CN105776200B - A kind of photo catalytic reduction continuously prepares the device and method of graphene - Google Patents
A kind of photo catalytic reduction continuously prepares the device and method of graphene Download PDFInfo
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- CN105776200B CN105776200B CN201610340432.6A CN201610340432A CN105776200B CN 105776200 B CN105776200 B CN 105776200B CN 201610340432 A CN201610340432 A CN 201610340432A CN 105776200 B CN105776200 B CN 105776200B
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Abstract
The invention discloses the device that a kind of photo catalytic reduction continuously prepares graphene, including reactor, peristaltic pump, precursor liquid storage bottle and graphene storage bottle, the reactor is transparent spiral glass tube, one end of transparent spiral glass tube is charging aperture, the other end is discharging opening, the peristaltic pump is arranged between charging aperture and precursor liquid storage bottle, and be connected between charging aperture and precursor liquid storage bottle by the wriggling pump hose of peristaltic pump, it is connected between the discharging opening and graphene storage bottle by discharge nozzle, by transparent glass tube, spiral winding forms after internal spiral that spiral winding is made from bottom to up further around the internal spiral to the transparent spiral glass tube from top to bottom, reflective membrane is enclosed with the outside of the reactor.In addition, continuously preparing the method for graphene the invention also discloses photo catalytic reduction.The present invention can realize that photo catalytic reduction process is continuously controllable, greatly improve the preparation efficiency of graphene, fully reduce cost, it is easy to accomplish prepared by industrial mass.
Description
Technical field
The invention belongs to technical field of nanometer material preparation, and in particular to a kind of photo catalytic reduction continuously prepares graphene
Device and method.
Background technology
Graphene is a kind of Two-dimensional structural carbon nanomaterial with monoatomic layer thickness.It has a kind of bi-dimensional cellular shape
Crystal structure, the carbon atom of its internal each hydbridized carbon atoms and surrounding constitutes stable hexagon.Graphene is the world
On most thin two-dimensional material, hydbridized carbon atoms can form the big pi bond of delocalization, and electronics can be moved freely inside it,
This special structure makes graphene have many excellent physics and chemical property.Graphene have outstanding mechanics, optics,
Calorifics and electrical properties, make it possess in all many-sides such as energy and material, super capacitor, composite, micro-nano electronic devices
Wide application prospect.
The preparation method of graphene has a lot, including mechanical stripping method, oxidation-reduction method, chemical vapour deposition technique, crystal
Epitaxial growth method, electrochemical process, arc process, cutting carbon nanotubes etc..Wherein, the graphene size hardly possible control that prepared by mechanical stripping method
System and low yield, are only applicable to laboratory and carry out basic research；Though the methods such as arc discharge method, epitaxial growth method, electrochemical process
High-quality graphene can be so prepared, but condition is just carved, low yield, it is impossible to meet the demand of actual large-scale application.
Compared with the above method, its preparation process of chemistry redox method is relatively easy, it is development side prepared by industrial mass
To.
It is general using (hydrazine hydrate, strong with toxicity or corrosive reducing agent during current traditional chemical restoring method
Alkali etc.), easily pollute environment；Reduction process is typically reacted using in quantitative vessel in heating stirring simultaneously, during reaction
Between it is longer, efficiency is low, it is impossible to realize serialization reduction preparation.
The content of the invention
The technical problems to be solved by the invention are that there is provided a kind of photo catalytic reduction for above-mentioned the deficiencies in the prior art
The continuous device for preparing graphene.The apparatus structure is simple, reasonable in design, using by transparent glass tube spiral winding from top to bottom
Formed after internal spiral further around the internal spiral transparent spiral glass tube that spiral winding is made from bottom to up as reactor,
It can realize that photo catalytic reduction process is continuously controllable, greatly improve the preparation efficiency of graphene.
In order to solve the above technical problems, the technical solution adopted by the present invention is：A kind of photo catalytic reduction continuously prepares graphite
The device of alkene, it is characterised in that including reactor, peristaltic pump, precursor liquid storage bottle and graphene storage bottle, the reactor is transparent
Spiral glass tube, one end of transparent spiral glass tube is charging aperture, and the other end is discharging opening, and the peristaltic pump is arranged at charging aperture
Be connected between precursor liquid storage bottle, and between charging aperture and precursor liquid storage bottle by the wriggling pump hose of peristaltic pump, it is described go out
It is connected between material mouth and graphene storage bottle by discharge nozzle, the transparent spiral glass tube is by transparent glass tube spiral shell from top to bottom
Rotation is wound after internal spiral further around the internal spiral that spiral winding is made from bottom to up, around the internal spiral from it is lower to
The structure of upper spiral winding formation is external spiral body, and the charging aperture is located at the transparent glass tube openend for forming internal spiral,
Discharging opening is located at the transparent glass tube openend for forming external spiral body, and charging aperture and discharging opening are respectively positioned on transparent spiral glass tube
Top, be enclosed with reflective membrane on the outside of the reactor.
A kind of above-mentioned photo catalytic reduction continuously prepares the device of graphene, it is characterised in that on the reflective membrane and position
Peep hole is offered in the middle part and bottom of reactor.
A kind of above-mentioned photo catalytic reduction continuously prepares the device of graphene, it is characterised in that the layer of the internal spiral
Number is 12~14 layers, and the number of plies of external spiral body is 14~16 layers.
A kind of above-mentioned photo catalytic reduction continuously prepares the device of graphene, it is characterised in that on the discharge nozzle and position
Ultraviolet Detector is provided between discharging opening and graphene storage bottle.
In addition, present invention also offers a kind of method that use said apparatus prepares graphene, it is characterised in that including with
Lower step：
Step 1: by reducing agent and graphene oxide according to 1:The mass ratio mixing of (0.5~2), then by reducing agent and
The mixture ultrasonic disperse of graphene oxide is dissolved in deionized water, is adjusted pH value to 7~10 with ammoniacal liquor, is obtained precursor liquid；Institute
The concentration for stating graphene oxide in precursor liquid is 0.1mg/mL~10mg/mL；
Step 2: light source to be placed in the middle part of the internal spiral of reactor and light source is opened, then by described in step one
Precursor liquid is placed in precursor liquid storage bottle, and the precursor liquid in precursor liquid storage bottle is continuously pumped into reactor by peristaltic pump, and controls
The residence time of precursor liquid processed in the reactor is 0.5h~1h, and the precursor liquid being pumped into reactor issues the third contact of a total solar or lunar eclipse in illumination condition
Flowed into after catalytic reaction through discharge nozzle in graphene storage bottle；The light source is iodine-tungsten lamp, incandescent lamp or uviol lamp；
Step 3: the material filtering collected in graphene storage bottle or centrifugation are removed into solvent, graphene is obtained, washing is obtained
Graphene, dry after obtain graphene powder.
Above-mentioned method, it is characterised in that reducing agent described in step one is ascorbic acid, formic acid, glucose, lemon
Acid, oxalic acid, ammonium carbonate or ammonium hydrogen carbonate.
Above-mentioned method, it is characterised in that in step 2 the power of iodine-tungsten lamp, incandescent lamp and uviol lamp be 20W~
3000W。
The present invention has advantages below compared with prior art：
1st, apparatus structure of the invention is simple, reasonable in design, using by transparent glass tube, spiral winding is formed from top to bottom
, can further around the internal spiral transparent spiral glass tube that spiral winding is made from bottom to up as reactor after internal spiral
Realize that photo catalytic reduction process is continuously controllable, greatly improve the preparation efficiency of graphene.
2nd, the present invention offers preferably on reflective membrane and peep hole positioned at the middle part and bottom of reactor, can be continuous
The color of in the middle part of transparent spiral glass tube and bottom is observed by the naked eye in course of reaction, the real-time monitoring of course of reaction is realized.
3rd, the present invention, can preferably on discharge nozzle and positioned at Ultraviolet Detector is provided between discharging opening and graphene storage bottle
The real-time detection of reaction product in tandem reaction sequence is realized, realizes that photo catalytic reduction process is continuously controllable.
4th, the present invention can be obviously promoted reduction reaction progress by introducing light irradiation catalysis redox graphene, real
Existing reduction process is continuously controllable, greatly improves preparation efficiency, fully reduces cost, it is easy to accomplish prepared by industrial mass.
5th, the present invention is reacted by using non-toxic, gentle reducing agent, it is possible to achieve prepared by environmental protection, simultaneously
Do not introduce metal ion, it is to avoid pollution environment.
6th, graphene powder size uniform prepared by the present invention, with 1~10 layer of monoatomic layer, minimum thickness is reachable
0.4nm, while graphene has good dispersiveness.
With reference to the accompanying drawings and examples, technical scheme is described in further detail.
Figure of description
Fig. 1 is that apparatus of the present invention remove the structural representation after reflective membrane.
Fig. 2 is the x diffraction θ -2 θ scanning figures of graphene prepared by the embodiment of the present invention 2.
Fig. 3 is the scanning electron microscope (SEM) photograph of graphene pattern prepared by the embodiment of the present invention 2.
Fig. 4 is the atomic force scanning figure of graphene prepared by the embodiment of the present invention 2.
Description of reference numerals：
1-precursor liquid storage bottle；2-peristaltic pump；3-wriggling pump hose；
4-charging aperture；5-discharging opening；6-reactor；
7-discharge nozzle；8-Ultraviolet Detector；9-graphene storage bottle.
Embodiment
Embodiment 1
As shown in figure 1, the photo catalytic reduction of the present embodiment continuously prepares the device of graphene, including reactor 6, peristaltic pump
2nd, precursor liquid storage bottle 1 and graphene storage bottle 9, the reactor 6 are transparent spiral glass tube, and one end of transparent spiral glass tube is
Charging aperture 4, the other end is discharging opening 5, and the peristaltic pump 2 is arranged between charging aperture 4 and precursor liquid storage bottle 1, and charging aperture 4 with
It is connected between precursor liquid storage bottle 1 by the wriggling pump hose 3 of peristaltic pump 2, is led between the discharging opening 5 and graphene storage bottle 9
Cross discharge nozzle 7 to be connected, by transparent glass tube, spiral winding is formed after internal spiral the transparent spiral glass tube from top to bottom
Further around the internal spiral, spiral winding is made from bottom to up, around the structure of internal spiral spiral winding formation from bottom to up
For external spiral body, the charging aperture 4 is located at the transparent glass tube openend for forming internal spiral, and discharging opening 5, which is located at, forms outer spiral shell
The transparent glass tube openend of body is revolved, and charging aperture 4 and discharging opening 5 are respectively positioned on the top of transparent spiral glass tube, the reaction
The outside of device 6 is enclosed with reflective membrane.
In the present embodiment, peep hole is offered on the reflective membrane and positioned at the middle part and bottom of reactor 6.
In the present embodiment, preferably 12~14 layers of the number of plies of the internal spiral, preferably 14~16 layers of the number of plies of external spiral body.
In the present embodiment, on the discharge nozzle 7 and positioned at being provided with ultraviolet detection between discharging opening 5 and graphene storage bottle 9
Instrument 8.
Embodiment 2
The number of plies that the present embodiment prepares internal spiral in graphene, device using the device of embodiment 1 is 12 layers, external spiral
The number of plies of body is 14 layers, and specific preparation method comprises the following steps：
Step 1: by reducing agent and graphene oxide according to 1:1 mass ratio mixing, then by reducing agent and graphite oxide
The mixture ultrasonic disperse of alkene is dissolved in deionized water, is adjusted pH value to 10 with ammoniacal liquor, is obtained precursor liquid；Oxygen in the precursor liquid
The concentration of graphite alkene is 0.1mg/mL；The reducing agent is ascorbic acid；
Step 2: light source to be placed in the middle part of the internal spiral of reactor 6 and light source is opened, then by described in step one
Precursor liquid is placed in precursor liquid storage bottle 1, and the precursor liquid in precursor liquid storage bottle 1 is continuously pumped into reactor 6 by peristaltic pump 2,
And control residence time of the precursor liquid in reactor 6 to be 0.5h, it is pumped into the precursor liquid in reactor 6 and occurs under illumination condition
Flowed into after light-catalyzed reaction through discharge nozzle 7 in graphene storage bottle 9；The light source is iodine-tungsten lamp, and power is 1000W；
Step 3: the material filtering collected in graphene storage bottle 9 is removed into solvent, graphene is obtained, obtained stone is washed
Black alkene, graphene powder is obtained after drying.
Fig. 2 is the x diffraction θ -2 θ scanning figures of graphene manufactured in the present embodiment, and as can be seen from the figure graphene has
CeO2(002) peak, and the dephasign peak without graphene oxide, display are fully reduced.Fig. 3 is graphite manufactured in the present embodiment
ESEM (SEM) figure of alkene, as can be seen from the figure graphene is in individual layer sheet, with good uniformity and dispersiveness,
Bright plication region is the natural shrinking of reduction process in figure.Fig. 4 scans for the atomic force of graphene manufactured in the present embodiment
(AFM) figure, it can be seen that the thickness of graphene is 0.4nm, it is individual layer to show graphene.Stone manufactured in the present embodiment
Black alkene piece footpath size is 1.5 microns, and thickness is 0.4nm, and graphene is individual layer, with good uniform dispersiveness.
Embodiment 3
The number of plies that the present embodiment prepares internal spiral in graphene, device using the device of embodiment 1 is 13 layers, external spiral
The number of plies of body is 15 layers, and specific preparation method comprises the following steps：
Step 1: by reducing agent and graphene oxide according to 1:2 mass ratio mixing, then by reducing agent and graphite oxide
The mixture ultrasonic disperse of alkene is dissolved in deionized water, is adjusted pH value to 8 with ammoniacal liquor, is obtained precursor liquid；Oxygen in the precursor liquid
The concentration of graphite alkene is 1mg/mL；The reducing agent is ammonium hydrogen carbonate；
Step 2: light source to be placed in the middle part of the internal spiral of reactor 6 and light source is opened, then by described in step one
Precursor liquid is placed in precursor liquid storage bottle 1, and the precursor liquid in precursor liquid storage bottle 1 is continuously pumped into reactor 6 by peristaltic pump 2,
And control residence time of the precursor liquid in reactor 6 to be 0.8h, it is pumped into the precursor liquid in reactor 6 and occurs under illumination condition
Flowed into after light-catalyzed reaction through discharge nozzle 7 in graphene storage bottle 9；The light source is uviol lamp, and power is 3000W；
Step 3: the material collected in graphene storage bottle 9 centrifugation is removed into solvent, graphene is obtained, obtained stone is washed
Black alkene, graphene powder is obtained after drying.
Graphene film footpath manufactured in the present embodiment size is 0.5~3 micron, and thickness is 1nm, and graphene is 3 layers, with good
Good uniform dispersiveness.
Embodiment 4
The number of plies that the present embodiment prepares internal spiral in graphene, device using the device of embodiment 1 is 14 layers, external spiral
The number of plies of body is 16 layers, and specific preparation method comprises the following steps：
Step 1: by reducing agent and graphene oxide according to 1:0.5 mass ratio mixing, then by reducing agent and oxidation stone
The mixture ultrasonic disperse of black alkene is dissolved in deionized water, is adjusted pH value to 7 with ammoniacal liquor, is obtained precursor liquid；In the precursor liquid
The concentration of graphene oxide is 10mg/mL；The reducing agent is glucose；
Step 2: light source to be placed in the middle part of the internal spiral of reactor 6 and light source is opened, then by described in step one
Precursor liquid is placed in precursor liquid storage bottle 1, and the precursor liquid in precursor liquid storage bottle 1 is continuously pumped into reactor 6 by peristaltic pump 2,
And controlling residence time of the precursor liquid in reactor 6 to be 1h, the precursor liquid being pumped into reactor 6 issues the third contact of a total solar or lunar eclipse in illumination condition
Flowed into after catalytic reaction through discharge nozzle 7 in graphene storage bottle 9；The light source is iodine-tungsten lamp, and power is 20W；
Step 3: the material filtering collected in graphene storage bottle 9 is removed into solvent, graphene is obtained, obtained stone is washed
Black alkene, graphene powder is obtained after drying.
Graphene film footpath manufactured in the present embodiment size reaches 2 microns, and thickness is 2nm, and graphene is 6 layers, with good
Uniform dispersiveness.
Embodiment 5
The number of plies that the present embodiment prepares internal spiral in graphene, device using the device of embodiment 1 is 14 layers, external spiral
The number of plies of body is 14 layers, and specific preparation method comprises the following steps：
Step 1: by reducing agent and graphene oxide according to 1:1.5 mass ratio mixing, then by reducing agent and oxidation stone
The mixture ultrasonic disperse of black alkene is dissolved in deionized water, is adjusted pH value to 9 with ammoniacal liquor, is obtained precursor liquid；In the precursor liquid
The concentration of graphene oxide is 5mg/mL；The reducing agent is formic acid；
Step 2: light source to be placed in the middle part of the internal spiral of reactor 6 and light source is opened, then by described in step one
Precursor liquid is placed in precursor liquid storage bottle 1, and the precursor liquid in precursor liquid storage bottle 1 is continuously pumped into reactor 6 by peristaltic pump 2,
And controlling residence time of the precursor liquid in reactor 6 to be 1h, the precursor liquid being pumped into reactor 6 issues the third contact of a total solar or lunar eclipse in illumination condition
Flowed into after catalytic reaction through discharge nozzle 7 in graphene storage bottle 9；The light source is incandescent lamp, and power is 20W；
Step 3: the material collected in graphene storage bottle 9 centrifugation is removed into solvent, graphene is obtained, obtained stone is washed
Black alkene, graphene powder is obtained after drying.
Graphene film footpath manufactured in the present embodiment size is 0.5~3 micron, and thickness is 3nm, and graphene is 10 layers, is had
Good uniform dispersiveness.
Embodiment 6
The number of plies that the present embodiment prepares internal spiral in graphene, device using the device of embodiment 1 is 14 layers, external spiral
The number of plies of body is 16 layers, and specific preparation method comprises the following steps：
Step 1: by reducing agent and graphene oxide according to 1:2 mass ratio mixing, then by reducing agent and graphite oxide
The mixture ultrasonic disperse of alkene is dissolved in deionized water, is adjusted pH value to 10 with ammoniacal liquor, is obtained precursor liquid；Oxygen in the precursor liquid
The concentration of graphite alkene is 6mg/mL；The reducing agent is citric acid；
Step 2: light source to be placed in the middle part of the internal spiral of reactor 6 and light source is opened, then by described in step one
Precursor liquid is placed in precursor liquid storage bottle 1, and the precursor liquid in precursor liquid storage bottle 1 is continuously pumped into reactor 6 by peristaltic pump 2,
And control residence time of the precursor liquid in reactor 6 to be 0.5h, it is pumped into the precursor liquid in reactor 6 and occurs under illumination condition
Flowed into after light-catalyzed reaction through discharge nozzle 7 in graphene storage bottle 9；The light source is uviol lamp, and power is 2000W；
Step 3: the material filtering collected in graphene storage bottle 9 is removed into solvent, graphene is obtained, obtained stone is washed
Black alkene, graphene powder is obtained after drying.
Graphene film footpath manufactured in the present embodiment size is 0.5~3 micron, and thickness is 2nm, and graphene is 6 layers, with good
Good uniform dispersiveness.
Embodiment 7
The number of plies that the present embodiment prepares internal spiral in graphene, device using the device of embodiment 1 is 14 layers, external spiral
The number of plies of body is 16 layers, and specific preparation method comprises the following steps：
Step 1: by reducing agent and graphene oxide according to 1:1 mass ratio mixing, then by reducing agent and graphite oxide
The mixture ultrasonic disperse of alkene is dissolved in deionized water, is adjusted pH value to 7 with ammoniacal liquor, is obtained precursor liquid；Oxygen in the precursor liquid
The concentration of graphite alkene is 2mg/mL；The reducing agent is oxalic acid；
Step 2: light source to be placed in the middle part of the internal spiral of reactor 6 and light source is opened, then by described in step one
Precursor liquid is placed in precursor liquid storage bottle 1, and the precursor liquid in precursor liquid storage bottle 1 is continuously pumped into reactor 6 by peristaltic pump 2,
And controlling residence time of the precursor liquid in reactor 6 to be 1h, the precursor liquid being pumped into reactor 6 issues the third contact of a total solar or lunar eclipse in illumination condition
Flowed into after catalytic reaction through discharge nozzle 7 in graphene storage bottle 9；The light source is uviol lamp, and power is 20W；
Step 3: the material filtering collected in graphene storage bottle 9 is removed into solvent, graphene is obtained, obtained stone is washed
Black alkene, graphene powder is obtained after drying.
Graphene film footpath manufactured in the present embodiment size is 0.5~3 micron, and thickness is 3nm, and graphene is 10 layers, is had
Good uniform dispersiveness.
Embodiment 8
The number of plies that the present embodiment prepares internal spiral in graphene, device using the device of embodiment 1 is 14 layers, external spiral
The number of plies of body is 16 layers, and specific preparation method comprises the following steps：
Step 1: by reducing agent and graphene oxide according to 1:1 mass ratio mixing, then by reducing agent and graphite oxide
The mixture ultrasonic disperse of alkene is dissolved in deionized water, is adjusted pH value to 10 with ammoniacal liquor, is obtained precursor liquid；Oxygen in the precursor liquid
The concentration of graphite alkene is 5mg/mL；The reducing agent is ammonium carbonate；
Step 2: light source to be placed in the middle part of the internal spiral of reactor 6 and light source is opened, then by described in step one
Precursor liquid is placed in precursor liquid storage bottle 1, and the precursor liquid in precursor liquid storage bottle 1 is continuously pumped into reactor 6 by peristaltic pump 2,
And controlling residence time of the precursor liquid in reactor 6 to be 1h, the precursor liquid being pumped into reactor 6 issues the third contact of a total solar or lunar eclipse in illumination condition
Flowed into after catalytic reaction through discharge nozzle 7 in graphene storage bottle 9；The light source is iodine-tungsten lamp, and power is 3000W；
Step 3: the material filtering collected in graphene storage bottle 9 is removed into solvent, graphene is obtained, obtained stone is washed
Black alkene, graphene powder is obtained after drying.
Graphene film footpath manufactured in the present embodiment size is 0.5~3 micron, and thickness is 2nm, and graphene is 5 layers, with good
Good uniform dispersiveness.
Embodiment 9
The number of plies that the present embodiment prepares internal spiral in graphene, device using the device of embodiment 1 is 14 layers, external spiral
The number of plies of body is 16 layers, and specific preparation method comprises the following steps：
Step 1: by reducing agent and graphene oxide according to 1:1 mass ratio mixing, then by reducing agent and graphite oxide
The mixture ultrasonic disperse of alkene is dissolved in deionized water, is adjusted pH value to 10 with ammoniacal liquor, is obtained precursor liquid；Oxygen in the precursor liquid
The concentration of graphite alkene is 5mg/mL；The reducing agent is ascorbic acid；
Step 2: light source to be placed in the middle part of the internal spiral of reactor 6 and light source is opened, then by described in step one
Precursor liquid is placed in precursor liquid storage bottle 1, and the precursor liquid in precursor liquid storage bottle 1 is continuously pumped into reactor 6 by peristaltic pump 2,
And controlling residence time of the precursor liquid in reactor 6 to be 1h, the precursor liquid being pumped into reactor 6 issues the third contact of a total solar or lunar eclipse in illumination condition
Flowed into after catalytic reaction through discharge nozzle 7 in graphene storage bottle 9；The light source is incandescent lamp, and power is 2000W；
Step 3: the material filtering collected in graphene storage bottle 9 is removed into solvent, graphene is obtained, obtained stone is washed
Black alkene, graphene powder is obtained after drying.
Graphene film footpath manufactured in the present embodiment size is 0.5~3 micron, and thickness is 1nm, and graphene is 3 layers, with good
Good uniform dispersiveness.
It is described above, only it is presently preferred embodiments of the present invention, any limitation is not done to the present invention, it is every according to invention skill
Any simple modification, change and equivalent structure change that art is substantially made to above example, still fall within the technology of the present invention
In the protection domain of scheme.
Claims (7)
1. a kind of photo catalytic reduction continuously prepares the device of graphene, it is characterised in that including reactor (6), peristaltic pump (2),
Precursor liquid storage bottle (1) and graphene storage bottle (9), the reactor (6) are transparent spiral glass tube, the one of transparent spiral glass tube
Hold as charging aperture (4), the other end is discharging opening (5), the peristaltic pump (2) be arranged at charging aperture (4) and precursor liquid storage bottle (1) it
Between, and be connected between charging aperture (4) and precursor liquid storage bottle (1) by the wriggling pump hose (3) of peristaltic pump (2), the discharging
Be connected between mouthful (5) and graphene storage bottle (9) by discharge nozzle (7), the transparent spiral glass tube by transparent glass tube from
Up to descending spiral winding to be formed after internal spiral, spiral winding is made from bottom to up further around the internal spiral, around the inside spin
The structure of body spiral winding formation from bottom to up is external spiral body, and the charging aperture (4) is located at the transparent glass for forming internal spiral
Glass tube opening end, discharging opening (5) is located at the transparent glass tube openend for forming external spiral body, and charging aperture (4) and discharging opening (5)
It is respectively positioned on the outside of the top of transparent spiral glass tube, the reactor (6) and is enclosed with reflective membrane.
2. a kind of photo catalytic reduction according to claim 1 continuously prepares the device of graphene, it is characterised in that described anti-
Peep hole is offered on light film and positioned at the middle part and bottom of reactor (6).
3. a kind of photo catalytic reduction according to claim 1 continuously prepares the device of graphene, it is characterised in that in described
The number of plies of conveyor screw is 12~14 layers, and the number of plies of external spiral body is 14~16 layers.
4. a kind of photo catalytic reduction according to claim 1 continuously prepares the device of graphene, it is characterised in that it is described go out
In expects pipe (7) and positioned at being provided with Ultraviolet Detector (8) between discharging opening (5) and graphene storage bottle (9).
5. a kind of method for preparing graphene using any claim described device in such as Claims 1-4, its feature exists
In comprising the following steps：
Step 1: by reducing agent and graphene oxide according to 1:The mass ratio mixing of (0.5~2), then by reducing agent and oxidation
The mixture ultrasonic disperse of graphene is dissolved in deionized water, is adjusted pH value to 7~10 with ammoniacal liquor, is obtained precursor liquid；Before described
The concentration for driving graphene oxide in liquid is 0.1mg/mL~10mg/mL；
Step 2: light source to be placed in the middle part of the internal spiral of reactor (6) and light source is opened, then by before described in step one
Drive liquid to be placed in precursor liquid storage bottle (1), the precursor liquid in precursor liquid storage bottle (1) is continuously pumped into by reactor by peristaltic pump (2)
(6) in, and residence time of the precursor liquid in reactor (6) is controlled to be 0.5h~1h, the precursor liquid being pumped into reactor (6) exists
Illumination condition is issued after third contact of a total solar or lunar eclipse catalytic reaction through in discharge nozzle (7) inflow graphene storage bottle (9)；The light source is iodine-tungsten lamp, in vain
Vehement lamp or uviol lamp；
Step 3: the material filtering collected in graphene storage bottle (9) or centrifugation are removed into solvent, graphene is obtained, washing is obtained
Graphene, dry after obtain graphene powder.
6. method according to claim 5, it is characterised in that reducing agent described in step one is ascorbic acid, formic acid, Portugal
Grape sugar, citric acid, oxalic acid, ammonium carbonate or ammonium hydrogen carbonate.
7. method according to claim 5, it is characterised in that the power of iodine-tungsten lamp, incandescent lamp and uviol lamp in step 2
It is 20W~3000W.
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| CN108363129A (en) * | 2018-04-20 | 2018-08-03 | 南开大学 | More structure combinatorial artificial resistance electromagnetic surfaces |
| CN110562965A (en) * | 2019-10-30 | 2019-12-13 | 武汉低维材料研究院有限公司 | Preparation method of graphene powder |
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