# US 10,312,503 B2 · Cohesive assembly of carbon and its application

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- Number: US 10,312,503 B2
- Document ID: US10312503B2
- Status: Granted
- Kind: B2
- Application number: 15/444,631
- Filed: 2017-02-28
- Published: 2017-07-06
- Granted: 2019-06-04
- Earliest claimed: 2011-06-20
- Assignees: Yazaki Corporation
- Applicants: Yazaki Corporation
- Inventors: Satyabrata Raychaudhuri; Yongan Yan; Leonid Grigorian
- Web page: https://patentgrep.com/patent/US10312503B2

## CPC

- H01M 4/133: Electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
- B82Y 30/00: Nanotechnology for materials or surface science, e.g. nanocomposites
- B82Y 40/00: Manufacture or treatment of nanostructures
- C01B 32/05: Preparation or purification of carbon not covered by groups C01B32/15, C01B32/20, C01B32/25, C01B32/30
- C01B 32/159: single-walled
- C01B 32/168: After-treatment
- C01B 32/174: Derivatisation; Solubilisation; Dispersion in solvents
- H01G 11/36: Nanostructures, e.g. nanofibres, nanotubes or fullerenes
- H01G 11/38: Carbon pastes or blends; Binders or additives therein
- H01G 11/68: characterised by their material
- H01G 11/86: specially adapted for electrodes (carbonisation or activation of carbon for the manufacture of electrodes H01G11/34)
- H01M 4/0402: {Methods of deposition of the material}
- H01M 4/0404: {by coating on electrode collectors}
- H01M 4/131: Electrodes based on mixed oxides or hydroxides, or on mixtures of oxides or hydroxides, e.g. LiCoOx
- H01M 4/1393: of electrodes based on carbonaceous material, e.g. graphite-intercalation compounds or CFx
- H01M 4/525: of mixed oxides or hydroxides containing iron, cobalt or nickel for inserting or intercalating light metals, e.g. LiNiO2, LiCoO2 or LiCoOxFy
- H01M 4/5825: {Oxygenated metallic salts or polyanionic structures, e.g. borates, phosphates, silicates, olivines}
- H01M 4/587: for inserting or intercalating light metals
- H01M 4/625: {Carbon or graphite}
- H01M 4/661: {Metal or alloys, e.g. alloy coatings (H01M4/669 take precedence)}
- H01M 4/663: {containing carbon or carbonaceous materials as conductive part, e.g. graphite, carbon fibres}
- H01M 4/8605: {Porous electrodes}
- H01M 4/8807: {Gas diffusion layers}
- H01M 4/8878: {Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body}
- H01M 4/9083: {on carbon or graphite}
- H01M 8/0234: Carbonaceous material
- H01M 8/1004: characterised by membrane-electrode assemblies [MEA] (H01M8/12 takes precedence)
- H01M 8/1007: with both reactants being gaseous or vaporised (H01M8/12 takes precedence)
- H01M 10/0525: Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
- C01B 2202/02: Single-walled nanotubes
- C01B 2202/22: Electronic properties
- H01G 11/28: arranged or disposed on a current collector; Layers or phases between electrodes and current collectors, e.g. adhesives
- H01M 4/0471: {involving thermal treatment, e.g. firing, sintering, backing particulate active material, thermal decomposition, pyrolysis}
- H01M 2004/027: {Negative electrodes}
- H01M 2008/1095: {Fuel cells with polymeric electrolytes}
- H01M 2220/20: Batteries in motive systems, e.g. vehicle, ship, plane
- H01M 2220/30: Batteries in portable systems, e.g. mobile phone, laptop
- H01M 2250/20: Fuel cells in motive systems, e.g. vehicle, ship, plane
- Y02E 60/10: Energy storage using batteries
- Y02E 60/13: Energy storage using capacitors
- Y02E 60/50: Fuel cells
- Y02P 70/50: Manufacturing or production processes characterised by the final manufactured product
- Y02T 90/40: Application of hydrogen technology to transportation, e.g. using fuel cells
- Y10S 977/75: Single-walled
- Y10S 977/842: for carbon nanotubes or fullerenes
- Y10S 977/892: Liquid phase deposition
- Y10S 977/948: Energy storage/generating using nanostructure, e.g. fuel cell, battery
- H01M: PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- B82Y: SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- 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)
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02T: CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
- Y10S: TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS

## Abstract

Cohesive carbon assemblies are prepared by obtaining a carbon starting material in the form of powder, particles, flakes, or loose agglomerates, dispersing the carbon in a selected organic solvent by mechanical mixing and/or sonication, and substantially removing the organic solvent, typically by evaporation, whereby the cohesive assembly of carbon is formed. The method is suitable for preparing free-standing, monolithic assemblies of carbon nanotubes in the form of films, wafers, or discs, having high carbon packing density and low electrical resistivity. The method is suitable for preparing adherent cohesive carbon assemblies on substrates comprising various materials. The assemblies have various potential applications, such as electrodes or current collectors in electrochemical capacitors, fuel cells, and batteries, or as electromagnetic interference shielding materials.

## Claims

### Claim 1

An energy storage device comprising two electrodes separated by an electrolyte, wherein at least one electrode comprises a cohesive carbon assembly that is a monolithic structure in which carbon is uniformly distributed, wherein the cohesive carbon assembly is prepared without using a liquid halogen as a dispersing solvent to disperse a carbon starting material, and the device is a battery, a fuel cell, or an electrochemical double-layer capacitor (EDLC).

### Claim 2 (depends on 1)

The energy storage device according to claim 1, which is a fuel cell.

### Claim 3 (depends on 2)

The fuel cell according to claim 2, wherein the electrode that comprises the cohesive carbon assembly is a free-standing electrode without a metal current collector and without any binder material.

### Claim 4 (depends on 2)

The fuel cell according to claim 2, wherein the cohesive carbon assembly is in a catalyst support layer and/or in a gas diffusion layer of the electrode.

### Claim 5 (depends on 4)

The fuel cell according to claim 4, wherein the cohesive carbon assembly is 5-20 μm thick in a catalyst support layer and/or 100-300 μm thick in a gas diffusion layer of the electrode.

### Claim 6 (depends on 2)

The fuel cell according to claim 2, wherein the cohesive carbon assembly comprises SWCNT and has a total pore volume greater than 1.0 cm3/g.

### Claim 7 (depends on 1)

The energy storage device according to claim 1, which is a battery.

### Claim 8 (depends on 7)

The battery according to claim 7, further comprising a metal substrate onto which the electrode is adherent without the use of a bonding material.

### Claim 9 (depends on 7)

The battery according to claim 7, wherein an anode comprises the cohesive carbon assembly without any binder material, and a cathode comprises Li-containing oxide.

### Claim 10 (depends on 9)

The battery according to claim 9, wherein the cohesive carbon assembly comprises SWCNT.

### Claim 11 (depends on 1)

The energy storage device according to claim 1, which is an EDLC.

### Claim 12 (depends on 11)

The EDLC according to claim 11, further comprising a metal substrate onto which the electrode is adherent without the use of a bonding material.

### Claim 13

An energy storage device comprising a current collector and an electrode on one side of an electrolyte, and another current collector and another electrode on the other side of the electrolyte, wherein at least one of the two current collectors comprises a cohesive carbon assembly that is a monolithic structure in which carbon is uniformly distributed, wherein the cohesive carbon assembly is prepared without using a liquid halogen as a dispersing solvent to disperse a carbon starting material, and the device is a battery, a fuel cell, or EDLC.

### Claim 14 (depends on 13)

The energy storage device according to claim 13, wherein one of the two electrodes comprises a second cohesive carbon assembly that is a monolithic structure in which carbon is uniformly distributed, wherein the second cohesive carbon assembly is prepared without using a liquid halogen as a dispersing solvent to disperse a carbon starting material.

### Claim 15 (depends on 14)

The energy storage device according to claim 14, wherein the electrode that comprises the second cohesive carbon assembly is a free-standing electrode without other conductive material and without any binder material.