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WO2010047079A1 - 積層型リチウムイオン二次電池 - Google Patents

積層型リチウムイオン二次電池 Download PDF

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Publication number
WO2010047079A1
WO2010047079A1 PCT/JP2009/005455 JP2009005455W WO2010047079A1 WO 2010047079 A1 WO2010047079 A1 WO 2010047079A1 JP 2009005455 W JP2009005455 W JP 2009005455W WO 2010047079 A1 WO2010047079 A1 WO 2010047079A1
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WO
WIPO (PCT)
Prior art keywords
ion secondary
battery element
plastic film
lithium ion
porous plastic
Prior art date
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Ceased
Application number
PCT/JP2009/005455
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English (en)
French (fr)
Inventor
大道寺孝夫
猪瀬耐
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Tokin Corp
Original Assignee
NEC Tokin Corp
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Filing date
Publication date
Application filed by NEC Tokin Corp filed Critical NEC Tokin Corp
Priority to CN2009801423937A priority Critical patent/CN102246345A/zh
Priority to US13/123,401 priority patent/US20110195300A1/en
Publication of WO2010047079A1 publication Critical patent/WO2010047079A1/ja
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/052—Li-accumulators
    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/116—Primary casings; Jackets or wrappings characterised by the material
    • H01M50/121—Organic material
    • 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/116—Primary casings; Jackets or wrappings characterised by the material
    • H01M50/124—Primary casings; Jackets or wrappings characterised by the material having a layered structure
    • 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/131—Primary casings; Jackets or wrappings characterised by physical properties, e.g. gas permeability, size or heat resistance
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/543—Terminals
    • H01M50/547—Terminals characterised by the disposition of the terminals on the cells
    • H01M50/55—Terminals characterised by the disposition of the terminals on the cells on the same side of the cell
    • 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
    • H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
    • 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
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H01M4/583—Carbonaceous material, e.g. graphite-intercalation compounds or CFx
    • H01M4/587—Carbonaceous material, e.g. graphite-intercalation compounds or CFx for inserting or intercalating light metals
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/409—Separators, membranes or diaphragms characterised by the material
    • H01M50/411—Organic material
    • H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
    • H01M50/417—Polyolefins
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/463—Separators, membranes or diaphragms characterised by their shape
    • H01M50/466—U-shaped, bag-shaped or folded
    • 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 laminated lithium ion secondary battery in which the entire surface of a battery element laminate is covered with a porous plastic film.
  • lithium ion secondary batteries have been used as a power source for portable devices such as mobile phones and digital still cameras due to demands for higher capacity and smaller size.
  • lithium ion secondary batteries with high energy density and no memory effect are used as power sources for electric bicycles, electric vehicles, and electric tools. Accordingly, lithium ion secondary batteries are required to have a long life and large volume energy density and mass energy density.
  • a plurality of flat plate-like positive electrode and negative electrode are laminated through a separator, electrode terminals connected to each are connected in parallel, and a laminated type using a film-like exterior material that is advantageous from the energy density of the battery Lithium ion secondary batteries have been proposed.
  • a stacked lithium ion secondary battery is composed of a battery element laminate in which a plurality of positive electrodes and negative electrodes are stacked opposite to each other with a separator interposed between a positive electrode terminal and a negative electrode terminal connected to each of the positive electrode and the negative electrode.
  • the positive electrode terminal and the negative electrode terminal are separated from each other so as not to contact each other, and the positive electrode terminal and the negative electrode terminal are connected in parallel, and sealed with a film-like packaging material so as to hold the electrolytic solution.
  • FIG. 6 is a diagram for explaining an example of a battery element laminate of a conventional lithium ion secondary battery.
  • the battery element laminate 20 in which the positive electrode 1 and the negative electrode 2 housed in a plurality of bag-like separators 3 are stacked to face each other is made of polypropylene having a width of about 20 mm in the vicinity of the center of each side.
  • the four adhesive tapes 21 are used to bind and fix four positions so that the positive electrode, the separator, and the negative electrode do not shift in position.
  • the battery element is fixed by wrapping the adhesive tape around the battery element laminate, and the battery element laminate has a space so that the adhesive tape does not stick to the side surface of the battery element laminate, thereby allowing better penetration of the electrolyte into the battery element Proposed batteries have been proposed.
  • Patent Document 1 Japanese Patent Document 1
  • the battery element laminate in which the positive electrode and the negative electrode are laminated via the separator is bonded and fixed at four places with an adhesive tape having a width of about 20 mm in the vicinity of the center of each of the four sides, the positional deviation is prevented. There has been a problem that the outermost electrode is torn along the sticking end of the adhesive tape due to external force or the like.
  • Patent Document 1 when a space is formed on the side surface of the battery element laminate, the volume energy density is reduced and the electrode terminal is not fixed with respect to the drawing direction of the electrode terminal. There is a concern about misalignment.
  • the present invention facilitates the holding of the electrolytic solution and the supply of the electrolytic solution to the battery element laminate, improving the cycle characteristics of the battery, and the positive displacement of the battery element laminate in which the positive electrode, the separator, and the negative electrode are laminated,
  • Another object of the present invention is to provide a laminated lithium ion secondary battery in which electrode breakage from the end face of the adhesive tape does not occur by preventing the negative electrode without attaching an adhesive tape or the like.
  • a positive electrode terminal is drawn from the positive electrode of a battery element laminate in which a positive electrode and a negative electrode are laminated via a separator, and a negative electrode terminal lead is drawn from the negative electrode.
  • the battery element laminate covered with a porous plastic film except for the positive electrode terminal and the lead-out portion of the negative electrode terminal, and the battery element laminate covered with the porous plastic film is sealed with a film-like exterior material It is a lithium ion secondary battery.
  • the said battery element laminated body is the said laminated lithium ion secondary battery sealed by the heat shrink of the said porous plastic film.
  • the porous plastic film is the above-described laminated lithium ion secondary battery having a porosity of 20% to 60% and a thickness of 20 ⁇ m to 100 ⁇ m.
  • the electrolytic solution can be held in the porous plastic film, and the cycle characteristics can be improved.
  • the electrolytic solution can be held in the porous plastic film, it is possible to reduce the ejection of the electrolytic solution when the inside of the battery is decompressed and sealed in the battery manufacturing process.
  • FIG. 1 is a diagram for explaining a battery element laminate of a laminated lithium ion secondary battery of the present invention.
  • FIG. 2 is a view for explaining a bag-like porous body made of a porous plastic film.
  • FIG. 3 is a view for explaining the battery element laminate-bag-like porous body composite.
  • FIG. 4 is a diagram illustrating a battery element laminate-bag-like porous body composite in which a positive electrode terminal and a negative electrode terminal are bonded to a positive electrode and a negative electrode, respectively.
  • FIG. 5 is a diagram for explaining a laminated lithium ion secondary battery sealed with the film-shaped exterior material of the present invention.
  • FIG. 6 is a diagram for explaining an example of a battery element laminate of a conventional laminated lithium ion secondary battery.
  • FIG. 1 is a diagram for explaining a battery element laminate of a laminated lithium ion secondary battery of the present invention.
  • a positive electrode 1 in which a positive electrode active material such as a lithium manganese composite oxide that occludes and releases lithium ions is coated on an aluminum foil, and a bag made of a three-layer porous film of polypropylene, polyethylene, or polypropylene / polyethylene / polypropylene
  • the battery element laminate 4 is prepared by alternately laminating the negative electrode 2 coated with a negative electrode active material such as graphite that occludes and releases lithium ions on a copper foil.
  • the produced battery element laminate 4 is housed in a bag-like porous body 5 made of a porous plastic film, as shown in FIG.
  • the positive electrode 1 and the negative electrode 2 are integrated by heat contraction and heat shrinkage to produce a battery element laminate-bag-like porous body composite 6.
  • the positive terminals 7 are joined to the plurality of positive electrodes 1 of the battery element, and the negative terminals 8 are similarly connected to the plurality of negative electrodes 2.
  • the battery element laminate-bag-like porous body composite 6 is sealed with a film-shaped exterior material 9 and sealed with the film-shaped exterior material 9.
  • the laminated lithium ion secondary battery 10 is manufactured.
  • the battery element laminate-bag-like porous body composite is formed by covering the entire surface of the battery element laminate 4 with the porous plastic film without using the bag-like porous body 5 as described above, and by the heat shrinkage of the porous plastic film. You may make a body.
  • Example 1 14 sheets of 0.18 mm-thick positive electrode accommodated in a bag-like polypropylene / polyethylene / polypropylene three-layer porous membrane separator and 15 sheets of 0.1 mm-thick negative electrode alternately
  • the laminate was stored using a plastic film and impregnated with a mixed solution of ethylene carbonate and diethylene carbonate containing 1 mol / L LiPF 6 as an electrolyte.
  • the film-shaped packaging material made of polyethylene / aluminum / polyethylene terephthalate is covered, and the film-shaped packaging material is overlapped with heat at 160 ° C. under a pressure of 0.4 MPa.
  • Ninety-six sealed stacked lithium ion secondary batteries were produced.
  • Each manufactured lithium ion secondary battery was charged at a constant current of up to 4.2 V at a current value of 5.0 A corresponding to 1 C at 45 ° C. and then switched to constant voltage charging for a total of 2.5 hours. After carrying out constant current constant voltage charging, a cycle charge / discharge cycle test was repeated in which 5.0 A constant current discharging was repeated until the battery voltage dropped to 3.0 V. Table 1 shows the arithmetic average value of the number of cycles until the discharge capacity becomes half of the first capacity as the number of cycles with a capacity retention ratio of 50%.
  • Comparative Example 1 As in Example 1, a laminate having a width of 70 mm, a length of 125 mm, and a thickness of 5 mm was produced by alternately laminating bag-shaped separators containing positive electrodes and negative electrodes, and four central portions of each ridge. Are bonded and fixed with an adhesive tape made of polypropylene having a width of 20 mm, covered with a film-like exterior material made of polyethylene / aluminum / polyethylene terephthalate, and the same amount of electrolyte as in Example 1 is injected to overlap the film-like exterior material. Under the pressure of 0.4 MPa, heat was applied at 160 ° C. to the sealed portion, and 96 laminated lithium ion secondary batteries of Comparative Sample 1 were sealed with a film-like packaging material.
  • Example 2 In the same manner as in Example 1, a charge / discharge test was performed on each comparative sample, the number of cycles until the discharge capacity became half of the first capacity was measured, and the arithmetic average value is shown in Table 1.
  • the cycle-type lithium ion secondary battery in which the battery element laminate was housed in the porous plastic film had better cycle characteristics.
  • the laminated lithium ion secondary batteries produced in Example 1 and Comparative Example 1 were disassembled after the charge / discharge test and compared, the laminated body bound and fixed with the polypropylene adhesive tape had the outermost negative electrode made of polypropylene.
  • the electrode was not broken, although the number of pieces that had been torn from the end face of the adhesive tape was 5.2%. It was.
  • Example 2 In the same manner as in Example 1, a battery element laminate having a width of 70 mm, a length of 125 mm, and a thickness of 5 mm was produced by alternately laminating bag-shaped separators containing positive electrodes and negative electrodes, and the thickness was 30 ⁇ m.
  • the laminate was accommodated using the same material as the separator containing the positive electrode as a porous plastic film, and sealed by shrinkage by applying a pressure of 3 Mpa and heat at 85 ° C. from the thickness direction of the laminate.
  • the battery element laminated body was accommodated in the film-shaped exterior material, and the film-shaped exterior materials were piled up, and 30 laminated type lithium ion secondary batteries were produced.
  • the prepared lithium ion secondary battery was subjected to a charge / discharge test in the same manner as in Example 1, and the number of cycles until the discharge capacity became half of the first capacity was set as the number of cycles with a capacity maintenance ratio of 50%.
  • the arithmetic mean value is shown in Table 1.
  • Example 3 A battery element laminate having a width of 70 mm, a length of 125 mm, and a thickness of 5 mm was produced by alternately laminating bag-like separators containing positive electrodes and negative electrodes, and Example 1 has a porosity of 20%,
  • the battery element laminates were housed in porous plastic films having the same characteristics except that the thickness was different from 30 ⁇ m.
  • the porous plastic film containing the battery element laminate is housed in a film-like exterior material, the film-like exterior materials are overlapped, and a temperature of 160 ° C. is applied under a pressure of 0.4 MPa and sealed. Five stacked lithium ion secondary batteries were produced.
  • the charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 2.
  • Example 4 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 3 except that a porous plastic film having a porosity of 30% and a thickness of 30 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 2.
  • Example 5 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 3 except that a porous plastic film having a porosity of 40% and a thickness of 30 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 2.
  • Example 6 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 3 except that a porous plastic film having a porosity of 50% and a thickness of 30 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 2.
  • Example 7 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 3 except that a porous plastic film having a porosity of 60% and a thickness of 30 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 2.
  • Example 8 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 3 except that a porous plastic film having a porosity of 10% and a thickness of 30 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 2.
  • Example 9 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 3 except that a porous plastic film having a porosity of 70% and a thickness of 30 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 2.
  • Example 10 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 3 except that a porous plastic film having a porosity of 80% and a thickness of 30 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 2.
  • Example 11 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 3 except that a porous plastic film having a porosity of 40% and a thickness of 20 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 3.
  • Example 12 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 11 except that a porous plastic film having a thickness of 30 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 3.
  • Example 13 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 11 except that a porous plastic film having a thickness of 50 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 3.
  • Example 14 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 11 except that a porous plastic film having a thickness of 70 ⁇ m was used. A charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic mean value is shown in Table 3.
  • Example 15 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 11 except that a porous plastic film having a thickness of 100 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 3.
  • Example 16 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 11 except that a porous plastic film having a thickness of 10 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 3.
  • Example 17 Five stacked lithium ion secondary batteries were produced in the same manner as in Example 11 except that a porous plastic film having a thickness of 150 ⁇ m was used. The charge / discharge test was performed in the same manner as in Example 1, the number of cycles until the discharge capacity reached 50% of the first capacity was measured, and the arithmetic average value is shown in Table 3.
  • Cycle characteristics were good when the thickness of the porous plastic film was in the range of 20 to 100 ⁇ m.
  • a battery element laminated body in which a positive electrode and a negative electrode are stacked to face each other via a separator is housed in a bag-like porous body made of a porous plastic film, so that the inside of the porous plastic film is accommodated.
  • workability in terms of manufacturing and production is also improved.

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Abstract

　正極電極と負極電極をセパレータを介して積層した電池要素積層体の前記正極電極から正極端子が引き出され、前記負極電極から負極端子が引き出されており、前記電池要素積層体は、正極端子および負極端子の引出部を除き、多孔質プラスチックフィルムで覆われており、前記多孔質プラスチックフィルムで覆われた前記電池要素積層体は、フィルム状外装材によって封口されたことを特徴とする積層型リチウムイオン二次電池。

Description

積層型リチウムイオン二次電池
　本発明は、電池要素積層体の全面を多孔質プラスチックフィルムで覆った、積層型リチウムイオン二次電池に関する。
　近年、携帯電話やデジタルスチールカメラなどの携帯機器用の電源として高容量化、小型化の要求により、リチウムイオン二次電池が用いられている。また、電動自転車、電気自動車、電動工具の電源としても、高エネルギー密度で、メモリー効果のないリチウムイオン二次電池が用いられている。これに伴いリチウムイオン二次電池には、高寿命であって、容積エネルギー密度および質量エネルギー密度が大きなものが要求されている。
　そこで、複数の平板状の正極電極および負極電極をセパレータを介して積層し、それぞれに接続した電極端子を並列に接続し、電池のエネルギー密度からも有利であるフィルム状外装材を用いた積層型リチウムイオン二次電池が提案されている。
　積層型リチウムイオン二次電池は複数枚の正極電極と負極電極がセパレータを介して対向して積層した電池要素積層体からなり、正極電極および負極電極のそれぞれに接続した正極端子および負極端子を、正極端子と負極端子が相互に接触することがないように離間させて、正極端子および負極端子を並列に接続し、電解液を保持するようにフィルム状外装材で封口されている。
　図６は、従来のリチウムイオン二次電池の電池要素積層体の一例を説明する図である。
　複数枚の袋状のセパレータ３に収納された正極電極１と負極電極２が対向して積層配置された電池要素積層体２０は、４辺の各辺中央部付近にて幅２０ｍｍ程度のポリプロピレン等からなる粘着テープ２１で、正極電極、セパレータ、および負極電極が位置ずれを起こさないように４ヶ所を結束固定している。
　また、粘着テープを電池要素積層体に巻きつけて電池要素を固定するとともに、電池要素積層体側面に粘着テープが貼りつかなように空間を設けることによって、電池要素への電解液の浸透を良好なものとした電池が提案されている。例えば、特許文献１参照。
特開２００２－１９８０９８号公報
　積層型リチウムイオン二次電池において、電解液が電池要素内に充分に浸透しない場合には、充放電サイクルを繰り返した場合に容量維持率をはじめとする電池特性が低下するという問題があった。
　また、正極電極と負極電極をセパレータを介して積層した電池要素積層体は四辺の各辺中央部付近にて幅２０ｍｍ程度の粘着テープなどで４ヶ所結束固定して、位置ずれを防止した場合に、外力等によって電極が粘着テープの貼付端に沿って最外層の電極が破れてしまうと言うこと問題があった。
　また特許文献１のように、電池要素積層体の側面に空間が形成した場合には、容積エネルギー密度が低下し、また電極端子の引出し方向に対して固定されていないため、外的衝撃によって電極の位置ずれが懸念される。
　本発明は、電解液の保持と電池要素積層体への電解液の供給を円滑にし、電池のサイクル特性を改善すると共に、正極、セパレータ、負極を積層した電池要素積層体の位置ずれを正極、または負極に粘着テープ等を貼り付けることなく防止することによって、粘着テープの貼り付け端面からの電極破れが発生しない積層型リチウムイオン二次電池を提供することにある。
　本発明は、正極電極と負極電極をセパレータを介して積層した電池要素積層体の前記正極電極から正極端子が引き出され、前記負極電極から負極端子引が引き出されており、前記電池要素積層体は、前記正極端子および前記負極端子の引出部を除き、多孔質プラスチックフィルムで覆われており、前記多孔質プラスチックフィルムで覆われた前記電池要素積層体は、フィルム状外装材によって封口された積層型リチウムイオン二次電池である。
　また、前記電池要素積層体は、前記多孔質プラスチックフィルムの熱収縮により封じた前記の積層型リチウムイオン二次電池である。
　また、前記多孔質プラスチックフィルムは、空孔率が２０％～６０％、厚さが２０μｍ～１００μｍである前記の積層型リチウムイオン二次電池である。
　本発明により、電池要素積層体の全面を多孔質プラスチックフィルムで覆い熱収縮により封じたため、多孔質プラスチックフィルム内に電解液を保持し、サイクル特性を改善することができる。また、電解液を多孔質プラスチックフィルム内に保持できるため、電池製造過程において、電池内部を減圧して封止する際に電解液の噴出を減少することができる。
　また、電池要素積層体を固定するための粘着テープ等の貼り付けの必要がなくなり、多孔質プラスチックフィルムで電池要素積層体の全体を収納するため、電池要素積層体の製造工程において外力等によって粘着テープ貼付端面からの電極破れが発生しない積層型リチウムイオン二次電池の提供が可能となった。
図１は、本発明の積層型リチウムイオン二次電池の電池要素積層体を説明する図である。 図２は、多孔質プラスチックフィルムで作製した袋状多孔質体を説明する図である。 図３は、電池要素積層体－袋状多孔質体複合体を説明する図である。 図４は、正極電極、負極電極に，それぞれ正極端子，負極端子を接合した電池要素積層体－袋状多孔質体複合体を説明する図である。 図５は、本発明のフィルム状外装材によって封口した積層型リチウムイオン二次電池を説明する図である。 図６は、従来の積層型リチウムイオン二次電池の電池要素積層体の一例を説明する図である。
　以下に、図面を参照して本発明を説明する。
　図１は、本発明の積層型リチウムイオン二次電池の電池要素積層体を説明する図である。
　アルミニウム箔上に、リチウムイオンを吸蔵、放出するリチウムマンガン複合酸化物等の正極活物質を塗布した正極電極１を、ポリプロピレン、ポリエチレンまたは、ポリプロピレン／ポリエチレン／ポリプロピレンの三層構造多孔質膜からなる袋状セパレータ３に収納したものを、銅箔上にリチウムイオンを吸蔵、放出するグラファイト等の負極活物質を塗布した負極電極２とを交互に積層して電池要素積層体４を作製する。
　次に、図２で示す、多孔質プラスチックフィルムで作製した袋状多孔質体５に、図３で示すように、作製した電池要素積層体４を収納して、電解液を含浸させて、上部の開口部を加熱して熱収縮によって，正極電極１および負極電極２とを一体化して、電池要素積層体－袋状多孔質体複合体６を作製する。
　次いで、図４で示すように、電池要素の複数の正極電極１に正極端子７を接合し、同様に複数の負極電極２に負極端子８を接続する。
　正極端子７および負極端子８を接合した後に、図５に示すように、フィルム状外装材９によって、電池要素積層体－袋状多孔質体複合体６封口して、フィルム状外装材９で封口した積層型リチウムイオン二次電池１０を作製する。
　なお、上記したような袋状多孔質体５を用いずに多孔質プラスチックフィルムによって電池要素積層体４の全面を覆い多孔質プラスチックフィルムの熱収縮により、電池要素積層体－袋状多孔質体複合体を作製しても良い。
実施例１
　袋状のポリプロピレン／ポリエチレン／ポリプロピレンの三層構造多孔質膜のセパレータに厚さ０．１８ｍｍの正極電極を収納したものを１４枚と、厚さ０．１ｍｍの負極電極の１５枚とを交互に積層させて、幅７０ｍｍ、長さ１２５ｍｍ、厚さ厚さ５ｍｍの電池要素積層体を作製し、空孔率４０％のポリプロピレン／ポリエチレン／ポリプロピレンの三層構造多孔質膜で厚さ３０μｍの多孔質プラスチックフィルムを使用して積層体を収納し電解液として１ｍｏｌ／ＬのＬｉＰＦ6 を含有したエチレンカーボネートとジエチレンカーボネートの混合溶液を含浸させた。
　次いで、ポリエチレン／アルミニウム／ポリエチレンテレフタレートからなるフィルム状外装材で覆い、フィルム状外装材重ね合わせた部分に、０．４ＭＰａの圧力下で１６０℃の熱を加えて封口して、フィルム状外装材で封口した積層型リチウムイオン二次電池の９６個を作製した。
　作製した各リチウムイオン二次電池を４５℃において、１Ｃに相当する５．０Ａの電流値にて４．２Ｖまでの定電流充電を行った後に、定電圧充電に切り換えて、総計２．５時間の定電流定電圧充電を行った後に、電池電圧が３．０Ｖまで低下するまで５．０Ａの定電流放電を繰り返すサイクル充放電サイクル試験を行った。放電容量が第１回目の容量の半分になるまでのサイクル数を容量維持率５０％のサイクル数としてその相加平均値を表１に示す。
比較例１
　実施例１と同様に、正極電極を収納した袋状のセパレータと負極電極を交互に積層させた、幅７０ｍｍ、長さ１２５ｍｍ、厚さ５ｍｍの積層体を作製し、各稜の中央部４個所を幅２０ｍｍのポリプロピレン製粘着テープで結束固定して、ポリエチレン／アルミニウム／ポリエチレンテレフタレートからなるフィルム状外装材で覆い、実施例１と同量の電解液を注液してフィルム状外装材を重ね合わせた部分に、０．４ＭＰａの圧力下で、１６０℃の熱を加えて封口して、フィルム状外装材で封口した比較試料１の積層型リチウムイオン二次電池を９６個を作製した。
　実施例１と同様にして、各比較試料について充放電試験を行い、放電容量が第１回目の容量の半分になるまでのサイクル数を測定し、その相加平均値を表１に示す。
　これらの結果から、多孔質プラスチックフィルムに、電池要素の積層体を収納した積層型リチウムイオン二次電池の方がサイクル特性が良好であった。
　また実施例１と比較例１で作製した積層型リチウムイオン二次電池を充放電試験後に解体して比較したところ、ポリプロピレン製粘着テープで結束固定した積層体は、最外層の負極電極がポリプロピレン製粘着テープ貼付端面から破れてしまっているものが５．２％の個数で発生していたが、実施例１の袋状多孔質プラスチックフィルムに収納した積層体では、電極の破れは発生していなかった。
　また実施例１の電池の作製時には、フィルム状外装材で減圧して封止する際には、電解液の噴き出し等は発生しなかったが、比較例１の電池の作製時には封止の際に電解液の吹き出しがあった。
実施例２
　実施例１と同様にして、正極電極を収納した袋状のセパレータと負極電極を交互に積層させた、幅７０ｍｍ、長さ１２５ｍｍ、厚さ５ｍｍの電池要素積層体を作製し、厚さ３０μｍの多孔質プラスチックフィルムとして正極電極を収納したセパレータと同じ材料を使用して積層体を収納し、そこに積層厚さ方向から３Ｍｐａの圧力と８５℃の熱を加えることにより熱収縮させて密封した。
　次いで、２５℃に冷却して電解液を含浸し、電池要素積層体をフィルム状外装材に収納してフィルム状外装材同士を重ね合わせて３０個の積層型リチウムイオン二次電池を作製した。
　作製したリチウムイオン二次電池を、実施例１と同様にして充放電試験を行って、放電容量が第１回目の容量の半分になるまでのサイクル数を容量維持率５０％のサイクル数とし、相加平均値を表1に示す。
表１
　実施例番号　　　容量維持率５０％のサイクル数　　　電極破損率（％）
　　実施例１　　　　　　　　　 ７０１　　　　　　　　　　 　０
　　実施例２　　　　　　　　　 ６８９　　　　　　　　　　　 ０
　　比較例１　　　　　　　　　 ５２２　　　　　　　　　 ５．２
実施例３
　正極電極を収納した袋状セパレータと、負極電極を交互に積層させた、幅７０ｍｍ、長さ１２５ｍｍ、厚さ５ｍｍの電池要素積層体を作製し、実施例１とは、空孔率２０％、厚さ３０μｍが異なる点を除き他の特性が同じ多孔質プラスチックフィルムで電池要素積層体をそれぞれ収納した。
　次いで、電池要素積層体を収納した多孔質プラスチックフィルムを、フィルム状外装材に収納してフィルム状外装材同士を重ね合わせて、０．４ＭＰａの圧力下で１６０℃の温度を加えて封口して５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表２に示す。
実施例４
　空孔率が３０％で厚さ３０μｍの多孔質プラスチックフィルムを使用した点を除き実施例３と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表２に示す。
実施例５
　空孔率が４０％で厚さ３０μｍの多孔質プラスチックフィルムを使用した点を除き実施例３と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表２に示す。
実施例６
　空孔率が５０％で厚さ３０μｍの多孔質プラスチックフィルムを使用した点を除き実施例３と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表２に示す。
実施例７
　空孔率が６０％で厚さ３０μｍの多孔質プラスチックフィルムを使用した点を除き実施例３と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表２に示す。
実施例８
　空孔率が１０％で厚さ３０μｍの多孔質プラスチックフィルムを使用した点を除き実施例３と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表２に示す。
実施例９
　空孔率が７０％で厚さ３０μｍの多孔質プラスチックフィルムを使用した点を除き実施例３と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表２に示す。
実施例１０
　空孔率が８０％で厚さ３０μｍの多孔質プラスチックフィルムを使用した点を除き実施例３と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表２に示す。
表２
実施例番号　　空孔率（％）　容量維持率５０％のサイクル数　
　３　　　　　　　２０　　　　　　　 ６９０　　　　　　　 
　４　　　　　　　３０　　　　　　　 ７０３　　　　　　　 
　５　　　　　　　４０　　　　　　　 ６８６　　　　　　　 
　６　　　　　　　５０　　　　　　　 ６９０　　　　　　　 
　７　　　　　　　６０　　　　　　　 ６９５　　　　　　　 
　８　　　　　　　１０　　　　　　　 ５６０　　　　　　　 
　９　　　　　　　７０　　　　　　　 ５６３　　　　　　　 
１０　　　　　　　８０　　　　　　　 ５５９　　　　　　　 
　これらの結果から、多孔質プラスチックフィルムの空孔率は２０～６０％の範囲でより好ましいサイクル特性が得られることがわかった。
実施例１１
　空孔率が４０％で厚さ２０μｍの多孔質プラスチックフィルムを使用した点を除き実施例３と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表３に示す。
実施例１２
　厚さ３０μｍの多孔質プラスチックフィルムを使用した点を除き、実施例１１と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表３に示す。
　実施例１３
　厚さが５０μｍの多孔質プラスチックフィルムを使用した点を除き、実施例１１と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表３に示す。
実施例１４
　厚さが７０μｍの多孔質プラスチックフィルムを使用した点を除き、実施例１１と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表３に示す。
実施例１５
　厚さが１００μｍの多孔質プラスチックフィルムを使用した点を除き、実施例１１と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表３に示す。
実施例１６
　厚さが１０μｍの多孔質プラスチックフィルムを使用した点を除き、実施例１１と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表３に示す。
実施例１７
　厚さが１５０μｍの多孔質プラスチックフィルムを使用した点を除き、実施例１１と同様にして、５個の積層型リチウムイオン二次電池を作製した。
　実施例１と同様にして、充放電試験を行い、放電容量が第１回目の容量の５０％になるまでのサイクル数を測定し、その相加平均値を表３に示す。
　表３
　実施例番号　フィルムの厚さ（μｍ）　　容量維持率５０％のサイクル数
　１１　　　　　２０　　　　　　 　　　７０５
　１２　　　　　３０　　　　　　　 　　６９８
　１３　　　　　５０　　　　　　　 　　６９５
　１４　　　　　７０　　　　　　　 　　６９０
　１５　　　　１００　　　　　　　　　 ６９1
　１６　　　　　１０　　　　　　　　　 ５５３
　１７　　　　１５０　　　　　　　　　 ５７０
　多孔質プラスチックフィルムの厚さは２０～１００μｍの範囲でサイクル特性が良好であった。
　本発明は、正極電極と負極電極がセパレータを介して対向して積層配置された電池要素積層体を、多孔質プラスチックフィルムからなる袋状多孔質体に収納することで、多孔質プラスチックフィルム内部への電解液染み込みによる電池特性、特にサイクル特性を向上が得られ、更に、電池要素積層体の位置ずれ防止のための粘着テープが必要ないので、粘着テープ貼付端面からの電極破れと防止する効果もあり、製造作製面での作業性も向上する。
　１　正極電極
　２　負極電極
　３　セパレータ
　４　電池要素積層体
　５　袋状多孔質体
　６　電池要素積層体－袋状多孔質体複合体
　７　正極端子
　８　負極端子
　９　フィルム状外装材
　１０　積層型リチウムイオン二次電池
　２０　電池要素積層体
　２１　粘着テープ

Claims (3)

  1. 　正極電極と負極電極をセパレータを介して積層した電池要素積層体の前記正極電極から正極端子が引き出され、前記負極電極から負極端子が引き出されており、前記電池要素積層体は、前記正極端子および前記負極端子の引出部を除き、多孔質プラスチックフィルムで覆われており、前記多孔質プラスチックフィルムで覆われた前記電池要素積層体は、フィルム状外装材によって封口されたことを特徴とする積層型リチウムイオン二次電池。
  2. 　前記電池要素積層体は、前記多孔質プラスチックフィルムの熱収縮により封じたことを特徴とする請求項１記載の積層型リチウムイオン二次電池。
  3. 　前記多孔質プラスチックフィルムは、空孔率が２０％～６０％、厚さが２０μｍ～１００μｍからなることを特徴とする請求項１または２記載の積層型リチウムイオン二次電池。
PCT/JP2009/005455 2008-10-20 2009-10-19 積層型リチウムイオン二次電池 Ceased WO2010047079A1 (ja)

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