CN113582324A - Method for removing organic pollutants in water by using sunlight - Google Patents
Method for removing organic pollutants in water by using sunlight Download PDFInfo
- Publication number
- CN113582324A CN113582324A CN202110918359.7A CN202110918359A CN113582324A CN 113582324 A CN113582324 A CN 113582324A CN 202110918359 A CN202110918359 A CN 202110918359A CN 113582324 A CN113582324 A CN 113582324A
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- CN
- China
- Prior art keywords
- titanium dioxide
- organic pollutants
- sunlight
- water
- carbon nitride
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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Images
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- 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
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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
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
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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
- C02F1/66—Treatment of water, waste water, or sewage by neutralisation; pH adjustment
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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
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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
- C02F1/722—Oxidation by peroxides
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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
- C02F1/76—Treatment of water, waste water, or sewage by oxidation with halogens or compounds of halogens
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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
- C02F1/78—Treatment of water, waste water, or sewage by oxidation with ozone
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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
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Abstract
A method for removing organic pollutants in water by utilizing sunlight relates to a method for removing organic pollutants in water. The invention aims to solve the problems that the light which is photolyzed by the existing oxidant is limited to an ultraviolet band, and the visible light in sunlight cannot effectively photolyze the oxidant to generate active substances such as free radicals and the like. The preparation method comprises the following steps: firstly, preparing a titanium dioxide/graphite phase carbon nitride heterojunction; secondly, adding a heterojunction of titanium dioxide/graphite phase carbon nitride and an oxidant into water containing organic pollutants; thirdly, removing under the irradiation of simulated sunlight; fourthly, filtering. The invention is used for removing organic pollutants in water by utilizing sunlight.
Description
Technical Field
The invention relates to a method for removing organic pollutants in water.
Background
Conventional processes in water and sewage plants, such as coagulation, sedimentation, filtration, disinfection and biodegradation, have difficulty in removing organic contaminants, such as persistent organics, pharmaceuticals and personal care products, from water. Although the ultraviolet-based advanced oxidation technology can effectively remove organic pollutants in water, the ultraviolet lamp has the problems of short service life, high energy consumption, secondary mercury pollution and the like, and sunlight is used as a renewable energy source in the nature, so that the defects of the ultraviolet lamp can be effectively overcome, and the ultraviolet lamp has a wide application prospect. However, the light that acts to photolyze the oxidant is limited to the ultraviolet band, and the visible light that occupies most of the energy of the entire spectrum of sunlight cannot effectively photolyze the oxidant to generate active species such as radicals, and thus the use of sunlight is limited at present.
Disclosure of Invention
The invention provides a method for removing organic pollutants in water by utilizing sunlight, aiming at solving the problems that the light which is used for photolysis of an existing oxidant is limited to an ultraviolet band, and the visible light in the sunlight cannot effectively photolyze the oxidant to generate active substances such as free radicals.
A method for removing organic pollutants in water by utilizing sunlight is carried out according to the following steps:
firstly, preparing a titanium dioxide/graphite phase carbon nitride heterojunction by using titanium dioxide and melamine as raw materials;
secondly, adding a titanium dioxide/graphite phase carbon nitride heterojunction and an oxidant into water containing organic pollutants, and adjusting the pH of the solution to 6.5-7.5 to obtain an adjusted solution;
the molar ratio of the oxidant to the organic pollutants is (1-20) to 1;
thirdly, removing the adjusted solution for 20-60 min under the conditions of simulating sunlight irradiation and stirring;
and fourthly, filtering to remove the heterojunction of the titanium dioxide/graphite phase carbon nitride to obtain the treated solution.
The invention has the beneficial effects that:
the invention aims to add a titanium dioxide/graphite phase carbon nitride heterojunction into a sunlight/oxidant system to form a sunlight/oxidant/heterojunction composite system and enhance the removal of organic pollutants in water by the sunlight/oxidant. Titanium dioxide and graphite phase carbon nitride are two widely studied photocatalysts and have the advantages of no toxicity, stable property, low price and the like. The heterojunction formed by titanium dioxide and graphite-phase carbon nitride can improve the absorption of the titanium dioxide in a visible light wave band, thereby improving the utilization rate of sunlight, effectively preventing photo-generated electrons from generating a composite reaction with photo-generated holes to cause energy dissipation, consuming the photo-generated electrons by an oxidant to further inhibit the recombination reaction, simultaneously activating and decomposing the photo-generated electrons to generate active species with strong oxidizing property, effectively removing organic pollutants in water, and removing the water containing the organic pollutants with the concentration of 10 mu mol/L within 60min to obtain the removal rate of more than 95%.
The invention is used for a method for removing organic pollutants in water by utilizing sunlight.
Drawings
FIG. 1 is a transmission electron micrograph of a titanium dioxide/graphite phase carbon nitride heterojunction prepared according to one step one of the example.
Detailed Description
The first embodiment is as follows: the embodiment of the method for removing the organic pollutants in the water by utilizing the sunlight comprises the following steps:
firstly, preparing a titanium dioxide/graphite phase carbon nitride heterojunction by using titanium dioxide and melamine as raw materials;
secondly, adding a titanium dioxide/graphite phase carbon nitride heterojunction and an oxidant into water containing organic pollutants, and adjusting the pH of the solution to 6.5-7.5 to obtain an adjusted solution;
the molar ratio of the oxidant to the organic pollutants is (1-20) to 1;
thirdly, removing the adjusted solution for 20-60 min under the conditions of simulating sunlight irradiation and stirring;
and fourthly, filtering to remove the heterojunction of the titanium dioxide/graphite phase carbon nitride to obtain the treated solution.
The amount of the titanium dioxide/graphite phase carbon nitride heterojunction added in step two can be determined according to the initial concentration of the specific organic contaminant and the ease of removal.
The molar ratio of oxidant to organic contaminant in step two may be determined based on the initial concentration of the particular organic contaminant and the ease of removal.
The beneficial effects of the embodiment are as follows:
the purpose of the embodiment is to add a titanium dioxide/graphite phase carbon nitride heterojunction into a sunlight/oxidant system to form a sunlight/oxidant/heterojunction composite system, so as to enhance the removal of organic pollutants in water by the sunlight/oxidant. Titanium dioxide and graphite phase carbon nitride are two widely studied photocatalysts and have the advantages of no toxicity, stable property, low price and the like. The heterojunction formed by titanium dioxide and graphite-phase carbon nitride can improve the absorption of the titanium dioxide in a visible light wave band, thereby improving the utilization rate of sunlight, effectively preventing photo-generated electrons from generating a composite reaction with photo-generated holes to cause energy dissipation, consuming the photo-generated electrons by an oxidant to further inhibit the recombination reaction, simultaneously activating and decomposing the photo-generated electrons to generate active species with strong oxidizing property, effectively removing organic pollutants in water, and removing the water containing the organic pollutants with the concentration of 10 mu mol/L within 60min to obtain the removal rate of more than 95%.
The second embodiment is as follows: the first difference between the present embodiment and the specific embodiment is: the titanium dioxide in the step one is rutile type titanium dioxide, anatase type titanium dioxide and brookite type titanium dioxide. The rest is the same as the first embodiment.
The third concrete implementation mode: this embodiment is different from the first or second embodiment in that: in the first step, titanium dioxide and melamine are used as raw materials, and the titanium dioxide/graphite phase carbon nitride heterojunction is obtained by calcining for 2-4 hours at the calcining temperature of 300-600 ℃. The other is the same as in the first or second embodiment.
The fourth concrete implementation mode: the difference between this embodiment mode and one of the first to third embodiment modes is: the mass ratio of the titanium dioxide to the melamine in the step one is 1 (0.1-20). The other is the same as in the first or second embodiment.
The fifth concrete implementation mode: the difference between this embodiment and one of the first to fourth embodiments is: the dosage of the titanium dioxide/graphite phase carbon nitride heterojunction in the second step is 5 mg/L-2000 mg/L. The rest is the same as the first to fourth embodiments.
The sixth specific implementation mode: the present embodiment is different from one or more of the first to fifth embodiments in that: the molar ratio of the oxidant to the organic pollutants in the second step is (1-10): 1. The rest is the same as the first to fifth embodiments.
The seventh embodiment: the difference between this embodiment and one of the first to sixth embodiments is: the oxidant in the second step is hydrogen peroxide, ozone, sodium percarbonate, peroxymonosulfate, peroxydisulfate, peroxyacetic acid, sodium hypochlorite, chlorine dioxide, potassium iodate, potassium periodate, potassium ferrate or potassium permanganate. The others are the same as the first to sixth embodiments.
The specific implementation mode is eight: the present embodiment differs from one of the first to seventh embodiments in that: the organic pollutant in the second step is nitrobenzene, carbamazepine, naproxen, ibuprofen, ketoprofen, benzoic acid, phthalic acid, dimethyl phthalate, diethyl phthalate, dibutyl phthalate, nonyl phenol, 17 alpha-ethinyl estradiol, atenolol, metoprolol, propranolol, chlormidone, paracetamol, antipyrine, trimethoprim, sulfadiazine, sulfamethoxazole, metronidazole, gemfibrozil, bezafibrate, diclofenac, clofibric acid, chloramphenicol, 4-chlorophenol, 2, 4-dichlorophenol, 2,4, 6-trichlorophenol, iopromide, iohexol, sodium diatrizoate, iodixanol, caffeine, atrazine, fruits, parathion, dichlorvos, glyphosate, chlorpyrifos, deltamethrin, dichlorflubenz, bisphenol A, bisphenol S, bisphenol A, and chlorpyrifos, One or more of bisphenol AF, roxarsone and p-amino phenylarsonic acid. The rest is the same as the first to seventh embodiments.
The specific implementation method nine: the present embodiment differs from the first to eighth embodiments in that: the stirring condition in the third step is 300 rpm-600 rpm; the simulated sunlight irradiation in the third step is irradiation by using a xenon lamp light source. The other points are the same as those in the first to eighth embodiments.
The detailed implementation mode is ten: the present embodiment differs from one of the first to ninth embodiments in that: the filtration in the fourth step is specifically the filtration by using a hydrophilic membrane with a pore size of 0.22 μm. The other points are the same as those in the first to ninth embodiments.
The following examples were used to demonstrate the beneficial effects of the present invention:
the first embodiment is as follows:
a method for removing organic pollutants in water by utilizing sunlight is carried out according to the following steps:
firstly, calcining titanium dioxide and melamine serving as raw materials for 3 hours at the calcining temperature of 500 ℃ to obtain a titanium dioxide/graphite phase carbon nitride heterojunction;
the mass ratio of the titanium dioxide to the melamine is 1: 0.4;
secondly, adding a titanium dioxide/graphite phase carbon nitride heterojunction and an oxidant into water containing organic pollutants with the concentration of 10 mu mol/L, and adjusting the pH value of the solution to 7.0 to obtain an adjusted solution;
the molar ratio of the oxidant to the organic pollutants is 10: 1;
thirdly, removing the adjusted solution for 40min under the conditions of simulating sunlight irradiation and stirring;
and fourthly, filtering to remove the heterojunction of the titanium dioxide/graphite phase carbon nitride to obtain the treated solution.
The titanium dioxide in the first step is anatase titanium dioxide.
The dosage of the titanium dioxide/graphite phase carbon nitride heterojunction in the step two is 20 mg/L.
And the oxidant in the second step is peroxymonosulfate.
And the organic pollutant in the second step is ibuprofen.
The stirring condition in the third step is magnetic stirring at 600 rpm; the simulated sunlight irradiation in the third step is specifically irradiation by using a 50W xenon lamp light source, wherein the main wavelength of the xenon lamp light source is concentrated in a visible light waveband.
The filtration in the fourth step is specifically the filtration by using a hydrophilic membrane with a pore size of 0.22 μm.
FIG. 1 is a transmission electron micrograph of a titanium dioxide/graphite phase carbon nitride heterojunction prepared according to step one of the example; as can be seen from the figure, two different crystal planes exist, namely a 101 crystal plane of titanium dioxide and a 002 crystal plane of graphite-phase carbon nitride, which indicates that the iso-junction is successfully prepared.
The concentration of ibuprofen in the solution treated in this example was 0.9. mu. mol/L, and the removal rate was 91%.
Example two: the difference between the present embodiment and the first embodiment is: the molar ratio of the oxidant to the organic pollutants in the step two is 5: 1; the organic pollutant in the step two is carbamazepine; the oxidant in the step two is sodium hypochlorite; the dosage of the titanium dioxide/graphite phase carbon nitride heterojunction in the second step is 10 mg/L; the adjusted solution was removed for 20min in step three. The rest is the same as the first embodiment.
The concentration of carbamazepine in the solution treated in the example was 0.4. mu. mol/L, and the removal rate was 96%.
Example three: the embodiment is different from the embodiment one: the molar ratio of the oxidant to the organic pollutants in the step two is 6: 1; the dosage of the titanium dioxide/graphite phase carbon nitride heterojunction in the second step is 50 mg/L; the oxidant in the step two is peroxydisulfate; the organic pollutant in the step two is metoprolol; the adjusted solution was removed for 30min in step three. The rest is the same as the first embodiment.
The metoprolol concentration in the solution treated in this example was 0.2. mu. mol/L, and the removal rate was 98%.
Comparison experiment one: the comparative experiment differs from the first example in that: and in the second step, a heterojunction of titanium dioxide/graphite phase carbon nitride is not added. The rest is the same as the first embodiment.
The concentration of ibuprofen in the solution treated by the comparative experiment is 5.2 mu mol/L, and the removal rate is 48%.
Comparative experiment two: the difference between this comparative experiment and example two is that: and in the second step, a heterojunction of titanium dioxide/graphite phase carbon nitride is not added. The other steps are the same as those of the embodiment.
The concentration of carbamazepine in the solution treated by the comparative experiment is 4.9 mu mol/L, and the removal rate is 51 percent.
A third comparative experiment: the difference between this comparative experiment and the third example is that: and in the second step, a heterojunction of titanium dioxide/graphite phase carbon nitride is not added. The other steps are the same as those of the embodiment.
The concentration of metoprolol in the solution treated by the comparative experiment is 3.8 mu mol/L, and the removal rate is 62%.
Claims (10)
1. A method for removing organic pollutants in water by utilizing sunlight is characterized by comprising the following steps:
firstly, preparing a titanium dioxide/graphite phase carbon nitride heterojunction by using titanium dioxide and melamine as raw materials;
secondly, adding a titanium dioxide/graphite phase carbon nitride heterojunction and an oxidant into water containing organic pollutants, and adjusting the pH of the solution to 6.5-7.5 to obtain an adjusted solution;
the molar ratio of the oxidant to the organic pollutants is (1-20) to 1;
thirdly, removing the adjusted solution for 20-60 min under the conditions of simulating sunlight irradiation and stirring;
and fourthly, filtering to remove the heterojunction of the titanium dioxide/graphite phase carbon nitride to obtain the treated solution.
2. The method of claim 1, wherein the titanium dioxide in the first step is rutile type titanium dioxide, anatase type titanium dioxide, or brookite type titanium dioxide.
3. The method for removing organic pollutants in water by using sunlight as claimed in claim 1, wherein in the step one, titanium dioxide and melamine are used as raw materials, and the titanium dioxide/graphite phase carbon nitride heterojunction is obtained by calcining for 2-4 h at the calcining temperature of 300-600 ℃.
4. The method for removing organic pollutants in water by using sunlight as claimed in claim 1, wherein the mass ratio of the titanium dioxide to the melamine in the step one is 1 (0.1-20).
5. The method for removing organic pollutants from water by using sunlight as claimed in claim 1, wherein the dosage of the titanium dioxide/graphite phase carbon nitride heterojunction in the second step is 5mg/L to 2000 mg/L.
6. The method for removing organic pollutants in water by using sunlight as claimed in claim 1, wherein the molar ratio of the oxidant to the organic pollutants in the second step is (1-10): 1.
7. The method of claim 1, wherein the oxidizing agent in step two is hydrogen peroxide, ozone, sodium percarbonate, peroxymonosulfate, peroxydisulfate, peroxyacetic acid, sodium hypochlorite, chlorine dioxide, potassium iodate, potassium periodate, potassium ferrate, or potassium permanganate.
8. The method of claim 1, wherein the organic contaminant in step two is nitrobenzene, carbamazepine, naproxen, ibuprofen, ketoprofen, benzoic acid, phthalic acid, dimethyl phthalate, diethyl phthalate, dibutyl phthalate, nonylphenol, 17 α -ethynyl estradiol, atenolol, metoprolol, propranolol, paminone, paracetamol, antipyrine, trimethoprim, sulfadiazine, sulfamethoxazole, metronidazole, gemfibrozil, bezafibrate, diclofenac, clofibric acid, chloramphenicol, 4-chlorophenol, 2, 4-dichlorophen, 2,4, 6-trichlorophenol, iopromide, iohexol, sodium diatrizoate, iodixanol, caffeine, atrazine, and a, One or a mixture of more of dimethoate, parathion, dichlorvos, glyphosate, chlorpyrifos, deltamethrin, DDT, bisphenol A, bisphenol S, bisphenol AF, roxarsone and p-amino phenylarsonic acid.
9. The method for removing organic pollutants in water by using sunlight as claimed in claim 1, wherein the stirring condition in the third step is 300-600 rpm; the simulated sunlight irradiation in the third step is irradiation by using a xenon lamp light source.
10. The method for removing organic pollutants in water by using sunlight as claimed in claim 1, wherein the filtration in the fourth step is a hydrophilic membrane filtration with a pore size of 0.22 μm.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN113976160A (en) * | 2021-11-12 | 2022-01-28 | 哈尔滨工业大学 | Preparation method and application of two-dimensional photocatalytic film with heterostructure |
| CN116216665A (en) * | 2023-02-01 | 2023-06-06 | 四川农业大学 | Method for degrading trimethoprim by using advanced oxidation technology |
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| CN101791565A (en) * | 2010-03-30 | 2010-08-04 | 湘潭大学 | TiO2@ graphite phase carbon nitride heterojunction composite photocatalyst and preparation method thereof |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113976160A (en) * | 2021-11-12 | 2022-01-28 | 哈尔滨工业大学 | Preparation method and application of two-dimensional photocatalytic film with heterostructure |
| CN113976160B (en) * | 2021-11-12 | 2023-11-03 | 哈尔滨工业大学 | Preparation method and application of two-dimensional photocatalytic film with heterostructure |
| CN116216665A (en) * | 2023-02-01 | 2023-06-06 | 四川农业大学 | Method for degrading trimethoprim by using advanced oxidation technology |
| CN116216665B (en) * | 2023-02-01 | 2024-02-23 | 四川农业大学 | Method for degrading trimethoprim by using advanced oxidation technology |
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