Conversion reactor for preparing synthesis gas through non-catalytic and catalytic coupling of hydrocarbon-containing gas and application of conversion reactor

Abstract

The invention relates to a multi-section reactor, and discloses a conversion reactor for preparing synthesis gas through non-catalytic and catalytic coupling of hydrocarbon-containing gas and application of the conversion reactor, an oxidation section is arranged at one end in a shell of the reactor, the oxidation section comprises a burner and a first raw material gas inlet connected to the burner, and the reactor further comprises a pre-catalytic section and a catalytic section; wherein the catalysis section is located in the shell, reaction gas heat of the oxidation section is used for supplying heat to the catalysis section, the pre-catalysis section is located in the shell or outside the shell, the pre-catalysis section comprises a pre-catalysis cavity filled with a catalyst, the pre-catalysis cavity is provided with a second raw material gas inlet and a pre-catalysis reaction gas outlet, and the second raw material gas inlet is communicated with the pre-catalysis reaction gas outlet. The catalytic section comprises a catalytic reaction chamber filled with a catalyst, all pre-catalytic reaction gas is introduced into the catalytic reaction chamber, the catalytic reaction chamber is provided with a synthesis gas outlet, and the synthesis gas heat of the catalytic section is used for supplying heat to the pre-catalytic section. The equipment occupied area and carbon emission can be reduced, the overall heat efficiency is high, and hydrogen and carbon components of product gas can be flexibly adjusted.

Description

Technical Field

[0001] This invention relates to the fields of energy chemical engineering and catalytic reaction engineering, and in particular to a multi-stage reactor. Background Technology

[0002] Hydrocarbon gases such as natural gas, coke oven gas, raw coal gas, LPG (Liquefied Petroleum Gas), and SNG (Substitute Natural Gas) are clean fossil fuels primarily composed of methane and are among the most economical raw materials for syngas production. Syngas, a key feedstock in chemical processes such as methanol, ammonia synthesis, and Fischer-Tropsch synthesis, consists of hydrogen (H2) and carbon monoxide (CO). Generally, natural gas can be used to produce syngas through processes such as partial oxidation (POX), steam reforming (SMR), and autothermal reforming (ATR). Taking methanol syngas as an example, the main technical routes for producing methanol syngas from natural gas include non-catalytic conversion and catalytic conversion. Furthermore, the methanol syngas produced must meet the hydrogen-to-carbon ratio requirement, i.e., (H2-CO2) / (CO+CO2) = 2.05.

[0003] Currently, conventional natural gas-to-methanol synthesis utilizes two technical routes: a non-catalytic conversion route and a natural gas SMR steam reformer followed by an ATR autothermal conversion route. These routes each employ a non-catalytic reactor, an SMR reactor, and an ATR reactor, each equipped with a preheating furnace. The non-catalytic reactor is hollow, lacking catalysts, heat exchangers, distributors, and other internal components; the SMR and ATR reactors must be loaded with catalysts and require a pre-combustion heater.

[0004] As a common non-catalytic conversion process, POX mainly converts natural gas into methanol syngas (H2+CO) through incomplete combustion. However, the methanol syngas produced by this method has a low hydrogen-to-carbon ratio, requiring the introduction of shift and decarbonization units to adjust the hydrogen-to-carbon ratio to meet the conditions for methanol production. In contrast, methanol syngas produced via catalytic conversion has a higher hydrogen-to-carbon ratio, and researchers are currently combining SMR and ATR to optimize the process. However, while optimizing the methanol syngas ratio, this method also introduces some new technical problems: firstly, the catalytic reaction requires a large amount of additional steam, and the large catalyst loading leads to high energy consumption in methanol synthesis and distillation; secondly, the high carbon dioxide content in the produced methanol syngas reduces methanol synthesis efficiency; and thirdly, the SMR process involves external heating through the combustion of natural gas, which produces carbon dioxide and nitrogen oxides (NOx). X The emissions of these substances contribute to the greenhouse effect and harm the ecological environment.

[0005] Chinese patent CN106431834A discloses a combined conversion method for methanol production, achieving large-scale methanol production through a single-line process integrating a gas heating converter (GHR), a steam methane converter (SMR), and a partial oxidation converter (POX). The method involves splitting the feedstock into a first feed stream and a second feed stream. The first feed stream is mixed with steam and fed into the GHR and SMR operating in series. The second feed stream is mixed with converted gas from the SMR and fed into the POX along with oxygen. However, this method uses a 45:55 volume ratio of the first feed stream used for catalytic conversion to the second feed stream used for non-catalytic conversion, which does not significantly reduce the catalytic reaction and its steam consumption. Furthermore, the non-catalytic conversion effluent is only used for heat exchange, without steam recovery. Additionally, the SMR uses fuel gas for heating, resulting in fuel gas emissions that require desulfurization.

[0006] In summary, current syngas production technologies still suffer from drawbacks such as high consumption of materials like steam and catalysts. Furthermore, the greenhouse gases and harmful gases emitted during production also pose environmental risks. Therefore, there is an urgent need to develop a syngas production device suitable for a new syngas production technology.

[0007] On August 24, 2025, the applicant filed two patent applications with the China National Intellectual Property Administration: CN202511186428.4, entitled "A non-catalytic, catalytic coupled syngas production apparatus and its use in producing syngas", and CN202511186427.X, entitled "A non-catalytic, catalytic coupled syngas production process containing hydrocarbon feed gas". For the purpose of implementing new technical routes, the syngas production process not explicitly described in this invention can be referred to the descriptions in the above application documents. Summary of the Invention

[0008] The technical problem to be solved by the present invention is to provide a non-catalytic and catalytic coupled syngas conversion reactor containing hydrocarbon gas. By improving the composition of the device, the non-catalytic conversion reaction and the catalytic conversion reaction are highly coupled, so that the reaction energy in the process of preparing syngas from hydrocarbon gas is optimized and the entire reaction device is free of carbon dioxide and NOx emissions.

[0009] The technical solution adopted by this invention to solve its technical problem is: a non-catalytic and catalytic coupled syngas conversion reactor containing hydrocarbon gas, the reactor including a shell, an oxidation section provided at one end of the shell, the oxidation section including a burner and a first feed gas inlet connected to the burner, the reactor also including a pre-catalytic section and a catalytic section, wherein the catalytic section is located inside the shell, the heat of the reaction gas in the oxidation section is used to heat the catalytic section, the pre-catalytic section is located inside or outside the shell, the pre-catalytic section includes a pre-catalytic chamber containing a catalyst, the pre-catalytic chamber is provided with a second feed gas inlet and a pre-catalytic reaction gas outlet, the catalytic section includes a catalytic reaction chamber containing a catalyst, all the pre-catalytic reaction gas is introduced into the catalytic reaction chamber, the catalytic reaction chamber is provided with a syngas outlet, the heat of the syngas in the catalytic section is used to heat the pre-catalytic section.

[0010] In the aforementioned conversion reactor, at least the oxidation section and the catalytic section are integrated into the same shell, which can be arranged vertically to save equipment floor space. The heat generated by the oxidation reaction in the oxidation section supplies the catalytic section, maintaining the high-temperature environment required by the catalytic section. The heat from the syngas at the catalytic section outlet can be used to heat the pre-catalytic section, thus fully utilizing the syngas heat. The oxidation reaction products and the uncatalyzed portion in the pre-catalytic section continue to react in the catalytic section, achieving a very high syngas conversion rate. By adjusting the composition and flow rate of the feed gas at the first and second feed gas inlets, the material temperature in each reaction section is adjusted, ensuring that each reaction section is in a stable state. This keeps the catalyst operating temperature relatively constant, preventing pulverization and deactivation, which is beneficial for reaction control and significantly extends the catalyst's lifespan. The gas flow rate, temperature, and composition in the unit can be maintained at a relatively constant state, which is beneficial for stable production in downstream units. In the later stages of the catalyst's lifespan, the reaction temperature can be appropriately increased by increasing the input of the first feed gas to maintain a high conversion rate.

[0011] To achieve optimal flow of raw materials and dynamic heat balance within the reactor, the shell contains, sequentially arranged, an oxidation section, a pre-catalytic section, and a catalytic section. Both the pre-catalytic section and the catalytic section are shell-and-tube heat exchange structures with catalysts arranged in the tubes. A second raw material gas inlet is located in the tube sheet cavity of the pre-catalytic section near the oxidation section. The outlet of the tube sheet cavity of the catalytic section away from the oxidation section serves as the syngas outlet and is connected to the shell side of the pre-catalytic section. The shell-side outlet of the pre-catalytic section also serves as the syngas outlet. The outlet gas from the oxidation section enters the shell side of the catalytic section through a long central tube, and the shell-side outlet of the catalytic section serves as the tail gas outlet. The outlet gas from the oxidation section does not enter the catalyst bed; it is only used to provide heat to the catalytic section, preventing the carbon black and other dust that may be generated in the oxidation section from affecting the catalyst bed.

[0012] Furthermore, a heat exchange section can be arranged between the pre-catalytic section and the catalytic section to regulate the temperature of the pre-catalytic section. The oxidation section, pre-catalytic section, heat exchange section and catalytic section are arranged sequentially from one end to the other in the shell. The pre-catalytic section, catalytic section and heat exchange section are all set as shell-and-tube heat exchange structures, and the catalyst is arranged on the tube side of the pre-catalytic section and the catalytic section. A second feed gas inlet is provided in the tube sheet cavity near the oxidation section end of the pre-catalytic section. The tube side outlet of the catalytic section is connected to the shell side of the heat exchange section, and the shell side of the heat exchange section is connected to the shell side of the pre-catalytic section. The shell side outlet of the pre-catalytic section serves as the product gas outlet. The outlet gas of the oxidation section enters the shell side of the catalytic section through the long central tube, and the shell side outlet of the catalytic section serves as the tail gas outlet.

[0013] Depending on the type of feed gas, when using a feed gas that is less likely to produce carbon black, the catalytic section can be located in the middle of the shell. Both the pre-catalytic section and the catalytic section are located inside the shell. One end of the catalytic section has a forced mixing section located near the oxidation section and connecting the oxidation section and the catalytic reaction chamber. The pre-catalytic section is located at the other end of the catalytic section inside the shell. A second feed gas inlet is connected to the pre-catalytic chamber via an inlet pipe located outside the shell. A short central pipe in the pre-catalytic chamber connects to the oxidation section. The second feed gas enters the pre-catalytic chamber through the inlet pipe, undergoes partial catalysis, and then enters the oxidation section through the short central pipe. The outlet gas of the pre-catalytic section and the outlet gas of the oxidation section can be forcibly mixed before entering the catalyst bed to complete the conversion of the feed gas, thereby achieving a high conversion rate.

[0014] To fully utilize the heat from the syngas produced by the catalytic reaction, the pre-catalytic section should ideally be configured with a shell-and-tube heat exchange structure. The catalyst should be located within the tubes, and the shell-side inlet of the pre-catalytic section should be connected to the catalytic reaction chamber of the catalytic section. The shell-side outlet of the pre-catalytic section should serve as the product gas outlet of the reactor. The heat generated by the catalytic reaction should be used for the pre-catalytic reaction.

[0015] Similarly, part of the shell-and-tube heat exchange structure can be used as a heat exchange section to further absorb the heat from the syngas that was not used in the pre-catalytic section.

[0016] To design a reasonable material flow path, the first raw material gas inlet and the second raw material gas inlet are respectively located at both ends of the shell, and the product gas outlet is located on the side of the shell near the second raw material gas inlet, so that the synthesis gas and the second raw material gas can exchange heat fully and improve the conversion rate of the pre-catalytic section.

[0017] To allow the gas in the pre-catalytic section to disperse into the oxidation section for partial mixing, one end of the short central tube located in the oxidation section is configured as an open pipe section with a top plate. The top plate has a heat insulation layer made of castable material. The sidewall of the open pipe section and / or the top plate have through holes, which are straight holes or oblique holes.

[0018] Since the feed gas entering the catalytic section contains components from both the oxidation section and the pre-catalytic section, the conversion efficiency of the catalytic section can be improved if the two components can be fully mixed in a small space. Therefore, the forced mixing section includes upper and lower sieve plates, with a gas dispersion component filling the space between the two sieve plates. The gas dispersion component extends the gas path before the mixed gas enters the catalytic reaction chamber, allowing the two components to be fully mixed.

[0019] The gas dispersion component is a ceramic ball, which has good high temperature resistance and requires no maintenance.

[0020] Alternatively, the precatalytic section can be placed outside the shell to reduce the height of the main body of the conversion reactor in some cases.

[0021] Therefore, the present invention provides a hydrocarbon gas non-catalytic and catalytic coupled syngas conversion reactor that integrates only an oxidation section and a catalytic section within the reactor. The reactor includes a shell, an oxidation section is provided at one end of the shell, the oxidation section includes a burner and a first feed gas inlet connected to the burner, and a catalytic section is provided at the other end of the shell. The catalytic section includes a catalytic reaction chamber containing a catalyst, and a forced mixing section is provided in the catalytic section adjacent to the oxidation section and connecting the oxidation section and the catalytic reaction chamber. The heat from the reaction gas in the oxidation section is used to heat the catalytic section. The catalytic reaction chamber is provided with a syngas outlet located on the shell, and a shell inlet connected to the oxidation section is provided on the shell.

[0022] The precatalytic section or precatalyst, which is used in conjunction with this type of reactor, is located outside the shell. The precatalytic section includes a precatalytic chamber in which a catalyst is placed. The precatalytic chamber is provided with a second raw material gas inlet and a precatalytic reaction gas outlet. The precatalytic reaction gas is completely introduced into the catalytic reaction chamber through the shell inlet.

[0023] The precatalytic section has a shell-and-tube heat exchange structure, with the catalyst located inside the tubes. The tube inlet of the precatalytic section is used as the second feed gas inlet, and the tube outlet of the precatalytic section is connected to the shell inlet as the precatalytic reaction gas outlet, allowing the precatalytic reaction gas to enter the forced mixing section. The shell inlet of the precatalytic section is connected to the synthesis gas outlet of the catalytic reaction chamber, and the shell outlet of the precatalytic section is used as the product gas outlet of the reactor.

[0024] The housing air inlet can be located at the other end of the housing away from the oxidation section. The housing air inlet is connected to the oxidation section through a central air inlet pipe. The synthesis gas outlet is located on the side of the housing near the housing air inlet.

[0025] Similarly, one end of the central air intake pipe located within the oxidation section can be configured as an open pipe section with a top plate. The top plate has a heat insulation layer made of castable refractory. The sidewall of the open pipe section and / or the top plate have through holes, which are straight holes or oblique holes.

[0026] In this case, the precatalytic section can be directly connected to the shell, or connected to the shell through a pipeline. The shell inlet can also be a side inlet located near the junction of the oxidation section and the forced mixing section. The syngas outlet of the reaction chamber of the catalytic section can be located at the end of the shell, or on the side of the shell at the end relatively away from the forced mixing section.

[0027] In the above case, a gas mixer with a spiral structure is arranged between the forced mixing section and the side air inlet. The top of the gas mixer has a heat insulation layer made of castable material, and the incoming air can enter from the top or from the side tangentially.

[0028] The shell is divided into at least two sections, which are connected by flanges.

[0029] The shell includes an outer steel plate and a fire-resistant layer and a water-cooled wall disposed on the inner side of the steel plate.

[0030] The present invention also provides the use of any of the above-mentioned hydrocarbon-containing non-catalytic or catalytic coupled syngas conversion reactors for the preparation of syngas.

[0031] This invention has the following characteristics: 1. The heat required for the conversion reaction in this invention is supplied by the oxidation section, eliminating the need for a combustion furnace, thereby significantly reducing investment and floor space requirements; 2. Because this invention eliminates the combustion heating furnace in the system, the device emits no carbon dioxide or NOx, making it more environmentally friendly and in line with national industrial policies; 3. This invention can flexibly adjust the hydrogen and carbon composition of the product gas to meet the production needs of different downstream products and reduce the production load and investment of downstream conversion and decarbonization processes. 4. The steam produced as a byproduct of the oxidation section reaction in this invention can be directly used as a raw material to enter the catalytic section to participate in the reaction, resulting in lower steam consumption compared to other conversion processes. 5. This invention can utilize the waste heat of the product gas to preheat the raw material gas, resulting in an overall thermal efficiency higher than other conversion processes. 6. In this invention, most of the raw gas passes through the oxidation section first, and carbon precipitation will not occur at high temperatures, thereby extending the service life of the catalyst; 7. The raw material gas used in this invention is a hydrocarbon-containing gas, including natural gas, SNG, LPG, coke oven tail gas, raw coal gas and other gases containing hydrocarbons. If the burner structure is changed, some liquid hydrocarbons can also be mixed in.

[0032] In summary, the beneficial effects of this invention are: diverse sources of raw material gas, high overall thermal efficiency, flexible adjustment of the hydrogen and carbon composition of the product gas, easy matching with subsequent processes, reduced equipment investment in subsequent processes, and long catalyst life. Attached Figure Description

[0033] Figure 1 This is a schematic diagram of the structure of Example 1 of the hydrocarbon gas non-catalytic and catalytic coupling synthesis gas conversion reactor of the present invention.

[0034] Figure 2 This is a schematic diagram of Example 2 of the hydrocarbon gas non-catalytic and catalytic coupled synthesis gas conversion reactor of the present invention.

[0035] Figure 3 This is a schematic diagram of Example 3 of the hydrocarbon gas non-catalytic and catalytic coupled synthesis gas conversion reactor of the present invention.

[0036] Figure 4 This is a schematic diagram of Example 4 of the hydrocarbon gas non-catalytic and catalytic coupled synthesis gas conversion reactor of the present invention.

[0037] Figure 5 This is a schematic diagram of Example 5 of the hydrocarbon gas non-catalytic and catalytic coupled synthesis gas conversion reactor of the present invention.

[0038] Figure 6 yes Figure 5 The diagram shown is a schematic of a hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor connected to a pre-catalytic section and a heat exchange section via pipelines.

[0039] Figure 7 yes Figure 5 The diagram shows another application state of the hydrocarbon-containing gas non-catalytic and catalytic coupled synthesis gas conversion reactor.

[0040] Figure 8 This is a schematic diagram of Example 6 of the syngas conversion reactor containing hydrocarbon gas through non-catalytic and catalytic coupling.

[0041] Figure 9 and Figure 10 yes Figure 8 The diagram shows the connection status of the hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor in application.

[0042] Figure 11 This is a schematic diagram of Example 7 of the hydrocarbon gas non-catalytic and catalytic coupled synthesis gas conversion reactor of the present invention.

[0043] Figure 12 and Figure 13 yes Figure 11 The diagram shows the connection status of the hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor in application.

[0044] Figure 14 This is a schematic diagram of a heat insulation layer installed on the top plate of the gas mixer in this invention.

[0045] Figure 15 This is a schematic diagram of the perforated pipe section structure provided at the pipe end in this invention.

[0046] The diagram is labeled as follows: 1-Oxidation section, 2-Pre-catalytic section, 3-Catalytic section, 4-Heat exchange section, 5-Perforated pipe section, 6-Gas mixer, 7-Long central pipe, 8-Catalyst, 9-Gas dispersion component, 10-Refractory layer, 11-Outer wall, 12-Burn, 13-First feed gas inlet, 14-Second feed gas inlet, 15-Synthesis gas outlet, 16-Connecting flange, 17-Short central pipe, 18-Inlet pipe, 19-Baffle plate, 20-Thermal insulation layer, 21-Pre-catalytic reaction gas outlet, 22-Tail gas outlet, 23-Shell inlet, 24-Side inlet, 25-Product gas outlet, 26-Gas distributor, 27-Central inlet pipe, 30-Forced mixing section, 50-Top plate, 51-Through hole, 90-Sieve plate. Detailed Implementation

[0047] The present invention will be further described below with reference to the accompanying drawings and embodiments.

[0048] like Figures 1 to 13 As shown, the present invention discloses a non-catalytic and catalytic coupled syngas conversion reactor for hydrocarbon-containing gas. The reactor includes a shell, with an oxidation section 1 located at one end of the shell. The oxidation section 1 includes a burner 12 and a first feed gas inlet 13 connected to the burner 12. A portion of the hydrocarbon-containing feed gas introduced into the oxidation section through the first feed gas inlet 13 undergoes an oxidation reaction through the burner 12, generating a mixed gas composed of H2, CO, CO2, and water vapor. The reactor also includes a pre-catalytic section 2 and a catalytic section 3, wherein at least the catalytic section 3 is located within the shell, and the pre-catalytic section 2 may be located within or outside the shell. The pre-catalytic section 2 includes a pre-catalytic chamber containing a catalyst 8, and the pre-catalytic chamber is provided with a second feed gas inlet 14 and a pre-catalytic converter. Catalytic reaction gas outlet 21. The reactions in the pre-catalytic chamber include conversion and shift reactions, producing gases including H2, CO, CO2, CH4, and water vapor. The catalytic section 3 includes a catalytic reaction chamber containing catalyst 8. All pre-catalytic reaction gas is introduced into the catalytic reaction chamber. The reactions in the catalytic reaction chamber include conversion and shift reactions. The catalytic reaction chamber is equipped with a syngas outlet 15. The main components of the mixed gas released from the syngas outlet 15 are H2, CO, and water vapor, and it also contains CH4, CO2, N2, etc. A small amount of oxidation reaction releases a large amount of heat. The heat from the reaction gas in the oxidation section 1 is used to heat the catalytic section 3, and the heat from the syngas in the catalytic section 3 can be used to heat the pre-catalytic section 2. Compared with conventional syngas reaction systems, this process can effectively reduce oxygen and electricity consumption.

[0049] like Figure 1As shown, to facilitate the manufacturing and installation of the shell, the shell can be divided into at least two sections, which are connected by a connecting flange 16. To extend the service life of the shell, a refractory layer 10 and a water-cooled wall (not shown in the figure) are provided on the inner side of the shell. The refractory layer 10 protects the metal outer wall 11 of the shell. The water-cooled wall can be divided into oxidation section, catalytic section, and pre-catalytic section, which can provide heat insulation and protect the metal outer wall of the equipment, and has a certain temperature regulation capability, which is beneficial for controlling the reaction process.

[0050] Example 1: like Figure 1 As shown, a non-catalytic and catalytic coupled syngas conversion reactor containing hydrocarbon gas is disclosed. The reactor includes a vertically arranged shell. An oxidation section 1, a pre-catalytic section 2, and a catalytic section 3 are sequentially arranged from one end to the other within the shell. The oxidation section 1 includes a burner 12 and a first feed gas inlet 13 connected to the burner 12. Both the pre-catalytic section 2 and the catalytic section 3 are configured as shell-and-tube heat exchange structures. A second feed gas inlet 14 is provided in the tube sheet cavity of the pre-catalytic section 2 near the oxidation section 1. Catalyst 8 is arranged along the tube side of the pre-catalytic section 2 as a pre-catalytic chamber. The feed gas entering through the second feed gas inlet 14 enters the pre-catalytic chamber through a gas distributor 5. Catalyst 8 is arranged along the tube side of the catalytic section 3 as a catalytic converter. In the catalytic reaction chamber, the outlet gas of oxidation section 1 enters the shell side of catalytic section 3 through the long central tube 7. The heat from the reaction gas in oxidation section 1 is used to heat catalytic section 3. After heating, the gas is discharged through the shell side outlet of catalytic section 3, i.e., the tail gas outlet 22 shown in the figure. The tube sheet outlet at the end of the catalytic reaction chamber away from oxidation section 1 serves as the synthesis gas outlet 15 and is connected to the shell side of precatalytic section 2. The shell sides of precatalytic section 2 and catalytic section 3 are separated by a partition 19. The heat from the synthesis gas in catalytic section 3 is used to heat precatalytic section 2. The precatalytic reaction gas outlet 21 of the precatalytic chamber is connected to the catalytic reaction chamber. All the precatalytic reaction gas is introduced into the catalytic reaction chamber. The shell side outlet of precatalytic section 2 serves as the product gas outlet 25.

[0051] When using the hydrocarbon-containing non-catalytic and catalytic coupled syngas conversion reactor of this embodiment, oxygen, a portion of the feed gas, and water vapor enter the oxidation section 1 from the top inlet. The outlet gas temperature of the oxidation section 1 is 1100℃~1400℃. Another portion of the feed gas and water vapor sequentially enter the pre-catalytic section 2 and catalytic section 3 from the top for feed gas conversion reaction. The pre-catalytic section 2 and catalytic section 3 can be designed as one or more sections, separated by shell-side partitions. The methane content of the outlet product gas can be controlled to ≤1.0% by volume. The outlet gas of the oxidation section 1 provides heat to the catalytic section 3 through the long central pipe 7 and then exits from the tail gas outlet 22 on the side of the equipment. The outlet gas of the catalytic section 3 returns to the shell side of the pre-catalytic section 2 to supply the heat required by the pre-catalytic section. Because the outlet gas of the oxidation section does not enter the catalyst bed, the carbon black and other dust that may be generated in the oxidation section are prevented from affecting the catalyst bed.

[0052] In addition, a steam inlet can be installed in the pre-catalytic chamber of the pre-catalytic section according to process requirements.

[0053] Example 2: like Figure 2 As shown, based on Example 1, a heat exchange section 4 is added. The heat exchange section 4 is arranged between the catalytic section and the pre-catalytic section 2. The shell side of the heat exchange section 4 is connected to the shell side of the pre-catalytic section, but the catalyst 8 is not arranged in the tube side of the heat exchange section 4. The catalyst 8 is only arranged in the tube side of the pre-catalytic section 2.

[0054] Example 3: like Figure 3 As shown, a non-catalytic and catalytic coupled syngas conversion reactor containing hydrocarbon gas is disclosed. The reactor includes a vertically arranged shell. From top to bottom, an oxidation section 1, a catalytic section 3, and a pre-catalytic section 2 are sequentially arranged within the shell. The oxidation section 1 includes a burner 12 located at one end of the shell and a first feed gas inlet 13 connected to the burner 12. The pre-catalytic section 2 is located at the other end of the shell and includes a pre-catalytic chamber containing a catalyst 8. A second feed gas inlet 14 located at the other end of the shell is connected to the pre-catalytic chamber by an inlet pipe 18 located outside the shell. The pre-catalytic chamber is connected to the oxidation section 1 by a short central pipe 17. The end of the short central pipe 17 within the oxidation section 1 is an open pipe section 5 with a top plate 50. The top plate 50 has a heat insulation layer 20 made of castable refractory material. Through holes, which can be straight or oblique, are formed on the sidewalls of the open pipe section 5 and / or on the top plate 50. The catalytic section 3 is located in the middle of the shell and includes a catalytic reaction chamber containing a catalyst 8. A forced mixing section 30 is provided at one end of the catalytic section 3 near the oxidation section 1. The forced mixing section 30 connects the oxidation section 1 and the catalytic reaction chamber. The forced mixing section 30 includes upper and lower sieve plates 90. The top of the sieve plate 90 near the oxidation section 1 has a heat insulation layer 20 made of castable material. Ceramic balls 9 are filled between the two sieve plates 90 as gas dispersants. The heat from the reaction gas in the oxidation section 1 is used to heat the catalytic section 3. The outlet gas of the pre-catalytic chamber is introduced into the oxidation section 1 through a short central pipe 17 and a gas distributor 5. After being forcibly mixed with the outlet gas of the oxidation section 1 in the forced mixing section 30, the gas enters the catalytic reaction chamber of the catalytic section 3. The catalytic reaction chamber is provided with a synthesis gas outlet 15. The heat from the synthesis gas in the catalytic section 3 is used to heat the pre-catalytic section 2 and then discharged through the product gas outlet 25 provided on the shell.

[0055] Example 4: like Figure 4 As shown, similar to Example 3, except that the burner structure is installed at the bottom and the second raw material gas inlet is installed at the top.

[0056] Example 5: like Figures 5-7As shown, a non-catalytic and catalytic coupled syngas conversion reactor containing hydrocarbon gas is disclosed. The reactor includes a vertically arranged shell, with an oxidation section 1 and a catalytic section 3 arranged vertically within the shell. The upper part of the shell is the oxidation section 1, which includes a burner 12 and a first feed gas inlet 13 connected to the burner 12. The catalytic section 3 is provided with a forced mixing section 30 located near the oxidation section 1 and connecting the oxidation section 1 and the catalytic section 3. The syngas outlet 15 of the catalytic reaction chamber is located on the side of the shell. A pre-catalytic section 2 and a heat exchange section 4 are located outside the shell and have an integrated shell-and-tube heat exchange structure. The tube side of the pre-catalytic section 2 contains a catalyst 8 as a pre-catalytic chamber, while the tube side of the heat exchange section 4 does not contain a catalyst 8. The tube side inlet is used as a second feed gas inlet 14. A central inlet pipe 27 is provided inside the shell. The tube-side outlets of the oxidation section 1 and the pre-catalytic section 2 are connected. The pre-catalytic reaction gas outlet 21 is connected to the inlet of the central inlet pipe 27. The end of the central inlet pipe 27 located within the oxidation section 1 is an open pipe section 5 with a top plate 50. It has openings on its sides and / or top, which can be straight or oblique holes. The top plate of the gas distributor 5 preferably also has a heat-insulating layer 20 made of castable refractory. After the pre-catalytic reaction gas enters the oxidation section 1, it is thoroughly mixed with the oxidation section products through the forced mixing section 30, and then all of it is introduced into the catalytic reaction chamber for further catalysis. The shell-side inlet of the pre-catalytic section 2 is connected to the synthesis gas outlet 15 of the catalytic reaction chamber. The heat from the synthesis gas in the catalytic section 3 is used to heat the pre-catalytic section 2 and the heat exchange section 4. The shell-side outlet of the shell-and-tube heat exchange structure serves as the product gas outlet 25 of the reactor. The heat from the reaction gas in the oxidation section 1 is used to heat the catalytic section 3. The inlet of the central inlet pipe 27 and the burner 12 are respectively arranged at both ends of the shell.

[0057] like Figure 6 , 7 As shown, the precatalytic section can be directly fixed to the shell, or it can be connected through a pipe.

[0058] Example 6: like Figures 8-10As shown, a non-catalytic and catalytic coupled syngas conversion reactor containing hydrocarbon gas is disclosed. The reactor includes a vertically arranged shell, with an oxidation section 1 and a catalytic section 3 respectively located at both ends of the shell. The catalytic section 3 includes a catalytic reaction chamber containing a catalyst 8. The oxidation section 1 includes a burner 12 and a first feed gas inlet 13 connected to the burner 12. The heat from the reaction gas in the oxidation section 1 is used to heat the catalytic section 3. The catalytic section 3 is provided with a forced mixing section 30 located near the oxidation section 1 and connecting the oxidation section 1 and the catalytic section 3. The syngas outlet 15 of the catalytic reaction chamber is located at the other end of the shell away from the oxidation section 1. The shell is provided with a shell inlet 23 connected to the oxidation section 1. The shell inlet 23 is a side inlet 24 located near the junction of the oxidation section 1 and the forced mixing section 30. The syngas outlet 15 is located outside the shell, with a pre-catalytic section 2 and a heat exchange section 4 located outside the shell. The pre-catalytic section 2 and the heat exchange section 4 have an integrated shell-and-tube heat exchange structure. The tube side of the heat exchange section 4 has no catalyst, while the tube side of the pre-catalytic section 2 has no catalyst. The process involves placing a catalyst 8 into a pre-catalytic chamber. The tube-side inlet serves as the second feed gas inlet 14, and the tube-side outlet is the pre-catalytic reaction gas outlet 21 of the pre-catalytic section 2, connected to the side inlet 24, which serves as the shell inlet 23. A gas mixer 6 with a spiral structure is installed between the side inlet 24 and the forced mixing section 30. The gas mixer 6 is installed on the sieve plate 90 on the upper side of the forced mixing section 30. Ceramic balls are filled between the upper and lower sieve plates 90 of the forced mixing section 30 as gas dispersion components 9, which can fully mix the pre-catalytic reaction gas with the oxidation section products before introducing them all into the catalytic reaction chamber. The catalytic reaction chamber is provided with a synthesis gas outlet 15. The shell-side inlet of the pre-catalytic section 2 is connected to the synthesis gas outlet 15 of the catalytic reaction chamber. The heat of the synthesis gas in the catalytic section 3 is first used to heat the pre-catalytic section 2, and the remaining heat is absorbed by the heat exchange section 4 for preheating the feed gas, generating steam, or for other purposes. The shell-side outlet located on one side of the heat exchange section 4 serves as the product gas outlet 25 of the reactor. The product gas outlet 25 and the burner 12 are respectively arranged at both ends of the housing.

[0059] like Figure 9 , 10 As shown, the precatalytic section can be directly fixed to the shell, or it can be connected through a pipe.

[0060] Example 7: like Figures 11-13 As shown, the general structure of this embodiment is the same as that of Embodiment 5, except that the syngas outlet 15 of the catalytic reaction chamber is located on the side of the shell away from the oxidation section 1. Similarly, the pre-catalytic section 2 can be directly fixed to the shell or connected via a pipeline. Figure 12 As shown, a heat exchange section 4, which is an integral heat exchange structure with the pre-catalytic section 2, can be provided, such as... Figure 13 As shown, heat exchange section 4 may not be required.

[0061] When using the hydrocarbon-containing non-catalytic and catalytic coupled syngas conversion reactors described in Examples 2-7 above, oxygen, a portion of the feed gas, and water vapor enter the oxidation section 1 to undergo an oxidation reaction and generate heat. The outlet gas temperature of the oxidation section is 1100℃~1400℃. Another portion of the feed gas and water vapor enter the pre-catalytic section 2 to undergo a partial conversion reaction. The outlet gases of the oxidation section 1 and the pre-catalytic section 2 are mixed and then enter the catalytic section 3 to complete the conversion of the feed gas. The methane content of the outlet gas of the catalytic section can be controlled to ≤1.0% by volume. The heat from the outlet gas of the catalytic section is supplied to the pre-catalytic section 2 or the heat exchange section 4 for recovery and reuse.

[0062] In the above embodiments, the structure of the gas mixer 6 is as follows: Figure 14 As shown, the gas mixer 6 has a tangential air intake direction, and both the gas mixer 6 and the top plate surface of the forced mixing section 30 facing the oxidation section have a heat insulation layer 20 made of castable material.

[0063] In the above embodiments, the pipe sections of the long central pipe 7, the short central pipe 17, and the central intake pipe 27 within the oxidation section 1 are as follows: Figure 15 The perforated pipe section 5 shown may have one of three structures as illustrated in (a), (b), and (c). The end of the perforated pipe section 5 is a top plate 50, with through holes 51 on its side and / or top. These through holes 51 can be straight or angled. The top plate 50 has a thermal insulation layer 20 made of castable refractory. The thermal insulation layer 20 helps resist the erosion of high-temperature gases in the oxidation section, and perforations may also be present in the thermal insulation layer 20 as needed.

[0064] This invention integrates non-catalytic and catalytic processes into a single housing. The housing structure prevents heat loss and fully utilizes the heat generated in the oxidation section to power the catalytic section, facilitating control. The pre-catalytic section, which requires a relatively lower reaction temperature, can be placed inside or outside the housing as needed. Furthermore, the ratio of feed gas entering the oxidation and pre-catalytic sections can be adjusted according to the requirements of the feed gas and syngas. If necessary, water vapor generated by the heat exchange section in conjunction with steam generator gas can be used as part of the feed gas to adjust the hydrogen-to-carbon ratio of the syngas.

Claims

1. A non-catalytic and catalytic coupled syngas conversion reactor containing hydrocarbon gas, the reactor comprising a shell, an oxidation section (1) provided at one end of the shell, the oxidation section (1) comprising a burner (12) and a first feed gas inlet (13) connected to the burner (12), characterized in that: The reactor further includes a pre-catalytic section (2) and a catalytic section (3), wherein the catalytic section (3) is located inside the shell, and the heat from the reaction gas of the oxidation section (1) is used to heat the catalytic section (3). The pre-catalytic section (2) is located inside or outside the shell. The pre-catalytic section (2) includes a pre-catalytic chamber containing a catalyst (8), and the pre-catalytic chamber is provided with a second raw material gas inlet (14) and a pre-catalytic reaction gas outlet (21). The catalytic section (3) includes a catalytic reaction chamber containing a catalyst (8), and all the pre-catalytic reaction gas is introduced into the catalytic reaction chamber. The catalytic reaction chamber is provided with a synthesis gas outlet (15), and the heat from the synthesis gas of the catalytic section (3) is used to heat the pre-catalytic section (2).

2. The hydrocarbon gas-containing non-catalytic and catalytic coupled syngas conversion reactor as described in claim 1, characterized in that: The shell contains an oxidation section (1), a pre-catalytic section (2), and a catalytic section (3) arranged sequentially from one end to the other. Both the pre-catalytic section (2) and the catalytic section (3) are shell-and-tube heat exchange structures with catalysts (8) arranged in the tube side. The tube sheet cavity of the pre-catalytic section (2) near the oxidation section (1) is provided with a second raw material gas inlet (14). The tube sheet cavity outlet of the catalytic section (3) away from the oxidation section (1) is connected to the shell side of the pre-catalytic section (2) as a synthesis gas outlet (15). The shell side outlet of the pre-catalytic section (2) is used as a product gas outlet (25). The outlet gas of the oxidation section (1) enters the shell side of the catalytic section (3) through a long central tube (7). The shell side outlet of the catalytic section (3) is used as a tail gas outlet (22).

3. The hydrocarbon gas-containing non-catalytic and catalytic coupled syngas conversion reactor as described in claim 1, characterized in that: The shell is arranged sequentially from one end to the other, including the oxidation section (1), the pre-catalytic section (2), the heat exchange section (4) and the catalytic section (3). The pre-catalytic section (2), the catalytic section (3) and the heat exchange section (4) are all set as shell-and-tube heat exchange structures. The catalyst (8) is arranged in the tube side of both the pre-catalytic section (2) and the catalytic section (3). The tube plate cavity of the pre-catalytic section (2) near the oxidation section (1) is provided with a second raw material gas inlet (14). The tube side outlet of the catalytic section (3) is connected to the shell side of the heat exchange section (4). The shell side of the heat exchange section (4) is connected to the shell side of the pre-catalytic section (2). The shell side outlet of the pre-catalytic section (2) is used as the product gas outlet (25). The outlet gas of the oxidation section (1) enters the shell side of the catalytic section (3) through the long central tube (7). The shell side outlet of the catalytic section (3) is used as the tail gas outlet (22).

4. The hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor as described in claim 2 or 3, characterized in that: A gas distributor (26) is arranged in the tube sheet cavity near the second raw material gas inlet (14) of the precatalytic section (2).

5. The hydrocarbon-containing gas non-catalytic or catalytic coupled syngas conversion reactor as described in claim 2 or 3, characterized in that: The long central tube (7) located in the oxidation section (1) is configured as an open pipe section (5) with a top plate (50). The top plate (50) has a heat insulation layer (20) made of castable material. The side wall of the open pipe section (5) and / or the top plate (50) have through holes, which are straight holes or oblique holes.

6. The hydrocarbon gas-containing non-catalytic and catalytic coupled syngas conversion reactor as described in claim 1, characterized in that: The pre-catalytic section (2) and the catalytic section (3) are both located inside the shell. The catalytic section (3) is located in the middle of the shell. One end of the catalytic section (3) is provided with a forced mixing section (30) that is close to the oxidation section (1) and connects the oxidation section (1) with the catalytic reaction chamber. The pre-catalytic section (2) is located at the other end of the catalytic section (3) inside the shell. The second raw material gas inlet (14) is connected to the pre-catalytic chamber by an inlet pipe (18) provided outside the shell. The pre-catalytic chamber is provided with a short central pipe (17) that connects to the oxidation section (1).

7. The hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor as described in claim 6, characterized in that: The precatalytic section (2) has a shell-and-tube heat exchange structure. The catalyst (8) of the precatalytic section (2) is located in the tube side. The shell side inlet of the precatalytic section (2) is connected to the catalytic reaction chamber of the catalytic section (3). The shell side outlet of the precatalytic section (2) serves as the product gas outlet (25) of the reactor.

8. The hydrocarbon-containing non-catalytic and catalytic coupled syngas conversion reactor as described in claim 7, characterized in that: The reactor is also equipped with a heat exchange section (4), which is a shell-and-tube heat exchange structure that is integrated with the pre-catalytic section (2), but the tube side of the heat exchange section (4) is not arranged with catalyst (8).

9. The hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor as described in claim 6, characterized in that: The first raw material gas inlet (13) and the second raw material gas inlet (14) are respectively located at both ends of the shell, and the product gas outlet (25) is located on the side of the shell near the end of the second raw material gas inlet (14).

10. The hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor as described in claim 6, characterized in that: The short central tube (17) located in the oxidation section (1) is configured as an open pipe section (5) with a top plate (50). The top plate (50) has a heat insulation layer (20) made of castable material. The side wall of the open pipe section (5) and / or the top plate (50) have through holes, which are straight holes or oblique holes.

11. The hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor as described in claim 6, characterized in that: The forced mixing section (30) includes upper and lower sieve plates (90), wherein the top of the sieve plate (90) near the oxidation section (1) has a heat insulation layer (20) made of castable material, and a gas dispersant (9) is filled between the two sieve plates (90).

12. The hydrocarbon gas-containing non-catalytic and catalytic coupled syngas conversion reactor as described in claim 11, characterized in that: The gas dispersant (9) is a ceramic ball.

13. A non-catalytic and catalytic coupled syngas conversion reactor containing hydrocarbon gas, characterized by: The reactor includes a shell, and an oxidation section (1) is provided at one end of the shell. The oxidation section (1) includes a burner (12) and a first raw material gas inlet (13) connected to the burner (12). The reactor is characterized in that a catalytic section (3) is provided at the other end of the shell. The catalytic section (3) includes a catalytic reaction chamber in which a catalyst (8) is placed. The catalytic section (3) is provided with a forced mixing section (30) located near the oxidation section (1) and connected to the oxidation section (1) and the catalytic reaction chamber. The heat of the reaction gas in the oxidation section (1) is used to heat the catalytic section (3). The catalytic reaction chamber is provided with a synthesis gas outlet (15) located on the shell. The shell is provided with a shell gas inlet (23) connected to the oxidation section (1).

14. The hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor as described in claim 13, characterized in that: The shell is provided with a pre-catalytic section (2), which includes a pre-catalytic chamber containing a catalyst (8). The pre-catalytic chamber is provided with a second raw material gas inlet (14) and a pre-catalytic reaction gas outlet (21). The pre-catalytic reaction gas is introduced into the catalytic reaction chamber through the shell inlet (23).

15. The hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor as described in claim 14, characterized in that: The precatalytic section (2) has a shell-and-tube heat exchange structure, with the catalyst (8) located inside the tube. The tube inlet of the precatalytic section (2) is used as the second raw material gas inlet (14), and the tube outlet of the precatalytic section (2) is connected to the shell gas inlet (23) as the precatalytic reaction gas outlet (21). The shell inlet of the precatalytic section (2) is connected to the synthesis gas outlet (15) of the catalytic reaction chamber, and the shell outlet of the precatalytic section (2) is used as the product gas outlet (25) of the reactor.

16. The hydrocarbon-containing non-catalytic and catalytic coupled syngas conversion reactor as described in claim 15, characterized in that: The pre-catalytic section (2) and the heat exchange section (4) are an integral shell-and-tube structure, wherein the heat exchange section (4) is arranged at one end of the synthesis gas outlet (15) near the catalytic reaction chamber.

17. The hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor as described in claim 13, characterized in that: The housing air inlet (23) is located at the other end of the housing away from the oxidation section. The housing air inlet (23) is connected to the oxidation section (1) through a central air inlet pipe (27). The synthesis gas outlet (15) is located on the side of the housing near the housing air inlet (23).

18. The hydrocarbon-containing non-catalytic and catalytic coupled syngas conversion reactor as described in claim 17, characterized in that: The central air inlet pipe (27) is located in the oxidation section (1) and one end is configured as an open pipe section (5) with a top plate (50). The top plate (50) has a heat insulation layer (20) made of castable material. The side wall of the open pipe section (5) and / or the top plate (50) have through holes, which are straight holes or oblique holes.

19. The hydrocarbon-containing non-catalytic and catalytic coupled syngas conversion reactor as described in claim 13, characterized in that: The housing air inlet (23) is a side air inlet (24) located near the junction of the oxidation section (1) and the forced mixing section (30), and the synthesis gas outlet (15) is located on the side of the housing away from the oxidation section (1) or away from the oxidation section (1).

20. The hydrocarbon-containing gas non-catalytic and catalytic coupled syngas conversion reactor as described in claim 19, characterized in that: A gas mixer (6) with a spiral structure is arranged between the forced mixing section (30) and the side air inlet (24), and the top of the gas mixer (6) has a heat insulation layer (20) made of castable material.

21. The hydrocarbon-containing gas non-catalytic or catalytic coupled syngas conversion reactor as described in claim 1 or 13, characterized in that: The shell is divided into at least two sections, which are connected by flanges.

22. The hydrocarbon-containing gas non-catalytic or catalytic coupled syngas conversion reactor as described in claim 1 or 13, characterized in that: The shell includes an outer steel plate and a fire-resistant layer (10) and a water-cooled wall disposed on the inner side of the steel plate.

23. The use of the hydrocarbon gas non-catalytic or catalytic coupled syngas conversion reactor according to any one of claims 1 to 22 for the preparation of syngas.

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