# US 10,766,772 B2 · Method for preparing three-dimensional graphene structure and energy storage device

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- Number: US 10,766,772 B2
- Document ID: US10766772B2
- Status: Granted
- Kind: B2
- Application number: 15/803,162
- Filed: 2017-11-03
- Published: 2018-05-10
- Granted: 2020-09-08
- Earliest claimed: 2016-11-04
- Assignees: Electronics and Telecommunications Research Institute; Gachon University of Industry-Academic Cooperation Foundation
- Applicants: Electronics and Telecommunications Research Institute; Gachon University of Industry-Academic Cooperation Foundation
- Inventors: Tae-Young Kim; In-Kyu You; Bit Na Kim; In Gyoo Kim; Sung-Hoon Jung; Seung-Jun Park
- Web page: https://patentgrep.com/patent/US10766772B2

## CPC

- C01B 32/198: Graphene oxide
- C01B 32/184: Preparation
- H01G 11/24: characterised by structural features of the materials making up or comprised in the electrodes, e.g. form, surface area or porosity; characterised by the structural features of powders or particles used therefor
- H01G 11/32: Carbon-based
- H01G 11/34: characterised by carbonisation or activation of carbon
- H01G 11/86: specially adapted for electrodes (carbonisation or activation of carbon for the manufacture of electrodes H01G11/34)
- H01M 4/366: {as layered products}
- H01M 4/625: {Carbon or graphite}
- C01P 2004/30: extending in three dimensions
- Y02E 60/10: Energy storage using batteries
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- H01G: CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE (selection of specified materials as dielectric H01B3/00; capacitors having potential barriers H10D1/62, H10K10/10)
- 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

## Abstract

A method for preparing a three-dimensional graphene structure, and an energy storage device are provided, the method including forming a graphene precursor by heating a carbohydrate and a gas generator, forming a graphene structure having a cavity therein by carbonizing the graphene precursor, and forming nanopores in the graphene structure, wherein the nanopores pass through an outer surface and an inner surface of the graphene structure, and are connected with the cavity.

## Claims

### Claim 1

A method for preparing a three-dimensional graphene structure, the method comprising:
forming a graphene precursor by heating a carbohydrate and a gas generator;
forming a graphene structure having a cavity therein by carbonizing the graphene precursor, the cavity having an average diameter of about 1 μm to 1 mm; and
forming nanopores in the graphene structure, wherein the nanopores pass through an outer surface and an inner surface of the graphene structure and are connected with the cavity.

### Claim 2 (depends on 1)

The method of claim 1, wherein the forming of the nanopores includes:
forming a mixture by adding an activating agent to the graphene structure; and
heat treating the mixture.

### Claim 3 (depends on 2)

The method of claim 2, wherein the activating agent includes at least one among potassium hydroxide (KOH), sodium hydroxide, phosphoric acid (H3PO4), and zinc chloride (ZnCl2).

### Claim 4 (depends on 2)

The method of claim 2, wherein the heat treatment of the mixture is carried out at temperature conditions of about 600° C. to 1000° C.

### Claim 5 (depends on 2)

The method of claim 2, wherein the forming of the nanopores further includes providing a reaction gas on the graphene structure at temperature conditions of 600° C. to 1000° C.

### Claim 6 (depends on 1)

The method of claim 1, wherein the forming of the nanopores includes providing a reaction gas on the graphene structure.

### Claim 7 (depends on 6)

The method of claim 6, wherein:
the reaction gas is provided on the graphene structure at temperature conditions of 600° C. to 1000° C.; and
the reaction gas includes carbon dioxide (CO2).

### Claim 8 (depends on 6)

The method of claim 6, wherein the carbonization of the graphene precursor is carried out at temperature conditions of about 800° C. to 1400° C.

### Claim 9 (depends on 1)

The method of claim 1, wherein the graphene structure includes a plurality of graphenes stacked.

### Claim 10 (depends on 1)

The method of claim 1, wherein
the nanopores have an average diameter of about 0.1 nm to 50 nm.

### Claim 11

An energy storage device comprising:
a first electrode structure including a first current collector and a first graphene structure disposed on the first current collector, in which the first graphene structure has a first cavity therein, the first cavity having an average diameter of about 1 μm to 1 mm, and first nanopores extending through an outer surface and an inner surface of the first graphene structure to be connected with the first cavity;
a second electrode structure spaced apart from the first electrode structure and including a second current collector and a second graphene structure disposed on the second current collector, wherein the second graphene structure has a second cavity therein, the second cavity having an average diameter of about 1 μm to 1 mm, and second nanopores extending through an outer surface and an inner surface of the second graphene structure to be connected with the second cavity;
an electrolyte interposed between the first electrode structure and the second electrode structure; and
a separation film in the electrolyte,
wherein the electrolyte is provided in the first cavity, the first nanopores, the second cavity, and the second nanopores.

### Claim 12 (depends on 11)

The energy storage device of claim 11, wherein the electrolyte physically contacts the inner surface and the outer surface of the first graphene structure, and the inner surface and the outer surface of the second graphene structure.

### Claim 13 (depends on 11)

The energy storage device of claim 11, wherein the first graphene structure is electrically connected with the first current collector.

### Claim 14 (depends on 1)

The method of claims 1, wherein forming the graphene precursor is performed by heating the carbohydrate and the gas generator at a temperature of about 250° C. to 300° C.

### Claim 15 (depends on 1)

The method of claims 1, wherein the graphene structure has a specific surface area of about 1800 m2/g to 3000 m2/g.
