# US 2024/0199441 A1 · Positive active material, method for preparing same, electrode plate, secondary battery, and electrical device

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- Number: US 2024/0199441 A1
- Document ID: US20240199441A1
- Status: Published application
- Kind: A1
- Application number: 18/412,601
- Filed: 2024-01-15
- Published: 2024-06-20
- Earliest claimed: 2022-06-08
- Assignees: Contemporary Amperex Technology Co., Limited
- Applicants: Contemporary Amperex Technology Co., Limited
- Inventors: Dong Zhao; Qi Wu; Chongheng Shen; Bangrun Wang; Qiang Chen; Jingpeng Fan; Na Liu
- Web page: https://patentgrep.com/patent/US20240199441A1

## CPC

- H01M 4/505: of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- C01G 53/50: of the type (MnO2)n-, e.g. Li(NixMn1-x)O2 or Li(MyNixMn1-x-y)O2
- C01G 53/502: containing lithium and cobalt
- H01M 4/131: Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
- H01M 4/1391: of electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
- H01M 4/36: Selection of substances as active materials, active masses, active liquids
- H01M 4/366: {as layered products}
- H01M 4/485: of mixed oxides or hydroxides for inserting or intercalating light metals, e.g. LiTi2O4 or LiTi2OxFy (H01M4/505, H01M4/525 take precedence)
- H01M 4/525: of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
- H01M 4/5825: {Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines}
- H01M 4/62: Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M 10/00: Secondary cells; Manufacture thereof
- H01M 10/052: Li-accumulators
- C01P 2002/08: Intercalated structures, i.e. with atoms or molecules intercalated in their structure
- C01P 2004/61: Micrometer sized, i.e. from 1-100 micrometer
- C01P 2004/84: one phase coated with the other
- C01P 2006/12: Surface area
- H01M 2004/021: {Physical characteristics, e.g. porosity, surface area}
- H01M 2004/028: {Positive electrodes}
- Y02E 60/10: Energy storage using batteries
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- C01G: COMPOUNDS CONTAINING METALS NOT COVERED BY SUBCLASSES C01D OR C01F (metal hydrides {monoborane, diborane or addition complexes thereof} C01B6/00; salts of oxyacids of halogens C01B11/00; peroxides, salts or peroxyacids C01B15/00; thiosulfates, dithionites, polythionates C01B17/64; compounds containing selenium, or tellurium C01B19/00; binary compounds of nitrogen with metals C01B21/06; azides C01B21/08; {compounds containing nitrogen, other non-metals and metal C01B21/082}; metal amides C01B21/092; nitrites C01B21/50; {compounds of noble gases C01B23/0005}; phosphides C01B25/08; salts of oxyacids of phosphorus C01B25/16; carbides C01B32/90; compounds containing silicon C01B33/00; compounds containing boron C01B35/00; compounds having molecular sieve properties but not having base-exchange properties C01B37/00; compounds having molecular sieve and base-exchange properties, e.g. crystalline zeolites, C01B39/00; cyanides C01C3/08; salts of cyanamide C01C3/16; thiocyanates C01C3/20)
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

This application relates to a positive active material, a method for preparing same, an electrode plate, a secondary battery, and an electrical device. The positive active material includes: a core material, including a lithium-rich manganese-based positive electrode material; and a cladding layer, covering an outer surface of the core material, where the cladding layer includes an oxygen-ion conductor and a lithium-ion conductor.

## Claims

### Claim 1

A positive active material, characterized in that the positive active material comprises:
a core material, comprising a lithium-rich manganese-based positive electrode material; and
a cladding layer, covering an outer surface of the core material, wherein the cladding layer comprises an oxygen-ion conductor and a lithium-ion conductor.

### Claim 2 (depends on 1)

The positive active material according to claim 1, characterized in that the oxygen-ion conductor comprises at least one of La2Mo2O9 or a fluorite-type oxygen-ion conductor.

### Claim 3 (depends on 2)

The positive active material according to claim 2, characterized in that the fluorite-type oxygen-ion conductor comprises at least one of ZrO2, CeO2, or GeO2.

### Claim 4 (depends on 1)

The positive active material according to claim 1, characterized in that the lithium-ion conductor comprises at least one of LiLaO2, Li2MoO4, Li3PO4, Li3BO3, or LiTaO3.

### Claim 5 (depends on 1)

The positive active material according to claim 1, characterized in that the oxygen-ion conductor comprises La2Mo2O9, and the lithium-ion conductor comprises LiLaO2 and Li2MoO4.

### Claim 6 (depends on 5)

The positive active material according to claim 5, characterized in that a molar ratio between a lanthanum atom and a molybdenum atom in the cladding layer is 1:(1.02 to 1.1), and optionally 1:(1.02 to 1.05).

### Claim 7 (depends on 5)

The positive active material according to claim 5, characterized in that a content of a molybdenum atom in the cladding layer is 300 ppm to 5000 ppm; and/or
a content of a lanthanum atom in the cladding layer is 500 ppm to 5000 ppm.

### Claim 8 (depends on 5)

The positive active material according to claim 5, characterized in that a content of a molybdenum atom in the cladding layer is 1000 ppm to 4000 ppm; and/or
a content of a lanthanum atom in the cladding layer is 1000 ppm to 3000 ppm.

### Claim 9 (depends on 5)

The positive active material according to claim 5, characterized in that a surface of the core material is doped with a lanthanum atom and a molybdenum atom.

### Claim 10 (depends on 9)

The positive active material according to claim 9, characterized in that a thickness of the surface of the core material doped with the lanthanum atom and the molybdenum atom is not greater than 3 μm, and optionally not greater than 2 μm.

### Claim 11 (depends on 1)

The positive active material according to claim 1, characterized in that a thickness of the cladding layer is 0.01 to 4 μm.

### Claim 12 (depends on 1)

The positive active material according to claim 1, characterized in that a thickness of the cladding layer is 0.02 to 1 μm.

### Claim 13 (depends on 1)

The positive active material according to claim 1, characterized in that a peak intensity ratio between IO22− and IO2− in the cladding layer is 0.5 to 1, and optionally 0.7 to 0.9, wherein
IO22− is a peak intensity value of an oxygen vacancy corresponding to 531 eV in an X-ray photoelectron spectroscopy test, and IO2− is a peak intensity value of lattice oxygen corresponding to 529 eV in the X-ray photoelectron spectroscopy test.

### Claim 14 (depends on 1)

The positive active material according to claim 1, characterized in that a molecular formula of the lithium-rich manganese-based positive electrode material is xLi2MnO3·(1-x)LiNiyCozMnaM1-y-z-aO2, wherein
0<x<1, 0≤y≤1, 0≤z≤1, 0≤a≤1, 0<y+z+a≤1; and M is at least one of Mg, B, Al, V, Ti, Zr, Sn, or Mo.

### Claim 15 (depends on 1)

The positive active material according to claim 1, characterized in that a particle type of the lithium-rich manganese-based positive electrode material is a secondary particle, a single crystal, or a quasi-single crystal; and/or
a specific surface area of the lithium-rich manganese-based positive electrode material is less than 2.0 m2/g, and optionally is 0.1 to 1 m2/g; and
a Dv50 particle diameter of the lithium-rich manganese-based positive electrode material is 1 to 20 μm, and optionally 3 to 15 μm.

### Claim 16 (depends on 1)

A method for preparing the positive active material according to claim 1, characterized in that the method comprises the following steps:
forming the cladding layer on a surface of the core material.

### Claim 17 (depends on 16)

The preparation method according to claim 16, characterized in that the oxygen-ion conductor comprises La2Mo2O9, and the lithium-ion conductor comprises LiLaO2 and Li2MoO4; and the preparation method comprises the following steps:
mixing a molybdenum salt, a lanthanum salt, and a lithium-rich manganese-based precursor in a solvent, and performing a hydrothermal reaction at 100° C. to 200° ° C. for 8 to 12 hours to obtain a lithium-rich manganese-based precursor, wherein, La2Mo2O9 is deposited in situ on a surface of the precursor; and
mixing a lithium salt with the lithium-rich manganese-based precursor containing the La2Mo2O9 deposited in situ on the surface, and then calcining the mixture to obtain a positive active material compositely coated with the oxygen-ion conductor and the lithium-ion conductor.

### Claim 18 (depends on 17)

The preparation method according to claim 17, characterized in that the lithium-rich manganese-based precursor is NibCocMndM(1-b-c-d)(OH)2, wherein
0<b<0.4, 0≤c≤0.05, 0.6≤d<1, and M is at least one of Mg, B, Al, V, Ti, Zr, Sn, or Mo.

### Claim 19 (depends on 17)

The preparation method according to claim 17, characterized in that the solvent is at least one of water, ethanol, methanol, or ethylene glycol; and/or
the molybdenum salt is at least one of ammonium molybdate, sodium molybdate, or potassium molybdate; and/or
the lanthanum salt is at least one of lanthanum chloride or lanthanum nitrate; and/or
the lithium salt is at least one of lithium carbonate, lithium hydroxide, or lithium acetate; and/or
a molar ratio between lithium in the lithium salt and all metal elements in the lithium-rich manganese-based precursor containing the La2Mo2O9 deposited in situ on the surface is 1:(1.1 to 1.8), and optionally 1:(1.1 to 1.5); and/or
a pH value of the hydrothermal reaction is 8 to 10; and/or
an atmosphere for the calcination is air; and/or
the calcination comprises steps of: pre-calcining at 300° C. to 500° C. for 2 to 5 hours, and then sintering at 700° C. to 900° C. for 10 to 20 hours.

### Claim 20 (depends on 1)

A positive electrode plate, characterized in that the positive electrode plate comprises:
a positive current collector; and
a positive active material layer, wherein the positive active material layer is located on a surface of the positive current collector, and ingredients of the positive active material layer comprise the positive active material according to claim 1.

### Claim 21 (depends on 20)

A secondary battery, characterized in that the secondary battery comprises the positive electrode plate according to claim 20.

### Claim 22 (depends on 21)

An electrical device, characterized in that the electrical device comprises the secondary battery according to claim 21.