An electrically driven reactor based on an integral honeycomb structure with conductive heating and its application
By employing an electrically driven reactor with an integral honeycomb structure and conductive heating in the methane reforming reactor, the problems of uneven temperature distribution and low heat utilization have been solved, achieving a highly efficient and environmentally friendly methane reforming process.
Patent Information
- Application Number
- CN202411381547.0
- Authority / Receiving Office
- CN · China
- Patent Type
- Patents(China)
- Current Assignee / Owner
- Filing Date
- 2024-09-30
- Publication Date
- 2025-12-02
- Estimated Expiration
- 2044-09-30
AI Technical Summary
Existing methane reforming reactors suffer from problems such as uneven internal temperature distribution, low heat utilization, complex operation, and high maintenance costs.
An electrically driven reactor based on an integral honeycomb structure for conductive heating is adopted. By setting an integral honeycomb structure heater inside the cylinder, Joule heating is used. The fluid channels are filled with catalyst particles, and the space between the outer wall and the cylinder is filled with insulation material to achieve uniform heat supply.
It improves heat transfer efficiency and energy utilization, reduces local overheating, has a simple structure and is easy to operate, reduces maintenance costs, and reduces carbon dioxide emissions.
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Figure CN119140016B_ABST
Abstract
Description
Technical Field
[0001] This invention belongs to the field of reactor design technology, specifically, it relates to an electrically driven reactor based on an integral honeycomb structure with conductive heating and its application. Background Technology
[0002] Methane reforming is an important industrial chemical process used to produce hydrogen and carbon monoxide. This technology is widely used in petrochemicals, ammonia synthesis, fuel cells, and other fields. The basic process of methane reforming involves reacting methane with one or more of water vapor, carbon dioxide, and oxygen at high temperatures using a catalyst to convert them into hydrogen and carbon monoxide. Common methane reforming processes include steam reforming, carbon dioxide reforming, combined reforming, and triple reforming. The methane reforming process is highly endothermic, therefore sufficient heat must be supplied to the reactor to meet the reaction requirements. Methane reforming typically requires high-temperature conditions; an unreasonable temperature distribution within the reactor can easily lead to carbon buildup, causing catalyst sintering and deactivation, and affecting the long-term stable operation of the unit.
[0003] For the tubular reactors commonly used in traditional reforming reactions, heat is transferred to the catalyst and reactant gases through the reactor walls via radiation and convection, resulting in relatively low thermal efficiency. Due to their endothermic reaction characteristics, the temperature distribution inside the reactor tubes is uneven, with the bed temperature near the wall being much higher than the center temperature, leading to low heat transfer efficiency and poor energy utilization. To improve the reaction conversion rate, the temperature of the outer wall of the reactor tubes needs to be increased to ensure that the center of the bed meets the reaction temperature requirements. However, the bed near the outer wall of the reactor tubes is prone to localized high temperatures, leading to carbon buildup and sintering deactivation of the catalyst. Therefore, maintaining a uniform temperature distribution inside the reactor and preventing localized high-temperature zones has become a major focus in endothermic reaction technologies such as methane reforming. To address the shortcomings of existing technologies, there is a need to develop a reactor with a simple and compact structure, uniform heat distribution, high energy utilization, and easy operation.
[0004] CN113301981A discloses a conductive honeycomb structure comprising a plurality of intersecting porous walls arranged to provide a pore matrix. Applying this invention to a catalytic reaction system requires coating the wall surfaces with catalyst, which is a complex process that is prone to detachment during use, resulting in high maintenance costs.
[0005] CN103204464A discloses a honeycomb oxygen carrier reactor for chemical reforming of methane, comprising a reactor body including an outer wall and an external heating cylinder, with a honeycomb oxygen carrier formed within the outer wall and heating cylinder. The main purpose of this invention is to use a honeycomb oxygen carrier reactor for chemical reforming of methane to produce syngas. The oxygen carrier transfers lattice oxygen and heat to the methane, eliminating the need for pure oxygen preparation and rapid circulation of driving solid particles, thus achieving mild operating conditions and isothermal operation. However, this reactor still requires external wall heating, resulting in a large heat transfer scale within the reactor; the reaction process does not require a catalyst, and the honeycomb oxygen carrier is integrally formed after high-temperature pressing and sintering, making the process more complex than directly filling catalyst particles; furthermore, the operation requires fuel reforming, gas purging, and air regeneration steps, leading to complex operation and low efficiency, thus presenting significant challenges for practical industrial application.
[0006] Therefore, for practical industrial applications, there is still a need to address the requirements of simple operation, long lifespan, and low maintenance costs. Summary of the Invention
[0007] The purpose of this invention is to overcome the shortcomings of existing external wall heating reactors, such as uneven internal temperature distribution, low heat transfer efficiency, low heat utilization rate, and inconvenient operation, and to provide an electrically driven reactor based on an integral honeycomb structure with conductive heating.
[0008] To achieve the above objectives, a first aspect of the present invention provides an electrically driven reactor based on a conductive heating integral honeycomb structure, comprising a cylindrical body, wherein an integral honeycomb structure heater that generates Joule heat under energized conditions is disposed inside the cylindrical body. The integral honeycomb structure heater is cylindrical, and a plurality of regularly arranged longitudinal fluid channels are formed inside the cylinder, which are filled with catalyst particles. Thermal insulation material is filled between the outer wall of the integral honeycomb structure heater and the inner wall of the cylindrical body. An upper end cap and a lower end cap are respectively provided at the upper and lower ends of the cylindrical body, with a gas inlet on the upper end cap and a gas outlet on the lower end cap. A gas distributor is provided between the upper end cap and the cylindrical body, and a catalyst support plate is provided between the lower end cap and the cylindrical body. A strip-shaped flow guide conductor is provided on the outer wall of the integral honeycomb structure heater, and a corresponding wire interface is provided on the cylindrical body at the position corresponding to the strip-shaped flow guide conductor. The strip-shaped flow guide conductor is led out of the reactor and connected to an external power source via a wire through the wire interface.
[0009] According to the present invention, the cross-section of the fluid channel is an equilateral triangle, a regular quadrilateral, or a regular hexagon, and all fluid channels have the same wall thickness.
[0010] According to the present invention, the shape of the catalyst particles filling the fluid channel is selected from one or more combinations of spherical, cylindrical, Raschig ring, four-hole column, and seven-hole column.
[0011] Preferably, the catalyst particles are randomly stacked from the bottom to the top of each fluid channel.
[0012] According to the present invention, the material of the integral honeycomb structure heater is selected from Fe, Cr, Ni, Cu, Al, Co, Si or alloys thereof; the material of the strip-shaped current-guiding conductor is selected from Fe, Cr, Ni, Cu, Al, Co, Si or alloys thereof, and the resistivity is lower than that of the material of the integral honeycomb structure heater.
[0013] According to the present invention, the upper end of the thermal insulation material is higher than the upper surface of the integral honeycomb structure heater, thereby forming a reactor cavity between the honeycomb structure heater and the gas distributor; the lower end of the thermal insulation material is flush with the lower end of the cylinder and the lower end of the integral honeycomb structure heater.
[0014] According to the present invention, the gas distributor is a disc shape that matches the inner wall of the cylinder, the outer edge of its lower surface abuts against the upper surface of the insulation layer, and the middle part corresponding to the region of the reactor cavity is provided with regularly arranged air holes that allow gas to pass through; preferably, the air holes are circular channels, and the arrangement of the air holes is circular.
[0015] According to the present invention, the catalyst support plate abuts against the bottom end of the integral honeycomb structure heater and the insulation material, and the contact area between the catalyst support plate and the bottom end of the integral honeycomb structure heater is provided with dense pores.
[0016] According to the present invention, the thermal insulation material is selected from one or more combinations of glass wool, rock wool, aluminum silicate, and composite silicates.
[0017] A second aspect of the invention provides the application of the above-described electrically driven reactor based on a conductive heating integral honeycomb structure for use in endothermic reaction systems of methane steam / dry gas reforming or methane combined / triple reforming.
[0018] The present invention has the following beneficial effects:
[0019] 1. The electric-driven reactor of the present invention uses electric heating instead of traditional fuel oil heating, which reduces carbon dioxide emissions and the footprint of the device; by setting an integral honeycomb structure heater in the cylinder, it can respond quickly when energized and reach the reaction temperature in a short time, saving start-up time.
[0020] 2. By filling the elongated fluid channels of the integral honeycomb structure heater with catalyst particles, the heat transfer path is effectively shortened. The continuous heating of the outer wall of the fluid channel and the uniform heat supply can reduce local overheating, further improving the heat transfer efficiency and energy utilization rate, making the reaction more complete and avoiding the reduction in reaction efficiency caused by uneven temperature.
[0021] 3. The electrically driven reactor based on the conductive heating integral honeycomb structure of the present invention has a simple structure, is easy to operate, and is energy-saving and environmentally friendly, which is conducive to its promotion and application in production practice. Attached Figure Description
[0022] Figure 1 This is a cross-sectional schematic diagram of the electrically driven reactor based on a conductive heating integral honeycomb structure according to the present invention.
[0023] Figure 2 for Figure 1 A schematic diagram of the gas distributor in the diagram.
[0024] Figure 3 A and 3B are schematic diagrams of the structure and cross-section of the electrically driven heater and the channel filled with spherical catalyst particles in Example 1, respectively.
[0025] Figure 4 A and 4B are schematic diagrams of the structure and cross-section of the electrically driven heater and the channel filled with Raschig ring catalyst particles, respectively, in Example 2.
[0026] Figure 5 A and 5B are schematic diagrams of the structure and cross-section of the electrically driven heater and the channel filled with seven-hole column catalyst particles, respectively, in Example 3. Detailed Implementation
[0027] The present invention will be further described below with reference to the accompanying drawings and specific embodiments. It should be understood that these embodiments are for illustrative purposes only and are not intended to limit the scope of the invention. Furthermore, it should be understood that after reading the teachings of this invention, those skilled in the art can determine the specific process conditions based on the disclosed principles, implementation methods, and the uses of related processes and common knowledge in the art. Process equipment or apparatus not specifically specified in the following embodiments are all conventional equipment or apparatus in the art.
[0028] In the description of this application, it should be understood that if terms such as "upper", "lower", "top", "bottom", "upper end", "lower end", "thickness", etc. appear, these terms indicate the orientation or positional relationship based on the orientation or positional relationship shown in the accompanying drawings, and are only for the convenience of describing this application and simplifying the description, and do not indicate or imply that the device or element referred to must have a specific orientation, or be constructed and operated in a specific orientation, and therefore should not be construed as a limitation of this application.
[0029] Example 1
[0030] This embodiment provides an electrically driven reactor based on a conductive heating integral honeycomb structure, suitable for endothermic reaction systems such as methane steam / dry gas reforming and methane combined / triple reforming. Figure 1 As shown, the electrically driven reactor includes a cylindrical body 4. Inside the cylindrical body 4 is an integral honeycomb structure heater 9 that generates Joule heat under energized conditions. The honeycomb structure heater 9 is cylindrical, and its interior forms several regularly arranged longitudinal, elongated fluid channels 12, which are filled with catalyst particles 10. A thermal insulation material 13 is filled between the outer wall of the honeycomb structure heater 9 and the inner wall of the cylindrical body 4 to prevent heat loss caused by heat exchange between the Joule heat generated by the honeycomb structure heater 9 and the environment through the wall of the cylindrical body 4. The upper end of the cylinder 4 is provided with an upper end cap 2 and a lower end cap 5, respectively. The upper end cap 2 is provided with a gas inlet 1 and the lower end cap 5 is provided with a gas outlet 6. A gas distributor 3 is provided between the upper end cap 2 and the cylinder 4 to optimize the airflow distribution. A catalyst support plate 8 is provided between the lower end cap 5 and the cylinder 4. A strip-shaped flow guide conductor 11 is provided on the outer wall of the honeycomb structure heater 9, and a corresponding wire interface 7 is provided on the cylinder 4 at the position of the strip-shaped flow guide conductor 11. The strip-shaped flow guide conductor 11 is led out of the reactor and connected to an external power source through the wire interface 7 via a wire.
[0031] In this embodiment, the diameter of the cylinder 4 is preferably 300mm to 600mm.
[0032] The cross-section of the fluid channel 12 is an equilateral triangle, a regular quadrilateral, or a regular hexagon. In this embodiment, the cross-section of the fluid channel 12 is a regular hexagon, with a side length of 30mm to 60mm and a length of 1000mm to 1500mm. Figure 3 A and Figure 3 As shown in B; preferably, all fluid channels 12 have the same wall thickness, and the DC power supply passes through the honeycomb structure heater 9 and forms a uniform current distribution; the Joule heat power generated by all outer walls of the fluid channels 12 is the same, and the overall temperature reaches above 1000°C.
[0033] The catalyst particles 10 filling the fluid channel 12 are selected from one or more combinations of spherical, cylindrical, Raschig ring, four-hole column, and seven-hole column. In this embodiment, they are spherical catalyst particles with a particle size of 10 mm to 20 mm. The catalyst particles 10 are randomly stacked from the bottom to the top of each fluid channel 12, and part of the outer wall of the catalyst particles 10 is close to the heating inner wall of the fluid channel 12.
[0034] The specific structural design of the internal fluid channels 12 of the aforementioned honeycomb structure heater 9 and the specific filling method of the catalyst particles 10 ensure that the thermal conductivity of each fluid channel 12 is consistent, which helps to form a uniform heat distribution inside the integral honeycomb structure heater 9, avoids local heat accumulation or loss, and thus improves energy transfer efficiency.
[0035] The current distribution in the integral honeycomb structure heater 9 is governed by Ohm's law. Under direct current, Ohm's law is defined as:
[0036] U = R·I
[0037] Where U is electric potential, and its unit is V; R is resistance, and its unit is Ω; I is current, and its unit is A.
[0038] When a direct current is applied to a three-dimensional geometric structure, the electric field vector E (in V / m) can be written as:
[0039] E = ρ res ·J
[0040] Where ρ res J is resistivity, with units of Ω·m; J is the current density vector, with units of A / m. 2 .
[0041]
[0042] Due to resistivity ρ res Due to the inherent properties of the material, the resistance R depends only on the geometry of the heater, meaning that the heat power supplied to the area can be adjusted by changing the cross-sectional area.
[0043] Preferably, the material of the integral honeycomb structure heater 9 is selected from Fe, Cr, Ni, Cu, Al, Co, Si or alloys thereof. Furthermore, the integral honeycomb structure heater 9 employs an integrated manufacturing process, such as 3D printing, extrusion molding, or other known processes, to ensure that the heater has good thermal conductivity and mechanical strength.
[0044] Furthermore, the strip-shaped current-guiding conductor 11 is disposed at the top and bottom of the outer wall of the integral honeycomb structure heater 9; preferably, the strip-shaped current-guiding conductor 11 surrounds the honeycomb structure heater 9 once at the top and bottom of the outer wall of the honeycomb structure heater 9, and is tightly fitted to it. The material of the strip-shaped current-guiding conductor 11 has a lower resistivity than the material of the integral honeycomb structure heater 9, and its material is selected from Fe, Cr, Ni, Cu, Al, Co, Si or alloys thereof.
[0045] The upper end of the insulation material 13 is higher than the upper surface of the honeycomb structure heater 9, thereby forming a reactor cavity 14 between the honeycomb structure heater 9 and the gas distributor 3; the lower end of the insulation material 13 is flush with the lower end of the cylinder 4 and the lower end of the honeycomb structure heater 9; the material of the insulation material 13 is selected from one or more combinations of glass wool, rock wool, aluminum silicate, and composite silicate.
[0046] The gas inlet 1 is located at the top of the upper head 2, and the interior of the upper head 2 has a sufficiently large cavity to ensure that the gas entering the reactor can flow fully; the gas outlet 6 is located at the bottom of the lower head 5, and the interior of the lower head has a sufficiently large cavity to ensure that the gas products flow out smoothly and reduce the disturbance of the gas distribution in the catalyst bed caused by the gas leaving the reactor.
[0047] like Figure 2 As shown, the gas distributor 3 is a disc-shaped device that matches the inner wall of the cylinder 4. The outer edge of its lower surface abuts against the upper surface of the insulation material 13. The central part, corresponding to the region of the reactor cavity 14, is provided with regularly arranged vents 15 that allow gas to pass through. Preferably, the vents 15 are circular channels, and the arrangement of the vents 15 is circular.
[0048] The catalyst support plate 8 abuts against the bottom of the integral honeycomb structure heater 9 and the insulation material 13, and the contact area between the catalyst support plate 8 and the bottom of the honeycomb structure heater 9 is provided with dense air holes, so as to support the catalyst particles 10 filled in the honeycomb structure heater 9 and its internal fluid channel 12, while ensuring that the gas in the catalyst bed can pass through smoothly, but intercepting the catalyst particles that are carried out of the bed due to gravity and gas passage.
[0049] Preferably, both the gas distributor 3 and the catalyst support plate 8 are made of insulating material and have certain mechanical strength and stability, ensuring that the current distribution is not disturbed when the integral honeycomb structure heater is powered on.
[0050] In this embodiment, the electrically driven reactor is used for methane co-reforming. The reactant gas, preheated and treated in the reactor's upstream process, enters the reactor through the gas inlet 1 at the top of the upper head 2. It flows freely within the cavity of the upper head 2, and after further optimization of the gas flow distribution by the gas distributor 3, it enters the catalyst bed inside the honeycomb structure heater 9, reacting with the catalyst particles in the fluid channel 12. Under the uniform Joule heating generated in the fluid channel 12, the catalyst particles 10 effectively catalyze the methane co-reforming reaction, partially or completely converting methane, water vapor, and carbon dioxide into hydrogen and carbon monoxide. The integral honeycomb structure heater 9 generates Joule heating via direct current, continuously heating within the reactor to ensure that the reactor temperature remains within a preset range. This design helps maintain a uniform heat distribution inside the reactor, reduces the occurrence of side reactions, and further improves the efficiency and energy conversion rate of the methane reforming reaction. The generated hydrogen, carbon monoxide, other products, or unreacted gases are discharged from the gas outlet 6 at the bottom of the lower head 5 and collected and treated.
[0051] When the reaction proceeds for a period of time, the catalyst activity decreases due to carbon buildup on the catalyst, and the catalyst needs to be regenerated. At this time, the gas inlet 1 at the top of the upper head 2 stops supplying the reaction gas and instead supplies the regeneration gas (which is a mixture of one or more gases such as air, oxygen, carbon dioxide, water vapor, and hydrogen). The DC current supplied to the reactor is set to meet the temperature requirements for catalyst regeneration. The waste gas generated in the reaction zone flows out through the gas outlet 6 at the top of the lower head 5.
[0052] Example 2
[0053] The structure and operating conditions of the electrically driven reactor based on the conductive heating integral honeycomb structure in this embodiment are basically the same as those in Embodiment 1. For example... Figure 4 A and Figure 4 As shown in B, the only difference from Example 1 is that the catalyst particles 10 filled in the fluid channel 12 are Raschig ring catalyst particles with an outer diameter of 10 mm to 20 mm and an inner diameter of 5 mm to 15 mm. The catalyst particles 10 are randomly stacked from the bottom of each fluid channel 12, forming a slender Raschig ring catalyst particle random stacking structure in each fluid channel 12.
[0054] The above configuration helps reduce the catalyst packing volume within the fluid channel 12, while the line-to-surface contact between the catalyst particles 10 improves the heat transfer efficiency of the bed within a single fluid channel 12. The special geometry of the Raschig ring catalyst particles increases the catalyst's surface area, thereby promoting sufficient contact between the reactant gas and the catalyst, and thus improving catalyst utilization. This design further enhances the overall reactor's reaction performance, ensuring higher conversion rates. This optimized structural design enables the reactor to provide a more stable and efficient methane reforming process in industrial applications, thereby meeting higher production demands.
[0055] Example 3
[0056] The structure and operating conditions of the electrically driven reactor based on the conductive heating integral honeycomb structure in this embodiment are basically the same as those in Embodiment 1. For example... Figure 5 A and Figure 5 As shown in B, the main difference from the embodiment is that the catalyst particles 10 filled in the fluid channel 12 are seven-hole column catalyst particles with an outer diameter of 10 mm to 20 mm and an inner diameter of 2 mm to 5 mm. The catalyst particles are randomly stacked from the bottom of each fluid channel 12, forming a slender catalyst particle random stacking structure in each fluid channel 12.
[0057] With the above configuration, the packing density of catalyst particles 10 within the fluid channel 12 is increased, and the heat transfer efficiency within a single fluid channel 12 is improved, thereby enhancing the overall reactor's reaction performance. Because the catalyst particles are densely packed within the fluid channel 12, the reactant gas can more fully contact the catalyst particles 10 as it passes through these fluid channels 12, thus improving the reaction conversion rate.
[0058] Example 4
[0059] The operating conditions of the electrically driven reactor based on the conductive heating integral honeycomb structure in this embodiment are the same as those in Embodiment 1. The main difference between the reactor structure and Embodiment 1 is that the fluid channel 12 inside the integral honeycomb structure heater 9 is a regular quadrilateral with a side length of 50mm to 80mm. The catalyst particles 10 filled in the fluid channel 12 are spherical catalyst particles with an outer diameter of 10mm to 20mm. The catalyst particles are randomly stacked from the bottom of each fluid channel 12, forming a slender random stacking structure of catalyst particles in each fluid channel 12.
[0060] Example 5
[0061] The operating conditions of the electrically driven reactor based on the conductive heating integral honeycomb structure in this embodiment are the same as those in Embodiment 4. The main difference between the reactor structure and Embodiment 4 is that the catalyst particles 10 filled in the fluid channels 12 of the integral honeycomb structure heater 9 are Raschig ring catalyst particles. The outer diameter of the catalyst particles is 10mm to 20mm and the inner diameter is 5mm to 15mm. The catalyst particles are randomly stacked from the bottom of each fluid channel 12, forming a slender random stacking structure of catalyst particles in each fluid channel 12.
[0062] Example 6
[0063] The operating conditions of the electrically driven reactor based on the conductive heating integral honeycomb structure in this embodiment are the same as those in Embodiment 4. The main difference between the reactor structure and Embodiment 4 is that the catalyst particles 10 filled in the fluid channels 12 of the integral honeycomb structure heater 9 are seven-hole column catalyst particles. The outer diameter of the catalyst particles is 10mm to 20mm, and the inner diameter is 2mm to 5mm. The catalyst particles are randomly stacked from the bottom of each fluid channel 12, forming a slender random stacking structure of catalyst particles in each fluid channel 12.
[0064] Application Example 1
[0065] This application embodiment, based on Embodiments 1-3, uses the same reactor for methane mixed reforming, differing only in the catalyst packing structure within the fluid channel 12 of the integral honeycomb structure heater 9. The channel is filled with spherical, Raschig ring, and seven-hole column catalyst particles with an outer diameter of 15 mm, respectively. The inner diameters of the Raschig rings and the seven-hole columns are 6 mm and 3 mm, respectively. By comparing the effects of different packing structures of the catalyst particles 10 within the integral honeycomb structure heater 9 on reactor performance, and further comparing it with a traditional tubular reactor heated by fuel oil, the advantages of the electrically driven reactor based on a conductive heating integral honeycomb structure of this invention are highlighted. Specifically, the process includes the following steps:
[0066] A mixture of 4212 L / h methane, 8424 L / h steam, and 1404 L / h carbon dioxide, preheated to 600°C, enters the reactor from the top via gas inlet 1. The mixture flows downwards through the upper head 2, where it is uniformly distributed by the gas distribution plate 15. After passing through the reactor cavity 14, the mixture fully develops and enters the bed of each fluid channel 12 in the integral honeycomb structure heater 9, where a methane co-reforming reaction occurs at a reaction temperature of 850°C. The fluid channels 12 are regular hexagons with sides of 60 mm and a length of 1200 mm. The reactant and product gases from each fluid channel 12 flow through the catalyst support plate 8 into the lower head 5, collect, and then exit through the gas outlet 6.
[0067] Comparative Example 1
[0068] To demonstrate the performance advantages of the electrically driven reactor based on the conductive heating integral honeycomb structure of the present invention, a conventional fuel oil-heated tubular reactor was used as a control 1. The operating conditions, including inlet composition, preheating temperature, catalyst loading amount, reaction temperature, and space velocity, were the same as those in Examples 1-3. The difference was that the conventional reactor adopted a tubular structure with 40 pipes, each with a diameter of 60 mm and a length of 1200 mm. The pipes were filled with seven-hole column catalyst particles with an outer diameter of 15 mm and an inner diameter of 3 mm. The heating condition was fuel oil combustion heating, and the reactor needed to reserve a fuel combustion cavity.
[0069] The methane and carbon dioxide conversion rates at the reactor outlets of Examples 1-3 and Control 1, as well as the radial temperature difference in the channels, are shown in Table 1.
[0070] Table 1: Outlet methane and carbon dioxide conversion rates and radial temperature difference in the channel
[0071] Methane conversion rate / % Channel radial temperature difference / ℃ Example 1 67.8 20 Example 2 69.3 17 Example 3 70.5 16 Comparison 1 65.2 32
[0072] Application Example 2
[0073] This application example, based on Examples 4-6, uses the same reactor for a methane mixed reforming reaction at a reaction temperature of 1150°C. The reactor performance is compared using a quadrilateral fluid channel 12 within an integral honeycomb heater 9, filled with catalyst particles 10 of different shapes. The operating conditions, including inlet composition, catalyst loading, inlet temperature, and space velocity, are identical to those in Application Example 1. The main difference is that the fluid channel 12 is a quadrilateral with a side length of 60 mm and a length of 1200 mm. The fluid channel 12 in Examples 4-6 is filled with spherical, Raschig ring, and seven-hole column catalysts, respectively. The structure and specifications of the catalyst particles are the same as in Application Example 1.
[0074] Comparative Example 2
[0075] The operating conditions of Comparative Example 2, including inlet composition, catalyst loading, catalyst geometry, and space velocity, were identical to those of Comparative Example 1. A conventional tubular reactor filled with seven-hole column catalyst particles was used as a control, with the number and specifications of the tubes remaining the same. The main difference was that the gas entering the conventional tubular reactor was preheated to 800°C, and the reaction temperature was 1150°C.
[0076] The methane and carbon dioxide conversion rates at the reactor outlets and the radial temperature differences in the channels for Examples 4-6 and Control 2 are shown in Table 2.
[0077] Table 2: Outlet methane and carbon dioxide conversion rates and radial temperature difference in the channel
[0078] Methane conversion rate / % Channel radial temperature difference / ℃ Example 4 86.8 37 Example 5 87.5 35 Example 6 87.9 34 Comparison 2 83.4 52
[0079] As shown in Tables 1 and 2, the electrically driven reactor based on the conductive heating integral honeycomb structure of the present invention has higher methane and carbon dioxide conversion rates. This is due to the uniform Joule heat generated on the outer wall of the channel to power the catalyst. The larger energy supply area and smaller heat transfer path reduce the radial temperature gradient of the catalyst bed within the channel, allowing for full utilization of the catalyst and lower energy consumption. Simultaneously, the electrically driven reactor based on the conductive heating integral honeycomb structure of the present invention eliminates the extra volume of the fuel oil combustion cavity, making the reactor more compact.
[0080] The above description is merely a detailed explanation of preferred embodiments and principles of the present invention. For those skilled in the art, there may be changes in specific implementation methods based on the ideas provided by the present invention, and these changes should also be considered within the scope of protection of the present invention.
Claims
1. An electrically driven reactor based on a conductive heating integral honeycomb structure, characterized in that, The electrically driven reactor includes a cylindrical body (4), inside which is a monolithic honeycomb structure heater (9) that generates Joule heat under energized conditions. The monolithic honeycomb structure heater (9) is cylindrical, and its interior has several regularly arranged longitudinal fluid channels (12), which are filled with catalyst particles (10). The outer wall of the monolithic honeycomb structure heater (9) and the inner wall of the cylindrical body (4) are filled with thermal insulation material (13). The upper and lower ends of the cylindrical body (4) are respectively provided with an upper end cap (2) and a lower end cap (5), and the upper end cap... The head (2) is provided with a gas inlet (1), and the lower head (5) is provided with a gas outlet (6); a gas distributor (3) is provided between the upper head (2) and the cylinder (4), and a catalyst support plate (8) is provided between the lower head (5) and the cylinder (4); a strip-shaped flow guide conductor (11) is provided on the outer wall of the integral honeycomb structure heater (9), and a corresponding wire interface (7) is provided on the cylinder (4) corresponding to the position of the strip-shaped flow guide conductor (11). The strip-shaped flow guide conductor (11) is led out of the reactor through the wire interface (7) and connected to an external power source. The catalyst particles (10) are randomly stacked from the bottom to the top of each fluid channel (12); The upper end of the insulation material (13) is higher than the upper surface of the integral honeycomb structure heater (9), thereby forming a reactor cavity (14) between the honeycomb structure heater (9) and the gas distributor (3); the lower end of the insulation material (13) is flush with the lower end of the cylinder (4) and the lower end of the integral honeycomb structure heater (9). The gas distributor (3) is a disc-shaped device that matches the inner wall of the cylinder (4). The outer edge of its lower surface abuts against the upper surface of the insulation material (13). The middle part, corresponding to the region of the reactor cavity (14), is provided with regularly arranged pores (15) that allow gas to pass through.
2. The electrically driven reactor according to claim 1, characterized in that, The cross-section of the fluid channel (12) is an equilateral triangle, a regular quadrilateral or a regular hexagon, and all fluid channels (12) have the same wall thickness.
3. The electrically driven reactor according to claim 1, characterized in that, The catalyst particles (10) filling the fluid channel (12) are selected from one or more combinations of spherical, cylindrical, Raschig ring, four-hole column, and seven-hole column.
4. The electrically driven reactor according to claim 1, characterized in that, The material of the integral honeycomb structure heater (9) is selected from Fe, Cr, Ni, Cu, Al, Co, Si or their alloys, and the material of the strip-shaped current-guiding conductor (11) is selected from Fe, Cr, Ni, Cu, Al, Co, Si or their alloys, and the resistivity is lower than that of the material of the integral honeycomb structure heater (9).
5. The electrically driven reactor according to claim 1, characterized in that, The pores (15) are circular channels, and the arrangement of the pores (15) is circular.
6. The electrically driven reactor according to claim 1, characterized in that, The catalyst support plate (8) abuts against the bottom of the integral honeycomb structure heater (9) and the insulation material (13), and the contact area between the catalyst support plate (8) and the bottom of the integral honeycomb structure heater (9) is provided with dense pores.
7. The electrically driven reactor according to claim 1, characterized in that, The insulation material (13) is selected from one or more combinations of glass wool, rock wool, aluminum silicate, and composite silicate.
8. The application of the electrically driven reactor based on the conductive heating integral honeycomb structure according to any one of claims 1 to 7, characterized in that, An endothermic reaction system for methane steam / dry gas reforming or methane combined / triple reforming.
Citation Information
Patent Citations
Cellular oxygen carrier chemical-looping reforming reactor
CN103204464A
Conductive ceramic honeycombs with resistive heating capability and methods of making the same
CN113301981A
Endothermic reactions heated by resistance heating
CN112203757A