Solid-gas dual-phase raw material co-processing integrated reaction system

Abstract

This invention relates to the field of solid-gas two-phase feedstock processing technology, specifically to an integrated reaction system for co-processing solid-gas two-phase feedstocks. The system includes: a feedstock pretreatment unit for pretreating and mixing multi-source solids to form solid feedstocks, while simultaneously purifying fermentation biogas to prepare gaseous feedstocks; a solid-gas coupling reactor for pyrolyzing the solid feedstocks into syngas and countercurrently mixing them with the gaseous feedstocks; a catalytic reaction unit for catalytic reforming the mixed gas using an integrated adsorption-catalysis material to produce hydrogen and remove impurities; a product separation unit for sequentially performing gas-solid separation and pressure swing adsorption purification on the reformed products to obtain high-purity hydrogen; a waste heat recovery unit for recovering reaction waste heat and using it to preheat the solid and gaseous feedstocks entering the system; and an intelligent control unit for monitoring key system parameters and automatically adjusting system operating conditions. This solves the problems of low integration and low reactor mass transfer efficiency in existing technologies.

Description

Technical Field

[0001] This invention relates to the field of solid-gas dual-phase feedstock processing technology, specifically to an integrated reaction system for co-processing solid-gas dual-phase feedstocks. Background Technology

[0002] With the global energy structure transitioning towards cleaner energy sources, hydrogen energy, as a zero-carbon secondary energy carrier, has attracted significant attention for its industrial development. Biomass hydrogen production, particularly the production of hydrogen from multi-source organic waste (such as household waste, tree branches, and livestock manure) through thermochemical or biochemical pathways, offers the dual benefits of waste resource utilization and clean energy production, making it an important research direction in this field. Among various processes, pyrolysis and gasification of solid biomass feedstocks, followed by co-catalytic reforming with gaseous feedstocks such as biogas produced through fermentation, is considered an effective way to improve feedstock adaptability, energy conversion efficiency, and hydrogen yield. However, the large-scale and efficient application of this technology still faces a series of key technological bottlenecks that urgently need to be addressed.

[0003] Existing technologies typically employ a series or separate process of "solid-phase gasification" and "gas-phase reforming," resulting in lengthy system flows, redundant equipment units, and high investment and operating costs. A more significant problem is that the processing of solid and gaseous feedstocks is independent, making it difficult to achieve synergistic complementarity and cascade utilization of energy and material flows. The overall system energy efficiency is generally below 45%, leading to poor economic performance. In the core reaction stage, traditional reaction devices (such as co-current or cross-current fixed beds) have limited contact area between the gas and solid phases, resulting in uneven mixing and low mass and heat transfer efficiency. This leads to incomplete reforming of syngas and biogas, with hydrogen yields consistently hovering at a low level of 0.2-0.25 m³ / kg feedstock. Furthermore, inherent impurities such as sulfur and nitrogen in the feedstock can easily cause irreversible poisoning and deactivation of the reforming catalyst. Traditional solutions rely on adding complex purification and removal devices before the reaction unit, further increasing system complexity and operation and maintenance costs. These shortcomings collectively limit the techno-economic feasibility of large-scale processing (e.g., 30 tons per day) and make it difficult to meet the requirements for commercialization. Therefore, developing an integrated reaction system that can achieve efficient synergy of solid and gaseous feedstocks, enhanced mass transfer, and integrated reaction and purification is of vital importance for promoting the advancement and industrial application of biomass hydrogen production technology. Summary of the Invention

[0004] This application provides an integrated reaction system for co-processing solid and gaseous two-phase feedstocks to solve the problems of low system integration and low reactor mass transfer efficiency in the prior art.

[0005] The first aspect of this application provides an integrated reaction system for co-processing solid and gas two-phase feedstocks, comprising: a feedstock pretreatment unit, a solid-gas coupling reactor, a catalytic reaction unit, a product separation unit, a waste heat recovery unit, and an intelligent control unit; wherein... The raw material pretreatment unit is used to pretreat and mix multi-source solid organic waste to produce solid raw materials, and simultaneously purify fermentation biogas to prepare gaseous raw materials. The solid-gas coupling reactor is equipped with a pyrolysis gasification zone and a gas-solid mixing zone with an internal microchannel structure, used to pyrolyze the solid raw materials into syngas and mix it countercurrently with the gaseous raw materials in the microchannels. The catalytic reaction unit is integrated into the reactor and is used to catalytically reform the mixed gas to produce hydrogen and simultaneously remove impurities through an adsorption-catalysis integrated material. The product separation unit is used to sequentially perform gas-solid separation and pressure swing adsorption purification on the reformed products to remove solid dust and obtain high-purity hydrogen. The waste heat recovery unit is used to recover the reaction waste heat generated during pyrolysis gasification and catalytic reforming and use it to preheat the solid and gaseous raw materials entering the system. The intelligent control unit is used to monitor the system's temperature, pressure, gas composition, and flow rate in real time and automatically adjust the system's operating conditions.

[0006] Preferably, the raw material pretreatment unit includes a crushing device, a screening device, a solid-liquid separation device, a mixing device, and a biogas pretreatment device. The crushing device is used to crush the tree raw materials into 2-5mm particles; the screening device is used to remove non-degradable impurities from domestic waste; the solid-liquid separation device is used to separate the solid and liquid components of the manure; the mixing device is used to mix the solid raw materials at a mass fraction of 30%-40%:40%-50%:10%-20% and control the moisture content to 15%-20% and the carbon-nitrogen ratio to 20-25:1; the biogas pretreatment device is used to dehydrate and desulfurize the fermented biogas, ensuring that the H2S content is ≤50ppm.

[0007] Preferably, the solid-gas coupling reactor is a vertical cylindrical structure, with a gas-solid mixing zone, a catalytic reaction zone, and a pyrolysis gasification zone arranged sequentially from top to bottom inside. The gas-solid mixing zone has a built-in microchannel structure with a channel size of 500 μm and a specific surface area ≥3000 m² / m³, employing a gas-solid countercurrent contact design with a gas flow rate of 0.8 m / s and a solid flow rate of 0.05 m / s. The catalytic reaction zone is filled with adsorption-catalysis integrated particles, with the particle layer height accounting for 60%-70% of the reaction zone volume. The pyrolysis gasification zone is equipped with an electric heating jacket and waste heat recovery heat exchange pipeline on its outer side, controlling the reaction temperature at 500-550℃ through external heating and waste heat recovery.

[0008] Preferably, the catalytic reaction unit includes integrated adsorption-catalysis particles and a reaction zone temperature and pressure control system; wherein, the integrated adsorption-catalysis particles are composed of an alumina-silica composite carrier, a Ni-Co alloy active component, and a molecular sieve and activated carbon composite adsorption component, with a particle size of 3-5 mm, a Ni-Co alloy active component mass percentage of 15%-20%, and a molecular sieve and activated carbon composite adsorption component mass percentage of 30%-40%; the reaction zone temperature and pressure control system includes distributed temperature sensors, pressure transmitters, and regulating valves, used to monitor and automatically control the temperature of the catalytic reaction zone at 400-600℃ and the pressure at 0.3-0.5 MPa in real time, ensuring the efficient and stable progress of the reforming reaction.

[0009] Preferably, the product separation unit includes a cyclone separator and a pressure swing adsorption (PSA) device. The cyclone separator is used to remove solid dust from the reaction products with a separation efficiency of ≥99%. The PSA device adopts a 5-tower process with an adsorption pressure of 2.0-2.5 MPa and a desorption pressure of 0.1-0.2 MPa, and is used to purify hydrogen to achieve a hydrogen purity of ≥99.2% and a hydrogen recovery rate of ≥90%.

[0010] Preferably, the threaded tube heat exchanger is used to recover the high-temperature waste heat generated in the pyrolysis gasification zone and the catalytic reaction zone; the heat storage tank is used to store the waste heat recovered by the heat exchanger and to preheat solid raw materials to 150°C and biogas to 100°C, with a system waste heat utilization rate of ≥85%.

[0011] Preferably, the intelligent control unit includes a controller, a sensor network, a parameter prediction model, and a remote monitoring terminal. The controller is used to link various sensors and actuators to automatically adjust the feed rate, reaction temperature, and pressure. The sensor network is used to collect temperature, pressure, gas composition, and flow rate data of each unit. The parameter prediction model is used to predict the trend of hydrogen yield changes and adjust operating parameters in advance. The remote monitoring terminal is used to view system operating data in real time, receive early warning information, and remotely control the system.

[0012] Preferably, the raw material pretreatment unit is connected to the solid-gas coupling reactor, and the solid-gas coupling reactor is connected to the product separation unit; the catalytic reaction unit is integrated inside the solid-gas coupling reactor; the waste heat recovery unit is connected to both the solid-gas coupling reactor and the raw material pretreatment unit; and the intelligent control unit is linked with each of the other units.

[0013] The second aspect of this application provides an integrated reaction method for co-processing solid and gaseous raw materials, comprising: obtaining solid raw materials and biogas; processing and mixing the solid raw materials to obtain pretreated solid raw materials, while simultaneously dehydrating and desulfurizing the biogas to obtain pretreated biogas; feeding the pretreated solid raw materials into a solid-gas coupling reactor for pyrolysis and gasification to generate syngas, and causing the syngas and the pretreated biogas to be mixed countercurrently within the microchannel structure of the reactor to obtain a mixed gas; introducing the mixed gas into a catalytic reaction zone for catalytic reforming to produce hydrogen and simultaneously remove impurities under the action of adsorption-catalysis integrated particles to obtain hydrogen-containing products; subsequently performing gas-solid separation and hydrogen purification on the hydrogen-containing products to obtain high-purity hydrogen; recovering the waste heat generated during the pyrolysis and gasification and catalytic reforming processes for preheating the pretreated solid raw materials and the pretreated biogas, while simultaneously monitoring and automatically controlling the operating parameters of the entire process in real time through an intelligent control unit.

[0014] A third aspect of this application provides an electronic device, including: a memory, a processor, and a computer program stored in the memory and executable on the processor. The processor executes the program to implement an integrated reaction method for co-processing solid and gaseous raw materials as described in the above embodiments.

[0015] Therefore, this application has the following beneficial effects: This application embodiment utilizes a raw material pretreatment unit to standardize the pretreatment of multi-source solid waste and biogas, providing the system with stable and qualified raw materials. The solid-gas coupling reaction unit, with its built-in microchannel countercurrent structure, greatly enhances the contact and mixing between the gas and solid phases, laying the foundation for efficient reaction. The catalytic reaction unit employs integrated adsorption-catalysis particles to simultaneously remove sulfur and nitrogen impurities while achieving efficient catalytic reforming for hydrogen production, ensuring long-term stable catalyst operation. The product separation unit, through the synergistic effect of gas-solid separation and pressure swing adsorption purification, ensures the production of high-purity hydrogen. The waste heat recovery unit efficiently recovers and utilizes the system's reaction heat in a cascade manner, significantly reducing overall energy consumption. The intelligent control unit, relying on a comprehensive sensing network and predictive models, autonomously optimizes and intelligently maintains all process parameters. This solves the problems of low system integration and low reactor mass transfer efficiency in existing technologies.

[0016] Additional aspects and advantages of this application will be set forth in part in the description which follows, and in part will be obvious from the description, or may be learned by practice of this application. Attached Figure Description

[0017] The above and / or additional aspects and advantages of this application will become apparent and readily understood from the following description of the embodiments taken in conjunction with the accompanying drawings, wherein: Figure 1 This is a schematic diagram of the components of an integrated reaction system for co-processing solid and gaseous feedstocks according to an embodiment of this application. Figure 2 This is a schematic diagram of an integrated reaction system for co-processing solid and gaseous raw materials according to an embodiment of this application; Figure 3 This is a flowchart of an integrated reaction method for co-processing solid and gas dual-phase feedstocks according to an embodiment of this application; Figure 4 This is a schematic diagram of an integrated reaction method for co-processing solid and gaseous raw materials according to an embodiment of this application; Figure 5 This is a schematic diagram of the structure of an electronic device provided according to an embodiment of this application. Detailed Implementation

[0018] The technical solutions of the embodiments of this application will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of this application, and not all embodiments. Based on the embodiments of this application, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of this application.

[0019] The following description, with reference to the accompanying drawings, illustrates an integrated solid-gas two-phase feedstock co-processing reaction system according to an embodiment of this application. Addressing the issue of low system integration mentioned in the background section, this application provides an integrated solid-gas two-phase feedstock co-processing reaction system. In this system, a feedstock pretreatment unit performs standardized pretreatment of multi-source solid waste and biogas, providing the system with stable and qualified feedstocks. The solid-gas coupling reaction unit, with its built-in microchannel countercurrent structure, greatly enhances the contact and mixing between the gas and solid phases, laying the foundation for efficient reaction. The catalytic reaction unit employs integrated adsorption-catalysis particles, simultaneously removing sulfur and nitrogen impurities while completing efficient catalytic reforming for hydrogen production, ensuring long-term stable catalyst operation. The product separation unit, through the synergistic effect of gas-solid separation and pressure swing adsorption purification, ensures the production of high-purity hydrogen. The waste heat recovery unit efficiently recovers and utilizes the system's reaction heat in a cascade manner, significantly reducing overall energy consumption. The intelligent control unit, relying on a comprehensive sensing network and predictive models, autonomously optimizes and intelligently maintains all process parameters. This solves the problems of low system integration and low reactor mass transfer efficiency in existing technologies.

[0020] Figure 1 This is a schematic diagram of the structure of an integrated reaction system for co-processing solid and gaseous raw materials, provided in an embodiment of this application.

[0021] This application provides an integrated reaction system for co-processing solid and gas dual-phase raw materials. The system 10 includes: a raw material pretreatment unit 100, a solid-gas coupling reactor 200, a catalytic reaction unit 300, a product separation unit 400, a waste heat recovery unit 500, and an intelligent control unit 600.

[0022] The system includes the following components: a raw material pretreatment unit 100 for pretreating and mixing multi-source solid organic waste to produce solid raw materials, and a purification unit for purifying fermented biogas to produce gaseous raw materials; a solid-gas coupling reactor 200 with a pyrolysis gasification zone and a gas-solid mixing zone with a built-in microchannel structure for pyrolyzing solid raw materials into syngas and mixing them countercurrently with gaseous raw materials within the microchannels; a catalytic reaction unit 300 integrated within the reactor for catalytic reforming the mixed gas to produce hydrogen and simultaneously removing impurities using an adsorption-catalysis integrated material; a product separation unit 400 for sequentially performing gas-solid separation and pressure swing adsorption purification on the reformed products to remove solid dust and obtain high-purity hydrogen; a waste heat recovery unit 500 for recovering the waste heat generated during pyrolysis gasification and catalytic reforming and using it to preheat the solid and gaseous raw materials entering the system; and an intelligent control unit 600 for real-time monitoring of key parameters such as system temperature, pressure, gas composition, and flow rate, and automatically adjusting system operating conditions.

[0023] It is understood that in this embodiment, the raw material pretreatment unit performs standardized pretreatment of multi-source solid waste and biogas to provide the system with qualified raw materials with stable composition; the solid-gas coupling reaction unit, with its built-in microchannel countercurrent structure, greatly enhances the contact and mixing between the gas and solid phases, laying the foundation for efficient reaction; the catalytic reaction unit uses adsorption-catalysis integrated particles to simultaneously remove sulfur and nitrogen impurities while completing efficient catalytic reforming for hydrogen production, ensuring long-term stable operation of the catalyst; the product separation unit ensures the production of high-purity hydrogen through the synergistic effect of gas-solid separation and pressure swing adsorption purification; the waste heat recovery unit efficiently recovers and utilizes the system's reaction heat in a cascade manner, significantly reducing overall energy consumption; the intelligent control unit, relying on a comprehensive sensing network and predictive model, completes autonomous optimization and intelligent operation and maintenance of the entire process parameters. Thus, it solves the problems of low system integration and low reactor mass transfer efficiency in existing technologies.

[0024] In this embodiment of the application, the raw material pretreatment unit 100 includes: a crushing device, a screening device, a solid-liquid separation device, a mixing device, and a biogas pretreatment device.

[0025] The system includes a crushing device for crushing tree materials into 2-5mm particles; a screening device for removing non-degradable impurities from domestic waste; a solid-liquid separation device for separating manure from its solid state; a mixing device for mixing solid materials at a mass fraction of 30%-40%:40%-50%:10%-20% and controlling the moisture content to 15%-20% and the carbon-nitrogen ratio to 20-25:1; and a biogas pretreatment device for dehydrating and desulfurizing fermented biogas to ensure that the H2S content is ≤50ppm.

[0026] It is understood that in this embodiment, the wood raw materials are uniformly crushed to a suitable particle size of 2-5mm by a crushing device, ensuring the reaction rate and uniformity of the solid raw materials in the subsequent pyrolysis and gasification process; the screening device effectively removes non-degradable impurities from domestic waste, avoiding equipment wear and pipeline blockage that may be caused by such impurities entering the reaction system; the solid-liquid separation device dehydrates the feces, precisely controlling the overall moisture content of the solid raw materials; the mixing device mixes the pretreated multi-source materials according to a scientific ratio and coordinates the moisture content and carbon-nitrogen ratio to prepare standardized solid raw materials with stable composition and uniform physicochemical properties; the biogas pretreatment device reduces the H2S content in the gaseous raw materials to below the threshold through deep dehydration and desulfurization processes, fundamentally eliminating the risk of catalyst sulfur poisoning. The coordinated operation of the above devices provides uniform, stable, clean and reliable raw materials for the subsequent solid-gas coupling reaction, laying the foundation for the efficient and stable operation of the system.

[0027] It should be noted that the aforementioned crushing, screening, solid-liquid separation, mixing, and biogas pretreatment devices do not operate in isolation, but rather constitute a coordinated and interconnected standardized raw material pretreatment system. The particle size uniformity ensured by the crushing device, the impurity removal achieved by the screening device, the moisture content controlled by the solid-liquid separation device, and the component and carbon-nitrogen ratio adjusted by the mixing device together constitute the physical and chemical baseline for the solid raw materials. Simultaneously, the deep desulfurization achieved by the biogas pretreatment device establishes the cleanliness standard for the gaseous raw materials. Through system integration and process linkage, these devices ultimately achieve precise control and standardized output of multi-source, heterogeneous feedstocks, providing high-quality raw materials with stable composition, uniform specifications, and controlled impurities for subsequent high-temperature and catalytic reaction units, thus ensuring the reaction efficiency, operational stability, and equipment reliability of the entire system from the source.

[0028] For example, in a biomass hydrogen production demonstration project with a daily processing capacity of 30 tons of solid raw materials, tree raw materials are processed by a hammer mill, converting them all into homogeneous particles of 2-5mm, with a single batch processing capacity of 10.5 tons; domestic waste is processed through a 10mm aperture drum screen to effectively separate and remove non-degradable impurities such as plastics and glass, with a processing capacity of 13.5 tons; and manure is dehydrated by a screw extrusion solid-liquid separator, producing 6 tons of manure residue with a moisture content of approximately 60%. The pretreated materials then enter a horizontal mixer, strictly mixing them according to a mass ratio of 35% tree particles, 45% domestic waste, and 20% manure residue. Adjustments are made to ensure that the moisture content of the mixed solid raw materials is stably controlled at 18%, and the carbon-to-nitrogen ratio is optimized to 22:1. Simultaneously, the project's supporting anaerobic fermentation system produces approximately 12,000 m³ of biogas per day. The biogas is then processed sequentially through condensation dehydration (dew point -20℃) and an iron oxide desulfurization tower, ultimately reducing the H2S content to below 30 ppm. Through this standardized pretreatment process, the system can provide approximately 30 tons of uniform and stable solid raw materials and 12,000 m³ of clean biogas to the subsequent solid-gas coupling reactor daily, ensuring the feed quality and operational stability of the core reaction unit from the source.

[0029] In this embodiment, the solid-gas coupling reactor 200 includes: a gas-solid mixing zone, a catalytic reaction zone, and a pyrolysis gasification zone.

[0030] The gas-solid mixing zone has a built-in microchannel structure with a channel size of 500μm and a specific surface area of ​​≥3000m² / m³. It adopts a gas-solid countercurrent contact design with a gas flow rate of 0.8m / s and a solid flow rate of 0.05m / s. The catalytic reaction zone is filled with adsorption-catalysis integrated particles, and the particle layer height accounts for 60%-70% of the reaction zone volume. The pyrolysis gasification zone is equipped with an electric heating jacket and a waste heat recovery heat exchange pipeline on the outside. The reaction temperature is controlled at 500-550℃ through external heating and waste heat recovery.

[0031] Understandably, the embodiments of this application, through microchannel structure design, greatly increase the contact area between the gas and solid phases. Combined with the countercurrent flow mode, this significantly enhances mass transfer and mixing effects, creating sufficient and uniform reaction conditions for subsequent catalytic reforming. Precise temperature control in the pyrolysis gasification zone ensures the efficient and stable conversion of solid feedstock into syngas rich in H2, CO, and CH4. This reactor, through its partitioned integrated design, compactly couples multiple key steps such as pyrolysis, mixing, and reforming into a single device, achieving extreme simplification of the process flow and improved energy efficiency.

[0032] It should be noted that the gas-solid mixing zone, catalytic reaction zone, and pyrolysis gasification zone are not simply stacked, but rather form a synergistic space with naturally optimized airflow and reaction paths. Syngas flows from bottom to top, while biogas is introduced from the middle for counter-mixing. This flow field design not only extends the effective contact time but also promotes the internal transfer and utilization of reaction heat. The integrated reactor structure fundamentally solves the problems of redundant equipment, severe heat loss, and low system energy efficiency in traditional phase-separated processes.

[0033] For example, in a demonstration reactor with a total volume of 20 m³, the pyrolysis gasification zone (10 m³) operates at 525 °C, converting solid feedstock into syngas. This syngas then enters the gas-solid mixing zone (3.3 m³), ​​where it is countercurrently mixed with biogas (flow rate 0.8 m / s) introduced from the center of the zone within microchannels. The thoroughly mixed gas then enters the catalytic reaction zone (6.7 m³) for reforming. This integrated design achieves a gas-solid contact area of ​​over 3200 m² / m³, increasing mass transfer efficiency by more than 40% compared to traditional reactors, laying a core physical foundation for achieving high hydrogen yield.

[0034] In this embodiment, the catalytic reaction unit 300 includes: an integrated adsorption-catalysis particle and a temperature and pressure control system for the reaction zone.

[0035] The adsorption-catalysis integrated particles consist of an alumina-silica composite carrier, a Ni-Co alloy active component, and a molecular sieve and activated carbon composite adsorption component. The particle size is 3-5 mm, with the Ni-Co alloy active component accounting for 15%-20% by mass and the molecular sieve and activated carbon composite adsorption component accounting for 30%-40% by mass. The reaction zone temperature and pressure control system includes distributed temperature sensors, pressure transmitters, and regulating valves, which are used to monitor and automatically regulate the temperature of the catalytic reaction zone at 400-600℃ and the pressure at 0.3-0.5 MPa in real time, ensuring the efficient and stable progress of the reforming reaction.

[0036] It is understood that the embodiments of this application integrate catalytic active sites and impurity adsorption sites into the same material through a unique adsorption-catalysis integrated particle design. The Ni-Co alloy active component efficiently catalyzes the reforming reaction of CH4 and CO to produce hydrogen, while the molecular sieve and activated carbon composite component simultaneously and in situ adsorbs impurities such as H2S and NH3 in the feed gas. This "reaction-while-purification" mode fundamentally avoids the risk of catalyst deactivation due to sulfur and nitrogen poisoning, ensuring the long-term high activity and service life of the catalyst.

[0037] It should be noted that the catalytic reaction unit does not rely solely on material innovation; its accompanying temperature and pressure control system is crucial for maintaining efficient reaction. The system monitors and automatically adjusts the reaction zone temperature in real time within the optimal range of 400-600℃ and pressure within 0.3-0.5MPa, ensuring the thermodynamic driving force and kinetic rate of the reforming reaction, while providing suitable conditions for the adsorption process. This synergy between materials and control achieves a balance between reaction depth, selectivity, and system stability.

[0038] For example, under optimal operating conditions (525℃, 0.4MPa), a catalytic reaction zone filled with 65% volumetric integrated particles was used to reform a mixed gas. The Ni-Co alloy active component, comprising 18% by mass (Ni:Co=3:1), achieved a hydrogen selectivity of over 95%; while the ZSM-5 molecular sieve and activated carbon composite adsorption component, comprising 35% by mass (ratio 2:1), achieved adsorption capacities of H2S ≥ 80 mg / g and NH3 ≥ 60 mg / g. Under these conditions, the system achieved a sulfur and nitrogen impurity removal rate exceeding 99%, and the catalyst maintained an activity retention rate of over 90% after 2000 hours of operation.

[0039] In this embodiment, the product separation unit 400 includes a cyclone separator and a pressure swing adsorption device.

[0040] Among them, the cyclone separator is used to remove solid dust from the reaction products, with a separation efficiency of ≥99%; the pressure swing adsorption device adopts a 5-tower process, with an adsorption pressure of 2.0-2.5MPa and a desorption pressure of 0.1-0.2MPa, and is used to purify hydrogen, so that the hydrogen purity is ≥99.2% and the hydrogen recovery rate is ≥90%.

[0041] It is understood that the embodiments of this application achieve efficient separation and purification of hydrogen through a two-stage purification strategy of "mechanical separation + precision adsorption". The cyclone separator first efficiently removes solid dust from the gas (separation efficiency ≥99%), protecting the downstream precision adsorption device from contamination and blockage. Subsequently, the pressure swing adsorption device utilizes the difference in adsorption performance between hydrogen and impurity gases such as CO2, CH4, and CO on the adsorbent, and selectively purifies the hydrogen to extremely high purity through periodic pressure changes.

[0042] It should be noted that the two-stage design of the product separation unit constitutes a complete purification chain. Cyclone separation, as a pretreatment, ensures the basic conditions for the long-term stable operation of the pressure swing adsorption system; while the optimized 5-tower PSA process, through reasonable timing control and pressure fluctuation, achieves high product purity (≥99.2%) while also obtaining a high hydrogen recovery rate (≥90%), minimizing the loss of effective components and improving the material utilization efficiency and economy of the entire system.

[0043] For example, the dust-laden gas discharged from the reactor first enters a high-efficiency cyclone separator, where over 99% of the solid dust is captured and discharged. This dust can be co-utilized with other waste residues from the system. The dust-free gas then enters a 5-tower pressure swing adsorption unit. Under an adsorption pressure of 2.2 MPa, hydrogen is preferentially desorbed and passes through, while CO2, CH4, and other impurities are retained by the adsorbent. The adsorption towers undergo desorption regeneration at 0.15 MPa, discharging impurity tail gas. This tail gas, still possessing calorific value, can be reused as fuel. After processing in this unit, high-quality hydrogen with a purity higher than 99.3% and a CO content lower than 80 ppm is finally obtained.

[0044] In this embodiment, the waste heat recovery unit 500 includes a threaded tube heat exchanger and a heat storage tank.

[0045] Among them, the threaded tube heat exchanger is used to recover the high-temperature reaction waste heat generated in the pyrolysis gasification zone and the catalytic reaction zone; the heat storage tank is used to store the waste heat recovered by the heat exchanger and to preheat solid raw materials to 150°C and biogas to 100°C, with a system waste heat utilization rate of ≥85%.

[0046] It is understood that the embodiments of this application, through the design of a highly efficient threaded tube heat exchanger, actively capture the excess heat released from the core high-temperature reaction process of the system (temperatures can reach above 525°C), converting the waste heat that might otherwise be lost into useful thermal energy resources. The configuration of the heat storage tank solves the problem of the mismatch between the time and intensity of heat generation and use, realizing the buffering and stable supply of energy, making waste heat utilization more flexible and reliable.

[0047] It should be noted that this unit is not an independent add-on component, but a key link deeply integrated into the system's energy flow. The recovered heat is directly used to preheat solid raw materials to approximately 150°C and biogas to approximately 100°C. This significantly reduces the external energy input required for the raw materials to reach the reaction temperature, effectively reducing the main energy consumption of the system operation. This internally circulating, cascaded heat utilization thermally couples multiple process steps, greatly improving the overall energy utilization efficiency of the entire system.

[0048] For example, the system recovers waste heat from pyrolysis and reforming reactions through a threaded tube heat exchanger (50 m²) located in the high-temperature zone of the reactor, achieving a heat exchange efficiency of 88%. The recovered heat energy is stored in a 50 m³ heat storage tank. This heat is then used to preheat solid feedstock from the pretreatment unit (from ambient temperature to 150°C) and biogas (from ambient temperature to 100°C). In this way, the system increases waste heat utilization to over 85%, reducing the overall energy consumption per ton of hydrogen production by approximately 30% compared to traditional processes without waste heat recovery.

[0049] In this embodiment, the intelligent control unit 600 includes: a controller, a sensor network, a parameter prediction model, and a remote monitoring terminal.

[0050] The controller is used to link various sensors and actuators to automatically adjust the feed rate, reaction temperature and pressure; the sensor network is used to collect temperature, pressure, gas composition and flow data of each unit; the parameter prediction model is used to predict the trend of hydrogen yield change and adjust the operating parameters in advance; the remote monitoring terminal is used to view the system operation data in real time, receive early warning information and remotely control the system.

[0051] It is understood that the embodiments of this application, by deploying a dense sensor network covering the entire process, achieve comprehensive, real-time, and accurate perception of the system's operating status, transforming complex physicochemical reaction processes into quantifiable digital information flows. Based on this, the controller can respond quickly (response time ≤ 5s), automatically adjusting key parameters such as feed rate, heating power, and valve opening, ensuring the system always operates within a preset optimal range, overcoming the lag and inaccuracy of manual operation.

[0052] It's important to note that the core advantage of intelligent control lies in its transcendence of simple PID feedback control by introducing a parameter prediction model. Based on historical and real-time data (such as membrane module pressure differential, inlet turbidity, and hydrogen yield trends), this model can predict potential problems in advance, such as catalyst activity degradation and reaction efficiency fluctuations, and issue early warnings or initiate adjustment procedures (such as adjusting the ratio or pre-cleaning). This "sensing-prediction-regulation" feedforward-feedback composite control mode greatly enhances the system's robustness and adaptability in the face of disturbances such as raw material fluctuations and equipment performance degradation.

[0053] For example, in a system using a PLC (S7-1200) as the controller, over 30 sensors of various types collect data every minute. When the hydrogen yield prediction model, based on real-time gas composition and flow data, determines that the yield is likely to decrease by 5% in the next two hours, the controller will preemptively fine-tune the biogas inlet rate and the set temperature of the reaction zone. Simultaneously, remote monitoring terminals (computer web interface and mobile app) allow operators to view the system status at any time, receive early warning information, and intervene remotely when necessary. This intelligent unit reduces the system's reliance on manual intervention by 70% and ensures the stability of the hydrogen yield (fluctuation ≤ ±2%) even when the feedstock composition fluctuates.

[0054] In this embodiment, the raw material pretreatment unit is connected to the solid-gas coupling reactor, and the solid-gas coupling reactor is connected to the product separation unit; the catalytic reaction unit is integrated inside the solid-gas coupling reactor; the waste heat recovery unit is connected to both the solid-gas coupling reactor and the raw material pretreatment unit; and the intelligent control unit is linked with each of the other units.

[0055] It is understood that, by directly connecting the raw material pretreatment unit to the solid-gas coupling reactor, this embodiment ensures that the pretreated solid and gaseous raw materials can be continuously and without pollution transported to the core reaction area, laying the material foundation for efficient reaction. By directly connecting the solid-gas coupling reactor to the product separation unit, high-temperature reaction products can be quickly introduced into the separation and purification process, minimizing process energy loss and preventing secondary pollution risks. By integrating the catalytic reaction unit inside the solid-gas coupling reactor, spatial unification of reaction and catalysis is achieved, significantly shortening the mass transfer path and improving reaction rate and selectivity. By connecting the waste heat recovery unit to both the reactor and the pretreatment unit, a cross-unit energy cascade utilization loop is constructed, precisely recycling high-temperature reaction waste heat for raw material preheating, significantly reducing the total energy consumption of the system. Through the linkage of the intelligent control unit with all units, centralized acquisition, intelligent analysis, and unified control of the entire process data are realized, constructing the central nervous system for stable, efficient, and adaptive operation of the system. The above-mentioned close and orderly connections together construct a highly integrated, optimized material and energy flow, and highly automated collaborative system.

[0056] This application proposes a solid-gas two-phase feedstock co-processing integrated reaction system. A feedstock pretreatment unit standardizes the pretreatment of multi-source solid waste and biogas, providing the system with stable and qualified feedstock. The solid-gas coupling reaction unit, with its built-in microchannel countercurrent structure, greatly enhances the contact and mixing between the gas and solid phases, laying the foundation for efficient reaction. The catalytic reaction unit uses integrated adsorption-catalysis particles to simultaneously remove sulfur and nitrogen impurities while efficiently catalytically reforming hydrogen production, ensuring long-term stable catalyst operation. The product separation unit, through the synergistic effect of gas-solid separation and pressure swing adsorption purification, ensures the production of high-purity hydrogen. The waste heat recovery unit efficiently recovers and utilizes the system's reaction heat in a cascade manner, significantly reducing overall energy consumption. The intelligent control unit, relying on a comprehensive sensing network and predictive models, autonomously optimizes and intelligently maintains all process parameters. This solves the problems of low system integration and low reactor mass transfer efficiency in existing technologies.

[0057] The following will illustrate a solid-gas dual-phase feedstock co-processing integrated reaction system through a specific embodiment, such as... Figure 2 As shown, it includes: Taking a biomass-to-hydrogen project processing 30 tons of solid feedstock as an example, the feedstock pretreatment unit receives 10.5 tons of branches and forestry waste, 13.5 tons of pre-sorted municipal solid waste, and 6 tons of livestock manure daily. The wood feedstock is processed by a 55kW hammer mill, where high-speed rotating hammers crush the feedstock. It is then graded through a 3mm mesh screen to ensure that all produced particles are strictly controlled within the 2-5mm range, yielding approximately 10.5 tons of homogeneous wood chips daily. The municipal solid waste is conveyed to a large rotary drum screen, which rotates at 8 revolutions per minute. Its 10mm mesh screen effectively separates non-degradable impurities such as plastic bags, glass bottles, and metal cans. Approximately 1.2 tons of impurities are removed daily for recycling, while the remaining approximately 12.3 tons of organic matter are retained. Livestock and poultry manure is processed by a screw extrusion solid-liquid separator, which removes free water under a mechanical pressure of 0.8 MPa, producing approximately 6 tons of loose manure residue with a moisture content of about 60% per day. The separated liquid is then introduced into the subsequent wastewater treatment system. The pre-treated sawdust, organic waste, and manure residue are fed together into a 5-cubic-meter horizontal twin-shaft mixer. The mixer precisely feeds the materials according to a preset mass ratio of 35% sawdust, 45% organic waste, and 20% manure residue. During the mixing process, an online near-infrared moisture meter monitors the mixture in real time, and an automatic atomized water spraying system is controlled to precisely adjust the overall moisture content of the mixture to 18%. This mixing ratio also ensures that the carbon-to-nitrogen ratio (C / N) of the mixed material remains stable within the ideal range of 22:1. The pretreatment unit produces approximately 30 tons of standardized solid raw materials with uniform composition and stable physical properties per day, which are temporarily stored in a raw material silo via a closed belt conveyor. On the parallel processing line, the anaerobic digester unit of the project produces approximately 12,000 cubic meters of crude biogas daily. This biogas first enters a condensation and dehydration tower, where the temperature is maintained at 5°C, allowing water vapor in the biogas to fully condense and precipitate, lowering its dew point to below -20°C. Subsequently, the dehydrated biogas enters a fixed-bed desulfurization tower filled with iron oxide desulfurizing agent. Under ambient temperature conditions, hydrogen sulfide (H2S) reacts chemically with the desulfurizing agent, reducing its concentration from the initial 800-1200 ppm to below 30 ppm, thus completing the purification process.

[0058] The pretreated solid feedstock is fed into the pyrolysis and gasification zone of the solid-gas coupling reactor at a stable rate of 1.25 tons per hour via a precision-metered variable-frequency screw feeder. This zone is a cylindrical space with a volume of approximately 10 cubic meters, surrounded by an electrically heated jacket precisely managed by an intelligent control system. During system operation, the heating jacket rapidly raises and stabilizes the internal temperature of the pyrolysis and gasification zone at 525°C. In this high-temperature and oxygen-deficient environment, the solid feedstock undergoes complex pyrolysis and partial gasification reactions, breaking down the organic macromolecular chains and converting them into syngas rich in hydrogen (H2), carbon monoxide (CO), and methane (CH4), while simultaneously generating small amounts of coke and ash. Monitoring data indicates that this process produces approximately 1.2 cubic meters of syngas per kilogram of solid feedstock, with a typical volumetric composition of approximately 16% H2, 22% CO, 11% CH4, and the remainder being CO2, N2, etc. The generated high-temperature syngas flows upward naturally under the pressure difference created within the system. Meanwhile, deeply purified biogas is uniformly injected into the gas-solid mixing zone from an annular distributor located in the center of the reactor at a constant flow rate of 525 cubic meters per hour. This zone is one of the core design features of the reactor, with densely packed honeycomb-like microchannels, each with an equivalent diameter strictly defined as 500 micrometers. The upward-flowing high-temperature syngas and the downward-injected ambient-temperature biogas form a strong countercurrent contact within these microchannels. This design increases the effective contact area between the gas and solid phases to approximately 3200 square meters per cubic meter of reactor volume. Under optimized operating conditions of a gas flow rate of 0.8 m / s and a solid particle apparent flow rate of 0.05 m / s, the two gas streams are intensely mixed within the channels, extending the contact time to approximately 15 seconds, ensuring uniform distribution of reactants at the molecular scale. The fully mixed gas reaches a temperature of approximately 500°C and then rises into the upper catalytic reaction zone. The entire reactor shell is made of carbon steel lined with a high-temperature resistant polytetrafluoroethylene anti-corrosion layer, designed to withstand temperatures up to 1000℃ and pressures up to 1.0MPa, providing reliable safety assurance for the aforementioned high-temperature and high-pressure reaction processes.

[0059] After the mixed gas enters the catalytic reaction zone, it flows through a 4.5 cubic meter integrated adsorption-catalysis particle bed, filling approximately 65% ​​of the zone's volume. These particles are the core materials for the system's efficient conversion and long-term operation. Their core is an alumina-silica composite support with a specific surface area exceeding 200 m² / g and a pore volume of 0.9 cm³ / g. On this support, 18% by mass of Ni-Co alloy nano-active components are uniformly loaded, with a nickel-to-cobalt atomic ratio of 3:1. Simultaneously, a composite adsorption component consisting of 35% by mass of ZSM-5 molecular sieves and high specific surface area activated carbon is uniformly dispersed within the particles, with a mass ratio of 2:1. When a mixed gas at 525℃ and a pressure maintained at 0.4MPa flows through this catalyst bed, two key processes occur simultaneously: On the one hand, the Ni-Co active sites efficiently catalyze the steam reforming reaction of methane (CH4+H2O→CO+3H2) and the conversion reaction of carbon monoxide (CO+H2O→CO2+H2), maximizing the conversion of CH4 and CO in the feed gas into the target product H2, with a hydrogen selectivity of over 95%; on the other hand, trace amounts of impurity molecules such as H2S and NH3 in the mixed gas are preferentially adsorbed and captured by the regular micropores of the molecular sieve and the large specific surface area of ​​the activated carbon as it passes through the bed. This integrated design of "catalysis and adsorption" achieves deep purification of the gas while generating hydrogen. Long-term operation tests show that after 2000 hours of continuous operation, the catalyst retains over 90% of its reforming catalytic activity, demonstrating its excellent resistance to poisoning and structural stability. After the catalytic reaction, the main components of the gas have been converted into hydrogen (about 65% by volume), carbon dioxide (about 30%), and a small amount of unreacted methane and water vapor. The temperature is still maintained at about 500°C, and then it is discharged from the top outlet of the reactor.

[0060] The high-temperature gas exiting from the top of the reactor first enters a high-efficiency cyclone separator. The gas enters the separator cylinder at high speed tangentially, creating a strong rotating flow field inside. Trace amounts of catalyst dust and ash particles entrained in the gas are thrown against the separator wall by the powerful centrifugal force and slide down to the bottom ash hopper for collection. Approximately 1.5 tons of solid dust are collected daily. This cyclone separator is designed with a separation efficiency of no less than 99%, ensuring that the dust content in the outlet process gas is below 10 mg / m³, effectively protecting downstream precision separation equipment from contamination and wear. The gas, after initial removal of solid impurities, then passes through a cooling system, reducing its temperature to approximately 40°C, before entering the pressure swing adsorption (PSA) hydrogen purification system. This system employs a mature five-tower process, with each adsorption tower filled with a specialized zeolite molecular sieve and activated carbon composite adsorbent that has strong adsorption capacity for impurities such as CO2, CH4, and CO, but extremely weak adsorption capacity for H2. Under the management of an automated programmable controller, the five adsorption towers cycle through adsorption, pressure equalization and depressurization, reverse depressurization, rinsing, pressure equalization and pressurization, and final pressurization. At an adsorption pressure of 2.2 MPa, hydrogen, as a weakly adsorbed component, preferentially passes through the adsorbent bed and is output as a high-purity product; while strong adsorbed components such as CO2 are selectively retained by the adsorbent. Subsequently, the pressure in the adsorption tower is reduced to 0.15 MPa for desorption, releasing the enriched impurity gases and forming desorption tail gas. This tail gas mainly consists of CO2 and a small amount of CH4, still possessing a calorific value of approximately 12 MJ / m³, and is reintroduced into the system as preheating fuel or auxiliary fuel, achieving energy reuse. Through this sophisticated pressure swing adsorption unit, the hydrogen recovery rate reaches over 90%, and approximately 9600 standard cubic meters of high-purity hydrogen product can be produced daily. The hydrogen product was continuously tested by an online trace gas analyzer, and its purity was consistently above 99.3%, with carbon monoxide content below 80 ppm and carbon dioxide and other impurities content below 500 ppm. All indicators fully meet the national quality standards for industrial hydrogen.

[0061] The waste heat recovery unit is deeply integrated into the system's energy flow, aiming to maximize energy utilization efficiency. The main recovery point is located on the outer wall of the pyrolysis gasification zone and catalytic reaction zone of the solid-gas coupling reactor, where a threaded tube heat exchanger with a total heat exchange area of ​​50 square meters is integrated. The high-temperature reactor wall transfers a large amount of excess heat to the heat transfer oil circulating in a closed loop within the threaded tubes through thermal radiation and conduction. After being heated to approximately 280°C, the heat transfer oil is pumped to a 50-cubic-meter heat storage tank. This heat storage tank uses high-performance insulation materials, with a daily heat loss rate of less than 2%. The stored high-grade heat has two main uses: firstly, through a raw material preheating heat exchanger, it preheats solid raw materials from the raw material silo from ambient temperature to approximately 150°C, significantly reducing the external energy input required for the raw materials to reach the reaction temperature in the pyrolysis gasification zone; secondly, through another biogas preheating heat exchanger, it heats the purified biogas about to enter the reactor from room temperature to 100°C. Actual operation calculations show that this highly efficient waste heat recovery and reuse system effectively captures and reintegrates over 85% of the high-temperature waste heat generated during the reaction process. This significantly improves the overall energy efficiency of the hydrogen production system. Compared to traditional processes without a highly efficient waste heat recovery system, the external energy consumption (such as steam and electricity) required to produce one ton of hydrogen is reduced by approximately 32%, resulting in significant economic benefits.

[0062] The entire system is centrally coordinated and monitored by an intelligent control unit. This unit, centered on a high-performance programmable logic controller (PLC), is connected via an industrial bus network to over 30 sensing points and actuators distributed throughout the process units. Temperature sensors, pressure transmitters, thermal gas mass flow meters, and online gas chromatographs collect real-time data every minute, covering everything from raw material moisture content, screw feeder speed, reactor zone temperature and pressure, real-time gas composition concentration, to product hydrogen purity. All data is transmitted to the controller in real time and processed and analyzed by its internal dedicated intelligent algorithm model. For example, a hydrogen yield prediction model, trained on extensive historical operating data, can predict potential yield fluctuations several hours in advance based on parameters such as the real-time composition of the inlet gas and reaction temperature. It automatically fine-tunes the opening of the biogas feed regulating valve or the reactor heating power, thereby stably controlling yield fluctuations within a narrow range of ±2%. When the sensor network detects an abnormal increase in the pressure difference between the inlet and outlet of the cyclone separator, or a deviation in the stepping timing of the pressure swing adsorption unit, the system immediately triggers an audible and visual alarm signal and can automatically initiate the corresponding maintenance or calibration procedures upon authorization. Furthermore, through a secure industrial IoT gateway, all critical operating data, real-time alarm information, and production performance reports (such as daily processing capacity, cumulative hydrogen production, raw material conversion rate, and overall energy consumption) are synchronized to the cloud server in real time. Operators and managers can not only monitor the real-time status of the entire plant on a large display screen in the central control room, but also remotely monitor from any location with network access via authorized mobile device applications, and remotely adjust key process parameters when necessary. This high level of automation and intelligence liberates the system from tedious daily manual operation and monitoring, enabling this large-scale plant with a daily processing capacity of 30 tons of raw materials to require only 2 to 3 operators per shift during normal operation, significantly reducing labor costs and fundamentally ensuring the long-term, stable, efficient, and safe operation of the entire production process.

[0063] In summary, during the aforementioned 30-day demonstration operation, the system achieved a solid feedstock conversion rate of 92.5% and a gaseous feedstock utilization rate of 98.3%. It produced 9,600 cubic meters of high-purity hydrogen per day, with product quality consistently meeting industrial standards. Simultaneously, the approximately 1.5 tons of solid dust generated daily, along with other process waste, were co-utilized to produce approximately 8.5 tons of organic fertilizer with a total nitrogen, phosphorus, and potassium content of no less than 5%. Through the high integration and synergistic optimization of six major units—feedstock pretreatment, solid-gas coupling reaction, catalytic reforming, product separation, waste heat recovery, and intelligent control—the entire system constructs a complete and efficient multi-source organic waste hydrogen production and resource utilization solution. This effectively solves the bottleneck problems of low system energy efficiency, poor mass transfer, catalyst poisoning, and complex operation and management inherent in traditional phase-separated treatment modes, demonstrating significant environmental and economic benefits.

[0064] Next, referring to the accompanying drawings, an integrated reaction method for co-processing solid and gas dual-phase raw materials according to an embodiment of this application is described.

[0065] like Figure 3 As shown, the integrated reaction method for co-processing solid and gas dual-phase raw materials includes the following steps: In step S101, solid raw materials and biogas are obtained.

[0066] It is understood that the embodiments of this application, by first obtaining solid raw materials and biogas, clarify the basis and source of material input for the entire treatment process. Ensuring a stable supply of multi-source solid organic waste and anaerobic fermentation products provides the necessary material prerequisites for subsequent standardized pretreatment and efficient synergistic reaction, thereby guaranteeing the continuity of system operation and the wide applicability of raw materials.

[0067] In step S102, the solid raw materials are processed and mixed to obtain pretreated solid raw materials, and the biogas is dehydrated and desulfurized to obtain pretreated biogas.

[0068] Among them, dehydration and desulfurization pretreatment refers to the process of removing water vapor and hydrogen sulfide and other impurity gases contained in biogas through physicochemical methods such as condensation, adsorption or chemical reaction.

[0069] It is understood that the embodiments of this application, through dehydration and desulfurization pretreatment of biogas, deeply remove moisture and corrosive and toxic impurities (such as H2S) from the gas feedstock, directly avoiding the interference of water vapor condensation in the subsequent high-temperature reaction, and fundamentally eliminating key factors such as hydrogen sulfide that lead to permanent poisoning and deactivation of the catalyst. This step provides a stable, pure, and reliable gas feedstock for the subsequent catalytic reforming reaction, and is one of the core prerequisites for ensuring the long-term, stable, and efficient operation of the entire system.

[0070] In step S103, the pretreated solid raw material is fed into a solid-gas coupling reactor for pyrolysis and gasification to generate syngas. The syngas and the pretreated biogas are then mixed countercurrently within the microchannel structure of the reactor to obtain a mixed gas.

[0071] Among them, microchannel structure refers to the internal components of a reactor that contain a large number of regular tiny channels with characteristic sizes at the micrometer level (usually tens to hundreds of micrometers), which can greatly increase the specific surface area and promote efficient mass transfer and mixing between fluids.

[0072] It is understood that the embodiments of this application, by designing a microchannel structure in the reactor, utilize its huge specific surface area and precise fluid distribution characteristics to achieve efficient and uniform countercurrent contact and mixing of high-temperature syngas and purified biogas over an extremely short distance. This greatly enhances the mass transfer process between the gas and gas phases, significantly shortens the mixing time, and provides a highly uniform and stable reactant distribution basis for subsequent catalytic reforming reactions, thereby directly improving the reaction rate, selectivity, and overall hydrogen production efficiency.

[0073] In step S104, the mixed gas is introduced into the catalytic reaction zone, where it undergoes catalytic reforming to produce hydrogen and removes impurities simultaneously under the action of adsorption-catalysis integrated particles, resulting in a hydrogen-containing product. Subsequently, the hydrogen-containing product is subjected to gas-solid separation and hydrogen purification to obtain high-purity hydrogen.

[0074] Among them, the adsorption-catalysis integrated particle is a multifunctional particulate material that integrates a catalytically active metal component (such as Ni-Co alloy) with a material with selective adsorption function (such as molecular sieve and activated carbon composite) on the same carrier.

[0075] It is understood that, by employing integrated adsorption-catalysis particles, this application simultaneously achieves the catalytic reforming of mixed gases for hydrogen production and the deep adsorption and removal of impurities such as sulfur and nitrogen in the same reaction process. This design eliminates the reliance on independent and complex subsequent purification devices, improves hydrogen yield and selectivity, fundamentally prevents catalyst deactivation due to poisoning, simplifies the process flow, reduces equipment investment and operating costs, and ensures long-term stable operation of the system.

[0076] In step S105, the waste heat generated during pyrolysis gasification and catalytic reforming is recovered and used to preheat the pretreated solid raw materials and pretreated biogas. At the same time, the intelligent control unit monitors and automatically adjusts the operating parameters of the entire process in real time.

[0077] Residual heat of reaction specifically refers to the excess heat energy released during the two main high-temperature chemical reactions of solid raw material pyrolysis and gasification and mixed gas catalytic reforming, which exceeds the thermal equilibrium required for the reaction itself.

[0078] It is understood that the embodiments of this application systematically recover waste heat from the reaction, transforming high-grade thermal energy that might otherwise be wasted into valuable resources, and precisely reusing it for preheating solid feedstocks and biogas. This measure significantly reduces the external energy input required for the feedstocks to reach the ideal reaction temperature, effectively improves the overall energy utilization efficiency of the entire system, directly reduces the overall energy consumption and operating cost per unit of hydrogen production, and realizes internal energy circulation and cascade utilization.

[0079] According to the embodiments of this application, an integrated reaction method for co-processing solid and gaseous raw materials is proposed. A raw material pretreatment unit performs standardized pretreatment of multi-source solid waste and biogas, providing the system with stable and qualified raw materials. The solid-gas coupling reaction unit, with its built-in microchannel countercurrent structure, greatly enhances the contact and mixing between the gas and solid phases, laying the foundation for efficient reaction. The catalytic reaction unit uses integrated adsorption-catalysis particles to simultaneously remove sulfur and nitrogen impurities while completing efficient catalytic reforming for hydrogen production, ensuring long-term stable operation of the catalyst. The product separation unit ensures the production of high-purity hydrogen through the synergistic effect of gas-solid separation and pressure swing adsorption purification. The waste heat recovery unit efficiently recovers and utilizes the system's reaction heat in a cascade manner, significantly reducing overall energy consumption. The intelligent control unit, relying on a comprehensive sensing network and predictive models, completes autonomous optimization and intelligent operation and maintenance of all process parameters. This solves the problems of low system integration and low reactor mass transfer efficiency in existing technologies.

[0080] The following will illustrate an integrated reaction method for co-processing solid and gas dual-phase feedstocks through a specific embodiment, such as... Figure 4 As shown, it includes: A medium-sized biomass hydrogen production plant is designed to process 30 tons of solid feedstock per day. Its standard feedstock composition is 35% tree pellets, 45% municipal solid waste, and 20% manure. During a continuous operating cycle, the actual composition of the incoming feedstock changes: the supply of tree pellets decreases, with its proportion dropping from 35% to 30%; the proportion of municipal solid waste increases accordingly to 50%; and the proportion of manure remains unchanged at 20%. The system first executes the feedstock acquisition step, receiving a total of 30 tons of mixed solid feedstock that day, specifically including 9 tons of tree pellets, 15 tons of municipal solid waste, and 6 tons of manure. These raw materials then enter a standardized pretreatment process: 9 tons of branches and wood waste are processed by a 55kW hammer crusher with a 3mm mesh size to ensure that all output particles are within the 2-5mm range; 15 tons of municipal solid waste are sorted through a 10mm mesh drum screen, which rotates at 8 revolutions per minute, effectively separating approximately 1.3 tons of non-degradable impurities such as plastic bags, broken glass, and small metal parts, leaving approximately 13.7 tons of organic components for the next stage; 6 tons of livestock and poultry manure are processed by a screw extrusion solid-liquid separator, where a large amount of water is removed under a mechanical pressure of 0.8MPa, producing manure residue with a moisture content of approximately 60%. Subsequently, these three types of pretreated intermediate materials are conveyed to a 5-cubic-meter horizontal twin-shaft mixer. The mixer automatically batches materials according to a new ratio (30% tree pellets, 50% household waste, and 20% manure). During the mixing process, an integrated online near-infrared moisture detection system monitors the moisture content of the mixture in real time and precisely adds moisture through a controllable atomizing spray device, adjusting and stabilizing the overall moisture content of the mixed solid materials at around 18%. At this point, the carbon-to-nitrogen ratio (C / N) of the mixture is approximately 21:1, still within the suitable range for pyrolysis. Simultaneously, a gas feed line operating in parallel with the solid feed processing also operates synchronously. On that day, the anaerobic fermentation system produced approximately 11,500 cubic meters of crude biogas. This gas first entered a condensation and dehydration tower with the temperature controlled at 5°C, where water vapor was condensed and released, lowering the biogas dew point to below -20°C. The dehydrated biogas was then fed into a fixed-bed reactor filled with iron oxide desulfurizing agent, where a chemical reaction occurred at room temperature, reducing the concentration of hydrogen sulfide (H2S) in the biogas from approximately 1000 ppm to below 40 ppm, thus completing the purification process and obtaining pretreated biogas that meets the feed requirements.

[0081] After the pretreatment stage, the solid raw materials are continuously and stably fed into the pyrolysis gasification zone of the solid-gas coupling reactor at a rate of approximately 1.2 tons per hour via a precision screw feeder driven by a variable frequency motor. This reaction zone is a high-temperature resistant chamber with a volume of approximately 10 cubic meters, externally enclosed by an electrically heated jacket. The intelligent control system sets and maintains the target temperature of the pyrolysis gasification zone at 520°C based on changes in the raw material composition. At this temperature, the solid raw materials undergo pyrolysis and partial gasification. Due to the decreased proportion of tree particles (which have high lignocellulose content and high calorific value) and the increased proportion of municipal solid waste (which has complex composition, relatively low calorific value, and large fluctuations), the total amount and composition of the syngas produced by pyrolysis undergo subtle changes: monitoring data shows that the volume fraction of hydrogen in the syngas slightly decreases from the conventional approximately 16% to 15.5%, and the ratio of carbon monoxide and methane is also slightly adjusted. Meanwhile, based on a comprehensive assessment of real-time analysis data on the solid composition and calorific value of the feed, as well as historical operating models, the system's intelligent control unit issues a command before the syngas enters the mixing zone, increasing the feed rate of purified biogas from the baseline of 525 cubic meters per hour to 550 cubic meters per hour. This pressurized purified biogas is uniformly injected through an annular porous distributor located in the center of the reactor, entering a specific structural section known as the gas-solid mixing zone. This region is densely packed with honeycomb microchannels with an equivalent diameter of only 500 micrometers. The upward-flowing hot syngas (temperature approximately 520°C) and the downward-injected room-temperature purified biogas create a strong countercurrent flow within these microchannels. The micrometer-scale channel size creates a huge gas-gas contact surface area, ensuring that even under the aforementioned gas volume adjustments and composition changes, the two gas streams achieve vigorous molecular-level turbulence and thorough mixing within a very short distance and time. The temperature of the mixed gas stabilizes at around 500°C, and its compositional uniformity lays a solid foundation for subsequent reactions.

[0082] The thoroughly mixed gas then rises and enters the catalytic reaction zone located at the top of the reactor. This zone is filled with an adsorption-catalysis integrated particle fixed bed approximately 2.5 meters high and 4.5 cubic meters in volume. These particles are supported by a high specific surface area, large pore volume alumina-silica composite, uniformly loaded with 18% Ni-Co alloy nanoparticles (as catalytic active centers) and 35% ZSM-5 molecular sieve and high specific surface area activated carbon composite (as adsorption centers). The mixed gas flows through this catalyst bed at a temperature of 525°C and a pressure of 0.4 MPa. In this environment, the Ni-Co active sites efficiently catalyze two key reactions: the steam reforming of methane (CH4 + H2O → CO + 3H2) and the carbon monoxide conversion reaction (CO + H2O → CO2 + H2), thereby maximizing the conversion of CH4 and CO in the feed gas into the target product H2. The intelligent system's decision to increase the biogas inflow rate played a crucial role: the increased biogas provided an additional methane carbon source, effectively compensating for the potential decrease in the overall C / H ratio of the syngas due to the reduction in tree particles in the solid feedstock, and preventing catalyst carbon buildup or a decrease in hydrogen yield that could be caused by reactant imbalances. Simultaneously, trace amounts of impurities such as hydrogen sulfide (H2S) and ammonia (NH3) in the gas flowing through the particles were selectively adsorbed and captured by the regular micropores of the molecular sieves and the large specific surface area of ​​the activated carbon within the particles. This integrated "reaction-while-purification" model ensured that while improving hydrogen yield and selectivity, in-situ deep removal of toxic impurities was achieved, resulting in extremely low impurity content in the catalyst bed outlet gas.

[0083] The gaseous products (mainly containing H2, CO2, a small amount of unreacted CH4, and water vapor) after catalytic reforming and purification are discharged from the top outlet of the reactor and enter the product separation and purification stage. First, the gas enters a high-efficiency cyclone separator tangentially at a high flow rate. In the strong swirling flow field formed inside, the trace amounts of catalyst powder and ash particles entrained in the gas are subjected to strong centrifugal force, thrown against the separator wall, and collected in the bottom ash hopper, with a daily collection volume of approximately 1.4 tons. The separator is designed to achieve a separation efficiency exceeding 99%. The gas, after solid dust removal, is then cooled to approximately 40°C through heat exchange and enters the next key unit—the pressure swing adsorption (PSA) hydrogen purification system. This system employs a five-tower process, with each tower filled with a specialized adsorbent that has a high selective adsorption capacity for impurities such as CO2 and CH4. Under the control of the central control system, each adsorption tower undergoes a cycle of pressurization adsorption, forward depressurization, reverse depressurization, rinsing, and pressure equalization and pressurization. At an adsorption pressure of 2.2 MPa, hydrogen, as a weakly adsorbed component, preferentially passes through the adsorption bed and is output as a high-purity product; while strongly adsorbed components such as CO2 are retained by the adsorbent. Subsequently, the pressure in the adsorption tower is reduced to 0.15 MPa for desorption, and impurity gases (CO2-rich tail gas) are discharged, which can be reused as fuel. Although the initial composition of the raw material fluctuates, the intelligent control of the front-end reaction ensures that the gas composition entering the PSA system remains relatively stable, thus the hydrogen purification process remains smooth. The system produces approximately 9,400 standard cubic meters of hydrogen per day. Continuous monitoring by the online analyzer shows that the purity of the product hydrogen is consistently above 99.3%, the carbon monoxide content is below 50 ppm, and the content of other impurities fully meets the technical specifications for high-purity hydrogen in GB / T3634.1 "Hydrogen". The daily hydrogen yield fluctuation is successfully controlled within a very small range of ±2%.

[0084] Energy management is carried out synchronously and efficiently during system operation. A threaded tube heat exchanger with a total heat exchange area of ​​50 square meters is integrated on the outer wall of the pyrolysis gasification zone and catalytic reaction zone of the solid-gas coupled reactor. A large amount of high-temperature waste heat released during the reaction (exhaust gas temperature above 500℃) is effectively recovered by the circulating heat transfer oil within the heat exchanger through thermal radiation and conduction, raising the heat transfer oil temperature to approximately 280℃. This portion of the high-temperature heat transfer oil is pumped to a 50-cubic-meter heat storage tank with excellent insulation performance for temporary storage, with a daily heat loss rate of less than 2%. The stored heat constitutes the core of the system's internal thermal energy cycle: part of it passes through a raw material preheater, continuously preheating newly supplied solid raw materials at ambient temperature to approximately 150℃; another part passes through a biogas preheater, heating purified biogas from room temperature to 100℃. Through this tightly coupled waste heat recovery and reuse system, the comprehensive utilization rate of high-grade waste heat generated during the reaction process remains above 85%. This means that the energy consumption of fresh steam and electricity obtained from the external power grid or boiler to maintain the required reaction temperature has been significantly reduced. Calculations show that, even on days with fluctuating feedstock, the overall energy consumption per ton of hydrogen produced is still about 30% lower than that of traditional processes operating with fixed parameters. The "nerve center" of the entire process—the intelligent control unit—collects massive amounts of operational data in real time at a frequency of up to one second through more than 30 sensor nodes distributed throughout the plant, monitoring temperature, pressure, flow rate, and gas composition. This data is not only used for real-time display and alarms but is also fed into embedded advanced process control models and hydrogen yield prediction algorithms. In this example, these models identified the changing trends of feedstock components in advance and quickly calculated optimized parameters such as biogas replenishment flux, directing the actuators to make adjustments. Simultaneously, they coordinated fine-tuned pyrolysis temperature and system pressure, achieving adaptive optimization operation of the entire process under disturbance conditions, demonstrating robustness and stability far exceeding traditional processes.

[0085] In summary, this example demonstrates the strong adaptability and stability of the solid-gas two-phase feedstock co-processing integrated reaction method when facing common fluctuations in feedstock composition in actual production. From flexible pretreatment and precise allocation of feedstocks to intelligent control and efficient mixing of gas flow in the core reactor; from the integrated particle system in the catalytic reaction zone enabling simultaneous reaction and purification to the strict quality assurance of the separation and purification section; and finally to the cascaded energy recovery and intelligent global management of the entire system, each step is interconnected and works synergistically. Ultimately, even under the unfavorable condition of a 5 percentage point decrease in the proportion of tree particles, the system successfully suppressed hydrogen yield fluctuations within ±2% by actively adjusting strategies such as biogas feed, ensuring stable and compliant hydrogen purity while maintaining low system energy consumption. This fully verifies the significant technical advantages of this method compared to traditional phase-separation processes with poor feedstock adaptability and frequent manual intervention, showcasing its core value in high efficiency, high stability, and strong anti-interference capabilities, and providing a practical and feasible process path for the large-scale, commercial, and reliable operation of biomass hydrogen production technology.

[0086] Figure 5 A schematic diagram of the structure of an electronic device provided in an embodiment of this application. The electronic device may include: The memory 501, the processor 502, and the computer program stored on the memory 501 and capable of running on the processor 502.

[0087] When processor 502 executes the program, it implements the integrated reaction method for co-processing solid and gas dual-phase raw materials provided in the above embodiments.

[0088] Furthermore, electronic devices also include: Communication interface 503 is used for communication between memory 501 and processor 502.

[0089] The memory 501 is used to store computer programs that can run on the processor 502.

[0090] The memory 501 may include high-speed RAM (Random Access Memory) memory, and may also include non-volatile memory, such as at least one disk storage.

[0091] If the memory 501, processor 502, and communication interface 503 are implemented independently, then the communication interface 503, memory 501, and processor 502 can be interconnected via a bus to complete communication between them. The bus can be an ISA (Industry Standard Architecture) bus, a PCI (Peripheral Component Interconnect) bus, or an EISA (Extended Industry Standard Architecture) bus, etc. The bus can be divided into address bus, data bus, control bus, etc. For ease of representation, Figure 5 The bus is represented by a single thick line, but this does not mean that there is only one bus or one type of bus.

[0092] Optionally, in a specific implementation, if the memory 501, processor 502, and communication interface 503 are integrated on a single chip, then the memory 501, processor 502, and communication interface 503 can communicate with each other through an internal interface.

[0093] The processor 502 may be a CPU (Central Processing Unit), an ASIC (Application Specific Integrated Circuit), or one or more integrated circuits configured to implement the embodiments of this application.

[0094] In the description of this specification, the references to "one embodiment," "some embodiments," "example," "specific example," or "some examples," etc., indicate that a specific feature, structure, material, or characteristic described in connection with that embodiment or example is included in at least one embodiment or example of this application. In this specification, the illustrative expressions of the above terms do not necessarily refer to the same embodiment or example. Furthermore, the specific features, structures, materials, or characteristics described may be combined in any suitable manner in one or more embodiments or examples. Moreover, without contradiction, those skilled in the art can combine and integrate the different embodiments or examples described in this specification, as well as the features of different embodiments or examples.

[0095] Furthermore, the terms "first" and "second" are used for descriptive purposes only and should not be construed as indicating or implying relative importance or implicitly specifying the number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include at least one of that feature. In the description of this application, "multiple" means at least two, such as two, three, etc., unless otherwise explicitly specified.

[0096] Any process or method description in the flowchart or otherwise herein can be understood as representing a module, segment, or portion of code comprising one or more executable instructions for implementing custom logic functions or processes, and the scope of the preferred embodiments of this application includes additional implementations in which functions may be performed not in the order shown or discussed, including substantially simultaneously or in reverse order depending on the functions involved, as should be understood by those skilled in the art to which embodiments of this application pertain.

[0097] It should be understood that various parts of this application can be implemented using hardware, software, firmware, or a combination thereof. In the above embodiments, multiple steps or methods can be implemented using software or firmware stored in memory and executed by a suitable instruction execution system. For example, if implemented in hardware as in another embodiment, it can be implemented using any of the following techniques known in the art, or a combination thereof: discrete logic circuits having logic gates for implementing logical functions on data signals, application-specific integrated circuits (ASICs) having suitable combinational logic gates, programmable gate arrays (PGAs), field-programmable gate arrays (FPGAs), etc.

[0098] Those skilled in the art will understand that all or part of the steps of the methods described in the above embodiments can be implemented by a program instructing related hardware, and the program can be stored in a computer-readable storage medium. When executed, the program includes one or a combination of the steps of the method embodiments.

[0099] Although embodiments of this application have been shown and described above, it is understood that the above embodiments are exemplary and should not be construed as limiting this application. Those skilled in the art can make changes, modifications, substitutions and variations to the above embodiments within the scope of this application.

Claims

1. An integrated reaction system for co-processing solid and gaseous raw materials, characterized in that, include: The system includes a raw material pretreatment unit, a solid-gas coupling reactor, a catalytic reaction unit, a product separation unit, a waste heat recovery unit, and an intelligent control unit; among which, The raw material pretreatment unit is used to pretreat multi-source solid organic waste and mix it into solid raw materials, while purifying fermented biogas to prepare gaseous raw materials. The solid-gas coupling reactor is provided with a pyrolysis gasification zone and a gas-solid mixing zone with a built-in microchannel structure, which is used to pyrolyze solid raw materials into syngas and mix them countercurrently with gaseous raw materials in the microchannel. The catalytic reaction unit is integrated into the reactor and is used to catalytically reform the mixed gas to produce hydrogen and simultaneously remove impurities through an adsorption-catalysis integrated material. The product separation unit is used to sequentially perform gas-solid separation and pressure swing adsorption purification on the reformed product to remove solid dust and obtain high-purity hydrogen. The waste heat recovery unit is used to recover the reaction waste heat generated during pyrolysis gasification and catalytic reforming, and to preheat the solid and gaseous raw materials entering the system. The intelligent control unit is used to monitor key parameters of the system, such as temperature, pressure, gas composition, and flow rate, in real time, and automatically adjust the system operating conditions.

2. The integrated reaction system for co-processing solid and gaseous raw materials according to claim 1, characterized in that, The raw material pretreatment unit includes a crushing device, a screening device, a solid-liquid separation device, a mixing device, and a biogas pretreatment device. The crushing device crushes the tree raw materials into 2-5mm particles; the screening device removes non-degradable impurities from domestic waste; the solid-liquid separation device separates the manure; the mixing device mixes the solid raw materials at a mass fraction of 30%-40%:40%-50%:10%-20% and controls the moisture content to 15%-20% and the carbon-to-nitrogen ratio to 20-25:1; the biogas pretreatment device dehydrates and desulfurizes the fermented biogas to ensure an H2S content ≤50ppm.

3. The integrated reaction system for co-processing solid and gaseous raw materials according to claim 1, characterized in that, The solid-gas coupling reactor is a vertical cylindrical structure, with a gas-solid mixing zone, a catalytic reaction zone, and a pyrolysis gasification zone arranged sequentially from top to bottom inside. The gas-solid mixing zone has a built-in microchannel structure with a channel size of 500 μm and a specific surface area ≥3000 m² / m³. It adopts a gas-solid countercurrent contact design with a gas flow rate of 0.8 m / s and a solid flow rate of 0.05 m / s. The catalytic reaction zone is filled with adsorption-catalysis integrated particles, with the particle layer height accounting for 60%-70% of the reaction zone volume. The pyrolysis gasification zone is equipped with an electric heating jacket and waste heat recovery heat exchange pipeline on its outer side. The reaction temperature is controlled at 500-550℃ through the coordinated control of external heating and waste heat recovery.

4. The integrated reaction system for co-processing solid and gaseous raw materials according to claim 1, characterized in that, The catalytic reaction unit includes integrated adsorption-catalysis particles and a reaction zone temperature and pressure control system. The integrated adsorption-catalysis particles consist of an alumina-silica composite carrier, a Ni-Co alloy active component, and a molecular sieve and activated carbon composite adsorption component, with a particle size of 3-5 mm. The Ni-Co alloy active component accounts for 15%-20% of the mass, and the molecular sieve and activated carbon composite adsorption component accounts for 30%-40% of the mass. The reaction zone temperature and pressure control system includes distributed temperature sensors, pressure transmitters, and regulating valves, used to monitor and automatically control the temperature of the catalytic reaction zone at 400-600℃ and the pressure at 0.3-0.5 MPa in real time, ensuring the efficient and stable progress of the reforming reaction.

5. The integrated reaction system for co-processing solid and gaseous raw materials according to claim 1, characterized in that, The product separation unit includes a cyclone separator and a pressure swing adsorption (PSA) device. The cyclone separator is used to remove solid dust from the reaction products with a separation efficiency of ≥99%. The PSA device adopts a 5-tower process with an adsorption pressure of 2.0-2.5 MPa and a desorption pressure of 0.1-0.2 MPa. It is used to purify hydrogen to achieve a hydrogen purity of ≥99.2% and a hydrogen recovery rate of ≥90%.

6. The integrated reaction system for co-processing solid and gaseous raw materials according to claim 1, characterized in that, The waste heat recovery unit includes a threaded tube heat exchanger and a heat storage tank. The threaded tube heat exchanger is used to recover the high-temperature waste heat generated in the pyrolysis gasification zone and the catalytic reaction zone. The heat storage tank is used to store the waste heat recovered by the heat exchanger and to preheat solid raw materials to 150°C and biogas to 100°C. The system waste heat utilization rate is ≥85%.

7. The integrated reaction system for co-processing solid and gaseous raw materials according to claim 1, characterized in that, The intelligent control unit includes a controller, a sensor network, a parameter prediction model, and a remote monitoring terminal. The controller is used to link various sensors and actuators to automatically adjust the feed rate, reaction temperature, and pressure. The sensor network is used to collect temperature, pressure, gas composition, and flow rate data of each unit. The parameter prediction model is used to predict the trend of hydrogen yield changes and adjust operating parameters in advance. The remote monitoring terminal is used to view system operating data in real time, receive early warning information, and remotely control the system.

8. The integrated reaction system for co-processing solid and gaseous raw materials according to claim 1, characterized in that, The raw material pretreatment unit is connected to the solid-gas coupling reactor, which is connected to the product separation unit; the catalytic reaction unit is integrated inside the solid-gas coupling reactor; the waste heat recovery unit is connected to both the solid-gas coupling reactor and the raw material pretreatment unit; and the intelligent control unit is linked with each of the other units.

9. An integrated reaction method for co-processing solid-gas dual-phase raw materials, characterized in that, include: Obtain solid raw materials and biogas; Solid raw materials are processed and mixed to obtain pretreated solid raw materials, while biogas is dehydrated and desulfurized to obtain pretreated biogas. The pretreated solid raw material is fed into a solid-gas coupling reactor for pyrolysis and gasification to generate syngas. The syngas and the pretreated biogas are then mixed countercurrently in the microchannel structure of the reactor to obtain a mixed gas. The mixed gas is introduced into the catalytic reaction zone, where it undergoes catalytic reforming to produce hydrogen and removes impurities simultaneously under the action of adsorption-catalysis integrated particles, yielding a hydrogen-containing product. Subsequently, the hydrogen-containing product is subjected to gas-solid separation and hydrogen purification to obtain high-purity hydrogen. The waste heat generated during the pyrolysis gasification and catalytic reforming process is recovered and used to preheat the pretreated solid raw materials and the pretreated biogas. At the same time, the entire process operation parameters are monitored and automatically adjusted in real time by an intelligent control unit.

10. An electronic device, characterized in that, include: The memory, the processor, and the computer program stored in the memory and executable on the processor, the processor executing the program to implement the integrated reaction method for co-processing solid and gaseous raw materials as described in claim 9.

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