DBD low-temperature plasma assisted gas-solid system catalytic reaction device

Abstract

The invention relates to the technical field of plasma catalysis, and particularly discloses a DBD low-temperature plasma assisted gas-solid system catalytic reaction device which comprises a continuous filler unit, a low-temperature plasma coupling thermal catalysis unit and a product separation unit which are sequentially connected in series, the continuous filler unit is provided with a filler buffer cavity, the low-temperature plasma coupling thermocatalysis unit is provided with a flue gas heating cavity and a DBD array tube in the flue gas heating cavity, and the flue gas heating cavity is configured with a convection and radiation composite heating mode; and the product separation unit comprises a product buffer cavity and a reverse shutter gas-solid separation structure. Through the design of'filler-reaction-separation 'three-cavity series connection and continuous flow of the catalyst, controllable descending and cyclic regeneration of catalyst particles in the reactor are achieved, the defects that a traditional DBD reactor catalyst is fixedly placed, the filling amount is small, and continuous operation cannot be achieved are overcome, the DBD reactor can adapt to high-temperature thermocatalytic reaction, and the service life of the DBD reactor is prolonged. The method is suitable for various plasma gas-solid catalytic systems such as pyrolysis gas catalytic hydrogenation and CO2 hydrogenation.

Description

Technical Field

[0001] This application relates to the field of plasma catalysis technology, and in particular to a DBD low-temperature plasma-assisted gas-solid system catalytic reaction device. Background Technology

[0002] Plasma catalysis technology, due to its unique reaction characteristics, has broad application prospects in energy and chemical engineering, environmental governance, and new material preparation. It can be applied to various scenarios such as nuclear fusion, plasma torch gasification and melting, plasma wastewater purification, and industrial fertilizer production. Among these, plasma generated by dielectric barrier discharge (DBD) offers advantages such as mild reaction conditions, flexible operation, and high energy utilization. When coupled with thermocatalysis, DBD low-temperature plasma can effectively activate reaction molecules, lower the reaction energy barrier, and significantly improve catalytic reaction efficiency and target product selectivity. Simultaneously, this coupled process can efficiently utilize fluctuating renewable electricity from wind and solar power, achieving cascaded energy utilization and low-carbon conversion, thus becoming an important research direction in the field of plasma catalysis.

[0003] In large-scale industrial production, catalytic reaction devices need to have the ability to operate continuously and stably. Currently, the large-scale industrial application of plasma-coupled thermocatalysis technology is mainly concentrated in high-temperature processes above 1000 °C, such as the gasification and melting treatment of industrial solid waste; while for low-temperature plasma catalysis in the range of several hundred degrees Celsius, related research and applications are mostly still in the laboratory pilot stage, making it difficult to achieve continuous industrial operation.

[0004] Due to limitations in the discharge principle and reaction characteristics of DBD low-temperature plasma, the suitable gas-solid reaction space is small. To ensure discharge stability, the catalyst needs to be fixed, which leads to the following problems: the catalyst loading capacity is limited, failing to meet the catalyst dosage requirements of industrial reactions; and it is difficult to achieve continuous feeding of gas-solid reactants and continuous discharge of reaction products. Currently, some plasma catalytic reactions that do not require heating (such as plasma catalytic conversion of pollutants in water or the atmosphere) have proposed using multi-tube array DBD plasma reactors. However, multi-tube arrays occupy a large space, and traditional thermocatalytic reactors mostly use resistance wire heating furnace radiation heating mode, making it difficult to achieve uniform heating of multiple tubes in a large space. Furthermore, it is difficult to accurately match the catalytic requirements in terms of reactor structure and temperature field distribution, further restricting the industrial scale-up of DBD low-temperature plasma in the field of thermocatalysis.

[0005] Therefore, overcoming the technical limitations imposed by the DBD plasma discharge principle, solving problems such as insufficient filling volume and inadequate catalytic efficiency due to fixed catalyst placement, and achieving continuous feeding and efficient contact between gas-solid reactants and catalyst; and simultaneously developing a heating method adapted to the multi-tube array plasma generation structure to achieve efficient matching between the plasma generation module and the heating module, thereby promoting the industrial continuous operation of DBD low-temperature plasma-assisted gas-solid thermocatalytic reaction device, has become a key technical challenge for the large-scale application of this technology. Summary of the Invention

[0006] To address the problems of fixed catalyst placement, low packing volume, difficulty in achieving continuous operation, and difficulty in matching multi-tube arrays and thermocatalytic systems in existing DBD plasma-assisted coupled thermocatalytic reactors, this application provides a DBD low-temperature plasma-assisted gas-solid system catalytic reactor.

[0007] The DBD low-temperature plasma-assisted gas-solid catalytic reaction device provided in this application adopts the following technical solution: A DBD low-temperature plasma-assisted gas-solid catalytic reaction device includes a continuous packing unit, a low-temperature plasma coupled thermal catalytic unit, and a product separation unit connected in series from top to bottom. The continuous packing unit includes a packing buffer chamber, and the upper part of the packing buffer chamber is provided with at least one gas inlet and at least one solid inlet; The low-temperature plasma coupled thermal catalytic unit includes a flue gas heating chamber and a DBD array tube disposed inside it. The packing buffer chamber and the flue gas heating chamber are separated by a buffer chamber bottom plate. The buffer chamber bottom plate is provided with several material discharge holes for connecting the packing buffer chamber and the DBD array tube. The flue gas heating chamber heats the DBD array tube using a combined convection heat transfer and thermal radiation mode. The product separation unit includes a product buffer chamber connected to the lower opening of the DBD array tube. The bottom of the product buffer chamber is connected to a main product channel, which is surrounded by multiple reverse louvered plates. A solid product outlet is provided at the lower part of the main product channel. A gas collection chamber is provided around the main product channel. Several openings for connecting the main product channel and the gas collection chamber are provided on the reverse louvered plates. A gas product outlet is provided on the gas collection chamber.

[0008] Furthermore, the reverse louver plate is provided with louver blades that correspond one-to-one with the openings, which are used to guide the gas in the main product channel to the gas collection chamber. The louver blades are tilted outwards, and their extension direction is opposite to the downward direction of the material in the main product channel.

[0009] Furthermore, the gas product outlet is connected to a negative pressure device to guide the gas down along the DBD array tube and the product buffer chamber, and then through the main product channel and the gas collection chamber before being discharged.

[0010] Furthermore, the volume of the gas collecting chamber is greater than the volume of the main product channel.

[0011] Furthermore, it also includes a stirring mechanism, which includes a stirring shaft that is axially disposed in the packing buffer chamber, the flue gas heating chamber and the product buffer chamber, and a plurality of stirring blades fixed to the stirring shaft; the stirring blades are located in the packing buffer chamber and the product buffer chamber.

[0012] Furthermore, the stirring paddle inside the packing buffer chamber is positioned close to the bottom plate of the buffer chamber to push and squeeze solid materials into the DBD array tube.

[0013] Furthermore, the solid inlet extends to the bottom of the packing buffer chamber and above the stirring area of ​​the agitator.

[0014] Furthermore, when the device is used for gas-solid catalytic reaction, solid catalyst particles fall from the packing buffer chamber into the DBD reaction tube and accumulate to form a moving catalytic bed. Under the propulsion of the stirring paddle and the control of solid product outlet discharge, the catalyst moves downward at a continuous and controllable rate. After the reaction, the waste catalyst is discharged through the product separation unit, regenerated by the external regeneration equipment, and returned to the continuous packing unit to form a catalyst circulation loop.

[0015] Furthermore, the flue gas heating chamber is provided with a hot flue gas inlet and an exhaust gas outlet, and a resistance wire heating device is provided on the wall of the flue gas heating chamber; the resistance wire heating device and the hot flue gas work together to control the temperature.

[0016] This application also provides the application of the aforementioned DBD low-temperature plasma-assisted gas-solid system catalytic reaction device in gas-solid mixed catalytic processes.

[0017] In summary, this application includes at least one of the following beneficial technical effects: 1. This application adopts an array structure with multiple DBD reaction tubes arranged in parallel, which effectively improves the problems of small catalyst filling amount and insufficient reaction space in a single reaction tube; at the same time, it adopts a composite heating mode that combines large-space hot flue gas convection heat exchange with traditional electric heating furnace wall radiation, enabling the reaction device to operate stably under high temperature conditions and meet the requirements of high-temperature plasma-assisted thermocatalytic reaction.

[0018] 2. Through the structural design of a three-chamber interconnected series of "packing-reaction-separation" and a dual-zone coaxial stirring mode, continuous flow of catalyst particles in the reaction device is achieved. This design overcomes the shortcomings of existing DBD reactors, which can only be fed intermittently due to the fixed placement of the catalyst and cannot operate continuously for a long time.

[0019] 3. This application adopts a design of unloading reverse louvered louvers and gas collection chamber to increase the gas escape space. With the help of a negative pressure device, the gas is guided to flow in a directional manner. On the one hand, the gas and solid are forced to flow downward in the same direction, so that the gaseous reactants and solid catalysts can fully contact each other to improve the catalytic pyrolysis efficiency. On the other hand, the gaseous products are directionally discharged from the louvered window into the gas collection chamber for collection, realizing gas-solid separation and avoiding the safety hazards caused by excessive material accumulation pressure.

[0020] 4. This device can not only be used as an independent reaction unit for various gas-solid-thermal catalytic systems, but also as an auxiliary unit in chemical systems to connect with multi-step processes; any technical solution involving gas-solid-thermal catalytic reactions can be inspired by this application and applied or modified. Attached Figure Description

[0021] Figure 1 This is a schematic diagram of the overall structure of a DBD low-temperature plasma-assisted gas-solid catalytic reaction device according to an embodiment of this application; Figure 2 This is a schematic diagram of the DBD array transistor structure in an embodiment of this application; Figure 3 This is a structural schematic diagram of the reverse louver panel, which is mainly used to illustrate the embodiments of this application.

[0022] Reference numerals: 1. Continuous packing unit; 2. Low-temperature plasma coupled thermocatalysis unit; 3. Product separation unit; 101. Packing buffer chamber; 102. First gas inlet; 103. Second gas inlet; 104. Stirring mechanism; 105. Catalyst inlet; 106. Stirring paddle; 107. Stirring shaft; 201. Flue gas heating chamber; 202. Hot flue gas inlet; 203. DBD array tube; 204. Tail gas outlet; 205. Metal electrode rod; 206. Metal electrode mesh; 207. Resistance wire heating device; 301. Product buffer chamber; 302. Product main channel; 303. Gas collection chamber; 304. Gas product outlet; 305. Solid product outlet; 306. Louver blade; 307. Opening. Detailed Implementation

[0023] The following is in conjunction with the appendix Figure 1-3 This application will be described in further detail.

[0024] This application discloses a DBD low-temperature plasma-assisted gas-solid catalytic reaction device for catalytic hydrogenation of biomass pyrolysis gas. This reaction device is connected downstream of the biomass pyrolysis reactor as a hydrogenation unit. The pyrolysis gas produced by biomass pyrolysis includes oxygen-containing macromolecules such as aldehydes, ketones, and acids, hydrocarbon macromolecules such as aromatics, and CO produced by pyrolysis volatilization. x H2 and C x H y Small molecule gases are introduced into this reaction device through an insulated pipe as reactants. The catalysts used in this reaction device include, but are not limited to, nickel-supported alumina, titanium dioxide, zeolite molecular sieves, molybdenum oxide, and other catalysts with hydrogenation catalytic activity. This embodiment uses a spherical Ni-Mo / ZSM5 catalyst as an example for illustration.

[0025] Reference Figure 1 The DBD low-temperature plasma-assisted gas-solid catalytic reaction device includes a continuous packing unit 1, a low-temperature plasma coupled thermal catalytic unit 2, and a product separation unit 3 connected in series from top to bottom.

[0026] Among them, reference Figure 1 The continuous packing unit 1 includes a packing buffer chamber 101. The upper part of the packing buffer chamber 101 is provided with a first gas inlet 102, a second gas inlet 103, and a catalyst inlet 105, which are used to input pyrolysis gas, hydrogen, and solid catalyst, respectively. The bottom of the packing buffer chamber 101 is provided with a buffer chamber bottom plate, and the buffer chamber bottom plate has several material discharge holes.

[0027] Reference Figure 1 and Figure 2 The low-temperature plasma coupled thermal catalytic unit 2 includes a flue gas heating chamber 201 and a DBD array tube 203 disposed inside it. The DBD array tube 203 has openings at both ends. Its upper opening is connected to the packing buffer chamber 101 through a material drop hole on the bottom plate of the buffer chamber, and its lower opening is connected to the product separation unit 3 through a through hole on the bottom plate of the flue gas heating chamber 201.

[0028] The flue gas heating chamber 201 uses a combined convection heat transfer and thermal radiation mode to heat the DBD array tube 203, as shown in the reference. Figure 1 The flue gas heating chamber 201 has a hot flue gas inlet 202 on one side and an exhaust gas outlet 204 on the other side. At the same time, a resistance wire heating device 207 is installed on the wall.

[0029] This embodiment involves the catalytic hydrogenation reaction of biomass pyrolysis gas (such as aldehydes, ketones, hydrocarbons, etc.) at a temperature of 400-600 °C and atmospheric pressure, catalyzed by Ni-Mo / ZSM5 to produce aromatics, alkanes, and cycloalkanes. The hydrogenation reaction temperature used in this embodiment is 500 °C. To provide the heat required for the reaction, this embodiment employs a composite heating mode combining large-space hot flue gas convection heat exchange with traditional electric heating furnace wall radiation. High-temperature flue gas introduced through hot flue gas inlet 202 acquires heat through convection heat exchange within the flue gas heating chamber 201. The heat-exchanged flue gas becomes low-temperature tail gas and is discharged through tail gas outlet 204. The hot flue gas temperature is 650 °C, and its source is the waste tail gas from the waste incinerator. Simultaneously, the resistance wire heating device 207 is set to 500 °C and temperature is controlled collaboratively by a PID control module.

[0030] The DBD array tube 203 serves as the reaction space and discharge medium for the catalytic hydrogenation of biomass pyrolysis gas. The DBD array tube 203 is an insulating medium, simultaneously acting as a reaction space carrier and a discharge blocking medium. Materials include, but are not limited to, glass, ceramics, polymers, mica, and other special materials, and the material selection depends on the required reaction temperature. In this embodiment, the required reaction temperature is 500 °C; therefore, an alumina corundum ceramic reaction tube is selected.

[0031] Reference Figure 1 and Figure 2 The DBD array tube 203 has a metal electrode rod 205 inside and a metal electrode mesh 206 on the outside. In this device, the DBD array tube 203 is composed of at least two reaction tubes arranged in an orderly array. In this embodiment, an array of 8 tubes in parallel is used, which are evenly distributed inside the flue gas heating chamber 201.

[0032] This device applies alternating current between the metal electrode rod 205 inside the DBD array tube 203 and the external metal electrode mesh 206. Through the dielectric barrier effect of the ceramic reaction tube, a uniform low-temperature plasma field can be generated between the electrodes to assist catalytic hydrogenation. This can improve the activity of reactants, the catalytic performance of the catalyst, and eliminate carbon deposits from side reactions, thereby improving the catalytic hydrogenation effect.

[0033] Since the catalytic hydrogenation reaction of pyrolysis gas is usually accompanied by side reactions such as carbon deposition and coking, long-term operation can easily lead to the accumulation of contaminants in the ceramic reaction tube, resulting in a reduction in effective reaction space, difficulty in catalyst flow, and a decrease in catalytic efficiency. To improve this problem, the DBD array tube 203 of this device adopts a detachable design, with its two ends connected to the bottom plate of the buffer chamber and the bottom plate of the heating chamber, respectively. The connection methods include, but are not limited to, bayonet connection, bolt connection, and tenon and mortise connection. In this embodiment, bolt connection is used.

[0034] In the low-temperature plasma-coupled thermocatalytic unit 2, the following reactions mainly occur: catalytic hydrogenation of biomass pyrolysis gas (such as aldehydes, ketones, hydrocarbons, etc.) to aromatics, alkanes, and cycloalkanes is carried out under Ni-Mo / ZSM5 catalysis at 400-600 °C and atmospheric pressure. Subsequently, the hydrogenation products (aromatics, alkanes, and cycloalkanes) and the catalyst enter the product separation unit 3 for gas-solid separation.

[0035] Reference Figure 1 The product separation unit 3 includes a product buffer chamber 301 connected to the lower opening of the DBD array tube 203. The bottom of the product buffer chamber 301 is connected to a product main channel 302. The product main channel 302 is surrounded by multiple reverse louvered plates. A sealed gas collection chamber 303 is coaxially surrounded outside the product main channel 302. A solid product outlet 305 is provided at the lower part of the product main channel 302. The solid product outlet 305 is equipped with a discharge valve.

[0036] Reference Figure 1 and Figure 3 The reverse louver panel includes a rectangular plate, with four reverse louvers forming a quadrangular prism-shaped main product channel 302. Several horizontal strip-shaped openings 307 are provided on the plate, connecting the main product channel 302 to the gas collection chamber 303. The volume of the gas collection chamber 303 is larger than that of the main product channel 302, and the pressure inside the gas collection chamber 303 is lower than that inside the main product channel 302, allowing the gaseous products in the main product channel 302 to easily escape from the openings 307 on the reverse louvers into the gas collection chamber 303.

[0037] A gas product outlet 304 is provided on the gas collection chamber 303. The gas product outlet 304 is connected to a negative pressure device to guide the gas downwards along the DBD array tube 203 and the product buffer chamber 301, and then sequentially through the main product channel 302 and the gas collection chamber 303 before being discharged. In one embodiment, the gas product outlet 304 can be connected to a condensing device via an insulated pipe for the separation of the target product (light aromatics) and byproduct (CO). x H2 and C x H y The non-condensable gas is condensed and separated; the condensation device is connected to negative pressure devices such as induced draft fans to facilitate gas pressure balance and gas flow.

[0038] To guide the gaseous products in the main product channel 302 to escape into the gas collection chamber 303, refer to Figure 1 and Figure 3Each of the multiple openings 307 of the reverse louver panel is equipped with a corresponding louver blade 306, the lower side of which is fixed to the outer side of the panel. The louver blades 306 are inclined outwards, their extension direction being opposite to the downward direction of the material in the main product channel 302. The inclination angle of the louver blades 306 is 30-60°, which is beneficial for guiding the high-temperature gas in the main product channel 302 to the gas collection chamber 303. If the inclination angle of the louver blades 306 is too small, the gap between the louver blades 306 and the openings 307 will be too small, which will not be conducive to the escape of gas in the main product channel 302; if the inclination angle of the louver blades 306 is too large, the guiding effect of the louver blades 306 on the gas flow will be insufficient.

[0039] To prevent solid material in the main product channel 302 from being squeezed out from the opening 307 on the reverse louver plate, the opening 307 on the reverse louver plate is covered with a louver plate screen, the pore size of which is smaller than the diameter of the catalyst used.

[0040] To prevent minute fly ash or carbon fragments from being discharged with the gaseous products, the gaseous product outlet 304 is covered with a screen. Further, refer to... Figure 1 The gas product outlet 304 is located on the upper side of the gas collecting chamber 303, higher than the solid product outlet 305, allowing fly ash or carbon fragments in the gas collecting chamber 303 to settle under gravity. In conjunction with the position of the gas product outlet 304, the lower part of the gas collecting chamber 303 has a conical structure, which facilitates the upward flow of gas in the gas collecting chamber 303 and its discharge from the gas product outlet 304. Furthermore, the conical structure at the bottom of the gas collecting chamber 303, the conical structure at the bottom of the reaction chamber, and the tilt direction of the louver blades 306 help optimize the directional flow path of gas in the gas collecting chamber 303.

[0041] Since gas-solid catalytic reactions are usually accompanied by side reactions, prolonged operation can easily lead to condensation and blockage at the outlet, causing certain safety hazards. To improve this problem, the reverse louver plate of this device is detachably connected to the lower part of the product buffer chamber 301, and the connection method includes, but is not limited to, bayonet connection, screw connection, tenon and mortise connection, etc.

[0042] To improve heat and mass transfer and mixing efficiency, refer to Figure 1 The reaction apparatus is also equipped with a stirring mechanism 104. The stirring mechanism 104 includes a stirring shaft 107 that is axially disposed in the packing buffer chamber 101, the flue gas heating chamber 201, and the product buffer chamber 301, and a plurality of stirring paddles 106 fixed to the stirring shaft 107; the stirring paddles 106 are located in the packing buffer chamber 101 and the product buffer chamber 301. The stirring paddles 106 may adopt a ribbon type, screw type, paddle type, anchor type, or other structures.

[0043] Furthermore, refer to Figure 1The stirring paddle 106 inside the packed buffer chamber 101 is positioned near the bottom plate of the buffer chamber and is used to push and compress the solid material into the DBD array tube 203. Solid catalyst particles fall from the packed buffer chamber 101 into the DBD reaction tube 203 and accumulate to form a moving catalyst bed. Under the pushing of the stirring paddle 106 and the control of the solid product outlet 305 discharge valve, the catalyst moves downward at a continuous and controllable rate.

[0044] To achieve catalyst recycling, the spent catalyst, after separation, can be regenerated by a riser regeneration device at 700-900 °C under air combustion conditions to remove surface carbon before re-entering the continuous packed unit 1 for a new round of catalysis. In this embodiment, the spent catalyst regeneration temperature is 800 °C. To prevent the high-temperature regenerated catalyst and the reaction gas from prematurely contacting and reacting in the packed buffer chamber 101, refer to... Figure 1 The catalyst inlet 105 extends to the bottom of the packing buffer chamber 101 and above the stirring area of ​​the agitator 106, so that the catalyst can directly contact the agitator 106 after falling, thereby entering the DBD array tube 203 as soon as possible, minimizing the contact between the catalyst and the pyrolysis gas and hydrogen, and avoiding violent reactions in the packing buffer chamber.

[0045] When the device in this embodiment is applied to the low-temperature plasma-assisted biomass pyrolysis gas catalytic hydrogenation process, its working mode is as follows: pyrolysis gas is introduced through the first gas inlet 102, hydrogen gas is introduced through the second gas inlet 103, and Ni-Mo / ZSM5 catalyst is introduced through the catalyst inlet 105. The solid catalyst descends sequentially within the three-chamber system of "packing-catalysis-separation" in the reactor. Under atmospheric pressure, 500 ℃ high temperature, and plasma conditions, the pyrolysis gas reactants undergo catalytic hydrogenation to produce aromatics, alkanes, and cycloalkanes. A negative pressure device guides the gas flow in a directional manner, forcing the gas and solid to flow downwards in the same direction, ensuring sufficient contact between the gaseous reactants and the solid catalyst to improve catalytic hydrogenation efficiency. Due to the special structure of the main product channel 302 and the gas collection chamber 303, the spent solid catalyst is discharged through the solid product outlet 305 at the bottom of the reactor. After subsequent recycling and regeneration, it re-enters the packing buffer chamber 101 for a new round of downward reaction. Meanwhile, the gaseous products escape directionally to the gas collection chamber 303 and are discharged through the gas product outlet 304. After subsequent condensation and separation, hydrocarbon liquid fuel is obtained.

[0046] The aforementioned device can be applied not only to gas-solid thermocatalytic processes such as catalytic hydrogenation of pyrolysis gas and gas-phase catalytic deposition of low-carbon hydrocarbons to produce carbon nanomaterials, which require high-temperature reactions, but also to CO2 hydrogenation processes with lower-temperature reaction requirements. This can be achieved simply by adjusting the combined heating mode of large-space hot flue gas convection heat exchange with traditional electric heating furnace wall radiation and the configuration of relevant reactant inlets. Through ingenious structural design, including a three-chamber series connection, a combined heating mode, and a detachable reverse louvered gas collection chamber, it can achieve efficient operation of large-scale DBD array tubes under high-temperature thermocatalytic conditions while effectively separating gas and solid products, ensuring continuous, safe, and stable operation of the device. This device can be used as an independent reaction unit for various gas-solid thermocatalytic systems, or as an auxiliary unit in chemical systems to integrate with multi-step processes. Any gas-solid thermocatalytic reaction can be inspired, applied, and modified based on the device described in this application.

[0047] The above are all preferred embodiments of this application, and are not intended to limit the scope of protection of this application. Therefore, all equivalent changes made in accordance with the structure, shape and principle of this application should be covered within the scope of protection of this application.

Claims

1. A DBD low-temperature plasma-assisted gas-solid catalytic reaction device, characterized in that: It includes a continuous packing unit, a low-temperature plasma-coupled thermocatalytic unit, and a product separation unit connected in series from top to bottom; The continuous packing unit includes a packing buffer chamber, and the upper part of the packing buffer chamber is provided with at least one gas inlet and at least one solid inlet; The low-temperature plasma coupled thermal catalytic unit includes a flue gas heating chamber and a DBD array tube disposed inside it. The packing buffer chamber and the flue gas heating chamber are separated by a buffer chamber bottom plate. The buffer chamber bottom plate is provided with several material discharge holes for connecting the packing buffer chamber and the DBD array tube. The flue gas heating chamber heats the DBD array tube using a combined convection heat transfer and thermal radiation mode. The product separation unit includes a product buffer chamber connected to the lower opening of the DBD array tube. The bottom of the product buffer chamber is connected to a main product channel, which is surrounded by multiple reverse louvered plates. A solid product outlet is provided at the lower part of the main product channel. A gas collection chamber is provided around the main product channel. Several openings for connecting the main product channel and the gas collection chamber are provided on the reverse louvered plates. A gas product outlet is provided on the gas collection chamber.

2. The DBD low-temperature plasma-assisted gas-solid catalytic reaction device according to claim 1, characterized in that: The reverse louver plate is provided with louver blades that correspond one-to-one with the openings, which are used to guide the gas in the main product channel to the gas collection chamber. The louver blades are tilted and open outwards, and their extension direction is opposite to the downward direction of the material in the main product channel.

3. The DBD low-temperature plasma-assisted gas-solid catalytic reaction device according to claim 2, characterized in that: The gas product outlet is connected to a negative pressure device to guide the gas down along the DBD array tube and the product buffer chamber, and then through the main product channel and the gas collection chamber before being discharged.

4. The DBD low-temperature plasma-assisted gas-solid catalytic reaction device according to claim 3, characterized in that: The volume of the gas collecting chamber is greater than the volume of the main product channel.

5. The DBD low-temperature plasma-assisted gas-solid catalytic reaction device according to claim 1, characterized in that: It also includes a stirring mechanism, which includes a stirring shaft that is axially disposed in the packing buffer chamber, the flue gas heating chamber and the product buffer chamber, and a plurality of stirring blades fixed to the stirring shaft; the stirring blades are located in the packing buffer chamber and the product buffer chamber.

6. The DBD low-temperature plasma-assisted gas-solid catalytic reaction device according to claim 5, characterized in that: The stirring paddle inside the packing buffer chamber is positioned close to the bottom plate of the buffer chamber and is used to push and squeeze solid materials into the DBD array tube.

7. The DBD low-temperature plasma-assisted gas-solid catalytic reaction device according to claim 6, characterized in that: The solid inlet extends to the bottom of the packing buffer chamber and above the stirring area of ​​the agitator.

8. The DBD low-temperature plasma-assisted gas-solid catalytic reaction device according to claim 6, characterized in that: When the device is used for gas-solid catalytic reaction, solid catalyst particles fall from the packing buffer chamber into the DBD reaction tube and accumulate to form a moving catalytic bed. Under the impetus of the stirring paddle and the control of solid product discharge, the catalyst moves downward at a continuous and controllable rate. After the reaction, the waste catalyst is discharged through the product separation unit, regenerated by the external regeneration equipment, and returned to the continuous packing unit to form a catalyst circulation loop.

9. The DBD low-temperature plasma-assisted gas-solid catalytic reaction device according to claim 1, characterized in that: The flue gas heating chamber is provided with a hot flue gas inlet and an exhaust gas outlet, and a resistance wire heating device is provided on the wall of the flue gas heating chamber; the resistance wire heating device and the hot flue gas work together to control the temperature.

10. The application of the DBD low-temperature plasma-assisted gas-solid system catalytic reaction device according to any one of claims 1-9 in a gas-solid mixed catalytic process.

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