CN101921016A - Method for removing byproduct bromate of ozone process from water - Google Patents
Method for removing byproduct bromate of ozone process from water Download PDFInfo
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- CN101921016A CN101921016A CN 201010262189 CN201010262189A CN101921016A CN 101921016 A CN101921016 A CN 101921016A CN 201010262189 CN201010262189 CN 201010262189 CN 201010262189 A CN201010262189 A CN 201010262189A CN 101921016 A CN101921016 A CN 101921016A
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Abstract
The invention discloses a method for removing a byproduct bromate of an ozone process from water. The method comprises the following steps of: (1) introducing nitrogen into a reactor filled with the aqueous solution of bromate so as to remove dissolved oxygen from the aqueous solution and ensure that the concentration of the dissolved oxygen in the bromate aqueous solution is less than or equal to 2 mg/L; and (2) adjusting the initial pH value of the aqueous solution in the reactor to be between 3.5 and 10.5 and the reaction temperature to be between 10 and 30 DEG C, and then adding nano-iron into the reactor and reacting for 10 to 30 minutes, wherein the mass concentration ratio of the nano-iron to the bromate in the aqueous solution is (5-40):1. Compared with the prior art, the method has the advantages of simple reaction conditions for removing the bromate, convenient operation, wide application range and high reaction efficiency; moreover, when a relatively small amount of nano-iron is added, the bromate removing rate is over 90 percent, and the iron content in the water is less than 0.3 mg/L, which meets the Standards for Drinking Water Quality (GB5749-2006).
Description
Technical field
The present invention relates to a kind of method of removing ozone in water process byproducts bromate, belong to water technology.
Background technology
Because the deterioration of source quality, traditional in the past drinking water treatment technology can't satisfy " drinking water sanitary standard " (GB5749-2006), so ozone oxidation even depth treatment technology is widely used in drinking water treatment.If but when containing bromide in the water source, after ozone Oxidation Treatment, can produce bromate by product with carcinogenesis.Bromate is decided to be 2B level (higher carcinogenic possibility) potential carcinogen by international cancer research institution.The grownup of one individual weight 70Kg, the 2L that drinks water every day, when bromate concentration was 5,0.5 and 0.05 μ g/L, then lifelong carcinogenic rate was 10
-4, 10
-5With 10
-6For this reason, " drinking water sanitary standard " of the new revision of China (GB5749-2006) also regulation bromate limit value be 10 μ g/L.Therefore carry out that research is controlled and removed to the bromate by product that produces because of the ozone advanced treatment in the tap water is very urgent.At present mainly comprising biological degradation method aspect the removal technical study of bromate, ion exchange method, charcoal absorption reduction method, ferrous ion reduction method, ultraviolet irradiation etc.
1. biological degradation method
People such as Hijnen find that denitrifying bacteria can be degraded to ion with bromate.Kirsits also finds the removal effect of biologic active carbon filtration to bromate.But the removal of bromate is subjected to the influence of DO concentration, nitrate concentration and conventional ion.NO
3 -Compare BrO
3 -More acceptant electronics, BrO
3 -Biodegradation rate compares NO
3 -Therefore slow at least 100 times of degradation rate exists NO
3 -The time, BrO
3 -Substantially do not degrade.And obtain ideal and remove removal effect, the reaction times is longer, in water at low temperature, generally wants 25～30 minutes.Behind the biodegrade bromate, carry out stronger aftertreatment, to remove organism in water and excess ethanol.These reasons have all limited the application of biological degradation bromate in actual water factory.
2. ion exchange method:
The ion exchange method facture is better to the removal effect of bromate, but reduced price is higher, the waste water that also can produce some high density bromates simultaneously need obtain other processing, that is to say that this method just with pollutent transfer has taken place, and is not real thorough removal.
3. charcoal absorption reduction method
In drinking water deep is handled, often ozone and gac are united use together, to obtain better treatment effect, increase water quality.Experiment shows that fresh granular carbon (GAC) can be removed bromate and be bromide anion.The removal process is mainly finished by two-step reaction: BrO at first
3 -Be adsorbed on the GAC surface; With the active group of activated carbon surface chemical reaction taking place, is degraded to Br then
-Reduce pH value, increase GAC dosage, prolonging the empty bench grafting time of touching can improve bromate removal rate.But there are natural organic matter and NO in the water
3 -, ClO
3 -, SO
4 2-Can reduce the ability that GAC removes bromate during plasma.And fresh gac is reduction trend to bromate removal rate when biological activated carbon (BAC) transforms, and is relatively poor to the removal effect of bromate.Therefore to the removal of bromate, the practical application of gac is limited.And each water factory's condition of water quality, factors such as operational conditions all can exert an influence to the removal effect of bromate.
4. ferrous ion reduction method
Under meta-alkalescence pH, bromate can be by Fe
2+Be reduced into Br
-, its reaction process is mainly: earlier by the dissolved oxygen in the nitrification control water of microorganism on ammonium salt and the gac; Again by the bromate in the reductibility removal water of ferrous sulfate.For obtaining removal effect preferably, Fe
2+Concentration requirement higher (10-30mg/L), however add too much Fe
2+After, the total concentration of iron of solvability in the water of reaction back surpasses the 0.3mg/L of regulation in " drinking water sanitary standard ".Also need at last further to remove excessive iron ion in the water by filtering unit.Still need further research so ferrous ion is removed the bromate technology, the ferrous ion dosage is excessive to solve, the microorganism nitrification is controlled problems such as lower, the total concentration of iron of DO efficient exceeds standard, technical process is long.
Summary of the invention
The objective of the invention is to overcome the deficiencies in the prior art, and a kind of method of effective removal ozone in water process byproducts bromate is provided.
For achieving the above object, the technical solution used in the present invention is: the method for this removal ozone in water process byproducts bromate comprises the steps:
(1) in the reactor that fills the bromate aqueous solution, feeds nitrogen to remove the dissolved oxygen in the aqueous solution, make the concentration≤2mg/L of dissolved oxygen in the described bromate aqueous solution.
(2) initial pH value of the aqueous solution is that 3.5-10.5, temperature of reaction are 10-30 ℃ in the conditioned reaction device, and the back adds nanometer iron reaction 10-30min in reactor, and the mass concentration ratio of bromate is 5～40: 1 in the described nanometer iron and the described aqueous solution.
Further, the mass concentration ratio of bromate is 5～10: 1 in the nanometer iron of the present invention and the described aqueous solution.
Further, the present invention is in step (2), and the initial pH value of regulating the described aqueous solution is 5.0～7.0.
Compared with prior art, the invention has the beneficial effects as follows: (1) the present invention is by adding nanometer iron as reductive agent in the water that contains the bromate pollutent, make under low dissolved axygen that bromate is reduced into bromide anion in the water, with the bromate pollutent in the direct removal water body, the starting point concentration of bromate pollutent in the water body is low to moderate below the 50 μ g/L.(2) to remove the reaction conditions of bromate simple in the present invention, reacts under 10～30 ℃ of temperature condition and all can carry out effectively.And reaction can be carried out in the pH of broad value scope (3.5～10.5) smoothly.(3) nanometer iron required for the present invention is easy to obtain, and can adopt the liquid phase reduction preparation, for example with FeSO4.7H2O and excessive N aBH
4Reaction, the promptly reducible nanometer iron that makes.(4) prior art is lower by the efficient of microorganism nitrification control dissolved oxygen, and the present invention only need can guarantee that the dissolved oxygen DO in the reactor is lower by logical nitrogen in reactor, and operating procedure is simple.(5) the invention belongs to surperficial contact reacts, nanometer iron has the advantages that specific surface area is big, reactive behavior is high, so the reaction efficiency height can more effectively be removed bromate, but oxygen in water can influence its reaction efficiency to a certain extent.The present invention can be at nanometer iron dosage than the bromate pollutent of removing effectively under the low condition in the water, bromate removal rate can reach more than 90%, and the content of total iron reaches " drinking water sanitary standard " (GB5749-2006) in the water below 0.3mg/L.(6) in the ferrous ion reduction method of prior art, the mass concentration ratio of ferrous ion and bromate is 36-109: more than 1; And the dosage of nanometer iron of the present invention is removed ferrous ion dosage in the bromate method well below ferrous ion, the mass concentration ratio of bromate is (5-10) in the used nanometer iron of the present invention and the aqueous solution: 1, when 10-30min is carried out in reaction, bromate removal rate can reach more than 90%, simultaneously, the present invention since in the water outlet content of total iron below 0.3mg/L, can reach " drinking water sanitary standard " (GB5749-2006), so need not as the ferrous ion reduction method, follow-up filtration process to be set because of the solvability concentration of iron exceeds standard, it is simpler to have technology, operational management is required lower, and advantage such as the pH value scope of application is wideer.(7) the present invention is particularly suitable for the water factory of small-scale cities and towns and rural water is transformed because its speed of response is fast, floor space is little, convenient operation and management, is convenient to realize integrated apparatus.
Embodiment
Embodiment 1
In being the container of sealing of 1.0L, volume adds the distilled water of 900ml and the NaBrO of 1mg/L
3Solution 100ml makes that overall solution volume is 1000ml, initial NaBrO
3Concentration is 100 μ g/L, with magnetic stirring apparatus continuously stirring under 400r/min, and continuously logical N in the container
2After 10 minutes, make that the concentration of dissolved oxygen equals 0.2mg/L. in the aqueous solution
The initial pH value of the aqueous solution is 7 in the conditioned reaction device, temperature of reaction is 20 ℃, the back adds 1mg nanometer iron (mass concentration ratio between nanometer iron and the bromate is 10: 1) in reactor, during reaction 30min, use the Dionex-2000 ion chromatograph that the concentration of bromate in the aqueous solution is detected, and use the ICE3500 atomic absorption spectrophotometer that the solvability total iron content in the aqueous solution is detected, discovery fails to detect bromate and solvability iron, show that thus the concentration of bromate is lower than the detection lower limit (0.50 μ g/L) of Dionex-2000 ion chromatograph in this moment aqueous solution, the solvability total iron content is lower than the detection lower limit (0.05mg/L) of ICE3500 atomic absorption spectrophotometer.As seen, the present invention can remove bromate effectively, under above-mentioned reaction conditions, can reach more than 99% bromate removal rate in the 30min, and the solvability total iron content also can reach the requirement of GB5749-2006 in the water outlet.
Embodiment 2
In being the container of sealing of 1.0L, volume adds the distilled water of 800ml and the NaBrO of 1mg/L
3Solution 200ml makes that overall solution volume is 1000ml, initial NaBrO
3Concentration is 200 μ g/L, with magnetic stirring apparatus continuously stirring under 400r/min, and continuously logical N in the container
2After 10 minutes, make that the concentration of dissolved oxygen equals 0.1mg/L. in the aqueous solution
The initial pH value of the aqueous solution is 7 in the conditioned reaction device, temperature of reaction is 20 ℃, the back adds 1mg nanometer iron (mass concentration ratio between nanometer iron and the bromate is 5: 1) in reactor, reaction uses when carrying out 10min the Dionex-2000 ion chromatograph to detect that bromate concentration is 4.48 μ g/L in the aqueous solution, use the ICE3500 atomic absorption spectrophotometer that the solvability total iron content in the aqueous solution is detected, discovery fails to detect solvability iron, show that thus the solvability total iron content is lower than the detection lower limit (0.05mg/L of ICE 3500 atomic absorption spectrophotometers in this moment aqueous solution.)。As seen, the present invention can remove bromate effectively, under above-mentioned reaction conditions, can reach 97.7% to bromate removal rate in the 10min, and the solvability total iron content also can reach the requirement of GB5749-2006 in the water outlet.
Embodiment 3
In being the container of sealing of 1.0L, volume adds the distilled water of 950ml and the NaBrO of 1mg/L
3Solution 50ml makes that overall solution volume is 1000ml, initial NaBrO
3Concentration is 50 μ g/L, with magnetic stirring apparatus continuously stirring under 400r/min, and continuously logical N in the container
2After 10 minutes, make that the concentration of dissolved oxygen equals 2mg/L in the aqueous solution.
The initial pH value of the aqueous solution is 7 in the conditioned reaction device, temperature of reaction is 20 ℃, the back adds 2mg nanometer iron (mass concentration ratio between nanometer iron and the bromate is 40: 1) in reactor, when 30min is carried out in reaction, use the Dionex-2000 ion chromatograph to detect that bromate concentration is 3.20 μ g/L in the aqueous solution, uses that the solvability total iron content is 0.11mg/L in the ICE 3500 atomic absorption spectrophotometers detection aqueous solution.As seen, the present invention can remove bromate effectively,, under above-mentioned reaction conditions, be 96.8% in the 30min, and the solvability total iron content also can reach the requirement of GB5749-2006 in the water outlet to bromate removal rate.
Embodiment 4
In being the container of sealing of 1.0L, volume adds the distilled water of 900ml and the NaBrO of 1mg/L
3Solution 100ml makes that overall solution volume is 1000ml, initial NaBrO
3Concentration is 100 μ g/L, with magnetic stirring apparatus continuously stirring under 400r/min, and continuously logical N in the container
2Behind the 10min, make that the concentration of dissolved oxygen equals 0.1mg/L. in the aqueous solution
The initial pH value of the aqueous solution is 7 in the conditioned reaction device, temperature of reaction is 10 ℃, the back adds 1mg nanometer iron (mass concentration ratio between nanometer iron and the bromate is 10: 1) in reactor, reaction is when carrying out 30min, uses the Dionex-2000 ion chromatograph to detect that bromate concentration is 3.60 μ g/L in the aqueous solution, uses ICE 3500 atomic absorption spectrophotometers to detect that the solvability total iron content is 0.07mg/L in the aqueous solution.As seen, the present invention can remove bromate effectively, under the appeal reaction conditions, can reach 96.4% to bromate removal rate in the 30min, and the solvability total iron content also can reach the requirement of GB5749-2006 in the water outlet.
Embodiment 5
In being the container of sealing of 1.0L, volume adds the distilled water of 900ml and the NaBrO of 1mg/L
3Solution 100ml makes that overall solution volume is 1000ml, initial NaBrO
3Concentration is 100 μ g/L, with magnetic stirring apparatus continuously stirring under 400r/min, and continuously logical N in the container
2Behind the 10min, the concentration that makes dissolved oxygen in the aqueous solution is less than 2mg/L.
The initial pH value of the aqueous solution is 7 in the conditioned reaction device, temperature of reaction is 30 ℃, the back adds 1mg nanometer iron (mass concentration ratio between nanometer iron and the bromate is 10: 1) in reactor, when 10min is carried out in reaction, use the Dionex-2000 ion chromatograph to detect that bromate concentration is 8.00 μ g/L in the aqueous solution, and use ICE 3500 atomic absorption spectrophotometers that the solvability total iron content in the aqueous solution is detected, discovery fails to detect bromate and solvability iron, show that thus this moment, the solvability total iron content was lower than the detection lower limit (0.05mg/L of ICE 3500 atomic absorption spectrophotometers.)。As seen, the present invention can remove bromate effectively, under above-mentioned reaction conditions, can reach 92% to bromate removal rate in the 10min, and the solvability total iron content also can reach the requirement of GB5749-2006 in the water outlet.
Embodiment 6
In being the container of sealing of 1.0L, volume adds the distilled water of 900ml and the NaBrO of 1mg/L
3Solution 100ml makes that overall solution volume is 1000ml, initial NaBrO
3Concentration is 100 μ g/L, with magnetic stirring apparatus continuously stirring under 400r/min, and continuously logical N in the container
2Behind the 10min, make that the concentration of dissolved oxygen equals 0.2mg/L. in the aqueous solution
The initial pH value of the aqueous solution is 3.5 in the conditioned reaction device, temperature of reaction is 20 ℃, the back adds 1mg nanometer iron (mass concentration ratio between nanometer iron and the bromate is 10: 1) in reactor, reaction is when carrying out 20min, uses the Dionex-2000 ion chromatograph to detect that bromate concentration is 9.90 μ g/L in the aqueous solution, uses ICE 3500 atomic absorption spectrophotometers to detect that the solvability total iron content is 0.30mg/L in the aqueous solution.As seen, the present invention can remove bromate effectively, under above-mentioned reaction conditions, can reach 90.1% to bromate removal rate in the 20min, and the solvability total iron content also can reach the requirement of GB5749-2006 in the water outlet.
Embodiment 7
In being the container of sealing of 1.0L, volume adds the distilled water of 900ml and the NaBrO of 1mg/L
3Solution 100ml makes that overall solution volume is 1000ml, initial NaBrO
3Concentration is 100 μ g/L, with magnetic stirring apparatus continuously stirring under 400r/min, and continuously logical N in the container
2Behind the 10min, make that the concentration of dissolved oxygen equals 0.1mg/L. in the aqueous solution
The initial pH value of the aqueous solution is 10.5 in the conditioned reaction device, temperature of reaction is 20 ℃, the back adds 1mg nanometer iron (mass concentration ratio between nanometer iron and the bromate is 10: 1) in reactor, when 30min is carried out in reaction, use the Dionex-2000 ion chromatograph to detect that bromate concentration is 20.23 μ g/L in the aqueous solution, and use ICE 3500 atomic absorption spectrophotometers that the solvability total iron content in the aqueous solution is detected, discovery fails to detect bromate and solvability iron, show that thus this moment, the solvability total iron content was lower than the detection lower limit (0.05mg/L of ICE3500 atomic absorption spectrophotometer.)。As seen, the present invention can remove bromate effectively, under above-mentioned reaction conditions, can reach 79.8% to bromate removal rate in the 30min, and the solvability total iron content can reach the requirement of GB5749-2006 in the water outlet.
Embodiment 8
In being the container of sealing of 1.0L, volume adds the distilled water of 900ml and the NaBrO of 1mg/L
3Solution 100ml makes that overall solution volume is 1000ml, initial NaBrO
3Concentration is 100 μ g/L, with magnetic stirring apparatus continuously stirring under 400r/min, and continuously logical N in the container
2Behind the 10min, the concentration that makes dissolved oxygen in the aqueous solution is less than 0.1mg/L.
The initial pH value of the aqueous solution is 5 in the conditioned reaction device, temperature of reaction is 20 ℃, the back adds 1mg nanometer iron (mass concentration ratio between nanometer iron and the bromate is 10: 1) in reactor, reaction is when carrying out 30min, uses the Dionex-2000 ion chromatograph to detect that bromate concentration is 3.28 μ g/L in the aqueous solution, uses ICE 3500 atomic absorption spectrophotometers to detect that the solvability total iron content is 0.10mg/L in the aqueous solution.As seen, the present invention can remove bromate effectively, under above-mentioned reaction conditions, can reach 96.7% to bromate removal rate in the 30min, and the solvability total iron content also can reach the requirement of GB5749-2006 in the water outlet.
Claims (3)
1. a method of removing ozone in water process byproducts bromate is characterized in that comprising the steps:
(1) in the reactor that fills the bromate aqueous solution, feeds nitrogen to remove the dissolved oxygen in the aqueous solution, make the concentration≤2mg/L of dissolved oxygen in the described bromate aqueous solution;
(2) initial pH value of the aqueous solution is that 3.5-10.5, temperature of reaction are 10-30 ℃ in the conditioned reaction device, and the back adds nanometer iron reaction 10-30min in reactor, and the mass concentration ratio of bromate is 5～40: 1 in the described nanometer iron and the described aqueous solution.
2. the method for bromate in the removal water according to claim 1 is characterized in that: the mass concentration ratio of bromate is 5～10: 1 in the described nanometer iron and the described aqueous solution.
3. the method for bromate in the removal water according to claim 1 and 2 is characterized in that: in step (2), the initial pH value of regulating the described aqueous solution is 5.0～7.0.
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| CN 201010262189 CN101921016A (en) | 2010-08-20 | 2010-08-20 | Method for removing byproduct bromate of ozone process from water |
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|---|---|---|---|
| CN 201010262189 CN101921016A (en) | 2010-08-20 | 2010-08-20 | Method for removing byproduct bromate of ozone process from water |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102381811A (en) * | 2011-09-21 | 2012-03-21 | 哈尔滨工业大学 | Method for removing pollutants in water through stepwise catalytic oxidation-biological activated carbon-ultraviolet (UV) combination |
| CN102815762A (en) * | 2012-08-30 | 2012-12-12 | 浙江大学 | Method for absorbing precipitation by nano iron and removing phosphate in water by magnetic separation technology |
| CN102976488A (en) * | 2012-11-20 | 2013-03-20 | 浙江大学 | Method for zero-valent nano-iron-reinforced biological removal of nitrogen and phosphorus |
| CN103232125A (en) * | 2013-05-13 | 2013-08-07 | 山东大学 | Method for removing bromate through ordered mesoporous carbon loaded nanoscale zero-valent iron material |
| CN113171739A (en) * | 2021-04-25 | 2021-07-27 | 中南民族大学 | Method for generating superoxide anion free radical by catalytically activating bromate and application of superoxide anion free radical generated by method |
-
2010
- 2010-08-20 CN CN 201010262189 patent/CN101921016A/en active Pending
Non-Patent Citations (1)
| Title |
|---|
| 《Environ. Sci. Technol》 20090327 QILIANG WANG et al. Aqueous Ethanol modified Nanoscale Zerovalent Iron in Bromate Reduction : Synthesis, Characterization, and Reactivity 第3293页左栏第49行至右栏第60行 1-3 第43卷, 2 * |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102381811A (en) * | 2011-09-21 | 2012-03-21 | 哈尔滨工业大学 | Method for removing pollutants in water through stepwise catalytic oxidation-biological activated carbon-ultraviolet (UV) combination |
| CN102815762A (en) * | 2012-08-30 | 2012-12-12 | 浙江大学 | Method for absorbing precipitation by nano iron and removing phosphate in water by magnetic separation technology |
| CN102976488A (en) * | 2012-11-20 | 2013-03-20 | 浙江大学 | Method for zero-valent nano-iron-reinforced biological removal of nitrogen and phosphorus |
| CN102976488B (en) * | 2012-11-20 | 2013-11-20 | 浙江大学 | Method for zero-valent nano-iron-reinforced biological removal of nitrogen and phosphorus |
| CN103232125A (en) * | 2013-05-13 | 2013-08-07 | 山东大学 | Method for removing bromate through ordered mesoporous carbon loaded nanoscale zero-valent iron material |
| CN113171739A (en) * | 2021-04-25 | 2021-07-27 | 中南民族大学 | Method for generating superoxide anion free radical by catalytically activating bromate and application of superoxide anion free radical generated by method |
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