Gas-liquid-solid three-phase large-area acousto-optic catalysis combined pulse discharge reactor

Abstract

The application discloses a gas-liquid-solid three-phase large-area sound-light catalysis combined pulse discharge reactor, relates to the generation of discharge plasma active components in a gas-liquid-solid three-phase environment and liquid-phase nitrogen fixation and water pollutant treatment technical fields, and the reactor comprises a box body and a bottom plate, the box body is located on the upper end face of the bottom plate, a reactor base is arranged on the lower side of the bottom plate, a mounting cover is arranged on the upper side of the box body, a large-area pulse discharge assembly is arranged in the box body, a pulse power interface assembly, an ultrasonic transducer module and a light radiation window are arranged on the outer wall of the box body, and the reactor base is used for feeding air into the box body and discharging treated water phase; high-voltage pulse discharge is generated in the box body, active components are generated in a gas-liquid-solid three-phase reaction region, and oxidation and reduction reactions in the liquid phase are promoted; and through the action of high-energy electrons, free radicals, ozone, nitrogen oxides and other active components generated by discharge, the nitrogen fixation in water or the degradation of pollutants is effectively improved.

Description

Technical Field

[0001] This invention relates to the field of reactor technology for generating active components through the interaction of discharge plasma and water, and for nitrogen fixation and water treatment, specifically a gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor. Background Technology

[0002] Depending on the electrode structure, underwater discharge electrode structures can be categorized into needle-needle, needle-plate, wire-cylinder, and linear array discharge devices. Each device has its own advantages in different application scenarios. While needle-needle and needle-plate discharges are simple in structure, their discharge areas are relatively small, limiting their practical applications. Wire-cylinder discharges have larger discharge areas, but their structural characteristics are more suitable for tubular or internal surface treatment applications, restricting their use. Linear array electrode structures offer advantages in terms of large discharge area and uniform discharge. Therefore, in gas-liquid-solid three-phase scenarios, combining ultrasound and catalysis to enhance the high-voltage pulse discharge effect is expected to solve problems such as high discharge difficulty, small discharge area, uneven discharge, and low generation and utilization rate of active components in underwater discharge, thus contributing to the practical promotion and application of underwater discharge technology.

[0003] Furthermore, the mechanical stirring effect of ultrasound can improve the mass transfer rate between the gas, liquid, and solid phases, promote the contact between reactants and catalysts, and enhance adsorption and desorption efficiency. For underwater bubble discharge, ultrasound can promote bubble generation and breakup, improving the discharge effect. Photocatalytic materials can effectively utilize ultraviolet radiation generated by discharge or external light source radiation to activate photocatalysis and generate electrons and holes. Utilizing the mechanical vibration effect of ultrasound can improve the separation efficiency of electrons and holes. Utilizing the anti-Stokes effect of carbon quantum dots (CQDs), more visible light can be converted into ultraviolet light that can activate the active sites of photocatalytic materials, effectively improving the utilization rate of discharge and external light sources. Utilizing the charge storage effect of carbon quantum dots can suppress the electron-hole recombination rate, effectively improving photocatalytic efficiency. In gas-liquid-solid three-phase environments, there are relatively few experiments combining ultrasound, carbon quantum dot composite photocatalytic materials, pulsed discharge, and fluid parameter control technologies, and research on the laws and mechanisms of active component generation in water is also limited. Summary of the Invention

[0004] The purpose of this invention is to provide a gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor to solve the problems of small discharge area, low generation and utilization rate of active ingredients in the prior art.

[0005] To achieve the above objectives, the present invention provides the following technical solution: a gas-liquid-solid three-phase large-area acoustic-photocatalytic combined pulse discharge reactor, the reactor comprising a housing and a base plate, the housing being located on the upper surface of the base plate, a reactor base being disposed on the lower side of the base plate, an air inlet being disposed on the side wall of the reactor base, a water outlet being disposed at the bottom of the reactor base, an installation cover being disposed on the upper side of the housing, the installation cover being disposed on the water inlet and an air outlet, a discharge assembly being disposed inside the housing, an ultrasonic module and a light radiation window being disposed on the outer wall of the housing, and sealing assemblies being disposed at the connection points of the various components inside the housing, the gas phase inside the housing being air or oxygen and nitrogen with an adjustable molar mass ratio, the liquid phase being water, and the solid phase being graphitic nitrogen carbide (g-C3N4) or aluminum oxide (Al2O3) microspheres, with CQDs, SnO2, CuO and other materials loaded on their surface to form a composite catalytic material. The housing and base plate provide support and a foundation for the entire three-phase pulse discharge reactor. The reactor base is used to install the exhaust pipe and aeration net. The inlet is used to add water to the housing, and the outlet is used to discharge the gas produced in the reaction, maintaining stable gas pressure inside the reactor. The outlet is used to supply gas into the reactor, and the outlet is used to discharge the water produced in the housing. The discharge assembly is used to generate high-voltage pulse discharge. The active components generated inside the gas-liquid-solid three-phase reactor, such as free electrons, electron holes, hydroxyl radicals, ultraviolet light, and nitrogen oxides, can be used for nitrogen fixation in water, effective degradation of pollutants in water, or elimination of microorganisms and viruses in water. The ultrasonic module, through high-frequency vibration, promotes the generation and collapse of bubbles, which is beneficial for generating high-voltage pulse discharge in the gas-liquid-solid three-phase environment. It also increases the desorption and adsorption rates of reactants and products on the catalyst surface, accelerating the reaction rate. The light radiation window facilitates the application of light radiation from the outside, which is beneficial for studying the effects of different spectral wavelengths and intensities on the reaction of the composite photocatalytic material and analyzing the optimization of reaction physical parameters. The sealing assembly is used to seal the housing to ensure the normal operation of the reaction.

[0006] The housing includes electrode plate one, electrode plate two, mounting plate, and light-transmitting plate. Electrode plate one and electrode plate two are located on two opposite sides of the housing. The mounting plate and light-transmitting plate are located on both sides of electrode plate one. The ultrasonic module is located on the mounting plate. The light-transmitting plate has a mounting groove, and the light radiation window is located in the mounting groove. A fixing plate is provided on one side of the light radiation window, and the fixing plate has a through groove with the same shape as the light radiation window. Electrode plate one and electrode plate two are used to fix the electrodes and the capacitor on the outside. The mounting plate is used to install the ultrasonic module, the light-transmitting plate is used to install the light radiation window, and the fixing plate is used to fix the light radiation window. The radiation surface of the ultrasonic module is a circle with a diameter of c. The effective area of ​​the ultrasonic module is also the discharge area. The light radiation window is a rectangular quartz plate of 3c × 1.75c. The light-transmitting plate has two square grooves with a width of b and a depth of 0.75b, and adhesive strips are provided inside.

[0007] The mounting plate and the light-transmitting plate have convex cross-sections, and the edges of the convex structures of the mounting plate and the light-transmitting plate connect with electrode plate one and electrode plate two at stepped surfaces. The stepped surfaces formed by the connection between the edges of the convex structures and another flat plate force the water flow to undergo two 90° turns before overflowing, effectively reducing leakage.

[0008] The mounting plate and the light-transmitting plate have two waterproof grooves on their raised edges. The sealing assembly includes a circular nitrile rubber strip located within the waterproof groove. A threaded hole is formed between two adjacent waterproof grooves, and a self-tapping screw is installed in the threaded hole. The width of the two waterproof grooves is b, the depth is 0.75b, and the diameter of the circular nitrile rubber strip is b. The self-tapping screw is then tightened to ensure that the circular nitrile rubber strip is fully compressed to achieve a waterproof effect.

[0009] The discharge assembly includes several discharge electrodes made of corrosion-resistant tungsten-molybdenum alloy or 316L stainless steel. The electrode surfaces are threaded to facilitate discharge in a gas-liquid-solid three-phase environment. The electrodes are staggered horizontally, with one electrode penetrating electrode plate one and semi-embedded in electrode plate two, while the remaining electrodes penetrate electrode plate two and semi-embedded in electrode plate one. A high-voltage capacitor is mounted at one end of each electrode penetrating electrode plate one and electrode plate two. High-voltage protective shields are mounted on electrode plate one and electrode plate two, with the capacitor located inside the high-voltage protective shields. One electrical terminal of the high-voltage capacitor is connected to the discharge electrode, and the other end is connected to the output terminal of a high-voltage pulse power supply. The reactor is powered by a nanosecond pulse power supply, the output of which is connected to the electrical terminal of the high-voltage capacitor. The electrodes discharge in the three-phase reaction region, and the generated active ingredients can be used to degrade pollutants in water, disinfect microorganisms, or fix nitrogen in the liquid phase. The high-voltage nanosecond pulse power supply supplies power to the electrodes through a high-voltage capacitor. The high-voltage capacitor plays a role in dynamic current limiting and balancing of discharge capacity among multiple discharge channels. When a gap between a group of electrodes breaks down, the impedance of that path will decrease rapidly. At this time, the energy of the high-voltage pulse power supply will be distributed to other electrode gaps with higher impedance, supporting the formation of new discharges in other electrode gaps. This cycle repeats, which can effectively avoid short circuits caused by the initial breakdown of individual branches, evenly distribute discharge energy, and obtain a uniform discharge effect over a large area.

[0010] One embodiment of a larger discharge area is as follows: the discharge assembly includes fifteen electrodes, five of which are staggered in the horizontal direction, three electrodes separated by a distance pass through electrode plate one and semi-embedded electrode plate two, and two electrodes separated by a distance pass through electrode plate two and semi-embedded electrode plate one, for a total of three columns.

[0011] Another embodiment with a smaller discharge area is as follows: the discharge assembly includes six electrodes, three of which are staggered in the horizontal direction, two electrodes separated by one pass through electrode plate one and semi-embedded electrode plate two, and one electrode separated by one pass through electrode plate two and semi-embedded electrode plate one, for a total of two columns.

[0012] Two sealing grooves are formed on the base plate. The sealing assembly includes a sealing strip located within the two sealing grooves. A filter screen is installed on the inner side of the base plate. The interior of the chamber is filled with CQDs composite catalyst microspheres. The sealing grooves and sealing strips are used to prevent leakage of the aqueous phase, and the filter screen is used to prevent the catalyst microspheres from leaking out. The weight of the catalyst microspheres themselves can hold down the filter screen. The catalyst pellet filling ratio is one of the core parameters in reaction engineering. The optimal value needs to be found through experimental and theoretical analysis. A reasonable filling ratio can significantly improve reaction efficiency while avoiding resource waste and operational problems. In practical applications, a comprehensive balance must be struck considering catalyst characteristics, reactor type, and economics. However, the filling ratio will vary depending on the size of the catalyst pellets used. The calculation process for the filling ratio is as follows: [Filling Ratio] The formula is:

[0013] To calculate the filling ratio, the volume occupied by the catalyst pellets needs to be calculated. Volume of the reaction zone The mass of the catalyst pellets can be weighed. Let the density of the small ball be... The volume of the small ball is...

[0014] Assume the electrode occupies a volume Container volume ,but

[0015] Therefore, the fill ratio is:

[0016] Therefore, to calculate the packing ratio of catalysts of different sizes, it is only necessary to measure the mass of the catalyst packed in.

[0017] An exhaust pipe is installed inside the reactor base, and the exhaust pipe is connected to the air inlet. Multiple branch pipes are installed on one side of the exhaust pipe, and multiple air holes are evenly arranged on each branch pipe. An aeration net is installed on the upper side of the exhaust pipe, and three or four supports are installed on the lower end face of the reactor base. Gas is dispersed into small bubbles through the exhaust pipe and aeration net, increasing the gas-liquid-solid contact area and improving the reaction rate.

[0018] The electrode tip and body are threaded. Electrode plate one and electrode plate two have several stepped holes located at the connection points between the electrode and electrode plate one and electrode plate two. A threaded hole is provided on one side of the capacitor, and the electrode is threadedly connected to the capacitor. The electrode is threadedly connected to the stepped hole. The horizontal electrode spacing is d, the row spacing is e, the electrode diameter is a, and D1 and D2 represent the distances from the center of the second and third electrodes to the center of the first electrode, respectively. The electrode spacing d is determined by the electrode arrangement and the electrode diameter.

[0019] d The reference value is 6.0mm~10.0mm. e The reference value is 28.0mm~32.0mm; The total length of the electrode is 85.5 mm. The first 21.0 mm and the last 5.0 mm of the electrode are machined into round bars with a diameter of 4.0 mm to facilitate insertion into the electrode plate for fixation. At the same time, the first 8.0 mm of the electrode needs to be machined with an M4 thread, which can be used to connect the capacitor and tighten the connection between the electrode and the electrode plate.

[0020] The sealing assembly also includes an O-ring located on the stepped surface of the stepped hole. During the tightening process, the electrode provides sufficient clamping force to the O-ring to ensure a sealing effect.

[0021] Electrode plate one, electrode plate two, mounting plate, and light-transmitting plate are made of polytetrafluoroethylene (PTFE), and the electrodes are made of tungsten-molybdenum alloy or 316L stainless steel. PTFE has excellent corrosion resistance and high-temperature resistance, effectively resisting corrosive chemicals and high-temperature environments that may be generated during the reaction process. Tungsten-molybdenum alloy or 316L stainless steel, due to their high corrosion resistance, are particularly suitable for highly corrosive environments, ensuring long-term stability and durability during the discharge process.

[0022] Compared with the prior art, the beneficial effects of the present invention are: 1. This invention connects high-voltage capacitors in series before each branch of the multi-electrode array to form a dynamic current limiting and energy equalization mechanism, which overcomes the uneven discharge and short circuit caused by the "path contention" of underwater bubble discharge, and realizes uniform discharge in a large area within the gas-liquid-solid three-phase reaction zone. This allows for the efficient utilization of active ingredients in a larger area, thereby effectively increasing the total amount of liquid-phase nitrogen fixation or water treatment.

[0023] 2. This invention promotes bubble generation and breakage and improves the contact between the gas, liquid, and solid phases by using an ultrasonic module, a translucent quartz surface, and composite photocatalytic materials. The ultraviolet light generated by the discharge or the light radiation provided by the outside effectively activates the active sites of the photocatalytic materials. The ultrasonic modulation of the charge storage effect of CQDs reduces the electron-hole recombination rate, thereby significantly improving the efficiency of the photocatalytic reaction.

[0024] 3. In terms of structure and sealing, this invention adopts a double-ring sealing groove of polytetrafluoroethylene plate and O-ring, stepped hole and threaded clamping at the electrode penetration point, etc., to meet the insulation and waterproof requirements of gas-liquid-solid three-phase and 20kV high voltage. The bottom step and filter screen prevent catalyst leakage, facilitate recycling and reuse, ensure long-term stable operation of the reactor and reduce costs. Attached Figure Description

[0025] Figure 1 This is a perspective view of the overall structure of the present invention; Figure 2 This is a perspective view of the internal structure of the high-voltage protective cover of the present invention; Figure 3 This is a perspective view of the internal structure of the housing of the present invention; Figure 4 This is an exploded view of the internal structure of the housing of the present invention; Figure 5 This is a top view of the internal structure of the housing of the present invention; Figure 6 This is a cross-sectional view of the connection between the electrode and the housing in this invention; Figure 7 This is a three-dimensional view of the electrodes of the present invention; Figure 8 This is a top view of the internal structure of the reactor base of the present invention; Figure 9 This is a top view of the filter structure of the present invention; Figure 10 This is a schematic diagram of the overall circuit structure of the present invention.

[0026] In the diagram: 1. Box body; 101. Electrode plate one; 102. Electrode plate two; 103. Mounting plate; 104. Light-transmitting plate; 2. Base plate; 3. Reactor base; 4. Bracket; 5. Mounting cover; 6. High-pressure protective cover; 7. Ultrasonic module; 8. Light radiation window; 9. Fixing plate; 10. Air inlet; 11. Water outlet; 12. Water inlet; 13. Air outlet; 14. Electrode; 15. Capacitor; 16. Exhaust pipe; 17. Filter screen; 18. O-ring; 19. Sealing strip; 20. Sealing groove. Detailed Implementation

[0027] The technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention.

[0028] Please see Figure 1-10 Figure 1 illustrates the technical solution provided by this invention: a gas-liquid-solid three-phase large-area acoustic-photocatalytic combined pulsed discharge reactor. The reactor includes a housing 1 and a base plate 2. The housing 1 is located on the upper surface of the base plate 2. A reactor base 3 is provided on the lower side of the base plate 2. An air inlet 10 is provided on the side wall of the reactor base 3. A water outlet 11 is provided at the bottom of the reactor base 3. An installation cover 5 is provided on the upper side of the housing 1. An inlet 12 and an air outlet 13 are provided on the installation cover 5. A discharge assembly is provided inside the housing 1. An ultrasonic module 7 and a light radiation window 8 are provided on the outer wall of the housing 1. Sealing assemblies are provided at the connection points of the various components inside the housing 1. The gas phase inside the housing 1 is air, the liquid phase is pure water or other water containing pollutants, and the solid phase is a CQDs composite catalyst. The housing 1 and base plate 2 provide support and installation foundation for the entire three-phase pulse discharge reactor. The reactor base 3 is used to install the exhaust pipe 16 and aeration net. The inlet 12 is used to add water phase into the housing 1. The outlet 13 is used to discharge the gas generated by the reaction and maintain stable gas pressure inside the reactor. The inlet 10 is used to transport gas into the reactor. The outlet 11 is used to discharge the water generated inside the housing 1. The discharge assembly is used to generate high-voltage pulse discharge. The generated active ingredients can effectively fix nitrogen in water, degrade pollutants in water, or disinfect microorganisms or toxins in water. The ultrasonic module 7 promotes the generation and collapse of bubbles through high-frequency vibration, reduces the discharge difficulty in the gas-liquid-solid three-phase environment, increases the contact between the catalyst and pollutants, and accelerates the reaction rate. The light radiation window 8 facilitates the application of light and can effectively utilize the ultraviolet radiation generated during the discharge process of the electrode 14 or the radiation of external light sources for photocatalytic reaction, effectively improving the efficiency of photocatalytic reaction. It is convenient to collect the spectrum generated by the reaction inside the reactor from the outside and analyze the relative concentration and changes of active ingredients in the discharge reaction area. The sealing assembly is used to seal the housing 1 to ensure the normal operation of the reaction.

[0029] The housing 1 includes an electrode plate 101, an electrode plate 102, a mounting plate 103, and a light-transmitting plate 104. The electrode plate 101 and the electrode plate 102 are located on two opposite sides inside the housing 1. The mounting plate 103 and the light-transmitting plate 104 are located on both sides of the electrode plate 101. The ultrasonic module 7 is located on the mounting plate 103. The light-transmitting plate 104 has a mounting groove. The light radiation window 8 is located in the mounting groove. A fixing plate 9 is provided on one side of the light radiation window 8. The fixing plate 9 has a through groove with the same shape as the light radiation window 8. Electrode plate 101 and electrode plate 102 are used to fix electrode 14 and capacitor 15 on the outside. Mounting plate 103 is used to install ultrasonic module 7. Light-transmitting plate 104 is used to install light radiation window 8. Fixing plate 9 is used to fix light radiation window 8. The radiation surface of ultrasonic module 7 is a circle with a diameter of c. The effective area of ​​ultrasonic module 7 is also the discharge area. Light radiation window 8 is a rectangle of 3c × 1.75c. Light-transmitting plate 104 is provided with two square grooves with a width of b and a depth of 0.75b, and adhesive strips are provided inside.

[0030] The mounting plate 103 and the light-transmitting plate 104 have convex cross-sections. The edges of the convex structures of the mounting plate 103 and the light-transmitting plate 104 are connected to the electrode plate 101 and the electrode plate 102 at stepped surfaces. The stepped surfaces formed by the connection between the edges of the convex structures and the other plate ensure that the water flow must make two 90° turns before overflowing, which can effectively reduce leakage.

[0031] The edges of the raised structures of mounting plate 103 and light-transmitting plate 104 each have two waterproof grooves. The sealing assembly includes a circular nitrile rubber strip located within the waterproof groove. A threaded hole is formed between two adjacent waterproof grooves, and a self-tapping screw is installed in the threaded hole. The width of the two waterproof grooves is b, the depth is 0.75b, and the diameter of the circular nitrile rubber strip is b. The self-tapping screw is then tightened to ensure that the circular nitrile rubber strip is fully compressed to achieve the waterproof effect.

[0032] The discharge assembly includes several electrodes 14, which are staggered in the horizontal direction. The interphase electrodes 14 penetrate electrode plate 101 and are semi-embedded in electrode plate 2 102. The remaining electrodes 14 penetrate electrode plate 2 102 and are semi-embedded in electrode plate 101. Capacitors 15 are respectively provided at one end of the electrodes 14 that penetrate electrode plate 101 and electrode plate 2 102. High voltage protective covers 6 are respectively provided on electrode plate 101 and electrode plate 2 102. The capacitors 15 are located inside the high voltage protective covers 6. The power supply of the reactor is a nanosecond pulse power supply, which is electrically connected to the capacitors 15. Electrode 14 discharges in the three-phase reaction region, and the generated plasma and free radicals can effectively decompose organic pollutants and microorganisms in the water, thereby achieving the effects of water treatment, sterilization and disinfection. Capacitor 15 supplies power to electrode 14. Using the dynamic current limiting method of capacitor 15, a high-voltage capacitor 15 is connected in series before each electrode 14 to balance the energy distribution during charging and discharging. After electrode 14 is connected in series with capacitor 15, when one electrode 14 breaks down, the impedance of that path will decrease. At this time, the energy will be distributed to other branches with higher impedance to support them to complete the next discharge. This cycle repeats, which can effectively avoid short circuits caused by individual branches breaking down first, and evenly distribute discharge energy, thus improving the uniformity of discharge.

[0033] One embodiment is as follows: the discharge assembly includes fifteen electrodes 14, five of which are staggered in the horizontal direction, three spaced electrodes 14 pass through electrode plate one 101 and semi-embedded electrode plate two 102, and two spaced electrodes 14 pass through electrode plate two 102 and semi-embedded electrode plate one 101, for a total of three rows.

[0034] The base plate 2 has two sealing grooves 20. The sealing assembly includes a sealing strip 19, which is located within the two sealing grooves 20. A filter screen 17 is installed on the inner side of the base plate 2. The interior of the housing 1 is filled with CQDs composite catalyst. The sealing grooves 20 and sealing strip 19 are used to prevent leakage of the aqueous phase. The filter screen 17 is used to prevent the catalyst balls from leaking out and to facilitate recycling. The weight of the catalyst balls themselves can hold down the filter screen 17. The catalyst pellet filling ratio is one of the core parameters in reaction engineering. The optimal value needs to be found through experimental and theoretical analysis. A reasonable filling ratio can significantly improve reaction efficiency while avoiding resource waste and operational problems. In practical applications, a comprehensive balance must be struck considering catalyst characteristics, reactor type, and economics. However, the filling ratio will vary depending on the size of the catalyst pellets used. The calculation process for the filling ratio is as follows: [Filling Ratio] The formula is:

[0035] To calculate the filling ratio, the volume occupied by the catalyst pellets needs to be calculated. Volume of the reaction zone The mass of the catalyst pellets can be weighed. Let the density of the small ball be... The volume of the small ball is...

[0036] Assume electrode 14 occupies a volume Container volume ,but

[0037] Therefore, the fill ratio is:

[0038] Therefore, to calculate the packing ratio of catalysts of different sizes, it is only necessary to measure the mass of the catalyst packed in.

[0039] An exhaust pipe 16 is installed inside the reactor base 3, and the exhaust pipe 16 is connected to the air inlet 10. Multiple branch pipes are installed on one side of the exhaust pipe 16, and multiple air holes are evenly arranged on the branch pipes. An aeration net is installed on the upper side of the exhaust pipe 16, and four supports 4 are installed at the four corners of the lower end face of the reactor base 3. The gas is dispersed into small bubbles through the exhaust pipe 16 and the aeration net, which increases the contact area between gas, liquid and solid and improves the reaction rate.

[0040] The front end and body of electrode 14 are provided with threads. Several stepped holes are opened on electrode plate 101 and electrode plate 102, located at the connection points between electrode 14 and electrode plate 101 and electrode plate 102. A threaded hole is provided on one side of capacitor 15, and electrode 14 is threadedly connected to capacitor 15. Electrode 14 is threadedly connected to the stepped hole. The horizontal spacing of the electrodes 14 is d, the row spacing is e, and the diameter of the electrodes 14 is a. D1 and D2 represent the distances from the center of the second and third electrodes 14 to the center of the first electrode 14, respectively. The spacing d between the electrodes 14 is determined by the arrangement of the electrodes 14 and the diameter of the electrodes 14.

[0041] d The reference value is 6.0mm~10.0mm. e The reference value is 28.0mm~32.0mm; The total length of electrode 14 is 85.5 mm. The front 21.0 mm and the rear 5.0 mm of electrode 14 are machined into round bars with a diameter of 4.0 mm to facilitate insertion into the electrode plate for fixation. At the same time, the front 8.0 mm part of electrode 14 needs to be machined with M4 threads, which can be used to connect capacitor 15 and fasten the connection between electrode 14 and electrode plate.

[0042] The sealing assembly also includes an O-ring 18, which is located on the stepped surface of the stepped hole. During the tightening process of the electrode 14, the electrode 14 provides sufficient clamping force to the O-ring 18 to ensure a sealing effect.

[0043] Electrode plate 101, electrode plate 102, mounting plate 103, and light-transmitting plate 104 are made of polytetrafluoroethylene (PTFE), while electrode 14 is made of 316L stainless steel. PTFE possesses excellent corrosion resistance and high-temperature resistance, effectively resisting corrosive chemicals and high-temperature environments that may be generated during the reaction process. 316L stainless steel, due to its high corrosion resistance and oxidation resistance, is particularly suitable for highly corrosive environments, ensuring long-term stability and durability during the discharge process.

[0044] The working principle of this invention is as follows: When the reactor is in use, gas and sewage are introduced into the air inlet 10 and water inlet 12, respectively. After passing through the exhaust pipe 16, the gas is dispersed into multiple small bubbles, increasing the contact area of ​​the gas-liquid cross section. When the power is turned on, the power supply supplies power to the electrode 14, generating a high-voltage pulse discharge between the electrode plate 101 and the electrode plate 102. At the same time, the ultrasonic module 7 accelerates the generation and collapse of bubbles through vibration, generating high temperature and high pressure through cavitation, which excites the bubbles in the chamber 1 under the action of the electric field, forming plasma. The plasma can generate a large number of high-energy electrons, ions and free radicals, which produce oxidation and reduction reactions on pollutants in the water, effectively removing organic pollutants and microorganisms from the water. During the discharge process, the ultraviolet light generated by the plasma is absorbed by the photocatalyst, thereby exciting the photocatalyst to generate electron-hole pairs, further enhancing the degradation rate of pollutants. The operator collects the spectrum generated by the reaction inside the reactor through the light radiation window 8, analyzes the concentration and changes of the reactants and products, and facilitates the adjustment of the flow rate at the air inlet 10 and water inlet 12. The treated gas and liquid are discharged from the reactor through the air outlet 13 and water outlet 11, respectively.

[0045] The electrode plates are connected in series with a high-voltage capacitor 15 to balance the energy distribution. When a certain electrode 14 breaks down due to current concentration, the capacitor 15 will adjust the energy distribution through the charging and discharging process, so that other electrodes 14 can continue to participate in the discharge, avoid the occurrence of short circuit, and ensure that the discharge effect of the entire reactor is uniform.

[0046] It will be apparent to those skilled in the art that the present invention is not limited to the details of the exemplary embodiments described above, and that the invention can be implemented in other specific forms without departing from its spirit or essential characteristics. Therefore, the embodiments should be considered in all respects as exemplary and non-limiting, and the scope of the invention is defined by the appended claims rather than the foregoing description. Thus, all variations falling within the meaning and scope of equivalents of the claims are intended to be included within the present invention. No reference numerals in the claims should be construed as limiting the scope of the claims.

Claims

1. A gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor, characterized in that: The reactor includes a box (1) and a base plate (2). The box (1) is located on the upper surface of the base plate (2). A reactor base (3) is provided on the lower side of the base plate (2). An air inlet (10) is provided on the side wall of the reactor base (3). A water outlet (11) is provided at the bottom of the reactor base (3). An installation cover (5) is provided on the upper side of the box (1). An inlet (12) and an air outlet (13) are provided on the installation cover (5). A discharge assembly is provided inside the box (1). An ultrasonic module (7) and a light radiation window (8) are provided on the outer wall of the box (1). A sealing assembly is provided at the connection of each component inside the box (1). The gas phase inside the box (1) is air, the liquid phase is pure water or water containing pollutants, and the solid phase is small spherical composite catalyst material supported by CQDs.

2. The gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor according to claim 1, characterized in that: The housing (1) includes an electrode plate one (101), an electrode plate two (102), a mounting plate (103), and a light-transmitting plate (104). The electrode plate one (101) and the electrode plate two (102) are located on two opposite sides inside the housing (1). The mounting plate (103) and the light-transmitting plate (104) are located on both sides of the electrode plate one (101). The ultrasonic module (7) is located on the mounting plate (103). The light-transmitting plate (104) has a mounting groove. The light radiation window (8) is located in the mounting groove. A fixing plate (9) is provided on one side of the light radiation window (8). The fixing plate (9) has a through groove with the same shape as the light radiation window (8).

3. The gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor according to claim 2, characterized in that: The cross-sections of the mounting plate (103) and the light-transmitting plate (104) are convex, and the edges of the protruding structures of the mounting plate (103) and the light-transmitting plate (104) are connected to the electrode plate one (101) and the electrode plate two (102) at the step surface.

4. The gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor according to claim 3, characterized in that: The mounting plate (103) and the light-transmitting plate (104) have two waterproof grooves on their raised edges respectively. The sealing assembly includes a circular nitrile rubber strip located in the waterproof groove. A threaded hole is provided between two adjacent waterproof grooves, and a self-tapping screw is provided in the threaded hole.

5. The gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor according to claim 4, characterized in that: The discharge assembly includes several electrodes (14) that are staggered in the horizontal direction. The electrodes (14) interspersedly pass through electrode plate one (101) and semi-embedded electrode plate two (102), while the remaining electrodes (14) pass through electrode plate two (102) and semi-embedded electrode plate one (101). A capacitor (15) is provided at one end of each electrode (14) that passes through electrode plate one (101) and electrode plate two (102). A high-voltage protective cover (6) is provided on each of electrode plate one (101) and electrode plate two (102). The capacitor (15) is located inside the high-voltage protective cover (6). The power supply of the reactor is a nanosecond pulse power supply, which is electrically connected to the capacitor (15).

6. The gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor according to claim 1, characterized in that: The base plate (2) has two sealing grooves (20), the sealing assembly includes a sealing strip (19), the sealing strip (19) is located in the two sealing grooves (20), and a filter screen (17) is provided on the inner side of the base plate (2).

7. The gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor according to claim 6, characterized in that: An exhaust pipe (16) is provided on the inner side of the reactor base (3). The exhaust pipe (16) is connected to the air inlet (10). Multiple branch pipes are provided on one side of the exhaust pipe (16). Multiple air holes are evenly arranged on the branch pipes. An aeration net is provided on the upper side of the exhaust pipe (16). Four supports (4) are provided at the four corners of the lower end face of the reactor base (3).

8. The gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor according to claim 5, characterized in that: The electrode (14) has threads on its front end and body. The electrode plate one (101) and electrode plate two (102) have several stepped holes. The stepped holes are located at the connection between the electrode (14) and the electrode plate one (101) and electrode plate two (102). The capacitor (15) has a threaded hole on one side. The electrode (14) is threadedly connected to the capacitor (15).

9. The gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor according to claim 8, characterized in that: The sealing assembly also includes an O-ring (18) located on the stepped surface of the stepped hole.

10. The gas-liquid-solid three-phase large-area acousto-photocatalytic combined pulsed discharge reactor according to claim 9, characterized in that: The electrode plate one (101), electrode plate two (102), mounting plate (103) and light-transmitting plate (104) are made of polytetrafluoroethylene material, and the electrode (14) is made of 316L stainless steel material.

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