CN101050036A - Method for controlling generation quantity of bromic acid radicle in treating procedure for oxidizing drinking water by ozone - Google Patents
Method for controlling generation quantity of bromic acid radicle in treating procedure for oxidizing drinking water by ozone Download PDFInfo
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- CN101050036A CN101050036A CN 200710072234 CN200710072234A CN101050036A CN 101050036 A CN101050036 A CN 101050036A CN 200710072234 CN200710072234 CN 200710072234 CN 200710072234 A CN200710072234 A CN 200710072234A CN 101050036 A CN101050036 A CN 101050036A
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Abstract
This invention relates to a method for controlling the quantity of bromate ions produced during treatment of ozone-oxidized drinking water. The method solves the problems of consuming residual chlorine, eroding pipes and meshes, and generating toxic substances by present techniques. The method controls the quantity of bromate ions by introducing cerium oxide, transition metal oxide-doped cerium oxide or supported cerium oxide catalyst for catalytic oxidation. The quantity of produced bromate ions is decreased by 80% when the bromic ions concentration is 100-200 mu.g/L and the consumption of cerium oxide is 100 mg/L. The method has a high efficiency in inhibiting the generation of bromate ions, and the yield of byproducts is 20-30% lower than that produced by pure ozone oxidation.
Description
Technical field
The present invention relates to a kind of method of controlling the bromate growing amount, be specifically related to a kind of method of bromate growing amount when using solid catalyst to reduce ozone oxidation bromine ion-containing water.
Background technology
In recent years, face of land water factory uses ozone more and more as the situation of tap water oxidation depollution measure.If contain bromide anion in the surface water, then can make ozone oxidation produce new problem.Bromide anion in the water can be changed into hypobromous acid and bromate by partial oxygen in the ozone oxidation process, residue does not have oxidized bromide anion also can be become hypobromous acid by oxychlorination in last chlorine disinfectant process, hypobromous acid be easy to surface water in natural organic matter (NOM) substitution reaction takes place, generate deleterious bromo by products such as bromofom, dibromo-acetonitrile, dibromoacetic acid, cyanogen bromide.Bromate is decided to be 2B level carcinogens by international cancer research institution, and each developed country's drinking water standard and China's Urban water supply water quality standard all maximum permissible concentration of regulation bromate are 10 μ g/L.The bromo by product is proved to be than chloro by product stronger toxicity and mutagenesis activity, and because the higher nucleidic mass of Br makes the overall control of disinfection byproduct (DBP) become difficult more.Handle owing to be associated with gac or biologic active carbon filtration after the ozone oxidation usually, brominated organic compound of part and bromo by product antecedent can be removed by physical adsorption or microbiological deterioration to a certain extent, but bromate can not be removed by active adsorption.Therefore, the problem of ozone oxidation by product in the tap water---bromate is just especially outstanding, and the problem of bromate has become ozone and has been applied to the restrictive factor that drinking water deep is handled most critical.
In recent ten years, the foreign study personnel have carried out more research to the method for control bromate growing amount in the ozone oxidation process.The method of research has: add acid and reduce the pH value, add hydrogen peroxide, add ammoniacal liquor and chlorination ammonia (Cl
2And NH
3Add in proportion).Wherein, ammonification and reduction pH value can reduce the bromate growing amount about 50%.Yet all there are some problems in actual applications in these methods.
Reduce pH and allow BrO
3 -Intermediate product HOBr/OBr in the forming process
-Balance move to left O
3Can only oxidation OBr
-, can not oxidation HOBr, therefore can suppress bromate and generate.But, can increase total organic bromine (TOBr) output like this.In addition, both inconvenience was also uneconomical for the water treatment mode of adjusting pH value.
Adding hydrogen peroxide is to utilize intermediate product HOBr/OBr
-Can be by H
2O
2Be reduced to Br
-Thereby, suppress HOBr/OBr
-Generate, reduce BrO
3 -Produce.But O
3/ H
2O
2Can produce more OH, the OH of increase also can make Br
-Approach by Br is oxidized to BrO
3 -In fact, only add excessive H
2O
2Could reduce BrO
3 -Excessive H
2O
2Can consume chlorine residue, and then influence the lasting sterilisation effect in the pipe network, and can cause piping corrosion.
Ammonification is to utilize HOBr/OBr
-With the reaction of ammonia bromine is changed into bromine ammonia, bromine ammonia is oxidized to NO lentamente by ozone
3 -And BrO
3 -, make BrO
3 -Generation lag behind.Add Cl
2-NH
3Be to add ammoniacal liquor ozone oxidation again behind the former water prechlorination.Br in the water
-At first be oxidized to HOBr, then HOBr and NH by HOCl
3Reaction generates NH
2Br.Add Cl
2-NH
3Can reduce by 40% bromate growing amount than ammonification.Because having consumed ozone, ammonia decomposes the hydroxyl radical free radical that produces, so ammonification and chlorination ammonia have also weakened the ability of ozone oxidation organic pollutant.Moreover, the use meeting of ammonia produces more nitrogenous disinfection byproduct (DBP) (HANs) when chlorine disinfectant.Current research shows that HANs is more much higher than the toxicity of carbon containing disinfection byproduct (DBP) (as halogen acetic acid), so the method for this control bromate is brought insoluble new problem again.
Summary of the invention
The objective of the invention is to introduce some chemical agents and reduce bromate growing amounts and have problems such as consuming chlorine residue, piping corrosion, generation toxic substance, and a kind of method of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes is provided in order to solve in the present oxidizing drinking water by ozone treating processes.The present invention introduces the metal oxide solid catalyzer in the oxidizing drinking water by ozone treating processes, effectively control the growing amount of bromate under the situation of not adding chemical agent in water.Method steps of the present invention is as follows: one, carry out ozone oxidation and solid metal oxide catalyst catalyzed oxidation through the filtered water after the traditional water treating processes processing (processing such as coagulation, precipitation, filtration); Two, the water after oxidation enters gac or biological activity carbon filterbed, and the control residence time is 5～20min, further removes the organism in anhydrating; Three, remove organic water and enter webmaster later on through chlorination.
Different with aforesaid method is in step 1, and after filtering water enters the ozone contact tower carries out ozone oxidation reaction 10s～5min, adding ozone among wherein every mgTOC is 0.1～4.0mg, the water that comes out from the ozone contact tower enters in the catalyst bed that inside is filled with solid metal oxide catalyst again, and the control catalyst catalyzed oxidation time is 10s～15min; Or water in step 1 after filtering enters the ozone contact tower that inside is filled with solid metal oxide catalyst and carries out the O3 catalytic oxidation reaction, and the reaction times is 10s～15min.Other steps are identical with aforesaid method with processing condition.
Solid metal oxide catalyst of the present invention is the cerium oxide that the method by the calcination metal nitrate obtains; Or the cerium oxide of the transition metal oxide that mixed; Or by metal nitrate through dipping, the calcination process loads to high silica alumina ratio zeolite and/or mesopore material, perhaps loads on the load type cerium oxide that obtains on the transition metal oxide; Or transition metal oxide is made the load type cerium oxide of promotor.
Through studies show that of contriver, cerium oxide has the efficient that higher control bromate produces, under the situation of bromide ion concentration 100～200 μ g/L, cerium oxide throwing amount 100mg/L can reduce by 80% bromate generation, obtain than adding the higher reduction bromate efficient of chemical agent, and the output of bromo disinfection byproduct (DBP) also reduces by 20～30% than simple ozone oxidation.The solubility product constant of cerium oxide in water is very low, its K
Sp=4 * 10
-51, therefore catalyzer can not take place discharges toxic metal ionic problem in water.The reason that cerium oxide control bromate produces is that its surperficial Ce (IV) has suppressed the oxidation of ozone for bromate intermediate oxidation product hypobromous acid root.The catalyst bed of dosing with cerium oxide or load type cerium oxide can carry out the extensive drinking water treatment of Continuous Flow, thereby realizes the target that the control bromate produces in water factory's drinking water deep processing under the situation of not adding chemical agent in water.
Embodiment
Embodiment one: the method for bromate growing amount in the control oxidizing drinking water by ozone treating processes in the present embodiment:, carry out ozone oxidation and solid metal oxide catalyst catalyzed oxidation through the filtered water after the traditional water treating processes processing (processing such as coagulation, precipitation, filtration); Two, the water after oxidation enters gac or biological activity carbon filterbed, and the control residence time is 5～20min, further removes the organism in anhydrating; Three, remove organic water and enter webmaster later on through chlorination.
In the process of present embodiment treating water, under the situation of bromide ion concentration 100～200 μ g/L, cerium oxide throwing amount 100mg/L ozone oxidation separately reduces by 80% bromate generation, obtain than adding the higher reduction bromate efficient of chemical agent, and the output of bromo disinfection byproduct (DBP) also reduces by 20～30% than simple ozone oxidation.The solubility product constant of cerium oxide in water is very low, its K
Sp=4 * 10
-51, therefore catalyzer can not take place discharges toxic metal ionic problem in water.
Embodiment two: present embodiment after filtering water in step 1 enters the ozone contact tower and carries out ozone oxidation reaction 10s～15min, and adding ozone among wherein every mg TOC is 0.1～4.0mg; The water that comes out from the ozone contact tower enters in the catalyst bed that inside is filled with solid metal oxide catalyst again, and control catalyst oxidization time is 10s～15min.Other step is identical with embodiment one with processing condition.
Embodiment three: present embodiment after filtering water in step 1 enters the ozone contact tower that inside is filled with solid metal oxide catalyst and carries out the O3 catalytic oxidation reaction, and the reaction times is 10s～15min.Other step is identical with embodiment one with processing condition.
Embodiment four: this implementation method with the difference of embodiment one to three is: the solid metal oxide catalyst in step 1 is a cerium oxide.Other step is identical with embodiment one to three with processing condition.
Embodiment five: cerium oxide prepares according to following method in the present embodiment: the cerous nitrate solid is calcined 30min～5h down at 350～850 ℃, obtain faint yellow ceria oxide powder.Other embodiment is identical with embodiment four.
Embodiment six: the difference of present embodiment and this implementation method and embodiment one to three is: the solid metal oxide catalyst in step 1 is the cerium oxide of promotor of having mixed, wherein to account for the ratio of gross weight be 0.02～15% to promotor, and promotor is one or more mixing in manganese oxide, ferric oxide, cupric oxide, zirconium white, nickel oxide, titanium oxide and the vanadium oxide.Other steps are identical with embodiment one to three with processing condition.
Present embodiment when promotor be in manganese oxide, ferric oxide, cupric oxide, zirconium white, nickel oxide, titanium oxide and the vanadium oxide during several mixing, by arbitrarily than mixing.
Embodiment seven: the difference of present embodiment and this implementation method and embodiment one to three is: the solid metal oxide catalyst in step 1 is a load type cerium oxide, the charge capacity of cerium oxide is 0.5～12wt.% (weight percent), and carrier is high silica alumina ratio zeolite and/or mesopore material.
When the carrier of present embodiment was mixture, zeolite mixed by arbitrary proportion with mesopore material.
Embodiment eight: the particle diameter of carrier is 0.5～6mm in the present embodiment.Other embodiment is identical with embodiment seven.
Embodiment nine: the particle diameter of carrier is 1.5～4mm in the present embodiment.Other embodiment is identical with embodiment seven.
Embodiment ten: the particle diameter of carrier is 3mm in the present embodiment.Other embodiment is identical with embodiment seven.
Embodiment 11: the high silica alumina ratio zeolite is one or more the mixing in high silica alumina ratio L zeolite, high silica alumina ratio Y zeolite and the mordenite with high silicon aluminum ratio in the present embodiment.Other is identical with embodiment seven.
Present embodiment when the high silica alumina ratio zeolite be in high silica alumina ratio L zeolite, high silica alumina ratio Y zeolite and the mordenite with high silicon aluminum ratio when several, press arbitrary proportion and mix.
Embodiment 12: mesopore material is one or more the mixing in mesoporous silicon sill, mesopore aluminophosphates material, mesoporous silicon aluminum, mesopore raw material of wood-charcoal material and the mesopore charcoal/silicon composite in the present embodiment.Other is identical with embodiment seven.
When present embodiment is mesoporous silicon sill, mesopore aluminophosphates material, mesoporous silicon aluminum, mesopore raw material of wood-charcoal material and several mixing of mesopore charcoal/silicon composite when the mesopore material, presses arbitrary proportion and mix.
Embodiment 13: the aperture of mesopore material is 3～45nm in the present embodiment.Other is identical with embodiment seven.
Embodiment 14: the aperture of mesopore material is 10～30nm in the present embodiment.Other is identical with embodiment seven.
Embodiment 15: the aperture of mesopore material is 20nm in the present embodiment.Other is identical with embodiment seven.
Embodiment 16: present embodiment and embodiment seven are different is that carrier is one or more the mixing in manganese oxide, ferric oxide, cupric oxide, zirconium white, nickel oxide, titanium oxide and the vanadium oxide, and cerium oxide load ratio is 0.001～25%wt.% (weight percent).Other is identical with embodiment seven.
Carrier is in manganese oxide, ferric oxide, cupric oxide, zirconium white, nickel oxide, titanium oxide and the vanadium oxide during several mixing in the present embodiment, by arbitrarily than mixing.
Embodiment 17: what present embodiment and embodiment seven were different is that load type cerium oxide prepares according to following step: a, be that the 0.1mol/L dilute hydrochloric acid that the carrier of 0.2～8mm is put into pH=1～3 soaked 4～12 hours with particle diameter; Carrier after b, flushing are soaked is put into the 1-50% cerous nitrate solution then and was soaked 4～24 hours; C, the carrier of b step was taken out under 80～120 ℃ of conditions dry 6～12 hours, calcine 30min～5h again under 350～850 ℃ of conditions, the charge capacity that obtains faint yellow cerium oxide is the load type cerium oxide of 0.5～12wt.% (weight percent).Other embodiment is identical with embodiment seven.
Embodiment 18: present embodiment and embodiment seven are different is to have mixed in manganese oxide, ferric oxide, cupric oxide, zirconium white, nickel oxide, titanium oxide and the vanadium oxide one or more as promotor, the charge capacity of promotor is 0.02～15% (wt.%), and cerium oxide load ratio is 0.001～25%wt.% (weight percent).Other is identical with embodiment seven.
Promotor is in manganese oxide, ferric oxide, cupric oxide, zirconium white, nickel oxide, titanium oxide and the vanadium oxide during several mixing in the present embodiment, presses arbitrary proportion and mixes.
Claims (10)
1, a kind of method of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes, the step of this method is as follows: the filtered water after, handling through the traditional water treating processes is carried out ozone oxidation and solid metal oxide catalyst catalyzed oxidation; Two, the water after oxidation enters gac or biological activity carbon filterbed, and the control residence time is 5～20min, further removes the organism in anhydrating; Three, remove organic water and enter webmaster later on through chlorination; It is characterized in that controlling the bromate growing amount with the method for solid metal oxide catalyst catalyzed oxidation in the oxidizing drinking water by ozone treating processes.
2, a kind of method of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes according to claim 1, it is characterized in that in step 1 after filtering water enters the ozone contact tower and carries out ozone oxidation reaction 10s～15min, adding ozone among wherein every mg TOC is 0.1～4.0mg, the water that comes out from the ozone contact tower enters in the catalyst bed that inside is filled with solid metal oxide catalyst again, and the control catalyst catalyzed oxidation time is 10s～15min.
3, a kind of method of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes according to claim 1, it is characterized in that in step 1 after filtering water enters the ozone contact tower that inside is filled with solid metal oxide catalyst and carries out the O3 catalytic oxidation reaction, the reaction times is 10s～15min.
4, according to claim 1,2 or 3 described a kind of methods of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes, it is characterized in that the solid metal oxide catalyst in step 1 is a cerium oxide.
5, a kind of method of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes according to claim 4, it is characterized in that cerium oxide prepares according to following method: the cerous nitrate solid is calcined 30min～5h down at 350～850 ℃, obtain faint yellow ceria oxide powder.
6, according to claim 1,2 or 3 described a kind of methods of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes, it is characterized in that solid metal oxide catalyst in step 1 is the cerium oxide of promotor of having mixed, wherein to account for the ratio of gross weight be 0.02～15% to promotor, and promotor is one or more mixing in manganese oxide, ferric oxide, cupric oxide, zirconium white, nickel oxide, titanium oxide and the vanadium oxide.
7, according to claim 1,2 or 3 described a kind of methods of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes, it is characterized in that the solid metal oxide catalyst in step 1 is a load type cerium oxide, the charge capacity of cerium oxide is 0.5～12wt.%, and carrier is high silica alumina ratio zeolite and/or mesopore material; Wherein the high silica alumina ratio zeolite is one or more the mixing in high silica alumina ratio L zeolite, high silica alumina ratio Y zeolite and the mordenite with high silicon aluminum ratio, the mixing of one or more in mesoporous silicon sill, mesopore aluminophosphates material, mesoporous silicon aluminum, mesopore raw material of wood-charcoal material and the mesopore charcoal/silicon composite.
8, a kind of method of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes according to claim 7 is characterized in that carrier is one or more the mixing in manganese oxide, ferric oxide, cupric oxide, zirconium white, nickel oxide, titanium oxide and the vanadium oxide.
9, a kind of method of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes according to claim 7 is characterized in that load type cerium oxide prepares according to following step: a, be that the 0.1mol/L dilute hydrochloric acid that the carrier of 0.2～8mm is put into pH=1～3 soaked 4～12 hours with particle diameter; Carrier after b, flushing are soaked is put into 1～50% cerous nitrate solution then and was soaked 4～24 hours; C, the carrier of b step was taken out under 80～120 ℃ of conditions dry 6～12 hours, calcine 30min～5h again under 350～850 ℃ of conditions, the charge capacity that obtains faint yellow cerium oxide is the load type cerium oxide of 0.5～12wt.%.Other embodiment is identical with embodiment seven.
10, a kind of method of controlling bromate growing amount in the oxidizing drinking water by ozone treating processes according to claim 7, it is characterized in that load type cerium oxide doping in manganese oxide, ferric oxide, cupric oxide, zirconium white, nickel oxide, titanium oxide and the vanadium oxide one or more as promotor, the charge capacity of promotor is 0.02～15wt.%, and cerium oxide load ratio is 0.001～25%wt.%.
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|---|---|---|---|---|
| CN102020372A (en) * | 2009-09-11 | 2011-04-20 | 董旭 | Ozone water purifying method capable of reducing and eliminating bromates |
| CN101259428B (en) * | 2008-04-24 | 2011-07-20 | 福州大学 | Preparation of catalyst for processing industrial wastewater and using method thereof |
| CN102234153A (en) * | 2010-04-27 | 2011-11-09 | 中国科学院生态环境研究中心 | Method for reducing generation amount of bromate in ozone water treatment process through catalysis of Ce-MCM-48 |
| CN102513088A (en) * | 2011-12-09 | 2012-06-27 | 西南交通大学 | Preparation method of compound catalyst for controlling generation of bromate in process of using ozone |
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| CN101259428B (en) * | 2008-04-24 | 2011-07-20 | 福州大学 | Preparation of catalyst for processing industrial wastewater and using method thereof |
| CN101613165B (en) * | 2009-07-20 | 2012-07-18 | 广东省微生物研究所 | Control method of bromate in bottled drinking water |
| CN102020372A (en) * | 2009-09-11 | 2011-04-20 | 董旭 | Ozone water purifying method capable of reducing and eliminating bromates |
| CN102234153A (en) * | 2010-04-27 | 2011-11-09 | 中国科学院生态环境研究中心 | Method for reducing generation amount of bromate in ozone water treatment process through catalysis of Ce-MCM-48 |
| CN102513088A (en) * | 2011-12-09 | 2012-06-27 | 西南交通大学 | Preparation method of compound catalyst for controlling generation of bromate in process of using ozone |
| CN102616916B (en) * | 2012-04-25 | 2014-01-01 | 南开大学 | Method for controlling formation quantity of bromate in ozone oxidized water treatment process by TiO2 |
| CN102616916A (en) * | 2012-04-25 | 2012-08-01 | 南开大学 | Method for controlling formation quantity of bromate in ozone oxidized water treatment process by TiO2 |
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| CN102942266A (en) * | 2012-11-13 | 2013-02-27 | 常州大学 | Bromo-aliphatic hydrocarbon compound production waste water treatment method |
| CN102976475A (en) * | 2012-12-20 | 2013-03-20 | 江南大学 | Ozonization water treatment method by taking fluorine-doped manganese dioxide nano composite material as catalyst |
| CN102976475B (en) * | 2012-12-20 | 2014-06-04 | 江南大学 | Ozonization water treatment method by taking fluorine-doped manganese dioxide nano composite material as catalyst |
| CN105080551A (en) * | 2014-05-06 | 2015-11-25 | 李小琴 | Efficient spherical particle ozonation catalyst and preparation method therefor |
| CN104129872A (en) * | 2014-07-02 | 2014-11-05 | 清华大学 | Method for controlling generation amount of bromate during treatment process of drinking water |
| CN104129872B (en) * | 2014-07-02 | 2016-02-24 | 清华大学 | The control method of bromate growing amount in drinking water treatment process |
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| CN109721148B (en) * | 2019-02-20 | 2022-06-10 | 北京林业大学 | Heterojunction interface electron transfer induced ozone catalytic oxidation water treatment method with bromate reduction capability |
| WO2023223058A1 (en) | 2022-05-20 | 2023-11-23 | Aristotle University Of Thessaloniki-E.L.K.E. | Method for the removal of micropollutants by the application of heterogeneous catalytic ozonation from water |
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