# US 10,873,104 B2 · Positive electrode active materials for secondary battery and secondary battery comprising the same

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- Number: US 10,873,104 B2
- Document ID: US10873104B2
- Status: Granted
- Kind: B2
- Application number: 15/760,071
- Filed: 2016-11-30
- Published: 2018-09-06
- Granted: 2020-12-22
- Earliest claimed: 2015-11-30
- Assignees: LG Chem, Ltd.
- Applicants: LG Chem, Ltd.
- Inventors: Sang Min Park; Wang Mo Jung; Byung Chun Park; Ju Kyung Shin; Ji Hoon Ryu; Sang Wook Lee
- Web page: https://patentgrep.com/patent/US10873104B2

## CPC

- H01M 10/052: Li-accumulators
- 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
- C01G 53/84: Hydroxides
- 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 4/364: {as mixtures}
- 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
- C01P 2002/50: Solid solutions
- C01P 2004/03: obtained by SEM
- C01P 2004/51: Particles with a specific particle size distribution
- C01P 2006/11: Powder tap density
- C01P 2006/12: Surface area
- C01P 2006/40: Electric properties
- 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

The present invention provides a positive electrode active material for a secondary battery, the positive electrode active material being a secondary particle that includes a primary particle having a rectangular parallelepiped shape, the rectangular parallelepiped having at least one portion of vertices and edges formed in a round shape that is convex outward, wherein 1% to 40% of a total surface area of the secondary particle has open porosity, and the primary particle includes a lithium composite metal oxide of Formula 1 herein so that intercalation and deintercalation of lithium are facilitated, elution of an active material-constituting metal element is suppressed, and excellent structural stability is exhibited, thereby decreasing resistance and improving output and lifespan characteristics when applied to a battery, and a secondary battery comprising the same.

## Claims

### Claim 1

A positive electrode active material for a secondary battery, the positive electrode active material being a secondary particle that includes a primary particle having a rectangular parallelepiped shape, the rectangular parallelepiped having at least one portion of vertices and edges formed in a round shape that is convex outward, wherein:
1% to 40% of a total surface area of the secondary particle has open porosity; and
the primary particle includes a lithium composite metal oxide of Formula 1 below:
LiaNi1-x-yCoxM1yM3zM2wO2 [Formula 1]
(In Formula 1, M1 is at least one selected from the group consisting of Al and Mn, M2 is any one or two or more elements selected from the group consisting of Zr, Ti, Mg, Ta, and Nb, M3 is any one or two or more elements selected from the group consisting of W, and Mo, and 1.0≤a≤1.5, 0<x≤0.5, 0<y≤0.5, 0.002≤z≤0.03, 0≤w≤0.02, 0<x+y≤0.7).

### Claim 2 (depends on 1)

The positive electrode active material of claim 1, wherein:
the primary particle has a rectangular parallelepiped shape in which at least one vertex portion of vertices of the rectangular parallelepiped has a round shape that is convex outward; and
a cross-section of the primary particle is rectangular when the particle is cut such that the rectangular parallelepiped includes a long axis that is parallel to two surfaces of the rectangular parallelepiped facing each other and passes through a center of the particle.

### Claim 3 (depends on 1)

The positive electrode active material of claim 1, wherein an aspect ratio of the primary particle which is a ratio between a long axis passing through the center of the primary particle and a short axis orthogonal to the long axis and passing through the center of the primary particle is 1.5 to 10.

### Claim 4 (depends on 1)

The positive electrode active material of claim 1, wherein less than 50% of the primary particles have an orientation oriented toward a center of the secondary particle.

### Claim 5 (depends on 1)

The positive electrode active material of claim 1, wherein the positive electrode active material further comprises a hollow inside the secondary particle.

### Claim 6 (depends on 1)

The positive electrode active material of claim 1, wherein at least one metal element of nickel, M1, and cobalt exhibits a concentration gradient that changes in the active material particle.

### Claim 7 (depends on 1)

The positive electrode active material of claim 1, wherein:
nickel, M1, and cobalt exhibit a concentration gradient that each independently changes throughout the active material;
the concentration of nickel decreases with a gradual concentration gradient in a direction from the center of the active material toward a surface thereof; and
the concentrations of cobalt and M1 independently increase with a concentration gradient in the direction from the center of the active material toward the surface thereof.

### Claim 8 (depends on 1)

The positive electrode active material of claim 1, wherein the M1 is Mn.

### Claim 9 (depends on 1)

The positive electrode active material of claim 1, wherein the positive electrode active material has an average particle size (D50) of 2 μm to 20 μm and a Brunauer-Emmett-Teller (BET) specific surface area of 0.5 m2/g to 1.9 m2/g.

### Claim 10 (depends on 1)

The positive electrode active material of claim 1, wherein the positive electrode active material has a tap density of 1.7 g/cc to 2.5 g/cc.

### Claim 11 (depends on 1)

A method of manufacturing the positive electrode active material for a secondary battery according to claim 1, the method comprising:
a step of preparing a needle-shaped precursor by adding an ammonium cation-containing complexing agent and a basic compound to a metal-containing solution, which is produced by mixing a nickel raw material, a cobalt raw material, and an M1 raw material (here, M1 is at least one element selected from the group consisting of Al and Mn), and causing a reaction at pH 9 to 11; and
a step of mixing the needle-shaped precursor with a lithium raw material and then sintering at 700° C. to 900° C.,
wherein an M3 raw material (here, M3 is any one or two or more elements selected from the group consisting of W, Mo, and Cr) is further added when producing the metal-containing solution or mixing the needle-shaped precursor with the lithium raw material.

### Claim 12 (depends on 11)

The method of claim 11, wherein the ammonium cation-containing complexing agent includes any one or a mixture of two or more selected from the group consisting of NH4OH, (NH4)2SO4, NH4 NO3, NH4 Cl, CH3 COONH4, and NH4 CO3.

### Claim 13 (depends on 11)

The method of claim 11, wherein the basic compound includes any one or a mixture of two or more selected from the group consisting of a hydrate of an alkali metal, a hydroxide of an alkali metal, a hydrate of an alkaline earth metal, and a hydroxide of an alkaline earth metal.

### Claim 14 (depends on 11)

The method of claim 11, wherein the lithium raw material is used such that a molar ratio between lithium included in the lithium raw material and a metal element (Me) included in the precursor (molar ratio of lithium/metal element (Me)) is 1.0 or higher.

### Claim 15 (depends on 11)

The method of claim 11, wherein the step of preparing the needle-shaped precursor includes further adding a metal-containing solution including nickel, cobalt, M1, and M3 in different concentrations from the metal-containing solution.

### Claim 16 (depends on 11)

The method of claim 11, wherein, when producing the metal-containing solution or mixing the needle-shaped precursor with the lithium raw material, an M2 raw material (here, M2 is any one or two or more elements selected from the group consisting of Zr, Ti, Mg, Ta, and Nb) is further added.

### Claim 17 (depends on 1)

A positive electrode for a secondary battery including the positive electrode active material of claim 1.

### Claim 18 (depends on 17)

A lithium secondary battery comprising the positive electrode of claim 17.