CN114988554B - Method for removing organic pollutants in water by activating peroxyacetic acid through dielectric barrier discharge - Google Patents
Method for removing organic pollutants in water by activating peroxyacetic acid through dielectric barrier discharge Download PDFInfo
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- CN114988554B CN114988554B CN202210685765.8A CN202210685765A CN114988554B CN 114988554 B CN114988554 B CN 114988554B CN 202210685765 A CN202210685765 A CN 202210685765A CN 114988554 B CN114988554 B CN 114988554B
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- dielectric barrier
- barrier discharge
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- peracetic acid
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- KFSLWBXXFJQRDL-UHFFFAOYSA-N Peracetic acid Chemical compound CC(=O)OO KFSLWBXXFJQRDL-UHFFFAOYSA-N 0.000 title claims abstract description 150
- 230000004888 barrier function Effects 0.000 title claims abstract description 47
- 238000000034 method Methods 0.000 title claims abstract description 33
- 239000002957 persistent organic pollutant Substances 0.000 title claims abstract description 32
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 title claims abstract description 27
- 230000003213 activating effect Effects 0.000 title description 11
- 238000009832 plasma treatment Methods 0.000 claims abstract description 10
- 239000012467 final product Substances 0.000 claims abstract description 3
- 239000000356 contaminant Substances 0.000 claims description 17
- 229960005404 sulfamethoxazole Drugs 0.000 claims description 17
- JLKIGFTWXXRPMT-UHFFFAOYSA-N sulphamethoxazole Chemical compound O1C(C)=CC(NS(=O)(=O)C=2C=CC(N)=CC=2)=N1 JLKIGFTWXXRPMT-UHFFFAOYSA-N 0.000 claims description 17
- PAYRUJLWNCNPSJ-UHFFFAOYSA-N Aniline Chemical compound NC1=CC=CC=C1 PAYRUJLWNCNPSJ-UHFFFAOYSA-N 0.000 claims description 6
- JYGXADMDTFJGBT-VWUMJDOOSA-N hydrocortisone Chemical compound O=C1CC[C@]2(C)[C@H]3[C@@H](O)C[C@](C)([C@@](CC4)(O)C(=O)CO)[C@@H]4[C@@H]3CCC2=C1 JYGXADMDTFJGBT-VWUMJDOOSA-N 0.000 claims description 6
- YNPNZTXNASCQKK-UHFFFAOYSA-N phenanthrene Chemical compound C1=CC=C2C3=CC=CC=C3C=CC2=C1 YNPNZTXNASCQKK-UHFFFAOYSA-N 0.000 claims description 6
- YFSUTJLHUFNCNZ-UHFFFAOYSA-N perfluorooctane-1-sulfonic acid Chemical compound OS(=O)(=O)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)F YFSUTJLHUFNCNZ-UHFFFAOYSA-N 0.000 claims description 5
- SNGREZUHAYWORS-UHFFFAOYSA-N perfluorooctanoic acid Chemical compound OC(=O)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)C(F)(F)F SNGREZUHAYWORS-UHFFFAOYSA-N 0.000 claims description 5
- SEEPANYCNGTZFQ-UHFFFAOYSA-N sulfadiazine Chemical compound C1=CC(N)=CC=C1S(=O)(=O)NC1=NC=CC=N1 SEEPANYCNGTZFQ-UHFFFAOYSA-N 0.000 claims description 5
- 229960004306 sulfadiazine Drugs 0.000 claims description 5
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical compound C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 claims description 4
- DNXHEGUUPJUMQT-UHFFFAOYSA-N (+)-estrone Natural products OC1=CC=C2C3CCC(C)(C(CC4)=O)C4C3CCC2=C1 DNXHEGUUPJUMQT-UHFFFAOYSA-N 0.000 claims description 3
- PROQIPRRNZUXQM-UHFFFAOYSA-N (16alpha,17betaOH)-Estra-1,3,5(10)-triene-3,16,17-triol Natural products OC1=CC=C2C3CCC(C)(C(C(O)C4)O)C4C3CCC2=C1 PROQIPRRNZUXQM-UHFFFAOYSA-N 0.000 claims description 3
- BFPYWIDHMRZLRN-UHFFFAOYSA-N 17alpha-ethynyl estradiol Natural products OC1=CC=C2C3CCC(C)(C(CC4)(O)C#C)C4C3CCC2=C1 BFPYWIDHMRZLRN-UHFFFAOYSA-N 0.000 claims description 3
- VOXZDWNPVJITMN-ZBRFXRBCSA-N 17β-estradiol Chemical compound OC1=CC=C2[C@H]3CC[C@](C)([C@H](CC4)O)[C@@H]4[C@@H]3CCC2=C1 VOXZDWNPVJITMN-ZBRFXRBCSA-N 0.000 claims description 3
- DNXHEGUUPJUMQT-CBZIJGRNSA-N Estrone Chemical compound OC1=CC=C2[C@H]3CC[C@](C)(C(CC4)=O)[C@@H]4[C@@H]3CCC2=C1 DNXHEGUUPJUMQT-CBZIJGRNSA-N 0.000 claims description 3
- BFPYWIDHMRZLRN-SLHNCBLASA-N Ethinyl estradiol Chemical compound OC1=CC=C2[C@H]3CC[C@](C)([C@](CC4)(O)C#C)[C@@H]4[C@@H]3CCC2=C1 BFPYWIDHMRZLRN-SLHNCBLASA-N 0.000 claims description 3
- IGFHQQFPSIBGKE-UHFFFAOYSA-N Nonylphenol Natural products CCCCCCCCCC1=CC=C(O)C=C1 IGFHQQFPSIBGKE-UHFFFAOYSA-N 0.000 claims description 3
- 239000004098 Tetracycline Substances 0.000 claims description 3
- 229940039407 aniline Drugs 0.000 claims description 3
- MXWJVTOOROXGIU-UHFFFAOYSA-N atrazine Chemical compound CCNC1=NC(Cl)=NC(NC(C)C)=N1 MXWJVTOOROXGIU-UHFFFAOYSA-N 0.000 claims description 3
- 229960002537 betamethasone Drugs 0.000 claims description 3
- UREBDLICKHMUKA-DVTGEIKXSA-N betamethasone Chemical compound C1CC2=CC(=O)C=C[C@]2(C)[C@]2(F)[C@@H]1[C@@H]1C[C@H](C)[C@@](C(=O)CO)(O)[C@@]1(C)C[C@@H]2O UREBDLICKHMUKA-DVTGEIKXSA-N 0.000 claims description 3
- 229940106691 bisphenol a Drugs 0.000 claims description 3
- 229960004703 clobetasol propionate Drugs 0.000 claims description 3
- CBGUOGMQLZIXBE-XGQKBEPLSA-N clobetasol propionate Chemical compound C1CC2=CC(=O)C=C[C@]2(C)[C@]2(F)[C@@H]1[C@@H]1C[C@H](C)[C@@](C(=O)CCl)(OC(=O)CC)[C@@]1(C)C[C@@H]2O CBGUOGMQLZIXBE-XGQKBEPLSA-N 0.000 claims description 3
- 229930182833 estradiol Natural products 0.000 claims description 3
- 229960005309 estradiol Drugs 0.000 claims description 3
- PROQIPRRNZUXQM-ZXXIGWHRSA-N estriol Chemical compound OC1=CC=C2[C@H]3CC[C@](C)([C@H]([C@H](O)C4)O)[C@@H]4[C@@H]3CCC2=C1 PROQIPRRNZUXQM-ZXXIGWHRSA-N 0.000 claims description 3
- 229960001348 estriol Drugs 0.000 claims description 3
- 229960003399 estrone Drugs 0.000 claims description 3
- 229960002568 ethinylestradiol Drugs 0.000 claims description 3
- 229960002714 fluticasone Drugs 0.000 claims description 3
- MGNNYOODZCAHBA-GQKYHHCASA-N fluticasone Chemical compound C1([C@@H](F)C2)=CC(=O)C=C[C@]1(C)[C@]1(F)[C@@H]2[C@@H]2C[C@@H](C)[C@@](C(=O)SCF)(O)[C@@]2(C)C[C@@H]1O MGNNYOODZCAHBA-GQKYHHCASA-N 0.000 claims description 3
- 229960000890 hydrocortisone Drugs 0.000 claims description 3
- SNQQPOLDUKLAAF-UHFFFAOYSA-N nonylphenol Chemical compound CCCCCCCCCC1=CC=CC=C1O SNQQPOLDUKLAAF-UHFFFAOYSA-N 0.000 claims description 3
- 229960002180 tetracycline Drugs 0.000 claims description 3
- 229930101283 tetracycline Natural products 0.000 claims description 3
- 235000019364 tetracycline Nutrition 0.000 claims description 3
- 150000003522 tetracyclines Chemical class 0.000 claims description 3
- 229960002117 triamcinolone acetonide Drugs 0.000 claims description 3
- YNDXUCZADRHECN-JNQJZLCISA-N triamcinolone acetonide Chemical compound C1CC2=CC(=O)C=C[C@]2(C)[C@]2(F)[C@@H]1[C@@H]1C[C@H]3OC(C)(C)O[C@@]3(C(=O)CO)[C@@]1(C)C[C@@H]2O YNDXUCZADRHECN-JNQJZLCISA-N 0.000 claims description 3
- 230000004913 activation Effects 0.000 abstract description 13
- 150000003254 radicals Chemical class 0.000 abstract description 7
- 239000003814 drug Substances 0.000 abstract description 6
- 238000006243 chemical reaction Methods 0.000 abstract description 5
- 239000003344 environmental pollutant Substances 0.000 abstract description 5
- 231100000719 pollutant Toxicity 0.000 abstract description 5
- 150000001723 carbon free-radicals Chemical class 0.000 abstract description 4
- 239000000463 material Substances 0.000 abstract description 4
- 230000003197 catalytic effect Effects 0.000 abstract description 3
- 239000002351 wastewater Substances 0.000 abstract description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 abstract description 2
- 230000005389 magnetism Effects 0.000 abstract description 2
- 150000002831 nitrogen free-radicals Chemical class 0.000 abstract description 2
- 239000001301 oxygen Substances 0.000 abstract description 2
- 229910052760 oxygen Inorganic materials 0.000 abstract description 2
- 208000028659 discharge Diseases 0.000 description 41
- 238000001994 activation Methods 0.000 description 12
- -1 hydroxyl radicals Chemical class 0.000 description 10
- 239000000243 solution Substances 0.000 description 10
- 230000000694 effects Effects 0.000 description 8
- 230000008569 process Effects 0.000 description 7
- 238000007254 oxidation reaction Methods 0.000 description 5
- 230000015556 catabolic process Effects 0.000 description 4
- 230000003647 oxidation Effects 0.000 description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- 238000006731 degradation reaction Methods 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 2
- 239000003242 anti bacterial agent Substances 0.000 description 2
- 229940088710 antibiotic agent Drugs 0.000 description 2
- 239000006227 byproduct Substances 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- 229910021645 metal ion Inorganic materials 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical class C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000011259 mixed solution Substances 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 230000001590 oxidative effect Effects 0.000 description 2
- 239000000047 product Substances 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 230000002195 synergetic effect Effects 0.000 description 2
- 229920002994 synthetic fiber Polymers 0.000 description 2
- 231100000331 toxic Toxicity 0.000 description 2
- 230000002588 toxic effect Effects 0.000 description 2
- 239000002253 acid Substances 0.000 description 1
- 230000000844 anti-bacterial effect Effects 0.000 description 1
- 125000004429 atom Chemical group 0.000 description 1
- 239000003899 bactericide agent Substances 0.000 description 1
- 239000007844 bleaching agent Substances 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000013043 chemical agent Substances 0.000 description 1
- 230000005495 cold plasma Effects 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000007547 defect Effects 0.000 description 1
- 230000000593 degrading effect Effects 0.000 description 1
- 239000000645 desinfectant Substances 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 229940079593 drug Drugs 0.000 description 1
- 230000005684 electric field Effects 0.000 description 1
- 230000005672 electromagnetic field Effects 0.000 description 1
- 238000004134 energy conservation Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000003912 environmental pollution Methods 0.000 description 1
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 1
- TUJKJAMUKRIRHC-UHFFFAOYSA-N hydroxyl Chemical compound [OH] TUJKJAMUKRIRHC-UHFFFAOYSA-N 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 150000001451 organic peroxides Chemical class 0.000 description 1
- 239000007800 oxidant agent Substances 0.000 description 1
- 239000000575 pesticide Substances 0.000 description 1
- 230000002186 photoactivation Effects 0.000 description 1
- 238000000678 plasma activation Methods 0.000 description 1
- 125000005575 polycyclic aromatic hydrocarbon group Chemical group 0.000 description 1
- 230000005855 radiation Effects 0.000 description 1
- 230000035484 reaction time Effects 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 238000007725 thermal activation Methods 0.000 description 1
Classifications
-
- 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
-
- 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
- C02F1/305—Treatment of water, waste water, or sewage by irradiation with electrons
-
- 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
- C02F1/32—Treatment of water, waste water, or sewage by irradiation with ultraviolet light
-
- 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
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/30—Wastewater or sewage treatment systems using renewable energies
- Y02W10/37—Wastewater or sewage treatment systems using renewable energies using solar energy
Landscapes
- Life Sciences & Earth Sciences (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Health & Medical Sciences (AREA)
- Toxicology (AREA)
- Organic Low-Molecular-Weight Compounds And Preparation Thereof (AREA)
Abstract
The invention relates to a method for removing organic pollutants in water by utilizing dielectric barrier discharge activated peroxyacetic acid, which comprises the following steps: (1) Adding peracetic acid into water containing organic pollutants to obtain a solution containing peracetic acid; (2) And performing dielectric barrier discharge low-temperature plasma treatment on the solution containing the peroxyacetic acid to obtain the final product. The invention adds peracetic acid into the waste water containing organic pollutant, then carries out dielectric barrier discharge low-temperature plasma treatment, and uses dielectric barrier discharge low-temperature plasma to generate electrons, light, heat and magnetism, cooperatively activates peracetic acid to generate a series of active oxygen free radicals, active nitrogen free radicals and carbon free radicals, and carries out chemical reaction with the organic pollutant in the water to degrade and mineralize the pollutant. Compared with the prior art, the method has higher peroxyacetic acid activation efficiency, does not need additional medicament or catalytic material, and does not introduce secondary pollution.
Description
Technical Field
The invention belongs to the technical field of environmental pollution treatment, and relates to a method for removing organic pollutants in water by utilizing dielectric barrier discharge activated peroxyacetic acid.
Background
Peracetic acid is an organic peroxide with a strong pungent odor, and currently the more common commercial peracetic acid solution is a mixture containing peracetic acid, acetic acid, hydrogen peroxide and water. The peroxyacetic acid has higher oxidation potential (1.96V), has the potential of degrading organic pollutants in water, and is widely used as disinfectant, bleaching agent, bactericide, oxidant and the like. The peroxyacetic acid oxidation has the advantages of low pH dependence, simple process, less generation of toxic byproducts after oxidation, and the like. However, the peroxyacetic acid molecule has high selectivity and poor universal applicability to common organic pollutants. By activating peracetic acid in some way to break its O-O bond, various active radicals such as hydroxyl radicals, acyl radicals, peroxy acyl radicals, methyl radicals, peroxy methyl radicals, etc., can be generated more efficiently than peracetic acid molecules. Wherein, the hydroxyl radical has strong oxidizing property and no selectivity to organic pollutant degradation; the half-life of the organic radicals such as acyl radicals, peroxy acyl radicals, methyl radicals, peroxy methyl radicals and the like is long, and the organic pollutants in water can be decomposed for a long time. Thus, the activated peroxyacetic acid can significantly improve the treatment efficiency of the peroxyacetic acid molecules on the organic wastewater. The existing common peroxyacetic acid activation modes mainly comprise light activation, heat activation, metal ion activation, activated carbon fiber activation, novel synthetic material activation and the like. But photoactivation and thermal activation are less efficient; the metal ion activation, the activated carbon fiber activation, the novel synthetic material activation and the like need additional medicaments or materials, and secondary pollution is easy to cause. Therefore, other efficient and environment-friendly peroxyacetic acid activation methods need to be developed.
Disclosure of Invention
The invention aims to provide a method for removing organic pollutants in water by utilizing dielectric barrier discharge activated peroxyacetic acid, so as to overcome the defects of low efficiency or secondary pollution caused by the need of adding a medicament or a catalytic material in the peroxyacetic acid activation method in the prior art.
The aim of the invention can be achieved by the following technical scheme:
a method for removing organic pollutants in water by using dielectric barrier discharge activated peroxyacetic acid, comprising the following steps:
(1) Adding peracetic acid into water containing organic pollutants to obtain a solution containing peracetic acid;
(2) And performing dielectric barrier discharge low-temperature plasma treatment on the solution containing the peroxyacetic acid to obtain the final product.
Further, in the step (1), the organic pollutant is one or more of sulfamethoxazole, sulfadiazine, perfluoro caprylic acid, perfluoro octane sulfonic acid, tetracycline, fluticasone, triamcinolone acetonide, betamethasone, clobetasol propionate, hydrocortisone, nonylphenol, bisphenol a, estrone, estradiol, estriol, ethinyl estradiol, aniline, phenanthrene or atrazine.
Further, in the step (1), the molar ratio of the peroxyacetic acid to the organic pollutant is (0.1 to 50): 1.
further, in step (1), the molar ratio of the peroxyacetic acid to the organic contaminant is 1.5:1.
further, in step (1), the molar ratio of the peroxyacetic acid to the organic contaminant is 3:1.
further, in step (1), the molar ratio of the peroxyacetic acid to the organic contaminant is 4.5:1.
in the step (2), the dielectric barrier discharge output power is 48-120W.
Further, in the step (2), the dielectric barrier discharge output power is 120W.
In the step (2), the dielectric barrier discharge low-temperature plasma treatment time is 5 to 90 minutes.
The invention provides a method for removing organic pollutants in water by activating peroxyacetic acid through dielectric barrier discharge, which is simple, convenient, efficient, free from secondary pollution and wide in industrial application prospect. Dielectric barrier discharge low temperature plasma is an advanced oxidation technique. Wherein, a non-equilibrium state gas discharge which is inserted into the discharge space through an insulating medium is also called dielectric barrier corona discharge or silent discharge. The low-temperature plasma generated by the dielectric barrier discharge has the potential of activating the peroxyacetic acid along with the synergistic effect of multiple factors such as ultraviolet radiation, high-energy electron bombardment effect, electromagnetic field, high-oxidation active particles and the like, and other chemical agents or catalytic materials are not introduced. Therefore, the dielectric barrier discharge low-temperature plasma is expected to efficiently and environmentally activate the peroxyacetic acid to remove organic pollutants in water. Low temperature plasma is a term of art in which "low temperature" is not meant to be a specific term for temperature. The plasma is the fourth state of matter following the solid, liquid, and gas states, and when the applied voltage reaches the breakdown voltage, the gas molecules are ionized, creating a mixture including electrons, ions, atoms, and radicals. The low-temperature plasma is a kind of plasma, different from the high-temperature plasma, the electron temperature is very high in the discharging process of the low-temperature plasma, but the temperature of heavy particles is very low, and the whole system is in a low-temperature state, so that the low-temperature plasma is called cold plasma and is also called non-equilibrium plasma. If the electron temperature is as close as the heavy particle temperature, it is a thermal plasma, or an equilibrium plasma.
The invention adds peracetic acid into the waste water containing organic pollutant, then carries out dielectric barrier discharge low-temperature plasma treatment, and uses dielectric barrier discharge low-temperature plasma to generate electrons, light, heat and magnetism, cooperatively activates peracetic acid to generate a series of active oxygen free radicals, active nitrogen free radicals and carbon free radicals, and carries out chemical reaction with the organic pollutant in the water to degrade and mineralize the pollutant. The method is used for activating the peroxyacetic acid to remove the organic pollutants in the water, and has the advantages of stable and efficient effect, wide application range, low medicament cost, no secondary pollution and wide industrial application prospect.
The dielectric barrier discharge output power is 48W-120W, and when the output power is too low, the electric field intensity is low, the electron density is low, and the generation of carbon free radicals, hydroxyl free radicals and the like by activating the peroxyacetic acid is not facilitated; when the output power is too high, a large amount of energy is dissipated in a heat form, the energy utilization efficiency is reduced, and the pollutant degradation with high efficiency and energy conservation is not facilitated. The dielectric barrier discharge low-temperature plasma treatment time is 5-90 minutes, the treatment time is too short, and the degradation rate of organic pollutants is low; the longer the treatment time, the more the temperature of the treated solution exceeds the ambient temperature, causing thermal pollution, and the lower the pH of the treated solution, the more acid pollution. The molar ratio of the peroxyacetic acid to the organic pollutant is (0.1-50): 1, the concentration of the peroxyacetic acid is too low, and the concentration of generated carbon free radicals is too low, so that the removal of organic pollutants is not facilitated; the concentration of the peracetic acid is too high, electrons generated by the plasma can compete with target pollutants, the removal rate of organic pollutants can be reduced, and the pH value of the solution is reduced along with the increase of the addition amount of the peracetic acid, so that the acid-base balance of the treated solution is not facilitated.
Compared with the prior art, the invention has the following advantages:
(1) The method has simple process and simple and convenient operation method: only adding peracetic acid, then placing the treatment object into a dielectric barrier discharge reactor, and adjusting the input voltage and current to the corresponding input voltage and current;
(2) The method for treating the organic pollutants does not need to add any medicament or catalyst and does not generate toxic byproducts, and electrons, free radicals and the like generated in the low-temperature plasma treatment process of the dielectric barrier discharge do not cause secondary pollution to the environment;
(3) The dielectric barrier discharge low-temperature plasma treatment and the peroxyacetic acid have obvious synergistic effect, the peroxyacetic acid has higher activation efficiency, the treatment effect can be improved, the treatment cost is reduced, the reaction time is short, and the operability in practical engineering application is strong;
(4) The method has wide application range of target pollutants, including perfluorinated compounds, medicines, personal care products, polycyclic aromatic hydrocarbons, pesticides and the like.
Drawings
FIG. 1 is a graph showing the effect of example 1 on the removal of sulfamethoxazole antibiotics from water by activating peracetic acid with non-activated peracetic acid alone, dielectric barrier discharge plasma alone, and dielectric barrier discharge plasma;
FIG. 2 is a graph showing the effectiveness of dielectric barrier discharge plasma activation of different doses of peracetic acid to remove sulfamethoxazole antibiotics from water in example 2.
Detailed Description
The invention will now be described in detail with reference to the drawings and specific examples. The present embodiment is implemented on the premise of the technical scheme of the present invention, and a detailed implementation manner and a specific operation process are given, but the protection scope of the present invention is not limited to the following examples.
In the following examples, unless otherwise specified, the raw materials or processing techniques are indicated as being conventional commercially available raw material products or conventional processing techniques in the art.
In the following examples, the plasma source was a high voltage power source available from south Beijing Su Man technologies.
Example 1:
three groups of solutions 1L were prepared, one group of which was directly subjected to double dielectric barrier discharge treatment (discharge power: 120W) without adding peracetic acid, the other group was subjected to 20mg/L peracetic acid (molar ratio of peracetic acid to organic contaminants: 1.5:1), the other group was not subjected to discharge treatment, and the last group was subjected to double dielectric barrier discharge treatment (discharge power: 120W) after adding 20mg/L peracetic acid (molar ratio of peracetic acid to organic contaminants: 1.5:1). The removal rate of the sulfamethoxazole in three groups of experiments in different time is shown in figure 1, and the best effect of removing the sulfamethoxazole by activating peroxyacetic acid by using the double-dielectric barrier discharge plasma can be known, the reaction rate is the fastest, and the removal rate of the sulfamethoxazole reaches 52% after 30 minutes of reaction. In comparison, the removal rate of sulfamethoxazole was 18% when treated with a single double dielectric barrier discharge plasma for 30 minutes. The peracetic acid which is not activated alone has no removal effect on sulfamethoxazole.
Example 2:
three groups of solutions were prepared, 1L of which had a sulfamethoxazole concentration of about 45mg/L, with the first group containing 20mg/L of peracetic acid (to a molar ratio of peracetic acid to organic contaminants of 1.5:1), the second group containing 40mg/L of peracetic acid (to a molar ratio of peracetic acid to organic contaminants of 3:1), and the third group containing 60mg/L of peracetic acid (to a molar ratio of peracetic acid to organic contaminants of 4.5:1). Three sets of solutions containing peroxyacetic acid at different concentrations were subjected to a double dielectric barrier discharge treatment (discharge power 120W). The change of the removal rate of the sulfamethoxazole in the three groups of experiments is shown as figure 2, and the effect of activating the peroxyacetic acid by double dielectric barrier discharge to remove the sulfamethoxazole in water is better along with the increase of the addition amount of the peroxyacetic acid. The effect of activating 60mg/L peracetic acid by double dielectric barrier discharge to remove the sulfamethoxazole in water is optimal, and the removal rate of the sulfamethoxazole reaches 40% when the reaction is carried out for 15 minutes.
Examples 3 to 20:
in comparison with example 1, the same general procedure was repeated except that sulfamethoxazole was replaced with one of sulfadiazine, perfluorooctanoic acid, perfluorooctane sulfonic acid, tetracycline, fluticasone, triamcinolone acetonide, betamethasone, clobetasol propionate, hydrocortisone, nonylphenol, bisphenol A, estrone, estradiol, estriol, ethinyl estradiol, aniline, phenanthrene, and atrazine in equal concentrations and volumes, respectively.
Example 21:
in comparison with example 1, the same general procedure was followed except that in this example, sulfamethoxazole was replaced with an equal volume of a mixed solution of sulfadiazine, perfluorooctanoic acid, and perfluorooctane sulfonic acid (molar ratio 1:1:1), and the total concentration of sulfadiazine, perfluorooctanoic acid, and perfluorooctane sulfonic acid in the mixed solution was the same as that in example 1.
Example 22:
most of the same as in example 1 except that the discharge power was changed to 48W at 120W in this example.
Example 23:
most of the same as in example 1 except that the discharge power was changed to 80W at 120W in this example.
Example 24:
the vast majority of the dielectric barrier discharge treatment process was identical to that of example 1, except that in this example, the dielectric barrier discharge treatment process was continued for 90 minutes.
Example 25:
most of the same as in example 1, except that in this example, the molar ratio of peracetic acid to organic contaminants was adjusted to 0.1:1.
example 26:
most of the same as in example 1, except that in this example, the molar ratio of peracetic acid to organic contaminants was adjusted to 50:1.
the previous description of the embodiments is provided to facilitate a person of ordinary skill in the art in order to make and use the present invention. It will be apparent to those skilled in the art that various modifications can be readily made to these embodiments and the generic principles described herein may be applied to other embodiments without the use of the inventive faculty. Therefore, the present invention is not limited to the above-described embodiments, and those skilled in the art, based on the present disclosure, should make improvements and modifications without departing from the scope of the present invention.
Claims (6)
1. A method for removing organic pollutants in water by using dielectric barrier discharge activated peroxyacetic acid, which is characterized by comprising the following steps:
step (1): adding peracetic acid into water containing organic pollutants to obtain a solution containing peracetic acid;
step (2): performing dielectric barrier discharge low-temperature plasma treatment on the solution containing the peroxyacetic acid to obtain the final product;
in the step (1), the organic pollutant is one or more of sulfamethoxazole, sulfadiazine, perfluorooctanoic acid, perfluorooctane sulfonic acid, tetracycline, fluticasone, triamcinolone acetonide, betamethasone, clobetasol propionate, hydrocortisone, nonylphenol, bisphenol A, estrone, estradiol, estriol, ethinyl estradiol, aniline, phenanthrene or atrazine;
in the step (1), the molar ratio of the peroxyacetic acid to the organic pollutant is (0.1-50): 1, a step of;
in the step (2), the dielectric barrier discharge output power is 48W-120W;
in the step (2), the dielectric barrier discharge low-temperature plasma treatment time is 5-90 minutes.
2. The method for removing organic pollutants from water by using dielectric barrier discharge activated peroxyacetic acid according to claim 1, wherein in step (1), the organic pollutant is sulfamethoxazole.
3. The method for removing organic contaminants from water by dielectric barrier discharge activated peracetic acid of claim 1, wherein in step (1), the molar ratio of peracetic acid to organic contaminants is 1.5:1.
4. the method for removing organic contaminants from water by dielectric barrier discharge activated peracetic acid of claim 1, wherein in step (1), the molar ratio of peracetic acid to organic contaminants is 3:1.
5. the method for removing organic contaminants from water by dielectric barrier discharge activated peracetic acid of claim 1, wherein in step (1), the molar ratio of peracetic acid to organic contaminants is 4.5:1.
6. the method for removing organic contaminants from water by using dielectric barrier discharge activated peroxyacetic acid according to claim 1 wherein in step (2), the dielectric barrier discharge output power is 120W.
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