WO2021172444A1 - リチウムイオン電池 - Google Patents

リチウムイオン電池 Download PDF

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Publication number
WO2021172444A1
WO2021172444A1 PCT/JP2021/007142 JP2021007142W WO2021172444A1 WO 2021172444 A1 WO2021172444 A1 WO 2021172444A1 JP 2021007142 W JP2021007142 W JP 2021007142W WO 2021172444 A1 WO2021172444 A1 WO 2021172444A1
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Prior art keywords
negative electrode
active material
positive electrode
electrode active
mixture layer
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Ceased
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PCT/JP2021/007142
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English (en)
French (fr)
Japanese (ja)
Inventor
和子 浅野
雪尋 沖
菜々美 竹田
日比野　光宏
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Panasonic Intellectual Property Management Co Ltd
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Panasonic Intellectual Property Management Co Ltd
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Priority to US17/800,768 priority Critical patent/US20230100030A1/en
Priority to CN202180013827.4A priority patent/CN115088102A/zh
Priority to JP2022503700A priority patent/JP7720569B2/ja
Publication of WO2021172444A1 publication Critical patent/WO2021172444A1/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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
    • H01M4/387—Tin or alloys based on tin
    • 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
    • H01M2004/026—Electrodes composed of, or comprising, active material characterised by the polarity
    • H01M2004/027—Negative electrodes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Definitions

  • a positive electrode having a positive electrode mixture layer containing a positive electrode active material, a negative electrode having a negative electrode mixture layer containing a negative electrode active material, and charging / discharging are performed by moving lithium ions between the positive electrode and the negative electrode.
  • a positive electrode having a positive electrode mixture layer containing a positive electrode active material, a negative electrode having a negative electrode mixture layer containing a negative electrode active material, and charging / discharging are performed by moving lithium ions between the positive electrode and the negative electrode.
  • lithium-ion batteries Regarding lithium-ion batteries.
  • Lithium-ion batteries in which charging and discharging are performed by moving lithium ions (Li ions) between the negative electrode and the positive electrode, are widely used.
  • a graphite-based material is often used as the negative electrode active material of the negative electrode mixture layer in this lithium ion battery.
  • the graphite-based negative electrode active material may be used together with Si, in which case the volume change during charging and discharging is large, the capacity retention characteristics are likely to deteriorate, and the cost is relatively high.
  • Patent Document 1 describes that an alloy having a La 3 Co 2 Sn 7 type crystal structure is used as the negative electrode active material.
  • a secondary battery using an intermetallic compound having a La 3 Ni 2 Sn 7 type crystal structure as a negative electrode active material tends to have a relatively low mass energy density.
  • lithium ions move between a positive electrode having a positive electrode mixture layer containing a positive electrode active material, a negative electrode having a negative electrode mixture layer containing a negative electrode active material, and the positive electrode and the negative electrode.
  • the negative electrode mixture layer is a lithium ion battery charged and discharged by the general formula La 3 (1-x) M 3x Ni 2 (1-y) Me 2y X 7 (M is Ca, Mg, Sr). , Me contains at least one of Mn, Co, Cu, Fe, and X contains at least one of Ge, Si, Sn, Al). 0.1 ⁇ x ⁇ 0.5 and 0 ⁇ y ⁇ 1.
  • the negative electrode active material in the negative electrode active material represented by the general formula La 3 (1-x) M 3x Ni 2 (1-y) Me 2y X 7, a part of La sites is Ca, Mg,
  • the charge / discharge capacity can be increased by substituting at least one of Sr and a part of the Ni site with at least one of Mn, Co, Cu, and Fe.
  • FIG. 1 is a vertical cross-sectional view of a cylindrical secondary battery 10 which is an example of an embodiment.
  • FIG. 2 is a graph showing the electrode potentials of Examples 1 to 5 and Comparative Example 1 during charging and discharging.
  • the negative electrode material of the lithium ion battery is preferably a material that satisfies high energy density and low expansion. Therefore, various researches and developments have been carried out, and it has been proposed to use an intermetallic compound having a La 3 Ni 2 Sn 7 type crystal structure as a negative electrode active material. Since such an intermetallic compound occludes and releases Li by an intercalation reaction, it is considered that the expansion rate is low and the life can be extended.
  • the intermetallic compound having a La 3 Ni 2 Sn 7 type crystal structure has a relatively low mass energy density as compared with the graphite type.
  • the La site of the La 3 Ni 2 Sn 7 type crystal structure is partially replaced with at least one of Ca, Mg, Sr, and a part of the Ni site is Mn, Co, Replace with at least one of Cu and Fe.
  • vacancies are likely to occur, and the number of sites that can occlude Li increases, which is thought to increase the charge / discharge capacity.
  • FIG. 1 is a vertical cross-sectional view of a cylindrical secondary battery 10 which is an example of an embodiment.
  • the electrode body 14 and the non-aqueous electrolyte are housed in the exterior body 15.
  • the electrode body 14 has a winding structure in which the positive electrode 11 and the negative electrode 12 are wound around the separator 13.
  • the non-aqueous solvent (organic solvent) of the non-aqueous electrolyte carbonates, lactones, ethers, ketones, esters and the like can be used, and two or more of these solvents can be mixed and used. ..
  • a mixed solvent containing a cyclic carbonate and a chain carbonate For example, ethylene carbonate (EC), propylene carbonate (PC), butylene carbonate (BC) and the like can be used as the cyclic carbonate, and dimethyl carbonate (DMC), ethyl methyl carbonate (EMC), and diethyl carbonate (diethyl carbonate) (as the chain carbonate). DEC) and the like can be used.
  • DEC dimethyl carbonate
  • EMC ethyl methyl carbonate
  • diethyl carbonate diethyl carbonate
  • electrolyte salt of the non-aqueous electrolyte LiPF 6 , LiBF 4 , LiCF 3 SO 3, etc. and a mixture thereof can be used.
  • the amount of the electrolyte salt dissolved in the non-aqueous solvent can be, for example, 0.5 to 2.0 mol / L.
  • the sealing body 16 side will be referred to as “top” and the bottom side of the exterior body 15 will be referred to as “bottom”.
  • the inside of the secondary battery 10 is sealed by closing the opening end of the exterior body 15 with the sealing body 16.
  • Insulating plates 17 and 18 are provided above and below the electrode body 14, respectively.
  • the positive electrode lead 19 extends upward through the through hole of the insulating plate 17 and is welded to the lower surface of the filter 22 which is the bottom plate of the sealing body 16.
  • the cap 26, which is the top plate of the sealing body 16 electrically connected to the filter 22, serves as the positive electrode terminal.
  • the negative electrode lead 20 extends to the bottom side of the exterior body 15 through the through hole of the insulating plate 18 and is welded to the inner surface of the bottom portion of the exterior body 15.
  • the exterior body 15 serves as a negative electrode terminal.
  • the negative electrode lead 20 passes through the outside of the insulating plate 18 and extends to the bottom side of the exterior body 15 and is welded to the inner surface of the bottom portion of the exterior body 15.
  • the exterior body 15 is, for example, a bottomed cylindrical metal exterior can.
  • a gasket 27 is provided between the exterior body 15 and the sealing body 16 to ensure the internal airtightness of the secondary battery 10.
  • the exterior body 15 has a grooved portion 21 that supports the sealing body 16 and is formed by pressing, for example, a side surface portion from the outside.
  • the grooved portion 21 is preferably formed in an annular shape along the circumferential direction of the exterior body 15, and the sealing body 16 is supported on the upper surface thereof via the gasket 27.
  • the sealing body 16 has a filter 22, a lower valve body 23, an insulating member 24, an upper valve body 25, and a cap 26, which are laminated in order from the electrode body 14 side.
  • Each member constituting the sealing body 16 has, for example, a disk shape or a ring shape, and each member except the insulating member 24 is electrically connected to each other.
  • the lower valve body 23 and the upper valve body 25 are connected to each other at their central portions, and an insulating member 24 is interposed between the peripheral portions thereof.
  • the positive electrode 11, the negative electrode 12, and the separator 13 constituting the electrode body 14 will be described, and in particular, the negative electrode active material constituting the negative electrode 12 will be described.
  • the positive electrode 11 has a positive electrode core body and a positive electrode mixture layer provided on the surface of the positive electrode core body.
  • a metal foil stable in the potential range of the positive electrode 11 such as aluminum, a film in which the metal is arranged on the surface layer, or the like can be used.
  • the thickness of the positive electrode core is, for example, 10 ⁇ m to 30 ⁇ m.
  • the positive electrode mixture layer contains a positive electrode active material, a binder, and a conductive material, and is preferably provided on both sides of the positive electrode core body excluding the portion to which the positive electrode lead 19 is connected.
  • a positive electrode mixture slurry containing a positive electrode active material, a binder, a conductive material, and the like is applied to the surface of a positive electrode core, the coating film is dried, and then compressed to form a positive electrode mixture layer. It can be manufactured by forming it on both sides of the core body.
  • the positive electrode active material contains lithium transition metal oxide as a main component.
  • the positive electrode active material may be substantially composed of only lithium transition metal oxide, and is one in which inorganic compound particles such as aluminum oxide and lanthanoid-containing compound are adhered to the particle surface of the lithium transition metal oxide. May be good.
  • One type of lithium transition metal oxide may be used, or two or more types may be used in combination.
  • Metal elements contained in the lithium transition metal oxide include nickel (Ni), cobalt (Co), manganese (Mn), aluminum (Al), boron (B), magnesium (Mg), titanium (Ti), and vanadium.
  • V Chromium (Cr), Iron (Fe), Copper (Cu), Zinc (Zn), Gallium (Ga), Strontium (Sr), Zirconium (Zr), Niobium (Nb), Indium (In), Tin (Sn), tantalum (Ta), tungsten (W) and the like can be mentioned.
  • lithium transition metal oxide is the general formula: Li ⁇ Ni x M (1-x) O 2 (0.1 ⁇ ⁇ ⁇ 1.2, 0.3 ⁇ x ⁇ 1, where M is Co, Mn. , Containing at least one of Al).
  • M is Co, Mn. , Containing at least one of Al.
  • NCA in which a part of nickel is replaced with cobalt and aluminum is added is used.
  • Examples of the conductive material contained in the positive electrode mixture layer include carbon materials such as carbon black, acetylene black, ketjen black, carbon nanotubes, carbon nanofibers, and graphite.
  • Examples of the binder contained in the positive electrode mixture layer include fluororesins such as polytetrafluoroethylene (PTFE) and polyvinylidene fluoride (PVDF), polyacrylonitrile (PAN), polyimide resins, acrylic resins, and polyolefin resins. .. These resins may be used in combination with cellulose derivatives such as carboxymethyl cellulose (CMC) or salts thereof, polyethylene oxide (PEO) and the like.
  • the negative electrode 12 has a negative electrode core body and a negative electrode mixture layer provided on the surface of the negative electrode core body.
  • a metal foil stable in the potential range of the negative electrode 12 such as copper, a film in which the metal is arranged on the surface layer, or the like can be used.
  • the thickness of the negative electrode core is, for example, 5 ⁇ m to 15 ⁇ m.
  • the negative electrode mixture layer contains a negative electrode active material and a binder, and is preferably provided on both sides of the negative electrode core body excluding the portion to which the negative electrode lead 20 is connected, for example.
  • a negative electrode mixture slurry containing a negative electrode active material and a binder is applied to the surface of the negative electrode core body, the coating film is dried, and then compressed to form a negative electrode mixture layer on both sides of the negative electrode core body. It can be produced by forming in. Further, a conductive material may be added to the negative electrode mixture slurry. The conductive material can make the conductive path uniform. Further, the negative electrode mixture layer may contain a conductive material such as acetylene black, similarly to the positive electrode mixture layer.
  • At least one of the general formula La 3 (1-x) M 3x Ni 2 (1-y) Me 2y X 7 (M is La, Ca, Mg, Sr) is used as the negative electrode active material.
  • Me contains at least one of Mn, Co, Cu and Fe, and
  • X contains at least one of Ge, Si, Sn and Al).
  • the particle size of La 3 (1-x) M 3x Ni 2 (1-y) Me 2y X 7 which is the negative electrode active material, is preferably 1 to 30 ⁇ m, more preferably 2 to 20 ⁇ m, and particularly preferably 2 to 10 ⁇ m. If the particle size of the negative electrode active material becomes too large, the reactivity with Li decreases, the contact area between the particles becomes small, and the resistance increases. On the other hand, if the particle size becomes too small, it is assumed that the packing density of the negative electrode active material decreases and the capacity decreases.
  • the average particle size of the negative electrode active material is, for example, 3 to 15 ⁇ m or 5 to 10 ⁇ m.
  • the particle size of the negative electrode active material is measured as the diameter of the circumscribed circle of the negative electrode active material particles in the cross-sectional image of the negative electrode mixture layer observed by a scanning electron microscope (SEM).
  • SEM scanning electron microscope
  • the average particle size is calculated by averaging the particle sizes of 100 arbitrary particles.
  • the intermetallic compound represented by La 3 (1-x) M 3x Ni 2 (1-y) Me 2y X 7 can be formed by arc melting, and it is preferable to anneal after arc melting.
  • the substitution rates for La and Ni are preferably 0.1 ⁇ x ⁇ 0.5 and 0 ⁇ y ⁇ 1. It is presumed that if the substitution rate is low, the effect is small, and if the substitution rate is large, impurities are generated, and the irreversible capacitance increases due to the alloying reaction. Further, La is preferably replaced with Ca, and Ni is preferably replaced with Mn. Further, good results have been obtained when X uses Sn.
  • the negative electrode active material contains La 3 (1-x) M 3x Ni 2 (1-y) Me 2y X 7 as a main component (the component having the highest mass ratio), and is substantially La 3 (1-x) M. It may be composed of only 3 x Ni 2 (1-y) Me 2y X 7.
  • the negative electrode active material includes a metal compound other than La 3 (1-x) M 3x Ni 2 (1-y) Me 2y X 7 , a carbon-based active material such as graphite, or a Si-based active material containing Si.
  • Other active substances may be used in combination. For example, when graphite is used in combination, the content of graphite may be 50 to 90% by mass with respect to the mass of the negative electrode active material.
  • binders can be used as the binder contained in the negative electrode mixture layer, and for example, a compound containing a cyano group is used.
  • a binder such as polyvinylidene fluoride (PVDF), which is commonly used, is used. If it is used, the negative electrode mixture slurry will gel and it will be difficult to apply the slurry.
  • PVDF polyvinylidene fluoride
  • binder containing a cyano group examples include polyacrylonitrile (PAN), polymethacrylonitrile, poly- ⁇ -chloroacrylonitrile, poly- ⁇ -ethylacrylonitrile, and the like. Among them, PAN or polymethaclonitrile is preferable, and PAN is particularly preferable.
  • the binder containing a cyano group is a solvent system, and it is necessary to use a solvent for coating.
  • a solvent for coating There is a demand to use an aqueous binder, and for example, carboxymethyl cellulose (CMC) can be used.
  • CMC carboxymethyl cellulose
  • NH 4-CMC ammonium carboxymethylcellulose
  • the mass ratio of the binder in the negative electrode mixture layer is preferably about 0.5% by mass to 7.0% by mass.
  • a porous sheet having ion permeability and insulating property is used as the separator 13.
  • the porous sheet include a microporous membrane, a woven fabric, a non-woven fabric and the like.
  • olefin resin such as polyethylene and polypropylene, cellulose and the like are suitable.
  • the separator 13 may have either a single-layer structure or a laminated structure.
  • a heat-resistant layer containing a heat-resistant material may be formed on the surface of the separator 13. Examples of the heat-resistant material include polyamide resins such as aliphatic polyamides and aromatic polyamides (aramid), and polyimide resins such as polyamideimide and polyimide.
  • an intermetallic compound La 3 (1-x) M 3x Ni 2 (1-y) Me 2y X 7 ) having a particle size of 2 to 20 ⁇ m and a La 2 Ni 2 Sn 7 type crystal structure is used.
  • NH 4- CMC and SBR (denoted as CMC / SBR) were used as the coating agent, and artificial graphite powder was used as the conductive material.
  • the negative electrode active material, the binder, and the conductive material are mixed at a mass ratio of 85.5: 3: 1.5: 10, and N-methyl-2-pyrrolidone (NMP) is used as a dispersion medium.
  • Negative electrode mixture slurry was prepared. Next, a negative electrode mixture slurry was applied onto a negative electrode core made of copper foil, the coating film was dried and compressed, and then cut to a predetermined electrode size to obtain a negative electrode.
  • the negative electrode and the positive electrode made of lithium metal foil were arranged to face each other via a separator to form an electrode body, and the electrode body was housed in a coin-shaped outer can. After injecting a predetermined non-aqueous electrolyte solution into the outer can, the outer can was sealed to obtain a coin-shaped test cell (non-aqueous electrolyte secondary battery).
  • Example 4 As the negative electrode active material, La 1.8 Ca 0.2 Ni 1.8 Cu 0.2 Sn 7 was used.
  • Comparative Example 3-6 the effect of Ca substitution was investigated by using La 3 (1-x) Ca 3 x Ni 2 Sn 7 and changing the Ca substitution rate x. Specifically, Comparative Example 3 had a Ca substitution amount of 0%, Comparative Example 4 had a Ca substitution amount of 10%, Comparative Example 5 had a Ca substitution amount of 40%, and Comparative Example 6 had a Ca substitution amount of 50%.
  • FIG. 2 is a diagram showing positive and negative electrode potentials in the charge / discharge tests of Examples 1-4 and Comparative Example 1-2, and Table 1 shows these charge / discharge capacities.
  • Example 1-4 the charge / discharge capacity is greatly (twice or more) increased as compared with Comparative Example 1. Further, in Comparative Example 2, the charge / discharge capacity is larger than that in Comparative Example 1, but the capacity is smaller than that in Example 1-4. Further, it can be seen that the Ni site of Example 1 replaced with Mn has a particularly large capacity. As described above, it was found that in addition to the substitution of La site, the substitution of Ni site with another 3d metal element improves the storage amount of Li and increases the charge / discharge capacity.
  • Table 2 shows the initial discharge capacity and efficiency of Comparative Example 3-6. Efficiency is the value obtained by dividing the initial discharge capacity by the initial charge capacity.
  • the charge / discharge capacity increases by substituting Ca for La.
  • the charge / discharge capacity increases at 10% to 40% of Ca substitution, and the charge / discharge capacity decreases at 50%.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Materials Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Secondary Cells (AREA)
PCT/JP2021/007142 2020-02-28 2021-02-25 リチウムイオン電池 Ceased WO2021172444A1 (ja)

Priority Applications (3)

Application Number Priority Date Filing Date Title
US17/800,768 US20230100030A1 (en) 2020-02-28 2021-02-25 Lithium ion battery
CN202180013827.4A CN115088102A (zh) 2020-02-28 2021-02-25 锂离子电池
JP2022503700A JP7720569B2 (ja) 2020-02-28 2021-02-25 リチウムイオン電池

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JP2020033553 2020-02-28
JP2020-033553 2020-02-28

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JPWO2021200924A1 (https=) * 2020-04-02 2021-10-07

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US20130236781A1 (en) * 2012-03-06 2013-09-12 Semiconductor Energy Laboratory Co., Ltd. Negative electrode for secondary battery and secondary battery

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JP2007073215A (ja) * 2005-09-05 2007-03-22 Toshiba Corp 非水電解質電池

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MATSUNO SHINSUKE, KOHNO TATSUOKI, TAKAMI NORIO, KAWASHIMA FUMIYUKI, SAWA TAKAO: "La[sub 3]Ni[sub 2]Sn[sub 7] Ternary Intermetallic Phase for Lithium Insertion and Deinsertion", ELECTROCHEMICAL AND SOLID-STATE LETTERS, IEEE SERVICE CENTER, PISCATAWAY, NJ., US, vol. 8, no. 4, 1 January 2005 (2005-01-01), US, pages A234, XP055850603, ISSN: 1099-0062, DOI: 10.1149/1.1870692 *
MATSUNO, SHINSUKE: "Electrochemical lithium insertion for La3Ni2Sn7 intermetallic compounds", LECTURE ABSTRACTS OF THE 46TH BATTERY SYMPOSIUM IN JAPAN, vol. 46, 30 November 2004 (2004-11-30) - 18 November 2005 (2005-11-18), pages 220 - 221, XP009530794 *

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPWO2021200924A1 (https=) * 2020-04-02 2021-10-07
EP4131478A4 (en) * 2020-04-02 2023-09-27 Panasonic Intellectual Property Management Co., Ltd. Lithium ion battery
JP7599138B2 (ja) 2020-04-02 2024-12-13 パナソニックＩｐマネジメント株式会社 リチウムイオン電池
US12580187B2 (en) 2020-04-02 2026-03-17 Panasonic Intellectual Property Management Co., Ltd. Lithium ion battery

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US20230100030A1 (en) 2023-03-30
CN115088102A (zh) 2022-09-20
JPWO2021172444A1 (https=) 2021-09-02
JP7720569B2 (ja) 2025-08-08

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