# US 10,370,774 B2 · Chemical vapor deposition growth of graphene

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- Number: US 10,370,774 B2
- Document ID: US10370774B2
- Status: Granted
- Kind: B2
- Application number: 14/759,134
- Filed: 2014-01-08
- Published: 2015-11-26
- Granted: 2019-08-06
- Earliest claimed: 2013-01-09
- Assignees: The Regents of the University of California
- Applicants: The Regents of the University of California
- Inventors: Xiangfeng Duan; Hailong Zhou
- Web page: https://patentgrep.com/patent/US10370774B2

## CPC

- C30B 25/186: {being specially pre-treated by, e.g. chemical or physical means}
- C01B 32/186: by chemical vapour deposition [CVD]
- C30B 29/02: Elements
- C01B 2204/02: Single layer graphene
- C01B 2204/32: Size or surface area
- C30B: SINGLE-CRYSTAL GROWTH (by using ultra-high pressure, e.g. for the formation of diamonds, B01J3/06); UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL (zone-refining of metals or alloys C22B); PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE (casting of metals, casting of other substances by the same processes or devices B22D; working of plastics B29; modifying the physical structure of metals or alloys C21D, C22F); SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE (for producing semiconductor devices or parts thereof H10); APPARATUS THEREFOR
- C01B: NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; {METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C}

## Abstract

A process of growing graphene includes: (1) providing a metal substrate; (2) annealing the metal substrate up to a growth temperature for an annealing time period and in the presence of a non-reducing gas; and (3) introducing a gas mixture to grow graphene over the metal substrate. The gas mixture includes a first gas and a second gas that is a carbon-containing precursor, a molar ratio of the first gas and the second gas is at least 100, and introducing the gas mixture is carried out at a pressure up to 100 mbar.

## Claims

### Claim 1

A process of growing graphene, comprising:
providing a metal substrate;
annealing the metal substrate up to a growth temperature for an annealing time period and in the presence of a non-reducing gas; and
introducing a gas mixture to grow graphene over the metal substrate, wherein the gas mixture includes a first gas that is hydrogen, and a second gas that is a carbon-containing precursor, a molar ratio of the first gas and the second gas is at least 100, and introducing the gas mixture is carried out at a pressure up to 100 mbar,
wherein the graphene is a single crystalline, monolayer graphene domain having a lateral size of at least 2.4 mm.

### Claim 2 (depends on 1)

The process of claim 1, wherein the metal substrate is a copper substrate.

### Claim 3 (depends on 1)

The process of claim 1, wherein the growth temperature is in the range of 900° C. to 1,200° C.

### Claim 4 (depends on 1)

The process of claim 1, wherein the annealing time period is less than 1 hour.

### Claim 5 (depends on 1)

The process of claim 1, wherein the non-reducing gas includes argon.

### Claim 6 (depends on 1)

The process of claim 1, wherein annealing the metal substrate is carried out in the absence of the first gas and the second gas.

### Claim 7 (depends on 1)

The process of claim 1, wherein the second gas is methane.

### Claim 8 (depends on 1)

The process of claim 1, wherein the molar ratio of the first gas and the second gas is at least 500.

### Claim 9 (depends on 1)

The process of claim 1, wherein the molar ratio of the first gas and the second gas is at least 1,000.

### Claim 10 (depends on 1)

The process of claim 1, wherein introducing the gas mixture is carried out at the pressure up to 10 mbar.

### Claim 11 (depends on 1)

The process of claim 1, wherein introducing the gas mixture is carried out at the pressure up to 5 mbar.

### Claim 12 (depends on 1)

The process of claim 1, wherein introducing the gas mixture is carried out subsequent to annealing the metal substrate.

### Claim 13 (depends on 1)

The process of claim 1, wherein the graphene is a first graphene layer, and further comprising growing a second graphene layer over the first graphene layer.

### Claim 14 (depends on 1)

The process of claim 1, wherein the non-reducing gas constitutes at least 95% by mole of all gases to which the metal substrate is exposed during annealing.

### Claim 15 (depends on 1)

The process of claim 1, wherein the non-reducing gas constitutes at least 99% by mole of all gases to which the metal substrate is exposed during annealing.

### Claim 16 (depends on 1)

The process of claim 1, wherein annealing the metal substrate is carried out in the absence of hydrogen.

### Claim 17 (depends on 1)

The process of claim 1, wherein the lateral size of the single crystalline, monolayer graphene domain is at least 3 mm.