CN114105280A - Method for treating organic wastewater based on activation of peroxydisulfate by nonmetal composite catalytic material - Google Patents
Method for treating organic wastewater based on activation of peroxydisulfate by nonmetal composite catalytic material Download PDFInfo
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- 230000003197 catalytic effect Effects 0.000 title claims abstract description 47
- 238000000034 method Methods 0.000 title claims abstract description 40
- 239000002351 wastewater Substances 0.000 title claims abstract description 35
- 229910052755 nonmetal Inorganic materials 0.000 title claims abstract description 32
- 239000002131 composite material Substances 0.000 title claims description 32
- JRKICGRDRMAZLK-UHFFFAOYSA-L peroxydisulfate Chemical compound [O-]S(=O)(=O)OOS([O-])(=O)=O JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 title claims description 27
- 230000004913 activation Effects 0.000 title description 13
- 239000002905 metal composite material Substances 0.000 claims abstract description 19
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- 239000003344 environmental pollutant Substances 0.000 claims abstract description 14
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- 238000003756 stirring Methods 0.000 claims abstract description 6
- 230000000593 degrading effect Effects 0.000 claims abstract description 5
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- 229910052799 carbon Inorganic materials 0.000 claims description 26
- 230000003213 activating effect Effects 0.000 claims description 13
- 239000008103 glucose Substances 0.000 claims description 12
- 238000001027 hydrothermal synthesis Methods 0.000 claims description 12
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- 239000000356 contaminant Substances 0.000 claims description 5
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- 238000001179 sorption measurement Methods 0.000 claims description 4
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- LCPVQAHEFVXVKT-UHFFFAOYSA-N 2-(2,4-difluorophenoxy)pyridin-3-amine Chemical group NC1=CC=CN=C1OC1=CC=C(F)C=C1F LCPVQAHEFVXVKT-UHFFFAOYSA-N 0.000 claims description 2
- 239000000975 dye Substances 0.000 claims description 2
- 238000005286 illumination Methods 0.000 claims description 2
- CHQMHPLRPQMAMX-UHFFFAOYSA-L sodium persulfate Substances [Na+].[Na+].[O-]S(=O)(=O)OOS([O-])(=O)=O CHQMHPLRPQMAMX-UHFFFAOYSA-L 0.000 claims description 2
- 229910052724 xenon Inorganic materials 0.000 claims description 2
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- 230000000694 effects Effects 0.000 abstract description 9
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- 238000004065 wastewater treatment Methods 0.000 abstract description 2
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J27/00—Catalysts comprising the elements or compounds of halogens, sulfur, selenium, tellurium, phosphorus or nitrogen; Catalysts comprising carbon compounds
- B01J27/24—Nitrogen compounds
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/20—Catalysts, in general, characterised by their form or physical properties characterised by their non-solid state
- B01J35/23—Catalysts, in general, characterised by their form or physical properties characterised by their non-solid state in a colloidal state
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J35/00—Catalysts, in general, characterised by their form or physical properties
- B01J35/30—Catalysts, in general, characterised by their form or physical properties characterised by their physical properties
- B01J35/39—Photocatalytic properties
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
- C02F2101/345—Phenols
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/10—Photocatalysts
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- Environmental & Geological Engineering (AREA)
- Hydrology & Water Resources (AREA)
- Life Sciences & Earth Sciences (AREA)
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Abstract
The invention relates to a method for treating organic wastewater based on activated peroxydisulfate of a non-metal composite catalytic material, which adds carbon-doped g-C of the non-metal composite catalytic material into wastewater containing organic pollutants3N4(CNC) stirring the mixture under the irradiation of a full-spectrum light source at room temperature, adding peroxodisulfate, and degrading organic pollutants under the irradiation of light, wherein the method can quickly activate PDS in the system to generate a large amount of SO4 .‑，.OH，O2 .‑And are and1O2the pollutants are attacked by free radicals and are rapidly oxidized and degraded; the method has good removal effect on organic pollutant wastewater such as PPCPs and the like; the invention can efficiently remove organic pollutants under neutral pH, and is more in line with the actual wastewater treatment; the photocatalytic degradation can realize high-efficiency and clean utilization of solar energy. The application of the invention has very important significance for solving the current energy crisis and environmental pollution.
Description
Technical Field
The invention relates to a method for treating organic wastewater by activating peroxydisulfate based on a non-metal composite catalytic material, belonging to the technical field of chemistry and environment.
Background
PPCPs are short for drugs and personal care products, and are a large class of pollutants which widely exist in natural environment, can stably exist in nature and are difficult to biodegrade, and finally cause harm through biological chain enrichment, and the pollutants are removed and simultaneously are continuously introduced into the environment, and are also called as 'pseudo-persistent' pollutants. Therefore, how to efficiently remove the PPCPs in the degraded water body is an urgent problem to be solved in the current environmental protection work. The existing chemical method is generally adopted to treat the PPCPs in the water body, and although the chemical method has good effect on treating the PPCPs, a large amount of reagents are consumed, the application cost is high, and secondary pollution is possibly caused.
With the rapid development of industrialization, the conditions of energy shortage and environmental pollution are increasingly severe. The photocatalytic technology has become a hot topic studied in the field of environmental protection as a relatively advanced environmental management technology. The advantages of the photocatalysis technology in environmental management and application are of great significance in effectively solving the current energy crisis and environmental pollution.
The photocatalytic oxidation technology has the characteristics of high degradation efficiency, simple operation, direct utilization of sunlight and the like, and has very wide attention in the aspects of treating environmental treatment such as atmospheric pollutants, wastewater pollutants and the like. Various photocatalysts have therefore been extensively studied, such as metal oxides, metal sulfides, noble metals, and the like. However, the metal photocatalyst has high cost and is easy to leak metal to cause secondary pollution. As a substitute of a metal photocatalyst, the metal-free photocatalyst has a wide application prospect in the field of environmental remediation as a green catalyst. At present, the application of the photocatalytic technology in the field of environmental remediation still has the following defects that (1) the solar energy utilization rate of the photocatalyst is low; (2) the photocatalyst photogenerated electron hole pair is quickly compounded; (3) the adding amount of the photocatalyst is large. Thus, an effective non-metallic photocatalyst is essential. In addition, as the times progress and the human demand increases, organic pollutants in the environment, in addition to conventional pollutants, new pollutants such as drugs and personal care products (PPCPs), Endocrine Disruptors (EDCs), perfluorinated compounds (PFCs), brominated flame retardants (BRPs), and the like, are discharged into wastewater to threaten human health. Traditional water treatment technologies cannot eliminate these new pollutants because they do not take such pollutants into account, which has increased the demand for new water treatment technologies, and it is more desirable in the times to achieve an efficient to effective transition of water treatment technologies.
The advanced oxidation technology based on the activated persulfate has the advantages of high oxidation-reduction potential of generated free radicals, simple and convenient generation, wide pH application range and the like, and becomes a new technology for treating persistent organic pollutants. The traditional activation methods include heat activation, alkali activation, ultraviolet light activation, transition metal activation and the like. Among them, the transition metal activation method has attracted much attention because of its mild reaction conditions, simple operation, and high catalytic efficiency. However, the introduced metal ions need further post-treatment after the reaction is finished, so that the operation cost is increased, and the risk of metal pollution in the effluent is increased, so that the nonmetal catalyst brings a new way for activating persulfate. The non-metal catalyst is excited by light to generate photo-generated electrons which are received by persulfate, so that the persulfate is activated. In summary, photocatalytic (non-metal) technology coupled with persulfate advanced oxidation technology is considered as one of the water treatment technologies.
At present, g-C3N4Is widely researched as an environment-friendly visible light response nonmetal photocatalyst. g-C3N4Stable physical and chemical properties, low cost and simple preparation. With conventional TiO2Comparative example g-C3N4Can effectively activate molecular oxygen to generate superoxide radical, and is used for photocatalytic conversion of organic functional groups and photocatalytic degradation of organic pollutants. Reported in the literature, g-C3N4Can directly convert energy activation into photo-generated electron-activated Persulfate (PS) to form g-C3N4the/PS system improves the photocatalytic performance of the system. But g-C3N4The light absorption range of the light source is small, and the light isThe electron-generating hole pairs are easy to recombine, and the system efficiency still needs to be improved. Therefore, it is necessary to control g-C3N4The modification is carried out to improve the light absorption range and the separation efficiency of the photo-generated electron hole pairs. Chinese patent document CN113231096A discloses a g-C3N4A metal hydroxide composite photocatalyst and application thereof in reducing chromium (VI). The catalyst is prepared by the reaction of a nitrogen-containing precursor, urea and soluble metal salt, namely, a metal hydroxide and g-C3N4The heterojunction is formed between the two layers, so that the separation capability of the photo-generated electron hole pair is promoted, and the chromium (VI) can be reduced by photocatalysis. Chinese patent document CN104209136A discloses a TiO2Porous g-C3N4The composite material improves the quantum efficiency of the catalytic material and increases the specific surface area of the catalytic material. However, the separation capability of the photo-generated electron hole pair is improved by introducing the metal compound, and the risk of metal pollution in the effluent is invisibly increased; relating to the development of non-metals g-C3N4The patents for catalysts are less. In addition, due to the wide variety of organic pollutants in today's water environment, highly efficient photocatalytic systems are essential.
Therefore, there is a need to develop an excellent non-metallic photocatalyst, which can be suitable for degrading organic pollutants in water environment.
Disclosure of Invention
Aiming at the defects of the prior art, the invention provides a method for treating organic wastewater by activating peroxydisulfate based on a non-metal composite catalytic material.
The method of the invention is based on the doping of g-C with non-metallic carbon3N4(CNC) composite catalytic material, carbon doping with g-C3N4The nonmetal composite catalytic material is coupled with persulfate, namely a CNC-PDS system, so that solar energy can be more fully utilized to treat organic wastewater, and the efficient and clean utilization of the solar energy is realized.
In order to realize the purpose, the invention is realized by the following technical scheme:
the method for treating organic wastewater by activating peroxydisulfate based on the nonmetal composite catalytic material comprises the following steps:
adding carbon-doped g-C of non-metallic composite catalytic material into wastewater containing organic pollutants3N4(CNC) stirring the mixture under the conditions of room temperature, pH of 3.0-9.0 and full-spectrum light irradiation, adding peroxydisulfate after adsorption balance, degrading organic pollutants under the condition of light irradiation, and doping the nonmetal composite catalytic material with carbon to obtain g-C3N4Is added in an amount to dope the carbon in the system with g-C3N4The concentration of (A) is 0.075-0.5g/L and the concentration of peroxodisulfate in the system is 0.1-0.5 g/L.
According to the invention, the wastewater containing organic pollutants is preferably wastewater containing PPCPs, bisphenol A or organic dyes; the concentration of the pollutants in the wastewater is 10-40 mg/L.
According to a preferred embodiment of the invention, the persulfate is sodium persulfate.
According to the invention, the concentration of peroxodisulfate in the system is preferably from 0.1 to 0.2g/L,
most preferably, the concentration of peroxodisulfate in the system is 0.2 g/L.
According to the invention, the non-metallic composite catalytic material is preferably doped with carbon3N4Is added in an amount to dope the carbon in the system with g-C3N4The concentration of (A) is 0.12-0.5 g/L.
Most preferably, the non-metallic composite catalytic material is carbon-doped g-C3N4Is added in an amount to dope the carbon in the system with g-C3N4The concentration of (2) was 0.25 g/L.
Preferably, according to the invention, the initial pH of the waste water is between 5 and 7.
Preferably, the light source of the full spectrum light according to the present invention is sunlight or a xenon lamp.
Carbon-doped g-C of non-metal composite catalytic material3N4Is prepared by the following method:
(1) calcining melamine in nitrogen atmosphere to obtain yellowish solid, grinding into powder to obtain g-C3N4；
(2) Taking g-C3N4And glucose in deionized water for 30min-1 h;
(3) transferring the solution after ultrasonic treatment to a high-pressure kettle, adding ammonia water, and uniformly stirring;
(4) placing the high-pressure autoclave in a blast drying box, carrying out hydrothermal reaction at the temperature of 120-200 ℃, and centrifugally drying after the reaction is finished to obtain the carbon-doped g-C of the non-metal composite catalytic material3N4；
Preferably, according to the invention, in step (1), the melamine calcination temperature is 500-550 ℃, and the temperature rise rate is 2.5-5 ℃/min.
Preferably, according to the invention, in step (2), g to C3N4The mass ratio of the glucose to the glucose is 0.1-7.2: 1.
Further preferably, in step (2), g to C3N4The mass ratio of the glucose to the glucose is 0.5-5.4: 1.
Preferably, according to the invention, in step (3), the amount of ammonia added is between 2 and 10 ml.
Further preferably, the amount of ammonia added is 5 to 10 ml.
According to the invention, the hydrothermal reaction temperature is 150-180 ℃, and the hydrothermal time is 2-5 h.
The invention is based on the carbon doping g-C of the non-metal composite catalytic material3N4(CNC) activation of peroxydisulfates, carbon doping of g-C3N4C-O is introduced into (CNC) and serves as an electron-withdrawing group, an active site is added for PDS activation, and a UV-Vis result shows that the CNC light absorption range is red-shifted and can absorb light with the wavelength less than 550 nm; 180-3CNC2.4Is excited and transferred to CB (conduction band) to form e-/h+And (4) carrying out pairing. Direct transfer of electrons from the valence band to S2O8 2-Or indirectly through C ═ O transfer, SO that the transfer speed of photo-generated electrons is accelerated, and PDS is quickly activated, and after PDS is quickly activated, a large amount of SO is generated4 .-，·OH，O2 .-And are and1O2the pollutants are attacked by free radicals and are rapidly oxidized and degraded.
The invention has the beneficial effects that:
1. the method is based on the carbon doping g-C of the non-metal composite catalytic material3N4(CNC) activation of peroxydisulfates, carbon doping of g-C3N4C ═ O is introduced into (CNC) and serves as an electron-withdrawing group, an active site is added for PDS activation, SO that the transfer speed of photo-generated electrons is accelerated, PDS is quickly activated, and after PDS is quickly activated, a large amount of SO is generated4 .-，.OH，O2 .-And are and1O2the pollutants are attacked by free radicals and are rapidly oxidized and degraded; the method has good removal effect on organic pollutant wastewater such as PPCPs and the like; can efficiently remove organic pollutants under neutral pH, and is more in line with the actual wastewater treatment.
2. The method is based on the carbon doping g-C of the non-metal composite catalytic material3N4(CNC) carbon doping with g-C3N4(CNC) has better stability and excellent catalytic performance. The light absorption range of the non-metallic material is redshifted, the reasonable development and the effective utilization of solar energy are realized, the recovery is easy, the reutilization is realized, the synthesis process is green, environment-friendly and efficient, the preparation method is simple, green and pollution-free, and the cost is low.
3. The method is based on the carbon doping g-C of the non-metal composite catalytic material3N4(CNC) is carried out, so that the high-efficiency and clean utilization of solar energy is realized, and a sustainable scheme is provided for the restoration of organic wastewater.
Drawings
FIG. 1 shows g-C under different preparation conditions3N4And XRD pattern of CNC;
FIG. 2 shows g-C under different preparation conditions3N4And an FT-IR spectrum of CNC;
FIG. 3 is g-C3N4(a) And CNC2.4(b) SEM picture of (1);
FIG. 4 shows g-C3N4And a uv-vis absorption spectrum of CNC;
FIG. 5 is g-C3N4And XPS spectra of CNC;
FIG. 6 is a graph showing the degradation effect of acetaminophen in different catalyst dosages in the application experimental examples;
FIG. 7 is a graph showing the effect of initial pH of acetaminophen degradation in different solutions in application examples;
fig. 8 is a graph of the degradation effect on different organic pollutants in application experimental examples (pH 7);
FIG. 9 is a diagram showing the recycling effect of materials in the experimental examples.
Detailed Description
The present invention will be further described with reference to the following detailed description of embodiments thereof, but not limited thereto, in conjunction with the accompanying drawings.
The starting materials used in the examples are all conventional commercial products.
Example 1:
the method for treating organic wastewater by activating peroxydisulfate based on the nonmetal composite catalytic material comprises the following steps:
adding carbon-doped g-C of non-metallic composite catalytic material into wastewater containing organic pollutants3N4(CNC) stirring the mixture under the conditions of room temperature, pH 5 and full spectrum light source irradiation, adding peroxydisulfate after adsorption balance, degrading organic pollutants under the irradiation of light, and doping the nonmetal composite catalytic material carbon with g-C3N4Is added in an amount to dope the carbon in the system with g-C3N4The concentration of (B) was 0.25g/L, and the concentration of peroxodisulfate in the system was 0.12 g/L.
Carbon-doped g-C of non-metal composite catalytic material3N4The (CNC) is prepared by the following method:
(1) calcining melamine under nitrogen atmosphere, grinding light yellow solid into powder to obtain g-C3N4。
(2) According to g-C3N4Weighing g-C with the mass ratio of 2.4 to glucose3N4Mixing with glucose, and ultrasonic treating in deionized water for 30min-1 h;
(3) transferring the solution after ultrasonic treatment to a high-pressure kettle, adding 10ml of ammonia water, and uniformly stirring;
(4) heating the autoclave in a forced air drying oven at 180 ℃ for 3 h;
(5) taking out the autoclave after the autoclave is cooled, and centrifugally drying the material to obtain the carbon-doped g-C3N4Composite photocatalyst marked as 180-3CNC2.4。
Example 2:
the method for treating organic wastewater by activating peroxydisulfate based on the non-metallic composite catalytic material is the same as that in example 1, except that:
carbon-doped g-C of non-metal composite catalytic material3N4In the preparation of (CNC), the hydrothermal reaction temperature is 180 ℃, the hydrothermal reaction time is 4h, and the carbon-doped g-C is prepared3N4Composite photocatalyst marked as 180-4CNC2.4。
Example 3:
the method for treating organic wastewater by activating peroxydisulfate based on the non-metallic composite catalytic material is the same as that in example 1, except that:
carbon-doped g-C of non-metal composite catalytic material3N4In the preparation of (CNC), the hydrothermal reaction temperature is 180 ℃, the hydrothermal reaction time is 4h, and the carbon-doped g-C is prepared3N4Composite photocatalyst marked as 180-5CNC2.4。
Example 4:
the method for treating organic wastewater by activating peroxydisulfate based on the non-metallic composite catalytic material is the same as that in example 1, except that:
carbon-doped g-C of non-metal composite catalytic material3N4In the preparation of (CNC), the hydrothermal reaction temperature is 180 ℃, the hydrothermal reaction time is 4h, and the carbon-doped g-C is prepared3N4Composite photocatalyst marked as 180-2CNC2.4。
Example 5:
the method for treating organic wastewater by activating peroxydisulfate based on the non-metallic composite catalytic material is the same as that in example 1, except that:
carbon-doped g-C of non-metal composite catalytic material3N4In the preparation of (CNC), the hydrothermal reaction temperature is 150 ℃, the hydrothermal reaction time is 3h, and the carbon-doped g-C is prepared3N4Composite photocatalyst, marked as 150-3CNC2.4。
Experimental example 1 characterization
Carbon doped g-C3N4The XRD, FT-IR spectrum, SEM image, ultraviolet visible absorption spectrum and XPS spectrum of the composite photocatalyst are shown in figures 1-5, 2 theta (13.1 degrees) (100) and 2 theta (27.6 degrees) with two g-C are observed in the XRD spectrum of figure 13N4Characteristic peak, after hydrothermal treatment, the intensity of the (100) diffraction peak decreases until disappearance, and some secondary peaks were observed at 2 θ ═ 6.2 °,2 θ ═ 12.3 °,2 θ ═ 21.3 °, and the like, which may be g — C3N4The cause of hydrolysis and melem formation. As shown in fig. 2, CNC2.4The sample is at 3400cm-1The peak value of (the characteristic peak of carbon) is higher than g-C3N4Indicating successful carbon loading on g-C3N 4. By the pair g-C3N4And CNC2.4Carrying out morphology analysis and finding CNC2.4The surface is provided with a plurality of spherical and rice-shaped substances which are probably formed into carbon loaded in different shapes, and further confirms that the carbon is successfully loaded in g-C3N4The above.
Visible in the ultraviolet-visible diffuse reflectance spectrum, CNC2.4Has a red shift in light absorption range compared with g-C3N4More visible light can be absorbed.
Example 6:
the method for treating organic wastewater by activating peroxydisulfate based on the non-metallic composite catalytic material is the same as that in example 1, except that:
carbon-doped g-C of non-metal composite catalytic material3N4Is added in an amount to dope the carbon in the system with g-C3N4The concentration of (B) was 0.125 g/L.
Example 7:
the method for treating organic wastewater by activating peroxydisulfate based on the non-metallic composite catalytic material is the same as that in example 1, except that:
carbon-doped g-C of non-metal composite catalytic material3N4Is added in an amount to dope the carbon in the system with g-C3N4The concentration of (2) was 0.5 g/L.
Example 8:
the method for treating organic wastewater by activating peroxydisulfate based on the non-metallic composite catalytic material is the same as that in example 1, except that:
the concentration of the peroxodisulfate in the system was 0.2 g/L.
Examples of the experiments
Paracetamol degradation experiment
200mL of a simulated wastewater (wastewater containing PPCPs) containing 10mg/L of acetaminophen as a contaminant was treated by the method of example 1, and 1mL of a sample was taken from a sampling tube at various reaction time points, and 1mL of methanol was added to terminate the catalytic reaction, followed by filtration through a filter membrane and measurement of the concentration of remaining acetaminophen by high performance liquid chromatography.
And (3) testing results:
different CNC2.4The acetaminophen degradation effect of the additive amount is shown in fig. 5, and the acetaminophen degradation efficiency increases with increasing catalyst addition. When CNC2.4When the addition amount is 0.5g/L, the acetaminophen is completely degraded only after ten minutes of light irradiation.
Under the same experimental conditions, comparative degradation experiments (pH 7) were performed on different representative contaminants, as shown in fig. 6, CNC2.4Exhibit different adsorption capacities for different contaminants due to the difference in intermolecular electrostatic forces. After illumination, X-3B, BPA, RB5 were completely removed in 30min and the degradation rates for CIP, MO and MB were 84%, 98.4% and 97.8% within 40min, respectively. These results indicate that organic contaminants can be removed efficiently in this system.
Cyclic utilization experiment
In order to research the stability of the material, the used material is recycled, cleaned and dried, and finally, the degradation effect of the acetaminophen can still reach 92.4% after the material is used for three times.
Claims (10)
1. The method for treating organic wastewater by activating peroxydisulfate based on the nonmetal composite catalytic material comprises the following steps:
adding carbon-doped g-C of non-metallic composite catalytic material into wastewater containing organic pollutants3N4(CNC) under the conditions of room temperature, pH 3.0-9.0, full spectrum light source irradiationStirring, adding peroxodisulfate after adsorption balance, degrading organic pollutant under illumination, and doping g-C in non-metal composite catalytic material3N4Is added in an amount to dope the carbon in the system with g-C3N4The concentration of (A) is 0.075-0.5g/L and the concentration of peroxodisulfate in the system is 0.1-0.5 g/L.
2. The method of claim 1, wherein the wastewater containing organic contaminants is wastewater containing PPCPs, bisphenol a or organic dyes; the concentration of the pollutants in the wastewater is 10-40 mg/L.
3. The method according to claim 1, wherein the persulfate is sodium persulfate; the concentration of the peroxodisulfate in the system is 0.1-0.2 g/L.
4. The method of claim 1, wherein the non-metallic composite catalytic material is carbon doped g-C3N4Is added in an amount to dope the carbon in the system with g-C3N4The concentration of (A) is 0.12-0.5 g/L; preferably, the non-metallic composite catalytic material is doped with carbon3N4Is added in an amount to dope the carbon in the system with g-C3N4The concentration of (2) was 0.25 g/L.
5. The method of claim 1, wherein the initial pH of the wastewater is 5 to 7 and the source of the full spectrum light is sunlight or xenon.
6. The method of claim 1, wherein the non-metallic composite catalytic material is carbon doped g-C3N4Is prepared by the following method:
(1) calcining melamine in nitrogen atmosphere to obtain yellowish solid, grinding into powder to obtain g-C3N4；
(2) Taking g-C3N4And glucose in deionized water for 30min-1 h;
(3) transferring the solution after ultrasonic treatment to a high-pressure kettle, adding ammonia water, and uniformly stirring;
(4) placing the high-pressure autoclave in a blast drying box, carrying out hydrothermal reaction at the temperature of 120-200 ℃, and centrifugally drying after the reaction is finished to obtain the carbon-doped g-C of the non-metal composite catalytic material3N4。
7. The method as claimed in claim 1, wherein in step (1), the melamine calcination temperature is 500-550 ℃ and the temperature rise rate is 2.5-5 ℃/min.
8. The method according to claim 1, wherein in step (2), g-C3N4The mass ratio of the glucose to the glucose is 0.1-7.2: 1; preferably, in step (2), g to C3N4The mass ratio of the glucose to the glucose is 0.5-5.4: 1.
9. The method according to claim 1, wherein the amount of the aqueous ammonia added in step (3) is 2 to 10ml, preferably 5 to 10 ml.
10. The method as claimed in claim 1, wherein the hydrothermal reaction temperature is 150 ℃ and 180 ℃ and the hydrothermal time is 2-5 h.
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