WO2023013182A1 - 炭化水素分解用構造体触媒の設計・配置方法、炭化水素分解反応装置の製造方法、炭化水素分解反応装置および反応炉 - Google Patents

炭化水素分解用構造体触媒の設計・配置方法、炭化水素分解反応装置の製造方法、炭化水素分解反応装置および反応炉 Download PDF

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WO2023013182A1
WO2023013182A1 PCT/JP2022/017567 JP2022017567W WO2023013182A1 WO 2023013182 A1 WO2023013182 A1 WO 2023013182A1 JP 2022017567 W JP2022017567 W JP 2022017567W WO 2023013182 A1 WO2023013182 A1 WO 2023013182A1
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Prior art keywords
catalyst
hydrocarbon
reactor
cracking
hydrocarbon cracking
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French (fr)
Japanese (ja)
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伊原良碩
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Ihara Co Ltd
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Ihara Co Ltd
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Priority to US18/554,993 priority Critical patent/US20240123415A1/en
Priority to CN202280028771.4A priority patent/CN117157247B/zh
Priority to EP22852611.7A priority patent/EP4321479A4/en
Priority to JP2022522233A priority patent/JPWO2023013182A1/ja
Priority to JP2023011436A priority patent/JP7242025B1/ja
Publication of WO2023013182A1 publication Critical patent/WO2023013182A1/ja
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    • C—CHEMISTRY; METALLURGY
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    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen; Reversible storage of hydrogen
    • C01B3/02—Production of hydrogen; Production of gaseous mixtures containing hydrogen
    • C01B3/22—Production of hydrogen; Production of gaseous mixtures containing hydrogen by decomposition of gaseous or liquid organic compounds
    • C01B3/24—Production of hydrogen; Production of gaseous mixtures containing hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons
    • C01B3/26—Production of hydrogen; Production of gaseous mixtures containing hydrogen by decomposition of gaseous or liquid organic compounds of hydrocarbons using catalysts
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/248—Reactors comprising multiple separated flow channels
    • B01J19/2485—Monolithic reactors
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
    • B01J35/54—Bars or plates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/0285—Heating or cooling the reactor
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J8/00—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes
    • B01J8/02—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds
    • B01J8/06—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds in tube reactors; the solid particles being arranged in tubes
    • B01J8/062—Chemical or physical processes in general, conducted in the presence of fluids and solid particles; Apparatus for such processes with stationary particles, e.g. in fixed beds in tube reactors; the solid particles being arranged in tubes being installed in a furnace
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen; Reversible storage of hydrogen
    • C01B3/02—Production of hydrogen; Production of gaseous mixtures containing hydrogen
    • C01B3/32—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air
    • C01B3/34—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide or air by reaction of hydrocarbons with gasifying agents using catalysts
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00106—Controlling the temperature by indirect heat exchange
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    • B01J2208/00—Processes carried out in the presence of solid particles; Reactors therefor
    • B01J2208/00008—Controlling the process
    • B01J2208/00017—Controlling the temperature
    • B01J2208/00504—Controlling the temperature by means of a burner
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00049—Controlling or regulating processes
    • B01J2219/00051—Controlling the temperature
    • B01J2219/0015—Controlling the temperature by thermal insulation means
    • B01J2219/00155—Controlling the temperature by thermal insulation means using insulating materials or refractories
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
    • B01J2219/322—Basic shape of the elements
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
    • B01J2219/322—Basic shape of the elements
    • B01J2219/32203—Sheets
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
    • B01J2219/322—Basic shape of the elements
    • B01J2219/32203—Sheets
    • B01J2219/32206—Flat sheets
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
    • B01J2219/322—Basic shape of the elements
    • B01J2219/32203—Sheets
    • B01J2219/3221—Corrugated sheets
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
    • B01J2219/322—Basic shape of the elements
    • B01J2219/32203—Sheets
    • B01J2219/32237—Sheets comprising apertures or perforations
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
    • B01J2219/322—Basic shape of the elements
    • B01J2219/32286—Grids or lattices
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/32—Details relating to packing elements in the form of grids or built-up elements for forming a unit of module inside the apparatus for mass or heat transfer
    • B01J2219/322—Basic shape of the elements
    • B01J2219/32296—Honeycombs
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0266—Processes for making hydrogen or synthesis gas containing a decomposition step
    • C01B2203/0277—Processes for making hydrogen or synthesis gas containing a decomposition step containing a catalytic decomposition step
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/085—Methods of heating the process for making hydrogen or synthesis gas by electric heating
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/10—Catalysts for performing the hydrogen forming reactions
    • C01B2203/1005—Arrangement or shape of catalyst
    • C01B2203/1011—Packed bed of catalytic structures, e.g. particles, packing elements
    • C01B2203/1017—Packed bed of catalytic structures, e.g. particles, packing elements characterised by the form of the structure
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • C01B2203/1241—Natural gas or methane
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • H01M8/0612—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants from carbon-containing material

Definitions

  • the present invention relates to a method for designing and arranging a structural catalyst for hydrocarbon cracking, a method for manufacturing a hydrocarbon cracking reactor, a hydrocarbon cracking reactor and a reactor.
  • the steam reforming catalyst When the steam reforming catalyst is a granular catalyst, it is usually filled in a certain space partitioned by partition walls and through which the raw material gas flows. The heat is transferred to one granular catalyst, and other packed granular catalysts are heated by heat radiation from the one granular catalyst and heat transfer via convection of the raw material gas (non-patent Reference 1).
  • heat transfer in the catalyst layer is mainly convective heat transfer via fluid, so the thermal efficiency is poor, and the raw material gas (hydrocarbon and steam) is preheated to nearly 500 ° C.
  • Patent Document 5, Patent Document 6, etc. the pressure loss in the catalyst layer is large, the responsiveness during load fluctuations and startup, the temperature rise of the reaction field, and the followability to temperature fluctuations are slow. There is also a problem that the reaction tube must be lengthened and the apparatus tends to be large.
  • JP-A-6-229530 Japanese Patent Application Laid-Open No. 2001-031403 Japanese Patent Application Laid-Open No. 2000-178004 WO2020/090245, Fig. 7b JP-A-2004-83332 Japanese Patent Publication No. 2019-529318
  • the reaction gas is first heated by a heater arranged around the reactor or along the center of the vertical axis.
  • a heating method Patent Document 2, Patent Document 4, FIG. 10
  • a method of arranging a structured catalyst so as to be in direct contact with a heater partition and heating the catalyst by conductive heat transfer Non-Patent Document 1
  • the former method has a large energy loss. , a more efficient heating technique is desired.
  • the latter method has high hurdles from the viewpoint of practicality, such as the problem of compatibility between the heater partition and the catalyst component, the problem that the entire heater partition must be replaced due to deterioration of the catalyst, the limitation of the catalyst area, and the like.
  • the present invention provides a method of designing and arranging a structural catalyst for cracking hydrocarbons, a hydrocarbon cracking reactor and a reactor, and a method of manufacturing the same, in order to realize more efficient heat utilization than conventional ones. for the purpose.
  • hydrocarbon cracking structure catalyst having a structure that allows reaction gas to flow from one end to the other end when properly arranged in a reaction chamber. and a heat source arranged inside or outside the reaction chamber and capable of heating the structured hydrocarbon cracking catalyst, wherein the structured hydrocarbon cracking catalyst is heated by a reaction gas.
  • the hydrocarbon cracking reactor has a shape surrounding a boundary wall or a boundary side separating the hydrocarbon cracking structure catalyst and the heat source in a cross-sectional view perpendicular to the flow direction of the hydrocarbon cracking reactor.
  • the shape of the hydrocarbon cracking reactor is symmetrical with respect to the normal to the boundary wall surface or the normal to the imaginary cylindrical side surface including the boundary side, starting from a point. According to such a structure, the radiant heat once absorbed and re-radiated or reflected by an arbitrary catalyst surface is highly likely to be received by the same catalyst surface or another catalyst surface in a symmetrical relationship with respect to the normal, and the radiant heat Efficient heat utilization that makes more effective use of
  • the heat source is preferably housed in a heater housing that occupies substantially the center of the reaction chamber in a cross-sectional view perpendicular to the flow direction of the reaction gas. According to such a configuration, the surface area is smaller than in the case of heating the outside of the reaction chamber, and it is away from the low-temperature outside air.
  • the heat source is a regenerative radiant tube burner, which is preferably housed in a rectangular heater housing that occupies substantially the center in a cross-sectional view perpendicular to the direction of flow of the reaction gas. According to such a configuration, it is possible to efficiently heat only the catalyst surface that contributes to the reaction while taking advantage of the high thermal efficiency of the regenerative radiant tube burner.
  • Another aspect of the present invention is a direct hydrocarbon cracking reactor equipped with the above hydrocarbon cracking reactor.
  • the steam heater, raw gas preheater, CO conversion device, and CCS device required for steam reforming become unnecessary, and the size can be overwhelmingly reduced compared to conventional hydrogen generators.
  • preheating of the raw material gas and the like and high pressure are not required, so it is considered to be advantageous.
  • the reactor for direct cracking of hydrocarbons is equipped with a second structure catalyst that can be brought into contact with the unreacted reaction gas coming out of the other end by convection.
  • a constant production rate is maintained by using not only a so-called permeation-type structured catalyst in which the reaction gas flows from one end to the other, but also a second structured catalyst that can come into contact with the reaction gas by convection.
  • the ratio of unreacted reaction gas can be reduced and the conversion rate can be improved.
  • the reactor for direct cracking of hydrocarbons is equipped with a hydrogen refining module for selectively discharging hydrogen in the reactor to reduce the partial pressure of hydrogen in the reactor and promote the cracking reaction of hydrocarbons. .
  • a hydrogen refining module for selectively discharging hydrogen in the reactor to reduce the partial pressure of hydrogen in the reactor and promote the cracking reaction of hydrocarbons.
  • Another aspect of the present invention is to determine the shape of the reaction chamber and the shape and placement of the heat source within or outside the reaction chamber, and to position the hydrocarbon cracking structural catalyst of the first shape in the first coordinate system.
  • calculating or actually measuring the radiant heat (E1) received per unit time by the structural body catalyst for cracking hydrocarbons in the first shape; deforming the structured catalyst and/or moving the coordinate system; and the radiant heat (E2) received per unit time by the structural catalyst for hydrocarbon cracking after deformation and/or coordinate movement in the reaction chamber is A method for designing and arranging a structured catalyst for cracking hydrocarbons, including confirming that the radiant heat (E1) received per unit time by the structured catalyst for cracking hydrocarbons in the shape of No. 1 is large.
  • the shape and arrangement of the hydrocarbon cracking structured catalyst are optimized by repeating the deformation of the shape of the hydrocarbon cracking structured catalyst and confirmation of the radiant heat value. can be done.
  • Another aspect of the present invention is a method for manufacturing a hydrocarbon cracking reactor including a method for designing and arranging the structure catalyst for cracking hydrocarbons. According to such a production method, even if the catalyst surface area is the same, it is possible to design and arrange the catalyst surface so that it is locally heated by radiant heat, and even without considering other heating factors such as heat conduction and convection from the reaction gas. Efficient heat utilization can be realized.
  • the heating efficiency of the structure catalyst for hydrocarbon cracking can be increased,
  • the reactor temperature can be lowered, and in some cases, it becomes possible to use inexpensive structural materials with low heat resistance as reactor materials.
  • FIG. 2 is a cross-sectional view along line BB of the first embodiment of the hydrocarbon cracking reactor of the present invention; AA enlarged cross-sectional view in the lower end open cylinder of FIG. (a) Side view and (b) AA end view of the catalyst arrangement of the second embodiment.
  • FIG. 5 is a cross-sectional view of the catalyst arrangement of the third embodiment as seen from a cross section perpendicular to the direction of reaction gas flow; (a) CC end view, (b) AA sectional view, and (c) BB sectional view of the catalyst arrangement of the fourth embodiment.
  • FIG. 3 is a cross-sectional view showing the arrangement of the decorated catalyst plates of Experimental Example 1; Graph of the results of Experimental Example 1.
  • FIG. Sectional drawing which shows the conventional catalyst structural example.
  • structure catalyst for hydrocarbon cracking refers to a structure of a reaction process for all or part of a steam reforming reaction of hydrocarbons, or a reaction process for all or part of a direct cracking reaction of hydrocarbons. Catalyst. Preferred hydrocarbons are methane, ethane, propane or naphtha.
  • structured catalyst refers to a plate (not only a flat plate, but also a flat plate subjected to arbitrary processing such as bending, bending, punching, notching, embossing, etc.), porous body, honeycomb (monolithic), felt, mesh, fabric or expanded metal.
  • the structure-based catalyst generally refers to the one obtained by impregnating a base material having a shape such as a honeycomb into a slurry containing catalyst components.
  • a non-supported catalyst layer (plated layer, sprayed layer) may be formed by, for example, exposing.
  • the term "flow direction of reactant gas” means a linear or curvilinear direction of flow of the reactant gas in the reaction chamber. Therefore, in order to promote stirring contact, even if the catalyst is decorated with projections or placed on the flow path, the flow of the reaction gas is locally and microscopically changed. However, it should be noted that the local and microscopic changes in the flow do not necessarily match the direction in which the reaction gas flows.
  • boundary wall means a macroscopic geometric boundary wall for defining linear heat radiators and/or normal vectors. Therefore, the fine surface condition of the wall surface is not considered.
  • the "boundary wall surface” may be the surface of the heat source itself, or may be the wall surface of a cylindrical partition wall or a hollow partition wall having a rectangular cross section that separates the heat source from the space in the reaction chamber.
  • boundary side means each side of a rectangular or square shape when the heat source or the partition wall is viewed perpendicularly to the flow direction of the reaction gas.
  • virtual cylinder side surface means a side surface of a virtual cylinder when a virtual cylinder including boundary sides is considered.
  • normal to the boundary wall surface or normal to the imaginary cylindrical side surface including the boundary edge means selected specific normals rather than all normals.
  • a typical hydrocarbon cracking reactor 1 shown in FIG. A supply pipe 6 that penetrates the lid 5 at the upper end of the open cylinder 4 to supply the reaction gas to the upper part of the cylinder 4 with the lower end open, and a gas containing the product gas that penetrates the lid 7 at the upper end of the product discharge container 2.
  • a hydrocarbon cracking structure catalyst 9 having a structure in which the reaction gas can flow from the upper end to the lower end when placed in the lower end open cylinder 4; and the upper lid 5 of the lower end open cylinder 4. It has a bottomed tube 11 penetrating through substantially the center and extending downward in the vertical direction, and a heat source 10 housed in the bottomed tube 11 .
  • the hydrocarbon-decomposing structure catalyst 9 in this embodiment has a chrysanthemum-like contour shape when viewed in a cross section perpendicular to the vertical direction of flow of the reaction gas. (boundary wall).
  • a chrysanthemum is composed of 23 single petals obtained by placing two curved catalysts facing each other, and the adjacent petals are combined so as to be integrated from the inner end to the center.
  • the petals have a tip 14 located on a normal line 13 to the boundary wall surface 12, and have a symmetrical shape with respect to the normal line 13 with that point as a starting point.
  • one side of the two curved catalysts is butted against each other at a portion corresponding to the tip of the petal.
  • a cylindrical hydrocarbon-decomposing structure catalyst 19 surrounding a bottomed cylinder 11 is viewed in cross section perpendicular to the vertical direction in which the reaction gas flows. It is different from the first embodiment in that it is corrugated as shown in 3(b).
  • the shape of the catalyst 19 is symmetrical with respect to the normal line 15 with respect to the normal line 15 with respect to the boundary wall surface 12 with the point 16 on the normal line 15 to the boundary wall surface 12 as a starting point in a cross-sectional view perpendicular to the vertical direction of flow of the reaction gas. It has become.
  • the heat source 20 includes a substantially W-shaped radiant tube 22 when viewed from the side, a pair of gas burners 24 disposed at both ends of the radiant tube 22, and the radiant tube 22.
  • a regenerative radiant tube burner 27 is provided with a pair of regenerators 26 provided at both ends.
  • the entire tube 22 of the burner 27 is housed in a rectangular parallelepiped heater housing 25 .
  • the flow direction of the reaction gas is the direction toward the depth of the paper surface of FIG. 5(a) and the direction from the top of the paper surface of FIGS.
  • U-shaped and horseshoe-shaped structure catalysts 39 for hydrocarbon cracking are arranged with their openings directed in a cross-sectional view perpendicular to the flow direction of the reaction gas.
  • the catalyst plates 39a, 39b, and 39c are arranged in close contact so that no gap is formed between them.
  • the shape of the catalysts 39a, 39b, and 39c starts from a point 38a on the normal line 37a to the boundary wall surface 32 in a cross-sectional view perpendicular to the vertical direction of flow of the reaction gas shown in FIG. 5(a).
  • the hydrocarbon cracking reactor 61a includes a single-end radiant tube burner 67 as a heat source, a corrugated catalyst 19 (first structure catalyst) shown in FIG. It is composed of a guide tube 64a that accommodates the upper end and introduces the reaction gas. Since the source gas passes through the inside of the corrugated catalyst 19 from the upper end to the lower end, it is a kind of gas permeable catalyst. Due to the shape, the raw material gas leaking from the lower end of the waved catalyst 19 also contacts the outside of the waved catalyst 19 and spreads over the entire reactor 62 .
  • the catalyst module 61b includes a second structure catalyst 69 that can be brought into contact with the unreacted reaction gas coming out of the lower end of the hydrocarbon cracking reactor 61a by convection, and a holder that holds the second structure catalyst 69 from above. It is different from the hydrocarbon cracking reactor 61a in that the second structure catalyst 69 does not surround the burner 67. As shown in FIG. As the second structured catalyst 69, the same or different material as that of the first structured catalyst 19 can be used.
  • the structure of the second structured catalyst since it is not necessary to have a heat source in the center of the structure, it is possible to apply not only a plate (not only a flat plate but also bending, bending, punching, notching, embossing, etc., to a flat plate). ), porous body, honeycomb (monolithic type), felt, mesh, fabric, or expanded metal, which is different from the structure of the first structure catalyst 19 may be used. Permissible.
  • a method for heating the second structure catalyst 69 it is possible to use the radiant heat generated by the gas permeable catalyst by installing it in a place facing the gas permeable catalyst, or to heat the catalyst by the convection of the high temperature gas in the furnace. Surface heating can also be used.
  • a reactant gas supply pipe 66a is connected to the upper end surface of the reactor 62 to supply the reactant gas to the hydrocarbon cracking reactor 61a.
  • the hydrocarbon cracking reactor 61a is also provided with a combustion gas introduction pipe 66b for supplying combustion gas to the burner 67 and a blower 68 for supplying air.
  • a desulfurizer 63 is provided between the source gas supply pipe 66 a and the source gas supply source 71 .
  • the desulfurizer 63 it is possible to remove the sulfur compound added as an odorant to the city gas or LPG, thereby preventing the structural catalyst from being poisoned or deteriorating in performance.
  • a lower end face of the reactor 62 is connected with a discharge and recovery device 72 for carbon produced by the hydrocarbon cracking reactor 61a and the catalyst module 61b.
  • a typical discharge recovery device is shown in Patent Document 4, and includes a decompression chamber communicating with a reactor lower opening of a reactor via a vent hole, a first on-off valve capable of opening and closing the vent hole, and a decompression chamber. a collection box that communicates through a channel, a second on-off valve that can open and close the channel, and a decompression pump that communicates with the collection box.
  • the crude refining device 65 is a device that lowers the concentration of hydrogen inside the reactor 62 and increases the concentration of hydrogen released outside the reactor 62 compared to the inside of the reactor.
  • Ceramic materials such as ⁇ -alumina, ⁇ -alumina, silica, zirconia, silicon nitride, silicon carbide, titania, and zeolite, or nickel, copper, iron, etc., described in JP-A-2006-007134, etc.
  • Pore-controlled silica membranes, palladium (Pd) membranes, palladium alloy (PdAg, PdCu, etc.) membranes, vanadium membranes, and zirconium carried or supported on porous substrates made of metal materials such as zinc and their alloys. /A nickel alloy film, a zeolite film, and the like.
  • the generated gas with a high hydrogen concentration that has passed through the crude refining device 65 is temporarily stored in a tank 74 using a pump 73, and after precision refining by a pressure swing adsorber (PSA) 75, it becomes product hydrogen.
  • PSA pressure swing adsorber
  • a commercially available pressure swing adsorber (PSA) can be used.
  • the methane separated by the PSA 75 may be merged with the reaction gas introduction pipe 66 through a return pipe (not shown) and reused as a reaction gas.
  • a method for designing and arranging a structured catalyst for cracking hydrocarbons (hereinafter referred to as the present method) is also another aspect of the present invention. Each step will be described below.
  • the method includes determining (S1) the shape of the reaction chamber and the shape and arrangement of heat sources inside or outside the reaction chamber.
  • the shape of the reaction chamber can adopt the shape of typical reaction chambers of tubular reactors, fixed bed reactors or packed bed catalytic reactors.
  • the shape and arrangement of the heat source is, for example, a cylindrical shape with a bottom that is arranged so as to occupy substantially the center of the reaction chamber in a cross-sectional view perpendicular to the flow direction of the reaction gas.
  • the method includes a step (S2) of placing a hydrocarbon cracking structure catalyst having a first shape at a first position in a first coordinate system.
  • the first shape is a plate-like catalyst, and the first position in the first coordinate system is radial in a cross-sectional view perpendicular to the flow direction of the reaction gas. It can be in the plane containing the normal to the boundary wall separating the heat source and the reaction chamber. Alternatively, the first shape can be a cylindrical shape open at both ends.
  • This method includes a step (S3) of calculating or actually measuring the radiant heat (E1) that the first shape hydrocarbon cracking structure catalyst receives per unit time.
  • the emissivity of the object can be determined based on known data, and simulation calculation can be performed according to Stefan Boltzmann's law.
  • thermography, thermocouples, etc. are used to observe the temperature distribution, temperature rise rate, etc. at various locations on the catalyst surface.
  • the method includes a step of deforming the first shape hydrocarbon cracking structure catalyst and/or moving the coordinate system (S4).
  • deformation is actually deformation, and movement of the coordinate system is performed by, for example, changing the position on the rack and changing the inclination.
  • the position and inclination can be changed, for example, by providing a large-diameter ring and a small-diameter ring at the upper end and the lower end of the rack, and radially providing bridges connecting the large-diameter ring and the small-diameter ring along the radial direction.
  • teeth are formed at regular intervals so that the upper end bridge and the lower end bridge are opposed to each other, and the position between the teeth that sandwiches the upper and lower ends of the catalyst is independently changed vertically.
  • the method includes a step of confirming that the reaction gas can flow from one end to the other end when the structural catalyst for hydrocarbon cracking after deformation and/or coordinate movement is placed in the reaction chamber (S5).
  • a virtual reaction gas inlet and a virtual catalyst are provided at predetermined positions in a virtual reaction chamber on a computer, and whether or not the fluid moves from one end of the catalyst to the other end is checked.
  • a simulation may be performed, or an introduction port for the reaction gas may be provided at a predetermined position in the actual reaction chamber, and it may be confirmed whether the reaction gas flows from one end of the catalyst to the other end.
  • a reaction gas inlet in the reaction chamber may be moved.
  • the present method is characterized in that the radiant heat (E2) received per unit time by the structural catalyst for hydrocarbon cracking after deformation and/or after coordinate movement in the reaction chamber is converted into the structural catalyst for hydrocarbon cracking of the first shape. is greater than the radiant heat (E1) received per unit time (S6).
  • E2 radiant heat
  • E1 radiant heat received per unit time
  • Example 1-Reaction test by internal heating reactor using decorated catalyst plate A heater housing cylinder 11 containing a 2 kW heater (manufactured by Sanyo Nekko Co., Ltd.) is inserted along the vertical central axis of a cylindrical SUS304 transmission type small reactor, and the thickness is 0.6 mm*width 37 mm*length 200 mm.
  • 46 catalyst plates 49 (nickel-based metal catalyst) are arranged around the heater housing cylinder 11 so as to bend in the same direction and with the same degree of curvature as shown in FIG.
  • the catalyst plate 49 was arranged and fixed, and a projection 46 was provided for promoting contact with stirring.
  • the total geometrical area of the catalyst amounted to 0.68 m 2 on both sides.
  • methane is introduced into the heater at a pressure of 0.3 MPa and a flow rate of 1000 mL/min so that the flow is parallel to the catalyst from the methane supply pipe that penetrates the upper lid of the furnace.
  • a direct carbon decomposition reaction experiment was conducted at a temperature of 950-1000° C. for about 2 hours and 25 minutes.
  • the hydrogen concentration was measured by a gas heat conduction type gas analyzer (zero gas: city gas 13A, span gas: 100% hydrogen, gas flow rate: 1.0 L/min, Chino Corporation (manufactured) was installed and measured. The results are shown in FIG.
  • the heater temperature is close to 950° C.
  • the reaction furnace temperature is as low as 650° C.
  • the boundary film portion of the catalyst plate 49 is not sufficiently heated, resulting in low hydrogen production efficiency.
  • the hydrogen production efficiency of the catalyst was only 10% even if the heater temperature was increased from 950°C to 1000°C, so the experiment was stopped.
  • Example 2-Radiation heating test in which the catalyst is arranged in a chrysanthemum-like pattern when viewed in cross section A set of two catalyst plates having the same size as in Experimental Example 1 was curved so as to face each other, and 23 sets were arranged around the heater housing cylinder. It was configured to have a chrysanthemum-like outline shape (Fig. 2) when viewed in cross section perpendicular to the direction of flow.
  • Fig. 2 chrysanthemum-like outline shape
  • the structure catalyst for hydrocarbon cracking has a symmetrical shape starting from a point on the normal line to the boundary wall surface in a cross-sectional view perpendicular to the flow direction of the reaction gas, so that on the surface of the catalyst plate It was found that the catalyst plate has a shape that allows the reflected heat radiation to be easily received. On the other hand, the surface of the catalyst plate opposite to the surface receiving heat radiation was at a lower temperature, indicating that the surface of the catalyst plate was locally heated.
  • Example 3-Reaction test using an internally heated reactor in which the catalyst is arranged as shown in FIG. 2 A catalyst and a heater with a total geometric area of 0.68 m 2 on the front and back, arranged as in Experimental Example 2, were housed along the vertical central axis of a small cylindrical permeation reactor, and through the methane flow path, Methane was introduced at a methane supply pressure of 0.3 MPa and a methane flow rate of 1 L/min, and a carbon direct decomposition reaction experiment was carried out. As a result, as shown in FIG. 9, compared to the internally heated reactor of Experimental Example 1, although the total geometric area of the catalyst was the same and the heater capacity was the same, hydrogen was generated.
  • the amount was good, the heater temperature was 1000°C, the reactor temperature was 650°C, and the hydrogen concentration was 55%. It was suggested that it is important to devise the layout of the catalyst so that it is susceptible to radiant heat and causes local heating on the surface of the catalyst plate.
  • the embodiments of the present invention are by no means limited to the above embodiments, and not all of the configurations described in the above embodiments are essential requirements of the present invention.
  • the present invention can take various forms such as modifications as long as it falls within the technical scope without departing from its technical idea.
  • the heater housing portion 25 is not necessarily required, and thermal efficiency is better without it. It is not necessary if the burner is highly airtight, like a regenerative radiant tube placed in a vacuum heat treatment furnace.
  • the second structure catalyst 69 is housed in the holding tube 64b only in its upper portion, it may be exposed to the reactor 62. FIG.
  • the hydrocarbon cracking reactor of the present invention is equipped with a device for increasing the purity of the hydrogen contained in the generated gas, so that it can be delivered to a fuel cell vehicle equipped with a polymer electrolyte fuel cell [PEFC] through an on-site station or the like. It can be suitably applied to hydrogen supply.
  • a device for increasing the purity of the hydrogen contained in the generated gas so that it can be delivered to a fuel cell vehicle equipped with a polymer electrolyte fuel cell [PEFC] through an on-site station or the like. It can be suitably applied to hydrogen supply.
  • PEFC polymer electrolyte fuel cell
  • SOFC solid oxide fuel cells
  • carbon deposition on the metallic nickel surface due to the thermal decomposition reaction of methane and performance deterioration due to the electrode reaction inhibition effect due to the adsorption of the generated CO on the metallic nickel surface have been recognized (Sato et al., " From the viewpoint of fuel cell and methane utilization technology", J. Plasma Fusion Res. Vol. 87, No. 1 (2011) pp. 36-41), the hydrocarbon cracking of the present invention as a fuel reformer arranged in the preceding stage
  • the use of a reactor is expected to lead to a reduction in carbon deposits and a longer service life in SOFCs.

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PCT/JP2022/017567 2021-08-04 2022-04-12 炭化水素分解用構造体触媒の設計・配置方法、炭化水素分解反応装置の製造方法、炭化水素分解反応装置および反応炉 Ceased WO2023013182A1 (ja)

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US18/554,993 US20240123415A1 (en) 2021-08-04 2022-04-12 Method for designing and arranging structural catalyst for decomposition of hydrocarbons, method for producing reactor for decomposition of hydrocarbons, reactor for decomposition of hydrocarbons and reaction furnace
CN202280028771.4A CN117157247B (zh) 2021-08-04 2022-04-12 烃分解用结构体催化剂的设计及布置方法、烃分解反应装置的制造方法、烃分解反应装置及反应炉
EP22852611.7A EP4321479A4 (en) 2021-08-04 2022-04-12 Design and positioning method for a structural hydrocarbon degradation catalyst, manufacturing method for the hydrocarbon degradation reaction device, hydrocarbon degradation reaction device, and reactor furnace
JP2022522233A JPWO2023013182A1 (https=) 2021-08-04 2022-04-12
JP2023011436A JP7242025B1 (ja) 2021-08-04 2023-01-28 炭化水素分解用構造体触媒の設計・配置方法、炭化水素分解反応装置の製造方法、炭化水素分解反応装置および反応炉

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