CN113024001A - Electrochemical-based sequencing batch leachate integrated decarbonization and denitrification device and method thereof - Google Patents
Electrochemical-based sequencing batch leachate integrated decarbonization and denitrification device and method thereof Download PDFInfo
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- 238000005262 decarbonization Methods 0.000 title claims abstract description 25
- 238000012163 sequencing technique Methods 0.000 title claims abstract description 20
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- 229910052757 nitrogen Inorganic materials 0.000 claims description 15
- 239000007789 gas Substances 0.000 claims description 14
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims description 12
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- 239000001569 carbon dioxide Substances 0.000 claims description 6
- 238000007210 heterogeneous catalysis Methods 0.000 claims description 6
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- VUZPPFZMUPKLLV-UHFFFAOYSA-N methane;hydrate Chemical compound C.O VUZPPFZMUPKLLV-UHFFFAOYSA-N 0.000 claims description 6
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- DXKGMXNZSJMWAF-UHFFFAOYSA-N copper;oxido(oxo)iron Chemical compound [Cu+2].[O-][Fe]=O.[O-][Fe]=O DXKGMXNZSJMWAF-UHFFFAOYSA-N 0.000 description 1
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- 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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- 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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- C02F1/48—Treatment of water, waste water, or sewage with magnetic or electric fields
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- C02F2101/16—Nitrogen compounds, e.g. ammonia
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Abstract
The invention discloses an electrochemical-based sequencing batch leachate integrated decarbonization and denitrification device and a method thereof, wherein the device comprises a first carbon material electrode, a second carbon material electrode, a first metal oxide electrode and a second metal oxide electrode which can synchronously rotate along with a rotating shaft in the vertical direction, and the axial direction of the rotating shaft is parallel to the water flow direction; the bottom of the inner cavity is provided with an electromagnetic device capable of adsorbing magnetic iron compound particles and an aeration device capable of supplying oxygen, and the inner cavity is also provided with a plurality of stirring devices. According to the integrated decarbonization and denitrification device and method for the leachate, a sequencing batch type leachate is formed by combining a heterogeneous electro-Fenton system and an electro-oxidation system, organic matters and ammonia nitrogen in the leachate can be removed with high efficiency step by step, the denitrification defect of a single electro-Fenton system and the decarbonization defect of the single electro-oxidation system are overcome, and the integrated decarbonization and denitrification device and method for the leachate have the advantages of small occupied area, strong in-situ retention of a catalyst, low risk of generation of chlorine-containing byproducts and the like.
Description
Technical Field
The invention belongs to the field of sewage treatment, and particularly relates to an electrochemical-based sequencing batch leachate integrated decarbonization and denitrification device and a method thereof.
Background
Currently, with the large increase in population and the rapid increase in consumer demand, the demand for domestic waste disposal is increasing continuously. At present, technologies such as landfill, incineration, aerobic composting and the like become important means for effectively solving the problem of the refuse city. However, the process of disposing of household garbage is accompanied by certain secondary pollution problems, wherein the pollution of leachate is one of the problems which cannot be ignored. The leachate usually contains high-concentration organic matters, high-concentration ammonia nitrogen and high-concentration chloride ions, belongs to a class of high-concentration organic salt-containing and nitrogen-containing wastewater, and can cause great threat to the ecological environment and human health if directly discharged into the external environment.
The combined process of biological treatment and membrane treatment is a common process for treating percolate, but the efficiency of the biological treatment process is often influenced by the change of the quality and the quantity of the percolate, and the membrane treatment process inevitably has the problems of membrane pollution and reverse osmosis concentrated water.
In recent years, electrochemical technology has been widely used in the treatment of leachate due to its environmental suitability, stability and ease of operation. electro-Fenton is a high-grade oxidation process based on traditional Fenton oxidation, can generate a Fenton reagent in situ, and has the advantages of no need of adding a medicament, high mineralization degree of organic matters and the like, but hydroxyl radicals, which are strong oxidizing substances generated in the electro-Fenton process, cannot effectively remove ammonia nitrogen, and have the defect of denitrification. Electrooxidation is an electrochemical process closely related to the properties of anode materials, sewage characteristics and other factors, and can convert chloride ions in waste water into hypochlorous acid through a chlorine analyzing anode in chlorine-containing waste water, so that the effective removal of ammonia nitrogen can be realized by utilizing the principle of breakpoint chlorination, but complete mineralization of organic matters cannot be realized, the defect of carbon removal exists, and the risk of generation of organic chlorides exists.
Disclosure of Invention
The invention aims to overcome the defects of the prior art, and provides an electrochemistry-based sequencing batch leachate integrated decarbonization and denitrification device and method by combining electro-Fenton and electro-oxidation pollutant removal mechanisms, so that the high-efficiency and clean removal of organic matters and ammonia nitrogen in leachate is realized.
The technical scheme adopted by the invention is as follows:
the invention provides an electrochemistry-based sequencing batch leachate integrated decarbonization and denitrification device, which comprises a reaction main body with a hollow inner cavity; the upper part of the side wall of one side of the reaction main body is provided with a water inlet pipe communicated with the inner cavity, the bottom of the side wall of the other opposite side is provided with a water outlet pipe communicated with the inner cavity, and the top of the side wall is provided with an exhaust pipe communicated with the inner cavity;
a first carbon material electrode, a second carbon material electrode, a first metal oxide electrode and a second metal oxide electrode are arranged in the inner cavity, the electrode plate surfaces of the first carbon material electrode and the second carbon material electrode are vertical to the water flow direction, and the initial positions of the electrode plate surfaces are both positioned below the water level in the inner cavity; the first carbon material electrode and the first metal oxide electrode are fixedly connected through a first binding post, and a first aeration device is arranged below the first carbon material electrode and the first metal oxide electrode; the second carbon material electrode and the second metal oxide electrode are fixedly connected through a second binding post, and a second aeration device is arranged below the second carbon material electrode and the second metal oxide electrode; the first binding post and the second binding post are fixedly connected with a rotating shaft which is horizontally arranged, so that the first carbon material electrode, the second carbon material electrode, the first metal oxide electrode and the second metal oxide electrode can synchronously rotate along with the rotating shaft in the vertical direction; the rotating shaft is positioned in the inner cavity, and the axis direction is parallel to the water flow direction; one end of the rotating shaft is electrically connected with a motor positioned outside the reaction main body, and the other end of the rotating shaft is movably connected with the side wall of the inner cavity; the first binding post is connected with one end of the electrode power supply device through a first lead, and the second binding post is connected with the other end of the electrode power supply device through a second lead;
the bottom of the inner cavity is provided with an electromagnetic device capable of adsorbing magnetic iron compound particles, and the inner cavity is also provided with a plurality of stirring devices.
Preferably, a water inlet valve is arranged on the water inlet pipe, and a water outlet valve is arranged on the water outlet pipe.
Preferably, the reaction body is a cylindrical structure which is horizontally placed, and the vertical cross section of the first carbon material electrode, the second carbon material electrode, the first metal oxide electrode and the second metal oxide electrode is in a half disc shape.
Preferably, the first carbon material electrode and the second carbon material electrode are both carbon felt electrodes, and the first metal oxide electrode and the second metal oxide electrode are both ruthenium iridium titanium mesh electrodes.
Preferably, the magnetic iron compound particles are natural magnetite fine powder.
Preferably, the motor is a stepping motor, and the electrode power supply device is a direct-current power supply with periodically switchable positive and negative polarities.
Preferably, the first aeration device and the second aeration device are membrane type microporous aerators.
Preferably, an alkali adding pipe and a pH probe which are connected with an external medicine adding system are also arranged in the inner cavity of the reaction main body.
Preferably, the stirring device is arranged on the side wall or the bottom of the inner cavity of the reaction body.
Another object of the invention is to provide a method for treating percolate according to any of the above mentioned devices, which is embodied as follows:
s1: opening a water inlet valve on the water inlet pipe to enable the leachate to be treated with the pH value adjusted to 2-4 to enter an inner cavity of the reaction main body through the water inlet pipe; when the liquid level of the leachate is higher than the first carbon material electrode and the second carbon material electrode and lower than the first metal oxide electrode and the second metal oxide electrode, closing the water inlet valve; the first carbon material electrode and the first metal oxide electrode are connected with the negative electrode of the electrode power supply device, and the second carbon material electrode and the second metal oxide electrode are connected with the positive electrode of the electrode power supply device; starting the electrode power supply device, the first aeration device and the stirring device, wherein the electromagnetic device is in a power-off state, and the magnetic iron compound particles are uniformly distributed in the leachate; the first carbon material electrode is used as a cathode to convert oxygen from the first aeration device into hydrogen peroxide, and the hydrogen peroxide is used to reduce metal ions (such as Fe) on the surface of the magnetic iron compound particles2+) The heterogeneous catalysis of the magnetic iron compound generates hydroxyl free radicals to generate a heterogeneous electro-Fenton carbon removal process, organic matters in the leachate are converted into carbon dioxide and water, and meanwhile, the magnetic iron compound particles dissolve reduced metal ions (such as Fe) in bulk phase solution2+) Or dissolved metal ions in an oxidized state (e.g. Fe)3+) Reduced metal ions (e.g. Fe) produced by reduction at the cathode2+) The hydrogen peroxide can be catalyzed to generate hydroxyl free radicals, the heterogeneous electro-Fenton carbon removal process is strengthened, and redundant gas is discharged out of the reaction main body through an exhaust pipe communicated with the outside;
powering off the first aeration device, and adjusting the pH value of the percolate to 5-7; the rotating shaft is driven by a motor to rotate 180 degrees, so that the positions of the first carbon material electrode and the second carbon material electrode are respectively exchanged with the positions of the first metal oxide electrode and the second metal oxide electrode; the first metal oxide electrode and the second metal oxide electrode after position conversion are immersed in the leachate, the second metal oxide electrode is used as an anode, and the leachate is treated by the methodThe chlorine ions are effectively converted into hypochlorous acid to generate an electro-oxidation denitrification process, ammonia nitrogen in the percolate is converted into nitrogen to be separated from the percolate, and meanwhile, the magnetic iron compound particles dissolve Fe into bulk phase solution2+Or dissolved Fe3+Reduction of Fe produced at the cathode2+All the nitrogen can be used as reducing species to realize the conversion of low-concentration nitrate nitrogen generated after electro-Fenton treatment to nitrogen, and the redundant gas is discharged out of the reaction main body through an exhaust pipe;
the electrode power supply device and the stirring device are powered off, the rotating shaft is driven by the motor to rotate 180 degrees, so that the first carbon material electrode and the second carbon material electrode are respectively exchanged with the first metal oxide electrode and the second metal oxide electrode in position, and the first carbon material electrode and the second carbon material electrode after position conversion are positioned below the first metal oxide electrode and the second metal oxide electrode; the electromagnetic device is electrified to work, and the magnetic iron compound particles are adsorbed at the bottom in the reaction tank; opening a water outlet valve of the water outlet pipe to enable the treated percolate to be discharged out of the reaction main body through the water outlet pipe; closing the water outlet valve, and powering off the electromagnetic device to finish the first percolate treatment period;
s2: after the first percolate treatment period is finished, opening a water inlet valve on the water inlet pipe, and enabling the percolate to be treated with the pH adjusted to 2-4 to enter an inner cavity of the reaction main body through the water inlet pipe; when the liquid level of the leachate is higher than the first carbon material electrode and the second carbon material electrode and lower than the first metal oxide electrode and the second metal oxide electrode, closing the water inlet valve; switching the positive and negative polarities of the electrode power supply device to enable the first carbon material electrode and the first metal oxide electrode to be connected with the positive electrode of the electrode power supply device, and the second carbon material electrode and the second metal oxide electrode to be connected with the negative electrode of the electrode power supply device; starting the electrode power supply device, the second aeration device and the stirring device, wherein the electromagnetic device is in a power-off state, and the magnetic iron compound particles are uniformly distributed in the leachate; the second carbon material electrode is used as a cathode for converting oxygen from the second aeration device into hydrogen peroxide, and the hydrogen peroxide is used for reducing metal ions (such as Fe) on the surfaces of the magnetic iron compound particles2+) Heterogeneous catalysis of (2) followed by generation of hydroxyl radicalsThe heterogeneous electro-Fenton decarbonization process is carried out to convert the organic matters in the percolate into carbon dioxide and water, and simultaneously, the magnetic iron compound particles dissolve reduced metal ions (such as Fe) in the bulk phase solution2+) Or dissolved metal ions in an oxidized state (e.g. Fe)3+) Reduced metal ions (e.g. Fe) produced by reduction at the cathode2+) The hydrogen peroxide can be catalyzed to generate hydroxyl free radicals, the heterogeneous electro-Fenton carbon removal process is strengthened, and redundant gas is discharged out of the reaction main body through an exhaust pipe communicated with the outside;
powering off the second aeration device, and adjusting the pH value of the percolate to 5-7; the rotating shaft is driven by a motor to rotate 180 degrees, so that the positions of the first carbon material electrode and the second carbon material electrode are respectively exchanged with the positions of the first metal oxide electrode and the second metal oxide electrode; the first metal oxide electrode and the second metal oxide electrode after the position conversion are immersed in the leachate, the first metal oxide electrode is used as an anode to effectively convert chloride ions in the leachate into hypochlorous acid to generate an electro-oxidation denitrification process, ammonia nitrogen in the leachate is converted into nitrogen to be separated from the leachate, and meanwhile, Fe dissolved out of magnetic iron compound particles into bulk phase solution2+Or dissolved Fe3+Reduction of Fe produced at the cathode2+All the nitrogen can be used as reducing species to realize the conversion of low-concentration nitrate nitrogen generated after electro-Fenton treatment to nitrogen, and the redundant gas is discharged out of the reaction main body through an exhaust pipe;
the electrode power supply device and the stirring device are powered off, the rotating shaft is driven by the motor to rotate 180 degrees, so that the first carbon material electrode and the second carbon material electrode are respectively exchanged with the first metal oxide electrode and the second metal oxide electrode in position, and the first carbon material electrode and the second carbon material electrode after position conversion are positioned below the first metal oxide electrode and the second metal oxide electrode; the electromagnetic device is electrified to work, and the magnetic iron compound particles are adsorbed at the bottom in the reaction tank; opening a water outlet valve of the water outlet pipe to enable the treated percolate to be discharged out of the reaction main body through the water outlet pipe; closing the water outlet valve, and powering off the electromagnetic device to finish a second percolate treatment period;
s3: the first percolate treatment period and the second percolate treatment period form an operation period together; and repeating the operation cycle to realize the sequencing batch treatment of the percolate.
Compared with the prior art, the invention has the following beneficial effects:
1) according to the invention, the leachate is treated by adopting the sequence of firstly removing carbon by electro-Fenton and then removing nitrogen by electro-oxidation, so that the organic matters and ammonia nitrogen in the leachate are removed step by step and efficiently, the defect of nitrogen removal of a single electro-Fenton system and the defect of carbon removal of a single electro-oxidation system are overcome, meanwhile, the organic matters are degraded by electro-Fenton, the way that the organic matters participate in the electro-oxidation process to generate chlorine-containing byproducts is effectively blocked, and the safety risk of treating effluent is reduced.
2) According to the invention, magnetic iron compound particles are coupled into a reaction system, on one hand, the magnetic iron compound particles are used as a heterogeneous catalyst in an electro-Fenton reaction to catalyze hydrogen peroxide generated by a cathode to generate hydroxyl radicals, so that advanced oxidative degradation of organic matters is realized under the condition of not adding a chemical reagent, and in-situ recycling of the catalyst can be realized through an electromagnetic device, and meanwhile, the magnetic iron compound particles have the advantages of no iron mud generation in the reaction process, standard chromaticity of treated water, wide applicable pH range and the like; on the other hand, Fe generated in a solution of magnetic iron compound particles in bulk phase2+As a reducing species, the conversion of low-concentration nitrate nitrogen generated after electro-Fenton treatment of percolate into nitrogen can be realized, and the integral denitrification effect of the system is enhanced.
3) The invention effectively alleviates the problem of scaling pollution on the surface of the electrode and prolongs the service life of the electrode material by periodically switching the positive polarity and the negative polarity of the electrode power supply device.
Drawings
FIG. 1 is a schematic diagram of the apparatus of the present invention;
FIG. 2 is a top view of the apparatus of the present invention;
FIG. 3 is a partial left side view of the apparatus of the present invention;
the reference numbers in the figures are: 1-a reaction body, 2-a first carbon material electrode, 3-a second carbon material electrode, 4-a first metal oxide electrode, 5-a second metal oxide electrode, 6-a first binding post, 7-a second binding post, 8-a rotating shaft, 9-a motor, 10-an electrode power supply device, 11-an electromagnetic device, 12-a first lead, 13-a second lead, 14-magnetic iron compound particles, 15-a first aeration device, 16-a second aeration device, 17-a stirring device, 18-a water inlet pipe, 19-a water outlet pipe, 20-an exhaust pipe, 21-an alkali adding pipe, 22-a pH probe, 23-a water inlet valve and 24-a water outlet valve.
Detailed Description
The invention will be further elucidated and described with reference to the drawings and the detailed description. The technical features of the embodiments of the present invention can be combined correspondingly without mutual conflict.
As shown in fig. 1 to 3, the electrochemical-based sequencing batch leachate integrated decarbonization and denitrification apparatus provided by the present invention includes a reaction body 1, a first carbon material electrode 2, a second carbon material electrode 3, a first metal oxide electrode 4, and a second metal oxide electrode 5. The reaction body 1 is a shell structure with a hollow inner cavity, a water inlet pipe 18 is arranged on the upper portion of one side wall of the reaction body 1, a water outlet pipe 19 is arranged at the bottom of the opposite side wall, and an exhaust pipe 20 is arranged at the top of the shell. One end of the water inlet pipe 18 is communicated with the inner cavity of the reaction main body 1, the other end is communicated with an external water supply device and is used for introducing the percolate to be treated into the reaction main body 1, and the water inlet pipe 18 is arranged at the position of the upper part of the side wall of the reaction main body 1 as far as possible so as to prevent the percolate liquid level in the inner cavity from submerging the position of the water inlet pipe 18 and further causing the backflow of the percolate. One end of the water outlet pipe 19 is communicated with the inner cavity of the reaction main body 1, the other end is communicated with the outside and used for discharging the treated percolate into the reaction main body 1, and the water outlet pipe 19 is arranged on the side wall far away from the position of the water inlet pipe 18, so that the percolate can stay in the reaction main body 1 for as much time as possible and can be fully reacted. In order to ensure the air pressure balance in the device, an exhaust pipe 20 communicated with the inner cavity is arranged at the top of the reaction main body 1.
In this embodiment, the reaction body 1 may have a horizontal cylindrical structure, i.e., the reaction body 1 has a circular cross section in the vertical direction. In order to better control the flow rate of the percolate entering and discharging, a water inlet valve 23 can be arranged on the water inlet pipe 18, and a water outlet valve 24 can be arranged on the water outlet pipe 19.
A first carbon material electrode 2, a second carbon material electrode 3, a first metal oxide electrode 4, and a second metal oxide electrode 5 are provided in the inner cavity of the reaction body 1. The first carbon material electrode 2 and the second carbon material electrode 3 are identical in structure and have a certain interval therebetween, the electrode faces of the first carbon material electrode 2 and the second carbon material electrode 3 are arranged oppositely and are perpendicular to the water flow direction, in an initial state, the first carbon material electrode 2 and the second carbon material electrode 3 are both located at the lower part of an inner cavity of the reaction main body 1, and when leachate to be treated is introduced into the inner cavity, the first carbon material electrode 2 and the second carbon material electrode 3 are both located below the liquid level of the leachate. The first metal oxide electrode 4 and the second metal oxide electrode 5 are identical in structure and have a certain interval therebetween, the electrode plate surfaces of the first metal oxide electrode 4 and the second metal oxide electrode 5 are arranged oppositely and are perpendicular to the water flow direction, the first metal oxide electrode 4 and the second metal oxide electrode 5 are both positioned at the upper part of the inner cavity of the reaction main body 1 in an initial state, and when the leachate to be treated is introduced into the inner cavity, the first metal oxide electrode 4 and the second metal oxide electrode 5 are both positioned above the liquid level of the leachate.
In the present embodiment, as shown in fig. 3, the first carbon material electrode 2, the second carbon material electrode 3, the first metal oxide electrode 4, and the second metal oxide electrode 5 may each have a half-disk shape in vertical cross section, and the first carbon material electrode 2 and the first metal oxide electrode 4 are disposed to be diametrically opposed to each other, and the second carbon material electrode 3 and the second metal oxide electrode 5 are disposed to be diametrically opposed to each other. The first carbon material electrode 2 and the second carbon material electrode 3 have large specific surface area, high catalytic activity, high dissolved oxygen transfer rate and are used for in-situ Fe generation2+The carbon felt electrode with strong capacity is used for improving the efficiency of hydrogen peroxide in situ production of the cathode in the electro-Fenton process, and the ruthenium iridium titanium mesh electrodes which have good chlorine catalytic activity and are applied industrially are adopted as the first metal oxide anode 4 and the second metal oxide electrode 5 so as to improve the chlorine separation efficiency in the electro-oxidation process.
The first carbon material electrode 2 and the first metal oxide electrode 4 are fixedly connected through a first connecting post 6, a first aeration device 15 is arranged below the first carbon material electrode 2 and the first metal oxide electrode 4, and the first aeration device 15 is used for carrying out aeration oxygen supply on the first carbon material electrode 2. The second carbon material electrode 3 and the second metal oxide electrode 5 are fixedly connected through a second terminal 7, a second aeration device 16 is arranged below the second carbon material electrode 3 and the second metal oxide electrode 5, and the second aeration device 16 is used for aerating and supplying oxygen to the second carbon material electrode 3. The first terminal 6 and the second terminal 7 are fixedly connected with a rotating shaft 8 which is horizontally arranged, so that the first carbon material electrode 2, the second carbon material electrode 3, the first metal oxide electrode 4 and the second metal oxide electrode 5 can synchronously rotate along with the rotating shaft 8 in the vertical direction. That is, during the rotation, the first carbon material electrode 2 and the second carbon material electrode 3 are kept in relative arrangement in real time, and the first metal oxide electrode 4 and the second metal oxide electrode 5 are kept in relative arrangement in real time.
The rotating shaft 8 is positioned in the inner cavity, and the axis direction is parallel to the water flow direction; one end of the rotating shaft 8 is electrically connected with a motor 9 positioned outside the reaction main body 1, and the other end is movably connected with the side wall of the inner cavity. In the present embodiment, the rotating shaft 8 should be fixed to the middle of the first and second terminals 6 and 7 such that only the first and second carbon material electrodes 2 and 3 or the first and second metal oxide electrodes 4 and 5 are located below the water surface of the leachate when the rotating shaft 8 is rotated 180 °.
The first terminal 6 is connected to one end of the electrode power supply device 10 through a first lead 12, and the second terminal 7 is connected to the other end of the electrode power supply device 10 through a second lead 13, so that the electrode electrical properties of the first carbon material electrode 2 and the first metal oxide electrode 4 connected to the first terminal 6 are opposite to the electrode electrical properties of the second carbon material electrode 3 and the second metal oxide electrode 5 connected to the second terminal 7.
An electromagnetic device 11 capable of adsorbing magnetic iron compound particles 14 is arranged at the bottom of the inner cavity of the reaction body 1 so as to prevent the reaction body from being usedThe particles 14 of the ferrimagnetic compound are lost as the leachate is drained. Specifically, the electromagnetic device 11 can realize the rapid separation of the magnetic iron compound particles 14 from the leachate, the magnetic iron compound particles 14 are natural magnetite fine powder which is easy to obtain, the main component of the magnetic iron compound particles is ferroferric oxide with an inverse spinel structure, and Fe is contained in octahedral positions of the ferroferric oxide at the same time2+And Fe3+So that the metal ions of the catalyst can perform reversible redox reaction at the same position in the Fenton reaction process, effectively catalyze the hydrogen peroxide to generate hydroxyl free radicals, and simultaneously, the ferroferric oxide can dissolve Fe with Fenton catalytic activity into bulk phase solution2+And can be reduced to Fe at the cathode2+Fe (b) of3+Effectively promote Fe2+The generation of hydroxyl free radicals is further strengthened, and the high-efficiency catalysis of the electro-Fenton reaction is finally realized; in addition, Fe produced from ferroferric oxide in bulk solution2+And from Fe3+Cathodic reduction of regenerated Fe2+And the nitrogen-containing organic nitrogen can also be used as a reducing species to realize the conversion of low-concentration nitrate nitrogen generated after electro-Fenton treatment to nitrogen and strengthen the integral denitrification effect of the system. In fact, the magnetic iron compound particles 14 may be maghemite (γ -Fe) in addition to natural magnetite fine powder2O3) Hexalepidocrocite (delta-FeOOH), spinel (e.g. CoFe)2O4、MnFe2O4And CuFe2O4) And perovskites (e.g., BiFeO)3) One or more natural ores in the above process.
A plurality of stirring devices 17 are also arranged in the inner cavity, and the stirring devices 17 can be arranged on the side wall or the bottom of the inner cavity of the reaction main body 1 so as to be used for homogenizing the percolate and simultaneously ensure that the percolate is fully contacted with the magnetic iron compound particles. An alkali adding pipe 21 and a pH probe 22 which are connected with an external medicine adding system are further arranged in the inner cavity of the reaction main body 1, alkali liquor can be added into the inner cavity through the alkali adding pipe 21, the pH value of the percolate can be detected through the pH probe 22, and the pH value of the percolate after electro-Fenton treatment is adjusted to be in an optimal state required by electro-oxidation reaction.
In this embodiment, the motor 9 is a stepping motor capable of rotating the rotating shaft 180 degrees, and the rotating shaft 8 is driven by the motor 9 to rotate 180 degrees, so that the exchange of the electrode positions can be realized. The electrode power supply device 10 is a direct current power supply with periodically switchable positive and negative polarities, and the electrode power supply device 10 is switched between the positive and negative polarities once after each batch of percolate is treated, so that the scaling pollution phenomenon on the surface of an electrode is reduced, and the service life of an electrode material is prolonged. The first aeration apparatus 15 and the second aeration apparatus 16 are membrane type microaeration apparatuses for supplying oxygen required for the production of hydrogen peroxide to the first carbon material electrode 2 or the second carbon material electrode 3.
The method for treating the percolate by using the sequencing batch integrated decarbonization and denitrification device comprises the following specific steps:
s1: and opening a water inlet valve 23 on the water inlet pipe 18 to enable the leachate to be treated with the pH value adjusted to 2-4 to enter the inner cavity of the reaction main body 1 through the water inlet pipe 18. And (3) closing the water inlet valve 23 when the leachate just submerges the first carbon material electrode 2 and the second carbon material electrode 3, namely the liquid level of the leachate is higher than the first carbon material electrode 2 and the second carbon material electrode 3 and lower than the first metal oxide electrode 4 and the second metal oxide electrode 5. At this time, the first carbon material electrode 2 and the first metal oxide electrode 4 are connected to the negative electrode of the electrode feeding device 10, and the second carbon material electrode 3 and the second metal oxide electrode 5 are connected to the positive electrode of the electrode feeding device 10.
The electrode power supply device 10, the first aeration device 15 and the stirring device 17 start to work by electrifying, the electromagnetic device 11 is in a power-off state, and the magnetite fine powder as the magnetic iron compound particles 14 is uniformly distributed in the percolate. Since the first carbon material electrode 2 is connected to the negative electrode of the power supply and the first carbon material electrode 2 serves as the cathode, oxygen from the first aeration device 15 is converted into hydrogen peroxide, which is Fe-based on the surface of the magnetic iron compound particles 142+The heterogeneous catalysis of (2) then generates hydroxyl free radicals with strong oxidizing property, a heterogeneous electro-Fenton carbon removal process is carried out, organic matters in the leachate are mineralized into carbon dioxide and water, and meanwhile, Fe dissolved out from the magnetic iron compound particles 14 into bulk phase solution2+Or dissolved Fe3+Reduction of Fe produced at the cathode2+And the catalyst can also be used as a Fenton catalyst to promote the generation of hydroxyl free radicals and strengthen the heterogeneous electro-Fenton carbon removal process, and redundant gas is discharged out of the reaction body 1 through an exhaust pipe 20 communicated with the outside.
After the leachate is treated by heterogeneous electro-Fenton reaction, the first aeration device 15 is powered off, the external automatic dosing system monitors the pH value of the leachate by means of the pH probe 22, alkali liquor is added into the leachate through the alkali adding pipe 21, and the pH value of the leachate is adjusted to be 5-7. The motor 9 starts to work by electrifying, drives the rotating shaft 8 to rotate 180 degrees, so that the positions of the first carbon material electrode 2 and the first metal oxide electrode 4 are exchanged, and the positions of the second carbon material electrode 3 and the second metal oxide electrode 5 are exchanged. The position-switched first metal oxide electrode 4 and second metal oxide electrode 5 are immersed in the leachate. The second metal oxide electrode 5 is used as an anode to effectively convert chloride ions in the percolate into hypochlorous acid, an electro-oxidation denitrification process is carried out by adopting a breakpoint chlorination principle, ammonia nitrogen in the percolate is converted into nitrogen to be separated from the percolate, and meanwhile, Fe dissolved out from the magnetic iron compound particles 14 to a bulk phase solution2+Or dissolved Fe3+Reduction of Fe produced at the cathode2+All of which can be used as reducing species to convert low-concentration nitrate nitrogen generated after electro-fenton treatment into nitrogen gas, and the excess gas is discharged out of the reaction body 1 through the exhaust pipe 20.
After the leachate is treated by the electro-oxidation reaction, the electrode power supply device 10 and the stirring device 17 are powered off, the rotating shaft 8 is driven by the motor 9 to rotate 180 degrees, so that the first carbon material electrode 2 and the second carbon material electrode 3 are respectively exchanged with the first metal oxide electrode 4 and the second metal oxide electrode 5, and the first carbon material electrode 2 and the second carbon material electrode 3 after position conversion are positioned below the first metal oxide electrode 4 and the second metal oxide electrode 5. The electromagnetic device 11 is electrified to work, and the magnetic iron compound particles 14 are quickly adsorbed at the bottom in the reaction tank 1, so that the separation from the percolate is realized. And opening a water outlet valve 24 of the water outlet pipe 19 to enable the treated percolate to be discharged out of the reaction main body 1 through the water outlet pipe 19. The outlet valve 24 is closed and the electromagnetic device 11 is powered off, thus completing the first percolate treatment cycle.
S2: complete the processAfter the first leachate treatment period, the water inlet valve 23 on the water inlet pipe 18 is opened, so that the leachate to be treated with the pH value adjusted to 2-4 enters the inner cavity of the reaction main body 1 through the water inlet pipe 18. And when the liquid level of the leachate is higher than the first carbon material electrode 2 and the second carbon material electrode 3 and lower than the first metal oxide electrode 4 and the second metal oxide electrode 5, closing the water inlet valve 23. The positive and negative polarities of the electrode feeder 10 are switched so that the first carbon material electrode 2 and the first metal oxide electrode 4 are connected to the positive electrode of the electrode feeder 10, and the second carbon material electrode 3 and the second metal oxide electrode 5 are connected to the negative electrode of the electrode feeder 10. The electrode power supply device 10, the second aeration device 16 and the stirring device 17 are started, the electromagnetic device 11 is in a power-off state, and magnetite fine powder serving as magnetic iron compound particles 14 is uniformly distributed in the percolate. The second carbon material electrode 3 serves as a cathode, and converts oxygen from the second aeration device 16 into hydrogen peroxide, which is Fe on the surface of the magnetic iron compound particles 142+Then generates hydroxyl free radicals under the action of heterogeneous catalysis, generates a heterogeneous electro-Fenton carbon removal process, converts organic matters in the percolate into carbon dioxide and water, and simultaneously, the magnetic iron compound particles 14 dissolve Fe into bulk phase solution2+Or dissolved Fe3+Reduction of Fe produced at the cathode2+And the catalyst can also be used as a Fenton catalyst to promote the generation of hydroxyl free radicals and strengthen the heterogeneous electro-Fenton carbon removal process, and redundant gas is discharged out of the reaction body 1 through an exhaust pipe 20 communicated with the outside.
And powering off the second aeration device 16, and adjusting the pH value of the percolate to 5-7. The rotating shaft 8 is driven by the motor 9 to rotate 180 degrees, so that the positions of the first carbon material electrode 2 and the second carbon material electrode 3 and the first metal oxide electrode 4 and the second metal oxide electrode 5 are exchanged respectively. The first metal oxide electrode 4 and the second metal oxide electrode 5 after the position conversion are immersed in the leachate, the first metal oxide electrode 4 is used as an anode to effectively convert chloride ions in the leachate into hypochlorous acid, an electro-oxidation denitrification reaction is carried out by a breakpoint chlorination principle, ammonia nitrogen in the leachate is converted into nitrogen to be separated from the leachate, and meanwhile, Fe dissolved out of the magnetic iron compound particles 14 into a bulk phase solution is added into the leachate2+Or dissolved Fe3+Reduction of Fe produced at the cathode2+Can be used as a reducing species to realize the conversion of low-concentration nitrate nitrogen generated after the electro-Fenton treatment process into nitrogen, and the redundant gas is discharged out of the reaction body 1 through the exhaust pipe 20.
And the electrode power supply device 10 and the stirring device 17 are powered off, the rotating shaft 8 is driven by the motor 9 to rotate 180 degrees, so that the first carbon material electrode 2 and the second carbon material electrode 3 are respectively exchanged with the first metal oxide electrode 4 and the second metal oxide electrode 5, and the first carbon material electrode 2 and the second carbon material electrode 3 after position conversion are positioned below the first metal oxide electrode 4 and the second metal oxide electrode 5. The electromagnetic device 11 is electrified to work, and the magnetic iron compound particles 14 are quickly adsorbed at the bottom in the reaction tank 1, so that the separation from the percolate is realized. And opening a water outlet valve 24 of the water outlet pipe 19 to enable the treated percolate to be discharged out of the reaction main body 1 through the water outlet pipe 19. The water outlet valve 24 is closed, the electromagnetic device 11 is powered off, and the second percolate treatment period is completed.
In general, in the second leachate treatment period, as the positive and negative polarities of the electrode power supply device 10 are switched, the second carbon material electrode 3 becomes a cathode in the electro-fenton reaction process, the first metal oxide electrode 4 becomes an anode in the electro-oxidation reaction process, the first aeration device 15 is in a power-off state in the electro-fenton reaction and the electro-oxidation reaction processes, the second aeration device 16 is powered on before the electro-fenton reaction starts and powered off before the electro-oxidation reaction starts, and other steps are the same as the first leachate treatment period.
S3: the first percolate treatment cycle and the second percolate treatment cycle jointly form an operating cycle. And repeating the operation cycle to realize the treatment of the percolate. When the device actually operates, the working period of the motor 9 and the electrode power supply device 10 can be regulated and controlled according to the concentration of organic matters, ammonia nitrogen and chloride ions in actual inlet water so as to set the hydraulic retention time of electro-Fenton reaction and electro-oxidation reaction and meet the treatment requirements of percolate with different water qualities. Meanwhile, the total cycle number of the operation period of the device can be regulated and controlled according to the water quantity which needs to be treated actually.
According to the integrated decarbonization and denitrification device and method, the heterogeneous electro-Fenton system and the electro-oxidation system are combined to form the integrated decarbonization and denitrification device and method, organic matters and ammonia nitrogen in the leachate can be removed step by step with high efficiency, the defect of denitrification of the single electro-Fenton system and the defect of decarbonization of the single electro-oxidation system are overcome, and the integrated decarbonization and denitrification device and method have the advantages of small occupied area, strong in-situ retention of a catalyst, low risk of generation of chlorine-containing byproducts and the like.
The above-described embodiments are merely preferred embodiments of the present invention, which should not be construed as limiting the invention. Various changes and modifications may be made by one of ordinary skill in the pertinent art without departing from the spirit and scope of the present invention. Therefore, the technical scheme obtained by adopting the mode of equivalent replacement or equivalent transformation is within the protection scope of the invention.
Claims (10)
1. An electrochemistry-based sequencing batch leachate integrated decarbonization and denitrification device is characterized by comprising a reaction main body (1) with a hollow inner cavity; a water inlet pipe (18) communicated with the inner cavity is arranged at the upper part of the side wall of one side of the reaction main body (1), a water outlet pipe (19) communicated with the inner cavity is arranged at the bottom of the side wall of the other opposite side, and an exhaust pipe (20) communicated with the inner cavity is arranged at the top;
a first carbon material electrode (2), a second carbon material electrode (3), a first metal oxide electrode (4) and a second metal oxide electrode (5) are arranged in the inner cavity, the electrode plate surfaces of the first carbon material electrode (2) and the second carbon material electrode (3) are vertical to the water flow direction, the initial positions of the electrode plate surfaces are both positioned below the water level in the inner cavity, the electrode plate surfaces of the first metal oxide electrode (4) and the second metal oxide electrode (5) are vertical to the water flow direction, and the initial positions of the electrode plate surfaces of the first metal oxide electrode and the second metal oxide electrode are both positioned above the water level in the inner cavity; the first carbon material electrode (2) and the first metal oxide electrode (4) are fixedly connected through a first binding post (6), and a first aeration device (15) is arranged below the first carbon material electrode (2) and the first metal oxide electrode (4); the second carbon material electrode (3) and the second metal oxide electrode (5) are fixedly connected through a second binding post (7), and a second aeration device (16) is arranged below the second carbon material electrode (3) and the second metal oxide electrode (5); the first binding post (6) and the second binding post (7) are fixedly connected with a rotating shaft (8) which is horizontally arranged, so that the first carbon material electrode (2), the second carbon material electrode (3), the first metal oxide electrode (4) and the second metal oxide electrode (5) can synchronously rotate along with the rotating shaft (8) in the vertical direction; the rotating shaft (8) is positioned in the inner cavity, and the axis direction is parallel to the water flow direction; one end of the rotating shaft (8) is electrically connected with a motor (9) positioned outside the reaction main body (1), and the other end of the rotating shaft is movably connected with the side wall of the inner cavity; the first binding post (6) is connected with one end of the electrode power supply device (10) through a first lead (12), and the second binding post (7) is connected with the other end of the electrode power supply device (10) through a second lead (13);
the bottom of the inner cavity is provided with an electromagnetic device (11) capable of adsorbing magnetic iron compound particles (14), and the inner cavity is also provided with a plurality of stirring devices (17).
2. The integrated decarbonization and denitrification device for sequencing batch leachate of claim 1, wherein the water inlet pipe (18) is provided with a water inlet valve (23), and the water outlet pipe (19) is provided with a water outlet valve (24).
3. The integrated decarbonization and denitrification device for sequencing batch leachate of claim 1, wherein the reaction body (1) is a horizontally placed cylindrical structure, and the vertical section of the first carbon material electrode (2), the second carbon material electrode (3), the first metal oxide electrode (4) and the second metal oxide electrode (5) is half disc-shaped.
4. The integrated decarbonization and denitrification device for the sequencing batch leachate of claim 1, wherein the first carbon material electrode (2) and the second carbon material electrode (3) are both carbon felt electrodes, and the first metal oxide electrode (4) and the second metal oxide electrode (5) are both ruthenium-iridium-titanium mesh electrodes.
5. The integrated decarbonization and denitrification device for leachate of sequencing batch type as set forth in claim 1, wherein the magnetic iron compound particles (14) are refined powder of natural magnetite.
6. The integrated decarbonization and denitrification device for leachate of sequencing batch type as claimed in claim 1, wherein the motor (9) is a stepping motor, and the electrode power supply device (10) is a dc power supply with periodically switchable positive and negative polarities.
7. The integrated decarbonization and denitrification device for sequencing batch leachate of claim 1, wherein the first aeration device (15) and the second aeration device (16) are membrane micro-porous aerators.
8. The integrated decarbonization and denitrification device for sequencing batch leachate of claim 1, wherein the inner cavity of the reaction body (1) is further provided with an alkali adding pipe (21) and a pH probe (22) connected with an external dosing system.
9. The integrated decarbonization and denitrification device for sequencing batch leachate of claim 1, wherein the stirring device (17) is disposed on the sidewall or bottom of the inner cavity of the reaction body (1).
10. A method for treating leachate according to any of claims 1 to 9, comprising the steps of:
s1: opening a water inlet valve (23) on the water inlet pipe (18) to enable the leachate to be treated with the pH value adjusted to 2-4 to enter an inner cavity of the reaction main body (1) through the water inlet pipe (18); when the liquid level of the leachate is higher than the first carbon material electrode (2) and the second carbon material electrode (3) and lower than the first metal oxide electrode (4) and the second metal oxide electrode (5), closing a water inlet valve (23); the first carbon material electrode (2) and the first metal oxide electrode (4) are connected with the negative electrode of an electrode power supply device (10), and the second carbon material electrode (3) and the second metal oxide electrode (5) are connected with the positive electrode of the electrode power supply device (10); starting an electrode power supply device (10), a first aeration device (15) and a stirring device (17), wherein an electromagnetic device (11) is in a power-off state, and magnetic iron compound particles (14) are uniformly distributed in the percolate; the first carbon material electrode (2) is used as a cathode, oxygen from the first aeration device (15) is converted into hydrogen peroxide, the hydrogen peroxide further generates hydroxyl radicals under the heterogeneous catalysis of the magnetic iron compound particles (14), a heterogeneous electro-Fenton carbon removal process is carried out, organic matters in percolate are converted into carbon dioxide and water, and redundant gas is discharged out of the reaction body (1) through an exhaust pipe (20) communicated with the outside;
powering off the first aeration device (15), and adjusting the pH value of the percolate to 5-7; the rotating shaft (8) is driven to rotate 180 degrees by the motor (9), so that the positions of the first carbon material electrode (2) and the second carbon material electrode (3) are respectively exchanged with the positions of the first metal oxide electrode (4) and the second metal oxide electrode (5); the first metal oxide electrode (4) and the second metal oxide electrode (5) after position conversion are immersed in the leachate, the second metal oxide electrode (5) is used as an anode to effectively convert chloride ions in the leachate into hypochlorous acid, an electro-oxidation denitrification process is carried out, ammonia nitrogen in the leachate is converted into nitrogen to be separated from the leachate, and redundant gas is discharged out of the reaction main body (1) through a gas exhaust pipe (20);
the electrode power supply device (10) and the stirring device (17) are powered off, the rotating shaft (8) is driven by the motor (9) to rotate 180 degrees, so that the first carbon material electrode (2) and the second carbon material electrode (3) are respectively exchanged with the first metal oxide electrode (4) and the second metal oxide electrode (5), and the first carbon material electrode (2) and the second carbon material electrode (3) after position conversion are positioned below the first metal oxide electrode (4) and the second metal oxide electrode (5); the electromagnetic device (11) is electrified to work, and the magnetic iron compound particles (14) are adsorbed at the bottom in the reaction tank (1); opening a water outlet valve (24) of the water outlet pipe (19) to enable the treated percolate to be discharged out of the reaction main body (1) through the water outlet pipe (19); closing the water outlet valve (24), and powering off the electromagnetic device (11) to complete the first percolate treatment period;
s2: after the first percolate treatment period is finished, opening a water inlet valve (23) on the water inlet pipe (18) to enable percolate to be treated with the pH value adjusted to be 2-4 to enter an inner cavity of the reaction main body (1) through the water inlet pipe (18); when the liquid level of the leachate is higher than the first carbon material electrode (2) and the second carbon material electrode (3) and lower than the first metal oxide electrode (4) and the second metal oxide electrode (5), closing a water inlet valve (23); switching the positive and negative polarities of the electrode power supply device (10) to connect the first carbon material electrode (2) and the first metal oxide electrode (4) with the positive electrode of the electrode power supply device (10), and connecting the second carbon material electrode (3) and the second metal oxide electrode (5) with the negative electrode of the electrode power supply device (10); starting an electrode power supply device (10), a second aeration device (16) and a stirring device (17), wherein an electromagnetic device (11) is in a power-off state, and magnetic iron compound particles (14) are uniformly distributed in the percolate; the second carbon material electrode (3) is used as a cathode, oxygen from the second aeration device (16) is converted into hydrogen peroxide, the hydrogen peroxide further generates hydroxyl radicals under the heterogeneous catalysis of the magnetic iron compound particles (14), a heterogeneous electro-Fenton carbon removal process is carried out, organic matters in percolate are converted into carbon dioxide and water, and redundant gas is discharged out of the reaction main body (1) through an exhaust pipe (20) communicated with the outside;
powering off the second aeration device (16), and adjusting the pH value of the percolate to 5-7; the rotating shaft (8) is driven to rotate 180 degrees by the motor (9), so that the positions of the first carbon material electrode (2) and the second carbon material electrode (3) are respectively exchanged with the positions of the first metal oxide electrode (4) and the second metal oxide electrode (5); the first metal oxide electrode (4) and the second metal oxide electrode (5) after position conversion are immersed in the leachate, the first metal oxide electrode (4) is used as an anode to effectively convert chloride ions in the leachate into hypochlorous acid, an electro-oxidation denitrification process is carried out, ammonia nitrogen in the leachate is converted into nitrogen to be separated from the leachate, and redundant gas is discharged out of the reaction main body (1) through a gas exhaust pipe (20);
the electrode power supply device (10) and the stirring device (17) are powered off, the rotating shaft (8) is driven by the motor (9) to rotate 180 degrees, so that the first carbon material electrode (2) and the second carbon material electrode (3) are respectively exchanged with the first metal oxide electrode (4) and the second metal oxide electrode (5), and the first carbon material electrode (2) and the second carbon material electrode (3) after position conversion are positioned below the first metal oxide electrode (4) and the second metal oxide electrode (5); the electromagnetic device (11) is electrified to work, and the magnetic iron compound particles (14) are adsorbed at the bottom in the reaction tank (1); opening a water outlet valve (24) of the water outlet pipe (19) to enable the treated percolate to be discharged out of the reaction main body (1) through the water outlet pipe (19); closing the water outlet valve (24), and powering off the electromagnetic device (11) to complete a second percolate treatment period;
s3: the first percolate treatment period and the second percolate treatment period form an operation period together; and repeating the operation cycle to realize the sequencing batch treatment of the percolate.
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