# US 2021/0172059 A1 · Method for depositing large-area graphene layer and apparatus for continuous graphene deposition

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- Number: US 2021/0172059 A1
- Document ID: US20210172059A1
- Status: Published application
- Kind: A1
- Application number: 17/116,656
- Filed: 2020-12-09
- Published: 2021-06-10
- Earliest claimed: 2019-12-10
- Assignees: Kuk-Il Graphene Co., Ltd.
- Applicants: Kuk-Il Graphene Co., Ltd
- Inventors: Dong Ho Yoon; Chul Kyu Song; Ji Hye Han; Soon Gil Yoon; Ji Ho Eom
- Web page: https://patentgrep.com/patent/US20210172059A1

## CPC

- C23C 16/26: Deposition of carbon only
- C23C 14/14: Metallic material, boron or silicon
- C23C 14/568: {Transferring the substrates through a series of coating stations (C23C14/562 takes precedence)}
- C23C 14/5826: {Treatment with charged particles (C23C14/582 takes precedence)}
- C23C 14/5846: {Reactive treatment}
- C23C 14/5873: {Removal of material}
- C23C 16/0281: {of metallic sub-layers (C23C16/029 takes precedence)}
- C23C 16/4408: {by purging residual gases from the reaction chamber or gas lines}
- C23C 16/50: using electric discharges {(generation and control of plasma in discharge tubes for surface treatment H01J37/32, H01J37/34)}
- C23C 16/545: {for coating elongated substrates}
- C23C 28/322: {only coatings of metal elements only}
- C23C 28/34: {including at least one inorganic non-metallic material layer, e.g. metal carbide, nitride, boride, silicide layer and their mixtures, enamels, phosphates and sulphates}
- C23C: COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL (making metal-coated products by extrusion B21C23/22; covering with metal by connecting pre-existing layers to articles, see the relevant places, e.g. B21D39/00, B23K; metallising of glass C03C; metallising mortars, concrete, artificial stone, ceramics or natural stone C04B41/00; enamelling of, or applying a vitreous layer to, metals C23D; treating metal surfaces or coating of metals by electrolysis or electrophoresis C25D; single-crystal film growth C30B; by metallising textiles D06M11/83; decorating textiles by locally metallising D06Q1/04)

## Abstract

A method for depositing a large-area graphene layer and an apparatus for continuous graphene deposition using the same are disclosed. The method can include forming a titanium (Ti) layer on a substrate by sputtering, reducing the titanium layer by spraying a reductant gas containing a hydrogen gas (H2) and a purge gas onto the titanium layer while moving in a first direction in relation to the substrate and exhausting the reductant gas and the purge gas. The method can also include forming graphene by spraying a reactant gas containing a graphene source and the purge gas onto the titanium layer while moving in a second direction opposite the first direction in relation to the substrate and exhausting the reactant gas and the purge gas.

## Claims

### Claim 1

A method for depositing a large-area graphene layer, the method comprising:
forming a titanium (Ti) layer on a substrate by sputtering;
reducing the titanium layer by spraying a reductant gas and a purge gas onto the titanium layer while moving in a first direction in relation to the substrate and exhausting the reductant gas and the purge gas, the reductant gas containing a hydrogen gas (H2); and
forming graphene by spraying a reactant gas and the purge gas onto the titanium layer while moving in a second direction opposite to the first direction and exhausting the reactant gas and the purge gas, the reactant gas containing a graphene source.

### Claim 2 (depends on 1)

The method of claim 1, wherein the titanium layer is reduced by generating a hydrogen plasma from the hydrogen gas and applying the hydrogen plasma,
and wherein the forming of the graphene comprises growing the graphene on the titanium layer by spraying the graphene source decomposed from a methane gas (CH4).

### Claim 3 (depends on 2)

The method of claim 2, wherein the titanium layer is reduced while moving once in the first direction,
and wherein the forming of the graphene comprises repeating:
growing graphene on the titanium layer while moving in the second direction; and
spraying an inert gas onto the titanium layer while moving in the first direction.

### Claim 4

An apparatus for continuous graphene deposition, the apparatus comprising:
a sputtering unit and an injector, the sputtering unit configured to form a titanium layer by depositing the titanium layer onto a surface of a substrate, the injector configured to grow graphene on the titanium layer,
wherein the injector comprises:
a reductant supply unit configured to supply a reductant gas to the substrate, the reductant gas containing a hydrogen gas (H2);
a reactant supply unit configured to supply a reactant gas to the substrate, the reactant gas containing a graphene source;
a purge supply unit arranged between the reductant supply unit and the reactant supply unit, the purge supply unit configured to supply a purge gas to the substrate; and
an exhaust unit configured to exhaust gases from the substrate,
and wherein the injector is configured to spray the reductant gas and the purge gas onto the titanium layer while moving in a first direction in relation to the substrate, and
wherein the injector is configured to spray the reactant gas and the purge gas onto the titanium layer while moving in a second direction opposite to the first direction.

### Claim 5 (depends on 4)

The apparatus of claim 4, wherein the reductant supply unit is configured to generate a hydrogen plasma from the hydrogen gas and apply the hydrogen plasma,
and wherein the reactant supply unit is configured to spray a graphene source decomposed from a methane gas (CH4).

### Claim 6 (depends on 5)

The apparatus of claim 5, wherein the injector is configured to move repeatedly in the first direction and the second direction in relation to the substrate in an oscillating movement, and
wherein, after the reductant supply unit performs reduction by applying the hydrogen plasma onto the titanium layer during an initial movement in the first direction in relation to the substrate,
wherein the injector is configured to repeatedly spray the graphene source and an inert gas,
wherein the injector is configured to spray the graphene source as the reactant supply unit sprays the graphene source onto the titanium layer while moving in the second direction in relation to the substrate, and
wherein the injector is configured to spray the inert gas as the reductant supply unit sprays the inert gas onto the titanium layer while moving in the first direction in relation to the substrate.

### Claim 7 (depends on 5)

The apparatus of claim 5, wherein the reactant supply unit further comprises:
an electrode rod configured to apply plasma power to decompose the methane gas and generate the graphene source; and
an electrode rod cover covering the electrode rod and configured to suppress an exposure of plasma to the substrate.

### Claim 8 (depends on 4)

The apparatus of claim 4, wherein the substrate comprises a film, wherein the apparatus further comprises a film transport unit equipped with a plurality of rollers, the film transport unit configured to supply and retrieve the film to and from the sputtering unit and the injector,
and wherein the apparatus is configured to form graphene continuously on the film by roll-to-roll processing.

### Claim 9 (depends on 8)

The apparatus of claim 8, wherein the film transport unit comprises a support roller arranged facing the injector, the support roller configured to support the film such that a surface of the film having the titanium formed thereon faces the injector,
wherein the injector has an inner curved surface formed to maintain a constant distance to the surface of the film supported by the support roller and is configured to supply the reductant gas, the reactant gas, and the purge gas to the inner curved surface,
and wherein the injector is configured to perform an oscillating movement following a circumferential direction of the support roller.

### Claim 10 (depends on 8)

The apparatus of claim 8, wherein the roll-to-roll processing comprises a film supply process, a titanium deposition process, a graphene deposition process, and a film retrieval process, wherein each process is performed separately in an independent chamber,
and wherein the chamber has a slit formed therein to allow a passage of the film and has a shutter installed thereon to adjust a width of the slit.