CN104071780B - A kind of preparation method of number of plies controllable grapheme - Google Patents
A kind of preparation method of number of plies controllable grapheme Download PDFInfo
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Abstract
The present invention relates to the preparation method of number of plies controllable grapheme, include following steps: put in heating furnace by amorphous carbon compound, it is passed through noble gas at ambient pressure to get rid of air, then start quickly to heat, after temperature reaches 200～1400 DEG C, being passed through halogen gas or the gas containing halogens under conditions of keeping noble gas gas flow, it forms halogenide with the non-carbon element reaction in carbide and discharges, thus leaves carbon material；After question response completes, keep temperature-resistant on the premise of, stopping being passed through halogen gas or the gas containing halogens, keep noble gas is passed through the halide gas to remove remnants and byproduct of reaction, the most under inert gas atmosphere temperature is cooled to room temperature.The invention have the advantages that and can meet the requirement that different field is different to the Graphene number of plies；Adhesive force between Graphene and substrate is less, it is simple to peel off from substrate；Can react under conditions of normal pressure is relatively mild.
Description
Technical field
The present invention relates to the preparation method of a kind of number of plies controllable grapheme, it is adaptable to the Graphene that the extensive preparation number of plies can control.
Technical background
Since the method being by mechanically pulling off for 2004 prepares Graphene [1], because Graphene has the electron transfer of excellence
Rate, high theoretical specific surface area, high heat-conductivity conducting rate and high chemical stability, and become the focus of research.[2-5] these excellences
And the performance of uniqueness makes Graphene have huge application prospect in terms of energy conversion and storage, such as fuel-cell catalyst, light
The fields such as catalysis and solar cell material.[4,5]
In order to the character of these excellences of Graphene is applied to practice, the synthesis number of plies controllable grapheme of large-scale low-cost is first
Certainly condition.In recent years, research worker proposes a lot of method for synthesizing graphite alkene.As mechanical stripping first put forward for
Synthesizing graphite alkene, but the hardly possible expanding production of this method [1]；By solution dispersion and the method for stripping graphene oxide
Can be used for synthesizing graphite alkene [6-8], but the Graphene number of plies prepared by the method cannot accurately control, and graphene film
Layer is easy to be stacked into more than 10 layers and form graphite linings, thus loses the excellent properties of Graphene；Table at some transition metal
Monolayer or which floor Graphene can be prepared by chemical vapour deposition technique on face (such as copper sheet), but this method energy consumption is the highest.
[9]；Under high temperature and ultrahigh vacuum, the particular crystal plane graphite with highly directional crystal SiC can be turned to the graphite that the number of plies is controlled
Alkene [10-15], graphene growth is brought into brand-new field by this epitaxial growth method, but this method needs almost ideal height
Orientation SiC and the harshest synthesis condition (such as high temperature more than 1250 degrees Celsius and fine vacuum) [10-16], the stone synthesized in addition
There is the strongest adhesion between ink alkene and SiC substrate, which has limited the further application of Graphene.In recent years, have been reported
Amorphous carbon compound can be become Graphene [16] by halogenation under low-temperature atmosphere-pressure, but does not has the research of number of plies controllable precise.
Inventor finds in research process, uses halogen process, and reacted by regulation temperature, the time, carbide composition (nothing
Setting carbide is a-M1-xCxX value) or the concentration of reacting gas realize accurately adjusting the purpose of the Graphene number of plies.Additionally,
Amorphous carbon compound is isotropism, it is not necessary to highly directional as crystalline state SiC, and therefore reaction condition can be normal pressure, lowest temperature
Degree can as little as 200 DEG C, and the response time can control within 4 hours, and yield can be by the simple scale expanding stove
Expand, therefore can be with the accurate adjustable Graphene of the synthesis number of plies of large-scale low-cost.At present, use halogen process is not yet had to close
The one-tenth number of plies can be with the relevant report of the Graphene of accuracy controlling.
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[2].Novoselov,K.S.,et al.Electric field effect in atomically thin carbon films.Science306,
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[3].Novoselov,K.S.,et al.Two-dimensional gas of massless Dirac fermions in graphene.Nature
438,197-200(2005).
[4]Geim,A.K.,et al.The rise of graphene.Nat.Mater.6,183-191(2007).
[5]Yin,Z.,et al.Graphene-Based Materials for Solar Cell Applications.Adv.Energy Mater.2013,
doi:10.1002/aenm.201300574
[6].Hernandez,Y.,et al,High-yield Production of graphene by liquid-phase exfoliation.Nature
Nanotech.3,563-568(2008).
[7].Stankovich,S.,et al.Graphene-based composite materials.Nature442,282–286(2006).
[8]Lotya,M.,et al.Liquid Phase Production of Graphene by Exfoliation of Graphite in
Surfactant/Water Solutions.J.Am.Chem.Soc.131,3611(2009).
[9].Li,X.,et al.Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper
Foils.Science324,1312-1314(2009).
[10].Bolen,M.L.,et al.Graphene formation mechanisms on 4H-SiC(0001).Phys.Rev.B80,
115433(2009).
[11].Forbeaux,I.,et al.Heteroepitaxial graphite on6H-SiC(0001):Interface formation through
conduction-band electronic structure.Phys.Rev.B58,16396-16406(1998).
[12].Virojanadara,C.,et al.Homogeneous large-area graphene layer growth on6H-SiC(0001).
Phys.Rev.B.78,245403(2008),.
[13].Kim,S.,et al.Origins of anomalous electronic structures of epitaxial graphene on silicon
carbide.Phys.Rev.Lett.100,176802(2008).
[14].Deng,D.,et al.Freestanding Graphene by Thermal Splitting of Silicon Carbide Granules.Adv.
Mater.22,2168–2171(2010),.
[15].Kim,J.et al.Layer-Resolved Graphene Transfer via Engineered Strain Layer.Science342,
833-836(2013).
[16].Peng,T.,et al.Direct Transformation of Amorphous Silicon Carbide into Graphene under
Low Temperature and Ambient Pressure.Sci.Rep.3,1148(2013).
Summary of the invention
Provided herein is a kind of amorphous carbon compound is prepared under the conditions of halogenation gas the number of plies can be with the side of the Graphene of accuracy controlling
Method.
The present invention solves above-mentioned technical problem and be the technical scheme is that the preparation method of a kind of number of plies controllable grapheme, including
There are following steps:
(1) amorphous carbon compound is put in heating furnace, be passed through noble gas at ambient pressure to get rid of air, then start quickly
Heating, after temperature reaches 200～1400 DEG C, is passed through halogen gas or containing halogen under conditions of keeping noble gas gas flow
The gas of element, it forms halogenide with the non-carbon element reaction in carbide and discharges, thus leaves carbon material；
(2) after question response completes, keep temperature-resistant on the premise of, stop being passed through halogen gas or containing the gas of halogens,
Keep noble gas is passed through the halide gas to remove remnants and byproduct of reaction, the most under inert gas atmosphere by temperature
It is cooled to room temperature, finally obtains the sample containing Graphene.
By such scheme, the formula of described amorphous carbon compound is a-M1-xCx, wherein M represent Si, Ti, Al, Mo,
Ta, Zr, B or W element, and 0 < x < 1.
By such scheme, described x span is 0.3～0.7.
By such scheme, described halogen gas is F2、Cl2、Br2And I2The mixing of any one or they in gas.
By such scheme, the described gas containing halogens is HF or HCl gas.
By such scheme, the described response time is 5 minutes～200 minutes.
By such scheme, the range of flow of described halogen gas or the gas containing halogens is 20ml/min～500ml/min.
The concrete pattern not requirement of amorphous carbon compound involved in the present invention, thin film (including nanometer, micron and macroscopic film),
Granule (to particle diameter not requirement, including nanometer, micron and macroscopic particles), macroscopic view block etc. all can react prepares Graphene.
Temperature that the number of plies of the Graphene prepared by the present invention can be reacted by regulation, time, carbide composition (change nothing
Setting carbide is a-M1-xCxX value, 0 < x < 1) or the concentration of reacting gas or flow precisely controlled.
Compared with existing background technology, the invention have the advantages that
1, the number of plies of Graphene can by temperature, time that regulation is reacted, (amorphous carbon compound is a-M to carbide composition1-xCxX value) or
The concentration of person's reacting gas obtains accuracy controlling, can meet the requirement that different field is different to the Graphene number of plies.
2, after amorphous carbon compound is converted into Graphene, the adhesive force between Graphene and substrate is less, it is simple to peel off from substrate.
3, can react under conditions of normal pressure is relatively mild, and minimum reaction temperature is 200 DEG C, the response time is
Short can control within 4 hours.
4, halogenation is a kind of economy and the mode of production of easily extension, and there had the method for factory's halogenation to produce carbide to be derivative
Thing, so halogenation is applied to produce Graphene is easy to large-scale production.
Accompanying drawing explanation
Fig. 1 is high-resolution-ration transmission electric-lens (HRTEM) picture of TiC in embodiment 1；
Fig. 2 is embodiment 1 gained Graphene HRTEM picture；
Fig. 3 is embodiment 1 gained Graphene HRTEM picture；
Fig. 4 is embodiment 3 gained Graphene HRTEM picture；
Fig. 5 is embodiment 5 gained Graphene HRTEM picture；
Fig. 6 is embodiment 5 gained Graphene HRTEM picture；
Fig. 7 is Raman (Raman) spectrum of gained Graphene in embodiment 1 to 5；
Fig. 8 is the 2D peak of the Raman spectrum of gained Graphene in embodiment 1 to 5；
Fig. 9 is embodiment 9 gained Graphene HRTEM picture；
Detailed description of the invention
Step 1: good seal in stove will be put into containing amorphous carbon compound, and check air-tightness, under conditions of an atmospheric pressure
Logical noble gas (He, Ar etc.) half an hour is to get rid of air.Keep being passed through noble gas and heating, when temperature reaches required anti-
Answer after temperature 200～1400 DEG C (heating rate can arbitrarily control), be passed through under conditions of keeping certain inert gas flow
The halogenation gas of given pace.
Step 2: after having reacted in step 1, keep temperature-resistant on the premise of, turn off halogen gas or containing halogen
The gas of element, but be intended to keep 0.5 hour or time that is passed through of above noble gas is to go out the halogenation gas of remnants and anti-
Answer by-product.
Step 3: keeping, under inert gas atmosphere, stove is cooled to room temperature, rate of temperature fall can arbitrarily control, finally obtain the number of plies
Can the sample of Graphene of accuracy controlling.
Below in conjunction with embodiment, the present invention will be further described in detail, but this explanation will not be construed as limiting the invention.
Embodiment 1
Weigh 2g surface and there is amorphous nanoshell a-Ti0.4C0.6Nano SiC, put it in quartz ampoule after good seal, with
The flow of 500ml/min is passed through high-purity He gas 30 minutes so that the air got rid of in quartz ampoule, stove is heated to 200 and takes the photograph
Family name's degree, on the premise of keeping He gas flow to be 100ml/min, during reaction, the flow with 500ml/min is passed through Cl2Gas,
Question response stops being passed through Cl after carrying out one hour2Gas and keep He gas to be passed through, keep reaction temperature 200 DEG C to drop after one hour
The nano-particle that surface has the graphene-structured of 1 to 3 layer is i.e. can get to room temperature.Fig. 1 is that surface has amorphous nanometer thin
The images of transmissive electron microscope (TEM) of the nano TiC of film；If Fig. 2 is that in embodiment 1,200 DEG C of halogenation rear surfaces have 2 layers of graphite
The images of transmissive electron microscope of the nano-particle of alkene structure, wherein crystalline state TiC within nano-TiC particle still retains；Shown in Fig. 3
There is the images of transmissive electron microscope of the nano-particle of 1-3 layer graphene structure, Qi Zhongna for 200 DEG C of halogenation rear surfaces in embodiment 1
Rice crystalline state TiC within TiC granule is also converted to amorphous C.
Embodiment 2
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reaction temperature is 400
℃.Final available surface has the nano-particle of the graphene-structured of layer 2-4.
Embodiment 3
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reaction temperature is 600
℃.Final available surface has the nano-particle of the graphene-structured of 4-5 layer.Fig. 4 is 600 DEG C of halogenation surfaces in embodiment 3
After having the nano TiC of amorphous nanoshell, surface has the images of transmissive electron microscope of the nano-particle of 5 layer graphene structures；
Embodiment 4
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reaction temperature is 800
℃.Final available surface has the nano-particle of the graphene-structured of 6-7 layer.
Embodiment 5
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reaction temperature is 1000
℃.Final available surface has the nano-particle of the graphene-structured of 7-8 layer.Fig. 5 is 1000 DEG C of halogenation tables in embodiment 5
After mask has the nano TiC of amorphous nanoshell, surface has the images of transmissive electron microscope of the nano-particle of 8 layer graphene structures；
Fig. 6 is the Graphene after halogenation surface has the nano TiC of amorphous nano thin-film, the nano-graphene lamella after stripping；Figure
7 is at identical chlorine gas concentration and response time same sample, (embodiment 1-5) reacted Raman collection of illustrative plates at different temperatures,
The change at the enlarged drawing display 2D peak of the inside, from 2673.3cm-1(200 DEG C), 2674.4cm-1(400 DEG C), 2679.1
cm-1(600 DEG C), 2680.7cm-1(800 DEG C) arrive 2686.5cm-1(1000 DEG C). the displacement at peak is due to graphene layer
The increase of number causes, and the change of such change and Fig. 2-5 is proved each other；Fig. 8 is 2D peak enlarged drawing (embodiment 1-5).
2D is by two interior peak 2D1(2670cm-1) and 2D2(2691cm-1) composition, 2D1(2670cm-1) area percentage along with
Reaction temperature increases and reduces, contrary 2D2(2691cm-1) area percentage along with temperature increase increase, this surface Graphene
The number of plies increases along with temperature.
Embodiment 6
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reaction temperature is 1200
℃.Final available surface has the nano-particle of the graphene-structured of 9-10 layer.
Embodiment 7
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g a-Zr0.3C0.7,
Reaction temperature is 800 DEG C.Final available surface has the nano-particle of the graphene-structured of 6-8 layer.
Embodiment 8
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g surface and have
Amorphous nanoshell a-Ti0.4C0.6Micron TiC, temperature is 400 DEG C, and during reaction, the flow of He gas is 100ml/min, Cl2
The flow of gas is 300ml/min.The micron particle of the graphene-structured that final available surface tool is of five storeys.
Embodiment 9
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g surface and have
Amorphous nanoshell a-Ti0.4C0.6Micron TiC, temperature is 600 DEG C, and during reaction, the flow of He gas is 100ml/min, Cl2
The flow of gas is 300ml/min.Final available surface has the micron particle of the graphene-structured of 8 layers.Fig. 9 is embodiment
After halogenation surface has the micron TiC of amorphous nano thin-film in 9, on the micron particle surface obtained, there are 8 layer graphenes.
Embodiment 10
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g surface and have
Amorphous nanoshell a-Ti0.3C0.7Nano TiC, temperature is 800 DEG C, and during reaction, the flow of He gas is 100ml/min, Cl2
The flow of gas is 500ml/min.Final available surface has the nano-particle of 8 layer graphene structures.
Embodiment 11
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g surface and have
Amorphous nanoshell a-Ti0.3C0.7Nano TiC, temperature is 800 DEG C, and during reaction, the flow of He gas is 100ml/min, Cl2
The flow of gas is 400ml/min.Final available 6 layers of surface has the nano-particle of graphene-structured.
Embodiment 12
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g surface and have
Amorphous nanoshell a-Ti0.3C0.7Nano TiC, temperature is 800 DEG C, and during reaction, the flow of He gas is 100ml/min, Cl2
The flow of gas is 300ml/min.Final available 6 layers of surface has the nano-particle of graphene-structured.
Embodiment 13
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g surface and have
Amorphous nanoshell a-Ti0.3C0.7Nano TiC, temperature is 800 DEG C, and during reaction, the flow of He gas is 100ml/min, Cl2
The flow of gas is 200ml/min.Final available 4 layers of surface has the nano-particle of graphene-structured.
Embodiment 14
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g surface and have
Amorphous nanoshell a-Ti0.3C0.7Nano TiC, temperature is 800 DEG C, and during reaction, the flow of He gas is 100ml/min, Cl2
The flow of gas is 100ml/min.Final available 2 layers of surface has the nano-particle of graphene-structured.
Embodiment 15
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g surface and have
Amorphous nanoshell a-Ti0.3C0.7Nano TiC, temperature is 800 DEG C, and during reaction, the flow of He gas is 100ml/min, Cl2
The flow of gas is 50ml/min.Final available 1 layer of surface has the nano-particle of graphene-structured.
Embodiment 16
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g surface and have
Amorphous nanoshell a-Ti0.5C0.5Nano TiC, reaction temperature 800 DEG C.Final available 5 layers of surface has graphene-structured
Nano-particle.
Embodiment 17
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: weigh 2g surface and have
Amorphous nanoshell a-Ti0.4C0.6Nano TiC, reaction temperature 800 DEG C, final available 3 layers of surface has graphene-structured
Nano-particle.
Embodiment 18
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reaction temperature is 600
DEG C, the response time is 10min, and final available surface has the nano-particle of 1-2 layer graphene structure.
Embodiment 19
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reaction temperature is 600
DEG C, the response time is 30min, and final available surface has the nano-particle of 3 layer graphene structures.
Embodiment 20
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reaction temperature is 600
DEG C, the response time is 50min, and final available surface has the nano-particle of 4 layer graphene structures.
Embodiment 21
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reaction temperature is 600
DEG C, the response time is 90min, and final available surface has the nano-particle of 6 layer graphene structures.
Embodiment 22
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reaction temperature is 600
DEG C, the response time is 120min, and final available surface has the nano-particle of 7 layer graphene structures.
Embodiment 23
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: with HCl and Cl2Mixed
Close other and replace Cl2Gas；Temperature is 1000 DEG C, and during reaction, the flow of Ar gas is 100ml/min, Cl2The flow of gas
For 200ml/min, the response time controls at 1h.Final available surface has the nano-particle of 7 layer graphene structures.
Embodiment 24
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: with having a-Ta0.4C0.6
Nanometer Ta of thin film4C replaces nanometer silicon carbide；Temperature is 1000 DEG C, and the flow of He gas is 500ml/min, Cl2Gas
Flow be 200ml/min.Final available surface has the nano-particle of 7 layer graphene structures.
Embodiment 25
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: with having a-Zr0.4C0.6
Nanometer ZrC of thin film replaces nanometer silicon carbide；Temperature is 1000 DEG C, and the flow of He gas is 500ml/min, Cl2Gas
Flow is 200ml/min.Final available surface has the nano-particle of 8 layer graphene structures.
Embodiment 26
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: with having a-Zr0.3C0.7
Nanometer ZrC of thin film replaces nanometer silicon carbide；Temperature is 1200 DEG C, and the flow of He gas is 500ml/min, Cl2Gas
Flow is 200ml/min,.Final available surface has the nano-particle of 8 layer graphene structures.
Embodiment 27
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: with having a-Si0.3C0.7
The nano SiC of thin film replaces nanometer silicon carbide；Temperature is 1200 DEG C, and the flow of He gas is 500ml/min, Cl2Gas
Flow is 200ml/min,.Final available surface has the nano-particle of 6 layer graphene structures.
Embodiment 28
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: with having a-B0.3C0.7
Nanometer BC of thin film replaces nanometer silicon carbide；Temperature is 1200 DEG C, and the flow of He gas is 500ml/min, Cl2The stream of gas
Amount is 200ml/min,.Final available surface has the nano-particle of 4 layer graphene structures.
Embodiment 29
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: with having a-W0.4C0.6
Nanometer WC of thin film replaces nanometer silicon carbide；Temperature is 800 DEG C, and the flow of He gas is 500ml/min, Cl2The stream of gas
Amount is 200ml/min,.Final available surface has the nano-particle of 5 layer graphene structures.
Embodiment 30
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: with having a-Al0.5C0.5
Nanometer Al of thin film4C3Replace nanometer silicon carbide；Temperature is 1200 DEG C, and the flow of He gas is 500ml/min, Cl2Gas
Flow is 200ml/min,.Final available surface has the nano-particle of 7 layer graphene structures.
Embodiment 31
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: with having a-Mo0.4C0.6
The nano SiC of thin film replaces nanometer silicon carbide；Temperature is 1200 DEG C, and the flow of He gas is 500ml/min, Cl2Gas
Flow is 200ml/min,.Final available surface has the nano-particle of 8 layer graphene structures.
Embodiment 32
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reacting gas is HCl.
Final available surface has the nano-particle of the graphene-structured of 3-4 layer.
Embodiment 33
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reacting gas is F2。
The nano-particle of the graphene-structured that final available surface tool is of five storeys.
Embodiment 34
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reacting gas is Br2,
Reaction temperature is 1000 degrees Celsius.Final available surface has the nano-particle of the graphene-structured of 4-5 layer.
Embodiment 35
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reacting gas is I2,
Reaction temperature is 1000 degrees Celsius.Final available surface has the nano-particle of the graphene-structured of 3-4 layer.
Embodiment 36
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reacting gas is HF.
Final available surface has the nano-particle of the graphene-structured of 4-5 layer.
Embodiment 37
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reacting gas is Cl2
With HCl mixed gas.Final available surface has the nano-particle of the graphene-structured of layer 2-3.
Embodiment 38
Preparation process in the present embodiment is identical with above-described embodiment 1 with step.Except for the difference that: reacting gas is Cl2
With HF mixed gas.Final available surface has the nano-particle of the graphene-structured of 2 layers.
Claims (4)
1. a preparation method for number of plies controllable grapheme, includes following steps:
(1) amorphous carbon compound is put in heating furnace, it is passed through noble gas at ambient pressure to get rid of air, then start quickly to heat, after temperature reaches 200～1400 DEG C, halogen gas or the gas containing halogens it is passed through under conditions of keeping noble gas gas flow, it forms halogenide with the non-carbon element reaction in carbide and discharges, thus leaves carbon material；The formula of described amorphous carbon compound is a-M1-xCx, wherein M represents Si, Ti, Al, Mo, Ta, Zr, B or W element, and 0 < x < 1；Described x span is 0.3～0.7；The described response time is 5 minutes～200 minutes；
(2) after question response completes, keep temperature-resistant on the premise of, stop being passed through halogen gas or the gas containing halogens, keep noble gas is passed through the halide gas to remove remnants and byproduct of reaction, the most under inert gas atmosphere temperature being cooled to room temperature, finally obtaining the number of plies can the sample containing Graphene of accuracy controlling.
The preparation method of number of plies controllable grapheme the most according to claim 1, it is characterised in that described halogen gas is F2、Cl2、Br2And I2The mixing of any one or they in gas.
The preparation method of number of plies controllable grapheme the most according to claim 1, it is characterised in that the described gas containing halogens is HF or HCl gas.
The preparation method of number of plies controllable grapheme the most according to claim 1, it is characterised in that the range of flow of described halogen gas or the gas containing halogens is 20mL/min～500mL/min.
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| CN101979315A (en) * | 2010-11-16 | 2011-02-23 | 中国科学院微电子研究所 | Preparation method of monoatomic-layer graphene film |
| CN102936746A (en) * | 2012-10-29 | 2013-02-20 | 武汉理工大学 | Method for directly converting amorphous carbide into graphene under low-temperature and normal-pressure halogenation conditions |
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| JP2000086223A (en) * | 1998-09-17 | 2000-03-28 | Ishikawajima Harima Heavy Ind Co Ltd | Carbon heating method and furnace |
| KR101443217B1 (en) * | 2007-09-12 | 2014-09-19 | 삼성전자주식회사 | Graphene shell and process for preparing the same |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101979315A (en) * | 2010-11-16 | 2011-02-23 | 中国科学院微电子研究所 | Preparation method of monoatomic-layer graphene film |
| CN102936746A (en) * | 2012-10-29 | 2013-02-20 | 武汉理工大学 | Method for directly converting amorphous carbide into graphene under low-temperature and normal-pressure halogenation conditions |
Non-Patent Citations (1)
| Title |
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| Direct Transformation of Amorphous Silicon Carbide into Graphene under Low Temperature and Ambient Pressure;Tao Peng et al.;《scientific reports》;20130128;第1-7页 * |
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