An apparatus and method for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid.

Abstract

This invention discloses a device and method for preparing catalytic gas-liquid two-phase discharge plasma activation liquid, belonging to the field of plasma-activated water preparation technology. It includes a discharge reaction device installed in a container, with a catalyst placement module inside. The discharge reaction device includes a quartz tube, with a high-voltage electrode placed inside via a fixed connection device. A discharge channel is formed between the high-voltage electrode and the quartz tube. A through-hole jet is located at the center of the bottom of the quartz tube, and multiple rings of identical-sized pores are evenly distributed around its perimeter. By setting a catalyst placement module at the bottom of the discharge reaction device, the liquid level inside the quartz tube is changed under the action of gas through the pores and jet, allowing the catalyst placement module to be positioned at pores at different heights within the quartz tube. This catalyst participates in the discharge and enriches the series of reactions occurring during the discharge process, effectively improving reactant conversion rate, product selectivity, and energy efficiency.

Description

Technical Field

[0001] This invention belongs to the field of plasma-activated water preparation technology, specifically relating to an apparatus and method for preparing catalytic gas-liquid two-phase discharge plasma activated liquid. Background Technology

[0002] The statements in this section are merely background information related to the present invention and do not necessarily constitute prior art.

[0003] Dielectric barrier discharge refers to discharge between two electrodes with at least one insulating dielectric layer. The main discharge structures are planar and coaxial, and the dielectric material is generally quartz glass or ceramic.

[0004] The prior art discloses a DBD reaction device, including a coaxial DBD reactor and an activated water reaction vessel. The coaxial DBD reactor has pores around its periphery, which can shorten the propagation distance of the plasma generated by the discharge and allow it to be introduced into the water with low loss. The number of pores is much greater than that of a conventional DBD reactor, which increases the diffusion path of active particles into the water, improves the diffusion efficiency and gas-liquid exchange rate, and forms plasma-activated water with oxidizing properties.

[0005] Although the above scheme can form plasma-activated water with oxidizing properties, it still has the following drawbacks: the reactant conversion rate, product selectivity and energy efficiency are still low, and the discharge region cannot be adjusted. Summary of the Invention

[0006] To address the aforementioned problems, this invention provides an apparatus and method for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid. By setting a catalyst placement module at the bottom of the discharge reaction device, and utilizing pores and jet nozzles to change the liquid level inside the quartz tube under the action of gas, the catalyst placement module is positioned at different heights of the pores in the quartz tube. This allows the catalyst to participate in the discharge and enrich a series of reactions occurring during the discharge process, providing more active sites and oxygen vacancies for the active particles generated by the discharge, effectively improving reactant conversion rate, product selectivity, and energy efficiency. Furthermore, by adjusting the height of the lifting baffle, isolation between the high-voltage electrode and the grounding grid is achieved, enabling adjustment of the discharge area.

[0007] To achieve the above objectives, the present invention adopts the following technical solution:

[0008] In a first aspect, an apparatus 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 disposed inside the discharge reaction device; the discharge reaction device includes a quartz tube, and a fixing connection device is connected to the top of the quartz tube, through which a high-voltage electrode is placed inside the quartz tube; a discharge channel is formed between the high-voltage electrode and the quartz tube.

[0009] The quartz tube consists of an upper cylindrical structure and a lower hemispherical structure. The inside of the quartz tube is hollow, with an open top and a closed bottom. A through jet port is set at the center of the bottom of the quartz tube. At a set distance above the jet port, multiple rings of air holes of the same size are evenly opened around 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 mesh-like grooves or grooves to evenly place the catalyst on the top of the catalyst placement module.

[0011] Preferably, the fixed connection device includes a fixed block, with a first external thread section at the upper end and a second external thread section at the lower end, and a first channel inside the fixed block; a second channel inside the first external thread section; and a third channel 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 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 diameter of the outer wall of the quartz tube.

[0013] Preferably, an air inlet hole is provided on the side of the fixed block, and the second channel is connected to the outside through the air inlet hole. A third internal thread section is provided inside the air inlet hole. A third external thread section is provided on the outer wall of the venting component to cooperate with the third internal thread section. An air injection channel is provided inside the venting component to connect to the air injection pipe of the air injection device to inject air into the fixed block.

[0014] Preferably, the first external thread segment is connected to the first nut, and the first nut has a first internal thread segment on its inner side; the second external thread segment is connected to the second nut, and the second nut has two internal thread segments on its inner side, the upper segment being the second internal thread segment and the lower segment being the fourth internal thread segment.

[0015] Preferably, the diameter of the fourth internal thread segment is smaller than the diameter of the second internal thread segment, and the thread direction of the fourth internal thread segment is opposite to that of the second internal thread segment; 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.

[0016] Preferably, the first external thread segment or the second external thread segment is designed with multiple uniformly slotted sections, dividing the first external thread segment or the second external thread segment into multiple uniform sections; when the first nut or the second nut is tightened, it can compress the three sections of the first external thread segment or the second external thread segment to compress and fix the high voltage electrode or quartz tube therein.

[0017] Preferably, the container includes a container body, a movable lid is provided on the top of the container body, the lid has an opening at the center, the size of which matches the outer quartz tube, a protruding threaded ring is provided on the outside of the opening, and a fourth external thread segment is provided on the outside of the protruding threaded ring, which is connected to a fourth internal thread segment.

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

[0019] Secondly, a novel method for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid is provided, which utilizes the aforementioned apparatus for preparing such a liquid. The specific steps are as follows:

[0020] Determine the type of catalyst and place it in the catalyst placement module; then place the catalyst placement module at the bottom of the quartz tube; next, connect the quartz tube and the high-voltage electrode through the fixing connection device and connect it to the cover; then install the grounding grid and storage tray on the outside of the quartz tube.

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

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

[0023] Stop blowing air, remove the cover and adjust the length of the lifting baffle so that the lifting baffle is below the aforementioned air hole ring; reinstall the cover and then blow air again;

[0024] Then, the high-voltage power supply is connected to the high-voltage electrode. The discharge is concentrated in the discharge channel in the area where the quartz tube and the grounding grid overlap and spreads to the vicinity of the pores, generating various active particles with oxidizing properties, which then act on the water or the aqueous solution to be treated.

[0025] After the discharge is complete, 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.

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

[0027] This invention utilizes a catalyst placement module at the bottom of a discharge reaction device. By employing pores and jet nozzles to alter the liquid level within a quartz tube under the influence of gas, the catalyst placement module is positioned at different heights within the pores of the quartz tube. This allows the catalyst to participate in the discharge process and enrich the series of reactions that occur during discharge. It provides more active sites and oxygen vacancies for the active particles generated during discharge, effectively improving reactant conversion rate, product selectivity, and energy efficiency. Furthermore, by adjusting the height of the lifting baffle, isolation between the high-voltage electrode and the grounding grid is achieved, enabling adjustment of the discharge area. Attached Figure Description

[0028] The accompanying drawings, which form part of this invention, are used to provide a further understanding of the invention. The illustrative embodiments of the invention and their descriptions are used to explain the invention and do not constitute an improper limitation of the invention.

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

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

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

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

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

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

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

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

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

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

[0039] In the picture:

[0040] 1. Discharge reaction device; 11. High voltage electrode; 12. Quartz tube; 121. Vent; 122. Jet nozzle; 13. Fixed connection device; 131. First nut; 132. Fixing block; 133. Ventilation component; 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. Receiving opening; 1462. Groove; 2. Container; 21. Protruding threaded ring; 22. Lid; 3. Catalyst placement module; 31. Catalyst. Detailed Implementation

[0041] It should be noted that the following detailed description is illustrative and intended to provide further explanation of the invention. Unless otherwise specified, all technical and scientific terms used herein have the same meaning as commonly understood by one of ordinary skill in the art to which this invention pertains.

[0042] The present invention will now be described in detail with reference to 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 set inside the discharge reaction device 1.

[0045] like Figure 2 As shown, the discharge reaction device 1 includes a quartz tube 12 with an opening at the top. A fixing connection device 13 is connected to the top of the quartz tube 12, and a grounding device 14 is connected to the portion of the quartz tube 12 located in the container 2. A high-voltage electrode 11 is placed inside the quartz tube 12 via the fixing connection device 13, forming a discharge channel between the high-voltage electrode and the quartz tube as a single-layer dielectric barrier discharge. In this embodiment, the high-voltage electrode and the quartz tube are maintained at a distance of 5 mm on both sides. The fixing connection device 13 also allows the entire discharge reaction device 1 to be placed inside the container 2.

[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, below the vent 121 of the quartz tube 12, there are multiple catalyst placement modules 3 for placing the catalyst 31.

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

[0048] At a predetermined distance above the jet outlet 122, multiple concentric rings of identical air holes 121 are evenly formed around the periphery of the quartz tube 12. Preferably, the number of rings of air holes 121 is one to five. In this embodiment, as... Figure 3 As shown, three rings of air holes 121 are provided.

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

[0050] It should be noted that the discharge effect is best when the catalyst is close to the ring of pores; and by placing the catalyst as close as possible to the bottom pores, the plasma discharged from the bottom can have a longer action time during its ascent from the bottom to the top of the liquid phase after entering the liquid phase.

[0051] When water or aqueous solution is added to container 2, the liquid level inside container 2 and quartz tube 12 is leveled through jet port 122 and vent 121. It should be noted that below the vent 121 near quartz tube 12, multiple catalyst placement modules 3 for placing catalysts are set up and float on the liquid surface under the buoyancy of water or aqueous solution.

[0052] like Figure 4 As shown, the fixed connection device 13 includes a fixing block 132. The upper end of the fixing block 132 has a first external thread section, and the lower end has a second external thread section. The fixing block 132 has a hollow, through-hole first channel inside; the first external thread section has a hollow, through-hole second channel inside; and the second external thread section has a hollow, through-hole third channel inside. 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 first, second, and third channels are coaxially arranged.

[0053] like Figure 4As shown, an air inlet is provided on the side of the fixing block 132. The second channel inside the fixing block 132 is connected to the outside through the air inlet. A third internal thread section is provided inside the air inlet. The third internal thread section inside the air inlet is connected to the air vent 133. A third external thread section is provided on the outer wall of the air vent 133. A through air injection channel is provided inside the air vent 133. The air vent 133 is connected to the air injection pipeline of the air injection device, which can inject air into the fixing block 132.

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

[0055] like Figure 4 As shown, a first nut 131 is connected to the upper part of the fixing block 132. The first nut 131 has a first internal thread section on its inner side for threaded connection with the first external thread section. A second nut 136 is connected to the lower part of the fixing block 132. The second nut 136 has two internal thread sections on its inner side. 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 diameter of the upper cylindrical body of the quartz tube 12.

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

[0057] It should be noted that both the first and second external thread segments are designed with circumferentially multi-segment uniform slotting. In this embodiment, the first or second external thread segment has three uniformly slotted segments in the circumferential direction, dividing the first or second external thread segment into three uniform segments. When the first or second nut is tightened, the three segments of the first or second external thread segment can be squeezed to compress and fix the high-voltage electrode or 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 diameter of the outer wall of the upper part of the quartz tube 12 is equal to the diameter of the third channel.

[0059] like Figure 4 As shown, the fixed connection device 13 also includes a first sealing rubber ring 134 and a second sealing rubber ring 135, wherein the first sealing rubber ring 134 is disposed in the third channel; and the second sealing rubber ring 135 is disposed outside the second external thread section.

[0060] like Figure 4As shown, during installation, first, the first sealing rubber ring 134 is placed into the third channel, and the first sealing rubber ring 134 is placed at the top of the third channel near the second channel. Then, the upper part of the quartz tube 12 is inserted into the third channel of the second external thread section, so that the upper part of the quartz tube 12 presses against the first sealing rubber ring 134. Then, the second sealing rubber ring 135 is placed outside the second external thread section and at the top of the second external thread section near the second channel. Finally, the upper end of the second internal thread section inside the second nut 136 is connected to the second external thread section. By tightening the second nut 136, the second external thread section is squeezed, thereby squeezing the upper part of the quartz tube 12, and the connection is completed.

[0061] After the quartz tube 12 is connected to the fixed connection device 13, the high voltage electrode 11 is passed through the first channel and the second channel until the length set inside the quartz tube 12 is reached (for example, below the bottom ring of air holes). Then the first nut 131 is threadedly connected to the first external thread section. By turning the first nut 131 to squeeze the first external thread section, the first external thread section squeezes the high voltage electrode 11, thus completing the connection.

[0062] like Figure 4 As shown, after the high-voltage electrode 11, quartz tube 12, and fixed connection device 13 are connected, the high-voltage electrode 11 seals the first channel, the quartz tube 12 seals the third channel, and the second channel is connected to the quartz tube 12, which actually forms a gas channel; gas is injected into the fixed block 132 through the venting device 133, and the gas flows into the quartz tube 12 through the second channel.

[0063] It is understandable that the first sealing rubber ring 134 and the second sealing rubber ring 135 play a role in strengthening the seal; at the above-mentioned threaded section connection, PTFE tape can be wrapped around the connection and fixed, which can further improve the airtightness of the connection.

[0064] Furthermore, a sealing rubber ring of appropriate size can 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 impact of other gases possibly mixing in when a single gas type is discharged.

[0065] It should be noted that the first nut 131, the fixing block 132, the second nut 136, and the venting component 133 are all made of polytetrafluoroethylene, 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, which are used to improve the airtightness of the fixing connection device 13.

[0066] like Figure 1 , Figure 8 , Figure 9As shown, container 2 includes a container body, and a movable cover 22 is provided on the top of the container body. The cover 22 has an opening at the center, the size of which matches the outer diameter of the outer quartz tube 12. A protruding threaded ring 21 is provided on the outside of the opening, and a fourth external thread section is provided on the outside of the protruding threaded ring 21 for connecting with the fourth internal thread section at the bottom of the inner side of the second nut 136 of the fixed connection device 13, thereby realizing the assembly of the cover 22 of the discharge reaction device 1 and container 2.

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

[0068] like Figure 1 , Figure 5 As shown, the grounding method of the discharge reaction device 1 is to connect the grounding device 14 to the part of the quartz tube 12 located in the container 2. Specifically, inside the container 2, the grounding device 14 includes a stainless steel grounding mesh 141 wrapped around the quartz tube 12; the grounding mesh 141 has a hollow cylinder in the middle, the diameter of which is larger than the outer diameter of the quartz tube 12, serving two purposes: firstly, to accommodate the quartz tube 12; and secondly, to provide a lifting partition 144 between the quartz tube 12 and the grounding mesh 141. The length of the grounding mesh 141 is equal to the distance between the bottom of the cover 22 and the bottommost vent. The lifting partition 144 is made of polytetrafluoroethylene (PTFE).

[0069] Bare electrode discharge in a single-layer dielectric tends to be a discharge form that combines gas and liquid. Covering the pores with a grounding grid can help draw plasma out from the pores.

[0070] like Figure 5 As shown, the top of the grounding grid 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 whose size is the same as that of the first magnet ring 137. Through the principle of attraction between opposite poles of the first magnet ring 137 and the second magnet ring 142, the top of the grounding grid 141 is connected to the cover 22, thereby covering the part of the quartz tube 12 inside the container 2 inside the grounding grid 141, which facilitates connection.

[0071] As described above: the catalyst should be placed as close as possible to the bottommost pores. This allows the plasma discharged from the bottom to have a longer interaction time during its ascent from the bottom to the top of the liquid phase after entering the liquid phase. Therefore, theoretically, it is desirable to utilize every ring of pores.

[0072] However, in practical applications, the flow rate of the working gas may be insufficient, preventing the gas from escaping through the bottom vents. In this case, some of the bottom vents are blocked by liquid, hindering plasma emission. Furthermore, the high-voltage electrode, under the influence of the grounding grid, will experience a slight electrical discharge in the water, affecting the device's discharge stability and causing a temperature rise. This may also exacerbate 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 size of the grounding grid so that it is kept as close as possible to the pores covered by the liquid.

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

[0075] The lifting partition 144 is slidably disposed in the storage tray 146; the storage tray 146 has a through receiving opening 1461 in the middle, the diameter of which is equal to the diameter of the upper cylinder of the quartz tube 12 (the diameter of the outer wall of the upper cylinder). The bottom of the quartz tube 12 is inserted into the receiving opening until the top surface of the storage tray 146 is located below the air hole on the bottom surface of the grounding grid 141, and the two are restricted by friction.

[0076] A circular groove 1462 is provided on the outer side of the center of the storage tray 146 and on the outer side of the receiving opening of the storage tray 146. The groove does not penetrate the top and bottom surfaces of the storage tray 146. The lifting partition 144 is slidably disposed inside the groove. It can be understood that the inner diameter of the groove is smaller than the diameter of the lifting partition 144, and the outer 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 through a rotating bearing; Figure 7 As shown, the lifting bolt 145 is threadedly connected to the storage tray 146. The lifting bolt 145 passes through the bottom of the storage tray 146 and is rotatably connected to the bottom of the lifting partition 144 through a rotating bearing.

[0078] Understandably, turning the two lifting bolts 145 moves them into the receiving tray 146, causing the lifting partition 144 to move upwards, allowing it to be positioned between the grounding grid 141 and the quartz tube 12. Adjusting the height of the lifting partition 144 via the lifting bolts 145, with the partition 144 positioned between the quartz tube and the grounding grid, isolates the high-voltage electrode from the grounding grid. This allows for selection of the discharge area, i.e., adjustment of the discharge region.

[0079] In addition, fixing bolt holes can be provided on the side of the storage tray 146 below the groove. Fixing bolts 143 are threaded into the fixing bolt holes, which connect the outer side of the storage tray 146 to the receiving opening, and the extension line of the fixing bolt holes passes through the center of the storage tray 146. Tightening the fixing bolts 143 into contact with the quartz tube 12 can strengthen the connection between the storage tray 146 and the quartz tube.

[0080] In this embodiment, the design of the magnetic suction structure and the adjustable lifting baffle facilitates the installation, disassembly, and length adjustment of the grounding grid, thereby facilitating the control of the discharge area.

[0081] like Figure 10 As shown, the catalyst placement module 3 can adopt a variety of different three-dimensional shapes, such as cube, cuboid, cylinder, and ring; however, all of them need to have mesh-like markings or grooves made on the top of the catalyst placement module 3 so that the catalyst 31 can be evenly placed on the mesh-like markings 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 or above the pores of the quartz tube where the gas and liquid phases are in contact through the catalyst placement module 3, and the working position of the catalyst is adjusted by the blowing of gas and the buoyancy of the catalyst placement module 3 itself.

[0083] When gas is blown in through the vent 133, the aqueous solution in the original discharge channel (between the quartz tube 12 and the high-voltage electrode) is squeezed downwards under the continuous blowing of gas. Eventually, the water or aqueous solution in the discharge channel is reduced to below a certain ring of vents. The specific height of the liquid level in the quartz tube 12 is related to the gas flow rate. Different gas flow rates can adjust the height of the liquid level in the quartz tube 12. By reasonably selecting the size of the catalyst placement module, the catalyst can be suspended on the liquid surface under its own buoyancy, thereby promoting the discharge.

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

[0085] During the discharge process, the catalyst acts on the adsorption and bonding processes, which enrich the series of reactions that occur during the discharge. 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. The electron-hole pairs formed further enhance the photocatalytic process. Therefore, filling the device with catalyst can effectively improve the reactant conversion rate, product selectivity and energy efficiency.

[0086] The range of vertical movement of the catalyst placement module can be appropriately adjusted by varying gas flow rates and its own dimensions.

[0087] In this embodiment, the selected catalysts are mostly nanoscale foam metal or oxide carrier-metal materials, which have small size and good effect, and are widely applicable.

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

[0089] Specifically, the high-voltage electrode 11 is connected to the high-voltage output terminal of a high-voltage AC source or pulse power supply. After the power is turned on, an obvious discharge phenomenon can be observed in the discharge channel of the quartz tube 12 covering the grounding grid 141. At the same time, the discharge effect of the gas and liquid phases can be observed at the pore 121.

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

[0091] Example 2

[0092] This embodiment discloses a method for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid, which uses the apparatus for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid disclosed in Example 1. The specific steps are as follows:

[0093] Before use, the type of catalyst must be determined and the catalyst placed in the catalyst placement module 3; the catalyst placement module 3 is placed at the bottom of the quartz tube 12; a catalyst placement module 3 of appropriate size or shape is selected so that the catalyst is concentrated on the liquid surface at the pore 121, which promotes the discharge.

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

[0095] Then, the grounding grid 141 is installed on the outside of the quartz tube 12, and the storage 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 storage tray 146 by fixing bolts 143.

[0096] Add water or aqueous solution to container 2 to prepare for the discharge process; then install the assembled discharge reaction device 1, together with the cover 22, onto container 2. At this time, due to the action of the jet port 122 at the bottom of the quartz tube 12, the liquid level in the quartz tube 12 is basically level with the liquid level of the water or aqueous solution in container 2, and the catalyst placement module 3 also floats on the liquid surface under its own buoyancy.

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

[0098] Stop blowing air, remove the cover 22, adjust the length of the lifting partition 144 so that the lifting partition 144 is below the aforementioned ring of air holes 121; reinstall the cover 22, and then blow air again.

[0099] Then, the high-voltage lead 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 of the overlapping area of ​​the quartz tube 12 and the grounding grid 141 and spreads to the vicinity of the vent 121. The 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 active particles with oxidizing properties, which then act 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, the high-voltage power supply is turned off and the gas supply is cut off, thus completing the process of preparing activated water or treating aqueous solution using the discharge plasma.

[0101] The entire discharge reaction device 1, container 2, and catalyst placement module 3 were cleaned and dried for future use.

[0102] While the specific embodiments of the present invention have been described above in conjunction with the accompanying drawings, this is not intended to limit the scope of protection of the present invention. Those skilled in the art should understand that various modifications or variations that can be made by those skilled in the art without creative effort based on the technical solutions of the present invention are still within the scope of protection of the present invention.

Claims

1. An apparatus for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid, characterized in that, It includes a discharge reaction device, which is installed in a container and has a catalyst placement module inside. The discharge reaction device includes a quartz tube, and a fixed connection device is connected to the top of the quartz tube. 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 consists of an upper cylindrical structure and a lower hemispherical structure. The inside of the quartz tube is hollow, with an open top and a closed bottom. A through jet port is set at the center of the bottom of the quartz tube. At a set distance above the jet port, multiple rings of air holes of the same size are evenly opened around the quartz tube. The catalyst placement module adopts a variety of different three-dimensional shapes. The top of the catalyst placement module is treated with mesh-like grooves or grooves to evenly place the catalyst on the top of the catalyst placement module. The catalyst placement module floats on the liquid inside the container by relying on buoyancy.

2. The apparatus for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid as described in claim 1, characterized in that, The fixed connection device includes a fixing block, with a first external thread section at the upper end and a second external thread section at the lower end. A first channel is provided inside the fixing block; a second channel is provided inside the first external thread section; and a third channel is provided inside the second external thread section.

3. The apparatus for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid as described in 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 diameter of the outer wall of the quartz tube.

4. The apparatus for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid as described in claim 2, characterized in that, A vent hole is provided on the side of the fixed block. The second channel is connected to the outside through the vent hole. A third internal thread section is provided inside the vent hole. A third external thread section is provided on the outer wall of the venting component to cooperate with the third internal thread section. A through-hole is provided inside the venting component. The venting component is connected to the venting pipe of the venting device to inject air into the fixed block.

5. The apparatus for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid as described in claim 2, characterized in that, The first external thread segment is connected to the first nut, and the first nut has a first internal thread segment on its inner side; the second external thread segment is connected to the second nut, and the second nut has two internal thread segments on its inner side, the upper segment being the second internal thread segment and the lower segment being the fourth internal thread segment.

6. The apparatus for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid as described in 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 direction of the fourth internal thread segment is opposite to that of the second internal thread segment; the diameter of the fourth internal thread segment is larger than that of the quartz tube; a first magnet ring is bonded and fixed to the bottom of the second nut.

7. The apparatus for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid as described in claim 5, characterized in that, Both the first external thread segment and the second external thread segment are designed with multiple uniform slots, 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 tightened, the three segments of the first external thread segment or the second external thread segment can be squeezed to compress and fix the high voltage electrode or quartz tube therein.

8. The apparatus for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid as described in claim 5, characterized in that, The container includes a container body, a movable lid on top of the container body, an opening at the center of the lid with a size matching the outer quartz tube, a protruding threaded ring on the outside of the opening, and a fourth external thread segment on the outside of the protruding threaded ring, which is connected to the fourth internal thread segment.

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

10. A method for preparing a catalytic gas-liquid two-phase discharge plasma activation liquid, characterized in that, The preparation apparatus for a novel catalytic gas-liquid two-phase discharge plasma activation liquid as described in any one of claims 1-9 is used, and the specific steps are as follows: Determine the type of catalyst and place it in the catalyst placement module; then place the catalyst placement module at the bottom of the quartz tube; next, connect the quartz tube and the high-voltage electrode through the fixing connection device and connect it to the cover; then install the grounding grid and storage tray on the outside of the quartz tube. Add water or an aqueous solution to the container, and attach the discharge reaction device along with the lid to 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 ring of air holes; Stop blowing air, remove the cover and adjust the length of the lifting baffle so that the lifting baffle is below the aforementioned air hole ring; reinstall the cover and then blow air again; Then, the high-voltage power supply is connected to the high-voltage electrode. The discharge is concentrated in the discharge channel in the area where the quartz tube and the grounding grid overlap and spreads to the vicinity of the pores, generating various active particles with oxidizing properties, which then act on the water or the aqueous solution to be treated. After the discharge is complete, 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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