CN113387348B - Method for preparing graphene by using composite ionic liquid - Google Patents
Method for preparing graphene by using composite ionic liquid Download PDFInfo
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- CN113387348B CN113387348B CN202010819805.4A CN202010819805A CN113387348B CN 113387348 B CN113387348 B CN 113387348B CN 202010819805 A CN202010819805 A CN 202010819805A CN 113387348 B CN113387348 B CN 113387348B
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Abstract
The invention provides a method for preparing graphene by using composite ionic liquid, which comprises the following steps: dividing graphite powder intoDispersing in an organic solvent, and grinding for pretreatment; mixing the hydrophilic ionic liquid and the hydrophobic ionic liquid which are heated to be liquid state to obtain composite ionic liquid; removing the organic solvent from the pretreated graphite powder, and uniformly mixing the graphite powder with the composite ionic liquid; adding the mixture into a high-temperature high-pressure reaction kettle, and introducing CO2Carrying out reaction under the protection of sealing; and transferring the reactant to an ultrasonic reactor, adding 5-aminovaleric acid, and carrying out ultrasonic reaction to obtain the graphene. According to the method, the surface tension of the composite ionic liquid matched with the graphene is utilized, the composite ionic liquid is immersed into the graphite layer to realize the stripping of the graphite, the dispersion of the graphene is stabilized through the coulomb effect between negative ions and positive ions, and the grade of the stripped graphene is improved.
Description
Technical Field
The invention belongs to the technical field of chemical material preparation, and particularly relates to a method for preparing graphene by using a composite ionic liquid.
Background
Graphene (Graphene) is a polymer made of carbon atoms in sp2The two-dimensional carbon nanomaterial which is formed by the hybrid orbit and is in a honeycomb lattice has excellent optical, electrical and mechanical properties, has important application prospects in the aspects of materials science, micro-nano processing, energy, biomedicine, drug delivery and the like, and is considered to be a revolutionary material in the future. Graphene materials have now proven a variety of applications, such as energy storage in structural nanocomposites, catalyst supports, electronic devices, batteries and supercapacitors. The premise of realizing wide application of the graphene is to realize large-scale production of the graphene.
The current methods for producing graphene include mechanical exfoliation, Hummers (chemical oxidation-reduction), chemical vapor deposition, epitaxial growth, liquid phase exfoliation, and carbon nanotube shearing. Among them, the bottom-up methods such as mechanical stripping, chemical oxidation, liquid phase stripping, etc. are relatively simple. Although the mechanical stripping method can prepare micron-sized graphene, the controllability is low. The chemical oxidation-reduction method is a method for preparing graphene on a large scale at present. The method is characterized in that natural graphite is oxidized by combining a strong acid environment and a strong oxidant, and then an oxygen-containing functional group is introduced, so that the pi-pi interaction of graphene is weakened. And then, the graphite oxide layer is stripped through stirring and ultrasound to obtain monodisperse Graphene Oxide (GO), but the graphene oxide obtained by the method has more defects and the production process pollutes the environment.
In order to avoid the problems, the method for directly and physically peeling off the bulk graphite in a proper solution can maintain the intrinsic state of the graphene, reduce the surface defects of the graphene, is simple and flexible to operate, does not need expensive growth substrates, and is a better way for producing the graphene on a large scale.
Disclosure of Invention
Aiming at the problems in the prior art, the invention aims to provide a method for preparing graphene by using a composite ionic liquid, which belongs to a liquid-phase physical stripping method, is simple to operate and is easy for large-scale production.
In order to achieve the purpose, the invention adopts the following technical scheme:
in one aspect, the present invention provides a method for preparing graphene using a composite ionic liquid, the method comprising the steps of:
(1) dispersing graphite powder in an organic solvent, and carrying out grinding pretreatment;
(2) mixing the hydrophilic ionic liquid and the hydrophobic ionic liquid which are heated to be liquid state to obtain composite ionic liquid;
(3) removing the organic solvent from the pretreated graphite powder obtained in the step (1), and uniformly mixing the pretreated graphite powder with the composite ionic liquid obtained in the step (2);
(4) adding the mixture obtained in the step (3) into a high-temperature high-pressure reaction kettle, and introducing CO2Carrying out reaction under the protection of sealing;
(5) And (5) transferring the reactant obtained in the step (4) to an ultrasonic reactor, adding 5-aminovaleric acid, and carrying out ultrasonic reaction to obtain graphene.
The ionic liquid of the present invention is a salt which is liquid at or near room temperature and is composed of anions and cations. The graphene composite material has the advantages of difficult volatilization, adjustable structure, adjustable hydrophobicity and the like, shows good dissolving capacity for a plurality of inorganic and organic matters, most importantly has surface tension matched with graphene, and can achieve stable dispersion of the graphene through coulomb effect between negative ions and positive ions.
In some embodiments of the present invention, the graphite powder is flake graphite or plate-type carbon nanofibers.
In some embodiments of the present invention, the organic solvent in step (1) is any one or a combination of at least two of N-methylpyrrolidone (NMP), Dimethylformamide (DMF), ethyl acetate, ethanol or acetone.
In some embodiments of the present invention, the hydrophilic ionic liquid in step (2) is selected from any one of 1-butyl-3-methylimidazole hexafluorophosphate, 1-butyl-3-methylimidazole chloride, 1-butyl-3-methyltetrafluoroborate or a combination of at least two thereof.
In one embodiment of the present invention, the hydrophobic ionic liquid in step (2) is 1-butyl-3-methylimidazole hexafluorophosphate and 1-butyl-3-methylimidazole bistrifluoromethanesulfonylimide salt, and the volume ratio of the two is 3: 1.
in one embodiment of the present invention, the volume ratio of the hydrophilic ionic liquid and the hydrophobic ionic liquid in the step (2) is 1: 4.
in some embodiments of the present invention, the mass-to-volume ratio of the graphite powder to the liquid composite ionic liquid in step (3) is 1g:20mL to 100mL, for example, 1g:20mL, 1g:25mL, 1g:30mL, 1g:35mL, 1g:40mL, 1g:50mL, 1g:60mL, 1g:70mL, 1g:80mL, 1g:90mL, 1g:100mL, etc.
In some embodiments of the present invention, the temperature of the reaction in step (4) is 180 to 300 ℃, such as 180 ℃, 190 ℃, 200 ℃, 220 ℃, 240 ℃, 250 ℃, 270 ℃, 290 ℃ or 300 ℃.
In some embodiments of the present invention, the reaction time in step (4) is 3 to 12 hours, such as 3 hours, 4 hours, 5 hours, 7 hours, 9 hours, 10 hours or 12 hours.
In some embodiments of the invention, the 5-aminopentanoic acid added in step (5) is 0.1 to 0.5% of the mass of the pretreated graphite powder obtained in step (1), such as 0.1%, 0.15%, 0.2%, 0.25%, 0.3%, 0.35%, 0.4%, 0.45% or 0.5%.
In some embodiments of the present invention, the ultrasonic reaction in step (5) is a batch reaction, and after each vibration for 15min, the vibration is continued for 5min, and the total time is 2-5 h, such as 2h, 3h, 4h, or 5 h.
In some embodiments of the present invention, the ultrasonic reaction in step (5) is followed by centrifugation, washing and drying.
In some embodiments of the invention, the centrifugation is performed at a speed of 2000 to 7500rmp/min (e.g., 2000rmp/min, 2500rmp/min, 3000rmp/min, 3500rmp/min, 4000rmp/min, 4500rmp/min, 5000rmp/min, 5500rmp/min, 6000rmp/min, 6500rmp/min, 7000rmp/min, or 7500rmp/min) and for a period of 30 to 60min (30min, 35min, 40min, 45min, 50min, 55min, or 60 min).
In some embodiments of the invention, the washing comprises washing with an organic solvent, preferably acetone or ethanol, and distilled water.
According to the invention, based on the composite ionic liquid, a graphite powder stripping medium system is prepared by regulating and controlling the structure of the ionic liquid and the proportion of the auxiliary agent, and technological parameters such as temperature, pressure, reaction time and the like are optimized, so that the efficiency of preparing graphene by ionic liquid phase stripping is improved.
According to the method, the surface tension of the composite ionic liquid matched with the graphene is utilized, the composite ionic liquid is immersed into the graphite layer to realize the stripping of the graphite, the dispersion of the graphene is stabilized through the coulomb effect between negative ions and positive ions, and the grade of the stripped graphene is improved.
Compared with the prior art, the invention has the following beneficial effects:
the graphene preparation method provided by the invention is used for preparing graphene by taking the composite ionic liquid as a liquid-phase medium through high-temperature intercalation and ultrasonic stripping, belongs to a liquid-phase physical stripping method, is less in damage to graphene, is simple to operate, has a yield of more than 68%, and is easy for industrial production.
Drawings
FIG. 1 is a scanning electron micrograph of the graphene prepared in example 1, with a scale of 1 μm.
FIG. 2 is a scanning electron micrograph of a raw material of flake graphite of example 1, with a scale of 10 μm.
Detailed Description
The technical solution of the present invention will be further described in detail with reference to the following examples. The following examples are only for illustrating the technical solutions of the present invention more clearly, and the protection scope of the present invention is not limited thereby.
Example 1
In this embodiment, the graphene is prepared by the following method, which specifically includes the following steps:
dispersing flake graphite with the purity of more than 99.9% and the particle size of 20-500 mu m in ethyl acetate, grinding for pretreatment, and centrifuging to remove an organic solvent to obtain the pretreated flake graphite.
Mixing the components in a volume ratio of 3: 1, uniformly mixing a mixture of 1-butyl-3-methylimidazolium hexafluorophosphate and 1-butyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt with 1-butyl-3-methylimidazolium hexafluorophosphate according to a volume ratio of 4:1, and mixing the mixture in a mass-to-volume ratio of 1 g: 20mL of pretreated crystalline flake graphite is added into the composite ionic liquid and uniformly stirred.
Adding 100mL of mixture of graphite and ionic liquid into a high-temperature high-pressure reaction kettle with the capacity of 200mL, and adding CO2Sealing and protecting, and reacting for 6 hours at the temperature of 180 ℃; after the reaction is finished, 5-aminovaleric acid with the dosage of 0.1 percent of the mass of the pretreated graphite is added, and the ultrasonic treatment is carried out for 3 hours. And transferring the obtained graphene ionic liquid mixture into a centrifuge at the rotating speed of 5000rmp/min for 40 min. And (4) taking the supernatant, carrying out vacuum filtration, washing with acetone once, washing with distilled water twice, and drying to obtain the graphene product.
Example 2
In this embodiment, the graphene is prepared by the following method, which specifically includes the following steps:
dispersing flake graphite with the purity of more than 99.9% and the particle size of 20-500 mu m in ethyl acetate, grinding for pretreatment, and centrifuging to remove an organic solvent to obtain the pretreated flake graphite.
Mixing the components in a volume ratio of 3: 1 of a mixture of 1-butyl-3-methylimidazole chloride salt and 1-butyl-3-methylimidazole bistrifluoromethanesulfonimide salt and 1-butyl-3-methylimidazole hexafluorophosphate salt in a volume ratio of 4: 1, uniformly mixing. Taking the mass volume ratio of 1 g: 20mL of pretreated crystalline flake graphite is added into the composite ionic liquid and uniformly stirred.
Adding 100mL of mixture of graphite and ionic liquid into a high-temperature high-pressure reaction kettle with the capacity of 200mL, and adding CO2Sealing and protecting, and reacting for 6 hours at the temperature of 180 ℃; after the reaction is finished, 5-aminovaleric acid with the dosage of 0.1 percent of the mass of the pretreated graphite is added, and the ultrasonic treatment is carried out for 3 hours. The obtained graphene ionic liquid mixture is transferred into a centrifuge at the rotating speed of 5000rmp/min for 40 min. And (4) taking the supernatant, carrying out vacuum filtration, washing with acetone once, washing with distilled water twice, and drying to obtain the graphene product.
Example 3
In this embodiment, the graphene is prepared by the following method, which specifically includes the following steps:
dispersing flake graphite with the purity of more than 99.9% and the particle size of 20-500 mu m in ethyl acetate, grinding for pretreatment, and centrifuging to remove an organic solvent to obtain the pretreated flake graphite.
Mixing the components in a volume ratio of 3: 1 of a mixture of 1-butyl-3-methyltetrafluoroborate and 1-butyl-3-methylimidazolium bistrifluoromethylsulfonimide salt and 1-butyl-3-methylimidazolium hexafluorophosphate in a volume ratio of 4: 1, and uniformly mixing. Taking the mass volume ratio of 1 g: 20mL of pretreated crystalline flake graphite is added into the composite ionic liquid and uniformly stirred.
Adding 100mL of mixture of graphite and ionic liquid into a high-temperature high-pressure reaction kettle with the capacity of 200mL, and adding CO2Sealing and protecting, and reacting for 6 hours at the temperature of 180 ℃; after the reaction is finished, 5-aminovaleric acid with the dosage of 0.1 percent of the mass of the pretreated graphite is added, and the ultrasonic treatment is carried out for 3 hours. The obtained graphene ionic liquid mixture is transferred into a centrifuge at the rotating speed of 5000rmp/min for 40 min. And (4) taking the supernatant, carrying out vacuum filtration, washing with acetone once, washing with distilled water twice, and drying to obtain the graphene product.
Example 4
In this embodiment, the graphene is prepared by the following method, which specifically includes the following steps:
dispersing flake graphite with the purity of more than 99.9% and the particle size of 20-500 mu m in ethyl acetate, grinding for pretreatment, and centrifuging to remove an organic solvent to obtain the pretreated flake graphite.
Mixing the components in a volume ratio of 3: 1 of a mixture of 1-butyl-3-methylimidazolium hexafluorophosphate and 1-butyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt and 1-butyl-3-methylimidazolium hexafluorophosphate in a volume ratio of 4: 1, uniformly mixing. Taking the mass volume ratio of 1 g: 60mL of pretreated crystalline flake graphite is added into the composite ionic liquid and uniformly stirred.
Adding 100mL of mixture of graphite and ionic liquid into a high-temperature high-pressure reaction kettle with the capacity of 200mL, and adding CO2Sealing and protecting, and reacting for 6 hours at the temperature of 180 ℃; after the reaction is finished, 5-aminovaleric acid with the dosage of 0.1 percent of the mass of the pretreated graphite is added, and the ultrasonic treatment is carried out for 3 hours. The obtained graphene ionic liquid mixture is transferred into a centrifuge at the rotating speed of 5000rmp/min for 40 min. And (4) taking the supernatant, carrying out vacuum filtration, washing with acetone once, washing with distilled water twice, and drying to obtain the graphene product.
Example 5
In this embodiment, the graphene is prepared by the following method, which specifically includes the following steps:
dispersing flake graphite with the purity of more than 99.9% and the particle size of 20-500 mu m in ethyl acetate, grinding for pretreatment, and centrifuging to remove an organic solvent to obtain the pretreated flake graphite.
Mixing the components in a volume ratio of 3: 1 of a mixture of 1-butyl-3-methylimidazolium hexafluorophosphate and 1-butyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt and 1-butyl-3-methylimidazolium hexafluorophosphate in a volume ratio of 4: 1, and uniformly mixing. Taking the mass volume ratio of 1 g: 60mL of pretreated crystalline flake graphite is added into the composite ionic liquid and uniformly stirred.
Adding 100mL of mixture of graphite and ionic liquid into a high-temperature high-pressure reaction kettle with the capacity of 200mL, and adding CO2Sealing and protecting at 240 deg.CReacting for 6 hours under the condition of (1); after the reaction is finished, 5-aminovaleric acid with the dosage of 0.1 percent of the mass of the pretreated graphite is added, and the ultrasonic treatment is carried out for 3 hours. The resulting graphene ions
Transferring the liquid mixture into a centrifuge at 5000rmp/min for 40 min. And (4) taking the supernatant, carrying out vacuum filtration, washing with acetone once, washing with distilled water twice, and drying to obtain the graphene product.
Example 6
In this embodiment, the graphene is prepared by the following method, which specifically includes the following steps:
dispersing flake graphite with the purity of more than 99.9% and the particle size of 20-500 mu m in ethyl acetate, grinding for pretreatment, and centrifuging to remove an organic solvent to obtain the pretreated flake graphite.
Mixing the components in a volume ratio of 3: 1 of a mixture of 1-butyl-3-methylimidazolium hexafluorophosphate and 1-butyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt and 1-butyl-3-methylimidazolium hexafluorophosphate in a volume ratio of 4: 1, uniformly mixing. Taking the mass volume ratio of 1 g: 60mL of pretreated crystalline flake graphite is added into the composite ionic liquid and uniformly stirred.
Adding 100mL of the mixture of graphite and ionic liquid into a high-temperature high-pressure reaction kettle with the capacity of 200mL, and adding CO2Sealing and protecting, and reacting for 6 hours at the temperature of 240 ℃; after the reaction is finished, aminopentanoic acid with the dosage of 0.5 percent of the mass of the pretreated graphite is added, and the ultrasonic treatment is carried out for 3 hours. And transferring the obtained graphene ionic liquid mixture into a centrifuge at the rotating speed of 5000rmp/min for 40 min. And (4) taking the supernatant, carrying out vacuum filtration, washing with acetone once, washing with distilled water twice, and drying to obtain the graphene product.
Example 7
In this embodiment, the graphene is prepared by the following method, which specifically includes the following steps:
dispersing flake graphite with the purity of more than 99.9% and the particle size of 20-500 mu m in ethyl acetate, grinding for pretreatment, and centrifuging to remove an organic solvent to obtain the pretreated flake graphite.
Mixing the components in a volume ratio of 3: 1 of a mixture of 1-butyl-3-methylimidazolium hexafluorophosphate and 1-butyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt and 1-butyl-3-methylimidazolium hexafluorophosphate in a volume ratio of 4: 1, and uniformly mixing. Taking the mass volume ratio of 1 g: 60mL of pretreated crystalline flake graphite is added into the composite ionic liquid and uniformly stirred.
Adding 100mL of mixture of graphite and ionic liquid into a high-temperature high-pressure reaction kettle with the capacity of 200mL, and adding CO2Sealing and protecting, and reacting for 6 hours at the temperature of 240 ℃; after the reaction is finished, 5-aminovaleric acid with the dosage of 0.5 percent of the mass of the pretreated graphite is added, and the ultrasonic treatment is carried out for 3 hours. And transferring the obtained graphene ionic liquid mixture into a centrifuge at the rotating speed of 7000rmp/min for 40 min. And (4) taking the supernatant, carrying out vacuum filtration, washing with acetone once, washing with distilled water twice, and drying to obtain the graphene product.
Example 8
In this embodiment, the graphene is prepared by the following method, which specifically includes the following steps:
dispersing flake graphite with the purity of more than 99.9% and the particle size of 20-500 mu m in ethyl acetate, grinding for pretreatment, and centrifuging to remove an organic solvent to obtain the pretreated flake graphite.
Mixing the components in a volume ratio of 3: 1 of a mixture of 1-butyl-3-methylimidazolium hexafluorophosphate and 1-butyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt and 1-butyl-3-methylimidazolium hexafluorophosphate in a volume ratio of 4: 1, uniformly mixing. Taking the mass volume ratio of 1 g: 60mL of pretreated crystalline flake graphite is added into the composite ionic liquid and uniformly stirred.
Adding 100mL of the mixture of graphite and ionic liquid into a high-temperature high-pressure reaction kettle with the capacity of 200mL, and adding CO2Sealing and protecting, and reacting for 6 hours at the temperature of 240 ℃; after the reaction is finished, 5-aminovaleric acid with the dosage of 0.5 percent of the mass of the pretreated graphite is added, and the ultrasonic treatment is carried out for 5 hours. And transferring the obtained graphene ionic liquid mixture into a centrifuge at the rotating speed of 7000rmp/min for 40 min. And (4) taking the supernatant, carrying out vacuum filtration, washing with acetone once, washing with distilled water twice, and drying to obtain the graphene product.
Example 9
In this embodiment, the graphene is prepared by the following method, which specifically includes the following steps:
dispersing flake graphite with the purity of more than 99.9% and the particle size of 20-500 mu m in ethyl acetate, grinding for pretreatment, and centrifuging to remove an organic solvent to obtain the pretreated flake graphite.
Mixing the components in a volume ratio of 3: 1 of a mixture of 1-butyl-3-methylimidazolium hexafluorophosphate and 1-butyl-3-methylimidazolium bistrifluoromethylsulfonyl imide salt and 1-butyl-3-methylimidazolium hexafluorophosphate in a volume ratio of 4: 1, uniformly mixing. Taking the mass volume ratio of 1 g: 60mL of pretreated crystalline flake graphite is added into the composite ionic liquid and uniformly stirred.
Adding 100mL of the mixture of graphite and ionic liquid into a high-temperature high-pressure reaction kettle with the capacity of 200mL, and adding CO2Sealing and protecting, and reacting for 6 hours at the temperature of 240 ℃; after the reaction is finished, 5-aminovaleric acid with the dosage of 0.5 percent of the mass of the pretreated graphite is added, and the ultrasonic treatment is carried out for 5 hours. And transferring the obtained graphene ionic liquid mixture into a centrifuge at the rotating speed of 7000rmp/min for 60 min. And (4) taking the supernatant, carrying out vacuum filtration, washing with acetone once, washing with distilled water twice, and drying to obtain the graphene product.
Scanning electron microscope (SU8020, hitachi, japan) characterization of the graphene product and the scale graphite raw material prepared in example 1, with the results shown in fig. 1 and fig. 2, respectively, shows that the scale graphite is effectively exfoliated by the composite ionic liquid, and graphene with a diameter of about 10 μm is obtained. The graphene products of examples 2-9 were also characterized by scanning electron microscopy, and the same conclusions were obtained.
The yields of the graphene products of examples 1-9 are given in table 1.
TABLE 1
As can be seen from Table 1, the method of the present invention enables the graphene yield to be as high as 68% or more.
Finally, it should be noted that: the above embodiments are merely illustrative and not restrictive of the technical solutions of the present invention, and any equivalent substitutions and modifications or partial substitutions made without departing from the spirit and scope of the present invention should be included in the scope of the claims of the present invention.
Claims (15)
1. A method for preparing graphene by using a composite ionic liquid is characterized by comprising the following steps:
(1) dispersing graphite powder in an organic solvent, and carrying out grinding pretreatment;
(2) mixing the hydrophilic ionic liquid and the hydrophobic ionic liquid which are heated to be liquid state to obtain composite ionic liquid;
(3) removing the organic solvent from the pretreated graphite powder obtained in the step (1), and uniformly mixing the pretreated graphite powder with the composite ionic liquid obtained in the step (2);
(4) adding the mixture obtained in the step (3) into a high-temperature high-pressure reaction kettle, and introducing CO2Carrying out reaction under the protection of sealing;
(5) and (5) transferring the reactant obtained in the step (4) to an ultrasonic reactor, adding 5-aminovaleric acid, and carrying out ultrasonic reaction to obtain graphene.
2. The method of claim 1, wherein the graphite powder is flake graphite or plate-type carbon nanofibers.
3. The method according to claim 1, wherein the organic solvent in step (1) is any one or a combination of at least two of N-methylpyrrolidone, dimethylformamide, ethyl acetate, ethanol or acetone.
4. The method according to claim 1, wherein the hydrophilic ionic liquid in step (2) is selected from any one of or a combination of at least two of 1-butyl-3-methylimidazole hexafluorophosphate, 1-butyl-3-methylimidazole chloride and 1-butyl-3-methyltetrafluoroborate.
5. The method according to claim 1, wherein the hydrophobic ionic liquid in step (2) is 1-butyl-3-methylimidazole hexafluorophosphate and 1-butyl-3-methylimidazole bistrifluoromethylsulfonyl imide salt in a volume ratio of 3: 1.
6. The method according to claim 1, wherein the volume ratio of the hydrophilic ionic liquid to the hydrophobic ionic liquid in step (2) is 1: 4.
7. The method according to claim 1, wherein the mass-to-volume ratio of the graphite powder to the liquid composite ionic liquid in the step (3) is 1g:20 mL-100 mL.
8. The method according to claim 1, wherein the temperature of the reaction in the step (4) is 180 to 300 ℃.
9. The method according to claim 1, wherein the reaction time in the step (4) is 3 to 12 hours.
10. The method according to claim 1, wherein the 5-aminopentanoic acid added in the step (5) accounts for 0.1-0.5% of the mass of the pretreated graphite powder obtained in the step (1).
11. The method according to claim 1, wherein the ultrasonic reaction in the step (5) is a batch reaction, and after 15min of vibration each time, the vibration is continued for 5min, and the total time is 2-5 h.
12. The method according to claim 1, wherein the ultrasonic reaction in step (5) is followed by centrifugation, washing and drying.
13. The method of claim 12, wherein the centrifugation is performed at a speed of 2000 to 7500rmp/min for 30 to 60 min.
14. The method of claim 12, wherein the washing comprises an organic solvent and distilled water washing.
15. The method of claim 14, wherein the organic solvent is acetone or ethanol.
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| CN102712779A (en) * | 2009-12-22 | 2012-10-03 | 徐光锡 | Graphene dispersion and graphene-ionic liquid polymer compound material |
| CN102730676A (en) * | 2012-07-18 | 2012-10-17 | 中国水产科学研究院黄海水产研究所 | Method for preparing graphene |
| KR20160150425A (en) * | 2015-06-22 | 2016-12-30 | 영남대학교 산학협력단 | Preparation method for the ultra thin cobalt oxide nanotubes-intercalated graphene composite |
| CN108383114A (en) * | 2018-04-18 | 2018-08-10 | 东华大学 | The method of conjugate ion liquid up-stripping preparing graphite alkene |
| CN110950331A (en) * | 2019-12-02 | 2020-04-03 | 陕西科技大学 | Method for preparing fluorinated graphene dispersion liquid on large scale |
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|---|---|---|---|---|
| CN102712779A (en) * | 2009-12-22 | 2012-10-03 | 徐光锡 | Graphene dispersion and graphene-ionic liquid polymer compound material |
| CN102730676A (en) * | 2012-07-18 | 2012-10-17 | 中国水产科学研究院黄海水产研究所 | Method for preparing graphene |
| KR20160150425A (en) * | 2015-06-22 | 2016-12-30 | 영남대학교 산학협력단 | Preparation method for the ultra thin cobalt oxide nanotubes-intercalated graphene composite |
| CN108383114A (en) * | 2018-04-18 | 2018-08-10 | 东华大学 | The method of conjugate ion liquid up-stripping preparing graphite alkene |
| CN110950331A (en) * | 2019-12-02 | 2020-04-03 | 陕西科技大学 | Method for preparing fluorinated graphene dispersion liquid on large scale |
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