# US 2014/0191166 A1 · Method for forming vapor grown graphite fibers composition and mixture formed by the same and applications thereof

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- Number: US 2014/0191166 A1
- Document ID: US20140191166A1
- Status: Published application
- Kind: A1
- Application number: 14/207,524
- Filed: 2014-03-12
- Published: 2014-07-10
- Earliest claimed: 2012-08-13
- Assignees: Yongyu Applied Technology Material Co., Ltd
- Applicants: Yongyu Applied Technology Material Co., Ltd
- Inventors: Chun-Shan WANG; Teng-Hui WANG
- Web page: https://patentgrep.com/patent/US20140191166A1

## CPC

- H01B 1/24: the conductive material comprising carbon-silicon compounds, carbon or silicon
- C01B 32/20: Graphite
- C01B 32/205: Preparation
- C08K 3/04: Carbon
- C08K 7/06: Elements
- D01F 9/127: by thermal decomposition of hydrocarbon gases or vapours {or other carbon-containing compounds in the form of gas or vapour, e.g. carbon monoxide, alcohols}
- H01B 1/04: mainly consisting of carbon-silicon compounds, carbon or silicon
- B82Y 30/00: Nanotechnology for materials or surface science, e.g. nanocomposites
- B82Y 40/00: Manufacture or treatment of nanostructures
- H01B: CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES (selection for magnetic properties H01F1/00; waveguides H01P {; printed circuits H05K})
- 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)
- D01F: CHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
- B82Y: SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES

## Abstract

A method for forming a vapor-grown graphite fibers (VGGF) composition and a VGGF composition formed by the method are provided. In this method, a transition metal compound catalyst and three organic co-catalysts are mixed with a hydrocarbon compound, and then are delivered into a tubular reactor and pyrolized and graphitized to produce the VGGF composition. The VGGF composition includes a carbon ingredient containing a carbon content of at least 99.9 wt %. The carbon ingredient has a graphitization degree of at least 75%, and the carbon ingredient includes non-fibrous carbon and fibrous VGGF, wherein an area ratio of the non-fibrous carbon to the fibrous VGGF is about equal to or smaller than 5%. The fibrous VGGF include graphite fibers having a 3-D linkage structure, wherein the content of the graphite fibers having the 3-D linkage structure in the fibrous VGGF is about between 5 area % and 50 area %.

## Claims

### Claim 1

A method for forming a vapor-grown graphite fibers (VGGF) composition, the method comprising:
preparing a liquid raw material by mixing a hydrocarbon compound, a transition metal compound catalyst and a co-catalyst mixture comprising a coordinating ligand containing a keto-enol tautomerism, an organic compound containing a polysulfide group, a bicyclic organic compound containing nitrogen;
vaporizing the liquid raw material, thereby forming raw material gas; and
introducing the raw material gas and hydrogen gas into a tubular reactor for performing a pyrolysis reaction, thereby producing a vapor-grown carbon fibers composition having pure carbon fibers with three-dimensional (3-D) linkage structures; and
performing a high-temperature graphitization treatment on the VGCF, thereby forming the VGGF composition.

### Claim 2 (depends on 1)

The method of claim 1, wherein the hydrocarbon compound is selected from the group consisting of an aliphatic hydrocarbon compound, an aromatic hydrocarbon compound and a combination thereof, and the aliphatic hydrocarbon is selected from the group consisting of methane, ethylene, styrene, acetylene, propane, liquefied petroleum gas, butane, butene, butadiene and a combination thereof, and the aromatic hydrocarbons is selected from the group consisting of benzene, toluene, xylene, styrene and a combination thereof.

### Claim 3 (depends on 1)

The method of claim 1, wherein the transition metal compound catalyst is ferrocene, and the content of the transition metal compound catalyst in the liquid raw material is substantially between 0.1 wt % and 10 wt %.

### Claim 4 (depends on 1)

The method of claim 1, wherein the coordinating ligand containing the keto-enol tautomerism has a molecular structure of Formula (I):
where R is an alkyl group of C1˜C6

### Claim 5 (depends on 1)

The method of claim 1, wherein the coordinating ligand containing the keto-enol tautomerism is ethyl 3-oxobutanoate, and the content of the coordination compound containing the keto-enol tautomerism in the liquid raw material is substantially between 0.5 wt % and 5 wt %.

### Claim 6 (depends on 1)

The method of claim 1, wherein the organic compound containing the polysulfide group has a molecular structure containing at least three sulfur atoms.

### Claim 7 (depends on 1)

The method of claim 1, wherein the organic compound containing the polysulfide group is Bis(dimethylthiocarbamyl)sulfide, and the content of the organic compound containing the polysulfide group in the liquid raw material is substantially between 0.1 wt % and 2 wt %.

### Claim 8 (depends on 1)

The method of claim 1, wherein the bicyclic organic compound containing nitrogen has a molecular structure containing at least one nitrogen atom.

### Claim 9 (depends on 1)

The method of claim 1, wherein the bicyclic organic compound containing nitrogen is Triethylenediamine, and the content of the bicyclic organic compound containing nitrogen in the liquid raw material is substantially between 0.1 wt % and 2 wt %.

### Claim 10 (depends on 1)

The method of claim 1, wherein a reaction temperature of the pyrolysis reaction is substantially between 800° C. and 1300° C.

### Claim 11 (depends on 1)

The method of claim 1, wherein a graphitization temperature of the high-temperature graphitization treatment is substantially between 2800° C. and 3000° C.

### Claim 12 (depends on 1)

A VGGF composition formed by the method of claim 1, the VGGF composition comprising
a carbon ingredient containing a carbon content of at least 99.9 wt %, wherein the carbon ingredient has a graphitization degree of at least 75%, the carbon ingredient comprising:
fibrous VGGF, comprising:
graphite fibers having 3-D linkage structures, wherein the content of the graphite fibers having the 3-D linkage structure in the fibrous VGGF measured by a scanning electron microscopy (SEM) is substantially between 5 area % and 50 area %; and
non-fibrous carbon, wherein an area ratio of the non-fibrous carbon to the fibrous VGGF measured by the SEM is substantially equal to or smaller than 5%.

### Claim 13 (depends on 12)

The VGGF composition of claim 12, wherein an averaged outer diameter of the fibrous VGGF is in a range substantially between 50 nm and 200 nm, and an averaged aspect ratio of the fibrous VGGF is in a range to substantially between 10 and 5000.

### Claim 14 (depends on 12)

The VGGF composition of claim 12, wherein, when a thermogravimetric analyzer (TGA) is used for analysis under test conditions including a temperature increasing rate of 10° C./min and an air flow rate ranged between 10 ml/min and 20 ml/min, a thermal decomposition onset temperature of the VGGF composition is substantially greater than 700° C.

### Claim 15 (depends on 12)

The VGGF composition of claim 12, wherein the VGGF composition has a water content of substantially less than 0.2 wt %.

### Claim 16 (depends on 12)

The VGGF composition of claim 12, wherein the VGGF composition has a metal content of substantially less than 200 ppm.

### Claim 17 (depends on 12)

The VGGF composition of claim 12, wherein the non-fibrous carbon is connected to, overlapped with or separated from the fibrous VGGF.

### Claim 18 (depends on 12)

The VGGF composition of claim 12, wherein the fibrous VGGF comprises an elongated hollow multi-layered structure formed by wrapping graphite having a carbon hexagonal net plane.

### Claim 19 (depends on 12)

A mixture, comprising:
a rubber, a plastic, a metal oxide or a carbon material; and
a VGGF composition of claim 12.