# US 12,224,440 B2 · Process for making a coated cathode active material, and coated cathode active material

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- Number: US 12,224,440 B2
- Document ID: US12224440B2
- Status: Granted
- Kind: B2
- Application number: 18/564,734
- Filed: 2022-06-14
- Published: 2024-08-22
- Granted: 2025-02-11
- Earliest claimed: 2021-06-28
- Assignees: BASF SE; Karlsruher Institut Fuer Technologie
- Applicants: BASF SE; Karlsruher Institut Für Technologie
- Inventors: Matteo Bianchini; Pascal Hartmann; Torsten Brezesinski; Katja Ramona Kretschmer; Soeren Lukas Dreyer
- Web page: https://patentgrep.com/patent/US12224440B2

## CPC

- 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}
- 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 4/366: {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 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- C01P 2002/52: containing elements as dopants
- C01P 2004/80: Particles consisting of a mixture of two or more inorganic phases
- C01P 2006/40: Electric properties
- H01M 2004/028: {Positive electrodes}
- H01M 2220/20: Batteries in motive systems, e.g. vehicle, ship, plane
- H01M 2220/30: Batteries in portable systems, e.g. mobile phone, laptop
- 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

Disclosed herein is a process for making a coated cathode active material, where the process includes the following steps: (a) providing an electrode active material according to general formula Li1+xTM1−xO2, where TM is a combination of metals according to general formula (I), and x is in the range of from zero to 0.2, with a moisture content in the range of from 500 to 1,500 ppm, (b) reacting the electrode active material with a silicon alkoxide and an alkyl aluminum compound in one or more sub-steps, and (c) heat-treating the material so obtained in an oxygen-containing atmosphere at a temperature in the range of from 100 to 400° C. for 10 minutes to 4 hours.

## Claims

### Claim 1

A process for making a coated cathode active material, wherein said process comprises the following steps:
(a) providing an electrode active material according to general formula Li1+xTM1−xO2, wherein TM is a combination of metals according to formula (I), and x is in a range of from zero to 0.2, with a moisture content in a range of from 500 to 1,500 ppm,
with
a being in a range of from 0.3 to 0.4,
b being in a range of from zero to 0.1,
c being in a range of from 0.6 to 0.7, and
d being in a range of from zero to 0.1,
M is Al or Ti or Zr or Mg, and
a
+
b
+
c
=
1
,
(b) reacting said electrode active material with a silicon alkoxide and an alkyl aluminum compound in one or more sub-steps, and
(c) heat-treating the material obtained in step (b) in an oxygen-containing atmosphere at a temperature in a range of from 100 to 400° C. for 10 minutes to 4 hours.

### Claim 2 (depends on 1)

A process according to claim 1, wherein the silicon alkoxide is selected from the group consisting of tetramethoxysilane and tetraethoxysilane.

### Claim 3 (depends on 1, 2)

A process according to claim 1 or 2, wherein the alkyl aluminum compound in step (b) is selected from the group consisting of trimethylaluminum and triethylaluminum.

### Claim 4 (depends on 1)

A process according to claim 1, wherein a molar ratio of silicon to aluminum in step (b) is in a range of from 1:10 to 10:1.

### Claim 5 (depends on 1)

A process according to claim 1, wherein step (b) is performed in a presence of at least one organic solvent.

### Claim 6 (depends on 1)

A process according to claim 1, wherein in step (b) or in a sub-step before or after step (b) a carbonyl compound or an organometallic compound of cobalt is applied to the electrode active material provided in step (a) or resulting from step (b).

### Claim 7

A particulate cathode active material comprising a core material according to general formula Li1+xTM1−xO2, wherein TM is a combination of metals according to formula (I), and x is in a range of from zero to 0.2, and wherein an outer surface of the core material is non-homogeneously coated with a mixed oxide of aluminum and silicon of uniform composition,
with
a being in a range of from 0.3 to 0.4,
b being in a range of from zero to 0.1,
c being in a range of from 0.6 to 0.7, and
d being in a range of from zero to 0.1,
M is Al or Ti or Zr or Mg, and
a
+
b
+
c
=
1
.

### Claim 8 (depends on 7)

The particulate material according to claim 7, wherein said coating comprises a compound selected from the group consisting of LiAlSiO4 and LiAlSi2O6 and a compound selected from the group consisting of Li4SiO4, Li2SiO3, and Li2Si3O7.

### Claim 9 (depends on 7)

The particulate material according to claim 7, wherein a molar ratio of silicon to aluminum is in a range of from 1:20 to 1:1.

### Claim 10 (depends on 7)

A cathode comprising:
(A) at least one particulate material according to claim 7,
(B) carbon in electrically conductive form, and
(C) a binder polymer.
