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WO2025206304A1 - Dispositif de production de combustible - Google Patents

Dispositif de production de combustible

Info

Publication number
WO2025206304A1
WO2025206304A1 PCT/JP2025/012751 JP2025012751W WO2025206304A1 WO 2025206304 A1 WO2025206304 A1 WO 2025206304A1 JP 2025012751 W JP2025012751 W JP 2025012751W WO 2025206304 A1 WO2025206304 A1 WO 2025206304A1
Authority
WO
WIPO (PCT)
Prior art keywords
catalyst layer
catalyst
fuel production
flow path
cells
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
PCT/JP2025/012751
Other languages
English (en)
Japanese (ja)
Inventor
玄将 大西
啓輔 丸市
義政 小林
雄樹 藤田
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
NGK Insulators Ltd
Original Assignee
NGK Insulators Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by NGK Insulators Ltd filed Critical NGK Insulators Ltd
Publication of WO2025206304A1 publication Critical patent/WO2025206304A1/fr
Pending legal-status Critical Current
Anticipated expiration legal-status Critical

Links

Classifications

    • 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
    • B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
    • B01J35/57—Honeycombs
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G2/00—Production of liquid hydrocarbon mixtures of undefined composition from oxides of carbon
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G45/00—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds
    • C10G45/58—Refining of hydrocarbon oils using hydrogen or hydrogen-generating compounds to change the structural skeleton of some of the hydrocarbon content without cracking the other hydrocarbons present, e.g. lowering pour point; Selective hydrocracking of normal paraffins
    • C—CHEMISTRY; METALLURGY
    • C10—PETROLEUM, GAS OR COKE INDUSTRIES; TECHNICAL GASES CONTAINING CARBON MONOXIDE; FUELS; LUBRICANTS; PEAT
    • C10G—CRACKING HYDROCARBON OILS; PRODUCTION OF LIQUID HYDROCARBON MIXTURES, e.g. BY DESTRUCTIVE HYDROGENATION, OLIGOMERISATION, POLYMERISATION; RECOVERY OF HYDROCARBON OILS FROM OIL-SHALE, OIL-SAND, OR GASES; REFINING MIXTURES MAINLY CONSISTING OF HYDROCARBONS; REFORMING OF NAPHTHA; MINERAL WAXES
    • C10G47/00—Cracking of hydrocarbon oils, in the presence of hydrogen or hydrogen- generating compounds, to obtain lower boiling fractions

Definitions

  • a catalyst for use in producing such synthetic fuels for example, a catalyst having a Fischer-Tropsch synthesis catalyst containing an alumina support and cobalt, and a beta zeolite membrane formed on the outer surface of the Fischer-Tropsch synthesis catalyst has been proposed (see, for example, Patent Document 1).
  • a primary object of the present invention is to provide a fuel production apparatus capable of improving the conversion rate of carbon oxides and efficiently producing synthetic fuel.
  • the second flow path is located on the opposite side of the second catalyst layer from the first catalyst layer.
  • a synthetic fuel produced by a hydrocracking reaction and/or an isomerization reaction of the hydrocarbon compound may flow into the second flow path.
  • the fuel production apparatus according to [2] above may include a honeycomb structure having a plurality of first cells including the first flow passages and a plurality of second cells including the second flow passages.
  • each of the plurality of first cells and the plurality of second cells may extend from a first end face to a second end face of the honeycomb structure.
  • the honeycomb structure may include first plugs. The first plugs are provided in at least some of the plurality of first cells.
  • the honeycomb structure may further include second plugs.
  • the second plugs are provided in at least some of the second cells.
  • the second plugs plug the ends of the second flow paths on the first end face side.
  • the honeycomb structure may include a honeycomb substrate.
  • the honeycomb substrate includes partition walls.
  • the partition walls define the plurality of first cells and the plurality of second cells.
  • the second catalyst layer may be laminated on a surface of the partition walls on the first flow path side.
  • the first catalyst layer may be located on the opposite side of the partition walls with respect to the second catalyst layer.
  • the first catalyst layer may be laminated on the second catalyst layer.
  • the porosity of the partition wall may be 25% to 70%.
  • the partition wall may have a thermal conductivity of 0.4 W/mK or more.
  • the partition wall may have a thermal conductivity of 8 W/mK or more.
  • the partition wall may contain cordierite and/or SiC.
  • the partition wall may contain SiC.
  • the first catalyst may contain at least one kind of transition metal.
  • the transition metal may contain Co and/or Fe.
  • the second catalyst may contain zeolite.
  • the first catalyst layer and/or the second catalyst layer may further contain a filler, and the filler may have a thermal conductivity of 0.1 W/m ⁇ K to 500 W/m ⁇ K.
  • FIG. 1 is a schematic cross-sectional view of a fuel production apparatus according to one embodiment of the present invention.
  • FIG. 2 is a schematic cross-sectional view of a fuel production apparatus according to another embodiment of the present invention.
  • FIG. 3 is a schematic perspective view of a fuel production apparatus according to yet another embodiment of the present invention.
  • FIG. 4 is a schematic cross-sectional view of the fuel production apparatus of FIG.
  • FIG. 5 is a schematic cross-sectional view of a fuel production apparatus according to yet another embodiment of the present invention.
  • FIG. 6 is a schematic cross-sectional view of a fuel production apparatus according to yet another embodiment of the present invention.
  • FIG. 7 is a schematic cross-sectional view of a fuel production apparatus according to yet another embodiment of the present invention.
  • FIG. 8 is a schematic cross-sectional view of a fuel production apparatus according to yet another embodiment of the present invention.
  • the fuel production apparatus 100 has a first flow path 4.
  • a feed gas containing carbon oxides and hydrogen is supplied to the first flow path 4.
  • carbon oxides include carbon monoxide (CO) and carbon dioxide ( CO2 ).
  • the feed gas typically contains carbon monoxide.
  • the fuel production device 100 includes a first catalyst layer 1 and a second catalyst layer 2.
  • the first catalyst layer 1 is disposed facing the first flow path 4.
  • the first catalyst layer 1 contains a first catalyst capable of promoting the FT reaction.
  • the second catalyst layer 2 is located on the opposite side of the first catalyst layer 1 from the first flow path 4.
  • the second catalyst layer 2 contains a second catalyst capable of promoting the hydrocracking reaction and/or the isomerization reaction of hydrocarbon compounds produced by the FT reaction.
  • the first catalyst layer containing the first catalyst capable of promoting the FT reaction faces the first flow path, so that the raw material gas can be brought into stable contact with the first catalyst, thereby allowing the FT reaction represented by the following formula (1) to proceed smoothly and improving the carbon monoxide conversion rate.
  • nCO+(2n+1)H 2 ⁇ C n H 2n+2 +nH 2 O...(1) This produces hydrocarbon compounds including alkanes ( C n H 2n +2 ), where n is an integer of 1 or more.
  • Hydrocarbon compounds typically include n-paraffins (straight-chain alkanes) and isoparaffins (branched alkanes).
  • n-paraffins straight-chain alkanes
  • isoparaffins branched alkanes
  • the fuel production apparatus 101 further includes a second flow path 5 in addition to the first flow path 4.
  • the second flow path 5 is located on the opposite side of the second catalyst layer 2 from the first catalyst layer 1.
  • a synthetic fuel produced by the hydrocracking reaction and/or the isomerization reaction of the hydrocarbon compounds flows into the second flow path 5, typically in a gaseous state.
  • a fluid flowing through the fuel production apparatus flows from the first flow path through the first and second catalyst layers in this order before entering the second flow path. Therefore, the raw material gas supplied to the first flow path flows through the first catalyst layer and comes into stable contact with the first catalyst contained in the first catalyst layer. As a result, hydrocarbon compounds are efficiently produced from the raw material gas.
  • the produced hydrocarbon compounds typically in a gaseous state, flow through the second catalyst layer and come into stable contact with the second catalyst contained in the second catalyst layer. This allows for efficient production of synthetic fuel from the hydrocarbon compounds.
  • the synthetic fuel then flows into the second flow path, typically in a gaseous state, allowing for smooth recovery of the synthetic fuel from the second flow path.
  • the fuel production device 102 includes a honeycomb structure 10.
  • the honeycomb structure 10 has a plurality of first cells 321 each including a first flow path 4 and a plurality of second cells 322 each including a second flow path 5.
  • the fuel production device 102 further includes a first sealing portion 6.
  • the first sealing portion 6 is provided in at least a portion of the plurality of first cells 321. In the illustrated example, the first sealing portion 6 is provided in all of the plurality of first cells 321.
  • the first sealing portion 6 seals the end of the first flow path 4 on the side of the second end face E2 (outlet end face). With this configuration, the first sealing portion seals the end of the first flow path on the outlet end face side, so that in the fuel production device, the fluid can stably flow from the first flow path through the first catalyst layer and the second catalyst layer in this order into the second flow path, thereby more efficiently producing synthetic fuel.
  • the fuel production device 102 may further include a second sealing portion 7.
  • the second sealing portion 7 is provided in at least a portion of the plurality of second cells 322. In the illustrated example, the second sealing portion 7 is provided in all of the plurality of second cells 322.
  • the second sealing portion 7 seals the end of the second flow path 5 on the side of the first end face E1 (inlet end face). With this configuration, the second sealing portion seals the end of the second flow path on the inlet end face side, which can prevent the raw material gas from accidentally flowing into the second flow path, thereby ensuring a stable supply of the raw material gas to the first flow path and enabling more efficient production of synthetic fuel gas.
  • the fuel production apparatus 100 has a flow-through type configuration.
  • the fuel production apparatus 100 includes a substrate 3, a second catalyst layer 2, and a first catalyst layer 1.
  • the substrate 3 supports the first catalyst layer 1 and/or the second catalyst layer 2.
  • the cylindrical substrate 3a includes a first flow path 4.
  • the first flow path 4 is a space formed inside the cylindrical substrate 3a.
  • the first flow path 4 is formed in a portion of the cross section of the cylindrical substrate 3a where the first catalyst layer 1 and the second catalyst layer 2 are not formed (typically the central portion).
  • the first flow path 4 extends from the first end face E1 (inlet end face) to the second end face E2 (outlet end face) of the fuel production device.
  • the first flow path 4 has any appropriate shape in a cross section perpendicular to the longitudinal direction.
  • the cross-sectional shape of the first flow path 4 can be the same as that of the cylindrical substrate 3a described above.
  • the cylindrical substrate 3a is configured to be substantially impermeable to synthetic fuel gas.
  • the thickness of the cylindrical substrate 3a is, for example, 0.1 mm to 10 mm, for example, 0.2 mm to 8 mm, or for example, 0.5 mm to 5 mm. The thickness is measured, for example, by observing a cross section with an SEM (scanning electron microscope).
  • the average pore diameter of the cylindrical substrate 3a is, for example, 0.05 ⁇ m to 1000 ⁇ m, and is measured by, for example, mercury intrusion porosimetry.
  • the porosity of the cylindrical substrate 3a is, for example, 0% to 50%. The porosity can be measured by, for example, mercury intrusion porosimetry. If the average pore size and/or porosity of the cylindrical substrate is within this range, the synthetic fuel can be prevented from permeating the cylindrical substrate and leaking out of the first flow passage.
  • the cylindrical substrate 3a is made of any appropriate material, such as a metal material or a ceramic material.
  • metal materials include stainless steel (SUS) and nickel alloys.
  • ceramic materials include cordierite, SiC, Si-SiC composite materials, mullite, alumina, spinel, silicon carbide-cordierite composite materials, lithium aluminum silicate, aluminum titanate, silicon nitride, and zirconia. The ceramic materials may be used alone or in combination.
  • the material of the cylindrical substrate 3a is preferably a ceramic material, more preferably cordierite, SiC, or a Si-SiC composite material, and even more preferably a Si-SiC composite material.
  • the thermal conductivity of the cylindrical substrate 3a is, for example, 0.1 W/mK or more, preferably 0.4 W/mK or more, more preferably 8.0 W/mK or more, and even more preferably 100 W/mK or more.
  • the upper limit of the thermal conductivity of the cylindrical substrate 3a is typically 500 W/mK.
  • the second catalyst layer 2 is provided on the inner surface of the cylindrical substrate 3a.
  • the second catalyst layer 2 may be provided on the entire inner surface of the cylindrical substrate 3a, or on only a portion of it.
  • the second catalyst layer 2 contains a second catalyst capable of promoting the hydrocracking reaction and/or the isomerization reaction of the hydrocarbon compound.
  • the second catalyst include zeolite, silica alumina, silica, alumina, titania, vanadium oxide, and molybdenum oxide.
  • the second catalyst may be used alone or in combination.
  • the second catalyst contains a zeolite.
  • hydrocarbon compounds can be stably hydrocracking and/or isomerized.
  • zeolites examples include ⁇ -type zeolite, ZSM-5-type zeolite, USY-type zeolite, and mordenite-type zeolite, with ⁇ -type zeolite and ZSM-5-type zeolite being preferred.
  • the content of the second catalyst in the second catalyst layer 2 is, for example, 30% to 100% by mass, and preferably 80% to 100% by mass. When the content of the second catalyst is within this range, the hydrocracking and/or isomerization of hydrocarbon compounds can be performed more stably.
  • the thermal conductivity of the second catalyst layer 2 is, for example, 0.01 W/m ⁇ K to 40 W/m ⁇ K, and preferably 0.1 W/m ⁇ K to 40 W/m ⁇ K.
  • the second catalyst layer 2 may contain an additive in addition to the second catalyst.
  • the additive include a filler, a binder, and a sintering inhibitor.
  • the additives may be used alone or in combination.
  • the addition ratio of the additive is, for example, 0 to 70 parts by mass, and preferably 0 to 20 parts by mass, relative to 100 parts by mass of the second catalyst.
  • Such a second catalyst layer 2 can be prepared by any suitable method.
  • methods for preparing the second catalyst layer include a coating method in which the material for the second catalyst layer is applied to a substrate to form the second catalyst layer, and a reaction method in which the second catalyst layer is formed by a reaction such as hydrothermal synthesis.
  • the average pore diameter in the second catalytic layer 2 is, for example, 0.8 ⁇ m to 25 ⁇ m, and preferably 1 ⁇ m to 20 ⁇ m.
  • the porosity in the second catalytic layer 2 is, for example, 30% to 80%, and preferably 30% to 70%.
  • the thickness of the second catalytic layer 2 is, for example, 3 ⁇ m to 200 ⁇ m, and preferably 5 ⁇ m to 100 ⁇ m.
  • the second catalyst layer 2 when the second catalyst layer 2 is prepared by a reaction method, the second catalyst layer 2 is formed as a denser thin film than when prepared by a coating method.
  • the thickness of the second catalyst layer 2 is, for example, 1 ⁇ m to 80 ⁇ m, and preferably 2 ⁇ m to 50 ⁇ m.
  • the first catalytic layer 1 is provided on the surface of the second catalytic layer 2 opposite the cylindrical substrate 3a (substrate 3).
  • the first catalytic layer 1 may be provided on the entire surface of the second catalytic layer 2 opposite the cylindrical substrate 3a, or on a portion of the surface. In the illustrated example, the first catalytic layer 1 is provided on the entire surface of the second catalytic layer 2 opposite the cylindrical substrate 3a. This allows the above-mentioned hydrocarbon compounds to be stably produced from the feed gas.
  • the first catalyst layer 1 contains a first catalyst capable of promoting the FT reaction.
  • the first catalyst typically contains any suitable active component, such as a transition metal, a noble metal, a rare earth metal, an alkali metal, or an alkaline earth metal.
  • the active components may be used alone or in combination.
  • transition metals include Co, Fe, Ni, Ru, Os, Mn, Cu, Ta, Mo, Zn, Cr, Re, V, Zr, and Ir, and preferably Fe, Co, Ni, and Ru.
  • noble metals include Pt, Pd, and Ru.
  • rare earth elements include La and Ce.
  • alkali metals include Li, Na, K, and Rb.
  • alkaline earth metals include Ca, Ba, and Sr.
  • the first catalyst may contain these elements in a metallic state (for example, pure metal, alloy) or in a compound state (for example, oxide, carbide).
  • the first catalyst preferably contains a transition metal, such as Co, Fe, Ni, or Ru, either singly or in combination.
  • the hydrocarbon compounds described above can be produced more stably from the feed gas.
  • the first catalyst contains Co and/or Fe.
  • the activity of the first catalyst can be improved.
  • the activity of the first catalyst can be further improved.
  • the first catalyst may further contain a support.
  • the support is capable of supporting the active component.
  • the support is composed of any suitable inorganic material depending on the application. Examples of inorganic materials include inorganic oxides such as mesoporous materials; carbon materials such as carbon nanotubes and nanoporous carbon; and zeolites. The inorganic materials may be used alone or in combination.
  • the support is composed of an inorganic oxide.
  • inorganic oxides include aluminum oxide, silicon oxide, magnesium oxide, titanium oxide, cerium oxide, zirconium oxide, and composite oxides thereof.
  • aluminum oxide is preferable.
  • the BET specific surface area of such a support is, for example, 10 m 2 /g to 1500 m 2 /g, preferably 30 m 2 /g to 1200 m 2 /g, and more preferably 60 m 2 /g to 1000 m 2 /g. If the BET specific surface area of the support is within this range, the support can support the active component in a sufficiently dispersed state, and the activity of the first catalyst can be further improved.
  • the pore size of the support is, for example, 3 nm to 50 nm, preferably 5 nm to 40 nm, and more preferably 7 nm to 30 nm.
  • the pore volume of the carrier is, for example, 0.1 cc/g to 4 cc/g, preferably 0.2 cc/g to 3.0 cc/g, and more preferably 0.3 cc/g to 2.0 cc/g.
  • the pore volume is measured, for example, by mercury intrusion porosimetry or water titration.
  • the content of the active component in the first catalyst is, for example, 1 to 30 parts by mass, and preferably 5 to 20 parts by mass, per 100 parts by mass of the carrier. If the content of the active component is within this range, the FT reaction can be stably promoted.
  • the first cell 321 includes the first flow path 4 described above.
  • the first cell 321 can be described in the same manner as the cylindrical substrate 3a described above.
  • the second catalyst layer 2 and the first catalyst layer 1 described above are laminated in this order on the inner surface of the first cell 321.
  • the second cell 322 includes the second flow path 5 described above.
  • the second cell 322 can be described similarly to the first cell 321 described above, except that the second cell 322 does not include the first catalyst layer 1 and the second catalyst layer 2.
  • the second flow path 5 is a space formed inside the second cell 322.
  • the second flow path 5 is defined by the inner surface of the second cell 322.
  • the second flow passage 5 extends from a first end face E1 (inlet end face) to a second end face E2 (outlet end face) of the fuel production apparatus.
  • the second flow path 5 has any appropriate shape in a cross section perpendicular to the longitudinal direction.
  • the cross-sectional shape of the second flow path 5 may be the same as that of the first flow path 4 described above.
  • the cross-sectional area of the second flow path 5 may be the same as the cross-sectional area of the first flow path 4 or may be different from the cross-sectional area of the first flow path 4 .
  • the first cell 321 and the second cell 322 are connected to each other so as to share the partition wall 31.
  • the partition wall 31 is located between the first flow path 4 and the second flow path 5. Therefore, the fluid flowing through the fuel production device 101 flows from the first flow path 4 through the partition wall 31 and into the second flow path 5.
  • the partition wall 31 is configured to be substantially permeable to synthetic fuel (typically synthetic fuel gas).
  • the thickness of the partition wall 31 is, for example, 60 ⁇ m to 550 ⁇ m, and preferably 150 ⁇ m to 510 ⁇ m.
  • the average pore diameter in the partition walls 31 is, for example, 5 ⁇ m to 30 ⁇ m, and preferably 8 ⁇ m to 25 ⁇ m.
  • the porosity of the partition walls 31 is, for example, 20% to 75%, and preferably 25% to 70%. If the partition walls have an average pore size and/or porosity within these ranges, synthetic fuel gas can be stably transmitted through them.
  • the continuous cylindrical substrate 3b is typically made of the ceramic material described above.
  • the range of thermal conductivity of the continuous cylindrical substrate 3b is, for example, the same as the range of thermal conductivity of the cylindrical substrate 3a described above.
  • the fuel production device 102 has a wall-flow type configuration.
  • the honeycomb structure 10 included in the fuel production device 102 includes a honeycomb substrate 3c as the substrate 3, in addition to the first catalytic layer 1 and the second catalytic layer 2.
  • the honeycomb substrate 3c includes partition walls 31 that define a plurality of first cells 321 and a plurality of second cells 322.
  • the first cells 321 and second cells 322 provided in the honeycomb substrate 3c can be described, for example, in the same manner as the first cells 321 and second cells 322 provided in the continuous-cylinder substrate 3b described above.
  • the second catalyst layer 2 and the first catalyst layer 1 described above are laminated in this order on the inner surface of each of the multiple first cells 321.
  • the first cells 321 and second cells 322 are arranged arbitrarily and appropriately depending on the application.
  • the first cells 321 and second cells 322 are typically arranged alternately.
  • the honeycomb substrate 3c may have any suitable shape (overall shape). Examples of shapes for the honeycomb substrate 3c include a cylindrical shape with a circular bottom, an elliptical cylindrical shape with an elliptical bottom, a rectangular prism with a polygonal bottom, and a cylindrical shape with an irregular bottom. In one embodiment, the honeycomb substrate 3c has a cylindrical shape. The outer diameter and length of the honeycomb substrate 3c can be appropriately set depending on the purpose.
  • the cell density of the honeycomb substrate 3c is, for example, 150 cpsi or more, preferably 200 cpsi or more, and more preferably 300 cpsi or more, whereas the cell density of the honeycomb substrate 3c is, for example, 1200 cpsi or less, and preferably 900 cpsi or less.
  • “cell density of a honeycomb structure” means the cell density of a cross section in the longitudinal direction (direction in which the cells extend) of the honeycomb structure
  • cpsi means the total number of first cells and second cells per 6.4516 cm 2 (1 square inch) of the cross section.
  • the honeycomb substrate 3c includes an outer wall 33 and a partition wall 31.
  • the outer wall 33 and the partition wall 31 may be formed integrally or as separate bodies.
  • the outer wall 33 and the partition wall 31 are formed integrally.
  • the outer wall 33 has a cylindrical shape.
  • the thickness of the outer wall 33 can be set appropriately depending on the application of the fuel production device.
  • the thickness of the outer wall 33 is, for example, 0.1 mm to 10 mm, or, for example, 0.2 mm to 8 mm, or, for example, 1 mm to 5 mm.
  • the partitions 31 are located inside the outer wall 33.
  • the partitions 31 have first partitions 311 and second partitions 312 that are perpendicular to each other, and the first partitions 311 and second partitions 312 define a plurality of first cells 321 and second cells 322.
  • Examples of the cross-sectional shapes of the first cells 321 and second cells 322 include triangles, rectangles, pentagons, polygons with hexagons or more, circles, and ellipses.
  • the cross-sectional shapes of the first cells 321 and second cells 322 are quadrilaterals except for the portions where the first partitions 311 and second partitions 312 contact the outer wall 33.
  • the configuration of the partitions is not limited to the partitions 31 described above.
  • the partitions may have first partitions extending radially and second partitions extending circumferentially, which define a plurality of cells.
  • the partition wall 31 is configured to be substantially permeable to synthetic fuel gas.
  • the range of thickness of the partition walls 31 of the honeycomb substrate 3c is, for example, the same as the range of thickness of the partition walls 31 of the continuous cylindrical substrate 3b described above.
  • the range of the average pore diameter in the partition walls 31 of the honeycomb substrate 3c is, for example, the same as the range of the average pore diameter in the partition walls 31 of the continuous cylindrical substrate 3b described above.
  • the porosity range of the partition walls 31 of the honeycomb substrate 3c is, for example, the same as the porosity range of the partition walls 31 of the continuous cylindrical substrate 3b described above.
  • the porosity of the partition walls 31 of the honeycomb substrate 3c is preferably 25% to 70%. If the partition walls have an average pore size and/or porosity within these ranges, synthetic fuel gas can be stably transmitted through them.
  • the partition wall 31 is typically made of the above-mentioned ceramic material.
  • the partition walls 31 contain cordierite and/or SiC.
  • the thermal conductivity of the partition walls can be improved.
  • the thermal conductivity of the partition walls can be significantly improved.
  • the thermal conductivity of the partition wall 31 is, for example, 0.1 W/mK or more, preferably 0.4 W/mK or more, and more preferably 8.0 W/mK or more.
  • the upper limit of the thermal conductivity of the partition wall 31 is typically 40 W/mK.
  • the second catalyst layer 2 is laminated on the surface of the partition wall 31 on the side facing the first flow path 4.
  • the first catalyst layer 1 is located on the opposite side of the partition wall 31 from the second catalyst layer 2, and is laminated on the second catalyst layer 2.
  • the first catalyst layer and the second catalyst layer are in direct contact with each other, which can prevent the precipitation of paraffin wax with a carbon number of 20 or more during the production of synthetic fuel, and can prevent the paraffin wax from clogging the first catalyst layer and/or the second catalyst layer.
  • the second sealing portion 7 is made of any appropriate material. Examples of the material for the second sealing portion 7 include the same materials as those for the first sealing portion 6. The materials for the second sealing portion 7 may be used alone or in combination. In the illustrated example, the second sealing portion 7 is fixed to the partition wall 31. The second sealing portion 7 may be formed integrally with the partition wall 31 or may be a separate body from the partition wall 31. In one embodiment, the second sealing portion 7 is formed integrally with the partition wall 31.
  • the fuel production apparatus 100 may include a plurality of first flow paths 4.
  • the substrate 3 has a plurality of cells 32 including the first flow paths 4.
  • Each of the plurality of cells 32 can be described in the same manner as the above-described first cell 321. That is, the above-described second catalyst layer 2 and the above-described first catalyst layer 1 are laminated in this order on the inner surface of each of the plurality of cells 32.
  • n-paraffins have a carbon number of, for example, 1 to 25
  • isoparaffins have a carbon number of, for example, 4 to 20.
  • the raw material gas containing carbon dioxide and hydrogen is supplied to the first flow path 4 of the fuel production device 102 .
  • the carbon dioxide content in the raw material gas is, for example, 20 to 40% by volume, and preferably 22 to 29% by volume.
  • the hydrogen content in the raw material gas is, for example, 60% to 80% by volume, and preferably 71% to 78% by volume.
  • the n-paraffins are hydrocracking and/or isomerized to be converted into isoparaffins.
  • the n-paraffins may be converted into olefins.
  • the carbon numbers of the n-paraffins, isoparaffins, and olefins are, for example, 4 to 15, and preferably 5 to 12.
  • the synthetic fuel is typically produced as a synthetic fuel gas.
  • the content of n-paraffins in the synthetic fuel gas is, for example, less than 80% by volume, preferably 70% by volume or less, while the content of n-paraffins in the synthetic fuel gas is, for example, 0% by volume or more, or, for example, 10% by volume or more.
  • the content of isoparaffins in the synthetic fuel gas is, for example, more than 15% by volume, preferably 20% by volume or more, while the content of isoparaffins in the synthetic fuel gas is, for example, 100% by volume or less, for example, less than 85% by volume, or for example, 80% by volume or less.
  • the olefin content in the synthetic fuel gas is, for example, 0% by volume or more, preferably more than 5% by volume, and preferably 10% by volume or more, while the olefin content in the synthetic fuel gas is, for example, less than 85% by volume, for example, 80% by volume or less, or for example, 70% by volume or less.
  • Such synthetic fuel typically in a gaseous state, flows from the first flow path 4 to the second flow path 5 and is then continuously discharged from the second flow path 5.
  • the first catalyst layer is disposed facing the first flow path, so that the synthetic fuel can be produced with an excellent conversion rate.
  • the carbon oxide conversion rate that can be achieved by the fuel production apparatus is, for example, 65% or more, preferably 70% or more, and more preferably 75% or more, while the upper limit of the carbon oxide conversion rate is 100%.
  • Example 1 Preparation of honeycomb substrate>> 80 parts by mass of SiC raw material powder and 20 parts by mass of metal Si powder were extruded into a clay, dried, calcined at 550°C for 3 hours in an oxidizing atmosphere, and then fired at 1450°C for 2 hours in a non-oxidizing atmosphere, thereby preparing a honeycomb substrate.
  • the honeycomb substrate had partition walls defining a plurality of first cells and a plurality of second cells, and an outer wall surrounding the partition walls. The cross-sectional shape of the cells was rectangular.
  • the honeycomb substrate had a cell density of 300 cpsi and a partition wall thickness of 0.254 mm.
  • the honeycomb substrate was composed of a porous body of a Si-SiC composite material.
  • the partition walls in the honeycomb substrate had a thickness of 0.254 mm, an average pore diameter of 28 ⁇ m, and a porosity of 63%.
  • the thermal conductivity of the honeycomb substrate is shown in Table 1. Furthermore, the honeycomb substrate was provided with a plurality of first plugs and a plurality of second plugs, wherein the first plugs plugged the ends of the first cells on the second end face side, and the second plugs plugged the ends of the second cells on the first end face side.
  • Second Catalyst Layer ⁇ Preparation of Second Catalyst Layer>>
  • HZSM-5 zeolite, manufactured by Nakamura Choukou Co., Ltd.
  • the obtained second catalyst particles were dispersed in distilled water to prepare a second catalyst slurry.
  • the catalyst particle content in the second catalyst slurry was 10 mass%.
  • the second catalyst slurry was flowed into a plurality of first cells provided in the honeycomb substrate prepared above under normal pressure (0.1 MPa) and room temperature (23°C). This resulted in the second catalyst slurry being applied to the surfaces of the partition walls.
  • the first catalyst slurry applied to the surfaces of the partition walls was then heated and dried at 100°C for 120 minutes. The above application and drying were repeated to form a second catalyst layer on the surfaces of the partition walls.
  • the second catalyst layer contained aggregates of the second catalyst particles.
  • the thickness of the second catalyst layer was 80 ⁇ m.
  • the amount of the second catalyst particles supported per unit area of the partition walls was 0.011 g/ cm2 .
  • Silicon (IV) dioxide particles were introduced into distilled water and then stirred under reduced pressure at room temperature (23°C) for 12 hours. This resulted in a dispersion of metal oxide particles. Furthermore, cobalt (II) nitrate hexahydrate was dissolved in distilled water to obtain an aqueous cobalt nitrate solution. Next, the aqueous cobalt nitrate solution was added to the dispersion of metal oxide particles and stirred at room temperature (23°C) for 2 hours. The mixture of the dispersion and the aqueous solution was then heated to 80°C while stirring to evaporate the water. The remaining solid was then heated at 500°C for 3 hours.
  • the first catalyst particles contained tricobalt tetroxide ( Co3O4 ) and silicon (IV) dioxide supporting tricobalt tetroxide ( Co3O4 ).
  • the first catalyst particles had a Co content of 20 parts by mass per 100 parts by mass of silicon dioxide.
  • the obtained first catalyst particles were dispersed in distilled water to prepare a first catalyst slurry.
  • the catalyst particle content in the first catalyst slurry was 10 mass%.
  • the first catalyst slurry was flowed into the first cell in which the second catalyst layer was formed at normal pressure (0.1 MPa) and room temperature (23°C). This resulted in the second catalyst slurry being applied to the surface of the second catalyst layer.
  • the first catalyst slurry applied to the surface of the second catalyst layer was then heated and dried at 100°C for 120 minutes. The above application and drying were repeated to form a first catalyst layer on the surface of the second catalyst layer.
  • the first catalyst layer contained aggregates of the first catalyst particles.
  • the thickness of the first catalyst layer was 150 ⁇ m.
  • the amount of the first catalyst particles supported per unit area of the partition wall was 0.011 g/ cm2 .
  • the fuel production apparatus shown in FIG. 5 was manufactured, which was equipped with a honeycomb substrate, a first catalyst layer, and a second catalyst layer.
  • Example 2 The fuel production apparatus shown in FIG. 5 was manufactured in the same manner as in Example 1, except that SiO 2 particles were further added as a filler to each of the first catalyst slurry and the second catalyst slurry.
  • the addition rate of SiO 2 particles in the first catalyst slurry was 20 parts by mass relative to 100 parts by mass of the first catalyst, and the addition rate of SiO 2 particles in the second catalyst slurry was 20 parts by mass relative to 100 parts by mass of the second catalyst.
  • the thermal conductivity of the SiO2 particles was 1.38 W/m ⁇ K, the average particle size of the SiO2 particles was 20 nm, and the aspect ratio of the SiO2 particles was 1.0.
  • Example 3 A fuel production apparatus shown in FIG. 5 was produced in the same manner as in Example 1, except that ⁇ -Al 2 O 3 particles were further added as a filler to each of the first catalyst slurry and the second catalyst slurry.
  • the addition rate of ⁇ -Al 2 O 3 particles in the first catalyst slurry was 20 parts by mass relative to 100 parts by mass of the first catalyst, and the addition rate of ⁇ -Al 2 O 3 particles in the second catalyst slurry was 20 parts by mass relative to 100 parts by mass of the second catalyst.
  • the thermal conductivity of the ⁇ -Al 2 O 3 particles was 30 W/m ⁇ K, the average particle size of the ⁇ -Al 2 O 3 particles was 400 nm, and the aspect ratio of the ⁇ -Al 2 O 3 particles was 10.
  • Example 4 Preparation of honeycomb substrate>> A honeycomb substrate was prepared in the same manner as in Example 1.
  • a first catalyst slurry was prepared by dispersing triiron tetroxide (Fe 3 O 4 ) particles as a first catalyst in distilled water.
  • the catalyst particle content in the first catalyst slurry was 10 mass%.
  • the first catalyst slurry was flowed into a plurality of first cells provided in the honeycomb substrate prepared above under atmospheric pressure (0.1 MPa) and room temperature (23°C). This resulted in the first catalyst slurry being applied to the surfaces of the partition walls.
  • the first catalyst slurry applied to the surfaces of the partition walls was then heated and dried at 100°C for 120 minutes. The above application and drying were repeated to form a first catalyst layer on the surfaces of the partition walls.
  • the thickness of the first catalyst layer was 40 ⁇ m.
  • the amount of first catalyst particles supported per unit area of the partition walls was 0.011 g/cm 2 .
  • Second Catalyst Layer ⁇ Preparation of Second Catalyst Layer>>
  • HZSM-5 zeolite, manufactured by Nakamura Choukou Co., Ltd.
  • the obtained second catalyst particles were dispersed in distilled water to prepare a second catalyst slurry.
  • the catalyst particle content in the second catalyst slurry was 10 mass%.
  • the second catalyst slurry was flowed into a plurality of second cells provided in the honeycomb substrate prepared above under normal pressure (0.1 MPa) and room temperature (23°C). This resulted in the second catalyst slurry being applied to the second flow path side surfaces of the partition walls.
  • the second catalyst slurry applied to the partition wall surfaces was then heated and dried at 100°C for 120 minutes. The above application and drying were repeated to form a second catalyst layer on the partition wall surfaces.
  • the thickness of the second catalyst layer was 80 ⁇ m.
  • the amount of second catalyst particles supported per unit area of the partition wall was 0.011 g/ cm2 . In this manner, the fuel production device shown in FIG. 6 was manufactured.
  • Example 5 A fuel production apparatus shown in FIG. 6 was produced in the same manner as in Example 4, except that the first catalyst slurry containing triiron tetroxide particles was changed to the first catalyst slurry used in Example 1.
  • Example 6 Except for changing the clay containing the SiC raw material powder and the metal Si powder to a clay containing cordierite (Cd), the fuel production apparatus shown in Fig. 5 was manufactured in the same manner as in Example 1.
  • the partition wall thickness was 0.254 mm
  • the average pore diameter of the partition walls was 11 ⁇ m
  • the porosity of the partition walls was 52%.
  • Example 7 Except for changing the clay containing the SiC raw material powder and the metal Si powder to a clay containing cordierite (Cd), the fuel production apparatus shown in Fig. 6 was manufactured in the same manner as in Example 5.
  • the partition wall thickness was 0.254 mm
  • the average pore diameter of the partition walls was 11 ⁇ m
  • the porosity of the partition walls was 52%.
  • Example 8 A honeycomb substrate provided with partition walls functioning as a second catalyst layer was prepared in the same manner as in Example 1, except that the clay containing the SiC raw material powder and the metal Si powder was changed to a clay containing HZSM-5 (zeolite, manufactured by Nakamura Choukou Co., Ltd.) as a second catalyst.
  • the thickness of the partition walls was 0.254 mm
  • the average pore diameter of the partition walls was 3 ⁇ m
  • the porosity of the partition walls was 40%.
  • a first catalyst slurry prepared in the same manner as in Example 1 was flowed into the multiple first cells of the honeycomb substrate prepared above at normal pressure (0.1 MPa) and room temperature (23°C).
  • first catalyst slurry being applied to the surfaces of the partition walls (second catalyst layer).
  • the first catalyst slurry applied to the surfaces of the partition walls was then heated and dried at 100°C for 120 minutes. The above application and drying were repeated to form a first catalyst layer on the surfaces of the partition walls.
  • the thickness of the first catalyst layer was 80 ⁇ m.
  • the amount of first catalyst particles supported per unit area of the partition walls was 0.011 g/ cm2 . In this manner, the fuel production device shown in FIG. 7 was manufactured.
  • ⁇ -zeolite-Co/Al 2 O 3 catalyst was prepared in the same manner as in Example 1 described in JP 2017-144426 A.
  • the catalyst had a core-shell structure with Co/Al 2 O 3 as the core and a ⁇ -zeolite membrane as the shell.
  • Quartz wool was placed on the top and bottom of the reaction tube, and the obtained ⁇ zeolite-Co/Al 2 O 3 catalyst was packed between the quartz wool in an amount equal to that in Example 1.
  • a fuel production device was manufactured in which the catalyst having a core-shell structure was filled in the gas flow passage.
  • ⁇ Synthetic fuel production test> The fuel production apparatus obtained in the examples and comparative examples was inserted into a reaction tube with an inner diameter of 21 mm. As a pretreatment for the reaction, the fuel production apparatus was heated to 240°C using an electric furnace installed around the outer periphery of the reaction tube, and hydrogen gas was introduced into the reaction tube to reduce the first catalyst. Next, nitrogen gas was passed through the reaction tube to lower the temperature of the electric furnace to 200°C, and then a feed gas containing 33 mol% carbon monoxide and 66 mol% hydrogen was introduced into the reaction tube at a space velocity SV of 1018 h -1 .
  • the raw material gas was supplied to the first flow path provided in the fuel production apparatus, and the synthetic fuel gas flowed out from the reaction tube.
  • the internal pressure of the first flow path was 1 MPa.
  • the composition of the synthetic fuel gas flowing out of the reaction tube after the heating of the electric furnace was stopped was measured using a gas chromatograph-thermal conductivity detector (GC-TCD).
  • C20+selectivity (%) (total amount (volume %) of hydrocarbon compounds exceeding C20 contained in synthetic fuel gas/total amount (volume %) of hydrocarbon compounds and carbon oxides contained in synthetic fuel gas) ⁇ 100 (E)
  • the isoparaffin selectivity (%) was calculated by the following formula (F).
  • Isoparaffin selectivity (%) (total amount of isoparaffin compounds contained in synthetic fuel gas (volume %)/total amount of hydrocarbon compounds and carbon oxides contained in synthetic fuel gas (volume %)) ⁇ 100 (F)
  • the olefin selectivity (%) was calculated by the following formula (G).
  • Olefin selectivity (%) (total amount (volume %) of olefin compounds contained in synthetic fuel gas/total amount (volume %) of hydrocarbon compounds and carbon oxides contained in synthetic fuel gas) ⁇ 100 (G)
  • the C5 to C20 yield (%) was calculated using the following formula (H).
  • C5 to C20 yield (%) (CO conversion (%) (A)) ⁇ (C5 to C20 selectivity (%) (D)) ⁇ 100 (H)
  • the isoparaffin yield (%) was calculated using the following formula (I).
  • Isoparaffin yield (%) (CO conversion (%)(A)) ⁇ (isoparaffin selectivity (%)(F)) ⁇ 100 (I)
  • the olefin yield (%) was calculated by the following formula (J).
  • Olefin yield (%) (CO conversion (%) (A)) ⁇ (olefin selectivity (%) (G)) ⁇ 100 (J)
  • the results are shown in Table 1.

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Abstract

Est proposé un dispositif de production de combustible qui peut améliorer le taux de conversion d'oxyde de carbone et produire efficacement un combustible synthétique. Le dispositif de production de combustible selon un mode de réalisation de la présente invention présente un premier chemin d'écoulement. Un gaz de matière première contenant de l'oxyde de carbone et de l'hydrogène est fourni au premier chemin d'écoulement. Le dispositif de production de combustible comprend une première couche de catalyseur et une seconde couche de catalyseur. La première couche de catalyseur est disposée en regard du premier chemin d'écoulement. La première couche de catalyseur comprend un premier catalyseur pouvant favoriser une réaction de Fischer-Tropsch. La seconde couche de catalyseur est positionnée sur le côté opposé de la première couche de catalyseur par rapport au premier chemin d'écoulement. La seconde couche de catalyseur comprend un second catalyseur pouvant favoriser la réaction d'hydrocraquage et/ou la réaction d'isomérisation de composés hydrocarbonés produits par la réaction de Fischer-Tropsch.
PCT/JP2025/012751 2024-03-29 2025-03-28 Dispositif de production de combustible Pending WO2025206304A1 (fr)

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Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS6138627A (ja) * 1984-07-31 1986-02-24 Hitachi Ltd 高温で安定な燃焼触媒及びその調製法ならびにその触媒を用いて化学反応を実施する方法
JP2000351608A (ja) * 1999-06-11 2000-12-19 Matsushita Electric Ind Co Ltd 水素精製装置
US6211255B1 (en) * 1997-02-28 2001-04-03 Den Norske Stats Oljeselskap A.S. Fischer-tropsch synthesis
JP2012514658A (ja) * 2008-10-10 2012-06-28 ヴェロシス，インク． マイクロチャネルプロセス技術を使用するプロセスおよび装置
JP2017144426A (ja) * 2016-02-15 2017-08-24 新日鐵住金株式会社 合成ガスから炭化水素を製造するための触媒、合成ガスから炭化水素を製造するための触媒の製造方法、及び炭化水素の製造方法
JP2018083186A (ja) * 2016-11-25 2018-05-31 小林　博 触媒作用をもたらす塗料の製造と触媒作用を発揮する積層体の形成
WO2024024142A1 (fr) * 2022-07-29 2024-02-01 株式会社日立製作所 Dispositif et procédé de production d'hydrocarbures

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS6138627A (ja) * 1984-07-31 1986-02-24 Hitachi Ltd 高温で安定な燃焼触媒及びその調製法ならびにその触媒を用いて化学反応を実施する方法
US6211255B1 (en) * 1997-02-28 2001-04-03 Den Norske Stats Oljeselskap A.S. Fischer-tropsch synthesis
JP2000351608A (ja) * 1999-06-11 2000-12-19 Matsushita Electric Ind Co Ltd 水素精製装置
JP2012514658A (ja) * 2008-10-10 2012-06-28 ヴェロシス，インク． マイクロチャネルプロセス技術を使用するプロセスおよび装置
JP2017144426A (ja) * 2016-02-15 2017-08-24 新日鐵住金株式会社 合成ガスから炭化水素を製造するための触媒、合成ガスから炭化水素を製造するための触媒の製造方法、及び炭化水素の製造方法
JP2018083186A (ja) * 2016-11-25 2018-05-31 小林　博 触媒作用をもたらす塗料の製造と触媒作用を発揮する積層体の形成
WO2024024142A1 (fr) * 2022-07-29 2024-02-01 株式会社日立製作所 Dispositif et procédé de production d'hydrocarbures

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