# US 12,002,958 B2 · Composite particles, negative electrode active material, and lithium-ion secondary battery

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- Number: US 12,002,958 B2
- Document ID: US12002958B2
- Status: Granted
- Kind: B2
- Application number: 17/928,195
- Filed: 2021-05-28
- Published: 2023-07-13
- Granted: 2024-06-04
- Earliest claimed: 2020-05-28
- Assignees: Resonac Corporation
- Applicants: Showa Denko K. K.
- Inventors: Naoto Kawaguchi; Yuji Ito; Masato Fujita; Hirofumi Inoue
- Web page: https://patentgrep.com/patent/US12002958B2

## CPC

- C01B 32/354: After-treatment
- H01M 4/587: for inserting or intercalating light metals
- C01B 32/05: Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30
- C01B 32/318: characterised by the starting materials
- C01B 32/336: characterised by gaseous activating agents
- C01B 32/342: characterised by non-gaseous activating agents
- C01B 32/372: Coating; Grafting; Microencapsulation
- H01M 4/133: Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M 4/134: Electrodes based on metals, Si or alloys
- H01M 4/1395: of electrodes based on metals, Si or alloys
- H01M 4/36: Selection of substances as active materials, active masses, active liquids
- H01M 4/364: {as mixtures}
- H01M 4/366: {as layered products}
- H01M 4/38: of elements or alloys
- H01M 4/386: {Silicon or alloys based on silicon}
- H01M 4/48: of inorganic oxides or hydroxides
- 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 4/622: {being polymers}
- H01M 4/625: {Carbon or graphite}
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- C01B 33/027: by decomposition or reduction of gaseous or vaporised silicon compounds other than silica or silica-containing material
- C01P 2002/02: Amorphous compounds
- C01P 2002/72: by d-values or two theta-values, e.g. as X-ray diagram
- C01P 2002/74: by peak-intensities or a ratio thereof only
- C01P 2002/82: by IR- or Raman-data
- C01P 2004/32: Spheres
- C01P 2004/61: Micrometer sized, i.e. from 1-100 micrometer
- C01P 2004/80: Particles consisting of a mixture of two or more inorganic phases
- C01P 2006/10: Solid density
- C01P 2006/12: Surface area
- C01P 2006/40: Electric properties
- H01M 2004/021: {Physical characteristics, e.g. porosity, surface area}
- H01M 2004/027: {Negative electrodes}
- Y02E 60/10: Energy storage using batteries
- Y02P 20/133: Renewable energy sources, e.g. sunlight
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS

## Abstract

The present invention relates to composite particles containing silicon and carbon, wherein a domain size region of vacancies of 2 nm or less is 44% by volume or more and 70% by volume or less when volume distribution information of domain sizes obtained by fitting a small-angle X-ray scattering spectrum of the composite particles with a spherical model in a carbon-vacancy binary system is accumulated in ascending order, and a true density calculated by dry density measurement by a constant volume expansion method using helium gas is 1.80 g/cm3 or more and 2.20 g/cm3 or less.

## Claims

### Claim 1

Composite particles comprising:
silicon and carbon,
wherein a domain size region of 2 nm or less is 44% by volume or more and 70% by volume or less when volume distribution information of domain sizes of vacancies obtained by fitting a small-angle X-ray scattering spectrum of the composite particles with a spherical model in a carbon-vacancy binary system is accumulated in ascending order, and
a true density calculated by dry density measurement by a constant volume expansion method using helium gas is 1.80 g/cm3 or more and 2.20 g/cm3 or less.

### Claim 2 (depends on 1)

The composite particles according to claim 1, wherein a content of silicon in the composite particles is 30% by mass or more and 80% by mass or less, and a content of oxygen is 0.1% by mass or more and 30% by mass or less when the content of silicon in the composite particles is designated as 100% by mass.

### Claim 3 (depends on 1)

The composite particles according to claim 1, wherein a peak attributed to silicon is present at 450 to 495 cm−1 in a Raman spectrum.

### Claim 4 (depends on 1)

The composite particles according to claim 1, wherein R value (ID/IG) in the Raman spectrum is 0.30 or more and less than 1.30.

### Claim 5 (depends on 1)

The composite particles according to claim 1, wherein (peak intensity of SiC111 plane)/(peak intensity of Si111 plane) is 0.01 or less, in an XRD pattern measured by powder XRD using a Cu-Kα radiation.

### Claim 6 (depends on 1)

The composite particles according to claim 1, wherein the composite particles have an average particle size DV50 of 1.0 μm or more and 30 μm or less, and have a BET specific surface area of 0.1 m2/g or more and 100 m2/g or less.

### Claim 7 (depends on 1)

The composite particles according to claim 1, wherein inorganic particles and a polymer are present on at least a part of surfaces of the composite particles, a content of polymer is 0.1% by mass to 10.0% by mass, and the inorganic particles are one or more selected from graphite and carbon black.

### Claim 8 (depends on 1)

The composite particles according to claim 1, wherein the carbon is amorphous carbon.

### Claim 9 (depends on 1)

A negative electrode active material comprising the composite particles according to claim 1.

### Claim 10 (depends on 9)

A negative electrode mixture layer comprising the negative electrode active material according to claim 9.

### Claim 11 (depends on 10)

A lithium-ion secondary battery comprising the negative electrode mixture layer according to claim 10.