WO2021043296A1 - Électrode et batterie à semi-conducteurs à base de particules d'oxyde inorganique - Google Patents

Électrode et batterie à semi-conducteurs à base de particules d'oxyde inorganique Download PDF

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Publication number
WO2021043296A1
WO2021043296A1 PCT/CN2020/113647 CN2020113647W WO2021043296A1 WO 2021043296 A1 WO2021043296 A1 WO 2021043296A1 CN 2020113647 W CN2020113647 W CN 2020113647W WO 2021043296 A1 WO2021043296 A1 WO 2021043296A1
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WIPO (PCT)
Prior art keywords
inorganic oxide
oxide particles
electrode
solid
active layer
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PCT/CN2020/113647
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English (en)
Chinese (zh)
Inventor
李长明
辛民昌
陈久存
吴超
辛程勋
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青岛九环新越新能源科技股份有限公司
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Publication of WO2021043296A1 publication Critical patent/WO2021043296A1/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
    • 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
    • H01M4/364—Composites as mixtures
    • 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
    • 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
    • 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
    • H01M4/485—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy
    • 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

  • the invention belongs to the technical field of energy storage equipment, and specifically is an electrode and a solid-state battery based on inorganic oxide particles.
  • Solid-state battery is a battery technology. Unlike lithium-ion batteries and lithium-ion polymer batteries commonly used today, solid-state batteries are batteries that use solid electrodes and solid electrolytes.
  • the traditional liquid lithium battery is vividly called "rocking chair battery” by scientists. The two ends of the rocking chair are the positive and negative poles of the battery, and the middle is the electrolyte (liquid). Lithium ions are like excellent athletes, running back and forth on both ends of the rocking chair. During the movement of lithium ions from the first capacitor electrode to the second capacitor electrode and then to the first capacitor electrode, the charging and discharging process of the battery is completed.
  • solid-state battery The principle of a solid-state battery is the same, except that its electrolyte is solid, with a density and structure that allows more charged ions to gather at one end, conduct a larger current, and then increase the battery capacity. Therefore, with the same amount of power, the volume of solid-state batteries will become smaller. Not only that, because there is no electrolyte in the solid-state battery, it will be easier to seal. When used in large equipment such as automobiles, there is no need to add additional cooling tubes, electronic controls, etc., which not only saves costs, but also effectively reduces weight.
  • the purpose of the present invention is to provide an electrode and a solid-state battery based on inorganic oxide particles, which can effectively increase the ion permeability in the electrode and reduce the interface resistance.
  • the present invention provides the following technical solutions:
  • the present invention first proposes an electrode based on inorganic oxide particles, which includes an electrode active layer containing inorganic oxide particles I for conducting ions.
  • the particle size of the inorganic oxide particles I is less than or equal to the thickness of the electrode active layer.
  • the inorganic oxide particles I include but are not limited to Li 1.5 Al 0.5 Ti 1.5 P 3 O 12 , Li 1.5 Al 0.5 Ge 1.5 P 3 O 12 , Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 , Li 6.5 La 3 Zr 1.5 Nb 0.5 O 12 , Li 6.28 Al 0.24 La 3 Zr 2 O 12 , Li 6.40 Ga 0.20 La 3 Zr 2 O 12 , Li 0.45 La 0.55 TiO 3 or Li x PO y N z .
  • it also includes an electrode current collector; the side of the inorganic oxide particles I facing away from the electrode current collector exposes the electrode active layer; or, at least two of the inorganic oxide particles I contact each other and form Inorganic oxide particle group I, in the inorganic oxide particle group I, at least one of the inorganic oxide particles I exposes the electrode active layer.
  • the present invention also provides a solid-state battery based on inorganic oxide particles, including a positive electrode, a negative electrode, and a solid electrolyte layer located between the positive electrode and the negative electrode.
  • the positive electrode and/or the negative electrode adopt the above-mentioned inorganic oxide-based Particle electrode.
  • the solid electrolyte layer contains inorganic oxide particles II.
  • the particle size of the inorganic oxide particles II is less than or equal to the thickness of the solid electrolyte layer.
  • the inorganic oxide particles II include but are not limited to Li 1.5 Al 0.5 Ti 1.5 P 3 O 12 , Li 1.5 Al 0.5 Ge 1.5 P 3 O 12 , Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 , Li 6.5 La 3 Zr 1.5 Nb 0.5 O 12 , Li 6.28 Al 0.24 La 3 Zr 2 O 12 , Li 6.40 Ga 0.20 La 3 Zr 2 O 12 , Li 0.45 La 0.55 TiO 3 or Li x PO y N z .
  • the solid electrolyte layer is exposed on both sides of the inorganic oxide particles II; or at least two of the inorganic oxide particles II are in contact with each other and form an inorganic oxide particle group II, the inorganic oxide particles In group II, at least two of the inorganic oxide particles II are respectively exposed on both sides of the solid electrolyte layer.
  • the inorganic oxide particles II arranged in the solid electrolyte layer are in contact with the inorganic oxide particles I arranged in the positive electrode and/or the negative electrode to realize ion transmission.
  • the electrode of the present invention is based on inorganic oxide particles.
  • the inorganic oxide particles I can conduct ions.
  • the inorganic oxide particles I can conduct ions to the inside of the electrode active layer. It can effectively increase the ion permeability in the electrode active layer and reduce the interface resistance.
  • Inorganic oxide particles I are arranged in the positive electrode and/or negative electrode, which can increase the ion permeability in the positive electrode and/or negative electrode and reduce the interface resistance;
  • Inorganic oxide particles II are arranged in the solid electrolyte layer.
  • the inorganic oxide particles II can effectively separate the positive electrode and the negative electrode. In this way, the positive electrode and the negative electrode can be prevented from contacting and short-circuit, and the solid electrolyte layer can be made thinner and reduced. Small internal resistance
  • the inorganic oxide particles II arranged in the solid electrolyte layer are in contact and coordination with the inorganic oxide particles I arranged in the positive electrode and the negative electrode, that is, ion transport channels can be formed between the inorganic oxide particles I and the inorganic oxide particles II. , Enhance ion transmission efficiency.
  • FIG. 1 is a schematic structural diagram of an embodiment of a solid-state battery based on inorganic oxide particles of the present invention
  • Figure 2 is a schematic diagram of the structure of an electrode based on inorganic oxide particles.
  • FIG. 1 it is a schematic structural diagram of an embodiment of a solid-state battery based on inorganic oxide particles of the present invention.
  • the solid-state battery based on inorganic oxide particles in this embodiment includes a positive electrode 1, a negative electrode 2, and a solid electrolyte layer 3 located between the positive electrode 1 and the negative electrode 2, and the positive electrode 1 and/or the negative electrode 2 are made of an electrode based on inorganic oxide particles.
  • Both the positive electrode 1 and the negative electrode 2 of this embodiment adopt electrodes based on inorganic oxide particles.
  • the positive electrode 1 as an electrode based on inorganic oxide particles to increase the ion permeability of the positive electrode 1, or only the negative electrode 2
  • An electrode based on inorganic oxide particles is used to increase the ion permeability of the negative electrode 2.
  • the electrode based on inorganic oxide particles of this embodiment includes an electrode active layer 4, and the electrode active layer 4 contains inorganic oxide particles I5 for conducting ions.
  • the particle size of the inorganic oxide particles I5 is less than or equal to the thickness of the electrode active layer 4, the particle size of the inorganic oxide particles I5 in this embodiment is equal to the thickness of the electrode active layer 4, and the mass of all the inorganic oxide particles I5 in this embodiment The ratio to the total mass of the electrode active layer 4 is less than or equal to 50%, so as to prevent the inorganic oxide particles I5 from excessively affecting the energy density of the electrode active layer 4.
  • the inorganic oxide particles I5 include but are not limited to Li 1.5 Al 0.5 Ti 1.5 P 3 O 12 , Li 1.5 Al 0.5 Ge 1.5 P 3 O 12 , Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 , Li 6.5 La 3 Zr 1.5 Nb 0.5 O 12 , Li 6.28 Al 0.24 La 3 Zr 2 O 12 , Li 6.40 Ga 0.20 La 3 Zr 2 O 12 , Li 0.45 La 0.55 TiO 3 or Li x PO y N z .
  • the solid electrolyte layer 3 contains inorganic oxide particles II6, and the particle size of the inorganic oxide particles II6 is less than or equal to the thickness of the solid electrolyte layer 3.
  • the particle size of the inorganic oxide particles II6 of this embodiment is equal to the thickness of the solid electrolyte layer 3. Since the ceramic material used in the inorganic oxide particles II6 can be used to transport ions, the ratio between the mass of the inorganic oxide particles II6 and the total mass of the solid electrolyte layer 3 may not be particularly limited.
  • the gelatinous material used in the solid electrolyte layer 3 On the one hand, the solid electrolyte material can be used to transport ions, and on the other hand, it can fill the space between the inorganic oxide particles II6. Therefore, the solid electrolyte layer 3 is obtained by curing the inorganic oxide particles II6 and the colloidal solid electrolyte material.
  • the inorganic oxide particles II6 include but are not limited to Li 1.5 Al 0.5 Ti 1.5 P 3 O 12 , Li 1.5 Al 0.5 Ge 1.5 P 3 O 12 , Li 6.5 La 3 Zr 1.5 Ta 0.5 O 12 , Li 6.5 La 3 Zr 1.5 Nb 0.5 O 12 , Li 6.28 Al 0.24 La 3 Zr 2 O 12 , Li 6.40 Ga 0.20 La 3 Zr 2 O 12 , Li 0.45 La 0.55 TiO 3 or Li x PO y N z .
  • the electrode of this embodiment further includes an electrode current collector 7; the side of the inorganic oxide particles I5 facing away from the electrode current collector 7 exposes the electrode active layer 4; or, at least two inorganic oxide particles I5 contact each other and form Inorganic oxide particle group I, in the inorganic oxide particle group I, at least one inorganic oxide particle I exposes the electrode active layer 4, that is, the inorganic oxide particle I5 exposes the electrode active layer 4 to facilitate ion conduction to the electrode active layer 4 internal.
  • the side of the inorganic oxide particles I5 facing away from the electrode current collector 7 of this embodiment exposes the electrode active layer 4.
  • the solid electrolyte layer 3 is exposed on both sides of the inorganic oxide particles II6; or at least two inorganic oxide particles II6 are in contact with each other to form an inorganic oxide particle group II.
  • the inorganic oxide particle group II there are at least two inorganic oxide particles.
  • the oxide particles II are respectively exposed on both sides of the solid electrolyte layer. In this way, ions can be directly conducted between the positive electrode 1 and the negative electrode 2 through the inorganic oxide particles II6, without the need to transfer the ions between the ceramic material and other solid electrolyte materials, which can effectively improve the ion transmission efficiency.
  • the solid electrolyte layer 3 is exposed on both sides of the inorganic oxide particles II6 of this embodiment.
  • the inorganic oxide particles II6 arranged in the solid electrolyte layer 3 are in contact with the inorganic oxide particles I5 arranged in the positive electrode 1 and/or the negative electrode 2 to achieve ion transmission.
  • the positive electrode 1 and the negative electrode 2 can transmit ions through the ion transmission channel constructed between the inorganic oxide particles I5 and the inorganic oxide particles II6, and can also transmit ions through other solid electrolyte materials, and the ion transmission efficiency is higher.
  • the present invention is a solid-state battery based on inorganic oxide particles.
  • the inorganic oxide particles I can conduct ions.
  • the inorganic oxide particles I can conduct ions to the inside of the electrode active layer. It can effectively increase the ion permeability in the electrode active layer and reduce the interface resistance.
  • Inorganic oxide particles I are arranged in the positive electrode and/or negative electrode, which can increase the ion permeability in the positive electrode and/or negative electrode and reduce the interface resistance;
  • Inorganic oxide particles II are arranged in the solid electrolyte layer.
  • the inorganic oxide particles II can effectively separate the positive electrode and the negative electrode. In this way, the positive electrode and the negative electrode can be prevented from contacting and short-circuit, and the solid electrolyte layer can be made thinner and reduced. Small internal resistance
  • the inorganic oxide particles II arranged in the solid electrolyte layer are in contact and coordination with the inorganic oxide particles I arranged in the positive electrode and the negative electrode, that is, ion transport channels can be formed between the inorganic oxide particles I and the inorganic oxide particles II. , Enhance ion transmission efficiency.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Composite Materials (AREA)
  • Materials Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Secondary Cells (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

L'invention concerne une électrode à base de particules d'oxyde inorganique, l'électrode comprenant une couche active d'électrode, des particules d'oxyde inorganique I pour conduire des ions étant incluses dans la couche active d'électrode. L'invention concerne en outre une batterie à semi-conducteurs à base de particules d'oxyde inorganique, la batterie à semi-conducteurs comprenant une électrode positive, une électrode négative, et une couche d'électrolyte à semi-conducteurs située entre l'électrode positive et l'électrode négative, l'électrode à base des particules d'oxyde inorganique étant utilisée en tant qu'électrode positive et/ou électrode négative. Dans l'électrode à base de particules d'oxyde inorganique de la présente invention, en fournissant des particules d'oxyde inorganique I à l'intérieur d'une couche active d'électrode, les particules d'oxyde inorganique I peuvent conduire des ions, de telle sorte que les ions peuvent être conduits vers l'intérieur de la couche active d'électrode en utilisant les particules d'oxyde inorganique I, et par conséquent, la perméabilité ionique dans la couche active d'électrode peut être efficacement améliorée, et la résistance d'interface peut être réduite.
PCT/CN2020/113647 2019-09-06 2020-09-06 Électrode et batterie à semi-conducteurs à base de particules d'oxyde inorganique WO2021043296A1 (fr)

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CN201910843248.7A CN112467091A (zh) 2019-09-06 2019-09-06 基于无机氧化物颗粒的电极及固态电池
CN201910843248.7 2019-09-06

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Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013157084A (ja) * 2012-01-26 2013-08-15 Toyota Motor Corp 全固体電池
CN104362288A (zh) * 2009-08-18 2015-02-18 精工爱普生株式会社 锂电池用电极体及锂电池
CN106104849A (zh) * 2014-03-06 2016-11-09 国际商业机器公司 离子传导复合隔膜
CN106560948A (zh) * 2015-10-05 2017-04-12 丰田自动车株式会社 全固体电池
CN107039640A (zh) * 2017-03-02 2017-08-11 清华大学 复合电极材料及其应用
JP2017216066A (ja) * 2016-05-30 2017-12-07 旭化成株式会社 固体電解質粒子膜の製造方法
CN210167439U (zh) * 2019-09-06 2020-03-20 青岛九环新越新能源科技股份有限公司 基于无机氧化物颗粒的电极及固态电池

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104362288A (zh) * 2009-08-18 2015-02-18 精工爱普生株式会社 锂电池用电极体及锂电池
JP2013157084A (ja) * 2012-01-26 2013-08-15 Toyota Motor Corp 全固体電池
CN106104849A (zh) * 2014-03-06 2016-11-09 国际商业机器公司 离子传导复合隔膜
CN106560948A (zh) * 2015-10-05 2017-04-12 丰田自动车株式会社 全固体电池
JP2017216066A (ja) * 2016-05-30 2017-12-07 旭化成株式会社 固体電解質粒子膜の製造方法
CN107039640A (zh) * 2017-03-02 2017-08-11 清华大学 复合电极材料及其应用
CN210167439U (zh) * 2019-09-06 2020-03-20 青岛九环新越新能源科技股份有限公司 基于无机氧化物颗粒的电极及固态电池

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