Magnetic photothermal hydrophobic melamine sponge and preparation method and application thereof

Abstract

The application belongs to the field of high polymers, and discloses a magnetic photothermal hydrophobic melamine sponge as well as a preparation method and application thereof. The preparation method is specifically as follows: melamine sponge is soaked in a mixed solution of Fe3O4, gallic acid and FeCl3 for 1h-5h, the adsorbed solution is squeezed and dried at 60 DEG C to obtain a magnetic melamine sponge, then the magnetic melamine sponge is soaked in a pyrrole solution for 30min-2h, the adsorbed solution is squeezed and dried at 60 DEG C to obtain a magnetic photothermal melamine sponge, then the magnetic photothermal melamine sponge is soaked in an octadecyltrichlorosilane alcohol aqueous solution for 1h-5h, the adsorbed solution is squeezed and dried at 60 DEG C to obtain a magnetic photothermal hydrophobic melamine sponge, which has the advantages of simple preparation process, energy saving, green environmental protection and low product cost. The magnetic photothermal hydrophobic melamine sponge can not only effectively separate oil-water mixture under magnetic driving, but also recover high-viscosity oil.

Description

TECHNICAL FIELD

[0001] The application belongs to the technical field of polymers, and relates to a magnetic photothermal hydrophobic melamine sponge as well as a preparation method and application thereof. BACKGROUND

[0002] There is an urgent need for a high-performance oil-water separation material to treat the pollution of water bodies caused by leaked oil and organic reagents. According to the essential phenomenon that oil and water are immiscible, selective separation by a material with special surface wetting properties is an effective method for treating oil pollution. A high-performance separation material needs to meet two conditions, that is, the material needs to have high selectivity to selectively separate and recover oil in an oil-water mixture, and the material needs to have high separation efficiency. Commercial melamine sponge material has a large storage space and is cheap, and can directly absorb leaked oil on the sea surface, and the blocky structure facilitates transportation after oil absorption, so it is the first choice for industrial oil-water separation materials. Therefore, it is necessary to prepare a commercial melamine sponge with simple preparation process, low cost and good oil-water separation performance. SUMMARY

[0003] Therefore, the application provides a magnetic photothermal hydrophobic melamine sponge as well as a preparation method and application thereof. The magnetic photothermal hydrophobic melamine sponge can effectively separate an oil-water mixture under magnetic driving and can recover high-viscosity oil. The magnetic photothermal hydrophobic melamine sponge has the advantages of simple preparation process, energy saving, environmental protection, and low product cost.

[0004] To solve the above problems, the application provides the following technical scheme.

[0005] A preparation method of a magnetic photothermal hydrophobic oil-absorbing melamine sponge, comprising the following steps:

[0006] S1. melamine sponge is soaked in a mixed solution of Fe3O4, gallic acid and FeCl3 for 1h-5h, the adsorbed solution is squeezed out, and the magnetic melamine sponge (Fe-GA-MS) is obtained by drying at 60℃;

[0007] S2. the magnetic melamine sponge is soaked in a pyrrole solution for 30-120min, the adsorbed solution is squeezed out, and the magnetic photothermal melamine sponge (Fe-GA-MS-Pyy-MS) is obtained by drying at 60℃;

[0008] S3. the magnetic photothermal melamine sponge is soaked in an octadecyltrichlorosilane alcohol aqueous solution for 1h-5h, the adsorbed solution is squeezed out, and the magnetic photothermal hydrophobic melamine sponge (Fe-GA-MS-Pyy-OTS-MS) is obtained by drying at 60℃.

[0009] Further, the particle size of the Fe3O4 is 20nm.

[0010] Further, in the mixed solution of Fe3O4, gallic acid and FeCl3, the mass concentration of Fe3O4 is 0.005-0.01 g / mL, the concentration of FeCl3 is 0.01 g / mL-0.1 g / mL, and the concentration of gallic acid is 0.004 g / mL-0.01 g / mL.

[0011] Further, the concentration of the pyrrole solution is 0.008-0.01 g / mL.

[0012] Further, in the aqueous solution of octadecyltrichlorosilane alcohol, the concentration of octadecyltrichlorosilane is 0.02-0.1 g / mL, and the mass ratio of the aqueous alcohol solvent to water is 1:1.

[0013] The application further provides the magnetic photothermal hydrophobic oil-absorbing melamine sponge prepared by the preparation method.

[0014] The application further provides application of the magnetic photothermal hydrophobic oil-absorbing melamine sponge in an oil-water mixture separation material.

[0015] The application further provides application of the magnetic photothermal hydrophobic oil-absorbing melamine sponge in a high-viscosity oil recovery material.

[0016] Compared with the prior art, the application has the following beneficial effects:

[0017] (1) The application utilizes the hydrogen bond effect of melamine sponge and gallic acid to connect gallic acid, and the chelation effect of gallic acid and Fe ions to wrap Fe3O4, so that Fe3O4 is stably combined on the surface of the sponge, and the Fe ions on the sponge can undergo an oxidation-reduction reaction with pyrrole to generate polypyrrole. The polypyrrole has excellent photothermal effect and can directly convert solar light energy into heat energy. The NH bond on the polypyrrole can undergo a hydrolysis-condensation reaction with octadecylchlorosilane to introduce long-chain alkyl groups to form a hydrophobic and oleophilic interface. The selective adsorption of oil and water is realized. The greatest innovation in the application is that Fe ions serve as bridging sites and penetrate between the basic functional layers. The functional layers are combined with each other by chemical bond force, and the performance is better. At the same time, the gallic acid is oxidized and polymerized to form a polygallic acid layer, the pyrrole is polymerized to form a polypyrrole layer, and the octadecylchlorosilane is hydrolyzed and polymerized to form a polysilane layer. The three are connected by hydrogen bonds to form a 3D interpenetrating polymer network, which further improves the mechanical and chemical stability of the target material.

[0018] (2) The chemical reagents involved in the project are common industrialized products and are non-toxic and harmless. The main reagents are derived from the natural environment, are abundant in content, and are low in price. The preparation method of the application does not require heating and does not need complex reaction instruments. The process is simple, green and environmentally friendly, and is more suitable for industrialized production. DETAILED DESCRIPTION

[0019] The technical solutions in the embodiments of the present application will be clearly and completely described below. Obviously, the described embodiments are only some of the embodiments of the present application but not all the embodiments.

[0020] Embodiment 1

[0021] Melamine sponge was soaked in 50 mL of a mixed solution of Fe3O4, gallic acid and FeCl3, wherein the particle size of Fe3O4 was 20 nm, the concentration of Fe3O4 was 0.005 g / mL, the concentration of gallic acid was 0.004 g / mL, the concentration of FeCl3 was 0.01 g / mL, and the soaking time was 1 h. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS. Fe-GA-MS was soaked in 50 mL of a pyrrole solution for 30 min, wherein the concentration of pyrrole in the pyrrole solution was 0.008 g / mL. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS-Pyy-MS. Fe-GA-MS-Pyy-MS was soaked in 50 mL of an octadecyltrichlorosilane alcohol aqueous solution for 1 h, wherein the concentration of octadecyltrichlorosilane was 0.02 g / mL. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS-Pyy-OTS-MS, which was marked as sample 1.

[0022] Embodiment 2

[0023] Melamine sponge was soaked in 50 mL of a mixed solution of Fe3O4, gallic acid and FeCl3, wherein the particle size of Fe3O4 was 20 nm, the concentration of Fe3O4 was 0.01 g / mL, the concentration of gallic acid was 0.004 g / mL, the concentration of FeCl3 was 0.01 g / mL, and the soaking time was 1 h. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS. Fe-GA-MS was soaked in 50 mL of a pyrrole solution for 30 min, wherein the concentration of pyrrole was 0.008 g / mL. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS-Pyy-MS. Fe-GA-MS-Pyy-MS was soaked in 50 mL of an octadecyltrichlorosilane alcohol aqueous solution for 1 h, wherein the concentration of octadecyltrichlorosilane was 0.02 g / mL. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS-Pyy-OTS-MS, which was marked as sample 2.

[0024] Embodiment 3

[0025] Melamine sponge was soaked into 50 mL mixed solution, in which Fe3O4 particle size was 20 nm, concentration was 0.005 g / mL, gallic acid concentration was 0.004 g / mL, FeCl3 concentration was 0.1 g / mL, and the soaking time was 1 h. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS. Fe-GA-MS was soaked into 50 mL pyrrole solution for 30 min, and the concentration of pyrrole was 0.008 g / mL. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS-Pyy-MS. Fe-GA-MS-Pyy-MS was soaked into 50 mL octadecyltrichlorosilane alcohol aqueous solution for 1 h, and the concentration of octadecyltrichlorosilane was 0.02 g / mL. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS-Pyy-OTS-MS, which was marked as sample 3.

[0026] Example 4

[0027] Melamine sponge was soaked into 50 mL mixed solution, in which Fe3O4 particle size was 20 nm, concentration was 0.005 g / mL, gallic acid concentration was 0.01 g / mL, FeCl3 concentration was 0.01 g / mL, and the soaking time was 1 h. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS. Fe-GA-MS was soaked into 50 mL pyrrole solution for 30 min, and the concentration of pyrrole was 0.01 g / mL. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS-Pyy-MS. Fe-GA-MS-Pyy-MS was soaked into 50 mL octadecyltrichlorosilane alcohol aqueous solution for 1 h, and the concentration of octadecyltrichlorosilane was 0.02 g / mL. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS-Pyy-OTS-MS, which was marked as sample 4.

[0028] Example 5

[0029] Melamine sponge was soaked into 50 mL mixed solution, in which Fe3O4 particle size was 20 nm, concentration was 0.005 g / mL, gallic acid concentration was 0.004 g / mL, FeCl3 concentration was 0.01 g / mL, and the soaking time was 1 h. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS. Fe-GA-MS was soaked into 50 mL pyrrole solution for 30 min, and the concentration of pyrrole was 0.008 g / mL. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS-Pyy-MS. Fe-GA-MS-Pyy-MS was soaked into 50 mL octadecyltrichlorosilane alcohol aqueous solution for 1 h, and the concentration of octadecyltrichlorosilane was 0.1 g / mL. The adsorbed solution was squeezed out and dried at 60°C to obtain Fe-GA-MS-Pyy-OTS-MS, which was marked as sample 5.

[0030] Finally, the water and oil (toluene) contact angle of each sample obtained in each embodiment was measured, and the results of the simulated sunlight photothermal measurement are shown in Tables 1 and 2.

[0031] Table 1 Water and oil contact angle of samples of Examples 1-5 and melamine sponge

[0032] Sample 1 2 3 4 5 Melamine sponge Water contact angle (°) 150 153 152 152 151 0 Toluene contact angle (°) 0 0 0 0 0 0

[0033] Table 2 Temperature change (℃) of samples of Examples 1-5 and melamine sponge after simulated sunlight irradiation

[0034] Sample 1 2 3 4 5 Melamine sponge 0 min 27.8 25.6 26.3 24.8 27.1 14 5 min 70.2 69.8 68.9 70.3 70.5 27.8

[0035] According to Table 1, the samples obtained in Examples 1-5 have single selective absorbency for oil and water, i.e. hydrophobic and oleophilic, which indicates that the oil-water mixture can be separated. It is known that the viscosity of oil decreases with increasing temperature, and the difficulty in recovering and separating high-viscosity oil is due to the viscosity problem. In Table 2, the temperature of the modified sponge can be quickly increased under sunlight irradiation, which reduces the viscosity of the oil, and thus high-viscosity oil can be separated and recovered.

Claims

1. A method for preparing a magnetic, photothermal, hydrophobic, and oil-absorbing melamine sponge, characterized in that, Includes the following steps: S1. Melamine sponge was soaked in a mixed solution of Fe3O4, gallic acid, and FeCl3 for 1-5 hours, the adsorbed solution was squeezed out, and dried at 60°C to obtain magnetic melamine sponge; the mass concentration of Fe3O4 in the mixed solution of Fe3O4, gallic acid, and FeCl3 was 0.005-0.01 g / mL, the concentration of FeCl3 was 0.01 g / mL-0.1 g / mL, and the concentration of gallic acid was 0.004 g / mL-0.01 g / mL. S2. Immerse the magnetic melamine sponge in a pyrrole solution for 30-120 minutes, squeeze out the adsorbed solution, and dry at 60°C to obtain a magnetic photothermal melamine sponge. S3. Soak the magnetic photothermal melamine sponge in an octadecyltrichlorosilane alcohol aqueous solution for 1-5 hours, squeeze out the adsorbed solution, and dry at 60°C to obtain a magnetic photothermal hydrophobic melamine sponge.

2. The preparation method according to claim 1, characterized in that, The Fe3O4 has a particle size of 20 nm.

3. The preparation method according to claim 1, characterized in that, The concentration of the pyrrole solution is 0.008~0.01 g / mL.

4. The preparation method according to claim 1, characterized in that, In the octadecyltrichlorosilane aqueous solution, the concentration of octadecyltrichlorosilane is 0.02~0.1 g / mL, and the alcohol-water solvent is ethanol and water in a mass ratio of 1:

1.

5. The magnetic, photothermal, hydrophobic, and oil-absorbing melamine sponge prepared by the preparation method according to any one of claims 1 to 4.

6. The application of the magnetic photothermal hydrophobic oil-absorbing melamine sponge according to claim 5 in oil-water mixture separation materials.

7. The application of the magnetic, photothermal, hydrophobic, and oil-absorbing melamine sponge as described in claim 5 in high-viscosity oil recovery materials.