Device and method for preparing plasma activating solution for catalyzing gas-liquid two-phase discharge

Abstract

The invention discloses a preparation device and method of a catalytic gas-liquid two-phase discharge plasma activation solution, and belongs to the technical field of plasma activated water preparation, the preparation device comprises a discharge reaction device, the discharge reaction device is mounted in a container, and a catalyst placement module is arranged in the discharge reaction device; the discharge reaction device comprises a quartz tube, and a high-voltage electrode is placed in the quartz tube through a fixed connecting device; a discharge channel is formed between the high-voltage electrode and the quartz tube; the center of the bottom end of the quartz tube is provided with a through jet orifice, and the periphery of the quartz tube is uniformly provided with multiple circles of air holes with the same size. A catalyst placing module capable of placing a catalyst is arranged at the bottom of the discharge reaction device, and the liquid level in a quartz tube is changed under the action of gas by utilizing gas holes and a jet orifice, so that the catalyst placing module is positioned at the gas holes at different heights of the quartz tube, participates in discharge and enriches a series of reactions generated in the discharge process; the reactant conversion rate, the product selectivity and the energy efficiency are effectively improved.

Description

Technical Field

[0001] The present invention belongs to the technical field of plasma-activated water preparation, and particularly relates to a device and method for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid. Background Art

[0002] The statements in this part only provide background technical information related to the present invention and do not necessarily constitute prior art.

[0003] Dielectric barrier discharge refers to the discharge with at least one insulating dielectric layer between two electrodes. The main discharge structures are flat plate type and coaxial type, and the dielectric materials generally use quartz glass, ceramics, etc.

[0004] The prior art discloses a DBD reaction device, including a coaxial DBD reactor and an activated water reaction container. The coaxial DBD reactor is provided with air holes around its body, which can shorten the propagation distance of the plasma generated by the discharge and make it flow into the water with low loss; the number of air holes is much larger than that of the traditional DBD reactor, increasing the diffusion path of active particles into the water, improving the diffusion efficiency and the gas-liquid exchange rate, and forming an oxidizing plasma-activated water.

[0005] In the above scheme, although an oxidizing plasma-activated water can be formed, there are still the following disadvantages: the reactant conversion rate, product selectivity and energy efficiency are still low, and the discharge area cannot be adjusted. Summary of the Invention

[0006] Aiming at the above problems, the present invention provides a device and method for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid. By setting a catalyst placement module that can place catalysts at the bottom of the discharge reaction device, and using air holes and jet ports, the liquid level in the quartz tube is changed under the action of gas, so that the catalyst placement module is located at the air holes at different heights of the quartz tube, participates in the discharge and enriches a series of reactions occurring during the discharge, provides more active sites and oxygen vacancies for the active particles generated by the discharge, effectively improves the reactant conversion rate, product selectivity and energy efficiency; by adjusting the height of the lifting partition, the isolation between the high-voltage electrode and the grounding grid is realized, and the discharge area can be adjusted.

[0007] To achieve the above object, the present invention adopts the following technical solutions:

[0008] In the first aspect, a device for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid is provided, including a discharge reaction device installed in a container, and a catalyst placement module is arranged inside the discharge reaction device; the discharge reaction device includes a quartz tube, and a fixed connection device is connected above the quartz tube, and a high-voltage electrode is placed inside the quartz tube through the fixed connection device; a discharge channel is formed between the high-voltage electrode and the quartz tube;

[0009] The quartz tube includes an upper cylindrical structure and a lower hemispherical structure. The inside of the quartz tube is hollow, with an open upper end and a closed bottom end. A through jet orifice is provided at the center of the bottom end of the quartz tube. At a set distance above the jet orifice, multiple circles of pores with the same size are evenly opened on the circumferential wall of the quartz tube;

[0010] The catalyst placement module adopts a variety of different three-dimensional shapes. The top of the catalyst placement module is treated with a mesh-like indentation or groove for evenly placing the catalyst on the top of the catalyst placement module.

[0011] Preferably, the fixed connection device includes a fixed block. The upper end of the fixed block is provided with a first external thread section, the lower end is provided with a second external thread section, and a first channel is arranged inside the fixed block; a second channel is arranged inside the first external thread section; a third channel is arranged inside the second external thread section.

[0012] Preferably, the first channel, the second channel, and the third channel are coaxially arranged. The diameter of the first channel is smaller than that of the second channel, and the diameter of the second channel is smaller than that of the third channel; the diameter of the first channel is equal to the diameter of the high-voltage electrode, and the diameter of the third channel is equal to the outer diameter of the quartz tube.

[0013] Preferably, an air intake hole is opened on the side of the fixed block. The second channel communicates with the outside through the air intake hole, and a third internal thread section is arranged inside the air intake hole; a third external thread section that cooperates with the third internal thread section is arranged on the outer wall of the air vent member, and a through gas injection channel is arranged inside, connecting the air vent member to the gas injection pipeline of the gas injection device to inject gas into the fixed block.

[0014] Preferably, the first external thread section is connected to a first nut, and a first internal thread section is arranged inside the first nut; the second external thread section is connected to a second nut, and two internal thread sections are arranged inside the second nut. The upper section is a second internal thread section, and the lower section is a fourth internal thread section.

[0015] Preferably, the diameter of the fourth internal thread section is smaller than that of the second internal thread section, and the thread directions of the fourth internal thread section and the second internal thread section are opposite; the diameter of the fourth internal thread section is larger than the diameter of the quartz tube; a first magnet ring is adhesively fixed to the bottom of the second nut.

[0016] Preferably, both the first external thread section or the second external thread section are designed with multiple evenly spaced slots, dividing the first external thread section or the second external thread section into evenly spaced multiple segments; when the first nut or the second nut is turned, it can squeeze the three segments of the first external thread section or the second external thread section to squeeze and fix the high-voltage electrode or the quartz tube therein.

[0017] Preferably, the container includes a container body, and an active lid is provided above the container body. An opening is provided at the center of the lid, with a size matching that of the outer quartz tube. A protruding threaded ring is provided outside the opening, and a fourth external thread section is provided outside the protruding threaded ring, which is connected to the fourth internal thread section.

[0018] Preferably, the part of the quartz tube located in the container is connected to a grounding device; the grounding device includes a grounding grid; the top of the grounding grid is connected to a second magnet ring, whose polarity is different from that of the first magnet ring and whose size is the same as that of the first magnet ring; it also includes a receiving tray, in which a lifting partition is slidably connected. The bottom of the lifting partition is rotatably connected to a lifting bolt, and the lifting bolt is threadedly connected to the receiving tray. The lifting partition is used to isolate the grounding grid from the quartz tube and adjust the discharge area.

[0019] In a second aspect, a method for preparing a novel catalytic gas-liquid two-phase discharge plasma-activated liquid is provided, which uses the above-mentioned preparation device for a catalytic gas-liquid two-phase discharge plasma-activated liquid. The specific steps are as follows:

[0020] Determine the type of catalyst and place the catalyst into the catalyst placement module; then place the catalyst placement module at the bottom inside the quartz tube; then connect the quartz tube and the high-voltage electrode through a fixed connection device and connect it to the lid; then install the grounding grid and the receiving tray outside the quartz tube;

[0021] Add water or an aqueous solution to the container, and install the discharge reaction device together with the lid on the container;

[0022] Open the gas cylinder and adjust the gas flow rate so that the liquid level inside the quartz tube is below a certain ring of air holes;

[0023] Stop blowing air, remove the lid and adjust the length of the lifting partition so that the lifting partition is below a certain ring of air holes determined above; reinstall the lid, and then blow air;

[0024] After that, connect the high-voltage power supply to the high-voltage electrode. The discharge is concentrated in the discharge channel in the overlapping area of the quartz tube and the grounding grid and spreads to the vicinity of the air holes, generating various oxidizing active particles, which then act on the water or the aqueous solution to be treated;

[0025] After the discharge is completed, turn off the high-voltage power supply, turn off the gas cylinder, and clean and dry the entire discharge reaction device, container, and catalyst placement module.

[0026] Compared with the prior art, the advantages and positive effects of the present invention are:

[0027] In the present invention, a catalyst placement module for placing a catalyst is provided at the bottom of the discharge reaction device. By using air holes and jet ports, the liquid level in the quartz tube is changed under the action of gas, so that the catalyst placement module is located at the air holes at different heights of the quartz tube, participates in the discharge and enriches a series of reactions occurring during the discharge process, provides more active sites and oxygen vacancies for the active particles generated by the discharge, and effectively improves the reactant conversion rate, product selectivity and energy efficiency; by adjusting the height of the lifting partition, the isolation between the high-voltage electrode and the grounding grid is achieved, and the discharge area can be adjusted. BRIEF DESCRIPTION OF THE DRAWINGS

[0028] The accompanying drawings forming a part of this specification are used to provide a further understanding of the present invention. The schematic embodiments of the present invention and their descriptions are used to explain the present invention and do not constitute an improper limitation of the present invention.

[0029] Figure 1 is a schematic diagram of the device of Embodiment 1 or 2 of the present invention;

[0030] Figure 2 is an assembly schematic diagram of the quartz tube, fixed connection device and high-voltage electrode of Embodiment 1 or 2 of the present invention;

[0031] Figure 3 is a schematic diagram of the quartz tube of Embodiment 1 or 2 of the present invention;

[0032] Figure 4 is a schematic diagram of the fixed connection device of Embodiment 1 or 2 of the present invention;

[0033] Figure 5 is a schematic diagram of the grounding device of Embodiment 1 or 2 of the present invention;

[0034] Figure 6 is a schematic diagram of the storage tray and the lifting partition of Embodiment 1 or 2 of the present invention;

[0035] Figure 7 is a schematic diagram of the storage tray and the fixing bolt of Embodiment 1 or 2 of the present invention;

[0036] Figure 8 is a schematic diagram of the container of Embodiment 1 or 2 of the present invention;

[0037] Figure 9 is a schematic diagram of the lid of Embodiment 1 or 2 of the present invention;

[0038] Figure 10 is a schematic diagram of the catalyst placement modules of various shapes of Embodiment 1 or 2 of the present invention;

[0039] In the figure:

[0040] 1. Discharge reaction device; 11. High voltage electrode; 12. Quartz tube; 121. Air hole; 122. Jet port; 13. Fixed connection device; 131. First nut; 132. Fixed block; 133. Ventilator; 134. First sealing rubber ring; 135. Second sealing rubber ring; 136. Second nut; 137. First magnet ring; 14. Grounding device; 141. Grounding grid; 142. Second magnet ring; 143. Fixing bolt; 144. Lifting partition; 145. Lifting bolt; 146. Storage tray; 1461. Accommodating port; 1462. Groove; 2. Container; 21. Protruding threaded ring; 22. Cover; 3. Catalyst placement module; 31. Catalyst. DETAILED DESCRIPTION

[0041] It should be noted that the following detailed descriptions are illustrative and intended to provide further explanation of the present invention. Unless otherwise specified, all technical and scientific terms used herein have the same meanings as those commonly understood by those skilled in the art to which the present invention belongs.

[0042] The present invention is described in detail below in conjunction with the accompanying drawings.

[0043] Example 1

[0044] This embodiment discloses a device for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid, such as Figure 1 As shown, it includes a discharge reaction device 1 and a container 2. The discharge reaction device 1 is installed in the container 2, and a catalyst placement module 3 is arranged inside the discharge reaction device 1.

[0045] like Figure 2 As shown, the discharge reaction device 1 includes a quartz tube 12, the top of the quartz tube 12 is open, the top of the quartz tube 12 is connected to a fixed connection device 13, and the part of the quartz tube 12 located in the container 2 is connected to a grounding device 14; the high-voltage electrode 11 is placed inside the quartz tube 12 through the fixed connection device 13, as a single-layer dielectric barrier discharge form of a bare electrode, and a discharge channel is formed between the high-voltage electrode and the quartz tube; in this embodiment, the high-voltage electrode and the quartz tube are kept at a distance of 5 mm on both sides. The discharge reaction device 1 can also be placed in the container 2 as a whole through the fixed connection device 13.

[0046] like Figure 2 , Figure 8 As shown, inside the discharge reaction device 1, between the quartz tube 12 and the high voltage electrode 11, and below the air holes 121 of the quartz tube 12, a plurality of catalyst placement modules 3 for placing catalysts 31 are arranged.

[0047] like Figure 3As shown, the quartz tube 12 includes an upper cylindrical structure and a hemispherical structure at the bottom. The inside of the quartz tube 12 is hollow, with an open upper end and a closed bottom end. At the center position of the bottom end of the quartz tube 12, a structure with a through jet orifice 122 is provided. When the quartz tube 12 is placed in the container 2, the jet orifice 122 can act as a communicating vessel.

[0048] At a set distance above the jet orifice 122, on the circumference of the quartz tube 12, multiple circles of pores 121 with the same size are evenly arranged. Preferably, the number of circles of pores 121 is one to five circles. In this embodiment, as Figure 3 shown, three circles of pores 121 are provided.

[0049] It should be noted that, in this embodiment, to make full use of the pores 121, the distance of the bottommost circle of pores is appropriately raised, so that the distance between the lowest circle of pores 121 and the set distance above the jet orifice 122 is 30 - 40 mm, the interval distance between each circle of pores 121 is 10 - 15 mm, and the diameter of the pores 121 is 0.1 - 1.0 mm; this is used to achieve different discharge effects and can generate relatively stable plasma during discharge.

[0050] It should be noted that when the catalyst is close to a certain circle of pores, the discharge effect is the best; and as much as possible, the catalyst is made close to the bottommost pores, so that the plasma discharged from the bottom can have a longer action time during the rising process from the bottom to the top of the liquid phase after entering the liquid phase.

[0051] When water or an aqueous solution is added to the container 2, through the jet orifice 122 and the pores 121, the liquid levels inside the container 2 and the quartz tube 12 are flush; it should be noted that, below the pores 121 close to the quartz tube 12, a plurality of catalyst placement modules 3 for placing the catalyst are provided, and they float on the liquid surface under the buoyancy of water or the aqueous solution.

[0052] As Figure 4 shown, the fixed connection device 13 includes a fixing block 132. The upper end of the fixing block 132 is provided with a first external thread section, the lower end is provided with a second external thread section, and the inside of the fixing block 132 is provided with a hollow and through first channel; the inside of the first external thread section is provided with a hollow and through second channel; the inside of the second external thread section is provided with a hollow and through third channel. Among them, the diameter of the first channel is smaller than that of the second channel, and the diameter of the second channel is smaller than that of the third channel. The first channel, the second channel, and the third channel are coaxially arranged.

[0053] As Figure 4As shown in the figure, an air intake hole is formed on the side surface of the fixed block 132. The second channel inside the fixed block 132 is connected to the outside through the air intake hole, and a third internal thread section is provided in the air intake hole; the third internal thread section in the air intake hole is connected to the air vent member 133. A third external thread section is provided on the outer wall of the air vent member 133, and a through air injection channel is provided inside the air vent member 133. Connecting the air vent member 133 to the air injection pipeline of the air injection device can inject air into the fixed block 132.

[0054] In this embodiment, the air injection device can adopt a gas cylinder and a gas flow meter; the gas cylinder, the gas flow meter and the air vent member 133 are connected through an air injection pipeline, and the gas flow meter is used to control the gas flow rate.

[0055] As Figure 4 shown in the figure, a first nut 131 is connected above the fixed block 132. A first internal thread section is provided inside the first nut 131 for threaded connection with the first external thread section; a second nut 136 is connected below the fixed block 132. Two internal thread sections are provided inside the second nut 136. The upper section is the second internal thread section for threaded connection with the second external thread section; the lower section is the fourth internal thread section for connection with the container 2. The diameter of the fourth internal thread section is smaller than the diameter of the second internal thread section, and the thread direction of the fourth internal thread section is opposite to that of the second internal thread section; the diameter of the fourth internal thread section is larger than the outer wall diameter (i.e., the outer diameter) of the upper cylindrical body of the quartz tube 12.

[0056] Furthermore, a first magnet ring 137 is adhesively fixed to the bottom of the second nut 136.

[0057] It should be noted that both the first external thread section and the second external thread section are designed with multiple circumferential evenly spaced grooves. In this embodiment, the first external thread section or the second external thread section is evenly provided with three sub-grooves in the circumferential direction, dividing the first external thread section or the second external thread section into three equal sections; when the first nut or the second nut is turned, it can squeeze the three segments of the first external thread section or the second external thread section to squeeze and fix the high-voltage electrode or the quartz tube therein.

[0058] It should also be noted that the high-voltage electrode 11 is a cylinder, and the diameter of the high-voltage electrode 11 is equal to the diameter of the first channel; the upper part of the quartz tube 12 is also a cylinder, and the outer wall diameter of the upper part of the quartz tube 12 is equal to the diameter of the third channel.

[0059] As Figure 4 shown in the figure, the fixed connection device 13 further includes a first sealing rubber ring 134 and a second sealing rubber ring 135. Among them, the first sealing rubber ring 134 is arranged in the third channel; the second sealing rubber ring 135 is arranged outside the second external thread section.

[0060] As Figure 4As shown in the figure, during installation, first place the first sealing rubber ring 134 into the third channel, position the first sealing rubber ring 134 at the top of the third channel close to the second channel, then insert the upper part of the quartz tube 12 into the third channel of the second external thread section, so that the upper part of the quartz tube 12 abuts against the first sealing rubber ring 134. Then place the second sealing rubber ring 135 outside the second external thread section and at the top of the second external thread section close to the second channel. Finally, connect the upper second internal thread section inside the second nut 136 to the second external thread section. By screwing the second nut 136 to squeeze the second external thread section, the second external thread section squeezes the upper part of the quartz tube 12 to complete the connection.

[0061] After the quartz tube 12 completes the connection with the fixed connection device 13, pass the high-voltage electrode 11 through the first channel and the second channel until it reaches the length setting inside the quartz tube 12 (for example, below the bottommost row of air holes), and then thread the first nut 131 onto the first external thread section. By screwing the first nut 131 to squeeze the first external thread section, the first external thread section squeezes the high-voltage electrode 11 to complete the connection.

[0062] As Figure 4 shown, after completing the connection of the high-voltage electrode 11, the quartz tube 12, and the fixed connection device 13, the high-voltage electrode 11 seals the first channel, the quartz tube 12 seals the third channel, and the second channel communicates with the quartz tube 12, actually forming a gas channel; inject gas into the fixed block 132 through the air vent 133, and the gas flows into the quartz tube 12 through the second channel.

[0063] It can be understood that the first sealing rubber ring 134 and the second sealing rubber ring 135 play a role in enhancing the seal; at the threaded section connections mentioned above, it is also possible to wrap a layer of raw tape around each and then connect and fix them, which can further improve the airtightness of the connections.

[0064] Furthermore, a sealing rubber ring of corresponding size can also be added at the connection between the first nut and the first external thread section to further improve the airtightness of the device and reduce the influence caused by possible mixing of other gases during the discharge of a single gas type.

[0065] It should be noted that the first nut 131, the fixed block 132, the second nut 136, and the air vent 133 are all made of polytetrafluoroethylene material, which has good insulation and corrosion resistance; the first sealing rubber ring 134 and the second sealing rubber ring 135 are made of nitrile rubber material to improve the airtightness of the fixed connection device 13.

[0066] As Figure 1 、 Figure 8 、 Figure 9As shown, the container 2 includes a container body, and an active lid 22 is provided above the container body. An opening is provided at the central position of the lid 22, and the size is matched with the outer layer of the quartz tube 12 (outer wall outer diameter). A protruding threaded ring 21 is provided outside the opening, and a fourth external thread section is provided outside the protruding threaded ring 21, which is used to connect with the fourth internal thread section at the inner bottom of the second nut 136 of the fixed connection device 13, so as to realize the assembly of the discharge reaction device 1 and the lid 22 of the container 2.

[0067] In this embodiment, the container 2 is made of acrylic material.

[0068] As Figure 1 , Figure 5 As shown, the grounding form of the discharge reaction device 1 is to select a part of the quartz tube 12 located in the container 2 and connect the grounding device 14. Specifically, inside the container 2, the grounding device 14 includes a grounding net 141 made of a layer of stainless steel material wrapped around the quartz tube 12; the middle of the grounding net 141 is a hollow cylinder, and the diameter of the cylinder is larger than the outer wall diameter of the quartz tube 12. One of the functions is to accommodate the quartz tube 12; the second function is to set a lifting partition 144 between the quartz tube 12 and the grounding net 141. The length of the grounding net 141 is equal to the distance between the bottom of the lid 22 and the bottommost air hole. The lifting partition 144 is made of polytetrafluoroethylene material.

[0069] The bare electrode discharge of the single-layer medium is more inclined to the discharge form of the gas-liquid two-phase combination. The grounding net covering the air holes can help the plasma to be led out from the air holes.

[0070] As Figure 5 As shown, the top of the grounding net 141 is connected to the second magnet ring 142, whose polarity is different from that of the first magnet ring 137 at the bottom of the second nut 136, and its size is the same as that of the first magnet ring 137; through the principle of the opposite-sex attraction of the first magnet ring 137 and the second magnet ring 142, the top of the grounding net 141 is connected to the lid 22, so as to cover the part of the quartz tube 12 in the container 2 inside the grounding net 141, which is convenient for connection.

[0071] As described above: make the catalyst as close as possible to the bottommost air hole, so that the plasma discharged from the bottom can have a longer action time during the rising process from the bottom to the top of the liquid phase after entering the liquid phase. Therefore, in theory, it is hoped that each circle of air holes can be utilized.

[0072] However, in actual application, the flow rate of the working gas may not be large enough to discharge the gas from the bottom pores. At this time, some of the pores at the bottom are covered by liquid, so the plasma cannot be discharged. However, under the action of the grounding grid, the high-voltage electrode itself will have a slight power discharge in the water, which will affect the discharge stability of the device and cause temperature rise. It may also aggravate the decomposition process of some active particles generated in the liquid phase, which needs to be avoided.

[0073] Therefore, it is necessary to reduce the scope of the grounding grid so that it can be kept as above the pores covered by the liquid as possible.

[0074] like Figure 5 , Figure 6 , Figure 7 As shown, the lifting baffle 144 is a hollow cylinder, whose inner radius is larger than the radius of the upper cylinder of the quartz tube 12 but smaller than the radius of the grounding grid 141 , so that the lifting baffle 144 can be arranged between the quartz tube 12 and the grounding grid 141 .

[0075] Among them, the lifting partition 144 is slidably set in the storage tray 146; a through accommodating port 1461 is opened in the middle of the storage tray 146, and the diameter of the accommodating port is equal to the diameter of the upper cylinder of the quartz tube 12 (the diameter of the outer wall of the upper cylinder), and the bottom of the quartz tube 12 is inserted into the accommodating port until the top surface of the storage tray 146 is located below the air holes on the bottom surface of the grounding grid 141, and the two are limited by friction.

[0076] An annular groove 1462 is provided outside the center of the storage tray 146 and outside the receiving opening of the storage tray 146. The groove does not penetrate the top and bottom surfaces of the storage tray 146, and the lifting partition 144 is slidably arranged inside the groove. It can be understood that the inner wall diameter of the groove is smaller than the diameter of the lifting partition 144, and the outer wall diameter of the groove is larger than the diameter of the lifting partition 144.

[0077] Two lifting bolts 145 are symmetrically arranged at the bottom of the lifting partition 144, and the bottom of the lifting partition 144 is connected to the lifting bolts 145 via a rotating bearing; Figure 7 As shown, the lifting bolt 145 is threadedly connected to the storage tray 146, and the lifting bolt 145 passes through the bottom of the storage tray 146 and is rotationally connected to the bottom of the lifting partition 144 through a rotating bearing.

[0078] It is understandable that by screwing the two lifting bolts 145, the lifting bolts 145 are moved into the storage tray 146, driving the lifting partition 144 to move upward, and can be set between the grounding grid 141 and the quartz tube 12. The height of the lifting partition 144 is adjusted by the lifting bolts 145. The lifting partition 144 is between the quartz tube and the grounding grid to achieve isolation between the high-voltage electrode and the grounding grid, so that the discharge area can be selected, that is, the discharge area can be adjusted.

[0079] In addition, fixing bolt holes can be provided on the side of the storage tray 146 below the groove. The fixing bolt holes are threadedly connected to the fixing bolts 143. The fixing bolt holes communicate with the outside of the storage tray 146 and the accommodating opening, and the extension line of the fixing bolt holes passes through the center of the storage tray 146. Tightening the fixing bolts 143 to contact the quartz tube 12 can strengthen the connection between the storage tray 146 and the quartz tube.

[0080] In this embodiment, the magnetic attraction structure and the design of adjusting the lifting partition can facilitate the installation, disassembly and length adjustment of the grounding grid, so as to facilitate the regulation of the discharge area.

[0081] As Figure 10 shown, the catalyst placement module 3 can adopt a variety of different three-dimensional shapes, such as a cube, a cuboid, a cylinder, a toroid; however, mesh marks or groove treatments need to be made on the top of the catalyst placement module 3, so that the catalyst 31 can be evenly placed on the mesh marks or grooves on the top of the catalyst placement module 3.

[0082] In this embodiment, the catalyst placement module 3 is also made of polytetrafluoroethylene or polyvinyl chloride; the catalyst placement module 3 can float on the liquid inside the container 2 by relying on buoyancy. The catalyst is mainly distributed near the air holes or above the air holes of the quartz tube where the gas-liquid phase contacts through the catalyst placement module 3, and the working position of the catalyst is adjusted by the blowing of the gas and the self-buoyancy of the catalyst placement module 3.

[0083] When the gas is blown in through the venting member 133, under the continuous blowing of the gas, the aqueous solution in the original discharge channel (i.e., between the quartz tube 12 and the high-voltage electrode) is squeezed downward, and finally the water or aqueous solution in the discharge channel drops below a certain circle of air hole positions; the specific height of the liquid level in the quartz tube 12 is related to the flow rate of the gas. Different gas flow rates can realize the adjustment of the liquid level height in the quartz tube 12. By reasonably selecting the size of the catalyst placement module, under the action of its own buoyancy, the catalyst can be suspended above the liquid level to achieve the promotion effect on discharge.

[0084] It should be noted that in this embodiment, even if the catalyst may dissolve in the liquid phase under the action of the gas, it will also form a suspension to play a role. After the reaction is completed, after filtration and separation, it can still be used continuously.

[0085] The catalyst acts during the discharge process. The processes of adsorption and bonding enrich a series of reactions occurring during the discharge process. At the same time, the presence of the catalyst can provide more active sites and oxygen vacancies for the active particles generated by the discharge, and the formed electron-hole pairs further enhance the photocatalysis process. Therefore, filling the device with the catalyst can effectively improve the reactant conversion rate, product selectivity, and energy efficiency.

[0086] The floating range of the catalyst placement module can be appropriately adjusted by different gas flow rates and its own size.

[0087] In this embodiment, the types of catalysts selected are mostly nanoscale foam metals or oxide support-metal materials, which have small sizes and good effects, and a wide range of adaptability.

[0088] In this embodiment, the bottom surface and the periphery of the bottom surface of the cylindrical high-voltage electrode 11 are polished, and it is customized from stainless steel material and directly connected to the high-voltage output terminal of the high-voltage power supply during discharge.

[0089] Specifically, the high-voltage electrode 11 is connected to the high-voltage output terminal of a high-voltage AC source or a pulsed power supply. After the power is turned on, obvious discharge phenomena can be observed in the discharge channel of the part of the grounding grid 141 covered by the quartz tube 12, and at the same time, the discharge effect of the gas-liquid two-phase can be observed at the air holes 121.

[0090] In this embodiment, the gas is selected from one or more of argon, helium, nitrogen, and air.

[0091] Example 2

[0092] A method for preparing a catalytic gas-liquid two-phase discharge plasma activation solution disclosed in this embodiment uses a device for preparing a catalytic gas-liquid two-phase discharge plasma activation solution disclosed in Example 1. The specific steps are as follows:

[0093] Before use, first determine the type of the catalyst and place the catalyst in the catalyst placement module 3; and place the catalyst placement module 3 at the bottom inside the quartz tube 12; select a catalyst placement module 3 with a suitable size or shape to make the catalyst concentrated on the liquid surface at the air holes 121, which has a promoting effect on the discharge.

[0094] Secondly, connect the quartz tube 12 and the high-voltage electrode 11 through the fixed connection device 13; form a bare electrode dielectric barrier discharge structure with a single-layer dielectric; pass the bottom of the quartz tube 12 through the lid 22 of the container 2 and connect it to the protruding threaded ring 21 of the lid 22 through the fixed connection device 13.

[0095] Then, the grounding grid 141 is installed outside the quartz tube 12, and at the same time, the receiving tray 146 is installed below the bottom air hole of the quartz tube 12. Then, the bottom of the quartz tube 12 is fixed to the receiving tray 146 through the fixing bolts 143;

[0096] Water or an aqueous solution is added to the container 2 to prepare for the discharge treatment process. After that, the assembled discharge reaction device 1, together with the lid 22, is installed on the container 2. At this time, due to the action of the jet port 122 at the bottom end of the quartz tube 12, the liquid level in the quartz tube 12 is basically flush with the liquid level of the water or aqueous solution in the container 2. The catalyst placement module 3 also floats on the liquid surface under the action of its own buoyancy;

[0097] The gas cylinder is opened, and the gas is introduced into the discharge reaction device 1 through the vent member 133. The gas fills the discharge channel and is blown out from the air holes 121 of the outer quartz tube 12. By adjusting the gas flow rate, the liquid level height in the quartz tube 12 will change to a certain extent; the liquid level in the quartz tube 12 will be below a certain circle of air holes 121; the catalyst placement module 3 floats on the liquid surface in the quartz tube 12; thus, the utilization of the air holes 121 at different heights of the quartz tube 12 can be realized;

[0098] Stop blowing, remove the lid 22, adjust the length of the lifting partition 144 so that the lifting partition 144 is below a certain circle of air holes 121 determined above; reinstall the lid 22, and then blow;

[0099] After that, the high-voltage lead-out wire of the high-voltage power supply is connected to the high-voltage electrode 11 of the discharge reaction device 1. After the high-voltage power supply is turned on, the discharge is concentrated in the discharge channel in the overlapping area of the quartz tube 12 and the grounding grid 141 and spreads to the vicinity of the air holes 121. A large amount of plasma generated by the discharge acts on the water or aqueous solution in the form of bubbles and discharge jets, generating various oxidizing active particles, and then acting on the water or the aqueous solution to be treated, realizing the preparation of plasma-activated water or the treatment of the solution;

[0100] After the discharge is completed, turn off the high-voltage power supply and cut off the gas supply to complete the process of preparing plasma-activated water or treating the aqueous solution in this discharge;

[0101] Clean and dry the entire set of discharge reaction device 1, container 2, and catalyst placement module 3 for the next use.

[0102] Although the specific embodiments of the present invention are described above in conjunction with the accompanying drawings, it is not a limitation to the protection scope of the present invention. Those skilled in the art should understand that based on the technical solutions of the present invention, various modifications or deformations that can be made by those skilled in the art without creative efforts are still within the protection scope of the present invention.

Claims

1. A device for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid, characterized in that: The invention comprises a discharge reaction device, which is installed in a container, and a catalyst placement module is arranged inside the discharge reaction device; the discharge reaction device comprises a quartz tube, and a fixed connection device is connected above the quartz tube, and a high-voltage electrode is placed inside the quartz tube through the fixed connection device; a discharge channel is formed between the high-voltage electrode and the quartz tube; The quartz tube includes an upper cylindrical structure and a lower hemispherical structure. The interior of the quartz tube is hollow, the upper end is open, and the bottom end is closed. A through jet port is arranged at the center of the bottom end of the quartz tube. At a set distance above the jet port, multiple circles of air holes of the same size are evenly arranged around the quartz tube. The catalyst placement module adopts a variety of different three-dimensional shapes, and the top of the catalyst placement module is processed with mesh notches or grooves to evenly place the catalyst on the top of the catalyst placement module.

2. The device for preparing a catalytic gas-liquid two-phase discharge plasma activation solution according to claim 1, characterized in that: The fixed connection device includes a fixed block, a first external thread segment is arranged at the upper end of the fixed block, a second external thread segment is arranged at the lower end, a first channel is arranged inside the fixed block; a second channel is arranged inside the first external thread segment; and a third channel is arranged inside the second external thread segment.

3. The device for preparing a catalytic gas-liquid two-phase discharge plasma activation solution according to claim 2, characterized in that: The first channel, the second channel and the third channel are coaxially arranged, the diameter of the first channel is smaller than the diameter of the second channel, and the diameter of the second channel is smaller than the diameter of the third channel; the diameter of the first channel is equal to the diameter of the high voltage electrode, and the diameter of the third channel is equal to the outer wall diameter of the quartz tube.

4. The device for preparing a catalytic gas-liquid two-phase discharge plasma activation solution according to claim 2, characterized in that: An air connection hole is provided on the side of the fixed block, and the second channel is connected to the outside through the air connection hole, and a third internal thread section is arranged in the air connection hole; a third external thread section used in conjunction with the third internal thread section is arranged on the outer wall of the ventilator, and a through air injection channel is arranged inside, and the ventilator is connected to the air injection pipeline of the air injection device to inject air into the fixed block.

5. The device for preparing a catalytic gas-liquid two-phase discharge plasma activation solution according to claim 2, characterized in that: The first external thread section is connected to the first nut, and the first internal thread section is arranged inside the first nut; the second external thread section is connected to the second nut, and two internal thread sections are arranged inside the second nut, the upper section is the second internal thread section, and the lower section is the fourth internal thread section.

6. The device for preparing a catalytic gas-liquid two-phase discharge plasma activation solution according to claim 5, characterized in that: The diameter of the fourth internal thread segment is smaller than that of the second internal thread segment, and the thread directions of the fourth internal thread segment and the second internal thread segment are opposite; the diameter of the fourth internal thread segment is larger than the diameter of the quartz tube; and a first magnet ring is bonded and fixed to the bottom of the second nut.

7. The device for preparing a catalytic gas-liquid two-phase discharge plasma activation solution according to claim 5, characterized in that: The first external thread segment or the second external thread segment is designed with multiple uniform grooves, dividing the first external thread segment or the second external thread segment into multiple uniform segments; when the first nut or the second nut is screwed, the three segments of the first external thread segment or the second external thread segment can be squeezed to fix the high-voltage electrode or quartz tube therein.

8. The device for preparing a catalytic gas-liquid two-phase discharge plasma activation solution according to claim 5, characterized in that: The container includes a container body, a movable cover is arranged above the container body, a hole is opened at the center of the cover, the size of which matches the outer quartz tube, a protruding thread ring is arranged outside the opening, and a fourth external thread segment is arranged outside the protruding thread ring and connected to the fourth internal thread segment.

9. The device for preparing a catalytic gas-liquid two-phase discharge plasma activation solution according to claim 6, characterized in that: The part of the quartz tube located in the container is connected to a grounding device; the grounding device includes a grounding grid; the top of the grounding grid is connected to a second magnet ring, whose polarity is different from that of the first magnet ring and whose size is consistent with that of the first magnet ring; it also includes a storage tray, in which a lifting partition is slidably connected, and the bottom of the lifting partition is rotatably connected to a lifting bolt, and the lifting bolt is threadedly connected to the storage tray, and the lifting partition is used to isolate the grounding grid and the quartz tube and adjust the discharge area.

10. A method for preparing a catalytic gas-liquid two-phase discharge plasma activation solution, characterized in that: A novel preparation device for catalytic gas-liquid two-phase discharge plasma activation liquid as described in any one of claims 1 to 9 is used, and the specific steps are as follows: Determine the type of catalyst and place the catalyst in the catalyst placement module; then place the catalyst placement module at the bottom of the quartz tube; then connect the quartz tube and the high-voltage electrode through a fixed connection device and connect it to the cover; then install the grounding grid and the storage tray on the outside of the quartz tube; Add water or an aqueous solution into the container, and install the discharge reaction device together with the cover on the container; Open the gas cylinder and adjust the gas flow rate so that the liquid level in the quartz tube is below a certain circle of air holes; Stop blowing, remove the cover and adjust the length of the lifting partition so that the lifting partition is located below a circle of air holes determined above; install the cover again and then blow; Then, the high voltage power supply is connected to the high voltage electrode, and the discharge is concentrated in the discharge channel in the overlapping area of ​​the quartz tube and the grounding grid and spreads to the vicinity of the pores, generating various active oxidizing particles, which then act on the water or the aqueous solution to be treated; After the discharge is completed, turn off the high-voltage power supply, shut off the gas cylinder, and clean and dry the entire discharge reaction device, container and catalyst placement module.

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