CN102070141A - Method for preparing graphene - Google Patents
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- CN102070141A CN102070141A CN 201110057535 CN201110057535A CN102070141A CN 102070141 A CN102070141 A CN 102070141A CN 201110057535 CN201110057535 CN 201110057535 CN 201110057535 A CN201110057535 A CN 201110057535A CN 102070141 A CN102070141 A CN 102070141A
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Abstract
The invention provides a method for preparing graphene. The graphene is prepared on a substrate with a catalyst metal nanocrystalline layer by utilizing the flame of carbon-containing fuels such as ethanol and the like; and nitrogen-doped graphene is directly prepared on the same substrate by utilizing the flame produced by amine liquid simultaneously containing carbon and nitrogen. The invention provides the novel method for preparing the graphene, which is easy to operate.
Description
Technical field
The invention belongs to the carbon material field, relate to a kind of preparation method of graphene.
Background technology
Graphene is a kind of special laminated structure, it found by scientist An Deliehaimu of Univ Manchester UK (Andre Geim) and Constantine Nuo Woxiaoluofu (Konstantin Novoselov) that (SCIENCE 2004 in 2004,306,666-669), and obtained Nobel prize for physics in 2010.They adopt the mechanically peel method, by repeatedly peeling off, have obtained the mono-layer graphite sheet that only is made of one deck carbon atom, i.e. Graphene from highly oriented pyrolytic graphite.Discover that Graphene has the excellent attributes of various super current materials far away, for example: high speed electronic mobility under the thinnest in the world material (single-layer graphene is 0.335 nm only), material, the toughness fabulous (Young's modulus can reach 1.1 TPa) that known strength is the highest at present, excellent impermeability (the He atom can't pass), the thermal conductivity of giving prominence to, the room temperature, (the theoretical specific surface area of single-layer graphene is up to 2630m for high specific surface area
2/ g), the lightest charge carrier etc.Utilize Graphene, can research and develop a series of novel materials with special property.For example, the transistorized transmission speed of Graphene is expected to be applied to the research and development of brand-new supercomputer considerably beyond present silicon transistor; Graphene can also be used to make touch-screen, luminescent screen, even solar cell.With other material mixing, Graphene also can be used for making more heat-resisting, more blocky electric conductor, thereby makes thinner, lighter, the more high resilience of novel material, so its application prospect is very wide.Graphene not only brings an electronic material revolution, but also will greatly promote the development of automobile, aircraft and space industry.
At present, preparation method of graphene mainly contains: mechanically peel method, chemical reduction method, SiC epitaxial growth method, chemical vapour deposition etc.
The mechanically peel method is to be that highly oriented pyrolytic graphite is cut into graphite flake at first, is bonded at the thin slice both sides with adhesive tape, tears adhesive tape then thin slice is divided into two, repeat above process and just can obtain Graphene, or even the Graphene of individual layer.The advantage of this method is the graphene film that can obtain very high quality; Shortcoming is that output is very low, and is difficult to the size and the number of plies of control graphene film.
Chemical reduction method is meant and utilizes the strong oxidizer graphite oxide, makes its interlamellar spacing become big, be easy to separate, and utilizes method such as ultrasonic to peel off graphite oxide, and the graphite oxide after reduction is peeled off can obtain Graphene.The starting material wide material sources of chemical reduction method, technology are simple, cost is lower, can be used for preparing in a large number Graphene; Shortcoming is that the quality of Graphene is lower, the number of plies is difficult to control, and mostly product is the mixture of individual layer, multi-layer graphene.
The SiC epitaxial growth method is to heat the SiC crystal in a vacuum, when temperature reaches 1200 ℃ ~ 1500 ℃, the C-Si key ruptures, and the Si atom that contains in the more plane of C atom is evaporated out, and remaining carbon atom can be arranged in graphene-structured on SiC crystal (0001) face.The advantage of this method is to prepare large-area Graphene; Shortcoming be yield poorly, the cost height, and graphene film is in uneven thickness.
Chemical Vapor deposition process utilizes the pyrolytic decomposition hydrocarbon gas, forms carbon nickel saturated solid solution in nickel catalyzator as thin as a wafer, then indigenous graphite alkene sheet lamella gradually in process of cooling.Its advantage is when obtaining high-quality Graphene, can also reasonably obtain comparatively ideal productive rate under the cost, is also possessing certain potentiality aspect the large-area Graphene of preparation in addition.
It is generally acknowledged, in Graphene, mix nitrogen-atoms can be able to change the energy band structure of Graphene, make it to take place from metallicity to the semiconductive fundamental change, in addition, nitrogen mixes and can also strengthen the biocompatibility of Graphene.Therefore nitrogen mixes the Application Areas of Graphene is enlarged.More common nitrogen-doped graphene method for making comprises at present: with ammonia and methane is that precursor gas prepares nitrogen-doped graphene by chemical Vapor deposition process; Utilize the plasma nitriding method to prepare nitrogen-doped graphene.And the nitrating process of these methods is all at high temperature carried out, and combining of nitrogen-atoms and Graphene is unstable, easily increases along with the time and runs off.Experiment showed, that the method for utilizing flame method directly to prepare the nitrating Graphene compares that existing nitrogen-doping method can obtain that nitrogen element content is higher, the better nitrogen-doped graphene of stability.
Summary of the invention
One of technical problem to be solved by this invention provides a kind of preparation method of graphene.
The technical solution used in the present invention in turn includes the following steps:
(1) selects resistant to elevated temperatures material as substrate, the surface of substrate is polished;
(2) at the nano-crystal film of polished substrate surface growth layer of metal, this layer metallic film is used as the catalyzer of the Graphene of growing;
(3) flame that substrate is placed carbonaceous fuel produce, the one side that is coated with catalyzer keep taking out after for some time towards flame core, after the cooling, are coated with the one side indigenous graphite alkene film of catalyst layer on the substrate.
Described catalyzer not only will help the cracking of fuel molecule, also wants to make the carbon that produces after the cracking form saturated solid solution therein.
In the such scheme, described substrate material is a kind of in the following material: pure metal plate, various alloy sheets, monocrystalline silicon piece, polysilicon chip etc.
Described catalyst metal comprises nickel, cobalt, copper, iron etc.
The preparation method of described catalyst film comprises any method that can the growing metal nano-crystal film such as pulse electrodeposition, magnetron sputtering.
Described carbonaceous fuel can be organism such as alcohols, ethers, also can be solid fuels such as coke, can also be geseous fuel such as methane, acetylene and noble gas mixtures.
Two of technical problem to be solved by this invention provides a kind of preparation method of nitrogen-doped graphene.In turn include the following steps:
(1) selects resistant to elevated temperatures material as substrate, the surface of substrate is polished;
(2) at the nano-crystal film of polished substrate surface growth layer of metal, this layer metallic film is used as the catalyzer of flame method growth Graphene;
(3) flame that substrate is placed the fuel of carbon containing and nitrogen simultaneously produce, the one side that is coated with catalyzer keeps taking out after for some time towards flame core, and after the cooling, the one side that is coated with catalyst layer on the substrate is separated out the nitrogen-doped graphene film.
Described catalyzer not only will help the cracking of fuel molecule, also wants to make the carbon that produces after the cracking form saturated solid solution therein.
In the such scheme, described substrate material is a kind of in the following material: pure metal plate, various alloy sheets, monocrystalline silicon piece, polysilicon chip etc.
Described catalyst metal comprises nickel, cobalt, copper, iron etc.
The fuel of described while carbon containing and nitrogen can be the one or any several mixture in the amine, also can be to add the mixture that forms behind any alcohols at any amine.
Beneficial effect of the present invention is:
(1) provides a kind of new method for preparing Graphene and nitrogen-doped graphene;
(2) simple to operate, be easy to control.
Description of drawings
Fig. 1 flame method prepares the Graphene setting drawing
The Graphene scanning electron microscope shape appearance figure that Fig. 2 embodiment 1 makes
The Raman spectrogram of the Graphene that Fig. 3 embodiment 1 makes
The nitrogen-doped graphene scanning electron microscope shape appearance figure that Fig. 4 embodiment 6 makes
The nitrogen-doped graphene Raman spectrogram that Fig. 5 embodiment 6 makes
The XPS spectrum figure of the nitrogen-doped graphene that Fig. 6 embodiment 6 makes.
Embodiment
Below in conjunction with drawings and Examples the present invention is further set forth, but therefore do not limit the present invention within the described scope of embodiments.
Embodiment 1: the conductive silicon chip with 2cm * 2cm size is a substrate, and wherein one side is polished to minute surface, utilizes numerical control pulse electrodeposition power supply with forward 3V, and oppositely the voltage of 1V is at nickeliferous ionic electroplate liquid (NiSO
46H
2O 300 g/L, NiCl
26H
2O 45 g/L, H
3BO
345 g/L, C
7H
5NO
3S 5 g/L) electroplated 40 seconds the surface electrical deposition one deck nickel nano-crystal film after polishing in.Lighting with the dehydrated alcohol is the spirit lamp of fuel, and the one side that above-mentioned silicon chip is coated with catalyzer places the flame envelope center towards flame core, keeps taking out after 1 minute, and naturally cools to room temperature, makes pure graphene film.
Utilize scanning electronic microscope and laser fibre Raman that the product that makes among the embodiment 1 is characterized respectively: shown in the scanning electron microscope shape appearance figure of Fig. 2, to observe the film like product in the product; This film product is carried out Raman spectrum analysis, and the result meets the chromatogram characteristic of Graphene as shown in Figure 3 fully.The result shows that success has made Graphene.
Embodiment 2: will be the experimental substrate that the fine copper plate of 99.9wt% cuts into 2cm * 2cm size with purity, wherein one side is handled to minute surface through sand papering, mechanical polishing, with forward 3V, oppositely the voltage of 1V is at nickeliferous ionic electroplate liquid (CuSO with numerical control pulse electrodeposition power supply
45H
2O 210 g/L, H
3BO
345 g/L, NaF 2.5g/L, C
7H
5NO
3S 5 g/L) electroplated 40 seconds deposition one deck nickel nano-crystal film in.Lighting with the dehydrated alcohol is the spirit lamp of fuel, and the one side that aforesaid substrate is coated with catalyzer places the flame envelope center towards flame core, keeps taking out after 1 minute, and naturally cools to room temperature, makes pure graphene film.
Embodiment 3: steel alloy is cut into the experimental substrate of 2cm * 2cm size, and wherein one side be handled to minute surface through sand papering, mechanical polishing, and with forward 3V, oppositely the voltage of 1V is at iron content ionic electroplate liquid (FeCl with numerical control pulse electrodeposition power supply
24H
2O 380 g/L, NaF 2.5g/L, H
3BO
320 g/L, C
7H
5NO
3S 5 g/L) electroplated 30 seconds deposition one deck iron nano-crystal film in.Lighting with methyl alcohol is the spirit lamp of fuel, and the one side that aforesaid substrate is coated with catalyzer places the flame envelope center towards flame core, keeps taking out after 3 minutes, and naturally cools to room temperature, makes pure graphene film.
Embodiment 4: the conductive silicon chip with 2cm * 2cm size is a substrate, and wherein one side is polished to minute surface, utilizes the surface deposition one deck cobalt nanocrystal film of magnetron sputtering technique after polishing.Lighting with methyl alcohol is the spirit lamp of fuel, and the one side that aforesaid substrate is coated with catalyzer places the flame envelope center towards flame core, keeps taking out after 3 minutes, and naturally cools to room temperature, makes pure graphene film.
Embodiment 5: embodiment 3: the experimental substrate that steel alloy is cut into 2cm * 2cm size, wherein one side is handled to minute surface through sand papering, mechanical polishing, with forward 3V, oppositely the voltage of 1V is at iron content ionic electroplate liquid (FeCl with numerical control pulse electrodeposition power supply
24H
2O 380 g/L, NaF 2.5g/L, H
3BO
320 g/L, C
7H
5NO
3S 5 g/L) electroplated 30 seconds deposition one deck iron nano-crystal film in.Light acetylene gas fuel, in acetylene torch, keep taking out after 1 minute, be cooled to room temperature, make pure graphene film.
Embodiment 6: the conductive silicon chip with 2cm * 2cm size is a substrate, and wherein one side is polished to minute surface, and with forward 3V, oppositely the voltage of 1V is at iron content ionic electroplate liquid (FeCl with numerical control pulse electrodeposition power supply
24H
2O 380 g/L, NaF 2.5g/L, H
3BO
320 g/L, C
7H
5NO
3S 5 g/L) electroplated 40 seconds deposition one deck iron nano-crystal film in.Lighting with 70wt % ethanol and 30wt% Tri N-Propyl Amine mixing solutions is the spirit lamp of fuel, the one side that aforesaid substrate is coated with iron catalyst places the flame envelope center towards flame core, keep taking out after 3 minutes, and naturally cool to room temperature, make the nitrogen-doped graphene film.
Utilize scanning electronic microscope, xps energy spectrum base and laser capture microdissection Raman that the product that embodiment makes is characterized respectively: shown in the scanning electron microscope shape appearance figure of Fig. 4, to observe the film like product in the product; This film product is carried out Raman spectrum analysis, and the result meets the chromatogram characteristic of Graphene as shown in Figure 5, but the strong and weak order at peak is different with Fig. 3; Again product is carried out X-ray photoelectron spectroscopic analysis, as shown in Figure 6, occurred tangible N peak among the result, the incorporation of N element is about 1%, wherein mixes for pyridine type nitrogen more than 70%.
Embodiment 7: will be the experimental substrate that the fine copper plate of 99.9wt% cuts into 2cm * 2cm size with purity, wherein one side be polished to minute surface, and with forward 3V, oppositely the voltage of 1V is at nickeliferous ionic electroplate liquid (NiSO with numerical control pulse electrodeposition power supply
46H
2O 300 g/L, NiCl
26H
2O 45 g/L, H
3BO
345 g/L, C
7H
5NO
3S 5 g/L) electroplated 40 seconds deposition one deck nickel nano-crystal film in.Lighting with 50wt % Tri N-Propyl Amine and 50wt% n-Butyl Amine 99 mixing solutions is the spirit lamp of fuel, the one side that aforesaid substrate is coated with nickel catalyzator places the flame envelope center towards flame core, keep taking out after 1 minute, and naturally cool to room temperature, make the nitrogen-doped graphene film.
Embodiment 8: the conductive silicon chip with 2cm * 2cm size is a substrate, and wherein one side is polished to minute surface, utilizes the surface deposition one deck cobalt nanocrystal film of magnetron sputtering technique after polishing.Lighting with the Isopropylamine is the spirit lamp of fuel, and the one side that aforesaid substrate is coated with catalyzer places the flame envelope center towards flame core, keeps taking out after 3 minutes, and naturally cools to room temperature, makes the nitrogen-doped graphene film.
Claims (8)
1. a preparation method of graphene is characterized in that, in turn includes the following steps:
Select resistant to elevated temperatures material as substrate, the surface of substrate is polished;
At the nano-crystal film of polished substrate surface growth layer of metal, this layer metallic film is as the catalyzer of growth Graphene;
With the flame that substrate places carbonaceous fuel to produce, the one side that is coated with catalyzer keeps taking out after for some time towards flame core, after the cooling, is coated with the one side indigenous graphite alkene film of catalyst layer on the substrate.
2. preparation method as claimed in claim 1 is characterized in that, described substrate material is pure metal plate, alloy sheets, monocrystalline silicon piece or polysilicon chip.
3. preparation method as claimed in claim 1 or 2 is characterized in that, described catalyst metal is nickel, cobalt, copper or iron.
4. preparation method as claimed in claim 1 or 2 is characterized in that, described carbonaceous fuel is alcohols, ethers, coke or acetylene and noble gas mixtures.
5. the preparation method of a nitrogen-doped graphene is characterized in that, in turn includes the following steps:
(1) selects resistant to elevated temperatures material as substrate, the surface of substrate is polished;
(2) at the nano-crystal film of polished substrate surface growth layer of metal, this layer metallic film is as the catalyzer of growth Graphene;
(3) flame that substrate is placed the fuel of carbon containing and nitrogen simultaneously produce, the one side that is coated with catalyzer keeps taking out after for some time towards flame core, and after the cooling, the one side that is coated with catalyst layer on the substrate is separated out the nitrogen-doped graphene film.
6. preparation method as claimed in claim 5 is characterized in that, described substrate material is pure metal plate, alloy sheets, monocrystalline silicon piece or polysilicon chip.
7. as claim 5 or 6 described preparation methods, it is characterized in that described catalyst metal is nickel, cobalt, copper or iron.
8. as claim 5 or 6 described preparation methods, it is characterized in that the fuel of described while carbon containing and nitrogen is the one or any several mixture in the amine, or amine adds the mixture that forms behind any alcohols arbitrarily.
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Cited By (7)
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CN102586869A (en) * | 2012-01-20 | 2012-07-18 | 中国科学院上海硅酸盐研究所 | Three-dimensional grapheme tube and preparation method thereof |
CN103208685A (en) * | 2013-04-12 | 2013-07-17 | 北京大学 | Corrosion-resistant electrode and manufacturing method and application thereof |
CN103924188A (en) * | 2014-05-07 | 2014-07-16 | 山东师范大学 | Method for graphene in-situ growth on insulation substrate through double-flame method under atmospheric environment |
CN104118864A (en) * | 2013-04-28 | 2014-10-29 | 国家纳米科学中心 | Graphene, preparation method of graphene, doped graphene and preparation method of doped graphene |
CN107316804A (en) * | 2017-07-07 | 2017-11-03 | 西安交通大学 | A kind of preparation method of the regular epitaxial graphene of metal atom doped large area |
CN107619036A (en) * | 2017-11-02 | 2018-01-23 | 北京化工大学 | The method that burning is oriented to quick preparation structure ordered carbon nanotube array |
CN113897075A (en) * | 2021-11-11 | 2022-01-07 | 四川烯都科技有限公司 | Preparation method of high-dispersity graphene |
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Cited By (10)
Publication number | Priority date | Publication date | Assignee | Title |
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CN102586869A (en) * | 2012-01-20 | 2012-07-18 | 中国科学院上海硅酸盐研究所 | Three-dimensional grapheme tube and preparation method thereof |
CN102586869B (en) * | 2012-01-20 | 2015-02-11 | 中国科学院上海硅酸盐研究所 | Three-dimensional grapheme tube and preparation method thereof |
CN103208685A (en) * | 2013-04-12 | 2013-07-17 | 北京大学 | Corrosion-resistant electrode and manufacturing method and application thereof |
CN104118864A (en) * | 2013-04-28 | 2014-10-29 | 国家纳米科学中心 | Graphene, preparation method of graphene, doped graphene and preparation method of doped graphene |
CN103924188A (en) * | 2014-05-07 | 2014-07-16 | 山东师范大学 | Method for graphene in-situ growth on insulation substrate through double-flame method under atmospheric environment |
CN103924188B (en) * | 2014-05-07 | 2016-06-08 | 山东师范大学 | The method of atmospheric environment lower pair flame method growth in situ Graphene on a dielectric base |
CN107316804A (en) * | 2017-07-07 | 2017-11-03 | 西安交通大学 | A kind of preparation method of the regular epitaxial graphene of metal atom doped large area |
CN107316804B (en) * | 2017-07-07 | 2019-07-23 | 西安交通大学 | A kind of preparation method of metal atom doped large area rule epitaxial graphene |
CN107619036A (en) * | 2017-11-02 | 2018-01-23 | 北京化工大学 | The method that burning is oriented to quick preparation structure ordered carbon nanotube array |
CN113897075A (en) * | 2021-11-11 | 2022-01-07 | 四川烯都科技有限公司 | Preparation method of high-dispersity graphene |
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Application publication date: 20110525 |