CN113292151A - Application of sodium azide in degradation of organic matters and method for treating organic wastewater by ozone - Google Patents
Application of sodium azide in degradation of organic matters and method for treating organic wastewater by ozone Download PDFInfo
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- CN113292151A CN113292151A CN202110565224.7A CN202110565224A CN113292151A CN 113292151 A CN113292151 A CN 113292151A CN 202110565224 A CN202110565224 A CN 202110565224A CN 113292151 A CN113292151 A CN 113292151A
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- 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
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/725—Treatment of water, waste water, or sewage by oxidation by catalytic oxidation
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- 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
- C02F1/72—Treatment of water, waste water, or sewage by oxidation
- C02F1/78—Treatment of water, waste water, or sewage by oxidation with ozone
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- 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
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- 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
- C02F2101/306—Pesticides
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- 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
- C02F2101/32—Hydrocarbons, e.g. oil
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- 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
- C02F2101/36—Organic compounds containing halogen
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- 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
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
- C02F2305/023—Reactive oxygen species, singlet oxygen, OH radical
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Abstract
The invention discloses application of sodium azide in degradation of organic matters and a method for treating organic wastewater by ozone. The organic matters in part of the wastewater have very stable structures and are difficult to degrade in the conventional oxidation process, and the substances usually have stronger biotoxicity, so the biodegradability is poor. The method comprises the steps of adding sodium azide in the process of oxidizing refractory organic matters by ozone, and utilizing free azide generated by the reaction of the ozone and the sodium azideRadical (N)3And (h) and hydroxyl free radicals (. OH) oxidize electron-poor refractory organics to open the ring of refractory organics, thereby realizing deep degradation of refractory organics and improving the biodegradability of organic wastewater. The azide free radical generated in the reaction can be converted into nitrite and nitrate radical after reacting with organic matters or directly added on the organic matters, so that a nitrogen source can be provided for subsequent biological treatment, and the operation flow of the subsequent biological treatment is simplified.
Description
Technical Field
The invention belongs to the technical field of organic wastewater treatment, and particularly relates to application of sodium azide in ozone oxidation treatment of organic wastewater.
Background
Some pesticides (such as atrazine and the like) and odor substances (such as 2, 6-dimethyl pyrazine and the like) in the water body have very stable structures and are difficult to degrade in the conventional oxidation process, and the substances generally have stronger biotoxicity, so the biodegradability is poor, and organic pollutants such as atrazine, 2, 6-dimethyl pyrazine and the like in the water body are difficult to remove by adopting a biodegradation method.
The ozone oxidation method is a commonly used method in the current water pollution control project, and ozone is generally used as a pretreatment or advanced treatment process in drinking water treatment, sewage treatment and environmental water purification technologies. However, ozone oxidation can only oxidize the organic matters rich in electrons in water, and cannot attack poor-electron refractory organic matters or open the rings of refractory organic matters. Therefore, the ozone oxidation technology has low removal efficiency on atrazine (namely 2-chloro-4-ethylamino-6-isopropylamino-1, 3, 5-triazine), 2, 6-dimethyl pyrazine and other substances which are difficult to degrade in the water body.
Ozone catalytic oxidation is an advanced oxidation technology based on ozone oxidation, and is an effective method for realizing deep degradation of refractory organic matters in water and improving biodegradability. Catalytic ozonation can be divided into two main categories, homogeneous ozonation and heterogeneous ozonation, according to the type of catalytic material. Heterogeneous ozone catalytic oxidation usually requires the addition of a solid catalyst, has high reaction requirements, and is difficult to separate catalytic materials from water. Compared with the prior art, the homogeneous method for catalyzing the ozone to generate the free radicals has the advantages of high speed, stability, convenience in adjusting the adding dosage and the like. The traditional homogeneous ozone catalysis method usually needs to add metal ions, or is initiated by methods such as UV, electricity, ultrasound and the like, the former can introduce the metal ions to cause pollution, and the latter needs to input a large amount of energy into a system and needs other large-scale equipment except an ozone generator, so the economical efficiency and the convenience degree are both limited.
Disclosure of Invention
The invention aims to catalyze ozone to generate azido free radical (N) with strong oxidizing ability by adding sodium azide3And hydroxyl radical (. OH) to provide a solution for degrading organic substances with stable structures,
in a first aspect, the invention provides an application of sodium azide in degradation of organic matters; in this application, ozone is required. Azido radical (N) generated by reaction of ozone and sodium azide3And (h) and hydroxyl radical (. OH) to oxidize electron-poor refractory organics and open the ring of refractory organics.
In a second aspect, the invention provides a method for treating refractory organic wastewater, which comprises the following specific processes: adding sodium azide into the organic wastewater to be treated and introducing ozone.
Preferably, the organic wastewater to be treated contains one or more of electron-poor organic matter and aromatic organic matter.
Preferably, the organic wastewater to be treated is subjected to a biological treatment after the reaction with sodium azide and ozone.
Preferably, the organic wastewater to be treated contains atrazine or 2, 6-dimethylpyrazine.
Preferably, the reaction temperature of the organic wastewater to be treated, sodium azide and ozone is 5 to 25 ℃.
Preferably, the COD value of the degraded organic wastewater is 0-1000 mg/L.
Preferably, the introduction amount of the ozone relative to the organic wastewater is 1-100 times of the COD value of the organic wastewater; the mass concentration of the sodium azide relative to the organic wastewater is 0.01-1 times of the mass concentration of the ozone relative to the organic wastewater.
Preferably, the adding time of the sodium azide is less than or equal to the ozone introducing time.
Preferably, the organic waste water is adjusted to acidic conditions before the addition of sodium azide and the introduction of ozone.
The invention has the beneficial effects that:
the method comprises the steps of adding sodium azide in the process of oxidizing refractory organic matters by using ozone, and using azido free radicals (N) generated by the reaction of the ozone and the sodium azide3And (h) and hydroxyl free radicals (. OH) oxidize electron-poor refractory organics to open the ring of refractory organics, thereby realizing deep degradation of refractory organics and improving the biodegradability of organic wastewater.
2. The azide free radical generated in the reaction can be converted into nitrite and nitrate radical after reacting with organic matters or directly added on the organic matters, so that a nitrogen source can be provided for subsequent biological treatment, and the operation flow of the subsequent biological treatment is simplified.
Drawings
FIG. 1 shows the formation of azide radicals (N) by ozone and sodium azide in the present invention3·) and hydroxyl radicals (· OH) degrade contaminants in water.
Fig. 2 is a graph showing the degradation profile of the pesticide atrazine in example 1.
FIG. 3 is a graph showing the degradation profile of the odorant, 2, 6-dimethylpyrazine, in water in example 6.
Detailed Description
The invention is further described below with reference to the accompanying drawings.
An application of sodium azide in ozone oxidation treatment of organic wastewater comprises the following specific processes: adding sodium azide into the organic wastewater difficult to degrade and introducing ozone. The COD value of the degraded organic wastewater is 0-1000 mg/L; for organic wastewater with COD value over 1000mg/L, the organic wastewater is firstly diluted to be within the range of 0-1000mg/L and then treated.
The introduction amount of the ozone relative to the organic wastewater is 1-100 times of the COD value of the organic wastewater, the introduction speed of the ozone is 10 mg/min-3 g/min, and the introduction time of the ozone is determined according to the introduction mass of the ozone divided by the introduction speed.
The adding mass of the sodium azide is 0.01-1 time of the introducing mass of the ozone. Specifically, the sodium azide is added in any one of a one-time adding mode, a small amount of adding mode for multiple times and a continuous adding mode. The adding time of the sodium azide is less than or equal to the ozone introducing time.
Because sodium azide can better promote ozone to generate azide free radicals and hydroxyl free radicals with extremely strong oxidizing ability under the acidic condition, the pH value in the system is controlled to be 0-7. For organic wastewater with the initial pH value of more than or equal to 7, the pH value is reduced by adding sulfuric acid, nitric acid, hydrochloric acid and the like.
In order to remove the refractory organic matters such as pesticide or odor substances in the actual water body at normal temperature, the reaction temperature is controlled between 5 ℃ and 25 ℃.
Example 1
The organic pollutant in the organic wastewater is atrazine. The initial concentration of atrazine is 1mg/L, the reaction temperature is 10 ℃, the reaction pH value is 3, and NaN3The adding amount of the ozone is 0.3mg/L, the adding amount of the ozone is 3mg/L, and NaN3The adding mode is one-time adding, and the reaction time is 30 min. Through detection, the removal rate of atrazine is 100%.
The degrading effect of the organic atrazine in example 1 is shown in FIG. 2, wherein the line drawn at point ■ indicates the absence of NaN3Degradation curve of atrazine, line □ shows NaN3Degradation profile of atrazine in presence. As can be seen from FIG. 2, no NaN was added when atrazine was treated for 10min3The residual rate of atrazine in the solution was about 50% and NaN was added3The remaining rate of atrazine in the solution of (a) was about 10%. No NaN addition as the reaction time was prolonged3The remaining rate of atrazine in the solution was maintained at substantially 50%, while NaN was added3The residual rate of atrazine in the solution is still slowly reduced, and the residual rate of atrazine in the solution is 0 percent when the treatment time reaches 30 min.
Example 2
The organic pollutant in the organic wastewater is atrazine. The initial concentration of atrazine is 10mg/L, the reaction temperature is 20 ℃, the reaction pH value is 3, and NaN3The dosage of the ozone is 5mg/L, the dosage of the ozone is 30mg/L, and NaN3The adding mode is that the adding is continuously carried out for 10min, and the reaction time is 60 min. Through detection, the removal rate of atrazine is 95%.
Example 3
The organic pollutant in the organic wastewater is atrazine. The initial concentration of atrazine is 100mg/L, the reaction temperature is 15 ℃, the reaction pH value is 7, and NaN3The dosage of the ozone is 100mg/L, the dosage of the ozone is 200mg/L, and NaN3The adding mode is that the adding is continuously carried out for 60min, and the reaction time is 60 min. Through detection, the removal rate of atrazine is 100%.
Example 4
The organic pollutant in the organic wastewater is atrazine. The initial concentration of atrazine is 50mg/L, and the reaction temperature is 20 ℃; adding HCl to reduce the pH value to 5, NaN3The dosage of the ozone is 50mg/L, the dosage of the ozone is 200mg/L, and NaN3The adding mode is that the adding is continuously carried out for 30min, and the reaction time is 30 min. Through detection, the removal rate of atrazine is 95%.
Example 5
The organic pollutant in the organic wastewater is atrazine. The initial concentration of atrazine is 20mg/L, the reaction temperature is 25 ℃, the reaction pH value is 5, and NaN3The dosage is 10mg/L, the dosage of ozone is 20mg/L, NaN3The adding mode is one-time adding, and the reaction time is 30 min. Through detection, the atrazine removal rate is 90%.
Example 6
The organic pollutant in the organic wastewater is 2, 6-dimethyl pyrazine. The initial concentration of 2, 6-dimethylpyrazine is 0.5mg/L, the reaction temperature is 10 ℃, the reaction pH value is 3, and NaN3The dosage is 0.5mg/L, the dosage of ozone is 3mg/L, NaN3The adding mode is one-time adding, and the reaction time is 30 min. Through detection, the removal rate of the 2, 6-dimethyl pyrazine is 88%.
Example 6 smelling substance 2, 6-dimethylThe degrading effect of the pyrazine is shown in FIG. 3, in which the line drawn at point ■ indicates the absence of NaN3The degradation curve of 2, 6-dimethylpyrazine is shown by the line at point □3Degradation profile of 2, 6-dimethylpyrazine in the presence. As can be seen from FIG. 3, when 2, 6-dimethylpyrazine was treated for 5min, NaN was not added3The residual rate of 2, 6-dimethylpyrazine in the solution of (1) was about 80%, and NaN was added3The remaining ratio of 2, 6-dimethylpyrazine in the solution of (1) is about 20%. No NaN addition as the reaction time was prolonged3The residual rate of 2, 6-dimethylpyrazine in the solution of (1) was maintained at substantially 80%, while NaN was added3The remaining ratio of 2, 6-dimethylpyrazine in the solution of (1) was substantially maintained at 20%.
Example 7
The organic pollutant in the organic wastewater is 2, 6-dimethyl pyrazine. The initial concentration of 2, 6-dimethyl pyrazine is 5mg/L, the reaction temperature is 10 ℃, the reaction pH value is 3, and NaN3The dosage is 5mg/L, the dosage of ozone is 30mg/L, NaN3The adding mode is that the adding is continuously carried out for 30min, and the reaction time is 30 min. Through detection, the removal rate of the 2, 6-dimethyl pyrazine is 90%.
Example 8
The organic pollutant in the organic wastewater is 2, 6-dimethyl pyrazine. The initial concentration of 2, 6-dimethyl pyrazine is 50mg/L, the reaction temperature is 20 ℃, the reaction pH value is 5, and NaN3The dosage is 100mg/L, the dosage of ozone is 100mg/L, NaN3The adding mode is that the adding is continuously carried out for 60min, the reaction time is 60min, and the removal rate of the 2, 6-dimethyl pyrazine is 95 percent through detection.
Example 9
The organic pollutant in the organic wastewater is 2, 6-dimethyl pyrazine. The initial concentration of 2, 6-dimethyl pyrazine is 20mg/L, the reaction temperature is 25 ℃, the reaction pH value is 7, and NaN3The adding amount is 25mg/L, the adding amount of ozone is 50mg/L, the adding is continued for 15min, the reaction time is 60min, and the removal rate of the 2, 6-dimethyl pyrazine is 80% through detection.
Example 10
The organic pollutant in the organic wastewater is 2, 6-dimethyl pyrazine. Initial concentration of 2, 6-dimethylpyrazine of 20mg/L, reaction temperature 15 deg.C, reaction pH 5, NaN3The dosage is 25mg/L, the dosage of ozone is 25mg/L, NaN3The adding mode is one-time adding, the reaction time is 30min, and the detection shows that the removal rate of the 2, 6-dimethyl pyrazine is 85%.
As can be seen from the combination of examples 1 to 10, NaN3Can rapidly promote the ozone decomposition to generate strong oxidizing free radicals (N)3And. OH) degradation of organic matter which is difficult to degrade in water. The method can obviously improve the defects that the common ozone oxidation can only degrade the organic matters rich in electrons in water and can not attack the poor-electron refractory organic matters or open the ring of the refractory organic matters, and effectively treat the refractory organic pollutants with very stable structures of pesticides (such as atrazine and the like) and smelly substances (such as 2, 6-dimethyl pyrazine and the like) in the water body.
Claims (10)
1. An application of sodium azide in degrading organic matters.
2. The use of sodium azide according to claim 1 in the degradation of organic matter, wherein the sodium azide is selected from the group consisting of: ozone is introduced in the process of degrading organic matters.
3. A method for treating refractory organic wastewater is characterized by comprising the following steps: adding sodium azide into the organic wastewater to be treated and introducing ozone.
4. The method for treating refractory organic wastewater according to claim 1, wherein the method comprises the following steps: the organic wastewater to be treated contains one or more of electron-poor organic matters and aromatic organic matters.
5. The method for treating refractory organic wastewater according to claim 1, wherein the method comprises the following steps: the organic wastewater to be treated contains atrazine or 2, 6-dimethyl pyrazine.
6. The method for treating refractory organic wastewater according to claim 1, wherein the method comprises the following steps: the organic wastewater to be treated is biologically treated after reacting with sodium azide and ozone.
7. The method for treating refractory organic wastewater according to claim 1, wherein the method comprises the following steps: the reaction temperature of the organic wastewater to be treated, sodium azide and ozone is 5-25 ℃.
8. The method for treating refractory organic wastewater according to claim 1, wherein the method comprises the following steps: the COD value of the degraded organic wastewater is 0-1000 mg/L; before adding sodium azide and introducing ozone, the organic wastewater is adjusted to be in an acidic condition.
9. The method for treating refractory organic wastewater according to claim 1, wherein the method comprises the following steps: the introduction amount of ozone relative to the organic wastewater is 1-100 times of the COD value of the organic wastewater; the mass concentration of the sodium azide relative to the organic wastewater is 0.01-1 times of the mass concentration of the ozone relative to the organic wastewater.
10. The method for treating refractory organic wastewater according to claim 1, wherein the method comprises the following steps: the adding time of the sodium azide is less than or equal to the ozone introducing time.
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Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20040077917A1 (en) * | 2002-10-22 | 2004-04-22 | Steris Inc. | Use of an ozone containing fluid to neutralize chemical and/or biological warfare agents |
| WO2009131615A2 (en) * | 2008-04-23 | 2009-10-29 | Siemens Water Technologies Corp. | Process for decontamination of inorganic hazardous components from a waste stream |
| CN101708883A (en) * | 2009-12-18 | 2010-05-19 | 哈尔滨工业大学 | Light promoting dehalogenation compound medicament/light combined method for removing halogenated organic matters in water |
| CN107935309A (en) * | 2017-12-01 | 2018-04-20 | 南京理工大学 | Priming produces waste water physicochemical pre-treat biological intensive treatment integrated technique |
-
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- 2021-05-24 CN CN202110565224.7A patent/CN113292151A/en active Pending
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20040077917A1 (en) * | 2002-10-22 | 2004-04-22 | Steris Inc. | Use of an ozone containing fluid to neutralize chemical and/or biological warfare agents |
| WO2009131615A2 (en) * | 2008-04-23 | 2009-10-29 | Siemens Water Technologies Corp. | Process for decontamination of inorganic hazardous components from a waste stream |
| CN101708883A (en) * | 2009-12-18 | 2010-05-19 | 哈尔滨工业大学 | Light promoting dehalogenation compound medicament/light combined method for removing halogenated organic matters in water |
| CN107935309A (en) * | 2017-12-01 | 2018-04-20 | 南京理工大学 | Priming produces waste water physicochemical pre-treat biological intensive treatment integrated technique |
Non-Patent Citations (2)
| Title |
|---|
| 侯艳君: "《臭氧金属氧化物催化降解水中有机物的研究》", 30 June 2013, 黑龙江大学出版社 * |
| 海关总署关税征管司: "《危险化学品归类指南 上》", 31 August 2017, 中国海关出版社 * |
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