CN103951102A - Method for killing viruses in drinking water - Google Patents
Method for killing viruses in drinking water Download PDFInfo
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- CN103951102A CN103951102A CN201410142384.0A CN201410142384A CN103951102A CN 103951102 A CN103951102 A CN 103951102A CN 201410142384 A CN201410142384 A CN 201410142384A CN 103951102 A CN103951102 A CN 103951102A
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Abstract
A provided method for killing viruses in drinking water comprises the following steps: (1) detecting chloride ion concentration and dissolved organic carbon concentration in water by employing a detection instrument; (2) if the chloride ion concentration and the dissolved organic carbon concentration are both 5 mg/L or less, performing no treatment; and if at least one of the chloride ion concentration and the dissolved organic carbon concentration exceeds 5 mg/L, performing pretreatment on to-be disinfected water to enable the two concentration to be both reduced to 5 mg/L or less; and (3) successively adding a trivalent copper ion stabilizing agent, a divalent copper salt and a persulfate into the to-be disinfected water. The method is mile in treatment conditions and free of secondary pollution, and helps to improve the killing efficiency of drinking water on viruses.
Description
Technical field
The present invention relates to the sterilization method of tap water, relate in particular to a kind of method for killing of drinking Inactivation of Enteric Viruses In Water.
Background technology
The control of pathogenic micro-organism is an importance that ensures water hygiene safety, in multiple pathogenic microorganisms, virus is individual little, pathogenic strong, the health event causing because of virus outbreak in tap water for a long time has report at home and abroad time, and therefore water hygiene should cause safely the attention that we are enough.But, only have at present minority developed country to have clear and definite regulation to drinking the degree for the treatment of of Inactivation of Enteric Viruses In Water, the new edition " drinking water sanitary standard " of China 2006 issuing and implementation still excludes for viral processing index in (GB5749-2006), has only increased the processing index for 4 microorganisms (colon bacillus, heat-resisting coliform, giardia lamblia stiles and hidden armful of sub-worm).The domestic method majority of killing for virus is limited to the field such as disinfecting, medical science sterilization at present, sterilization sample size is less, the directive function that virus in practical large-scale water treatment is killed is very limited, therefore for efficient method for killing Drinking Water in China is significant safely of drinking Inactivation of Enteric Viruses In Water.
At at present common actual sterilizing agent ozone, chlorine, dioxide peroxide, hydrogen peroxide, the chloramines of being applied to, through relatively their required Ct values (Ct value refers to that sterilization reaches the certain concentration of the needed sterilizing agent of eradicative rate and product in reaction times) of test, the required minimum virus killing of Ct value of ozone is most effective, chlorine and dioxide peroxide take second place, and the efficiency of hydrogen peroxide and chloramines is minimum.Although cupric ion or silver ions and chlorine combined disinfection are found to strengthen viral insect killing effect, but there is the generation of harmful disinfection byproduct (DBP) (halomethane, halogen acetic acid etc.).The studied person of Peracetic Acid thinks a kind of surrogate of good chlorine-containing disinfectant, but it is extremely unstable, also can explode at-20 DEG C.
Ultraviolet Disinfection is widely used in feedwater and dirty water purification, but the Generating Problems of the carcinogens nitrite anions of uv induction is not also resolved, and can cause secondary pollution to water body.Characterization of adsorption based on viral and micro-filtration and the ultra-filtration technique developed are classified as the control techniques of drinking Inactivation of Enteric Viruses In Water by EPA, but the viral insect killing efficiency of this technology reduces gradually along with the aggravation of film pollution, need frequent micro-filtration or the ultra-filtration membrane changed, cost is higher.
In recent years, Fenton or class Fenton technology are considered to the more promising virus of a class and kill technology.The active substance of this class technique functions kill activity mainly contains super oxygen root free radical (O
2 -) and hydroxyl radical free radical (OH).But this class technology also has twice " outpost of the tax office " to need to cross over from practical application: (1) is in view of O
2 -with the non-selectivity of OH, can only be applicable to comparatively clean water body of background, in the time there is background material (as natural organic matter, carbonate etc.) in system, O
2 -can react with background material in large quantities with OH, reduce O
2 -with the OH viricidal efficiency of going out, thereby need more oxygenant and longer treatment time, obviously increase processing cost; (2) this technology need need be controlled at the pH value of water to be sterilized under acidic conditions, and the pH value of actual water body often approaches neutrality, can accomplish gigantic project although the pH value of extensive water body to be sterilized is adjusted to acidity in actual sterilizing process, expense is high, impracticable.
In sum, in prior art, also do not have reality feasible, efficiently, economy and non-secondary pollution for the method for killing of drinking Inactivation of Enteric Viruses In Water.
Summary of the invention
The invention provides a kind of method for killing of drinking Inactivation of Enteric Viruses In Water, the method working conditions gentleness, economy and non-secondary pollution, the insect killing efficiency of virus is high.
The technical scheme that the present invention deals with problems is:
A method for killing of drinking Inactivation of Enteric Viruses In Water, comprises the steps:
(1) detect chlorine ion concentration and the dissolved organic carbon concentration in water to be sterilized;
(2) if chlorine ion concentration and dissolved organic carbon concentration all below 5mg/L, do not deal with; If at least one exceedes 5mg/L among chlorine ion concentration and dissolved organic carbon concentration, treat sterilized water and carry out pre-treatment, the two concentration is all dropped to below 5mg/L;
(3) in water to be sterilized, add means of trivalent copper ion stabilizer, cupric salt, persulphate successively.
Wherein, in step (1), with ion chromatograph chlorine detection ion, use total organic carbon detector to detect dissolved organic carbon concentration.
Described pre-treatment is mainly to remove organism in water, common are MIEX magnetic ion exchange resin method, ultrafiltrationmembrane process and active carbon adsorption etc., wherein MIEX magnetic ion exchange resin method is better for remove in chlorion and water organism effect simultaneously, and processing efficiency is higher, preferably, described pre-treatment is to adopt MIEX magnetic ion exchange resin method.
Principle of the present invention is: first in water to be sterilized, add means of trivalent copper ion stabilizer, then after persulphate (Persulfate) and cupric salt are added in water to be sterilized, the bivalent cupric ion (Cu that persulphate ionizes out at cupric salt
2+) effect under produce sulfate radical free radical (SO
4 -), the sulfate radical free radical (SO of generation
4 -) some and bivalent cupric ion (Cu
2+) further reaction generation means of trivalent copper ion (Cu
3+).Sulfate radical free radical (SO
4 -) be a kind of single electron selectivity strong oxidizer, be subject in water the impact of organism and carbonate little compared with hydroxyl radical free radical, thereby demonstrate the viral insect killing efficiency stronger than the hydroxyl radical free radical generating in Fenton's reaction; And Cu
3+virus is had to good exclusive kill activity.The synergy of the two can be killed Inactivation of Enteric Viruses In Water and microorganism efficiently.SO
4 -redox potential be 2.5-3.1V, Cu
3+/ Cu
2+the right redox potential of electricity is 1.57V.
The present invention has also added cupric ion stablizer, can suppress Cu
3+transform, keep Cu
3+there is higher concentration.Comparing Fenton technology can only apply under acidic conditions, and the present invention can use under neutrallty condition.
In every liter of water to be sterilized, the consumption of persulphate is no more than 2mmol, in the consumption of cupric salt and water, original copper ion concentration sum is no more than 15 μ mol, preferably, in every liter of water to be sterilized, in step (3), means of trivalent copper ion stabilizer consumption is 0.2～1 μ mol, and cupric salt consumption is 0～15 μ mol, and persulphate consumption is 0～2mmol.
As further preferred: in every liter of water to be sterilized, means of trivalent copper ion stabilizer consumption 0.2～1 μ mol in step (3), cupric salt consumption 5～15 μ mol, persulphate consumption is 0.5～2mmol.
As preferably, described means of trivalent copper ion stabilizer is a kind of in citric acid and gallic acid or both mixtures; Described cupric salt is the mixing of a kind of in copper sulfate and neutralized verdigris or two kinds; Described persulphate is one or more the mixing in ammonium persulphate, Sodium Persulfate, Potassium Persulphate, monopersulfate ammonium, monopersulfate sodium and Potassium Monopersulfate.Cupric salt provides bivalent cupric ion after being dissolved in water, and therefore cupric salt must be water-soluble, and can not introduce the ion of other polluted waters; Select the principle of persulphate and select cupric salt similar, persulphate is water-soluble can provide persulfate, can not introduce harmful ion simultaneously.
Contriver finds, use separately citric acid or use separately gallic acid can reach general effect as means of trivalent copper ion stabilizer, but in the time adding citric acid and gallic acid, effect is particularly outstanding simultaneously, and the usage ratio of citric acid and gallic acid is also larger on the impact of result.
As means of trivalent copper ion stabilizer preferably, described means of trivalent copper ion stabilizer is the mixture of citric acid and gallic acid, the mol ratio of citric acid and gallic acid is 1～3:1.
Vicinal hydroxyl groups in gallic acid can with Cu
3+form inner complex by Cu
3+protect, citric acid is rich in carboxyl, and itself and sulfate radical Free Radical can produce carbonic acid gas free radical (CO
2 -), carbonic acid gas free radical can be strengthened Cu
3+to the regeneration after divalence form transformation, the acting in conjunction of citric acid and gallic acid can extend Cu
3+transformation period, increase Cu
3+css, improve inactivation of virus efficiency.
As preferably, described citric acid and the purity of gallic acid are food grade.
In the selection of solubility cupric salt, consider sterilization effect, the least possible secondary pollution and cost simultaneously, preferably, described cupric salt is that foreign matter content is no more than 0.05% copper sulfate.
As preferably, in step (3), the pH value of water to be sterilized is 5.5～7.5.The pH of water to be sterilized is less than at 5.5 o'clock, and the productive rate of means of trivalent copper ion reduces; When pH is higher than 7.5 time, thereby the bivalent cupric ion effective concentration of free state reduces the productive rate that also reduces means of trivalent copper ion.Means of trivalent copper ion productive rate is lower, and sterilisation effect is poorer.General water to be sterilized itself is exactly neutral or approaches neutrality, just in time meets with conditions for sterilization of the present invention, therefore substantially needn't adjust pH value, has improved processing efficiency.
Method of the present invention is not high to temperature requirement, under normal temperature, can carry out, but the useful range of guarantee to sterilize best effect and definite treatment temp, preferably, in step (3), the temperature of water to be sterilized is 5～40 DEG C.
The invention has the beneficial effects as follows:
Can under very common condition, kill efficiently the common virus in water (rotavirus, hepatitis virus, enterovirus etc.), and cost is more much lower than other technique, also can not produce secondary pollution.The present invention does not need expensive equipment and assembly, and simple to operation, safe enough, and efficiency is high, can meet the requirement of large-scale application completely.Management and operation are all very convenient, can realize automatic management control completely.The reagent relating in the present invention is as persulphate, soluble copper salt, citric acid and gallic acid, not only safe but also cheap.Related material easily obtains, and final reacting product is the material of the nontoxic or readily biodegradable such as sulfate radical and small molecules carboxylic acid.
The present invention can also with the coupling of ultraviolet virus method, without changing the structure of sterilization pool, only need to add ultraviolet lamp and quartz socket tube.
Brief description of the drawings
Fig. 1 be a kind of method for killing of drinking Inactivation of Enteric Viruses In Water of the present invention process flow sheet;
Fig. 2 be use separately copper sulfate and use separately Potassium Persulphate as disinfectant and embodiment 1 the insect killing effect comparison diagram to MS2 phage;
Fig. 3 is the insect killing effect comparison diagram of virus in embodiment 2,3 and 4.
Embodiment
Below in conjunction with step shown in specific embodiment and Fig. 1, the present invention is described in further detail.
Embodiment 1
Detect chlorion and the dissolved organic carbon in water to be sterilized with ion chromatograph and total organic carbon detector, if the two concentration is no more than 5mg/L, can not process; If the two concentration exceedes 5mg/L, adopt MIEX magnetic ion exchange resin (Beijing Ao Ruikai company) to treat sterilized water and carry out pre-treatment, when resin concentration is 200mL/L, duration of contact is when 5min, contain the former water of 10mg/L chlorion and 8mg/L dissolved organic carbon after treatment, chlorine ion concentration is 3.5mg/L, and dissolved organic carbon concentration is 4.5mg/L, and pH value is 6.8.Chlorion in water and the total concn of dissolved organic carbon are no more than under the prerequisite of 5mg/L, in every liter of water to be sterilized: first add 10
10pFU MS2 bacterium liquid, then adds the citric acid of 0.5 μ mol food grade and the gallic acid of 0.5 μ mol food grade, adds afterwards 10 μ mol copper sulfate, after these three kinds of medicaments mix, then adds Potassium Persulphate 1.5mmol.
These several medicaments that guarantee adds and water body to be sterilized are in sterilization pool or disinfection tank more than contact reacts 10min, and MS2 phage eradicative rate exceedes 90%.MS2 phage is usually used as indicator virus, for Evaluation of Disinfection, thereby the eradicative rate of simulating virus in actual treatment with the eradicative rate of MS2 phage.If will further improve viral eradicative rate, can the proper extension treatment time.
Fig. 2 uses separately CuSO
4with independent use Potassium Persulphate as disinfectant and embodiment 1 the insect killing effect comparison diagram to MS2 phage.X-coordinate is for killing the time, and ordinate zou is the quantity ([MS2] of the quantity ([MS2]) of MS2 phage while the reaction times being t minute MS2 phage during with 0 minute
0) logarithmic value of ratio.
Process after 10min, embodiment 1 logarithm eradicative rate reaches 93%, and uses separately the eradicative rate of copper sulfate or Potassium Persulphate to be no more than 36.9%.As can be seen from Figure 2, in the method for embodiment 1, killing of MS2 phage can force rate be used separately CuSO
4with independent use Potassium Persulphate to kill ability much better than.
Embodiment 2
Detect chlorion and the dissolved organic carbon in water to be sterilized with ion chromatograph and total organic carbon detector, if the two concentration is no more than 5mg/L, can not process; If the two concentration exceedes 5mg/L, adopt MIEX magnetic ion exchange resin (Beijing Ao Ruikai company) to treat sterilized water and carry out pre-treatment, when resin concentration is 200mL/L, duration of contact is when 5min, contain the former water of 10mg/L chlorion and 8mg/L dissolved organic carbon after treatment, chlorine ion concentration is 3.5mg/L, and dissolved organic carbon concentration is 4.5mg/L, and pH value is 6.8.Chlorion in water and the total concn of dissolved organic carbon are no more than under the prerequisite of 5mg/L, in every liter of water to be sterilized: first add 10
10pFU MS2 bacterium liquid, then adds the citric acid of 0.15 μ mol food grade and the gallic acid of 0.05 μ mol food grade, adds afterwards 5 μ mol copper sulfate, after these three kinds of medicaments mix, then adds Potassium Persulphate 0.5mmol.
Embodiment 3
Detect chlorion and the dissolved organic carbon in water to be sterilized with ion chromatograph and total organic carbon detector, if the two concentration is no more than 5mg/L, can not process; If the two concentration exceedes 5mg/L, adopt MIEX magnetic ion exchange resin (Beijing Ao Ruikai company) to treat sterilized water and carry out pre-treatment, when resin concentration is 200mL/L, duration of contact is when 5min, contain the former water of 10mg/L chlorion and 8mg/L dissolved organic carbon after treatment, chlorine ion concentration is 3.5mg/L, and dissolved organic carbon concentration is 4.5mg/L, and pH value is 6.8.Chlorion in water and the total concn of dissolved organic carbon are no more than under the prerequisite of 5mg/L, in every liter of water to be sterilized: first add 10
10pFU MS2 bacterium liquid, then adds the citric acid of 0.15 μ mol food grade and the gallic acid of 0.05 μ mol food grade, adds afterwards 15 μ mol copper sulfate, after these three kinds of medicaments mix, then adds Potassium Persulphate 2mmol.
Embodiment 4
Detect chlorion and the dissolved organic carbon in water to be sterilized with ion chromatograph and total organic carbon detector, if the two concentration is no more than 5mg/L, can not process; If the two concentration exceedes 5mg/L, adopt MIEX magnetic ion exchange resin (Beijing Ao Ruikai company) to treat sterilized water and carry out pre-treatment, when resin concentration is 200mL/L, duration of contact is when 5min, contain the former water of 10mg/L chlorion and 8mg/L dissolved organic carbon after treatment, chlorine ion concentration is 3.5mg/L, and dissolved organic carbon concentration is 4.5mg/L, and pH value is 6.8.Chlorion in water and the total concn of dissolved organic carbon are no more than under the prerequisite of 5mg/L, in every liter of water to be sterilized: first add 10
10pFU MS2 bacterium liquid, then adds the citric acid of 0.75 μ mol food grade and the gallic acid of 0.25 μ mol food grade, adds afterwards 5 μ mol copper sulfate, after these three kinds of medicaments mix, then adds Potassium Persulphate 0.5mmol.
Fig. 3 is that embodiment 2,3 and 4 treats after sterilized water processing 10min, the insect killing effect comparison diagram of Inactivation of Enteric Viruses In Water, X-coordinate is for killing the time, and ordinate zou is the quantity ([MS2] of the quantity ([MS2]) of MS2 phage while the reaction times being 10 minutes MS2 phage during with 0 minute
0) logarithmic value of ratio.In embodiment 2, the logarithm clearance of MS2 phage is 42.5%; In embodiment 3, the logarithm clearance of MS2 phage is 82.3%; In embodiment 4, the logarithm clearance of MS2 phage is 99.1%.Can find out from this group correlation data, the consumption of persulphate and mantoquita increases, and virus is killed ability to be increased, and means of trivalent copper ion stabilizer consumption increases, and virus is killed ability to be increased.
For the ease of detecting the insect killing effect of Inactivation of Enteric Viruses In Water to be sterilized, in each embodiment of the present invention, specially add indicator virus MS2 phage, in actual treatment, omit this step.And the impact for fear of pre-treatment on MS2 phage activity, therefore after finishing, pre-treatment just adds MS2 phage to water to be sterilized.
Claims (8)
1. a method for killing of drinking Inactivation of Enteric Viruses In Water, comprises the steps:
(1) detect chlorine ion concentration and the dissolved organic carbon concentration in water to be sterilized;
(2) if chlorine ion concentration and dissolved organic carbon concentration all below 5mg/L, do not deal with; If at least one exceedes 5mg/L among chlorine ion concentration and dissolved organic carbon concentration, treat sterilized water and carry out pre-treatment, the two concentration is all dropped to below 5mg/L;
(3) in water to be sterilized, add means of trivalent copper ion stabilizer, cupric salt, persulphate successively.
2. the method for killing of drinking Inactivation of Enteric Viruses In Water as claimed in claim 1, it is characterized in that: in every liter of water to be sterilized, in step (3), means of trivalent copper ion stabilizer consumption is 0.2～1 μ mol, and cupric salt consumption is 0～15 μ mol, and persulphate consumption is 0～2mmol.
3. the method for killing of drinking Inactivation of Enteric Viruses In Water as claimed in claim 2, it is characterized in that: in every liter of water to be sterilized, means of trivalent copper ion stabilizer consumption 0.2～1 μ mol in step (3), cupric salt consumption 5～15 μ mol, persulphate consumption is 0.5～2mmol.
4. the method for killing of drinking as claimed in claim 2 or claim 3 Inactivation of Enteric Viruses In Water, is characterized in that: described means of trivalent copper ion stabilizer is a kind of in citric acid and gallic acid or both mixtures; Described cupric salt is the mixing of a kind of in copper sulfate and neutralized verdigris or two kinds; Described persulphate is one or more the mixing in ammonium persulphate, Sodium Persulfate, Potassium Persulphate, monopersulfate ammonium, monopersulfate sodium and Potassium Monopersulfate.
5. the efficient method for killing of drinking Inactivation of Enteric Viruses In Water as claimed in claim 4, is characterized in that: described means of trivalent copper ion stabilizer is the mixture of citric acid and gallic acid, the mol ratio of citric acid and gallic acid is 1～3:1.
6. the method for killing of drinking Inactivation of Enteric Viruses In Water as claimed in claim 4, is characterized in that: described cupric salt is that foreign matter content is no more than 0.05% copper sulfate.
7. the method for killing of drinking Inactivation of Enteric Viruses In Water as described in claim 1 or 2 or 3, is characterized in that: in step (3), the pH value of water to be sterilized is 5.5～7.5.
8. the method for killing of drinking Inactivation of Enteric Viruses In Water as described in claim 1 or 2 or 3, is characterized in that: in step (3), the temperature of water to be sterilized is 5～40 DEG C.
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| CN201410142384.0A CN103951102B (en) | 2014-04-10 | 2014-04-10 | A kind of method for killing drinking Inactivation of Enteric Viruses In Water |
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| CN201410142384.0A CN103951102B (en) | 2014-04-10 | 2014-04-10 | A kind of method for killing drinking Inactivation of Enteric Viruses In Water |
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Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4492618A (en) * | 1979-03-22 | 1985-01-08 | Bernd Eder | Method of disinfecting water, in particular swimming pool water |
| CN87102687A (en) * | 1982-10-22 | 1988-10-26 | 克莱斯塔尔克莱公司Sa | The method of water treatment and product |
| DE102005059135A1 (en) * | 2005-12-10 | 2007-06-14 | Chemoform Gmbh & Co. Kg | Disinfectant in the form of substance arrays for swimming pool water, comprises separate units containing chemical substances |
| CN101973622A (en) * | 2010-10-19 | 2011-02-16 | 哈尔滨工业大学 | Method for accelerating monopersulfate and persulfate to produce free sulfate radicals |
-
2014
- 2014-04-10 CN CN201410142384.0A patent/CN103951102B/en not_active Expired - Fee Related
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4492618A (en) * | 1979-03-22 | 1985-01-08 | Bernd Eder | Method of disinfecting water, in particular swimming pool water |
| CN87102687A (en) * | 1982-10-22 | 1988-10-26 | 克莱斯塔尔克莱公司Sa | The method of water treatment and product |
| DE102005059135A1 (en) * | 2005-12-10 | 2007-06-14 | Chemoform Gmbh & Co. Kg | Disinfectant in the form of substance arrays for swimming pool water, comprises separate units containing chemical substances |
| CN101973622A (en) * | 2010-10-19 | 2011-02-16 | 哈尔滨工业大学 | Method for accelerating monopersulfate and persulfate to produce free sulfate radicals |
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