collector. Also good.
  • a powder containing an element that can be alloyed with Li may be used in combination with a negative electrode active material (for example, a carbon material such as graphite) capable of inserting and extracting Li ions.
  • a negative electrode active material for example, a carbon material such as graphite
  • the negative electrode 32 has the metal surface layer 46 on both surfaces of the metal base layer 45.
  • the metal surface layer 46 may be provided only on one surface of the metal base layer 45.
  • the positive electrode may be disposed so that the positive electrode active material layer is positioned at a position facing the metal surface layer 46 with the separator 33 interposed therebetween.
  • the positive electrode 31 and the negative electrode 32 each formed in a strip shape are overlapped with the separator 33 such that the separator 33 is positioned between the two and the lower side of the positive electrode 31, for example.
  • the order in which the positive electrode 31, the negative electrode 32, and the separator 33 are stacked may be any order as long as the secondary battery can be configured.
  • the positive electrode 31 of the electrode body 30 is electrically connected to the outer can 10, but this is not restrictive, and the negative electrode 32 may be electrically connected to the outer can 10.
  • the present invention is applicable to a wound battery having an electrode body formed by winding a positive electrode, a negative electrode, and a separator.

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Abstract

This wound-type battery has an electrode body obtained by winding, in an overlapping manner, a positive electrode, a negative electrode, and a separator that are each shaped as a band, wherein the negative electrode contains a metal alloyed with Li. The trailing end of the wound negative electrode is prevented from disintegrating and falling out as a result of charging and discharging. This wound-type battery is provided with a columnar electrode body 30 that extends in the axial direction and in which a positive electrode 31, a negative electrode 32, and a separator 33 that are each shaped as a band are wound such that the separator 33 is positioned between the positive electrode 31 and the negative electrode 32. The negative electrode 32 contains an element that is alloyable with Li. The trailing end of the wound negative electrode 32 in the electrode body 30 is covered by a protective member 55.

Description

巻回型電池Winding battery
　本発明は、それぞれ帯状に形成された正極、負極及びセパレータを重ね合わせた状態で巻回してなる電極体を有する巻回型電池に関する。 The present invention relates to a wound battery having an electrode body formed by winding a positive electrode, a negative electrode, and a separator, each formed in a strip shape, in an overlapped state.
　従来より、それぞれ帯状に形成された正極、負極及びセパレータを重ね合わせた状態で巻回してなる電極体を有する巻回型電池が知られている。このような巻回型電池において、例えば特許文献１には、巻芯を用いて、正極板と、負極板と、それらの電極板間に介在するセパレータとを巻回することにより、円筒型の電極体を作製し、該電極体をプレスすることにより、扁平渦巻電極体を得る方法が開示されている。 Conventionally, a winding type battery having an electrode body formed by winding a positive electrode, a negative electrode, and a separator, each of which is formed in a strip shape, is known. In such a wound type battery, for example, Patent Document 1 discloses a cylindrical type by winding a positive electrode plate, a negative electrode plate, and a separator interposed between the electrode plates using a winding core. A method of obtaining a flat spiral electrode body by producing an electrode body and pressing the electrode body is disclosed.
　ここで、上述のような扁平渦巻電極体を有する二次電池として、負極に、負極活物質としてリチウム合金を含む構成が知られている。例えば特許文献２には、負極活物質として、リチウムと、アルミニウム、鉛、亜鉛、スズなどとの合金を用いる点が開示されている。また、前記特許文献２には、このようなリチウム合金を負極活物質として用いた場合に、電池の充放電に伴って、リチウム合金にデンドライトが生成されて、微粉化する点も開示されている。 Here, as a secondary battery having a flat spiral electrode body as described above, a structure including a lithium alloy as a negative electrode active material in a negative electrode is known. For example, Patent Document 2 discloses that an alloy of lithium and aluminum, lead, zinc, tin or the like is used as the negative electrode active material. Patent Document 2 also discloses that when such a lithium alloy is used as a negative electrode active material, dendrites are generated in the lithium alloy and become fine powder as the battery is charged and discharged. .
特許第４７８９５８４号公報Japanese Patent No. 4789854 特開平５－８２１２８号公報JP-A-5-82128
　ところで、前記特許文献２に開示されているように、負極活物質としてリチウム合金を用いた場合、電池の充放電によって、負極のリチウム合金が微粉化する可能性がある。そうすると、電池内で、微粉化したリチウム合金の一部が、負極から脱落する可能性がある。 By the way, as disclosed in Patent Document 2, when a lithium alloy is used as the negative electrode active material, there is a possibility that the lithium alloy of the negative electrode is pulverized by charging and discharging of the battery. If it does so, a part of micronized lithium alloy may fall out from a negative electrode within a battery.
　特に、前記特許文献１に開示されているように、正極、負極及びセパレータを重ねた状態で巻回することにより得られる電極体では、負極の巻き終わりの端部が上述のように微粉化した場合、該端部から微粉化した粒子が脱落しやすい。ここで、電極体における負極の巻き終わり端部とは、負極の長手方向の端部で且つ電極体において負極の最外周に位置する部分を意味する。 In particular, as disclosed in Patent Document 1, in the electrode body obtained by winding the positive electrode, the negative electrode, and the separator in a stacked state, the end of the negative electrode winding end was pulverized as described above. In this case, the finely divided particles are likely to fall off from the end. Here, the end of winding end of the negative electrode in the electrode body means the end of the negative electrode in the longitudinal direction and the portion located on the outermost periphery of the negative electrode in the electrode body.
　上述のように負極で微粉化が生じて一部が脱落した場合、該脱落した部分において、負極の電気特性に影響を与える。そのため、巻回型電池の電池特性が低下する可能性がある。 As described above, when pulverization occurs in the negative electrode and a part thereof falls off, the dropped part affects the electrical characteristics of the negative electrode. Therefore, the battery characteristics of the wound battery may be deteriorated.
　本発明の目的は、それぞれ帯状に形成された正極、負極及びセパレータを重ね合わせた状態で巻回してなる電極体を有し、前記負極がＬｉと合金化する金属を含む巻回型電池において、前記負極の巻き終わりの端部が、充放電によって微細化して脱落することを防止することにある。 An object of the present invention is to provide a wound battery including an electrode body formed by winding a positive electrode, a negative electrode, and a separator, each formed in a strip shape, and the negative electrode contains a metal alloyed with Li. It is to prevent the end portion of the negative electrode from being wound down and falling off due to charge / discharge.
　本発明の一実施形態に係る巻回型電池は、それぞれ帯状に形成された正極、負極及びセパレータが、前記正極と前記負極との間に前記セパレータが位置するように巻回され、軸線方向に延びる柱状の電極体を備える。前記負極は、Ｌｉと合金化可能な元素を含む。前記電極体における前記負極の巻き終わり端部は、保護部材によって覆われている。 In a wound battery according to an embodiment of the present invention, a positive electrode, a negative electrode, and a separator each formed in a strip shape are wound so that the separator is positioned between the positive electrode and the negative electrode, An extending columnar electrode body is provided. The negative electrode includes an element that can be alloyed with Li. The end of winding of the negative electrode in the electrode body is covered with a protective member.
　本発明の一実施形態に係る巻回型電池によれば、電極体は、正極と負極との間にセパレータが位置するように巻回された柱状である。前記負極は、Ｌｉと合金化可能な元素を含み、前記電極体における前記負極の巻き終わり端部は、保護部材によって覆われている。これにより、電池の充放電によって負極が微粉化して一部が脱落することを防止できる。したがって、巻回型電池の電池特性の低下を防止することができる。 According to the wound battery according to an embodiment of the present invention, the electrode body has a columnar shape wound so that the separator is positioned between the positive electrode and the negative electrode. The negative electrode includes an element that can be alloyed with Li, and a winding end portion of the negative electrode in the electrode body is covered with a protective member. Thereby, it can prevent that a negative electrode pulverizes by charging / discharging of a battery and one part falls off. Accordingly, it is possible to prevent the battery characteristics of the wound battery from being deteriorated.
図１は、実施形態に係る巻回型電池の概略構成を示す斜視図である。FIG. 1 is a perspective view illustrating a schematic configuration of the wound battery according to the embodiment. 図２は、巻回型電池の構成を図１のＩＩ－ＩＩ線断面で示す断面図である。FIG. 2 is a cross-sectional view showing the configuration of the wound battery along the line II-II in FIG. 図３は、正極、負極及びセパレータの配置を模式的に示す図である。FIG. 3 is a diagram schematically showing the arrangement of the positive electrode, the negative electrode, and the separator. 図４は、正極、負極及びセパレータを厚み方向に重ねた状態で巻回する様子を模式的に示す図である。FIG. 4 is a diagram schematically illustrating a state where the positive electrode, the negative electrode, and the separator are wound in a state where they are stacked in the thickness direction. 図５は、電極体の概略構成を示す斜視図である。FIG. 5 is a perspective view showing a schematic configuration of the electrode body. 図６は、電極体の巻き終り側の端部の構成を図５のＶＩ－ＶＩ線断面で示す断面図である。6 is a cross-sectional view showing the configuration of the end portion on the winding end side of the electrode body, taken along the line VI-VI in FIG. 図７は、その他の実施形態に係る巻回型電池の概略構成を示す斜視図である。FIG. 7 is a perspective view showing a schematic configuration of a wound battery according to another embodiment.
　本発明の一実施形態に係る巻回型電池は、それぞれ帯状に形成された正極、負極及びセパレータが、前記正極と前記負極との間に前記セパレータが位置するように巻回され、軸線方向に延びる柱状の電極体を備える。前記負極は、Ｌｉと合金化可能な元素を含む。前記電極体における前記負極の巻き終わり端部は、保護部材によって覆われている（第１の構成）。 In a wound battery according to an embodiment of the present invention, a positive electrode, a negative electrode, and a separator each formed in a strip shape are wound so that the separator is positioned between the positive electrode and the negative electrode, An extending columnar electrode body is provided. The negative electrode includes an element that can be alloyed with Li. The end of winding of the negative electrode in the electrode body is covered with a protective member (first configuration).
　Ｌｉと合金化可能な元素を含む負極には、電池の充電時にＬｉとの合金が生成される。そのため、前記負極では、電池の充放電によって微粉化が生じる可能性がある。これに対し、上述の構成のように、電極体における前記負極の巻き終わり端部を保護部材によって覆うことにより、該保護部材によって覆われた部分では、Ｌｉとの合金が生成されない。よって、前記保護部材によって覆われた部分では、電池の充放電によって微粉化が生じない。ここで、電極体における負極の巻き終わり端部とは、負極の長手方向の端部で且つ電極体において負極の最外周に位置する部分を意味する。 In the negative electrode containing an element that can be alloyed with Li, an alloy with Li is generated when the battery is charged. Therefore, in the said negative electrode, micronization may arise by charging / discharging of a battery. On the other hand, as in the above-described configuration, the end of winding of the negative electrode in the electrode body is covered with a protective member, so that an alloy with Li is not generated in the portion covered with the protective member. Therefore, in the part covered with the said protection member, pulverization does not arise by charging / discharging of a battery. Here, the end of winding end of the negative electrode in the electrode body means the end of the negative electrode in the longitudinal direction and the portion located on the outermost periphery of the negative electrode in the electrode body.
　これにより、前記電極体における前記負極の巻き終わり端部において、電池の充放電によって微粉化が生じて負極の一部が脱落することを防止できる。よって、充放電に伴う負極の微粉化による電池特性の低下を防止できる。 Thereby, at the winding end of the negative electrode in the electrode body, it is possible to prevent pulverization due to charging / discharging of the battery and a part of the negative electrode from dropping off. Accordingly, it is possible to prevent the battery characteristics from being deteriorated due to the pulverization of the negative electrode accompanying charge / discharge.
　しかも、上述のように、前記電極体における前記負極の巻き終わり端部を、保護部材によって覆うことにより、前記端部によってセパレータが損傷を受けることを防止できる。 Moreover, as described above, the end of the negative electrode in the electrode body is covered with a protective member, so that the separator can be prevented from being damaged by the end.
　前記第１の構成において、前記保護部材は、前記負極の巻き終わり端部を、前記負極の短手方向の一方の端部から他方の端部に亘って覆うように設けられている（第２の構成）。 In the first configuration, the protective member is provided so as to cover the end of winding of the negative electrode from one end to the other end in the short direction of the negative electrode (second). Configuration).
　これにより、電極体における負極の巻き終わり端部において、電池の充放電によって微粉化して一部が脱落することをより確実に防止できる。しかも、上述の構成により、前記負極の巻き終わり端部によって、セパレータが損傷を受けることをより確実に防止できる。 Thereby, it is possible to more surely prevent a part of the electrode body from being pulverized due to charging / discharging and dropping off at the end of winding of the negative electrode in the electrode body. In addition, the above configuration can more reliably prevent the separator from being damaged by the winding end portion of the negative electrode.
　前記第１または第２の構成において、前記保護部材は、前記負極の巻き終わり端部と、前記負極の短手方向の端部において前記巻き終わり端部から所定範囲の部分とを覆うように設けられている（第３の構成）。 In the first or second configuration, the protective member is provided so as to cover a winding end end portion of the negative electrode and a portion within a predetermined range from the winding end end portion in the short-side end portion of the negative electrode. (Third configuration).
　これにより、電極体の負極の巻き終わり端部だけでなく、前記負極の短手方向の端部において前記巻き終わり端部から所定範囲の部分でも、電池の充放電によって微粉化して一部が脱落することを防止できる。よって、電池特性の低下をより確実に防止できる。 As a result, not only at the end of winding of the negative electrode of the electrode body, but also at the end in the short direction of the negative electrode at a portion within a predetermined range from the end of winding, part of the electrode body falls off due to charge / discharge of the battery Can be prevented. Therefore, it is possible to more reliably prevent the battery characteristics from being degraded.
　しかも、上述の構成により、負極の巻き終わり側によってセパレータが損傷を受けることを防止できる。よって、負極によるセパレータの損傷発生をより確実に防止できる。 Moreover, with the above-described configuration, the separator can be prevented from being damaged by the winding end side of the negative electrode. Therefore, it is possible to more reliably prevent the separator from being damaged by the negative electrode.
　前記第１から第３の構成のいずれか一つの構成において、前記正極は、正極活物質層を含む。前記保護部材は、前記負極の巻き終わり端部のうち、前記電極体の径方向において、前記セパレータを挟んで前記正極活物質層と重なる部分に設けられている（第４の構成）。 In any one of the first to third configurations, the positive electrode includes a positive electrode active material layer. The protective member is provided in a portion of the winding end portion of the negative electrode that overlaps the positive electrode active material layer with the separator interposed therebetween in a radial direction of the electrode body (fourth configuration).
　電極体における負極の巻き終わり端部のうち該電極体の径方向においてセパレータを挟んで正極活物質層と重なる部分では、電池の充電時にＬｉとの合金が生成される。そのため、前記部分に保護部材を設けることにより、電池の充放電によって前記部分が微粉化して一部が脱落することを効果的に防止することができる。 In the end of the negative electrode winding end portion of the electrode body, in the radial direction of the electrode body, the portion overlapping the positive electrode active material layer with the separator interposed therebetween, an alloy with Li is generated when the battery is charged. Therefore, by providing a protective member in the part, it is possible to effectively prevent the part from being pulverized due to charge / discharge of the battery and a part of the part to fall off.
　しかも、前記部分では、負極によってセパレータが損傷を受けた場合、前記負極と正極活物質層とが接触して短絡を生じる可能性がある。これに対し、上述の構成のように、前記部分に保護部材を設けることにより、前記負極によってセパレータが損傷を受けて前記負極と前記正極活物質層とが短絡することを防止できる。 In addition, in the portion, when the separator is damaged by the negative electrode, the negative electrode and the positive electrode active material layer may come into contact with each other to cause a short circuit. On the other hand, by providing a protective member in the portion as described above, it is possible to prevent the negative electrode and the positive electrode active material layer from being short-circuited due to damage to the separator by the negative electrode.
　前記第１から第４の構成のうちいずれか一つの構成において、前記保護部材は、前記負極の巻き終わり端部の両面を覆うように設けられている（第５の構成）。これにより、電池の充放電によって、電極体における負極の巻き終わり端部が微粉化して一部が脱落することをより確実に防止できる。 In any one of the first to fourth configurations, the protective member is provided so as to cover both surfaces of the winding end portion of the negative electrode (fifth configuration). Thereby, it can prevent more reliably that the winding end part of the negative electrode in an electrode body pulverizes and a part falls off by charging / discharging of a battery.
　前記第１から第５の構成のうちいずれか一つの構成において、前記保護部材は、一部が前記負極の厚み方向に延びる端面を覆うように設けられている（第６の構成）。これにより、電極体における負極の巻き終わり端部において厚み方向に延びる端面に、バリや突起等が形成されている場合に、該端面がセパレータに直接、接触して該セパレータが損傷を受けることを防止できる。 In any one of the first to fifth configurations, the protective member is provided so as to partially cover an end surface extending in the thickness direction of the negative electrode (sixth configuration). As a result, when burrs, protrusions, etc. are formed on the end surface extending in the thickness direction at the end of winding of the negative electrode in the electrode body, the end surface is in direct contact with the separator and the separator is damaged. Can be prevented.
　前記第１から第６の構成のうちいずれか一つの構成において、前記保護部材は、電気絶縁材料で且つ電池反応に寄与しない材料によって構成されている（第７の構成）。これにより、負極に設けられた保護部材によって、電池の内部で短絡が生じることを防止できるとともに、電池特性に影響を与えることを防止できる。 In any one of the first to sixth configurations, the protection member is made of an electrically insulating material that does not contribute to the battery reaction (seventh configuration). Thereby, the protective member provided on the negative electrode can prevent a short circuit from occurring inside the battery and can also prevent the battery characteristics from being affected.
　前記第１から第７の構成のうちいずれか一つの構成において、前記負極は、電池の充電後に、負極活物質として、Ｌｉ－Ａｌ合金を含む（第８の構成）。このように、電池の充電によって負極にＬｉ－Ａｌ合金が生成される構成では、電池の充放電によって前記負極が微粉化する。このように負極にＬｉ－Ａｌ合金が生成される構成の場合でも、上述の第１から第７の構成を適用することにより、電極体における負極の巻き終わり端部が微粉化して一部脱落することを効果的に抑制できる。 In any one of the first to seventh configurations, the negative electrode includes a Li—Al alloy as a negative electrode active material after charging the battery (eighth configuration). As described above, in the configuration in which the Li—Al alloy is generated on the negative electrode by charging the battery, the negative electrode is pulverized by charging and discharging of the battery. Even in the case where the Li—Al alloy is generated in the negative electrode in this way, by applying the first to seventh configurations described above, the winding end portion of the negative electrode in the electrode body is pulverized and partly falls off. This can be effectively suppressed.
　前記第８の構成において、前記負極は、Ｌｉと合金化しない金属基材層と、前記金属基材層の厚み方向の少なくとも一方に接合された金属表面層とを有する積層体である。前記金属表面層の少なくとも表面側は、電池の充電後に、前記Ｌｉ－Ａｌ合金を含む（第９の構成）。 In the eighth configuration, the negative electrode is a laminate having a metal base layer that is not alloyed with Li and a metal surface layer joined to at least one of the metal base layers in the thickness direction. At least the surface side of the metal surface layer contains the Li—Al alloy after charging the battery (ninth configuration).
　上述の構成においても、上述の第１から第７の構成を適用することにより、電池の充放電によって、電極体における負極の巻き終わり端部が微粉化して一部脱落することを抑制できる。 Also in the above-described configuration, by applying the above-described first to seventh configurations, it is possible to suppress the pulverization end portion of the negative electrode in the electrode body from being pulverized and partially falling off due to charge / discharge of the battery.
　しかも、上述の構成のように、負極が金属基材層と金属表面層とを有する構成の場合、前記負極の剛性が高い。そのため、正極、負極及びセパレータが重ねられた状態で巻回された電極体では、負極の巻き終わり端部には、前記電極体の径方向に変位する力がより生じやすい。よって、前記電極体における負極の巻き終わり端部がセパレータに損傷を与える可能性が高い。 Moreover, when the negative electrode has a metal base layer and a metal surface layer as in the above-described configuration, the negative electrode has high rigidity. Therefore, in an electrode body wound with the positive electrode, the negative electrode, and the separator being stacked, a force that is displaced in the radial direction of the electrode body is more likely to be generated at the end of winding of the negative electrode. Therefore, there is a high possibility that the winding end portion of the negative electrode in the electrode body will damage the separator.
　これに対し、上述の第１から第７の構成のような保護部材を、前記電極体における負極の巻き終わり端部に設けることにより、該巻き終わり端部がセパレータに損傷を与えることを防止できる。したがって、上述の第１から第７の構成は、上述のような構成を有する負極を用いて巻回された電極体において、セパレータの損傷防止により効果的である。 On the other hand, by providing a protective member as in the first to seventh configurations described above at the end of winding of the negative electrode in the electrode body, the end of winding can be prevented from damaging the separator. . Therefore, the first to seventh configurations described above are more effective in preventing the separator from being damaged in the electrode body wound using the negative electrode having the configuration described above.
　以下、図面を参照し、本発明の実施の形態を詳しく説明する。図中の同一または相当部分については同一の符号を付してその説明は繰り返さない。 Hereinafter, embodiments of the present invention will be described in detail with reference to the drawings. The same or corresponding parts in the drawings are denoted by the same reference numerals and description thereof will not be repeated.
　（全体構成）
　図１は、本発明の実施形態に係る巻回型電池１の概略構成を示す斜視図である。この巻回型電池１は、有底筒状の外装缶１０と、外装缶１０の開口を覆う蓋板２０と、外装缶１０内に収納される電極体３０とを備えている。外装缶１０に蓋板２０を取り付けることによって、内部に直方体状の空間を有する直方体状の電池ケース２（外装体）が構成される。なお、この電池ケース２内には、電極体３０以外に、非水電解液も封入されている。 (overall structure)
FIG. 1 is a perspective view showing a schematic configuration of a wound battery 1 according to an embodiment of the present invention. The wound battery 1 includes a bottomed cylindrical outer can 10, a cover plate 20 that covers an opening of the outer can 10, and an electrode body 30 that is accommodated in the outer can 10. By attaching the cover plate 20 to the outer can 10, a rectangular parallelepiped battery case 2 (exterior body) having a rectangular parallelepiped space is formed. In addition to the electrode body 30, a non-aqueous electrolyte is also enclosed in the battery case 2.
　外装缶１０は、アルミニウム合金製の有底筒状部材であり、蓋板２０とともに電池ケース２を構成する。外装缶１０は、図１に示すように、上面視で長方形の底面１１を有する有底筒状の部材である。詳しくは、外装缶１０は、底面１１と、扁平筒状の側壁１２とを備えている。すなわち、外装缶１０は、底面１１の短辺方向に対応する厚み方向の寸法が、底面１１の長辺方向に対応する幅方向よりも小さくなるように、扁平形状に形成されている。また、この外装缶１０は、図示しない正極リードに接続される蓋板２０と接合されているため、巻回型電池１の正極端子も兼ねている。なお、電極体３０の後述する正極３１は、図示しない正極リードによって、蓋板２０に接続されている。 The outer can 10 is a bottomed cylindrical member made of an aluminum alloy, and constitutes the battery case 2 together with the cover plate 20. As shown in FIG. 1, the outer can 10 is a bottomed cylindrical member having a rectangular bottom surface 11 in a top view. Specifically, the outer can 10 includes a bottom surface 11 and a flat cylindrical side wall 12. That is, the outer can 10 is formed in a flat shape such that the dimension in the thickness direction corresponding to the short side direction of the bottom surface 11 is smaller than the width direction corresponding to the long side direction of the bottom surface 11. Further, since the outer can 10 is joined to a lid plate 20 connected to a positive electrode lead (not shown), it also serves as a positive electrode terminal of the wound battery 1. A positive electrode 31 described later of the electrode body 30 is connected to the lid plate 20 by a positive electrode lead (not shown).
　蓋板２０は、外装缶１０の開口部を覆うように、外装缶１０の開口部に溶接によって接合されている。これにより、蓋板２０によって、電池ケース２の上面が形成される。蓋板２０は、外装缶１０と同様、アルミニウム合金製の部材からなり、該外装缶１０の開口部の内側に嵌合可能なように長方形状に形成されている。また、蓋板２０には、その長手方向の中央部分に貫通孔２０ａが形成されている（図２参照）。 The lid plate 20 is joined to the opening of the outer can 10 by welding so as to cover the opening of the outer can 10. Thereby, the upper surface of the battery case 2 is formed by the cover plate 20. Similar to the outer can 10, the lid plate 20 is made of a member made of an aluminum alloy and is formed in a rectangular shape so as to be fitted inside the opening of the outer can 10. Moreover, the through-hole 20a is formed in the center part of the longitudinal direction at the cover board 20 (refer FIG. 2).
　図２に示すように、蓋板２０の貫通孔２０ａ内には、ポリプロピレン製の絶縁パッキング２１及びステンレス鋼製の負極端子２２が挿通されている。具体的には、概略柱状の負極端子２２が挿通された概略円筒状の絶縁パッキング２１が貫通孔２０ａの周縁部に嵌合されている。負極端子２２は、円柱状の軸部の両端に平面部がそれぞれ一体形成された構成を有する。負極端子２２は、平面部が外部に露出する一方、軸部が絶縁パッキング２１内に位置付けられるように、絶縁パッキング２１に対して配置されている。この負極端子２２には、ステンレス鋼製のリード板２７が接続されている。これにより、負極端子２２は、リード板２７及び後述する負極リード３５を介して、電極体３０の負極３２に電気的に接続されている。なお、リード板２７と蓋板２０との間には、絶縁体２６が配置されている。 As shown in FIG. 2, an insulating packing 21 made of polypropylene and a negative electrode terminal 22 made of stainless steel are inserted into the through hole 20 a of the cover plate 20. Specifically, a substantially cylindrical insulating packing 21 into which a substantially columnar negative electrode terminal 22 is inserted is fitted to the peripheral edge of the through hole 20a. The negative electrode terminal 22 has a configuration in which flat portions are integrally formed at both ends of a cylindrical shaft portion. The negative electrode terminal 22 is arranged with respect to the insulating packing 21 so that the flat surface portion is exposed to the outside and the shaft portion is positioned in the insulating packing 21. A stainless steel lead plate 27 is connected to the negative terminal 22. Thereby, the negative electrode terminal 22 is electrically connected to the negative electrode 32 of the electrode body 30 via the lead plate 27 and the negative electrode lead 35 described later. An insulator 26 is disposed between the lead plate 27 and the lid plate 20.
　蓋板２０に取り付けられた負極端子２２と、電極体３０との間には、樹脂製の絶縁板３６が配置されている。絶縁板３６には、負極リード３５が貫通している。なお、図示しない正極リードは、絶縁板３６を貫通して、または、絶縁板３６の側方を通って、蓋板２０まで延びている。 Between the negative electrode terminal 22 attached to the cover plate 20 and the electrode body 30, a resin insulating plate 36 is disposed. A negative electrode lead 35 penetrates the insulating plate 36. Note that a positive electrode lead (not shown) extends to the lid plate 20 through the insulating plate 36 or through the side of the insulating plate 36.
　図２に示すように、蓋板２０には、負極端子２２と並んで非水電解液の注入口２４が形成されている。注入口２４は、平面視で略円形状に形成されている。また、注入口２４は、蓋板２０の厚み方向に径が２段階で変化するように小径部及び大径部を有する。この注入口２４は、該注入口２４の径の変化に対応して段状に形成された封止栓２５によって封止されている。そして、封止栓２５と注入口２４の周縁部との間に隙間が生じないように、該封止栓２５の大径部側の外周部と注入口２４の周縁部とはレーザー溶接によって接合されている。なお、注入口２４及び封止栓２５は、上述の構成に限らず、電池ケース２内に非水電解液を注入した後に封止可能な構成であれば、どのような構成であってもよい。 As shown in FIG. 2, a non-aqueous electrolyte inlet 24 is formed in the lid plate 20 along with the negative electrode terminal 22. The injection port 24 is formed in a substantially circular shape in plan view. The injection port 24 has a small diameter portion and a large diameter portion so that the diameter changes in two steps in the thickness direction of the lid plate 20. The injection port 24 is sealed by a sealing plug 25 formed in a step shape corresponding to a change in the diameter of the injection port 24. The outer peripheral portion on the large diameter side of the sealing plug 25 and the peripheral portion of the injection port 24 are joined by laser welding so that no gap is generated between the sealing plug 25 and the peripheral portion of the injection port 24. Has been. The inlet 24 and the sealing plug 25 are not limited to the above-described configuration, and may have any configuration as long as it can be sealed after injecting the nonaqueous electrolytic solution into the battery case 2. .
　（電極体）
　電極体３０は、それぞれ帯状に形成された正極３１及び負極３２を、両者の間及び該正極３１の下側にセパレータ３３がそれぞれ位置するように重ね合わせた状態（図３参照）で、図３における白抜き矢印の方向に、正極３１、負極３２及びセパレータ３３を巻回することによって形成された巻回電極体である。正極３１、負極３２及びセパレータ３３を巻回することによって電極体３０を構成する様子を、図４に模式的に示す。電極体３０は、正極３１、負極３２及びセパレータ３３を重ね合わせた状態で巻回した後、押しつぶして扁平状に形成される（図５参照）。すなわち、電極体３０は、軸線Ｌに沿って延びる円柱状の巻回体を押し潰して扁平状にすることにより得られる。図２に示すように、扁平状に形成された電極体３０は、電池ケース２内に収容される。 (Electrode body)
The electrode body 30 is formed in a state in which the positive electrode 31 and the negative electrode 32 formed in a strip shape are overlapped with each other so that the separators 33 are positioned between them and below the positive electrode 31 (see FIG. 3). The wound electrode body is formed by winding the positive electrode 31, the negative electrode 32, and the separator 33 in the direction of the white arrow in FIG. A state in which the electrode body 30 is configured by winding the positive electrode 31, the negative electrode 32, and the separator 33 is schematically shown in FIG. The electrode body 30 is formed in a flat shape after being wound in a state where the positive electrode 31, the negative electrode 32, and the separator 33 are overlapped (see FIG. 5). That is, the electrode body 30 is obtained by crushing a cylindrical wound body extending along the axis L to make it flat. As shown in FIG. 2, the flat electrode body 30 is accommodated in the battery case 2.
　図５に示すように、上述のように扁平状に形成された電極体３０は、正極３１、負極３２及びセパレータ３３が厚み方向に折り返されるように曲げられた一対の曲げ部３０ａを有する。一対の曲げ部３０ａは、電極体３０を側方から見て、幅方向の端部に位置する。 As shown in FIG. 5, the electrode body 30 formed flat as described above has a pair of bent portions 30a bent so that the positive electrode 31, the negative electrode 32, and the separator 33 are folded back in the thickness direction. The pair of bent portions 30a are located at the ends in the width direction when the electrode body 30 is viewed from the side.
　なお、図２に示す電極体３０は、外周側の数層分しか図示されていない。しかしながら、この図２では電極体３０の内周側部分の図示を省略しているだけであり、当然のことながら、電極体３０の内周側にも正極３１、負極３２及びセパレータ３３が存在する。 Note that the electrode body 30 shown in FIG. 2 is only shown for several layers on the outer peripheral side. However, in FIG. 2, the illustration of the inner peripheral side portion of the electrode body 30 is omitted, and naturally, the positive electrode 31, the negative electrode 32, and the separator 33 are also present on the inner peripheral side of the electrode body 30. .
　また、図３では、正極３１、負極３２及びセパレータ３３を重ね合わせた状態を図示するために、正極３１、負極３２及びセパレータ３３の位置を実際の配置から移動させて斜視で示している。また、図３では、正極３１、負極３２及びセパレータ３３を区別するために、断面ではないが、正極３１の正極集電体４１、正極活物質層４２及び負極３２にハッチングを付している。 Further, in FIG. 3, the positions of the positive electrode 31, the negative electrode 32, and the separator 33 are moved from the actual arrangement and shown in perspective in order to illustrate a state in which the positive electrode 31, the negative electrode 32, and the separator 33 are overlapped. In FIG. 3, in order to distinguish the positive electrode 31, the negative electrode 32, and the separator 33, the positive electrode current collector 41, the positive electrode active material layer 42, and the negative electrode 32 of the positive electrode 31 are hatched, although not in cross section.
　以下の説明において、電極体３０の軸線方向とは、軸線Ｌに沿った方向を意味している。また、電極体３０の径方向とは、電極体３０を構成する正極３１、負極３２及びセパレータ３３の厚み方向に沿った方向を意味する。 In the following description, the axial direction of the electrode body 30 means a direction along the axis L. The radial direction of the electrode body 30 means a direction along the thickness direction of the positive electrode 31, the negative electrode 32, and the separator 33 constituting the electrode body 30.
　正極３１は、図６に示すように、正極活物質を含有する正極活物質層４２を、アルミニウム等の金属箔製の正極集電体４１の片面または両面に設けたものである（図６に示す例では、正極活物質層４２が正極集電体４１の両面に設けられている）。詳しくは、正極３１は、リチウムイオンを吸蔵・放出可能なリチウム含有酸化物である正極活物質、導電助剤及びバインダなどを含む正極合剤を、アルミニウム箔などからなる正極集電体４１上に塗布して乾燥させることによって形成される。なお、本実施形態では、図３に示すように、正極活物質層４２は、正極集電体４１に対し、長手方向の一方の端部以外に形成されている。 As shown in FIG. 6, the positive electrode 31 has a positive electrode active material layer 42 containing a positive electrode active material provided on one or both sides of a positive electrode current collector 41 made of a metal foil such as aluminum (see FIG. 6). In the example shown, the positive electrode active material layer 42 is provided on both surfaces of the positive electrode current collector 41). Specifically, the positive electrode 31 has a positive electrode active material that is a lithium-containing oxide capable of occluding and releasing lithium ions, a positive electrode mixture containing a conductive additive and a binder on a positive electrode current collector 41 made of aluminum foil or the like. It is formed by applying and drying. In the present embodiment, as shown in FIG. 3, the positive electrode active material layer 42 is formed on the positive electrode current collector 41 other than one end in the longitudinal direction.
　正極活物質であるリチウム含有酸化物としては、例えば、Ｌｉ１＋ｘＭ１Ｏ２（－０．１＜ｘ＜０．１、Ｍ１：Ｃｏ、Ｎｉ、Ｍｎ、Ａｌ、Ｍｇ、Ｔｉ、Ｚｒなどより選択される１種以上の元素）で表される層状構造のリチウム含有複合酸化物、ＬｉＭｎ２Ｏ４やその元素の一部を他元素で置換したスピネル構造のリチウムマンガン複合酸化物、Ｌｉ４／３Ｔｉ５／３Ｏ４やその元素の一部を他元素で置換したスピネル構造のリチウムチタン複合酸化物、ＬｉＭｎ３Ｏ６などの組成で表される、低温で合成されるリチウムマンガン複合酸化物、ＬｉＭ２ＰＯ４（Ｍ２：Ｃｏ、Ｎｉ、Ｍｎ、Ｆｅなどより選択される１種以上の元素）で表されるオリビン型化合物などが挙げられる。前記層状構造のリチウム含有複合酸化物としては、ＬｉＣｏＯ２などのコバルト酸リチウムや、ＬｉＮｉ１－ａＣｏａ－ｂＡｌｂＯ２（０．１≦ａ≦０．３、０．０１≦ｂ≦０．２）、少なくともＣｏ、ＮｉおよびＭｎを含む酸化物（ＬｉＭｎ１／３Ｎｉ１／３Ｃｏ１／３Ｏ２、ＬｉＭｎ５／１２Ｎｉ５／１２Ｃｏ１／６Ｏ２、ＬｉＮｉ３／５Ｍｎ１／５Ｃｏ１／５Ｏ２など）などのリチウム含有ニッケル複合酸化物、などを例示することができる。なお、正極活物質として、１種類の物質のみを用いてもよいし、２種類以上の物質を用いてもよい。また、正極活物質は、上述の物質に限られない。 Examples of the lithium-containing oxide that is a positive electrode active material include Li 1 + x M 1 O 2 (−0.1 <x <0.1, M 1 : Co, Ni, Mn, Al, Mg, Ti, Zr, and the like. Lithium-containing composite oxide having a layered structure represented by one or more selected elements), LiMn 2 O 4 or a lithium manganese composite oxide having a spinel structure in which a part of the element is substituted with another element, Li 4 / 3 Ti 5/3 O 4 and a lithium manganese composite oxide synthesized at a low temperature represented by a composition such as a lithium titanium composite oxide having a spinel structure in which part of the element is substituted with another element, LiMn 3 O 6 And an olivine type compound represented by LiM 2 PO 4 (M 2 : one or more elements selected from Co, Ni, Mn, Fe, etc.). Examples of the lithium-containing composite oxide having a layered structure include lithium cobalt oxide such as LiCoO 2 and LiNi 1-a Co ab Al b O 2 (0.1 ≦ a ≦ 0.3, 0.01 ≦ b ≦ 0.2), an oxide containing at least Co, Ni and Mn (LiMn 1/3 Ni 1/3 Co 1/3 O 2 , LiMn 5/12 Ni 5/12 Co 1/6 O 2 , LiNi 3/5 Examples thereof include lithium-containing nickel composite oxides such as Mn 1/5 Co 1/5 O 2 . Note that only one type of material may be used as the positive electrode active material, or two or more types of materials may be used. Further, the positive electrode active material is not limited to the above-described materials.
　二次電池の正極活物質が不可逆容量の大きな材料である場合には、負極集電体とＡｌ層との積層体を負極前駆体として用いて電池を組み立てて、組み立てた電池を充電して負極のＬｉ－Ａｌ合金を生成するようにすれば、正極の不可逆容量の一部または全部を負極で相殺することができるので好ましい。 When the positive electrode active material of the secondary battery is a material with a large irreversible capacity, the battery is assembled using a laminate of the negative electrode current collector and the Al layer as the negative electrode precursor, and the assembled battery is charged to form the negative electrode It is preferable to produce this Li—Al alloy because part or all of the irreversible capacity of the positive electrode can be offset by the negative electrode.
　正極合剤に係るバインダには、ポリフッ化ビニリデン（ＰＶＤＦ）、ポリテトラフルオロチレン（ＰＴＦＥ）、スチレンブタジエンゴム（ＳＢＲ）、カルボキシメチルセルロース（ＣＭＣ）などや、イミド系バインダ（ポリアミドイミド、ポリイミドなど）、アミド系バインダ（ポリアミド、アラミドなど）などを用いることができる。 Examples of binders for the positive electrode mixture include polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), styrene butadiene rubber (SBR), carboxymethyl cellulose (CMC), and imide binders (polyamideimide, polyimide, etc.), An amide binder (polyamide, aramid, etc.) can be used.
　また、正極合剤に係る導電助剤には、天然黒鉛（鱗片状黒鉛など）、人造黒鉛などの黒鉛（黒鉛質炭素材料）；アセチレンブラック、ケッチェンブラック、チャンネルブラック、ファーネスブラック、ランプブラック、サーマルブラックなどのカ－ボンブラック；炭素繊維；などの炭素材料などを用いることができる。 In addition, conductive assistants related to the positive electrode mixture include graphite (graphite carbon material) such as natural graphite (flaky graphite), artificial graphite; acetylene black, ketjen black, channel black, furnace black, lamp black, Carbon materials such as carbon black such as thermal black; carbon fiber; and the like can be used.
　また、正極活物質層４２と正極集電体４１とを有する正極３１は、例えば、正極活物質、導電助剤およびバインダなどを水またはＮ－メチル－２－ピロリドン（ＮＭＰ）などの有機溶媒に分散させて正極合剤含有組成物（スラリー、ペーストなど）を調製し（バインダは溶媒に溶解していてもよい）、これを正極集電体４１上に塗布して乾燥させ、必要に応じてカレンダ処理などのプレス処理を施す工程を経ることにより、製造することができる。 The positive electrode 31 having the positive electrode active material layer 42 and the positive electrode current collector 41 includes, for example, a positive electrode active material, a conductive additive, a binder, and the like in water or an organic solvent such as N-methyl-2-pyrrolidone (NMP). Disperse to prepare a positive electrode mixture-containing composition (slurry, paste, etc.) (the binder may be dissolved in a solvent), which is applied onto the positive electrode current collector 41 and dried, and if necessary It can manufacture by passing through the process of performing press processes, such as a calendar process.
　正極合剤における正極活物質の含有量は、８０～９８．８質量％であることが好ましい。また、正極合剤における導電助剤の含有量は、１．５～１０質量％であることが好ましい。更に、正極合剤におけるバインダの含有量は、０．３～１０質量％であることが好ましい。正極活物質層４２の厚み（集電体の片面あたりの厚み）は、３０～３００μｍであることが好ましい。 The content of the positive electrode active material in the positive electrode mixture is preferably 80 to 98.8% by mass. The content of the conductive auxiliary in the positive electrode mixture is preferably 1.5 to 10% by mass. Further, the binder content in the positive electrode mixture is preferably 0.3 to 10% by mass. The thickness of the positive electrode active material layer 42 (thickness per one side of the current collector) is preferably 30 to 300 μm.
　正極集電体４１としては、Ａｌ及びＡｌ合金などの金属の箔、パンチングメタル、網、エキスパンドメタルなどを用い得るが、通常、Ａｌ箔が好適に用いられる。正極集電体４１の厚みは、１０～３０μｍであることが好ましい。 As the positive electrode current collector 41, a metal foil such as Al and Al alloy, a punching metal, a net, an expanded metal, or the like can be used, but an Al foil is usually preferably used. The thickness of the positive electrode current collector 41 is preferably 10 to 30 μm.
　特に図示しないが、正極３１には、正極集電体４１のうち正極合剤が塗布されていない部分、すなわち、正極集電体４１が露出した部分に、正極リードが接続されている。 Although not particularly illustrated, the positive electrode lead is connected to a portion of the positive electrode current collector 41 where the positive electrode mixture is not applied, that is, a portion where the positive electrode current collector 41 is exposed.
　負極３２は、図６に示すように、銅合金を含む金属基材層４５と、金属基材層４５の両面上にそれぞれ位置し且つアルミニウム合金を含む金属表面層４６とを有する。負極３２は、例えば、銅合金を含む層と、その層の両面上にそれぞれ位置するアルミニウム合金を含む層とからなるクラッド材によって構成される。負極３２は、平面視で、正極３１の正極活物質層４２よりも長手方向及び短手方向の寸法がそれぞれ大きい。 As shown in FIG. 6, the negative electrode 32 has a metal base layer 45 containing a copper alloy, and a metal surface layer 46 located on both surfaces of the metal base layer 45 and containing an aluminum alloy. The negative electrode 32 is made of, for example, a clad material composed of a layer containing a copper alloy and a layer containing an aluminum alloy positioned on both surfaces of the layer. The negative electrode 32 has a longer dimension and a shorter dimension in the plan view than the positive electrode active material layer 42 of the positive electrode 31.
　負極３２は、巻回型電池１の充電後に、金属表面層４６のうちセパレータ３３を挟んで正極３１の正極活物質層４２と厚み方向に重なる部分の少なくとも表面側に、Ｌｉ－Ａｌ合金を含む。すなわち、金属基材層４５及び金属表面層４６を有する負極３２を前駆体として、上述の正極３１とともに組み立てられた巻回型電池１を充電することにより、金属表面層４６のうちセパレータ３３を挟んで正極３１の正極活物質層４２と厚み方向に重なる部分を、非水電解液中のＬｉイオンと電気化学的に反応させる。これにより、負極３２の金属表面層４６のうち、セパレータ３３を挟んで正極３１の正極活物質層４２と厚み方向に重なる部分の少なくとも表面側に、Ｌｉ－Ａｌ合金が生成される。 The negative electrode 32 contains a Li—Al alloy on at least the surface side of the portion of the metal surface layer 46 that overlaps the positive electrode active material layer 42 of the positive electrode 31 in the thickness direction with the separator 33 interposed therebetween after charging of the wound battery 1. . That is, the negative electrode 32 having the metal base layer 45 and the metal surface layer 46 is used as a precursor to charge the wound battery 1 assembled together with the positive electrode 31 described above, thereby sandwiching the separator 33 in the metal surface layer 46. The portion of the positive electrode 31 that overlaps the positive electrode active material layer 42 in the thickness direction is electrochemically reacted with Li ions in the non-aqueous electrolyte. As a result, a Li—Al alloy is formed on at least the surface side of the metal surface layer 46 of the negative electrode 32 that overlaps the positive electrode active material layer 42 of the positive electrode 31 in the thickness direction with the separator 33 interposed therebetween.
　金属基材層４５は、ニッケルなどによって構成されていてもよい。金属基材層４５は、金属表面層４６と圧着などによって積層されていてもよい。金属表面層４６は、金属基材層４５の片面のみに設けられていてもよい。また、金属表面層４６の代わりに、Ｌｉと合金化可能な元素（例えばＳｉやＳｎなど）を含む金属層を、金属基材層４５の片面または両面に設けてもよい。 The metal base layer 45 may be made of nickel or the like. The metal substrate layer 45 may be laminated with the metal surface layer 46 by pressure bonding or the like. The metal surface layer 46 may be provided only on one side of the metal base layer 45. Further, instead of the metal surface layer 46, a metal layer containing an element that can be alloyed with Li (for example, Si or Sn) may be provided on one side or both sides of the metal base layer 45.
　金属表面層４６は、金属基材層４５の一方の面上に設けられる層の厚みが、５μｍ以上であることが好ましく、１０μｍ以上であることがより好ましく、１５μｍ以上であることが更に好ましい。また、金属表面層４６は、金属基材層４５の一方の面上に設けられる層の厚みが、１５０μｍ以下であることが好ましく、７０μｍ以下であることがより好ましく、５０μｍ以下であることが更に好ましい。 The thickness of the metal surface layer 46 provided on one surface of the metal base layer 45 is preferably 5 μm or more, more preferably 10 μm or more, and further preferably 15 μm or more. The metal surface layer 46 has a thickness of 150 μm or less, more preferably 70 μm or less, and more preferably 50 μm or less, on the one surface of the metal base layer 45. preferable.
　負極３２には、負極３２の長手方向の端部で且つ電極体３０において負極３２の最外周に位置する部分、すなわち、巻き終わりの端部に、電気絶縁性を有し且つ電池反応に寄与しない樹脂製の保護部材５５が設けられている。保護部材５５は、詳しくは後述するが、負極３２の巻き終わりの端部に設けられることにより、電池の充放電時に負極３２で微粉化が生じて一部が脱落することを防止する。本実施形態では、保護部材５５は、負極３２の長手方向における巻き終わり側の端部及び該端部から長手方向に所定範囲の部分に設けられている。保護部材５５の詳しい構成については、後述する。 The negative electrode 32 has an electrical insulating property at the end of the negative electrode 32 in the longitudinal direction and at the outermost periphery of the negative electrode 32 in the electrode body 30, that is, at the end of the winding end, and does not contribute to the battery reaction. A resin protection member 55 is provided. As will be described in detail later, the protective member 55 is provided at the end of the negative electrode 32 at the end of winding, thereby preventing the negative electrode 32 from being pulverized and partially falling off during charging and discharging of the battery. In the present embodiment, the protective member 55 is provided at an end portion on the winding end side in the longitudinal direction of the negative electrode 32 and a portion within a predetermined range from the end portion in the longitudinal direction. A detailed configuration of the protection member 55 will be described later.
　セパレータ３３は、８０℃以上（より好ましくは１００℃以上）１７０℃以下（より好ましくは１５０℃以下）において、その孔が閉塞する性質（すなわちシャットダウン機能）を有することが好ましい。また、セパレータ３３は、通常の非水電解質二次電池などで使用されているセパレータ、例えば、ポリエチレン（ＰＥ）やポリプロピレン（ＰＰ）などのポリオレフィン製の微多孔膜を用いることができる。セパレータ３３を構成する微多孔膜は、例えば、ＰＥのみを使用したものやＰＰのみを使用したものであってもよく、また、ＰＥ製の微多孔膜とＰＰ製の微多孔膜との積層体であってもよい。セパレータ３３の厚みは、例えば、１０～３０μｍであることが好ましい。 The separator 33 preferably has a property (that is, a shutdown function) that closes the pores at 80 ° C. or higher (more preferably 100 ° C. or higher) and 170 ° C. or lower (more preferably 150 ° C. or lower). Moreover, the separator 33 can use the separator used for the normal nonaqueous electrolyte secondary battery etc., for example, the microporous film made from polyolefin, such as polyethylene (PE) and polypropylene (PP). The microporous membrane constituting the separator 33 may be, for example, one using only PE or one using only PP, or a laminate of a PE microporous membrane and a PP microporous membrane. It may be. The thickness of the separator 33 is preferably 10 to 30 μm, for example.
　また、耐熱性を高めるために、上述のようなポリオレフィン製の微多孔膜の表面に、無機フィラーなどを含有する耐熱性の多孔質層を設けた積層型のセパレータや、テトラフルオロエチレン－パーフルオロアルコキシエチレン共重合体（ＰＦＡ）などのフッ素樹脂、ポリフェニレンサルファイド（ＰＰＳ）、ポリエーテルエーテルケトン（ＰＥＥＫ）、ポリブチレンテレフタレート（ＰＢＴ）、ポリメチルペンテン、セルロース、アラミド、ポリイミド、ポリアミドイミドなどの耐熱樹脂製の不織布セパレータなどを使用することもできる。 In addition, in order to improve heat resistance, a laminated separator in which a heat-resistant porous layer containing an inorganic filler or the like is provided on the surface of a polyolefin microporous film as described above, or tetrafluoroethylene-perfluoro Fluorine resins such as alkoxyethylene copolymers (PFA), polyphenylene sulfide (PPS), polyether ether ketone (PEEK), polybutylene terephthalate (PBT), polymethylpentene, cellulose, aramid, polyimide, polyamideimide, and other heat resistant resins A non-woven fabric separator or the like can also be used.
　次に、本実施形態に係る巻回型電池１で用いられる非水電解液中の非水電解質について説明する。 Next, the non-aqueous electrolyte in the non-aqueous electrolyte used in the wound battery 1 according to this embodiment will be described.
　非水電解質の溶媒には、例えば、エチレンカーボネート（ＥＣ）、プロピレンカーボネート（ＰＣ）、ブチレンカーボネート（ＢＣ）、ジメチルカーボネート（ＤＭＣ）、ジエチルカーボネート（ＤＥＣ）、メチルエチルカーボネート（ＭＥＣ）、ラクトン環を有する化合物、１，２－ジメトキシエタン（ＤＭＥ）、テトラヒドロフラン（ＴＨＦ）、ジメチルスルフォキシド（ＤＭＳＯ）、１，３－ジオキソラン、ホルムアミド、ジメチルホルムアミド（ＤＭＦ）、ニトロメタン、蟻酸メチル、酢酸メチル、酢酸エチル、燐酸トリエステル（燐酸トリメチル、燐酸トリエチルなど）、トリメトキシメタン、スルホラン、３－メチル－２－オキサゾリジノン、ジエチルエーテルなどの非プロトン性有機溶媒もしくはその誘導体（２－メチルテトラヒドロフランなど）などを１種単独で、または２種以上を混合した混合溶媒として用いることができる。 Nonaqueous electrolyte solvents include, for example, ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC), dimethyl carbonate (DMC), diethyl carbonate (DEC), methyl ethyl carbonate (MEC), and lactone rings. Compounds having 1,2-dimethoxyethane (DME), tetrahydrofuran (THF), dimethyl sulfoxide (DMSO), 1,3-dioxolane, formamide, dimethylformamide (DMF), nitromethane, methyl formate, methyl acetate, ethyl acetate An aprotic organic solvent such as phosphoric acid triester (trimethyl phosphate, triethyl phosphate, etc.), trimethoxymethane, sulfolane, 3-methyl-2-oxazolidinone, diethyl ether, etc. Rahidorofuran etc.) and the like can be used as alone in a mixed solvent or a mixture of two or more.
　非水電解質に係るリチウム塩としては、例えば、ＬｉＣｌＯ４、ＬｉＰＦ６、ＬｉＢＦ４、ＬｉＡｓＦ６、ＬｉＳｂＦ６、ＬｉＣＦ３ＳＯ３、ＬｉＣＦ３ＣＯ２、Ｌｉ２Ｃ２Ｆ４（ＳＯ３）２、ＬｉＮ（ＦＳＯ２）２、ＬｉＮ（ＣＦ３ＳＯ２）２、ＬｉＣ（ＣＦ３ＳＯ２）３、ＬｉＣｎＦ２ｎ＋１ＳＯ３（ｎ≧２）、ＬｉＮ（ＲｆＯＳＯ２）２〔ここでＲｆはフルオロアルキル基〕などから選ばれる少なくとも１種が挙げられる。これらのリチウム塩の非水電解質の濃度は、０．６～１．８ｍｏｌ／ｌであることが好ましく、０．９～１．６ｍｏｌ／ｌであることがより好ましい。２種以上のリチウム塩を併用することも可能であり、その場合は、それぞれのリチウム塩の濃度の合計が前記範囲となるよう調整すればよい。 The lithium salt according to the non-aqueous electrolyte, for example, LiClO 4, LiPF 6, LiBF4 , LiAsF 6, LiSbF 6, LiCF 3 SO 3, LiCF 3 CO 2, Li 2 C 2 F 4 (SO 3) 2, LiN ( FSO 2 ) 2 , LiN (CF 3 SO 2 ) 2 , LiC (CF 3 SO 2 ) 3 , LiC n F 2n + 1 SO 3 (n ≧ 2), LiN (RfOSO 2 ) 2 [where Rf is a fluoroalkyl group] And at least one selected from the above. The concentration of the non-aqueous electrolyte of these lithium salts is preferably 0.6 to 1.8 mol / l, more preferably 0.9 to 1.6 mol / l. Two or more lithium salts may be used in combination, and in that case, the total concentration of the lithium salts may be adjusted to fall within the above range.
　また、これらの非水電解質に、電池の各種特性を更に向上させる目的で、ビニレンカーボネート類、１，３－プロパンスルトン、１，３－プロペンスルトンなどの環状スルトン化合物、ジフェニルジスルフィドなどのジスルフィド化合物、シクロヘキシルベンゼン、ビフェニル、フルオロベンゼン、ｔ－ブチルベンゼンなどのベンゼン類化合物、４－フルオロ－１，３－ジオキソラン－２－オン（ＦＥＣ）などのフッ素置換された環状カーボネート、リチウムテトラキス（アセテート）ボレートやリチウムビス（オキサレート）ボレート（ＬｉＢＯＢ）などの有機ホウ酸リチウム塩、などの添加剤を適宜加えることもできる。 In addition, to these non-aqueous electrolytes, for the purpose of further improving various characteristics of the battery, vinylene carbonates, cyclic sultone compounds such as 1,3-propane sultone and 1,3-propene sultone, disulfide compounds such as diphenyl disulfide, Benzene compounds such as cyclohexylbenzene, biphenyl, fluorobenzene, t-butylbenzene, fluorine-substituted cyclic carbonates such as 4-fluoro-1,3-dioxolan-2-one (FEC), lithium tetrakis (acetate) borate, Additives such as lithium organic borate such as lithium bis (oxalate) borate (LiBOB) can be added as appropriate.
　更に、非水電解質には、前記の溶液（非水電解液）に、公知のポリマーなどのゲル化剤を用いてゲル状（ゲル状電解質）としたものを用いてもよい。 Furthermore, as the non-aqueous electrolyte, the above-mentioned solution (non-aqueous electrolyte) may be used in the form of a gel (gel electrolyte) using a known polymer or other gelling agent.
　（保護部材）
　既述のように、巻回型電池１を充電することにより、負極３２の金属表面層４６のうちセパレータ３３を挟んで正極活物質層４２と対向する部分の少なくとも表面側には、Ｌｉ－Ａｌ合金が生成される。一方、充電した巻回型電池１を放電する際には、負極３２の金属表面層４６に生成されたＬｉ－Ａｌ合金からＬｉが放出される。このように、巻回型電池１の充放電を繰り返すことにより、負極３２では、Ｌｉ－Ａｌ合金の生成及びＬｉの放出が繰り返される。これにより、負極３２の金属表面層４６のうち、Ｌｉ－Ａｌ合金が生成された部分は微粉化する。このように微粉化した部分では、負極の一部が脱落する可能性がある。 (Protective member)
As described above, when the wound battery 1 is charged, at least the surface side of the portion of the metal surface layer 46 of the negative electrode 32 facing the positive electrode active material layer 42 with the separator 33 interposed therebetween is Li—Al. An alloy is produced. On the other hand, when the charged wound battery 1 is discharged, Li is released from the Li—Al alloy generated on the metal surface layer 46 of the negative electrode 32. In this way, by repeating charging and discharging of the wound battery 1, in the negative electrode 32, generation of Li—Al alloy and release of Li are repeated. As a result, the portion of the metal surface layer 46 of the negative electrode 32 where the Li—Al alloy is generated is pulverized. In such a pulverized portion, a part of the negative electrode may fall off.
　これに対し、本実施形態では、図５に示すように、負極３２において、電極体３０の巻き終わり端部（負極３２の長手方向の端部で且つ電極体３０において負極３２の最外周に位置する部分）に、保護部材５５が設けられている。保護部材５５は、負極３２の長手方向において、電極体３０における巻き終わり端部に、負極３２の短手方向の一方の端部から他方の端部に亘って設けられた第１保護部５５ａを有する。また、保護部材５５は、負極３２の短手方向の両端部に、負極３２の長手方向において、前記巻き終わり側の端部から所定範囲に設けられた第２保護部５５ｂを有する。すなわち、保護部材５５は、厚み方向から見て、負極３２の巻き終わり側にコの字状に設けられている。 On the other hand, in this embodiment, as shown in FIG. 5, in the negative electrode 32, the winding end end portion of the electrode body 30 (the end portion in the longitudinal direction of the negative electrode 32 and the outermost periphery of the negative electrode 32 in the electrode body 30). The protective member 55 is provided on the portion to be protected. In the longitudinal direction of the negative electrode 32, the protective member 55 is provided with a first protective portion 55 a provided from one end portion in the short direction of the negative electrode 32 to the other end portion at the winding end end portion of the electrode body 30. Have. Further, the protection member 55 has second protection portions 55 b provided in a predetermined range from the end portion on the winding end side in the longitudinal direction of the negative electrode 32 at both ends in the short direction of the negative electrode 32. That is, the protection member 55 is provided in a U shape on the winding end side of the negative electrode 32 when viewed from the thickness direction.
　なお、保護部材５５は、負極３２の長手方向において、負極３２の巻き終わり側の端部に設けられた第１保護部５５ａのみを有していてもよいし、第２保護部５５ｂが負極３２の短手方向の一方の端部のみに設けられていてもよい。 The protection member 55 may have only the first protection part 55 a provided at the end of the negative electrode 32 on the winding end side in the longitudinal direction of the negative electrode 32, or the second protection part 55 b may be the negative electrode 32. It may be provided only at one end in the short direction.
　前記所定範囲は、巻回型電池１の充電によって負極３２に微粉化が生じる範囲である。負極３２に微粉化が生じる範囲は、負極３２の金属表面層４６にＬｉ－Ａｌ合金が生成される範囲である。Ｌｉ－Ａｌ合金が生成される範囲は、負極３２を厚み方向に見て、負極３２が正極活物質層４２と重なる範囲と、Ｌｉ－Ａｌ合金が生成される際に、電池の充放電の繰り返しによってＬｉ－Ａｌ合金化が進行する範囲とを含む。前記所定範囲は、負極３２の長手方向の一方の端部から他方の端部までであってもよい。 The predetermined range is a range in which pulverization occurs in the negative electrode 32 by charging the wound battery 1. The range in which pulverization occurs in the negative electrode 32 is a range in which a Li—Al alloy is generated in the metal surface layer 46 of the negative electrode 32. The range in which the Li—Al alloy is generated includes the range in which the negative electrode 32 overlaps the positive electrode active material layer 42 when the negative electrode 32 is viewed in the thickness direction, and the repeated charging and discharging of the battery when the Li—Al alloy is generated. And the range in which Li—Al alloying proceeds. The predetermined range may be from one end in the longitudinal direction of the negative electrode 32 to the other end.
　また、保護部材５５の第１保護部５５ａは、電極体３０における負極３２の巻き終わり端部に、負極３２の短手方向の一部のみに設けられていてもよい。 Further, the first protection part 55 a of the protection member 55 may be provided only at a part of the negative electrode 32 in the short direction at the winding end end of the negative electrode 32 in the electrode body 30.
　保護部材５５は、負極３２の巻き終わり側の端部のうち、電極体３０において、厚み方向に正極活物質層４２と重なる部分に設けられていることが好ましい。これにより、負極３２の巻き終わり側の端部のうち、巻回型電池１の充放電によって、負極３２で微粉化が生じる部分、すなわち金属表面層４６にＬｉ－Ａｌ合金が形成される部分に、保護部材５５を設けることができる。よって、負極３２の巻き終わり側の端部において、負極３２で微粉化が生じることをより確実に防止できる。 The protective member 55 is preferably provided in a portion of the end portion on the winding end side of the negative electrode 32 that overlaps the positive electrode active material layer 42 in the thickness direction in the electrode body 30. As a result, in the end portion on the winding end side of the negative electrode 32, the portion where pulverization occurs in the negative electrode 32 due to charging / discharging of the wound battery 1, that is, the portion where the Li—Al alloy is formed on the metal surface layer 46. A protective member 55 can be provided. Accordingly, it is possible to more reliably prevent the pulverization of the negative electrode 32 at the end of the negative electrode 32 on the winding end side.
　本実施形態では、保護部材５５は、負極３２の巻き終わり側の端部の両面に、該端部の端面を跨ぐように設けられている。すなわち、保護部材５５は、負極３２の長手方向に直交する方向の断面で見て、コの字状に設けられている（図６参照）。このように、負極３２の厚み方向に延びる端面にも保護部材５５を設けることにより、該端面にバリや突起等が形成されている場合に該バリや突起等によってセパレータ３３が損傷を受けることを防止できる。 In this embodiment, the protective member 55 is provided on both surfaces of the end portion of the negative electrode 32 on the winding end side so as to straddle the end surface of the end portion. That is, the protection member 55 is provided in a U-shape when viewed in a cross section perpendicular to the longitudinal direction of the negative electrode 32 (see FIG. 6). In this way, by providing the protective member 55 on the end surface extending in the thickness direction of the negative electrode 32, when the burr or the projection is formed on the end surface, the separator 33 is damaged by the burr or the projection. Can be prevented.
　なお、保護部材５５は、負極３２の巻き終わり側の両面のみに設けられていてもよい。すなわち、保護部材５５は、負極３２の巻き終わり側の端部の端面に設けられていなくてもよい。 The protective member 55 may be provided only on both surfaces of the negative electrode 32 on the winding end side. That is, the protection member 55 may not be provided on the end surface of the end portion on the winding end side of the negative electrode 32.
　保護部材５５は、後述するようにテープや樹脂によって成形されていて、負極３２とは別の部材である。これにより、保護部材５５の厚みを容易に調整することができる。 The protective member 55 is formed of tape or resin as will be described later, and is a member different from the negative electrode 32. Thereby, the thickness of the protection member 55 can be adjusted easily.
　保護部材５５は、樹脂製のテープ（ポリエチレンテレフタラート（ＰＥＴ）テープ、ポリプロピレン（ＰＰ）テープ、ポリフェニレンサルファイド樹脂（ＰＰＳ）テープ、ポリイミドテープ等）、または、各種樹脂や紫外線によって硬化する紫外線硬化樹脂によって成形された部材、各種樹脂によって構成された粘着剤など、電気絶縁材料で且つ電池反応に寄与しない材料によって構成されている。 The protective member 55 is made of resin tape (polyethylene terephthalate (PET) tape, polypropylene (PP) tape, polyphenylene sulfide resin (PPS) tape, polyimide tape, etc.), or various resins or ultraviolet curable resins that are cured by ultraviolet rays. It is made of an electrically insulating material that does not contribute to the battery reaction, such as a molded member or an adhesive made of various resins.
　これにより、負極の巻き終わり端部によってセパレータ３３が損傷を受けた場合でも、電極体３０内で短絡が生じることを防止できるとともに、保護部材５５が巻回型電池１の電池特性に影響を与えることを防止できる。 Thereby, even when the separator 33 is damaged by the winding end portion of the negative electrode, it is possible to prevent a short circuit from occurring in the electrode body 30 and the protective member 55 affects the battery characteristics of the wound battery 1. Can be prevented.
　本実施形態に係る巻回型電池１では、電池の充電によって、負極３２の金属表面層４６の表面側で、且つ、負極３２の厚み方向から見て少なくとも正極活物質層４２と重なる部分に、Ｌｉ－Ａｌ合金を含む層を形成することができる。これにより、耐熱性の高い巻回型電池１が得られる。 In the wound battery 1 according to the present embodiment, by charging the battery, on the surface side of the metal surface layer 46 of the negative electrode 32 and at least a portion overlapping the positive electrode active material layer 42 when viewed from the thickness direction of the negative electrode 32, A layer containing a Li—Al alloy can be formed. Thereby, the winding type battery 1 with high heat resistance is obtained.
　しかも、電極体３０における負極３２の巻き終わり端部は、保護部材５５によって覆われている。これにより、巻回型電池１の充放電によって、負極３２の巻き終わり端部に微粉化が生じることを防止できる。したがって、負極３２の巻き終わり端部において、微粉化によって負極３２の一部が脱落することを防止できる。よって、巻回型電池１の電池特性の低下を防止することができる。 Moreover, the end of winding of the negative electrode 32 in the electrode body 30 is covered with a protective member 55. Thereby, it can prevent that pulverization arises in the winding end part of the negative electrode 32 by charging / discharging of the winding type battery 1. FIG. Therefore, it is possible to prevent a part of the negative electrode 32 from falling off due to pulverization at the winding end end of the negative electrode 32. Therefore, it is possible to prevent the battery characteristics of the wound battery 1 from being deteriorated.
　しかも、保護部材５５を、負極３２の巻き終わり端部に、負極３２の短手方向の一方の端部から他方の端部に亘って覆うように設けることにより、前記巻き終わり端部で負極３２の微粉化及び一部脱落が生じることをより確実に防止できる。 In addition, the protective member 55 is provided at the winding end of the negative electrode 32 so as to cover from one end of the negative electrode 32 in the short direction to the other end, so that the negative electrode 32 is provided at the winding end. Can be more reliably prevented from being pulverized and partly falling off.
　また、保護部材５５を、負極３２の巻き終わり端部と、負極３２の短手方向の端部において前記巻き終わり端部から所定範囲の部分とを覆うように設けることにより、負極３２の巻き終わり側に位置する部分で微粉化及び一部脱落が生じることをより確実に防止できる。 Further, by providing the protective member 55 so as to cover the end of winding of the negative electrode 32 and the end of the negative electrode 32 in a short direction, the end of winding of the negative electrode 32 is covered. It can prevent more reliably that pulverization and partial drop-off occur at the portion located on the side.
　特に、保護部材５５を、負極３２の巻き終わり端部のうち、電極体３０の径方向において、セパレータ３３を挟んで正極活物質層４２と重なる部分に設けることにより、前記巻き終わり端部において、巻回型電池１の充放電によって微粉化が生じることをより確実に防止できる。 In particular, the protective member 55 is provided in a portion of the winding end end of the negative electrode 32 that overlaps the positive electrode active material layer 42 across the separator 33 in the radial direction of the electrode body 30. It can prevent more reliably that pulverization arises by charging / discharging of the winding type battery 1. FIG.
　（その他の実施形態）
　以上、本発明の実施の形態を説明したが、上述した実施の形態は本発明を実施するための例示に過ぎない。よって、上述した実施の形態に限定されることなく、その趣旨を逸脱しない範囲内で上述した実施の形態を適宜変形して実施することが可能である。 (Other embodiments)
While the embodiments of the present invention have been described above, the above-described embodiments are merely examples for carrying out the present invention. Therefore, the present invention is not limited to the above-described embodiment, and the above-described embodiment can be appropriately modified and implemented without departing from the spirit of the invention.
　前記実施形態では、電極体３０は、直方体状の電池ケース２内に収容されている。しかしながら、電極体３０は、他の構成を有する外装体内に収容されていてもよい。例えば、ラミネートフィルム外装体内に電極体３０が収容されていてもよいし、他の缶構造を有する電池ケース内に収容されていてもよい。 In the embodiment, the electrode body 30 is accommodated in the rectangular battery case 2. However, the electrode body 30 may be accommodated in an exterior body having another configuration. For example, the electrode body 30 may be accommodated in the laminate film exterior body, or may be accommodated in a battery case having another can structure.
　電極体３０が収容される他の外装体の一例として、図７に、ラミネートフィルム外装体１１０（外装体）内に電極体３０が収容された巻回型電池１０１の例を示す。 As an example of another exterior body in which the electrode body 30 is accommodated, FIG. 7 shows an example of a wound battery 101 in which the electrode body 30 is accommodated in a laminate film exterior body 110 (exterior body).
　巻回型電池１０１は、電極体３０がラミネートフィルム外装体１１０によって覆われた平面視で長方形状の二次電池である。巻回型電池１０１は、電極体３０と、電極体３０を覆うラミネートフィルム外装体１１０とを備える。また、巻回型電池１０１は、電極体３０の正極３１及び負極３２にそれぞれ電気的に接続される正極接続端子１２１及び負極接続端子１２２を備える。なお、巻回型電池１の内部には、上述の実施形態と同様の非水電解液も封入されている。 The wound battery 101 is a secondary battery having a rectangular shape in a plan view in which the electrode body 30 is covered with the laminate film exterior body 110. The wound battery 101 includes an electrode body 30 and a laminate film exterior body 110 that covers the electrode body 30. The wound battery 101 includes a positive electrode connection terminal 121 and a negative electrode connection terminal 122 that are electrically connected to the positive electrode 31 and the negative electrode 32 of the electrode body 30, respectively. In addition, a non-aqueous electrolyte similar to that in the above-described embodiment is also enclosed in the wound battery 1.
　ラミネートフィルム外装体１１０は、アルミニウム製の金属箔の一面側がナイロンで覆われ、且つ、他面側がポリプロピレンで覆われた材料からなる。すなわち、ラミネートフィルム外装体１１０は、アルミニウムをナイロン及びポリプロピレンでラミネートした材料からなる。これにより、ラミネートフィルム外装体１１０は、ラミネートフィルム外装体１１０同士を重ね合わせた状態で加熱しながら圧力を加えることによって、溶着される。なお、金属箔は、アルミニウムに限らず、ステンレス等の他の金属材料によって形成されていてもよい。 The laminate film exterior body 110 is made of a material in which one side of an aluminum metal foil is covered with nylon and the other side is covered with polypropylene. That is, the laminate film exterior body 110 is made of a material obtained by laminating aluminum with nylon and polypropylene. Thereby, the laminate film exterior body 110 is welded by applying pressure while heating in a state where the laminate film exterior bodies 110 are overlapped. The metal foil is not limited to aluminum but may be formed of other metal materials such as stainless steel.
　また、ラミネートフィルム外装体１１０は、略長方形状に形成されている。一対のラミネートフィルム外装体１１０によって電極体３０を挟んだ状態で、該ラミネートフィルム外装体１１０の外周側同士を溶着することにより、図７に示すような膨出部１０１ａ及びシール部１０１ｂが形成される。すなわち、ラミネートフィルム外装体１１０が電極体３０を覆うことにより膨出部１０１ａが形成され、該膨出部１０１ａの周囲でラミネートフィルム外装体１１０同士を溶着することにより該膨出部１０１ａを囲むようにシール部１０１ｂが形成される。 Further, the laminate film outer package 110 is formed in a substantially rectangular shape. In a state where the electrode body 30 is sandwiched between the pair of laminate film exterior bodies 110, the outer peripheral sides of the laminate film exterior body 110 are welded together to form a bulging portion 101a and a seal portion 101b as shown in FIG. The That is, the bulging portion 101a is formed by covering the electrode body 30 with the laminate film exterior body 110, and the bulging portion 101a is surrounded by welding the laminate film exterior body 110 to each other around the bulging portion 101a. The seal portion 101b is formed.
　シール部１０１ｂのうち、巻回型電池１０１の長手方向の端部側に位置する部分では、正極接続端子１２１及び負極接続端子１２２が、一対のラミネートフィルム外装体１１０に挟み込まれた状態で、ラミネートフィルム外装体１１０同士が溶着されることにより固定されている。正極接続端子１２１及び負極接続端子１２２は、それぞれ、電極体３０に取り付けられた正極リード及び負極リード３５に接続されている。これにより、ラミネートフィルム外装体１１０によって覆われた電極体３０を、外部に対して電気的に接続することができる。 In the portion of the seal portion 101b located on the end side in the longitudinal direction of the wound battery 101, the positive electrode connection terminal 121 and the negative electrode connection terminal 122 are laminated with the pair of laminate film exterior bodies 110 sandwiched therebetween. The film exterior bodies 110 are fixed by welding. The positive electrode connection terminal 121 and the negative electrode connection terminal 122 are respectively connected to a positive electrode lead and a negative electrode lead 35 attached to the electrode body 30. Thereby, the electrode body 30 covered with the laminate film exterior body 110 can be electrically connected to the outside.
　なお、上述の説明では、一対のラミネートフィルム外装体１１０の外周側同士を溶着する構成について説明したが、この限りではなく、１枚のラミネートフィルム外装体を、電極体３０を挟み込むように折り返して溶着してもよい。ラミネートフィルム外装体を折り返す方向については、電極体３０に対する正極接続端子１２１及び負極接続端子１２２の延伸方向であってもよいし、幅方向であってもよい。 In the above description, the configuration in which the outer peripheral sides of the pair of laminate film exterior bodies 110 are welded to each other has been described. However, the present invention is not limited to this, and one laminate film exterior body is folded back so as to sandwich the electrode body 30 therebetween. It may be welded. The direction in which the laminate film exterior body is folded back may be the extending direction of the positive electrode connection terminal 121 and the negative electrode connection terminal 122 with respect to the electrode body 30 or the width direction.
　前記実施形態では、電極体３０は扁平状の断面を有する。しかしながら、電極体は、円形状の断面を有する円柱状であってもよい。 In the embodiment, the electrode body 30 has a flat cross section. However, the electrode body may have a cylindrical shape having a circular cross section.
　前記実施形態では、負極３２は、金属基材層４５と金属表面層４６とからなるクラッド材によって構成されている。しかしながら、負極３２は、金属基材層及び金属表面層を有する構成であれば、クラッド材以外の構成であってもよい。また、負極３２は、Ｌｉと合金化可能な元素を含む粉末をバインダなどと共に合剤化して、これを集電体となる金属箔（金属基材層）の表面に塗布することによって形成されてもよい。このような構成において、Ｌｉと合金化可能な元素を含む粉末を、Ｌｉイオンを吸蔵・脱離可能な負極活物質（たとえば黒鉛等の炭素材料）と併用してもよい。なお、クラッド材以外の構成によって負極を構成した場合には、電極として機能する部分が本発明の負極に対応する。 In the above embodiment, the negative electrode 32 is constituted by a clad material composed of the metal base layer 45 and the metal surface layer 46. However, the negative electrode 32 may have a configuration other than the clad material as long as it has a metal base layer and a metal surface layer. The negative electrode 32 is formed by combining a powder containing an element that can be alloyed with Li with a binder or the like, and applying the mixture onto the surface of a metal foil (metal substrate layer) that serves as a current collector. Also good. In such a configuration, a powder containing an element that can be alloyed with Li may be used in combination with a negative electrode active material (for example, a carbon material such as graphite) capable of inserting and extracting Li ions. In addition, when a negative electrode is comprised by structures other than a cladding material, the part which functions as an electrode respond | corresponds to the negative electrode of this invention.
　前記実施形態では、負極３２は、金属基材層４５の両面に金属表面層４６を有する。しかしながら、金属表面層４６は、金属基材層４５の片側の面のみに設けられていてもよい。この場合、正極は、金属表面層４６に対して、セパレータ３３を挟んで対向する位置に正極活物質層が位置付けられるように、配置すればよい。 In the above embodiment, the negative electrode 32 has the metal surface layer 46 on both surfaces of the metal base layer 45. However, the metal surface layer 46 may be provided only on one surface of the metal base layer 45. In this case, the positive electrode may be disposed so that the positive electrode active material layer is positioned at a position facing the metal surface layer 46 with the separator 33 interposed therebetween.
　前記実施形態では、それぞれ帯状に形成された正極３１及び負極３２を、例えば両者の間及び正極３１の下側にセパレータ３３がそれぞれ位置するように、セパレータ３３に重ね合わせている。しかしながら、正極３１、負極３２及びセパレータ３３を重ねる順番は、二次電池を構成可能な順番であれば、どのような順番であってもよい。 In the embodiment, the positive electrode 31 and the negative electrode 32 each formed in a strip shape are overlapped with the separator 33 such that the separator 33 is positioned between the two and the lower side of the positive electrode 31, for example. However, the order in which the positive electrode 31, the negative electrode 32, and the separator 33 are stacked may be any order as long as the secondary battery can be configured.
　前記実施形態では、外装缶１０に電極体３０の正極３１を電気的に接続しているが、この限りではなく、外装缶１０に負極３２を電気的に接続してもよい。 In the above embodiment, the positive electrode 31 of the electrode body 30 is electrically connected to the outer can 10, but this is not restrictive, and the negative electrode 32 may be electrically connected to the outer can 10.
　本発明は、正極、負極及びセパレータを巻回してなる電極体を有する巻回型電池に利用可能である。 The present invention is applicable to a wound battery having an electrode body formed by winding a positive electrode, a negative electrode, and a separator.

Claims (9)

  1. 　それぞれ帯状に形成された正極、負極及びセパレータが、前記正極と前記負極との間に前記セパレータが位置するように巻回され、軸線方向に延びる柱状の電極体を備え、
    　前記負極は、Ｌｉと合金化可能な元素を含み、
    　前記電極体における前記負極の巻き終わり端部は、保護部材によって覆われている、巻回型電池。     Each of the positive electrode, the negative electrode, and the separator formed in a strip shape is wound so that the separator is positioned between the positive electrode and the negative electrode, and includes a columnar electrode body extending in the axial direction.
    The negative electrode contains an element that can be alloyed with Li,
    A winding type battery in which a winding end portion of the negative electrode in the electrode body is covered with a protective member.
  2. 　請求項１に記載の巻回型電池において、
    　前記保護部材は、前記負極の巻き終わり端部を、前記負極の短手方向の一方の端部から他方の端部に亘って覆うように設けられている、巻回型電池。     The wound battery according to claim 1,
    The said protection member is a winding type battery provided so that the winding end end part of the said negative electrode may be covered over from the one edge part of the transversal direction of the said negative electrode to the other edge part.
  3. 　請求項１または２に記載の巻回型電池において、
    　前記保護部材は、前記負極の巻き終わり端部と、前記負極の短手方向の端部において前記巻き終わり端部から所定範囲の部分とを覆うように設けられている、巻回型電池。     The wound battery according to claim 1 or 2,
    The said protection member is a winding type battery provided so that the winding end edge part of the said negative electrode and the part of a predetermined range may be covered from the said winding end edge part in the edge part of the transversal direction of the said negative electrode.
  4. 　請求項１から３のいずれか一つに記載の巻回型電池において、
    　前記正極は、正極活物質層を含み、
    　前記保護部材は、前記負極の巻き終わり端部のうち、前記電極体の径方向において、前記セパレータを挟んで前記正極活物質層と重なる部分に設けられている、巻回型電池。     The wound battery according to any one of claims 1 to 3,
    The positive electrode includes a positive electrode active material layer,
    The said protection member is a winding type battery provided in the part which overlaps with the said positive electrode active material layer on both sides of the said separator in the radial direction of the said electrode body among the winding end ends of the said negative electrode.
  5. 　請求項１から４のいずれか一つに記載の巻回型電池において、
    　前記保護部材は、前記負極の巻き終わり端部の両面を覆うように設けられている、巻回型電池。     In the wound battery according to any one of claims 1 to 4,
    The said protection member is a winding type battery provided so that both surfaces of the winding end edge part of the said negative electrode may be covered.
  6. 　請求項１から５のいずれか一つに記載の巻回型電池において、
    　前記保護部材は、一部が前記負極の厚み方向に延びる端面を覆うように設けられている、巻回型電池。     The wound battery according to any one of claims 1 to 5,
    The said protection member is a winding type battery provided so that a part may cover the end surface extended in the thickness direction of the said negative electrode.
  7. 　請求項１から６のいずれか一つに記載の巻回型電池において、
    　前記保護部材は、電気絶縁材料で且つ電池反応に寄与しない材料によって構成されている、巻回型電池。     The wound battery according to any one of claims 1 to 6,
    The said protection member is a winding type battery comprised with the material which is an electrically insulating material and does not contribute to a battery reaction.
  8. 　請求項１から７のいずれか一つに記載の巻回型電池において、
    　前記負極は、電池の充電後に、負極活物質として、Ｌｉ－Ａｌ合金を含む、巻回型電池。     The wound battery according to any one of claims 1 to 7,
    The negative electrode is a wound battery including a Li—Al alloy as a negative electrode active material after the battery is charged.
  9. 　請求項８に記載の巻回型電池において、
    　前記負極は、Ｌｉと合金化しない金属基材層と、前記金属基材層の厚み方向の少なくとも一方に接合された金属表面層とを有する積層体であり、
    　前記金属表面層の少なくとも表面側は、電池の充電後に、前記Ｌｉ－Ａｌ合金を含む、巻回型電池。     The wound battery according to claim 8,
    The negative electrode is a laminate having a metal base layer that is not alloyed with Li and a metal surface layer bonded to at least one of the thickness directions of the metal base layer.
    At least a surface side of the metal surface layer is a wound battery including the Li—Al alloy after the battery is charged.
PCT/JP2017/010543 2017-01-20 2017-03-15 Wound-type battery WO2018135011A1 (en)

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JP2001085066A (en) * 1999-07-09 2001-03-30 Matsushita Electric Ind Co Ltd Nonaqueous electrolyte battery
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WO2021106763A1 (en) * 2019-11-28 2021-06-03 株式会社村田製作所 Secondary battery, electronic device, and electric power tool

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