# US 10,770,717 B2 · Composition for secondary battery negative electrode and negative electrode for secondary battery using the same and secondary battery

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- Number: US 10,770,717 B2
- Document ID: US10770717B2
- Status: Granted
- Kind: B2
- Application number: 16/232,085
- Filed: 2018-12-26
- Published: 2019-07-04
- Granted: 2020-09-08
- Earliest claimed: 2017-12-28
- Assignees: Jnc Corporation; Jnc Petrochemical Corporation
- Applicants: Jnc Corporation; Jnc Petrochemical Corporation
- Inventors: Soichiro Sato; Yoshihito Takano; Hirotsuna Yamada; Keiichiro Kanao; Miwako Nishimura; Tetsuro Kizaki
- Web page: https://patentgrep.com/patent/US10770717B2

## CPC

- H01M 4/134: Electrodes based on metals, Si or alloys
- H01M 4/133: Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M 4/364: {as mixtures}
- H01M 4/366: {as layered products}
- H01M 4/386: {Silicon or alloys based on silicon}
- H01M 4/483: {for non-aqueous cells (H01M4/485 takes precedence)}
- H01M 4/587: for inserting or intercalating light metals
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- H01M 2004/027: {Negative 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
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION

## Abstract

A composition for a secondary battery negative electrode including a carbonaceous material (a) and a silicon oxide structure (b), wherein the silicon oxide structure (b) includes a silicon oxide framework containing Si and O in its atomic composition and silicon-based nanoparticles that are chemically bonded to the silicon oxide framework as components, wherein the silicon oxide structure (b) is contained in a proportion of 15 mass % or more with respect to a total amount of the carbonaceous material (a) and the silicon oxide structure (b), and wherein the silicon oxide structure (b) satisfies the following conditions (i) to (iii): (i) having an atomic composition represented by a general formula SiOx2Hy2 (0.3<x2<1.5, 0.01<y2<0.35), (ii) having Si—H bonds, and (iii) being essentially free of carbon.

## Claims

### Claim 1

A composition for a secondary battery negative electrode comprising:
a carbonaceous material (a); and
a silicon oxide structure (b),
wherein the silicon oxide structure (b) comprises a silicon oxide framework containing Si and O in its atomic composition and silicon-based nanoparticles that are chemically bonded to the silicon oxide framework as components,
wherein the silicon oxide structure (b) is contained in a proportion of 15 mass % or more with respect to a total amount of the carbonaceous material (a) and the silicon oxide structure (b), and
wherein the silicon oxide structure (b) satisfies the following conditions (i) to (iii):
(i) having an atomic composition represented by a general formula SiOx2Hy2, wherein 0.3<x2<1.5, 0.01<y2<0.35;
(ii) having Si—H bonds; and
(iii) being essentially free of carbon.

### Claim 2 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein the silicon oxide structure (b) is contained in a proportion of 18 to 90 mass % with respect to the total amount of the carbonaceous material (a) and the silicon oxide structure (b).

### Claim 3 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein the silicon oxide structure (b) is contained in a proportion of 18 to 85 mass % with respect to the total amount of the carbonaceous material (a) and the silicon oxide structure (b).

### Claim 4 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein the silicon oxide structure (b) comprises secondary aggregates in which the silicon-based nanoparticles are aggregated as primary particles.

### Claim 5 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein the silicon oxide structure (b) additionally satisfies the following condition (iv):
(iv) in a spectrum obtained through infrared spectroscopy measurement, having a ratio (I1/I2) between an intensity (I1) of a peak 1 derived from Si—H bonds at 820 to 920 cm−1 and an intensity (I2) of a peak 2 derived from Si—O—Si bonds at 1,000 to 1200 cm−1 that is in a range of 0.01 to 0.35.

### Claim 6 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein the silicon oxide structure (b) additionally satisfies the following condition (v):
(v) in a spectrum obtained through infrared spectroscopy measurement, among peaks derived from Si—O—Si bonds, having a ratio (I2-1/I2-2) between an intensity (I2-1) of a peak 2-1 closest to 1,170 cm−1 and an intensity (I2-2) of a peak 2-2 closest to 1,070 cm−1 that exceeds 1.

### Claim 7 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein at least some of the silicon-based nanoparticles are bonded to the silicon oxide framework through Si—O—Si bonds.

### Claim 8 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein a metal oxide containing at least one selected from among titanium, zinc, zirconium, aluminum, and iron is additionally contained as a constituent element, and
the silicon oxide structure (b) is coated with the metal oxide or composited with the metal oxide.

### Claim 9 (depends on 8)

The composition for a secondary battery negative electrode according to claim 8,
wherein the metal oxide contains titanium as the constituent element.

### Claim 10 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein a volume-based average particle diameter of the silicon-based nanoparticles is 100 nm to 500 nm.

### Claim 11 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein the silicon-based nanoparticles are contained in a proportion of 5 to 65 mass % with respect to a total mass of the silicon oxide structure (b).

### Claim 12 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein the carbonaceous material (a) is a powder including substantially spherical particles and with a volume-based average particle diameter of 1 to 100 μm.

### Claim 13 (depends on 1)

The composition for a secondary battery negative electrode according to claim 1,
wherein the carbonaceous material (a) is graphite.

### Claim 14 (depends on 1)

A negative electrode for a secondary battery comprising the composition for a secondary battery negative electrode according to claim 1.

### Claim 15 (depends on 14)

A secondary battery comprising the negative electrode for a secondary battery according to claim 14.

### Claim 16 (depends on 15)

The secondary battery according to claim 15,
wherein the secondary battery is a lithium ion secondary battery.

### Claim 17 (depends on 2)

The composition for a secondary battery negative electrode according to claim 2,
wherein the silicon oxide structure (b) is contained in a proportion of 18 to 85 mass % with respect to the total amount of the carbonaceous material (a) and the silicon oxide structure (b).

### Claim 18 (depends on 2)

The composition for a secondary battery negative electrode according to claim 2,
wherein the silicon oxide structure (b) comprises secondary aggregates in which the silicon-based nanoparticles are aggregated as primary particles.

### Claim 19 (depends on 3)

The composition for a secondary battery negative electrode according to claim 3,
wherein the silicon oxide structure (b) comprises secondary aggregates in which the silicon-based nanoparticles are aggregated as primary particles.

### Claim 20 (depends on 2)

The composition for a secondary battery negative electrode according to claim 2,
wherein the silicon oxide structure (b) additionally satisfies the following condition (iv):
(iv) in a spectrum obtained through infrared spectroscopy measurement, having a ratio (I1/I2) between an intensity (I1) of a peak 1 derived from Si—H bonds at 820 to 920 cm−1 and an intensity (I2) of a peak 2 derived from Si—O—Si bonds at 1,000 to 1200 cm−1 that is in a range of 0.01 to 0.35.