WO2020261757A1 - 正極材料、および、電池 - Google Patents

正極材料、および、電池 Download PDF

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Publication number
WO2020261757A1
WO2020261757A1 PCT/JP2020/018121 JP2020018121W WO2020261757A1 WO 2020261757 A1 WO2020261757 A1 WO 2020261757A1 JP 2020018121 W JP2020018121 W JP 2020018121W WO 2020261757 A1 WO2020261757 A1 WO 2020261757A1
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WIPO (PCT)
Prior art keywords
positive electrode
solid electrolyte
active material
electrode active
battery
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Ceased
Application number
PCT/JP2020/018121
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English (en)
French (fr)
Japanese (ja)
Inventor
出 佐々木
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Panasonic Intellectual Property Management Co Ltd
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Panasonic Intellectual Property Management Co Ltd
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Filing date
Publication date
Application filed by Panasonic Intellectual Property Management Co Ltd filed Critical Panasonic Intellectual Property Management Co Ltd
Priority to EP20830569.8A priority Critical patent/EP3993093A4/en
Priority to JP2021527428A priority patent/JP7507385B2/ja
Priority to CN202080018871.XA priority patent/CN113614948B/zh
Publication of WO2020261757A1 publication Critical patent/WO2020261757A1/ja
Priority to US17/506,720 priority patent/US12224430B2/en
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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01F—COMPOUNDS OF THE METALS BERYLLIUM, MAGNESIUM, ALUMINIUM, CALCIUM, STRONTIUM, BARIUM, RADIUM, THORIUM, OR OF THE RARE-EARTH METALS
    • C01F17/00—Compounds of rare earth metals
    • 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
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
    • H01M10/0562—Solid materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/13—Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
    • H01M4/131—Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
    • 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
    • H01M4/362—Composites
    • H01M4/366—Composites as layered products
    • 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
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/62—Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
    • 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
    • H01M2004/028—Positive electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • H01M2300/008—Halides
    • 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

Definitions

  • Patent Document 2 discloses an all-solid-state lithium battery containing a lithium ion conductive solid electrolyte containing sulfide and an active material whose surface is coated with a lithium ion conductive oxide.
  • FIG. 1 is a cross-sectional view showing a schematic configuration of a positive electrode material according to the first embodiment.
  • FIG. 2 is a cross-sectional view showing a schematic configuration of the battery according to the second embodiment.
  • FIG. 3 is a graph showing the initial charge / discharge efficiency of the batteries of Examples 1 to 4 and Comparative Examples 1 to 3.
  • the coverage of the coating material on the surface of the positive electrode active material is 91.1% or more. There may be.
  • the present inventors have found that in a battery containing a halide solid electrolyte in the positive electrode material, the effect of improving the charge / discharge efficiency by the coating material containing lithium carbonate is higher than the effect of the coating material containing lithium niobate. I found it to be significantly higher. That is, the present inventors have found that the coating material that exerts a remarkable effect differs depending on the type of solid electrolyte. The principle is not clear. However, various factors such as the withstand voltage of the coating material, the withstand voltage of the lithium ion conductive solid electrolyte, the reactivity of the coating material with the active material, and the reactivity of the coating material with the solid electrolyte are involved in a complex manner. It is thought that there is.
  • the ionic conductivity of the solid electrolyte can be further improved.
  • the charge / discharge efficiency of the battery can be further improved.
  • the first solid electrolyte may be represented by the following composition formula (A1).
  • X is two or more elements selected from the group consisting of F, Cl, Br, and I.
  • X is two or more elements selected from the group consisting of F, Cl, Br, and I.
  • the ionic conductivity of the first solid electrolyte can be further improved.
  • the charge / discharge efficiency of the battery can be further improved.
  • the first solid electrolyte may be represented by the following composition formula (A3).
  • FIG. 1 is a cross-sectional view showing a schematic configuration of the positive electrode material 1000 according to the first embodiment.
  • the positive electrode active material particles 110 coated with the coating material are immersed in water to elute the coating material.
  • the amount of eluted carbonate ions is quantified by ion chromatography.
  • the weight of lithium carbonate is calculated from the amount of carbonate ions. Using the weight of the positive electrode active material particles 110 used for production and the weight of lithium carbonate described above, the ratio of the weight of lithium carbonate contained in the coating material to the weight of the positive electrode active material particles 110 is calculated.
  • the peak area of C1s, the peak area of Ni2p 1/2 , the peak area of Ni2p 3/2 , the peak area of Co2p 1/2 , the peak area of Co2p 3/2 , the peak area of Mn2p 1/2 , and Mn2p 3 Calculate the peak area of / 2 .
  • the carbon abundance ratio (atom%) is calculated from the peak area of C with respect to the sum of the peak areas of C, Ni, Co, and Mn.
  • the abundance ratio of Ni (atom%), the abundance ratio of Co (atom%), and the abundance ratio of Mn (atom%) are calculated.
  • the abundance ratio (atom%) of the transition metal element is the sum of the abundance ratio of Ni, the abundance ratio of Co, and the abundance ratio of Mn.
  • the coating layer 111 may uniformly cover the positive electrode active material particles 110.
  • the direct contact between the positive electrode active material particles 110 and the first solid electrolyte particles 100 can be suppressed, and the side reaction of the first solid electrolyte particles 100 can be suppressed. Therefore, the charge / discharge efficiency of the battery can be improved.
  • the thickness of the coating layer 111 may be 10 nm or more and 40 nm or less.
  • the median diameter of the first solid electrolyte particles 100 may be 100 ⁇ m or less.
  • the positive electrode active material particles 110 and the first solid electrolyte particles 100 can form a good dispersed state in the positive electrode material 1000. Therefore, the charge / discharge characteristics of the battery are improved.
  • the median diameter of the first solid electrolyte particles 100 may be 10 ⁇ m or less.
  • the charge / discharge efficiency of the battery can be improved.
  • the halide solid electrolyte contained in the electrolyte layer 202 may contain Y as a metal element.
  • the material shown as the first solid electrolyte particles 100 in the first embodiment can be used.
  • the negative electrode 203 contains a material having the property of occluding and releasing metal ions (for example, lithium ions).
  • the negative electrode 203 contains, for example, a negative electrode active material.
  • the negative electrode 203 may contain a solid electrolyte.
  • the solid electrolyte the solid electrolyte exemplified as the material constituting the electrolyte layer 202 may be used. According to the above configuration, the lithium ion conductivity inside the negative electrode 203 is enhanced, and the battery can operate at a high output.
  • the thickness of the negative electrode 203 may be 10 ⁇ m or more and 500 ⁇ m or less. When the thickness of the negative electrode 203 is 10 ⁇ m or more, sufficient energy density of the battery can be secured. When the thickness of the negative electrode 203 is 500 ⁇ m or less, the battery can operate at a high output.
  • At least one of the positive electrode 201 and the negative electrode 203 may contain a conductive auxiliary agent for the purpose of increasing electron conductivity.
  • the conductive auxiliary agent include graphites of natural graphite and artificial graphite, carbon blacks such as acetylene black and Ketjen black, conductive fibers such as carbon fibers and metal fibers, and metal powders such as carbon fluoride and aluminum. Classes, conductive whiskers such as zinc oxide and potassium titanate, conductive metal oxides such as titanium oxide, and conductive polymer compounds such as polyaniline, polypyrrole, and polythiophene can be used.
  • a carbon conductive auxiliary agent is used as the conductive auxiliary agent, the cost can be reduced.
  • the powder after drying was placed in an alumina crucible and heat-treated at 400 ° C. for 10 hours in an oxygen atmosphere.
  • the coating material is lithium carbonate.
  • a positive electrode of Example 3 was obtained by the same method as in Example 1 except that the positive electrode active material used was changed to the positive electrode active material of Example 3.
  • Comparative Example 1 [Preparation of positive electrode active material]
  • the positive electrode active material of Comparative Example 1 was obtained by the same method as in Example 1 except that the positive electrode active material was changed to untreated NCM.
  • a positive electrode of Comparative Example 1 was obtained by the same method as in Example 1 except that the positive electrode active material used was changed to the positive electrode active material of Comparative Example 1.
  • the treated powder was placed in an alumina crucible and taken out in an air atmosphere.
  • the coating material is lithium niobate (LiNbO 3 ).
  • a positive electrode of Comparative Example 3 was obtained by the same method as in Example 1 except that the positive electrode active material used was changed to the positive electrode active material of Comparative Example 3.
  • the metal In (thickness 200 ⁇ m), the metal Li (thickness 300 ⁇ m), and the metal In (thickness 200 ⁇ m) were laminated in this order on the side of the solid electrolyte layer opposite to the side in contact with the positive electrode. This was pressure-molded at a pressure of 80 MPa to prepare a laminate composed of a positive electrode, a solid electrolyte layer, and a negative electrode.
  • the theoretical capacity per weight of NCM was set to 200 mAh / g, and the theoretical capacity of the battery was calculated.
  • the initial charge / discharge efficiency of the batteries of Examples 1 to 4 was higher than the initial charge / discharge efficiency of the batteries of Comparative Examples 1 to 3.
  • the reason for this is that the batteries of Examples 1 to 4 satisfy the relationship that the ratio of the weight of lithium carbonate contained in the coating material to the weight of the positive electrode active material is 1.3% by weight or more and 4.0% by weight or less. It can be mentioned that it was.
  • the coverage of lithium carbonate on the surface of the positive electrode active material was 91.1% or more.
  • the initial charge / discharge efficiency of the batteries of Examples 1 to 4 was higher than the initial charge / discharge efficiency of the batteries of Comparative Example 3. The reason for this is that the positive electrode active material used in the batteries of Examples 1 to 4 was coated with lithium carbonate.
  • the battery of the present disclosure can be used as, for example, an all-solid-state lithium secondary battery.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Inorganic Chemistry (AREA)
  • Composite Materials (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • General Physics & Mathematics (AREA)
  • Physics & Mathematics (AREA)
  • Organic Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Geology (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Secondary Cells (AREA)
PCT/JP2020/018121 2019-06-26 2020-04-28 正極材料、および、電池 Ceased WO2020261757A1 (ja)

Priority Applications (4)

Application Number Priority Date Filing Date Title
EP20830569.8A EP3993093A4 (en) 2019-06-26 2020-04-28 Positive electrode material, and battery
JP2021527428A JP7507385B2 (ja) 2019-06-26 2020-04-28 正極材料、および、電池
CN202080018871.XA CN113614948B (zh) 2019-06-26 2020-04-28 正极材料和电池
US17/506,720 US12224430B2 (en) 2019-06-26 2021-10-21 Positive electrode material and battery

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2019-118144 2019-06-26
JP2019118144 2019-06-26

Related Child Applications (1)

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US17/506,720 Continuation US12224430B2 (en) 2019-06-26 2021-10-21 Positive electrode material and battery

Publications (1)

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WO2020261757A1 true WO2020261757A1 (ja) 2020-12-30

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PCT/JP2020/018121 Ceased WO2020261757A1 (ja) 2019-06-26 2020-04-28 正極材料、および、電池

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US (1) US12224430B2 (https=)
EP (1) EP3993093A4 (https=)
JP (1) JP7507385B2 (https=)
CN (1) CN113614948B (https=)
WO (1) WO2020261757A1 (https=)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2022119107A (ja) * 2021-02-03 2022-08-16 三星エスディアイ株式会社 全固体二次電池
JP7853764B2 (ja) 2021-02-03 2026-04-30 三星エスディアイ株式会社 全固体二次電池

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* Cited by examiner, † Cited by third party
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EP3745504B1 (en) 2018-01-26 2023-07-12 Panasonic Intellectual Property Management Co., Ltd. Electrode material and battery
CN119297221A (zh) * 2024-09-12 2025-01-10 惠州亿纬动力电池有限公司 正极材料及其制备方法、正极浆料、正极极片、锂离子电池及其制备方法

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2022119107A (ja) * 2021-02-03 2022-08-16 三星エスディアイ株式会社 全固体二次電池
JP7853764B2 (ja) 2021-02-03 2026-04-30 三星エスディアイ株式会社 全固体二次電池

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EP3993093A4 (en) 2022-08-03
CN113614948A (zh) 2021-11-05
CN113614948B (zh) 2024-08-20
US20220045318A1 (en) 2022-02-10
US12224430B2 (en) 2025-02-11
JP7507385B2 (ja) 2024-06-28
EP3993093A1 (en) 2022-05-04
JPWO2020261757A1 (https=) 2020-12-30

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