A methane reforming and syngas conversion system and method

Abstract

The application provides a methane reforming and syngas conversion system and method, which comprises a light source device, a reaction device and a collection device; the reaction device comprises a gas inlet, a gas outlet, a first porous material layer, a methane reforming reaction chamber and a syngas conversion chamber; the first porous material layer is arranged between the methane reforming reaction chamber and the syngas conversion chamber; the methane reforming reaction chamber is located above the syngas conversion chamber; the syngas generated in the methane reforming reaction chamber enters the syngas conversion chamber for syngas conversion through the first porous material layer; the gas inlet is arranged on the methane reforming reaction chamber; and the gas outlet is arranged on the syngas conversion chamber; the light source device is located above the reaction device; and the collection device is connected with the gas outlet. The system provided by the application can realize the series connection of methane reforming and syngas conversion, and realize the preparation of high-value chemicals by taking methane, water and CO2 as raw materials.

Description

Technical Field

[0001] This application relates to the field of syngas conversion technology, and in particular to a methane reforming tandem syngas conversion system and method. Background Technology

[0002] The catalytic conversion of syngas (mainly including hydrogen and carbon monoxide) is a core scientific problem in industrial catalysis. Syngas is usually produced by the catalytic conversion of coal or oil and participates in downstream reactions as an important platform molecule. The key is to achieve the efficient conversion of C1 platform molecules into a variety of high-value-added compounds.

[0003] Methane reforming includes dry reforming (methane reacts with carbon dioxide) and wet reforming (methane reacts with water), as well as ternary reforming processes involving both carbon dioxide and water. Methane reforming is an important hydrogen production process in industrial catalysis, converting methane, carbon dioxide, and water into syngas. Syngas can then be further catalytically converted into various high-value-added chemicals. However, methane reforming typically requires high temperatures of 800°C to 1000°C, while syngas conversion requires relatively lower temperatures. Furthermore, the hydrogen-to-carbon monoxide ratio in the syngas produced by methane reforming often does not match the ratio required for syngas conversion. Therefore, it is difficult to connect the methane reforming and syngas conversion processes in the same reaction system. Summary of the Invention

[0004] The purpose of this application is to provide a methane reforming and syngas conversion system and method, so as to realize the methane reforming and syngas conversion processes in the same system to prepare high-value chemicals. The specific technical solution is as follows:

[0005] The first aspect of this application provides a methane reforming tandem syngas conversion system, comprising a light source device, a reaction device, and a collection device; the reaction device includes an inlet, an outlet, a first porous material layer, a methane reforming reaction chamber, and a syngas conversion chamber, wherein the first porous material layer is disposed between the methane reforming reaction chamber and the syngas conversion chamber, the methane reforming reaction chamber being located above the syngas conversion chamber, and the syngas generated in the methane reforming reaction chamber entering the syngas conversion chamber through the first porous material layer for syngas conversion; the inlet is disposed on the methane reforming reaction chamber, and the outlet is disposed on the syngas conversion chamber; the light source device is located above the reaction device, and the collection device is connected to the outlet.

[0006] In some embodiments of this application, the methane reforming reaction chamber includes a first catalyst bed and a first temperature control device. The temperature of the first catalyst bed is 800°C to 1000°C. The catalyst in the first catalyst bed is selected from at least one of catalyst-supported nickel catalyst, supported platinum catalyst, supported cobalt catalyst, and supported ruthenium catalyst. The first catalyst bed is located on the first porous material layer, and the gas inlet is located above the first catalyst bed. The first porous material layer is movable in the vertical direction.

[0007] In some embodiments of this application, the syngas conversion chamber includes a second catalyst bed, a second porous material layer, and a second temperature control device. The second catalyst bed is located on the second porous material layer, which is located above the gas outlet. The second porous material layer is movable in the vertical direction.

[0008] In some embodiments of this application, the syngas conversion chamber includes a catalyst liquid layer and a third temperature control device, the catalyst liquid layer being located at the bottom of the syngas conversion chamber, and the gas outlet being located on the side wall of the syngas conversion chamber and above the catalyst liquid layer.

[0009] In some embodiments of this application, the light source device includes at least one of xenon lamp, halogen lamp, LED light source and natural sunlight.

[0010] In some embodiments of this application, the reaction occurring in the syngas reforming chamber is Fischer-Tropsch synthesis, the temperature of the second catalyst bed is 200°C to 360°C, the catalyst of the second catalyst bed is selected from at least one of iron-based catalysts, cobalt-based catalysts and ruthenium-based catalysts, and the molar ratio of methane, CO2 and water introduced into the methane reforming reaction chamber is 2:1:1 to 1:1:0.5.

[0011] In some embodiments of this application, the reaction occurring in the syngas reforming chamber is methanol synthesis, the temperature of the second catalyst bed is 180°C to 300°C, the catalyst of the second catalyst bed is selected from at least one of copper-based catalysts, indium-based catalysts, zinc zirconium oxide-based catalysts, and zinc chromium oxide-based catalysts, and the molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber is 3:1:1 to 2:1:0.5.

[0012] In some embodiments of this application, the reaction occurring in the syngas reforming chamber is ethanol synthesis, the temperature of the second catalyst bed is 220°C to 350°C, and the catalyst in the second catalyst bed is selected from at least one of rhodium-based catalysts, molybdenum-based catalysts, iron-copper-based modified Fischer-Tropsch catalysts, cobalt-copper-based modified Fischer-Tropsch catalysts, and copper-based modified methanol synthesis catalysts. The molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber is 2:1:1 to 1:1:0.5.

[0013] In some embodiments of this application, the reaction occurring in the syngas reforming chamber is a hydroformylation reaction, the temperature of the catalyst liquid layer is 80°C to 120°C, the catalyst in the catalyst liquid layer is selected from at least one of rhodium-based catalysts and cobalt-based catalysts, and the molar ratio of methane, CO2 and water introduced into the methane reforming reaction chamber is 1:1:0.

[0014] The second aspect of this application provides a method for methane reforming tandem syngas conversion using the system provided in the first aspect of this application.

[0015] The beneficial effects of this application are:

[0016] This application provides a methane reforming tandem syngas conversion system and method. The system includes a light source, a reaction apparatus, and a collection apparatus. The reaction apparatus includes an inlet, an outlet, a first porous material layer, a methane reforming reaction chamber, and a syngas conversion chamber. The first porous material layer is disposed between the methane reforming reaction chamber and the syngas conversion chamber, with the methane reforming reaction chamber located above the syngas conversion chamber. Syngas generated in the methane reforming reaction chamber enters the syngas conversion chamber through the first porous material layer for syngas conversion. The inlet and outlet are both located on the methane reforming reaction chamber. The light source is located above the reaction apparatus, and the collection apparatus is connected to the outlet. On one hand, by designing two reaction chambers, utilizing the residual heat from methane reforming, and through thermal field analysis, the problem of temperature mismatch between methane reforming and syngas conversion is solved. On the other hand, based on the hydrogen-to-carbon molar ratio of the feedstocks required for syngas conversion (i.e., the molar ratio of H2 to CO), the proportions of methane, water, and CO2 introduced into the methane reforming reaction chamber were controlled. Furthermore, the temperature and catalyst type of the methane reforming reaction were adjusted to achieve a hydrogen-to-carbon molar ratio in methane reforming that matches that of syngas conversion. Ultimately, the tandem operation of methane reforming and syngas conversion was realized within the same system, enabling the production of high-value chemicals from methane, water, and CO2. This not only improves resource utilization but also reduces greenhouse gas emissions and optimizes resource storage and transportation methods. Attached Figure Description

[0017] To more clearly illustrate the technical solutions in the embodiments of this application, the accompanying drawings used in the description of the embodiments will be briefly introduced below. Obviously, the accompanying drawings described below are only some embodiments of this application. For those skilled in the art, other embodiments can be obtained based on these accompanying drawings.

[0018] Figure 1 This is a diagram of a reaction apparatus according to one embodiment of this application;

[0019] Figure 2 This is a diagram of a reaction apparatus according to another embodiment of this application.

[0020] In the figure, 1. Inlet, 2. Methane reforming reaction chamber, 3. First porous material layer, 4. Syngas conversion chamber, 5. Outlet, 21. First catalyst bed, 22. First temperature control device, 41. Second catalyst bed, 42. Second temperature control device, 43. Second porous material layer, 44. Catalyst liquid layer, 45. Third temperature control device. Detailed Implementation

[0021] The technical solutions of this application will be clearly and completely described below with reference to the embodiments and accompanying drawings. Obviously, the described embodiments are only some embodiments of this application, and not all embodiments. All other embodiments obtained by those skilled in the art based on this application are within the scope of protection of this application.

[0022] The current mainstream syngas conversion processes include Fischer-Tropsch synthesis, methanol synthesis, ethanol synthesis, and hydroformylation. The temperature mismatch between methane reforming and syngas conversion is a key issue limiting the coupling of these two processes. Syngas conversion occurs at relatively low temperatures, making it impossible to directly connect the two steps in the same reactor in traditional industrial processes and scientific research. Furthermore, methane reforming for hydrogen production is energy-intensive, requiring high energy injection and exhibiting low thermal efficiency. In addition to the temperature mismatch, there is also a mismatch between the hydrogen-to-carbon molar ratio in the methane reforming products and the hydrogen-to-carbon molar ratio required for syngas conversion. Complete dry reforming of methane yields a hydrogen-to-carbon molar ratio of 1:1, while complete wet reforming yields a ratio of 4:1. In syngas conversion, Fischer-Tropsch synthesis typically requires a hydrogen-to-carbon molar ratio of 1:1-3:1, methanol synthesis requires 2:1-3:1, ethanol synthesis requires 2:1-3:1, and hydroformylation typically requires a hydrogen-to-carbon molar ratio of 1:1. Therefore, the products obtained from dry or wet reforming of methane alone cannot be directly applied to all syngas conversion processes; the hydrogen-to-carbon molar ratio needs to be adjusted. Furthermore, methane reforming may be accompanied by side reactions such as water-gas shift, reverse water-gas shift, and carbon deposition, affecting the hydrogen-to-carbon molar ratio in the products and making the system more complex. Based on this, this application provides a methane reforming-syngas conversion system through thermal field analysis and feedstock balance, enabling the simultaneous implementation of methane reforming and syngas conversion processes within the same system for the preparation of high-value chemicals.

[0023] The first aspect of this application provides a methane reforming tandem syngas conversion system, which includes a light source device, a reaction device, and a collection device; the reaction device is as follows: Figure 1 and Figure 2 As shown, the apparatus includes an inlet 1, an outlet 5, a first porous material layer 3, a methane reforming reaction chamber 2, and a syngas conversion chamber 4. The first porous material layer 3 is disposed between the methane reforming reaction chamber 2 and the syngas conversion chamber 4. The methane reforming reaction chamber 2 is located above the syngas conversion chamber 4. The syngas generated in the methane reforming reaction chamber 2 enters the syngas conversion chamber 4 through the first porous material layer 3 for syngas conversion. The inlet 1 is disposed on the methane reforming reaction chamber 2, and the outlet 5 is disposed on the syngas conversion chamber 4. A light source device is located above the reaction apparatus, and a collection device is connected to the outlet 5.

[0024] Thermal field analysis allows for precise temperature distribution within the two reaction chambers. The hydrogen-to-carbon molar ratio of syngas produced from methane reforming is related to the proportions of methane, water, and CO2 in the feedstock and the specific reaction conditions. Thermodynamic calculations and fine-tuning of the feedstock ratios are used to determine the optimal ratio of methane, water, and CO2 to meet the hydrogen-to-carbon molar ratio requirements for syngas conversion. This thermal field analysis and feedstock balance not only enables precise control of the syngas conversion reaction temperature but also allows for the selection of appropriate temperature ranges and the proportions of methane, water, and CO2 based on the specific syngas conversion reaction and catalyst.

[0025] In some embodiments of this application, such as Figure 1 and Figure 2 As shown, the methane reforming reaction chamber 2 includes a first catalyst bed 21 and a first temperature control device 22. The temperature of the first catalyst bed 21 is 800℃~1000℃. The catalyst in the first catalyst bed 21 is selected from at least one of supported nickel catalysts, supported platinum catalysts, supported cobalt catalysts, and supported ruthenium catalysts. The first catalyst bed 21 is located on a first porous material layer 3, and the gas inlet 1 is located above the first catalyst bed 21. The first porous material layer 3 is movable in the vertical direction. For example, the temperature of the first catalyst bed 21 can be 800℃, 850℃, 880℃, 920℃, 960℃, 1000℃, or a range of any two of these values. The first temperature control device 22 is used to control the temperature of the first catalyst bed 21. The catalyst is used to catalyze the methane reforming reaction, which occurs in the first catalyst bed 21.

[0026] This application does not impose any particular restrictions on the type of support for the above-mentioned supported catalyst. For example, the type of support may include, but is not limited to, silicon dioxide, titanium dioxide, cerium dioxide, aluminum oxide, and zirconium dioxide.

[0027] In some embodiments of this application, such as Figure 1 As shown, the syngas conversion chamber 4 includes a second catalyst bed 41, a second porous material layer 43, and a second temperature control device 42. The second catalyst bed 41 is located on the second porous material layer 43, which is located above the gas outlet 5. The second porous material layer 43 is movable in the vertical direction. The second temperature control device 42 is used to control the temperature of the second catalyst bed 41, which is used to catalyze the syngas conversion, and the syngas conversion occurs in the second catalyst bed 41.

[0028] In some embodiments of this application, such as Figure 2 As shown, the syngas conversion chamber 4 includes a catalyst liquid layer 44 and a third temperature control device 45. The catalyst liquid layer 44 is located at the bottom of the syngas conversion chamber 4, and the gas outlet 5 is located on the side wall of the syngas conversion chamber 4 and above the catalyst liquid layer 44. The aforementioned third temperature control device 45 is used to control the temperature of the catalyst liquid layer 44, which is used to catalyze the syngas conversion, and the syngas conversion occurs in the catalyst liquid layer 44.

[0029] In this application, heterogeneous catalysts are used for Fischer-Tropsch synthesis, methanol synthesis, and ethanol synthesis, such as... Figure 1 The reaction apparatus shown in the diagram is used for the hydroformylation reaction, which employs a homogeneous catalyst, such as... Figure 2 The reaction apparatus shown in the diagram is used.

[0030] In this application, the first porous material layer 3 and the second porous material layer 43 are movable in the vertical direction. That is, the distance between the first catalyst bed 21 and the second catalyst bed 41 (the vertical distance from the bottom surface of the first catalyst bed 21 to the upper surface of the second catalyst bed 41) is adjustable, and adjusting this distance can affect the temperature of the second catalyst bed 41. Alternatively, the distance between the first catalyst bed 21 and the catalyst liquid layer 44 (the vertical distance from the bottom surface of the first catalyst bed 21 to the upper surface of the catalyst liquid layer 44) is adjustable, and adjusting this distance can affect the temperature of the catalyst liquid layer 44. This application does not particularly limit the material and pore size of the first porous material layer 3 and the second porous material layer 43, as long as the purpose of this application is achieved. For example, a porous SiC material with a pore size in the micrometer range can be used to support the catalyst bed while allowing gas to pass through.

[0031] This application does not impose any particular restrictions on the first temperature control device 22, the second temperature control device 42, and the third temperature control device 45, as long as they can achieve the purpose of this application. For example, they can be infrared cameras or thermocouples.

[0032] In some embodiments of this application, the light source device includes at least one of a xenon lamp, a halogen lamp, an LED light source, and natural sunlight. The aforementioned light source device can provide light energy for the methane reforming reaction, reducing the energy consumption of the reaction and improving the overall efficiency of producing high-value chemicals from methane through light energy injection. The light intensity emitted by the light source device is adjustable, and the intensity also affects the temperature of the second catalyst bed 41 or the catalyst liquid layer 44.

[0033] In some implementations, the light intensity is 5 W / cm². 2 ~50W / cm 2 .

[0034] In this application, based on the temperature of the first catalyst bed 21, the light intensity, and the required temperature for the second layer of syngas conversion, the distance from the first catalyst bed 21 to the second catalyst bed 41 or the distance from the first catalyst bed 21 to the catalyst liquid layer 44 can be determined through thermal field analysis, which is beneficial for accurately matching the temperature range of methane reforming and syngas conversion.

[0035] In some embodiments of this application, the reaction occurring in the syngas reforming chamber 4 is a Fischer-Tropsch synthesis, the temperature of the second catalyst bed 41 is 200°C to 360°C, and the catalyst in the second catalyst bed 41 is selected from at least one of iron-based catalysts, cobalt-based catalysts, and ruthenium-based catalysts. The molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber 2 is 2:1:1 to 1:1:0.5. For example, the temperature of the second catalyst bed 41 can be 200°C, 230°C, 280°C, 310°C, 360°C, or any combination of two of these values, and the molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber 2 can be 1:1:0.5, 1.5:1:0.5, 2:1:0.5, 1:1:1, 1.5:1:1, 2:1:1, or any combination of two of these values. By adjusting the temperature of the second catalyst bed 41, the type of catalyst in the second catalyst bed 41, and the molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber 2 within the aforementioned ranges, and simultaneously adjusting the temperature of the first catalyst bed 21 and the type of catalyst in the first catalyst bed 21 within the scope of this application, the molar ratio of H2 and CO generated by methane reforming can be matched with the hydrogen-carbon molar ratio required for Fischer-Tropsch synthesis, and Fischer-Tropsch synthesis can occur in the second catalyst bed 41.

[0036] In some embodiments of this application, the reaction occurring in the syngas reforming chamber 4 is methanol synthesis. The temperature of the second catalyst bed 41 is 180°C to 300°C. The catalyst in the second catalyst bed 41 is selected from at least one of copper-based catalysts, indium-based catalysts, zinc-zirconium oxide-based catalysts, and zinc-chromium oxide-based catalysts. The molar ratio of methane, CO2, and water introduced into the methane reforming chamber 2 is 3:1:1 to 2:1:0.5. For example, the temperature of the second catalyst bed 41 can be 180°C, 200°C, 240°C, 270°C, 300°C, or any combination of two of these values. The molar ratio of methane, CO2, and water introduced into the methane reforming chamber 2 can be 3:1:1, 2.5:1:1, 2:1:1, 3:1:0.5, 2.5:1:0.5, 2:1:0.5, or any combination of two of these values. By adjusting the temperature of the second catalyst bed 41, the type of catalyst in the second catalyst bed 41, and the molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber 2 within the aforementioned ranges, and simultaneously adjusting the temperature of the first catalyst bed 21 and the type of catalyst in the first catalyst bed 21 within the scope of this application, the molar ratio of H2 and CO generated by methane reforming can be matched with the hydrogen-carbon molar ratio required for methanol synthesis, and methanol synthesis can occur in the second catalyst bed 41.

[0037] In some embodiments of this application, the reaction occurring in the syngas reforming chamber 4 is ethanol synthesis, the temperature of the second catalyst bed 41 is 220°C to 350°C, and the catalyst in the second catalyst bed 41 is selected from at least one of rhodium-based catalysts, molybdenum-based catalysts, iron-copper-based modified Fischer-Tropsch catalysts, cobalt-copper-based modified Fischer-Tropsch catalysts, and copper-based modified methanol synthesis catalysts. The molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber 2 is 2:1:1 to 1:1:0.5. For example, the temperature of the second catalyst bed 41 can be 220°C, 250°C, 280°C, 310°C, 350°C, or any combination of two of these values, and the molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber 2 can be 2:1:1, 1.5:1:1, 1:1:1, 2:1:0.5, 1.5:1:0.5, 1:1:0.5, or any combination of two of these values. By adjusting the temperature of the second catalyst bed 41, the type of catalyst in the second catalyst bed 41, and the molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber 2 within the aforementioned ranges, and simultaneously adjusting the temperature of the first catalyst bed 21 and the type of catalyst in the first catalyst bed 21 within the scope of this application, the molar ratio of H2 and CO generated by methane reforming can be matched with the hydrogen-carbon molar ratio required for ethanol synthesis, and ethanol synthesis can occur in the second catalyst bed 41.

[0038] In some embodiments of this application, the reaction occurring in the syngas reforming chamber 4 is a hydroformylation reaction. The temperature of the catalyst liquid layer 44 is 80°C to 120°C, and the catalyst in the catalyst liquid layer 44 is selected from at least one of rhodium-based and cobalt-based catalysts. The molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber 2 is 1:1:0. For example, the temperature of the catalyst liquid layer 44 can be 80°C, 90°C, 100°C, 110°C, 120°C, or any combination of two of these values. By controlling the temperature of the catalyst liquid layer 44, the type of catalyst in the catalyst liquid layer 44, and the molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber 2 within the above ranges, and simultaneously controlling the temperature of the first catalyst bed 21 and the type of catalyst in the first catalyst bed 21 within the scope of this application, the molar ratio of H2 and CO generated by methane reforming can be matched with the hydrogen-carbon molar ratio required for the hydroformylation reaction, and the hydroformylation reaction occurs in the catalyst liquid layer 44.

[0039] In this application, the catalyst liquid layer 44 also includes liquid olefins. This application does not have any particular restrictions on the type of liquid olefins, as long as they can achieve the purpose of this application. For example, they can be pentene.

[0040] This application does not impose any particular restrictions on the source of the catalysts described above, as long as they can achieve the purpose of this application. Exemplarily, they can be obtained by purchase or prepared by methods known in the art, such as co-precipitation or impregnation.

[0041] In this application, the high-value chemicals obtained through Fischer-Tropsch synthesis, methanol synthesis, and ethanol synthesis are all processed... Figure 1 The gas exit 5 shown enters the collection device for collection, while the high-value chemicals obtained through the hydroformylation reaction remain in the catalyst liquid layer 44, and their gaseous products pass through... Figure 2 The air outlet 5 shown enters the collection device for collection.

[0042] This application does not specifically limit the collection device, as long as it can achieve the purpose of this application. For example, the collection device can be a cold trap and a hot trap. The temperature of the hot trap can be 170℃~180℃, used to receive high-carbon substances with high boiling points and prevent the device from clogging. The temperature of the cold trap can be -4℃~4℃, used to receive products with low boiling points, such as low-carbon hydrocarbons and low-carbon alcohols. The products collected by the hot trap and the cold trap can be analyzed offline by chromatography respectively; or the collection device can be a chromatograph, and high-value chemicals can be directly and fully insulated into the chromatograph for online analysis.

[0043] The second aspect of this application provides a method for methane reforming in series with syngas conversion using the system provided in the first aspect of this application. It includes the following steps: methane, CO2, and water in the required molar ratio are introduced into the methane reforming reaction chamber 2 through inlet 1; a light source is turned on, and the temperature of the first catalyst bed 21 is controlled at 800℃~1000℃ to carry out the methane reforming reaction via photothermal catalysis; the product enters the syngas conversion chamber 4 through the first porous material layer 3; the temperature of the second catalyst bed 41 or the catalyst liquid layer 44 is controlled, and a syngas conversion reaction occurs in the second catalyst bed 41 or the catalyst liquid layer 44; the product enters the collection device through outlet 5 for collection, completing the entire process of methane reforming in series with syngas conversion, and realizing the preparation of high-value chemicals.

[0044] Example

[0045] The embodiments and comparative examples provided below illustrate the implementation of this application in more detail. Various tests and evaluations were conducted according to the methods described below. Furthermore, unless otherwise specified, "parts" and "%" are quality standards.

[0046] Example 1

[0047] <Fischer-Tropsch Synthesis>

[0048] The methane reforming reaction chamber 2 (inner diameter 10 cm) was illuminated with a xenon lamp source at an intensity of 20 W / cm². 2Methane, CO2, and water are introduced into the methane reforming reaction chamber 2 in a molar ratio of 2:1:1. The water is pumped in via a plunger pump (not shown in the figure) and has been fully vaporized. The first temperature control device 22 is inserted into the first catalyst bed 21 with a thermocouple to control the temperature of the first catalyst bed 21 at 800°C. The catalyst in the first catalyst bed 21 is a supported nickel catalyst (Ni loading is 10wt%, and the support is commercial CeO2 solid powder). The methane reforming reaction occurs in the first catalyst bed 21 to obtain syngas with a hydrogen-to-carbon molar ratio of 2:1. The syngas enters the syngas conversion chamber 4 (with an inner diameter of 10 cm) through the first porous material layer 3. Through thermal field analysis, the distance between the second catalyst bed 41 and the first catalyst bed 21 is adjusted to 1.5 cm, and a thermocouple from the second temperature control device 42 is inserted into the second catalyst bed 41 to control its temperature at approximately 240 °C. The catalyst in the second catalyst bed 41 is a ruthenium-based catalyst. Fischer-Tropsch synthesis takes place in the second catalyst bed 41, and the product enters the collection device through the gas outlet 5. The temperature of the cold trap is controlled at approximately 0 °C, and the temperature of the hot trap at approximately 170 °C, and the product is collected. The product is analyzed by gas chromatography. The chromatographic analysis shows that the methane reforming tandem syngas conversion system of this application generates high-value olefins through methane reforming and Fischer-Tropsch synthesis.

[0049] Example 2

[0050] Methanol Synthesis

[0051] The methane reforming reaction chamber 2 (inner diameter 10 cm) was illuminated with a xenon lamp source at an intensity of 15 W / cm². 2 Methane, CO2, and water in a molar ratio of 2:1:0.5 are introduced into the methane reforming reaction chamber 2. The water is pumped in by a plunger pump and has been fully vaporized. The first temperature control device 22 is inserted into the first catalyst bed 21 with a thermocouple to control the temperature of the first catalyst bed 21 at 800°C. The catalyst in the first catalyst bed 21 is a supported platinum catalyst (Pt loading of 1 wt%, and the support is commercial CeO2 solid powder). The methane reforming reaction occurs in the first catalyst bed 21 to obtain syngas with a hydrogen-to-carbon molar ratio of 3:1. The syngas enters the syngas conversion chamber 4 (with an inner diameter of 10 cm) through the first porous material layer 3. Through thermal field analysis, the distance between the second catalyst bed 41 and the first catalyst bed 21 is adjusted to 2 cm. The second temperature control device 42 is inserted into the second catalyst bed 41 with a thermocouple, controlling the second catalyst bed 41 to approximately 220 °C. The catalyst in the second catalyst bed 41 is a copper-based catalyst. Methanol synthesis takes place in the second catalyst bed 41. The product is kept at a constant temperature and enters the gas chromatograph through the outlet 5 for analysis. The chromatographic analysis shows that the high-value chemical methanol is generated through methane reforming and methanol synthesis using the methane reforming tandem syngas conversion system of this application.

[0052] Example 3

[0053] <Ethanol Synthesis>

[0054] The methane reforming reaction chamber 2 (inner diameter 10 cm) was illuminated with a xenon lamp source at an intensity of 20 W / cm². 2 Methane, CO2, and water are introduced into the methane reforming reaction chamber 2 in a molar ratio of 2:1:1. The water is pumped in by a plunger pump and has been fully vaporized. The first temperature control device 22 is inserted into the first catalyst bed 21 with a thermocouple to control the temperature of the first catalyst bed 21 at 800°C. The first catalyst bed 21 is a supported nickel catalyst (Ni loading is 10wt%, and the support is commercial CeO2 solid powder). The methane reforming reaction occurs in the first catalyst bed 21 to obtain syngas with a hydrogen-to-carbon molar ratio of 2:1. The syngas enters the syngas conversion chamber 4 (inner diameter 10 cm) through the first porous material layer 3. Through thermal field analysis, the distance between the second catalyst bed 41 and the first catalyst bed 21 is adjusted to 1.2 cm. A thermocouple from the second temperature control device 42 is inserted into the second catalyst bed 41 to control its temperature at approximately 300°C. The catalyst in the second catalyst bed 41 is an iron-copper based modified Fischer-Tropsch catalyst (a FeCu bulk catalyst synthesized by co-precipitation, with a Cu to Fe molar ratio of approximately 4:1). Ethanol synthesis occurs in the second catalyst bed 41, and the product enters the collection device through the outlet 5. The temperature of the cold trap is controlled at approximately 0°C, and the temperature of the hot trap at approximately 170°C. The product is collected. Gas chromatography analysis of the product shows that the methane reforming tandem syngas conversion system of this application successfully produces the high-value chemical ethanol through methane reforming and ethanol synthesis.

[0055] Example 4

[0056] <Hyformylation reaction>

[0057] The methane reforming reaction chamber 2 (with an inner diameter of 10 cm) was illuminated with a xenon lamp source at an intensity of 10 W / cm². 2Methane, CO2, and water are introduced into the methane reforming reaction chamber 2 in a molar ratio of 1:1:0. The water is pumped in by a plunger pump and has been fully vaporized. The first temperature control device 22 is inserted into the first catalyst bed 21 with a thermocouple to control the temperature of the first catalyst bed 21 at 800°C. The catalyst in the first catalyst bed 21 is a supported platinum-based catalyst (Pt loading of 1 wt%, and the support is commercial CeO2 solid powder). The methane reforming reaction occurs in the first catalyst bed 21 to obtain syngas with a hydrogen-to-carbon molar ratio of 1:1. The syngas enters the syngas conversion chamber 4 (inner diameter 10 cm) through the first porous material layer 3. Through thermal field analysis, the distance between the catalyst liquid layer 44 and the first catalyst bed 21 is adjusted to 3.5 cm. A third temperature control device 45 (thermocouple) is inserted into the catalyst liquid layer 44 to control the temperature of the catalyst liquid layer 44 at approximately 100 °C. The catalyst liquid layer 44 includes a rhodium-based catalyst (Rh loading of 0.1 wt%, supported by commercial CeO2 solid powder) and pentene. A hydroformylation reaction occurs in the catalyst liquid layer 44, and the resulting high-value chemical aldehydes remain in the catalyst liquid layer 44. A sample from the catalyst liquid layer 44 is taken, an internal standard is added, and the sample is centrifuged. The supernatant is then analyzed by gas chromatography. The gaseous products are analyzed by gas chromatography through the outlet 5. The chromatographic analysis shows that the methane reforming tandem syngas conversion system of this application generates high-value chemicals such as hexanal through methane reforming and hydroformylation reactions.

[0058] The above description is only a preferred embodiment of this application and is not intended to limit this application. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of this application should be included within the scope of protection of this application.

Claims

1. A methane reforming tandem syngas conversion system, comprising a light source device, a reaction device, and a collection device; the reaction device includes an inlet, an outlet, a first porous material layer, a methane reforming reaction chamber, and a syngas conversion chamber, wherein the first porous material layer is disposed between the methane reforming reaction chamber and the syngas conversion chamber, the methane reforming reaction chamber is located above the syngas conversion chamber, and the syngas generated in the methane reforming reaction chamber enters the syngas conversion chamber through the first porous material layer for syngas conversion; the inlet is disposed on the methane reforming reaction chamber, and the outlet is disposed on the syngas conversion chamber; The light source device is located above the reaction device, and the collection device is connected to the gas outlet.

2. The system according to claim 1, wherein, The methane reforming reaction chamber includes a first catalyst bed and a first temperature control device. The temperature of the first catalyst bed is 800℃~1000℃. The catalyst in the first catalyst bed is selected from at least one of supported nickel catalyst, supported platinum catalyst, supported cobalt catalyst, and supported ruthenium catalyst. The first catalyst bed is located on the first porous material layer, and the gas inlet is located above the first catalyst bed. The first porous material layer is movable in the vertical direction.

3. The system according to claim 1, wherein, The syngas conversion chamber includes a second catalyst bed, a second porous material layer, and a second temperature control device. The second catalyst bed is located on the second porous material layer, which is located above the gas outlet. The second porous material layer is movable in the vertical direction.

4. The system according to claim 1, wherein, The syngas conversion chamber includes a catalyst liquid layer and a third temperature control device. The catalyst liquid layer is located at the bottom of the syngas conversion chamber, and the gas outlet is located on the side wall of the syngas conversion chamber and above the catalyst liquid layer.

5. The system according to claim 1, wherein, The light source device includes at least one of xenon lamp, halogen lamp, LED light source and natural sunlight.

6. The system according to claim 3, wherein, The reaction occurring in the syngas reforming chamber is Fischer-Tropsch synthesis. The temperature of the second catalyst bed is 200°C to 360°C. The catalyst in the second catalyst bed is selected from at least one of iron-based catalysts, cobalt-based catalysts, and ruthenium-based catalysts. The molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber is 2:1:1 to 1:1:0.

5.

7. The system according to claim 3, wherein, The reaction occurring in the syngas conversion chamber is methanol synthesis. The temperature of the second catalyst bed is 180℃~300℃. The catalyst in the second catalyst bed is selected from at least one of copper-based catalysts, indium-based catalysts, zinc zirconium oxide-based catalysts, and zinc chromium oxide-based catalysts. The molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber is 3:1:1 to 2:1:0.

5.

8. The system according to claim 3, wherein, The reaction occurring in the syngas reforming chamber is ethanol synthesis. The temperature of the second catalyst bed is 220℃~350℃. The catalyst in the second catalyst bed is selected from at least one of rhodium-based catalysts, molybdenum-based catalysts, iron-copper-based modified Fischer-Tropsch catalysts, cobalt-copper-based modified Fischer-Tropsch catalysts, and copper-based modified methanol synthesis catalysts. The molar ratio of methane, CO2, and water introduced into the methane reforming reaction chamber is 2:1:1 to 1:1:0.

5.

9. The system according to claim 4, wherein, The reaction occurring in the syngas reforming chamber is a hydroformylation reaction. The temperature of the catalyst liquid layer is 80℃~120℃. The catalyst in the catalyst liquid layer is selected from at least one of rhodium-based catalysts and cobalt-based catalysts. The molar ratio of methane, CO2 and water introduced into the methane reforming reaction chamber is 1:1:

0.

10. A method for methane reforming tandem syngas conversion using the system of any one of claims 1 to 9.

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