CN108404689B - Graphene oxide/polyacrylamide composite filter film and preparation and application thereof - Google Patents

Graphene oxide/polyacrylamide composite filter film and preparation and application thereof Download PDF

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CN108404689B
CN108404689B CN201810399585.7A CN201810399585A CN108404689B CN 108404689 B CN108404689 B CN 108404689B CN 201810399585 A CN201810399585 A CN 201810399585A CN 108404689 B CN108404689 B CN 108404689B
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graphene oxide
polyacrylamide
membrane
film
aqueous solution
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CN108404689A (en
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黄林军
王彦欣
程萌萌
唐建国
王瑶
李海东
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Xinhua Shanghai Equipment Co ltd
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Qingdao University
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    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D71/00Semi-permeable membranes for separation processes or apparatus characterised by the material; Manufacturing processes specially adapted therefor
    • B01D71/06Organic material
    • B01D71/58Other polymers having nitrogen in the main chain, with or without oxygen or carbon only
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D67/00Processes specially adapted for manufacturing semi-permeable membranes for separation processes or apparatus
    • B01D67/0079Manufacture of membranes comprising organic and inorganic components
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D69/00Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B01D69/12Composite membranes; Ultra-thin membranes
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00Treatment of water, waste water, or sewage
    • C02F1/44Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00Nature of the contaminant
    • C02F2101/30Organic compounds
    • C02F2101/34Organic compounds containing oxygen
    • CCHEMISTRY; METALLURGY
    • C02TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02FTREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2101/00Nature of the contaminant
    • C02F2101/30Organic compounds
    • C02F2101/38Organic compounds containing nitrogen

Abstract

The invention discloses a graphene oxide/polyacrylamide composite filter film, which is a nano-sized graphene oxide/polyacrylamide composite film with enhanced water flux and filtering performance, prepared by using high-molecular polyacrylamide as a spacer of a graphene oxide lamella; the film has a graphene oxide sheet layer stacking structure, hydrophilic flexible high-molecular polyacrylamide is uniformly attached to the surface of each graphene oxide sheet layer in the structure through electrostatic adsorption, and the composite film comprises the following components in percentage by mass: the graphene oxide accounts for 90% +/-3%, the polyacrylamide accounts for 10% +/-3%, and the molecular weight of the polyacrylamide is 100-300 ten thousand. Experiments prove that the film disclosed by the invention has more excellent hydrophilicity than a graphene oxide film, the interlayer spacing is 0.68nm, and the film has excellent water flux and filtering performance, so that the film is widely applied to preparation of water flux or filtering performance equipment.

Description

Graphene oxide/polyacrylamide composite filter film and preparation and application thereof
Technical Field
The invention belongs to the technical field of inorganic/high-molecular functional materials, and relates to a graphene oxide/polyacrylamide composite filter membrane with enhanced water flux and filtering performance, and preparation and application thereof.
Background
The membrane separation technology plays an important role in water treatment, food processing, chemical industry and pharmaceutical industry. The adoption of materials such as carbon nanotubes, nanoporous graphene, graphene oxide, etc., having nanopores and nanochannels is a new field of research and has great potential. The potential use of these materials for separation has attracted considerable interest to researchers in recent years. Graphene membranes are very promising in the fields of filtration, separation, seawater desalination, biomimetic selective mass transfer mechanism, energy storage and conversion, and the like. Graphene oxide has also received great attention as a derivative of graphene.
Due to the two-dimensional structure and adjustable physicochemical properties of the graphene oxide, the graphene oxide has the function of screening by superposing graphene oxide lamella. The graphene oxide film is prepared by vacuum filtration, layer-by-layer assembly, spraying or spin coating and other methods. The sheets of graphene oxide have the ability to permeate water, selectively reject other species, and form unique two-dimensional nanochannels.
By adjusting the physical and chemical properties of the nano-pores and the number of layers of the graphene film, the required membrane flux ideal for various gases and liquids can be obtained. Small inter-lamellar spacing can be achieved by reducing the graphene oxide partially to reduce the size of the hydrated functional groups or stacking graphene oxide nanoplatelets via small molecular covalent bonds to overcome the hydration forces. Instead, the distance between the sheets can be increased by inserting large, rigid chemical groups or soft polymer chains, even larger sized nanoparticles or nanofibers being used as spacers.
The nano-sized graphene oxide and polyacrylamide composite film with the filtering function and the preparation method and application thereof are not reported by retrieval by using polyacrylamide with positive charges as a spacer of a graphene oxide lamella.
Disclosure of Invention
Aiming at the defects of the prior art, the invention aims to provide a graphene oxide/polyacrylamide composite filter membrane and preparation and application thereof.
The graphene oxide/polyacrylamide composite filter film is a nano-sized graphene oxide/polyacrylamide composite filter film with enhanced water flux and filtering performance, which is prepared by using high-molecular polyacrylamide as a spacer of a graphene oxide sheet layer; the method is characterized in that: the composite film has a graphene oxide sheet layer stacking structure, hydrophilic flexible high-molecular polyacrylamide is uniformly attached to the surface of each graphene oxide sheet layer in the structure through electrostatic adsorption, and the composite film comprises the following components in percentage by mass: the graphene oxide accounts for 90% +/-3%, the polyacrylamide accounts for 10% +/-3%, the molecular weight of the polyacrylamide is 100-300 ten thousand, the interlayer spacing of graphene oxide sheets in the composite film structure can be influenced by changing the addition amount of the polyacrylamide, and if the addition amount of the polyacrylamide is increased, the interlayer spacing of the graphene oxide sheets is increased.
In the above graphene oxide/polyacrylamide composite filter membrane: the graphene oxide/polyacrylamide composite filter membrane preferably comprises the following components in percentage by mass: 90% of graphene oxide, 10% of polyacrylamide and 100-200 million of polyacrylamide molecular weight; the interlayer spacing of the graphene oxide/polyacrylamide composite filter film is 0.68 nm; the contact angle between the graphene oxide/polyacrylamide composite filter membrane and water is 65.1 degrees.
The interlayer spacing (nanochannel) of the graphene oxide/polyacrylamide composite filter membrane was determined by XRD.
The preparation method of the graphene oxide/polyacrylamide composite filter membrane comprises the following steps:
(1) preparing a graphene oxide aqueous solution with the concentration of 0.5-1 mg/mL, and ultrasonically dispersing until the graphene oxide aqueous solution is uniform;
(2) preparing polyacrylamide aqueous solution with the concentration of 0.05 mg/mL-0.1 mg/mL and the molecular weight of 100-300 ten thousand, and stirring at room temperature until the polyacrylamide aqueous solution is completely dissolved;
(3) dropwise adding the polyacrylamide aqueous solution prepared in the step (2) into the graphene oxide aqueous solution prepared in the step (1) under the stirring condition, wherein the mass percentage of graphene oxide and polyacrylamide is as follows: the graphene oxide accounts for 90% +/-3%, and the polyacrylamide accounts for 10% +/-3%, so that a graphene oxide/polyacrylamide compound is obtained;
(4) carrying out suction filtration on the graphene oxide/polyacrylamide compound by a vacuum filtration method to form a membrane, and naturally drying the membrane to obtain the graphene oxide/polyacrylamide compound filter membrane; the graphene oxide/polyacrylamide composite filtering films prepared by taking different suction filtration amounts of graphene oxide/polyacrylamide composites have different thicknesses, and the thickness of the formed film is larger when the suction filtration amount is larger.
Further, the preferable steps of the preparation method of the graphene oxide/polyacrylamide composite filter membrane are as follows:
(1) preparing a graphene oxide aqueous solution with the concentration of 0.5, and ultrasonically dispersing until the graphene oxide aqueous solution is uniform;
(2) preparing 0.05mg/mL polyacrylamide aqueous solution with the molecular weight of 100-200 ten thousand, and stirring at room temperature until the polyacrylamide aqueous solution is completely dissolved;
(3) dropwise adding the polyacrylamide aqueous solution prepared in the step (2) into the graphene oxide aqueous solution prepared in the step (1) under the stirring condition, stirring for 2 hours, uniformly mixing, and enabling the mass percentages of the graphene oxide and the polyacrylamide to be as follows: 90% of graphene oxide and 10% of polyacrylamide to obtain a graphene oxide/polyacrylamide compound;
(4) and (3) filtering 10mL of the graphene oxide/polyacrylamide compound to form a membrane by a vacuum filtration method, and naturally drying the membrane to obtain the graphene oxide/polyacrylamide compound filter membrane.
The graphene oxide/polyacrylamide composite filtering film disclosed by the invention is applied to preparation of equipment with water flux or filtering performance.
According to the invention, the graphene oxide with negative charges and the polyacrylamide with positive charges are combined through electrostatic adsorption to obtain a graphene oxide-polyacrylamide colloidal solution, and then the quantitative colloidal solution is prepared into the composite film through vacuum filtration. The experiment proves that: the contact angle between the graphene oxide filtering membrane and water is 78.1 degrees, the contact angle between the reduced graphene oxide filtering membrane and water is 110.5 degrees, and the hydrophilicity of the graphene oxide/polyacrylamide composite filtering membrane is superior to that of the graphene oxide/polyacrylamide composite filtering membrane and is 65.1 degrees. According to XRD test analysis, the interlayer spacing of the graphene oxide filtering membrane is about 0.85nm, the interlayer spacing of the reduced graphene oxide filtering membrane is 0.36nm, and the interlayer spacing of the graphene oxide/polyacrylamide composite filtering membrane is 0.68nm, so that the defects of the surface of the graphene oxide are filled up by flexible polyacrylamide molecules under the action of pressure.
The prepared film is subjected to performance tests of water flux and rhodamine B rejection rate, and the water flux test results of different samples show that the water flux of the reduced graphene oxide filtering membrane is the minimum, the water flux of the graphene oxide filtering membrane is the maximum, and the water flux of the graphene oxide/polyacrylamide composite filtering film is between the water flux of the graphene oxide filtering membrane and the water flux of the reduced graphene oxide filtering membrane under the same sample volume, so that polyacrylamide plays a certain role between graphene oxide sheet layers. Also, the larger the volume of the solution used, i.e., the larger the membrane thickness, the smaller the water flux for the same sample. The result of the retention rate test of different samples on rhodamine B shows that compared with the reduced graphene oxide filter membrane, the graphene oxide/polyacrylamide composite filter membrane has weaker retention capacity on rhodamine B; the rejection for rhodamine B increases with increasing volume of solution, i.e., the thickness of the film, for the same sample. The addition of polyacrylamide changes the interlayer spacing of the graphene oxide filtering membrane, shows different water fluxes and rhodamine B retention rates, and has a wide application prospect in preparation of water flux or filtering performance equipment in a prediction period.
The invention provides a graphene oxide/polyacrylamide composite filter membrane and preparation and application thereof. The nano-sized graphene oxide and polyacrylamide composite film with the filtering function is prepared by taking polyacrylamide with the molecular weight of 100-300 ten thousand as a spacer of a graphene oxide lamella. According to the preparation method of the nano-sized polyacrylamide and graphene oxide composite film, graphene oxide with negative charges and polyacrylamide with positive charges are combined through electrostatic adsorption to obtain a graphene oxide-polyacrylamide colloidal solution, and then the graphene oxide-polyacrylamide colloidal solution is prepared into the composite film through vacuum filtration. According to the invention, the polyacrylamide is added as a graphene oxide interlayer spacer to increase the interlayer spacing, so that selective filtration of some substances is realized, and finally the graphene oxide/polyacrylamide composite film is obtained.
The method has the advantages that after the graphene oxide/polyacrylamide composite solution is obtained, the graphene oxide/polyacrylamide composite film is obtained by directly utilizing vacuum filtration, the whole preparation process is green and pollution-free, the film has excellent filtering performance, and particularly has higher rejection rate for rhodamine B. The graphene oxide/polyacrylamide composite filtering film disclosed by the invention is expected to be widely applied to preparation of equipment with water flux or filtering performance.
Drawings
FIG. 1: is an SEM of the graphene oxide/polyacrylamide composite filter membrane prepared in example 1; as can be seen from the figure, the polyacrylamide is distributed more uniformly on the graphene oxide sheets (a), and the composite filter membrane exhibits a layer-by-layer stacked structure (b).
FIG. 2: FE-SEM pictures of the graphene oxide filtration membrane (a), the reduced graphene oxide filtration membrane (b), and the graphene oxide/polyacrylamide composite filtration membrane (c) prepared in example 2; as can be seen from fig. 2(a), 2(b) and 2(c), the tightness of the various filter membrane layer-by-layer stacks varies.
Fig. 3 is a contact angle picture of three different filter film samples, namely, a graphene oxide filter film (a), a reduced graphene oxide filter film (b) and a graphene oxide/polyacrylamide composite filter film (c), wherein it can be seen from the picture that the contact angle of the graphene oxide/polyacrylamide composite filter film is the smallest, which indicates that the composite filter film has the best hydrophilicity.
FIG. 4 is an XRD test chart of three different samples, from which it can be seen that the characteristic peak position of XRD is shifted, and the interlayer spacing of the graphene oxide/polyacrylamide composite filter membrane is about 0.68nm as calculated by Bragg equation.
Fig. 5 shows the results of thermogravimetric analysis of the graphene oxide/polyacrylamide composite filter membrane, and it can be seen from the graph that the thermal decomposition of polyacrylamide molecules in the graphene oxide/polyacrylamide composite filter membrane starts at about 450 ℃ and ends at 700 ℃, which illustrates that the presence of graphene oxide has a certain protection effect on polyacrylamide, and thus the thermal stability of the composite filter membrane is increased.
FIG. 6 is a graph showing the results of water flux tests on different samples
As can be seen from the figure, the water flux of the reduced graphene oxide filtration membrane is the smallest, the water flux of the graphene oxide filtration membrane is the largest, and the water flux of the graphene oxide/polyacrylamide composite filtration membrane is between the two, which indicates that polyacrylamide plays a role between graphene oxide sheets. Also, the larger the volume of the solution used, i.e., the larger the membrane thickness, the smaller the water flux for the same sample.
FIG. 7 is a graph showing the results of retention tests for different samples
As can be seen from the figure, compared with the reduced graphene oxide filter membrane, the graphene oxide/polyacrylamide composite filter membrane has weaker retention capacity on rhodamine B; the rejection for rhodamine B increases with increasing volume of solution, i.e., the thickness of the film, for the same sample.
Detailed Description
Example 1
(1) Dissolving 50mg of graphene oxide in 100mL of distilled water to prepare a graphene oxide aqueous solution with the concentration of 0.5mg/mL, and performing ultrasonic dispersion until the graphene oxide aqueous solution is uniform;
(2) dissolving 5mg of polyacrylamide with the molecular weight of 100 ten thousand in 100mL of distilled water to prepare a polyacrylamide aqueous solution with the concentration of 0.05mg/mL, and stirring until the polyacrylamide aqueous solution is completely dissolved;
(3) dropwise adding the polyacrylamide aqueous solution obtained in the step (2) into the graphene oxide aqueous solution obtained in the step (1) under the stirring condition, and stirring for 2 hours to uniformly mix;
(4) and after the mixture is uniformly mixed, measuring a 10mL sample of the graphene oxide/polyacrylamide composite solution, carrying out suction filtration to form a membrane by adopting a vacuum filtration method, and naturally drying the membrane to obtain the graphene oxide/polyacrylamide composite film.
Fig. 1 is an SEM of the composite film of example 1, and it can be seen from fig. 1(a) that polyacrylamide is uniformly distributed on the surface of graphene oxide.
FIG. 1(b) is a cross-sectional view of a composite film, which is a multi-layer structure, as can be seen, with a large amount of polyacrylamide between the layers.
Fig. 5 is a thermogravimetric analysis diagram of the composite membrane, and it can be seen from the diagram that the thermal decomposition of polyacrylamide molecules in the graphene oxide/polyacrylamide composite filter membrane starts at about 450 ℃ and ends at 700 ℃, which illustrates that the existence of graphene oxide has a certain protection effect on polyacrylamide, so that the thermal stability of the composite filter membrane is increased.
Example 2
Firstly, dissolving 25mg of freeze-dried graphene oxide powder in 100mL of distilled water, and performing ultrasonic dispersion to prepare a graphene oxide aqueous solution with the concentration of 0.25 mg/mL; then transferring the solution into a 100mL three-neck flask and stirring, transferring 25uL of 35% hydrazine hydrate solution by using a liquid transfer gun, and dropwise adding the hydrazine hydrate solution into the three-neck flask; after stirring uniformly, dropwise adding an ammonia water solution with the mass fraction of 28%, and adjusting the pH of the reaction system to 10; finally, the temperature of the reaction system was raised to 90 ℃ and reacted at this temperature for 2 hours. Measuring 10mL of different solution samples with the same concentration, performing suction filtration to form a membrane by adopting a vacuum suction filtration method, and naturally drying the membrane to obtain a graphene oxide filter membrane, a reduced graphene oxide filter membrane and a graphene oxide/polyacrylamide composite filter membrane.
FIG. 2 is an FE-SEM photograph of different membranes of example 2. As can be seen from FIG. 3, the tightness of the stacking of the various filtration membranes is different from that of FIG. 2(a), FIG. 2(b) and FIG. 2 (c).
Fig. 3 is a contact angle graph of different membranes of example 2, and it can be seen from the graph that the contact angle between the graphene oxide filtration membrane and water is 78.1 ° (a), the contact angle between the reduced graphene oxide filtration membrane and water is 110.5 ° (b), and the contact angle between the graphene oxide/polyacrylamide composite filtration membrane is 65.1 ° (c), which illustrates that the composite filtration membrane has the best hydrophilicity.
Fig. 4 is an XRD test chart of different films of example 2, from which it can be seen that characteristic peak positions of XRD are shifted, and it can be known from the calculation of bragg equation that the interlayer spacing of the graphene oxide/polyacrylamide composite filter film is about 0.68nm, and the interlayer spacing of the reduced graphene oxide filter film is the smallest, which is 0.36 nm.
Example 3
(1) Dissolving graphene oxide in distilled water to prepare a graphene oxide aqueous solution, and ultrasonically dispersing until the graphene oxide aqueous solution is uniform;
(2) dissolving polyacrylamide in distilled water to prepare a polyacrylamide aqueous solution, and stirring until the polyacrylamide aqueous solution is completely dissolved;
(3) dropwise adding the polyacrylamide aqueous solution obtained in the step (2) into the graphene oxide aqueous solution obtained in the step (1) under the stirring condition, and stirring for 2 hours to uniformly mix;
(4) and after the mixture is uniformly mixed, measuring a 10mL sample of the graphene oxide/polyacrylamide composite solution, carrying out suction filtration to form a membrane by adopting a vacuum filtration method, and naturally drying the membrane to obtain the graphene oxide/polyacrylamide composite film.
(5) And then preparing a reduced graphene oxide solution with the concentration of 0.25mg/mL and a graphene oxide solution with the concentration of 0.25mg/mL, and performing vacuum filtration on the equal-volume solution to form a film for comparison.
(6) And (3) carrying out performance tests on the water flux and the rhodamine B rejection rate of the prepared film.
Wherein: the concentration of the graphene oxide in the step (1) is 0.5 mg/mL; the molecular weight of the polyacrylamide in the step (2) is 100 ten thousand, and the concentration is 0.05 mg/mL; mixing the equal volume of the graphene oxide aqueous solution and the polyacrylamide aqueous solution, wherein the concentration of the graphene oxide in the mixed solution is 0.25 mg/mL; the volumes of the graphene oxide aqueous solution used for suction filtration in the steps (4) and (5), the reduced graphene oxide aqueous solution and the graphene oxide/polyacrylamide composite solution are respectively 1.0mL, 2.0mL, 3.0mL, 4.0mL, 5.0mL, 6.0mL, 7.0mL, 8.0mL, 9.0mL and 10.0 mL.
TABLE 1 Water flux test results for different samples
Figure BDA0001645389660000051
Water flux testing of different volumes of sample:
FIG. 6 is a graph showing the results of water flux tests on samples of different volumes, wherein the pure water flux and the thickness of the filtration membrane are in negative correlation regardless of the graphene oxide filtration membrane, the graphene filtration membrane or the GO/PAM filtration membrane, and the pure water flux is increased when the volume of the aqueous solution used as the membrane is smaller and the thickness of the filtration membrane is smaller; when the volume of the aqueous solution used for the filtration membrane is larger, the thickness of the filtration membrane is also larger, and the corresponding pure water flux is smaller. And it is easy to find from the figure that when the amount of the aqueous solution is higher than a certain value, i.e. after the membrane reaches a certain thickness, the pure water flux of the membrane is maintained at a lower value and does not decrease with the increase of the membrane thickness.
Under the condition that the using amount of the aqueous solution is certain, namely when the thicknesses of the filtering membranes are the same, the pure water flux of the graphene oxide filtering membrane is greater than that of the GO/PAM filtering membrane and is greater than that of the graphene. The interlayer spacing of the filtering membrane is determined, and a large number of oxygen-containing groups are arranged on the surface of the graphene oxide, so that the interlayer spacing of the obtained filtering membrane is large, and a channel which is beneficial to pure water to pass is formed; most of oxygen-containing groups on the surface of the graphene are reduced, so that the obtained filtering membrane has a tighter structure and smaller interlayer spacing, and channels for pure water to pass through are reduced; in the GO/PAM filtering membrane, due to the flexibility of polyacrylamide, partial chain segments of the polyacrylamide enter a channel formed by stacking graphene oxide, and the pure water flux of the GO/PAM filtering membrane is also reduced. And the results of the test of pure water fluxes of the different filtration membranes also match those of the X-ray diffraction of FIG. 4.
Table 2. result of retention rate test of different samples on rhodamine B
Figure BDA0001645389660000061
The retention rate of rhodamine B by samples of different volumes was tested:
FIG. 7 is a picture of the result of the rhodamine B retention rate test of samples with different volumes, and it can be seen from FIG. 7 that the retention rate is in positive correlation with the thickness of the filter membrane, that is, the rhodamine B molecule retention efficiency is higher and higher with the increase of the thickness of the filter membrane. And when the thickness of the filtering membrane reaches a certain value, the interception effect of the filtering membrane on rhodamine B molecules tends to be stable, the interception rate is stabilized between 98% and 99%, and when the thickness of the filtering membrane is increased, the interception rate is not changed.
For different types of filtering membranes with the same thickness, the interception effect of the graphene filtering membrane on rhodamine B molecules is obviously higher than that of a GO/PAM filtering membrane and that of a graphene oxide filtering membrane, and the main reason is that the interlayer spacing of the different filtering membranes is different. For example, when the dosage of the aqueous solution is 2ml (the concentration is 0.1mg/ml), the interception rate of the graphene filtering membrane on rhodamine B molecules is the highest and reaches 97.06%, the interception rate of the GO/PAM filtering membrane on rhodamine B molecules is the second order and is about 95.43%, and the interception rate of the graphene oxide filtering membrane on rhodamine B molecules is the smallest and is 85.03%.

Claims (1)

1. The application of the graphene oxide/polyacrylamide composite filter membrane in the preparation of equipment with filtering performance is characterized in that: the composite filtering film has a graphene oxide sheet layer stacking structure, hydrophilic flexible high-molecular polyacrylamide is uniformly attached to the surface of each graphene oxide sheet layer in the structure through electrostatic adsorption, and the composite filtering film comprises the following components in percentage by mass: 90% of graphene oxide, 10% of polyacrylamide and 100-200 million of polyacrylamide molecular weight; the interlayer spacing of the graphene oxide/polyacrylamide composite filter film is 0.68 nm; the contact angle between the graphene oxide/polyacrylamide composite filter membrane and water is 65.1 degrees; the graphene oxide/polyacrylamide composite filter membrane is prepared by the following preparation method:
(1) preparing a graphene oxide aqueous solution with the concentration of 0.5mg/mL, and ultrasonically dispersing until the graphene oxide aqueous solution is uniform;
(2) preparing 0.05mg/mL polyacrylamide aqueous solution with the molecular weight of 100-200 ten thousand, and stirring at room temperature until the polyacrylamide aqueous solution is completely dissolved;
(3) dropwise adding the polyacrylamide aqueous solution prepared in the step (2) into the graphene oxide aqueous solution prepared in the step (1) under the stirring condition, stirring for 2 hours, uniformly mixing, and enabling the mass percentages of the graphene oxide and the polyacrylamide to be as follows: 90% of graphene oxide and 10% of polyacrylamide to obtain a graphene oxide/polyacrylamide compound;
(4) and (3) filtering 10mL of the graphene oxide/polyacrylamide compound to form a membrane by a vacuum filtration method, and naturally drying the membrane to obtain the graphene oxide/polyacrylamide compound filter membrane.
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CN109758926B (en) * 2018-10-31 2022-02-11 浙江工业大学 Functionalized graphene-based nanofiltration membrane as well as preparation method and application thereof
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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102145305A (en) * 2011-04-08 2011-08-10 南京航空航天大学 Method for preparing graphene-loaded nano alloy catalyst
WO2015042583A3 (en) * 2013-09-23 2015-05-14 Anand Srinivasan Systems, devices, & methods for microbial detection & identification, and antimicrobial susceptibility testing
CN107261859A (en) * 2017-06-22 2017-10-20 浙江工业大学 A kind of preparation method of graphene oxide/polymer solvent-resistant compound nanofiltration membrane

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102145305A (en) * 2011-04-08 2011-08-10 南京航空航天大学 Method for preparing graphene-loaded nano alloy catalyst
WO2015042583A3 (en) * 2013-09-23 2015-05-14 Anand Srinivasan Systems, devices, & methods for microbial detection & identification, and antimicrobial susceptibility testing
CN107261859A (en) * 2017-06-22 2017-10-20 浙江工业大学 A kind of preparation method of graphene oxide/polymer solvent-resistant compound nanofiltration membrane

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