CN113877637A - Preparation method and application of nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst - Google Patents

Preparation method and application of nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst Download PDF

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CN113877637A
CN113877637A CN202111156466.7A CN202111156466A CN113877637A CN 113877637 A CN113877637 A CN 113877637A CN 202111156466 A CN202111156466 A CN 202111156466A CN 113877637 A CN113877637 A CN 113877637A
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valent iron
nano zero
carbon fiber
aerogel
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沈孝东
张艳
梅其国
孙伯旺
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Nanjing Hengfeng Medical Equipment Co ltd
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    • B01J35/58
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D53/00Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34Chemical or biological purification of waste gases
    • B01D53/38Removing components of undefined structure
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D53/00Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34Chemical or biological purification of waste gases
    • B01D53/74General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86Catalytic processes
    • B01D53/8659Removing halogens or halogen compounds
    • B01D53/8662Organic halogen compounds
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D53/00Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34Chemical or biological purification of waste gases
    • B01D53/74General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/86Catalytic processes
    • B01D53/8668Removing organic compounds not provided for in B01D53/8603 - B01D53/8665
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    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J21/00Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
    • B01J21/18Carbon
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/70Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of the iron group metals or copper
    • B01J23/74Iron group metals
    • B01J23/745Iron
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J31/00Catalysts comprising hydrides, coordination complexes or organic compounds
    • B01J31/02Catalysts comprising hydrides, coordination complexes or organic compounds containing organic compounds or metal hydrides
    • B01J31/0234Nitrogen-, phosphorus-, arsenic- or antimony-containing compounds
    • B01J31/0235Nitrogen containing compounds
    • B01J31/0244Nitrogen containing compounds with nitrogen contained as ring member in aromatic compounds or moieties, e.g. pyridine
    • B01J35/61
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01JCHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J37/00Processes, in general, for preparing catalysts; Processes, in general, for activation of catalysts
    • B01J37/06Washing
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2257/00Components to be removed
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    • B01D2257/206Organic halogen compounds
    • B01D2257/2064Chlorine
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
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    • B01D2257/70Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
    • BPERFORMING OPERATIONS; TRANSPORTING
    • B01PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01DSEPARATION
    • B01D2258/00Sources of waste gases
    • B01D2258/02Other waste gases
    • B01D2258/0283Flue gases

Abstract

The invention discloses a preparation method and application of a nano zero-valent iron modified aerogel coated carbon fiber heterogeneous Fenton catalyst. Growing the nano zero-valent iron into a melamine-formaldehyde aerogel matrix in an in-situ embedded manner, adding the cleaned carbon fibers, and sequentially replacing the carbon fibers with ethanol and acetone to obtain the nano zero-valent iron-formaldehyde aerogel matrix. The composite catalyst prepared by the invention has the advantages of strong Fenton reaction activity, high porosity, large specific surface area and the like, and simultaneously utilizes the interaction between the carrier and the active component to further enhance the reaction activity and the stability of the catalyst, so that the composite catalyst is suitable for removing the nondegradable moxibustion smoke wastewater by Fenton catalytic oxidation.

Description

Preparation method and application of nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst
Technical Field
The invention relates to a preparation method and application of a chemical material, in particular to a preparation method of a nano zero-valent iron modified aerogel coated carbon fiber heterogeneous Fenton catalyst.
Background
Moxibustion is a therapeutic method in which a lighted moxa stick is used to cauterize and warm-iron selected acupoints or regions. Recorded in Ming Yi Bie Lu (famous physicians and miscellaneous records) that "ai Ye is bitter, slightly warm, nontoxic and mainly cures various diseases by moxibustion. Moxibustion has effects of warming channels for dispelling cold, strengthening yang, relieving depletion, removing blood stasis, resolving hard mass, preventing diseases, promoting health, and inducing heat for external application. Modern medical research also shows that: moxibustion can regulate viscera function, promote metabolism, and improve immunity, thereby preventing and treating diseases. In recent years, with the vigorous development of the traditional Chinese medicine industry, moxibustion therapy is also popular in the primary medical service stations in various regions.
However, moxibustion burns with a certain volume of smoke. The moxa smoke can not only cause environmental pollution, but also bring huge potential safety hazards to human bodies after long-term inhalation of the moxa smoke. Questionnaire survey shows that after moxibustion, a doctor has 61.11% of symptoms such as pharyngeal discomfort or cough, and moxa smoke may increase the risk of acupuncture doctors suffering from chronic pharyngolaryngitis. After gas chromatography-mass spectrometry analysis, the moxa smoke mainly comprises 26 organic compounds such as phenol, m-methyl phenol, o-methyl phenol, 3, 4-xylenol, p-ethyl phenol, catechol, hydroquinone, indole, caryophyllene, pentadecanyl chloroacetate and the like. Wherein, if the amount of the phenolic compound entering the human body exceeds the detoxification function of the normal human body, the excessive part can be accumulated in each organ tissue in the human body to cause chronic poisoning, and various chronic digestive tract symptoms such as dizziness, headache, rash, skin pruritus, uneasiness, anemia, various nervous system symptoms and inappetence, dysphagia, salivation, vomiting, diarrhea and the like appear. Therefore, the moxa smoke weakens the health care function of moxibustion therapy to a certain extent and is an important obstacle for further popularization and application of moxibustion therapy. Therefore, moxa smoke treatment has become a focus of attention for researchers. CN112657290A discloses an intelligence chinese mugwort cigarette processing apparatus who is equipped with filtration, can carry out accurate filtration absorption to chinese mugwort cigarette. CN112891198A discloses an integrated device for moxibustion smoke treatment and filtration, which is provided with a moxa smoke filter on the opening of a moxibustion cylinder to filter the moxa smoke. CN213251204U discloses a bed formula chinese mugwort cigarette processing apparatus, including box, bottom filter layer, advance cigarette hole, surge bin, advance structures such as mouth, middle part filter layer, top filter layer, play tobacco pipe, surge bin and advance the cigarette hole and can make chinese mugwort cigarette evenly get into the filter layer, and bottom filter layer, middle part filter layer and top filter layer can be to the flue gas stage filtration, are favorable to improving filtration quality and filtration efficiency.
Although the relevant patents have certain treatment effect, the main treatment mode mainly adopts physical adsorption, and the toxic and harmful substances in the moxa smoke cannot be truly and chemically degraded. Simultaneously, use the filter layer and need often change the washing to the filter core, not only improved moxibustion therapy's use cost, change abluent process and still cause the secondary damage to the purger very easily. Therefore, it is necessary to develop a new chemical degradation means for harmless treatment of moxa smoke.
Advanced oxidation processes are one of the contaminant degradation technologies that have received much attention in recent years. The basic characteristic is that hydroxyl free radical (OH) is used as main oxidant to react with organic matter, the produced organic free radical can take part in OH chain reaction continuously, or the produced organic peroxide free radical can take part in oxidative decomposition continuously until the pollutant is mineralized into final product CO2And H2And O. The Fenton reaction method is one of the most widely used advanced oxidation methods, and the main principle of the Fenton reaction is H2O2In Fe2+Generates OH under the catalytic action of the catalyst to degrade organic pollutants. H used due to Fenton reaction2O2 and the iron compound are relatively cheap, so the Fenton oxidation methodThe method has huge application and research values in wastewater treatment.
The aerogel is a novel low-density nano porous material, has a unique nano three-dimensional network structure, and simultaneously has extremely low density, high specific surface area and high porosity, so the aerogel shows extremely high adsorption performance. The nanometer zero-valent iron is the zero-valent iron particles with the size of 1-100 nanometers, and has the surface effect which is peculiar to nanometer materials. The surface effect means that the specific surface area of the particles is rapidly increased along with the reduction of the particle size, so that a plurality of surface defects exist on the structure of the nanoparticles, the surface has high activity, and other atoms are easily combined. Aerogels doped with metallic elements are widely used in the field of environmental protection. CN107324454B discloses a graphene aerogel electrode material for loading copper ions in an electro-Fenton reaction system and applying the graphene aerogel electrode material to degradation of organic dye sewage. CN107434270B combines molecular imprinting technology with aerogel to prepare iron carbon aerogel with pollutant molecular imprinting and uses it as cathode of electro-Fenton reaction. CN103785394A discloses a preparation method of a three-dimensional nano perovskite type composite heterogeneous Fenton catalyst, which is characterized in that carbon aerogel is used as a matrix, and nano perovskite type bismuth iron oxide is loaded by a sol-gel method to obtain the carbon aerogel loaded with the nano perovskite type bismuth iron composite, namely the three-dimensional nano perovskite type composite heterogeneous Fenton catalyst. Therefore, the construction of the composite aerogel Fenton catalyst by doping metals such as iron and copper into the aerogel with huge specific surface area becomes an important technical means in the current environmental treatment.
Disclosure of Invention
The purpose of the invention is as follows: the invention aims to provide a preparation method of a nano zero-valent iron modified aerogel coated carbon fiber heterogeneous Fenton catalyst, which can quickly remove pollutants difficult to degrade, high in toxicity and low in concentration.
The technical scheme is as follows: the invention provides a preparation method of a nano zero-valent iron modified aerogel coated carbon fiber heterogeneous Fenton catalyst. According to the invention, the nano zero-valent iron is grown in the melamine-formaldehyde aerogel platform in an in-situ 3D embedded manner for the first time and is coated on the treated carbon fiber bundle, so that the adsorption performance of the catalyst is increased, the technical problems that the nano catalyst is difficult to recover and is easy to poison are solved, the carbon fiber bundle is applied to the waste water absorbing moxibustion smoke, and the integrated process of online adsorption-degradation of moxa smoke pollutants is realized.
Further, the preparation method of the nano zero-valent iron modified aerogel coated carbon fiber heterogeneous Fenton catalyst comprises the following steps:
(1) mixing anhydrous ethanol and triethanolamine uniformly;
(2) putting melamine into the mixture, sequentially adding sodium carbonate and ultrapure water, stirring in a hot water bath, adding a formaldehyde solution and an iron salt, continuously stirring until the solution is clear, adjusting the pH value, adding cleaned carbon fibers, and standing to obtain a precursor solution;
(3) and (3) pouring the mixed solution prepared in the step (1) into the solution prepared in the step (2) while stirring, drying, heating, cooling, adding absolute ethyl alcohol and acetone for replacement, and finally obtaining the carbon fiber bundle with the surface coated with the nano zero-valent iron-doped melamine-formaldehyde aerogel.
Further, the mass ratio of the absolute ethyl alcohol to the triethanolamine to the sodium carbonate to the ultrapure water is 15: 0.5-2.5: 0.01-0.02: 10-30.
Further, the mass ratio of the melamine to the formaldehyde to the ferric salt is 1: 6: 0.5 to 2.5.
Further, the precursor solution prepared in the step (2) is placed in a hot water bath at 50-70 ℃.
Further, the precursor solution prepared in the step (2) is placed in a hot water bath at 50-70 ℃.
Further, the organic solvent used for replacement in the step (3) is absolute ethyl alcohol and acetone, and the specific replacement process comprises adding absolute ethyl alcohol, replacing once every 6 hours, and replacing once every 6 hours with acetone after three times.
Further, the prepared nano zero-valent iron modified aerogel coated carbon fiber heterogeneous Fenton catalyst is applied to the field of moxa smoke treatment.
Has the advantages that: compared with the prior art, the invention has the following advantages:
1. according to the invention, a heterogeneous Fenton oxidation method with ultrahigh oxidation capacity is combined with aerogel with an ultra-large specific surface area, so that efficient adsorption and low-energy-consumption oxidative degradation are realized, and organic pollutants with high toxicity and low concentration are efficiently removed.
2. Compared with the existing Fenton reaction catalyst, the invention adopts the porous material melamine-formaldehyde aerogel as the substrate framework doped with the catalyst, has higher specific surface area, provides good conditions for the Fenton reaction to occur in situ in nano holes, simultaneously, the addition of the nano zero-valent iron provides the catalyst for the Fenton reaction, and the special surface defects of the nano particles can adsorb pollutants, thereby realizing the integration of adsorption and degradation on the surface of the nano zero-valent iron.
3. The catalyst prepared by the invention can rapidly remove pollutants which are difficult to degrade, high in toxicity and low in concentration under a weak acid condition, and has a good application prospect.
4. The preparation method has the advantages of simple preparation process, easily controlled reaction conditions, simple and convenient reaction operation, low price of raw materials, low preparation cost, high efficiency and stability.
Drawings
FIG. 1 is an SEM image of a carbon fiber bundle coated with nano zero-valent iron-doped aerogel prepared according to the present invention;
FIG. 2 is a comparison of the catalytic effect of the present invention with other catalysts such as nano zero-valent iron;
FIG. 3 is a diagram showing the effect of the catalyst prepared by the present invention.
Detailed Description
Example 1:
step (1): weighing 15 unit weight of absolute ethyl alcohol and 1 unit weight of triethanolamine, adding into a container, stirring and mixing uniformly
Step (2): weighing 1 unit weight of melamine, putting the melamine into a wide-mouth beaker, sequentially adding 0.015 unit weight of sodium carbonate and 20 unit weight of ultrapure water, putting the beaker into a hot water bath at 70 ℃ for stirring, adding 6 unit weight of formaldehyde solution and a proper amount of ferric sulfate (the mass ratio of the melamine to the iron simple substance is controlled to be 1: 0.5), continuously stirring until the solution is clear, adjusting the pH value to 1.5 by using hydrochloric acid, putting the cleaned carbon fiber, and standing to obtain a precursor solution.
And (3): pouring the solution prepared in the step (1) into the solution prepared in the step (2) while stirring, drying for 24-30 hours at the temperature of 60 ℃, and then heating for 20-40 hours at the temperature of 90 ℃. Standing at room temperature for 70-75 hr, adding anhydrous ethanol, and changing every 6 hr. And after three times, replacing once every 6 hours by using acetone for three times to finally obtain the nano zero-valent iron modified melamine-formaldehyde aerogel coated carbon fiber heterogeneous Fenton catalyst with the mass ratio of melamine to nano iron simple substance of 1: 0.5.
Example 2:
step (1): weighing 15 unit weight of absolute ethyl alcohol and 1 unit weight of triethanolamine, adding into a container, stirring and mixing uniformly
Step (2): weighing 1 unit weight of melamine, putting the melamine into a wide-mouth beaker, sequentially adding 0.015 unit weight of sodium carbonate and 20 unit weight of ultrapure water, putting the beaker into a hot water bath at 70 ℃ for stirring, adding 6 unit weight of formaldehyde solution and a proper amount of ferric sulfate (the mass ratio of the melamine to the iron simple substance is controlled to be 1: 1), continuously stirring until the solution is clarified, adjusting the pH value to 1.5 by using hydrochloric acid, putting the cleaned carbon fiber, and standing to obtain a precursor solution.
And (3): pouring the solution prepared in the step (1) into the solution prepared in the step (2) while stirring, drying for 24-30 hours at the temperature of 60 ℃, and then heating for 20-40 hours at the temperature of 90 ℃. Standing at room temperature for 70-75 hr, adding anhydrous ethanol, and changing every 6 hr. And after the three times, replacing the carbon fiber with acetone every 6 hours to finally obtain the nano zero-valent iron modified melamine-formaldehyde aerogel coated carbon fiber heterogeneous Fenton catalyst with the mass ratio of melamine to the nano iron simple substance of 1: 1.
Example 3:
step (1): weighing 15 unit weight of absolute ethyl alcohol and 1 unit weight of triethanolamine, adding into a container, stirring and mixing uniformly
Step (2): weighing 1 unit weight of melamine, putting the melamine into a wide-mouth beaker, sequentially adding 0.015 unit weight of sodium carbonate and 20 unit weight of ultrapure water, putting the beaker into a hot water bath at 70 ℃ for stirring, adding 6 unit weight of formaldehyde solution and a proper amount of ferric sulfate (the mass ratio of the melamine to the iron simple substance is controlled to be 1: 1.5), continuously stirring until the solution is clear, adjusting the pH value to 1.5 by using hydrochloric acid, putting the cleaned carbon fiber, and standing to obtain a precursor solution.
And (3): pouring the solution prepared in the step (1) into the solution prepared in the step (2) while stirring, drying for 24-30 hours at the temperature of 60 ℃, and then heating for 20-40 hours at the temperature of 90 ℃. Standing at room temperature for 70-75 hr, adding anhydrous ethanol, and changing every 6 hr. And after the three times, acetone is used for replacing every 6 hours, and finally the carbon fiber bundle of which the surface is coated with the nano zero-valent iron-doped melamine-formaldehyde aerogel and the mass ratio of the melamine to the nano iron simple substance is 1: 1.5 is obtained.
Example 4:
step (1): weighing 15 unit weight of absolute ethyl alcohol and 1 unit weight of triethanolamine, adding into a container, stirring and mixing uniformly
Step (2): weighing 1 unit weight of melamine, putting the melamine into a wide-mouth beaker, sequentially adding 0.015 unit weight of sodium carbonate and 20 unit weight of ultrapure water, putting the beaker into a hot water bath at 70 ℃ for stirring, adding 6 unit weight of formaldehyde solution and a proper amount of ferric sulfate (the mass ratio of the melamine to the iron simple substance is controlled to be 1: 2), continuously stirring until the solution is clarified, adjusting the pH value to 1.5 by using hydrochloric acid, putting the cleaned carbon fiber, and standing to obtain a precursor solution.
And (3): pouring the solution prepared in the step (1) into the solution prepared in the step (2) while stirring, drying for 24-30 hours at the temperature of 60 ℃, and then heating for 20-40 hours at the temperature of 90 ℃. Standing at room temperature for 70-75 hr, adding anhydrous ethanol, and changing every 6 hr. And after the three times, acetone is used for replacing every 6 hours, and finally the carbon fiber bundle of which the surface is coated with the nano zero-valent iron-doped melamine-formaldehyde aerogel and the mass ratio of the melamine to the nano iron simple substance is 1: 2 is obtained.
Example 5:
step (1): weighing 15 unit weight of absolute ethyl alcohol and 1 unit weight of triethanolamine, adding into a container, stirring and mixing uniformly
Step (2): weighing 1 unit weight of melamine, putting the melamine into a wide-mouth beaker, sequentially adding 0.015 unit weight of sodium carbonate and 20 unit weight of ultrapure water, putting the beaker into a hot water bath at 70 ℃ for stirring, adding 6 unit weight of formaldehyde solution and a proper amount of ferric sulfate (the mass ratio of the melamine to the iron is controlled to be 1: 2.5), continuously stirring until the solution is clear, adjusting the pH value to 1.5 by using hydrochloric acid, putting the cleaned carbon fiber, and standing to obtain a precursor solution.
And (3): pouring the solution prepared in the step (1) into the solution prepared in the step (2) while stirring, drying for 24-30 hours at the temperature of 60 ℃, and then heating for 20-40 hours at the temperature of 90 ℃. Standing at room temperature for 70-75 hr, adding anhydrous ethanol, and changing every 6 hr. And after the three times, acetone is used for replacing every 6 hours, and finally the carbon fiber bundle of which the surface is coated with the nano zero-valent iron-doped melamine-formaldehyde aerogel and the mass ratio of the melamine to the nano iron simple substance is 1: 2.5 is obtained.
The moxa smoke treatment process is that the moxa smoke generated after moxibustion is introduced into a condensation chamber of moxa smoke treatment equipment (the moxa smoke treatment equipment is another patent application, and the equipment does not belong to the technical object claimed by the invention, so the structure and the use condition of the moxa smoke treatment equipment are not described in detail in the invention), NaOH aqueous solution with pH of 9-11 is stored in the condensation chamber, the moxa smoke with the temperature of above 300 ℃ is rapidly cooled to 30-50 ℃ in the condensation chamber, non-combustible large particles in the moxa smoke are deposited at the bottom of the condensation chamber and adsorbed on the surface of aerogel, 26 organic compounds such as phenol, m-methyl phenol, o-methyl phenol, 3, 4-dimethyl phenol, p-ethyl phenol, catechol, hydroquinone, indole, caryophyllene, pentadecanoyl chloroacetate and the like generated in the combustion process of the moxa smoke can be dissolved in the water body of the condensation chamber, and the main phenolic compounds can form phenol sodium salt with NaOH, so that the solubility in water is greatly improved. After 10-15 moxibustion treatment courses, the condensing chamber is detached from the moxa smoke treatment equipment, COD (chemical oxygen demand) of the solution measured by a rapid digestion spectrophotometry is 800-1200mg/L, TOC (total organic carbon) of the solution measured by a high-temperature catalytic combustion oxidation method is 500-700mg/L, and TN (total nitrogen) of the solution measured by an ultraviolet spectrophotometry is 50-100mg/L, which greatly exceed the national standards related to surface water quality evaluation.
When the method is used specifically, the prepared iron-doped aerogel-coated carbon fiber bundle is placed in a condensation chamber of moxa smoke treatment equipment, the pH value is adjusted to 2-3 by using 1mol/L diluted hydrochloric acid, and 2.0-4.0mL of 8% household H is added2O2The COD of the disinfectant is reduced to 100-200mg/L, the TOC is reduced to 50-100mg/L, and the TN is reduced to about 1.0mg/L after the reaction is carried out for 24 hours, and a plurality of main evaluation indexes of the water quality meet the national standard of surface V-type water, and the disinfectant can be directly discharged or further treated. In addition, the total iron content measured by an ultraviolet-visible spectrophotometry is below 1.0mg/L, and the iron dissolution is considered to be less and meets the relevant national standards. The reuse experiment shows that the catalyst can be recycled for at least more than half a year by calculating the use frequency of 3 times in 1 day, namely the requirement of moxa smoke treatment of more than 500 times of moxibustion treatment can be met.

Claims (8)

1. A preparation method of a nano zero-valent iron modified aerogel coated carbon fiber heterogeneous Fenton catalyst is characterized by comprising the following steps of: growing the nano zero-valent iron into a melamine-formaldehyde aerogel matrix in an in-situ embedded manner, adding the cleaned carbon fibers, and sequentially replacing the carbon fibers with ethanol and acetone to obtain the nano zero-valent iron-formaldehyde aerogel matrix.
2. The preparation method of the nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst according to claim 1, characterized in that: the method comprises the following steps:
(1) mixing anhydrous ethanol and triethanolamine uniformly;
(2) putting melamine into the mixture, sequentially adding sodium carbonate and ultrapure water, stirring in a hot water bath, adding a formaldehyde solution and an iron salt, continuously stirring until the solution is clear, adjusting the pH value, adding cleaned carbon fibers, and standing to obtain a precursor solution;
(3) and (3) pouring the mixed solution prepared in the step (1) into the solution prepared in the step (2) while stirring, drying, heating, cooling, adding absolute ethyl alcohol and acetone for replacement, and finally obtaining the carbon fiber bundle with the surface coated with the nano zero-valent iron-doped melamine-formaldehyde aerogel.
3. The preparation method of the nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst according to claim 2, characterized in that: the mass ratio of the absolute ethyl alcohol to the triethanolamine to the sodium carbonate to the ultrapure water is 15: 0.5-2.5: 0.01-0.02: 10-30.
4. The preparation method of the nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst according to claim 2, characterized in that: the mass ratio of the melamine to the formaldehyde to the ferric salt is 1: 6: 0.5-2.5.
5. The preparation method of the nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst according to claim 2, characterized in that: and (3) placing the precursor solution prepared in the step (2) in a hot water bath at the temperature of 50-70 ℃.
6. The preparation method of the nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst according to claim 2, characterized in that: and (3) after the reaction solution is obtained in the step (3), drying the reaction solution for 24 to 30 hours at the temperature of 60 ℃, heating the reaction solution for 20 to 40 hours at the temperature of 90 ℃, standing the reaction solution for 70 to 75 hours at the normal temperature, and then replacing the reaction solution by using an organic solvent.
7. The preparation method of the nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst according to claim 2, characterized in that: the organic solvent used for replacement in the step (3) is absolute ethyl alcohol and acetone, and the specific replacement process comprises the steps of adding the absolute ethyl alcohol, replacing once every 6 hours with acetone after three times, and replacing three times.
8. The application of the nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst prepared by any one of claims 1 to 7 in the field of moxa smoke treatment.
CN202111156466.7A 2021-09-29 2021-09-29 Preparation method and application of nano zero-valent iron modified aerogel-coated carbon fiber heterogeneous Fenton catalyst Pending CN113877637A (en)

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20150001155A1 (en) * 2013-06-26 2015-01-01 Corning Incorporated Methods and apparatus for synthesis of stabilized zero valent nanoparticles
CN107983303A (en) * 2017-11-09 2018-05-04 马鞍山市心洲葡萄专业合作社 A kind of preparation method of organic wastewater absorption degradation modified carbon fiber
CN110841639A (en) * 2019-11-21 2020-02-28 南开大学 Three-dimensional graphene-based nano zero-valent iron material and preparation method and application thereof
CN111939960A (en) * 2020-08-20 2020-11-17 南开大学 Preparation method and application of nitrogen-doped three-dimensional graphene aerogel loaded nano zero-valent iron

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20150001155A1 (en) * 2013-06-26 2015-01-01 Corning Incorporated Methods and apparatus for synthesis of stabilized zero valent nanoparticles
CN107983303A (en) * 2017-11-09 2018-05-04 马鞍山市心洲葡萄专业合作社 A kind of preparation method of organic wastewater absorption degradation modified carbon fiber
CN110841639A (en) * 2019-11-21 2020-02-28 南开大学 Three-dimensional graphene-based nano zero-valent iron material and preparation method and application thereof
CN111939960A (en) * 2020-08-20 2020-11-17 南开大学 Preparation method and application of nitrogen-doped three-dimensional graphene aerogel loaded nano zero-valent iron

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
吕群: "工业甲醛除铁离子的简便方法", 精细化工, no. 05 *

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