CN110759437A - Method for electrochemical-UV composite treatment of refractory organic matters - Google Patents

Method for electrochemical-UV composite treatment of refractory organic matters Download PDF

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CN110759437A
CN110759437A CN201910967504.3A CN201910967504A CN110759437A CN 110759437 A CN110759437 A CN 110759437A CN 201910967504 A CN201910967504 A CN 201910967504A CN 110759437 A CN110759437 A CN 110759437A
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chlorine
electrochemical
electrode
anode electrode
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CN110759437B (en
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王玉珏
张银巧
展巨宏
余刚
黄�俊
邓述波
王斌
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Tsinghua Suzhou Institute Of Environmental Innovation
Tsinghua University
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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
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/467—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction
    • C02F1/4672—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation
    • C02F1/4674—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis by electrochemical disinfection; by electrooxydation or by electroreduction by electrooxydation with halogen or compound of halogens, e.g. chlorine, bromine
    • 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
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2201/00—Apparatus for treatment of water, waste water or sewage
    • C02F2201/32—Details relating to UV-irradiation devices
    • C02F2201/322—Lamp arrangement
    • C02F2201/3225—Lamps immersed in an open channel, containing the liquid to be treated

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  • Organic Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Hydrology & Water Resources (AREA)
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  • Environmental & Geological Engineering (AREA)
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Abstract

The invention discloses a method for electrochemical-UV composite treatment of refractory organic matters, which comprises the step of placing an electrode group comprising at least one pair of anode electrode and cathode electrode connected with a power supply into a degradation pool, wherein the anode electrode is a chlorine evolution electrode. A UV lamp was placed close to the anode electrode. Injecting organic polluted water containing PPCPs into a degradation pool, and adjusting the concentration of chloride ions to be not less than 30 mg/L. The power supply is connected, so that an electric field is formed between the anode electrode and the cathode electrode, the chlorine-containing water is subjected to electrochemical reaction, and chlorine ions in the chlorine-containing water lose electrons on the surface of the anode electrode to generate free chlorine; the irradiation of the UV lamp enables free chlorine to further generate strong oxidizing substances comprising hydroxyl radicals and active chlorine, and the organic pollutants which are difficult to degrade in the chlorine-containing water are oxidized and degraded. The method is cooperated with electrochemical oxidation and UV, realizes high-efficiency removal of refractory organic pollutants by using chlorine contained in water, and has the advantages of simple method, good removal effect and the like.

Description

Method for electrochemical-UV composite treatment of refractory organic matters
Technical Field
The invention relates to a method for electrochemical-UV composite treatment of refractory organic matters, belonging to the technical field of water treatment.
Background
The refractory organic matter includes polycyclic aromatic hydrocarbon, halohydrocarbon, heterocyclic compound, organic cyanide, organic phosphorus pesticide, surfactant, organic dye, etc. The treatment research is always a hotspot and a difficulty of the water pollution prevention and treatment research.
With the rapid development of economy and the improvement of living standards of people, PPCPs (pharmaceutical and personal care products, PPCPs for short) are a new class of organic pollutants, which are receiving increasing attention as a class of novel organic pollutants, and the number of PPCPs is continuously increasing, the number of PPCPs which can be detected at present is as many as 101, including sulfonamides (19), fluoroquinolones (14), β -lactams (11), macrolides (7), tetracyclines (7), bactericides (6), antipyretic and analgesic drugs (5) and other antibiotic drugs (32), and the organic pollutants have potential threats to ecological systems and human health, most of which have difficult degradability and are difficult to remove by adopting a traditional or single water treatment process, such as a biological method or a single ozone, chlorine and Ultraviolet (UV) method.
Comparison of UV/H2O2UV/chlorine is an emerging advanced oxidation technology, and has shown good removal effect in the aspect of removing the refractory organic pollutants. With UV/H2O2Compared with UV/chlorine, and HClO is more economical than H2O2The quantum absorption for UV is higher. The main reaction mechanism of the UV/chlorine process is shown in equations (1) to (6). Not only can non-selective HO be generated in the UV/chlorine process*Optionally, Cl can also be generated*、Cl2 *—And ClO*。HO*Is a strong oxidant, oxidation-reduction potential E02.8V, it is easily treated by natural organic substances, HCO, in actual water treatment3 -/CO3 -And (4) equal-matrix capture. Except for HO*，Cl*、Cl2 *—And ClO*The oxidant is also a high-efficiency oxidant, and the oxidation-reduction potentials of the oxidant are 2.4V, 2.0V and 1.5-1.8V respectively. There are many reports in the literature that the UV/chlorine process can achieve efficient removal of micro-contaminants in the class of pharmaceuticals and personal care products. Thus, UV/chlorine is an effective technique for the removal of pollutants in practical bodies of water.
Figure BDA0002230986190000011
Figure BDA0002230986190000012
HO*+HOCl→ClO*+H2O (3)
HO*+OCl—→ClO*+OH—(4)
Cl*+HOCl→ClO*+H++Cl—(5)
Cl*+OCl—→ClO*+Cl—(6)
Although UV/chlorine is considered a new and viable advanced oxidation technology, its application is somewhat limited. As in decentralized water treatment systems, NaClO and HClO are corrosive and HClO is extremely unstable, storage and transport of chlorine limits the application and spread of UV/chlorine for contaminant removal.
Disclosure of Invention
The invention aims to provideThe method for electrochemical-UV composite treatment of refractory organic matters fully utilizes the characteristic that chloride ions usually exist in water, generates an electric field by an electrode, and generates the chloride ions in the chlorine-containing water to form HClO and ClO on the surface of a chlorine-separating anode electrode-And Cl2And further reacting the free chlorine under the action of UV light to produce HO*And active chlorine (including Cl)*、Cl2 *—And ClO*) Thereby efficiently removing the organic pollutants in the water body.
The invention is realized by the following technical scheme:
the electrochemical-UV composite treatment method of refractory organic matter includes,
placing an electrode group comprising at least one pair of anode electrode and cathode electrode into a degradation pool, wherein the anode electrode and the cathode electrode are respectively connected with a power supply; the anode electrode is a chlorine evolution electrode;
disposing a UV lamp between and proximate to the anode electrode and the cathode electrode;
injecting organic polluted water containing refractory organics into a degradation pool, and adjusting the concentration of chloride ions in the organic polluted water to be not less than 30 mg/L;
connecting a power supply to form an electric field between the anode electrode and the cathode electrode, so that the chlorine-containing water is subjected to electrochemical reaction, and chlorine ions in the chlorine-containing water lose electrons on the surface of the anode electrode to generate HClO and ClO-And Cl2Free chlorine of (a); the UV light emitted by the UV lamp irradiates to enable free chlorine to further generate strong oxidizing substances including hydroxyl radicals and active chlorine, and the refractory organic pollutants in the chlorine-containing water are oxidized and degraded. The active chlorine includes Cl*、Cl2 *—And ClO*。
In the technical scheme, the organic polluted water is adjusted in chloride ion concentration by adding chloride salt, wherein the chloride salt is any one or a mixture of sodium chloride, magnesium chloride and potassium chloride.
In the technical scheme, the refractory organic matters comprise PPCPs, pesticide residues or industrial chemicals; the industrial chemicals include organic solvents, dyes or phenols.
In the above technical scheme, the anode electrode and the cathode electrode are both rod-shaped or sheet-shaped electrodes.
In the above technical scheme, the current density I of the anode electrode and the cathode electrode is 0<I≤500mA/cm2。
In the technical scheme, the UV lamp is arranged in the degradation pool and is immersed in the organic polluted water.
Among the above-mentioned technical scheme, the UV lamp is close to the degradation pond wall and sets up outside the degradation pond, and is provided with a degradation pond side wall of UV lamp and chooses for use the material that can see through the UV light.
In the technical scheme, the UV lamp is arranged above the degradation pool along the liquid level of the degradation pool.
In the technical scheme, the retention time of the chlorine-containing water in the degradation tank is 0.5-180 min.
The invention has the following advantages and beneficial effects: under the action of the cooperation of electrochemical oxidation and UV, pollutants which are difficult to degrade can be efficiently and quickly removed; the treatment method is simple and easy to implement, a large amount of free chlorine reagents such as chlorine, hypochlorous acid and hypochlorite are not required to be stored and consumed, and the cost is saved.
Drawings
FIG. 1 is a schematic view of an electrochemical-UV device according to one embodiment of the present invention.
Fig. 2 is a schematic view of an electrochemical-UV device according to another embodiment of the present invention.
FIG. 3 is a graph showing the removal effect of metoprolol drug by different processes, wherein □ represents Electrolysis only (Electrolysis), ● represents UV irradiation only (UV), and ▲ represents electrochemical-UV/Chlorine (E-UV/Chlorine).
In the figure: 1-a power supply; 2-a cathode electrode; 3-an anode electrode; 4-UV lamp; and 5, a degradation tank.
Detailed Description
The following describes the embodiments and operation of the present invention with reference to the accompanying drawings.
The terms of orientation such as up, down, left, and right in the present specification are established based on the positional relationship shown in the drawings. The corresponding positional relationship may also vary depending on the drawings, and therefore, should not be construed as limiting the scope of protection.
As shown in fig. 1, an electrode group including at least one pair of an anode electrode 3 and a cathode electrode 2 is placed in a degradation tank 5, and the anode electrode 3 and the cathode electrode 2 are respectively connected to a power source 1. According to the requirement, the electrode group can be provided with a plurality of pairs of anode electrodes and cathode electrodes, and each pair of anode electrodes and cathode electrodes are connected with a power supply in a one-to-one correspondence mode. The lower part of the degradation tank 5 is provided with a water inlet, and the upper part is provided with a water outlet, so that water to be treated can enter and exit the degradation tank.
The anode electrode 3 is a chlorine-separating electrode, and comprises a titanium ruthenium-plated electrode, a titanium iridium-plated electrode and a titanium ruthenium iridium-plated electrode. The cathode electrode 2 is a metal electrode, including platinum, stainless steel or titanium electrode, or a carbon electrode, including graphite, carbon black, carbon nanotube electrode, etc. The anode electrode 3 and the cathode electrode 2 can be rod-shaped or sheet-shaped electrodes.
The UV lamp 4 is disposed near the anode electrode 3, and various types of mercury lamps or UV-LED lamps can be used as the UV lamp. In one embodiment, as shown in fig. 1, a UV lamp 4 is vertically inserted into the degradation tank 5 and disposed near the anode electrode 3. Another kind of embodiment is, the vertical 5 wall settings in degradation pond that are close to of UV lamp 4 are outside degradation pond 5, and are provided with 5 lateral wall of degradation pond of UV lamp 4 and select for use the material that can see through the UV light. In another embodiment, as shown in fig. 2, the UV lamp 4 is disposed above the degradation tank 5 against the liquid surface of the degradation tank 5.
Because the organic polluted water of the refractory organic matters often contains chloride ions, the method of the invention fully utilizes the chloride ions.
Injecting organic polluted water containing refractory organics into a degradation pool.
And measuring the concentration of the chloride ions in the organic polluted water by using an instrument such as a chloride ion concentration meter, and when the concentration of the chloride ions in the organic polluted water is lower than 30mg/L, adjusting the concentration of the chloride ions in the organic polluted water to be not lower than 30mg/L by adding chloride salt. The chloride salt is selected from one or more of sodium chloride, magnesium chloride and potassium chloride. The refractory organic substances comprise PPCPs, pesticide residues, industrial chemicals and the like, and the industrial chemicals comprise organic solvents, dyes, phenols and the like.
The power supply is connected, because the rate of electrochemically generating active chlorine and the current density are in a certain direct proportion relationship, the current is required to be adjusted to control the generation rate of the active chlorine according to the water amount, the required active chlorine amount and the like, so that the current density I of the anode electrode and the cathode electrode is 0<I≤500mA/cm2At this time, an electric field is formed between the anode and the cathode to cause the chlorine-containing water to electrochemically react, and chlorine ions in the chlorine-containing water lose electrons on the surface of the anode to generate HClO and ClO-And Cl2Free chlorine of (a). In this process, part of the water is also ionized to generate hydroxyl radicals. Meanwhile, the UV light emitted by the UV lamp irradiates to enable free chlorine to further generate strong oxidizing substances including hydroxyl radicals and active chlorine, and the organic pollutants which are difficult to degrade in the chlorine-containing water are oxidized and degraded. The active chlorine includes Cl*、Cl2 *—And ClO*。
The retention time of the chlorine-containing water in the degradation tank is 0.5-180 minutes (min). The treated water is discharged from the water outlet.
The following examples further illustrate the performance of the process of the present invention. In the examples, the water samples to be treated are the same surface water, the pH value is 7.6, the conductivity is 296 mu S/cm, and the water sample is 700mL, wherein 100 mu g/L metoprolol (metoprolol), Cl is dissolved in the water sample-The concentration is 5.5-300 mg/L, Cl-The concentration was adjusted by adding different amounts of NaCl. Metoproll is a drug that is slowly removed by both UV irradiation and HClO oxidation.
Example 1
The initial chloride ion concentration in the water sample to be treated is 100 mg/L. Adding a water sample to be treated into a cylindrical reactor, vertically and parallelly inserting a DSA anode and a stainless steel cathode into the reactor to immerse the DSA anode and the stainless steel cathode in water, correspondingly connecting the electrodes with a direct current power supply, and simultaneously inserting a UV lamp for irradiation. The distance between the two electrodes is 1cm, and the distance between the UV lamp and the anode is 1 cm. Meanwhile, the reactor is placed on a magnetic stirrer, so that the treated water sample is uniformly mixed.
The DSA anode is a titanium ruthenium-iridium plated electrode with the size of 4cm multiplied by 12 cm; the size of the cathode stainless steel electrode is 4cm multiplied by 12 cm; under the electrification of a direct current power supply, the current at two ends of the cathode and the anode is 200mA, namely the current density is 4.2mA/cm2. The UV lamp is a 10W low-pressure mercury lamp.
The treatment time is about 3min, and the removal rate of metoprolol can reach 90%.
Example 2
In this embodiment, the magnitude of the cathode and anode currents in embodiment 1 is replaced by 400mA, i.e. the current density is 8.3mA/cm2。
The treatment time is about 2min, and the removal rate of metoprolol can reach 90%.
Example 3
In this example, the magnitude of the cathode and anode currents in example 1 was changed to 800mA, i.e., the current density was 16.7mA/cm2。
The treatment time is about 1.7min, and the removal rate of metoprolol can reach 90%.
Example 4
This example replaces the chloride ion concentration in example 2 with 30 mg/L.
The treatment time is about 2min, and the removal rate of metoprolol can reach 90%.
Example 5
This example replaces the chloride ion concentration of example 2 with 300 mg/L.
The treatment time is about 0.8min, and the removal rate of metoprolol can reach 90%.
As can be seen from the above examples, the electrochemical-UV/Chlorine (E-UV/Chlorine) method of the present invention has a significant treatment effect. FIG. 2 further shows a comparison of the treatment effects of several methods, and it is also concluded that the electrochemical-UV/Chlorine (E-UV/Chlorine) method of the present invention has a significantly better treatment effect than Electrolysis (Electrolysis) or UV irradiation (UV).
The electrochemical-UV composite treatment method is not only limited to the treatment of PPCPs, but also is suitable for treating various industrial chemical wastewater, pesticide residue, medical wastewater and the like which are difficult to degrade.
The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention, and various modifications and changes may be made by those skilled in the art. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims (9)

1. The method for electrochemical-UV composite treatment of refractory organics is characterized by comprising the following steps:
placing an electrode group comprising at least one pair of anode electrode and cathode electrode into a degradation pool, wherein the anode electrode and the cathode electrode are respectively connected with a power supply; the anode electrode is a chlorine evolution electrode;
disposing a UV lamp between and proximate to the anode electrode and the cathode electrode;
injecting organic polluted water containing refractory organics into a degradation pool, and adjusting the concentration of chloride ions in the organic polluted water to be not less than 30 mg/L;
connecting a power supply, so that an electric field is formed between the anode electrode and the cathode electrode, the chlorine-containing water is subjected to electrochemical reaction, and chlorine ions in the chlorine-containing water lose electrons on the surface of the anode electrode to generate free chlorine; the UV light emitted by the UV lamp irradiates to enable free chlorine to further generate strong oxidizing substances including hydroxyl radicals and active chlorine, and the refractory organic pollutants in the chlorine-containing water are oxidized and degraded.
2. The method for electrochemical-UV composite treatment of refractory organics as claimed in claim 1, wherein the organic contaminated water is adjusted in chloride ion concentration by adding chloride salt, wherein the chloride salt is selected from any one or more of sodium chloride, magnesium chloride and potassium chloride.
3. The electrochemical-UV composite treatment method for refractory organics according to claim 1, characterized in that the refractory organics comprises PPCPs, pesticide residues or industrial chemicals; the industrial chemicals include organic solvents, dyes or phenols.
4. The method for electrochemical-UV combined treatment of refractory organics as claimed in claim 1, wherein the anode electrode and the cathode electrode are rod-shaped or sheet-shaped electrodes.
5. The electrochemical-UV combined treatment method for refractory organics as claimed in claim 1 or 2, wherein the current density I of the anode electrode and cathode electrode is 0<I≤500mA/cm2。
6. The electrochemical-UV composite treatment method for refractory organics according to claim 1, characterized in that the UV lamp is arranged in a degradation tank and is immersed in the organic polluted water.
7. The method for electrochemical-UV combined treatment of refractory organics as claimed in claim 1, wherein the UV lamp is disposed outside the degradation tank near the wall of the degradation tank, and the wall of the degradation tank on which the UV lamp is disposed is made of a material that can transmit UV light.
8. The method for electrochemical-UV composite treatment of refractory organics according to claim 1, wherein the UV lamp is arranged above the degradation tank along the liquid level of the degradation tank.
9. The method for electrochemical-UV composite treatment of refractory organics as claimed in claim 1, wherein the retention time of the chlorine-containing water in the degradation tank is 0.5-180 min.
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CN111646539A (en) * 2020-06-04 2020-09-11 浙江大学 UVC-LED-DSA electrode coupled photoelectrochemistry oxidized ammonia nitrogen synergistic removal system
CN111977865A (en) * 2020-06-30 2020-11-24 中山大学 Ballast water treatment device for removing electrolytic coupling LED photocatalysis series-connection halogenated matters
CN111620493A (en) * 2020-07-03 2020-09-04 中国农业科学院农业环境与可持续发展研究所 Method and special equipment for removing antibiotic resistant bacteria and resistant genes in sewage
CN112429801A (en) * 2020-09-30 2021-03-02 南昌航空大学 Method for treating high-concentration organic wastewater by ultraviolet light in cooperation with electrochemical oxidation
CN112340905A (en) * 2020-10-28 2021-02-09 清华苏州环境创新研究院 Method and device for multi-wavelength ultraviolet-electrochemical sectional treatment of wastewater
CN112340905B (en) * 2020-10-28 2023-08-11 苏州清初环境科技有限公司 Method and device for multi-wavelength ultraviolet-electrochemical sectional treatment of wastewater
CN113023972A (en) * 2021-03-12 2021-06-25 南通寰宇博新化工环保科技有限公司 High-salt organic wastewater treatment method based on electrochemical coupling hydrogen peroxide
CN113060879A (en) * 2021-03-30 2021-07-02 上海应用技术大学 Method for removing fluoroquinolone antibiotics in water based on ultraviolet/chlorine dioxide

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