Flow synthesis reaction device

Abstract

Provided is a flow synthesis reaction device with which it is possible to improve the yield of a target compound. A flow synthesis reaction device according to one embodiment comprises a honeycomb substrate, a filter, and an end member. The honeycomb substrate has a first end surface and a second end surface in a prescribed direction. The filter is disposed so as to face the first end surface. The end member is affixed to an end of the honeycomb substrate so as to cover the filter. Each of a plurality of cells of the honeycomb substrate includes a flow path through which a fluid can pass. The end member has a supply port and a plurality of grooves. The plurality of grooves are provided in a facing surface of the end member, said surface facing the filter. When viewed from the direction in which the honeycomb substrate extends, the plurality of grooves intersect one another at a position overlapping with the supply port and overlap all of the flow paths included in the plurality of cells.

Description

Flow synthesis reactor

[0001] This invention relates to a flow synthesis reactor.

[0002] Conventionally, flow reactions have attracted attention because they offer superior energy productivity and reduce waste compared to batch reactions. As a reactor applicable to such flow reactions, for example, a reactor has been proposed that comprises a porous body having multiple flow channels, the flow channels separated by porous walls containing a reaction catalyst, and a solution supply unit that supplies a solution containing a gas-phase reactant and a liquid-phase reactant to the porous body (see Patent Document 1).

[0003] Japanese Patent Publication No. 2020-040022

[0004] In recent years, flow precision synthesis, which involves combining multiple flow reactions to synthesize structurally complex organic compounds, has been investigated. In such flow precision synthesis, each flow reaction is carried out under various reaction conditions (e.g., fluid velocity, temperature, pressure) depending on the target product. However, in the reaction apparatus described in Patent Document 1, the yield of the target compound may be insufficient depending on the reaction conditions. The main object of the present invention is to provide a flow synthesis reaction apparatus that can improve the yield of the target compound.

[0005] [1] A flow synthesis reactor according to one embodiment of the present invention comprises a honeycomb substrate, a filter, and an end member. The honeycomb substrate extends in a predetermined direction. The honeycomb substrate has a first end face and a second end face in the predetermined direction. The filter is positioned opposite the first end face. The end member is fixed to the end of the honeycomb substrate so as to cover the filter. The honeycomb substrate has a plurality of cells. Each of the plurality of cells extends from the first end face to the second end face of the honeycomb substrate. Each of the plurality of cells contains a flow path through which a fluid can pass. The end member has a supply port and a plurality of grooves. A fluid is supplied to the supply port. The supply port penetrates the end member in the direction in which the honeycomb substrate extends. The plurality of grooves are provided on the opposing surface of the end member that faces the filter. The plurality of grooves intersect each other at a position that overlaps with the supply port when viewed from the direction in which the honeycomb substrate extends, and overlap with all of the flow paths contained in the plurality of cells. [2] In the flow synthesis reactor described in [1] above, the dimensions of the filter in the direction in which the honeycomb substrate extends may be 1 mm to 10 mm. [3] In the flow synthesis reactor described in [1] or [2] above, each of the plurality of grooves may extend linearly. In addition, each of the plurality of cells may have a rectangular shape in cross-section in a direction perpendicular to the direction in which the honeycomb substrate extends. In this case, the width of each of the plurality of grooves is smaller than the dimension of the longest side of the cross-sectional shape of each of the plurality of cells.

[0006] According to embodiments of the present invention, a flow synthesis reactor capable of improving the yield of the target compound can be realized.

[0007] Figure 1 is a schematic diagram of a flow synthesis reactor according to one embodiment of the present invention. Figure 2 is a schematic bottom view of the first end member of the flow synthesis reactor of Figure 1. Figure 3 is a schematic perspective view of the honeycomb substrate of the flow synthesis reactor of Figure 1. Figure 4 is a schematic perspective view of the honeycomb substrate of the flow synthesis reactor according to another embodiment of the present invention. Figure 5 is a schematic bottom view of the filter of the flow synthesis reactor of Figure 1. Figure 6 is a schematic bottom view of the first end member applied to the honeycomb substrate of Figure 4. Figure 7 is a schematic diagram of a flow synthesis reactor according to yet another embodiment of the present invention.

[0008] Embodiments of the present invention will be described below with reference to the drawings, but the present invention is not limited to these embodiments. Furthermore, in order to clarify the explanation, the drawings may schematically represent the width, thickness, shape, etc., of each part compared to the embodiments; however, these are merely examples and do not limit the interpretation of the present invention.

[0009] A. Flow Synthesis Reactor Figure 1 is a schematic diagram of a flow synthesis reactor according to one embodiment of the present invention; Figure 2 is a schematic bottom view of the first end member of the flow synthesis reactor in Figure 1; and Figure 3 is a schematic perspective view of the honeycomb substrate of the flow synthesis reactor in Figure 1. In Figure 2, for convenience, the cells of the honeycomb substrate are shown with dotted lines.

[0010] As shown in Figure 1, a flow synthesis reactor 100 according to one embodiment of the present invention comprises a honeycomb substrate 1, a filter 2, and a first end member 3 as an end member. The honeycomb substrate 1 extends in a predetermined direction. The honeycomb substrate 1 has a first end face E1 (inlet end face) and a second end face E2 (outlet end face) in the direction of extension. The second end face E2 is located away from the first end face E1 in the direction of extension of the honeycomb substrate 1. The honeycomb substrate 1 has a plurality of cells 12. Each of the plurality of cells 12 extends from the first end face E1 to the second end face E2 of the honeycomb substrate 1. Each of the plurality of cells 12 includes a flow channel 14 through which a fluid can pass. The flow channel 14 is typically filled with any suitable catalyst depending on the application. The filter 2 is positioned facing the first end face E1 of the honeycomb substrate 1. The filter 2 is through which a fluid can pass. The first end member 3 is fixed to the end of the honeycomb substrate 1 so as to cover the filter 2. The first end member 3 has a supply port 32 and a plurality of grooves 31. Fluid is supplied from the outside through the supply port 32. The supply port 32 penetrates the first end member 3 in the direction in which the honeycomb substrate 1 extends. The plurality of grooves 31 are provided on the opposing surface 3a of the first end member 3 that faces the filter 2. As shown in Figure 2, the plurality of grooves 31 intersect each other at a position that overlaps with the supply port 32 when viewed from the direction in which the honeycomb substrate 1 extends, and overlap with all of the flow paths 14 that contain the plurality of cells 12. The inventors have discovered that when the flow velocity of the fluid supplied to the flow synthesis reactor is small (for example, 1.0 ml / min or less when the inner diameter of the flow path is 10 mm), the supply of fluid to the plurality of flow paths contained in the honeycomb substrate becomes unstable in the conventional configuration, and the amount of fluid passing through the plurality of flow paths may vary. Therefore, after diligently studying the supply of fluid to the flow channels, we found that by placing a filter on the end face of the honeycomb substrate and forming multiple grooves in the end members, it is possible to stably supply fluid to multiple flow channels.Specifically, the first end member is fixed to the end of the honeycomb substrate so as to cover the filter, and the multiple grooves provided in the first end member intersect each other at a position that overlaps with the supply port when viewed from the direction in which the honeycomb substrate extends, and overlap with all of the flow paths contained in the multiple cells. Therefore, when a fluid containing any appropriate raw material component is supplied to the supply port, the fluid flows into the multiple grooves, flows along the multiple grooves, and passes through the filter. As a result, even if the flow velocity of the fluid supplied to the supply port is small (for example, 1.0 ml / min or less when the inner diameter of the flow path is 10 mm), the fluid can be sufficiently supplied to the multiple flow paths, and variations in the amount of fluid passing through the multiple flow paths can be suppressed. This makes it possible to utilize the entire catalyst packed in the multiple flow paths and improve the uniformity of the heat distribution in the flow synthesis reactor. This allows the desired chemical reaction to proceed smoothly in each of the multiple flow paths, and improves the yield of the target compound in the flow synthesis reactor. Examples of fluids supplied to the flow synthesis reactor include liquids, gases, and mixtures of liquids and gases.

[0011] A-1. Honeycomb Substrate As shown in Figure 3, the honeycomb substrate 1 has any suitable shape (overall shape). Examples of shapes for the honeycomb substrate 1 include a cylindrical shape with a circular base, an elliptical columnar shape with an elliptical base, a prismatic columnar shape with a polygonal base, and a columnar shape with an irregular base. In one embodiment, the honeycomb substrate 1 has a prismatic shape. In the illustrated example, the base of the honeycomb substrate 1 has a square shape. The outer diameter and length of the honeycomb substrate 1 can be appropriately set according to the purpose. The length (dimension in the extending direction) of the honeycomb substrate 1 is, for example, 50 mm to 300 mm.

[0012] In the illustrated example, the honeycomb substrate 1 comprises an outer wall 13 and a partition wall 11 located inside the outer wall 13. The outer wall 13 and the partition wall 11 may be formed integrally or as separate components. In the illustrated example, the outer wall 13 and the partition wall 11 are formed integrally.

[0013] The outer wall 13 has a rectangular tubular shape. The thickness of the outer wall 13 is set arbitrarily and appropriately. The thickness of the outer wall 13 is, for example, 1 mm to 10 mm, and preferably 3 mm.

[0014] The partition wall 11 defines a plurality of cells 12. The cells 12 have any suitable shape in a cross-section perpendicular to the longitudinal direction of the honeycomb substrate 1. Examples of cell cross-sectional shapes include triangles, squares, pentagons, polygons with hexagons or more, circles, and ellipses. The cross-sectional shapes and sizes of the cells may all be the same, or at least some may differ. Among such cell cross-sectional shapes, squares are preferred, and more preferably squares or rectangles. When a cell has a square cross-sectional shape, the dimension of one side of the cell is, for example, 0.1 cm to 0.5 cm, and preferably 0.2 cm to 0.4 cm.

[0015] In the illustrated example, the inner surface of cell 12 defines the flow path 14. The flow path 14 is a space formed inside cell 12 and extends from the first end face E1 (inlet end face) to the second end face E2 (outlet end face), similar to cell 12 (see Figure 1). The flow path 14 has any suitable shape in a cross-section perpendicular to the length direction of the honeycomb substrate 1. The cross-sectional shape of the flow path 14 can be the same as that of cell 12 described above, preferably a quadrilateral, and more preferably a square or rectangle. The cross-sectional shape and size of the flow paths 14 may all be the same, or at least some may differ. The cross-sectional area of ​​each of the multiple flow paths is, for example, 0.01 cm². ２ ~0.25cm ２ Preferably 0.04 cm ２ ~0.16cm ２ That is the case.

[0016] The cell density in the honeycomb substrate 1 is, for example, 50 cpsi to 900 cpsi, preferably 50 cpsi to 300 cpsi. When the cell density is within this range, the fluid can be stably supplied to the flow channels containing the cells in the flow synthesis reactor. In this specification, "cell density of the honeycomb substrate" refers to the cell density in a cross-section perpendicular to the longitudinal direction (the direction in which the cells extend) of the honeycomb substrate, and "cpsi" refers to the 6.4516 cm² of the said cross-section. ２ This refers to the number of cells per square inch.

[0017] In the illustrated example, the partition wall 11 has a first partition wall 11a and a second partition wall 11b that are orthogonal to each other, and the first partition wall 11a and the second partition wall 11b define a plurality of cells 12. However, the configuration of the partition wall is not limited to the partition wall 11 described above. The partition wall may have a first partition wall extending in the radial direction and a second partition wall extending in the circumferential direction, and these may define a plurality of cells.

[0018] The thickness of the partition wall 11 can be set arbitrarily and appropriately. Typically, the thickness of the partition wall 11 is thinner than the thickness of the outer wall 13. The thickness of the partition wall 11 is, for example, 0.15 mm to 0.50 mm, and preferably 0.20 mm to 0.50 mm. The thickness of the partition wall is measured, for example, by cross-sectional observation using an SEM (scanning electron microscope).

[0019] The porosity of the partition wall 11 can be appropriately set depending on the purpose. For example, the porosity of the partition wall 11 is 50% or less, preferably 40% or less. On the other hand, the porosity of the partition wall 11 is, for example, 0% or more, and also, for example, 5% or more. The porosity is measured, for example, by the mercury intrusion method.

[0020] The partition wall 11 may or may not have pores. If the partition wall 11 has multiple pores, the average pore diameter in the partition wall 11 is, for example, 0.4 μm or more, preferably 1.0 μm or more. On the other hand, the average pore diameter in the partition wall 11 is, for example, 18 μm or less, preferably 12 μm or less. The average pore diameter is measured, for example, by the mercury intrusion method.

[0021] The density of the partition walls 11 can be appropriately set depending on the purpose. The density of the partition walls 11 is, for example, 0.32 g / cm ３ to 0.80 g / cm ３ , and preferably 0.32 g / cm ３ to 0.59 g / cm ３ . The density is measured, for example, by mercury porosimetry.

[0022] As shown in FIG. 4, in another embodiment, the honeycomb substrate 1 has a cylindrical shape. The honeycomb substrate 1 having a cylindrical shape is described in the same manner as the honeycomb substrate 1 having a prismatic shape described above, except for the outer shape. Therefore, the description of the honeycomb substrate having a cylindrical shape is omitted as appropriate. The honeycomb substrate 1 having a cylindrical shape includes an outer wall 13 and partition walls 11. The outer wall 13 has a cylindrical shape. The partition walls 11 include first partition walls 11a and second partition walls 11b, and define a plurality of cells 12. In the illustrated example, the cross-sectional shape of the cells 12 is quadrangular, except for portions where the first partition walls 11a and the second partition walls 11b are in contact with the outer wall 13.

[0023] Examples of materials constituting the honeycomb substrate 1 include ceramic materials. Specific examples of ceramic materials include zirconia-based materials, alumina-titanium carbide-based composite materials, Si-SiC-based composite materials, aluminum nitride, aluminum oxide, silicon nitride, silicon carbide, zirconia, cordierite, and mullite. These ceramic materials may be used alone or in combination. Among these ceramic materials, Si-SiC-based composite materials are preferable. Specific examples of Si-SiC-based composite materials include Si-impregnated SiC, Si-impregnated Si-SiC, (Si+Al)-impregnated SiC, metal-composite SiC, and recrystallized SiC. These Si-SiC-based composite materials are described, for example, in Japanese Patent Application Laid-Open No. 2024-131748. The entire content of this publication is incorporated herein by reference.

[0024] The thermal conductivity of such a honeycomb substrate 1 at 25°C is, for example, 20 W / m·K or more, preferably 30 W / m·K or more, more preferably 100 W / m·K or more, even more preferably 150 W / m·K or more, and particularly preferably 180 W / m·K or more. As long as the thermal conductivity of the honeycomb substrate (each of the partition walls and outer walls) is above this lower limit, the reaction can proceed stably. On the other hand, the upper limit of the thermal conductivity of the honeycomb substrate 1 is typically 300 W / m·K. The thermal conductivity is measured, for example, in accordance with JIS R1611.

[0025] As described above, the multiple channels 14 provided in the honeycomb substrate 1 are filled with a catalyst. The catalyst is arbitrarily and appropriately selected according to the organic synthesis reaction carried out in the flow synthesis reactor 100. The catalyst contains an active component that includes a metal element (e.g., a noble metal element, a transition metal element). The active component may include a metal element in a metallic state, a salt of a metal element, or an oxide of a metal element. In addition to the active component, the catalyst may further contain a carrier that supports the active component (e.g., carbon, an oxide). Examples of catalysts include palladium catalysts, platinum catalysts, rhodium catalysts, ruthenium catalysts, iridium catalysts, nickel catalysts, and cobalt catalysts. Examples of catalyst shapes include particulate, bulk, pelletized, and monolithic forms. The amount of active component of the catalyst packed into the channel 14 is, for example, 0.5% to 1.0%, preferably 0.7% to 0.8%, when the internal volume of the channel is considered to be 100%. Each of the multiple channels 14 may be further filled with a buffer material as needed. Examples of the filler material include Celite and the ceramic materials mentioned above. The filler material can be used alone or in combination. The total amount of catalyst and filler material packed into the flow path 14 is, for example, 50% to 80%, preferably 70% to 80%, when the internal volume of the flow path is considered to be 100%.

[0026] A-2. Filter As shown in Figure 1, in one embodiment, the filter 2 is in contact with the first end face E1 of the honeycomb substrate 1. In the illustrated example, the flow synthesis reactor 100 further includes a filter 2 in contact with the second end face E2 of the honeycomb substrate 1, in addition to the filter 2 in contact with the first end face E1 of the honeycomb substrate 1. Hereinafter, the filter 2 in contact with the first end face E1 of the honeycomb substrate 1 may be referred to as the first filter 2a, and the filter 2 in contact with the second end face E2 of the honeycomb substrate 1 may be referred to as the second filter 2b. If the flow synthesis reactor is equipped with a second filter, it is possible to suppress the outflow of catalyst from the flow path.

[0027] The filters 2 (the first filter 2a and the second filter 2b, respectively) typically have a plate shape with thickness in the direction in which the honeycomb substrate 1 extends.

[0028] In one embodiment, the filter 2 has the same shape and size as the first end face E1 of the honeycomb substrate 1 when viewed from the direction in which the honeycomb substrate 1 extends. As shown in Figure 5, when the honeycomb substrate 1 has a prismatic shape (see Figure 3), the filter 2 preferably has a polygonal shape when viewed from the thickness direction. In the illustrated example, the filter 2 has a square shape.

[0029] The corners of the polygonal filter 2 may have vertices or may be chamfered in a curved shape. In one embodiment, the corners of the polygonal filter 2 are chamfered in a curved shape. Chamfering the corners of the filter can reduce catalyst leakage from the discharge port, which will be described later. The radius of curvature of the chamfered portion of the filter 2 is, for example, 5 mm to 30 mm, preferably 10 mm to 30 mm. Also, as shown in Figure 6, when the honeycomb substrate 1 has a cylindrical shape (see Figure 4), the filter 2 preferably has a circular shape when viewed from the thickness direction.

[0030] The thickness of filter 2 (the dimension in the direction in which the honeycomb substrate extends) is, for example, 1.0 mm or more, preferably 1.5 mm or more, more preferably 2.0 mm or more, and even more preferably 3.0 mm or more. On the other hand, the thickness of filter 2 is, for example, 10.0 mm or less, preferably 5.0 mm or less. When the filter thickness is within this range, the fluid can be stably supplied to multiple flow paths.

[0031] Filter 2 is typically composed of a porous material having continuous pores. The average pore diameter in filter 2 is, for example, 1 μm or more, preferably 5 μm or more, and more preferably 10 μm or more. On the other hand, the average pore diameter in filter 2 is, for example, 50 μm or less, and preferably 30 μm or less. The porosity of filter 2 is, for example, 35% to 60%, and preferably 35% to 40%.

[0032] The pore size of the filter 2 may be substantially uniform throughout the filter 2, or it may vary in parts within the filter 2. As shown in Figures 5 and 6, in one embodiment, the filter 2 has portions with different average pore sizes. In the illustrated example, the filter 2 integrally has a central portion 21 and a peripheral portion 22 with different average pore sizes. The central portion 21 includes the center of the filter 2. The peripheral portion 22 surrounds the central portion 21 when viewed from the thickness direction of the filter 2. The average pore size in the central portion 21 may be smaller than or larger than the average pore size in the peripheral portion 22. The average pore size in the central portion 21 is, for example, 1 μm to 80 μm, preferably 20 μm to 60 μm. The volume percentage of the central portion 21 in the filter 2 is, for example, 15% to 35%, preferably 15% to 25%. The average pore size in the peripheral portion 22 is, for example, 5 μm to 70 μm, preferably 10 μm to 50 μm. The volume percentage of the peripheral portion 22 in the filter 2 is, for example, 65% to 85%, preferably 75% to 85%.

[0033] The filter 2 is made of any appropriate material. Typical examples of the material for the filter 2 include resin materials. Specific examples of the resin materials include: fluorine-based resins such as polytetrafluoroethylene (PTFE); polyolefin-based resins such as polyethylene and polypropylene; aromatic polyether ketone-based resins such as polyether ether ketone (PEEK); polyphenylene sulfide (PPS); and elastomers. The materials of the filter 2 may be used alone or in combination.

[0034] In one embodiment, the filter 2 is made of a fluorine-based resin. The fluorine-based resin preferably comprises PTFE.

[0035] A-3. First End Member The first end member 3 is made of any appropriate material. Examples of the material for the first end member 3 include SUS materials and the same resin materials as those for the filter 2; aromatic polyether ketone-based resins are preferred, and PEEK is more preferred. As shown in FIG. 1, in one embodiment, the first end member 3 includes a main body plate 34, a flange portion 35, and a protruding portion 36.

[0036] The main body plate 34 is located on the opposite side of the first end face E1 of the honeycomb base material 1 with respect to the first filter 2a. Typically, the main body plate 34 has a thickness in the extending direction of the honeycomb base material 1.

[0037] The flange portion 35 protrudes in the extending direction of the honeycomb substrate 1 from the peripheral edge on the surface of the main body plate 34 on the first filter 2a side. The flange portion 35 has a cylindrical shape extending in the same direction as the honeycomb substrate 1. In the illustrated example, the portion surrounded by the flange portion 35 in the surface of the main body plate 34 on the first filter 2a side is configured as the opposing surface 3a described above. In the illustrated example, the opposing surface 3a is in contact with the first filter 2a except for the plurality of groove portions 31. Therefore, the first filter 2a is sandwiched between the first end face E1 of the honeycomb substrate 1 and the opposing surface 3a of the first end member 3. The inner surface of the flange portion 35 is typically formed along the outer shape of the end portion of the honeycomb substrate 1. In the illustrated example, the flange portion 35 has a rectangular tubular shape (see FIG. 2). When the honeycomb substrate 1 has a cylindrical shape (see FIG. 4), the inner surface of the flange portion 35 may have a circular shape when viewed from the thickness direction of the main body plate 34 (see FIG. 6).

[0038] The protruding portion 36 is provided on the surface of the main body plate 34 on the side opposite to the flange portion 35. The protruding portion 36 protrudes from the main body plate 34 in the extending direction of the honeycomb substrate 1. The protruding portion 36 typically protrudes from the central portion of the main body plate 34.

[0039] As described above, the first end member 3 includes the supply port 32 and the plurality of groove portions 31.

[0040] In one embodiment, the supply port 32 penetrates the protruding portion 36 and the main body plate 34 in the extending direction of the honeycomb substrate 1. The supply port 32 has any appropriate shape in a cross section perpendicular to the extending direction of the honeycomb substrate 1. Examples of the cross-sectional shape of the supply port 32 include a triangle, a quadrangle, a pentagon, a polygon having six or more sides, a circle, and an ellipse, with a circle being preferred. The cross-sectional area of the supply port 32 is, for example, 0.008 cm ２ to 3.14 cm ２ , preferably 0.08 cm ２ to 0.157 cm ２ .

[0041] Multiple grooves 31 are provided on the opposing surfaces 3a of the main plate 34. Each of the multiple grooves 31 is recessed from the opposing surface 3a in the thickness direction of the main plate 34 (the direction in which the honeycomb base material 1 extends). In the illustrated example, each of the multiple grooves 31 extends linearly in a direction perpendicular to the thickness direction of the main plate 34.

[0042] The groove 31 has any suitable shape in a cross-section perpendicular to the direction in which the groove 31 extends. Examples of cross-sectional shapes of the groove 31 include a U-shape and a V-shape. In the illustrated example, the groove 31 has a U-shaped cross-section that opens toward the first filter 2a.

[0043] In one embodiment, when the cell 12 has a rectangular cross-sectional shape, the width of each of the multiple grooves 31 (the dimension in the direction perpendicular to the direction in which the groove extends) is smaller than the dimension of the longest side among the sides of the cross-sectional shape of the multiple cells 12. When the width of the groove and the side of the cell are in this relationship, fluid can be supplied more stably to the multiple flow paths. The width of the groove 31 is, for example, 0.5 mm to 2.0 mm, preferably 1.0 mm to 2.0 mm. The depth of the groove 31 is, for example, 0.5 mm to 3.0 mm, preferably 1.0 mm to 2.0 mm.

[0044] In one embodiment, the bottom surface of each of the multiple grooves 31 is inclined to approach the first filter 2a as it moves away from the supply port 32. In other words, the bottom surfaces of the multiple grooves 31 form a mortar-like shape that is recessed toward the supply port 32 in a cross-section obtained by cutting the first end member 3 in the thickness direction of the main plate 34. This allows the fluid supplied from the supply port to be stably distributed through multiple flow paths. As shown in Figure 7, the bottom surface of each of the multiple grooves 31 may be substantially parallel to the first end surface E1 of the honeycomb substrate 1.

[0045] As shown in Figure 2, the multiple grooves 31 intersect each other at a position that overlaps with the supply port 32 when viewed from the thickness direction of the main plate 34. In other words, the intersection points of the multiple grooves 31 overlap with the supply port 32 in the thickness direction of the main plate 34. As a result, the multiple grooves 31 are connected to each other, and the grooves 31 and the supply port 32 are connected to each other. In the illustrated example, the multiple grooves 31 extend radially from the supply port 32 when viewed from the thickness direction of the main plate 34.

[0046] Furthermore, the multiple grooves 31 overlap with all of the multiple flow channels 14 contained in the honeycomb substrate 1 when viewed from the thickness direction of the main plate 34. When the multiple grooves 31 are projected onto the honeycomb substrate 1 in the direction in which the honeycomb substrate 1 extends, the projected area of ​​the grooves 31 that overlap with each flow channel 14 is, for example, 50% to 80%, preferably 60% to 80%, when the area of ​​each flow channel 14 is taken as 100%. When the grooves overlap with the flow channels in this way, the fluid supplied from the supply port can be distributed uniformly to the multiple flow channels. Note that the ratio of the projected area of ​​the grooves that overlap with the flow channels may be different for each of the multiple flow channels, or it may be the same for each.

[0047] The number of grooves 31 can be arbitrarily and appropriately changed according to the number of flow channels 14 contained in the honeycomb substrate 1. The number of grooves 31 can be, for example, 2 to 8, and preferably 4 to 8.

[0048] As shown in Figure 1, the first end member 3 is fixed to the end of the honeycomb substrate 1 on the first end face E1 side by any suitable fixing means. In the illustrated example, the flange portion 35 of the first end member 3 is fixed to the honeycomb substrate 1 via a sealing member 5 and a retaining plate 6. The retaining plate 6 is fixed to the outer wall 13 of the honeycomb substrate 1. The sealing member 5 is typically made of an elastic fluororesin. With the sealing member 5 sandwiched between the flange portion 35 of the first end member 3 and the retaining plate 6, the flange portion 35 and the retaining plate 6 are connected by a connector (for example, a screw). With this configuration, airtightness between the first end member and the honeycomb substrate can be ensured, and the first end member can be sufficiently fixed to the honeycomb substrate.

[0049] In one embodiment, the flow synthesis reactor 100 further comprises a second end member 4. The second end member 4 is fixed to the end of the honeycomb substrate 1 on the second end face E2 side by any suitable fixing means. In the illustrated example, the second end member 4 is fixed to the honeycomb substrate 1 via a sealing member 5 and a retaining plate 6, similar to the first end member 3. The second end member 4 has any suitable configuration that, while fixed to the end of the honeycomb substrate 1, can form a space that communicates with a plurality of flow channels 14. In the illustrated example, the second filter 2b is sandwiched between the second end face E2 of the honeycomb substrate 1 and the second end member 4.

[0050] In the illustrated example, the second end member 4 has the same configuration as the first end member 3, except that it has an outlet 41 instead of a supply port 32. The outlet 41 can discharge fluid containing the target compound generated in the flow path 14 of the honeycomb substrate 1. The outlet 41 has any suitable shape in the cross-section in a direction perpendicular to the extending direction of the honeycomb substrate 1. An example of the cross-sectional shape of the outlet 41 is the same as the cross-sectional shape of the supply port 32 described above. The range of the cross-sectional area of ​​the outlet 41 is, for example, the same as the range of the cross-sectional area of ​​the supply port 32 described above.

[0051] The present invention will be specifically described below with reference to examples, but the present invention is not limited to these examples.

[0052] <<Example 1>> After extruding a clay mixture containing SiC powder and a binder, it was dried to prepare the honeycomb substrate shown in Figure 3. Next, with the Si-containing material in contact with the honeycomb substrate, it was heated at 1500°C for 4 hours to impregnate the honeycomb substrate with molten metal containing Si. This prepared a honeycomb substrate composed of a Si-SiC composite material.

[0053] The honeycomb substrate had a prismatic shape. The dimension of the honeycomb substrate in the direction of extension (axial direction) was 100 mm, and the dimension of one side of the honeycomb substrate was 10 mm. The honeycomb substrate had partition walls defining multiple cells and an outer wall surrounding the partition walls. The cross-sectional shape of the cells was square. The length of one side of the cross-sectional shape of the cells was 0.3 cm. In addition, there were 9 cells in the honeycomb substrate, the thickness of the partition walls was 0.4 mm, and the porosity of the partition walls was 2%.

[0054] Next, all of the cells (i.e., the flow channels) were filled with a palladium-based catalyst and Celite (a diluent). The palladium-based catalyst contained an active component containing palladium and a carbon support that carried the active component. The palladium content in the palladium-based catalyst was 10% by mass. When the total volume of the cells was set to 100%, the amount of palladium-based catalyst filling was 7%, and the total amount of palladium-based catalyst and diluent filling was 70%.

[0055] Next, a first filter and a second filter, both made of fluororesin, were prepared. The thickness and average pore size of the filters (the first filter and the second filter, respectively) are shown in Table 1.

[0056] Next, the first end member shown in Figures 1 and 2 was prepared. The first end member was made of PEEK. The cross-sectional area of ​​the supply port was 0.01 cm². ２ The width of the groove was 0.15 cm, and the depth of the groove was 0.2 cm. Next, the first filter was placed on the first end face of the honeycomb substrate, and the first end member was fixed to the end of the honeycomb substrate on the first end face side so as to cover the first filter. More specifically, the first end member was fixed to the end of the honeycomb substrate using a sealing member, a retaining plate, and screws. As a result, the first filter was sandwiched between the opposing surface of the first end member and the first end face of the honeycomb substrate. Similarly, the second filter was placed on the second end face of the honeycomb substrate, and the second end member, made of PEEK, was fixed to the end of the honeycomb substrate on the second end face side. The cross-sectional area of ​​the outlet was 0.03 cm². ２ Therefore, a flow synthesis reactor was manufactured.

[0057] <<Example 2>> A flow synthesis reactor was manufactured in the same manner as in Example 1, except that the thickness of the filters (the first filter and the second filter, respectively) was changed as shown in Table 1.

[0058] <<Example 3>> A flow synthesis reactor was manufactured in the same manner as in Example 1, except that the filters (the first filter and the second filter, respectively) were changed to filters having a central portion and a peripheral portion with different average pore sizes. The volume proportion of the central portion of the filter was 25%, and the volume proportion of the peripheral portion of the filter was 75%. The average pore sizes of the central and peripheral portions are shown in Table 1.

[0059] <<Example 4>> A flow synthesis reactor was manufactured in the same manner as in Example 3, except that the thickness of the filters (the first filter and the second filter, respectively) was changed as shown in Table 1.

[0060] <<Comparative Example 1>> A flow synthesis reactor was manufactured in the same manner as in Example 1, except that the first end member did not have multiple grooves.

[0061] <<Comparative Example 2>> A flow synthesis reactor was manufactured in the same manner as in Example 1, except that the first end member did not have multiple grooves and the filter thickness was changed to 1 mm.

[0062] <Evaluation: Flow Synthesis> 0.5 mmol of bromoacetone, 0.6 mmol of phenylboronic acid, and 1.0 mmol of sodium hydroxide were added to a mixed solvent of dioxane and water (dioxane:water = 1:3) and stirred to prepare the starting material solution. Next, the flow synthesis reactor prepared in the examples and comparative examples was heated to 80°C, and the starting material solution was supplied to the feed port at a flow rate of 0.5 mL / min. Subsequently, the effluent containing the target compound, acetylbiphenyl, was collected from the outlet. Next, the solvent was removed from the collected effluent to obtain a crude containing the reaction substrate (reactants) and / or reaction product. Next, the crude was dissolved in deuterated chloroform and subjected to nuclear magnetic resonance (CRN) testing. １The reaction substrate and reaction product were evaluated according to the following criteria, with yields calculated based on the internal standard tetrachloroethane using 1H-NMR. The results are shown in Table 1. A (◎◎): Reaction rate of 90% or more. B (◎): Reaction rate of 80% or more and less than 90%. C (〇): Reaction rate of 70% or more and less than 80%. D (△): Reaction rate of 50% or more and less than 70%. E (×): Reaction rate of less than 50%.

[0063]

[0064] <Evaluation> As shown in Table 1, if the first end member has multiple grooves, and these grooves intersect each other at a position overlapping with the supply port, and overlap with all of the flow paths containing the multiple cells, it can be seen that the desired flow synthesis reaction can proceed efficiently and the yield of the target compound can be improved.

[0065] The flow synthesis reactor according to the embodiment of the present invention can be applied to various flow synthesis reactions and is particularly suitable for flow precision synthesis.

[0066] 1 Honeycomb substrate 12 Cell 14 Flow channel 2 Filter 3 First end member 31 Groove 32 Supply port 3a Opposing surface 100 Flow synthesis reactor

Claims

1. A flow synthesis reactor comprising: a honeycomb substrate extending in a predetermined direction, having a first end face and a second end face in the direction of extension of the honeycomb substrate; a filter positioned opposite the first end face; and an end member fixed to the end of the honeycomb substrate so as to cover the filter, wherein the honeycomb substrate has a plurality of cells extending from the first end face to the second end face, each of the plurality of cells including a flow path through which a fluid can pass; the end member has a supply port for supplying fluid, the supply port penetrating the end member in the direction of extension of the honeycomb substrate; and a plurality of grooves provided on the opposing surface facing the filter, wherein the plurality of grooves intersect each other at a position overlapping with the supply port when viewed from the direction of extension of the honeycomb substrate, and overlap with all of the flow paths included in the plurality of cells.

2. The flow synthesis reactor according to claim 1, wherein the dimensions of the filter in the direction in which the honeycomb substrate extends are 1 mm to 10 mm.

3. The flow synthesis reactor according to claim 1 or 2, wherein each of the plurality of grooves extends linearly, each of the plurality of cells has a rectangular shape in a cross-section perpendicular to the direction in which the honeycomb substrate extends, and the width of each of the plurality of grooves is smaller than the dimension of the longest side of the cross-sectional shape of each of the plurality of cells.

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