CN102431999B - Method for preparing high-quality graphene - Google Patents
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- CN102431999B CN102431999B CN201110282370.5A CN201110282370A CN102431999B CN 102431999 B CN102431999 B CN 102431999B CN 201110282370 A CN201110282370 A CN 201110282370A CN 102431999 B CN102431999 B CN 102431999B
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Abstract
The invention relates to the field of graphene, and specifically relates to a method for preparing high-quality graphene. According to the invention, a graphite intercalation compound with a halogen or a metal halide as an intercalating agent is adopted as a raw material; expansion is carried our by using an oxalic acid solution or a hydrogen peroxide solution; and the material is subject to ultrasonic exfoliation in a solvent, such that the high-quality graphene is prepared. The method comprises specific steps that: after the graphite intercalation process, graphite intercalation compound powder is added into an oxalic acid solution or a hydrogen peroxide solution; expansion is carried out, such that highly expanded worm-shaped graphene aggregates are obtained; the worm-shaped graphene aggregates are subject to an ultrasonic oscillation in organic solvents such as alcohol and ketone, or an aqueous solution of a surfactant, such that exfoliation is realized, and a graphene dispersion liquid is obtained; the graphene dispersion liquid is dried, the solvent is removed, such that high-quality graphene powder can be obtained. The method provided by the invention is simple and is easy to control. With the method, high-efficiency, high-yield and low-cost productions of high-quality graphene can be realized; problems in current graphene preparation technologies of high cost, low yield, and poor quality can be solved.
Description
Technical field
The present invention relates to Graphene field, be specially a kind of graphite intercalation compound take halogen or metal halide as intercalator as raw material, in oxalic acid or superoxol, expand and solvent in ultrasonic peel off to combine prepare the method for high-quality graphene.
Background technology
Since 2004 are found, Graphene receives much concern as a kind of new carbon.It is that a kind of thickness being made up of the carbon atom of sp2 hydridization is completely only the accurate two dimensional crystal material of monoatomic layer or several monoatomic layers, there is the performance that high light transmittance and electroconductibility, high-specific surface area, high strength and snappiness etc. are excellent, be expected to obtain widespread use in fields such as high-performance nanometer electronic device, photoelectric device, gas sensor, matrix material, field emmision material and stored energies.But low cost, a large amount of preparation of high-quality graphene are still faced adverse conditions, and have restricted development and the application of this material.
At present, the preparation of a large amount of Graphenes is mainly, based on Hummer method, graphite is carried out to oxide treatment, obtains after graphite oxide, then it is peeled off and obtains graphene oxide, obtains Graphene finally by crossing reduction processing.Because oxidising process is understood the structure of havoc graphene sheet layer conventionally, although process through reduction, still there is larger gap with high-quality Graphene in the property indices of gained grapheme material.In addition, the oxidising process of graphite needs a large amount of strongly-acid oxygenants as the vitriol oil, concentrated nitric acid, dichromic acid and potassium permanganate, SODIUMNITRATE etc. conventionally; And in order reduction process, need pyroprocessing or use the toxic chemical substances such as hydrazine, dimethylhydrazine, not only energy consumption is large, efficiency is low, cost is high but also contaminate environment.Therefore, in the urgent need to develop a kind of can be in a large number, low cost and the eco-friendly novel method of preparing high-quality graphene.
Summary of the invention
The preparation method who the object of the present invention is to provide a kind of a large amount of, low cost, high-quality graphene, solves the problems such as the cost existing in prior art is high, productive rate is low, of poor quality.
Technical scheme of the present invention is:
Prepare a method for high-quality graphene, the graphite intercalation compound take halogen or metal halide as intercalator is as raw material, in oxalic acid or superoxol, expand and solvent in ultrasonic peel off to combine prepare high-quality graphene.First graphite intercalation compound powder is joined in the oxalic acid or superoxol of concentration (massfraction) more than 15wt%, then under the condition of 0～100 ℃, process and carry out expansion process in 0.5～24 hour, obtain the quasiflake graphite alkene aggregate of high level expansion.And then, by gained quasiflake graphite alkene aggregate after expansion process in the aqueous solution or organic solvent solution of organic solvent or various tensio-active agents, ultrasonic oscillation is processed 1 minute～5 hours, and realization is peeled off, and Graphene is dispersed in and in solvent, forms graphene solution.Utilize the dry or cryodesiccated method of spraying to remove after organic solvent or various tensio-active agent, can obtain high-quality graphene powder.
Take halogen or metal halide, in the graphite intercalation compound of intercalator, intercalator is bromine, iodine chloride, iodine bromide IBr, aluminum chloride, nickelous chloride, antimony chloride, iron(ic) chloride or antimonic fluoride etc.
In gained graphene powder, the number of plies of graphene film below 10 layers, lateral dimension more than 1 micron, and crystallographic property is good, carbon-to-oxygen ratio is more than 20.Preferable range is: 3～8 layers of the numbers of plies of graphene film, 5～50 microns of lateral dimensions, carbon-to-oxygen ratio 30～120.
In the present invention, in oxalic acid or superoxol, the massfraction of oxalic acid or hydrogen peroxide is preferably 40～80wt%, and all the other are water.
In the time carrying out expansion process, the preferred time is 2～5 hours, and preferred temperature range is 10～40 ℃.
In the present invention, every 1 liter of oxalic acid or superoxol can be processed 1～500 gram of graphite intercalation compound, and preferred treatment capacity is 15～20 grams.
In the present invention, to gained quasiflake graphite alkene aggregate ultrasonic oscillation treatment time in the aqueous solution of organic solvent or various tensio-active agents after expansion process be preferably 30 minutes～1 hour.Wherein, organic solvent can be alcohols, ketone, aldehydes, organic acid, N-Methyl pyrrolidone, dimethyl formamide, N,N-DIMETHYLACETAMIDE, chlorobenzene or dichlorobenzene etc., tensio-active agent can be sodium lauryl sulphate, Sodium dodecylbenzene sulfonate or cetyl trimethylammonium bromide etc., and the strength of solution of tensio-active agent is 0.1-5wt%.
In the present invention, the graphite intercalation compound take halogen or metal halide as intercalator is as raw material, and this intercalation technique refers to document Intercalation compounds of graphite.Dresselhaus, M.S.; Dresselhaus, G., Advances in Physics 1981,30,1-186.
Advantage of the present invention:
1, in the present invention, the technique of graphite intercalation compound is comparatively ripe, the graphite intercalation compound take halogen or metal halide as intercalator can be in normal atmospheric environment long-time stable existence, sufficient raw material can be provided.
2, the expansion process in the present invention is liquid-phase chemical reaction, and the degrees of expansion of graphite and homogeneity are all very high, can guarantee high yield and homogeneity.
3, the present invention is less than 12 hours at the 1 needed time of batch products of producing; Single batch of Graphene product with respect to the productive rate of raw material graphite (not comprising intercalator quality) higher than 70%.
4, the present invention's stripping process that expands destroys the structure of Graphene hardly, can farthest retain structure and electricity and the mechanical property of Graphene.
5, the intercalator that the present invention is present in graphite layers can spontaneously be removed in expansion process, therefore can guarantee to obtain highly purified Graphene product.
6, whole reaction process is very little on the impact of environment, and the processing cost of waste liquid is low.
Accompanying drawing explanation
Fig. 1 be graphite intercalation compound intercalation and expand after image.In figure, (a) the not original section before intercalation of natural flake graphite, (b) cross section of graphite intercalation compound, (c) graphite intercalation compound is reacted to the quasiflake graphite alkene aggregate generating with 30wt% oxalic acid solution, (d) the local enlarged photograph of quasiflake graphite alkene aggregate, it is inflated the Graphene of peeling off slabbing as seen.
Fig. 2 expands-peels off-macro morphology (optical photograph, the about 0.1g of sample total mass) of Graphene after being dried.
Fig. 3 expands-peels off-microscopic appearance of Graphene after being dried.
Fig. 4 is x-ray photoelectron spectroscopy (XPS) spectrogram (2 points) of Graphene after (a)-(c) expand-peel off-dry.Fig. 4 (a) composes entirely for XPS; Fig. 4 (b) is the meticulous spectrum of C 1s peak position; The meticulous spectrum of Fig. 4 (c) Cl 2p peak position; Fig. 4 (d) is the degree of each element in the Graphene sample calculating according to XPS spectrum.
Embodiment
As shown in Fig. 1 a-b, the model ylid bloom action power of the graphite raw material interlayer of process intercalation processing is weakened, and interlamellar spacing is expanded effectively.
Due to structural integrity, gained Graphene still keeps very strong hydrophobicity, therefore, in the oxalic acid or superoxol take water as primary solvent, presents the vermiform state of aggregation as shown in Fig. 1 c and d, and we are referred to as quasiflake graphite alkene aggregate.This quasiflake graphite alkene aggregate can be in the organic solvent of low surface tension or added in the aqueous solution of tensio-active agent be aided with the short period of time, Graphene is peeled off in lower powered ultrasonic concussion completely, obtains graphene dispersing solution.After utilizing conventional lyophilize or the dry removal of spraying solvent, can obtain fluffy graphene powder as shown in Figures 2 and 3.X-ray photoelectron spectroscopy (XPS, characterization result Fig. 4) shows that chlorine atomic percent remaining in powder is about 0.1%, carbon-to-oxygen ratio is greater than 90, can't detect residual metal ion and has existed, and shows that it has good crystallinity, extremely low oxygen level and higher purity.
In Fig. 4 (d), the atomic percent of Cl, C and O following (table 1):
Table 1: the atomic percent of Cl, C and O in gained Graphene sample
| Cl2p | C1s | O1s |
| Atomic percent (%) | Atomic percent (%) | Atomic percent (%) |
| 0.0993329 | 98.7434 | 1.1573 |
| 0.0980622 | 98.6365 | 1.26543 |
Embodiment 1:
Graphite intercalation compound by 1g take bromine as intercalator is (in graphite intercalation compound, the consumption of bromine is 0.6g) join in the oxalic acid solution that 100mL concentration is 60wt%, controlling solution temperature is 30 ℃, slowly stir 4 hours, obtain swimming in the adequately expanded quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 1L N-Methyl pyrrolidone solution, utilize the ultrasonic oscillation that power density is 0.5W/mL within 30 minutes, to obtain graphene dispersing solution.
After utilizing spray-drying process to remove N-crassitude, obtain pulverous Graphene, the mass yield of not calculating bromine intercalator in raw material is about 72%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 2:
Graphite intercalation compound by 10g take iodine chloride as intercalator is (in graphite intercalation compound, the consumption of iodine chloride is 6.5g) join in the superoxol that 500mL concentration is 50wt%, controlling solution temperature is 30 ℃, slowly stir 2.5 hours, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 2L dimethyl formamide (DMF), utilize the ultrasonic oscillation that power density is 0.5W/mL within 2 hours, to obtain graphene dispersing solution.
After utilizing spray-drying process to remove dimethyl formamide (DMF), obtain pulverous Graphene product, quality is about 3g, and the mass yield of not calculating iodine chloride intercalator in raw material is about 75%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 3:
Graphite intercalation compound by 15g take iodine bromide IBr as intercalator is (in graphite intercalation compound, the consumption of iodine bromide IBr is 10g) join in the oxalic acid solution that 500mL concentration is 60wt%, controlling solution temperature is 30 ℃, slowly stir 2 hours, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 2L dichlorobenzene (DCB), utilize power density within 30 minutes, to obtain graphene dispersing solution for 1W/mL ultrasonic oscillation.
After utilizing spray-drying process to remove DCB, obtain pulverous Graphene product, quality is about 5g, and the mass yield of not calculating iodine bromide IBr intercalator in raw material is about 78%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 4:
Graphite intercalation compound by 50g take aluminum chloride as intercalator is (in graphite intercalation compound, the consumption of aluminum chloride is 30g) join in the superoxol that 1L concentration is 70wt%, controlling solution temperature is 50 ℃, slowly stir 1.5 hours, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 5L ethanol, utilize the ultrasonic oscillation that power density is 1W/mL within 30 minutes, to obtain graphene dispersing solution.
After utilizing spray-drying process to remove ethanol, can obtain pulverous Graphene, the mass yield of not calculating raw material aluminum chloride intercalator is about 75%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 5:
Graphite intercalation compound by 50g take nickelous chloride as intercalator is (in graphite intercalation compound, the consumption of nickelous chloride is 30g) join in the oxalic acid solution that 2L concentration is 80wt%, controlling solution temperature is 0 ℃, slowly stir 1 hour, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 5L propyl alcohol, utilize the ultrasonic oscillation that power density is 0.5W/mL within 60 minutes, to obtain graphene dispersing solution.
After utilizing spray-drying process to remove propyl alcohol, obtain pulverous Graphene, the mass yield of not calculating nickelous chloride intercalator in raw material is about 70%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 6:
Graphite intercalation compound by 1kg take iron(ic) chloride as intercalator is (in graphite intercalation compound, the consumption of iron(ic) chloride is 0.66kg) join in the superoxol that 10L concentration is 90wt%, controlling solution temperature is 0 ℃, slowly stir 0.5 hour, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 30L butanols, utilize the ultrasonic oscillation that power density is 0.5W/mL within 60 minutes, to obtain graphene dispersing solution.
After utilizing spray-drying process to remove butanols, obtain pulverous Graphene product, quality is about 360g, and the mass yield of not calculating iron(ic) chloride intercalator in raw material is about 76%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 7:
Graphite intercalation compound by 5g take antimonic fluoride as intercalator is (in graphite intercalation compound, the consumption of antimonic fluoride is 3g) join in the superoxol that 200mL concentration is 70wt%, controlling solution temperature is 60 ℃, slowly stir 1.5 hours, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 1L propyl alcohol, utilize the ultrasonic oscillation that power density is 0.5W/mL within 2 hours, to obtain graphene dispersing solution.
After utilizing spray-drying process to remove propyl alcohol, obtain pulverous Graphene product, the mass yield of not calculating antimonic fluoride intercalator in raw material is about 72%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 8:
Graphite intercalation compound by 10g take antimony chloride as intercalator is (in graphite intercalation compound, the consumption of antimony chloride is 4.8g) join in the superoxol that 500mL concentration is 60wt%, controlling solution temperature is 60 ℃, slowly stir 2 hours, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 1L formaldehyde, utilize the ultrasonic oscillation 1h that power density is 0.5W/mL to obtain graphene dispersing solution.
After utilizing spray-drying process to remove formaldehyde, obtain pulverous Graphene product, the mass yield of not calculating antimony chloride intercalator in raw material is about 72%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 9:
Graphite intercalation compound by 20g take bromine as intercalator is (in graphite intercalation compound, the consumption of bromine is 12g) join in the oxalic acid solution that 500mL concentration is 50wt%, controlling solution temperature is 80 ℃, slowly stir 2.5 hours, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, after repeatedly colourless to scavenging solution by washed with de-ionized water, drain, join in 1L N-Methyl pyrrolidone (NMP), utilize the ultrasonic oscillation that power density is 0.5W/mL within 1 hour, to obtain graphene dispersing solution.
After utilizing freeze-drying to remove N-Methyl pyrrolidone (NMP), obtain pulverous Graphene product, quality is about 6g, and the mass yield of not calculating bromine intercalator in raw material is about 75%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 10:
Graphite intercalation compound by 100g take aluminum chloride as intercalator is (in graphite intercalation compound, the consumption of aluminum chloride is 65g) join in the superoxol that 1L concentration is 40wt%, controlling solution temperature is 80 ℃, slowly stir 3 hours, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 2L dimethyl formamide (DMF), utilize the ultrasonic oscillation that power density is 1W/mL within 1 hour, to obtain graphene dispersing solution.
After utilizing freeze-drying to remove dimethyl formamide (DMF), obtain pulverous Graphene product, quality is about 35g, and the mass yield of not calculating aluminum chloride intercalator in raw material is about 78%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 11:
Graphite intercalation compound by 50g take iron(ic) chloride as intercalator is (in graphite intercalation compound, the consumption of iron(ic) chloride is 35g) join in the oxalic acid solution that 1L concentration is 50wt%, controlling solution temperature is 80 ℃, slowly stir 2.5 hours, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 2L dichlorobenzene (DCB), utilize the ultrasonic oscillation that power density is 1W/mL within 3 hours, to obtain graphene dispersing solution.
After utilizing freeze-drying to remove DCB, obtain pulverous Graphene product, quality is about 16g, and the mass yield of not calculating iron(ic) chloride intercalator in raw material is about 78%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 12:
Graphite intercalation compound by 100g take nickelous chloride as intercalator is (in graphite intercalation compound, the consumption of nickelous chloride is 51g) join that in the superoxol that 2L concentration is 60wt%, to control solution temperature be 0 ℃, slowly stir 2 hours, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 4L ethanol, utilize the ultrasonic oscillation that power density is 0.5W/mL within 2 hours, to obtain graphene dispersing solution.
Utilize freeze-drying to remove after ethanol and obtain pulverous Graphene product, quality is about 30g, and the productive rate while not calculating the quality of nickelous chloride intercalator in raw material is about 78%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 13:
Graphite intercalation compound by 100g take antimony chloride as intercalator is (in graphite intercalation compound, the consumption of antimony chloride is 70g) join in the oxalic acid solution that 2L concentration is 70wt%, controlling solution temperature is 30 ℃, slowly stir 1.5 hours, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, drain after repeatedly colourless to scavenging solution by washed with de-ionized water, join in 1.5L acetone, utilize the ultrasonic oscillation that power density is 1W/mL within 60 minutes, to obtain graphene dispersing solution.
After utilizing freeze-drying to remove acetone, obtain pulverous Graphene product, quality is about 36g, and the mass yield of not calculating antimony chloride intercalator in raw material is about 75%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Embodiment 14:
Graphite intercalation compound by 1kg take antimonic fluoride as intercalator is (in graphite intercalation compound, the consumption of antimonic fluoride is 0.55kg) join in the superoxol that 20L concentration is 80wt%, controlling solution temperature is 40 ℃, slowly stir 1 hour, obtain swimming in the quasiflake graphite alkene aggregate on liquid level.
Gained quasiflake graphite alkene aggregate is taken out, after repeatedly colourless to scavenging solution by washed with de-ionized water, drain, join in the lauryl sodium sulfate aqueous solution that 20L concentration is 1wt%, utilize the ultrasonic oscillation that power density is 0.1W/mL within 5 hours, to obtain graphene dispersing solution.
After utilizing freeze-drying to remove water, can arrive pulverous Graphene product, quality is about 380g, does not calculate antimonic fluoride intercalator mass yield in raw material and is about 72%.
In the present embodiment gained graphene powder, the number of plies of graphene film is that 5-8 layer, lateral dimension are 10-20 micron, and good crystallinity, and carbon-to-oxygen ratio is 80-100.
Claims (4)
1. prepare the method for high-quality graphene for one kind, it is characterized in that, graphite intercalation compound take bromine, iodine chloride, iodine bromide IBr, aluminum chloride, antimony chloride, iron(ic) chloride or antimonic fluoride as intercalator is raw material, oxalic acid or superoxol expand and solvent in ultrasonic peel off to combine prepare high-quality graphene; First graphite intercalation compound powder is joined to concentration in the oxalic acid or superoxol of 40 ~ 80 wt%, then under the condition of 30 ~ 100 ℃, carry out 0.5 ~ 24 hour expansion process, obtain the quasiflake graphite alkene aggregate of high level expansion; And then, by gained quasiflake graphite alkene aggregate after expansion process in the aqueous solution or organic solvent solution of organic solvent or various tensio-active agents, ultrasonic oscillation is processed 30 minutes ~ 1 hour, and realization is peeled off, and Graphene is dispersed in and in solvent, forms graphene solution; Utilize the dry or cryodesiccated method of spraying to remove after organic solvent or various tensio-active agent, obtain high-quality graphene powder; In gained graphene powder, 3 ~ 8 layers of the numbers of plies of graphene film, 5 ~ 50 microns of lamella sizes, carbon-to-oxygen ratio 30 ~ 120;
Every 1 liter of oxalic acid or superoxol are processed 1 ~ 500 gram of graphite intercalation compound.
2. according to the method for preparing high-quality graphene claimed in claim 1, it is characterized in that, in the time carrying out expansion process, the time is 2 ~ 5 hours, and temperature range is 30 ~ 40 ℃.
3. according to the method for preparing high-quality graphene claimed in claim 1, it is characterized in that, every 1 liter of oxalic acid or superoxol are processed 15 ~ 20 grams of graphite intercalation compounds.
4. according to the method for preparing high-quality graphene claimed in claim 1, it is characterized in that, organic solvent is alcohols, ketone, aldehydes, organic acid, N-Methyl pyrrolidone, dimethyl formamide, N,N-DIMETHYLACETAMIDE, chlorobenzene or dichlorobenzene, tensio-active agent is sodium lauryl sulphate, Sodium dodecylbenzene sulfonate or cetyl trimethylammonium bromide, and the strength of solution of tensio-active agent is 0.1-5 wt %.
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| CN101746755B (en) * | 2009-12-14 | 2012-07-04 | 重庆大学 | Method for preparing multi-layer graphene |
| CN101993065B (en) * | 2010-12-17 | 2012-09-05 | 中国科学院上海微***与信息技术研究所 | Method for preparing graphene powder |
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