# US 2020/0403228 A1 · Positive electrode material for rechargeable lithium ion batteries

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- Number: US 2020/0403228 A1
- Document ID: US20200403228A1
- Status: Published application
- Kind: A1
- Application number: 17/007,464
- Filed: 2020-08-31
- Published: 2020-12-24
- Earliest claimed: 2018-03-02
- Assignees: Umicore AG & Co. KG; Umicore Korea Ltd.
- Applicants: Umicore; Umicore Korea Ltd.
- Inventors: Dae-Hyun KIM; Jens PAULSEN; Shinichi KUMAKURA; YuRi LEE; Liang ZHU; TaeHyeon YANG
- Web page: https://patentgrep.com/patent/US20200403228A1

## CPC

- H01M 4/364: {as mixtures}
- C01G 51/06: Carbonates
- C01G 51/42: containing alkali metals, e.g. LiCoO2
- C01G 53/42: containing alkali metals, e.g. LiNiO2
- C01G 53/502: containing lithium and cobalt
- 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 53/506: with the molar ratio of nickel with respect to all the metals other than alkali metals higher than or equal to 0.8, e.g. Li(MzNixCoyMn1-x-y-z)O2 with x ≥ 0.8
- C01G 53/82: Compounds containing nickel, with or without oxygen or hydrogen, and containing two or more other elements
- 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 4/134: Electrodes based on metals, Si or alloys
- H01M 4/366: {as layered products}
- 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 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- C01P 2002/20: Two-dimensional structures
- C01P 2002/52: containing elements as dopants
- C01P 2004/03: obtained by SEM
- C01P 2004/51: Particles with a specific particle size distribution
- C01P 2004/53: bimodal size distribution
- C01P 2004/54: Particles characterised by their aspect ratio, i.e. the ratio of sizes in the longest to the shortest dimension
- C01P 2004/61: Micrometer sized, i.e. from 1-100 micrometer
- 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

A bimodal lithium transition metal oxide based powder mixture comprises a first and a second lithium transition metal oxide based powder. The first powder comprises particles of a material A comprising the elements Li, a transition metal based composition M and oxygen. The first powder has a particle size distribution characterized by a (D90−D10)/D50≤1.5. The second powder comprises a material B having single crystal particles, said particles having a general formula Li+bN′−bO2, wherein −0.03≤b≤0.10, and N′=NixM″yCozEd, wherein 0.30≤x≤0.92, 0.05≤y≤0.40, 0.05≤z≤0.40 and 0≤d≤0.10, wherein M″ is one or both of Mn or Al, and E is a dopant different from M″. The first powder has an average particle size D50 between 10 and 40 μm. The second powder has a D50 between 2 and 4.5 μm. The weight ratio of the second powder in the mixture is between 15 and 60 wt %.

## Claims

### Claim 1

A bimodal lithium transition metal oxide based powder mixture for a rechargeable battery, comprising:
a first lithium transition metal oxide based powder, comprising particles of a material A having a layered crystal structure comprising the elements Li, a transition metal based composition M and oxygen, the first powder having a particle size distribution characterized by (D90−D10)/D50≤1.5; and
a second lithium transition metal oxide based powder, comprising a material B having single crystal particles, said particles having a general formula Li1+bN′1−bO2, wherein −0.03≤b≤0.10, and N′=NixM″yCozEd, wherein 0.30≤x≤0.92 0.05≤y≤0.40, 0.05≤z≤0.40 and 0≤d≤0.10, with M″ being one or both of Mn or Al, and with E being a dopant different from M″, the first powder having an average particle size D50 between 10 and 40 μm, the second powder having an average particle size D50 between 2 and 4.5 μm; and wherein the weight ratio of the second powder in the bimodal mixture is between 15 and 60 wt %.

### Claim 2 (depends on 1)

The bimodal powder mixture of claim 1, wherein the particles of material A have a general formula Li1+aCo1−m M′mO2, with −0.05≤a≤0.05 and 0≤m≤0.05, the material A having a D50≥20 μm, and wherein M′ comprises one or more metals of the group consisting of Al, Ca, Si, Ga, B, Ti, Mg, W, Zr, Cr and V, and wherein the weight ratio of the second powder in the bimodal mixture is between 15 and 25 wt %.

### Claim 3 (depends on 1)

The bimodal powder mixture of claim 1, wherein the material A is polycrystalline and has particles having a general formula Li1+a′M1−a′O2, with −0.03≤a′≤0.10 and M=Nix′Mny′Coz′Ed′, wherein 0.30≤x′≤0.92, 0≤y′≤0.40, 0.05≤z′≤0.40, 0≤d′≤0.05 and x′+y′+z′+d′=1, and with E′ being one or more elements of the group consisting of Al, Ca, Si, Ga, B, Ti, Mg, W, Zr, Cr, V, S, F and N, and wherein the weight ratio of the second powder in the bimodal mixture is between 20 and 60 wt %.

### Claim 4 (depends on 3)

The bimodal powder mixture of claim 3, wherein 0.60≤x′≤0.92, 0≤y′≤0.30, and 0.10≤z′≤0.3.

### Claim 5 (depends on 1)

The bimodal powder mixture of claim 1, wherein E is one or more elements of the group consisting of Al, Ca, Si, Ga, B, Ti, Mg, W, Zr, Cr, V, S, F and N.

### Claim 6 (depends on 3)

The bimodal powder mixture of claim 3, wherein the first powder has a particle size distribution characterized by an average particle size D50 between 10 and 25 μm and a (D90−D10)/D50≤0.8.

### Claim 7 (depends on 1)

The bimodal powder mixture of claim 1, wherein both the first and the second powder have an aspect ratio substantially equal to 1.

### Claim 8 (depends on 1)

The bimodal powder mixture of claim 1, wherein the bimodal powder has a first corrected pressed density ≥3.2 g/cm3, wherein the first corrected pressed density is calculated with the formula PD/100×(100+ID10); wherein PD is the pressed density under a pressure of 200 MPa and ID10 is the increase of the D10 value in the particle size distribution of the bimodal powder calculated as follows:
ID


10
=
D


10


after


PDM
-
D


10


before


PDM
D


10


before


PDM
×
100


(
in


%
)
wherein (D10 after PDM) and (D10 before PDM) are respectively the D10 values after and before the application of a pressure of 200 MPa.

### Claim 9 (depends on 1)

The bimodal powder mixture of claim 1, wherein the bimodal powder has a second corrected pressed density ≥3.0 g/cm3, wherein the second corrected pressed density is calculated with the formula PD/100×(100−IB); wherein PD is the pressed density under a pressure of 200 MPa and IB is the increase of the specific surface area BET of the bimodal powder calculated as follows:
IB
=
BET


after


PDM
-
BET


before


PDM
BET


before


PDM
×
100


(
in


%
)
wherein (BET after PDM) and (BET before PDM) are respectively the BET values after and before the application of a pressure of 200 MPa.

### Claim 10 (depends on 3)

The bimodal powder mixture of claim 3, wherein the particles of the powder mixture have a surface layer comprising an intimate mixture of the elements of M, LiF and Al2O3.

### Claim 11 (depends on 1)

A positive electrode mixture for a rechargeable battery comprising the bimodal powder mixture of claim 1, a binder and a conductive agent, wherein the weight ratio of the bimodal powder mixture in the positive electrode mixture is at least 90 wt % and wherein the positive electrode mixture has a density of at least 3.65 g/cm3 when pressed under 1765.2 N.