CN114477439A - Method for anaerobic biodegradation of halogenated phenol by static magnetic field enhancement - Google Patents
Method for anaerobic biodegradation of halogenated phenol by static magnetic field enhancement Download PDFInfo
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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
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/28—Anaerobic digestion processes
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
- C02F3/342—Biological treatment of water, waste water, or sewage characterised by the microorganisms used characterised by the enzymes used
-
- 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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- Life Sciences & Earth Sciences (AREA)
- Microbiology (AREA)
- Biodiversity & Conservation Biology (AREA)
- Hydrology & Water Resources (AREA)
- Engineering & Computer Science (AREA)
- Environmental & Geological Engineering (AREA)
- Water Supply & Treatment (AREA)
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Purification Treatments By Anaerobic Or Anaerobic And Aerobic Bacteria Or Animals (AREA)
- Removal Of Specific Substances (AREA)
Abstract
The invention discloses a method for carrying out enhanced anaerobic biodegradation on halogenated phenol by a static magnetic field. The method comprises the following steps: adding simulated wastewater with the concentration of halogenated phenol of 10-50 mg/L into anaerobic sludge to finish sludge domestication; placing the domesticated anaerobic sludge in a magnetic field to construct a static magnetic field coupling anaerobic biological system; adding the halogenated phenol wastewater into a static magnetic field coupling anaerobic biological system to degrade the halogenated phenol. According to the invention, a low-strength static magnetic field is introduced into the anaerobic microorganism system, so that extracellular polymer and enzyme activity of bacteria can be effectively promoted, the capability of the anaerobic organism for resisting external complex environment fluctuation is improved, the long-term stability of the anaerobic organism system is promoted, and the removal rate of the halogenated phenol in the wastewater can reach more than 98% under the optimal condition. The method has low cost, high efficiency and simplicity, and reduces the treatment cost of the wastewater.
Description
Technical Field
The invention belongs to the technical field of halogenated phenol-containing industrial wastewater treatment, and relates to a method for degrading halogenated phenol by static magnetic field enhanced anaerobic biodegradation.
Background
The halogenated phenols in the phenol compounds have an electron-withdrawing effect due to the halogenated groups on the benzene rings, so that the molecular polarity of the phenol compounds is enhanced, p electrons of halogen atoms and pi electrons on the benzene rings can form a very stable conjugated system, and the phenol compounds are easy to combine with enzyme systems in organisms to generate long-term chronic toxic action on the organisms. Halogenated phenols, especially bromophenol, widely exist in waste water discharge of fuel, paint, photography, pesticide, fire retardant and wood preservative industries, have the characteristics of carcinogenicity, teratogenicity, mutagenicity and the like, are difficult to degrade under natural conditions, have persistence and bioaccumulation, and are continuously found in plants, animals and even human bodies.
At present, the treatment method of the waste water containing halogenated phenols mainly comprises a physical and chemical method and a biological method. The physical and chemical methods comprise an adsorption method, a solvent extraction method, a Fenton method, a photocatalytic degradation method, an ozone oxidation method, a membrane separation method, an electrochemical oxidation method and the like, and although the method has good effect and high speed, the method has the defects of high cost and high energy consumption, and even has the condition of secondary pollution. Biological methods include aerobic biological methods and anaerobic biological methods. Due to the action of certain phenolic organic pollutants and the electron-withdrawing group halogenated group on the benzene ring of the halogenated phenol, the electron cloud density of the benzene ring is reduced, thereby inhibiting electrophilic attack of oxidase and making it difficult to realize aerobic degradation. The anaerobic biological method has the advantages of capability of recovering biological energy from organic waste, low biomass (excess sludge) yield, strong tolerance to high organic load and the like, so the waste water containing the halogenated phenol is generally treated by the anaerobic method. The traditional anaerobic method has the advantages of low cost, high benefit and environmental friendliness, but has the problems of long degradation period, poor stability, large demand of electron donors and the like.
At present, an anaerobic system is usually reinforced by using catalysts such as external light, electricity, heat and the like to solve the problem of low biodegradation efficiency. However, such techniques usually require additional continuous addition of catalysts and chemical reagents to maintain the stability of the biological system, and may cause secondary pollution of wastewater, thereby increasing the cost of wastewater treatment. Reports show that the addition of the magnetic field in an aerobic system can influence the microbial community structure, help to accelerate the removal of ammonia nitrogen in domestic wastewater, realize the standard discharge of domestic wastewater, accelerate the solid-liquid separation of sludge and facilitate the sludge sedimentation. Hu et al investigated the effect of static magnetic field on the performance of anoxic/aerobic sequencing batch reactors and found that magnetic field strength of 39.5mT increased the removal rate of total nitrogen in domestic wastewater (Hu B, Wang Y, Quan J, Huang K, Gu X, Zhu J T, Yan Y, Wu P, Yang L and ZHao J. effects of static magnetic field on the performance of aerobic/aerobic sequencing batch reactor [ J ]. Bioresource Technology,2020,309). However, magnetic fields may also have negative effects on organisms, and all others have explored the influence of static magnetic fields applied to biofilters on the removal of trichloroethylene, which is greatly suppressed when the magnetic field strength is 130mT (Quan Y, Wu H, Yin Z, Fan Y and Yin C. effect of static magnetic field on dechlorinated ethylene removal in a Bioresin filter [ J ]. Bioresour Technol,2017,239: 7-16).
Disclosure of Invention
The invention aims to provide a method for strengthening anaerobic biodegradation of halogenated phenol by using a static magnetic field, which utilizes the static magnetic field to promote Extracellular Polymers (EPS) of bacteria and improve the dehalogenase activity of the halogenated phenol so as to strengthen the degradation-resistant halogenated phenol pollutants in the industrial wastewater of anaerobic biological reduction.
The technical scheme for realizing the purpose of the invention is as follows:
the static magnetic field reinforced anaerobic biodegradation process of phenol halide includes the following steps:
and 3, adding the halogenated phenol wastewater into the static magnetic field-anaerobic biological system to degrade the halogenated phenol.
The halogenated phenol is a halogenated phenol pollutant commonly seen in industrial wastewater, and comprises but is not limited to compounds such as fluorine phenol, chlorophenol, bromophenol, iodophenol and the like.
Preferably, in step 1, the simulated wastewater has the following composition: 1.53g/L Na2HPO4·12H2O，0.38g/L NaH2PO4·2H2O，0.2g/L MgSO4·7H2O，0.4g/L NHCl4，0.05g/L CaCl2，1.0g/L CH3COONa and 1mL/L of trace element (SL-4).
Preferably, in the step 2, the concentration of the halogenated phenol in the simulated wastewater containing the halogenated phenol is 50-100 mg/L.
Preferably, in step 2, the acclimation time is 10 days or more.
Preferably, in step 2, the magnetic field strength is 21.25mT to 30.41 mT.
Preferably, in step 3, the halogenated phenol wastewater is added in a sequencing batch manner.
Preferably, in step 3, the degradation of the halogenated phenol is performed under shaking conditions, and the rotation speed is 180 r/min.
Preferably, in step 3, the operating temperature of the static magnetic field-anaerobic biological system is 35 ± 1 ℃.
Compared with the prior art, the invention has the following advantages:
(1) the invention utilizes the static magnetic field to strengthen the anaerobic biodegradation of the halogenated phenol, and gradually strengthens the degradation capability of the anaerobic organism to the halogenated phenol through magnetic stimulation under the action of the external magnetic field, does not need complex reaction requirements and conditions, can strengthen the degradation rate of the anaerobic organism to the halogenated phenol by only adding the static magnetic field, and improves the removal rate of the halogenated phenol in the waste water by 20 to 40 percent compared with the anaerobic control group under the optimal condition.
(2) The invention utilizes the magnetic field to treat the wastewater, is safe and convenient, does not introduce other harmful substances, and can be continuously used for decades because the permanent magnet has stable property, small change of magnetism along with time and extremely long service life, thereby reducing the treatment cost of the wastewater.
Drawings
FIG. 1 is a graph showing the effect of enhancing the degradation of 4-BP in an anaerobic biological system using different magnetic field strengths in example 1.
FIG. 2 is a graph showing the effect of static magnetic field on anaerobic biodegradation of 4-BP in example 2 at various salt concentrations.
FIG. 3 is a graph showing the effect of bromophenol dehalogenase and extracellular polymeric substance under static magnetic field conditions in example 3.
FIG. 4 is a graph showing the effect of 4-BP degradation by an anaerobic biological system under different carbon sources in comparative example 1.
Detailed Description
The invention is further described below with reference to examples and figures. The following examples are only for illustrating the performance of the present invention more clearly and are not limited to the following examples.
The target pollutant of the invention is halogenated phenol, such as compounds containing fluorine phenol, chlorophenol, bromophenol, iodophenol and the like, the p electron of the halogen atom and the pi electron on the benzene ring can form a very stable conjugated system, and the target pollutant is easy to combine with an enzyme system in an organism to generate long-term chronic toxic action on the organism.
In the following examples, the simulated wastewater composition was: 5-100 mg/L4-bromophenol (4-BP), 1.53g/L Na2HPO4·12H2O、0.38g/L NaH2PO4·2H2O、0.2g/L MgSO4·7H2O、0.4g/L NHCl4、0.05g/L CaCl2、1.0g/L CH3COONa and trace element (SL-4)1 mL/L. Wherein the trace elements (SL-4) consist of: 0.03g/L H3BO4、0.002g/L NiCl2·6H2O、0.001g/L CuCl2·2H2O、0.003g/L MnCl2·4H2O、0.02g/L CoCl2·6H2O、0.01g/L ZnSO4·7H2O、0.003g/L Na2MoO4·2H2O、0.2g/L FeSO4·7H2O、0.5g/L EDTA。
Example 1
(1) Sludge domestication: and (3) aerating nitrogen for 15min before simulating the use of the wastewater to exhaust residual oxygen in the wastewater to an anaerobic state. Adding initial simulation wastewater containing 4-BP with the concentration of 5mg/L into a 125mL anaerobic bottle, adding anaerobic sludge with the sludge concentration of 2.47g/L, and sealing the anaerobic bottle. After 4-BP in the simulated wastewater is completely degraded, gradually increasing the concentration of the 4-BP in the wastewater to 50mg/L, and after the water quality of the effluent is stable, completing sludge domestication.
(2) Constructing a static magnetic field-anaerobic biological system: adding the acclimated sludge into a magnetic field, respectively setting the magnetic field intensity to be 1.25mT, 11.65mT, 21.25mT, 30.41mT and 40.1mT, introducing simulated wastewater containing 4-BP with the concentration of 50mg/L, acclimating for 10d, and constructing a static magnetic field-anaerobic biological system.
(3) Degradation of 4-BP: adding simulated wastewater with the concentration of 4-BP being 50mg/L into a static magnetic field-anaerobic biological system constructed under different magnetic field strengths, placing the system in a constant temperature oscillator, controlling the rotating speed to be 180r/min and the temperature to be 35 ℃, and degrading the 4-BP. In the degradation period, at the set sampling time point, after a water sample is filtered by a 0.22 mu m filter membrane, the content of 4-BP is measured by a High Performance Liquid Chromatography (HPLC), and the wavelength of an ultraviolet detector is 225 nm.
Meanwhile, a single magnetic field biological-free system group which only applies a magnetic field and does not add anaerobic sludge and an anaerobic biological control system which only adds anaerobic sludge without applying a magnetic field are arranged.
As shown in FIG. 1, the concentration of 4-BP was stable in the single-field system without biology, and the change value was less than 5% after 6 hours of reaction, which indicates that the static magnetic field alone has no degradation capability for 4-BP. In the anaerobic control system and the static magnetic field-anaerobic biological system, 4-BP can be degraded gradually with the prolonging of the reaction time, the magnetic field intensity is 21.25mT after 5 hours of reaction, the residual rate of the 4-BP of the static magnetic field-anaerobic biological system is 3.49 +/-1.29 percent, and in the anaerobic biological control system, the residual rate is 38.04 +/-1.46 percent, and the removal rate is 34.55 +/-0.17 percent higher than that of a control group. In addition, the concentration of 4-BP in the static magnetic field-anaerobic organism system group is lower than that of an anaerobic organism control system in the reaction time, and the removal efficiency of 4-BP by different magnetic field strengths is shown as follows: 21.25mT >30.41mT >40.1mT >11.65mT >1.25mT >0 mT. The above results show that the applied magnetic field can significantly promote the degradation of 4-BP in anaerobic biological systems.
The principle of the invention is as follows: the magnetic field exposure can increase the activity of bromophenol dehalogenase in an anaerobic system, promote the debromination reduction degradation of 4-BP, simultaneously promote microorganisms to synthesize EPS, and benzene rings of the EPS can be combined with aromatic compounds to form pi-pi accumulation, thereby being beneficial to trapping 4-BP. Under the stress action of high-concentration 4-BP, the magnetic field can improve the electron mass transfer capacity of microorganisms, simultaneously sludge flocs are easier to gather, the biomass is increased by 18.18%, the stability of anaerobic sludge in a complex environment is improved, and the removal of the 4-BP by the microorganisms is further enhanced. The magnetic field exposure can also increase the content and activity of bromophenol dehalogenase in an anaerobic biological system, promote the debromination reduction degradation of 4-BP and enhance the removal efficiency of 4-BP in the anaerobic system.
Example 2
From the experimental data of example 1, an analysis experiment was conducted to examine the influence of the static magnetic field on anaerobic organisms under complicated water quality conditions by selecting an optimum magnetic field strength of 21.25mT and setting different salt concentrations (NaCl concentrations of 0, 15, 20 and 25g/L, respectively) in the same manner as in example 1.
As shown in FIG. 2, the removal rate of 4-BP by anaerobic organisms is gradually reduced along with the increase of salt concentration, and when the concentration of NaCl is 0g/L and the magnetic field strength is 0mT, the removal rate of 50mg/L of 4-BP can reach more than 60% within 5 h; when the salinity is increased to 20g/L, the removal rate of 4-BP with 50mg/L is only 37.05 +/-2.76%. In contrast, under the action of a static magnetic field of 21.25mT, when the concentration of NaCl is 0g/L, the removal rate of 4-BP by 50mg/L reaches more than 95.0 percent after 5 hours; the removal rate of 15g/L NaCl and 21.25mT static magnetic field-organism 4-BP in 72h is 66.44 +/-3.91 percent, which is 12.85 percent higher than the removal rate of 0mT 4-BP. Even if the NaCl concentration was increased to 25g/L, the removal rate of 4-BP was 48.4. + -. 1.35% at 72 hours after the addition of the static magnetic field of 21.25mT, which was significantly higher than the removal rate (37.91. + -. 0.219%) without the addition of the static magnetic field. In conclusion, under the condition of the same salt concentration, the removal rate of the activated sludge with the magnetic field intensity of 21.25mT applied to the 4-BP is higher than that of the corresponding treatment without the static magnetic field, and the difference between the removal rate of the static magnetic field to the 4-BP and the removal rate of the 0mT is gradually reduced along with the increase of the salt concentration. Therefore, the salt tolerance of the microorganisms is improved by the magnetic field strength of 21.25mT, and the long-term stability of an anaerobic biological system is promoted.
Example 3
According to the experimental data of the example 1, the experiment is analyzed, the optimal magnetic field intensity is selected to be 21.25mT, the long-term influence of the magnetic field on the microorganisms is studied under the same other conditions as the example 1, the continuous domestication degradation experiment is carried out for 20 days, and the influence of the static magnetic field on the secretion of the bromophenol dehalogenase and the EPS by the microorganisms is studied.
As shown in FIG. 3, the activity of bromophenol dehalogenase increased with increasing magnetic exposure time, which increased by 3.79% on the first day relative to no magnetic field exposure, and increased more slowly, with increasing magnetic exposure times of 5d, 10d and 20d, respectively, and with increasing magnetic exposure time, the activity of bromophenol dehalogenase increased 28.41%, 28.51% and 42.69%, respectively. With increasing magnetic exposure time, the EPS content also increased significantly, 205.86mg/MLVSS and 218.77mg/MLVSS at 5d and 20d, respectively, by 20% and 28% respectively, compared to no magnetic field exposure. EPS is a unique high molecular polymer, is produced by excretion, secretion, cell lysis and adsorption of microorganisms in sewage treatment plants or bacterial strains, generally consists of protein and polysaccharide, and the microorganisms protect themselves by secreting more EPS under severe environmental conditions. The extracted EPS can be obtained by scanning through a three-dimensional fluorescence instrument, in a static magnetic field-anaerobic biological system, an aromatic protein peak and a tyrosine peak are obviously enhanced, wherein the aromatic protein can protect microorganisms in a severe environment, and a benzene ring in the tyrosine can be combined with an aromatic compound to form pi-pi accumulation, so that the method is favorable for capturing the target pollutant halogenated phenol. Under the influence of a magnetic field, the contents of the bromophenol dehalogenase and the EPS are both increased remarkably. The magnetic field improves the bromophenol dehalogenase activity, promotes EPS secretion and accelerates the reductive degradation of 4-BP by anaerobic organisms, thereby achieving the purpose of strengthening the anaerobic biodegradation of 4-BP.
Comparative example 1
This comparative example is essentially the same as example 2, except that the effect of different carbon sources in the simulated wastewater on anaerobic biodegradation of 4-BP was investigated, and the salt concentration was 1% (NaCl concentration 10 g/L).
The results are shown in FIG. 4, where the reactor with sodium acetate as the carbon source of influent water removed 4-BP more efficiently than the other three groups, followed by sodium formate, sodium propionate and finally glucose, in the degradation of 4-BP by four different carbon sources (sodium formate, sodium acetate, sodium propionate and glucose). At 24h, the removal rate of the sodium acetate serving as a water inlet carbon source to the 4-BP reaches 64.01 +/-3.60 percent; the removal rate of the sodium formate serving as a water inlet carbon source to the 4-BP reaches 49.98 +/-3.81 percent. And sodium propionate and glucose are used as the carbon source of the influent water, and the removal rate of 4-BP is only 22.60 +/-2.53% and 28.52 +/-3.39%. At 36h, the removal rate of the sodium acetate serving as a water inlet carbon source to the 4-BP reaches 100%, is 41.39 +/-6.01% higher than that of a sodium propionate group and is 49.24 +/-3.57% higher than that of a glucose group. The experiment shows that sodium acetate is used as a water inlet carbon source to be beneficial to the removal of 4-BP by anaerobic organisms.
The above is only a preferred mode of the invention, and it should be noted that, for those skilled in the art, various changes and modifications can be made without departing from the inventive concept of the present invention, and these should also be considered as within the scope of the present invention.
Claims (9)
1. The method for anaerobic biodegradation of halogenated phenol by static magnetic field enhancement is characterized by comprising the following steps:
step 1, adding simulated wastewater with 5-10 mg/L of halogenated phenol into anaerobic sludge, gradually increasing the concentration of the halogenated phenol in the wastewater to 50-100 mg/L after the halogenated phenol in the simulated wastewater is completely degraded, and completing sludge domestication after the effluent quality is stable;
step 2, adding the acclimated sludge into a magnetic field, setting the magnetic field intensity to be 1.25 mT-40 mT, introducing simulated wastewater containing halogenated phenol, and acclimating to construct a static magnetic field-anaerobic biological system;
and 3, adding the halogenated phenol wastewater into the static magnetic field-anaerobic biological system to degrade the halogenated phenol.
2. The method of claim 1, wherein the halogenated phenol is a fluorophenol, chlorophenol, bromophenol, or iodophenol.
3. The method of claim 1, wherein in step 1, the simulated wastewater comprises: 1.53g/L Na2HPO4·12H2O，0.38g/L NaH2PO4·2H2O，0.2g/L MgSO4·7H2O，0.4g/L NHCl4，0.05g/L CaCl2，1.0g/L CH3COONa and 1mL/L of trace elements.
4. The method according to claim 1, wherein in the step 2, the concentration of the halogenated phenol in the simulated wastewater containing the halogenated phenol is 50-100 mg/L.
5. The method according to claim 1, wherein the acclimation time is 10 days or more in step 2.
6. The method according to claim 1, wherein in step 2, the magnetic field strength is 21.25mT to 30.41 mT.
7. The method as claimed in claim 1, wherein the halogenated phenol wastewater is added in a batch manner in step 3.
8. The method as claimed in claim 1, wherein in step 3, the degradation of the halogenated phenol is performed under shaking conditions at a rotation speed of 180 r/min.
9. The method as claimed in claim 1, wherein the static magnetic field-anaerobic biological system is operated at a temperature of 35 ± 1 ℃ in step 3.
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