# US 12,015,148 B2 · Silicon particles for anode materials of lithium ion batteries

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- Number: US 12,015,148 B2
- Document ID: US12015148B2
- Status: Granted
- Kind: B2
- Application number: 16/484,822
- Filed: 2017-02-09
- Published: 2020-01-23
- Granted: 2024-06-18
- Earliest claimed: 2017-02-09
- Assignees: Wacker Chemie AG
- Applicants: Wacker Chemie AG
- Inventors: Sefer Ay; Dominik Jantke; Jürgen Stohrer; Sebastian Suckow; Harald Voit
- Web page: https://patentgrep.com/patent/US12015148B2

## CPC

- H01M 4/386: {Silicon or alloys based on silicon}
- H01M 4/134: Electrodes based on metals, Si or alloys
- H01M 4/366: {as layered products}
- H01M 4/587: for inserting or intercalating light metals
- H01M 4/625: {Carbon or graphite}
- H01M 10/052: Li-accumulators
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- H01M 2004/021: {Physical characteristics, e.g. porosity, surface area}
- 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

The invention relates to spherical, nonporous Silicon particles having average particle sizes (d50) of 1 to 10 pm and a silicon content of 97 to 99.8 wt. %, the silicon content relating to the total weight of the silicon particles minus any oxygen content.

## Claims

### Claim 1

Anode materials for lithium-ion batteries comprising:
one or more binders,
optionally graphite,
optionally one or more further electrically conductive components,
optionally one or more additives, and
non-aggregated, spherical, non-porous silicon particles having average particle sizes of 1 to 10 μm and a silicon content of 97% to 99.8% by weight, wherein the silicon content is based on the total weight of the silicon particles minus any oxygen contents, the silicon is in elemental form, and wherein ≥80% of the silicon particles have an orthogonal axial ratio R of 0.60≤R≤1.0, wherein the orthogonal axial ratio R is the quotient of the two largest mutually orthogonal diameters through a silicon particle and the larger diameter forms the denominator and the smaller diameter forms the numerator of the quotient, as determined by SEM image.

### Claim 2 (depends on 1)

The anode materials for lithium-ion batteries of claim 1, wherein ≥85% of the silicon particles have an orthogonal axial ratio R of 0.70≤R≤1.0, wherein the orthogonal axial ratio R is the quotient of the two largest mutually orthogonal diameters through a silicon particle and the larger diameter forms the denominator and the smaller diameter forms the numerator of the quotient, as determined by SEM image.

### Claim 3 (depends on 1)

The anode materials for lithium-ion batteries of claim 1, wherein the silicon particles have an average orthogonal axial ratio R of 0.70≤R≤1.0, wherein the orthogonal axial ratio R is the quotient of the two largest mutually orthogonal diameters through a silicon particle and the larger diameter forms the denominator and the smaller diameter forms the numerator of the quotient, as determined by SEM image.

### Claim 4 (depends on 1)

The anode materials for lithium-ion batteries of claim 1, wherein the silicon particles have been coated with carbon.

### Claim 5 (depends on 1)

The anode materials for lithium-ion batteries of claim 1, wherein the spherical, non-porous silicon particles are obtained by atomizing silicon.

### Claim 6 (depends on 5)

The anode materials for lithium-ion batteries of claim 5, wherein the spherical, non-porous silicon particles are obtained from molten silicon, by melting silicon or employing silicon in the form of a melt, forming the molten silicon into droplets, and cooling the droplets to a temperature below the melting point of silicon.

### Claim 7 (depends on 1)

The anode materials for lithium-ion batteries of claim 1, wherein the spherical, non-porous silicon particles are obtained by plasma rounding of silicon particles.

### Claim 8 (depends on 7)

The anode materials for lithium-ion batteries of claim 7, wherein the spherical, non-porous silicon particles are obtained by fully or partially melting silicon particles by plasma irradiation, and subsequently cooling to a temperature below the melting point of silicon.

### Claim 9 (depends on 1)

The anode materials of claim 1, wherein the non-aggregated spherical, non-porous silicon particles have silicon oxide SiOx where x≥1.3 on surfaces thereof.

### Claim 10 (depends on 1)

The anode materials of claim 1, wherein the non-aggregated spherical, non-porous silicon particles are coated with carbon, the content of carbon being ≤20 weight percent based on the total weight of the carbon-coated silicon particles.

### Claim 11 (depends on 1)

The anode materials of claim 1, wherein the non-aggregated spherical, non-porous silicon particles have an average orthogonal axial ratio R of greater than or equal to 0.80.

### Claim 12 (depends on 1)

The anode materials of claim 1, wherein the non-aggregated spherical, non-porous silicon particles have an average orthogonal axial ratio R of greater than or equal to 0.85.

### Claim 13 (depends on 1)

The anode materials of claim 1, wherein non-aggregated, spherical, non-porous silicon particles are carbon-coated, wherein the carbon content is from 0.1 to 10% by weight based on the total weight of the carbon-coated particles.

### Claim 14 (depends on 1)

The anode materials of claim 1, wherein non-aggregated, spherical, non-porous silicon particles are carbon-coated, wherein the carbon content is from 0.5 to 5% by weight based on the total weight of the carbon-coated particles.

### Claim 15 (depends on 1)

The anode particles of claim 1, wherein the non-aggregated, spherical, non-porous silicon particles have a silicon oxide coating on surfaces thereof, having the formula SiOx where x≥1.3, and a further coating of carbon derived by carbonizing one or more carbon precursors which have been coated onto the silicon particles having a silicon oxide coating, with the proviso that the carbon precursors are converted into carbon, and the carbon content of the carbon-coated particles is ≤20 weight percent based on the total weight of the coated particles.

### Claim 16 (depends on 1)

The anode material of claim 1, wherein the non-aggregated, spherical, non-porous silicon particles have no coating thereon, or which are coated with a silicon oxide coating with a layer thickness of <10 nm.

### Claim 17 (depends on 1)

The anode material of claim 1, wherein the non-aggregated, spherical, non-porous particles are melt-rounded fragments of metallurgical grade silicon having a silicon content of from 98 to 99% by weight based on the total weight of said particles.

### Claim 18 (depends on 1)

Lithium-ion batteries comprising:
a cathode,
an anode,
a separator, and
an electrolyte, wherein the anode is based on the anode material of claim 1.

### Claim 19 (depends on 18)

The lithium-ion batteries of claim 18, wherein, in the fully charged lithium-ion battery, the ratio of lithium atoms to silicon atoms in the anode material is ≤2.2.

### Claim 20 (depends on 18)

The lithium-ion batteries of claim 18, wherein the capacity of the silicon of the anode material of the lithium-ion battery is utilized to an extent of ≤50%, based on the maximum capacity of 4200 mAh per gram of silicon.