CN112897635A - Method for removing organic chloramine in drinking water - Google Patents
Method for removing organic chloramine in drinking water Download PDFInfo
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- CN112897635A CN112897635A CN202110109871.7A CN202110109871A CN112897635A CN 112897635 A CN112897635 A CN 112897635A CN 202110109871 A CN202110109871 A CN 202110109871A CN 112897635 A CN112897635 A CN 112897635A
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- chloramine
- organic chloramine
- ultraviolet
- drinking water
- water
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- QDHHCQZDFGDHMP-UHFFFAOYSA-N Chloramine Chemical compound ClN QDHHCQZDFGDHMP-UHFFFAOYSA-N 0.000 title claims abstract description 68
- 238000000034 method Methods 0.000 title claims abstract description 47
- 239000003651 drinking water Substances 0.000 title claims abstract description 17
- 235000020188 drinking water Nutrition 0.000 title claims abstract description 17
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 38
- 239000000460 chlorine Substances 0.000 claims description 32
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 claims description 30
- 229910052801 chlorine Inorganic materials 0.000 claims description 30
- 230000005855 radiation Effects 0.000 claims description 9
- QSHDDOUJBYECFT-UHFFFAOYSA-N mercury Chemical compound [Hg] QSHDDOUJBYECFT-UHFFFAOYSA-N 0.000 claims description 4
- 229910052753 mercury Inorganic materials 0.000 claims description 4
- 238000009281 ultraviolet germicidal irradiation Methods 0.000 claims description 4
- 238000005286 illumination Methods 0.000 claims description 3
- 238000004659 sterilization and disinfection Methods 0.000 abstract description 31
- 239000006227 byproduct Substances 0.000 abstract description 27
- 238000005660 chlorination reaction Methods 0.000 abstract description 9
- 239000000645 desinfectant Substances 0.000 abstract description 4
- OPTASPLRGRRNAP-UHFFFAOYSA-N cytosine Chemical compound NC=1C=CNC(=O)N=1 OPTASPLRGRRNAP-UHFFFAOYSA-N 0.000 description 16
- 229940104302 cytosine Drugs 0.000 description 8
- 230000035484 reaction time Effects 0.000 description 8
- 230000003647 oxidation Effects 0.000 description 6
- 238000007254 oxidation reaction Methods 0.000 description 6
- 239000005708 Sodium hypochlorite Substances 0.000 description 5
- SUKJFIGYRHOWBL-UHFFFAOYSA-N sodium hypochlorite Chemical compound [Na+].Cl[O-] SUKJFIGYRHOWBL-UHFFFAOYSA-N 0.000 description 5
- HEDRZPFGACZZDS-UHFFFAOYSA-N Chloroform Chemical compound ClC(Cl)Cl HEDRZPFGACZZDS-UHFFFAOYSA-N 0.000 description 4
- 241000195493 Cryptophyta Species 0.000 description 4
- STZZWJCGRKXEFF-UHFFFAOYSA-N Dichloroacetonitrile Chemical compound ClC(Cl)C#N STZZWJCGRKXEFF-UHFFFAOYSA-N 0.000 description 4
- 230000000694 effects Effects 0.000 description 4
- 150000001412 amines Chemical class 0.000 description 3
- 125000003277 amino group Chemical group 0.000 description 3
- 239000002075 main ingredient Substances 0.000 description 3
- 244000005700 microbiome Species 0.000 description 3
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 3
- JRKICGRDRMAZLK-UHFFFAOYSA-L peroxydisulfate Chemical compound [O-]S(=O)(=O)OOS([O-])(=O)=O JRKICGRDRMAZLK-UHFFFAOYSA-L 0.000 description 3
- 239000002243 precursor Substances 0.000 description 3
- 230000015572 biosynthetic process Effects 0.000 description 2
- 239000013043 chemical agent Substances 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 239000003814 drug Substances 0.000 description 2
- 238000012986 modification Methods 0.000 description 2
- 230000004048 modification Effects 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 231100000331 toxic Toxicity 0.000 description 2
- 230000002588 toxic effect Effects 0.000 description 2
- HFFLGKNGCAIQMO-UHFFFAOYSA-N trichloroacetaldehyde Chemical compound ClC(Cl)(Cl)C=O HFFLGKNGCAIQMO-UHFFFAOYSA-N 0.000 description 2
- QNGVNLMMEQUVQK-UHFFFAOYSA-N 4-n,4-n-diethylbenzene-1,4-diamine Chemical compound CCN(CC)C1=CC=C(N)C=C1 QNGVNLMMEQUVQK-UHFFFAOYSA-N 0.000 description 1
- USVZHTBPMMSRHY-UHFFFAOYSA-N 8-[(6-bromo-1,3-benzodioxol-5-yl)sulfanyl]-9-[2-(2-chlorophenyl)ethyl]purin-6-amine Chemical compound C=1C=2OCOC=2C=C(Br)C=1SC1=NC=2C(N)=NC=NC=2N1CCC1=CC=CC=C1Cl USVZHTBPMMSRHY-UHFFFAOYSA-N 0.000 description 1
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 description 1
- DRUIESSIVFYOMK-UHFFFAOYSA-N Trichloroacetonitrile Chemical compound ClC(Cl)(Cl)C#N DRUIESSIVFYOMK-UHFFFAOYSA-N 0.000 description 1
- 238000009303 advanced oxidation process reaction Methods 0.000 description 1
- 230000002238 attenuated effect Effects 0.000 description 1
- 230000015556 catabolic process Effects 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000006731 degradation reaction Methods 0.000 description 1
- JSYGRUBHOCKMGQ-UHFFFAOYSA-N dichloramine Chemical compound ClNCl JSYGRUBHOCKMGQ-UHFFFAOYSA-N 0.000 description 1
- 239000003344 environmental pollutant Substances 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- QEHKBHWEUPXBCW-UHFFFAOYSA-N nitrogen trichloride Chemical compound ClN(Cl)Cl QEHKBHWEUPXBCW-UHFFFAOYSA-N 0.000 description 1
- 125000001477 organic nitrogen group Chemical group 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 238000006303 photolysis reaction Methods 0.000 description 1
- 230000015843 photosynthesis, light reaction Effects 0.000 description 1
- 231100000719 pollutant Toxicity 0.000 description 1
- 239000000047 product Substances 0.000 description 1
- 238000000746 purification Methods 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 230000001954 sterilising effect Effects 0.000 description 1
- 231100000419 toxicity Toxicity 0.000 description 1
- 230000001988 toxicity Effects 0.000 description 1
Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/66—Treatment of water, waste water, or sewage by neutralisation; pH adjustment
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/30—Treatment of water, waste water, or sewage by irradiation
- C02F1/32—Treatment of water, waste water, or sewage by irradiation with ultraviolet light
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
Abstract
The invention relates to a method for removing organic chloramine in drinking water, which directly irradiates a water body with the organic chloramine, namely realizes the removal of the organic chloramine in the water body. Compared with the prior art, the method can safely and efficiently remove the generated organic chloramine, and simultaneously reduces the generation amount of disinfection byproducts, thereby reducing the misjudgment of the residual amount of the effective disinfectant in water in the subsequent chlorination disinfection process and improving the technical level of water quality safety guarantee.
Description
Technical Field
The invention belongs to the technical field of water treatment, and relates to a method for removing organic chloramine in drinking water.
Background
Various soluble organic nitrogen substances commonly exist in source water, and many of the substances contain-NH2Or amino groups such as-NH-free chlorine orIn the reaction of chloramine, H on amino group is easily substituted by Cl to produce a kind of chloro derivative organic chloramine. This form of chloramine is associated with inorganic monochloramine (NH)2Cl), dichloramine (NHCl)2) And trichloroamine (NCl)3) Similarly, when the total chlorine is measured by conventional N, N-diethyl-p-phenylenediamine (DPD) color method, it is detected as a part of the total chlorine (Water Research,2007,41, 3097-. However, unlike inorganic chloramines, these organic chloramines have poor oxidizing sterilization capabilities (Water Research,2003,37, 1557-. Once generated, part of organic chloramine can exist in Water stably for a long time, for example, when Research shows that a high algae Water source is subjected to pre-chlorination treatment, a large amount of organic chloramine can be generated, and the organic chloramine is stable in Water, so that the addition and the allowance control of chlorine (amine) disinfectant in the subsequent Water treatment disinfection process are seriously interfered (Water Research,2016,103, 189-. In addition, some organic chloramines are further degraded and converted into "trihalo" toxic disinfection byproducts such as trihalomethanes, haloacetonitrile, halonitromethanes, etc. in the presence of excess free chlorine or chloramines (Chemosphere,2018,195, 673-682). Therefore, it is not advisable to increase the dosage of chlorine (amine) to make up for the interference judgment of organic chloramine, which not only increases the cost of the medicament, but also causes the risk of the effluent of waterworks and the overproof disinfection by-products on the peripheral water surface of pipe networks.
Chinese patent CN102381740A discloses a method for removing nitrogen-containing disinfection byproducts in water based on persulfate/light combination, which comprises the steps of firstly adding persulfate into water containing nitrogen-containing disinfection byproducts, and then carrying out light irradiation to complete the method. Although the patent also adopts a method of reducing nitrogen-containing disinfection byproducts by ultraviolet radiation, the method must rely on the previously added compound medicament such as persulfate to generate free radicals, so that after treatment, the method is easy to cause the generation of new pollutants, such as excessive sulfate and the like, and is not suitable for the treatment of drinking water.
Disclosure of Invention
The invention aims to provide a method for removing organic chloramine from drinking water, which is safe and economical without adding other chemical agents and can minimize the risk of other disinfection byproducts in the removal process through the limitation of specific reaction conditions.
The purpose of the invention can be realized by the following technical scheme:
a method for removing organic chloramine in drinking water is characterized in that ultraviolet irradiation is directly carried out on a water body with the organic chloramine, so that the organic chloramine in the water body is removed.
Furthermore, the pH value of the water body is adjusted to 7-9 before ultraviolet irradiation, so that higher organic chloramine removal rate can be realized, and the generation amount of disinfection byproducts is ensured to be at a lower level. More preferably, the pH of the water is adjusted to 9 prior to UV irradiation.
Further, the ultraviolet light source used for ultraviolet irradiation is a low-pressure ultraviolet mercury lamp. Further, the wavelength of ultraviolet light emitted from the low-pressure ultraviolet mercury lamp was 254 nm. The method has low cost and easy realization, and has better control effect on the removal of the organic chloramine and the generation of disinfection byproducts compared with other wavelength light sources.
Further, the illumination intensity of the ultraviolet irradiation is 100-150 muW/cm2The ultraviolet radiation dose is kept at 400mJ/cm2In the above, a higher removal rate of organic chloramine and a lower amount of disinfection by-products can be achieved.
Furthermore, the time of ultraviolet irradiation is 20-60 min.
Further, the time of ultraviolet irradiation is 60 min.
Further, the whole process is carried out at normal temperature and normal pressure.
Further, the water body is a water body which is added with free chlorine or chloramine to react to generate organic chloramine.
Compared with the prior art, the invention has the following advantages:
(1) the invention solves the problems that organic chloramine is difficult to remove and disinfection byproducts are difficult to control in the water purification process.
(2) The method is simple and easy to realize, can be realized by adopting the ultraviolet irradiation process commonly used for water treatment and disinfection at present, does not need to add other chemical agents, and is safe and economic.
(3) The pH range applicable to the method is highly consistent with the actual pH value of the drinking water, and the method can be carried out at normal temperature and normal pressure, and is convenient and quick to regulate and control.
(4) The method can improve the determination accuracy of the residual disinfectant in water in the subsequent chlorination (amine) process after treatment, and avoid biosafety risks caused by overestimation of the residual effective disinfectant.
Drawings
FIG. 1 is a graph of the effect of chlorine alone, UV alone, and UV/chlorine advanced oxidation on the removal of organic chloramines;
FIG. 2 is a comparison of disinfection by-product formation during the removal of organic chloramine by chlorine alone, ultraviolet alone, and ultraviolet/chlorine advanced oxidation;
FIG. 3 is a graph showing the removal rate of organic chloramine and the formation of disinfection byproducts by UV photolysis at various pH's.
Detailed Description
The invention is described in detail below with reference to the figures and specific embodiments. The present embodiment is implemented on the premise of the technical solution of the present invention, and a detailed implementation manner and a specific operation process are given, but the scope of the present invention is not limited to the following embodiments.
In the following examples, unless otherwise specified, raw material reagents and processing techniques are all conventional commercial products or conventional processing techniques in the art.
Example 1
The method takes cytosine which is a main ingredient in DNA of algae and microorganisms widely existing in water source water as a precursor, and generates the target organic chloramine by pre-chlorination (the initial concentration of the cytosine is 100 mu M, the pH value is 7, the adding amount of sodium hypochlorite is 300 mu M, and the reaction time is 3 h). Then, chlorine is added separately, ultraviolet radiation is added separately, and ultraviolet/chlorine is added simultaneously to remove and compare organic chloramine by different methods, wherein the adding amount of sodium hypochlorite is 100 mu M, the ultraviolet illumination intensity is 111 mu W/cm2The pH is controlled to be 7, the reaction time is controlled to be 0, 2, 10,20. Samples were taken at corresponding time points for analysis of the organic chloramine concentration at 40 and 60 min.
As can be seen from FIG. 1(a), the organic chloramine generated by chlorination of cytosine is chemically very stable without any treatment and hardly changes in water with time; when the chlorination is carried out again, the generated organic chloramine is not degraded but has a trend of increasing obviously in a short time, because a plurality of amino groups are arranged on the molecular structure of the cytosine, the yield of the organic chloramine is increased under the condition of excessive residual chlorine, the organic chloramine is attenuated along with the reaction time, the whole organic chloramine is kept stable, and the initial concentration is not reduced obviously; when the treatment is carried out by adopting ultraviolet irradiation or ultraviolet/chlorine advanced oxidation (ultraviolet and chlorine are added simultaneously), the organic chloramine is obviously degraded, and the degradation effects of the two methods are basically consistent. As summarized in FIG. 1(b), the generated organic chloramine can be removed by ultraviolet irradiation alone or by ultraviolet/chlorine advanced oxidation at 60min (corresponding to an ultraviolet irradiation dose of 400 mJ/cm)2) The removal rate can reach more than 60 percent, and the chlorine addition alone can not remove the organic chloramine but promote the concentration of the organic chloramine to rise again.
Example 2
The method takes cytosine which is a main ingredient in DNA of algae and microorganisms widely existing in water source water as a precursor, and generates the target organic chloramine by pre-chlorination (the initial concentration of the cytosine is 100 mu M, the pH value is 7, the adding amount of sodium hypochlorite is 300 mu M, and the reaction time is 3 h). Then, chlorine is added separately, ultraviolet irradiation is carried out separately, and ultraviolet/chlorine is added simultaneously to carry out organic chloramine removal comparison in different methods. Wherein the sodium hypochlorite dosage is 100 μ M, and the ultraviolet irradiation intensity is 111 μ W/cm2pH was controlled to 7, reaction time was controlled to 0, 2, 10, 20, 40 and 60min, and samples were taken at the respective time points to analyze the amount of generated disinfection byproducts.
As is evident from FIG. 2, treatment of organic chloramine by three means produced disinfection byproducts, with 3 disinfection byproducts detected during chlorine addition alone and ultraviolet irradiation alone, including chloroform, chloral, and dichloroacetonitrile, and 4 disinfection byproducts detected during ultraviolet/chlorine advanced oxidation treatment, including chloroform, chloral, dichloroacetonitrile, and trichloroacetonitrile. The use of chlorine alone for the treatment of organic chloramines produces minimal total amounts of disinfection by-products and tends to increase slightly with reaction time. The concentration of disinfection by-products generated by adopting ultraviolet/chlorine advanced oxidation and independent ultraviolet irradiation is integrally increased and then reduced along with the reaction time, wherein the total amount of the disinfection by-products generated in the ultraviolet/chlorine advanced oxidation process is obviously higher than that of the disinfection by-products generated by independent ultraviolet and independent chlorine addition. While ultraviolet radiation alone produces a slightly higher total amount of disinfection by-products than chlorine alone, but significantly less than the ultraviolet/chlorine process, ultraviolet radiation alone is preferred as the optimal removal method for organochlorine, given that chlorine alone has no significant effect on organochlorine removal.
In addition, the dosage of the ultraviolet radiation is continuously increased to be higher than 133mJ/cm2Then, the disinfection by-products generated by the independent ultraviolet irradiation are gradually reduced and reach 400mJ/cm2Above, the concentration produced is further reduced, even lower than in the chlorination process alone. In combination with the results of example 1, the removal rate of organic chloramine is over 60% at most, so that the ultraviolet radiation dose of 400mJ/cm is preferred2The above is taken as the optimum dosage range for ultraviolet removal of organic chloramine.
Example 3
The method takes cytosine which is a main ingredient in DNA of algae and microorganisms widely existing in water source water as a precursor, and generates the target organic chloramine by pre-chlorination (the initial concentration of the cytosine is 100 mu M, the pH value is 7, the adding amount of sodium hypochlorite is 300 mu M, and the reaction time is 3 h). Then a separate uv irradiation treatment is performed. Wherein the ultraviolet radiation dose is 400mJ/cm2The pH was controlled at 5,6, 7, 8, and 9, respectively, and the organic chloramine removal rate and the amount of disinfection byproducts generated were analyzed at different pH.
As can be seen from FIG. 3, the removal rate of organic chloramine increases with increasing pH, which is about 80% at pH 9. The amount of the disinfection by-products generated is slightly lower than that of the disinfection by-products generated under the neutral and alkaline conditions, but the total concentration is below 35 mu g/L, and the total amount of the disinfection by-products is basically kept unchanged in the pH range of 7-9, but dichloroacetonitrile with strong toxicity tends to increase. The present invention preferably controls the pH between 7 and 9, considering that the removal rate of organic chloramine can exceed 60% at pH 7-9, while avoiding the production of too much of the more toxic dichloroacetonitrile.
The embodiments described above are described to facilitate an understanding and use of the invention by those skilled in the art. It will be readily apparent to those skilled in the art that various modifications to these embodiments may be made, and the generic principles described herein may be applied to other embodiments without the use of the inventive faculty. Therefore, the present invention is not limited to the above embodiments, and those skilled in the art should make improvements and modifications within the scope of the present invention based on the disclosure of the present invention.
Claims (10)
1. The method for removing the organic chloramine in the drinking water is characterized in that ultraviolet irradiation is directly carried out on a water body with the organic chloramine, so that the organic chloramine in the water body is removed.
2. The method for removing organic chloramine from drinking water according to claim 1, wherein the pH of the water body is adjusted to 7-9 before the UV irradiation.
3. The method for removing organic chloramine from drinking water according to claim 1, wherein the pH of the water body is adjusted to 9 before the UV irradiation.
4. The method for removing organic chloramine from drinking water according to claim 1, wherein the ultraviolet light source used for ultraviolet irradiation is a low pressure ultraviolet mercury lamp.
5. The method of claim 4, wherein the ultraviolet light from the low pressure ultraviolet mercury lamp has a wavelength of 254 nm.
6. The method for removing organic chloramine from drinking water as claimed in claim 1Characterized in that the illumination intensity of the ultraviolet irradiation is 100-150 mu W/cm2The ultraviolet radiation dose is kept at 400mJ/cm2The above.
7. The method for removing organic chloramine from drinking water as claimed in claim 6, wherein the time of ultraviolet irradiation is 20-60 min.
8. The method for removing organic chloramine from drinking water as claimed in claim 6, wherein the time of ultraviolet irradiation is 60 min.
9. The method for removing organic chloramine from drinking water according to claim 1, wherein the whole process is carried out at normal temperature and pressure.
10. The method for removing organic chloramine from drinking water according to claim 1, wherein the water body is a water body which is added with free chlorine or chloramine to react to generate organic chloramine.
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