CN105129786A - Preparing method for massive single-layer graphene - Google Patents
Preparing method for massive single-layer graphene Download PDFInfo
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- CN105129786A CN105129786A CN201510542235.8A CN201510542235A CN105129786A CN 105129786 A CN105129786 A CN 105129786A CN 201510542235 A CN201510542235 A CN 201510542235A CN 105129786 A CN105129786 A CN 105129786A
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Abstract
A preparing method for massive single-layer graphene comprises the following steps that firstly, a metal material sheet is put into a tube furnace, heating is carried out under the normal-pressure condition in the inert gas atmosphere to increase the temperature to the calcination temperature of 800-1,040 DEG C, then hydrogen is introduced, and calcination is carried out in the inert gas and hydrogen atmosphere for 5-30 minutes; secondly, the calcination temperature is maintained, carbon-source gas and hydrogen are introduced into the tube furnace, and graphene growing is carried out for 30-120 min; thirdly, the carbon-source gas and the hydrogen are closed, and the graphene is quickly cooled to the room temperature in the inert gas. The preparing technology is simple, and massive production can be achieved; the prepared graphene has the advantages of having a single layer and being high in quality, massive, and the like; the used metal material sheet can be completely removed; the obtained graphene is stable in material structure and good in performance.
Description
Technical field
The invention belongs to field of functional materials.Relate to Graphene and preparation method thereof.
Background technology
Graphene, as a kind of novel two-dimension nano materials, is the Two Dimensional Free state atomic crystal of the unique existence found at present.Since being found experimentally from 2004, due to the physicals of its excellence and the potential application at following carbon electronics, Graphene not only receives very big concern in pure science, also show at numerous areas such as Materials science, catalysis, solid state physics, electronics, biomedicine, magnetics, optics, nano electrochemical, sensor and energy storage and there is huge application potential, cause the broad interest of scientific circles and industrial community.Current people have utilized the methods such as the reduction of mechanically peel, silicon carbide carbon epitaxial method, graphite oxide, chemical vapour deposition (CVD) method to prepare Graphene.Wherein chemical vapour deposition (CVD) method preparation method is simple, and gained Graphene quality is higher, is a kind of method of the most potential large-scale industry growing graphene at present.But the method preparing extensive high quality monolayer Graphene in atmospheric conditions rarely has report, the application that high quality monolayer Graphene applies in photovoltaic, sensor, lithium ion battery, fuel cell, ultracapacitor and various energy storage field is significant.
Summary of the invention
The object of this invention is to provide a kind of preparation method of extensive single-layer graphene, prepare high quality monolayer Graphene on a large scale in atmospheric conditions.
The present invention is achieved by the following technical solutions.
The preparation method of extensive single-layer graphene of the present invention, comprises the following steps:
(1) metal material sheet is put into tube furnace, in atmospheric conditions, be heated to calcining temperature 800-1040 DEG C in inert gas atmosphere, then pass into hydrogen, in the atmosphere of rare gas element and hydrogen, carry out calcining 5-30 minute;
(2) maintain calcining temperature, in tube furnace, pass into carbon-source gas and logical hydrogen, carry out the growth of Graphene, growth 30-120min, deposited graphite alkene in metal material sheet after firing;
(3) close carbon-source gas and hydrogen, in rare gas element, be cooled fast to room temperature.
Metal material sheet described in step of the present invention (1) is any one in copper, nickel or cobalt, and described rare gas element is argon gas.
Carbon-source gas described in step of the present invention (2) is organic molecule gas, optimization methane or the acetylene of carbon containing.
Described carbon-source gas and the volume ratio of hydrogen are 1:20-1:1, and the volume ratio of hydrogen and rare gas element is 1:10.When described carbon-source gas is methane, the airshed of methane is 2-100sccm; When described carbon-source gas is acetylene, the airshed of acetylene is 1-70sccm.
In step of the present invention (1), metal material sheet before use can successively with Glacial acetic acid, nitric acid, cleaning drying up with nitrogen.
The metal of the extensive high quality monolayer Graphene of growth provided by the present invention and Graphene both as electrode materials, can be used for energy storage as energy storage material again.
The present invention has following useful effect.
(1) preparation technology of the present invention is simple, can be mass-produced; (2) Graphene prepared by the present invention has individual layer, high quality and the advantages such as large-scale; (3) the present invention's metal material sheet used can remove completely; (4) the grapheme material Stability Analysis of Structures that obtains of the present invention, excellent performance; (5) the high quality monolayer Graphene that the present invention obtains can directly be used for carrying out physical property detection, and applies in energy related products.
Accompanying drawing explanation
Fig. 1 is the experimental installation structural representation of invention preparation high quality monolayer Graphene.
Fig. 2 is the field emission scanning electron microscope figure of extensive high quality monolayer Graphene prepared by embodiment 1.
Fig. 3 is the field emission scanning electron microscope figure of extensive high quality monolayer Graphene prepared by embodiment 2.
Fig. 4 is the field emission scanning electron microscope figure of extensive high quality monolayer Graphene prepared by embodiment 3.
Fig. 5 is the field emission scanning electron microscope figure of extensive high quality monolayer Graphene prepared by embodiment 4.
Fig. 6 is the opticmicroscope figure of extensive high quality monolayer Graphene prepared by embodiment 1.
Fig. 7 is the opticmicroscope figure of extensive high quality monolayer Graphene prepared by embodiment 2.
Fig. 8 is the opticmicroscope figure of extensive high quality monolayer Graphene prepared by embodiment 3.
Fig. 9 is the opticmicroscope figure of extensive high quality monolayer Graphene prepared by embodiment 4.
Figure 10 is the Raman spectrogram of embodiment 1 high quality monolayer Graphene prepared by the present invention.
Figure 11 is the Raman spectrogram of embodiment 2 high quality monolayer Graphene prepared by the present invention.
Figure 12 is the Raman spectrogram of embodiment 3 high quality monolayer Graphene prepared by the present invention.
Figure 13 is the Raman spectrogram of embodiment 4 high quality monolayer Graphene prepared by the present invention.
Embodiment
Below in conjunction with the drawings and specific embodiments, the present invention is described in detail.
Method described in embodiment below, if no special instructions, is ordinary method; Described material agents, if no special instructions, all can obtain from commercial channels.
Embodiment 1.
(1) copper sheet is cleaned.
Copper sheet is used successively Glacial acetic acid, deionized water, salpeter solution (concentrated nitric acid: deionized water=1:3), deionized water, Glacial acetic acid, deionized water respectively clean 10min, dry up with nitrogen afterwards.
(2) copper sheet is calcined.
Copper sheet as shown in Figure 1, is put into tube furnace silica tube by experimental installation used, in atmospheric conditions, passes into argon gas 600sccm and is exhausted 2min, then heat temperature raising, when temperature rises to 1040 DEG C, pass into hydrogen 60sccm, and keep 20min.
(3) growing graphene.
Holding temperature 1040 DEG C, after 20min, argon gas amount is adjusted to 1000sccm, and amounts of hydrogen is adjusted to 100sccm, methane 30sccm, growth 10min, closes carbon source and hydrogen, argon gas keeps 1000sccm, and fast cooling closes argon gas to room temperature, namely obtains extensive high quality monolayer Graphene.
(4) sign of material.
The Graphene that (3) step obtains is carried out Raman (Raman) Electronic Speculum and characterize (Fig. 6), be extensive high quality monolayer from the known Graphene of Fig. 2 and Figure 10, be evenly distributed.
Embodiment 2.
By the preparation method in embodiment 1, be 20sccm unlike passing into methane content.
Fig. 7 is the Raman spectrogram of the present embodiment high quality monolayer Graphene, is extensive high quality monolayer, is evenly distributed from the known Graphene of Fig. 3 and Figure 11.
Embodiment 3.
By the preparation method in embodiment 1, it is 800 DEG C unlike calcining temperature.
Fig. 8 is the Raman spectrogram of the present embodiment high quality monolayer Graphene, is extensive high quality monolayer, is evenly distributed from the known Graphene of Fig. 4 and Figure 12.
Embodiment 4.
By the preparation method in embodiment 1, acetylene is as carbon source, and its flux is 25sccm.
Fig. 9 is the Raman spectrogram of the present embodiment high quality monolayer Graphene, is extensive high quality monolayer, is evenly distributed from the known Graphene of Fig. 5 and Figure 13.
Claims (3)
1. a preparation method for extensive single-layer graphene, is characterized in that comprising the following steps:
(1) metallic substance is put into tube furnace, in atmospheric conditions, be heated to calcining temperature 800-1040 DEG C in inert gas atmosphere, then pass into hydrogen, in the atmosphere of rare gas element and hydrogen, carry out calcining 5-30 minute;
(2) maintain calcining temperature, in tube furnace, pass into carbon-source gas and logical hydrogen, carry out the growth of Graphene, growth 30-120min;
(3) close carbon-source gas and hydrogen, in rare gas element, be cooled fast to room temperature;
Metallic substance described in step (1) is any one in copper, nickel or cobalt;
Carbon-source gas described in step (2) is the organic molecule gas of carbon containing; Described carbon-source gas and the volume ratio of hydrogen are 1:20-1:1, and the volume ratio of hydrogen and rare gas element is 1:10; When described carbon-source gas is methane, the airshed of methane is 2-100sccm; When described carbon-source gas is acetylene, the airshed of acetylene is 1-70sccm.
2. the preparation method of extensive single-layer graphene according to claim 1, is characterized in that described in step (1), rare gas element is argon gas.
3. the preparation method of extensive single-layer graphene according to claim 1, is characterized in that described in step (2), carbon-source gas is methane or acetylene.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106495136A (en) * | 2016-09-27 | 2017-03-15 | 南昌大学 | A kind of preparation method of circular graphitic alkene |
| CN107619042A (en) * | 2017-10-09 | 2018-01-23 | 南昌大学 | A kind of extensive method for preparing graphene nano wall |
| CN107640763A (en) * | 2017-11-17 | 2018-01-30 | 信阳师范学院 | A kind of preparation method of individual layer single crystal graphene |
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| CN102212794A (en) * | 2011-04-13 | 2011-10-12 | 中国科学院上海微系统与信息技术研究所 | Copper plating substrate-based method for preparing large-area graphene film |
| WO2013094840A1 (en) * | 2011-12-22 | 2013-06-27 | 한국생산기술연구원 | Method for manufacturing large-scale three-dimensional transparent graphene electrodes by electrospraying, and large-scale three-dimensional transparent graphene electrode manufactured by using the method |
| WO2013180662A1 (en) * | 2012-06-01 | 2013-12-05 | National University Of Singapore | Synthesis of three-dimensional graphene foam: use as supercapacitors |
| CN103708448A (en) * | 2014-01-03 | 2014-04-09 | 中国科学院化学研究所 | Atmospheric pressure controlled growth method for graphene |
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2015
- 2015-08-31 CN CN201510542235.8A patent/CN105129786A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102212794A (en) * | 2011-04-13 | 2011-10-12 | 中国科学院上海微系统与信息技术研究所 | Copper plating substrate-based method for preparing large-area graphene film |
| WO2013094840A1 (en) * | 2011-12-22 | 2013-06-27 | 한국생산기술연구원 | Method for manufacturing large-scale three-dimensional transparent graphene electrodes by electrospraying, and large-scale three-dimensional transparent graphene electrode manufactured by using the method |
| WO2013180662A1 (en) * | 2012-06-01 | 2013-12-05 | National University Of Singapore | Synthesis of three-dimensional graphene foam: use as supercapacitors |
| CN103708448A (en) * | 2014-01-03 | 2014-04-09 | 中国科学院化学研究所 | Atmospheric pressure controlled growth method for graphene |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106495136A (en) * | 2016-09-27 | 2017-03-15 | 南昌大学 | A kind of preparation method of circular graphitic alkene |
| CN107619042A (en) * | 2017-10-09 | 2018-01-23 | 南昌大学 | A kind of extensive method for preparing graphene nano wall |
| CN107640763A (en) * | 2017-11-17 | 2018-01-30 | 信阳师范学院 | A kind of preparation method of individual layer single crystal graphene |
| CN107640763B (en) * | 2017-11-17 | 2020-02-04 | 信阳师范学院 | Preparation method of single-layer single crystal graphene |
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