System and method for plasma-driven co-pyrolysis of biomass and hydrogen-rich feedstock for upgrading

Abstract

The application relates to the field of biomass high-value technology, and particularly discloses a plasma-driven biomass and hydrogen-rich material synergistic pyrolysis upgrading system and method, which comprises a pyrolysis reaction system, a plasma synergistic upgrading reaction system and a condensation system. In the pyrolysis reaction system, a hydrogen-rich material pyrolysis reactor and a biomass pyrolysis reactor pyrolyze corresponding raw materials respectively, and a valve is switched to select a gas / gas or gas / solid synergistic reaction mode. The plasma synergistic upgrading reaction system excites plasma through dielectric barrier discharge, catalytically hydrogenates and deoxidizes pyrolysis gas online, and outputs target hydrogenation products. The condensation system separates hydrogenation products into gas and liquid. The application has the advantages of gas / gas or gas / solid modes, utilizes hydrogen-rich material pyrolysis gas and biomass pyrolysis gas to perform synergistic catalytic hydrogenation reaction under normal pressure, generates high-value hydrocarbon liquid fuel, has good applicability to different types of biomass, and has the advantages of high raw material utilization rate, convenient flexible regulation and control and high safety compared with traditional processes.

Description

Technical Field

[0001] This application relates to the field of biomass value enhancement technology, and in particular to a plasma-driven synergistic pyrolysis system and method for upgrading biomass and hydrogen-rich feedstock. Background Technology

[0002] With the increasing global demand for sustainable energy and environmentally friendly materials, the efficient synergistic conversion technology of biomass and hydrogen-rich feedstocks has become a research hotspot. Biomass (crop straw, sawdust, etc.), as an important renewable resource, suffers from technical bottlenecks in direct upgrading processes due to the oxygen-containing characteristics of its pyrolysis products, such as low hydrodeoxygenation efficiency and severe coking. Pyrolysis of hydrogen-rich feedstocks (plastics, rubber, etc.) can produce valuable pyrolysis products, such as olefins and aromatics. However, when processing these pyrolysis products alone, the product distribution is complex, the yield of high-quality products is low, and carbon deposition is easily generated during pyrolysis, affecting the stable operation of the pyrolysis equipment. By synergistically processing biomass and hydrogen-rich feedstocks, the hydrogen-rich gas from the pyrolysis of hydrogen-rich feedstocks can be used as a hydrogen source for the hydrodeoxygenation of the gaseous volatiles from biomass pyrolysis, reducing the need for additional hydrogen.

[0003] The current defects of biomass and hydrogen-rich feedstock co-conversion technology are mainly reflected in: (1) the single reaction mode cannot adapt to the differences in physical properties of multiple biomass sources, resulting in insufficient precision in the regulation of oxygen-containing components; (2) the hydrogen source allocation strategy is rigid and it is difficult to cope with the dynamic changes in feedstock supply; (3) the process of pre-hydrogenation and deep hydrogenation is separated, resulting in low hydrogen energy utilization efficiency. Summary of the Invention

[0004] The inventive concept of this application is as follows: Using hydrogen-rich feedstock pyrolysis gas as an independent hydrogen source for direct hydrogenation and upgrading of biomass pyrolysis gas (gas-gas mode) can reduce the external hydrogen supply requirement by utilizing its hydrogen-rich characteristics. However, for high-oxygen biomass (such as straw-based herbaceous feedstocks), its deoxygenation efficiency is limited by the insufficient depth of the single-stage hydrogenation reaction. While a gas-solid synergistic mode (gas-solid mode) in which hydrogen-rich feedstock pyrolysis gas is pre-introduced into the biomass pyrolysis section can achieve preliminary deoxygenation in the pyrolysis stage through in-situ hydrogenation, thereby improving hydrogenation efficiency, it consumes some active hydrogen components, leading to the need for a higher amount of hydrogen to be added in subsequent upgrading stages. More importantly, biomass types differ significantly: hardwood feedstocks (such as pine) have high lignin content and relatively low oxygen content in their pyrolysis gas, making them suitable for direct gas-gas synergistic hydrogenation; while gramineous feedstocks (such as straw) have a high cellulose / hemicellulose ratio and high oxygen content in their pyrolysis gas, requiring flexible selection and combination of gas-solid mode pre-hydrogenation and gas-gas mode deep deoxygenation to achieve efficient conversion and flexible control of multiple biomass sources. In addition, the supply of hydrogen-rich feedstock fluctuates in actual production. When raw materials such as plastics are sufficient, the gas-gas mode can give full play to its hydrogen source advantage; while when the supply is insufficient, the gas-solid mode can prioritize ensuring the pretreatment needs of high oxygen content biomass.

[0005] To address the shortcomings of current technologies for the co-conversion of biomass and hydrogen-rich feedstocks, this application provides a plasma-driven system and method for the co-pyrolysis and upgrading of biomass and hydrogen-rich feedstocks.

[0006] The plasma-driven biomass and hydrogen-rich feedstock co-pyrolysis upgrading system provided in this application adopts the following technical solution: A plasma-driven biomass and hydrogen-rich feedstock co-pyrolysis and upgrading system includes: A pyrolysis reaction system includes a hydrogen-rich feedstock pyrolysis reactor, a biomass pyrolysis reactor, and a valve connecting the two. The hydrogen-rich feedstock pyrolysis reactor is connected to a hydrogen-rich feedstock pyrolysis gas discharge pipe. The biomass pyrolysis reactor is provided with a gas inlet and is connected to a biomass pyrolysis gas discharge pipe. The valve is used to guide the hydrogen-rich feedstock pyrolysis gas discharged from the hydrogen-rich feedstock pyrolysis reactor into the hydrogen-rich feedstock pyrolysis gas discharge pipe or into the biomass pyrolysis reactor through the gas inlet. The plasma-assisted quality improvement reaction system includes a assisted reactor that uses dielectric barrier discharge technology to generate plasma for online catalytic hydrogenation and deoxygenation of pyrolysis gas; the assisted reactor is connected to the hydrogen-rich feedstock pyrolysis gas discharge pipeline and the biomass pyrolysis gas discharge pipeline. A condensation system is used to perform gas-liquid separation on the hydrogenation products of the plasma-assisted quality improvement reaction system.

[0007] This application achieves flexible switching between gas-gas mode and gas-solid mode by switching the flow direction of hydrogen-rich feedstock pyrolysis gas through valve switching, and is applicable to various reaction systems with different oxygen contents and different hydrogen-rich feedstock supply.

[0008] The gas-gas mode is primarily used when hydrogen-rich feedstock is readily available. In this mode, the valve is closed, and the hydrogen-rich feedstock pyrolysis gas enters the co-catalytic reactor through the pyrolysis gas discharge pipe, where it undergoes a co-catalytic hydrogenation reaction with the biomass pyrolysis gas already entering the reactor. The hydrogen-rich components in the pyrolysis gas can be excited to generate hydrogen plasma, thereby reducing energy consumption and the amount of external hydrogen used by the hydrogenation module, using the pyrolysis gas as an effective hydrogen source.

[0009] The gas-solid mode is mainly used when hydrogen-rich feedstock is plentiful but relatively scarce. In this mode, the valve is opened, and the hydrogen-rich feedstock pyrolysis gas enters the biomass pyrolysis reactor through the gas inlet. It undergoes a co-pyrolysis reaction with the biomass solids, and the hydrogen-rich feedstock pyrolysis gas pre-hydrogenates the biomass to improve the efficiency of subsequent reactions. The biomass pyrolysis gas discharged from the biomass pyrolysis reactor enters the co-reactor for catalytic hydrogenation.

[0010] The combination of the two modes highlights the flexible control capability of this application for multi-source biomass. It can select the most suitable reaction mode according to the supply of hydrogen-rich feedstock and the oxygen content of biomass, effectively solving the technical problems in the prior art where a single reaction mode cannot adapt to the differences in the physical properties of multi-source biomass and the rigid hydrogen source allocation strategy is difficult to cope with the dynamic changes in feedstock supply. This improves the system's adaptability to different biomass feedstocks and the overall reaction efficiency.

[0011] Furthermore, the co-reactor is equipped with multiple high-voltage electrodes arranged in a ring and multiple concentrically arranged ring-shaped grounding electrodes.

[0012] Furthermore, the lower part of the synergistic reactor is provided with a conical cavity, and the inner wall of the conical cavity is provided with a helical track.

[0013] Helical orbitals are used to ensure sufficient contact between the catalyst and reactants, thereby improving catalytic efficiency and helping to reduce coking.

[0014] Furthermore, the condensation system includes multiple condensation tanks connected in series.

[0015] Multiple condensers connected in series perform multi-stage condensation of the hydrogenation products.

[0016] Furthermore, the co-reactor is connected to a reaction product discharge pipe, the reaction product discharge pipe is connected to a circulating gas discharge pipe, the outlet end of the circulating gas discharge pipe is connected to the co-reactor, and a circulating gas pump is installed on the circulating gas discharge pipe.

[0017] By using a bypass reflux recycling method, part of the hydrogenation product is recycled back to the co-reactor to achieve secondary or multiple hydrogenation, thereby realizing cyclic hydrogenation. The pyrolysis gas that was not fully reacted in the first reaction is recycled for hydrogenation reaction, thereby improving the overall conversion rate.

[0018] Furthermore, it also includes a regeneration system for regenerating the spent catalyst produced by the co-reactor and re-introducing it into the co-reactor.

[0019] Furthermore, it also includes a separation system for separating the regenerated catalyst and hot air output from the regeneration system, and inputting a portion of the regenerated catalyst into the co-reactor.

[0020] This application also provides a plasma-driven synergistic pyrolysis and upgrading method for biomass and hydrogen-rich feedstock, including the following steps: Hydrogen-rich feedstock and biomass pyrolysis: Hydrogen-rich feedstock and carrier gas are fed into the hydrogen-rich feedstock pyrolysis reactor, where the hydrogen-rich feedstock pyrolysis produces hydrogen-rich feedstock pyrolysis gas and solid products; biomass feedstock and carrier gas are fed into the biomass pyrolysis reactor, where the biomass pyrolysis produces biomass pyrolysis gas and pyrolysis char; by opening or closing valves and selecting gas-to-gas or gas-to-solid mode, the hydrogen-rich feedstock pyrolysis gas is introduced into the hydrogen-rich feedstock pyrolysis gas discharge pipe or introduced into the biomass pyrolysis reactor through the gas inlet; Pyrolysis gas co-processed online upgrading and hydrogenation: using dielectric barrier discharge technology to generate plasma for online catalytic hydrogenation and deoxygenation of pyrolysis gas; Product condensation and separation: The hydrogenation products of the plasma-coordinated upgrading reaction system are separated into gas and liquid phases by a condensation system.

[0021] Furthermore, in gas-gas mode, the valve is closed, and the hydrogen-rich feedstock pyrolysis gas enters the co-reactor through the hydrogen-rich feedstock pyrolysis gas discharge pipe, where it undergoes a co-catalytic hydrogenation reaction with the biomass pyrolysis gas entering the co-reactor.

[0022] Furthermore, in the gas-solid mode, the valve is opened, and the hydrogen-rich feedstock pyrolysis gas enters the biomass pyrolysis reactor through the gas inlet, where it undergoes a co-pyrolysis reaction with the biomass solid. The hydrogen-rich feedstock pyrolysis gas also pre-hydrogenates the biomass pyrolysis gas. The pyrolysis gas discharged from the biomass pyrolysis reactor enters the co-reactor for catalytic hydrogenation.

[0023] In summary, the gas-gas / gas-solid dual-mode synergistic mechanism of this application enables the cascade hydrogenation of biomass pyrolysis gas and flexible allocation of hydrogen sources, and has the following significant advantages: 1. Wide adaptability to raw materials: In response to the differences in oxygen content characteristics of different biomass raw materials (hardwood, herbaceous plants, etc.), the system can be flexibly switched between gas-solid mode pre-hydrogenation (suitable for high oxygen content straw) and gas-gas mode deep deoxygenation (suitable for low oxygen content pine). While ensuring hydrogenation efficiency, the system improves its adaptability to different biomass raw materials and has a high raw material utilization rate. This is different from the existing single reaction mode technology and effectively solves the problem of insufficient precision in oxygen content component control. 2. Dynamic control of hydrogen source: The flow direction of hydrogen-rich feedstock pyrolysis gas is switched by valves, which is convenient to control. When the hydrogen-rich feedstock is sufficient, the gas-gas mode is activated to directly utilize its hydrogen-rich characteristics to excite plasma, reducing the demand for external hydrogen supply. When the hydrogen-rich feedstock is scarce, the gas-solid mode is switched to prioritize the pre-hydrogenation of high oxygen-containing biomass to alleviate the pressure of subsequent hydrogen addition and ensure the stable operation of the system under hydrogen source fluctuations. This effectively solves the problem of rigid hydrogen source allocation strategy in the existing technology and improves the practicality and stability of the technology. 3. Dual improvement in energy efficiency and product quality: Plasma-assisted catalysis technology activates hydrogen radicals in situ through dielectric barrier discharge, achieving molecular-level reconstruction of pyrolysis gas under normal pressure with high safety; combined with catalyst helical orbital enhanced contact, it improves hydrodeoxygenation efficiency while reducing coking rate; 4. Process integration and low carbonization: Through the catalyst regeneration system and heat self-supply design, the recycling of spent catalysts and the self-balancing of reaction heat energy are realized, and the overall energy consumption is reduced compared with the traditional multi-stage hydrogenation process.

[0024] 5. Dual-mode synergistic combined with circulating hydrogenation: Based on the gas-gas / gas-solid dual-mode synergistic mechanism, bypass reflux circulating hydrogenation is carried out, and part of the hydrogenation products are recycled back to the synergistic reactor to achieve secondary or multiple hydrogenation. This allows circulating hydrogenation to better adapt to different reaction stages and different feed characteristics, further improving the overall conversion rate. Attached Figure Description

[0025] Figure 1 This is a schematic diagram of the overall structure of the plasma-driven biomass and hydrogen-rich feedstock synergistic pyrolysis and upgrading system according to an embodiment of this application; Figure 2 This is a schematic diagram of the structure of the plasma-assisted quality improvement reactor according to an embodiment of this application; Figure 3 This is a schematic diagram of the gas-solid process in the plasma-driven synergistic pyrolysis and upgrading method for biomass and hydrogen-rich feedstock in the embodiments of this application. Figure 4 This is a schematic diagram of the gas-to-gas flow path in the plasma-driven synergistic pyrolysis and upgrading method for biomass and hydrogen-rich feedstock in the embodiments of this application.

[0026] Figure reference numerals: 1. Pyrolysis reaction system; 101. Hydrogen-rich feedstock pyrolysis reactor; 102. Hydrogen-rich feedstock inlet; 103. Inert gas inlet I; 104. Solid product outlet; 105. Hydrogen-rich feedstock pyrolysis gas valve; 106. Biomass pyrolysis reactor; 107. Biomass inlet; 108. Inert gas inlet II; 109. Biomass pyrolysis char outlet; 110. Outlet; 111. Hydrogen-rich feedstock pyrolysis gas outlet; 112. Gas inlet; 2. Plasma-coordinated quality improvement reaction system; 201. Co-reactor; 202. Catalyst inlet; 203. Regenerated catalyst inlet; 204. Waste catalyst outlet; 205. Reaction product outlet; 206. Hydrogen inlet; 207. High-voltage electrode; 208. Reaction product discharge pipeline; 209. Circulating gas outlet; 210. Circulating gas inlet; 211. Circulating gas pump; 212. Condensate discharge pipeline; 213. Circulating gas discharge pipeline; 214. Hydrogen-rich feedstock pyrolysis gas discharge pipeline; 215. Biomass pyrolysis gas discharge pipeline; 3. Condensation system; 301. First condenser; 302. Reaction product inlet; 303. Non-condensable gas outlet; 304. Condensate outlet; 305. Second condenser; 306. Third condenser; 4. Regeneration system; 401. Catalyst regenerator; 402. Regeneration mixture outlet; 403. Used catalyst inlet; 404. Air inlet; 405. Re-separation insulated pipe; 406. Used catalyst discharge pipe; 5. Separation system; 501. Separator; 502. Air outlet; 503. Regenerated mixture inlet; 504. Catalyst regeneration outlet I; 505. Separator valve; 506. Catalyst regeneration outlet II; 507. Regenerated catalyst discharge pipe. Detailed Implementation

[0027] The following is in conjunction with the appendix Figure 1-4 This application will be described in further detail.

[0028] Example 1 This application discloses a plasma-driven synergistic pyrolysis and upgrading system for biomass and hydrogen-rich feedstock. For example... Figure 1 As shown, the plasma-driven biomass and hydrogen-rich feedstock co-pyrolysis upgrading system includes a pyrolysis reaction system 1, a plasma co-upgrading reaction system 2, and a condensation system 3.

[0029] like Figure 1 As shown, the pyrolysis reaction system 1 includes a hydrogen-rich feedstock pyrolysis reactor 101 and a biomass pyrolysis reactor 106, which are used to pyrolyze the hydrogen-rich feedstock and biomass to produce hydrogen-rich feedstock pyrolysis gas and biomass pyrolysis gas, respectively. A valve 105 is connected between the hydrogen-rich feedstock pyrolysis reactor 101 and the biomass pyrolysis reactor 106.

[0030] The hydrogen-rich feedstock pyrolysis reactor 101 is connected to a hydrogen-rich feedstock pyrolysis gas discharge pipe 214, and the biomass pyrolysis reactor 106 is equipped with a gas inlet 112 and is connected to a biomass pyrolysis gas discharge pipe 215. When the hydrogen-rich feedstock is sufficient, valve 105 is closed, and the hydrogen-rich feedstock pyrolysis gas is introduced into the hydrogen-rich feedstock pyrolysis gas discharge pipe 214 (gas-gas mode), directly utilizing its hydrogen-rich characteristics to excite plasma and reducing the external hydrogen supply requirement. When the hydrogen-rich feedstock is scarce, valve 105 is opened, and the hydrogen-rich feedstock pyrolysis gas is introduced into the biomass pyrolysis reactor 106 through the gas inlet 112 (gas-solid mode), prioritizing pre-hydrogenation of high-oxygen-content biomass to alleviate subsequent hydrogenation pressure and ensure stable system operation under hydrogen source fluctuations.

[0031] The plasma-assisted quality improvement reaction system 2 includes a assisted reactor 201, which uses dielectric barrier discharge technology to generate plasma and perform online catalytic hydrogenation and deoxygenation on pyrolysis gas; the assisted reactor 201 is connected to the hydrogen-rich feedstock pyrolysis gas discharge pipe 214 and the biomass pyrolysis gas discharge pipe 215.

[0032] The condensation system 3 is used for gas-liquid separation of the hydrogenation products of the plasma-coordinated mass enhancement reaction system 2.

[0033] The plasma-driven biomass and hydrogen-rich feedstock co-pyrolysis upgrading system provided in this embodiment combines gas-gas / gas-solid reactions. By exciting plasma through dielectric barrier discharge technology, a catalytic hydrogenation reaction is carried out between the pyrolysis gas of hydrogen-rich feedstock and the pyrolysis gas of biomass under normal pressure. This achieves molecular-level co-reforming of the biomass pyrolysis gas and the cracked gas of hydrogen-rich feedstock, generating high-value-added hydrocarbon liquid fuels. This system improves upon the significant shortcomings of traditional processes, such as lengthy processes, large material losses, and high energy consumption. Furthermore, the online upgrading reaction is easy to control and is suitable for various reaction systems with different oxygen contents and different hydrogen-rich feedstock supply amounts, facilitating the design of multi-reaction integration and compact reactors.

[0034] In this embodiment, as Figure 1 As shown, the hydrogen-rich feedstock pyrolysis reactor 101 is also equipped with a hydrogen-rich feedstock inlet 102, an inert gas inlet 1103, a solid product outlet 104, and a hydrogen-rich feedstock pyrolysis gas outlet 111.

[0035] Specifically, the hydrogen-rich feed inlet 102 is located at the top of the hydrogen-rich feed pyrolysis reactor 101 for introducing the hydrogen-rich feed. Hydrogen-rich feed includes, but is not limited to, waste plastics (polyethylene, polypropylene, polystyrene, polyvinyl chloride, etc.), methanol, rubber, and greases; this embodiment does not limit the specific materials. In this particular embodiment, the hydrogen-rich feed is waste polyethylene (PE), and the waste plastic pyrolysis temperature is set to 500-800℃. In this particular embodiment, the waste plastic pyrolysis temperature is set to 600℃, and the heat is self-supplied by the heat within the hydrogen-rich feed pyrolysis reactor 101.

[0036] Furthermore, such as Figure 1 As shown, the inert gas inlet I103 is located on the side of the pyrolysis reactor 101. The inert gas inlet I103 is used to add inert gas, commonly nitrogen, argon, or industrially usable pyrolysis tail gas. The solid product outlet 104 is located at the bottom of the hydrogen-rich feedstock pyrolysis reactor 101 and is used to discharge solid products. The hydrogen-rich feedstock pyrolysis gas outlet 111 is located at the top of the hydrogen-rich feedstock pyrolysis reactor 101 and is connected to the hydrogen-rich feedstock pyrolysis gas discharge pipe 214. The hydrogen-rich feedstock pyrolysis gas outlet 111 is used to discharge hydrogen-rich feedstock pyrolysis gas.

[0037] like Figure 1As shown, the biomass pyrolysis reactor 106 is also equipped with a biomass feed inlet 107, an inert gas inlet II 108, an outlet 110, and a gas inlet 112.

[0038] Specifically, the biomass inlet 107 is located at the top of the biomass pyrolysis reactor 106 for feeding biomass, which includes, but is not limited to, crop straw, fruit peels, fruit pits, bagasse, sawdust, and livestock manure. This embodiment does not limit the specific biomass used. In this particular embodiment, the biomass is rice straw. The biomass pyrolysis temperature is set to 400-800℃; in this particular embodiment, the biomass pyrolysis temperature is set to 600℃, and the heat is self-supplied by the biomass pyrolysis reactor 106.

[0039] Furthermore, such as Figure 1 As shown, the inert gas inlet II108 is located on the side of the biomass pyrolysis reactor 106. The inert gas inlet II108 is used to add inert gas, commonly nitrogen, argon, or industrially usable pyrolysis tail gas. The biomass pyrolysis char outlet 109 is located at the bottom of the biomass pyrolysis reactor 106 and is used to discharge pyrolysis char. The gas inlet 112 is located at the top of the biomass pyrolysis reactor 106 and is used to introduce hydrogen-rich feedstock pyrolysis gas. The gas inlet 112 is connected to the hydrogen-rich feedstock pyrolysis gas outlet 111.

[0040] like Figure 1 As shown, the co-reactor 201 is equipped with a catalyst inlet 202, a high-voltage electrode 207, a reaction product outlet 205, and a hydrogen inlet 206.

[0041] Specifically, the top of the co-reactor 201 is connected to the outlet 110 via a biomass pyrolysis gas discharge pipe 215, through which biomass pyrolysis gas enters the co-reactor 201; at the same time, the top of the co-reactor 201 is connected to a hydrogen-rich feedstock pyrolysis gas discharge pipe 214, through which hydrogen-rich feedstock pyrolysis gas enters the co-reactor 201.

[0042] Furthermore, the catalyst inlet 202 is located at the top of the cylindrical cavity for adding the catalyst. The catalyst type includes, but is not limited to, metal oxide catalysts and zeolite molecular sieve catalysts; the specific type can be selected according to the target product requirements. In this embodiment, a nickel-molybdenum oxide catalyst with granular titanium dioxide as a support is used. The reaction product outlet 205 is used to discharge the hydrogenation product. The hydrogen inlet 206 is used to replenish the hydrogen supply.

[0043] In this embodiment, as Figure 1 and Figure 2As shown, multiple high-voltage electrodes 207 are arranged in a ring structure in the co-reactor 201, and multiple ring-shaped grounding electrodes are arranged concentrically. Both the high-voltage electrodes 207 and the grounding electrodes are covered with an insulating medium, the material of which includes, but is not limited to, quartz, ceramic, etc. Highly active plasma is generated in situ through dielectric barrier discharge between the high-voltage electrodes 207 and the grounding electrodes. The co-reactor 201 uses the plasma and catalyst to perform online catalytic hydrogenation and deoxygenation of the pyrolysis gas to generate hydrogenation products.

[0044] The temperature of the online catalytic hydrodeoxygenation in the co-reactor 201 is 300-600℃, and the heat is supplied by the heat generated by the combustion in the catalyst regenerator 401 through the regenerated catalyst.

[0045] like Figure 1 and Figure 2 As shown, the lower part of the co-reactor 201 is provided with a conical cavity, and the inner wall of the conical cavity is a spiral track. Due to the different radial forces, the catalyst will spirally roll and sink in the reactor cavity, so that the catalyst and reactants can fully contact and react, thereby improving the catalytic efficiency and helping to reduce coking, thus alleviating the problem of catalyst carbon deposition and deactivation.

[0046] The hydrogen-rich raw material pyrolysis gas discharge pipe 214 and the biomass pyrolysis gas discharge pipe 215 are insulated pipes. The waste plastic pyrolysis gas is insulated through the hydrogen-rich raw material pyrolysis gas discharge pipe 214, and the biomass pyrolysis gas is insulated through the biomass pyrolysis gas discharge pipe 215.

[0047] In this embodiment, as Figure 1 and Figure 2 As shown, the bottom of the co-reactor 201 is provided with a spent catalyst outlet 204. Specifically, the spent catalyst outlet 204 is located at the bottom of the conical cavity and is used to discharge the spent catalyst.

[0048] like Figure 1 As shown, the bottom of the co-reactor 201 is also connected to a reaction product discharge pipe 208. A reaction product outlet 205 is provided on the side of the reaction product discharge pipe 208, and a used catalyst outlet 204 is provided at the bottom of the reaction product discharge pipe 208. The reaction product discharge pipe 208 is vertically arranged so that solid particles (used catalyst) sink down and are discharged along the reaction product discharge pipe 208, and the reaction product (gaseous) is extracted through the side of the reaction product discharge pipe 208.

[0049] The condensation system 3 includes a first condensation tank 301, a second condensation tank 305, and a third condensation tank 306 connected in series. The first condensation tank 301 is provided with a reaction product inlet 302, and the third condensation tank 306 is provided with a condensate outlet 304 and a non-condensable gas outlet 303. The reaction product inlet 302 is connected to the reaction product outlet 205. The reaction product enters the first condensation tank 301 through the reaction product inlet 302. The first condensation tank 301, the second condensation tank 305, and the third condensation tank 306 are used in sequence to condense the reaction product to obtain condensate and non-condensable gas. The condensate outlet 304 is used to discharge the condensate, and the non-condensable gas outlet 303 is used to discharge the non-condensable gas.

[0050] In this embodiment, both the condensate and the non-condensable gas are effective products. The pyrolytic carbon can be used to prepare carbon materials, including but not limited to carbon fertilizer, activated carbon, carbon electrode carbon, etc. The condensate, depending on the catalyst used, includes but is not limited to one or more types of aromatics, alkanes, and olefins. The non-condensable gas mainly consists of CO2, CO, and a small amount of low-carbon hydrocarbons, which can be subsequently used as gaseous fuels or chemical raw materials.

[0051] In this embodiment, as Figure 1 As shown, it also includes a condensate discharge pipe 212 and a recirculating gas discharge pipe 213. The hydrogenation product is divided into a first part and a second part. One end of the condensate discharge pipe 212 is connected to the reaction product outlet 205, and the other end of the condensate discharge pipe 212 is connected to the reaction product inlet 302, so that the first part of the reaction product is discharged into the first condensation tank 301. A recirculating gas outlet 209 is provided on the condensate discharge pipe 212, and a recirculating gas inlet 210 is provided on the co-reactor 201. One end of the recirculating gas discharge pipe 213 is connected to the recirculating gas outlet 209, and the other end of the recirculating gas discharge pipe 213 is connected to the recirculating gas inlet 210, so that the second part of the hydrogenation product enters the co-reactor 201 for recirculating hydrogenation.

[0052] In this embodiment, the condensate discharge pipe 212 and the circulating gas discharge pipe 213 are both insulated pipes, which are used to insulate the hydrogenation products of the first part and the hydrogenation products of the second part, respectively.

[0053] By using a bypass reflux recycling method, part of the hydrogenation product is recycled back to the co-reactor 201 to achieve secondary or multiple hydrogenation, and the pyrolysis gas that was not fully reacted in the first reaction is recycled for hydrogenation reaction, thereby improving the overall conversion rate.

[0054] Furthermore, such as Figure 1As shown, a circulating gas pump 211 is installed on the circulating gas discharge pipe 213. The circulating gas pump 211 is used to extract the hydrogenation product of the second part for circulating hydrogenation. The ratio of hydrogenation product condensation to circulation is controlled by the power of the circulating gas pump 211, wherein the circulation flow rate through the circulating pump does not exceed 80% of the flow rate of the reaction product flowing out of the reaction product outlet 205.

[0055] like Figure 1 As shown in the embodiment of this application, the plasma-driven biomass and hydrogen-rich feedstock co-pyrolysis upgrading system also includes a regeneration system 4, which is used to regenerate the waste catalyst generated by the co-reactor 201 and re-input it into the co-reactor 201.

[0056] Specifically, such as Figure 1 As shown, the regeneration system 4 includes a spent catalyst discharge pipe 406 and a catalyst regenerator 401. The catalyst regenerator 401 is equipped with a regeneration mixture outlet 402, a spent catalyst inlet 403, and an air inlet 404. One end of the spent catalyst discharge pipe 406 is connected to the bottom end of the reaction product discharge pipe 208, and the other end of the spent catalyst discharge pipe 406 is connected to the feed end of the catalyst regenerator 401, so that the spent catalyst can enter the catalyst regenerator 401. The spent catalyst discharge pipe 406 is inclined at a certain angle to facilitate the spent catalyst to slide into the catalyst regenerator 401. The catalyst regenerator 401 is used to remove carbon deposits on the spent catalyst to generate a regenerated catalyst. The discharge end of the catalyst regenerator 401 is connected to the co-reactor 201 so that the regenerated catalyst can re-enter the co-reactor 201. The regeneration mixture outlet 402 is used to discharge the regenerated catalyst mixed with hot air, and the air inlet 404 is used to introduce air.

[0057] Among them, the waste catalyst discharge pipe 406 is an insulated pipe to ensure that the waste catalyst is kept warm in the waste catalyst discharge pipe 406.

[0058] like Figure 1 As shown, the discharge end of the regeneration system 4 is connected to the separation system 5. The separation system 5 is located between the catalyst regenerator 401 and the co-reactor 201. The separation system 5 is used to separate the regenerated catalyst and hot air, and input a portion of the regenerated catalyst into the co-reactor 201.

[0059] Specifically, such as Figure 1As shown, the separation system 5 includes a separator 501, an air outlet 502, a regeneration mixture inlet 503, a catalyst regeneration outlet I 504, and a catalyst regeneration outlet II 506. The separator 501 separates the hot air mixed in the regenerated catalyst to dry the regenerated catalyst, generating a first portion and a second portion of the regenerated catalyst. The regeneration mixture inlet 503 is connected to the regeneration mixture outlet 402 via a re-separation insulated pipe 405 to allow the regenerated catalyst to enter the separator 501. The air outlet 502 discharges the hot air. The catalyst regeneration outlet I 504 is connected to the regenerated catalyst inlet 203 on the co-reactor 201 via a regenerated catalyst discharge pipe 507 to allow the first portion of the regenerated catalyst to enter the co-reactor 201. The catalyst regeneration outlet II 506 discharges the second portion of the regenerated catalyst.

[0060] In this embodiment, the regenerated catalyst discharge pipe 507 is an insulated pipe to ensure that the regenerated catalyst in the first part is kept warm.

[0061] like Figure 1 As shown, the separation system 5 also includes a separator valve 505. The separator 501 has a discharge port at its bottom. The separator valve 505 has one inlet and two outlets. The inlet of the separator valve 505 is connected to the discharge port of the separator 501. One of the outlets of the separator valve 505 serves as the catalyst regeneration outlet I504 to discharge the first part of the regenerated catalyst and is connected to the regenerated catalyst inlet 203. The other outlet of the separator valve 505 serves as the catalyst regeneration outlet II506 to discharge the second part of the regenerated catalyst. The discharge time and flow rate of the first part and the second part of the regenerated catalyst can be determined by engineering effects.

[0062] In this embodiment, the catalyst regenerator 401 is a riser structure. Air is introduced to carry the particles upward into the separation system 5 for combustion reaction. The carbon deposits on the waste catalyst are removed by combustion, and most of the heat generated by combustion is carried by the hot catalyst particles into the co-reactor 201 to maintain the hydrogenation reaction temperature.

[0063] In summary, this application combines gas-gas and gas-solid synergistic reaction modes, allowing for flexible switching between the two modes and enabling dynamic control of the hydrogen source. While ensuring biomass hydrogenation efficiency, it improves the system's adaptability to different biomass feedstocks, resulting in high feedstock utilization. By exciting plasma through dielectric barrier discharge, catalytic hydrogenation is achieved between hydrogen-rich feedstock pyrolysis gas and biomass pyrolysis gas under atmospheric pressure. This enables molecular-level synergistic reforming of biomass pyrolysis gas and hydrogen-rich feedstock cracked gas, generating high-value-added hydrocarbon liquid fuels. This improves upon the significant drawbacks of traditional processes, such as lengthy flow, large material losses, and high energy consumption. Furthermore, online quality-enhancing reaction control is simple, facilitating the design of multi-reaction integration and compact reactors.

[0064] This application achieves improved catalyst utilization efficiency through reactor structure design. The lower part of the co-reactor 201 adopts an inclined conical shape, with the inner wall of the conical cavity forming a helical track. Due to varying radial forces, the catalyst can roll and sink within the reactor, ensuring sufficient contact between the catalyst and reactants, thereby improving catalytic efficiency and mitigating the problem of catalyst deactivation due to carbon buildup. The catalyst regenerator 401 employs a riser structure, enabling the removal of carbon deposits on the spent catalyst through combustion and conveying them to the separator 501. The separated catalyst particles can then be reused in the co-reactor 201.

[0065] This application utilizes a bypass reflux recycling method to return a portion of the hydrogenation products to the co-reactor 201 for secondary or multiple hydrogenation. It also allows for the recycling of incompletely reacted pyrolysis gas from the initial reaction, thereby improving the overall conversion rate. Furthermore, catalyst regeneration is achieved through riser combustion, enabling catalyst reuse and reducing the amount of catalyst added at the catalyst inlet, thus improving overall process economy.

[0066] This application achieves self-sufficiency in heat supply for the entire process by utilizing the hydrogen-rich feedstock pyrolysis reactor 101 and the biomass pyrolysis reactor 102, as well as the heat from the catalyst regeneration process to the co-reactor 201, eliminating the need for external heating. The high-voltage electrode 207 used in this application can not only be powered by the power grid but can also be driven by renewable energy sources such as wind power, photovoltaic power, and hydropower, enabling immediate and local consumption of renewable energy power, addressing the instability of renewable energy power, and further achieving a clean and low-carbon overall process.

[0067] Example 2 This application discloses a plasma-driven synergistic pyrolysis and upgrading method for biomass and hydrogen-rich feedstock, employing the plasma-driven synergistic pyrolysis and upgrading system for biomass and hydrogen-rich feedstock disclosed in Example 1. Figure 3 and Figure 4 As shown, the method includes the following steps: S1: Hydrogen-rich feedstock and biomass pyrolysis: Hydrogen-rich feedstock and dry carrier gas are fed into hydrogen-rich feedstock pyrolysis reactor 101. The hydrogen-rich feedstock pyrolysis and heat self-supply are achieved by ignition and air volume control, so that the hydrogen-rich feedstock pyrolysis produces hydrogen-rich feedstock pyrolysis gas and solid products. Dry biomass feedstock and dry carrier gas are fed into biomass pyrolysis reactor 106. The biomass pyrolysis and heat self-supply are achieved by ignition and air volume control, so that the biomass pyrolysis produces biomass pyrolysis gas and pyrolysis char.

[0068] S2-1: Gas-solid mode: When hydrogen-rich raw material is in short supply, the hydrogen-rich raw material pyrolysis gas valve 105 is opened, and the hydrogen-rich raw material pyrolysis gas is discharged from the hydrogen-rich raw material pyrolysis gas outlet 111 and enters the biomass pyrolysis reactor 106 through the gas inlet 112 to pyrolyze with the biomass solid. The hydrogen-rich raw material pyrolysis gas pre-hydrogenates the biomass pyrolysis gas. S2-2: Gas-gas mode: When there is sufficient hydrogen-rich feedstock, close the hydrogen-rich feedstock pyrolysis gas valve 105. The hydrogen-rich feedstock pyrolysis gas will be discharged from the hydrogen-rich feedstock pyrolysis gas outlet 111 and enter the co-reactor 201 through the hydrogen-rich feedstock pyrolysis gas discharge pipe 214. The biomass pyrolysis gas generated by the biomass pyrolysis reactor 106 enters the co-reactor 201 through the biomass pyrolysis gas discharge pipe 215.

[0069] S2: Pyrolysis gas co-processed online upgrading and hydrogenation: The catalyst enters the co-processing reactor 201 from the catalyst inlet 202. Highly active plasma is generated in situ through dielectric barrier discharge between the high voltage electrode 207 and the ground electrode. The pyrolysis gas is subjected to online catalytic hydrogenation and deoxygenation in the co-processing reactor 201 to generate hydrogenation products and produce waste catalyst. The reaction product outlet 208 is used to discharge the reaction products.

[0070] S3: Product condensation and separation: The reaction products of the co-reactor 201 are discharged from the reaction product outlet 208 and then pass through the reaction product inlet 302 in sequence through the first condensation tank 301, the second condensation tank 305 and the third condensation tank 306 for condensation. The condensed liquid is discharged through the condensed liquid outlet 304 and the non-condensable gas is discharged through the non-condensable gas outlet 303.

[0071] In this embodiment, when cyclic hydrogenation is required, step S4 is also included: product cyclic hydrogenation: the first part of the hydrogenated product discharged from the reaction product outlet 205 enters the first condenser tank 301 from the reaction product inlet 302 through the condensate product discharge pipe 212, and the second part of the hydrogenated product is drawn back to the cyclic gas inlet 210 by the cyclic gas discharge pipe 213 and re-enters the co-reactor 201 to perform step S2.

[0072] In this embodiment, when a regeneration system 4 is provided, step S5 is also included: catalyst recycling and regeneration: the waste catalyst enters the catalyst regenerator 401 from the waste catalyst inlet 403 after passing through the reaction product discharge pipe 208 and the waste catalyst discharge pipe 406. Air enters the catalyst regenerator 401 from the air inlet 404. The waste catalyst particles and air undergo a combustion reaction, and the carbon deposits on the waste catalyst are removed. The regenerated mixture enters the separator 501 from the regenerated mixture outlet 402 to achieve gas-solid separation. Hot air is discharged from the upper air outlet 502, and the regenerated catalyst is discharged from the regenerated catalyst outlet 1504. After passing through the regenerated catalyst discharge pipe 507, it enters the co-reactor 201 through the regenerated catalyst inlet 203 to perform step S2.

[0073] In summary, the plasma-driven biomass and hydrogen-rich feedstock co-pyrolysis upgrading method disclosed in this embodiment achieves flexible switching between gas-gas / gas-solid modes and dynamic control of the hydrogen source by switching the flow direction of the pyrolysis gas from the hydrogen-rich feedstock through valve switching. While ensuring hydrogenation efficiency, it improves the system's adaptability to different biomass feedstocks and achieves high feedstock utilization.

[0074] 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 plasma-driven biomass and hydrogen-rich feedstock co-pyrolysis and upgrading system, characterized in that: include: A pyrolysis reaction system includes a hydrogen-rich feedstock pyrolysis reactor, a biomass pyrolysis reactor, and a valve connecting the two. The hydrogen-rich feedstock pyrolysis reactor is connected to a hydrogen-rich feedstock pyrolysis gas discharge pipe, and the biomass pyrolysis reactor is equipped with a gas inlet and a biomass pyrolysis gas discharge pipe. The valve is used to guide the hydrogen-rich feedstock pyrolysis gas discharged from the hydrogen-rich feedstock pyrolysis reactor into the hydrogen-rich feedstock pyrolysis gas discharge pipe or into the biomass pyrolysis reactor through the gas inlet. In gas-gas mode, the valve is closed, and the hydrogen-rich feedstock pyrolysis gas enters the co-catalytic reactor through the hydrogen-rich feedstock pyrolysis gas discharge pipe to undergo a co-catalytic hydrogenation reaction with the biomass pyrolysis gas. In gas-solid mode, the valve is open, and the hydrogen-rich feedstock pyrolysis gas enters the biomass pyrolysis reactor through the gas inlet to undergo a co-catalytic hydrogenation reaction with the biomass solid and to pre-hydrogenate the biomass pyrolysis gas. A plasma-assisted quality improvement reaction system includes a assisted reactor that uses dielectric barrier discharge technology to generate plasma for online catalytic hydrogenation and deoxygenation of pyrolysis gas. The assisted reactor is connected to the discharge pipe of the hydrogen-rich feedstock pyrolysis gas and the discharge pipe of the biomass pyrolysis gas. The hydrogen-rich components in the hydrogen-rich feedstock pyrolysis gas are used to excite the generation of hydrogen plasma, thereby reducing the amount of external hydrogen introduced. A condensation system is used to perform gas-liquid separation on the hydrogenation products of the plasma-assisted quality improvement reaction system.

2. The plasma-driven biomass and hydrogen-rich feedstock synergistic pyrolysis and upgrading system according to claim 1, characterized in that: The co-reactor is equipped with multiple high-voltage electrodes arranged in a ring and multiple concentrically arranged ring-shaped grounding electrodes.

3. The plasma-driven biomass and hydrogen-rich feedstock synergistic pyrolysis and upgrading system according to claim 1, characterized in that: The lower part of the synergistic reactor is provided with a conical cavity, and the inner wall of the conical cavity is provided with a spiral track.

4. The plasma-driven biomass and hydrogen-rich feedstock synergistic pyrolysis and upgrading system according to claim 1, characterized in that: The condensation system includes multiple condensation tanks connected in series.

5. The plasma-driven biomass and hydrogen-rich feedstock synergistic pyrolysis and upgrading system according to claim 1, characterized in that: The co-reactor is connected to a reaction product discharge pipe, which is connected to a circulating gas discharge pipe. The outlet of the circulating gas discharge pipe is connected to the co-reactor, and a circulating gas pump is installed on the circulating gas discharge pipe.

6. The plasma-driven biomass and hydrogen-rich feedstock synergistic pyrolysis and upgrading system according to claim 1, characterized in that: It also includes a regeneration system for regenerating the spent catalyst produced by the co-reactor and re-feeding it back into the co-reactor.

7. The plasma-driven biomass and hydrogen-rich feedstock synergistic pyrolysis and upgrading system according to claim 6, characterized in that: It also includes a separation system for separating the regenerated catalyst and hot air output from the regeneration system, and inputting a portion of the regenerated catalyst into the co-reactor.

8. A plasma-driven biomass and hydrogen-rich feedstock co-pyrolysis upgrading method, employing the plasma-driven biomass and hydrogen-rich feedstock co-pyrolysis upgrading system according to any one of claims 1-7, characterized in that: Includes the following steps: Hydrogen-rich feedstock and biomass pyrolysis: Hydrogen-rich feedstock and carrier gas are fed into the hydrogen-rich feedstock pyrolysis reactor, where the hydrogen-rich feedstock pyrolysis produces hydrogen-rich feedstock pyrolysis gas and solid products; biomass feedstock and carrier gas are fed into the biomass pyrolysis reactor, where the biomass pyrolysis produces biomass pyrolysis gas and pyrolysis char; by opening or closing valves and selecting gas-to-gas or gas-to-solid mode, the hydrogen-rich feedstock pyrolysis gas is introduced into the hydrogen-rich feedstock pyrolysis gas discharge pipe or introduced into the biomass pyrolysis reactor through the gas inlet; Pyrolysis gas co-processed online upgrading and hydrogenation: using dielectric barrier discharge technology to generate plasma for online catalytic hydrogenation and deoxygenation of pyrolysis gas; Product condensation and separation: The hydrogenation products of the plasma-coordinated upgrading reaction system are separated into gas and liquid phases by a condensation system.

9. The plasma-driven synergistic pyrolysis and upgrading method for biomass and hydrogen-rich feedstock according to claim 8, characterized in that: In gas-gas mode, the valve is closed, and the hydrogen-rich feedstock pyrolysis gas enters the co-catalytic reactor through the hydrogen-rich feedstock pyrolysis gas discharge pipe, where it undergoes a co-catalytic hydrogenation reaction with the biomass pyrolysis gas entering the co-catalytic reactor.

10. The plasma-driven synergistic pyrolysis and upgrading method for biomass and hydrogen-rich feedstock according to claim 8, characterized in that: In gas-solid mode, the valve is opened, and the hydrogen-rich feedstock pyrolysis gas enters the biomass pyrolysis reactor through the gas inlet, where it undergoes pyrolysis reaction together with the biomass solid. The hydrogen-rich feedstock pyrolysis gas also pre-hydrogenates the biomass pyrolysis gas. The pyrolysis gas discharged from the biomass pyrolysis reactor enters the co-reactor for catalytic hydrogenation.

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