WO2014038803A1

WO2014038803A1 - Catalyst metal film-supporting device and method and apparatus for synthesizing multiple graphene films

Info

Publication number: WO2014038803A1
Application number: PCT/KR2013/007517
Authority: WO
Inventors: Na-Young Kim
Original assignee: Samsung Techwin Co., Ltd
Priority date: 2012-09-04
Filing date: 2013-08-22
Publication date: 2014-03-13
Also published as: KR20140030977A

Abstract

A catalyst metal film-supporting device, an apparatus for synthesizing multiple graphene films including the catalyst metal film-supporting device, and a method of synthesizing multiple graphene films. The catalyst metal film-supporting device includes: a base unit; at least one support unit coupled to the base unit and extending in one direction so that the plurality of catalyst metal films are inserted and disposed; and spacers coupled to the at least one support unit between the plurality of catalyst metal films so that the plurality of catalyst metal films are prevented from contacting each other.

Description

CATALYST METAL FILM-SUPPORTING DEVICE AND METHOD AND APPARATUS FOR SYNTHESIZING MULTIPLE GRAPHENE FILMS

The present invention relates to a method and apparatus for synthesizing graphene, and more particularly, to a catalyst metal film-supporting device, an apparatus for synthesizing multiple graphene films including the catalyst metal film-supporting device, and a method of synthesizing multiple graphene films.

Currently, graphene has been prominent as a new material having high electrical conductivity, excellent chemical stability, transparency, and flexibility. In addition, chemical vapor deposition (CVD) is used to synthesize graphene. CVD for synthesizing graphene uses a method of contacting a mixture gas of argon, hydrogen, and methane with a catalyst metal in a high temperature chamber. A transient metal including copper may be used as the catalyst metal. According to CVD, graphene is synthesized on a surface of the catalyst metal, and then the catalyst metal is removed, and thus only graphene may be obtained.

The present invention provides a method and apparatus for stably synthesizing multiple graphene films using chemical vapor deposition (CVD).

According to an aspect of the present invention, there is provided a device for supporting a plurality of catalyst metal films in a chemical vapor deposition (CVD) chamber, the device including: a base unit; at least one support unit coupled to the base unit and extending in one direction so that the plurality of catalyst metal films are inserted and disposed; and spacers coupled to the at least one support unit between the plurality of catalyst metal films so that the plurality of catalyst metal films are prevented from contacting each other.

The at least one support unit may be disposed in both directions with respect to the base unit.

The base unit may include temperature sensors for measuring a temperature of the CVD chamber

The spacers may be received by the at least one support bar in a length direction of the at least one support bar.

The spacers may have spaces therein, and may be formed in shapes corresponding to boundaries of the plurality of catalyst metal films.

According to another aspect of the present invention, there is provided a device for supporting a plurality of catalyst metal films in a chemical vapor deposition (CVD) chamber, the device including: a base unit; at least one support unit coupled to the base unit and extending in one direction; and a plurality of frames coupled to at least one side of the plurality of catalyst metal film, coupled to the at least one support bar, and arranged in parallel to each other.

The plurality of frames may include through spaces therein, wherein the plurality of catalyst metal films are disposed in the through spaces of the plurality of frames.

The device may further include: hinge members having one sides hinge-coupled to the plurality of frames and other sides coupled to the plurality of catalyst metal films.

Gravity may act on the hinge members in a direction to which the plurality of catalyst metal films are unfolded.

The device may further include a frame holding structure including a plurality of slots accommodating the plurality of frames.

According to another aspect of the present invention, there is provided a device for supporting a plurality of catalyst metal films in a chemical vapor deposition (CVD) chamber, the device including: a frame holding structure including a plurality of slots for supporting a plurality of catalyst metal films; and a plurality of frames coupled to at least one sides of the plurality of catalyst metal films and inserted into the plurality of slots of the frame holding structure.

According to another aspect of the present invention, there is provided a multiple graphene films synthesizing apparatus including: a chemical vapor deposition (CVD) chamber including an injection unit and an ejection unit of a raw material gas; the device for supporting the plurality of catalyst metal films disposed in the CVD chamber and heating sources heating the inside of the CVD chamber.

The multiple graphene films synthesizing apparatus may further include: a movement support unit having at least one part disposed to come in and out the CVD chamber, wherein the device for supporting the plurality of catalyst metal films is disposed in at least a part of the movement support unit.

According to another aspect of the present invention, there is provided a multiple graphene films synthesizing method including: placing a plurality of catalyst metal films in parallel to each other in a chemical vapor deposition (CVD) chamber; placing spacers between the plurality of catalyst metal films so that the plurality of catalyst metal films are prevented from contacting each other; heating the inside of the CVD chamber; and injecting a raw material gas into the CVD chamber.

The placing of the plurality of catalyst metal films in parallel to each other in the CVD chamber may include: inserting the plurality of catalyst metal films in parallel to each other into support bars extending in one direction, and wherein the placing of the spacers between the plurality of catalyst metal films includes: coupling the spacers to the support bars between the plurality of catalyst metal films.

The spacers may be received by the support bars in a length direction of the support bars.

According to another aspect of the present invention, there is provided a multiple graphene films synthesizing method including: installing a plurality of catalyst metal films in a plurality of frames; placing the plurality of frames in which the plurality of catalyst metal films are installed in a chemical vapor deposition (CVD) chamber to be spaced apart from each other in parallel to each other; injecting a raw material gas into the CVD chamber; and heating the inside of the CVD chamber.

The placing of the plurality of frames in which the plurality of catalyst metal films may be installed in the CVD chamber to be spaced apart from each other in parallel to each other includes: preparing a frame holding structure including a plurality of slots that individually accommodate the plurality of frames, inserting the plurality of frames into the plurality of slots of the frame holding structure, and inserting the frame holding structure into the CVD chamber.

According to an embodiment of the present invention, a catalyst metal film-supporting device and a method and apparatus for synthesizing multiple graphene films may concurrently and stably synthesize multiple graphene films.

These and/or other aspects will become apparent and more readily appreciated from the following description of the embodiments, taken in conjunction with the accompanying drawings in which:

FIG. 1 is a schematic perspective view of a catalyst metal film-supporting device according to an embodiment of the present invention;

FIG. 2 is a schematic exploded perspective view of a part of the catalyst metal film-supporting device of FIG. 1;

FIG. 3 is a schematic view of a multiple graphene films synthesizing apparatus including the catalyst metal film-supporting device of FIG. 1;

FIG. 4 is a schematic flowchart of a multiple graphene films synthesizing method according to an embodiment of the present invention;

FIGS. 5A and 5B are graphs of results of a Raman analysis conducted to inspect whether graphene films are well synthesized by the multiple graphene films synthesizing apparatus of FIG. 3;

FIGS. 6A through 7D are graphs of results obtained by measuring a surface resistance of graphene synthesized by using the multiple graphene films synthesizing apparatus of FIG. 3;

FIG. 8 is a schematic exploded perspective view of a catalyst metal film-supporting device according to another embodiment of the present invention;

FIG. 9 is a schematic view of a part of a multiple graphene films synthesizing apparatus including the catalyst metal film-supporting device of FIG. 8;

FIG. 10 is a schematic view of a modification of an element of the catalyst metal film-supporting device of FIG. 8;

FIG. 11 is a schematic exploded perspective view of a catalyst metal film-supporting device according to another embodiment of the present invention;

FIG. 12 is a schematic view of a part of a multiple graphene films synthesizing apparatus including the catalyst metal film-supporting device of FIG. 11;

FIG. 13 is a schematic flowchart of a multiple graphene films synthesizing method according to another embodiment of the present invention;

FIGS. 14A and 14B are graphs of results of a Raman analysis conducted to inspect whether graphene films are synthesized well by the multiple graphene films synthesizing apparatus of FIG. 12;

FIGS. 15A through 16B are graphs of results obtained by measuring a surface resistance of graphene synthesized by using the multiple graphene films synthesizing apparatus of FIG. 12;

FIG. 17 is a schematic view of a modification of an element of the catalyst metal film-supporting device of FIG. 11;

FIG. 18 is a schematic exploded perspective view of a catalyst metal film-supporting device according to another embodiment of the present invention;

FIG. 19 is a schematic view of a part of a multiple graphene films synthesizing apparatus including the catalyst metal film-supporting device of FIG. 18;

FIG. 20 is a schematic view of an operation of the multiple graphene films synthesizing apparatus of FIG. 19; and

FIG. 21 is a schematic flowchart for explaining a multiple graphene films synthesizing method according to another embodiment of the present invention.

Reference will now be made in detail to embodiments, examples of which are illustrated in the accompanying drawings.

FIG. 1 is a schematic perspective view of a catalyst metal film-supporting device 1 according to an embodiment of the present invention. FIG. 2 is a schematic exploded perspective view of a part of the catalyst metal film-supporting device 1 of FIG. 1.

Referring to FIGS. 1 and 2, the catalyst metal film-supporting device 1 according to the present embodiment stably supports catalyst metal films 200 in a chemical vapor deposition (CVD) chamber, and includes a base unit 100, a plurality of support bars 130, and a plurality of spacers 300. The catalyst metal film 200 used in the present embodiment functions as a catalyst in synthesizing graphene using CVD, and may be formed of at least one of selected from a group consisting of iron (Fe), nickel (Ni), cobalt (Co), platinum (Pt), iridium (Ir), gold (Au), aluminum (Al), chrome (Cr), copper (Cu), magnesium (Mg), manganese (Mn), silicon (Si), titanium (Ti), and rubidium (Ru). An example of using copper thin films as the catalyst metal films 200 is described in the present embodiment.

The base unit 100 is used to support the support bars 130 and is fixedly installed in the CVD chamber. The base unit 100 includes a chamber coupling unit 110 and a support bar installation unit 120.

The chamber coupling unit 110 is coupled to the CVD chamber such that the catalyst metal film-supporting device 1 may be stably located in the CVD chamber. The coupling between the chamber coupling unit 110 and the CVD chamber may include mechanical coupling having various formats such as a screw coupling, an insertion coupling, etc. Also, an interface for transmitting and receiving an electrical signal is provided in the CVD chamber so that the catalyst metal film-supporting device 1 may receive and transmit an electrical signal from and to the outside of the CVD chamber. The chamber coupling unit 110 may be electrically coupled to the interface.

The support bar installation unit 120 is coupled to the support bars 130, is coupled to the chamber coupling unit 110, and protrudes from the chamber coupling unit 110 in one direction. Data measured by a temperature sensor 140 may be transmitted to the outside of the CVD chamber through the interface provided in the CVD chamber.

The support bars 130 are coupled to the support bar installation unit 120 of the base unit 100 and protrude in both directions with respect to the support bar installation unit 120. A screw thread may be formed on an outer circumferential surface of each of the support bars 130. The support bars 130 are disposed corresponding to

holes

201 and 202 formed in the catalyst metal films 200 so that the support bars 130 may be inserted into the catalyst metal films 200 . The holes 202 disposed in both sides of the catalyst metal films 200 may be larger than the holes 201 disposed in the center thereof in order to prevent the catalyst metal films 200 from being curved due to a thermal expansion in the CVD chamber.

The spacers 300 are disposed between the catalyst metal films 200 and between the catalyst metal films 200 and the support bar installation unit 120 of the base unit 100 and function to prevent the catalyst metal films 200 from contacting each other or the catalyst metal films 200 from contacting the base unit 100. Screw threads may be formed in inner holes of the spacers 300 so that the spacers 300 may be screwed onto the support units 130. The spacers 300 alternate the catalyst metal films 200 and are received by the support bars 130 so that the spacers 300 may be disposed between the catalyst metal films 200.

A multiple graphene films synthesizing apparatus including the catalyst metal film-supporting device 1 of the present embodiment will now be described.

FIG. 3 is a schematic view of a multiple graphene films synthesizing apparatus 10 including the catalyst metal film-supporting device 1 of FIG. 1.

Referring to FIG. 3, the multiple graphene films synthesizing apparatus 10 of the present embodiment includes a CVD chamber 400, the catalyst metal film-supporting device 1 of FIG. 1, susceptors 600, and heating sources 500.

The CVD chamber 400 has a space therein, and includes gas injection units 410 and gas ejection units 420. A raw material gas G, for example, a mixture gas of argon, oxygen, and methane, for synthesizing graphene is injected by the gas injection units 410 of the CVD chamber 400. The gas injection units 410 may be disposed at side surfaces, upper sides, or lower sides of the catalyst metal film-supporting device 1 such that the raw material gas G may pass through the catalyst metal films 200 installed in the catalyst metal film-supporting device 1. The gas ejection units 410 may be disposed opposite to the gas injection units 410 with respect to the catalyst metal film-supporting device 1 such that the raw material gas G injected into the CVD chamber 400 may be ejected from the CVD chamber 400 after contacting the catalyst metal films 200.

The catalyst metal film-supporting device 1 is disposed inside the CVD chamber 400 to which the base unit 100 is coupled so that a location thereof is fixed. Thus, the catalyst metal film-supporting device 1 may stably maintain its location when the raw material gas G is injected. The construction of the catalyst metal film-supporting device 1 is the same as described above.

The susceptors 600 are disposed at both sides of the catalyst metal film-supporting device 1, and transfers heat generated in the heating sources 500 to the catalyst metal film-supporting device 1. The susceptors 600 are formed in a face shape so that the heat generated by the heating sources 500 may be uniformly spread spatially. That is, spaces between the susceptors 600 are uniformly heated generally so that the catalyst metal films 200 disposed between the susceptors 600 may also be uniformly heated equally.

The heating sources 500 are used to heat the inside of the CVD chamber 400 by emitting radiant heat using electrical energy. The heating sources 500 may heat the CVD chamber 400 at a temperature of 1000 °C or higher such that graphene may be synthesized on surfaces of the catalyst metal films 200. The heat generated by the heating sources 500 is transmitted to the catalyst metal film-supporting device 1 through the susceptors 600, which prevent a specific part of the CVD chamber 400 from being intensively heated and allow the inside of the CVD chamber 400 to be uniformly heated.

A multiple graphene films synthesizing method according to an embodiment of the present invention by using the above-described multiple graphene films synthesizing apparatus will now be described.

FIG. 4 is a schematic flowchart of a multiple graphene films synthesizing method according to an embodiment of the present invention.

Referring to FIG. 4, the multiple graphene films synthesizing method of the present embodiment includes operation S10 of placing the plurality of catalyst metal films 200 in parallel to each other, operation S20 of placing the spacers 300 between the catalyst metal films 200, operation S30 of heating the inside of the CVD chamber 400, and operation S40 of injecting the raw material gas G into the CVD chamber 400.

Operation S10 of placing the plurality of catalyst metal films 200 in parallel to each other is an operation of installing the plurality of catalyst metal films 200 on the support bars 130 of the catalyst metal film-supporting device 1. A process of installing the plurality of catalyst metal films 200 in the CVD chamber 400 may be performed by placing the catalyst metal film-supporting device 1 in the CVD chamber 400 and then installing the catalyst metal films 200 on the catalyst metal film-supporting device 1 or by installing the catalyst metal films 200 on the catalyst metal film-supporting device 1 outside the CVD chamber 400 and then inserting the catalyst metal film-supporting device 1 on which the catalyst metal films 200 are installed into the CVD chamber 400.

Operation S20 of placing the spacers 300 between the catalyst metal films 200 is performed concurrently with operation S10 of placing the plurality of catalyst metal films 200 in parallel to each other. That is, operation S20 may be performed in a way that the spacers 300 are installed between the catalyst metal films 200 while installing the catalyst metal films 200 on the catalyst metal film-supporting device 1.

Although operation S20 of placing the spacers 300 between the catalyst metal films 200 is performed concurrently with operation S10 of placing the plurality of catalyst metal films 200 in parallel to each other in the present embodiment, operation S20 may be performed after installing the catalyst metal films 200 on the catalyst metal film-supporting device 1. For example, if the spacers 300 are C-shaped and are able to be laterally coupled to the support bars 130, the spacers 30 may be placed between the catalyst metal films 200 by installing the plurality of catalyst metal films 200 in parallel to each other on the catalyst metal film-supporting device 1 and then laterally coupling the spacers 300 to the support bars 130 between the catalyst metal films 200.

Operation S30 of heating the inside of the CVD chamber 400 is an operation of operating the heating sources 500 when the catalyst metal film-supporting device 1 on which the catalyst metal films 200 are installed is disposed inside of the CVD chamber 400 and increasing a temperature of the inside of the CVD chamber 400 to a graphene synthesizing temperature.

Operation S40 of injecting the raw material gas G into the CVD chamber 400 is an operation of injecting the raw material gas G for synthesizing graphene into the CVD chamber 400 having a high temperature environment. The injected raw material gas G flows to spaces between the catalyst metal films 200 installed in the catalyst metal film-supporting device 1 and contacts surfaces of the catalyst metal films 200, and thus a chemical reaction occurs. After a graphene synthesis reaction, gas is ejected to the outside of the CVD chamber 400 through the gas ejection units 420. Operation S40 may be performed after or concurrently with operation S30 according to circumstances.

By undergoing the above-described process, thin film graphene may be synthesized on both surfaces of each of the catalyst metal films 200 installed in the catalyst metal film-supporting device 1. That is, multiple graphene films may be concurrently synthesized through a single CVD process.

The applicant conducted a Raman analysis and an experiment of measuring a surface resistance of synthesized graphene in order to acknowledge an actual effect of a graphene synthesizing method according to the above-described multiple graphene films synthesizing method. In the experiment conducted by the applicant, the CVD process was performed by placing a total of four sheets, two per side, of the catalyst metal films 200 at both sides of the support bar installation unit 120 of the base unit 100 of the catalyst metal film-supporting device 1.

FIGS. 5A and 5B are graphs of Raman analysis results for two sheets of the catalyst metal films 200 disposed left of the base unit 100 and two sheets of the catalyst metal films 200 disposed right thereof, respectively. In accordance with the Raman analysis results of FIGS. 5A and 5B, graphene films having a thickness corresponding to a single layer are successfully formed on both surfaces of all the four sheets of the catalyst metal films 200.

FIGS. 6A through 7D are graphs of results obtained by measuring a surface resistance of graphene synthesized by using the multiple graphene films synthesizing apparatus 10 of FIG. 3. More specifically, FIGS. 6A and 6B show surface resistance values of graphene formed in one surface and the other surface of the catalyst metal film 200 disposed leftmost from of the base unit 100. FIGS. 6C and 6D show surface resistance values of graphene formed in one surface and the other surface of the catalyst metal film 200 disposed on the left neighboring the base unit 100. FIGS. 7A and 7B show surface resistance values of graphene formed in one surface and the other surface of the catalyst metal film 200 disposed rightmost from the base unit 100. FIGS. 7C and 7D show surface resistance values of graphene formed in one surface and another surface of the catalyst metal film 200 disposed on the right neighboring the base unit 100.

Referring to FIGS. 6A through 7D, graphene synthesized on both surfaces of four sheets of the catalyst metal films 200 in total have excellent surface resistance characteristics since gaps between the catalyst metal films 200 are stably maintained by the catalyst metal film-supporting device 1 of the present embodiment. That is, in spite of a flow of the raw material gas G and a thermal expansion of the catalyst metal films 200, the catalyst metal films 200 do not contact each other, and thus graphene may be uniformly formed on surfaces of the catalyst metal films 200.

However, referring to FIGS. 6A through 6D, although the graphene synthesized on the catalyst metal film 200 disposed left of the base unit 100 has a minor deviation in surface resistance values, since the graphene synthesized on the catalyst metal film 200 disposed right of the base unit 100 has no deviation in surface resistance values, the deviation in the surface resistance values of the graphene synthesized on the catalyst metal film 200 disposed left of the base unit 100 is understood as a mere deviation in surface resistance values due to wrinkles caused by handling of the catalyst metal films 200.

FIG. 8 is a schematic exploded perspective view of a catalyst metal film-supporting device 2 according to another embodiment of the present invention.

Referring to FIG. 8, the catalyst metal film-supporting device 2 of the present embodiment includes a base unit 101, the plurality of support bars 130, and a plurality of

spacers

301 and 302. The functions and operations of the base unit 101, the support bars 130, and the

spacers

301 and 302 of the catalyst metal film-supporting device 2 of the present embodiment are similar to those of the base unit 100, the support bars 130, and the spacers 300 of the catalyst metal film-supporting device 1 of FIG. 1, and thus redundant descriptions thereof are omitted here and differences therebetween will now be described.

The base unit 101 includes a chamber coupling unit 111 and a support bar installation unit 121. The chamber coupling unit 111 is a part coupled to a CVD chamber. A plurality of temperature sensors 141 may be disposed on the chamber coupling unit 111. The support bar installation unit 121 is coupled to the chamber coupling unit 111 and is separated into upper and lower parts. The support bar installation unit 121 is separated into the upper and lower parts so that a raw material gas may more easily flow through spaces between the catalyst metal films 200 at both sides neighboring the support bar installation unit 121.

The plurality of support bars 130 protrude toward both sides of the support bar installation unit 121. Screw threads 132 may be formed only on end sides of the support bars 130.

The spacers include frame spacers 301 and nut spacers 302.

Through holes 3011 are formed in the center of the frame spacers 301. The frame spacers 301 have shapes corresponding to boundaries of the catalyst metal films 200. The frame spacers 301 receive the support bars 130 and are disposed between the catalyst metal films 200 and the catalyst metal films 200 and the support bar installation unit 121 of the base unit 101. Thus, the neighboring catalyst metal films 200 face each other through the through holes 3011 of the frame spacers 301.

The nut spacers 302 are disposed between the frame spacers 301 and the catalyst metal films 200 and between the frame spacers 301 and the support bar installation unit 121 of the base unit 101, and are received by the support bars 130. The nut spacers 302 are disposed between the frame spacers 301 so that the neighboring frame spacers 301 are spaced apart from each other.

The frame spacers 301 having the shapes corresponding to the boundaries of the catalyst metal films 200 are disposed between the catalyst metal films 200 thereby more effectively preventing the catalyst metal films 200 from contacting each other when moving.

The catalyst metal film-supporting device 2 of the present embodiment may also be employed in a multiple graphene films synthesizing apparatus.

FIG. 9 is a schematic view of a part of a multiple graphene films synthesizing apparatus including the catalyst metal film-supporting device 2, excluding a CVD chamber and heating sources. The CVD chamber and the heating sources are materially the same as those of the multiple graphene films synthesizing apparatus 10 of FIG. 3, and thus redundant descriptions are omitted here.

Referring to FIG. 9, spaces between the frame spacers 301 are spaces where the raw material gas G may flow during a subsequent CVD process. The spaces between the frame spacers 301 contact the catalyst metal films 200 and thus, the raw material gas G may readily contact surfaces of the catalyst metal films 200. Thus, graphene may be readily synthesized on both surfaces of each of the catalyst metal films 200 by the multiple graphene films synthesizing apparatus of the present embodiment.

The frame spacers 301 may be modified in various ways. FIG. 10 is a schematic view of a modification of the frame spacer 301. The support bar 130 may not be inserted into a frame spacer 303 shown in FIG. 10 but the frame spacer 303 may be disposed on an upper side of the support bar 130. That is, an upper side of a through hole 3031 may be placed on the support bar 130, and a lower side of the frame spacer 303 may be placed on the support bar 130. In this regard, a groove is formed in a portion corresponding to the support bar 130 of the frame spacer 303 and thus, the support bar 130 may be inserted into the groove. In this case, the frame spacer 303 may stably maintain its location without moving with respect to the support bar 130.

A catalyst metal film-supporting device according to another embodiment of the present invention will now be described.

FIG. 11 is a schematic exploded perspective view of a catalyst metal film-supporting device 3 according to another embodiment of the present invention. Referring to FIG. 11, the catalyst metal film-supporting device 3 includes a base unit 101 and frames 305.

The base unit 101 is materially similar to the base unit 101 of the catalyst metal film-supporting device 2 of FIG. 8, and thus a redundant description thereof is omitted here. However, with respect to the base unit 101 of the present embodiment, temperature sensors 142 protrude toward the center of the catalyst metal films 200. In this case, a temperature of the center of the catalyst metal films 200 may be more effectively measured.

The frames 305 include through spaces therein. A plurality of projections 3052 are formed in front and rear surfaces of the frames 305. Coupling holes are formed in the projections 3052 so that the support bars 130 may be inserted into the coupling holes. That is, the projections 3052 receive the support bars 130 and thus, the frames 305 are coupled to the support bars 130, and portions of the neighboring frames 305 except for the projections 3052 are spaced apart from each other by the projections 3052.

The catalyst metal films 200 are disposed in the through spaces of the center of the frames 305. In this regard, the catalyst metal films 200 are coupled to the frames 305 by fixing members 3054 so that the catalyst metal films 200 may be stably supported by the frames 305. As long as the catalyst metal films 200 and the frames 305 may be stably coupled to each other in a high temperature CVD chamber environment, any fixing members may be employed. For example, as the fixing members 3054, copper wires may be used to couple the catalyst metal films 200 to the frames 305 by being inserted into the holes 201 of the catalyst metal films 200.

If the frames 305 on which the catalyst metal films 200 are installed are prepared, the frames 305 are sequentially received by the support bars 130. Nuts 3056 are coupled to end sides of the support bars 130 and thus, the frames 305 may not be separated from the support bars 130.

The catalyst metal film-supporting device 3 of the present embodiment may also be employed in a multiple graphene films synthesizing apparatus.

FIG. 12 is a schematic view of a part of a multiple graphene films synthesizing apparatus including the catalyst metal film-supporting device 3, excluding a CVD chamber and heating sources. The CVD chamber and the heating sources are materially the same as those of the multiple graphene films synthesizing apparatus 10 of FIG. 3, and thus redundant descriptions are omitted here.

Referring to FIG. 12, inner portions of the frames 305 are spaced apart from each other by the projections 3052. The catalyst metal films 200 are disposed in the through spaces of the inside of the frames 305 so that the catalyst metal films 200 are spaced apart from each other. The raw material gas G may flow to spaces between the catalyst metal films 200. Thus, the raw material gas G may readily contact both surfaces of each of the catalyst metal films 200. Therefore, when a CVD process is performed by using the multiple graphene films synthesizing apparatus of the present embodiment, graphene may be effectively synthesized in both surfaces of each of the catalyst metal films 200.

FIG. 13 is a schematic flowchart of a multiple graphene films synthesizing method according to another embodiment of the present invention. The above-described multiple graphene films synthesizing apparatus may be used. Referring to FIG. 13, the multiple graphene films synthesizing method of the present embodiment may include operation S11 of installing the catalyst metal films 200 in the frames 305, operation S21 of placing the frames 305 in parallel to each other in a CVD chamber, operation S30 of heating the inside of the CVD chamber, and operation S40 of injecting the raw material gas G into the CVD chamber.

Operation S11 of installing the catalyst metal films 200 in the frames 305 is an operation of placing the catalyst metal films 200 in through spaces of the frames 305 and coupling the catalyst metal films 200 and the frames 305 by using the fixing members 3054. Operation S11 is repeatedly performed on the frames 305 and thus the catalyst metal films 200 are coupled to the frames 305, respectively.

Operation S21 of placing the frames 305 in parallel to each other in the CVD chamber is an operation of coupling the frames 305 to which the catalyst metal films 200 are coupled to the support bars 130 of the base unit 101 and placing the catalyst metal film-supporting device 3 in the CVD chamber. In this regard, the frames 305 coupled to the support bars 130 of the base unit 101 are disposed in parallel to each other and spaced apart from each other, excluding the projections 3052.

Operation S30 of heating the inside of the CVD chamber and operation S40 of injecting the raw material gas G into the CVD chamber are operations of heating the catalyst metal film-supporting device 3 disposed in the CVD chamber and spraying the raw material gas G to the catalyst metal film-supporting device 3 to allow graphene to be synthesized on surfaces of the catalyst metal films 200 coupled to the catalyst metal film-supporting device 3. Spaces are formed between the frames 305, and thus the raw material gas G flows through the spaces and contacts the catalyst metal films 200 so that graphene may be readily synthesized.

The applicant conducted a Raman analysis and an experiment of measuring a surface resistance of synthesized graphene in order to acknowledge an actual effect of a graphene synthesizing method according to the above-described multiple graphene films synthesizing method. In the experiment conducted by the applicant, the CVD process is performed by placing a total of four sheets, two per side, of the catalyst metal films 200 at both sides of the support bar installation unit 121 of the base unit 101 of the catalyst metal film-supporting device 3.

FIGS. 14A and 14B are graphs of Raman analysis results for two sheets of the catalyst metal films 200 disposed left of the base unit 101 and two sheets of the catalyst metal films 200 disposed right thereof, respectively. In accordance with the Raman analysis results of FIGS. 14A and 14B, graphene films having a thickness of a single layer are successfully formed on both surfaces of four sheets of the catalyst metal films 200 in total.

FIGS. 15A through 15B are graphs of results obtained by measuring a surface resistance of synthesized graphene. More specifically, FIG. 15A shows surface resistance values of graphene formed in one surface of the catalyst metal film 200 disposed in the left boundary of the base unit 101. FIG. 15B shows surface resistance values of graphene formed in one surface of the catalyst metal film 200 disposed left neighboring the base unit 101. FIG. 16A shows surface resistance values of graphene formed in one surface of the catalyst metal film 200 disposed in the right boundary of the base unit 101. FIG. 16B shows surface resistance values of graphene formed in one surface of the catalyst metal film 200 disposed right neighboring the base unit 101. The graphene films formed in both surfaces of each of the catalyst metal films 200 have very similar characteristics, and thus results obtained by measuring the graphene formed in one surface of each of the catalyst metal films 200 are described.

Averages, standard deviations, minimum values, and maximum values of the surface resistance values of the graphene synthesized on the surfaces of the catalyst metal films 200 may be calculated as shown in Table 1 below.

Table 1

	Left Boundary	Left Inner Side	Right Inner Side	Right Boundary
Surface Resistance Average (Ohm/sq.)	297	382	343	376
Standard Deviation (%)	9.4	16.5	5.3	14.2
Minimum Value (Ohm/sq.)	115	313	308	311
Maximum Value (Ohm/sq.)	368	566	380	612

As a result of measuring the surface resistance, all four graphene films have average values of 300~380 Ohm/sq. (STDEV 5~15%), and thus the graphene films are determined to have a relatively uniform quality.

That is, according to the multiple graphene films synthesizing method of the present embodiment, multiple graphene films may be effectively synthesized since the frames 305 stably support the catalyst metal films 200 to be spaced apart from each other, and thus the catalyst metal films 200 are effectively prevented from being modified or sticking to each other.

The frames 305 of the catalyst metal film-supporting device 3 may be configured in different ways. FIG. 17 is a schematic view of a modification of the frames 305 of the catalyst metal film-supporting device 3 of FIG. 11. A frame 307 of FIG. 17 includes a plurality of

hinge members

3072 and 3076 to couple the frame 307 and the catalyst metal film 200.

The

hinge members

3072 and 3076 are disposed in upper and lower sides of the frame 307. One side of each of the

hinge members

3072 and 3076 is hinge-coupled to the frame 307 and the

other sides

3074 and 3078 of the

hinge members

3072 and 3076 are inserted into the holes 201 formed in the catalyst metal film 200.

Hinge units 3073 that are hinge-coupled to the frame 307 and formed in a pair of the hinge members 3072 disposed in the upper side of the frame 307 are disposed outward compared to the holes 201 formed in the catalyst metal film 200. Thus, force is applied by the hinge members 3072 disposed in the upper side of the frame 307 in a direction towards the other sides 3074 inserted into the holes 201 of the catalyst metal film 200 due to gravity of the hinge members 3072, i.e. a direction indicated by an arrow of FIG. 17

Hinge units 3077 that are hinge-coupled to the frame 307 and formed in a pair of the hinge members 3076 disposed in the lower side of the frame 307 are disposed inward compared to the holes 201 formed in the catalyst metal film 200. Thus, force is applied by the hinge members 3076 disposed in the lower side of the frame 307 in a direction towards the other sides 3078 inserted into the holes 201 of the catalyst metal film 200 due to gravity of the hinge members 3076, i.e. a direction indicated by an arrow of FIG. 17

As described above, gravity is applied in the direction in which the

hinge members

3072 and 3076 turn outward, i.e. a direction to which the catalyst metal film 200 is unfolded, and thus the catalyst metal film 200 is effectively unfolded when thermally expanding in a high temperature CVD chamber. Thus, the catalyst metal film 200 may be effectively prevented from being curved or wrinkled when thermally expanding. Therefore, a flatness of the catalyst metal film 200 is effectively maintained during a CVD process, and graphene synthesized on a surface of the catalyst metal film 200 may be also uniformly formed.

Although the left and

right hinge members

3072 and 3076 are hinge-coupled to the frame 307, the left or

right hinge member

3072 or 3076 may be fixed to the frame 307 and another one may be hinge-fixed thereto.

FIG. 18 is a schematic exploded perspective view of a catalyst metal film-supporting device 4 according to another embodiment of the present invention. Referring to FIG. 18, the catalyst metal film-supporting device 4 of the present embodiment includes frames 309 and a frame holding structure 700.

The frames 309 are used to support the catalyst metal films 200, and include frame holding units 3092 and lateral support units 3094. The frame holding units 3092 are disposed on upper sides of the catalyst metal films 200 and protrude extending in a width direction of the catalyst metal films 200. The lateral support units 3094 extend from lower sides of the frame holding units 3092 and are coupled to both sides of the catalyst metal films 200 to stably fix the catalyst metal films 200. Projections 3095 are formed in the lateral support units 3094 and hold the catalyst metal films 200 so that the lateral support units 3094 may be coupled to the catalyst metal films 200.

The frame holding structure 700 includes a plurality of slots 710 so as to accommodate the frames 309. The frames 309 may be respectively inserted into the slots 710, whereas some of them may be inserted into each of the slots 710. In the present embodiment, the frames 309 may approach an upper side of the frame holding structure 700 and be inserted into the slots 710. Coupling grooves 722 may be provided in the upper side of the frame holding structure 700 in such a way that the frame holding units 3092 of the frames 309 may be inserted into the coupling grooves 722. The coupling grooves 722 may be formed between projections 720 disposed on the upper side of the frame holding structure 700. Spaces between the coupling grooves 722 to which the frame holding units 3092 of the frames 309 may be coupled may be determined in such a way that the frames 309 may be spaced apart from each other. Thus, the catalyst metal films 200 disposed in the frames 309 are spaced apart from each other and flow spaces of the raw material gas G are formed therebetween so that the raw material gas G and the catalyst metal films 200 may effectively contact each other in a CVD process.

While the frames 309 are inserted in a direction of the upper side of the frame holding structure 700 in the present embodiment, the frames 309 may approach a lateral side of the frame holding structure 700 and be inserted into the frame holding structure 700.

Also, as long as the frames 309 may stably support the catalyst metal films 200 and may be inserted into and seated in the slots 710 of the frame holding structure 700, shapes of the frames 309 may differ from those of FIG. 18, for example, shapes of the frames 309 may be those of FIG. 11 or 17.

The above-described catalyst metal film-supporting device 4 of the present embodiment may also be employed in a multiple graphene films synthesizing apparatus. FIGS. 19 through 21 are schematic views of an example of a multiple graphene films synthesizing apparatus 20.

Referring to FIGS. 19 through 21, the multiple films synthesizing apparatus 20 of the present embodiment includes a CVD chamber 400, a movement support unit 800, the catalyst metal film-supporting device 4, a heating source (not shown), and a susceptor (not shown). The heating source and the susceptor are materially the same as described in the embodiments above, and thus redundant descriptions thereof are omitted here.

The CVD chamber 400 includes a main body 401 and a door 402. The door 402 is movably disposed with respect to the main body 401 so that the CVD chamber 400 may be opened and closed.

One side of the movement support unit 800 is coupled to the inside of the CVD chamber 400, and a part thereof is movably disposed in such a way that the movement support unit 800 may come in and out the CVD chamber 400 when the door 402 is opened. In the present embodiment, the movement support unit 800 includes a coupling unit 810 coupled to the CVD chamber 400, a driving unit 820 disposed to slidingly move with respect to the coupling unit 810, and an access unit 830 coupled to the driving unit 820 and coming in and out the CVD chamber 400.

The catalyst metal film-supporting device 4 is the same as shown in FIG. 18 and is disposed in the access unit 830 of the movement support unit 800. Thus, the catalyst metal film-supporting device 4, along with the access unit 830 of the movement support unit 800, may come in and out the CVD chamber 40. In this regard, the frame holding structure 700 of the catalyst metal film-supporting device 4 may be coupled to the access unit 830 of the movement support unit 800 whereas the frames 309 to which the catalyst metal films 200 are fixed may be detached from the frame holding structure 700.

FIG. 21 is a schematic flowchart for explaining a multiple graphene films synthesizing method according to another embodiment of the present invention. The multiple graphene films synthesizing method may be performed by the above-described multiple graphene films synthesizing apparatus 20.

Referring to FIG. 21, the multiple graphene films synthesizing method of the present embodiment includes operation S210 of preparing the frame holding structure 700 including the slots 710 that accommodates the frames 309, operation S220 of inserting the frames 309 into the slots 710 of the frame holding structure 700, and operation S230 of placing the frame holding structure 700 in the CVD chamber 400.

Operation S210 of preparing the frame holding structure 700 including the slots 710 that accommodates the frames 309 is an operation of preparing the frame holding structure 700 that accommodates the frames 309 supporting the catalyst metal films 200, by using the catalyst metal film-supporting device 4 shown in FIG. 18.

Operation S220 of inserting the frames 309 into the slots 710 of the frame holding structure 700 is an operation of inserting the frames 309, in which the catalyst metal films 200 are mounted, into the slots 710 of the frame holding structure 700. The frames 309 inserted into the frame holding structure 700 are spaced apart from each other and thus the catalyst metal films 200 that are mounted in the frames 309 are also spaced apart from each other. As shown in FIG. 20, operation S220 may be performed by inserting the frames 309 into the slots 710 of the frame holding structure 700 in a state where the frame holding structure 700 is disposed outside the CVD chamber 400.

Operation S230 of placing the frame holding structure 700 in the CVD chamber 400 is an operation of placing the catalyst metal film-supporting device 4, in which the catalyst metal films 200 are mounted, in the CVD chamber 400. Operation S230 is performed by placing the catalyst metal film-supporting device 4 in the CVD chamber 400 and closing the door 402, as shown in FIG. 19. In this regard, the catalyst metal film-supporting device 4 is supported by the movement support unit 800 and thus easily inserted into the CVD chamber 400 by a sliding movement.

As described above, if a CVD process is performed in a state where the catalyst metal film-supporting device 4 is inserted into the CVD chamber 400, since the raw material gas G may flow between the catalyst metal films 200, graphene may be effectively synthesized on both surfaces of each of the catalyst metal films 200.

According to the multiple graphene films synthesizing method of the present embodiment, multiple graphene films may be effectively synthesized as well as multiple sheets of the catalyst metal films 200 may easily come in and out the CVD chamber 400, and may be very conveniently exchanged.

Although the catalyst metal film-supporting device seated in the movement support unit 800 of the multiple graphene films synthesizing apparatus 20 is the catalyst metal film-supporting device 4 of FIG. 18, the catalyst metal film-supporting device seated in the movement support unit 800 of the multiple graphene films synthesizing apparatus 20 may be the catalyst metal film-supporting

devices

1, 2, and 3 of in FIGS. 1, 8, and 11. In this case, the

base units

100 and 101 of the catalyst metal film-supporting

devices

1, 2, and 3 may be coupled to the access unit 830 of the movement support unit 800.

As described above, according to the one or more of the above embodiments of the present invention, a catalyst metal film-supporting device and a method and apparatus for synthesizing multiple graphene films may concurrently and stably synthesize multiple graphene films.

While the present invention has been particularly shown and described with reference to exemplary embodiments thereof, it will be understood by those of ordinary skill in the art that various changes in form and details may be made therein without departing from the spirit and scope of the present invention as defined by the following claims.

Claims

A device for supporting a plurality of catalyst metal films in a chemical vapor deposition (CVD) chamber, the device comprising:

a base unit;

at least one support unit coupled to the base unit and extending in one direction so that the plurality of catalyst metal films are inserted and disposed; and

spacers coupled to the at least one support unit between the plurality of catalyst metal films so that the plurality of catalyst metal films are prevented from contacting each other.
The device of claim 1, wherein the at least one support unit is disposed in both directions with respect to the base unit.
The device of claim 2, wherein the base unit comprises temperature sensors for measuring a temperature of the CVD chamber.
The device of claim 1, wherein the spacers are received by the at least one support bar in a length direction of the at least one support bar.
The device of claim 1, wherein the spacers have spaces therein, and are formed in shapes corresponding to boundaries of the plurality of catalyst metal films.
A device for supporting a plurality of catalyst metal films in a chemical vapor deposition (CVD) chamber, the device comprising:

a base unit;

at least one support unit coupled to the base unit and extending in one direction; and

a plurality of frames coupled to at least one side of the plurality of catalyst metal film, coupled to the at least one support bar, and arranged in parallel to each other.
The device of claim 7, wherein the plurality of frames comprise through spaces therein,

wherein the plurality of catalyst metal films are disposed in the through spaces of the plurality of frames.
The device of claim 7, further comprising: hinge members having one sides hinge-coupled to the plurality of frames and other sides coupled to the plurality of catalyst metal films.
The device of claim 8, wherein gravity acts on the hinge members in a direction to which the plurality of catalyst metal films are unfolded.
The device of claim 6, further comprising a frame holding structure comprising a plurality of slots accommodating the plurality of frames.
A device for supporting a plurality of catalyst metal films in a chemical vapor deposition (CVD) chamber, the device comprising:

a frame holding structure comprising a plurality of slots for supporting a plurality of catalyst metal films; and

a plurality of frames coupled to at least one sides of the plurality of catalyst metal films and inserted into the plurality of slots of the frame holding structure.
A multiple graphene films synthesizing apparatus comprising:

a chemical vapor deposition (CVD) chamber comprising an injection unit and an ejection unit of a raw material gas;

the device for supporting the plurality of catalyst metal films disposed in the CVD chamber of any one of claims 1 through 11 and

heating sources heating the inside of the CVD chamber.
The multiple graphene films synthesizing apparatus of claim 13, further comprising: a movement support unit having at least one part disposed to come in and out the CVD chamber,

wherein the device for supporting the plurality of catalyst metal films is disposed in at least a part of the movement support unit.
A multiple graphene films synthesizing method comprising:

placing a plurality of catalyst metal films in parallel to each other in a chemical vapor deposition (CVD) chamber;

placing spacers between the plurality of catalyst metal films so that the plurality of catalyst metal films are prevented from contacting each other;

heating the inside of the CVD chamber; and

injecting a raw material gas into the CVD chamber.
The multiple graphene films synthesizing method of claim 14, wherein the placing of the plurality of catalyst metal films in parallel to each other in the CVD chamber comprises: inserting the plurality of catalyst metal films in parallel to each other into support bars extending in one direction, and

wherein the placing of the spacers between the plurality of catalyst metal films comprises: coupling the spacers to the support bars between the plurality of catalyst metal films.
The multiple graphene films synthesizing method of claim 14, wherein the spacers are received by the support bars in a length direction of the support bars.
The multiple graphene films synthesizing method of claim 14, wherein the spacers have spaces therein, and are formed in shapes corresponding to boundaries of the plurality of catalyst metal films.
A multiple graphene films synthesizing method comprising:

installing a plurality of catalyst metal films in a plurality of frames;

placing the plurality of frames in which the plurality of catalyst metal films are installed in a chemical vapor deposition (CVD) chamber to be spaced apart from each other in parallel to each other;

injecting a raw material gas into the CVD chamber; and

heating the inside of the CVD chamber.
The multiple graphene films synthesizing method of claim 18, wherein the placing of the plurality of frames in which the plurality of catalyst metal films are installed in the CVD chamber to be spaced apart from each other in parallel to each other comprises:

preparing a frame holding structure comprising a plurality of slots that individually accommodate the plurality of frames,

inserting the plurality of frames into the plurality of slots of the frame holding structure, and

inserting the frame holding structure into the CVD chamber.