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WO2019203432A1 - Composite métallique pour matériau actif de cathode, matériau actif de cathode le comprenant et son procédé de fabrication - Google Patents

Composite métallique pour matériau actif de cathode, matériau actif de cathode le comprenant et son procédé de fabrication Download PDF

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Publication number
WO2019203432A1
WO2019203432A1 PCT/KR2019/002127 KR2019002127W WO2019203432A1 WO 2019203432 A1 WO2019203432 A1 WO 2019203432A1 KR 2019002127 W KR2019002127 W KR 2019002127W WO 2019203432 A1 WO2019203432 A1 WO 2019203432A1
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WO
WIPO (PCT)
Prior art keywords
active material
shell
metal composite
positive electrode
electrode active
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/KR2019/002127
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English (en)
Korean (ko)
Inventor
윤성훈
이일복
배중호
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.)
Industry Academic Cooperation Foundation of Chung Ang University
Original Assignee
Industry Academic Cooperation Foundation of Chung Ang University
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Industry Academic Cooperation Foundation of Chung Ang University filed Critical Industry Academic Cooperation Foundation of Chung Ang University
Publication of WO2019203432A1 publication Critical patent/WO2019203432A1/fr
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
    • 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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01G—COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F
    • C01G53/00—Compounds of nickel
    • C01G53/40—Complex oxides containing nickel and at least one other metal element
    • C01G53/42—Complex oxides containing nickel and at least one other metal element containing alkali metals, e.g. LiNiO2
    • 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
    • H01M4/48—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
    • 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
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2004/00—Particle morphology
    • C01P2004/80—Particles consisting of a mixture of two or more inorganic phases
    • C01P2004/82—Particles consisting of a mixture of two or more inorganic phases two phases having the same anion, e.g. both oxidic phases
    • C01P2004/84—Particles consisting of a mixture of two or more inorganic phases two phases having the same anion, e.g. both oxidic phases one phase coated with the other
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01P—INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
    • C01P2006/00—Physical properties of inorganic compounds
    • C01P2006/40—Electric properties
    • 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

  • LiCoO 2 used in the positive electrode is a cobalt-based positive electrode active material, which is a typical positive electrode active material for lithium secondary batteries.
  • studies on LiNiCoO 2 cathode active materials have been actively conducted, but have not yet obtained satisfactory properties.
  • the metal complex preferably has a particle size of 1 ⁇ m to 300 ⁇ m.
  • the first metal salt solution includes at least one of nickel (Ni), manganese (Mn), and cobalt (Co).
  • FIG 3 is a view of a metal composite prepared through a comparative example of the present invention.
  • 4 to 5 are diagrams for the test results on the coin cell manufactured according to an embodiment of the present invention.
  • the particle size of this metal composite is preferably 1 ⁇ m to 300 ⁇ m.
  • the cathode active material according to an embodiment of the present invention includes the metal composite for the cathode active material described above, and the cathode active material includes a porous layer between the core portion and the surface portion, and structural stability is improved by the porous layer. .
  • the metal complex preferably has a particle size of 1 ⁇ m to 300 ⁇ m.
  • the reactor may contain distilled water, and the first metal salt solution may be introduced into the reactor containing distilled water.
  • the metal salt concentration in the second metal salt solution is preferably 0.01 M to 2.0 M.
  • the metal salt concentration is less than 0.01 M, the production rate may be low because the amount of metal added is too small as a whole, and when it exceeds 2.0 M, stable colloid formation may be difficult.
  • the growth time of the first shell is preferably controlled to 1 to 15 hours.
  • the residence time of the mixed solution in the reactor may be 1 hour to 15 hours.
  • the reactor residence time may be to be added at a constant rate by adjusting the addition rate of each solution to 5 to 15 hours.
  • the residence time may be 10 hours, when the residence time is less than 5 hours, the overall productivity may decrease, and when it exceeds 15 hours, the problem that the formation of particles becomes difficult may occur.
  • the addition of the second metal salt solution is terminated and the second shell surrounding the first shell is grown. It is preferable to control the growth time of the second shell to 1 to 100 hours.
  • a plurality of porous layers can be alternately disposed between the core portion and the surface portion.
  • a plurality of porous layers may be arranged in a plural form from the center of the particle toward the surface.
  • the metal complex (metal complex 1) may be a precursor of the positive electrode active material.
  • Example 4 (Preparation Example 1: Manufacture of positive electrode active material lithium ion battery)
  • Each of the two cathode active materials prepared according to Example 3, PVDF (Polyvinylidene Fluoride) as a binder, and denca black (commercial name: super p) as a conductive material were mixed in a ratio of 94: 3: 3. After mixing, it was coated with an aluminum current collector, then dried and roll pressed to prepare a coin cell using an electrode prepared. At this time, 1M LiPF 6 EC / EMC (1: 2) was used as the electrolyte.
  • Example 1 for the cathode material prepared in Example 1, the initial efficiency was excellent about 96.3%, the reversible discharge capacity was confirmed to be about 227 mAh / g at 0.1 C-rate, at a speed of 4 C It can be seen that it shows an excellent speed characteristic of 73.8% compared to the speed of 0.1 C. The cycle test also showed excellent stability of 74.7% at the 100th cycle, which was confirmed to be superior to Example 2 (Comparative Example 1).
  • Example 1 Anode Material 0.1C / 0.1C 236/227 96.3 73.8 88.9 74.7 0.5C / 0.1C 219/225 102.6 0.5C / 0.2C 222/213 95.9 0.5C / 0.5C 214/207 96.8 0.5C / 1.0C 207/197 95.4 0.5C / 2.0C 196/184 94.0 0.5C / 4.0C 182/166 90.7
  • Example 2 (Comparative Example 1) Anode Material 0.1C / 0.1C 237/217 91.5 80.0 78.1 46.6 0.5C / 0.1C 221/219 99.1 0.5C / 0.2C 221/215 97.2 0.5C / 0.5C 216/207 95.8 0.5C / 1.0C 208/199 95.8 0.5C / 2.0C 199/190 95.5 0.5C / 4.0C 190/175 92.2

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

Abstract

L'invention concerne un composite métallique pour matériau actif de cathode, un matériau actif de cathode l'utilisant, une batterie secondaire l'utilisant, et son procédé de fabrication. Le procédé de l'invention permet, d'une part de résoudre des problèmes d'une technologie classique, telle que l'instabilité de régulation du pH, la non-formation de phase de précipitation, le traitement compliqué, le défaut de reproductibilité et le retard de croissance de grain; et, d'autre part, de fabriquer un composite métallique contenant une couche poreuse dans des particules. La mise en œuvre du composite métallique contenant une couche poreuse dans des particules peut empêcher une dégradation des performances de la batteriela conduisant à une détérioration d'électrode due à la formation de fissures dans un matériau actif.
PCT/KR2019/002127 2018-04-20 2019-02-21 Composite métallique pour matériau actif de cathode, matériau actif de cathode le comprenant et son procédé de fabrication Ceased WO2019203432A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
KR1020180045936A KR101905362B1 (ko) 2018-04-20 2018-04-20 양극활물질용 금속 복합체, 이를 포함하는 양극활물질 및 이의 제조 방법
KR10-2018-0045936 2018-04-20

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Publication Number Publication Date
WO2019203432A1 true WO2019203432A1 (fr) 2019-10-24

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WO (1) WO2019203432A1 (fr)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112250091A (zh) * 2020-10-30 2021-01-22 浙江帕瓦新能源股份有限公司 一种高镍三元前驱体、正极材料以及制备方法
CN113929156A (zh) * 2021-10-19 2022-01-14 厦门厦钨新能源材料股份有限公司 电池正极材料前驱体及其制备方法和应用

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR101905362B1 (ko) * 2018-04-20 2018-10-05 중앙대학교 산학협력단 양극활물질용 금속 복합체, 이를 포함하는 양극활물질 및 이의 제조 방법
KR102735520B1 (ko) * 2020-07-24 2024-11-29 주식회사 엘지화학 양극 활물질 전구체 및 이의 제조 방법
KR20230146344A (ko) 2022-04-12 2023-10-19 에스케이온 주식회사 리튬 이차 전지용 양극, 이를 포함하는 리튬 이차 전지 및 이의 제조 방법
WO2025071120A1 (fr) * 2023-09-25 2025-04-03 주식회사 엘지화학 Procédé de production d'un précurseur de matériau actif d'électrode positive et précurseur de matériau actif d'électrode positive

Citations (5)

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KR20130063868A (ko) * 2011-12-07 2013-06-17 삼성에스디아이 주식회사 리튬 이차전지용 양극 활물질, 이의 제조방법 및 이를 포함하는 리튬 이차 전지
KR20150045784A (ko) * 2013-10-21 2015-04-29 주식회사 엘지화학 리튬 이차전지용 양극 활물질 및 그의 제조방법
KR20160040016A (ko) * 2014-10-02 2016-04-12 주식회사 엘지화학 코어-쉘 구조의 양극 활물질 및 이를 포함하는 리튬 이차전지
KR20160149162A (ko) * 2015-06-17 2016-12-27 주식회사 엘지화학 이차전지용 양극활물질, 이의 제조방법 및 이를 포함하는 이차전지
KR101905362B1 (ko) * 2018-04-20 2018-10-05 중앙대학교 산학협력단 양극활물질용 금속 복합체, 이를 포함하는 양극활물질 및 이의 제조 방법

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20130063868A (ko) * 2011-12-07 2013-06-17 삼성에스디아이 주식회사 리튬 이차전지용 양극 활물질, 이의 제조방법 및 이를 포함하는 리튬 이차 전지
KR20150045784A (ko) * 2013-10-21 2015-04-29 주식회사 엘지화학 리튬 이차전지용 양극 활물질 및 그의 제조방법
KR20160040016A (ko) * 2014-10-02 2016-04-12 주식회사 엘지화학 코어-쉘 구조의 양극 활물질 및 이를 포함하는 리튬 이차전지
KR20160149162A (ko) * 2015-06-17 2016-12-27 주식회사 엘지화학 이차전지용 양극활물질, 이의 제조방법 및 이를 포함하는 이차전지
KR101905362B1 (ko) * 2018-04-20 2018-10-05 중앙대학교 산학협력단 양극활물질용 금속 복합체, 이를 포함하는 양극활물질 및 이의 제조 방법

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN112250091A (zh) * 2020-10-30 2021-01-22 浙江帕瓦新能源股份有限公司 一种高镍三元前驱体、正极材料以及制备方法
CN113929156A (zh) * 2021-10-19 2022-01-14 厦门厦钨新能源材料股份有限公司 电池正极材料前驱体及其制备方法和应用

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