CN114590873A - Three-dimensional electro-catalysis device and method for synchronously removing organic pollutants and total nitrogen - Google Patents
Three-dimensional electro-catalysis device and method for synchronously removing organic pollutants and total nitrogen Download PDFInfo
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- CN114590873A CN114590873A CN202210263220.8A CN202210263220A CN114590873A CN 114590873 A CN114590873 A CN 114590873A CN 202210263220 A CN202210263220 A CN 202210263220A CN 114590873 A CN114590873 A CN 114590873A
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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
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- 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
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46109—Electrodes
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- 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
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46109—Electrodes
- C02F2001/46133—Electrodes characterised by the material
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- 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
- C02F1/46104—Devices therefor; Their operating or servicing
- C02F1/46109—Electrodes
- C02F2001/46133—Electrodes characterised by the material
- C02F2001/46138—Electrodes comprising a substrate and a coating
- C02F2001/46142—Catalytic coating
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- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
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- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
- C02F2101/163—Nitrates
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- C02F2101/30—Organic compounds
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- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2201/00—Apparatus for treatment of water, waste water or sewage
- C02F2201/46—Apparatus for electrochemical processes
- C02F2201/461—Electrolysis apparatus
- C02F2201/46105—Details relating to the electrolytic devices
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- C02F2201/46—Apparatus for electrochemical processes
- C02F2201/461—Electrolysis apparatus
- C02F2201/46105—Details relating to the electrolytic devices
- C02F2201/4612—Controlling or monitoring
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- C02F2201/00—Apparatus for treatment of water, waste water or sewage
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- C02F2201/461—Electrolysis apparatus
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- C02F2209/06—Controlling or monitoring parameters in water treatment pH
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- C02F2209/08—Chemical Oxygen Demand [COD]; Biological Oxygen Demand [BOD]
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Abstract
The invention relates to a three-dimensional electro-catalysis device and a three-dimensional electro-catalysis method for removing organic pollutants, nitrate nitrogen and ammonia nitrogen. Treating the wastewater by using a three-dimensional electrode catalytic system; the three-dimensional electrode catalytic system comprises the following components: the titanium metal is used as an anode, a coating is arranged on the surface of the anode plate, the coating is made of Gd-doped titanium-based tin dioxide and is used as the anode, the titanium metal is used as a cathode, a particle electrode is arranged between the cathode and the anode, and the particle electrode is bentonite loaded with nano zero-valent iron, wherein the bentonite is doped with copper and manganese metal elements. The method improves the treatment effect of organic wastewater, especially sewage containing refractory organic matters and nitrate nitrogen, on the basis of not adding medicaments.
Description
Technical Field
The invention belongs to the technical field of electrochemistry and sewage treatment, and particularly relates to a three-dimensional electro-catalysis device and method for removing organic pollutants, nitrate nitrogen and ammonia nitrogen.
Background
The information in this background section is only for enhancement of understanding of the general background of the invention and is not necessarily to be construed as an admission or any form of suggestion that this information forms the prior art that is already known to a person of ordinary skill in the art.
The three-dimensional electrocatalysis technology is to fill particle materials between the traditional two-dimensional electrodes, the electrode materials are the core of the three-dimensional electrocatalysis oxidation method, so that the three-dimensional electrocatalysis device has electrocatalysis characteristics, and in the using process, strong oxidizing substances (such as hydroxyl free radicals) are generated to treat organic wastewater and nitrate nitrogen, thereby realizing the rapid degradation of pollutants. The inventor finds that the existing three-dimensional electrode assembly has poor removal effects on organic matters and nitrate nitrogen in organic wastewater and simultaneously removes the organic matters and the nitrate nitrogen.
Disclosure of Invention
Aiming at the problems in the prior art, the invention aims to provide a three-dimensional electrocatalysis device and a method for removing organic pollutants, nitrate nitrogen and ammonia nitrogen.
In order to solve the technical problems, the technical scheme of the invention is as follows:
in a first aspect, a three-dimensional electrocatalysis method for removing organic pollutants, nitrate nitrogen and ammonia nitrogen comprises the following steps: treating the wastewater by using a three-dimensional electrode catalytic system;
the three-dimensional electrode catalytic system comprises the following components: the metal titanium is used as an anode, a coating is arranged on the surface of the anode plate, the coating is made of Gd-doped titanium-based tin dioxide and is used as an anode, the metal titanium is used as a cathode, a particle electrode is arranged between the cathode and the anode, and the particle electrode is formed by loading nanometer zero-valent iron on bentonite doped with copper and manganese metal elements.
Aiming at the problem that the waste water contains organic matters which are difficult to degrade and simultaneously contains a certain amount of nitrate nitrogen. The invention provides a three-dimensional electrode catalytic system, wherein a coating material on an anode is Gd-doped titanium-based tin dioxide, and the Gd-doped titanium-based tin dioxide has higher oxygen release overpotential under the coordination of voltage and current, so that the Gd-doped titanium-based tin dioxide has the capability of generating substances with strong oxidizing property (such as hydroxyl free radicals) and improving the capability of removing organic matters. The particle electrode is matched with the anode to treat nitrate nitrogen, organic nitrogen is firstly degraded into ammonia nitrogen at the anode and then is oxidized into nitrate nitrogen, and the filled particle electrode can adsorb the nitrate nitrogen on the surface of the particle electrode and further catalytically reduce the nitrate nitrogen into nitrogen. Under the action of the formed three-dimensional electrode, the particle electrode is helped to better catalyze and reduce nitrate nitrogen into nitrogen.
The cooperation of the particle electrodes and the anode, under the action of a three-dimensional electrode system, each particle electrode is polarized and charged under the action of an electric field, a single particle electrode forms a tiny battery, and the surface of the particle electrode has higher oxidation-reduction potential and can promote the generation of strong radicals, such as hydroxyl radicals, in a solution system. Pollutants in the wastewater are enriched in the particle electrode between the anode and the cathode, hydroxyl radicals generated by the anode enter the particle electrode, and the particle electrode promotes the generation of the hydroxyl radicals in a solution system, so that the effect of partially treating the pollutants in the wastewater by the particle electrode is better; when the reactor works, the filling particles greatly increase the specific surface of the reaction and improve the mass transfer rate. The treatment effect of organic wastewater, especially sewage containing refractory organic matters is improved on the basis of no addition of medicament.
In some embodiments of the invention, the Gd-doped titanium-based tin dioxide is prepared by: soaking a titanium substrate in an immersion liquid, wherein the immersion liquid consists of SnCl4、SbCl3、Gd(NO3)3Water, hydrochloric acid, ethanol, propanol and isopropanol, drying the titanium matrix after impregnation, then carrying out heat treatment at 350 ℃, and then carrying out heat treatment at 700 ℃ to obtain Gd-doped titanium-based tin dioxide. Further, Sn: sb: gd is 100:6:2 (molar mass ratio); further, the heat treatment time is 25-35min at 350 ℃ and 2-4h at 700 ℃.
In some embodiments of the invention, the particle electrode is prepared by: mixing an iron trichloride aqueous solution, a manganese chloride tetrahydrate aqueous solution and a copper chloride dihydrate aqueous solution, then adding bentonite, lignin and sodium borohydride, then adding acrylamide and N ', N' -methylene-bisacrylamide, and finally adding potassium persulfate and N ', N' -tetramethyl-ethylenediamine, and reacting to obtain the particle electrode. Further, the proportion of ferric trichloride, bentonite, lignin, sodium borohydride, acrylamide, N ' -methylene-bisacrylamide, potassium persulfate and N ', N ' -tetramethyl-ethylenediamine is 9.66g to 1.5g to 2g to 3.54g to 5g to 0.2g to 0.5g to 100 mu L; further, the molar ratio of iron to copper was 1:0.35, and the molar ratio of iron to manganese was 1: 0.16. Further, the particle diameter of the particle electrode is 3-5 mm. The particle size of the particle electrode is small, the particle electrode is uniformly distributed between the anode plate and the cathode plate, the bypass current and the short-circuit current are reduced, and the mass transfer capacity and the unit effective reaction area of the reactor are effectively improved.
In some embodiments of the invention, the operating current is 1.5 to 2.5A during wastewater treatment. The operating current contributes to the material of the three-dimensional electrode system to exert better redox capacity.
In some embodiments of the invention, air is introduced into the three-dimensional electrode catalytic system during wastewater treatment. Oxygen is introduced to facilitate H generation on the cathode surface2O2The generation of hydroxyl free radicals is increased, the treatment effect of the organic wastewater is better, and the catalytic oxidation reaction capability of the organic wastewater is further improved.
In a second aspect, a three-dimensional electro-catalytic device for removing organic pollutants, nitrate nitrogen and ammonia nitrogen comprises: the device comprises a supporting layer, and an anode plate, a cathode plate, a particle electrode and an aeration device which are arranged above the supporting layer, wherein the particle electrode is positioned between the anode plate and the cathode plate, the anode plate is made of a titanium matrix, a coating is arranged on the surface of the titanium matrix, the aeration device is arranged below the supporting layer, and the supporting layer is provided with air holes.
The aeration device is matched with the anode plate, the cathode plate and the particle electrode, so that the generation of hydroxyl radicals is facilitated, and the wastewater treatment effect is improved.
In some embodiments of the present invention, the anode plate and the cathode plate are provided in a plurality, and the anode plate and the cathode plate are arranged at intervals. Further, a plurality of anode plates and cathode plates are vertically arranged. Furthermore, the distance between the anode plate and the cathode plate is 10-20 cm. The distance between the anode plate and the cathode plate is beneficial to the movement of internal ions and the oxidation-reduction process.
In some embodiments of the invention, the water inlet is located below the anode plate side of the edge portion, and the water outlet is located at an upper portion of the side opposite to the water inlet. The shell is made of stainless steel or carbon steel, and is lined with epoxy coal tar pitch anticorrosive paint.
In some embodiments of the present invention, the water outlet further comprises an electromagnetic region, the electromagnetic region is connected to the water outlet, and an electromagnetic device is disposed inside the electromagnetic region. Furthermore, a water outlet is arranged at the upper part of the electromagnetic area. When the waste water flows into the electromagnetic area, partial particle electrodes are arranged, and in order to prevent the particle electrodes from flowing out of the water outlet, an electromagnetic device is arranged below the electromagnetic area and used for adsorbing the particle electrodes to achieve the purpose of precipitation. When the electromagnetic device adsorbs the particle electrodes to reach a certain amount, the electromagnetic device is closed, and the particle electrodes deposited at the bottom are refluxed to the water outlet.
In some embodiments of the invention, a dc power source is further included and is connected to the anode plate and the cathode plate.
In some embodiments of the present invention, the aeration device comprises an aeration pipeline, an aeration head and a blower, wherein the aeration pipeline is connected with the aeration head, and the blower is connected with the aeration pipeline. The aeration pipeline is supported by an aeration pipeline support, the cathode plate and the anode plate are supported by a polar plate support, and the aeration pipeline support and the polar plate support are fixed on the inner wall of the shell. The purposes of full mixing and COD reduction are achieved through continuous aeration and oxidation.
The filled particle electrode material and the cathode and anode electrodes form a three-dimensional electrode. Under the action of an external electric field formed by the main electrode, the particle electrodes are polarized through electrostatic induction, one end of each particle electrode becomes an anode, the other end of each particle electrode becomes a cathode, a micro electrolytic tank is formed between every two adjacent particle electrodes, electrochemical reaction simultaneously occurs on each particle electrode, the addition of the particle electrodes effectively utilizes the electrolytic space, shortens the distance between the two electrodes, reduces the migration path of the reaction and plays a role in strengthening the electric field. The method effectively breaks through the limitations of small treatment capacity, low current efficiency, high energy consumption and the like of the traditional two-dimensional electrocatalysis. Compared with a two-dimensional electrochemical process, the three-dimensional electrochemical process has higher specific surface area and shorter mass transfer distance, so that the three-dimensional electrochemical process has better effect in wastewater treatment.
In the three-dimensional electrode system, the main reaction mechanism comprises direct oxidation and indirect oxidation, and H is generated through electrochemical reaction2O2、O3And the indirect oxidation of strong oxidation species such as OH and the like is in a leading position, and the addition of the particle electrode prepared by the method increases the surface area of the electrode for generating electrochemical reaction, so that the electrochemical reaction extends to the three-dimensional space of the whole electrolytic cell from the two-dimensional plane of the main electrode. The cathode has a very high O in the bulk system2Electrochemical reduction activity, O under the catalytic action of the particle electrode2Can generate a large amount of H2O2. Thus, the addition of a particle electrode to an electrolytic cell allows for the in situ generation of the Fenton reagent (H)2O2) Extends from the electrode plane into the reactor space to form a three-dimensional electro-Fenton system, and electrochemically reduces O due to the increase of the specific surface of the electrode2Correspondingly increases the number of active sites, thereby promoting the electrochemical generation of H2O2The reaction is carried out H2O2The generation rate and the generation amount of (2) are both greatly improved, and H is generated in large quantity2O2The surface of the particle electrode is catalyzed to generate free radicals with stronger oxidation capacity, so that the oxidation capacity of the three-dimensional electrode system is improved, and the treatment efficiency of the whole reaction system is finally improved.
The granular electrode which takes bentonite as a substrate and is loaded with various catalytic metals is added between the two polar plates, the material can prevent the generation of short-circuit current, has the advantages of good corrosion resistance, conductivity, electrocatalysis and the like, can keep a stable state in a wider pH range, and can ensure that liquid in a reactor smoothly passes through. The particle electrode can adsorb organic pollutants in water to the surface of the particle electrode, a high-concentration area is formed locally, the mass transfer of the pollutants is greatly enhanced, the electrocatalysis efficiency is improved, and the electric energy utilization rate is obviously improved.
One or more technical schemes of the invention have the following beneficial effects:
the invention provides a three-dimensional electro-catalysis method and a three-dimensional electro-catalysis device for removing organic pollutants, nitrate nitrogen and ammonia nitrogen, wherein a three-dimensional electrode catalysis system is used for treating wastewater; in the three-dimensional electrode catalytic system: the anode plate body or the body is doped with Ga metal and is provided with the oxide coating, so that the catalytic performance is improved, the addition of iron salt and hydrogen peroxide is reduced, and during operation, nitrogen-containing organic wastewater can be directly introduced into the three-dimensional electrocatalysis device for synchronizing organic pollutants and total nitrogen, so that the operation is simple and convenient, and the generation of iron mud is reduced. The transition metal oxide layer is positioned on the surface of the anode plate, and compared with the transition metal oxide layer in the solution, the COD and the BOD of the treated organic wastewater5The content is lower, the oxygen evolution potential is improved by visible transition metal, and the catalytic oxidation performance is improved.
The particle electrode in the three-dimensional electrode system is matched with the anode to treat nitrate nitrogen and refractory organic matters, so that the effect of treating organic wastewater, especially sewage containing refractory organic matters and nitrate nitrogen, is improved on the basis of no addition of medicament.
Drawings
The accompanying drawings, which are incorporated in and constitute a part of this specification, are included to provide a further understanding of the invention, and are incorporated in and constitute a part of this specification, illustrate embodiments of the invention and together with the description, serve to explain the invention and not to limit the invention.
FIG. 1 is a schematic diagram of the overall structure of a three-dimensional electrocatalysis device for removing organic pollutants, nitrate nitrogen and ammonia nitrogen;
FIG. 2 is a schematic view of a top view of a three-dimensional electrocatalytic device for removing organic pollutants, nitrate nitrogen and ammonia nitrogen;
the device comprises a water inlet, a water outlet, a particle electrode, a water outlet, a water inlet, a water outlet, a water inlet, a water outlet, a water inlet, a water outlet, a direct current power supply, a water outlet, a water inlet, a water outlet and a water outlet, a water outlet and a water outlet, a water outlet and a water outlet, a water outlet.
Detailed Description
It is to be understood that the following detailed description is exemplary and is intended to provide further explanation of the invention as claimed. Unless defined otherwise, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention belongs.
It is noted that the terminology used herein is for the purpose of describing particular embodiments only and is not intended to be limiting of example embodiments according to the present application. As used herein, the singular forms "a", "an" and "the" are intended to include the plural forms as well, and it should be understood that when the terms "comprises" and/or "comprising" are used in this specification, they specify the presence of stated features, steps, operations, devices, components, and/or combinations thereof, unless the context clearly indicates otherwise.
Preparing anode by using Gd-doped titanium-based tin dioxide (Ti/Gd-SnO)2) Comprises the processing of a Ti matrix and the preparation of a surface layer. The Ti matrix treatment comprises grinding, alkali washing and acid washing etching, the Ti matrix is firstly ground by using 60-mesh coarse abrasive paper, then ground by using 300-mesh fine abrasive paper to remove surface oxides, then soaked by using 30% NaOH solution to remove organic matters such as oils and the like, soaked in water bath at 80 ℃ for 2.0h, ultrasonically washed by using distilled water, finally etched by using 10% oxalic acid solution, soaked in water bath at 98 ℃ for 2.0h, ultrasonically washed by using distilled water for standby, and stored in absolute ethyl alcohol for standby application, the treated titanium matrix loses metallic luster, and the surface is in a rough surface state. The impregnating solution is composed of SnCl4、SbCl3、Gd(NO3)3Water, hydrochloric acid, ethanol, propanol and isopropanol, Sn: sb: gd is 100:6:2 (molar mass ratio), the treated Ti matrix is completely immersed in the immersion liquid, the Ti matrix is taken out and dried in a constant-temperature drying box at 80 ℃, the operation is repeated for 5 times, then the heat treatment is carried out at 350 ℃ for 30min, the operation is repeated for 5 times, and the electrode is subjected to the heat treatment at 700 ℃ for 3.0h to prepare the Ti/Gd-SnO2And an anode.
Preparation of particle electrode ferric chloride was dissolved in deionized water and the solution was transferred to a three-necked flask. A certain amount of manganese chloride tetrahydrate and copper chloride dihydrate is dissolved in deionized water and added into a three-neck flask, and the stirring is kept. Then, a certain amount of bentonite and lignin are added into the three-neck flask and stirred, and then sodium borohydride is dissolved in deionized water and added into the three-neck flask dropwise. Then, certain amounts of acrylamide and N ', N' -methylenebisacrylamide were added to the three-necked flask. Finally, potassium persulfate and N, N, N ', N' -tetramethylethylenediamine were added to the reactor. Filtering the solution to obtain particles of 2-5mm, namely the particle electrode. The preparation method can increase the stability of the particle electrode and prevent the influence on the dispersion degree due to the agglomeration of magnetism and the like in water.
Example 1
A three-dimensional electro-catalytic device for removing organic pollutants, nitrate nitrogen and ammonia nitrogen comprises: the device comprises a supporting layer 13, an anode plate 7, a cathode plate 9, a particle electrode 8 and an aeration device which are arranged above the supporting layer 13, wherein the particle electrode 8 is positioned between the anode plate 7 and the cathode plate 9, the anode plate 7 is made of a titanium matrix, a coating is arranged on the surface of the titanium matrix, the aeration device is arranged below the supporting layer, and the supporting layer 13 is provided with air holes.
A plurality of anode plates 7 and a plurality of cathode plates 9 are arranged, and the anode plates and the cathode plates are arranged at intervals. Further, a plurality of anode plates and cathode plates are vertically arranged. Furthermore, the distance between the anode plate and the cathode plate is 10-20 cm. In one embodiment, 5 sets of plates are provided.
The water inlet and the water outlet are arranged on the shell, the water inlet 5 is located below the side of the anode plate on the edge, and the water outlet is located on the upper portion of the side opposite to the water inlet 5. The shell is made of stainless steel or carbon steel, and is lined with epoxy coal tar pitch anticorrosive paint. The water inlet pipeline connected with the water inlet is provided with a valve 6 for controlling the water inflow and cutting off.
Still include the electromagnetism district, the electromagnetism district is connected with the delivery port, and the inside in electromagnetism district sets up electromagnetic means 12. Further, a water outlet 10 is arranged at the upper part of the electromagnetic area. Further, the bottom in electromagnetic area sets up the return water mouth, the return water mouth passes through return line 2 with the water inlet and is connected. The return pipeline 2 is provided with a return water pump 1.
The device also comprises a direct current power supply 11, and the direct current power supply 11 is connected with the anode plate and the cathode plate. The pole plate is connected with a direct current power supply 11 through a lead. The direct current power supply 11 can regulate current, and the current is about 2A when the equipment runs. The lead is led out from the positive pole of the direct current power supply, is sequentially connected with the anode plate from the left end, and the other lead is led out from the negative pole of the direct current power supply and is connected with the cathode plate from the left side at one time.
The aeration device comprises an aeration pipeline 4, an aeration head 3 and a blower, wherein the aeration pipeline 4 is connected with the aeration head 3, and the blower is connected with the aeration pipeline 4. The aeration pipeline 4 is supported by an aeration pipeline bracket, the cathode plate and the anode plate are supported by a polar plate bracket, and the aeration pipeline bracket and the polar plate bracket are both fixed on the inner wall of the shell. The gas generated by the aeration device enters the upper space through the air holes on the supporting layer 13.
The conventional electrocatalysts described in examples 2 and 3 were (titanium matrix for the anode and cathode plates, respectively, without particle electrodes, and without coating of the anode surface).
Example 2
The main pollutants of the wastewater produced by Shandong chemical industry Co Ltd are formaldehyde, methanol, N-methyl pyrrolidone, tetrahydrofuran, toluene and the like, the wastewater is in a yellow turbid state and has irritant gas, COD is 3600mg/L, total nitrogen is 100mg/L, and the pH value is 7.0. And starting a direct-current power supply, and synchronously removing organic pollutants and total nitrogen. And adjusting the air flow rate of the aeration pipe to be 6L/min. The wastewater enters from the water inlet, is degraded by electrocatalysis and then flows out from the water outlet. By comparing the same water quality on site, one uses the three-dimensional electrocatalysis device of example 1, and one uses the common electrocatalysis device. After 120min of reaction, the COD of the effluent of the device in example 1 was 1000mg/L, the total nitrogen was 40mg/L, the COD of the effluent of a common electro-catalytic device was 2600mg/L, and the total nitrogen was 94 mg/L.
Example 3
The industrial wastewater of certain pharmaceutical company in Shandong contains residual products, reactants, catalytic substances, solvents and the like, and belongs to complex organic wastewater with high concentration, high chroma and difficult biochemical treatment, wherein the chemical oxygen demand of the high-concentration wastewater is 3000mg/L, and the total nitrogen is 70 mg/L. One with the three-dimensional electrocatalysis device of example 1 and one with the ordinary electrocatalysis device for the same water quality on the project site. And starting a direct-current power supply, and synchronously removing organic pollutants and total nitrogen. And adjusting the air flow rate of the aeration pipe to be 6L/min. The wastewater enters from the water inlet, is degraded by electrocatalysis and then flows out from the water outlet. After 120min of reaction, the COD of the effluent of example 1 is 900mg/L, the total nitrogen is 23mg/L, the COD of the effluent of a common electro-catalytic device is 2200mg/L, and the total nitrogen is 60 mg/L.
Comparative example 1
The same treatment method as that of the wastewater of example 2 was used, except that the particle electrode in the three-dimensional electrocatalysis apparatus of example 1 was changed to nano zero-valent iron.
The COD of the effluent was 1600mg/L and the total nitrogen was 45 mg/L.
Comparative example 2
The same treatment method as in example 2 was used, except that the coating layer (Gd-doped titanium-based tin dioxide) on the surface of the anode in the three-dimensional electrocatalytic device of example 1 was removed.
The COD of the effluent was 1700mg/L and the total nitrogen was 48 mg/L.
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 (10)
1. A three-dimensional electrocatalysis method for removing organic pollutants, nitrate nitrogen and ammonia nitrogen is characterized in that: treating the wastewater by using a three-dimensional electrode catalytic system;
the three-dimensional electrode catalytic system comprises the following components: the metal titanium is used as an anode, a coating is arranged on the surface of the anode plate, the coating is made of Gd-doped titanium-based tin dioxide and is used as an anode, the metal titanium is used as a cathode, a particle electrode is arranged between the cathode and the anode, and the particle electrode is formed by loading nanometer zero-valent iron on bentonite doped with copper and manganese metal elements.
2. The three-dimensional electrocatalytic method for removing organic pollutants, nitrate nitrogen and ammonia nitrogen as recited in claim 1, wherein: the preparation method of the Gd-doped titanium-based tin dioxide comprises the following steps: soaking a titanium substrate in an immersion liquidThe composition of the impregnating solution is SnCl4、SbCl3、Gd(NO3)3Water, hydrochloric acid, ethanol, propanol and isopropanol, drying the titanium matrix after impregnation, then carrying out heat treatment at 350 ℃, and then carrying out heat treatment at 700 ℃ to obtain Gd-doped titanium-based tin dioxide.
3. The three-dimensional electrocatalytic method for removing organic pollutants, nitrate nitrogen and ammonia nitrogen as recited in claim 1, wherein: the preparation method of the particle electrode comprises the following steps: mixing an iron trichloride aqueous solution, a manganese chloride tetrahydrate aqueous solution and a copper chloride dihydrate aqueous solution, then adding bentonite, lignin and sodium borohydride, then adding acrylamide and N ', N' -methylene-bisacrylamide, finally adding potassium persulfate and N ', N' -tetramethyl-ethylenediamine, and reacting to obtain the particle electrode.
4. The three-dimensional electrocatalytic method for removing organic pollutants, nitrate nitrogen and ammonia nitrogen as recited in claim 1, wherein: in the process of wastewater treatment, the running current is 1.5-2.5A.
5. The three-dimensional electrocatalytic method for removing organic pollutants, nitrate nitrogen and ammonia nitrogen as recited in claim 1, wherein: in the process of wastewater treatment, air is introduced into the three-dimensional electrode catalytic system.
6. The utility model provides an organic pollutant, nitro-nitrogen and ammonia nitrogen get rid of three-dimensional electro-catalytic device which characterized in that: the method comprises the following steps: the device comprises a supporting layer, and an anode plate, a cathode plate, a particle electrode and an aeration device which are arranged above the supporting layer, wherein the particle electrode is positioned between the anode plate and the cathode plate, the anode plate is made of a titanium matrix, a coating is arranged on the surface of the titanium matrix, the aeration device is arranged below the supporting layer, and the supporting layer is provided with air holes.
7. The three-dimensional electrocatalytic device for removing organic pollutants, nitrate nitrogen and ammonia nitrogen as recited in claim 6, wherein: the anode plate and the cathode plate are arranged in a plurality of numbers, and the anode plates and the cathode plates are arranged at intervals.
8. The three-dimensional electrocatalytic device for removing organic pollutants, nitrate nitrogen and ammonia nitrogen as recited in claim 6, wherein: the distance between the anode plate and the cathode plate is 10-20 cm.
9. The three-dimensional electrocatalytic device for removing organic pollutants, nitrate nitrogen and ammonia nitrogen as recited in claim 6, wherein: still include the electromagnetism district, the electromagnetism district is connected with the delivery port, and the inside in electromagnetism district sets up electromagnetic means.
10. The three-dimensional electrocatalytic device for removing organic pollutants, nitrate nitrogen and ammonia nitrogen as recited in claim 6, wherein: the aeration device comprises an aeration pipeline, an aeration head and a blower, wherein the aeration pipeline is connected with the aeration head, and the blower is connected with the aeration pipeline.
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