Parallel amplification device of plate type plasma reactor and application of parallel amplification device in synthesis of hydrogen peroxide

Abstract

The invention belongs to the technical field of plasma synthesis of fine chemicals, and relates to a parallel amplification device of a plate type plasma reactor and application of the parallel amplification device in synthesis of hydrogen peroxide. The parallel amplification device comprises a power supply system, an air inlet system, a reactor system and a collection system. High-voltage electrode cavities and grounding electrode cavities of a plurality of reactors are respectively connected together to realize parallel discharge of the plurality of reactors, and a cooling plate circulating coolant is designed between the electrode cavities of the adjacent reactors to realize electrode heat removal. The device provided by the invention can realize continuous, safe and stable synthesis of hydrogen peroxide, and realizes parallel discharge of a plurality of reactors.

Description

Technical Field

[0001] This invention belongs to the field of plasma synthesis of fine chemicals, and relates to a parallel scale-up device for a plate plasma reactor and its application in the synthesis of hydrogen peroxide. Background Technology

[0002] Hydrogen peroxide, as a green oxidant, is widely used in water treatment and environmental remediation, pharmaceutical disinfection, food industry, bleaching, and pulp processing due to its strong oxidizing properties and harmless decomposition. Since its first synthesis from barium peroxide and nitric acid in 1818, hydrogen peroxide has received widespread attention, and today it is recognized as one of the 100 most important chemicals in the world.

[0003] Since its inception in the 1940s, the anthraquinone oxidation process has been the primary method for producing hydrogen peroxide, currently accounting for over 95% of hydrogen peroxide production. The anthraquinone process mainly involves anthraquinone hydrogenation, hydrogen anthraquinone oxidation, hydrogen peroxide extraction, and working fluid purification and recovery. This process involves extensive material recycling, gas compression (hydrogen and air), heating, cooling, and distillation separation, all of which consume significant amounts of electricity and steam, resulting in high overall energy consumption per unit product. Furthermore, the 5,6,7,8-tetrahydroanthraquinone produced by the side reaction reduces the purity and yield of hydrogen peroxide. The reaction also generates waste gas (aromatic vapors), waste liquid (aromatics and alkali), and solid waste (Al₂O₃). In addition, hydrogen peroxide produced by the anthraquinone process presents safety concerns during transportation. These drawbacks have prompted researchers to seek a green technology for the synthesis of hydrogen peroxide. Therefore, the direct synthesis of hydrogen peroxide from hydrogen and oxygen via noble metal catalysis has attracted increasing attention (Edwards JK et al., 2009, DOI:10.1002 / anie.200904115; Freakley SJ et al., 2016, DOI:10.1126 / science.aad5705; Ricciardulli T et al., 2021, DOI:10.1021 / jacs.1c00539). Photocatalysis is another promising approach, making progress in covalent organic frameworks through dynamic charge traps (Ma F et al., 2025, DOI:10.1038 / s41467-025-62286-9), bond engineering (Yang J et al., 2025, DOI:10.1038 / s41467-025-62937-x), and heterocyclic isomer incorporation (Ju Y et al., 2025, DOI:10.1038 / s41467-025-60960-6). Photocatalysis is environmentally friendly and requires less equipment, but its yield is low and it is heavily dependent on the light source, making large-scale production difficult. Electrocatalysis provides a green alternative through two-electron oxygen reduction or water oxidation pathways.Catalysts have evolved from studies on carbon oxide surfaces (Lu Z et al., 2018, DOI:10.1038 / s41929-017-0017-x) and defective graphene oxide (Kim HW et al., 2018, DOI:10.1038 / s41929-018-0044-2) to Co–N–C single-atom catalysts (Jung E et al., 2020, DOI:10.1038 / s41563-019-0571-5) and supramolecular tuning of cobalt phthalocyanine (Lee BH et al., 2023, DOI:10.1038 / s41929-023-00924-5). Although electrochemical methods have shown superior environmental friendliness, their high cost and low yield limit the application of this process.

[0004] Plasma synthesis, a novel technique for the direct synthesis of hydrogen peroxide from hydrogen and oxygen, has garnered significant attention due to its numerous recognized advantages. This method boasts a simple process flow, enabling the reaction to be completed in a single step at ambient temperature and pressure, without the need for any catalysts or solvents. These characteristics allow for the direct production of high-purity (up to electronic grade), high-concentration (up to 90 wt.%) hydrogen peroxide solutions, with water as the sole byproduct. Since this technology eliminates the energy-intensive purification and concentration steps of traditional processes, equipment investment costs are significantly reduced. Furthermore, this technology is suitable for small-scale, on-site preparation applications, thus avoiding the safety risks associated with transporting and storing high-concentration hydrogen peroxide.

[0005] The inventors of this application previously conducted exploratory research on coaxial cylindrical reactors. The reactor evolved from an early single-dielectric barrier discharge (SDBD) design to a crucial self-cooled double-dielectric barrier discharge (DDBD) design. The DDBD reactor, through a dual-water electrode or later a metal powder electrode (MP-DDBD), can generate uniform, dispersed low-temperature plasma. A key characteristic of this plasma is its low electron density and average electron energy. This low electron density and low electron energy characteristic is fundamental to controlling reaction selectivity. Reaction mechanism studies show that the formation of H2O2 follows a chain termination pathway: electron-activated H2 produces H atoms, which react with ground-state O2 to generate the crucial HO2 radical, ultimately composed of two HO2 radicals. The formation of the byproduct H2O and the risk of explosion originate from a branched reaction pathway, which involves highly reactive oxygen species (O, O2). This process is initiated by high electron energy and electron density, and the generation of these reactive oxygen species requires high electron energy and electron density. Furthermore, the study revealed the "single-molecule catalysis" of Ar and H₂O: the metastable state of Ar (Ar... This process selectively promotes the dissociation of H2, while H2O molecules effectively promote the formation and stabilization of the key intermediate HO2, thereby synergistically improving the yield and energy efficiency of H2O2. Ultimately, by employing a continuously operating and parallel-scale-upgraded MP-DDBD reactor, combined with a deep understanding of the reaction mechanism, the safe and stable direct synthesis of electronic-grade high-purity H2O2 with a concentration as high as 65-90 wt.% was achieved within the explosion limits.

[0006] Although coaxial cylindrical reactors have shown great potential in the direct synthesis of hydrogen peroxide from plasma, the transformation of laboratory results into large-scale industrial production inevitably requires an expansion of production capacity. However, the capacity scaling-up path has encountered key bottlenecks: (1) the scheme of increasing the output by increasing the length of a single reactor will cause mechanical vibration during discharge due to the excessive length of the central electrode, which not only affects the stability of the discharge but also brings serious safety hazards; (2) the high-voltage electrode of the tubular reactor is located in the center of the cylinder and is surrounded by H2 / O2 plasma, which cannot come into contact with the cooling medium, resulting in the high-voltage electrode not being cooled efficiently, which makes the tubular reactor susceptible to damage due to the temperature rise of the high-voltage electrode.

[0007] Unlike coaxial cylindrical reactors, plate reactors expose both their high-voltage and grounding electrodes to the external environment, creating favorable conditions for achieving a dual-stability and dual-cooling structure. Based on this consideration, Guo Hongchen, Yi Yanhui, and others invented a plate reactor capable of simultaneously cooling both the high-voltage and grounding electrodes, which was used for the direct synthesis of H2O2 via hydrogen-oxygen plasma (application number: 2024109048531). It is important to note that while filling the high-voltage electrode with cooling oil can provide heat dissipation and insulation against external discharge, a layer of cooling oil inevitably exists between the plate metal electrode immersed in the oil and the barrier medium. This layer of oil, with its high insulation properties, restricts dielectric barrier discharge, significantly increasing the initial discharge voltage and consequently reducing the reaction efficiency and energy efficiency of H2O2 synthesis via dielectric barrier discharge. Summary of the Invention

[0008] This invention improves the high-voltage electrode of a plate reactor by using cooled brine as the electrode and employing an external contact cooling plate. This ensures effective cooling while avoiding insulation issues within the high-voltage electrode, thereby improving reaction efficiency and safety. Based on this improved reactor, multiple plate reactors are connected in parallel by sharing a cooling plate at the same electrode, thus assembling a plate reactor stack. Finally, by integrating the plate reactor stack, power supply matching, cooling system series connection, and feed / discharge piping distribution, a parallel scale-up device for a plate plasma reactor is provided, which is applied to the direct synthesis of hydrogen peroxide from hydrogen and oxygen.

[0009] Simultaneously, modular scale-up integration can be achieved through the parallel connection of cooling and electrode structures. This invention utilizes a plate reactor designed and fabricated using 3D printing technology, which achieves device integration through parallel connection, thereby enabling the scale-up synthesis of hydrogen peroxide.

[0010] This invention is achieved through the following technical solution: A parallel scale-up device for a plate plasma reactor includes a power supply system 1, an air inlet system 2, a reactor system 3, and a collection system 4.

[0011] The power supply system 1 connects the high-voltage electrode chamber and the grounding electrode chamber of all reactors in the reactor system 3.

[0012] The power system 1 is one of AC power, high frequency power, pulse power, transformer drive power and semiconductor power.

[0013] The air intake system 2 is a system in which hydrogen and oxygen are mixed in proportion in a mixing chamber and then introduced into each reactor of the reactor system 3 through a gas distributor.

[0014] The gas splitter is a single-inlet, multi-outlet structure that divides the gas into several outlets for outflow and inflow into the reactor.

[0015] The reactor system 3 includes multiple reactors placed side by side, with the electrode chambers of adjacent reactors being adjacent to each other with the same polarity, and a cooling plate 20 placed between adjacent reactors.

[0016] The cooling plate 20 has a hollow internal structure with an inlet and an outlet, and the coolant circulates inside the cooling plate 20.

[0017] The cooling plate 20 is made of one or more of the following materials: gold, silver, copper, aluminum, silicon, carbon nanotubes, graphite, boron nitride, and copper-aluminum alloy.

[0018] The coolant circulating inside the cooling plate 20 is one or more of the following: water, ethylene glycol, fluorinated liquid, oil, carbon dioxide, ammonia, and liquid nitrogen.

[0019] The cooling plate 20 can simultaneously cool two electrode chambers of adjacent reactors with the same polarity, and all cooling plates 20 are connected in series, with the coolant circulating in all cooling plates 20.

[0020] The reactor system 3 gathers all the high-voltage electrode cavity wires of the reactor together and connects them to the high-voltage line of the power supply system 1, and gathers all the grounding electrode cavity wires together and connects them to the grounding line.

[0021] The collection system 4 connects the product outlet 6 of each reactor to a multi-inlet single-outlet collector, and the outlet of the collector is connected to a gas-liquid separator.

[0022] The gas-liquid separator is connected to the collector outlet at the top. The gas-liquid separator has an outlet on the side and a bottom. The side outlet is used to discharge unreacted gas, and the bottom outlet is used to discharge hydrogen peroxide products.

[0023] The reactor is a plate reactor, comprising a high-voltage electrode chamber, a grounding electrode chamber, and a plasma discharge chamber.

[0024] The high-voltage electrode cavity, the grounding electrode cavity, and the plasma discharge cavity are all located within the outer frame 9. The thickness of the outer frame 9 is greater than the sum of the thicknesses of the high-voltage electrode cavity, the grounding electrode cavity, and the plasma discharge cavity. The high-voltage electrode cavity and the grounding electrode cavity are located on opposite sides of the plasma discharge cavity.

[0025] The plasma discharge cavity is mainly composed of a gas shunt bar 10 and two blocking media 11.

[0026] The outer frame 9 is a plate-like structure with a certain thickness. The middle part is a hollowed-out pentagon with a symmetrical structure. The two adjacent interior angles are right angles, and the side between the two right angles is the bottom side. A gas diversion strip placement platform 18 is provided on the inner side of the bottom side for placing the gas diversion strip 10. In addition to the bottom side, the middle of the inner side of the other sides is provided with an inner boss 17. The inner boss 17 and the gas diversion strip placement platform 18 have a height difference. Two blocking media 11 are installed on the two sides of the inner boss 17 respectively. The shape of the blocking media 11 is the same as the hollowed-out pentagon on the outer frame 9, but the size is different. The side of the gas diversion strip 10 near the cavity is provided with a groove. The two blocking media 11 are clamped in the groove with the corresponding sides of the gas diversion strip 10. The gas diversion strip 10 clamps the two blocking media 11. The other sides of the two blocking media 11 are in close contact with the inner boss 17. A sealed space is formed between the two blocking media 11 as a discharge space.

[0027] The gas diversion strip 10 is provided with several small holes, and a capillary tube 19 is inserted into each small hole; the gas diversion strip 10 is also provided with a protruding collecting channel, one end of the capillary tube 19 is connected to the discharge space, and the other end is gathered into the collecting channel and enters the air inlet 5 on the outer frame 9.

[0028] The high-voltage electrode cavity and the grounding electrode cavity have the same structure, both consisting of a blocking medium 11, an electrode cavity metal mesh 12, an electrode cavity grid 13, an electrode cavity support 14, an outer medium 15 of the electrode cavity, and an outer medium pressure frame 16 of the electrode cavity; the high-voltage electrode cavity and the plasma discharge cavity share a blocking medium 11, and the grounding electrode cavity and the plasma discharge cavity share another blocking medium 11.

[0029] The blocking medium 11, electrode cavity metal mesh 12, electrode cavity grid 13, electrode cavity support 14, electrode cavity outer medium 15, and electrode cavity outer medium pressure frame 16 are all pentagonal, with the same shape as the pentagonal hollowed out of the outer frame 9, but different in size; the size is slightly smaller than the pentagonal space hollowed out of the outer frame 9, but does not reach the root of the inner boss 17.

[0030] The electrode cavity grid 13 and electrode cavity support 14 have a certain thickness; the electrode cavity support 14 is a pentagonal ring structure, which is fitted around the outside of the electrode cavity grid 13. The electrode cavity metal mesh 12 is pressed onto the blocking medium 11 by the electrode cavity grid 13; one side of the electrode cavity grid 13 presses the electrode cavity metal mesh 12, and the other side is attached to the outer medium 15 of the electrode cavity. The outer medium pressure frame 16 of the electrode cavity is a pentagonal ring structure, which is pressed onto the outer medium 15 of the electrode cavity, thereby forming a sealed space inside the electrode cavity grid 13 as the electrode cavity. The electrode cavity is located inside the pentagon hollowed out on the outer frame 9.

[0031] The electrode cavity support 14 and the electrode cavity grid 13 each have a channel on one side of the bottom edge and the side opposite to the bottom edge, which respectively connect to the electrode cavity filling port 7 and the electrode cavity discharge port 8 of the outer frame 9.

[0032] The outer frame 9 is provided with an air inlet 5 and a product outlet 6. The air inlet 5 is located on the outer frame 9 corresponding to the bottom edge of the hollowed-out pentagon, and the product outlet 6 is located at the top of the pentagon structure. The air inlet 5 and the product outlet 6 are coaxial. The inlet end of the air inlet 5 is connected to the outside, and the outlet end is connected to the collecting channel of the gas diversion strip 10. The inlet end of the product outlet 6 is connected to the discharge space, and the outlet end of the product outlet 6 is connected to the outside.

[0033] The outer frame 9 is also provided with two electrode cavity filling ports 7 and two electrode cavity outlet ports 8. The high voltage electrode cavity and the grounding electrode cavity each correspond to one electrode cavity filling port 7 and one electrode cavity outlet port 8.

[0034] The electrode cavity filling port 7 and the electrode cavity outlet port 8 are located at positions corresponding to the electrode cavity; wherein, the electrode cavity filling port 7 is located outside the bottom edge of the hollowed-out pentagon on the outer frame 9, and the electrode cavity outlet port 8 is located outside the outer frame 9 opposite to the electrode cavity filling port.

[0035] The outer frame 9 and the gas diversion strip 10 are printed by 3D printing technology, and the material is one or more of thermoplastic, acrylic, nylon, silicone and resin.

[0036] The material of the blocking medium 11 is one or more of the following: silicate glass, borosilicate glass, borosilicate glass, ordinary glass, tempered glass, glass ceramic, alumina ceramic, polytetrafluoroethylene, non-metallic composite material, and optical glass, with a thickness of 0.5-3mm and a distance of 0.5-10mm between them.

[0037] The outer frame 9 has a length of 100-500mm, a width of 25-300mm, and a thickness of 3-15mm.

[0038] The thickness of the inner boss 17 is 0.5-10mm.

[0039] The electrode cavity metal mesh 12, electrode cavity grid 13, electrode cavity support 14, electrode cavity outer medium 15 and electrode cavity outer medium pressure frame 16 are provided with glue injection gaps at the contact positions with the inner side of the outer frame 9 for glue injection and sealing.

[0040] The injection gap is used to fill the sealant to ensure good airtightness of the reactor; the sealant is one or more of the following: silicone sealant, polyurethane sealant, acrylic sealant, ethylene-propylene sealant, epoxy resin sealant, polysiloxane sealant, and polyurethane silicone sealant.

[0041] The high-voltage electrode cavity and the grounding electrode cavity are filled with conductive material through the electrode cavity filling port 7, and the conductive material is discharged through the electrode cavity outlet 8 after the discharge is completed.

[0042] The conductive material includes solid conductive particles composed of one or more of gold, silver, platinum, palladium, rhodium, iridium, iron, cobalt, nickel, copper, zinc, aluminum and stainless steel, as well as conductive solutions composed of one or more of gold, silver, platinum, palladium, rhodium, iridium, iron, cobalt, nickel, copper, zinc, aluminum, potassium, sodium and mercury.

[0043] The electrode cavity support 14, electrode cavity grid 13, and electrode cavity outer dielectric pressure frame 16 are printed by 3D printing technology, and their materials are one or more of thermoplastic plastic, acrylic, nylon, silicone, and resin.

[0044] The electrode cavity metal mesh 12 is made of one or more of the following materials: gold, silver, platinum, palladium, rhodium, iridium, iron, cobalt, nickel, copper, zinc, aluminum, and stainless steel.

[0045] The electrode cavity outer medium 15 is made of one or more of silicate glass, borosilicate glass, borosilicate glass, ordinary glass, tempered glass, glass ceramic, and optical glass, with a thickness of 0.5-3mm. The distance between the electrode cavity outer medium 15 and the blocking medium 11 is 0.5-10mm.

[0046] The parallel scale-up device of the above-mentioned plate plasma reactor is applied to the direct synthesis of hydrogen peroxide from hydrogen and oxygen. The specific steps are as follows: Step 1. Mix hydrogen and oxygen in a mixing chamber according to a certain ratio, and then introduce the mixture into each reactor; Step 2. Turn on the thermostatic circulation pump to fill the series-connected cooling plates with coolant; Step 3. Turn on the power to start discharging, slowly increase the discharge voltage and adjust the power according to the frequency; the reaction products will be collected by the collector into the gas-liquid separator, and the gas will be discharged from the gas-liquid separator and enter the chromatogram for analysis; Step 4. After the discharge is complete, turn off the thermostatic circulating pump, turn off the power, turn off the gas, and open the bottom outlet switch of the gas-liquid separator to discharge the product.

[0047] The effects and benefits of this invention are as follows: By connecting the high-voltage electrode chambers and grounding electrode chambers of multiple plate reactors together and connecting them to a plasma power source, this invention achieves parallel discharge of multiple reactors. Furthermore, the cooling plates between the reactors enable common cooling between adjacent electrodes. Simultaneously, the electrodes of the same polarity of adjacent reactors are attached to both sides of the cooling plates, preventing discharge between reactors. This achieves safe parallel discharge between multiple reactors. Attached Figure Description

[0048] Figure 1 This is a schematic diagram of a parallel scale-up device for a plate plasma reactor; Figure 2 This is a schematic diagram of a plate reactor; Figure 3 This is a schematic diagram of the decomposition of a plate reactor; Figure 4 Figures (a) to (c) are schematic diagrams of the outer frame of the plate reactor, the gas splitting strip, and the structure after the two are assembled, respectively. Figure 5 This is a schematic diagram of the electrode cavity of a plate reactor. Figure 6 This is a schematic diagram of the electrode cavity of a plate reactor; Figure 7 This is a schematic diagram of heat dissipation from the cooling plate; Figure 8 This is a schematic diagram of multiple plate reactors connected in parallel.

[0049] In the diagram: 1 Power supply system; 2 Inlet system; 3 Reactor system; 4 Collection system; 5 Inlet; 6 Product outlet; 7 Electrode cavity filling port; 8 Electrode cavity outlet; 9 Outer frame; 10 Gas diverter bar; 11 Barrier medium; 12 Metal mesh; 13 Electrode cavity grid; 14 Electrode cavity support; 15 Electrode cavity outer medium; 16 Electrode cavity outer medium pressure frame; 17 Inner boss; 18 Gas diverter bar placement platform; 19 Capillary tube; 20 Cooling plate. Detailed Implementation

[0050] The specific embodiments of the present invention are described in detail below with reference to the technical solutions and accompanying drawings.

[0051] like Figure 1 This is a parallel scale-up device for plate plasma reactors. The entire device includes a power supply system 1, an air intake system 2, a reactor system 3, and a collection system 4. The power supply system 1 connects the high-voltage electrode chamber and the grounding electrode chamber of reactor system 3. The power supply system 1 can be one of AC power, high-frequency power, pulse power, transformer-driven power, or semiconductor power. The air intake system 2 mixes hydrogen and oxygen in a mixing chamber in a specific ratio and then introduces them into each reactor. Reactor system 3 consists of multiple reactors placed side-by-side, with cooling plates 20 placed between adjacent reactors. The side-by-side placement of multiple reactors means that the electrode chambers of adjacent reactors are adjacent at the same pole, and heat is removed between the two electrode chambers of adjacent reactors by the cooling plates 20. The cooling plates 20 are hollowed out and have inlets and outlets for circulating coolant. The high-voltage electrode chamber wires of all reactors in reactor system 3 are collected and connected to the high-voltage line of the power supply system, and the grounding electrode chamber wires are collected and connected to the grounding wire. Reactor system 3 consists of multiple plate reactors placed side-by-side, each plate reactor including a high-voltage electrode chamber, a grounding electrode chamber, and a plasma discharge chamber. The collection system 4 connects the product outlet 6 of each reactor to a multi-inlet, single-outlet collector, whose outlet is connected to a gas-liquid separator. The gas-liquid separator has an outlet at the top connected to the collector's outlet, and one outlet on the side and one at the bottom. The side outlet is used to discharge unreacted gas, and the bottom outlet allows hydrogen peroxide products to be discharged when it is open.

[0052] The plate reactor of the present invention, such as Figure 2-6 As shown. A schematic diagram of the outer frame is shown below. Figure 4 As shown in (a), the outer frame 9 is a plate-like structure with a certain thickness. The center is a hollowed-out pentagon. A gas distribution strip placement platform 18 is provided on the side between the two right angles inside the hollowed-out pentagon for placing the gas distribution strip 10. Inner bosses 17 are provided on the inner sides of the remaining four sides, excluding the side between the two right angles. There is a height difference between the inner bosses 17 and the gas distribution strip placement platform 18. Two blocking media 11 are placed on both sides of the inner bosses 17. The space between the two blocking media 11 constitutes the discharge space. Figure 4 As shown in (b), the gas splitter 10 has several small holes, into which a capillary tube 19 is inserted. All the capillary tubes 19 converge above the small holes of the gas splitter 10 into a collecting channel protruding from the gas splitter 10. The structure of the gas splitter 10 placed on the outer frame 9 is as follows. Figure 4As shown in (c), the outer frame 9 has an air inlet 5, a product outlet 6, a high-voltage electrode cavity filling port, a high-voltage electrode cavity outlet, and a high-voltage electrode cavity discharge port on its outer side. The air inlet 5 and the product outlet 6 are coaxial, with the air inlet 5 located outside the middle side of the two right angles of the hollowed-out pentagon, and the air inlet 5 is connected to the collecting channel of the gas diversion strip 10. The product outlet 6 is located at the top of the pentagonal structure, opposite to the middle side of the two right angles and the air inlet 5. The inlet end of the product outlet 6 is connected to the internal space formed by the hollowed-out pentagonal structure, and the outlet end of the product outlet 6 is connected to the outside. The high-voltage electrode cavity filling port 7 and the high-voltage electrode cavity discharge port 8 are at the same height of the outer frame 9, located on one side of the air inlet 5 and the product outlet 6. The high-voltage electrode cavity filling port 7 is located outside the middle side of the two right angles of the pentagonal space, and the high-voltage electrode cavity discharge port 8 is located outside the outer frame 9 opposite to the high-voltage electrode cavity filling port 7. The structure of the grounding electrode cavity is the same as that of the high-voltage electrode cavity.

[0053] Combination Figure 5 Schematic diagram of the electrode cavity of a plate reactor and Figure 6 A schematic diagram of the electrode cavity of the plate reactor is shown. The high-pressure electrode cavity and the grounding electrode cavity have the same structure, both consisting of a barrier medium 11, an electrode cavity metal mesh 12, an electrode cavity grid 13, an electrode cavity support 14, an outer electrode cavity medium 15, and an outer electrode cavity medium pressure frame 16. The barrier medium 11, electrode cavity metal mesh 12, electrode cavity grid 13, electrode cavity support 14, outer electrode cavity medium 15, and outer electrode cavity medium pressure frame 16 are all pentagonal, slightly smaller than the pentagonal space hollowed out by the outer frame 9, but not reaching the root of the inner boss 17. The electrode cavity metal mesh 12 is pressed onto the barrier medium 11 by the electrode cavity grid 13. The electrode cavity support 14 is fitted around the outside of the electrode cavity grid 13. One side of the electrode cavity grid 13 presses against the electrode cavity metal mesh 12, while the other side is attached to the outer electrode cavity medium 15. The outer electrode cavity medium pressure frame 16 is pressed onto the outer electrode cavity medium 15. The electrode cavity support 14 and the electrode cavity grid 13 each have a channel on one side of the base and the side opposite to the base, which coincides with the electrode cavity filling port 7 and the electrode cavity discharge port 8 of the outer frame 9. The electrode cavity metal mesh 12, the electrode cavity grid 13, the electrode cavity support 14, the electrode cavity outer dielectric 15, and the electrode cavity outer dielectric pressure frame 16 have glue injection gaps on the inner side of the outer frame 9 for glue injection sealing. The electrode cavity is filled with conductive material through the electrode cavity filling port 7, and the conductive material is discharged through the electrode cavity discharge port 8 after discharge.

[0054] like Figure 7 Schematic diagram of heat dissipation from cooling plate and Figure 8The schematic diagram shows multiple plate reactors connected in parallel. Multiple reactors are placed in parallel, with cooling plates 20 positioned between adjacent reactors to absorb heat generated by the electrodes on both sides. A circulating coolant is connected in series between the cooling plates. The high-voltage electrode cavity wires of each reactor are combined and connected to the high-voltage line of the power supply system, while the grounding electrode cavity wires are combined and connected to the ground wire. Furthermore, the electrodes on both sides of the cooling plate 20 are of the same polarity, which prevents discharge between adjacent reactors.

[0055] The scale-up device used in the following embodiments has the following specific parameters: the outer frame 9 of a single reactor is 112.6 mm wide, 180.0 mm long, and 25 mm thick; the barrier medium 11 is made of 1 mm thick ordinary hard glass, 89.6 mm wide and 153.5 mm long; the outer medium 15 of the high electrode cavity is made of 2 mm thick ordinary hard glass, 89.6 mm wide and 153.5 mm long; the inner boss 17 is 3 mm wide and 1.5 mm thick; the air inlet 5 and the product... The diameter of the outlet 6 is 1mm, and the diameters of the inlet 5, product outlet 6, electrode cavity filling port 7, and electrode cavity outlet 8 are 2mm. The electrode cavity support 14 is 89.6mm wide and 153.5mm long. The outer frame 9 is made of R4600 resin, and the electrode cavity support 14, electrode cavity grid 13, and outer dielectric pressure frame 16 are all made of PETG material, all of which are 3D printed. The electrode cavity metal mesh 12 is made of stainless steel. The adhesive used for encapsulation is 704 silicone. The cooling plate is made of aluminum-magnesium-silicon alloy.

[0056] Block the electrode cavity outlet 8, and inject NaCl solution into the high-voltage electrode cavity and grounding electrode cavity of the reactor through the electrode cavity filling port 7. All high-voltage electrode cavities of the reactor are interconnected by wires and connected to the plasma power supply CTP2000K. All grounding electrode cavities are interconnected by wires and grounded. Transformer oil at 0℃ is circulated in the cooling plate 20 cavity.

[0057] pass Figure 1 The overall apparatus shown was used to conduct an experiment on the synthesis of H2O2 using the hydrogen-oxygen plasma method, as detailed below: Example 1 A single reactor is discharged. There is a cooling plate on the outside of the high-voltage electrode chamber and the grounding electrode chamber. The inside of the reactor is rinsed with deionized water for 10 seconds and then the deionized water is blown out with air. Hydrogen and oxygen are mixed evenly through a mass flow meter to make the oxygen content in the hydrogen-oxygen mixture 4 mol%, and the total hydrogen-oxygen gas velocity is 500 ml / min. Then it is introduced into the reactor.

[0058] Connect the AC high-voltage power supply, slowly increase the discharge voltage and adjust the power according to the frequency to adjust the SEI to 4.68kJ / L, discharge for 1 hour, and the oxygen from the tail gas enters the gas chromatograph for analysis. The H2O2 content in the liquid phase is determined by titration using iodometric titration.

[0059] Example 2 Repeat Example 1, with two reactors discharged in parallel, total gas velocity 1000 ml / min, SEI maintained at 4.68 kJ / L, for 1 hour.

[0060] Example 3 Repeat Example 1, with three reactors discharged in parallel, total gas velocity 1500 ml / min, SEI maintained at 4.68 kJ / L, for 1 hour.

[0061] Example 4 Repeat Example 1, with four reactors discharged in parallel, total gas velocity 2000 ml / min, SEI maintained at 4.68 kJ / L, for 1 hour.

[0062] Example 5 Repeat Example 1, with five reactors discharged in parallel, total gas velocity 2500 ml / min, SEI maintained at 4.68 kJ / L, for 1 hour.

[0063] Example 6 Repeat Example 1, with twenty reactors discharged in parallel, a total gas velocity of 10 L / min, and the SEI maintained at 4.68 kJ / L for 1 hour.

[0064] Example 7 Repeat Example 1, with twenty reactors discharged in parallel, a total gas velocity of 10 L / min, and the SEI maintained at 4.68 kJ / L for 120 hours.

[0065] The O2 conversion rate and H2O2 selectivity of each embodiment are shown in Table 1. As can be seen from the table, as the number of reactors increases, the oxygen conversion rate and hydrogen peroxide selectivity remain basically constant, and the hydrogen peroxide production is proportional to the number of parallel reactors, thus achieving parallel discharge reaction of 20 reactors.

[0066] Table 1. O2 conversion rate, H2O2 selectivity, and mass of H2O2 generated in different embodiments.

Claims

1. A parallel scale-up device for a plate plasma reactor, characterized in that, The parallel device of the plate plasma reactor includes a power supply system (1), an air inlet system (2), a reactor system (3), and a collection system (4). The power supply system (1) connects the high-voltage electrode chamber and the grounding electrode chamber of all reactors in the reactor system (3); The aforementioned air intake system (2) is a system in which hydrogen and oxygen are mixed in proportion in a mixing chamber and then introduced into each reactor of the reactor system (3) through a gas distributor; The reactor system (3) includes multiple reactors placed side by side, with the electrode chambers of adjacent reactors being adjacent to each other on the same pole, and a cooling plate (20) placed between adjacent reactors. The reactor system (3) gathers the high-voltage electrode cavity wires of all reactors together and connects them to the high-voltage line of the power supply system (1), and gathers the grounding electrode cavity wires together and connects them to the grounding line. The collection system (4) connects the product outlet (6) of each reactor to a multi-inlet single-outlet collector, the outlet of which is connected to a gas-liquid separator.

2. The parallel scale-up device for a plate plasma reactor according to claim 1, characterized in that, The power supply system (1) is one of AC power supply, high frequency power supply, pulse power supply, transformer drive power supply and semiconductor power supply; The gas splitter is a single-inlet, multi-outlet structure that divides the gas into several outlets for outflow and inflow into the reactor. The gas-liquid separator is connected to the collector outlet at the top. The gas-liquid separator has an outlet on the side and a bottom. The side outlet is used to discharge unreacted gas, and the bottom outlet is used to discharge hydrogen peroxide products.

3. The parallel scale-up device for a plate plasma reactor according to claim 1, characterized in that, The cooling plate (20) has a hollow structure inside and is provided with an inlet and an outlet. The coolant circulates inside the cooling plate (20). The cooling plate (20) is made of one or more of the following materials: gold, silver, copper, aluminum, silicon, carbon nanotubes, graphite, boron nitride, and copper-aluminum alloy. The coolant circulating inside the cooling plate (20) is one or more of the following: water, ethylene glycol, fluorinated liquid, oil, carbon dioxide, ammonia, and liquid nitrogen.

4. The parallel scale-up device for a plate plasma reactor according to claim 1, characterized in that, The reactor is a plate reactor, comprising a high-voltage electrode chamber, a grounding electrode chamber, and a plasma discharge chamber; The high-voltage electrode cavity, the ground electrode cavity, and the plasma discharge cavity are all located inside the outer frame (9). The thickness of the outer frame (9) is greater than the sum of the thicknesses of the high-voltage electrode cavity, the ground electrode cavity, and the plasma discharge cavity. The high-voltage electrode cavity and the ground electrode cavity are located on both sides of the plasma discharge cavity. The plasma discharge cavity is mainly composed of a gas splitter bar (10) and two blocking media (11); The outer frame (9) is a plate-like structure with a certain thickness. The middle part is a hollowed-out pentagon. The pentagon is a symmetrical structure, where two adjacent interior angles are right angles. The side between the two right angles is the bottom side. A gas distribution strip placement platform (18) is provided on the inner side of the bottom side for placing the gas distribution strip (10). In addition to the bottom side, an inner boss (17) is provided in the middle of the inner side of the other sides. There is a height difference between the inner boss (17) and the gas distribution strip placement platform (18). Two blocking media are installed on the two sides of the inner boss (17). (11); The shape of the blocking medium (11) is the same as the pentagon hollowed out on the outer frame (9), but the size is different; the gas diversion strip (10) has a groove on the side near the cavity, and the two blocking media (11) are stuck in the groove with the corresponding sides of the gas diversion strip (10). The two blocking media (11) are clamped by the gas diversion strip (10), and the remaining sides of the two blocking media (11) are in close contact with the inner boss (17). A closed space is formed between the two blocking media (11) as a discharge space; The gas diversion strip (10) is provided with several small holes, and a capillary tube (19) is inserted into each small hole; the gas diversion strip (10) is also provided with a protruding collection channel, one end of the capillary tube (19) is connected to the discharge space, and the other end is gathered into the collection channel and then enters the air inlet (5) on the outer frame (9); The high-voltage electrode cavity and the grounding electrode cavity have the same structure, both consisting of a blocking medium (11), an electrode cavity metal mesh (12), an electrode cavity grid (13), an electrode cavity support (14), an outer dielectric (15) of the electrode cavity, and an outer dielectric pressure frame (16) of the electrode cavity; the high-voltage electrode cavity and the plasma discharge cavity share a blocking medium (11), and the grounding electrode cavity and the plasma discharge cavity share another blocking medium (11). The blocking medium (11), electrode cavity metal mesh (12), electrode cavity grid (13), electrode cavity support (14), electrode cavity outer medium (15), and electrode cavity outer medium pressure frame (16) are all pentagonal, which are the same shape as the pentagonal hollowed out of the outer frame (9), but different in size; the size is slightly smaller than the pentagonal space hollowed out of the outer frame (9), but does not reach the root of the inner boss (17); The electrode cavity grid (13) and electrode cavity support (14) have a certain thickness; the electrode cavity support (14) is a pentagonal ring structure, which is fitted on the outside of the electrode cavity grid (13); the electrode cavity metal mesh (12) is pressed by the electrode cavity grid (13) onto the blocking medium (11); the electrode cavity grid (13) presses the electrode cavity metal mesh (12) on one side and attaches to the electrode cavity outer medium (15) on the other side; the electrode cavity outer medium pressure frame (16) is a pentagonal ring structure, which is pressed onto the electrode cavity outer medium (15), thereby forming a closed space inside the electrode cavity grid (13) as the electrode cavity, and the electrode cavity is located in the pentagon hollowed out on the outer frame (9); The electrode cavity support (14) and the electrode cavity grid (13) each have a channel on one side of the bottom edge and the side opposite to the bottom edge, which respectively connect to the electrode cavity filling port (7) and the electrode cavity outlet (8) of the outer frame (9); The outer frame (9) is provided with an air inlet (5) and a product outlet (6). The air inlet (5) is located on the outer frame (9) corresponding to the bottom edge of the hollowed-out pentagon, and the product outlet (6) is located at the top of the pentagon structure. The air inlet (5) and the product outlet (6) are coaxial. The inlet end of the air inlet (5) is connected to the outside, and the outlet end is connected to the collection channel of the gas diversion strip (10). The inlet end of the product outlet (6) is connected to the discharge space, and the outlet end of the product outlet (6) is connected to the outside. The outer frame (9) is also provided with two electrode cavity filling ports (7) and two electrode cavity outlet ports (8). The high voltage electrode cavity and the grounding electrode cavity each correspond to one electrode cavity filling port (7) and one electrode cavity outlet port (8). The electrode cavity filling port (7) and electrode cavity outlet (8) are located at positions corresponding to the electrode cavity; wherein, the electrode cavity filling port (7) is located outside the bottom edge of the hollowed-out pentagon on the outer frame (9), and the electrode cavity outlet (8) is located outside the outer frame (9) opposite to the electrode cavity filling port.

5. The parallel scale-up device for a plate plasma reactor according to claim 1, characterized in that, The outer frame (9) and gas diversion strip (10) are printed by 3D printing technology and are made of one or more of thermoplastic plastic, acrylic, nylon, silicone and resin. The material of the blocking medium (11) is one or more of the following: silicate glass, borosilicate glass, borosilicate glass, ordinary glass, tempered glass, glass ceramics, alumina ceramics, polytetrafluoroethylene, non-metallic composite materials, and optical glass.

6. The parallel scale-up device for a plate plasma reactor according to claim 1, characterized in that, The thickness of the blocking medium (11) is 0.5-3mm, and the distance between them is 0.5-10mm; The outer frame (9) is 100-500mm long, 25-300mm wide, and 3-15mm thick; The thickness of the inner boss (17) is 0.5-10mm.

7. The parallel scale-up device for a plate plasma reactor according to claim 1, characterized in that, The electrode cavity metal mesh (12), electrode cavity grid (13), electrode cavity support (14), electrode cavity outer medium (15) and electrode cavity outer medium pressure frame (16) are provided with glue injection gaps at the contact positions with the inner side of the outer frame (9) for glue injection and sealing. The injection gap is used to fill the sealant to ensure good airtightness of the reactor; the sealant is one or more of the following: silicone sealant, polyurethane sealant, acrylic sealant, ethylene-propylene sealant, epoxy resin sealant, polysiloxane sealant, and polyurethane silicone sealant.

8. The parallel scale-up device for a plate plasma reactor according to claim 1, characterized in that, The high-voltage electrode cavity and the grounding electrode cavity are filled with conductive material through the electrode cavity filling port (7), and the conductive material is discharged through the electrode cavity outlet (8) after the discharge is completed. The conductive material includes solid conductive particles composed of one or more of gold, silver, platinum, palladium, rhodium, iridium, iron, cobalt, nickel, copper, zinc, aluminum and stainless steel, as well as conductive solutions composed of one or more of gold, silver, platinum, palladium, rhodium, iridium, iron, cobalt, nickel, copper, zinc, aluminum, potassium, sodium and mercury.

9. A parallel scale-up device for a plate plasma reactor according to claim 1, characterized in that, The electrode cavity support (14), electrode cavity grid (13), and electrode cavity outer dielectric pressure frame (16) are printed by 3D printing technology, and their materials are one or more of thermoplastic plastic, acrylic, nylon, silicone, and resin. The electrode cavity metal mesh (12) is made of one or more of the following materials: gold, silver, platinum, palladium, rhodium, iridium, iron, cobalt, nickel, copper, zinc, aluminum, and stainless steel. The electrode cavity outer medium (15) is made of one or more of the following materials: silicate glass, borosilicate glass, borosilicate glass, ordinary glass, tempered glass, glass ceramic, and optical glass, with a thickness of 0.5-3mm. The distance between the electrode cavity outer medium (15) and the blocking medium (11) is 0.5-10mm.

10. The application of a parallel scale-up device for a plate plasma reactor according to any one of claims 1-9 in the synthesis of hydrogen peroxide, characterized in that, The specific steps are as follows: Step 1. Mix hydrogen and oxygen in a mixing chamber according to a certain ratio, and then introduce the mixture into each reactor; Step 2. Turn on the thermostatic circulation pump to fill the series-connected cooling plates with coolant; Step 3. Turn on the power to start discharging, slowly increase the discharge voltage and adjust the power according to the frequency; the reaction products will be collected by the collector into the gas-liquid separator, and the gas will be discharged from the gas-liquid separator and enter the chromatogram for analysis; Step 4. After the discharge is complete, turn off the thermostatic circulating pump, turn off the power, turn off the gas, and open the bottom outlet switch of the gas-liquid separator to discharge the product.

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