WO2020003846A1 - Batterie secondaire au lithium-ion - Google Patents

Batterie secondaire au lithium-ion Download PDF

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Publication number
WO2020003846A1
WO2020003846A1 PCT/JP2019/020847 JP2019020847W WO2020003846A1 WO 2020003846 A1 WO2020003846 A1 WO 2020003846A1 JP 2019020847 W JP2019020847 W JP 2019020847W WO 2020003846 A1 WO2020003846 A1 WO 2020003846A1
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Prior art keywords
lithium ion
ion secondary
secondary battery
separator
negative electrode
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PCT/JP2019/020847
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English (en)
Japanese (ja)
Inventor
良太 柳澤
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株式会社エンビジョンＡｅｓｃエナジーデバイス
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Priority to CN201980041983.4A priority Critical patent/CN112335091B/zh
Priority to JP2020527295A priority patent/JP7027648B2/ja
Publication of WO2020003846A1 publication Critical patent/WO2020003846A1/fr

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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
    • 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
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0566—Liquid materials
    • 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
    • H01M10/0583—Construction or manufacture of accumulators with folded construction elements except wound ones, i.e. folded positive or negative electrodes or separators, e.g. with "Z"-shaped electrodes or 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
    • H01M4/36—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
    • H01M4/52—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron
    • H01M4/525—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of nickel, cobalt or iron of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
    • 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
    • H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
    • H01M50/105—Pouches or flexible bags
    • 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
    • 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 lithium ion secondary battery.
  • Lithium ion secondary batteries have the feature of high energy density, and are widely used as power sources for mobile phones, notebook computers, electric vehicles, and the like.
  • a self-folding structure lithium ion secondary battery is known.
  • Patent Literature 1 Japanese Patent Application Laid-Open No. 2009-218105
  • Patent Literature 2 Japanese Patent Application Laid-Open No. 2016-143550
  • Patent Document 1 has a rectangular battery element in which a flat positive electrode, a separator, and a flat negative electrode are stacked, and one surface of the battery element is provided in each of the positive electrode and the negative electrode.
  • the positive electrode terminal connection part and the plate-shaped negative electrode terminal connection part are both drawn out terminal connection part extraction surfaces, and the projection in which the positive electrode terminal connection part and the negative electrode terminal connection part are respectively projected perpendicularly to the extending surface of the positive electrode and the negative electrode
  • the surfaces do not intersect with each other, and the positive electrode and the negative electrode have different areas of the surfaces facing each other, and all the projection portions projecting the electrode having the smaller area on the facing surface of the electrode having the larger area are on the larger side.
  • Each electrode is arranged so as to be located on the electrode surface of the separator, the separator is provided with an abutting portion that abuts the positive electrode end surface and the negative electrode end surface and regulates the movement of the positive electrode and the negative electrode.
  • the portion is formed by a fold or a joint between adjacent separators among the separators arranged on each electrode surface, and all the separators laminated on the electrode surface are joined by the fold or the joint.
  • Patent Literature 2 discloses a secondary battery in which a plurality of positive plates including a positive electrode active material and a plurality of negative plates including a negative electrode active material are sandwiched between separators folded in a zigzag manner. Wherein the separator has a plurality of protrusions protruding from the positive electrode plate and the negative electrode plate, and at least a portion of the protrusions has a tensile strength at break smaller than the remaining portion. A folded structure of a secondary battery having a break portion is described.
  • the conventional outermost layer separator of a lithium ion secondary battery having a meandering structure may be altered (discoloration, embrittlement, etc.).
  • the present invention has been made in view of the above circumstances, and provides a self-folding structure lithium-ion secondary battery in which the deterioration of the outermost layer separator is suppressed.
  • the inventor of the present invention has conducted intensive studies to solve the above-described problems, and has found that the separator located on the surface of the outermost negative electrode on which the SEI film is not formed is easily decomposed by the reaction with the electrolytic solution.
  • the present inventor has further studied diligently based on the above findings, and found that by controlling the separator on the outermost negative electrode to be located on the SEI film formed on the surface of the outermost negative electrode, the quality of the separator of the outermost layer was deteriorated. (Discoloration, embrittlement, etc.) can be suppressed, and the present invention has been completed.
  • the present invention has been made based on such knowledge.
  • a battery body including at least one power generating element composed of at least a positive electrode, an electrolytic solution, a separator and a negative electrode, An exterior body for enclosing the battery body therein; A pair of electrode terminals electrically connected to the battery body, and at least a part of which is exposed outside the exterior body;
  • a lithium ion secondary battery comprising:
  • the battery body has a structure in which the positive electrode and the negative electrode are respectively arranged between the separators folded in a zigzag manner, A solid electrolyte interface (SEI) film is formed on at least a peripheral portion of a surface of the outermost negative electrode, which is located on the outermost side of the electrode including the positive electrode and the negative electrode in the battery body, and does not face the positive electrode.
  • SEI solid electrolyte interface
  • the length L 1 of the outermost negative electrode of the SEI layer, said outermost negative electrode of the separator and the length L 2 is provided a lithium ion secondary battery which satisfies the relationship L 1 ⁇ L 2> 0 Is done. (Where the length L 1 of the SEI film, the end of the SEI film at the center of one side of the side where the electrode terminals are not exposed in the lithium ion secondary cell, the other of the SEI film the length of the end portion, and a length in a direction perpendicular to said one side.
  • the separator length L 2 is, on the side where the electrode terminals of the lithium ion secondary battery is not exposed (The length from the end of the separator on the outermost negative electrode at the center of one side to the other end of the separator, and the length in the direction perpendicular to the one side.)
  • FIG. 2 is an exploded perspective view schematically showing an example of the structure of the battery body according to the embodiment of the present invention. It is the perspective view which showed typically an example of the structure of the battery main body of embodiment which concerns on this invention.
  • FIG. 3 is a cross-sectional view schematically illustrating an example of the structure of a battery main body according to an embodiment of the present invention, and is a cross-sectional view in the A-A ′ direction illustrated in FIG. 2. It is the top view which showed typically an example of the structure of the battery main body of embodiment which concerns on this invention.
  • 1 is a perspective view schematically showing an example of the structure of a lithium ion secondary battery according to an embodiment of the present invention.
  • FIG. 1 is an exploded perspective view schematically showing an example of the structure of the battery main body 10 according to the embodiment of the present invention.
  • FIG. 2 is a perspective view schematically showing an example of the structure of the battery main body 10 of the embodiment according to the present invention.
  • FIG. 3 is a cross-sectional view schematically illustrating an example of the structure of the battery main body 10 according to the embodiment of the present invention, and is a cross-sectional view in the A-A ′ direction illustrated in FIG.
  • FIG. 4 is a plan view schematically showing an example of the structure of the battery main body 10 of the embodiment according to the present invention.
  • FIG. 5 is a perspective view schematically showing an example of the structure of the lithium ion secondary battery 100 of the embodiment according to the present invention.
  • a lithium ion secondary battery 100 includes a battery main body 10 including at least one power generating element including at least a positive electrode 15, an electrolytic solution, a separator 18, and a negative electrode 20,
  • the battery pack includes an exterior body for enclosing the battery body therein, and a pair of electrode terminals electrically connected to the battery body and at least partially exposed to the outside of the exterior body.
  • the battery main body 10 has a structure in which the positive electrode 15 and the negative electrode 20 are respectively arranged between the separators 18 folded in a zigzag manner, and is located at the outermost position among the electrodes composed of the positive electrode 15 and the negative electrode 20 in the battery main body 10.
  • the length L 1 of the SEI film 25 on the outermost negative electrode 20A and the length L 2 of the separator 18 on the outermost negative electrode 20A is, satisfy the relationship of L 1 ⁇ L 2> 0.
  • the length L 1 of the SEI film, as shown in FIG. 4, from the end of the SEI film 25 at the center of the side of one side 28 of the electrode terminal 30 in a lithium ion secondary battery 100 is not exposed, The length is the length to the other end of the SEI film 25 and the length in the direction perpendicular to one side 28.
  • the length L 2 of the separator, the end portion of the separator 18 on the outermost negative electrode 20A at the center of the side of one side 28 of the electrode terminal 30 in a lithium ion secondary battery 100 is not exposed, the other end of the separator 18 It is the length to the part and the length in the direction perpendicular to one side 28.
  • the conventional outermost layer separator of a lithium ion secondary battery having a zigzag structure may be altered (discoloration, embrittlement, etc.).
  • the inventors of the present invention have made intensive studies to realize a lithium ion secondary battery having a meandering structure in which deterioration of the outermost layer of the separator is suppressed. As a result, it was found that the separator located on the surface of the outermost negative electrode where the SEI film was not formed was easily decomposed by the reaction with the electrolytic solution.
  • the present inventor has further studied diligently based on the above findings, and found that by controlling the separator on the outermost negative electrode to be located on the SEI film formed on the surface of the outermost negative electrode, the quality of the separator of the outermost layer was deteriorated. (Discoloration, embrittlement, etc.) can be suppressed for the first time. That is, according to the present embodiment, the solid electrolyte interface (SEI) film 25 is formed on at least the peripheral portion of the surface of the outermost negative electrode 20 ⁇ / b> A located on the outermost side of the electrodes including the positive electrode 15 and the negative electrode 20 in the battery body 10.
  • SEI solid electrolyte interface
  • the length L 2 of the separator 18 on the outermost negative electrode 20A is the relationship of L 1 ⁇ L 2> 0
  • the separator located on the outermost negative electrode is decomposed by the reaction with the electrolytic solution, and is likely to deteriorate.
  • the ester bond is easily decomposed by the reaction with the electrolytic solution, when the separator contains a polyester resin, the quality of the outermost separator tends to be remarkable.
  • the separator located on the portion where the SEI film is formed does not directly contact the outermost negative electrode, a decomposition reaction hardly occurs.
  • the length L 1 of the SEI film 25 on the outermost negative electrode 20A, the length L 2 of the separator 18 on the outermost negative electrode 20A is, by satisfying the relationship of L 1 ⁇ L 2> 0, the outermost Since the ratio of the separator in direct contact with the negative electrode decreases, decomposition of the separator is suppressed. As a result, it is considered that the lithium ion secondary battery 100 having the meandering structure in which the deterioration of the outermost layer of the separator is suppressed can be obtained.
  • the SEI film is usually formed on the surface facing the positive electrode, but lithium ions for forming the SEI film also go around the surface not facing the positive electrode.
  • the SEI film 25 is also formed on at least the peripheral portion 20B of the surface not facing the positive electrode 15.
  • the length L 1 of the SEI film 25 on the outermost negative electrode 20A can be measured by XPS analysis. Specifically, since the ratio of Li is large in the portion where the SEI film is formed, the presence or absence of the SEI film can be checked by the ratio of Li. By examining whether or not the SEI film is formed in the portion, it can be determined whether or not the relationship of L 1 ⁇ L 2 > 0 is satisfied.
  • the length L 2 of the separator 18, the more the viewpoint of suppressing deterioration of the outermost layer of the separator is preferably less than 15.0 mm, more preferably 10. 0 mm or less, further preferably 8.0 mm or less, still more preferably 5.0 mm or less, and particularly preferably 4.0 mm or less.
  • the lower limit of the length L 2 of the separator 18 is not particularly limited, it is preferably at 0.1mm or more, more preferably 0.5mm or more.
  • the average length L 3 of the SEI film 25 on the outermost negative electrode 20A, on the outermost negative electrode 20A It is preferable that the average length L 4 of the separator 18 satisfies the relationship of L 3 ⁇ L 4 > 0.
  • the length of the SEI film 25 in the direction perpendicular to the side 28 was measured at 10 points, and the obtained 10 points were measured.
  • the average length and the average length L 3 of the SEI film was measured 10 points the vertical length of the separator to an edge 28, the average length of 10 points obtained average of the separator 18 the length L 4.
  • the average length and the average length L 3 of the SEI film was measured 10 points the vertical length of the separator to an edge 28, the average length of 10 points obtained average of the separator 18 the length L 4.
  • one side 28 is divided into ten pieces at equal intervals, and each central part (a total of ten points) can be selected.
  • the average length L 4 of the separator 18 is preferably less than 15.0 mm, more preferably 10 0.0 mm or less, more preferably 8.0 mm or less, still more preferably 5.0 mm or less, particularly preferably 4.0 mm or less.
  • lower limit of the average length L 4 of the separator 18 is not particularly limited, it is preferably at 0.1mm or more, more preferably 0.5mm or more.
  • the lithium ion secondary battery according to the present embodiment preferably has a cell rated capacity of 7 Ah or more.
  • the number of laminations or the number of windings of the positive electrode in the central portion is preferably 10 or more, more preferably 15 or more, and even more preferably 20 or more. .
  • the capacity of the lithium ion secondary battery according to the present embodiment can be increased.
  • the lithium ion secondary battery according to the present embodiment has excellent short circuit resistance and can suppress thermal runaway of the battery.
  • the battery body according to the present embodiment includes, for example, one or more power generating elements in which a positive electrode and a negative electrode are alternately stacked via a separator folded in a zigzag manner. These power generating elements are housed in a container formed of an exterior body together with an electrolytic solution (not shown). Electrode terminals (a positive electrode terminal and a negative electrode terminal) are electrically connected to the power generating element, and part or all of the electrode terminals are drawn out of the exterior body.
  • the positive electrode is provided with a coated portion of the positive electrode active material (positive electrode active material layer) and an uncoated portion on the front and back of the positive electrode current collector layer
  • the negative electrode is provided with a negative electrode active material on the front and back of the negative electrode current collector layer. (A negative electrode active material layer) and an uncoated portion are provided.
  • An uncoated portion of the positive electrode active material in the positive electrode current collector layer is used as a positive electrode tab for connecting to the positive electrode terminal, and an uncoated portion of the negative electrode active material in the negative electrode current collector layer is used as a negative electrode tab for connecting to the negative electrode terminal.
  • the positive electrode tabs are assembled on the positive electrode terminal and connected together with the positive electrode terminal by ultrasonic welding or the like, and the negative electrode tabs are assembled on the negative electrode terminal and connected with the negative electrode terminal by ultrasonic welding or the like. Then, one end of the positive electrode terminal is drawn out of the exterior body, and one end of the negative electrode terminal is also drawn out of the exterior body.
  • the battery main body according to the present embodiment can be manufactured according to a known method.
  • the positive electrode can be appropriately selected from the positive electrodes that can be used in known lithium ion secondary batteries, depending on the application and the like.
  • the positive electrode active material used for the positive electrode a material having high electron conductivity that can reversibly release and occlude lithium ions and facilitate electron transport is preferable.
  • the positive electrode active material used for the positive electrode is not particularly limited.
  • a lithium composite oxide having a layered rock salt structure or a spinel structure, or lithium iron phosphate having an olivine structure is used.
  • the lithium composite oxide include lithium manganate (LiMn 2 O 4 ); lithium cobalt oxide (LiCoO 2 ); lithium nickelate (LiNiO 2 ); and at least a part of the manganese, cobalt, and nickel portions of these lithium compounds.
  • One of these positive electrode active materials may be used alone, or two or more thereof may be used in combination.
  • a lithium-containing composite oxide having a layered crystal structure a lithium-nickel-containing composite oxide is exemplified.
  • this lithium-nickel-containing composite oxide an oxide in which part of nickel at nickel sites is replaced with another metal can be used.
  • the metal other than Ni occupying nickel sites include at least one metal selected from Mn, Co, Al, Mg, Fe, Cr, Ti, and In.
  • the lithium nickel-containing composite oxide preferably contains Co as a metal other than Ni occupying nickel sites. More preferably, the lithium nickel-containing composite oxide contains Mn or Al in addition to Co, that is, lithium nickel cobalt manganese composite oxide (NCM) having a layered crystal structure, lithium nickel having a layered crystal structure Cobalt aluminum composite oxide (NCA) or a mixture thereof can be suitably used.
  • NCM lithium nickel cobalt manganese composite oxide
  • NCA Cobalt aluminum composite oxide
  • lithium nickel-containing composite oxide having a layered crystal structure for example, an oxide represented by the following formula (1) can be used.
  • Me1 is Mn or Al
  • Me2 is at least one selected from the group consisting of Mn, Al, Mg, Fe, Cr, Ti, and In (excluding metals of the same type as Me1); ⁇ 0.5 ⁇ a ⁇ 0.1, 0.1 ⁇ b ⁇ 1, 0 ⁇ c ⁇ 0.5, 0 ⁇ d ⁇ 0.5)
  • the average particle diameter of the positive electrode active material is, for example, preferably from 0.1 to 50 ⁇ m, more preferably from 1 to 30 ⁇ m, and still more preferably from 2 to 25 ⁇ m, from the viewpoint of reactivity with the electrolytic solution and rate characteristics.
  • the average particle diameter means a particle diameter (median diameter: D 50 ) at an integrated value of 50% in a particle size distribution (by volume) by a laser diffraction scattering method.
  • the positive electrode includes, for example, a positive electrode current collector layer and a positive electrode active material layer on the positive electrode current collector layer.
  • the positive electrode is arranged such that the positive electrode active material layer faces the negative electrode active material layer on the negative electrode current collector layer via the separator.
  • the positive electrode according to the present embodiment can be manufactured by a known method. For example, by dispersing a positive electrode active material, a binder resin, and a conductive additive in an organic solvent to obtain a positive electrode slurry, applying and drying the positive electrode slurry on a positive electrode current collector layer, and pressing if necessary.
  • a method of forming a positive electrode active material layer on a positive electrode current collector layer can be employed.
  • the slurry solvent used for producing the positive electrode for example, N-methyl-2-pyrrolidone (NMP) can be used.
  • a resin generally used as a binder resin for a positive electrode such as polytetrafluoroethylene (PTFE) and polyvinylidene fluoride (PVDF) can be used.
  • PTFE polytetrafluoroethylene
  • PVDF polyvinylidene fluoride
  • the content of the binder resin in the positive electrode active material layer is preferably 0.1 part by mass or more and 10.0 parts by mass or less when the whole of the positive electrode active material layer is 100 parts by mass, and is 0.5 part by mass. It is more preferably at least 5.0 parts by mass and even more preferably at least 1.0 part by mass and not more than 5.0 parts by mass.
  • the content of the binder resin is within the above range, the balance between the coating properties of the positive electrode slurry, the binding properties of the binder, and the battery characteristics is further improved.
  • the content of the binder resin is equal to or less than the above upper limit, the ratio of the positive electrode active material increases, and the capacity per positive electrode mass increases, which is preferable. It is preferable that the content of the binder resin be equal to or more than the lower limit, because the electrode peeling is suppressed.
  • the positive electrode active material layer can include a conductive auxiliary in addition to the positive electrode active material and the binder resin.
  • the conductive assistant is not particularly limited as long as it improves the conductivity of the positive electrode, and examples thereof include carbon black, Ketjen black, acetylene black, natural graphite, artificial graphite, and carbon fiber. These conductive aids may be used alone or in combination of two or more.
  • the content of the conductive additive in the positive electrode active material layer is preferably 1.0 part by mass or more and 4.0 parts by mass or less, when the whole positive electrode active material layer is 100 parts by mass, and is 1.2 parts by mass. It is more preferably not less than 3.5 parts by mass, more preferably not less than 1.5 parts by mass and not more than 3.5 parts by mass, and more preferably not less than 2.0 parts by mass and not more than 3.5 parts by mass. Particularly preferred. When the content of the conductive additive is within the above range, the balance between the coating properties of the positive electrode slurry, the binding properties of the binder resin, and the battery characteristics is further improved.
  • the content of the conductive auxiliary agent be equal to or less than the above upper limit, because the ratio of the positive electrode active material increases and the capacity per positive electrode mass increases. It is preferable that the content of the conductive auxiliary agent be equal to or more than the above lower limit, because the conductivity of the positive electrode is further improved and the battery characteristics of the lithium ion secondary battery are improved.
  • the positive electrode current collector layer aluminum, stainless steel, nickel, titanium, an alloy thereof, or the like can be used.
  • Examples of the shape include a foil, a flat plate, and a mesh.
  • an aluminum foil can be suitably used.
  • the thickness of the positive electrode current collector layer is not particularly limited, but is, for example, 1 ⁇ m or more and 30 ⁇ m or less.
  • the density of the positive electrode active material layer is not particularly limited, for example, it is preferably, 2.4 g / cm 3 or more 3.8 g / cm 3 or less or less 2.0 g / cm 3 or more 4.0 g / cm 3 More preferably, it is 2.8 g / cm 3 or more and 3.6 g / cm 3 or less.
  • the thickness of the positive electrode active material layer (the sum of the thicknesses of both surfaces) is not particularly limited, and can be appropriately set according to desired characteristics. For example, it can be set thicker from the viewpoint of energy density, and can be set thinner from the viewpoint of output characteristics.
  • the thickness of the positive electrode active material layer (the sum of the thicknesses of both surfaces) can be appropriately set, for example, in the range of 20 ⁇ m or more and 500 ⁇ m or less, preferably 40 ⁇ m or more and 400 ⁇ m or less, more preferably 60 ⁇ m or more and 300 ⁇ m or less.
  • the thickness of the positive electrode active material layer (one-side thickness) is not particularly limited, and can be appropriately set according to desired characteristics.
  • the thickness (one-sided thickness) of the positive electrode active material layer can be appropriately set, for example, in the range of 10 ⁇ m to 250 ⁇ m, preferably 20 ⁇ m to 200 ⁇ m, and more preferably 30 ⁇ m to 150 ⁇ m.
  • the negative electrode can be appropriately selected from the negative electrodes that can be used in known lithium ion secondary batteries, depending on the application and the like.
  • the negative electrode active material used for the negative electrode can be appropriately set depending on the use and the like as long as it can be used for the negative electrode.
  • the negative electrode includes, for example, a negative electrode current collector layer and a negative electrode active material layer formed on the negative electrode current collector layer.
  • the negative electrode active material layer preferably contains, for example, a negative electrode active material and a binder resin, and further contains a conductive auxiliary from the viewpoint of increasing conductivity.
  • the negative electrode active material is not particularly limited as long as it is an active material for a negative electrode capable of inserting and extracting lithium ions, but a carbonaceous material can be used.
  • the carbonaceous material include graphite, amorphous carbon (for example, graphitizable carbon and non-graphitizable carbon), diamond-like carbon, fullerene, carbon nanotube, and carbon nanohorn.
  • graphite natural graphite and artificial graphite can be used, and in terms of material cost, inexpensive natural graphite is preferable.
  • the amorphous carbon include those obtained by heat-treating coal pitch coke, petroleum pitch coke, acetylene pitch coke, and the like.
  • a lithium metal material an alloy material such as silicon or tin, an oxide material such as Nb 2 O 5 or TiO 2 , or a composite thereof can be used.
  • the negative electrode active material only one kind may be used alone, or two or more kinds may be used in combination.
  • the average particle size of the negative electrode active material is preferably 2 ⁇ m or more, more preferably 5 ⁇ m or more, from the viewpoint of suppressing a side reaction during charge and discharge and suppressing a decrease in charge and discharge efficiency.
  • the thickness is preferably 40 ⁇ m or less, and more preferably 30 ⁇ m or less.
  • the average particle diameter means a particle diameter (median diameter: D 50 ) at an integrated value of 50% in a particle size distribution (volume basis) by a laser diffraction scattering method.
  • the negative electrode in the present embodiment can be manufactured by a known method.
  • a method in which a negative electrode active material and a binder resin are dispersed in a solvent to obtain a slurry, the slurry is applied to a negative electrode current collector layer, dried, and pressed as necessary to form a negative electrode active material layer can be adopted.
  • the method for applying the negative electrode slurry include a doctor blade method, a die coater method, and a dip coating method. If necessary, additives such as an antifoaming agent and a surfactant may be added to the slurry.
  • the content of the binder resin in the negative electrode active material layer is preferably 0.1 parts by mass or more and 10.0 parts by mass or less, when the whole of the negative electrode active material layer is 100 parts by mass, and is 0.5 part by mass. It is more preferably at least 8.0 parts by mass, more preferably at least 1.0 parts by mass and at most 5.0 parts by mass, particularly preferably at least 1.0 part by mass and at most 3.0 parts by mass. preferable.
  • the content of the binder resin is within the above range, the balance between the coating properties of the negative electrode slurry, the binding properties of the binder resin, and the battery characteristics is further improved.
  • the content of the binder resin is equal to or less than the above upper limit, the ratio of the negative electrode active material is increased, and the capacity per mass of the negative electrode is preferably increased. It is preferable that the content of the binder resin be equal to or more than the lower limit, because the electrode peeling is suppressed.
  • an organic solvent such as N-methyl-2-pyrrolidone (NMP) or water
  • NMP N-methyl-2-pyrrolidone
  • a binder resin for an organic solvent such as polyvinylidene fluoride (PVDF)
  • PVDF polyvinylidene fluoride
  • a rubber-based binder for example, SBR (styrene-butadiene rubber)
  • acrylic-based binder resin can be used.
  • Such an aqueous binder resin may be in the form of an emulsion.
  • water it is preferable to use an aqueous binder and a thickener such as CMC (carboxymethyl cellulose) in combination.
  • the negative electrode active material layer may contain a conductive aid as needed.
  • a conductive material generally used as a conductive aid for a negative electrode such as a carbonaceous material such as carbon black, Ketjen black, and acetylene black, can be used.
  • the content of the conductive additive in the negative electrode active material layer is preferably 0.1 part by mass or more and 3.0 parts by mass or less, when the whole of the negative electrode active material layer is 100 parts by mass, It is more preferable that the amount is from 2.0 parts by mass to 2.0 parts by mass, and particularly preferable is from 0.2 parts by mass to 1.0 parts by mass.
  • the content of the conductive assistant is within the above range, the balance between the coating properties of the negative electrode slurry, the binding properties of the binder resin, and the battery characteristics is further improved.
  • the content of the conductive auxiliary agent be equal to or less than the above upper limit, because the proportion of the negative electrode active material increases and the capacity per mass of the negative electrode increases. It is preferable that the content of the conductive auxiliary agent be equal to or more than the above lower limit, because the conductivity of the negative electrode is further improved.
  • the average particle size (primary particle size) of the conductive additive used in the positive electrode active material layer and the negative electrode active material layer is preferably in the range of 10 to 100 nm.
  • the average particle size (primary particle size) of the conductive additive is preferably 10 nm or more, more preferably 30 nm or more, and a sufficient number of contact points, from the viewpoint of suppressing excessive aggregation of the conductive additive and uniformly dispersing it in the negative electrode. Is preferably 100 nm or less, and more preferably 80 nm or less, from the viewpoint of forming a good conductive path.
  • the conductive additive When the conductive additive is in a fibrous form, examples thereof include those having an average diameter of 2 to 200 nm and an average fiber length of 0.1 to 20 ⁇ m.
  • the average particle diameter of the conductive additive is a median diameter (D 50 ), which means a particle diameter at an integrated value of 50% in a particle size distribution (volume basis) by a laser diffraction scattering method.
  • the thickness of the negative electrode active material layer (the sum of the thicknesses of both surfaces) is not particularly limited, and can be appropriately set according to desired characteristics. For example, it can be set thicker from the viewpoint of energy density, and can be set thinner from the viewpoint of output characteristics.
  • the thickness of the negative electrode active material layer (total thickness of both surfaces) can be appropriately set, for example, in the range of 40 ⁇ m or more and 1000 ⁇ m or less, preferably 80 ⁇ m or more and 800 ⁇ m or less, and more preferably 120 ⁇ m or more and 600 ⁇ m or less.
  • the thickness of the negative electrode active material layer (one-side thickness) is not particularly limited, and can be appropriately set according to desired characteristics.
  • the thickness of the negative electrode active material layer can be appropriately set, for example, in the range of 20 ⁇ m or more and 500 ⁇ m or less, preferably 40 ⁇ m or more and 400 ⁇ m or less, and more preferably 60 ⁇ m or more and 300 ⁇ m or less.
  • the density of the negative electrode active material layer is not particularly limited, but is preferably, for example, 1.2 g / cm 3 or more and 2.0 g / cm 3 or less, and is 1.3 g / cm 3 or more and 1.9 g / cm 3 or less. More preferably, it is 1.4 g / cm 3 or more and 1.8 g / cm 3 or less.
  • the negative electrode current collector layer copper, stainless steel, nickel, titanium, or an alloy thereof can be used.
  • the shape include a foil, a flat plate, and a mesh.
  • the thickness of the negative electrode current collector layer is not particularly limited, but is, for example, 1 ⁇ m or more and 20 ⁇ m or less.
  • the electrolytic solution according to the present embodiment is obtained by dissolving an electrolyte in a solvent.
  • the electrolytic solution used in the present embodiment is, for example, a non-aqueous electrolytic solution containing a lithium salt, and may be appropriately selected from known ones according to the type of the electrode active material and the use of the lithium ion secondary battery. it can.
  • lithium salt for example, LiClO 4, LiBF 6, LiPF 6, LiCF 3 SO 3, LiCF 3 CO 2, LiAsF 6, LiSbF 6, LiB 10 Cl 10, LiAlCl 4, LiCl, LiBr, LiB (C 2 H 5 ) 4 , CF 3 SO 3 Li, CH 3 SO 3 Li, LiC 4 F 9 SO 3 , Li (CF 3 SO 2 ) 2 N, lithium lower fatty acid carboxylate, and the like can be given.
  • the solvent for dissolving the lithium salt is not particularly limited as long as it is generally used as a liquid for dissolving the electrolyte.
  • the separator according to this embodiment is not particularly limited as long as it has a function of electrically insulating the positive electrode and the negative electrode and transmitting lithium ions.
  • a porous separator can be used.
  • the separator according to the present embodiment preferably includes a resin layer containing a heat-resistant resin as a main component.
  • the resin layer is formed of a heat-resistant resin as a main component.
  • the “main component” means that the proportion in the resin layer is 50% by mass or more, preferably 70% by mass or more, more preferably 90% by mass or more, and 100% by mass. Means that you may.
  • the resin layer constituting the separator according to this embodiment may be a single layer or two or more layers.
  • heat-resistant resin forming the resin layer examples include polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, poly-m-phenylene terephthalate, poly-p-phenylene isophthalate, polycarbonate, polyester carbonate, aliphatic polyamide, Aromatic polyamide, semi-aromatic polyamide, wholly aromatic polyester, polyphenylene sulfide, polyparaphenylene benzobisoxazole, polyimide, polyarylate, polyetherimide, polyamideimide, polyacetal, polyetheretherketone, polysulfone, polyethersulfone, One type or two or more types selected from a fluorine-based resin, polyether nitrile, modified polyphenylene ether, and the like can be given.
  • polyester resins such as polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate, wholly aromatic polyester, aliphatic polyamide, and wholly aromatic, from the viewpoint of excellent balance among heat resistance, mechanical strength, elasticity, and price.
  • polyamide resins such as aromatic polyamides and semi-aromatic polyamides
  • polyesters selected from polyethylene terephthalate, polybutylene terephthalate, polyethylene naphthalate and wholly aromatic polyester A system resin is more preferred, and polyethylene terephthalate is even more preferred.
  • the melting point of the separator according to this embodiment is preferably 220 ° C. or higher, more preferably 230 ° C. or higher, and more preferably 240 ° C. or higher, from the viewpoint of improving the safety of the lithium ion secondary battery. More preferred.
  • the separator according to the present embodiment preferably does not show a melting point, and preferably has a decomposition temperature of 220 ° C or higher, and 230 ° C or higher. Is more preferably 240 ° C. or higher, and particularly preferably 250 ° C. or higher.
  • the melting point or the decomposition temperature of the separator according to the present embodiment By setting the melting point or the decomposition temperature of the separator according to the present embodiment to the above lower limit or more, the battery generates heat, and even when the battery becomes hot, it is possible to suppress thermal contraction of the separator, and as a result, the positive electrode and the negative electrode Can be suppressed. Thereby, thermal runaway of the lithium ion secondary battery and the like can be suppressed, and safety can be further improved.
  • the upper limit of the melting point of the separator according to this embodiment is not particularly limited, but is, for example, 500 ° C. or less, and preferably 400 ° C. or less from the viewpoint of elasticity.
  • the upper limit of the decomposition temperature of the separator according to this embodiment is not particularly limited, but is, for example, 500 ° C. or less, and preferably 400 ° C. or less from the viewpoint of elasticity.
  • the resin layer constituting the separator according to the present embodiment is preferably a porous resin layer.
  • the porosity of the porous resin layer is preferably from 20% to 80%, more preferably from 30% to 70%, and more preferably from 40% to 60%, from the viewpoint of balance between mechanical strength and lithium ion conductivity. Is particularly preferred.
  • ⁇ porosity (%)
  • Ws basis weight (g / m 2 )
  • ds true density (g / cm 3 )
  • t film thickness ( ⁇ m).
  • the planar shape of the separator according to this embodiment is not particularly limited, and can be appropriately selected according to the shape of the electrode or the current collector, and may be, for example, a rectangle.
  • the thickness of the separator according to the present embodiment is preferably 5 ⁇ m or more and 50 ⁇ m or less, more preferably 10 ⁇ m or more and 40 ⁇ m or less, and still more preferably 10 ⁇ m or more and 30 ⁇ m or less, from the viewpoint of balance between mechanical strength and lithium ion conductivity. It is.
  • the separator according to the embodiment further includes a ceramic layer on at least one surface of the resin layer from the viewpoint of further improving heat resistance.
  • the ceramic layer is preferably provided only on one surface of the resin layer from the viewpoint of handleability of the separator according to the present embodiment and productivity, but further improves the heat resistance of the separator. From the viewpoint of causing the resin layer to be provided, the resin layer may be provided on both surfaces. Since the separator according to the present embodiment further includes the ceramic layer, the heat shrinkage of the separator can be further reduced, and the short circuit between the electrodes can be further prevented.
  • the ceramic layer can be formed, for example, by applying and drying a ceramic layer forming material on the resin layer.
  • a ceramic layer forming material for example, a material obtained by dissolving or dispersing an inorganic filler and a binder resin in an appropriate solvent can be used.
  • the inorganic filler used for the ceramic layer can be appropriately selected from known materials used for a separator of a lithium ion secondary battery.
  • highly insulating oxides, nitrides, sulfides, carbides, and the like are preferable, and are selected from aluminum oxide, boehmite, titanium oxide, silicon oxide, magnesium oxide, barium oxide, zirconium oxide, zinc oxide, iron oxide, and the like. More preferably, one or two or more types of ceramics are adjusted to particles.
  • aluminum oxide, boehmite and titanium oxide are preferred.
  • the binder resin is not particularly limited, and examples thereof include a cellulosic resin such as carboxymethylcellulose (CMC); an acrylic resin; and a fluororesin such as polyvinylidene fluoride (PVDF).
  • a cellulosic resin such as carboxymethylcellulose (CMC); an acrylic resin; and a fluororesin such as polyvinylidene fluoride (PVDF).
  • PVDF polyvinylidene fluoride
  • the binder resin only one kind may be used alone, or two or more kinds may be used in combination.
  • the solvent for dissolving or dispersing these components is not particularly limited, and is appropriately selected from, for example, water, alcohols such as ethanol, N-methylpyrrolidone (NMP), toluene, dimethyl carbonate (DMC), and ethyl methyl carbonate (EMC). Can be used.
  • alcohols such as ethanol, N-methylpyrrolidone (NMP), toluene, dimethyl carbonate (DMC), and ethyl methyl carbonate (EMC).
  • NMP N-methylpyrrolidone
  • DMC dimethyl carbonate
  • EMC ethyl methyl carbonate
  • the thickness of the ceramic layer is preferably 0.1 ⁇ m or more and 50 ⁇ m or less, more preferably 0.5 ⁇ m or more and 30 ⁇ m or less, from the viewpoint of the balance between heat resistance, mechanical strength, handleability, and lithium ion conductivity. Preferably it is 1 ⁇ m or more and 15 ⁇ m or less.
  • the electrolyte layer is a layer disposed so as to be interposed between the positive electrode and the negative electrode.
  • the electrolyte layer contains a separator and an electrolyte, and examples thereof include a porous separator in which a non-aqueous electrolyte is impregnated.
  • the exterior body according to the present embodiment has, for example, a substantially rectangular planar shape.
  • the exterior body according to the present embodiment includes, for example, a housing portion for housing the battery body, and a joint portion in which the heat-fusible resin layers located on the peripheral edge of the housing portion are directly or via electrode terminals.
  • the exterior body according to the present embodiment has at least a heat-fusible resin layer and a barrier layer, and is capable of enclosing the battery body therein.
  • a laminated film having at least a heat-fusible resin layer and a barrier layer may be selected from those having a barrier property such as preventing leakage of electrolyte and intrusion of moisture from the outside.
  • stainless steel (SUS) foil, aluminum foil, aluminum alloy foil, copper foil, titanium foil A barrier layer made of a metal such as a foil can be used.
  • the thickness of the barrier layer is, for example, 10 ⁇ m or more and 100 ⁇ m or less, preferably 20 ⁇ m or more and 80 ⁇ m or less, and more preferably 30 ⁇ m or more and 50 ⁇ m or less.
  • the resin material constituting the heat-fusible resin layer is not particularly limited, for example, polyethylene, polypropylene, nylon, polyethylene terephthalate (PET) and the like can be used.
  • the thickness of the heat-fusible resin layer is, for example, 20 ⁇ m or more and 200 ⁇ m or less, preferably 30 ⁇ m or more and 150 ⁇ m or less, and more preferably 50 ⁇ m or more and 100 ⁇ m or less.
  • the heat-fusible resin layer and the barrier layer of the laminated film according to the present embodiment are not limited to one layer each, and may be two or more layers.
  • the exterior body can be formed by causing the heat-fusible resin layers to face each other with the battery body interposed therebetween and heat-sealing the periphery of the portion housing the battery body.
  • a resin layer such as a nylon film or a polyester film can be provided on the outer surface of the exterior body, which is the surface opposite to the surface on which the heat-fusible resin layer is formed.
  • the heating temperature at the time of performing heat fusion between the heat-fusible resin layers depends on the melting point of the resin material constituting the heat-fusible resin layer. In this case, the temperature is preferably from 140 ° C. to 185 ° C., and more preferably from 150 ° C. to 180 ° C. In addition, the heat sealing time when performing heat fusion between the heat-fusible resin layers is, for example, 10 seconds to 50 seconds, preferably 12 seconds to 30 seconds.
  • Electrode terminal In the present embodiment, known members can be used for the pair of electrode terminals 30 (the positive electrode terminal and the negative electrode terminal).
  • the positive electrode terminal for example, one made of aluminum or an aluminum alloy can be used
  • the negative electrode terminal for example, copper or a copper alloy or one obtained by plating them with nickel can be used.
  • Each terminal is drawn out of the container, and a heat-fusible resin layer is provided in advance at a portion of each terminal located at a portion where the periphery of the outer package is thermally welded.
  • the positive electrode terminal and the negative electrode terminal are drawn from the same side of the package, but the positive terminal and the negative terminal may be drawn from different sides of the package.
  • Example 1 ⁇ Preparation of positive electrode> 93.9 parts by mass of a lithium nickel-containing composite oxide (chemical formula: LiNi 0.8 Co 0.15 Al 0.05 O 2 , average particle size: 6 ⁇ m) as a positive electrode active material, and carbon black as a conductive auxiliary agent. 0 parts by mass, 3.0 parts by mass of polyvinylidene fluoride (PVDF) as a binder resin, and 0.1 parts by mass of oxalic anhydride as an additive were used. These were dispersed in an organic solvent to prepare a positive electrode slurry.
  • PVDF polyvinylidene fluoride
  • This positive electrode slurry is continuously applied to a 15 ⁇ m-thick aluminum foil (tensile elongation: 6%), which is a positive electrode current collector, dried, and then pressed to form a coated portion of the positive electrode current collector (positive electrode).
  • An active material layer a positive electrode roll having a thickness of 60 ⁇ m on one side, a density of 3.35 g / cm 3 ) and an uncoated portion not coated was prepared. This positive electrode roll was punched out so that an uncoated portion serving as a tab for connecting to the positive electrode terminal was left, thereby forming a positive electrode.
  • An active material layer a negative electrode roll having a thickness of 90 ⁇ m on one side, a density of 1.55 g / cm 3 ) and an uncoated portion not coated was prepared. This negative electrode roll was punched out such that an uncoated portion serving as a tab for connecting to the negative electrode terminal was left to form a negative electrode.
  • a positive electrode and a negative electrode were laminated in a zigzag structure with a separator interposed therebetween, and a negative electrode terminal and a positive electrode terminal were provided thereon, thereby obtaining a laminate.
  • an electrolyte solution in which 1M LiPF 6 was dissolved in a solvent composed of ethylene carbonate, diethyl carbonate, and ethyl methyl carbonate, and the obtained laminate were accommodated in a flexible film, thereby forming a laminate type laminated battery. Obtained.
  • the rated capacity of this laminated battery was 9.2 Ah, the positive electrode had 28 layers, and the negative electrode had 29 layers.
  • a separator 1 (thickness: 25 ⁇ m, porosity: 56%, resin layer melting point: 250 ° C.) including a porous resin layer made of polyethylene terephthalate (PET) and a ceramic layer made of boehmite particles was used. . Further, the average length L 4 and the length L 2 of the outermost negative electrode of the separator was adjusted to a value shown in Table 1.
  • ⁇ porosity (%)
  • Ws basis weight (g / m 2 )
  • ds true density (g / cm 3 )
  • t film thickness ( ⁇ m).
  • the obtained lithium ion secondary battery was subjected to a constant current constant voltage (CC-CV) method at 25 ° C. and a constant current of 0.2 C.
  • the battery was charged at a constant current up to 2 V, then charged at a constant voltage of 4.2 V at a constant voltage up to a charge termination current of 0.015 C, and then subjected to CC discharge at a discharge rate of 0.2 C and a discharge termination voltage of 2.5 V.
  • the lithium ion secondary battery after the first charge / discharge was allowed to stand at 45 ° C. for 168 hours to perform an aging treatment.
  • the obtained lithium ion secondary battery was disassembled, the deterioration of the outermost layer separator was visually observed, and each was evaluated according to the following criteria.
  • ⁇ No discolored portion is observed on the outermost layer of the separator surface. :: One or two discolored portions having a diameter of about 1 to 5 mm are observed, but deterioration of the entire separator is suppressed. :: Length One or two light brown discolored portions having a size of 5 mm to 20 mm and a width of about 1 to 5 mm are observed, but deterioration of the entire separator is suppressed.
  • ⁇ Light brown discolored portion over the entire outermost layer separator surface Are observed, but deterioration is suppressed in the entire separator.
  • ⁇ A dark brown discolored portion is observed over the entire outermost surface of the separator, and the entire separator is deteriorated.
  • Example 1 (Examples 2 to 4 and Comparative Example 1) L 2 and L 4 was replaced with the values shown in Table 1 were prepared with different lithium ion secondary battery in the same manner as in Example 1, was subjected to the same evaluation as in Example 1, respectively. Table 1 shows the obtained evaluation results.

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Abstract

La batterie secondaire au lithium-ion (100) selon l'invention comprend : un corps principal de batterie (10) comprenant au moins un élément de génération d'énergie comprenant au moins des électrodes positives (15), un électrolyte, un séparateur (18) et des électrodes négatives (20) ; un boîtier externe (40), à l'intérieur duquel le corps principal de batterie (10) est inséré ; et une paire de bornes d'électrode (30), connectées électriquement au corps principal de batterie (10) et dont au moins une partie est apparente à l'extérieur du boîtier (40). Le corps principal de batterie (10) comporte : une structure permettant d'agencer chacune des électrodes positives (15) et des électrodes négatives (20) entre les plis d'un séparateur (18) plié en zigzag ; une membrane (25) d'interface d'électrolyte solide (SEI), formée dans au moins une section périphérique (20B) d'une surface d'une électrode négative (20A) se situant le plus à l'extérieur sur un côté ne faisant pas face aux électrodes positives (15), ladite électrode négative la plus extérieure étant positionnée le plus à l'extérieur parmi les électrodes comprenant les électrodes positives (15) et les électrodes négatives (20) dans le corps principal de batterie (10) ; et la longueur L1 de la membrane SEI (25) sur l'électrode négative la plus extérieure (20A) et la longueur L2 du séparateur sur l'électrode négative la plus extérieure (20A) satisfont la relation L1 ≥ L2 > 0.
PCT/JP2019/020847 2018-06-29 2019-05-27 Batterie secondaire au lithium-ion WO2020003846A1 (fr)

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