# US 11,028,242 B2 · Modified silicon particles for silicon-carbon composite electrodes

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- Number: US 11,028,242 B2
- Document ID: US11028242B2
- Status: Granted
- Kind: B2
- Application number: 16/430,290
- Filed: 2019-06-03
- Published: 2020-12-03
- Granted: 2021-06-08
- Earliest claimed: 2019-06-03
- Assignees: Enevate Corporation
- Applicants: Enevate Corporation
- Inventors: Ian Russell Browne; Liwen Ji; Rahul R. Kamath; Monika Chhorng
- Web page: https://patentgrep.com/patent/US11028242B2

## CPC

- C08J 5/18: Manufacture of films or sheets
- C01B 33/02: Silicon (forming single crystals or homogeneous polycrystalline material with defined structure C30B)
- C08K 3/02: Elements
- C08K 5/32: Compounds containing nitrogen bound to oxygen
- C08K 5/5419: containing at least one Si—C bond
- C08K 9/06: with silicon-containing compounds
- H01M 4/0471: {involving thermal treatment, e.g. firing, sintering, backing particulate active material, thermal decomposition, pyrolysis}
- H01M 4/13: Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- H01M 4/1395: of electrodes based on metals, Si or alloys
- H01M 4/364: {as mixtures}
- H01M 4/386: {Silicon or alloys based on silicon}
- H01M 4/583: Carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M 4/625: {Carbon or graphite}
- H01M 10/052: Li-accumulators
- C08J 2361/04: Condensation polymers of aldehydes or ketones with phenols only
- C08J 2379/08: Polyimides; Polyester-imides; Polyamide-imides; Polyamide acids or similar polyimide precursors
- C08K 2003/023: {Silicon}
- H01M 2004/027: {Negative electrodes}
- Y02E 60/10: Energy storage using batteries
- C08J: WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H (working, e.g. shaping, of plastics B29)
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- C08K: Use of inorganic or non-macromolecular organic substances as compounding ingredients (paints, inks, varnishes, dyes, polishes, adhesives C09)
- 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

Methods of forming a composite material film can include providing a mixture comprising a precursor and silane-treated silicon particles. The methods can also include pyrolysing the mixture to convert the precursor into one or more carbon phases to form the composite material film with the silicon particles distributed throughout the composite material film.

## Claims

### Claim 1

A method of forming a composite material film, the method comprising:
providing a mixture comprising a precursor and silane-treated silicon particles; and
pyrolysing the mixture to convert the precursor into one or more carbon phases to form the composite material film with the silicon particles distributed throughout the composite material film, wherein:
silane-treated silicon particles comprise silicon particles treated with one or more organosilanes;
the one or more organosilanes comprise one or more silanols, silyl ethers, silyl chlorides, dialkylaminosilanes, silyl hydrides, or cyclic azasilanes; and
the one or more organosilanes comprise dodecylsilane.

### Claim 2 (depends on 1)

The method of claim 1, wherein the silane-treated silicon particles comprise silicon oxide surfaces reacted with the one or more organosilanes.

### Claim 3 (depends on 1)

The method of claim 1, wherein the one or more organosilanes comprise one or more aminoalkyl functional groups.

### Claim 4 (depends on 3)

The method of claim 3, wherein the one or more organosilanes comprise 3-aminopropyltriethoxysilane, N-(2-aminoethyl)-3-aminopropyltrimethoxysilane, or 2,2-dimethoxy-1,6-diaza-2-silacyclooctane.

### Claim 5 (depends on 3)

The method of claim 3, wherein the precursor comprises polyimide.

### Claim 6 (depends on 1)

The method of claim 1, wherein the one or more organosilanes comprise an epoxide linker.

### Claim 7 (depends on 6)

The method of claim 6, wherein the epoxide linker comprises 5,6-epoxyhexyltriethoxysilane.

### Claim 8 (depends on 6)

The method of claim 6, wherein the precursor comprises a phenolic resin.

### Claim 9 (depends on 1)

The method of claim 1, wherein the one or more organosilanes comprise an aromatic functional group.

### Claim 10 (depends on 9)

The method of claim 9, wherein the one or more organosilanes comprise benzyltriethoxysilane.

### Claim 11 (depends on 9)

The method of claim 9, wherein the precursor comprises polycyclic aromatic hydrocarbon.

### Claim 12 (depends on 1)

The method of claim 1, wherein the one or more organosilanes comprise (N,N-dimethylamino)trimethylsilane.

### Claim 13 (depends on 1)

The method of claim 1, wherein the silicon particles are suspended in liquid comprising the one or more organosilanes.

### Claim 14 (depends on 1)

The method of claim 1, wherein the silicon particles are exposed to one or more organosilane vapors.

### Claim 15 (depends on 1)

The method of claim 1, wherein the mixture comprises the one or more organosilanes.

### Claim 16 (depends on 1)

The method of claim 1, wherein the composite material film comprises the silicon particles at about 50% to about 99% by weight.

### Claim 17 (depends on 1)

The method of claim 1, wherein the composite material film is electrochemically active.

### Claim 18 (depends on 1)

The method of claim 1, wherein at least one of the one or more types of carbon phases is a continuous phase that holds the composite material film.

### Claim 19 (depends on 1)

A method of forming a battery electrode, wherein the electrode comprises the composite material film of claim 1.

### Claim 20 (depends on 19)

The method of claim 19, wherein the electrode is an anode.

### Claim 21

A method of forming a composite material film, the method comprising:
providing a mixture comprising a precursor and silane-treated silicon particles; and
pyrolysing the mixture to convert the precursor into one or more carbon phases to form the composite material film with the silicon particles distributed throughout the composite material film, wherein:
silane-treated silicon particles comprise silicon particles treated with one or more organosilanes;
the one or more organosilanes comprise one or more silanols, silyl ethers, silyl chlorides, dialkylaminosilanes, silyl hydrides, or cyclic azasilanes; and
the one or more organosilanes comprise (N,N-dimethylamino)trimethylsilane.

### Claim 22 (depends on 21)

The method of claim 21, wherein the silane-treated silicon particles comprise silicon oxide surfaces reacted with the one or more organosilanes.

### Claim 23 (depends on 21)

The method of claim 21, wherein the one or more organosilanes comprise one or more aminoalkyl functional groups.

### Claim 24 (depends on 23)

The method of claim 23, wherein the one or more organosilanes comprise 3-aminopropyltriethoxysilane, N-(2-aminoethyl)-3-aminopropyltrimethoxysilane, or 2,2-dimethoxy-1,6-diaza-2-silacyclooctane.

### Claim 25 (depends on 23)

The method of claim 23, wherein the precursor comprises polyimide.

### Claim 26 (depends on 21)

The method of claim 21, wherein the one or more organosilanes comprise an epoxide linker.

### Claim 27 (depends on 26)

The method of claim 26, wherein the epoxide linker comprises 5,6-epoxyhexyltriethoxysilane.

### Claim 28 (depends on 21)

The method of claim 21, wherein the precursor comprises a phenolic resin.

### Claim 29 (depends on 21)

The method of claim 21, wherein the one or more organosilanes comprise an aromatic functional group.

### Claim 30 (depends on 29)

The method of claim 29, wherein the one or more organosilanes comprise benzyltriethoxysilane.

### Claim 31 (depends on 21)

The method of claim 21, wherein the precursor comprises polycyclic aromatic hydrocarbon.

### Claim 32 (depends on 21)

The method of claim 21, wherein the silicon particles are suspended in liquid comprising the one or more organosilanes.

### Claim 33 (depends on 21)

The method of claim 21, wherein the silicon particles are exposed to one or more organosilane vapors.

### Claim 34 (depends on 21)

The method of claim 21, wherein the mixture comprises the one or more organosilanes.

### Claim 35 (depends on 21)

The method of claim 21, wherein the composite material film comprises the silicon particles at about 50% to about 99% by weight.

### Claim 36 (depends on 21)

The method of claim 21, wherein the composite material film is electrochemically active.

### Claim 37 (depends on 21)

The method of claim 21, wherein at least one of the one or more types of carbon phases is a continuous phase that holds the composite material film.

### Claim 38 (depends on 21)

A method of forming a battery electrode, wherein the electrode comprises the composite material film of claim 21.

### Claim 39 (depends on 38)

The method of claim 38, wherein the electrode is an anode.

### Claim 40

A method of forming a composite material film, the method comprising:
providing a mixture comprising a precursor and silane-treated silicon particles; and
pyrolysing the mixture to convert the precursor into one or more carbon phases to form the composite material film with the silicon particles distributed throughout the composite material film, wherein:
silane-treated silicon particles comprise silicon particles treated with one or more organosilanes; and
the silicon particles are exposed to one or more organosilane vapors.

### Claim 41 (depends on 40)

The method of claim 40, wherein the silane-treated silicon particles comprise silicon oxide surfaces reacted with the one or more organosilanes.

### Claim 42 (depends on 40)

The method of claim 40, wherein the one or more organosilanes comprise one or more silanols, silyl ethers, silyl chlorides, dialkylaminosilanes, silyl hydrides, or cyclic azasilanes.

### Claim 43 (depends on 42)

The method of claim 42, wherein the one or more organosilanes comprise one or more aminoalkyl functional groups.

### Claim 44 (depends on 43)

The method of claim 43, wherein the one or more organosilanes comprise 3-aminopropyltriethoxysilane, N-(2-aminoethyl)-3-aminopropyltrimethoxysilane, or 2,2-dimethoxy-1,6-diaza-2-silacyclooctane.

### Claim 45 (depends on 43)

The method of claim 43, wherein the precursor comprises polyimide.

### Claim 46 (depends on 42)

The method of claim 42, wherein the one or more organosilanes comprise an epoxide linker.

### Claim 47 (depends on 46)

The method of claim 46, wherein the epoxide linker comprises 5,6-epoxyhexyltriethoxysilane.

### Claim 48 (depends on 46)

The method of claim 46, wherein the precursor comprises a phenolic resin.

### Claim 49 (depends on 42)

The method of claim 42, wherein the one or more organosilanes comprise an aromatic functional group.

### Claim 50 (depends on 49)

The method of claim 49, wherein the one or more organosilanes comprise benzyltriethoxysilane.

### Claim 51 (depends on 49)

The method of claim 49, wherein the precursor comprises polycyclic aromatic hydrocarbon.

### Claim 52 (depends on 40)

The method of claim 40, wherein the silicon particles are suspended in liquid comprising the one or more organosilanes.

### Claim 53 (depends on 40)

The method of claim 40, wherein the mixture comprises the one or more organosilanes.

### Claim 54 (depends on 40)

The method of claim 40, wherein the composite material film comprises the silicon particles at about 50% to about 99% by weight.

### Claim 55 (depends on 40)

The method of claim 40, wherein the composite material film is electrochemically active.

### Claim 56 (depends on 40)

The method of claim 40, wherein at least one of the one or more types of carbon phases is a continuous phase that holds the composite material film.

### Claim 57 (depends on 40)

A method of forming a battery electrode, wherein the electrode comprises the composite material film of claim 40.

### Claim 58 (depends on 57)

The method of claim 57, wherein the electrode is an anode.
