CN108101033A - A kind of method that graphene is prepared as electrolyte electrochemical cathodic disbonding graphite using DTAB - Google Patents
A kind of method that graphene is prepared as electrolyte electrochemical cathodic disbonding graphite using DTAB Download PDFInfo
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- CN108101033A CN108101033A CN201810032036.6A CN201810032036A CN108101033A CN 108101033 A CN108101033 A CN 108101033A CN 201810032036 A CN201810032036 A CN 201810032036A CN 108101033 A CN108101033 A CN 108101033A
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- graphene
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- C01—INORGANIC CHEMISTRY
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- C01B2204/00—Structure or properties of graphene
- C01B2204/20—Graphene characterized by its properties
- C01B2204/32—Size or surface area
Abstract
The invention discloses a kind of method for preparing graphene as electrolyte electrochemical cathodic disbonding graphite using DTAB, it is characterized in that, include the following steps：1）Stock；2）Prepare electric stripper；3）The electric stripping off device of assembling；4）Electricity is removed；5）Filtering, washing；6）Ultrasonic disperse；7）The aqueous solution for being freeze-dried obtained graphene is freeze-dried into graphene powder.The advantages of this method is to prepare that raw material is simple and easy to get, operation is easy, at low cost, technical process is simple, step is few, with short production cycle, and the small number of plies of graphene degree of imperfection of preparation is few, is extremely suitable for industrial production.
Description
Technical field
The present invention relates to graphene technologies, and specifically one kind is using DTAB as electrolyte electrochemical cathodic disbonding graphite
The method for preparing graphene.
Background technology
Graphene be only there are one carbon atom thickness two-dimensional material, be one kind by carbon atom with sp2Hybridized orbit forms
Hexangle type is in the flat film of honeycomb lattice, is a kind of individual layer sheet new material being made of carbon atom.Graphene is both most thin
Material and most tough material, 200 times more taller than best steel of fracture strength, while it has good bullet again
Property, stretch range can reach the 20% of own dimensions, it is that current nature is most thin, the highest material of intensity.With uniqueness
Carrier properties, electron mobility prestige 2 × 105cm2140 times of electron mobility in/V.S, about silicon, 20 times of GaAs,
Temperature stability is high, and electrical conductivity is up to 108Ω/m, surface resistance are about 31 Ω/m2, it is lower than copper and Yin Geng, it is conductive at room temperature
Best material.Specific surface area (2630m2/ g), thermal conductivity (5000W/m.K at room temperature) is 36 times of silicon, 20 times of GaAs,
It is copper (401W.m.K) more than ten times.Therefore it is widely applied to physics, materialogy, electronic information, computer, aviation boat
The fields such as it.
A kind of graphene novel nano-material most strong as presently found most thin, maximum intensity, electrical and thermal conductivity performance,
It is referred to as " dark fund ", is " king of new material ", scientist even foretell graphene will " thoroughly change 21 century, it is most likely that
Start a subversiveness new technology new industrial revolution have swept the globe.
At present, the main method for preparing graphene has；
(1) Hummers methods prepare graphene：The key step of the method is divided into：The synthesis of one, graphene oxides；Two, are reduced
Graphene oxide.Hummers methods are to utilize strong acid (dense H first2SO4) and with strong oxidizing property metal salt (KMnO4) certain
Under conditions of natural flake graphite is prepared into graphene oxide, then graphene oxide quilt under the action of strong reductant (hydrazine)
It reduces and generates graphene.It is this in practical operation although preparing graphene using Hummers methods to be widely used
The step of method, is more, more to the influence factor of building-up process, caused by graphene yield it is relatively low, and synthesize graphene
Degree of imperfection is larger, of low quality；
(2) chemical vapor deposition (CVD) method：The method at high temperature splits carbon source using carbon compounds such as methane as carbon source
Solution generation carbon atom is simultaneously penetrated into metallic matrix, and after reducing temperature, carbon atom can be precipitated out of metallic matrix, and then generate stone
Black alkene, however, chemical vapor deposition (CVD) method is of high cost, process is complicated, limit to a certain extent three-dimensional grapheme into
One step develops, and the specific porous metal material of chemical vapor deposition (CVD) method needs, as substrate, this can greatly increase it
Cost；
(3) template：The method, by electrostatic interaction or intermolecular force, forms cladding using graphene oxide as raw material
Graphene oxide is reduced into after graphene and removes template and can prepare graphene by the graphene oxide of template, maximum excellent of the method
Gesture is that aperture can regulate and control, you can to prepare the graphene of different pore size by changing template, but the method preparation procedure is more, mistake
Journey is complicated, and time-consuming；
These above-mentioned methods are there are a series of shortcoming, such as：Prepare graphene degree of imperfection is high, preparation process is complicated,
It is of high cost, time-consuming, not easy to operate etc..
So far, the preparation of graphene is also in the elementary step, since graphene has larger specific surface area and leads
Electrically preferably, therefore graphene will be widely used in the electrode material of energy storage device.
The content of the invention
The purpose of the present invention is in view of the deficiencies of the prior art, and provide a kind of electrochemical cathode using DTAB as electrolyte
Remove the method that graphite prepares graphene.The advantages of this method be prepare raw material it is simple and easy to get, operation easily, cost
It is low, technical process is simple, step is few, the with short production cycle, structure of product produced and electrochemical performance, is particularly suitable for
In industrial production.
Realizing the technical solution of the object of the invention is：
A kind of method that graphene is prepared as electrolyte electrochemical cathodic disbonding graphite using DTAB, including walking as follows
Suddenly：
1) stock up：Graphite electrode, absolute ethyl alcohol, DTAB, D.C. regulated power supply, iron stand and conductive clamp are ready to standby
With；
2) electric stripper is prepared：The ready absolute ethyl alcohol of step 1), DTAB are weighed, is configured to 0.1mol/L DTAB electricity
Chemical stripping graphene electricity stripper；
3) electric stripping off device is assembled：Using graphite electrode as cathode and anode, by two electrodes are vertical and parallel immersion
Into electric stripper, there is spacing distance between two electrodes, two electrodes are connected with D.C. regulated power supply；
4) electricity is removed：The voltage that powers on is arranged to 15V electrochemical strippings 120 minutes；
5) filter, wash：Graphene forerunner's body detergent filtration washing in electric stripper after step 4) is removed
Obtain substance A；
6) ultrasonic disperse：Substance A ultrasonic disperse after step 5) is washed, obtains the aqueous solution of graphene, ultrasonic disperse
Effect be by the graphene after washing spread out again and be generation graphene size than more uniform；
7) it is freeze-dried：The aqueous solution freeze-drying for the graphene that step 6) is obtained is freeze-dried into graphene powder
Effect be that the deionized water in graphene aqueous solution is made to be dried and removed that the reunion of graphene is prevented to be conducive to graphene
Generation.
DTAB described in step 1) is dodecyl trimethyl ammonium bromide.
Electric stripper solute is DTAB in step 2), and solvent is absolute ethyl alcohol.
Graphite electrode described in step 3) be graphite, graphite be " crystal " graphite, " crystal " graphite crystallization structure
It makes, degree of graphitization is high.
The distance between two graphite electrodes described in step 3) are 4cm.
In step 4) when the voltage between two graphite electrodes be 15V when DTAB generate C in the electrolytic solution15H34N+Ion moves
Move cathode graphite electrode, and C15H34N+Graphite can be inserted between layers.Applied voltage underthrust enter to graphite linings it
Between C15H34N+Reduction reaction generation CH occurs for ion4、H2、N2、NH3Gases are waited, the gas subsequently generated struts graphite linings,
Then graphene is generated.
Detergent described in step 5) is deionized water and the mixed solution of absolute ethyl alcohol, and effect is to wash away to be blended in stone
Impurity in black alkene, such as：CH3CH2OH、DTAB、Br-、C15H34N+。
The technical program compared with existing method prepare graphene preparation method have the advantages that it is following a series of：
1. graphene is prepared with operation is easy, raw material is simple and easy to get, at low cost, technique mistake according to the technical program method
The characteristics of journey is simple, step is few, structure with short production cycle, product is excellent, environmentally friendly, is extremely suitable for industrial production.
2. using the graphene that electrochemical stripping graphite is produced can be widely applied to the energy, environment, sensing and
The numerous areas such as biochemical industry, with important scientific value and widely application prospect.
The advantages of this method be prepare raw material is simple and easy to get, operation is easy, at low cost, technical process is simple, step is few,
With short production cycle, the small number of plies of graphene degree of imperfection of preparation is few, environmentally friendly, is extremely suitable for industrial production.
Description of the drawings
Fig. 1 is the SEM figures of the graphene obtained in implementation column；
Fig. 2 is the TEM figures of graphene in implementation column；
Fig. 3 is the Raman figures of graphene in implementation column；
Fig. 4 is the XPS figures of graphene in implementation column；
Fig. 5 is the isothermal adsorption desorption graph of graphene in implementation column.
Specific embodiment
Present invention is described further with reference to the accompanying drawings and examples, but is not limitation of the invention.
Embodiment：
A kind of method that graphene is prepared as electrolyte electrochemical cathodic disbonding graphite using DTAB, including walking as follows
Suddenly：
1) stock up：Graphite electrode, absolute ethyl alcohol, DTAB, D.C. regulated power supply, iron stand and conductive clamp are ready to standby
With；
2) electric stripper is prepared：The ready absolute ethyl alcohol of step 1) is weighed, DTAB, is configured to 0.1mol/L DTAB electricity
Chemical stripping graphene electricity stripper；
3) electric stripping off device is assembled：Using graphite electrode as cathode and anode, by two electrodes are vertical and parallel immersion
Into electric stripper, there is spacing distance between two electrodes, two electrodes are connected with D.C. regulated power supply；
4) electricity is removed：The voltage that powers on is arranged to 15V electrochemical strippings 120 minutes；
5) filter, wash：Graphene forerunner's body detergent filtration washing in electric stripper after step 4) is removed
Obtain substance A；
6) ultrasonic disperse：Substance A ultrasonic disperse after step 5) is washed, obtains the aqueous solution of graphene, ultrasonic disperse
Effect be by the graphene after washing spread out again and be generation graphene size than more uniform；
7) it is freeze-dried：The aqueous solution freeze-drying for the graphene that step 6) is obtained is freeze-dried into graphene powder
Effect be that the deionized water in graphene aqueous solution is made to be dried and removed that the reunion of graphene is prevented to be conducive to graphene
Generation.
DTAB described in step 1) is dodecyl trimethyl ammonium bromide.
Electric stripper solute is DTAB in step 2), and solvent is absolute ethyl alcohol.
Graphite electrode described in step 3) be graphite, graphite be " crystal " graphite, " crystal " graphite crystallization structure
It makes, degree of graphitization is high.
The distance between two graphite electrodes are 4cm.
In step 4) when the voltage between two graphite electrodes be 15V when DTAB generate C in the electrolytic solution15H34N+Ion moves
Move cathode graphite electrode, and C15H34N+Graphite can be inserted between layers.Applied voltage underthrust enter to graphite linings it
Between C15H34N+Reduction reaction generation CH occurs for ion4、H2、N2、NH3Gases are waited, the gas subsequently generated struts graphite linings,
Then graphene is generated.
Detergent described in step 5) is deionized water and the mixed solution of absolute ethyl alcohol, and effect is to wash away to be blended in stone
Impurity in black alkene, such as：CH3CH2OH、DTAB、Br-、C15H34N+。
Specifically：
1) stock up：It is accurate to weigh 9.2502gDTAB, 300ml absolute ethyl alcohol, graphite, iron stand, directly
Flow regulated power supply：
2) electrolyte quota：9.2502gDTAB in step 1) is dissolved into 300ml absolute ethyl alcohols, is configured to
0.1mol/LDTAB electrochemical stripping liquid；
3) electric stripping off device assembling：Using graphite electrode as negative and positive the two poles of the earth, they are fixed on iron using the clip with copper wire
On pallet, and by they it is vertical and it is parallel be immersed in electric stripper, spacing is 4cm between two electrodes, by two electrodes with leading
Line is connected on the positive and negative anodes of DC power supply respectively；
4) electricity is removed：The voltage that powers on is arranged to 15V electrochemical strippings 120 minutes；
5) filter, wash：Graphene presoma deionized water in electric stripper and anhydrous second after step 4) is removed
Alcohol repeatedly washs the foreign ion CH removed on graphene3CH2OH, DTAB, Br-、C15H34N+；
6) ultrasonic disperse：Graphene after step 5) repeatedly washing is added to ultrasonic disperse 100 in deionized water to divide
Clock；
7) it is freeze-dried：With liquid nitrogen then the aqueous solution of the graphene after step 6) ultrasonic disperse is frozen into blocks of solid
Into graphene powder after freeze-drying 36H.
As shown in Figure 1, it is understood by SEM image in Fig. 1 using DTAB as electrolyte electrochemical cathodic disbonding graphite system
It is standby go out graphene sheet layer it is larger and pattern is preferable；
As shown in Fig. 2, understanding that graphene crystallinity is preferable by TEM in Fig. 2 and selective electron diffraction figure, the number of plies is less, and
Graphene has relatively thin lamellar structure；
As shown in figure 3, understand that the ratio between D peaks and G peaks are 0.51 (I by Fig. 3 Ramans curveD/IG=0.51), Gu graphene
Degree of imperfection is relatively low, and the quality of gained graphene is preferable；
As shown in figure 4, understanding that graphene oxygen content is 0.41wt% by Fig. 4 XPS figures, and-OH is contained only in graphene and is taken
Dai Ji, admittedly the impurity content of the graphene generated is seldom and purity is very high；
As shown in figure 5, it is understood by Fig. 5 adsorption desorption isothermal curves and combines BET formulaWhen V-balance pressure is P, the total volume of adsorbed gas, Vm-catalysis
The volume of required gas when agent surface covering first layer is full, pressure when P-adsorbate balances under adsorption temp, Ps-
Saturated vapour pressure, C-with by the related constant of absorption) the specific surface area greatly 583m of graphene can be extrapolated2/ g, Gu with
DTAB is that the graphene that electrolyte electrochemical cathodic disbonding graphite is prepared has larger specific surface area.
Claims (6)
1. a kind of method that graphene is prepared as electrolyte electrochemical cathodic disbonding graphite using DTAB, it is characterized in that, bag
Include following steps：
1）Stock：Graphite electrode, absolute ethyl alcohol, DTAB, D.C. regulated power supply, iron stand and conductive clamp are ready to spare；
2）Prepare electric stripper：Weigh step 1）Absolute ethyl alcohol, the DTAB prepared is configured to the stripping of 0.1mol/LDTAB electrochemistry
From graphene electricity stripper；
3）The electric stripping off device of assembling：It is using graphite electrode as cathode and anode, two electrodes are vertical and parallel be immersed in electricity
In stripper, there is spacing distance between two electrodes, two electrodes are connected with D.C. regulated power supply；
4）Electricity is removed：The voltage that powers on is arranged to 15V electrochemical strippings 120 minutes；
5）Filtering, washing：By step 4）Graphene forerunner's body detergent filtration washing in electric stripper after stripping obtains
Substance A；
6）Ultrasonic disperse：By step 5）Substance A ultrasonic disperse after washing, obtains the aqueous solution of graphene；
7）Freeze-drying：By step 6）The aqueous solution of obtained graphene is freeze-dried into graphene powder.
2. the side according to claim 1 that graphene is prepared using DTAB as electrolyte electrochemical cathodic disbonding graphite
Method, it is characterised in that：Step 1）Described in DTAB be dodecyl trimethyl ammonium bromide.
3. the side according to claim 1 that graphene is prepared using DTAB as electrolyte electrochemical cathodic disbonding graphite
Method, it is characterised in that：Step 2）Middle electricity stripper solute is DTAB, and solvent is absolute ethyl alcohol.
4. the side according to claim 1 that graphene is prepared using DTAB as electrolyte electrochemical cathodic disbonding graphite
Method, it is characterised in that：Step 3）Described in graphite electrode be graphite, graphite be " crystal " graphite.
5. the side according to claim 1 that graphene is prepared using DTAB as electrolyte electrochemical cathodic disbonding graphite
Method, it is characterised in that：Step 3）Described in the distance between two graphite electrodes be 4cm.
6. the side according to claim 1 that graphene is prepared using DTAB as electrolyte electrochemical cathodic disbonding graphite
Method, it is characterised in that：Step 5）Described in detergent for deionized water and absolute ethyl alcohol mixed solution.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112047330A (en) * | 2020-09-23 | 2020-12-08 | 广西师范大学 | Synchronous stripping and collecting method for producing graphene by electrochemical method |
| CN114604864A (en) * | 2022-04-11 | 2022-06-10 | 东北大学 | Method for preparing graphene by stripping graphite material by virtue of confined electrochemical method |
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| CN102807213A (en) * | 2012-08-30 | 2012-12-05 | 中国科学院苏州纳米技术与纳米仿生研究所 | Method for electrochemically preparing graphene |
| CN102923697A (en) * | 2012-11-19 | 2013-02-13 | 中南大学 | Method for preparing graphene energy storing material through electrochemical cathodic disbonding |
| CN104264179A (en) * | 2014-09-17 | 2015-01-07 | 中国科学院山西煤炭化学研究所 | Method for preparing graphene from raw graphite ores through electrolysis |
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2018
- 2018-01-12 CN CN201810032036.6A patent/CN108101033A/en active Pending
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102807213A (en) * | 2012-08-30 | 2012-12-05 | 中国科学院苏州纳米技术与纳米仿生研究所 | Method for electrochemically preparing graphene |
| CN102923697A (en) * | 2012-11-19 | 2013-02-13 | 中南大学 | Method for preparing graphene energy storing material through electrochemical cathodic disbonding |
| CN104264179A (en) * | 2014-09-17 | 2015-01-07 | 中国科学院山西煤炭化学研究所 | Method for preparing graphene from raw graphite ores through electrolysis |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112047330A (en) * | 2020-09-23 | 2020-12-08 | 广西师范大学 | Synchronous stripping and collecting method for producing graphene by electrochemical method |
| CN114604864A (en) * | 2022-04-11 | 2022-06-10 | 东北大学 | Method for preparing graphene by stripping graphite material by virtue of confined electrochemical method |
| CN114604864B (en) * | 2022-04-11 | 2023-08-22 | 东北大学 | Method for preparing graphene by stripping graphite material through limited-area electrochemical method |
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