# US 11,111,147 B2 · Carbon nanotube composite structure and method for making the same

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- Number: US 11,111,147 B2
- Document ID: US11111147B2
- Status: Granted
- Kind: B2
- Application number: 16/899,800
- Filed: 2020-06-12
- Published: 2020-10-01
- Granted: 2021-09-07
- Earliest claimed: 2018-08-24
- Assignees: Tsinghua University; Hon Hai Precision Industry Co., Ltd.
- Applicants: Tsinghua University; Hon Hai Precision Industry Co., Ltd.
- Inventors: Yue-Gang Zhang; Lu-Jie Jia; Jian Wang; Yang Wu; Shou-Shan Fan
- Web page: https://patentgrep.com/patent/US11111147B2

## CPC

- C01B 32/174: Derivatisation; Solubilisation; Dispersion in solvents
- B82Y 30/00: Nanotechnology for materials or surface science, e.g. nanocomposites
- B82Y 40/00: Manufacture or treatment of nanostructures
- C01B 2202/08: Aligned nanotubes
- C01B 2202/22: Electronic properties
- C01B 2202/26: Mechanical properties
- C01B 2202/34: Length
- C01B 2202/36: Diameter
- C01P 2004/03: obtained by SEM
- C01P 2004/04: obtained by TEM, STEM, STM or AFM
- C01P 2004/13: Nanotubes
- C01P 2006/40: Electric properties
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}
- B82Y: SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- C01P: INDEXING SCHEME RELATING TO STRUCTURAL AND PHYSICAL ASPECTS OF SOLID INORGANIC COMPOUNDS

## Abstract

A method for making a carbon nanotube composite structure includes the following steps: dispersing a plurality of carbon nanotubes in water, to form a carbon nanotube dispersion; adding an aniline solution into the carbon nanotube dispersion, to form a mixed solution; adding an initiator into the mixed solution, to form a carbon nanotube composite structure preform; freeze-drying the carbon nanotube composite structure preform in a vacuum environment; and carbonizing the carbon nanotube composite structure preform in a protective gas after freeze-drying. The present application also relates to the carbon nanotube composite structure.

## Claims

### Claim 1

A carbon nanotube composite structure, comprising:
a carbon nanotube network structure comprising a plurality of carbon nanotubes entangled to each other; and
a sulfur, nitrogen-codoped carbon layer coated on outer surfaces of the plurality of carbon nanotubes and intersections of the plurality of carbon nanotubes, and the plurality of carbon nanotubes bonded together at the intersections by the sulfur, nitrogen-codoped carbon layer; the sulfur, nitrogen-codoped carbon layer consists of nitrogen elements (N), sulfur elements (S), and carbon elements (C); an atomic percentage of the carbon elements, the nitrogen elements, and the sulfur elements is C:N:S=95.4%:3.2%:1.4%; and a polyaniline is a dopant source of the carbon elements and the nitrogen elements, and an ammonium persulphate is both an initiator that initiates the polyaniline and a dopant source of the nitrogen element and the sulfur element.

### Claim 2 (depends on 1)

The carbon nanotube composite structure of claim 1, wherein the carbon nanotube network structure is porous and comprises pores between the plurality of carbon nanotubes.

### Claim 3 (depends on 1)

The carbon nanotube composite structure of claim 1, wherein the sulfur, nitrogen-codoped carbon layer covers entire outer surfaces of each of the plurality of carbon nanotubes.

### Claim 4 (depends on 1)

The carbon nanotube composite structure of claim 1, wherein the plurality of carbon nanotubes are single-walled, double-walled, multi-walled carbon nanotubes, or their combinations.

### Claim 5 (depends on 1)

The carbon nanotube composite structure of claim 1, wherein diameters of the plurality of carbon nanotubes range from about 20 nanometers to about 30 nanometers.

### Claim 6 (depends on 1)

The carbon nanotube composite structure of claim 1, wherein the sulfur, nitrogen-codoped carbon layer is formed by carbonizing a carbon nanotube composite structure preform comprising carbon nanotubes, the polyaniline, and the initiator.

### Claim 7 (depends on 1)

The carbon nanotube composite structure of claim 1, wherein the sulfur, nitrogen-codoped carbon layer comprises sulfur elements formed by carbonizing the ammonium persulphate.

### Claim 8 (depends on 1)

The carbon nanotube composite structure of claim 1, wherein the carbon nanotube composite structure consists of the carbon nanotube network structure and the sulfur, nitrogen-codoped carbon layer.

### Claim 9 (depends on 1)

The carbon nanotube composite structure of claim 1, wherein the sulfur, nitrogen-codoped carbon layer is formed by carbonizing a carbon nanotube composite structure preform consisting of carbon nanotubes, the polyaniline, and the initiator; the atomic percentage of the carbon elements, the nitrogen elements, and the sulfur elements is C:N:S=95.4%:3.2%:1.4%; and a Young's modulus of the carbon nanotube composite structure is 810.12 MPa.

### Claim 10

A carbon nanotube composite structure, comprising:
a carbon nanotube network structure comprising a plurality of carbon nanotubes; and
a sulfur, nitrogen-codoped carbon layer coated on outer surfaces of the plurality of carbon nanotubes, wherein the sulfur, nitrogen-codoped carbon layer comprises nitrogen elements (N), sulfur elements (S), and carbon elements (C); a polyaniline is a dopant source of the carbon elements and the nitrogen elements, and an ammonium persulphate is both an initiator that initiates the polyaniline and a dopant source of the nitrogen element and the sulfur element: the sulfur, nitrogen-codoped carbon layer is formed by carbonizing a carbon nanotube composite structure preform consisting of carbon nanotubes, the polyaniline, and the initiator; the atomic percentage of the carbon elements, the nitrogen elements, and the sulfur elements is C:N:S=95.4%:3.2%:1.4%; and a Young's modulus of the carbon nanotube composite structure is 810.12 MPa.

### Claim 11 (depends on 10)

The carbon nanotube composite structure of claim 10, wherein the carbon nanotube network structure is porous and comprises pores between the plurality of carbon nanotubes.

### Claim 12 (depends on 10)

The carbon nanotube composite structure of claim 10, wherein the sulfur, nitrogen-codoped carbon layer covers entire outer surfaces of each of the plurality of carbon nanotubes.

### Claim 13 (depends on 10)

The carbon nanotube composite structure of claim 10, wherein an atomic percentage of the carbon elements, the nitrogen elements, and the sulfur elements is C:N:S=95.4%:3.2%:1.4%.

### Claim 14 (depends on 10)

The carbon nanotube composite structure of claim 10, wherein the plurality of carbon nanotubes are single-walled, double-walled, multi-walled carbon nanotubes, or their combinations.

### Claim 15 (depends on 10)

The carbon nanotube composite structure of claim 10, wherein diameters of the plurality of carbon nanotubes range from about 20 nanometers to about 30 nanometers.

### Claim 16 (depends on 10)

The carbon nanotube composite structure of claim 10, wherein the sulfur, nitrogen-codoped carbon layer is formed by carbonizing a carbon nanotube composite structure preform comprising carbon nanotubes, the polyaniline, and the initiator.

### Claim 17 (depends on 10)

The carbon nanotube composite structure of claim 10, wherein the sulfur, nitrogen-codoped carbon layer comprises sulfur elements formed by carbonizing the ammonium persulphate.

### Claim 18 (depends on 10)

The carbon nanotube composite structure of claim 10, wherein the plurality of carbon nanotubes are entangled to each other.