CN112138631A - Preparation method of graphene oxide/activated carbon composite material - Google Patents

Preparation method of graphene oxide/activated carbon composite material Download PDF

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CN112138631A
CN112138631A CN202010707283.9A CN202010707283A CN112138631A CN 112138631 A CN112138631 A CN 112138631A CN 202010707283 A CN202010707283 A CN 202010707283A CN 112138631 A CN112138631 A CN 112138631A
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graphene oxide
mixed solution
stirring
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CN112138631B (en
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李欣
乔骊竹
刘国强
李现化
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Zhongxin Environmental Protection Technology Co ltd
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J20/00Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
    • B01J20/02Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
    • B01J20/20Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising free carbon; comprising carbon obtained by carbonising processes
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2220/00Aspects relating to sorbent materials
    • B01J2220/40Aspects relating to the composition of sorbent or filter aid materials
    • B01J2220/48Sorbents characterised by the starting material used for their preparation
    • B01J2220/4806Sorbents characterised by the starting material used for their preparation the starting material being of inorganic character
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2220/00Aspects relating to sorbent materials
    • B01J2220/40Aspects relating to the composition of sorbent or filter aid materials
    • B01J2220/48Sorbents characterised by the starting material used for their preparation
    • B01J2220/4812Sorbents characterised by the starting material used for their preparation the starting material being of organic character

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Abstract

The invention relates to a preparation method of a graphene oxide/activated carbon composite material, which comprises the following steps: s1, preparing a graphene oxide solution; s2, dropwise adding a polyvinyl alcohol solution to the graphene oxide solution, and stirring for a first preset time to obtain a first mixed solution; s3, adding coconut shell carbon into the first mixed solution, stirring for a second preset time, and standing to obtain a second mixed solution; s4, adding soluble starch, formaldehyde and pentane into the second mixed solution, and fully stirring to obtain a third mixed solution; s5, dropwise adding concentrated sulfuric acid into the third mixed solution, sending the third mixed solution into a drying oven to be cured at a first preset temperature for a third preset time, and washing the cured product for multiple times by using deionized water to obtain the graphene oxide/active carbon composite material. The process for foaming the graphene oxide can avoid stacking of graphene oxide sheets and keep the characteristics of graphene oxide single sheets.

Description

Preparation method of graphene oxide/activated carbon composite material
Technical Field
The invention relates to the field of composite material preparation, in particular to a preparation method of a graphene oxide/activated carbon composite material.
Background
The activated carbon has ultrahigh specific surface area, but the oxygen-containing functional groups on the surface of the activated carbon are limited, and the active sites provided by the activated carbon are also limited; meanwhile, the macropores of the activated carbon provide limited specific surface area.
Graphene has good electrical and mechanical properties, but the graphene is difficult to exist stably due to the characteristic of a two-dimensional structure of the graphene, and the graphene is usually agglomerated. Particularly, the graphene oxide obtained after the graphene lamellar layer is grafted with the oxygen-containing functional group can be stably dispersed in an aqueous solution. However, the solid graphene oxide hardly maintains the characteristics of a single layer.
Therefore, how to combine the activated carbon and the graphene oxide is a problem to be solved urgently.
Disclosure of Invention
The invention aims to provide a preparation method of a graphene oxide/activated carbon composite material, which can obtain a stable graphene oxide/activated carbon composite material.
In order to achieve the above object, the present invention provides a method for preparing a graphene oxide/activated carbon composite material, comprising the following steps:
s1, preparing a graphene oxide solution;
s2, dropwise adding a polyvinyl alcohol solution to the graphene oxide solution, and stirring for a first preset time to obtain a first mixed solution;
s3, adding coconut shell carbon into the first mixed solution, stirring for a second preset time, and standing to obtain a second mixed solution;
s4, adding soluble starch, formaldehyde and pentane into the second mixed solution, and fully stirring to obtain a third mixed solution;
s5, dropwise adding concentrated sulfuric acid into the third mixed solution, sending the third mixed solution into a drying oven to be cured at a first preset temperature for a third preset time, and washing the cured product for multiple times by using deionized water to obtain the graphene oxide/active carbon composite material.
According to an aspect of the invention, in the step S1, the concentration of the graphene oxide in the graphene oxide solution is 1-3 mg/ml.
According to one aspect of the invention, the polyvinyl alcohol solution is prepared by dissolving polyvinyl alcohol in deionized water, and the concentration of the polyvinyl alcohol is 0.03-0.1 g/ml.
According to one aspect of the invention, the first preset time is 0.5-1.5 h.
According to one aspect of the invention, in step S3. The second preset time is 4 hours, and the second mixed solution is obtained after stirring for at least 12 hours after standing.
According to one aspect of the invention, in step S4. The amount of soluble starch added to the second mixed solution is 5-9g, the amount of formaldehyde is 10-12ml, and the amount of pentane is 5-8 ml.
According to an aspect of the present invention, in step S5, concentrated sulfuric acid is dropwise added to the third mixed solution in an amount of 5 to 10 ml.
According to one aspect of the invention, the first preset temperature is 50-70 ℃ and the third preset time is 1-2 h.
According to an aspect of the present invention, the step S1 includes:
s11, preparing a first solution from flake graphite, concentrated sulfuric acid and potassium permanganate, heating the first solution to a second preset temperature, carrying out oxidation reaction for a fourth preset time to obtain a second solution, and dropwise adding deionized water into the second solution according to a first preset addition amount. After the dropwise addition is finished, heating to a third preset temperature, reacting for a fifth preset time, adding deionized water again to terminate the reaction, cooling the reacted solution to room temperature, and dropwise adding hydrogen peroxide until no bubbles are generated and obtaining a third solution;
s12, filtering and washing the third solution until the solution is neutral to obtain a graphite oxide solution, and performing mechanical ultrasonic treatment on the graphite oxide solution to obtain the graphene oxide solution.
10. The method according to claim 9, wherein the step of preparing the first solution with flake graphite, concentrated sulfuric acid and potassium permanganate in step S1 includes:
s111, stirring the crystalline flake graphite in an ice-water bath and adding concentrated sulfuric acid into the crystalline flake graphite;
s112, adding the potassium permanganate into the solution obtained in the step S111, and stirring in an ice-water bath to obtain the first solution.
According to one aspect of the invention, in step S111, the flake diameter of the flake graphite is 5000-325 meshes, and the mass ratio of the flake graphite to the concentrated sulfuric acid is 1:45-1: 55.
According to an aspect of the invention, in step S111, the concentrated sulfuric acid is stirred for 10-30min after the addition is completed.
According to one aspect of the invention, in step S112, the addition rate of the potassium permanganate is 1g/min, and the mass ratio of the crystalline flake graphite to the potassium permanganate is 1:1 to 1: 4.
According to an aspect of the invention, step S112. the potassium permanganate is stirred for 30-60min after the addition is completed.
According to one aspect of the invention, the second preset temperature is 30-40 ℃, and the fourth preset time is 1-3 hours;
the third preset temperature is 70-85 ℃, and the fifth preset time is 30-60 min.
According to one aspect of the present invention, the first predetermined addition amount is 100-.
According to one aspect of the invention, in step S4. And in the step of adding soluble starch, formaldehyde and pentane into the second mixed solution and fully stirring to obtain a third mixed solution, the stirring speed is 350-600 r/min.
According to an aspect of the present invention, in the step of terminating the reaction by adding deionized water again in step S11, the amount of deionized water added is 1 to 1.5L.
According to a scheme of the invention, the process for foaming graphene oxide can avoid the stacking of graphene oxide sheets and keep the characteristics of graphene oxide single sheets.
According to one scheme of the invention, the graphene oxide foam fills gaps of the activated carbon, so that the specific surface area of the activated carbon is increased.
According to one scheme of the invention, the graphene oxide sheet layer has rich oxygen-containing functional groups, and provides more reactive active sites for the graphene oxide/activated carbon composite material.
According to one scheme of the invention, stacking of sheets can occur in the drying process of the graphene oxide, the specific surface area of the material is reduced, the foam structure can avoid the problem, and the graphene oxide with a loose three-dimensional structure can provide a larger specific surface area and abundant reactive sites.
According to one scheme of the invention, the number of oxygen-containing functional groups of the activated carbon is limited, the activated carbon is mainly subjected to pore physical adsorption in the adsorption application process, the adsorption is unstable and easy to desorb, the chemical adsorption ratio is increased by adding the graphene oxide rich in the oxygen-containing functional groups, and the adsorption effect is more stable.
According to one scheme of the invention, the structure of the three-dimensional foam can be influenced by the difference of the sheet diameters of the graphite in the oxidation process, the sheet diameter is large, and the three-dimensional foam structure is loose; the sheet diameter is small, and the three-dimensional foam structure is compact. The tightness and looseness degree of the structure affects the transmission resistance (transmission speed) of a gas phase or a liquid phase in the subsequent adsorption process, the speed of the transmission speed can affect the contact time of a substance to be adsorbed and the graphene oxide/active carbon composite material, and further the sheet diameter of the crystalline flake graphite is optimized and adjusted by adopting the arrangement, so that the adsorption performance of the product is further improved.
In addition, the adjustment of the graphite flake diameter has certain influence on the process, and the concentration and the reaction time of potassium permanganate have little influence on the flake diameter of the graphene oxide. The larger the sheet diameter is, the milder the required oxidation reaction is, and the longer the reaction time is; the sheet diameter is small, and no obvious requirements are made on the oxidation degree and the reaction time. Furthermore, the sheet diameter of the crystalline flake graphite provided by the invention is arranged, so that the production efficiency is improved, the consumption of potassium permanganate is effectively reduced, and the production cost is saved.
According to one scheme of the invention, the graphene oxide/activated carbon composite material has a compact foam structure, a target adsorbate has large resistance through the composite material, the time of passing through an adsorption path is long, the contact time is long, the adsorption is thorough, and the adsorption effect is good.
Drawings
FIG. 1 schematically represents a block diagram of the steps of a manufacturing process according to one embodiment of the invention;
Detailed Description
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings used in the embodiments will be briefly described below. It is obvious that the drawings in the following description are only some embodiments of the invention, and that for a person skilled in the art, other drawings can be derived from them without inventive effort.
In describing embodiments of the present invention, the terms "longitudinal," "lateral," "upper," "lower," "front," "rear," "left," "right," "vertical," "horizontal," "top," "bottom," "inner," "outer," and the like are used in an orientation or positional relationship that is based on the orientation or positional relationship shown in the associated drawings, which is for convenience and simplicity of description only, and does not indicate or imply that the referenced device or element must have a particular orientation, be constructed and operated in a particular orientation, and thus, the above-described terms should not be construed as limiting the present invention.
The present invention is described in detail below with reference to the drawings and the specific embodiments, which are not repeated herein, but the embodiments of the present invention are not limited to the following embodiments.
As shown in fig. 1, according to an embodiment of the present invention, a method for preparing a graphene oxide/activated carbon composite material includes the following steps:
s1, preparing a graphene oxide solution;
s2, dropwise adding a polyvinyl alcohol solution to the graphene oxide solution, and stirring for a first preset time to obtain a first mixed solution;
s3, adding coconut shell charcoal into the first mixed solution, stirring for a second preset time, and standing to obtain a second mixed solution;
s4, adding soluble starch, formaldehyde and pentane into the second mixed solution, and fully stirring to obtain a third mixed solution;
s5, dropwise adding concentrated sulfuric acid into the third mixed solution, sending the third mixed solution into a drying oven to be cured at a first preset temperature for a third preset time, and washing the cured product for multiple times by using deionized water to obtain the graphene oxide/active carbon composite material.
According to an embodiment of the present invention, in the step S1, the concentration of the graphene oxide in the prepared graphene oxide solution is 1-3 mg/ml. Through the arrangement, the method is favorable for ensuring and improving the performance and the quality of the final finished product, and if the conditions are exceeded or fallen below the above conditions, the defect that the finished product is easy to lose efficacy is easily caused.
According to one embodiment of the present invention, in step S2, a polyvinyl alcohol (PVA) solution is prepared by dissolving PVA in deionized water, and the concentration of PVA is 0.03-0.1 g/ml. Through the arrangement, the internal bonding strength of the material is ensured, the internal tiny cracks of the finished product in the subsequent production process are effectively reduced or avoided, the performance and the quality of the final finished product are ensured and improved, and if the internal tiny cracks exceed or are lower than the conditions, the finished product is easy to crack due to excessive cracks.
According to an embodiment of the present invention, in step S1, in the case of stirring the graphene oxide solution obtained in step S1, a polyvinyl alcohol solution is added, and stirring is continued for a first preset time after the addition is completed. In the present embodiment, the first predetermined time is 0.5 to 1.5 hours. By the arrangement, the materials can be fully mixed, the performance and the quality of the final finished product are ensured and improved,
according to one embodiment of the invention, step S3. Adding coconut shell carbon into the first mixed solution, uniformly stirring for a second preset time, stirring for the second preset time, and standing for at least 12 hours to obtain a second mixed solution. In the present embodiment, the second preset time 4 h. The sufficient contact between the solution and the coconut shell carbon is ensured by setting the stirring time and the standing time which are long enough, the good performance of the prepared second mixed solution is ensured,
according to one embodiment of the invention, step S4. The amount of the soluble starch added to the second mixed solution is 5-9g per 100ml of the graphene oxide solution, the amount of the formaldehyde is 10-12ml per 100ml of the graphene oxide solution, and the amount of the pentane is 5-8ml per 100ml of the graphene oxide solution. In the embodiment, after the starch, the formaldehyde and the pentane are added, the mixture is vigorously stirred at the rotating speed of 350-600r/min, so that the mixture can be fully reacted. Through the arrangement, the added materials can be uniformly stirred in a short time, and the performance and the quality of a final finished product are ensured and improved.
According to one embodiment of the present invention, in step S5, concentrated sulfuric acid is added dropwise in an amount of 5 to 10ml to the third mixed solution. In this embodiment, after the addition of the concentrated sulfuric acid is completed, the obtained product is dried and cured in an oven at a first preset temperature and for a third preset time, where the first preset temperature is 50-70 ℃ and the third preset time is 1-2 hours. Through the arrangement, the added materials can be fully reacted, and the method is favorable for ensuring and improving the performance and quality of the final finished product.
According to an embodiment of the present invention, step S1 includes:
s11, preparing a first solution from flake graphite, concentrated sulfuric acid and potassium permanganate, heating the first solution to a second preset temperature, carrying out oxidation reaction for a fourth preset time to obtain a second solution, and dropwise adding deionized water into the second solution according to a first preset adding amount. After the dropwise addition is finished, heating to a third preset temperature, reacting for a fifth preset time, adding deionized water again to terminate the reaction, cooling the reacted solution to room temperature, and dropwise adding hydrogen peroxide until no bubbles are generated and obtaining a third solution; in the present embodiment, the first predetermined addition amount is 100-400 ml.
S12, filtering and washing the third solution until the solution is neutral to obtain a graphite oxide solution, and performing mechanical ultrasonic treatment on the graphite oxide solution to obtain the graphene oxide solution.
According to one embodiment of the present invention, in the step of terminating the reaction by adding deionized water again, the amount of deionized water added is 1 to 1.5L.
According to an embodiment of the present invention, the step of preparing the first solution with flake graphite, concentrated sulfuric acid, and potassium permanganate in step S11 includes:
and S111, stirring the crystalline flake graphite in an ice water bath, and adding concentrated sulfuric acid into the crystalline flake graphite. In the embodiment, the flake diameter of the flake graphite is 5000-325 meshes, and the mass ratio of the flake graphite to concentrated sulfuric acid is 1:45-1: 55. In this embodiment, the concentrated sulfuric acid is stirred for 10-30min after the addition is completed. Through the arrangement, the added materials can be fully reacted, and the method is favorable for ensuring and improving the performance and quality of the final finished product.
And S112, adding potassium permanganate into the solution in the step S111, and stirring in an ice-water bath to obtain a first solution. In the embodiment, the adding speed of the potassium permanganate is 1g/min, and the mass ratio of the crystalline flake graphite to the potassium permanganate is 1:1 to 1: 4. In this embodiment, the potassium permanganate is stirred for 30-60min after addition is complete. Through the arrangement, the added materials can be fully reacted, and the method is favorable for ensuring and improving the performance and quality of the final finished product.
According to an embodiment of the present invention, in the step S11, in the step of heating the first solution to the second predetermined temperature and performing the oxidation reaction for the fourth predetermined time to obtain the second solution, the first solution is slowly heated to the second predetermined temperature, and the second predetermined temperature is 30-40 ℃. And after the temperature rise is finished, keeping the constant temperature for a fourth preset time, wherein the fourth preset time is 1-3 h. In this embodiment, after the second solution is maintained at a constant temperature, 400ml of deionized water with the first predetermined addition amount is slowly added dropwise, and after the water is added, the temperature is raised to the third predetermined temperature, and the constant-temperature stirring is performed for a fifth predetermined time. In this embodiment, the third predetermined temperature is 70-85 deg.C, and the fifth predetermined time is 30-60 min. Through the arrangement, the added materials can be fully reacted, and the method is favorable for ensuring and improving the performance and quality of the final finished product.
To further illustrate the present invention, an example based on the above scheme is illustrated.
Preparation of graphene oxide solution
Selecting 9g of flake graphite with the diameter of 5000-325 meshes as a raw material, adding 240ml of concentrated sulfuric acid into the graphite under the condition of stirring, wherein the mass ratio of the flake graphite to the concentrated sulfuric acid is 1:45-1:55, and then placing reaction equipment into an ice water bath to stir for 10-30min so that the graphite is uniformly dispersed in the concentrated sulfuric acid;
and slowly adding potassium permanganate under the stirring of an ice water bath, wherein the mass ratio of the crystalline flake graphite to the potassium permanganate d is 1:1-1: 4. In the embodiment, the adding speed of the potassium permanganate is 1g/min, and after the potassium permanganate is added, the mixture is stirred for 30-60min in an ice-water bath to completely dissolve the potassium permanganate;
slowly heating to 30-40 ℃, keeping the temperature for 1-3h, slowly dripping 100-400ml of deionized water, heating to 80 ℃ after adding water, stirring at constant temperature for 30min, adding a large amount of deionized water to dilute an acid solution to terminate the reaction, and slowly dripping hydrogen peroxide until no bubbles are generated;
and filtering and washing the solution after the reaction is finished to be neutral to obtain a graphite oxide solution, and then carrying out mechanical ultrasonic treatment to obtain a graphene oxide solution. In the present embodiment, the concentration of the graphene oxide solution is 1 to 3 mg/ml.
Obtaining graphene oxide/activated carbon composite material
Completely dissolving 1-3g of PVA in 30ml of deionized water, dropwise adding the PVA to 100ml of the prepared graphene oxide solution under the condition of stirring, stirring for 0.5-1.5h, then mixing the uniformly mixed solution with coconut shell carbon, standing overnight after stirring for 4h to ensure that the solution is fully contacted with the coconut shell carbon, then adding 5-8g of soluble starch, then adding 10-12ml of formaldehyde and 5-8ml of pentane into the solution, stirring vigorously, dropwise adding 5-10ml of concentrated sulfuric acid after full reaction, and then curing the product in an oven at 60 ℃ for 1.5 h. And finally, washing the composite material by deionized water for 3 times to obtain the graphene oxide/active carbon composite material.
According to the invention, the graphene oxide can be stacked in a drying process, the specific surface area of the material is reduced, the foam structure can avoid the problem, and the graphene oxide with a loose three-dimensional structure can provide a larger specific surface area and abundant reactive sites.
According to the invention, the active carbon has limited oxygen-containing functional groups, mainly adopts porous physical adsorption in the adsorption application process, is unstable in adsorption and easy to desorb, and the addition of graphene oxide rich in oxygen-containing functional groups increases the proportion of chemical adsorption, so that the adsorption effect is more stable.
According to the invention, the structure of the three-dimensional foam can be influenced by the difference of the sheet diameters of the graphite in the oxidation process, the sheet diameter is large, and the three-dimensional foam structure is loose; the sheet diameter is small, and the three-dimensional foam structure is compact. The tightness and looseness degree of the structure affects the transmission resistance (transmission speed) of a gas phase or a liquid phase in the subsequent adsorption process, the speed of the transmission speed can affect the contact time of a substance to be adsorbed and the graphene oxide/active carbon composite material, and further the sheet diameter of the crystalline flake graphite is optimized and adjusted by adopting the arrangement, so that the adsorption performance of the product is further improved.
In addition, the adjustment of the graphite flake diameter has certain influence on the process, and the concentration and the reaction time of potassium permanganate have little influence on the flake diameter of the graphene oxide. The larger the sheet diameter is, the milder the required oxidation reaction is, and the longer the reaction time is; the sheet diameter is small, and no obvious requirements are made on the oxidation degree and the reaction time. Furthermore, the sheet diameter of the crystalline flake graphite provided by the invention is arranged, so that the production efficiency is improved, the consumption of potassium permanganate is effectively reduced, and the production cost is saved.
According to the graphene oxide/activated carbon composite material disclosed by the invention, the foam structure is compact, the resistance of a target adsorbate passing through the composite material is large, the time of passing through an adsorption path is long, the contact time is long, the adsorption is thorough, and the adsorption effect is good.
The foregoing is merely exemplary of particular aspects of the present invention and devices and structures not specifically described herein are understood to be those of ordinary skill in the art and are intended to be implemented in such conventional ways.
The above description is only one embodiment of the present invention, and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims (18)

1. A preparation method of a graphene oxide/activated carbon composite material comprises the following steps:
s1, preparing a graphene oxide solution;
s2, dropwise adding a polyvinyl alcohol solution to the graphene oxide solution, and stirring for a first preset time to obtain a first mixed solution;
s3, adding coconut shell carbon into the first mixed solution, stirring for a second preset time, and standing to obtain a second mixed solution;
s4, adding soluble starch, formaldehyde and pentane into the second mixed solution, and fully stirring to obtain a third mixed solution;
s5, dropwise adding concentrated sulfuric acid into the third mixed solution, sending the third mixed solution into a drying oven to be cured at a first preset temperature for a third preset time, and washing the cured product for multiple times by using deionized water to obtain the graphene oxide/active carbon composite material.
2. The method according to claim 1, wherein in step S1, the concentration of the graphene oxide in the graphene oxide solution is 1 to 3 mg/ml.
3. The preparation method of claim 1, wherein the polyvinyl alcohol solution is prepared by dissolving polyvinyl alcohol in deionized water, and the concentration of the polyvinyl alcohol is 0.03-0.1 g/ml.
4. The method according to claim 3, wherein the first predetermined time is 0.5 to 1.5 hours.
5. The method according to claim 1, wherein in step S3. The second preset time is 4 hours, and the second mixed solution is obtained after stirring for at least 12 hours after standing.
6. The method according to claim 1, wherein in step S4. The amount of soluble starch added to the second mixed solution is 5-9g, the amount of formaldehyde is 10-12ml, and the amount of pentane is 5-8 ml.
7. The production method according to claim 1, wherein in step S5, concentrated sulfuric acid is added dropwise to the third mixed solution in an amount of 5 to 10 ml.
8. The method according to claim 7, wherein the first predetermined temperature is 50-70 ℃ and the third predetermined time is 1-2 hours.
9. The method according to any one of claims 1 to 8, wherein step S1 includes:
s11, preparing a first solution from flake graphite, concentrated sulfuric acid and potassium permanganate, heating the first solution to a second preset temperature, carrying out oxidation reaction for a fourth preset time to obtain a second solution, and dropwise adding deionized water into the second solution according to a first preset addition amount. After the dropwise addition is finished, heating to a third preset temperature, reacting for a fifth preset time, adding deionized water again to terminate the reaction, cooling the reacted solution to room temperature, and dropwise adding hydrogen peroxide until no bubbles are generated and obtaining a third solution;
s12, filtering and washing the third solution until the solution is neutral to obtain a graphite oxide solution, and performing mechanical ultrasonic treatment on the graphite oxide solution to obtain the graphene oxide solution.
10. The method according to claim 9, wherein the step of preparing the first solution with flake graphite, concentrated sulfuric acid and potassium permanganate in step S1 includes:
s111, stirring the crystalline flake graphite in an ice-water bath and adding concentrated sulfuric acid into the crystalline flake graphite;
s112, adding the potassium permanganate into the solution obtained in the step S111, and stirring in an ice-water bath to obtain the first solution.
11. The preparation method according to claim 10, wherein in step S111, the flake graphite has a flake diameter of 5000-325 mesh, and the mass ratio of the flake graphite to the concentrated sulfuric acid is 1:45-1: 55.
12. The method according to claim 11, wherein in step S111, the concentrated sulfuric acid is stirred for 10 to 30min after the addition is completed.
13. The method according to any one of claims 10 to 12, wherein in step S112, the addition rate of the potassium permanganate is 1g/min, and the mass ratio of the crystalline flake graphite to the potassium permanganate is 1:1 to 1: 4.
14. The preparation method according to any one of claims 1 to 3, characterized in that in step S112, the potassium permanganate is stirred for 30-60min after the addition is completed.
15. The method according to claim 14, wherein the second predetermined temperature is 30-40 ℃ and the fourth predetermined time is 1-3 hours;
the third preset temperature is 70-85 ℃, and the fifth preset time is 30-60 min.
16. The method as set forth in claim 15, wherein the first predetermined amount is 400 ml.
17. The method according to claim 1, wherein in step S4. And in the step of adding soluble starch, formaldehyde and pentane into the second mixed solution and fully stirring to obtain a third mixed solution, the stirring speed is 350-600 r/min.
18. The method according to claim 9, wherein in the step of terminating the reaction by adding deionized water again in step S11, the amount of deionized water added is 1 to 1.5L.
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Cited By (2)

* Cited by examiner, † Cited by third party
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CN113000023A (en) * 2021-03-04 2021-06-22 上海晶宇环境工程股份有限公司 Graphene oxide modified activated carbon, preparation method thereof and water treatment method
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