CN105036293A - Method for removing organic pollutants in water by ferrate reinforced ozone oxidation - Google Patents
Method for removing organic pollutants in water by ferrate reinforced ozone oxidation Download PDFInfo
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- CN105036293A CN105036293A CN201510534616.1A CN201510534616A CN105036293A CN 105036293 A CN105036293 A CN 105036293A CN 201510534616 A CN201510534616 A CN 201510534616A CN 105036293 A CN105036293 A CN 105036293A
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Abstract
The invention relates to a water treatment method, particularly a method for removing organic pollutants in water by ferrate reinforced ozone oxidation, which aims to solve the problem of high ozone addition amount due to great influence by background components and low effective concentrations of ozone and hydroxy free radicals in the existing ozone-oxidation-process exposed water. The treatment method comprises the following steps: adding ferrate into source water containing organic pollutants to perform preoxidation treatment, stirring to react, introducing ozone, and continuing stirring to react, thereby removing the organic pollutants in water by ferrate reinforced ozone oxidation, wherein the ferrate is one or mixture of potassium ferrate and sodium ferrate. The ferrate is used as a strong oxidant, has a co-oxidation action with ozone, and reduces the trapping consumption of the background component for ozone and hydroxy free radicals. Compared with the oxidation by single ozone, the pollutant removal rate is enhanced by 30-50%, and the ozone addition amount is decreased by 20-50%.
Description
Technical field
The present invention relates to a kind of water treatment method, be specifically related to a kind of method that ozone oxidation removes organic pollutants.
Background technology
Ozone oxidation is applied very extensive in water treatment.Ozone, as a kind of strong oxidizer, can effectively be removed colourity, smell taste and multiple organic micro-pollutants.Independent ozone oxidation has selectivity, can only oxidized portion organic pollutant (containing electron rich group), and the change of great majority just structure, molecular weight, and mineralization degree is not high.Therefore need to adopt catalytic ozonation, such as UV/O
3, H
2o
2/ O
3and the catalysis ozone such as transition-metal catalyst decomposes and produces hydroxyl radical free radical.Hydroxyl radical free radical is the high reactivity species with strong oxidizing property, does not have selectivity to organic oxidation, significantly can improve the removal efficiency to organic micro-pollutants.But existing ozone oxidation and catalytic ozonation are subject to the impact of background material in water very large.Such as, at H
2o
2/ O
3find in engineering reality for the process of Sewage Plant secondary effluent, even if add a large amount of H
2o
2, ozone removes the efficiency of hardly degraded organic substance also without significantly improving.Because the background organism competition in water consumes a large amount of ozone and hydroxyl radical free radical, the effective concentration of ozone, hydroxyl radical free radical is reduced.Reach good Micropollutants removal effect, just must improve ozone dosage, cause running cost to increase, and the raising of ozone dosage can increase the brominated generation containing iodine disinfection byproduct (DBP) (bromate, bromo organism, iodo organism etc.).
Summary of the invention
The object of the invention is to affect greatly in order to solve existing Ozonation by background component in water, ozone and hydroxyl radical free radical effective concentration low, cause the problem that ozone dosage is large, and provide a kind of water treatment method utilizing ferrate to strengthen ozone oxidation removal organic pollutants.
The method that the present invention utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 0.1 ~ 30mg/L ferrate in the source water of organic pollutant, the ozone passing into 0.2 ~ 30mg/L after stirring reaction 1 ~ 30min continues stirring reaction, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is one or both the mixture in potassium ferrate, Na2Fe04.
Ferrate of the present invention itself, can optionally oxidized portion Micropollutants as a kind of strong oxidizer, play with ozone the effect be jointly oxidized; Secondly, ferrate and organism react generated in-situ peroxidation Hydrogen Energy and cause ozone decomposed and produce highly reactive form of oxygen agent hydroxyl radical free radical
greatly improve the removal efficiency to hardly degraded organic substance.Meanwhile, ferrate is background organism in preoxidation stage oxidation water, reduces background component and catches consumption to ozone and hydroxyl radical free radical, improve the effective concentration of ozone, hydroxyl radical free radical, reduce ozone dosage, brominated few containing iodine disinfection byproduct (DBP) growing amount, be applicable to large-scale application.
This method utilizing ferrate to strengthen ozone oxidation removal organic pollutants is oxidized separately compared to ozone and improves 30% ~ 50% to the clearance of pollutent, the throwing amount of ozone is made to reduce 20% ~ 50%, bromate generation can be made to reduce 40% ~ 70%, can make to reduce 30% ~ 60% containing iodine by product generation.
Embodiment
Embodiment one: the method that present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 0.1 ~ 30mg/L ferrate in the source water of organic pollutant, the ozone passing into 0.2 ~ 30mg/L after stirring reaction 1 ~ 30min continues stirring reaction, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is one or both the mixture in potassium ferrate, Na2Fe04.
The dosage of present embodiment ferrate is in Fe.Ferrate is potassium ferrate and Na2Fe04 can be mixed by any ratio when being mixture.Add 0.1 ~ 30mg/L ferrate to containing in the source water of organic pollutant, refer to that the concentration of ferrate in source water is 0.1 ~ 30mg/L herein.
Ferrate described in present embodiment is a kind of Green Oxidant, within the scope of wider pH, have strong oxidizing property, and its oxidation has selectivity, is easy to be oxidized the compound containing electron rich group, as phenols, amine, olefines and compound that is nitrogenous, sulphur.The final reduzate of ferrate is ferric iron, and hydrolysis has certain coagulation effect further, is removed at coagulation, precipitation, filtration stage, and environmentally friendly, nontoxic after discharge.The hydrogen peroxide that ferrate reaction process situ generates causes ozone generation hydroxyl radical free radical, greatly improves the removal efficiency to Recalcitrant chemicals; Ferrate removes the background component consuming ozone and free radical in water at preoxidation stage oxidation, reduce ozone dosage, improves productive rate and the utilization ratio of subsequent free radical.
Embodiment two: present embodiment and embodiment one are 0.00001 ~ 1000 μ g/L unlike the concentration of the Organic Pollutants in Source Water containing organic pollutant.Other step and parameter identical with embodiment one.
Embodiment three: present embodiment and embodiment one or two are oil of mirbane unlike described organic pollutant, estradiol, oestrone, trihydroxy-oestrin, stilboestrol, 17 α-lynoral, isoflavones, zearalenone, nonyl phenol, octyl phenol, Carbamzepine erythromycin, sulfamethoxazole, trimethoprim, Roxithromycin, Ofloxacine USP 23, if Flucloxacillin, atenolol USP 23, stable, Ketoprofen BP 93, clofibric acid, carbadipimidine, Naproxen Base, Ibuprofen BP/EP, clotrimazole, Paracetamol, iodine amic metadiazine, paraxin, diclofenac, bezafibrate, gemfibrozil, Carbamzepine, atrazine, SD-1750, glyphosate, Chlorpyrifos 94, heptachlor, Malathion, Pentachlorophenol, phenyl-hexachloride, Rogor, thiophos, bentazone, parathion-methyl, m-tetrachlorophthalodinitrile, Furadan, lindane, Deltamethrin, 2,4-drips, dichlorodiphenyl trichloroethane, prussiate, vinylidene chloride, 1,2-dichloroethene, 1,2-dichlorobenzene, Isosorbide-5-Nitrae-dichlorobenzene, trieline, trichlorobenzene, hexachlorobutadiene, acrylamide, zellon, toluene, epoxy chloropropane, benzene, vinylbenzene, benzopyrene, vinylchlorid, chlorobenzene, two (2-ethylhexyl) adipic acid ester, sym-dibromoethane, dioxin, ground depth, pentachloropropane, dihydroxyphenyl propane, vinyl cyanide, vinylformic acid, propenal, tetraethyllead, glutaraldehyde, methyl isoborneol-2, polycyclic aromatic hydrocarbons, polychlorobiphenyl, diethyl phthalate, dibutyl phthalate, naphthenic acid, methyl-phenoxide, 2-Naphthol, butyl xanthic acid, mercuric ethyl chloride, Iopromide, Schering AG), urografic acid methylglucamine salt, Sodium Diatrizoate, iodized oil, one or more mixtures in Visipaque 320.Other step and parameter identical with embodiment one or two.
Embodiment four: one of present embodiment and embodiment one to three are drinking water resource or Sewage Plant secondary effluent unlike the described source water containing organic pollutant.Other step and parameter identical with one of embodiment one to three.
Embodiment five: one of present embodiment and embodiment one to four carry out pre-oxidation treatment unlike with the form of solid ferrate or ferrate solution to containing adding 0.1 ~ 30mg/L ferrate in the source water of organic pollutant.Other step and parameter identical with one of embodiment one to four.
Embodiment six: one of present embodiment and embodiment one to five carry out pre-oxidation treatment unlike to containing adding 2 ~ 20mg/L ferrate in the source water of organic pollutant.Other step and parameter identical with one of embodiment one to five.
Embodiment seven: present embodiment and embodiment six carry out pre-oxidation treatment unlike to containing adding 3 ~ 12mg/L ferrate in the source water of organic pollutant.Other step and parameter identical with embodiment six.
Embodiment eight: one of present embodiment and embodiment one to seven continue stirring reaction unlike the ozone passing into 2 ~ 20mg/L.Other step and parameter identical with one of embodiment one to seven.
Embodiment nine: one of present embodiment and embodiment one to eight continue stirring reaction 2 ~ 30min unlike the ozone passing into 0.2 ~ 30mg/L.Other step and parameter identical with one of embodiment one to eight.
Embodiment ten: one of present embodiment and embodiment one to nine unlike the dosing method of ozone for passing into ozone gas.Other step and parameter identical with one of embodiment one to nine.
Embodiment one: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 2mg/L ferrate (in Fe) in the drinking water resource of 0.001 μ g/L oestrone, the ozone passing into 2mg/L after stirring reaction 10min continues stirring reaction 20min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is the aqueous solution of potassium ferrate and Na2Fe04 mixture.
In the present embodiment water outlet, the concentration of oestrone is 0.00025 μ g/L, and clearance reaches 75%, and compared to independent ozone oxidation, the clearance of oestrone improves 30%, and ozone dosage reduces 20%.
Embodiment two: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 5mg/L ferrate (in Fe) in the Sewage Plant secondary effluent of 0.04 μ g/L oestrone, the ozone passing into 10mg/L after stirring reaction 20min continues stirring reaction 20min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is the aqueous solution of potassium ferrate and Na2Fe04 mixture.
In the present embodiment water outlet, the concentration of oestrone is 0.002 μ g/L, and clearance reaches 95%, and compared to independent ozone oxidation, the clearance of oestrone improves 45%, and ozone dosage reduces 35%.
Embodiment three: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 2mg/L ferrate (in Fe) in the drinking water resource of 30 μ g/L Carbamzepines, the ozone passing into 2mg/L after stirring reaction 10min continues stirring reaction 25min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is the aqueous solution of potassium ferrate and Na2Fe04 mixture.
In the present embodiment water outlet, the concentration of Carbamzepine is 0.12 μ g/L, and clearance reaches 99.6%, and compared to independent ozone oxidation, the clearance of Carbamzepine improves 40%, and ozone dosage reduces 20%.
Embodiment four: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 10mg/L ferrate (in Fe) in the drinking water resource of 250 μ g/L Carbamzepines, the ozone passing into 15mg/L after stirring reaction 30min continues stirring reaction 25min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is the aqueous solution of potassium ferrate and Na2Fe04 mixture.
In the present embodiment water outlet, the concentration of Carbamzepine is 0.5 μ g/L, and clearance reaches 99.8%, and compared to independent ozone oxidation, the clearance of Carbamzepine improves 50%, and ozone dosage reduces 50%.
Embodiment five: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
To containing 0.3 μ g/L diclofenac, add 3mg/L ferrate (in Fe) in the drinking water resource of the bromide anion of 50 μ g/L and carry out pre-oxidation treatment, the ozone passing into 2mg/L after stirring reaction 10min continues stirring reaction 10min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is the aqueous solution of potassium ferrate and Na2Fe04 mixture.
In the present embodiment water outlet, the concentration of diclofenac is 0.05 μ g/L, and clearance reaches 83.3%, and compared to independent ozone oxidation, the clearance of diclofenac improves 45%, and ozone dosage reduces 50%, and the generation of bromate reduces 60%.
Embodiment six: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 20mg/L ferrate (in Fe) in the Sewage Plant secondary effluent of 5 μ g/L diclofenacs, the ozone passing into 30mg/L after stirring reaction 15min continues stirring reaction 20min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is the aqueous solution of potassium ferrate and Na2Fe04 mixture.
In the present embodiment water outlet, the concentration of diclofenac is 0.17 μ g/L, and clearance reaches 96.6%, and compared to independent ozone oxidation, the clearance of diclofenac improves 50%, and ozone dosage reduces 60%.
Embodiment seven: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 10mg/L ferrate (in Fe) in the drinking water resource of 100 μ g/L Iopromides, the ozone passing into 20mg/L after stirring reaction 15min continues stirring reaction 10min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is the aqueous solution of potassium ferrate and Na2Fe04 mixture.
In the present embodiment water outlet, the concentration of Iopromide is 1.2 μ g/L, and clearance reaches 98.8%, and compared to independent ozone oxidation, the clearance of Iopromide improves 46%, and ozone dosage reduces 58%, produces without iodo by product.
Embodiment eight: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 20mg/L ferrate (in Fe) in the Sewage Plant secondary effluent of 500 μ g/L Iopromides, the ozone passing into 20mg/L after stirring reaction 20min continues stirring reaction 25min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is the aqueous solution of potassium ferrate and Na2Fe04 mixture.
In the present embodiment water outlet, the concentration of Iopromide is 1.9 μ g/L, and clearance reaches 99.6%, and compared to independent ozone oxidation, the clearance of Iopromide improves 50%, and ozone dosage reduces 60%, produces without iodo by product.
Embodiment nine: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
In the drinking water resource containing 200 μ g/L oil of mirbane and 500 μ g/L iodide ions, add 5mg/L ferrate (in Fe) carry out pre-oxidation treatment, the ozone passing into 20mg/L after stirring reaction 10min continues stirring reaction 20min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water.
In the present embodiment water outlet, the concentration of oil of mirbane is 1.3 μ g/L, clearance reaches 99.4%, the clearance of oil of mirbane improves 30% compared to independent ozone oxidation after measured, and ozone dosage reduces 42%, reduces 48% relative to the independent iodine oxide of ozone for by product generation.
Embodiment ten: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
In the Sewage Plant secondary effluent containing 5000 μ g/L oil of mirbane and 500 μ g/L iodide ions, add 15mg/L ferrate (in Fe) carry out pre-oxidation treatment, the ozone passing into 20mg/L after stirring reaction 15min continues stirring reaction 30min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water.
In the present embodiment water outlet, the concentration of oil of mirbane is 2.7 μ g/L, clearance reaches 99.9%, the clearance of oil of mirbane improves 40% compared to independent ozone oxidation after measured, and ozone dosage reduces 45%, reduces 50% relative to the independent iodine oxide of ozone for by product generation.
Embodiment 11: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 5mg/L ferrate (in Fe) in the drinking water resource of 50 μ g/L atrazines, the ozone passing into 20mg/L after stirring reaction 10min continues stirring reaction 20min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water.
In the present embodiment water outlet, the concentration of atrazine is 0.5 μ g/L, and clearance reaches 99.0%, and the clearance of atrazine improves 30% compared to independent ozone oxidation after measured, and ozone dosage reduces 42%.
Embodiment 12: the method that the present embodiment utilizes ferrate to strengthen ozone oxidation removal organic pollutants follows these steps to realize:
Pre-oxidation treatment is carried out to containing adding 10mg/L ferrate (in Fe) in the Sewage Plant secondary effluent of 150 μ g/L atrazines, the ozone passing into 20mg/L after stirring reaction 15min continues stirring reaction 20min, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water.
In the present embodiment water outlet, the concentration of atrazine is 0.75 μ g/L, and clearance reaches 99.5%, and the clearance of atrazine improves 40% compared to independent ozone oxidation after measured, and ozone dosage reduces 50%.
Claims (10)
1. utilize ferrate to strengthen a method for ozone oxidation removal organic pollutants, it is characterized in that following these steps to realize:
Pre-oxidation treatment is carried out to containing adding 0.1 ~ 30mg/L ferrate in the source water of organic pollutant, the ozone passing into 0.2 ~ 30mg/L after stirring reaction 1 ~ 30min continues stirring reaction, thus completes the organic pollutant in ferrate strengthening ozone oxidation removal water; Wherein said ferrate is one or both the mixture in potassium ferrate, Na2Fe04.
2. a kind of method utilizing ferrate to strengthen ozone oxidation removal organic pollutants according to claim 1, is characterized in that the concentration of the Organic Pollutants in Source Water containing organic pollutant is 0.00001 ~ 1000 μ g/L.
3. a kind of method utilizing ferrate to strengthen ozone oxidation removal organic pollutants according to claim 1, is characterized in that described organic pollutant is oil of mirbane, estradiol, oestrone, trihydroxy-oestrin, stilboestrol, 17 α-lynoral, isoflavones, zearalenone, nonyl phenol, octyl phenol, Carbamzepine erythromycin, sulfamethoxazole, trimethoprim, Roxithromycin, Ofloxacine USP 23, if Flucloxacillin, atenolol USP 23, stable, Ketoprofen BP 93, clofibric acid, carbadipimidine, Naproxen Base, Ibuprofen BP/EP, clotrimazole, Paracetamol, iodine amic metadiazine, paraxin, diclofenac, bezafibrate, gemfibrozil, Carbamzepine, atrazine, SD-1750, glyphosate, Chlorpyrifos 94, heptachlor, Malathion, Pentachlorophenol, phenyl-hexachloride, Rogor, thiophos, bentazone, parathion-methyl, m-tetrachlorophthalodinitrile, Furadan, lindane, Deltamethrin, 2,4-drips, dichlorodiphenyl trichloroethane, prussiate, vinylidene chloride, 1,2-dichloroethene, 1,2-dichlorobenzene, Isosorbide-5-Nitrae-dichlorobenzene, trieline, trichlorobenzene, hexachlorobutadiene, acrylamide, zellon, toluene, epoxy chloropropane, benzene, vinylbenzene, benzopyrene, vinylchlorid, chlorobenzene, two (2-ethylhexyl) adipic acid ester, sym-dibromoethane, dioxin, ground depth, pentachloropropane, dihydroxyphenyl propane, vinyl cyanide, vinylformic acid, propenal, tetraethyllead, glutaraldehyde, methyl isoborneol-2, polycyclic aromatic hydrocarbons, polychlorobiphenyl, diethyl phthalate, dibutyl phthalate, naphthenic acid, methyl-phenoxide, 2-Naphthol, butyl xanthic acid, mercuric ethyl chloride, Iopromide, Schering AG), urografic acid methylglucamine salt, Sodium Diatrizoate, iodized oil, one or more mixture in Visipaque 320.
4. a kind of method utilizing ferrate to strengthen ozone oxidation removal organic pollutants according to claim 1, is characterized in that the described source water containing organic pollutant is drinking water resource or Sewage Plant secondary effluent.
5. a kind of method utilizing ferrate to strengthen ozone oxidation removal organic pollutants according to claim 1, is characterized in that carrying out pre-oxidation treatment with the form of solid ferrate or ferrate solution to containing adding 0.1 ~ 30mg/L ferrate in the source water of organic pollutant.
6. a kind of method utilizing ferrate to strengthen ozone oxidation removal organic pollutants according to claim 1, is characterized in that carrying out pre-oxidation treatment to containing adding 2 ~ 20mg/L ferrate in the source water of organic pollutant.
7. a kind of method utilizing ferrate to strengthen ozone oxidation removal organic pollutants according to claim 6, is characterized in that carrying out pre-oxidation treatment to containing adding 3 ~ 12mg/L ferrate in the source water of organic pollutant.
8. a kind of method utilizing ferrate to strengthen ozone oxidation removal organic pollutants according to claim 1, is characterized in that the ozone passing into 2 ~ 20mg/L continues stirring reaction.
9. a kind of method utilizing ferrate to strengthen ozone oxidation removal organic pollutants according to claim 1, is characterized in that the ozone passing into 0.2 ~ 30mg/L continues stirring reaction 2 ~ 30min.
10. a kind of method utilizing ferrate to strengthen ozone oxidation removal organic pollutants according to claim 1, is characterized in that the dosing method of ozone is for passing into ozone gas.
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