Gas reaction synthesis unit and gas reaction synthesis device

Abstract

This gas reaction synthesis unit 2 is for reacting and synthesizing a starting material gas 30 and comprises a honeycomb structure 20 having one or a plurality of honeycomb structure parts 21 having an outer peripheral wall 22 and partition walls 23 which are installed inside the outer peripheral wall 22 and act as partitions to form a plurality of cells 24 forming flow paths extending from one end face to the other end face. In at least one of the one or the plurality of honeycomb structure parts 21, the plurality of cells 24 include a heating cell 5 which includes a conductor and / or a magnetic body 5a, a reaction cell 6 through which the starting material gas 30 flows, and a cooling cell 7 through which a cooling gas 40 flows.

Description

Gas reaction synthesis unit and gas reaction synthesis device

[0001] The present invention relates to a gas reaction synthesis unit and a gas reaction synthesis apparatus for synthesizing a raw material gas by reacting it.

[0002] As disclosed in the following Patent Document 1, honeycomb structures are widely used as chemical reactors for purifying automobile exhaust gases. However, in automotive applications, there is no need to cool the honeycomb structure because cooling would deteriorate the purification performance of the automobile catalyst.

[0003] Furthermore, heat exchangers using honeycomb structures have also been proposed for application to exothermic reactions, as disclosed in the following Patent Documents 2 to 5. However, the configurations proposed in Patent Documents 2 to 5 do not take into consideration heating the catalyst to the reaction initiation temperature, and it is necessary to separately and appropriately control the temperature of the reaction gas.

[0004] Japanese Patent Application Laid-Open No. 2013-22573 Japanese Patent Application Laid-Open No. 55-102891 Japanese Utility Model Application Laid-Open No. 60-091969 Japanese Patent Application Laid-Open No. 2010-271031 U.S. Patent No. 4,041,591

[0005] As described above, conventional configurations have only one of the functions of heating and cooling. However, for example, when a raw material gas is reacted to synthesize the raw material, if the reaction is an exothermic reaction, it is necessary to heat the catalyst and the reaction gas up to the reaction initiation temperature, and also to cool the reaction heat. In other words, conventional configurations having only one of the functions of heating and cooling are insufficient for use alone in the reaction synthesis of raw material gases.

[0006] The present invention has been made to solve the above-mentioned problems, and one of its objects is to provide a gas reaction synthesis unit and a gas reaction synthesis apparatus that can independently realize both heating and cooling.

[0007] Item 1. In one embodiment, the present invention relates to a gas reaction synthesis unit for reacting and synthesizing raw material gases, the gas reaction synthesis unit comprising a honeycomb structure having one or more honeycomb structure sections each having an outer peripheral wall and partition walls disposed inside the outer peripheral wall to define a plurality of cells that form flow paths extending from one end face to the other end face, wherein in at least one of the one or more honeycomb structure sections, the plurality of cells include a heating cell containing a conductor and / or a magnetic material, a reaction cell through which the raw material gas is flowed, and a cooling cell through which a cooling gas is flowed.

[0008] Item 2. The present invention may relate to the gas reaction synthesis unit according to Item 1, wherein the reaction of the raw material gas is an exothermic reaction, and the ratio (RA / CA) of the surface area (RA) of the reaction cell in contact with the raw material gas to the surface area (CA) of the cooling cell in contact with the cooling gas is set to satisfy the relationship of (amount of heat generated by reaction per unit gas flow rate in the exothermic reaction) × (mixed flow rate of raw material gases) × (amount of heat transferred to the honeycomb structure per unit flow rate of raw material gases)≦(amount of heat transferred from the honeycomb structure to the cooling gas per unit time, unit flow rate, and unit area) × (flow rate of cooling gas).

[0009] Item 3. The present invention may relate to the gas reaction synthesis unit according to Item 1 or 2, wherein a reaction zone provided with a reaction cell is adjacent to a pair of cooling zones provided with cooling cells, and a heating cell is provided within the reaction zone.

[0010] Item 4. The present invention may relate to the gas reaction synthesis unit according to Item 3, wherein the partition walls include a permeable partition wall configured to allow permeation of the raw material gas and the cooling gas, and a permeation-restricting partition wall positioned between the cooling region and the reaction region and configured to restrict permeation of the raw material gas and the cooling gas compared to the permeable partition wall.

[0011] Item 5. The present invention may relate to the gas reaction synthesis unit according to Item 4, wherein the wall thickness of the permeation restricting partition walls is set to be thicker than the wall thickness of the permeable partition walls, and / or a material that restricts the flow of the source gas and the cooling gas is applied to the wall surfaces or inside of the permeation restricting partition walls.

[0012] Item 6. The present invention may relate to the gas reaction synthesis unit according to Item 4 or 5, wherein the cooling gas contains at least a part of the raw material gas.

[0013] Item 7. The present invention may relate to the gas reaction synthesis unit according to any one of Items 3 to 6, wherein the direction in which the cooling gas flows in the cooling cell is at least partially parallel to or opposite to the direction in which the raw material gas flows in the reaction cell.

[0014] Item 8. The present invention may relate to the gas reaction synthesis unit according to any one of Items 3 to 7, wherein the honeycomb structure portion has a first surface and a second surface that are different from each other and arranged in non-opposing positions, the reaction cells are open in the first surface, and openings communicating with the cooling cells are provided in the second surface.

[0015] Item 9. The present invention may relate to the gas reaction synthesis unit according to any one of Items 3 to 8, wherein the source gas includes a first source gas and a second source gas different from the first source gas, the reaction cells include a first reaction cell into which the first source gas is introduced and a second reaction cell into which the second source gas is introduced, and the partition wall is located between the first reaction cell and the second reaction cell and includes a permeability coefficient-controlled partition wall configured so that the permeability coefficients of the first source gas and the second source gas change in the extension direction of the multiple cells.

[0016] Item 10. The present invention may relate to the gas reaction synthesis unit according to Item 9, wherein the permeability coefficients on the inlet sides of the first reaction cell and the second reaction cell are lower than the permeability coefficients on the outlet sides of the first reaction cell and the second reaction cell.

[0017] Item 11. The present invention may relate to the gas reaction synthesis unit according to Item 9 or 10, wherein the permeability coefficient control partition has a partition body and a permeability coefficient control film provided on the surface of the partition body.

[0018] Item 12. The present invention may relate to the gas reaction synthesis unit according to Item 11, wherein the permeability coefficient of the permeability coefficient-control partition walls is changed by at least one of changing the thickness of the partition wall body in the stretching direction of the plurality of cells, changing the thickness of the permeability coefficient control membrane in the stretching direction of the plurality of cells, and changing the density of the permeability coefficient control membrane in the stretching direction of the plurality of cells.

[0019] Item 13. The present invention may relate to the gas reaction synthesis unit according to Item 11 or 12, wherein the permeability control membrane includes at least one of ceramics, metals, and organic materials.

[0020] Item 14. The present invention may relate to the gas reaction synthesis unit according to Item 13, wherein the ceramic contained in the permeability coefficient control film contains at least one selected from the group consisting of cordierite, silicon carbide, silicon, silica, and alumina.

[0021] Item 15. The present invention may relate to the gas reaction synthesis unit according to any one of Items 9 to 14, wherein the honeycomb structure portion has a first surface, a second surface, and a third surface that are different from each other and arranged in non-opposing positions, the first reaction cell is open in the first surface, an opening communicating with the cooling cell is provided in the second surface, and the second reaction cell is open in the third surface.

[0022] Item 16. The present invention may relate to the gas reaction synthesis unit according to any one of Items 1 to 15, further comprising an induction heating coil arranged on the outer periphery of the honeycomb structure, and configured so that the conductor and / or magnetic material can be inductively heated by magnetic flux from the induction heating coil.

[0023] Item 17. The present invention may relate to the gas reaction synthesis unit according to Item 16, wherein the conductor and / or magnetic material is present in at least a portion of the honeycomb structure in the radial direction and the axial direction.

[0024] Item 18. The present invention may relate to the gas reaction synthesis unit according to Item 16 or 17, wherein the conductor and / or magnetic material is present inside the outer wall, inside the partition wall, inside the cell, and / or on the outer wall.

[0025] Item 19. The present invention may relate to the gas reaction synthesis unit according to Item 18, wherein the conductor and / or magnetic material present inside the cell is filled in the cell or coated on the surface of the partition wall.

[0026] Item 20. The present invention may relate to the gas reaction synthesis unit according to any one of Items 16 to 19, further comprising a magnetic shield disposed around the outer periphery of the induction heating coil.

[0027] Item 21. The present invention may relate to the gas reaction synthesis unit according to any one of Items 16 to 20, wherein the honeycomb structure contains at least one selected from the group consisting of cordierite, silicon carbide, silicon, silica, and alumina.

[0028] Item 22. The present invention may relate to the gas reaction synthesis unit according to any one of Items 16 to 21, wherein the conductor and / or magnetic material contains at least one selected from the group consisting of Fe, Cr, Ni, Mn, Zn, Co, Cu, and Si.

[0029] Item 23. The present invention may relate to the gas reaction synthesis unit according to any one of Items 16 to 22, wherein the magnetic material has a Curie point of 100° C. or higher.

[0030] Item 24. The present invention may relate to the gas reaction synthesis unit according to any one of Items 1 to 23, wherein at least one of the one or more honeycomb structure sections contains a catalyst.

[0031] Item 25. The present invention may relate to the gas reaction synthesis unit according to any one of Items 1 to 24, wherein the honeycomb structure includes one or more first honeycomb structure parts provided with reaction cells and one or more second honeycomb structure parts provided with cooling cells.

[0032] Item 26. In one embodiment, the present invention relates to a gas reaction synthesis apparatus comprising the gas reaction synthesis unit according to any one of Items 1 to 25, a raw material gas supply source connected to the reaction cell, and a cooling gas supply source connected to the cooling cell.

[0033] Item 27. The present invention may relate to a gas reaction synthesis apparatus according to Item 26 reciting any one of Items 16 to 23, further comprising a power supply circuit connected to an induction heating coil, and configured so that a conductor and / or a magnetic material can be inductively heated by a magnetic flux from the induction heating coil before or when a raw material gas is passed through the reaction cell.

[0034] Item 28. The present invention may relate to the gas reaction synthesis apparatus according to Item 26 or 27, wherein the raw material gas includes methanol gas, carbon monoxide, carbon dioxide, hydrogen, nitrogen, and / or steam.

[0035] According to one embodiment of the gas reaction synthesis unit and gas reaction synthesis apparatus of the present invention, in at least one of the one or more honeycomb structure parts, the multiple cells include a heating cell containing a conductor and / or a magnetic material, a reaction cell through which a raw material gas flows, and a cooling cell through which a cooling gas flows, so that both heating and cooling can be achieved independently.

[0036] 1 is an explanatory diagram showing a gas reaction synthesis apparatus and a gas reaction synthesis unit according to a first embodiment of the present invention. FIG. 1 is a perspective view showing the gas reaction synthesis unit of FIG. 1. FIG. 1 is a front view showing the honeycomb structure of FIG. 1. FIG. 3 is a front view showing a modified example of the honeycomb structure of FIG. 3. FIG. 1 is a perspective view showing the honeycomb structure, reaction cells, and cooling cells of FIG. 1. FIG. 5 is a cross-sectional view of the honeycomb structure of FIG. 5. FIG. 1 is a circuit diagram showing the power supply circuit of FIG. 1. FIG. 2 is a front view showing the honeycomb structure of FIG. 2 and its periphery. FIG. 1 is an explanatory diagram showing a first example of an existence mode of conductors and / or magnetic materials in the honeycomb structure of FIG. 1. FIG. 1 is an explanatory diagram showing a second example of an existence mode of conductors and / or magnetic materials in the honeycomb structure of FIG. 1. FIG. 1 is an explanatory diagram showing a third example of an existence mode of conductors and / or magnetic materials in the honeycomb structure of FIG. 1. FIG. 1 is an explanatory diagram showing a gas reaction synthesis apparatus and a gas reaction synthesis unit according to a second embodiment of the present invention. FIG. 12 is a perspective view showing openings communicating with the honeycomb structure, reaction cells, and cooling cells of FIG. 12. FIG. 13 is a cross-sectional view of the honeycomb structure of FIG. 13. FIG. 14 is a cross-sectional view showing a modified example of the honeycomb structure of FIG. 14. 25 is an explanatory diagram showing a gas reaction synthesis apparatus and a gas reaction synthesis unit according to embodiment 3 of the present invention. FIG. 16 is a perspective view showing openings communicating with the honeycomb structure, reaction cells, and cooling cells of FIG. 16. FIG. 17 is a cross-sectional view of the honeycomb structure of FIG. 17. FIG. 18 is a cross-sectional view showing a modified example of the honeycomb structure of FIG. 17. FIG. 26 is an explanatory diagram showing a gas reaction synthesis apparatus and a gas reaction synthesis unit according to embodiment 4 of the present invention. FIG. 27 is a front view showing the honeycomb structure of FIG. 20. FIG. 28 is a rear view showing the honeycomb structure of FIG. 20. FIG. 29 is a front view showing a modified example of the honeycomb structure of FIG. 21. FIG. 30 is a rear view showing a modified example of the honeycomb structure of FIG. 21. FIG. 31 is a perspective view showing the honeycomb structure, reaction cells, and cooling cells of FIG. 20. FIG. 32 is a perspective view showing the honeycomb structure, reaction cells, and cooling cells of FIG. 20 as viewed from the opposite direction to that of FIG. 25. FIG. 33 is an explanatory diagram showing a gas reaction synthesis apparatus and a gas reaction synthesis unit according to embodiment 5 of the present invention. FIG. 34 is a perspective view showing openings communicating with the honeycomb structure, reaction cells, and cooling cells of FIG. 27. 28 is a perspective view showing the honeycomb structure portion, the reaction cells, and the openings communicating with the cooling cells in FIG. 27 when viewed from the opposite direction to that in FIG. 28. It is an explanatory diagram showing a gas reaction synthesis apparatus and a gas reaction synthesis unit according to a sixth embodiment of the present invention.Fig. 31 is a perspective view showing openings communicating with the honeycomb structure part, reaction cells, and cooling cells of Fig. 30. Fig. 32 is a perspective view showing openings communicating with the honeycomb structure part, reaction cells, and cooling cells of Fig. 30 when viewed from the opposite direction to Fig. 31. Fig. 33 is a perspective view showing a gas reaction synthesis unit according to embodiment 7 of the present invention.

[0037] Hereinafter, embodiments of the present invention will be described with reference to the drawings. The present invention is not limited to each embodiment, and the components can be modified and embodied without departing from the spirit of the present invention. Furthermore, various inventions can be formed by appropriately combining multiple components disclosed in each embodiment. For example, some components may be omitted from all the components shown in the embodiments. Furthermore, components of different embodiments may be appropriately combined.

[0038] Embodiment 1. Figure 1 is an explanatory diagram showing a gas reaction synthesis apparatus 1 and a gas reaction synthesis unit 2 according to embodiment 1 of the present invention, Figure 2 is a perspective view showing the gas reaction synthesis unit 2 of Figure 1, Figure 3 is a front view showing the honeycomb structure 21 of Figure 1, and Figure 4 is a front view showing a modified example of the honeycomb structure 21 of Figure 3. Also, Figure 5 is a perspective view showing the honeycomb structure 21, reaction cells 6, and cooling cells 7 of Figure 1, and Figure 6 is a cross-sectional view of the honeycomb structure 21 of Figure 5. Also, Figure 7 is a circuit diagram showing the power supply circuit 8 of Figure 1, and Figure 8 is a front view showing the honeycomb structure 20 of Figure 2 and its periphery. In addition, Figure 9 is an explanatory diagram showing a first example of the presence mode of the conductor and / or magnetic material 5a in the honeycomb structure part 21 of Figure 1, Figure 10 is an explanatory diagram showing a second example of the presence mode of the conductor and / or magnetic material 5a in the honeycomb structure part 21 of Figure 1, and Figure 11 is an explanatory diagram showing a third example of the presence mode of the conductor and / or magnetic material 5a in the honeycomb structure part 21 of Figure 1.

[0039] The gas reaction synthesis apparatus 1 and the gas reaction synthesis unit 2 shown in Figures 1 and 2 are an apparatus and a unit for synthesizing a raw material gas 30 by reacting it. The gas reaction synthesis apparatus 1 is configured to obtain a predetermined synthesis gas 30a by synthesizing the raw material gas 30 by reacting it in the gas reaction synthesis unit 2. The synthesis gas 30a may contain unreacted raw material gas 30.

[0040] The source gas 30 may contain a first source gas 31 and a second source gas 32 different from the first source gas 31. The first source gas 31 and the second source gas 32 may be introduced into the gas reaction synthesis unit 2 in a pre-mixed state, or may be mixed within the gas reaction synthesis unit 2. In this embodiment, the first source gas 31 and the second source gas 32 are introduced into the gas reaction synthesis unit 2 in a pre-mixed state.

[0041] Various gases can be used as the feed gas 30, and the feed gas 30 may include methanol gas (CHOH), carbon monoxide (CO), carbon dioxide (CO), hydrogen (H), nitrogen (N), and / or steam (H0). For example, carbon monoxide (CO) can be used in the Fischer-Tropsch reaction, carbon dioxide (CO) can be used in the Sabatier reaction, and nitrogen (N) can be used in ammonia synthesis. For example, when CO and H react (the Sabatier reaction), CH and H0 are synthesized. When CO and H react, CHOH is synthesized. When N and H react, NH is synthesized.

[0042] The gas reactions include exothermic reactions that generate heat when the raw material gas 30 reacts, and endothermic reactions that absorb heat when the raw material gas 30 reacts. The gas reaction synthesis apparatus 1 and gas reaction synthesis unit 2 of this embodiment may be used in an embodiment involving either reaction. However, the gas reaction synthesis apparatus 1 and gas reaction synthesis unit 2 of this embodiment are configured to independently realize both heating and cooling, as described below, and are particularly suitable for use in an embodiment involving an exothermic reaction. The above-mentioned Fischer-Tropsch reaction, Sabatier reaction, and ammonia synthesis are all exothermic reactions.

[0043] As shown in FIG. 1, the gas reaction synthesis apparatus 1 includes a gas reaction synthesis unit 2, a raw material gas supply source 3, and a cooling gas supply source 4.

[0044] The gas reaction synthesis unit 2 is for synthesizing the raw material gases by reaction as described above. The gas reaction synthesis unit 2 has a honeycomb structure 20.

[0045] The honeycomb structure 20 has one or more honeycomb structure portions 21. FIG. 2 shows a honeycomb structure 20 having multiple honeycomb structure portions 21. As particularly shown in FIG. 2, the honeycomb structure portion 21 has an outer peripheral wall 22 and partition walls 23 disposed inside the outer peripheral wall 22 to define multiple cells 24 that form flow paths extending from one end face to the other end face. The honeycomb structure portion 21 may have a columnar outer shape. A columnar shape can be understood as a three-dimensional shape having a predetermined thickness in the axial direction AD. The axial direction AD may be the extension direction 24E of the multiple cells 24. The ratio (aspect ratio) of the axial length of the honeycomb structure portion 21 to the diameter or width of the end face of the honeycomb structure portion 21 may be any ratio. The columnar shape may include a shape (flat shape) in which the axial length of the honeycomb structure portion 21 is shorter than the diameter or width of the end face. The external shape of the honeycomb structure portion 21 is not particularly limited, but may be a columnar shape with square end faces (quadratic column shape) as shown in FIG. 2, a columnar shape with circular or oval end faces, or a columnar shape with polygonal end faces having fewer or more corners (triangular, pentagonal, hexagonal, heptagonal, octagonal, etc.).

[0046] The material of the honeycomb structure portion 21 (the outer peripheral wall 22 and the partition walls 23) is not particularly limited, but is usually formed of a ceramic material. The honeycomb structure portion 21 preferably contains at least one selected from the group consisting of cordierite, silicon carbide, silicon, silica, and alumina. More specifically, examples of the material of the honeycomb structure portion 21 include cordierite, silicon carbide, aluminum titanate, silicon nitride, mullite, alumina, silica, a silicon-silicon carbide-based composite material, and a silicon carbide-cordierite-based composite material. More preferably, the honeycomb structure portion 21 is formed of cordierite, alumina, silica, silicon carbide, or a silicon-silicon carbide-based composite material. In this specification, silicon carbide-based and cordierite-based mean that the outer peripheral wall 22 and the partition walls 23 contain silicon carbide or cordierite in an amount of 50 mass% or more of the entire outer peripheral wall 22 and the partition walls 23.

[0047] The shape of the cells 24 is not particularly limited, but is preferably a polygon such as a triangle, a rectangle, a pentagon, a hexagon, or an octagon, a circle, or an ellipse in a cross section perpendicular to the central axis of the honeycomb structure portion 21, or may be other irregular shapes. A polygon is preferable.

[0048] The thickness of the partition walls 23 is preferably 0.05 to 0.50 mm, and from the viewpoint of ease of production, more preferably 0.07 to 0.38 mm. For example, when the thickness is 0.05 mm or more, the strength of the honeycomb structure portion 21 is further improved, and when the thickness is 0.50 mm or less, pressure loss can be reduced. Note that the thickness of the partition walls 23 is an average value measured by observing a cross section in the central axis direction with a microscope.

[0049] The porosity of the partition walls 23 is preferably 20 to 70%. From the viewpoint of ease of production, the porosity of the partition walls 23 is preferably 20% or more, and if it is 70% or less, the strength of the honeycomb structure portion 21 can be maintained.

[0050] The average pore diameter of the partition walls 23 is preferably 2 to 30 μm, and more preferably 5 to 25 μm. When the average pore diameter of the partition walls 23 is 2 μm or more, manufacturing becomes easy, and when it is 30 μm or less, the strength of the honeycomb structure portion 21 can be maintained. In this specification, the terms "average pore diameter" and "porosity" refer to the average pore diameter and porosity measured by mercury intrusion porosimetry.

[0051] The density of the cells 24 is not particularly limited, but is preferably 5 to 150 cells / cm. 2 The range is preferably 16 to 100 cells / cm 2 More preferably, the range is 31 to 100 cells / cm 2 It is more preferable that the range is:

[0052] Such a honeycomb structure 21 is produced by forming a honeycomb formed body by molding a clay containing ceramic raw materials into a honeycomb shape having partition walls 23 that define a plurality of cells 24 that extend from one end face to the other and serve as fluid flow paths, and then drying and firing the honeycomb formed body. The peripheral wall 22 may be a peripheral wall 22 extruded integrally with the honeycomb formed body. Alternatively, after molding or firing the honeycomb formed body, the periphery of the honeycomb formed body or sintered honeycomb body may be ground to a predetermined shape, and a coating material may be applied to the ground honeycomb formed body or sintered honeycomb body to form a peripheral coating, which serves as the peripheral wall 22 (in this case, only the peripheral coating constitutes the peripheral wall 22). Alternatively, the peripheral wall 22 extruded integrally with the honeycomb formed body may be formed without being ground, and a peripheral coating may be formed on it (the peripheral wall 22 has a two-layer structure consisting of the peripheral wall of the honeycomb sintered body or the like and the peripheral coating).

[0053] The honeycomb structure 21 is not limited to an integrated honeycomb structure 21 in which the partition walls 23 are integrally formed, but may be, for example, a honeycomb structure 21 (bonded honeycomb structure) having a structure in which a plurality of columnar honeycomb segments, each having ceramic partition walls 23 and a plurality of cells 24 formed by the partition walls 23 as fluid flow paths, are combined together via a bonding material layer.

[0054] In at least one of the one or more honeycomb structure portions 21, the multiple cells 24 include a heating cell 5 including a conductor and / or a magnetic material 5a, a reaction cell 6 through which a raw material gas 30 flows, and a cooling cell 7 through which a cooling gas 40 flows. In the figure, the heating cell 5 is shown with a darker hatching, the reaction cell 6 is shown with a lighter hatching than the heating cell 5, and the cooling cell 7 is shown with a lighter hatching than the reaction cell 6.

[0055] The gas reaction synthesis apparatus 1 of this embodiment is configured so that the honeycomb structure 21 or honeycomb structure 20 (hereinafter, sometimes simply referred to as the "honeycomb structure 21, etc.") can be heated through the conductor and / or magnetic material 5a and the heating cell 5 before or when the raw material gas 30 is passed through the reaction cell 6. This allows the raw material gas 30 to be heated through the honeycomb structure 21, etc., thereby reducing the need for an external heating means or heat exchanger. When an external heating means, etc. is provided, the size is large and heating is indirect, leaving room for improvement in terms of heating efficiency and size. In other words, the gas reaction synthesis apparatus 1 and gas reaction synthesis unit 2 of this embodiment can improve heating efficiency and size compared to when an external heating means, etc. is provided.

[0056] Furthermore, in the gas reaction synthesis apparatus 1 of this embodiment, when the raw material gas 30 is passed through the reaction cell 6, the honeycomb structure portion 21 and the like can be cooled by flowing the cooling gas 40 through the cooling cell 7. This reduces the need to provide an external cooling means.

[0057] That is, the gas reaction synthesis apparatus 1 and the gas reaction synthesis unit 2 of this embodiment are configured to be able to independently realize both heating and cooling, and are able to heat the raw material gas 30 to promote the reaction, and also to cool the honeycomb structure section 21 etc. that has been heated by the heat of the exothermic reaction. For this reason, the gas reaction synthesis apparatus 1 and the gas reaction synthesis unit 2 of this embodiment are particularly suitable for use in an embodiment involving an exothermic reaction.

[0058] The raw material gas supply source 3 is for supplying a raw material gas 30 to the honeycomb structure portion 21 and the like, and the cooling gas supply source 4 is for supplying a cooling gas 40 to the honeycomb structure portion 21 and the like. Although detailed connections are not shown in FIG. 1 , the raw material gas supply source 3 is connected to the reaction cell 6, and the cooling gas supply source 4 is connected to the cooling cell 7 through optional piping or the like. The raw material gas supply source 3 and the cooling gas supply source 4 may be constituted, for example, by a container (cylinder) storing a liquefied gas or a gas generator. An example of the gas generator is a nitrogen gas generator. As described below, the cooling gas 40 may contain at least a portion of the raw material gas 30 (the first raw material gas 31 and the second raw material gas 32), and the raw material gas supply source 3 and the cooling gas supply source 4 may include a piping system for circulating the raw material gas 30 used as the cooling gas 40.

[0059] When the reaction of the raw material gas 30 is an exothermic reaction, it is preferable that the ratio (RA / CA) of the surface area (RA) of the reaction cell 6 in contact with the raw material gas 30 to the surface area (CA) of the cooling cell 7 in contact with the cooling gas 40 is set so as to satisfy the relationship expressed by the following formula 1. Amount of heat generated by reaction per unit gas flow rate in exothermic reaction × mixed flow rate of raw material gas 30 × amount of heat transferred to the honeycomb structure 20 per unit flow rate of raw material gas 30≦amount of heat transferred from the honeycomb structure 20 to the cooling gas 40 per unit time, unit flow rate, and unit area × flow rate of cooling gas 40 (Formula 1)

[0060] The reaction heat value (KJ / mol) per unit gas flow rate (mol) in an exothermic reaction is known as a thermochemical reaction formula. For example, in the case of ammonia synthesis, the reaction heat value per unit gas flow rate in an exothermic reaction may be 92.4 KJ / mol.

[0061] The mixed flow rate (mol / s) of the source gas 30 can be determined by using a flow meter to measure the flow rate of the source gas 30. For example, when the flow rate of nitrogen is 1 mol / s and the flow rate of hydrogen is 3 mol / s, the mixed flow rate of the source gas 30 can be 4 mol / s.

[0062] The amount of heat transferred to the honeycomb structure 20 per unit flow rate of the raw material gas 30 (W / m 2The heat transfer rate (K) can be obtained by measuring the temperatures (K) of the raw material gas 30 and the honeycomb structure 20, measuring the amount of heat transfer (J), and calculating the contact area between the honeycomb structure 20 and the raw material gas 30. For example, when the temperature difference between the raw material gas 30 and the honeycomb structure 20 is 100 K, the amount of heat transfer is 10 J, and the contact area is 0.01 m 2 When the flow rate of the raw material gas 30 is 10 W / m, the amount of heat transferred to the honeycomb structure 20 per unit flow rate of the raw material gas 30 is 10 W / m. 2 ・It can be K.

[0063] The amount of heat transferred from the honeycomb structure 20 to the cooling gas 40 per unit time, unit flow rate and unit area (W / m 2 The heat transfer coefficient (K) can be obtained by measuring the temperatures (K) of the cooling gas 40 and the honeycomb structure 20, measuring the amount of heat transfer (W) from the honeycomb structure 20 to the cooling gas 40 per unit time and unit flow rate, and calculating the contact area between the honeycomb structure 20 and the cooling gas 40. For example, if the temperature difference between the cooling gas 40 and the honeycomb structure 20 is 100 K, the amount of heat transfer from the honeycomb structure 20 to the cooling gas 40 per unit time and unit flow rate is 10 W, and the contact area between the honeycomb structure 20 and the cooling gas 40 is 0.01 m 2 When the above equation is satisfied, the amount of heat transferred from the honeycomb structure 20 to the cooling gas 40 per unit time, per unit flow rate, and per unit area is 10 W / m 2 ・It can be K.

[0064] The flow rate (mol / s) of the cooling gas 40 can be determined by using a flow meter to measure the flow rate of the cooling gas 40. For example, when 1 mol of the cooling gas 40 flows per second, the flow rate of the cooling gas 40 can be 11 mol / s.

[0065] The surface area (RA) of the reaction cell 6 that comes into contact with the raw material gas 30 (m 2 ) can be calculated from the cell shape and the area of ​​the opening.

[0066] The surface area (CA) of the cooling cell 7 that is in contact with the cooling gas 40 (m 2 ) can be calculated from the cell shape and the area of ​​the opening.

[0067] The left side of Equation 1 represents the effect of heat generated by the exothermic reaction, and the right side of Equation 1 represents the cooling capacity of the gas reaction synthesis apparatus 1 and the gas reaction synthesis unit 2. The larger the surface area (RA) of the reaction cell 6, the larger the left side (particularly, "the amount of heat transferred to the honeycomb structure 20 per unit flow rate of the raw material gas 30"). Increasing the surface area can be synonymous with increasing the cell density. On the other hand, the larger the surface area (CA) of the cooling cell 7, the larger the right side (particularly, "the amount of heat transferred from the honeycomb structure 20 to the cooling gas 40 per unit time, unit flow rate, and unit area"). Whether the ratio (RA / CA) satisfies the relationship expressed by Equation 1 can be determined by checking whether the temperature of the reaction gas drops to a target temperature.

[0068] As shown in Figures 1, 3, and 4, it is preferable that the reaction region R1 in which the reaction cell 6 is provided is adjacent to a pair of cooling regions R2 in which the cooling cell 7 is provided, and the heating cell 5 is provided within the reaction region R1.

[0069] 3 and 4, when the end face of the honeycomb structure section 21 is viewed from the front, the cooling regions R2 may be arranged at both ends (upper and lower parts in the drawings) in the first width direction 21W1 of the honeycomb structure section 21, and the reaction region R1 may be arranged in the center in the first width direction 21W1. In other words, the reaction region R1 may be sandwiched between a pair of cooling regions R2.

[0070] The heating cells 5 may be arranged arbitrarily within the reaction region R1. The heating cells 5 may be arranged to extend in a second width direction 21W2 perpendicular to the first width direction 21W1. As shown in FIG. 3, the heating cells 5 may be arranged to extend linearly in the second width direction 21W2 at the center of the reaction region R1 in the first width direction 21W1. As shown in FIG. 4, the heating cells 5 may be arranged adjacent to the reaction cells 6 in at least one of the first width direction 21W1 and the second width direction 21W2 within the reaction region R1. In FIG. 4, the heating cells 5 are arranged adjacent to the reaction cells 6 in both the first width direction 21W1 and the second width direction 21W2. It is preferable that the heating cells 5 are not adjacent to the cooling cells 7. In other words, it is preferable that the reaction cells 6 are arranged between the heating cells 5 and the cooling cells 7.

[0071] The partition wall 23 may include a permeable partition wall 231 configured to allow permeation of the source gas 30 and the cooling gas 40 (hereinafter, sometimes simply referred to as "source gas 30, etc."), and a permeation-restricting partition wall 232 located between the cooling region R2 and the reaction region R1 and configured to suppress permeation of the source gas 30, etc., compared to the permeable partition wall 231. In the drawing, the permeation-restricting partition wall 232 is indicated by dark shading.

[0072] The permeation coefficient (mol m (s m 2 ・Pa) -1 ) can be 1 / 10 or more times the permeability coefficient of the source gas 30, etc., of the permeable partition wall 231. When the permeability coefficient of the permeation restricting partition wall 232 is 1 / 10 of the permeability coefficient of the permeation restricting partition wall 231, the cooling gas and the reactant gas can be separated. For example, the permeability coefficient of the permeation restricting partition wall 232 may be 1 / 20 or less of that of a wall without permeation control. The permeability coefficient is determined by the gas permeation amount (mol), wall thickness (m), pressure difference (Pa), permeation area (m 2 ) and measurement time (s).

[0073] Any method can be used to configure the permeation-restricting partition 232 so as to suppress permeation of the raw material gas 30, etc., but the permeation-restricting partition 232 can be configured to suppress permeation of the raw material gas 30, etc. by setting the wall thickness of the permeation-restricting partition 232 to be thicker than the wall thickness of the permeable partition 231, and / or by applying a material that suppresses the flow of the raw material gas 30, etc. to the wall surface or inside of the permeation-restricting partition 232.

[0074] When the wall thickness of the permeable partition wall 231 is T1 (mm) and the wall thickness of the permeation restricting partition wall 232 is T2 (mm), T2 can be 1 / 30 to 1 / 2 times T1. When T2 is 1 / 5 or more times T1, permeation of the source gas 30 and the like can be more reliably suppressed. When T2 is 1 / 10 or less times T1, a portion of the cooling gas can be used as a reaction gas. The wall thicknesses of the permeable partition wall 231 and the permeation restricting partition wall 232 can be determined by measurement using a microscope or the like.

[0075] Examples of materials that can be applied to the wall surfaces or interior of the permeation restricting partition walls 232 include silicic acid. Such materials are not applied to the wall surfaces or interior of the permeable partition walls 231. Such materials can be applied to the wall surfaces of the permeation restricting partition walls 232 by controlling the particle size. Furthermore, such materials can be applied to the interior of the permeation restricting partition walls 232 by miniaturizing the particles. That is, the particle size of the material applied to the wall surfaces or interior of the permeation restricting partition walls 232 is smaller than the diameter of the pores in the wall to which the material is applied, in order to penetrate into the pores.

[0076] The cooling gas 40 may be a gas separate from the raw material gas 30, or may contain at least a portion of the raw material gas 30 (the first raw material gas 31 and the second raw material gas 32). In other words, at least a portion of the raw material gas 30 may be passed through the cooling cell 7 before being introduced into the reaction cell 6. The gas reaction synthesis apparatus 1 and the gas reaction synthesis unit 2 may have a piping system for introducing at least a portion of the raw material gas 30 that has passed through the cooling cell 7 into the reaction cell 6 as the cooling gas 40. At least a portion of the raw material gas 30 used as the cooling gas 40 may contain at least a portion of the first raw material gas 31 and the second raw material gas 32. When the cooling gas 40 contains at least a portion of the raw material gas 30, the raw material gas 30 can be preheated by the heat of the honeycomb structure portion 21, etc.

[0077] The direction in which the cooling gas 40 flows in the cooling cell 7 may be at least partially parallel to or opposite to the direction in which the raw material gas 30 flows in the reaction cell 6. "Parallel" may mean that the cooling gas 40 and the raw material gas 30 flow in the same direction, and "opposite" may mean that the cooling gas 40 and the raw material gas 30 flow in opposite directions.

[0078] 1, 5, and 6 show a configuration in which the direction in which the cooling gas 40 flows in the cooling cell 7 is opposed to the direction in which the raw material gas 30 flows in the reaction cell 6 at all parts. As the reaction of the raw material gas 30 progresses in the honeycomb structure section 21, heat is generated. For this reason, the temperature of the honeycomb structure section 21 tends to be higher on the downstream side in the flow direction of the raw material gas 30 than on the upstream side. By opposing the flow direction of the cooling gas 40 to the flow direction of the raw material gas 30, it is possible to strengthen the cooling of the honeycomb structure section 21 on the downstream side, and to make the temperature of the honeycomb structure section 21 more uniform.

[0079] On the other hand, when the raw material gas 30 (the first raw material gas 31 and the second raw material gas 32) is introduced into the gas reaction synthesis apparatus 1 and the gas reaction synthesis unit 2 in a pre-mixed state, it may be preferable to strengthen the cooling on the upstream side (inlet side) of the flow direction of the raw material gas 30. This may occur when the reaction of the raw material gas 30 occurs vigorously on the upstream side (inlet side). In such a case, it is preferable to make the flow direction of the cooling gas 40 parallel to the flow direction of the raw material gas 30 in order to increase the cooling capacity on the upstream side.

[0080] The conductor and / or magnetic material 5a may be heated by any method. For example, the conductor and / or magnetic material 5a may be heated by passing an electric current through them. The gas reaction synthesis unit 2 of this embodiment further includes an induction heating coil 25 arranged on the outer periphery of the honeycomb structure 20. The gas reaction synthesis apparatus 1 of this embodiment further includes a power supply circuit 8 connected to the induction heating coil 25. The gas reaction synthesis apparatus 1 and the gas reaction synthesis unit 2 of this embodiment are configured so that the conductor and / or magnetic material 5a can be induction heated by the magnetic flux from the induction heating coil 25 before or when the raw material gas 30 is passed through the reaction cell 6.

[0081] The conductor and / or magnetic material 5a may be present in at least a part of the radial direction and the axial direction AD within the honeycomb structure 20. Furthermore, the conductor and / or magnetic material 5a may be present inside the outer peripheral wall 22, inside the partition wall 23, inside the cell 24, and / or on the outer peripheral wall 22. The conductor and / or magnetic material 5a present inside the cell 24 may be filled in the cell 24 or coated on the surface of the partition wall 23.

[0082] 9 shows an embodiment in which conductors and / or magnetic materials 5a are filled in some of the cells 24. The conductors and / or magnetic materials 5a may have a columnar outer shape that matches the shape of the cells 24. The conductors and / or magnetic materials 5a may have such an outer shape before being filled in the cells 24, or may have such an outer shape after being filled in the cells 24. In other words, the conductors and / or magnetic materials 5a may constitute a shaped material having a predetermined shape, or may constitute a paste-like amorphous material.

[0083] The shaped material and the unshaped material may be composed of a composite composition of a conductor and / or magnetic material 5a and a binder or adhesive material. Examples of binders include materials primarily composed of metal or glass. Examples of adhesive materials include materials primarily composed of silica or alumina. In addition to the binder or adhesive material, an organic or inorganic substance may also be contained. The conductor and / or magnetic material 5a may be filled all the way from one end face to the other end face of the honeycomb structure 20. Alternatively, the conductor and / or magnetic material 5a may be filled from one end face of the honeycomb structure 20 to partway through the cells 24.

[0084] The conductor and / or magnetic material 5 a is induction-heated by the magnetic flux from the induction heating coil 25, and the generated heat heats the honeycomb structure portion 21. By filling some of the cells 24 with the conductor and / or magnetic material 5 a, it becomes possible for the cells 24 to function as heaters in the honeycomb structure 20.

[0085] 10 shows an embodiment in which the conductive and / or magnetic material 5 a is coated on the surfaces of the partition walls 23. In the illustrated embodiment, the conductive and / or magnetic material 5 a is coated on the surfaces of the partition walls 23 of all the cells 24, but the conductive and / or magnetic material 5 a may be coated on the surfaces of only the partition walls 23 of some of the cells 24.

[0086] The conductor and / or magnetic material 5a coated on the surface of the partition wall 23 can form a coating layer together with an adhesive material in which the conductor and / or magnetic material 5a are dispersed. Examples of the adhesive material that can be used include glass containing silicic acid, boric acid, or borosilicate, crystallized glass, ceramics, and glass containing other oxides, crystallized glass, ceramics, etc. The conductor and / or magnetic material 5a may extend from one end face to the other end face of the honeycomb structure portion 21, or may extend over a portion of the honeycomb structure portion 21 in the axial direction AD. The amount of conductor and / or magnetic material 5a contained in the coating layer may be varied in the radial direction and the axial direction AD within the honeycomb structure 20.

[0087] The conductor and / or magnetic material 5 a is induction-heated by the magnetic flux from the induction heating coil 25, and the honeycomb structure portion 21 and the like are heated by the heat. By coating the surfaces of the partition walls 23 with the conductor and / or magnetic material 5 a, it becomes possible to make the cells 24 function as heaters in the honeycomb structure 20, similar to the case where the conductor and / or magnetic material 5 a is filled in the cells 24. On the other hand, the raw material gas 30 can also pass through the cells 24 in which the surfaces of the partition walls 23 are coated with the conductor and / or magnetic material 5 a, and in the embodiment in which the surfaces are coated with the conductor and / or magnetic material 5 a, the passage resistance of the raw material gas 30 can be reduced compared to the embodiment in which the cells 24 are filled with the conductor and / or magnetic material 5 a.

[0088] 11 shows an embodiment in which the conductor and / or magnetic material 5a is present inside the partition walls 23. The honeycomb structure part 21 (partition walls 23) is usually formed of a ceramic material such as cordierite. By manufacturing the honeycomb structure part 21 in a state in which the conductor and / or magnetic material 5a is mixed with or coated on the ceramic material, the conductor and / or magnetic material 5a can be present inside the partition walls 23. By adopting such an embodiment, it becomes possible for the partition walls 23 to function as a heater in the honeycomb structure 20.

[0089] The conductor and / or magnetic material 5a may contain at least one selected from the group consisting of Fe, Cr, Ni, Mn, Zn, Co, Cu, and Si. As the conductor and / or magnetic material 5a, for example, the balance Co-20 mass% Fe, the balance Co-25 mass% Ni-4 mass% Fe, the balance Fe-15 to 35 mass% Co, the balance Fe-17 mass% Co-2 mass% Cr-1 mass% Mo, the balance Fe-49 mass% Co-2 mass% V, the balance Fe-18 mass% Co-10. Mass%Cr-2mass%Mo-1mass%Al, balance Fe-27mass%Co-1mass%Nb, balance Fe-20mass%Co-1mass%Cr-2mass%V , balance Fe-35% by mass Co-1% by mass Cr, pure cobalt, pure iron, electromagnetic soft iron, balance Fe-0.1 to 0.5% by mass Mn, balance Fe-3% by mass Si, balance Part Fe-6.5% by mass Si, remainder Fe-18% by mass Cr, remainder Fe-16% by mass Cr-8% by mass Al, remainder Ni-13% by mass Fe-5.3% by mass Mo, balance Fe-45% by mass Ni, balance Fe-10% by mass Si-5% by mass Al, balance Fe-36% by mass Ni, balance Fe-45% by mass Ni, balance Fe Metals such as -35% by mass Cr, balance Fe-13% by mass Cr-2% by mass Si, balance Fe-20% by mass Cr-2% by mass Si-2% by mass Mo, balance Fe-20% by mass Co-1% by mass V, balance Fe-13% by mass Cr-2% by mass Si, balance Fe-17% by mass Co-2% by mass Cr-1% by mass Mo. The conductor and / or magnetic material 5a may also be an oxide such as Mn-Zn ferrite, Cu-Zn ferrite, Ni-Zn ferrite, Cu-Zn-Mg ferrite, etc. Each of these conductors and / or magnetic materials 5a has a different Curie point, and is selected appropriately depending on the heating temperature required for the reaction and synthesis of the gas.

[0090] At least one of the one or more honeycomb structure portions 21 may contain a catalyst. Examples of the catalyst include atoms such as Pt, Pd, Ni, La, Ce, Ru, Co, and Fe, and / or compounds such as metal oxides such as MnO2, SnO2, and TiO2. The catalyst may be fixed to the honeycomb structure portion 21 in a state where it is fixed to the surface of a material such as Al2O3 particles, or may be fixed directly on the honeycomb structure portion 21. The catalyst may be provided in the reaction cell 6.

[0091] The induction heating coil 25 is disposed on the outer periphery of the honeycomb structure 20. The induction heating coil 25 may be formed by winding a conductor 250 around a predetermined axis. The axis of the induction heating coil 25 may be parallel to the axial direction AD of the honeycomb structure 20. The axis may be coaxial with the central axis of the honeycomb structure 20. While FIG. 1 shows a band-shaped conductor 250 with a rectangular cross section, the conductor 250 may have any shape, such as a circular or tubular shape. The conductor 250 may be molded with an insulating material 251. Examples of the insulating material 251 that can be used include alumina, mullite, and / or heat-resistant resin. FIG. 1 shows an embodiment in which the conductor 250 molded with the insulating material 251 is fitted onto the outer surface of the outer wall 22 of the honeycomb structure 20.

[0092] A power supply circuit 8 is connected to the induction heating coil 25. As shown in FIG. 7 , the power supply circuit 8 may include a DC power supply 80, an inverter 81, a transformer 82, and a resonant capacitor 83. DC power from the DC power supply 80 is converted to AC power by the inverter 81. The transformer 82 is used when it is necessary to amplify the current flowing through the induction heating coil 25. The transformer 82 has a primary coil 82a connected to the inverter 81 and a secondary coil 82b connected to the resonant capacitor 83 and the induction heating coil 25. The turns ratio of the primary coil 82a to the secondary coil 82b is N:1, where N is a number greater than 1, and the transformer 82 can amplify the AC power current. The capacitance of the resonant capacitor 83 is set to adjust the resonant frequency of the power supply circuit 8. The induction heating coil 25 is connected in series to the resonant capacitor 83 and may be connected to both ends of the secondary coil 82b together with the resonant capacitor 83.

[0093] When an alternating current is supplied from the power supply circuit 8 to the induction heating coil 25, a magnetic flux is generated in the vicinity of the induction heating coil 25. The honeycomb structure 20 and the conductor and / or magnetic body 5a can be induction heated by the magnetic flux from the induction heating coil 25.

[0094] By selecting the Curie point of the conductor and / or magnetic material 5a, the heating temperature of the conductor and / or magnetic material 5a by induction heating can be adjusted. The conductor and / or magnetic material 5a is heated for the purpose of reacting and synthesizing the raw material gas 30, but if the temperature rises too high, problems such as the catalyst falling outside its optimal operating temperature range or a decrease in the specific surface area of ​​the catalyst or the material supporting the catalyst may occur, resulting in early deterioration of the catalytic function. By selecting a conductor and / or magnetic material 5a with a low Curie point, such problems can be suppressed. The conductor and / or magnetic material 5a may have a Curie point of 100°C or higher. The Curie point of the conductor and / or magnetic material 5a is preferably 200°C or higher.

[0095] The gas reaction synthesis unit 2 may further include a magnetic shield 26 arranged around the outer periphery of the induction heating coil 25. The magnetic shield 26 may be arranged to surround the induction heating coil 25. The magnetic shield 26 may be made of a magnetic material. In the illustrated embodiment, the magnetic shield 26 is a tubular member that is arranged around the outer periphery of the induction heating coil 25 and has wall portions that protrude radially inward at both ends. The length of the magnetic shield 26 in the axial direction of the induction heating coil 25 may be longer than the length of the induction heating coil 25 in the same direction. By providing such a magnetic shield 26, heat generation by the induction heating coil 25 can be suppressed.

[0096] As shown in FIG. 8 , a glass or crystalline body 27 containing Al and / or Si may be disposed between the honeycomb structure 20 and the induction heating coil 25. Alternatively, a glass or crystalline body 27 containing Al and / or Si may be disposed between the induction heating coil 25 and the magnetic shield 26. By disposing the glass or crystalline body 27 containing Al and / or Si (hereinafter simply referred to as "crystal body 27") in these positions, electrical short circuits between the honeycomb structure 20, the induction heating coil 25, and the magnetic shield 26 can be prevented, and components such as moisture contained in the gas flowing through the honeycomb structure 20 can be prevented from coming into contact with the induction heating coil 25. While FIG. 8 shows the crystal body 27 as a rectangular frame body surrounding the honeycomb structure portion 21, etc., the crystal body 27 may have other shapes. For example, the crystal body 27 may be a plate-like body overlapping only one side of the honeycomb structure portion 21, etc. Note that while FIG. 8 exaggerates the distance between the honeycomb structure 20 and the induction heating coil 25, this is merely for ease of understanding.

[0097] The honeycomb structure 20 may have only one honeycomb structure portion 21, or may have a plurality of honeycomb structure portions 21 as shown in Fig. 2. Fig. 2 shows an embodiment in which three rectangular parallelepiped honeycomb structure portions 21 extending long in the axial direction AD (gas flow direction) are arranged in parallel. Two induction heating coils 25 are provided for each honeycomb structure portion 21, and one magnetic shield 26 is provided to surround the entire three honeycomb structure portions 21. The two induction heating coils 25 are arranged at the front and rear of the honeycomb structure portion 21 in the axial direction AD.

[0098] One of the parallelly arranged honeycomb structure sections 21 is referred to as the first honeycomb structure section, and the one arranged adjacent to the first honeycomb structure section is referred to as the second honeycomb structure section. When the first honeycomb structure section has the conductor and / or magnetic material 5a as described above, the multiple cells 24 in the second honeycomb structure section do not need to include reaction cells 6. This is because the second honeycomb structure section can be heated by heat generated in the first honeycomb structure section. Second honeycomb structure sections without reaction cells 6 may be arranged on both sides of a first honeycomb structure section with reaction cells 6, or first honeycomb structure sections with reaction cells 6 may be arranged on both sides of a second honeycomb structure section without reaction cells 6. The configuration of the second honeycomb structure section may be the same as that of the honeycomb structure section 21 described above, except that it does not have reaction cells 6.

[0099] Furthermore, multiple honeycomb structure sections 21 may be arranged in series in the axial direction AD. One of the multiple honeycomb structure sections 21 arranged in series is called the upstream honeycomb structure section, and the one arranged downstream of the upstream honeycomb structure section in the gas flow direction is called the downstream honeycomb structure section. When the upstream honeycomb structure section has a reaction cell 6 as described above, the downstream honeycomb structure section does not need to have a reaction cell 6. This is because the downstream honeycomb structure section can be heated by heat generated in the upstream honeycomb structure section. The configuration of the downstream honeycomb structure section may be the same as the configuration of the honeycomb structure section 21 described above, except that it does not have a reaction cell 6.

[0100] Embodiment 2. Fig. 12 is an explanatory diagram showing a gas reaction synthesis apparatus 1 and a gas reaction synthesis unit 2 according to embodiment 2 of the present invention, Fig. 13 is a perspective view showing the honeycomb structure 21 of Fig. 12, the reaction cells 6, and the openings 7a communicating with the cooling cells 7, Fig. 14 is a cross-sectional view of the honeycomb structure 21 of Fig. 13, and Fig. 15 is a cross-sectional view showing a modified example of the honeycomb structure 21 of Fig. 14.

[0101] As particularly shown in Figure 13, the honeycomb structure part 21 has a first surface S1 and a second surface S2 which are different from each other and arranged in non-opposing positions, and the reaction cell 6 opens on the first surface S1, and an opening 7a communicating with the cooling cell 7 is provided on the second surface S2.

[0102] The first surface S1 may be a surface intersecting, preferably perpendicular to, the extension direction 24E of the plurality of cells 24. The first surface S1 may be one end surface of the honeycomb structure section 21 relating to the extension direction 24E of the plurality of cells 24. The honeycomb structure section 21 of the second embodiment is a columnar body (rectangular column shape) with a square end surface, and the second surface S2 is a surface adjacent to the first surface S1. When the direction in which the reaction cells 6 extend at the end surface of the honeycomb structure section 21 is defined as the second width direction 21W2 and the direction perpendicular to the second width direction 21W2 is defined as the first width direction 21W1, the second surface S2 may be a surface extending from an end of the first surface S1 relating to the first width direction 21W1. The extension width of the openings 7 a in the second width direction 21W2 may be 50% or more, or 75% or more, of the extension width of the second surface S2 in the second width direction 21W2, and may be 100% excluding the outer peripheral wall 22. However, when the honeycomb structure portion 21 is a columnar body having polygonal end faces with many angles (pentagon, hexagon, heptagon, octagon, etc.), the second surface S2 may be a surface located at a position separated from the first surface S1 in the circumferential direction of the honeycomb structure portion 21.

[0103] The end faces of the honeycomb structure section 21 may be provided with plugging sections 28 arranged at the positions of the cooling cells 7. The outer peripheral wall 22, the plugging sections 28, and the permeation suppressing partition walls 232 define an internal space 28a arranged between the cooling cells 7 and the openings 7a communicating with the cooling cells 7. The cooling gas 40 from the openings 7a can be introduced into the cooling cells 7 through the internal space 28a. The cooling gas 40 does not need to be parallel to or opposite to the direction in which the raw material gas 30 flows in the reaction cells 6 during the process from the openings 7a to the cooling cells 7.

[0104] The end portions 7b of the cooling cells 7 in the extension direction 24E of the multiple cells 24 may be aligned along the width direction 21W (first width direction 21W1) of the honeycomb structure section 21 as shown in Fig. 14, or may be arranged at an angle with respect to the width direction 21W so that the cooling cells 7 on the central side in the width direction 21W of the honeycomb structure section 21 are longer and the cooling cells 7 on the outer sides are shorter as shown in Fig. 15. The other configurations are the same as those in the first embodiment.

[0105] Embodiment 3. Fig. 16 is an explanatory diagram showing a gas reaction synthesis apparatus 1 and a gas reaction synthesis unit 2 according to embodiment 3 of the present invention, Fig. 17 is a perspective view showing the honeycomb structure 21 of Fig. 16, and the openings 7a communicating with the reaction cells 6 and the cooling cells 7, Fig. 18 is a cross-sectional view of the honeycomb structure 21 of Fig. 17, and Fig. 19 is a cross-sectional view showing a modified example of the honeycomb structure 21 of Fig. 17.

[0106] In the second embodiment, the second surface S2 provided with the opening 7a communicating with the cooling cell 7 is described as a surface extending from an end of the first surface S1 in the first width direction 21W1. However, as shown in FIG. 17 , the second surface S2 provided with the opening 7a communicating with the cooling cell 7 may be a surface extending from an end of the first surface S1 in the second width direction 21W2. The opening 7a communicating with the cooling cell 7 may be arranged on the second surface S2 at a distance in the first width direction 21W1 so as to avoid the reaction cell 6. The extension width of the opening 7a in the first width direction 21W1 may be less than 50% of the extension width of the second surface S2 in the first width direction 21W1. The other configurations are the same as those of the first and second embodiments.

[0107] Embodiment 4. Figure 20 is an explanatory diagram showing a gas reaction synthesis apparatus 1 and a gas reaction synthesis unit 2 according to embodiment 4 of the present invention, Figure 21 is a front view showing the honeycomb structure 21 of Figure 20, Figure 22 is a back view showing the honeycomb structure 21 of Figure 20, Figure 23 is a front view showing a modified example of the honeycomb structure 21 of Figure 21, Figure 24 is a back view showing a modified example of the honeycomb structure 21 of Figure 21, Figure 25 is a perspective view showing the honeycomb structure 21, reaction cells 6 and cooling cells 7 of Figure 20, and Figure 26 is a perspective view showing the honeycomb structure 21, reaction cells 6 and cooling cells 7 of Figure 20 when viewed from the opposite direction to that of Figure 25.

[0108] In the first to third embodiments, the first raw material gas 31 and the second raw material gas 32 are described as being introduced into the honeycomb structure portion 21, etc. (gas reaction synthesis apparatus 1 and gas reaction synthesis unit 2) in a premixed state. However, the first raw material gas 31 and the second raw material gas 32 may be introduced separately into the honeycomb structure portion 21, etc., and mixed in the gas reaction synthesis unit 2. That is, as shown in FIGS. 20 to 26 , the reaction cell 6 may include a first reaction cell 61 into which the first raw material gas 31 is introduced, and a second reaction cell 62 into which the second raw material gas 32 is introduced. The first reaction cell 61 and the second reaction cell 62 are separate cells 24 separated by a partition wall 23. In the present embodiment, the first reaction cell 61 and the second reaction cell 62 are open on one side of the honeycomb structure portion 21 (the front side shown in FIG. 21 ). The first reaction cell 61 may be plugged by plugging portions 61a on the other surface (the back surface shown in FIG. 22) of the honeycomb structure portion 21. In the drawing, the second reaction cell 62 is shown with a darker shade than the first reaction cell 61.

[0109] In the illustrated embodiment, the second reaction cell 62 is disposed outside the first reaction cell 61 in the width direction 21W of the honeycomb structure section 21, and is configured so that the first raw material gas 31 in the first reaction cell 61 passes through the partition wall 23 and enters the second reaction cell 62. This can be achieved by setting the pressure of the first raw material gas 31 in the first reaction cell 61 higher than the pressure of the second raw material gas 32 in the second reaction cell 62. In this case, it is preferable to use at least a portion of the outer second raw material gas 32 as the cooling gas 40. This is because even if the permeation-restricting partition wall 232 is imperfect, this is unlikely to cause any problems. Conversely, the second raw material gas 32 in the outer second reaction cell 62 may be configured so that it passes through the partition wall 23 and enters the first reaction cell 61. When the cooling gas 40 is reused as the source gas 30, from the viewpoint of preventing contamination of the source gas 30, it is possible to eliminate internal and external restrictions by setting the pressures in the following order: cooling gas 40 pressure > first source gas 31 pressure > second source gas 32 pressure. If the cell through which the cooling gas 40 flows does not contain a catalyst, it can also be used only for cooling.

[0110] The partition wall 23 may include a permeability coefficient control partition wall 233 that is located between the first reaction cell 61 and the second reaction cell 62 and is configured so that the permeability coefficients of the first source gas 31 and the second source gas 32 change in the extension direction 24E of the multiple cells 24. By including such a permeability coefficient control partition wall 233 in the partition wall 23, it is possible to control the progress of mixing of the first source gas 31 and the second source gas 32 in the gas reaction synthesis unit 2. In the drawing, the permeability coefficient control partition wall 233 is shown with a lighter shade than the permeation suppressing partition wall 232.

[0111] The permeability coefficient of the permeability coefficient control partition 233 (mol m (s m 2 ・Pa) -1 ) is the gas permeation amount (mol), wall thickness (m), pressure difference (Pa), permeation area (m 2 ) and the measurement time (s).

[0112] The permeability coefficients at the inlet sides (sides where the first source gas 31 and the second source gas 32 are introduced) of the first reaction cell 61 and the second reaction cell 62 may be set lower than the permeability coefficients at the outlet sides (sides where the first source gas 31 and the second source gas 32 exit) of the first reaction cell 61 and the second reaction cell 62. By setting the permeability coefficients at the inlet sides lower than the permeability coefficients at the outlet sides, it is possible to prevent the mixing of the first source gas 31 and the second source gas 32 from concentrating on the inlet side, and it is possible to suppress the amount of heat generated at the inlet side.

[0113] The permeability coefficient at the inlet side is calculated by the gas permeation amount (mol), pressure difference (Pa), and permeation area (m 2 ), and measurement time (s), and the gas permeation amount (mol), pressure difference (Pa), and permeation area (m 2 ) and the measurement time (s).

[0114] When the pressures of the first source gas 31 and the second source gas 32 are the same, the permeability coefficient at the inlet side is preferably, for example, 0.8 times or less than the permeability coefficient at the outlet side. This more reliably prevents the mixing of the first source gas 31 and the second source gas 32 from concentrating on the inlet side. The permeability coefficient at the inlet side is more preferably, for example, 0.65 times or less, and even more preferably, 0.5 times or less, the permeability coefficient at the outlet side. The permeability coefficient at the inlet side is, for example, 0.01 mol / (m 2 s Pa) etc.

[0115] The permeability coefficient of the permeability coefficient control partition 233 may change continuously or stepwise in the stretching direction 24E of the cell 24. The permeability coefficient of the permeability coefficient control partition 233 may change in proportion to the distance from the inlet side or the outlet side.

[0116] Although not specifically shown, the permeability coefficient control partition walls 233 may have a partition wall body and a permeability coefficient control film provided on the surface of the partition wall body. The partition wall body may be formed of the same material as the honeycomb structure portion 21 (the outer peripheral wall 22 and the partition walls 23). The permeability coefficient control film may contain at least one of ceramics, metal, and organic material. More specifically, the permeability coefficient control film must be a material that is not corroded by the raw material gas and reaction products, and may be formed of materials such as cordierite, mullite, alumina, spinel, silicon carbide, silicon, silicic acid, silicon nitride, aluminum titanate, SiO2, and metal particles such as Fe—Cr—Al. The permeability coefficient control film may be provided on the surface of the partition wall body by any method. The permeability coefficient control partition walls 233 are formed by the method described below. Note that the method described below is an example of a more specific manufacturing method. First, the side opposite to the reaction gas inlet side of the cells 24 constituting the permeability control partition walls 233 of the gas reaction synthesizer (honeycomb structure 20) is plugged, and a gaseous permeability control film raw material containing a powder such as a cordierite raw material is introduced from the reaction gas inlet side. Examples of the powder contained in the permeability control film raw material include a cordierite raw material having a particle size distribution in the range of 0.5 to 6 μm and an average particle size (D50) of 0.5 μm. By injecting the gaseous permeability control film raw material into the cells 24, the suspended permeability control film raw material (powder such as cordierite raw material) is deposited on the surfaces of the partition walls 23 and in the pores inside the partition walls 23, forming a layer (permeability control film) made of the permeability control film raw material on the surfaces and inside the partition walls 23. Immediately after being blown in, the permeability control membrane raw material adheres to the cells 24 that constitute the permeability control partition walls, and as the raw material particles accumulate, the permeability resistance of the partition walls 23 that constitute the permeability control partition walls 233 increases.

[0117] The permeability coefficient of the permeability coefficient control partition 233 may be changed by at least one of changing the thickness of the partition body in the extension direction 24E of the plurality of cells 24, changing the thickness of the permeability coefficient control film in the extension direction 24E of the plurality of cells 24, and changing the density of the permeability coefficient control film in the extension direction 24E of the plurality of cells 24.

[0118] The thickness of the partition wall body can be determined by measurement using, for example, a microscope or a scanning electron microscope (SEM). The thickness of the permeability coefficient control film can be determined by measurement using an SEM. The density of the permeability coefficient control film can be determined by observing a cross section of the permeability coefficient control partition wall 233 using an SEM and processing the image. Other configurations are the same as those of the first to third embodiments.

[0119] Embodiment 5. Figure 27 is an explanatory diagram showing a gas reaction synthesis apparatus 1 and a gas reaction synthesis unit 2 according to embodiment 5 of the present invention. Figure 28 is a perspective view showing the honeycomb structure 21, the reaction cells 6, and the openings 7a communicating with the cooling cells 7 of Figure 27. Figure 29 is a perspective view showing the honeycomb structure 21, the reaction cells 6, and the openings 7a communicating with the cooling cells 7 of Figure 27 when viewed from the opposite direction to Figure 28. When the reaction cells 6 include a first reaction cell 61 and a second reaction cell 62 as in embodiment 4, the first reaction cell 61 and the second reaction cell 62 may be open on the first surface S1, and the openings 7a communicating with the cooling cell 7 may be provided on the second surface S2 (see Figures 27 to 29). The other configurations are the same as those of embodiments 1 to 4.

[0120] Embodiment 6. Figure 30 is an explanatory diagram showing a gas reaction synthesis apparatus 1 and a gas reaction synthesis unit 2 according to embodiment 6 of the present invention, Figure 31 is a perspective view showing the openings 7a communicating with the honeycomb structure portion 21, reaction cells 6, and cooling cells 7 of Figure 30, and Figure 32 is a perspective view showing the openings 7a communicating with the honeycomb structure portion 21, reaction cells 6, and cooling cells 7 of Figure 30 when viewed from the opposite direction to Figure 31. In embodiments 4 and 5, the first reaction cell 61 and the second reaction cell 62 have been described as opening on the same surface (first surface S1) of the honeycomb structure portion 21. However, the first reaction cell 61 and the second reaction cell 62 may open on different surfaces.

[0121] 31 , the honeycomb structure section 21 has a first surface S1, a second surface S2, and a third surface S3 that are different from one another and arranged in non-opposing positions, the first reaction cell 61 may be open on the first surface S1, an opening 7a communicating with the cooling cell 7 may be provided on the second surface S2, and the second reaction cell 62 may be open on the third surface S3. The third surface S3 may be a surface adjacent to the first surface S1 and the second surface S2. When the direction in which the reaction cells 6 extend on the end face of the honeycomb structure section 21 is defined as the second width direction 21W2, the third surface S3 on which the second reaction cell 62 opens may be a surface extending from the end of the first surface S1 in the second width direction 21W2. Although not shown, when the direction perpendicular to the second width direction 21W2 is defined as the first width direction 21W1, the third surface S3 into which the second reaction cell 62 opens may be a surface extending from the end of the first surface S1 in the first width direction 21W1. The other configurations are the same as those of Embodiments 1 to 5.

[0122] Seventh Embodiment Fig. 33 is a perspective view showing a gas reaction synthesis unit 2 according to a seventh embodiment of the present invention. As shown in Fig. 33, the honeycomb structure section 21 may include one or more first honeycomb structure sections 211 each provided with a reaction cell 6, and one or more second honeycomb structure sections 212 each provided with a cooling cell 7. In the illustrated embodiment, one first honeycomb structure section 211 is arranged between two second honeycomb structure sections 212. However, the number and arrangement of the first honeycomb structure sections 211 and the second honeycomb structure sections 212 may be changed as desired.

[0123] The first honeycomb structure portion 211 and the second honeycomb structure portion 212 may be bonded together with a bonding material having high thermal conductivity, such as a paste containing a copper-based, Ag-based, Ag-Pd-based, or Au-based material. A carbon paste or sheet may also be used as the bonding material.

[0124] The heating cells 5 may be provided in the first honeycomb structure portion 211 in which the reaction cells 6 are provided. Although not shown, the honeycomb structure portion 21 may additionally or alternatively have a third honeycomb structure portion in which the heating cells 5 are provided. Other configurations are the same as those of the first to sixth embodiments.

[0125] Although the preferred embodiments of the present invention have been described in detail above with reference to the accompanying drawings, the present invention is not limited to these examples. It is clear that a person skilled in the art to which the present invention pertains can conceive of various modifications and alterations within the scope of the technical ideas set forth in the claims, and it is understood that these also naturally fall within the technical scope of the present invention.

[0126] The present invention will be described in more detail below with reference to examples, but the present invention is not limited to these examples.

[0127] Example 1 The present inventors prepared the gas reaction synthesis apparatus 1 and the gas reaction synthesis unit 2 described in the first embodiment, and synthesized hydrocarbons by reacting carbon monoxide (CO) with hydrogen (H) by the Fischer-Tropsch process.

[0128] The honeycomb structure 21 of the gas reaction synthesis unit 2 was 150 mm x 150 mm x 200 mm. The thickness of the partition walls 23 was about 0.3 mm, and the opening of the cells 24 was 0.97 mm (wall thickness 12 mil, cell density 400 cpsi).

[0129] As shown in Figure 3, when the end face of the honeycomb structure section 21 is viewed from the front, cooling regions R2 are arranged at both ends (top and bottom in the figure) of the honeycomb structure section 21 in the first width direction 21W1, and a reaction region R1 is arranged in the center in the first width direction 21W1. The heating cells 5 are arranged so as to extend linearly in the second width direction 21W2 at the center position of the reaction region R1 in the first width direction 21W1. The number of cooling cells 7 is twice the number of reaction cells 6, and the number of heating cells 5 is one-third the number of reaction cells 6. When the end face of the honeycomb structure section 21 is viewed from the front, the dimensions of the heating cells 5, reaction cells 6, and cooling cells 7 are the same.

[0130] To easily achieve a uniform temperature distribution, Si-bonded SiC was used as the material for the honeycomb structure 20. The heating cells 5 accounted for 16% of the total number of cells, the reaction cells 6 accounted for 33% of the total number of cells, and the cooling cells 7 accounted for 51% of the total number of cells. The internal surface area of ​​each cell was 720 cm 2 , 1,485 cm2 , 2,295 cm 2 This becomes:

[0131] Before starting the introduction of the raw material gas 30, the temperature of the reaction cell 6 was raised by induction heating to the reaction initiation temperature (250°C) of the raw material gas 30. After the temperature of the reaction cell 6 was raised, the induction heating was stopped, and the raw material gas 30 and the cooling gas 40 were introduced into the reaction cell 6 and the cooling cell 7.

[0132] A mixture of carbon monoxide (CO) and hydrogen (H) was introduced into the reaction cell 6 as the raw material gas 30. The temperature of the raw material gas 30 when introduced into the reaction cell 6 was 100°C, and the pressure of the raw material gas 30 was 25 atmospheres. The flow rate of the raw material gas 30 was 1 (m 3 In general, the calorific value (energy released in the synthesis) generated in the synthesis of carbon monoxide (CO) and hydrogen (H2) is said to be 150 to 167 kJ / mol.

[0133] As the cooling gas 40, carbon monoxide (CO) was used as the raw material gas 30 before being introduced into the reaction cell 6. The temperature of the cooling gas 40 when introduced into the cooling cell 7 was 100°C. The flow rate of the cooling gas 40 was 0.5 (m 3 / s).

[0134] As a result, the reaction was initiated efficiently using only the amount of heat needed to heat the honeycomb structure 20, without using energy to heat the entire gas reaction synthesis apparatus 1. Furthermore, the heat generated by the reaction was effectively used as a heat source for the raw material gas 30. In other words, by using the temperature of the raw material gas 30 to prevent excessive heat generation, it was possible to maintain the reaction under temperature conditions that allowed the target hydrocarbons to be obtained efficiently. This confirmed that the induction heating device (heating cell 5) and cooling channel (cooling cell 7) were functioning effectively.

[0135] (Comparative Example 1) As described above, in Example 1, the number of cooling cells 7 is twice the number of reaction cells 6. As Comparative Example 1, the inventors prepared a gas reaction synthesis apparatus 1 and a gas reaction synthesis unit 2 in which the number of cooling cells 7 was the same as the number of reaction cells 6, and synthesized hydrocarbons by reacting carbon monoxide (CO) with hydrogen (H2) by the Fischer-Tropsch process in the same manner as in Example 1. Example 1 and Comparative Example 1 are the same except for the number of cooling cells 7. Note that Example 1 satisfies the relationship expressed by the following formula 1, while Comparative Example 1 does not. Amount of reaction heat per unit gas flow rate in exothermic reaction × mixed flow rate of raw material gas 30 × amount of heat transferred to honeycomb structure 20 per unit flow rate of raw material gas 30 ≦ amount of heat transferred from honeycomb structure 20 to cooling gas 40 per unit time, unit flow rate, and unit area × flow rate of cooling gas 40 (Formula 1)

[0136] In Comparative Example 1, as in Example 1, the reaction was efficiently initiated using only the heat required to heat the honeycomb structure 20, without using energy to heat the entire reactor. However, when the heat generated by the reaction was reused as a heat source for the raw material gas 30, the temperature of the raw material gas 30 deviated from the optimum point for the reaction, and the target hydrocarbons could not be efficiently obtained. This confirmed that the reaction gas can be efficiently obtained by satisfying the relationship in Equation 1.

[0137] Example 2 The present inventors prepared the gas reaction synthesis apparatus 1 and the gas reaction synthesis unit 2 described in the fourth embodiment, and synthesized hydrocarbons by reacting carbon dioxide (CO2) as the first raw material gas 31 with hydrogen (H2) as the second raw material gas 32 in the Sabatier reaction.

[0138] The dimensions of each part of the honeycomb structure 21 of the gas reaction synthesis unit 2 are the same as those in the first embodiment.

[0139] The arrangement and number of the heating cells 5, reaction cells 6 and cooling cells 7 are the same as in Example 1. In the reaction cells 6, the number of the first reaction cells 61 is twice the number of the second reaction cells 62.

[0140] The permeability coefficient control partition wall 233 between the first reaction cell 61 and the second reaction cell 62 was formed as follows. That is, in a honeycomb fired body (element of the honeycomb structure portion 21) provided with the reaction cells 6 and the cooling cells 7, a film-forming gas such as nitrogen gas mixed with SiO fine particles was flowed into the first reaction cell 61 or the second reaction cell 62 located at the boundary between the first reaction cell 61 and the second reaction cell 62, thereby providing a permeability coefficient control film made of SiO fine particles on the surface of the partition wall body, thereby forming the permeability coefficient control partition wall 233. At this time, the permeability coefficient control film was formed thicker on the side where the film-forming gas was introduced. With respect to the flow direction of the first raw material gas 31 and the second raw material gas 32, the thickness of the permeability coefficient control membrane on the inlet side of the first reaction cell 61 and the second reaction cell 62 is made thicker than the thickness of the permeability coefficient control membrane on the outlet side, thereby making the permeability coefficient on the inlet side lower than the permeability coefficient on the outlet side, so that the first raw material gas 31 and the second raw material gas 32 are gradually mixed.

[0141] In the Sabatier reaction, 4 mol of hydrogen (H) is required for 1 mol of carbon dioxide (CO), so the pressure of hydrogen (H) was set to twice the pressure of carbon dioxide (CO) in consideration of introducing it into twice the cell 24.

[0142] Before starting the introduction of the first source gas 31 and the second source gas 32, the temperatures of the first reaction cell 61 and the second reaction cell 62 were raised by induction heating to the reaction initiation temperature (400° C.) of the first source gas 31 and the second source gas 32. After the temperatures of the first reaction cell 61 and the second reaction cell 62 were raised, the induction heating was stopped, and the first source gas 31, the second source gas 32, and the cooling gas 40 were introduced into the first reaction cell 61, the second reaction cell 62, and the cooling cell 7.

[0143] The temperature of the first source gas 31 (carbon dioxide) when introduced into the first reaction cell 61 was 400° C. The flow rate of the first source gas 31 was 1 m 3 The temperature of the second source gas 32 (hydrogen) when introduced into the second reaction cell 62 was 400° C. The flow rate of the second source gas 32 was 2 m 3 / s.

[0144] The cooling gas 40 was hydrogen, which was the second source gas 32. The temperature of the cooling gas 40 when introduced into the cooling cell 7 was 100° C. The flow rate of the cooling gas 40 was 2 m 3 / s. The temperature of the cooling gas 40 is increased by using part of the temperature of the reaction gas as residual heat for the cooling gas 40. By reducing the temperature difference between the reaction gas and the cooling gas 40, damage to the honeycomb structure portion 21 due to thermal stress can be suppressed.

[0145] As a result, the reaction was initiated efficiently using only the amount of heat needed to heat the honeycomb structure 20, without using energy to heat the entire gas reaction synthesis apparatus 1. Furthermore, the heat generated by the reaction was effectively used as a heat source for the raw material gas 30. In other words, by using the temperature of the raw material gas 30 to prevent excessive heat generation, it was possible to maintain the reaction under temperature conditions that allowed the target hydrocarbons to be obtained efficiently. This confirmed that the induction heating device (heating cell 5) and cooling channel (cooling cell 7) were functioning effectively.

[0146] 1: Gas reaction synthesis apparatus 2: Gas reaction synthesis unit 20: Honeycomb structure 21: Honeycomb structure part 22: Permeable wall 23: Partition wall 231: Permeable partition wall 232: Permeation suppressing partition wall 233: Permeability coefficient controlling partition wall 24: Cell 25: Induction heating coil 26: Magnetic shield 3: Raw material gas supply source 30: Raw material gas 31: First raw material gas 32: Second raw material gas 4: Cooling gas supply source 40: Cooling gas 5: Heating cell 5a: Magnetic body 6: Reaction cell 61: First reaction cell 62: Second reaction cell 7: Cooling cell 7a: Opening 8: Power supply circuit R1: Reaction region R2: Cooling region

Claims

1. A gas reaction synthesis unit for synthesizing raw material gases by reacting them, comprising a honeycomb structure having one or more honeycomb structure sections each having an outer peripheral wall and partition walls disposed inside the outer peripheral wall to define a plurality of cells that form flow paths extending from one end face to the other end face, wherein in at least one of the one or more honeycomb structure sections, the plurality of cells include a heating cell containing a conductor and / or a magnetic material, a reaction cell through which the raw material gas is flowed, and a cooling cell through which a cooling gas is flowed.

2. The gas reaction synthesis unit according to claim 1, wherein the reaction of the raw material gas is an exothermic reaction, and the ratio (RA / CA) of the surface area (RA) of the reaction cell in contact with the raw material gas to the surface area (CA) of the cooling cell in contact with the cooling gas is set to satisfy the relationship: reaction heat amount per unit gas flow rate in the exothermic reaction × mixed flow rate of raw material gas × amount of heat transfer to the honeycomb structure per unit flow rate of raw material gas ≦ amount of heat transfer from the honeycomb structure to the cooling gas per unit time, unit flow rate and unit area × flow rate of the cooling gas.

3. The gas reaction synthesis unit according to claim 2, wherein the reaction region in which the reaction cell is provided is adjacent to a pair of cooling regions in which the cooling cell is provided, and the heating cell is provided within the reaction region.

4. The gas reaction synthesis unit according to claim 3, wherein the partition walls include: a permeable partition wall configured to allow the source gas and the cooling gas to pass through; and a permeation-restricting partition wall located between the cooling region and the reaction region and configured to restrict the permeation of the source gas and the cooling gas compared to the permeable partition wall.

5. The gas reaction synthesis unit according to claim 4, wherein the wall thickness of the permeation-restricting partition walls is set to be thicker than the wall thickness of the permeable partition walls, and / or a material that restricts the flow of the source gas and the cooling gas is applied to the wall surfaces or inside of the permeation-restricting partition walls.

6. The gas reaction synthesis unit according to claim 4, wherein said cooling gas contains at least a portion of said raw material gas.

7. The gas reaction synthesis unit according to claim 3, wherein the direction in which the cooling gas flows in the cooling cell is at least partially parallel to or opposite to the direction in which the raw material gas flows in the reaction cell.

8. A gas reaction synthesis unit as described in claim 3, wherein the honeycomb structure portion has first and second surfaces that are different from each other and arranged in non-opposing positions, the reaction cells are open in the first surface, and an opening communicating with the cooling cells is provided in the second surface.

9. The gas reaction synthesis unit according to claim 3, wherein the raw material gas includes a first raw material gas and a second raw material gas different from the first raw material gas, the reaction cells include a first reaction cell into which the first raw material gas is introduced and a second reaction cell into which the second raw material gas is introduced, and the partition wall is located between the first reaction cell and the second reaction cell and includes a permeability coefficient control partition wall configured to change the permeability coefficients of the first raw material gas and the second raw material gas in the extension direction of the plurality of cells.

10. The gas reaction synthesis unit according to claim 9, wherein the permeability coefficients at the inlet sides of the first reaction cell and the second reaction cell are lower than the permeability coefficients at the outlet sides of the first reaction cell and the second reaction cell.

11. The gas reaction synthesis unit according to claim 9, wherein the permeability coefficient control partition has a partition body and a permeability coefficient control film provided on the surface of the partition body.

12. The gas reaction synthesis unit according to claim 11, wherein the permeability coefficient of the permeability coefficient control partition wall is changed by at least one of changing the thickness of the partition wall body in the extension direction of the plurality of cells, changing the thickness of the permeability coefficient control membrane in the extension direction of the plurality of cells, and changing the density of the permeability coefficient control membrane in the extension direction of the plurality of cells.

13. The gas reaction synthesis unit according to claim 11, wherein the permeability control membrane comprises at least one of ceramics, metals, and organic materials.

14. The gas reaction synthesis unit according to claim 13, wherein the ceramic contained in the permeability control film includes at least one selected from the group consisting of cordierite, silicon carbide, silicon, silica, and alumina.

15. A gas reaction synthesis unit according to claim 9, wherein the honeycomb structure portion has first, second and third surfaces which are different from one another and arranged in non-opposing positions, the first reaction cell opens in the first surface, an opening communicating with the cooling cell is provided in the second surface, and the second reaction cell opens in the third surface.

16. The gas reaction synthesis unit according to claim 2, further comprising an induction heating coil arranged on the outer periphery of the honeycomb structure, and configured so that the conductor and / or magnetic material can be induction heated by magnetic flux from the induction heating coil.

17. The gas reaction synthesis unit according to claim 16, wherein the conductive and / or magnetic material is present in at least a portion of the honeycomb structure in the radial and axial directions.

18. The gas reaction synthesis unit according to claim 16, wherein the conductive and / or magnetic material is present inside the outer peripheral wall, inside the partition wall, inside the cell, and / or on the outer peripheral wall.

19. The gas reaction synthesis unit according to claim 18, wherein the conductive and / or magnetic material present inside the cell is filled in the cell or coated on the surface of the partition wall.

20. The gas reaction synthesis unit according to claim 16, further comprising a magnetic shield disposed around the outer periphery of said induction heating coil.

21. The gas reaction synthesis unit according to claim 16, wherein the honeycomb structure portion contains at least one selected from the group consisting of cordierite, silicon carbide, silicon, silica, and alumina.

22. The gas reaction synthesis unit according to claim 16, wherein the conductor and / or magnetic material contains at least one selected from the group consisting of Fe, Cr, Ni, Mn, Zn, Co, Cu, and Si.

23. The gas reaction synthesis unit according to claim 16, wherein the magnetic material has a Curie point of 100°C or higher.

24. The gas reaction synthesis unit of claim 2, wherein at least one of said one or more honeycomb structures includes a catalyst.

25. The gas reaction synthesis unit according to claim 1, wherein the honeycomb structure includes one or more first honeycomb structure parts in which the reaction cells are provided, and one or more second honeycomb structure parts in which the cooling cells are provided.

26. A gas reaction synthesis apparatus comprising: a gas reaction synthesis unit according to any one of claims 1 to 25; a raw material gas supply source connected to the reaction cell; and a cooling gas supply source connected to the cooling cell.

27. A gas reaction synthesis apparatus according to claim 26, which cites any one of claims 16 to 23, further comprising a power supply circuit connected to the induction heating coil, and which is configured so that the conductor and / or magnetic material can be inductively heated by magnetic flux from the induction heating coil before or when the raw material gas is passed through the reaction cell.

28. The gas reaction synthesis apparatus according to claim 26, wherein the source gas comprises methanol gas, carbon monoxide, carbon dioxide, hydrogen, nitrogen, and / or steam.

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