# US 11,898,261 B2 · Method for manufacturing graphene-coated object, negative electrode of secondary battery including graphene-coated object, and secondary battery including the negative electrode

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- Number: US 11,898,261 B2
- Document ID: US11898261B2
- Status: Granted
- Kind: B2
- Application number: 17/569,540
- Filed: 2022-01-06
- Published: 2022-04-28
- Granted: 2024-02-13
- Earliest claimed: 2011-08-19
- Assignees: Semiconductor Energy Laboratory Co., Ltd.
- Applicants: Semiconductor Energy Laboratory Co., Ltd.
- Inventors: Teppei Oguni; Takeshi Osada; Toshihiko Takeuchi
- Web page: https://patentgrep.com/patent/US11898261B2

## CPC

- C25D 13/02: with inorganic material
- B82Y 30/00: Nanotechnology for materials or surface science, e.g. nanocomposites
- C25D 13/22: Servicing or operating {apparatus or multistep processes}
- H01M 4/0416: {involving impregnation with a solution, dispersion, paste or dry powder (H01M4/0438 takes precedence)}
- H01M 4/0452: {from solutions}
- H01M 4/13: Electrodes for accumulators with non-aqueous electrolyte, e.g. for lithium-accumulators; Processes of manufacture thereof
- 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 4/139: Processes of manufacture
- H01M 4/1393: of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M 4/1395: of electrodes based on metals, Si or alloys
- H01M 4/366: {as layered products}
- 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
- C25D: PROCESSES FOR THE ELECTROLYTIC OR ELECTROPHORETIC PRODUCTION OF COATINGS; ELECTROFORMING; APPARATUS THEREFOR
- B82Y: SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- 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

To form graphene to a practically even thickness on an object having an uneven surface or a complex surface, in particular, an object having a surface with a three-dimensional structure due to complex unevenness, or an object having a curved surface. The object and an electrode are immersed in a graphene oxide solution, and voltage is applied between the object and the electrode. At this time, the object serves as an anode. Graphene oxide is attracted to the anode because of being negatively charged, and deposited on the surface of the object to have a practically even thickness. A portion where graphene oxide is deposited is unlikely coated with another graphene oxide. Thus, deposited graphene oxide is reduced to graphene, whereby graphene can be formed to have a practically even thickness on an object having surface with complex unevenness.

## Claims

### Claim 1

An electrode comprising:
an object comprising silicon and an oxide; and
a film-like carbon-based material on the object,
wherein the film-like carbon-based material includes a plurality of sheets of graphene, and
wherein the object comprises a nonconductive film between the silicon and the film-like carbon-based material.

### Claim 2 (depends on 1)

The electrode according to claim 1,
wherein the object has a spherical shape or a semispherical shape.

### Claim 3 (depends on 1)

The electrode according to claim 1,
wherein the object has a depression on the film-like carbon-based material, and
wherein the object has a projection on the film-like carbon-based material.

### Claim 4

An electrode comprising:
a first object comprising silicon and an oxide;
a second object comprising silicon and an oxide; and
a film-like carbon-based material on the first object and the second object,
wherein the film-like carbon-based material comprising graphene, and
wherein the first object comprises a nonconductive film between the silicon and the film-like carbon-based material.

### Claim 5 (depends on 4)

The electrode according to claim 4,
wherein the film-like carbon-based material has a substantially even thickness.

### Claim 6 (depends on 4)

The electrode according to claim 4,
wherein each of the first object and the second object has a spherical shape or a semispherical shape.

### Claim 7 (depends on 6)

The electrode according to claim 6,
wherein the film-like carbon-based material a substantially even thickness also on the depression and the projection.

### Claim 8 (depends on 1)

The electrode according to claim 1,
wherein the nonconductive film comprises oxide.

### Claim 9 (depends on 4)

The electrode according to claim 4,
wherein the nonconductive film comprises oxide.
