CN108249430A - A kind of vapour deposition process of silicon doped graphene - Google Patents
A kind of vapour deposition process of silicon doped graphene Download PDFInfo
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- CN108249430A CN108249430A CN201810181251.2A CN201810181251A CN108249430A CN 108249430 A CN108249430 A CN 108249430A CN 201810181251 A CN201810181251 A CN 201810181251A CN 108249430 A CN108249430 A CN 108249430A
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Abstract
The invention discloses a kind of vapour deposition processes of silicon doped graphene, and step 1, graphene powder is added in into absolute ethyl alcohol, seal 30 60min of ultrasonic reaction, graphene suspension is obtained after cooling；Step 2, polyethylene glycol is added in into graphene suspension, mechanical agitation obtains graphene dispersion alcohol liquid to being completely dissolved；Step 3, graphene dispersion alcohol liquid is put into 2 5h of vacuum distillation reaction in vacuum distillation reaction kettle, obtains viscous fluid, drying obtains fluffy graphene block；Step 4, graphene block is added in reaction kettle, heating stands 20 40min, then passes to silane gas and reacts 3 8h, graphene Attraction block is obtained after naturally cold；Step 5, graphene Attraction block is added in into 30 60min of ultrasonic reaction in absolute ethyl alcohol, silicon doping precipitation is obtained after filtering；Step 6, silicon doping is deposited in heating 3 6h of compressive reaction in hydrogen reaction kettle, silicon doped graphene is obtained after cooling.The present invention have it is simple for process, silicon doping rate controllability is strong, suitable for large area produce.
Description
Technical field
The invention belongs to technical field of graphene, and in particular to a kind of vapour deposition process of silicon doped graphene.
Background technology
The discovery of graphene confirms the new stage of the research for being stabilized and opening two-dimensional material of two-dimensional material,
Graphene has excellent photoelectric properties as a kind of carbon material of monoatomic layer, causes the interest of scientist, such as it
Carrier mobility can reach 200,000cm2/ V.s, this can manufacture the electronics of high-frequency operation for it and provide the foundation, single
Layer graphene is absorbed as 2.3% to light, this enables it to become a kind of important material of photoelectric device research.But stone
While black alkene possesses excellent photoelectric characteristic, it have there are one it is very serious the defects of, i.e., energy gap is zero, this causes it
In the application of micro-nano opto-electronic device, there are certain restriction effects.In current experiment, it is typically employed to prepare graphene
The methods such as nanobelt open the energy band of graphene, but energy band size is all in below 300meV.In addition, scientists are using doping
The mode of graphene adjusts the fermi level of graphene, so as to changing the electrical properties of graphene and optical property.It is adulterating
Mode in, generally use chemical doping and electrically doped mode, for example, N doping, boron doping and add grid voltage doping etc..
The drawbacks of this kind of doping way, can change over time with the property of graphene after doping, it is impossible to be stabilized.
In comparison, the displacement doping way of the carbon atom in silicon atom replacement graphene is better able to keep doped graphene property
Stablize, and not yet someone obtains the graphene of silicon doping at present.
Invention content
For the problems of the prior art, the present invention provides a kind of vapour deposition process of silicon doped graphene, solves stone
Blank in terms of black alkene silicon doping techniques, have it is simple for process, silicon doping rate controllability is strong, suitable for large area produce.
For realization more than technical purpose, the technical scheme is that：
A kind of vapour deposition process of silicon doped graphene, the vapour deposition process is in accordance with the following steps：
Step 1, graphene powder is added in into absolute ethyl alcohol, seals ultrasonic reaction 30-60min, stone is obtained after cooling
Black alkene suspension；
Step 2, polyethylene glycol is added in into graphene suspension, mechanical agitation obtains graphene point to being completely dissolved
Dissipate alcohol liquid；
Step 3, graphene dispersion alcohol liquid is put into vacuum distillation reaction 2-5h in vacuum distillation reaction kettle, obtained sticky
Liquid, drying obtain fluffy graphene block；
Step 4, graphene block is added in reaction kettle, heating stands 20-40min, then passes to silane gas reaction 3-
8h obtains graphene Attraction block after naturally cold；
Step 5, graphene Attraction block is added in into ultrasonic reaction 30-60min in absolute ethyl alcohol, it is heavy that silicon doping is obtained after filtering
It forms sediment；
Step 6, silicon doping is deposited in heating compressive reaction 3-6h in hydrogen reaction kettle, silicon doped graphite is obtained after cooling
Alkene.
A concentration of 20-40g/L of the graphene in absolute ethyl alcohol in the step 1, the frequency of the sealing ultrasonic reaction
Rate is 5-10kHz, and temperature is 50-70 DEG C.
The addition of polyethylene glycol in the step 2 is the 40-60% of graphene powder quality, described churned mechanically
Mixing speed is 2000-4000r/min.
The pressure of vacuum distillation reaction in the step 3 is the 50-70% of atmospheric pressure, and temperature is 60-80 DEG C, described viscous
The volume of magma is the 10-15% of graphene dispersion alcohol liquid.
The temperature that heating in the step 4 is stood is 500-700 DEG C.
Silane intake in the step 4 is the 20-40% of graphene quality, and the speed that is passed through of the silane gas is
20-40mL/min。
Absolute ethyl alcohol addition is the 60-80% of graphene powder quality in the step 5, the ultrasound of the ultrasonic reaction
Frequency is 10-15kHz.
Added hydrogen in the step 6 is the 50-60% of graphene quality.
The temperature of the heating compressive reaction is 300-400 DEG C, pressure 2-4MPa.
Graphene powder is stirred by ultrasonic step 1 in absolute ethyl alcohol, can form good suspended state, and to ensure
The dispersion of graphene in ethanol, ultrasonic temperature are no more than 75 DEG C.
Step 2 adds in polyethylene glycol into suspension, can form good dispersion effect, while polyethylene glycol is in itself
, can be by graphene dispersion to absolute ethyl alcohol with good dispersion effect, while there is good adhesive, it can be in second
Graphene is bonded after alcoholic solvent removal, forms more slack and undisciplined graphene-structured.
Step 3 will be removed absolute ethyl alcohol by way of vacuum distillation in graphene dispersion alcohol liquid, after forming viscous fluid,
Remaining graphene is removed by way of drying, obtains the graphene block that polyethylene glycol is binding agent.
Loose graphene block is carried out heating standing by step 4, can ensure polyethylene glycol complete oxidation, is formed and is stablized knot
Structure, while ensure the loose structure of graphene block；Silane gas be passed through can quick adsorption in graphene surface, formed good
Doping adsorption effect.
Step 5 by the graphene Attraction block adsorbed can in absolute ethyl alcohol ultrasonic reaction, at this time will be in graphene
Oxidation polyethylene glycol is dissolved completely in absolute ethyl alcohol, and silicon doped graphene re-forms powdery at this time, and uniformly disperses to nothing
In water-ethanol, the precipitation of relatively stable silicon doping is obtained after filtering.
The progress pressurized, heated reaction under the action of being deposited in hydrogen that step 6 adulterates silicon, obtains good silicon doping stone
Black alkene material.
From the above, it can be seen that the present invention has advantages below：
1. the present invention solves the blank in terms of graphene silicon doping techniques, there is simple for process, silicon doping rate controllability
By force, it is produced suitable for large area.
2. silicon doped graphene prepared by the present invention is not only stable for the optical property and electric property of graphene, moreover it is possible to protect
Graphene performance efficiency is demonstrate,proved to stablize, passage not at any time and change.
3. the present invention makes full use of the alcohol-soluble of polyethylene glycol using polyethylene glycol as binding agent, adsorbent and parsing agent,
It ensure that the enrichment, infiltration and doping of silane gas.
4. the present invention can utilize the excellent permeability of gas using gas reduction method, reduction effect is promoted, can be formed
Relatively stable silicon adulterates effect.
Specific embodiment
The present invention will be described in detail in conjunction with the embodiments, but does not do any restriction to the claim of the present invention.
Embodiment 1
A kind of vapour deposition process of silicon doped graphene, the vapour deposition process is in accordance with the following steps：
Step 1, graphene powder is added in into absolute ethyl alcohol, seals ultrasonic reaction 30min, graphene is obtained after cooling
Suspension；
Step 2, polyethylene glycol is added in into graphene suspension, mechanical agitation obtains graphene point to being completely dissolved
Dissipate alcohol liquid；
Step 3, graphene dispersion alcohol liquid is put into vacuum distillation reaction 2h in vacuum distillation reaction kettle, obtains viscous fluid,
Drying obtains fluffy graphene block；
Step 4, graphene block being added in reaction kettle, heating stands 20min, then passes to silane gas reaction 3-8h,
Naturally graphene Attraction block is obtained after cold；
Step 5, graphene Attraction block is added in into ultrasonic reaction 30min in absolute ethyl alcohol, silicon doping precipitation is obtained after filtering；
Step 6, silicon doping is deposited in heating compressive reaction 3h in hydrogen reaction kettle, silicon doped graphite is obtained after cooling
Alkene.
A concentration of 20g/L of the graphene in absolute ethyl alcohol in the step 1, the frequency of the sealing ultrasonic reaction are
5kHz, temperature are 50 DEG C.
The addition of polyethylene glycol in the step 2 is the 40% of graphene powder quality, described churned mechanically to stir
Speed is mixed as 2000r/min.
The pressure of vacuum distillation reaction in the step 3 is the 50% of atmospheric pressure, and temperature is 60 DEG C, the viscous fluid
Volume is the 10% of graphene dispersion alcohol liquid.
The temperature that heating in the step 4 is stood is 500 DEG C.
Silane intake in the step 4 is the 20% of graphene quality, and the speed that is passed through of the silane gas is
20mL/min。
Absolute ethyl alcohol addition is the 60% of graphene powder quality in the step 5, the supersonic frequency of the ultrasonic reaction
Rate is 10kHz.
Added hydrogen in the step 6 is the 50% of graphene quality.
The temperature of the heating compressive reaction is 300 DEG C, pressure 2MPa.
Embodiment 2
A kind of vapour deposition process of silicon doped graphene, the vapour deposition process is in accordance with the following steps：
Step 1, graphene powder is added in into absolute ethyl alcohol, seals ultrasonic reaction 60min, graphene is obtained after cooling
Suspension；
Step 2, polyethylene glycol is added in into graphene suspension, mechanical agitation obtains graphene point to being completely dissolved
Dissipate alcohol liquid；
Step 3, graphene dispersion alcohol liquid is put into vacuum distillation reaction 5h in vacuum distillation reaction kettle, obtains viscous fluid,
Drying obtains fluffy graphene block；
Step 4, graphene block being added in reaction kettle, heating stands 40min, then passes to silane gas reaction 3-8h,
Naturally graphene Attraction block is obtained after cold；
Step 5, graphene Attraction block is added in into ultrasonic reaction 60min in absolute ethyl alcohol, silicon doping precipitation is obtained after filtering；
Step 6, silicon doping is deposited in heating compressive reaction 6h in hydrogen reaction kettle, silicon doped graphite is obtained after cooling
Alkene.
A concentration of 40g/L of the graphene in absolute ethyl alcohol in the step 1, the frequency of the sealing ultrasonic reaction are
10kHz, temperature are 70 DEG C.
The addition of polyethylene glycol in the step 2 is the 60% of graphene powder quality, described churned mechanically to stir
Speed is mixed as 4000r/min.
The pressure of vacuum distillation reaction in the step 3 is the 70% of atmospheric pressure, and temperature is 80 DEG C, the viscous fluid
Volume is the 15% of graphene dispersion alcohol liquid.
The temperature that heating in the step 4 is stood is 700 DEG C.
Silane intake in the step 4 is the 40% of graphene quality, and the speed that is passed through of the silane gas is
40mL/min。
Absolute ethyl alcohol addition is the 80% of graphene powder quality in the step 5, the supersonic frequency of the ultrasonic reaction
Rate is 15kHz.
Added hydrogen in the step 6 is the 60% of graphene quality.
The temperature of the heating compressive reaction is 400 DEG C, pressure 4MPa.
Embodiment 3
A kind of vapour deposition process of silicon doped graphene, the vapour deposition process is in accordance with the following steps：
Step 1, graphene powder is added in into absolute ethyl alcohol, seals ultrasonic reaction 50min, graphene is obtained after cooling
Suspension；
Step 2, polyethylene glycol is added in into graphene suspension, mechanical agitation obtains graphene point to being completely dissolved
Dissipate alcohol liquid；
Step 3, graphene dispersion alcohol liquid is put into vacuum distillation reaction 4h in vacuum distillation reaction kettle, obtains viscous fluid,
Drying obtains fluffy graphene block；
Step 4, graphene block being added in reaction kettle, heating stands 30min, then passes to silane gas reaction 3-8h,
Naturally graphene Attraction block is obtained after cold；
Step 5, graphene Attraction block is added in into ultrasonic reaction 45min in absolute ethyl alcohol, silicon doping precipitation is obtained after filtering；
Step 6, silicon doping is deposited in heating compressive reaction 5h in hydrogen reaction kettle, silicon doped graphite is obtained after cooling
Alkene.
A concentration of 30g/L of the graphene in absolute ethyl alcohol in the step 1, the frequency of the sealing ultrasonic reaction are
8kHz, temperature are 60 DEG C.
The addition of polyethylene glycol in the step 2 is the 50% of graphene powder quality, described churned mechanically to stir
Speed is mixed as 3000r/min.
The pressure of vacuum distillation reaction in the step 3 is the 60% of atmospheric pressure, and temperature is 70 DEG C, the viscous fluid
Volume is the 13% of graphene dispersion alcohol liquid.
The temperature that heating in the step 4 is stood is 600 DEG C.
Silane intake in the step 4 is the 30% of graphene quality, and the speed that is passed through of the silane gas is
30mL/min。
Absolute ethyl alcohol addition is the 70% of graphene powder quality in the step 5, the supersonic frequency of the ultrasonic reaction
Rate is 13kHz.
Added hydrogen in the step 6 is the 55% of graphene quality.
The temperature of the heating compressive reaction is 350 DEG C, pressure 3MPa.
In conclusion the present invention has the following advantages：
1. the present invention solves the blank in terms of graphene silicon doping techniques, there is simple for process, silicon doping rate controllability
By force, it is produced suitable for large area.
2. silicon doped graphene prepared by the present invention is not only stable for the optical property and electric property of graphene, moreover it is possible to protect
Graphene performance efficiency is demonstrate,proved to stablize, passage not at any time and change.
3. the present invention makes full use of the alcohol-soluble of polyethylene glycol using polyethylene glycol as binding agent, adsorbent and parsing agent,
It ensure that the enrichment, infiltration and doping of silane gas.
4. the present invention can utilize the excellent permeability of gas using gas reduction method, reduction effect is promoted, can be formed
Relatively stable silicon adulterates effect.
It is understood that above with respect to the specific descriptions of the present invention, it is merely to illustrate the present invention and is not limited to this
The described technical solution of inventive embodiments.It will be understood by those of ordinary skill in the art that still the present invention can be carried out
Modification or equivalent replacement, to reach identical technique effect；As long as meeting using needs, all protection scope of the present invention it
It is interior.
Claims (9)
1. a kind of vapour deposition process of silicon doped graphene, it is characterised in that：The vapour deposition process is in accordance with the following steps：
Step 1, graphene powder is added in into absolute ethyl alcohol, seals ultrasonic reaction 30-60min, graphene is obtained after cooling
Suspension；
Step 2, polyethylene glycol is added in into graphene suspension, mechanical agitation obtains graphene dispersion alcohol to being completely dissolved
Liquid；
Step 3, graphene dispersion alcohol liquid is put into vacuum distillation reaction 2-5h in vacuum distillation reaction kettle, obtains viscous fluid, dry
It is dry to obtain fluffy graphene block；
Step 4, graphene block being added in reaction kettle, heating stands 20-40min, then passes to silane gas reaction 3-8h, from
So it is cold after obtain graphene Attraction block；
Step 5, graphene Attraction block is added in into ultrasonic reaction 30-60min in absolute ethyl alcohol, silicon doping precipitation is obtained after filtering；
Step 6, silicon doping is deposited in heating compressive reaction 3-6h in hydrogen reaction kettle, silicon doped graphene is obtained after cooling.
2. a kind of vapour deposition process of silicon doped graphene according to claim 1, it is characterised in that：In the step 1
A concentration of 20-40g/L of the graphene in absolute ethyl alcohol, the frequency of the sealing ultrasonic reaction is 5-10kHz, and temperature is
50-70℃。
3. a kind of vapour deposition process of silicon doped graphene according to claim 1, it is characterised in that：In the step 2
Polyethylene glycol addition be graphene powder quality 40-60%, the churned mechanically mixing speed be 2000-
4000r/min。
4. a kind of vapour deposition process of silicon doped graphene according to claim 1, it is characterised in that：In the step 3
Vacuum distillation reaction pressure be atmospheric pressure 50-70%, temperature be 60-80 DEG C, the volume of the viscous fluid is graphene
Disperse the 10-15% of alcohol liquid.
5. a kind of vapour deposition process of silicon doped graphene according to claim 1, it is characterised in that：In the step 4
Heating stand temperature be 500-700 DEG C.
6. a kind of vapour deposition process of silicon doped graphene according to claim 1, it is characterised in that：In the step 4
Silane intake be graphene quality 20-40%, the silane gas is passed through speed as 20-40mL/min.
7. a kind of vapour deposition process of silicon doped graphene according to claim 1, it is characterised in that：In the step 5
Absolute ethyl alcohol addition is the 60-80% of graphene powder quality, and the supersonic frequency of the ultrasonic reaction is 10-15kHz.
8. a kind of vapour deposition process of silicon doped graphene according to claim 1, it is characterised in that：In the step 6
Added hydrogen be graphene quality 50-60%.
9. a kind of vapour deposition process of silicon doped graphene according to claim 1, it is characterised in that：The heating pressurization
The temperature of reaction is 300-400 DEG C, pressure 2-4MPa.
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| CN111392719A (en) * | 2020-03-12 | 2020-07-10 | 兰州大学 | Silicon-doped graphene, preparation method thereof and silicon-doped graphene-based chemical resistance type nitrogen oxide room temperature sensor |
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| CN104591168A (en) * | 2015-01-16 | 2015-05-06 | 浙江大学 | Preparation method of silicon-doped graphene material |
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| CN104591168A (en) * | 2015-01-16 | 2015-05-06 | 浙江大学 | Preparation method of silicon-doped graphene material |
| CN105463401A (en) * | 2015-12-02 | 2016-04-06 | 浙江大学 | Method for preparing silicon-doped graphene materials through chemical vapor deposition |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN111392719A (en) * | 2020-03-12 | 2020-07-10 | 兰州大学 | Silicon-doped graphene, preparation method thereof and silicon-doped graphene-based chemical resistance type nitrogen oxide room temperature sensor |
| CN111392719B (en) * | 2020-03-12 | 2021-02-09 | 兰州大学 | Silicon-doped graphene, preparation method thereof and silicon-doped graphene-based chemical resistance type nitrogen oxide room temperature sensor |
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