CN111889042A - Preparation method of magnetic graphene-based aerogel with photocatalytic function - Google Patents
Preparation method of magnetic graphene-based aerogel with photocatalytic function Download PDFInfo
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- CN111889042A CN111889042A CN202010908333.XA CN202010908333A CN111889042A CN 111889042 A CN111889042 A CN 111889042A CN 202010908333 A CN202010908333 A CN 202010908333A CN 111889042 A CN111889042 A CN 111889042A
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- based aerogel
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- photocatalytic function
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 105
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 105
- 239000004964 aerogel Substances 0.000 title claims abstract description 64
- 230000001699 photocatalysis Effects 0.000 title claims abstract description 46
- 238000002360 preparation method Methods 0.000 title claims abstract description 44
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 34
- 229910052742 iron Inorganic materials 0.000 claims abstract description 15
- 239000000463 material Substances 0.000 claims abstract description 14
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 claims description 37
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- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 26
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 24
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 claims description 21
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 claims description 16
- 239000011259 mixed solution Substances 0.000 claims description 16
- 239000000725 suspension Substances 0.000 claims description 14
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 claims description 13
- 229960002089 ferrous chloride Drugs 0.000 claims description 13
- NMCUIPGRVMDVDB-UHFFFAOYSA-L iron dichloride Chemical compound Cl[Fe]Cl NMCUIPGRVMDVDB-UHFFFAOYSA-L 0.000 claims description 13
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- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 9
- GSEJCLTVZPLZKY-UHFFFAOYSA-N Triethanolamine Chemical compound OCCN(CCO)CCO GSEJCLTVZPLZKY-UHFFFAOYSA-N 0.000 claims description 9
- 239000012286 potassium permanganate Substances 0.000 claims description 9
- 229910052979 sodium sulfide Inorganic materials 0.000 claims description 9
- GRVFOGOEDUUMBP-UHFFFAOYSA-N sodium sulfide (anhydrous) Chemical compound [Na+].[Na+].[S-2] GRVFOGOEDUUMBP-UHFFFAOYSA-N 0.000 claims description 9
- 229910000033 sodium borohydride Inorganic materials 0.000 claims description 8
- 239000012279 sodium borohydride Substances 0.000 claims description 8
- 239000003381 stabilizer Substances 0.000 claims description 8
- 238000001035 drying Methods 0.000 claims description 7
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- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 6
- 239000007788 liquid Substances 0.000 claims description 6
- 230000007935 neutral effect Effects 0.000 claims description 6
- IEQIEDJGQAUEQZ-UHFFFAOYSA-N phthalocyanine Chemical compound N1C(N=C2C3=CC=CC=C3C(N=C3C4=CC=CC=C4C(=N4)N3)=N2)=C(C=CC=C2)C2=C1N=C1C2=CC=CC=C2C4=N1 IEQIEDJGQAUEQZ-UHFFFAOYSA-N 0.000 claims description 6
- VWDWKYIASSYTQR-UHFFFAOYSA-N sodium nitrate Inorganic materials [Na+].[O-][N+]([O-])=O VWDWKYIASSYTQR-UHFFFAOYSA-N 0.000 claims description 6
- NTZMSBAAHBICLE-UHFFFAOYSA-N 4-nitrobenzene-1,2-dicarbonitrile Chemical compound [O-][N+](=O)C1=CC=C(C#N)C(C#N)=C1 NTZMSBAAHBICLE-UHFFFAOYSA-N 0.000 claims description 5
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- QAOWNCQODCNURD-UHFFFAOYSA-N sulfuric acid Substances OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 5
- 238000001782 photodegradation Methods 0.000 claims description 4
- 229920000036 polyvinylpyrrolidone Polymers 0.000 claims description 4
- 239000001267 polyvinylpyrrolidone Substances 0.000 claims description 4
- 235000013855 polyvinylpyrrolidone Nutrition 0.000 claims description 4
- 238000009210 therapy by ultrasound Methods 0.000 claims description 4
- 229910021642 ultra pure water Inorganic materials 0.000 claims description 4
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- VSTXCZGEEVFJES-UHFFFAOYSA-N 1-cycloundecyl-1,5-diazacycloundec-5-ene Chemical compound C1CCCCCC(CCCC1)N1CCCCCC=NCCC1 VSTXCZGEEVFJES-UHFFFAOYSA-N 0.000 claims description 3
- 229910052757 nitrogen Inorganic materials 0.000 claims description 3
- 238000010992 reflux Methods 0.000 claims description 3
- 239000002904 solvent Substances 0.000 claims description 3
- 229910006297 γ-Fe2O3 Inorganic materials 0.000 claims description 3
- DBMJMQXJHONAFJ-UHFFFAOYSA-M Sodium laurylsulphate Chemical compound [Na+].CCCCCCCCCCCCOS([O-])(=O)=O DBMJMQXJHONAFJ-UHFFFAOYSA-M 0.000 claims description 2
- 229920002125 Sokalan® Polymers 0.000 claims description 2
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- 238000002156 mixing Methods 0.000 claims description 2
- 239000004584 polyacrylic acid Substances 0.000 claims description 2
- 238000002390 rotary evaporation Methods 0.000 claims description 2
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 claims 3
- 238000005057 refrigeration Methods 0.000 claims 3
- KMHSUNDEGHRBNV-UHFFFAOYSA-N 2,4-dichloropyrimidine-5-carbonitrile Chemical compound ClC1=NC=C(C#N)C(Cl)=N1 KMHSUNDEGHRBNV-UHFFFAOYSA-N 0.000 claims 1
- ZCHPKWUIAASXPV-UHFFFAOYSA-N acetic acid;methanol Chemical compound OC.CC(O)=O ZCHPKWUIAASXPV-UHFFFAOYSA-N 0.000 claims 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims 1
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- 229910052760 oxygen Inorganic materials 0.000 claims 1
- 239000002994 raw material Substances 0.000 claims 1
- FMMWHPNWAFZXNH-UHFFFAOYSA-N Benz[a]pyrene Chemical compound C1=C2C3=CC=CC=C3C=C(C=C3)C2=C2C3=CC=CC2=C1 FMMWHPNWAFZXNH-UHFFFAOYSA-N 0.000 abstract description 33
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- 230000000694 effects Effects 0.000 abstract description 4
- 238000011068 loading method Methods 0.000 abstract description 2
- 238000007885 magnetic separation Methods 0.000 abstract description 2
- 238000007112 amidation reaction Methods 0.000 abstract 1
- 239000006249 magnetic particle Substances 0.000 abstract 1
- 239000000126 substance Substances 0.000 description 14
- 238000012360 testing method Methods 0.000 description 13
- 229910001566 austenite Inorganic materials 0.000 description 10
- NUJOXMJBOLGQSY-UHFFFAOYSA-N manganese dioxide Chemical compound O=[Mn]=O NUJOXMJBOLGQSY-UHFFFAOYSA-N 0.000 description 8
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 6
- UFWIBTONFRDIAS-UHFFFAOYSA-N Naphthalene Chemical compound C1=CC=CC2=CC=CC=C21 UFWIBTONFRDIAS-UHFFFAOYSA-N 0.000 description 6
- 238000002347 injection Methods 0.000 description 6
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- 239000011702 manganese sulphate Substances 0.000 description 3
- 235000007079 manganese sulphate Nutrition 0.000 description 3
- SQQMAOCOWKFBNP-UHFFFAOYSA-L manganese(II) sulfate Chemical compound [Mn+2].[O-]S([O-])(=O)=O SQQMAOCOWKFBNP-UHFFFAOYSA-L 0.000 description 3
- 238000000926 separation method Methods 0.000 description 3
- 206010007269 Carcinogenicity Diseases 0.000 description 2
- 230000000711 cancerogenic effect Effects 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 231100000315 carcinogenic Toxicity 0.000 description 2
- 231100000260 carcinogenicity Toxicity 0.000 description 2
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- 239000000706 filtrate Substances 0.000 description 2
- 239000005457 ice water Substances 0.000 description 2
- BAUYGSIQEAFULO-UHFFFAOYSA-L iron(2+) sulfate (anhydrous) Chemical compound [Fe+2].[O-]S([O-])(=O)=O BAUYGSIQEAFULO-UHFFFAOYSA-L 0.000 description 2
- 229910000359 iron(II) sulfate Inorganic materials 0.000 description 2
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- 238000010813 internal standard method Methods 0.000 description 1
- VBMVTYDPPZVILR-UHFFFAOYSA-N iron(2+);oxygen(2-) Chemical compound [O-2].[Fe+2] VBMVTYDPPZVILR-UHFFFAOYSA-N 0.000 description 1
- SZVJSHCCFOBDDC-UHFFFAOYSA-N iron(II,III) oxide Inorganic materials O=[Fe]O[Fe]O[Fe]=O SZVJSHCCFOBDDC-UHFFFAOYSA-N 0.000 description 1
- 230000000813 microbial effect Effects 0.000 description 1
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 1
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- 125000001424 substituent group Chemical group 0.000 description 1
- 238000005303 weighing Methods 0.000 description 1
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- B01J13/00—Colloid chemistry, e.g. the production of colloidal materials or their solutions, not otherwise provided for; Making microcapsules or microballoons
- B01J13/0091—Preparation of aerogels, e.g. xerogels
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- B01J31/181—Cyclic ligands, including e.g. non-condensed polycyclic ligands, comprising at least one complexing nitrogen atom as ring member, e.g. pyridine
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Abstract
The invention provides a preparation method of a magnetic graphene-based aerogel with a photocatalytic function, which comprises the steps of preparing a photocatalytic material, namely tetra-amino phthalocyanine iron, then loading magnetic particles on a graphene base to prepare the magnetic graphene-based aerogel, and finally grafting the tetra-amino phthalocyanine iron to the surface of the magnetic graphene-based aerogel by virtue of an amidation reaction to obtain the magnetic graphene-based aerogel material with the photocatalytic function. The material has the integrated adsorption-degradation effect and the physical magnetic separation function, can be widely applied to adsorption degradation of a polluted system containing benzo alpha pyrene (BaP), and has potential application prospects.
Description
Technical Field
The invention belongs to the technical field of environmental pollutant treatment, and particularly relates to a preparation method of magnetic graphene-based aerogel with a photocatalytic function
Background
Currently, environmental problems caused by air pollution have become a focus. Carcinogenic Polycyclic Aromatic Hydrocarbons (PAHs) are the most attractive hazardous substances, more than 90 percent of carcinogenic PAHs exist in a PM2.5 granular phase, and benzo alpha pyrene (BaP) in the PAHs has wide sources, difficult degradation and strong carcinogenicity and is considered as a great influence environmental pollutant. At present, methods for removing BaP in the environment include microbial degradation, photocatalytic degradation, adsorption, etc., wherein the adsorption method has been widely paid attention due to low cost, simple operation and strong versatility, and is the most effective method for removing BaP at present. The existing adsorption method can not completely convert the harmful substances into harmless substances and has the limitations of difficult recovery or separation and the like. Therefore, a new composite adsorption and degradation material which has large capacity, high adsorption speed, convenient separation and can degrade the BaP is urgently needed so as to efficiently and economically remove the BaP pollutants.
In the composite adsorption degradation material in recent years, graphene is a two-dimensional novel carbon adsorption material with huge development potential. The graphene-based aerogel has ultrahigh porosity and specific surface area and good adsorption effect. However, graphene-based aerogel only has high adsorbability and does not have the integral adsorption-degradation effect, and the separation of the adsorption material from the adsorption environment is also an urgent problem to be solved. Graphene-based aerogels have been prepared in the prior art, for example, patent No. CN110104636A discloses a Fe3O4Graphene aerogel and a preparation method thereof.
From the existing patents, most of the existing graphene-based materials are complex to prepare, are easy to cause secondary pollution, and have a fresh report on the adsorption and degradation of benzo-alpha-pyrene (BaP). Therefore, the graphene is used as a molecular framework to load various substances, and the graphene has an adsorption-degradation integrated effect and a physical magnetic separation function. The research of the multifunctional novel adsorption degradation material has important reference value for the adsorption degradation of the air polycyclic alkane.
Disclosure of Invention
In order to solve the problems of difficult degradation and strong carcinogenicity of benzo alpha pyrene (BaP) in the existing air pollutant polycyclic aromatic hydrocarbon, the invention provides a preparation method of graphene-based aerogel with photocatalytic degradation function and large adsorption capacity, which can be widely applied to adsorption degradation of a system containing benzo alpha pyrene (BaP) pollution and has potential application prospect.
The invention is realized by the following technical scheme:
a preparation method of magnetic graphene-based aerogel with photocatalytic function comprises the following steps:
(1) preparation of iron tetranitrophthalocyanine
Dissolving 4-nitrophthalonitrile, ferrous chloride and 1, 8-diazabicycloundec-7-ene in ethylene glycol, and refluxing for 3-5 h at 175-200 ℃ under the protection of nitrogen; filtering, washing, removing impurities, drying and grinding the mixture while the mixture is hot after the reaction is finished to obtain black powdery tetranitroiron phthalocyanine;
the mass-volume ratio of the 4-nitrophthalonitrile, the ferrous chloride, the 1, 8-diazabicycloundecen-7-ene and the ethylene glycol is (3.0-3.5 g): 1 g: (3-4 mL): (30-40 mL);
washing is sequentially carried out for 2-3 times by using ethylene glycol, methanol and acetone respectively, washing is carried out until the solution is colorless by using 2-4% hydrochloric acid, washing is carried out until the solution is neutral by using deionized water, and finally washing is carried out by using ethanol.
Preferably, the drying condition is vacuum drying at 90-100 ℃ for 12-15 h.
(2) Preparation of iron tetra-amino phthalocyanine (FeTAPc)
Adding the tetranitro phthalocyanine iron prepared in the step (1) and sodium sulfide into N, N-dimethylformamide, slowly stirring to dissolve crystallized sodium sulfide, heating to 70-75 ℃, accelerating the stirring speed, and reacting for 2-4 h; and carrying out suction filtration, washing, drying, cooling and grinding while the mixture is hot to obtain black powdery tetra-amino iron phthalocyanine FeTAPc.
The mass volume ratio of the tetranitro phthalocyanine iron to the sodium sulfide to the N, N-dimethylformamide is 1 g: (4-4.5 g): (25-30 mL).
And washing for 2-3 times by using methanol, and then washing to be neutral by using deionized water.
Preferably, the drying condition is vacuum drying at 90-100 ℃ for 12-15 h.
(3) Preparation of graphene oxide-based aerogel
Mixing graphene and anhydrous NaNO3Adding KMnO at the same time4Oxidizing in concentrated sulfuric acid, adding hydrogen peroxide to reduce excessive KMnO after the reaction is finished4And obtaining Graphene Oxide (GO) suspension, and freeze-drying to obtain the graphene oxide based aerogel.
The graphene and anhydrous NaNO3、KMnO4The mass-volume ratio of concentrated sulfuric acid is 1 g: (0.35-0.75 g): (2.5-4.5 g): (20-36 mL).
Preferably, the mass fraction of the hydrogen peroxide is 30-35%.
(4) Magnetic nano iron oxide loaded graphene oxide (gamma-Fe)2O3Preparation of/rGO)
Dispersing the graphene oxide GO suspension in ultrapure water, carrying out ultrasonic treatment for 2-4 h, and adjusting the pH value of a 5-10% NaOH solution to 7.0-7.5. Adding a mixed solution of a stabilizer and a ferrous chloride ethanol solution into the graphene oxide GO suspension, slowly adding a sodium borohydride solution, stirring and reacting for 4-6 hours to obtain the magnetic nano-iron oxide loaded graphene oxide gamma-Fe2O3solid/rGO.
The mass ratio of the stabilizer to the ferrous chloride is 1g to (0.02-0.05).
Preferably, the mass concentration of the ferrous chloride ethanol solution is 2-5 mg.L < -1 >.
The mass ratio of the graphene oxide to the stabilizer is 1g to (5-6).
Preferably, the stabilizer is one selected from polyvinylpyrrolidone, sodium lauryl sulfate and polyacrylic acid.
The mass ratio of the ferrous chloride to the sodium borohydride is 1g to (1.5-2.5).
Preferably, the mass fraction of the sodium borohydride solution is 10-15%.
(5) Preparation of magnetic graphene-based aerogel photodegradation material with photocatalytic function
Carrying out magnetic loading on the nano iron oxide graphene (gamma-Fe) prepared in the step (4)2O3and/rGO) and the tetra-amino iron phthalocyanine (Fe-TAPc) prepared in the step (2) are dispersed in a mixed solution of water and triethanolamine, and are stirred and reacted for 24-36 hours at the temperature of 80-90 ℃. And rotationally evaporating the solvent, pouring the residual liquid into absolute ethyl alcohol under the condition of vigorous stirring, refrigerating for 14-18 h at 4-5 ℃, centrifuging, washing, and freeze-drying to obtain the photocatalytic function graphene-based aerogel photodegradation material.
The magnetic nano iron oxide-loaded graphene oxide (gamma-Fe)2O3The mass volume ratio of the mixed solution of the/rGO, the tetra-amino iron phthalocyanine (FeTAPc), water and triethanolamine is 1 g: (2.2-2.6 g): (25-30 mL).
The volume ratio of water to triethanolamine in the mixed solution of water and triethanolamine is 1.3-1.6 mL: 1 mL.
And washing for 3-5 times by using a mixed solution of water and ethanol.
Compared with the prior art, the invention has the beneficial effects that:
1. the graphene-based aerogel material with the photocatalytic degradation function, the efficient adsorption function and the magnetic response function can effectively perform photocatalytic degradation and adsorption on benzo alpha pyrene (BaP) in an air environment, and can be widely applied to adsorption degradation of a polluted system containing benzo alpha pyrene (BaP).
2. The graphene is a molecular framework, and various loaded substances have the functions of small volume and high enrichment, optimize the chemical properties of the graphene and the loaded substances, and have the advantages of simple and convenient operation and high adsorption efficiency.
Drawings
Fig. 1 is a preparation route of photocatalytic magnetic graphene-based aerogel;
FIG. 2 shows the magnetically supported nano-iron oxide graphene (. gamma. -Fe) prepared in example 22O3/rGO) TEM images;
fig. 3 shows the adsorption performance of the photocatalytic magnetic graphene-based aerogel prepared in example 1 on benzo α pyrene (BaP).
Fig. 4 shows the reusability of the photocatalytic magnetic graphene-based aerogel prepared in example 1.
Detailed Description
The technical solution of the present invention is further described in detail below with reference to the following detailed description and the accompanying drawings:
example 1:
a preparation method of magnetic graphene-based aerogel with photocatalytic function comprises the following steps:
(1) preparation of iron tetranitrophthalocyanine
60mL of ethylene glycol, 6.02g of 4-nitrophthalonitrile, 2g of ferrous chloride and 6mL of 1, 8-diazabicycloundec-7-ene are sequentially added into a 250mL three-neck flask; installing a condensing tube, introducing nitrogen for protection, and refluxing for 3h at 180 ℃; filtering while hot after the reaction is finished, sequentially washing with ethylene glycol, methanol and acetone twice respectively, washing with 2% hydrochloric acid until colorless, washing with deionized water until neutral, and washing with ethanol; cooling, grinding, and vacuum drying at 90 ℃ for 12-15 h to obtain black powdery tetranitro phthalocyanine iron.
(2) Preparation of iron tetra-amino phthalocyanine (FeTAPc)
Weighing 3.20g of the iron powder of tetranitro phthalocyanine and 12.4g of sodium sulfide, placing the powder and the sodium sulfide in a 250mL flask, adding about 70mLN, N-dimethylformamide, slowly stirring to dissolve the crystallized sodium sulfide, accelerating the stirring speed when the temperature reaches 70 ℃, and reacting for 2 hours at constant temperature; after the reaction is finished, carrying out suction filtration by using a sand core funnel while the reaction is hot, firstly washing twice by using methanol, and then washing to be neutral by using deionized water; vacuum drying at 100 deg.C for 12h, cooling, grinding, and vacuum drying at 90 deg.C for 12h to obtain black powdery iron tetra-amino phthalocyanine (FeTAPc).
(3) Preparation of graphene oxide-based aerogel
Placing 30mL of 98% concentrated sulfuric acid into an ice-water bath, adding 1g of graphene and 0.5g of anhydrous NaNO3, slowly adding 3.0g of potassium permanganate under strong stirring, controlling the temperature to be below 20 ℃, stirring for 3 hours, placing the beaker into a constant-temperature water bath at 35 ℃ (± 3 ℃), continuously stirring for 30 minutes, moving the beaker into an oil bath at 98 ℃, continuously adding deionized water during stirring, keeping the temperature of the suspension to be not higher than 100 ℃, keeping stirring for 15 minutes, diluting the suspension with 100mL of deionized water, adding a proper amount of 30% hydrogen peroxide to reduce residual potassium permanganate and generated manganese dioxide insoluble substances to enable the potassium permanganate and the generated manganese dioxide to become colorless soluble manganese sulfate, washing with HCl solution and deionized water under the treatment of hydrogen peroxide until no sulfate radical is detected in filtrate to obtain a Graphene Oxide (GO) suspension, and (5) freeze-drying to obtain the graphene oxide-based aerogel.
(4) Magnetic loaded nano oxygenIron-oxidized graphene (gamma-Fe)2O3Preparation of/rGO)
30mL of GO suspension liquid is weighed into 250mL of ultrapure water, ultrasonic treatment is carried out for 2 hours, and the pH value is adjusted to 7.0 by 5% NaOH solution. 8g of polyvinylpyrrolidone was added to 150mL of 5 mg. multidot.L-1The ferrous sulfate ethanol solution to prepare a mixed solution. N is a radical of2Under the atmosphere, adding the mixed solution into GO solution, stirring for 15min, slowly adding 25mL of 10% sodium borohydride solution, stirring for reaction for 4h, filtering, washing the product with absolute ethyl alcohol for more than 3 times, and drying in vacuum at 60 ℃ for 2d to obtain the magnetic nano iron oxide-loaded reduced graphene oxide gamma-Fe2O3solid/rGO.
(5) Preparation of magnetic graphene-based aerogel with photocatalytic function
1.0g of reduced graphene oxide gamma-Fe magnetically loaded with nano iron oxide2O3The solid/rGO and 2.26g of tetra-amino iron phthalocyanine (FeTAPc) are dispersed in a mixed solution of 15mL of water and 10mL of triethanolamine, and the mixture is stirred and reacted for 24 hours at 85 ℃. Most of the solvent is evaporated by rotary evaporation, the residual liquid is poured into 500mL of absolute ethyl alcohol under the condition of vigorous stirring, the liquid is placed in a refrigerator at 4 ℃ after 1h, and the solid product is obtained by centrifugation after 18 h. And washing the solution with a mixed solution of water and ethanol for 3 times, and freeze-drying to obtain the magnetic graphene-based aerogel with the photocatalytic function.
Example 2:
magnetic nano iron oxide loaded graphene oxide (gamma-Fe)2O3/rGO) preparation process comprising the following steps:
(1) preparation of graphene oxide-based aerogel
30mL of 98% concentrated sulfuric acid was placed in an ice-water bath, and 1g of graphene and 0.5g of anhydrous NaNO were added3Slowly adding 3.0g of potassium permanganate under strong stirring, controlling the temperature below 20 ℃, stirring for 3h, then placing a beaker in a constant-temperature water bath at 35 ℃ (± 3 ℃), continuing stirring for 30min, moving the beaker into an oil bath at 98 ℃, continuously adding deionized water while stirring, keeping stirring for 15min while ensuring that the temperature of the suspension does not exceed 100 ℃, diluting the suspension with 100mL of deionized water, then adding proper amount of deionized waterReducing the residual potassium permanganate and the generated manganese dioxide insoluble substances by using 30% hydrogen peroxide to convert the residual potassium permanganate and the generated manganese dioxide insoluble substances into colorless and soluble manganese sulfate, washing the manganese sulfate insoluble substances by using HCl solution and deionized water under the treatment of hydrogen peroxide until no sulfate radical is detected in the filtrate to obtain Graphene Oxide (GO) suspension, and freeze-drying the graphene oxide based aerogel to obtain the graphene oxide based aerogel.
(2) Magnetic nano iron oxide loaded graphene oxide (gamma-Fe)2O3Preparation of/rGO)
30mL of GO suspension liquid is weighed into 250mL of ultrapure water, ultrasonic treatment is carried out for 2 hours, and the pH value is adjusted to 7.0 by 5% NaOH solution. 8g of polyvinylpyrrolidone was added to 150mL of 5 mg. multidot.L-1The ferrous sulfate ethanol solution to prepare a mixed solution. N is a radical of2Under the atmosphere, adding the mixed solution into GO solution, stirring for 15min, slowly adding 25mL of 10% sodium borohydride solution, stirring for reaction for 4h, filtering, washing the product with absolute ethyl alcohol for more than 3 times, and vacuum-drying at 60 ℃ for 2d to obtain the magnetic nano iron oxide-loaded reduced graphene oxide (gamma-Fe)2O3/rGO) solid.
Test example 1:
magnetic nano iron oxide loaded graphene oxide (gamma-Fe)2O3/rGO) morphology testing.
Test samples: example 2 magnetic nano iron oxide-loaded graphene oxide (γ -Fe)2O3/rGO)。
Graphene oxide (gamma-Fe) magnetically loaded with nano iron oxide prepared in example 22O3the/rGO) adopts a Scanning Electron Microscope (SEM) to represent the apparent morphology of the final product, the working voltage is 15kV, and the scanning electron micrograph is shown as an attached figure 2. It can be seen that the nano Fe loaded on the graphene oxide rGO2O3The shape of the nano iron oxide is rod-shaped and spherical, and the nano iron oxide is consistent with the original shape of the nano iron oxide, so that the nano iron oxide is successfully loaded on the surface of the graphene oxide.
Test example 2:
and (3) testing the adsorption performance of the magnetic graphene-based aerogel with the photocatalytic function.
Test samples: example 1 prepared photocatalytic functional magnetic graphene-based aerogel.
Adsorption test: adding 10 groups of 5mL cigarette concentrated solution into conical flask, respectively adding 0.4g magnetic graphene-based aerogel with photocatalytic function, oscillating at constant temperature of 25 deg.C for 5, 10, 20, 30, 45, 60, 120, 240, 480 and 720min in dark place, and accurately transferring 1.0mL supernatant and 150 ng. mL-1The internal standard substance solution is put in a sample injection bottle, GC-MS automatic sample injection is carried out to detect BaP, and the BaP is quantified by adopting an internal standard method (naphthalene is taken as an internal standard substance). The adsorption capacity at different times was calculated and the adsorption kinetics curve was plotted as shown in figure 3. The graph shows that the adsorption amount of the aerogel to the benzo alpha pyrene (BaP) is gradually increased along with the increase of time. Benzo alpha pyrene (BaP) is adsorbed on the surface by pi-pi and p-pi conjugation and interaction between C-C and C-O bonds on the surface of rGO and benzene rings and other polar substituents of PAHs in smoke.
Test example 2:
and testing the photodegradability of the magnetic graphene-based aerogel with the photocatalytic function.
Test samples: example 1 prepared photocatalytic functional magnetic graphene-based aerogel.
5 groups of 5.0mL cigarette concentrated solution are put into a conical flask, and 0.4g of magnetic graphene-based aerogel with photocatalytic function is respectively added. After dark treatment for 8h, 5 groups of samples are placed under an ultraviolet lamp irradiator for 1, 2, 4, 8 and 12h respectively and are kept stand, and 1.0mL of supernatant and 150ng & mL of supernatant are accurately transferred-1The naphthalene internal standard substance solution is put in a sample injection bottle, GC-MS automatic sample injection quantitative detection is carried out on BaP, the degradation rate of BaP is calculated, and a chart is drawn as shown in Table 1. It can be seen that the longer the exposure time to visible light is, the lower the concentration of BaP in the solution is, the higher the degradation rate is, and the good photodegradability of the photocatalytic magnetic graphene-based aerogel is proved
TABLE 1 degradation assay results for the prepared samples
Test example 3:
and (4) testing the repeated performance of the magnetic graphene-based aerogel with the photocatalytic function.
Test samples: example 1 prepared photocatalytic functional magnetic graphene-based aerogel.
Adding 5mL cigarette concentrate into conical flask, adding 0.4g magnetic graphene-based aerogel with photocatalytic function, oscillating at 25 deg.C in dark for 480min, placing under ultraviolet lamp for radiation for 8 hr, and accurately transferring 1.0mL supernatant and 150 ng/mL-1The naphthalene internal standard substance solution is put in a sample injection bottle, GC-MS automatic sample injection quantitative detection of BaP is carried out, and the BaP degradation rate is calculated. The adsorption and degradation experiments were repeated 5 times each, and the adsorption amount and degradation rate were calculated and plotted as shown in FIG. 4. From the figure, after 5 times of repeated adsorption degradation cycles, the equilibrium adsorption capacity of the aerogel on BaP is still over 86% of the original equilibrium adsorption capacity, and the degradation rate is over 79%. The magnetic graphene-based aerogel with the photocatalytic function has excellent cycle performance, is convenient for repeated adsorption and degradation of BaP, and has wide application prospect.
Claims (18)
1. A preparation method of magnetic graphene-based aerogel with photocatalytic function is characterized by comprising the following steps:
(1) preparation of iron tetranitrophthalocyanine
Dissolving 4-nitrophthalonitrile, ferrous chloride and 1, 8-diazabicycloundec-7-ene in ethylene glycol for reaction, washing and drying to obtain black powdery tetranitrophthalocyanine iron;
(2) preparation of iron tetraaminophthalocyanine
Adding the tetranitro phthalocyanine iron prepared in the step (1) and sodium sulfide into N, N-dimethylformamide, slowly stirring to dissolve crystallized sodium sulfide, heating to 70-75 ℃, accelerating the stirring speed, and reacting for 2-4 h; hot filtering, washing and drying to obtain black powdery tetra-amino iron phthalocyanine;
(3) preparation of graphene oxide-based aerogel
Mixing graphene and anhydrous NaNO3Adding KMnO at the same time4And oxygen in concentrated sulfuric acidAfter the reaction is finished, adding hydrogen peroxide to reduce excessive KMnO4Obtaining graphene oxide suspension, and freeze-drying to obtain graphene oxide-based aerogel;
(4) preparation of magnetic nano iron oxide-loaded graphene oxide
Dispersing the graphene oxide GO suspension in ultrapure water, carrying out ultrasonic treatment for 2-4 h, and adjusting the pH value of a 5-10% NaOH solution to 7.0-7.5. Adding a mixed solution of a stabilizer and a ferrous chloride ethanol solution into the graphene oxide GO suspension, slowly adding a sodium borohydride solution, stirring and reacting for 4-6 hours to obtain the magnetic nano-iron oxide loaded graphene oxide gamma-Fe2O3(ii)/rGO solid;
(5) preparation of magnetic graphene-based aerogel photodegradation material with photocatalytic function
And (3) dispersing the magnetic nano iron oxide-loaded graphene oxide prepared in the step (4) and the tetra-amino iron phthalocyanine prepared in the step (2) in a mixed solution of water and triethanolamine to react completely, performing rotary evaporation on the solvent, pouring the residual liquid into absolute ethyl alcohol under the condition of vigorous stirring, and performing refrigeration, washing and freeze drying to obtain the photocatalytic graphene-based aerogel photodegradation material.
2. The preparation method of the magnetic graphene-based aerogel with photocatalytic function according to claim 1, wherein the reaction conditions in the step (1) are reflux for 3-5 hours at 175-200 ℃ under the protection of nitrogen.
3. The preparation method of the magnetic graphene-based aerogel with photocatalytic function according to claim 1, wherein in the step (1), the mass-to-volume ratio of 4-nitrophthalonitrile, ferrous chloride, 1, 8-diazabicycloundecen-7-ene and ethylene glycol is (3.0-3.5 g): 1 g: (3-4 mL): (30-40 mL).
4. The preparation method of the magnetic graphene-based aerogel with the photocatalytic function according to claim 1, wherein the washing in the step (1) is sequentially carried out for 2-3 times by using ethylene glycol, methanol and acetone respectively, the washing is carried out for 2-4% until the washing is colorless, the washing is carried out for neutral by using deionized water, and finally the washing is carried out by using ethanol.
5. The preparation method of the photocatalytic magnetic graphene-based aerogel according to claim 1, wherein the mass-to-volume ratio of the tetranitro iron phthalocyanine, the sodium sulfide and the N, N-dimethylformamide in the step (2) is 1 g: (4-4.5 g): (25-30 mL).
6. The preparation method of the photocatalytic magnetic graphene-based aerogel according to claim 1, wherein the washing in the step (2) is performed 2-3 times with methanol and then with deionized water until the solution is neutral.
7. The preparation method of the photocatalytic magnetic graphene-based aerogel according to claim 1, wherein the graphene and anhydrous NaNO in the step (3) are used as raw materials3、KMnO4The mass-volume ratio of concentrated sulfuric acid is 1 g: (0.35-0.75 g): (2.5-4.5 g): (20-36 mL).
8. The preparation method of the magnetic graphene-based aerogel with the photocatalytic function according to claim 1, wherein the mass fraction of hydrogen peroxide in the step (3) is 30-35%.
9. The method for preparing the magnetic graphene-based aerogel with photocatalytic function according to claim 1, wherein the stabilizer in the step (4) is one selected from polyvinylpyrrolidone, sodium dodecyl sulfate and polyacrylic acid.
10. The preparation method of the magnetic graphene-based aerogel with the photocatalytic function according to claim 1, wherein the mass ratio of the stabilizer to the ferrous chloride in the step (4) is 1: 0.02-0.05; wherein the mass concentration of the ferrous chloride ethanol solution is 2-5 mg.L-1。
11. The preparation method of the magnetic graphene-based aerogel with the photocatalytic function according to claim 1, wherein the mass ratio of the graphene oxide to the stabilizer in the step (4) is 1g to (5-6).
12. The preparation method of the magnetic graphene-based aerogel with photocatalytic function according to claim 1, wherein the volume ratio of methanol to acetic acid in the methanol-acetic acid solution in the step (4) is (8-9) mL: 1 mL.
13. The preparation method of the magnetic graphene-based aerogel with the photocatalytic function according to claim 1, wherein the mass ratio of the ferrous chloride to the sodium borohydride in the step (4) is 1: 1.5-2.5; wherein the mass fraction of the sodium borohydride solution is 10-15%.
14. The preparation method of the magnetic graphene-based aerogel with photocatalytic function according to claim 1, wherein the mass-to-volume ratio of the mixed solution of graphene oxide magnetically loaded with nano iron oxide, iron tetraaminophthalocyanine, water and triethanolamine in step (5) is 1 g: (2.2-2.6 g): (25-30) mL.
15. The preparation method of the photocatalytic magnetic graphene-based aerogel according to claim 1, wherein the volume ratio of water to triethanolamine in the mixed solution of water and triethanolamine in the step (5) is 1.3-1.6 mL: 1 mL.
16. The preparation method of the magnetic graphene-based aerogel with photocatalytic function according to claim 1, wherein the washing in the step (5) is performed 3 to 5 times with a mixed solution of water and ethanol.
17. The preparation method of the magnetic graphene-based aerogel with the photocatalytic function according to claim 1, wherein the reaction condition in the step (5) is stirring reaction at 80-90 ℃ for 24-36 h.
18. The preparation method of the magnetic graphene-based aerogel with photocatalytic function according to claim 1, wherein the refrigeration condition in the step (5) is refrigeration at 4-5 ℃ for 14-18 h.
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| CN114618529B (en) * | 2022-04-06 | 2023-09-22 | 中国科学院大学 | Magnetic graphene-based photocatalyst GO-Fe 3 O 4 @SiO 2 @CdS and preparation method and application thereof |
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