CN102674327A - Environment-friendly method for preparing water-soluble grapheme at normal temperature - Google Patents
Environment-friendly method for preparing water-soluble grapheme at normal temperature Download PDFInfo
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Abstract
The invention relates to a method for preparing water-soluble grapheme at the normal temperature, which relates to a grapheme preparation method. The method for preparing water-soluble grapheme at the normal temperature aims to overcome the defects that the traditional method for preparing grapheme has the disadvantages of high reaction temperature, is poisonous in the reaction process, is harmful to the environment and is not suitable for large-scale production, and also solve the problems of the dispersibility and the water solubility of the traditional grapheme. The method comprises the following steps: taking graphite powder, concentrated sulfuric acid, sodium nitrate, potassium permanganate and deionized water as raw materials to prepare graphene oxide; adding the graphene oxide into sodium hydroxide solution; processing the sodium hydroxide solution added with the graphene oxide through ultrasonic under the vacuum condition; then stirring the sodium hydroxide solution added with the graphene oxide with magnetic force for 24-60 hours; and drying sedimentary resultants in a vacuum drying chamber so as to obtain the water-soluble grapheme after the resultants are washed and filtered. The method disclosed by the invention has the advantages of low process cost, environmental protection and no pollution, and can be used for large-scale protection. The solubility of the prepared grapheme is 1.5-2.0mg/ml, and the prepared grapheme can be stably dispersed in the water without generating sediments within 4-6 months. The graphene prepared with the method disclosed by the invention can be used in the fields of biological medicine, energy, electron and the like.
Description
Technical field
The present invention relates to preparation method of graphene.
Background technology
From the Andre Geim of Univ Manchester UK in 2004 professor and Kostya Novoselov adopt first tape stripping obtain Graphene (Graphene, GN) since, the research of Graphene just receives vast scientific research person's extensive concern.Therefore two chemists of Britain in 2010 obtain Nobel prize for physics, Graphene become another great discovery after soccerballene and carbon nanotube (Science, 2004,306,666-669).Graphene be a kind of two dimension pile up the carbon material form by six-ring.Each carbon atom is sp2 hydridization, and the remaining electronics of p track forms big conjugated system and big π track, and electronics can move freely at the π track (Angew.Chem., Int.Ed., 2009,48,7752-7777).Graphene has good electrical conductivity, physical strength, catalytic performance, optical property, absorption property, and Graphene has good heat-conducting and very high transparency in addition, and Graphene is the lightest in the known materials at present; Material (C.Lee, X.Wei, J.W.Kysar and J.Hone that intensity is maximum; Science; 2008,321,385-388; Y.Zhang, Y.-W.Tan, H.L.Stormer and P.Kim, Nature, 2005,438,201-204).Because these physicalies, Graphene is widely used in every field, as: transmitter, pharmaceutical engineering, catalysis, the energy (O.C.Compton and S.T.Nguyen; Small, 2010,6; 711-723.S.Park and R.S.Ruoff, Nat.Nanotechnol., 2009; 4,217-224).
The compound method of Graphene mainly adopts physical method and chemical process now.
The physical method employing is carried out micromechanics to raw material Graphite Powder 99 (Graphite) and is peeled off method (Micromechenical cleavage method) preparation Graphene, is the Geim professor seminar of the discoverer Univ Manchester UK of Graphene the earliest.They peel off graphite repeatedly with adhesive tape, last success make the Graphene single chip architecture.Though it is simple to operate that micromechanics is peeled off method, cost is lower, and poor repeatability yields poorly, and is difficult to scale operation.
Chemical process preparation mainly is Graphite Powder 99 to be carried out oxidation prepare the intermediate product graphite oxide rare (graphene oxide GO), utilizes graft process or peel off method to obtain graphene oxide.Introduce a large amount of oxy functional groups in graphite layers after graphite is oxidized, like functional groups such as C=O, C-OH and COOH.The introducing of these Sauerstoffatoms makes the π key of graphite layers rupture, and can graphene oxide be reduced through chemical reduction, thereby obtain Graphene.
Method of reducing commonly used has:
1.RuoffRS utilize Hydrazine Hydrate 80 redox graphene under the condition of 80～100 ℃ of heating to prepare Graphene Deng the people.Be easy between this method Graphene take place to reunite and pile up, brought very big obstacle for the application of Graphene.This seminar improves this method again afterwards; Promptly in the reductive process, add specific superpolymer Lewatit; Graphene surface after making it be adsorbed onto reduction; Thereby hindered the reunion between the graphene film of reduction back, obtained the graphene suspension of stable dispersion in the aqueous solution.
This method shortcoming: temperature of reaction height, the poisonous explosive of raw material Hydrazine Hydrate 80, the complicated product amount of reaction are few; Can not large-scale production; Prepared graphene is difficult for disperseing; And this method is fit to be applied in biomedical sector, and improved exactly method is removed and can be dispersed in the water China and foreign countries, still has above-mentioned shortcoming.
2.Zhang people such as FB are in the aqueous solution of highly basic NaOH or KOH, also can obtain to stablize graphene suspension by redox graphene through heating, but this method shortcoming is: reaction needed is carried out under comparatively high temps.
3.Ra.iamathi M. etc. utilize pure hot method also can reduce the preparation Graphene, the shortcoming of this method is that reaction needed is carried out under high temperature, highly compressed situation, and reaction is not thorough.
4. it is rare to also have some biomacromolecules to be used for reduction-oxidation graphite in addition, as: amino acid, glucose, Trisodium Citrate, serum proteins, although these method of reducing close friend is nontoxic, it is also poor that its reducing degree is compared Hydrazine Hydrate 80, reduces not thorough.
Recently Huang C Z (RSC Adv., 2012,2,2322-2328) wait people's research with Vitrum AB graphite oxide also, this method synthetic Graphene can stable dispersion, but reaction needed carries out under the condition of heating, and reduction is not thorough.
The synthesizing graphite alkene technical difficult points is: low-cost, environment friendly and pollution-free, scale operation, stable dispersed and water-soluble.
Summary of the invention
The method that the present invention will solve the existing preparation Graphene exists that temperature of reaction is high, poisonous in the reaction process, harm environment, can not scale operation and existing Graphene dispersiveness and bad water-solubility, and a kind of water at normal temperature dissolubility Graphene environment-friendly preparation method thereof is provided.
Water at normal temperature dissolubility Graphene environment-friendly preparation method thereof of the present invention carries out according to the following steps:
One, takes by weighing Graphite Powder 99, the vitriol oil, SODIUMNITRATE, potassium permanganate, deionized water; Wherein the ratio of the Graphite Powder 99 and the vitriol oil is 1g: (20～80mL); The ratio of Graphite Powder 99 and SODIUMNITRATE is 1g: (0.5～2.0g); The ratio of Graphite Powder 99 and potassium permanganate is 1g: (3～10g); The ratio of Graphite Powder 99 and deionized water is 1g: (100～200mL); The massfraction of the vitriol oil is 98%;
Two, the exsiccant beaker is placed ice bath, in beaker, add Graphite Powder 99, the vitriol oil and the SODIUMNITRATE that takes by weighing in the step 1, after mixing; Add potassium permanganate; Control reaction temperature is no more than 10 ℃, continues magnetic agitation 2～3h, accomplishes peeling off of graphite;
Three, the beaker of step 2 being transferred to temperature is in 30～50 ℃ the water-bath, continues magnetic agitation, progressively adds the deionized water that takes by weighing in the part steps one; The volume that adds is (1/6～1/2) of the deionized water TV that takes by weighing in the step 1, and control reaction temperature is 30～50 ℃, water-bath 30～60min; Progressively add the deionized water that takes by weighing in the remaining step 1 then; Control reaction temperature is no more than 98 ℃, and water-bath 30～120min obtains the brown mixture; In beaker, add ydrogen peroxide 50 then, become glassy yellow by brown to the color of mixture;
Four, the glassy yellow mixture that obtains with aqueous hydrochloric acid washing step three, topple over fall supernatant liquid after, use 20～30 ℃ of deionized water filtration washings again, it is to dry in 40～60 ℃ the vacuum drying oven that gained is deposited in temperature, obtains graphene oxide;
Five, the graphene oxide of step 4 gained being joined the pH value is in 9～12 the sodium hydroxide solution; Ultrasonic 30～90min under vacuum condition; Then with rotating speed magnetic agitation 24～60h of 150～250r/min; With absolute ethanol washing 3～5 times, it is dry 24～48h in 40～60 ℃ the vacuum drying oven that gained is deposited in temperature, obtains water-soluble Graphene; Wherein the ratio of graphene oxide and sodium hydroxide solution is 100mg: (100～250mL).
The invention has the beneficial effects as follows:
1, Graphene normal temperature reduction preparation, behind synthetic graphene oxide, the not heating of the whole process of reduction Graphene; At room temperature carry out, pollution-free environmental protection reduces production costs; And can scale operation, form industrial chain, use for every field and provide safeguard;
2, directly have functional group after the Graphene reduction, and have good water-solubility;
3, Graphene of the present invention has reliable stability and adsorptivity; Prepared graphene is that Zeta potential in 7～12 the aqueous solution is 40～60mV at pH; The solubleness that graphite is rare is 1.5～2.0mg/ml, and deposition did not appear in 4～6 months in can be stable be dispersed in the water.According to document (nature nanotechnology, 2008,3,101-105; Nano Lett.; 2008; 8 (6) 1679-1682) and U.S. ASTM (American Society for Testing and Materials) D4187-82 standard; Zeta potential has " good stability " greater than the water solution system of ± 40mV, and the prepared graphene aqueous solution of the present invention has stable dispersiveness.
Prepared graphene of the present invention can be used for fields such as biological medicine, the energy and electronics, and for solving human disease treatment and diagnosis from now on, and the current energy is anxious lacks, and the hyundai electronics development in science and technology furnishes ample material.
Description of drawings
Fig. 1 is the stereoscan photograph of embodiment one prepared graphene;
Fig. 2 is the transmission electron microscope photo of embodiment one prepared graphene;
Fig. 3 is the XRD spectra of graphite;
Fig. 4 is the XRD spectra of the graphene oxide of embodiment one prepared graphene and embodiment one step 4 gained; The spectrogram that wherein is marked with G (001) peak position is the XRD spectra of graphene oxide; The spectrogram that is marked with G (002) peak position is the XRD spectra of Graphene;
Fig. 5 is the infrared spectrogram of the graphene oxide of embodiment one step 4 gained;
Fig. 6 is the infrared spectrogram of embodiment one prepared graphene;
Fig. 7 is the concentration and the charge capacity graph of a relation of the absorption 5-fluorine pyrimidine of embodiment one prepared graphene;
Fig. 8 is the concentration and the charge capacity graph of a relation of the absorption Frosst) of embodiment one prepared graphene;
Fig. 9 is that to be dispersed in pH be the photo in 10 the aqueous solution to embodiment one prepared graphene.
Embodiment
Technical scheme of the present invention is not limited to following cited embodiment, also comprises the arbitrary combination between each embodiment.
Embodiment one: this embodiment water at normal temperature dissolubility Graphene environment-friendly preparation method thereof carries out according to the following steps:
One, takes by weighing Graphite Powder 99, the vitriol oil, SODIUMNITRATE, potassium permanganate, deionized water; Wherein the ratio of the Graphite Powder 99 and the vitriol oil is 1g: (20～80mL); The ratio of Graphite Powder 99 and SODIUMNITRATE is 1g: (0.5～2.0g); The ratio of Graphite Powder 99 and potassium permanganate is 1g: (3～10g); The ratio of Graphite Powder 99 and deionized water is 1g: (100～200mL); The massfraction of the vitriol oil is 98%;
Two, the exsiccant beaker is placed ice bath, in beaker, add Graphite Powder 99, the vitriol oil and the SODIUMNITRATE that takes by weighing in the step 1, after mixing; Add potassium permanganate; Control reaction temperature is no more than 10 ℃, continues magnetic agitation 2～3h, accomplishes peeling off of graphite;
Three, the beaker of step 2 being transferred to temperature is in 30～50 ℃ the water-bath, continues magnetic agitation, progressively adds the deionized water that takes by weighing in the part steps one; The volume that adds is (1/6～1/2) of the deionized water TV that takes by weighing in the step 1, and control reaction temperature is 30～50 ℃, water-bath 30～60min; Progressively add the deionized water that takes by weighing in the remaining step 1 then; Control reaction temperature is no more than 98 ℃, and water-bath 30～120min obtains the brown mixture; In beaker, add ydrogen peroxide 50 then, become glassy yellow by brown to the color of mixture;
Four, the glassy yellow mixture that obtains with aqueous hydrochloric acid washing step three, topple over fall supernatant liquid after, use 20～30 ℃ of deionized water filtration washings again, it is to dry in 40～60 ℃ the vacuum drying oven that gained is deposited in temperature, obtains graphene oxide;
Five, the graphene oxide of step 4 gained being joined the pH value is in 9～12 the sodium hydroxide solution; Ultrasonic 30～90min under vacuum condition; Then with rotating speed magnetic agitation 24～60h of 150～250r/min; With absolute ethanol washing 3～5 times, it is dry 24～48h in 40～60 ℃ the vacuum drying oven that gained is deposited in temperature, obtains water-soluble Graphene; Wherein the ratio of graphene oxide and sodium hydroxide solution is 100mg: (100～250mL).
The beneficial effect of this embodiment is:
1, Graphene normal temperature reduction preparation, behind synthetic graphene oxide, the not heating of the whole process of reduction Graphene; At room temperature carry out, pollution-free environmental protection reduces production costs; And can scale operation, form industrial chain, use for every field and provide safeguard;
2, directly have functional group after the Graphene reduction, and have good water-solubility;
3, this embodiment prepared graphene has reliable stability and adsorptivity; Prepared graphene is that Zeta potential in 7～12 the aqueous solution is 40～60mV at pH; The solubleness that graphite is rare is 1.5～2.0mg/ml; Deposition did not appear in 4～6 months in can be stable be dispersed in the water, and this embodiment prepared graphene aqueous solution has stable dispersiveness.
Embodiment two: what this embodiment and embodiment one were different is: the ratio of the Graphite Powder 99 and the vitriol oil is 1g in the step 1: (40～70mL); The ratio of Graphite Powder 99 and SODIUMNITRATE is 1g: (1.0～1.5g); The ratio of Graphite Powder 99 and potassium permanganate is 1g: (5～8g); The ratio of Graphite Powder 99 and deionized water is 1g: (120～180mL).Other is identical with embodiment one.
Embodiment three: what this embodiment was different with embodiment one or two is: the temperature of reaction in the step 2 is 5～8 ℃.Other is identical with embodiment one or two.
Embodiment four: what this embodiment was different with one of embodiment one to three is: the speed of magnetic agitation is 100～200r/min in the step 2.Other is identical with one of embodiment one to three.
Embodiment five: what this embodiment was different with one of embodiment one to four is: progressively add the deionized water that takes by weighing in the part steps one in the step 3; The volume that adds is (1/4～1/3) of the deionized water TV that takes by weighing in the step 1; Control reaction temperature is 35～45 ℃, and water-bath 35～50min progressively adds the deionized water that takes by weighing in the remaining step 1 then; Control reaction temperature is 80～95 ℃, water-bath 60～90min.Other is identical with one of embodiment one to four.
Embodiment six: what this embodiment was different with one of embodiment one to five is: the speed of magnetic agitation is 100～200r/min in the step 3.Other is identical with one of embodiment one to five.
Embodiment seven: what this embodiment was different with one of embodiment one to six is: the volume(tric)fraction of ydrogen peroxide 50 described in the step 3 is 30%.Other is identical with one of embodiment one to six.
Embodiment eight: what this embodiment was different with one of embodiment one to seven is: the massfraction of aqueous hydrochloric acid is 3%～8% in the step 4.Other is identical with one of embodiment one to seven.
Embodiment nine: what this embodiment was different with one of embodiment one to eight is: ultransonic power is 100～400W in the step 5.Other is identical with one of embodiment one to eight.
Embodiment ten: what this embodiment was different with one of embodiment one to nine is: the ratio of graphene oxide and sodium hydroxide solution is 100mg in the step 5: (120～200mL).Other is identical with one of embodiment one to nine.
Adopt following examples to verify beneficial effect of the present invention:
Embodiment one:
Present embodiment water at normal temperature dissolubility Graphene environment-friendly preparation method thereof carries out according to the following steps:
One, taking by weighing 1g Graphite Powder 99,50mL massfraction is 98% the vitriol oil, 0.7g SODIUMNITRATE, 5g potassium permanganate, 100mL deionized water;
Two, the exsiccant beaker is placed ice bath, in beaker, add Graphite Powder 99, the vitriol oil and the SODIUMNITRATE that takes by weighing in the step 1, after mixing; Add potassium permanganate; Control reaction temperature is no more than 8 ℃, with the speed magnetic agitation 2h of 100/min, accomplishes peeling off of graphite;
Three, the beaker of step 2 being transferred to temperature is that the speed magnetic agitation with 120r/min progressively adds the deionized water that takes by weighing in the 30mL step 1 in 35 ℃ the water-bath; Control reaction temperature is 35～50 ℃; Water-bath 30～60min progressively adds the deionized water that takes by weighing in the remaining 70mL step 1 then, and control reaction temperature is no more than 98 ℃; Water-bath 30～120min; Obtain the brown mixture, in beaker, add ydrogen peroxide 50 then, become glassy yellow by brown to the color of mixture;
Four, using massfraction is the glassy yellow mixture that 5% aqueous hydrochloric acid washing step three obtains, topple over fall supernatant liquid after, use 40 ℃ of deionized water filtration washings again, it is to dry in 50 ℃ the vacuum drying oven that gained is deposited in temperature, obtains graphene oxide.
Five, the graphene oxide of step 4 gained being joined the pH value is in 10 the sodium hydroxide solution; Ultrasonic 60min under vacuum condition; Then with the rotating speed magnetic agitation 36h of 200r/min; With absolute ethanol washing 3 times, it is dry 24h in 50 ℃ the vacuum drying oven that gained is deposited in temperature, obtains water-soluble Graphene; Wherein the ratio of graphene oxide and sodium hydroxide solution is 100mg: 150mL.
In the step 2 of present embodiment, the sufficient reacting oxidation thorough, make the abundant intercalation of sulfuric acid molecule to graphitized mesophase, realization graphite is peeled off; In the step 3, the effect of ydrogen peroxide 50 is unreacted permanganic acid of neutralization and Manganse Dioxide, and the advantage that present embodiment prepares graphene oxide is to have reduced preoxidation process, and the cycle is shorter.
Broad property Graphene to the present embodiment gained carries out performance test, and the result is following:
Fig. 1 is the stereoscan photograph of present embodiment prepared graphene; High-visible Graphene is a multilayer from figure, edge curl.
Fig. 2 is the transmission electron microscope photo of present embodiment prepared graphene; High-visible Graphene is a multiwalled, transparent and fold arranged from figure.
Fig. 3 is the XRD spectra of graphite; Be 26.5 ° in diffraction peak and locate to have occurred tangible graphite (002) diffraction peak, interlamellar spacing is about 0.34nm.
Fig. 4 is the XRD spectra of the graphene oxide (GO) of present embodiment prepared graphene (GN) and present embodiment step 4 gained; The spectrogram that wherein is marked with G (001) peak position is the XRD spectra of graphene oxide; The spectrogram that is marked with G (002) peak position is the XRD spectra of Graphene; Behind the graphite oxidation, the characteristic peak of graphite 26.5 ° (002) disappears, and 10.62 ° of (001) peaks occurred, and the sample layer spacing increases to 0.885nm, and this explanation graphite oxidation is complete, has formed graphene oxide.Graphene oxide is through the reduction of NaOH; 10.62 the shape at 26.5 ° of (002) steamed bun peaks has appearred in ° (001) peak completely dissolve, the carbon-coating spacing is dwindled; Explain that graphene oxide is reduced; A small amount of graphite linings is piled into graphite-structure again, as a result Graphene sample diffraction peak intensity a little less than, percent crystallinity also obviously descends.
Fig. 5 is that embodiment one step 4 graphite is through forming the infrared spectrum of GO behind the vitriol oil, SODIUMNITRATE and the potassium permanganate oxidation; As can be seen from the figure, after peroxo-, the quantity of functional group and intensity obviously improve in the graphite-structure.Concrete analysis is: 3420cm
-1Be O-H vibration absorption peak, 1728cm
-1The absorption peak of carboxylic acid-COOH functional group-C=O appears in the place, and this explanation oxide treatment can be introduced carboxyl graphite-structure is modified.1621cm
-1Be C-C skeletal vibration peak, show that graphite-structure is not destroyed after oxide treatment, still have the typical structure of graphite.1218 is the C-OH vibration absorption peak, and 1028cm-1 is the vibration absorption peak of C-O.
Fig. 6 is the infrared spectrogram of embodiment one prepared graphene; As can be seen from the figure; The sodium hydroxide reduction is different with hydrazine hydrate reduction, does not destroy the functional group on original graphene oxide, and just skew has taken place in functional group; But still the surface functional group of carboxyl and hydroxyl is arranged, be dispersed in the water so Graphene equally can be stable.
Respectively cancer therapy drug 5-fluorine pyrimidine and two kinds of medicines of Frosst) are carried out load test, obtain corresponding absorption result such as Fig. 7 and shown in Figure 8 through the absorption drug test.Fig. 7 is the concentration and the charge capacity graph of a relation of the absorption 5-fluorine pyrimidine of embodiment one prepared graphene; Fig. 8 is the concentration and the charge capacity graph of a relation of the absorption Frosst) of embodiment one prepared graphene; The result shows; The load saturation of load cancer therapy drug 5-fluorine pyrimidine is 0.28mg/mg (being the graphene-supported 0.28 gram 5-fluorine pyrimidine of every gram), and the charge capacity of load Frosst) is 3.34mg/mg (being the graphene-supported 3.34 gram Frosst) of every gram).
Fig. 9 is that to be dispersed in pH be the photo in 10 the aqueous solution to embodiment one prepared graphene; The present embodiment prepared graphene has reliable stability and adsorptivity; Prepared graphene is that Zeta potential in 10 the aqueous solution is 50mV at pH; The solubleness that graphite is rare is 2.0mg/ml, and deposition did not appear in 4～6 months in can be stable be dispersed in the water.According to document (nature nanotechnology, 2008,3,101-105; Nano Lett.; 2008; 8 (6) 1679-1682) and U.S. ASTM (American Society for Testing and Materials) D4187-82 standard; Zeta potential has " good stability " greater than the water solution system of ± 40mV, and the prepared graphene aqueous solution of the present invention has stable dispersiveness.
Claims (10)
1. water at normal temperature dissolubility Graphene environment-friendly preparation method thereof is characterized in that water at normal temperature dissolubility Graphene environment-friendly preparation method thereof carries out according to the following steps:
One, takes by weighing Graphite Powder 99, the vitriol oil, SODIUMNITRATE, potassium permanganate, deionized water; Wherein the ratio of the Graphite Powder 99 and the vitriol oil is 1g: (20～80mL); The ratio of Graphite Powder 99 and SODIUMNITRATE is 1g: (0.5～2.0g); The ratio of Graphite Powder 99 and potassium permanganate is 1g: (3～10g); The ratio of Graphite Powder 99 and deionized water is 1g: (100～200mL); The massfraction of the vitriol oil is 98%;
Two, the exsiccant beaker is placed ice bath, in beaker, add Graphite Powder 99, the vitriol oil and the SODIUMNITRATE that takes by weighing in the step 1, after mixing; Add potassium permanganate; Control reaction temperature is no more than 10 ℃, continues magnetic agitation 2～3h, accomplishes peeling off of graphite;
Three, the beaker of step 2 being transferred to temperature is in 30～50 ℃ the water-bath, continues magnetic agitation, progressively adds the deionized water that takes by weighing in the part steps one; The volume that adds is (1/6～1/2) of the deionized water TV that takes by weighing in the step 1, and control reaction temperature is 30～50 ℃, water-bath 30～60min; Progressively add the deionized water that takes by weighing in the remaining step 1 then; Control reaction temperature is no more than 98 ℃, and water-bath 30～120min obtains the brown mixture; In beaker, add ydrogen peroxide 50 then, become glassy yellow by brown to the color of mixture;
Four, the glassy yellow mixture that obtains with aqueous hydrochloric acid washing step three, topple over fall supernatant liquid after, use 20～30 ℃ of deionized water filtration washings again, it is to dry in 40～60 ℃ the vacuum drying oven that gained is deposited in temperature, obtains graphene oxide;
Five, the graphene oxide of step 4 gained being joined the pH value is in 9～12 the sodium hydroxide solution; Ultrasonic 30～90min under vacuum condition; Then with rotating speed magnetic agitation 24～60h of 150～250r/min; With absolute ethanol washing 3～5 times, it is dry 24～48h in 40～60 ℃ the vacuum drying oven that gained is deposited in temperature, obtains water-soluble Graphene; Wherein the ratio of graphene oxide and sodium hydroxide solution is 100mg: (100～250mL).
2. water at normal temperature dissolubility Graphene environment-friendly preparation method thereof according to claim 1 is characterized in that the ratio of Graphite Powder 99 and the vitriol oil is 1g in the step 1: (40～70mL); The ratio of Graphite Powder 99 and SODIUMNITRATE is 1g: (1.0～1.5g); The ratio of Graphite Powder 99 and potassium permanganate is 1g: (5～8g); The ratio of Graphite Powder 99 and deionized water is 1g: (120～180mL).
3. water at normal temperature dissolubility Graphene environment-friendly preparation method thereof according to claim 1 is characterized in that the temperature of reaction in the step 2 is 5～8 ℃.
4. water at normal temperature dissolubility Graphene environment-friendly preparation method thereof according to claim 1 is characterized in that the speed of magnetic agitation is 100～200r/min in the step 2.
5. water at normal temperature dissolubility Graphene environment-friendly preparation method thereof according to claim 1; It is characterized in that progressively adding in the step 3 deionized water that takes by weighing in the part steps one, the volume of adding is (1/4～1/3) of the deionized water TV that takes by weighing in the step 1, and control reaction temperature is 35～45 ℃; Water-bath 35～50min; Progressively add the deionized water that takes by weighing in the remaining step 1 then, control reaction temperature is 80～95 ℃, water-bath 60～90min.
6. water at normal temperature dissolubility Graphene environment-friendly preparation method thereof according to claim 1 is characterized in that the speed of magnetic agitation is 100～200r/min in the step 3.
7. water at normal temperature dissolubility Graphene environment-friendly preparation method thereof according to claim 1, the volume(tric)fraction that it is characterized in that ydrogen peroxide 50 described in the step 3 is 30%.
8. water at normal temperature dissolubility Graphene environment-friendly preparation method thereof according to claim 1, the massfraction that it is characterized in that aqueous hydrochloric acid in the step 4 is 3%～8%.
9. water at normal temperature dissolubility Graphene environment-friendly preparation method thereof according to claim 1 is characterized in that ultransonic power is 100～400W in the step 5.
10. water at normal temperature dissolubility Graphene environment-friendly preparation method thereof according to claim 1 is characterized in that the ratio of graphene oxide and sodium hydroxide solution is 100mg in the step 5: (120～200mL).
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| CN110627668A (en) * | 2018-06-22 | 2019-12-31 | 天津理工大学 | Preparation method of carbon-based harmful gas scavenger |
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