CN112791745A - Preparation method of graphene composite aerogel and application of graphene composite aerogel in oxidation removal of wastewater organic matters - Google Patents
Preparation method of graphene composite aerogel and application of graphene composite aerogel in oxidation removal of wastewater organic matters Download PDFInfo
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- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 claims abstract description 10
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- 230000001590 oxidative effect Effects 0.000 claims description 9
- 239000000725 suspension Substances 0.000 claims description 9
- RBTBFTRPCNLSDE-UHFFFAOYSA-N 3,7-bis(dimethylamino)phenothiazin-5-ium Chemical compound C1=CC(N(C)C)=CC2=[S+]C3=CC(N(C)C)=CC=C3N=C21 RBTBFTRPCNLSDE-UHFFFAOYSA-N 0.000 claims description 8
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- 229960000907 methylthioninium chloride Drugs 0.000 claims description 8
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- DBMJMQXJHONAFJ-UHFFFAOYSA-M Sodium laurylsulphate Chemical compound [Na+].CCCCCCCCCCCCOS([O-])(=O)=O DBMJMQXJHONAFJ-UHFFFAOYSA-M 0.000 claims description 6
- PYWVYCXTNDRMGF-UHFFFAOYSA-N rhodamine B Chemical compound [Cl-].C=12C=CC(=[N+](CC)CC)C=C2OC2=CC(N(CC)CC)=CC=C2C=1C1=CC=CC=C1C(O)=O PYWVYCXTNDRMGF-UHFFFAOYSA-N 0.000 claims description 6
- 229940043267 rhodamine b Drugs 0.000 claims description 6
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- 229910000359 iron(II) sulfate Inorganic materials 0.000 claims description 5
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 claims description 4
- MCDLETWIOVSGJT-UHFFFAOYSA-N acetic acid;iron Chemical compound [Fe].CC(O)=O.CC(O)=O MCDLETWIOVSGJT-UHFFFAOYSA-N 0.000 claims description 3
- GVGUFUZHNYFZLC-UHFFFAOYSA-N dodecyl benzenesulfonate;sodium Chemical compound [Na].CCCCCCCCCCCCOS(=O)(=O)C1=CC=CC=C1 GVGUFUZHNYFZLC-UHFFFAOYSA-N 0.000 claims description 3
- 229960002089 ferrous chloride Drugs 0.000 claims description 3
- NMCUIPGRVMDVDB-UHFFFAOYSA-L iron dichloride Chemical compound Cl[Fe]Cl NMCUIPGRVMDVDB-UHFFFAOYSA-L 0.000 claims description 3
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- DAJSVUQLFFJUSX-UHFFFAOYSA-M sodium;dodecane-1-sulfonate Chemical compound [Na+].CCCCCCCCCCCCS([O-])(=O)=O DAJSVUQLFFJUSX-UHFFFAOYSA-M 0.000 claims description 2
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- 229910052723 transition metal Inorganic materials 0.000 description 2
- 230000010718 Oxidation Activity Effects 0.000 description 1
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J31/00—Catalysts comprising hydrides, coordination complexes or organic compounds
- B01J31/02—Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides
- B01J31/0215—Sulfur-containing compounds
- B01J31/0225—Sulfur-containing compounds comprising sulfonic acid groups or the corresponding salts
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
- B01J23/70—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
- B01J23/74—Iron group metals
- B01J23/745—Iron
-
- B01J35/33—
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
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- Hydrology & Water Resources (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
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Abstract
A preparation method of graphene composite aerogel and application of graphene composite aerogel in removing organic matters in wastewater by oxidation belong to the technical field of nano composite materials. The method comprises the steps of uniformly mixing graphene oxide, an anionic surfactant and ferrous salt, and passing the mixture through a bubble template and Fe2+Preparing graphene composite hydrogel by in-situ reduction and hydrothermal self-assembly technology; and washing, freezing and drying to obtain the graphene composite aerogel. The graphene composite aerogel has the characteristics of uniform pores, excellent mechanical property, high electrocatalytic activity, easiness in recycling and the like, and is suitable for three-dimensional electrode construction and oxidation elimination of organic matters in water. The preparation method is simple, the raw materials are simple and easily obtained, and the preparation method is environment-friendly and suitable for useHas wide application.
Description
Technical Field
The invention relates to a preparation method of graphene composite aerogel and a wastewater organic matter removal method by oxidizing the graphene composite aerogel, and belongs to the technical field of nano composite material preparation and environmental protection.
Background
Due to the increasing problems of water pollution caused by industrial production and human life, the development of novel and efficient water treatment technology is urgent. Advanced oxidation processes, such as electrochemical oxidation, fenton oxidation, photochemical oxidation, catalytic wet oxidation, sonochemical oxidation, ozone oxidation, etc., have been widely used and developed in the field of directly mineralizing organic pollutants or improving the biodegradability of organic pollutants by oxidation. Among them, the three-dimensional electrode technology, as one of the important methods of electrochemical oxidation, has the advantages of large specific surface area of the electrode, short mass transfer distance, low energy consumption, high current efficiency, no secondary pollution and the like, and has great attention to its application potential.
The three-dimensional electrode improves the capacity of electrocatalytic oxidation of organic pollutants by adding granular or chippy particle electrodes between the electrodes of the traditional two-dimensional electrolytic cell. Organic pollutants in the wastewater are directly oxidized and degraded on the anode and the particle electrode or various intermediate products such as OH and H generated in the electrode reaction process are utilized2O2、O3Or Cl2And (4) indirectly degrading the equal-strength oxidant. If the particle electrode contains transition metal elements, the transition metal elements will react with O on the cathode2H generated by reduction reaction2O2The electro-Fenton reaction is carried out, thereby generating OH with strong oxidation activity and greatly accelerating the efficiency of degrading the waste water. Therefore, the three-dimensional electrode and the Fenton technology are combined, and the method has a wide application prospect in the field of treatment of the organic wastewater difficult to degrade.
The graphene is formed by passing sp through carbon atoms2The two-dimensional plane structure with the thickness of the monoatomic layer is constructed by a hybridization mode and is a basic construction unit of all graphite carbon materials. The large specific surface area, versatile surface chemistry and excellent mechanical properties of graphene-based nanoplatelets enable it to form high-performance monolithic graphene aerogels. In view of the above characteristics, the graphene aerogel is widely used in the field of wastewater treatment. However, it is not limited toAnd the electrochemical performance and the mechanical performance of a pure graphene aerogel particle electrode are poor, so that the wastewater organic matters are difficult to be subjected to thorough oxidative degradation, and meanwhile, the graphene aerogel particle electrode is difficult to recycle and is not beneficial to practical application. Therefore, from the aspect of practical application, the electrochemical performance and the mechanical performance of the graphene aerogel particle electrode are improved, and the method has important significance for eliminating organic pollutants in wastewater through efficient oxidation of the three-dimensional electrode.
Disclosure of Invention
In order to overcome the defects in the prior art, the invention aims to provide a preparation method of graphene composite aerogel for oxidizing organic wastewater by using a three-dimensional electrode. The preparation method is simple, safe to operate and low in cost, the prepared graphene composite aerogel is excellent in mechanical property and good in stability, and when the graphene composite aerogel is used for oxidizing organic wastewater by a three-dimensional electrode, an electro-Fenton reaction can occur, so that the electrochemical property is enhanced, and the efficient and stable application of the three-dimensional electrode is greatly promoted.
In order to achieve the purpose of the invention and solve the problems in the prior art, the invention adopts the technical scheme that: a preparation method of graphene composite aerogel for oxidizing organic wastewater by using a three-dimensional electrode comprises the following steps:
step 1, taking 12mL of graphene oxide suspension liquid with the concentration of 2-5 mg/mL, adding 1mL of anionic surfactant aqueous solution with the concentration of 30-60 mg/mL into the graphene oxide suspension liquid, wherein the anionic surfactant comprises at least one of sodium dodecyl sulfate, sodium dodecyl sulfate and sodium dodecyl benzene sulfonate, magnetically stirring for 30min, stirring speed of a magnetic stirrer is 500-800 r/min, after reactants are uniformly mixed, adding 0.25-2 mL of ferrous salt aqueous solution with the concentration of 9-18 mg/mL, wherein the ferrous salt comprises one or more of ferrous sulfate, ferrous chloride and ferrous acetate, magnetically stirring for 2h to enable ferrous ions to be adsorbed on graphene oxide sheet layers through electrostatic attraction, and the speed of the stirrer is controlled to be 1400-r/min;
and 2, transferring the mixture solution obtained in the step 1 to a 20mL hydrothermal kettle, carrying out hydrothermal reaction at the temperature of 90-110 ℃, controlling the reaction time to be 8-12 h, taking out the graphene composite hydrogel product after the reaction is finished, repeatedly soaking the washing material for 6-10 times by using deionized water, freezing the washing material for 6-12 h at the temperature of-10-20 ℃ in a refrigerator, and finally drying the washing material for 44-48 h at the temperature of-40-60 ℃ in a freeze dryer to obtain the graphene composite aerogel.
And (2) assembling the inert titanium-based ruthenium iridium sheet electrode as an anode and the stainless steel sheet as a cathode with the graphene composite aerogel prepared in the step (2) to form a three-dimensional electrode, placing the three-dimensional electrode in 180mL of organic wastewater with the concentration of 20-50 mg/L, wherein the organic wastewater comprises one of methylene blue solution, rhodamine B solution and phenol solution, the pH range of the solution is 2-9, the concentration of electrolyte anhydrous sodium sulfate is 0.01-0.1 mol/L, and the current density is 1-4 mA/cm2The degradation effect of the organic wastewater was tested.
The invention has the beneficial effects that: a preparation method of graphene composite aerogel for oxidizing organic wastewater by using a three-dimensional electrode comprises the following steps: uniformly mixing graphene oxide, an anionic surfactant and ferrous salt in sequence according to a certain mass ratio, transferring the mixed solution into a hydrothermal kettle for hydrothermal reaction, and finally performing freeze drying to obtain the graphene composite aerogel.
The invention has the following advantages: through the electrostatic interaction between the anionic surfactant and the surface of the graphene oxide, the aggregation between graphene sheet layers and Fe are effectively inhibited2+For graphene oxide in-situ reduction and self oxidation to nano iron oxyhydroxide which is uniformly distributed on the surface of the reduced graphene oxide, a rich and uniform micron-scale pore structure is generated by the double-template effect of anionic surfactant bubbles and frozen ice crystals, so that the graphene composite aerogel is endowed with good mechanical properties and electrocatalytic activity. Three-dimensional electrode is constructed by graphene composite aerogel, and H generated by reduction of iron-based catalyst and cathode in graphene composite aerogel2O2The electro-fenton reaction occurs to improve the efficiency of oxidizing the organic wastewater. The method has the advantages of simple process, simple and easily obtained raw materials, and stable properties of the prepared target material, and is beneficial to practical application.
Drawings
Fig. 1 is a representation of the compressive recoverable elasticity of the graphene composite aerogel material prepared in example 1.
Fig. 2 is a scanning electron microscope image of the pore structure of the graphene composite aerogel prepared in example 2.
Fig. 3 is a scanning electron microscope image of the surface of reduced graphene oxide loaded with nano FeOOH in the graphene composite aerogel prepared in example 2.
Fig. 4 is a performance demonstration of oxidative degradation of methylene blue dye by graphene composite aerogel material prepared in example 4.
Detailed Description
The present invention will be further described with reference to the following examples.
Example 1
Taking 5.15mL of 7mg/mL graphene oxide and 6.85mL deionized water by using a liquid transfer gun, and placing the materials in a beaker for ultrasonic dispersion for 30min to prepare 3mg/mL graphene oxide suspension; then, adding 1mL of 50mg/mL sodium dodecyl sulfate aqueous solution, fully stirring for 30min, controlling the rotating speed of a stirrer at 500r/min, after the mixture is uniformly mixed, adding 1mL of 18mg/mL ferrous sulfate aqueous solution, fully stirring for 2h, controlling the rotating speed of the stirrer at 1600r/min, transferring the mixture into a 20mL hydrothermal kettle, carrying out hydrothermal reaction at the temperature of 100 ℃, controlling the reaction time at 12h, after the reaction is finished, taking out the graphene composite hydrogel, repeatedly soaking and cleaning the graphene composite hydrogel for 8 times by using deionized water, freezing the graphene composite hydrogel in a refrigerator for 8h, controlling the freezing temperature at minus 10-20 ℃, completely freezing the graphene composite hydrogel, and drying the graphene composite aerogel in a freeze dryer for 48h to obtain the target material graphene composite aerogel.
Assembling the prepared graphene composite aerogel into a three-dimensional electrode by taking an inert titanium-based ruthenium electrode, a stainless steel sheet as a cathode and an upper iridium sheet electrode as an anode, placing the three-dimensional electrode into 180mL of 30mg/L rhodamine B solution, wherein the pH of the solution is 7, the concentration of electrolyte anhydrous sodium sulfate is 0.1mol/L, and the current density is 4mA/cm2Under the condition, the degradation rate of the rhodamine B solution in 90min is up to 99.5 percent.
The restorable elasticity of the graphene composite aerogel material upon compression is shown in fig. 1. The graph shows that the graphene composite aerogel is compressed and rebounded under the pressure action of the dip-coating machine, the compression deformation reaches 70% from the original state, and after the pressure is released, the graphene composite aerogel rebounds to the original state basically, so that the graphene composite aerogel has excellent mechanical properties and is beneficial to application in actual water.
Example 2
Taking 5.65mL of 8.5mg/mL graphene oxide and 6.35mL of deionized water by using a liquid transfer gun, and placing the materials in a beaker for ultrasonic dispersion for 30min to prepare 4mg/mL graphene oxide suspension; then, adding 1mL of 60mg/mL sodium dodecyl benzene sulfonate aqueous solution, fully stirring for 30min, controlling the rotating speed of a stirrer at 500r/min, after the mixture is uniformly mixed, adding 0.5mL of 18mg/mL ferrous sulfate aqueous solution, fully stirring for 2h, controlling the rotating speed of the stirrer at 1400r/min, transferring the mixture to a 20mL hydrothermal kettle, carrying out hydrothermal reaction at 100 ℃, controlling the reaction time at 12h, after the reaction is finished, taking out the graphene composite hydrogel, repeatedly soaking and cleaning the graphene composite hydrogel for 6 times by using deionized water, freezing the graphene composite hydrogel in a refrigerator for 12h, controlling the freezing temperature at minus 10-20 ℃, completely freezing the graphene composite aerogel, and drying the graphene composite aerogel in a freeze dryer for 46h to obtain the target material graphene composite aerogel.
Inert titanium-based ruthenium iridium sheet electrode is used as an anode, a stainless steel sheet is used as a cathode, the inert titanium-based ruthenium iridium sheet electrode and the prepared graphene composite aerogel are combined into a three-dimensional electrode, the three-dimensional electrode is placed in 180mL of 20mg/L phenol solution, the pH value of the solution is 5, the electrolyte anhydrous sodium sulfate is 0.05mol/L, and the current density is 2mA/cm2Under the condition (2), the degradation rate of the phenol solution in 120min is as high as 97.6 percent.
Fig. 2 is a scanning electron microscope image of the pore structure of the graphene composite aerogel according to the embodiment, and it can be seen from the image that the composite aerogel has an abundant pore structure, and the diameters of pores are mainly distributed in the range of 3 to 15um, so that the graphene composite aerogel is endowed with good mechanical properties and electrocatalytic activity.
Fig. 3 is a scanning electron microscope image of the surface of reduced graphene oxide loaded with nano FeOOH in the graphene composite aerogel in this embodiment, and it can be seen from the image that nano FeOOH uniformly grows on a graphene sheet layer, and due to the small particle size and uniform distribution, the nano FeOOH can effectively activate H in an electro-fenton reaction2O2Generates rich OH, thereby greatly improving the efficiency of degrading the organic wastewater.
Example 3
8.57mL of 7mg/mL graphene oxide and 3.43mL deionized water are taken by a pipette and placed in a beaker for ultrasonic dispersion for 60min to prepare 5mg/mL graphene oxide suspension; then, adding 1mL of 30mg/mL sodium dodecyl sulfate aqueous solution, fully stirring for 30min, controlling the rotating speed of a stirrer at 500r/min, after the mixture is uniformly mixed, adding 2mL of 9mg/mL ferrous chloride aqueous solution, fully stirring for 2h, controlling the rotating speed of the stirrer at 2400r/min, transferring the mixture into a 20mL hydrothermal kettle, carrying out hydrothermal reaction at the temperature of 100 ℃, controlling the reaction time at 12h, after the reaction is finished, taking out the graphene composite hydrogel, repeatedly soaking and cleaning the graphene composite hydrogel for 8 times by using deionized water, then putting the graphene composite hydrogel into a refrigerator for freezing for 9h, controlling the freezing temperature at minus 10-20 ℃, completely freezing the graphene composite hydrogel, and then putting the graphene composite aerogel into a freeze dryer for drying for 45h to obtain the target material graphene composite aerogel.
Inert titanium-based ruthenium iridium sheet electrode is used as an anode, a stainless steel sheet is used as a cathode, the inert titanium-based ruthenium iridium sheet electrode and the prepared graphene composite aerogel are combined into a three-dimensional electrode, the three-dimensional electrode is placed in 180mL of methylene blue solution with the concentration of 50mg/L, the pH value of the solution is 5, the concentration of electrolyte anhydrous sodium sulfate is 0.1mol/L, and the current density is 1mA/cm2Under the condition, the degradation rate of the methylene blue solution in 90min is up to 99.9 percent.
Example 4
Taking 4.23mL of 8.5mg/mL graphene oxide and 7.77mL deionized water by using a liquid transfer gun, and placing the materials in a beaker for ultrasonic dispersion for 50min to prepare 3mg/mL graphene oxide suspension; then, adding 1mL of 40mg/mL sodium dodecyl sulfate aqueous solution, fully stirring for 30min, controlling the rotating speed of a stirrer at 500r/min, after the mixture is uniformly mixed, adding 2mL of 18mg/mL ferrous sulfate aqueous solution, fully stirring for 2h, controlling the rotating speed of the stirrer at 1400r/min, transferring the mixture into a 20mL hydrothermal kettle, carrying out hydrothermal reaction at the temperature of 100 ℃, controlling the reaction time at 12h, after the reaction is finished, taking out the graphene composite hydrogel, repeatedly soaking and cleaning the graphene composite hydrogel for 6 times by using deionized water, freezing the graphene composite hydrogel in a refrigerator for 8h, controlling the freezing temperature at minus 10-20 ℃, completely freezing the graphene composite hydrogel, and drying the graphene composite aerogel in a freeze dryer for 46h to obtain the target material graphene composite aerogel.
Inert titanium-based ruthenium iridium sheet electrode is used as an anode, a stainless steel sheet is used as a cathode, the inert titanium-based ruthenium iridium sheet electrode and the prepared graphene composite aerogel are combined into a three-dimensional electrode, the three-dimensional electrode is placed in 180mL of methylene blue solution with the concentration of 40mg/L, the pH value of the solution is 3, the concentration of electrolyte anhydrous sodium sulfate is 0.05mol/L, and the current density is 3 mA/cm2Under the condition, the degradation rate of the methylene blue solution in 30min is up to 98 percent.
Fig. 4 shows the performance of the graphene composite aerogel material for oxidative degradation of methylene blue dye, and it can be seen from the graph that the graphene aerogel loaded with iron oxyhydroxide in the embodiment reaches a removal rate of 98% in about 30 min; at 30min, the removal rate of the pure graphene aerogel is only 51%, and 120min is required for achieving the removal rate close to 98%, and the required time is 4 times of the time for aerogel in the embodiment. H generated by reduction of iron-based catalyst and cathode in graphene composite aerogel2O2The efficiency of oxidizing the organic wastewater is improved by the electro-Fenton reaction, and the performance of the aerogel is remarkably improved.
Example 5
3.75mL of 6.4mg/mL graphene oxide and 8.25mL deionized water are taken by a pipette and placed in a beaker for ultrasonic dispersion for 40min to prepare 2mg/mL graphene oxide suspension; then, adding 1mL of a 50mg/mL sodium dodecanesulphonate aqueous solution, fully stirring for 30min, controlling the rotation speed of a stirrer at 500r/min, after the mixture is uniformly mixed, adding 2mL of a 18mg/mL ferrous acetate aqueous solution, fully stirring for 2h, controlling the rotation speed of the stirrer at 1400r/min, transferring the mixture into a 20mL hydrothermal kettle, carrying out hydrothermal reaction at the temperature of 100 ℃, controlling the reaction time at 12h, after the reaction is finished, taking out the graphene composite hydrogel, repeatedly soaking and cleaning the graphene composite hydrogel for 8 times by using deionized water, freezing the graphene composite hydrogel in a refrigerator for 8h, controlling the freezing temperature at minus 10-20 ℃, completely freezing the graphene composite hydrogel, and drying the graphene composite aerogel in a freeze dryer for 48h to obtain the target material graphene composite aerogel.
An inert titanium-based ruthenium iridium sheet electrode is used as an anode, a stainless steel sheet is used as a cathode, the inert titanium-based ruthenium iridium sheet electrode and the prepared graphene composite aerogel are combined into a three-dimensional electrode, the three-dimensional electrode is placed in 180mL of rhodamine B solution with the concentration of 30mg/L, the pH value of the solution is 9, the concentration of electrolyte anhydrous sodium sulfate is 0.05mol/L, and the current density is 3 mA/cm2Under the condition, the degradation rate of the rhodamine B solution within 120min reaches 98.6 percent.
Claims (3)
1. The preparation method of the graphene composite aerogel is characterized by comprising the following steps:
s1, taking 12mL of graphene oxide suspension liquid with the concentration of 2-5 mg/mL, adding 1mL of anionic surfactant aqueous solution with the concentration of 30-60 mg/mL into the graphene oxide suspension liquid, magnetically stirring for 30min, wherein the stirring speed of a magnetic stirrer is 500-800 r/min, after reactants are uniformly mixed, adding 0.25-2 mL of ferrite aqueous solution with the concentration of 9-18 mg/mL, magnetically stirring for 2h, adsorbing ferrous ions on graphene oxide sheet layers through electrostatic attraction, and controlling the speed of the stirrer to be 1400-2400 r/min;
the anionic surfactant comprises at least one of sodium dodecyl sulfate, sodium dodecyl sulfonate and sodium dodecyl benzene sulfonate; the ferrous salt is one or more of ferrous sulfate, ferrous chloride and ferrous acetate;
s2, transferring the mixture solution obtained in the step S1 to a hydrothermal kettle, carrying out hydrothermal reaction at the temperature of 90-110 ℃, controlling the reaction time to be 8-12 h, and after the reaction is finished; taking out the graphene composite hydrogel product, soaking the washing material in deionized water for 6-10 times, and freezing at-10-20 ℃ for 6-12 hours; and finally, drying the graphene composite aerogel in a freeze dryer at the temperature of minus 40-60 ℃ for 44-48 h to obtain the graphene composite aerogel.
2. The application of the aerogel prepared by the graphene composite aerogel preparation method according to claim 1, wherein the application is characterized in that: the graphene composite aerogel is used in three-dimensional electrode oxidation organic wastewater, and the organic wastewater comprises one of methylene blue solution, rhodamine B solution and phenol solution.
3. The application of the aerogel prepared by the graphene composite aerogel preparation method according to claim 2 is characterized in that: the process of using the graphene composite aerogel for oxidizing organic wastewater by the three-dimensional electrode comprises the following steps: an inert titanium-based ruthenium-iridium sheet electrode is used as an anode, a stainless steel sheet is used as a cathode, and the inert titanium-based ruthenium-iridium sheet electrode and graphene composite aerogel are assembled into a three-dimensional electrode; placing the three-dimensional electrode in 180mL of organic wastewater with the concentration of 20-50 mg/L, wherein the pH range of the solution is 2-9, the concentration of electrolyte anhydrous sodium sulfate is 0.01-0.1 mol/L, and the current density is 1-4 mA/cm2The organic wastewater is degraded under the condition (2).
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| CN116873907A (en) * | 2023-07-11 | 2023-10-13 | 中国地质大学（武汉） | Compound high-gas-storage-capacity gas hydrate rapid generation accelerator and preparation method and application thereof |
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