# US 10,374,227 B2 · Positive electrode active material, method for preparing the same and lithium secondary battery including the same

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- Number: US 10,374,227 B2
- Document ID: US10374227B2
- Status: Granted
- Kind: B2
- Application number: 15/531,107
- Filed: 2015-12-04
- Published: 2017-11-09
- Granted: 2019-08-06
- Earliest claimed: 2014-12-05
- Assignees: LG Chem, Ltd.
- Applicants: LG Chem, Ltd.
- Inventors: Dong Kwon Lee; Seung Beom Cho; Jun Seok Nho; Byung Hyun Min; Bae Jung Kim
- Web page: https://patentgrep.com/patent/US10374227B2

## CPC

- H01M 4/366: {as layered products}
- B60L 50/64: Constructional details of batteries specially adapted for electric vehicles
- C01G 25/00: Compounds of zirconium
- C01G 25/006: {Compounds containing zirconium, with or without oxygen or hydrogen, and containing two or more other elements}
- C01G 53/504: with the molar ratio of nickel with respect to all the metals other than alkali metals higher than or equal to 0.5, e.g. Li(MzNixCoyMn1-x-y-z)O2 with x ≥ 0.5
- H01M 4/0471: {involving thermal treatment, e.g. firing, sintering, backing particulate active material, thermal decomposition, pyrolysis}
- 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 4/505: of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
- 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 4/62: Selection of inactive substances as ingredients for active masses, e.g. binders, fillers
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- C01P 2002/72: by d-values or two theta-values, e.g. as X-ray diagram
- C01P 2004/03: obtained by SEM
- C01P 2004/04: obtained by TEM, STEM, STM or AFM
- C01P 2004/61: Micrometer sized, i.e. from 1-100 micrometer
- C01P 2004/64: Nanometer sized, i.e. from 1-100 nanometer
- C01P 2004/84: one phase coated with the other
- C01P 2006/40: Electric properties
- H01M 10/052: Li-accumulators
- H01M 2004/028: {Positive electrodes}
- H01M 2220/20: Batteries in motive systems, e.g. vehicle, ship, plane
- Y02E 60/10: Energy storage using batteries
- Y02T 10/70: Energy storage systems for electromobility, e.g. batteries
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- B60L: PROPULSION OF ELECTRICALLY-PROPELLED VEHICLES (arrangements or mounting of electrical propulsion units or of plural diverse prime-movers for mutual or common propulsion in vehicles B60K1/00, B60K6/20; arrangements or mounting of electrical gearing in vehicles B60K17/12, B60K17/14; preventing wheel slip by reducing power in rail vehicles B61C15/08; dynamo-electric machines H02K; control or regulation of electric motors H02P); SUPPLYING ELECTRIC POWER FOR AUXILIARY EQUIPMENT OF ELECTRICALLY-PROPELLED VEHICLES (electric coupling devices combined with mechanical couplings of vehicles B60D1/64; electric heating for vehicles B60H1/00); ELECTRODYNAMIC BRAKE SYSTEMS FOR VEHICLES IN GENERAL (control or regulation of electric motors H02P); MAGNETIC SUSPENSION OR LEVITATION FOR VEHICLES; MONITORING OPERATING VARIABLES OF ELECTRICALLY-PROPELLED VEHICLES; ELECTRIC SAFETY DEVICES FOR ELECTRICALLY-PROPELLED VEHICLES
- 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
- Y02T: CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION

## Abstract

The present invention provides a positive electrode active material prepared using a preparation method including mixing lithium complex metal oxide particles with a nanosol of a ceramic-based ion conductor and heat treating the resultant to form a coating layer including the ceramic-based ion conductor on the lithium complex metal oxide particles, thereby forming a coating layer including a ceramic-based ion conductor to a uniform thickness on a lithium complex metal oxide particle surface, and as a result, capable of minimizing capacity decline and enhancing a lifespan property when used in a secondary battery, a method for preparing the same, and a lithium secondary battery including the same.

## Claims

### Claim 1

A method for preparing a positive electrode active material comprising mixing lithium complex metal oxide particles with a nanosol of a ceramic-based ion conductor and heat treating the resultant to form a coating layer including the ceramic-based ion conductor on the lithium complex metal oxide particles, and
wherein the nanosol of the ceramic-based ion conductor is prepared by dissolving and reacting a precursor of a metal for forming a ceramic-based ion conductor in a glycol-based solvent, and then adding water thereto,
the method further comprising a process of heat treatment at a temperature from 120° C. to a boiling point of a glycol-based solvent after dissolving the precursor of the metal for forming a ceramic-based ion conductor and prior to adding water.

### Claim 2 (depends on 1)

The method for preparing a positive electrode active material of claim 1, wherein the ceramic-based ion conductor includes any one or a mixture of two or more selected from the group consisting of zirconia-based ceramic, ceria-based ceramic, lanthanum-based ceramic, and cermets thereof.

### Claim 3 (depends on 1)

The method for preparing a positive electrode active material of claim 1, wherein the ceramic-based ion conductor includes any one or a mixture of two or more selected from the group consisting of yttria-stabilized zirconia, gadolinia-doped ceria, samarium-doped ceria, lanthanum strontium cobalt ferrite, lanthanum strontium gallate magnesite, lanthanum strontium manganite, calcia-stabilized zirconia, scandia-stabilized zirconia, and nickel-yttria-stabilized zirconia cermet.

### Claim 4 (depends on 1)

The method for preparing a positive electrode active material of claim 1, wherein the ceramic-based ion conductor includes any one or a mixture of two or more selected from the group consisting of yttria-stabilized zirconia, calcia-stabilized zirconia, gadolinia-doped ceria, lanthanum strontium gallate magnesite and scandia-stabilized zirconia.

### Claim 5 (depends on 4)

The method for preparing a positive electrode active material of claim 4, wherein the yttria-stabilized zirconia is Zr(i−x)YxO2−x/2(0.01≤x≤0.30).

### Claim 6 (depends on 4)

The method for preparing a positive electrode active material of claim 4, wherein the calcia-stabilized zirconia includes CaO in 1 mol % to 20 mol % to the total weight of the calcia-stabilized zirconia.

### Claim 7 (depends on 4)

The method for preparing a positive electrode active material of claim 4, wherein the scandia-stabilized zirconia includes any one or a mixture of two or more selected from the group consisting of (ZrO2)1−2x(Sc2O3)X, (ZrO2)1−2x(Sc2O3)x−z(Y2O3)z and (ZrO2)1−2x−z(Sx2O3)x(CeO2)z(0.01≤x≤0.2 and 0.01≤z≤0.1).

### Claim 8 (depends on 1)

The method for preparing a positive electrode active material of claim 1, wherein the ceramic-based ion conductor is noncrystalline.

### Claim 9 (depends on 1)

The method for preparing a positive electrode active material of claim 1, wherein the ceramic-based ion conductor has a hydroxide form.

### Claim 10 (depends on 1)

The method for preparing a positive electrode active material of claim 1, wherein the ceramic-based ion conductor has an average particle diameter (D50) of 1 nm to 100 nm.

### Claim 11 (depends on 1)

The method for preparing a positive electrode active material of claim 1, wherein the nanosol of a ceramic-based ion conductor uses the ceramic-based ion conductor in an amount to have the content of 50 ppm to 300,000 ppm to the total weight of the positive electrode active material.

### Claim 12 (depends on 1)

The method for preparing a positive electrode active material of claim 1, wherein the nanosol of a ceramic-based ion conductor further includes any one, two or more metals selected from the group consisting of aluminum (Al), niobium (Nb), titanium (Ti), tungsten (W), molybdenum (Mo), chromium (Cr), copper (Cu), vanadium (V) and zinc (Zn), or is mixed and used with a nanosol including the metal.

### Claim 13 (depends on 1)

The method for preparing a positive electrode active material of claim 1, wherein the heat treatment is carried out in a temperature range of 100° C. to 600° C.

### Claim 14 (depends on 1)

A positive electrode active material prepared using the preparation method of claim 1, comprising:
lithium complex metal oxide particles; and
a coating layer located on the lithium complex metal oxide particles,
wherein the coating layer includes a ceramic-based ion conductor.

### Claim 15 (depends on 14)

The positive electrode active material of claim 14, wherein the lithium complex metal oxide comprises a compound of the following Chemical Formula 1:
Li1+aNi1−b−cMnbCocO2 <Chemical Formula 1>
wherein, in Chemical Formula 1, 0≤a≤0.33, 0≤b≤0.5 and 0≤c≤0.5.

### Claim 16 (depends on 14)

The positive electrode active material of claim 14, wherein the ceramic-based ion conductor has a single phase peak in an X-ray analysis.

### Claim 17 (depends on 14)

The positive electrode active material of claim 14, wherein the coating layer further includes a metal oxide including any one selected from the group consisting of Al, Nb, Ti, W, Mo, Cr, Cu, V and Zn, or two or more types of metals among these.

### Claim 18 (depends on 14)

The positive electrode active material of claim 14, which has an average particle diameter (D50) of 3 μm to 25 μm.