Chemical reaction method, chemical reaction device and manufacturing method

By designing a special structure of the catalyst layer, cooling surface and permeable wall in a chemical reaction device, the problem of difficulty in improving product reaction yield in the prior art is solved, and the effect of improving product yield without changing the conditional parameters is achieved.

CN115989081BActive Publication Date: 2025-04-01SUMITOMO CHEM CO LTD
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Patent Information

Application Number
CN202180052217.5
Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
Priority Date
2020-08-31
Filing Date
2021-08-30
Publication Date
2025-04-01
Estimated Expiration
2041-08-30

AI Technical Summary

Technical Problem

In the conventional chemical reaction method in which catalyst is used in the gas phase, it is difficult to increase the reaction yield of the product without changing the ratio of pressure, temperature, and catalyst amount to feed rate (W/F).

Method used

By designing a special structure of the catalyst layer, cooling surface and permeable wall in a chemical reaction device, the distance between the surface in contact with the permeable wall and the cooling surface of the catalyst layer and the height of the catalyst layer reach more than 500 mm2, thereby improving the yield of the product.

Benefits of technology

It is achieved that the reaction yield of the product is improved without changing the conditional parameters, and the bias of chemical equilibrium is enhanced, thereby advancing the process of the reaction.

✦ Generated by Eureka AI based on patent content.

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Abstract

In a chemical reaction device (100) for performing a reaction in which the yield of a product is improved and the progress of the reaction in the gas phase is constrained by the chemical equilibrium between the raw material and the product, the product of the distance L between the surface of the catalyst layer (3) in contact with the permeable wall (40) and the outer surface of the cooling surface (53) and the height H of the catalyst layer (3) corresponding to the above-mentioned outer surface having the distance L is accumulated in the height direction from one end to the other end of the cooling surface (53) to obtain a cumulative value of 500 mm 2 above.
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Description

Technical Field

[0001] The present invention relates to a chemical reaction apparatus and a chemical reaction method for performing a chemical reaction for obtaining a product from a raw material gas in a gas phase using a catalyst. Background Art

[0002] Patent Document 1 discloses a method for synthesizing methanol by reacting a raw material gas containing hydrogen and carbon monoxide or carbon dioxide as main components in the presence of a catalyst and an apparatus for the method. In the method, methanol liquefied on a cooling surface is extracted out of the reaction system, and the reaction for synthesizing methanol is carried out by exceeding the equilibrium conversion rate.

[0003] Prior art literature

[0004] Patent Literature

[0005] Patent Document 1: Japanese Patent Application Publication No. 2005-298413 (published on October 27, 2005) Summary of the invention

[0006] Problems to be solved by the invention

[0007] In a reaction method carried out in a gas phase using a catalyst, including a reaction method using the reaction apparatus described in Patent Document 1, it is known that changing the condition parameters such as the pressure, temperature and ratio of the catalyst amount to the raw material supply rate (W / F) of the reaction system helps to improve the reaction yield of the product.

[0008] An object of one embodiment of the present invention is to provide a chemical reaction method and a chemical reaction apparatus, which can improve the yield of a product by changing the internal structure of the reaction apparatus without changing the condition parameters.

[0009] Methods used to solve problems

[0010] In order to solve the above-mentioned problems, a chemical reaction method in one embodiment of the present invention is a chemical reaction method for carrying out a reaction in which a product contains a component having a higher boiling point than a component in a raw gas and the progress of the reaction in the gas phase is constrained by a chemical equilibrium between the raw material and the product, wherein a chemical reaction device is used, the chemical reaction device comprising: a catalyst layer containing a catalyst that promotes the above-mentioned reaction, a cooling surface that is arranged spaced apart from the above-mentioned catalyst layer and is maintained at a temperature below the dew point of the reaction gas generated in the above-mentioned reaction and extends in a specified direction, and a permeable wall that is arranged at a boundary between the above-mentioned catalyst layer and the above-mentioned space and through which the above-mentioned reaction gas can pass, and the product of the distance between the surface of the above-mentioned catalyst layer in contact with the above-mentioned permeable wall and the above-mentioned cooling surface and the height of the above-mentioned catalyst layer corresponding to the above-mentioned cooling surface having the distance is accumulated from one end to the other end of the above-mentioned cooling surface in the above-mentioned specified direction to obtain a cumulative value of 500 mm2 As described above, the chemical reaction is advanced by supplying the raw material gas to the catalyst layer, and a part of the product generated in the chemical reaction is condensed on the cooling surface and in the space.

[0011] A chemical reaction device according to one embodiment of the present invention is a chemical reaction device for carrying out a reaction in which a product contains a component having a higher boiling point than a component in a raw gas and the progress of the reaction in the gas phase is constrained by a chemical equilibrium between the raw material and the product, wherein the chemical reaction device comprises: a catalyst layer to which the raw gas is supplied and which contains a catalyst that promotes the reaction, a cooling surface which is arranged spaced apart from the catalyst layer, maintained at a temperature below the dew point of the reaction gas and extending in a specified direction, and a permeable wall which is arranged at a boundary between the catalyst layer and the space and through which the reaction gas generated in the reaction can pass, wherein the product of the distance between the surface of the catalyst layer in contact with the permeable wall and the outer surface of the cooling surface and the height of the catalyst layer corresponding to the outer surface having the distance is accumulated from one end to the other end of the cooling surface in the specified direction to obtain a cumulative value of 500 mm. 2 In the above, a part of the product is condensed on the surface of the cooling surface and in the space.

[0012] A chemical reaction device according to one embodiment of the present invention comprises a reaction container, wherein the reaction container comprises at least one multi-structured reaction tube, wherein a reaction is carried out in the multi-structured reaction tube so that a component having a higher boiling point than a component in a raw gas is included in the product and the progress of the reaction in the gas phase is subject to the chemical equilibrium between the raw material and the product, wherein each of the at least one reaction tube comprises: an inner tube through which a reaction gas generated in the reaction can pass, an outer tube in which the inner tube is arranged, a cooling tube arranged in the inner tube and extending in a prescribed direction, and a catalyst layer arranged between the inner tube and the outer tube, wherein the product of the distance between the surface of the catalyst layer in contact with the inner tube and the outer surface of the cooling tube and the height of the catalyst layer corresponding to the outer surface having the distance is accumulated from one end to the other end of the cooling tube in the prescribed direction to obtain a cumulative value of 500 mm 2 As described above, the temperature of the outer surface of the cooling pipe is maintained at a temperature lower than the dew point of the reaction gas, and a part of the product is condensed in the space formed between the cooling pipe and the inner cylinder.

[0013] A chemical reaction device according to one embodiment of the present invention comprises a reaction container, wherein the reaction container comprises at least one multi-structured reaction tube, wherein a reaction is carried out in the multi-structured reaction tube so that a component having a higher boiling point than a component in a raw gas is included in the product and the progress of the reaction in the gas phase is constrained by a chemical equilibrium between the raw material and the product, wherein each of the at least one reaction tube comprises: an inner cylinder through which a reaction gas generated in the reaction can pass, an outer cylinder in which the inner cylinder is arranged and extends in a prescribed direction, and a catalyst layer arranged in the inner cylinder, wherein a product of a distance between a surface of the catalyst layer in contact with the inner cylinder and an inner surface of the outer cylinder and a height of the catalyst layer corresponding to the inner surface having the distance is accumulated from one end to the other end of the inner surface in the prescribed direction to obtain a cumulative value of 500 mm 2 In the above, the temperature of the inner surface of the outer cylinder is maintained at a temperature lower than the dew point of the reaction gas, and a part of the product is condensed in the space formed between the outer cylinder and the inner cylinder.

[0014] A method for producing methanol according to one embodiment of the present invention is a method for producing methanol in which a product contains a component having a higher boiling point than a component in a raw gas and the progress of a reaction in a gas phase is subject to a chemical equilibrium between the raw material and the product, wherein the raw gas contains carbon oxides and hydrogen, and a chemical reaction device is used, the chemical reaction device comprising: a catalyst layer containing a catalyst for methanol synthesis, a cooling surface arranged in a space apart from the catalyst layer and maintained at a temperature below the dew point of the reaction gas generated in the reaction and extending in a specified direction, and a permeable wall provided at a boundary between the catalyst layer and the space and through which the reaction gas can pass, the product of the distance between the surface of the catalyst layer in contact with the permeable wall and the cooling surface and the height of the catalyst layer corresponding to the cooling surface having the distance being accumulated from one end to the other end of the cooling surface in the specified direction to obtain a cumulative value of 500 mm 2 As described above, the chemical reaction is caused to proceed by supplying the raw material gas to the catalyst layer, and a part of the reaction gas generated in the chemical reaction is condensed on the cooling surface and in the space.

[0015] Effects of the Invention

[0016] According to one embodiment of the present invention, the yield of the product can be improved by changing the internal structure of a reaction apparatus in which the progress of the reaction in the gas phase is controlled by the chemical equilibrium between the raw material and the product. BRIEF DESCRIPTION OF THE DRAWINGS

[0017] Figure 1 It is a cross-sectional view of the reaction device in Embodiment 1.

[0018] Figure 2 It is a partial schematic cross-sectional view of the reaction device of Embodiment 1.

[0019] Figure 3 It is a cross-sectional view of the reaction device of Embodiment 2.

[0020] Figure 4 It is a cross-sectional view of a reaction tube included in the reaction apparatus according to the second embodiment.

[0021] Figure 5 It is a cross-sectional view of the reaction device of embodiment 3.

[0022] Figure 6 It is a cross-sectional view of a reaction tube included in the reaction apparatus according to the third embodiment.

[0023] Figure 7 It is a graph showing the relationship between the distance L and the height H for the comparative example and Examples 1 to 5.

[0024] Figure 8 It is a graph showing the relationship between the integrated value of the product of the distance L and the height H and the methanol production rate in the comparative example and Examples 1 to 5. DETAILED DESCRIPTION

[0025] [Implementation Method 1]

[0026] (Configuration of Reaction Device 100)

[0027] Hereinafter, one embodiment of the present invention will be described in detail. Figure 1 It is a cross-sectional view of the reaction device 100 (chemical reaction device) of embodiment 1 when it is cut with a plane perpendicular to the bottom surface. The reaction device 100 is a chemical reaction device in which the product contains a component having a higher boiling point than the main component of the raw material gas 31 and the reaction in the gas phase is subject to the chemical equilibrium between the raw material and the product. It should be noted that the X-axis, Y-axis and Z-axis in the accompanying drawings specify the directions in the three-dimensional space in each of the accompanying drawings. The "height" in this specification corresponds to the length in the Z-axis direction of the accompanying drawings. Hereinafter, in this specification, the X-axis, Y-axis and Z-axis respectively represent the same direction.

[0028] In the reaction device 100, the product is condensed and recovered from the reaction container, thereby shifting the chemical equilibrium to the product side, thereby advancing the reaction. In particular, the reaction device 100 can be suitably used as a device for performing the chemical reactions represented by the following formulas (1) to (3), in which the raw material gas 31 contains carbon oxides and hydrogen, and the above-mentioned product contains methanol.

[0029]

[0030]

[0031]

[0032] When methanol is produced by the chemical reaction represented by the above formulas (1) to (3), a catalyst containing copper and zinc can be used as a catalyst for methanol synthesis (catalyst 30 described in detail below). Examples of carbon oxides used in the chemical reaction include carbon dioxide and carbon monoxide. In the chemical reaction, a gas containing at least one of carbon dioxide and carbon monoxide and hydrogen can be used as a raw material gas.

[0033] In addition to the above-mentioned methanol synthesis reaction, the reaction apparatus 100 can also be used to carry out a reaction for producing dimethyl ether or ammonia as a product.

[0034] like Figure 1 As shown, the reaction device 100 includes a reaction container 1, a first heat exchange part 22, a catalyst layer 3 in contact with the first heat exchange part 22, a permeable wall 40, and a second heat exchange part 52 arranged to be separated from the permeable wall 40 by a space 4. The permeable wall 40 is provided on the side of the catalyst layer 3 opposite to the side where the first heat exchange part 22 is located. The reaction container 1 is, for example, a pressure-resistant metal container made of stainless steel.

[0035] The first heat exchange section 22 is a heat exchanger composed of the inner wall surface of the reaction container 1 and the first heat exchange wall 20 and having a heat transfer surface 23 on the catalyst layer 3 side. A first heat medium area 2 is formed inside the first heat exchange section 22 so that the first heat medium 21 can flow. A first heat medium supply port 25 for supplying the first heat medium 21 to the first heat medium area 2 and a first heat medium recovery port 26 for discharging the first heat medium 21 from the first heat medium area 2 are formed on the first heat exchange section 22. The first heat exchange wall 20 includes a component through which fluid cannot pass, and the heat transfer surface 23 of the first heat exchange wall 20 functions as a first heat exchange surface. Figure 1 In the figure, the first heat exchange wall 20 is shown as a plate-shaped member, but its shape is not limited to a plate-shaped member. The first heat exchange wall 20 may also be formed into a corrugated surface. In addition, the shape of the first heat exchange portion 22 is also not limited to Figure 1 The shape can be a variety of shapes such as multi-tube and spiral shapes to improve the efficiency of heat exchange.

[0036] The first heat exchange part 22 can keep the heat transfer surface 23 at a temperature higher than the dew point of the reaction gas 32 by circulating the first heat medium 21 in the first heat medium region 2. When the reaction occurring in the catalyst layer 3 is an exothermic reaction, the first heat medium 21 functions as a heat medium for cooling the reaction heat generated by the reaction. When the reaction occurring in the catalyst layer 3 is an endothermic reaction, the first heat medium functions as a heat medium for applying heat to the catalyst layer 3 in order to keep the temperature of the catalyst layer 3 at or above the dew point of the reaction gas 32.

[0037] Here, the “dew point of the reaction gas 32 ” refers to the temperature at which the reaction gas 32 begins to condense when the reaction gas 32 is cooled under the condition that the reaction in the gas phase reaches chemical equilibrium at the temperature and pressure at which the reaction gas 32 exists in the catalyst layer 3 .

[0038] The dew point of the reaction gas 32 can be obtained simultaneously with the condensate composition by performing appropriate gas-liquid equilibrium calculation using a gas-liquid equilibrium model if the gas phase composition and pressure are given. In the case of a high pressure greater than 1 MPa, an expanded cubic state equation such as the Peng-Robinson equation or the Redich-Kwong-Soave equation can be used as the gas-liquid equilibrium model.

[0039] The temperature of the heat transfer surface 23 is more preferably a temperature that keeps the catalyst layer 3 as a whole at a temperature higher than the dew point of the reaction gas 32. By having the heat transfer surface 23, the reaction device 100 can keep the temperature of the catalyst layer 3 at a temperature suitable for the reaction, which can improve the efficiency of the reaction. As the first heat medium 21, when the product is methanol, for example, high-pressure boiler water at 220°C to 265°C (for example, saturated water at 2.2MPaG to 5.0MPaG), molten metal salts (for example, a mixture of sodium nitrite and potassium nitrate), and heat medium oil can be used. It should be noted that in this specification, "A to B" means above A and below B.

[0040] The second heat exchange section 52 is a heat exchanger composed of the inner wall surface of the reaction container 1 and the second heat exchange wall 50. A second heat medium area 5 is formed inside the second heat exchange section 52 for circulating the second heat medium 51. A second heat medium supply port 55 for supplying the second heat medium 51 to the second heat medium area 5 and a second heat medium recovery port 56 for discharging the second heat medium 51 from the second heat medium area 5 are formed on the second heat exchange section 52. The second heat exchange wall 50 includes a component through which the fluid cannot pass. The second heat exchange section 52 has a cooling surface 53 on the space 4 side. The cooling surface 53 extends in the Z-axis direction, and by maintaining the temperature of the reaction gas 32 below the dew point, the reaction gas 32 in the space 4 is cooled, and the product is condensed on the surface of the cooling surface 53 and in the space 4. Figure 1In the figure, the second heat exchange wall 50 is shown as a plate-shaped member, but its shape is not limited to the plate shape. That is, the cooling surface 53 can also be formed into a corrugated shape. In addition, the shape of the second heat exchange part 52 is also not limited to Figure 1 The shape can be a variety of shapes such as multi-tube and spiral shapes to improve the efficiency of heat exchange.

[0041] The second heat exchange unit 52 can maintain the temperature of the cooling surface 53 below the dew point of the reaction gas 32 by circulating the second heat medium 51 in the second heat medium region 5. As the second heat medium 51, when the product is methanol, for example, low-pressure boiler water of 80°C to 150°C (for example, saturated water of -0.05 MPaG to 0.4 MPaG), cooling water of -20°C to 100°C (for example, methanol aqueous solution, ethylene glycol aqueous solution), industrial water, ammonia aqueous solution, hydrocarbon compounds such as pentane, and freon compounds such as 1,1,1,3,3-pentafluoropropane can be used.

[0042] More specifically, when the reaction catalyzed by the catalyst 30 is an exothermic reaction performed at a temperature higher than the dew point of the reaction gas 32 by 80° C. or more, the temperature of the first heat medium 21 is preferably 5° C. to 30° C. lower than the average temperature of the catalyst layer 3, and the temperature of the second heat medium 51 is preferably 20° C. or more lower than the dew point of the reaction gas 32. Here, the temperature of the first heat medium and the second heat medium refers to the average of the temperature of each supply port and the temperature of the recovery port.

[0043] It should be noted that in Figure 1 In the embodiment, the first heat medium supply port 25 and the first heat medium recovery port 26 and the second heat medium supply port 55 and the second heat medium recovery port 56 are formed at the lower part and the upper part of the reaction container 1. However, it should be understood that their positions can be set at appropriate positions in an appropriate manner according to the pressure of the heat medium used. In addition, the supply temperature and supply pressure of the first heat medium 21 and the second heat medium 51 can be set to appropriate values ​​according to the temperature of the reaction carried out in the reaction container 1 and the dew point of the reaction gas 32.

[0044] The catalyst layer 3 is filled with a catalyst 30 suitable for the reaction. The catalyst layer 3 is a region containing the catalyst 30 and where the raw gas 31 contacts the catalyst 30 to react. As the catalyst 30, for example, a catalyst having copper and zinc oxide as main components can be used. The space between the catalyst layer 3 and the reaction container 1 can be filled with a filler 300. In addition, in order to support the catalyst 30, a support plate (not shown) including a porous member can also be provided at the bottom of the catalyst layer 3.

[0045] Figure 2 This is a partially enlarged view of a cross-sectional view of the reaction apparatus 100 according to Embodiment 1 cut along a plane perpendicular to the bottom surface. Figure 2 FIG. 4 shows an example in which a plurality of convex portions are formed in the Z-axis direction of the cooling surface 53. Figure 2 As shown, the catalyst layer 3 has a distance L X The height H corresponding to the cooling surface 53 (x=1, 2, ...) X (x=1, 2, ...). Distance L X It is the distance between the surface of the catalyst layer 3 in contact with the permeable wall 40 and the cooling surface 53. Specifically, there are heights H1 corresponding to the distance L1, H2 corresponding to the distance L2, ... corresponding to the distance L n Height H n In this case, the height H of the catalyst layer 3 can be X The sum of (H1+H2+…+H n It should be noted that when the surface of the catalyst layer 3 in contact with the permeable wall 40 and the cooling surface 53 are flat in the Z-axis direction, the distance L X The distance is the same over the entire cooling surface 53. Therefore, the distance at the predetermined position in this case can be simply expressed as the distance L.

[0046] like Figure 2 As shown, when the catalyst layer 3 is constituted as a collection of a plurality of discontinuous catalyst layers, the height H of the catalyst layer 3 can be X The sum of (H1+H2+…+H n )express.

[0047] Depending on the filling condition of the catalyst 30, the upper end surface or the lower end surface of the catalyst layer 3 may be uneven, or the upper end surface and the lower end surface may not be parallel. In this case, in this specification, the height H of the catalyst layer 3 refers to the height of the catalyst layer 3 at the contact surface with the permeable wall 40. In the case where the surface of the catalyst layer 3 that contacts the permeable wall 40 is not a plane, the distance L is also specified in the same manner as when the above-mentioned convex portion is formed on the cooling surface 53. X and height H X .

[0048] From the perspective of the processing capacity of each reactor 1, the height H X The sum of the height H is preferably 1,000 mm or more. X The sum of is preferably 20,000 mm or less.

[0049] The permeable wall 40 is provided at the boundary between the catalyst layer 3 and the space 4, and is a member through which the reaction gas 32 can pass. The permeable wall 40 is composed of, for example, a metal member made of stainless steel. The permeable wall 40 uses a member through which the reaction gas 32 can pass but the catalyst 30 cannot pass, such as a metal mesh with an appropriate hole size. The reaction gas 32 contains unreacted raw material gas and uncondensed reaction product gas.

[0050] The space 4 is formed between the permeable wall 40 and the cooling surface 53. A condensate storage portion 47 is formed at the lower portion of the space 4. The condensate storage portion 47 can store a product obtained by condensation and liquefaction on and / or near the cooling surface 53. The condensate 41 is recovered through a condensate recovery port 46 provided at the bottom of the condensate storage portion 47.

[0051] Here, the distance L between the surface of the catalyst layer 3 in contact with the permeable wall 40 and the cooling surface 53 is X It is preferably 0.5 mm or more and 500 mm or less. When the partial area of ​​the cooling surface 53 facing the catalyst layer 3 is added together, the distance L X The range of L is preferably realized in an area of ​​more than 80% of the vertical length of the total area after the addition, and more preferably in an area of ​​more than 95%. From the perspective of ensuring space for the condensed droplets to fall due to gravity, the distance L X It is satisfactory to be 0.5 mm or more. X If the distance L is less than 0.5 mm, the product may condense in the catalyst layer 3. X If the distance L is greater than 500 mm, the size of the reaction vessel 1 will increase, which will lead to various costs and may cause economic disadvantages. X It is preferably 0.5 mm or more and 500 mm or less.

[0052] (About cumulative value)

[0053] In the reaction device 100 of the present embodiment, the distance L between the surface of the catalyst layer 3 in contact with the permeable wall 40 and the cooling surface 53 is set to X and with a distance L X The height H of the catalyst layer 3 corresponding to the cooling surface X The product of the accumulated value from one end to the other end of the cooling surface 53 in the Z-axis direction is 500 mm. 2 above.

[0054] In the present invention, the cumulative value accumulated from one end to the other end of the cooling surface 53 in the predetermined direction is 500 mm. 2It means that the cumulative value accumulated from one end to the other end of the cooling surface 53 in the Z-axis direction at at least one predetermined point satisfies 500 mm. 2 In the case where the cumulative value varies depending on the specified position in the X-axis direction, the cumulative value obtained by accumulating from one end to the other end of the cooling surface 53 in the Z-axis direction in an area of ​​more than 50%, preferably more than 80%, more preferably more than 95%, and particularly preferably 100% in the X-axis direction can be 500 mm 2 .

[0055] The cumulative value of the reaction device 100 accumulated from one end to the other end of the cooling surface 53 in the Z-axis direction at at least one predetermined point in the X-axis direction satisfies 500 mm. 2 Therefore, the cumulative value is less than 500 mm in the 100% area in the X-axis direction. 2 Compared with the reaction device of the present invention, even if the condition parameters are the same, the reaction yield of the product can be improved. The condition parameters include the pressure, temperature and the ratio of the catalyst amount to the raw material supply rate (W / F) of the reaction system.

[0056] In the above reaction in which the chemical equilibrium is shifted to the product side by condensing the product and recovering it from the reaction container, the reaction rate of the reaction occurring in the catalyst layer 3, the diffusion rate of the product to the cooling surface 53, and the condensation rate at the cooling surface 53 all dominate the overall reaction rate. X This will reduce the driving force that moves the chemical equilibrium toward the product side, so increasing the distance L is usually not done. X However, the present inventors have found that by forming the internal structure of the reaction device 100 so that the cumulative value is 500 mm 2 The above structure can actually increase the reaction yield of the product.

[0057] On the other hand, as mentioned above, from an economic point of view, the distance L X Preferably less than 500 mm, height H X The sum of is preferably 20,000 mm or less, therefore, the above cumulative value is preferably 10,000,000 mm 2 Below. By having the above cumulative value of 500mm 2 Above and 10,000,000mm 2 The following configuration, the reaction apparatus 100 and the chemical reaction method using the reaction apparatus 100 can improve the reaction yield of the product. In addition, the reaction apparatus 100 and the chemical reaction method which are also preferred from an economical point of view can be provided.

[0058] (Reaction process)

[0059] The raw gas 31 is supplied from the raw gas inlet 35 provided at the upper part of the catalyst layer 3, and the reaction proceeds by contacting with the catalyst 30 filled in the catalyst layer 3. The reaction gas 32 generated by the reaction enters the space 4 through the permeable wall 40, and is cooled to below the dew point of the reaction gas 32 on the cooling surface 53, thereby condensing the product. The condensed and liquefied product falls into the condensate storage part 47, and is recovered as the condensate 41 through the condensate recovery port 46.

[0060] The reaction gas 32 passing through the permeable wall 40 from the catalyst layer 3 side also contains unreacted raw gas. However, the main components contained in the unreacted raw gas are not condensed on the cooling surface 53. In addition, by providing the condensate storage part 47 at the lower part of the space 4, the unreacted raw gas is not discharged from the condensate recovery port 46 together with the condensate 41, but returns to the catalyst layer 3 again.

[0061] Here, in order to avoid that the ratio of the unreacted raw gas that passes through the space 4 and goes to the outlet of the catalyst layer 3 is too large, it is preferable to keep the gas flow rate through the permeable wall 40 within an appropriate range. In order to keep the above-mentioned gas flow rate within an appropriate range, for example, the opening rate of the porous member forming the permeable wall 40 can be adjusted. Alternatively, in order to keep the above-mentioned gas flow rate within an appropriate range, a member that becomes a resistance to the gas flow can also be inserted into the space 4.

[0062] The reaction gas 32 containing the raw material that has not reacted in the catalyst layer 3 is recovered from the reaction gas recovery port 36 .

[0063] (Recovery of reaction heat and condensation heat)

[0064] The first heat medium 21 is supplied from the first heat medium supply port 25 in the form of, for example, boiler water of 2.2 MPaG to 5.0 MPaG. In the case of an exothermic reaction, the reaction heat generated in the catalyst layer 3 is heat exchanged via the first heat exchange wall 20 and recovered by the first heat medium 21. The first heat medium 21 is recovered to a high-pressure steam separation drum (not shown) through the first heat medium recovery port 26. Then, the high-pressure steam obtained by performing gas-liquid separation is used, for example, as a power source for compressing raw materials.

[0065] The second heat medium 51 is supplied from the second heat medium supply port 55 in the form of, for example, 0.05 MPaG boiler water. In order to reduce the temperature of the reaction gas 32 in the space 4 to below the dew point on the surface of the cooling surface 53, the second heat medium 51 performs heat exchange via the second heat exchange wall 50, thereby recovering the heat of the reaction gas 32 to the second heat medium 51. The second heat medium 51 is recovered to the low-pressure steam separation drum (not shown) through the second heat medium recovery port 56. Then, the low-pressure steam obtained by performing gas-liquid separation is used, for example, as a heat source in the refining process of the product.

[0066] (Effects of Embodiment 1)

[0067] As described above, the reaction device 100 of the first embodiment is a chemical reaction device that causes the product to contain a component with a higher boiling point than the component in the raw material gas 31 and causes the progress of the reaction in the gas phase to be subject to the chemical equilibrium between the raw material and the product. In addition, the chemical reaction method of the first embodiment is a method using the reaction device 100. The reaction device 100 includes: a catalyst layer 3 to which the raw material gas 31 is supplied and which includes a catalyst 30 that promotes the above reaction, a cooling surface 53 that is arranged apart from the catalyst layer 3 with a space 4, is maintained at a temperature below the dew point of the reaction gas 32 and extends in a predetermined direction, and a permeable wall 40 that is provided at the boundary between the catalyst layer 3 and the space 4 and through which the reaction gas 32 generated in the above reaction can pass. The distance L between the surface of the catalyst layer 3 that contacts the permeable wall 40 and the cooling surface 53 is set to X and with a distance L X The catalyst layer height H corresponding to the cooling surface 53 X The cumulative value obtained by accumulating the product from one end to the other end of the cooling surface 53 in the height direction is 500 mm. 2 The reaction device 100 condenses a part of the product on the surface of the cooling surface 53 and in the space 4 .

[0068] According to the reaction apparatus 100 and the chemical reaction method using the reaction apparatus 100 , the product is recovered as the condensate 41 from the reaction container 1 , thereby making it possible to cause the reaction to proceed at a conversion rate exceeding the equilibrium in a reaction system where the progress of the reaction in the gas phase is governed by chemical equilibrium.

[0069] In addition, the cumulative value of the reaction device 100 accumulated from one end to the other end of the cooling surface 53 in the Z-axis direction at at least one predetermined point in the X-axis direction satisfies 500 mm. 2 Thus, the reaction device 100 and the chemical reaction method using the reaction device 100 have the cumulative value less than 500 mm even when the cumulative value is less than 100% of the area in the X-axis direction. 2 Under the same reaction conditions and parameters of the reaction apparatus, the reaction yield of the product can also be improved.

[0070] In the reaction apparatus 100 and the chemical reaction method using the reaction apparatus 100 , according to the method for producing methanol containing carbon oxides and hydrogen as the raw material gas 31 and using a methanol synthesis catalyst as the catalyst 30 , the reaction yield of methanol can be improved.

[0071] [Implementation Method 2]

[0072] Another embodiment of the present invention will be described below. It should be noted that, for the sake of convenience, components having the same functions as those described in Embodiment 1 are denoted by the same reference numerals, and description thereof will not be repeated.

[0073] Figure 3 This is a cross-sectional view of the reaction apparatus 100A according to the second embodiment cut along a plane perpendicular to the bottom surface. Figure 4 This is a cross-sectional view of the reaction tube 10A included in the reaction apparatus 100A cut along a plane perpendicular to the long axis of the reaction tube 10A. The basic principle of the reaction apparatus 100A is the same as that of the reaction apparatus 100. The reaction apparatus 100A is different from the reaction apparatus 100 in that a cylindrical reaction tube is used.

[0074] Like the reaction apparatus 100, the reaction apparatus 100A can be suitably used as an apparatus for performing a chemical reaction in which the raw material gas 31 contains carbon oxides and hydrogen and the product contains methanol. The reaction apparatus 100A can also be used for performing a reaction in which dimethyl ether or ammonia is produced as a product.

[0075] In the raw gas 31, the impurities shown below are preferably reduced to a level that does not have an excessive effect on the production of methanol. Sulfur compounds and sulfur elements (e.g., hydrogen sulfide, carbonyl sulfide, carbon disulfide, sulfur oxide, thiophene, methyl thiocyanate), halogen compounds and halogen elements (e.g., hydrogen chloride, chlorinated hydrocarbons), metal carbonyl compounds (e.g., carbonyl Fe, carbonyl Ni), metal compounds (e.g., metal compounds containing vanadium and alkali metals), nitrogen compounds (e.g., ammonia, amines, nitrogen oxides, nitriles, hydrogen cyanide), liquid and solid substances (e.g., tar, carbon black, coal, ash, metal powder) and unsaturated hydrocarbons. It should be noted that as the catalyst 30, there is no particular limitation as long as it is a catalyst that promotes the reaction, and it can be a catalyst containing Cu and Zn, or a catalyst containing Al, Mg, Cr, Mn, V, Ti, Zr, Ta, Mo, W, Si, rare earths, Ga, etc.

[0076] (Reaction device 100A)

[0077] like Figure 3As shown, the reaction device 100A has a plurality of reaction tubes 10A extending in the Z-axis direction inside the reaction container 1A. The number of reaction tubes 10A provided inside the reaction container 1A is not particularly limited and may be one or more. If the efficiency of the reaction is considered, the number of reaction tubes 10A is preferably two or more. A raw gas supply section 37A is formed on the upper side of the plurality of reaction tubes 10A, and the raw gas supply section 37A is filled with the raw gas 31 supplied to each reaction tube 10A. A storage section 48A is formed on the lower side of the plurality of reaction tubes 10A, and the storage section 48A stores the liquid condensed inside the reaction tube 10A and the gas passing through the catalyst layer 3A. A second heat medium recovery section 58A is formed on the lower side of the storage section 48A, and the second heat medium recovery section 58A stores the second heat medium 51 discharged from the second heat exchange section 52A (cooling pipe) described later. Further, a second heat medium supply unit 57A is formed below the second heat medium supply unit 57A for storing the second heat medium 51 supplied to the second heat exchange unit 52A. The above-mentioned units are formed by partitioning the internal space of the reaction container 1A with metal plates, for example, stainless steel plates.

[0078] The reaction tube 10A is open to a metal plate 11A located at the upper portion of the reaction tube 10A and a metal plate 12A located at the lower portion of the reaction tube 10A, and an outer tube 20A of the reaction tube 10A and the metal plates 11A / 12A are joined by welding.

[0079] like Figure 2 and Figure 4 As shown, the reaction tube 10A has, from the outside, an outer tube 20A, a cylindrical catalyst layer 3A in contact with the inner wall surface of the outer tube 20A, an inner tube 40A disposed inside the catalyst layer 3A, and a second heat exchange portion 52A (cooling tube). The second heat exchange portion 52A is separated from the inner tube 40A by a space 4A (first space).

[0080] The first heat exchange section 22A is a heat exchanger composed of a part of the inner wall surface of the reaction container 1A, the outer wall surface of the outer tube 20A and the metal plates 11A / 12A, and having a heat transfer surface 23A on the catalyst layer 3A side. Inside the first heat exchange section 22A, a first heat medium area 2A common to a plurality of reaction tubes 10A is formed. In the first heat medium area 2A, a first heat medium 21 (heat medium) flows. The first heat medium 21 is a heat medium for keeping the outer tube 20A at a temperature higher than the dew point of the reaction gas 32. The outer tube 20A includes a component through which the fluid cannot pass, and the heat transfer surface 23A of the outer tube 20A functions as a first heat exchange surface.

[0081] A first heat medium supply port 25A for supplying the first heat medium 21 to the first heat medium region 2A and a first heat medium recovery port 26A for discharging the first heat medium 21 from the first heat medium region 2A are formed on the side wall of the reaction container 1A. The first heat exchange portion 22A allows the first heat medium 21 to flow through the first heat medium region 2A, thereby maintaining the heat transfer surface 23A at a temperature higher than the dew point of the reaction gas 32. By having the heat transfer surface 23A, the reaction device 100A can maintain the temperature of the catalyst layer 3A at a temperature suitable for the reaction, and can improve the efficiency of the reaction.

[0082] like Figure 3 and Figure 4 As shown, the second heat exchange part 52A has a second heat exchange wall 50A and an inner tube 59A. A second heat medium area 5A is formed between the second heat exchange wall 50A and the inner tube 59A. The second heat medium area 5A is an area where the second heat medium 51 flows. The second heat exchange part 52A has a double tube structure. The second heat medium 51 in the second heat medium supply part 57A is supplied to the second heat exchange part 52A through the inner tube 59A. On the other hand, the flow path between the outer wall surface of the inner tube and the inner wall surface of the second heat exchange wall 50A is connected to the inside of the second heat medium recovery part 58A. The second heat medium 51 that comes out of the second heat medium supply part 57A and reaches the upper end of the inner tube passes through the above-mentioned flow path and is discharged to the second heat medium recovery part 58A through the outflow outlet 54A formed on the upper wall surface of the second heat medium recovery part 58A.

[0083] The second heat exchange wall 50A includes a fluid-impermeable member, and the cooling surface 53A (outer surface of the cooling tube) of the second heat exchange wall 50A functions as a second heat exchange surface. The second heat exchange portion 52A allows the second heat medium 51 to flow through the second heat medium region 5A, thereby maintaining the temperature of the second heat exchange wall 50A and the cooling surface 53A below the dew point of the reaction gas 32.

[0084] The catalyst layer 3A is filled with a catalyst 30 suitable for the reaction. The upper end of the reaction tube 10A is covered with a metal cover except for the upper end of the catalyst layer 3A, and is formed in a state where the gas cannot flow. An opening 38A is formed above the catalyst layer 3A, and the raw gas 31 is supplied to the catalyst layer 3A through the opening 38A. The upper end of the catalyst layer 3A and the opening 38A may not be on the same plane, and a filler 300A may be filled between the upper end of the catalyst layer 3A and the opening 38A. An opening 39A is formed below the catalyst layer 3A. The lower end of the catalyst layer 3A and the opening 39A may not be on the same plane, and a filler 300A may be filled between the lower end of the catalyst layer 3A and the opening 39A. A support member including a metal mesh is provided at the lower end of the catalyst layer 3A, for example, and the support member plays a role in preventing the catalyst 30 from falling.

[0085] The catalyst layer 3A extends in the Z-axis direction and has a distance L from A The height H corresponding to the cooling surface 53A A . Distance L A It is the distance between the surface of the catalyst layer 3A in contact with the inner cylinder 40A and the cooling surface 53A. When the cooling surface 53A is a curved surface without concavities and convexities in the Z-axis direction, the length from the upper end to the lower end of the catalyst layer 3A can be simply expressed as the height H A On the other hand, when the cooling surface 53A has irregularities in the Z-axis direction, the distance L A When the catalyst layer 3A is not constant, the distance L X The corresponding height H X Specifically, it has a height H1 corresponding to the distance L1, a height H2 corresponding to the distance L2, and so on corresponding to the distance L n Height H n In this case, the length from the upper end to the lower end of the catalyst layer 3 can be changed by the height H X The sum of (H1+H2+…+H n )express.

[0086] Distance L X It is preferably 0.5 mm or more and 500 mm or less. When the partial area of ​​the cooling surface 53A facing the catalyst layer 3A is added together, the distance L X The range is preferably achieved in an area of ​​80% or more of the length of the vertical direction of the total area after the addition, and more preferably achieved in an area of ​​95% or more.

[0087] Height X The sum of is preferably not less than 1,000 mm and not more than 20,000 mm. When the sum is less than 1,000 mm, in order to ensure a sufficient amount of catalyst filled in the reaction device 100A, it is necessary to increase the number of reaction tubes 10A. The increase in the number of reaction tubes 10A leads to an increase in manufacturing costs, etc. Therefore, from an economic point of view, the above sum is preferably not less than 1,000 mm. When the above sum is greater than 20,000 mm, it is necessary to manufacture very long reaction tubes 10A and high reaction devices 100A. Such reaction tubes 10A and reaction devices 100A lead to an increase in manufacturing costs, etc. Therefore, from an economic point of view, the above sum is preferably not more than 20,000 mm.

[0088] The inner tube 40A includes a gas-permeable porous member, and can allow the gas including the product generated in the catalyst layer 3A and the unreacted raw material to permeate to the second heat exchange section 52A side.

[0089] The space 4A is a space formed between the inner tube 40A and the second heat exchange wall 50A. In the present embodiment, a condensate flow pipe (communication pipe) 42A is provided on the vertical lower side of the space 4A. The condensate flow pipe 42A is configured to extend the space 4A downward in the vertical direction and includes a liquid-impermeable member. More specifically, the condensate flow pipe 42A forms a space (second space) 6A continuous with the space 4A between the surface of the second heat exchange part 52A and the condensate flow pipe 42A.

[0090] A storage portion 48A is formed at the lower side of the reaction tube 10A, and the storage portion 48A stores the condensate 41 generated in the space 4A and the gas that has passed through the catalyst layer 3A at the lower side in the vertical direction of the space 4A. A condensate flow pipe 42A is provided inside the storage portion 48A, and the lower end of the condensate flow pipe 42A is positioned so as to be immersed in the condensate 41 stored at the bottom of the storage portion 48A (referred to as a condensate storage portion 47A).

[0091] In addition, the uncondensed gas 32A passing through the catalyst layer 3A is stored in the upper space (referred to as the gas recovery region 49A) inside the storage section 48A. The uncondensed gas 32A is the gas discharged after the reaction gas 32 passes through the catalyst layer 3A without condensing and contacts the condensate storage section (liquid storage section) 47A via the gas recovery region 49A (storage section 48A). The storage section 48A has an uncondensed gas recovery port 36A (exhaust section) for discharging the uncondensed gas 32A stored in the gas recovery region 49A. The uncondensed gas recovery port 36A is provided at a position vertically higher than the lower end of the condensate flow pipe 42A.

[0092] The condensate 41 as a product condensed in the space 4A is discharged to the condensate storage part 47A through the inside of the condensate flow pipe 42A. The condensate 41 in the condensate storage part 47A is recovered through the condensate recovery port 46A provided near the bottom of the storage part 48A. Here, the discharge of the fluid from the condensate recovery port 46A is controlled so that the reaction gas 32 is not recovered from the condensate recovery port 46A.

[0093] (About cumulative value)

[0094] In the reaction device 100A of this embodiment, the distance L X With height H X The product of the cooling surface 53A from one end to the other end is 500 mm. 2 When the reaction apparatus 100A is a multi-tube reactor including a plurality of reaction tubes 10A, the above-mentioned cumulative value is 500 mm for each reaction tube 10A. 2 above.

[0095] In the present invention, the cumulative value accumulated from one end to the other end of the cooling surface 53A in the predetermined direction is 500 mm. 2 It means that the cumulative value accumulated from one end to the other end of the cooling surface 53A in the Z-axis direction at at least one predetermined point satisfies 500 mm. 2 In the case where the value of the cumulative value varies depending on the specified position in the X-axis direction, the cumulative value obtained by accumulating from one end to the other end of the cooling surface 53A in the Z-axis direction in an area of ​​more than 50%, preferably more than 80%, more preferably more than 95%, and particularly preferably 100% in the X-axis direction is 500 mm. 2 It should be noted that the X-axis direction in the present embodiment refers to the circumferential direction of the cooling surface 53A having a cylindrical shape.

[0096] The inventors have found through experiments that the cumulative value obtained by integrating the cooling surface 53A from one end to the other end in the Z-axis direction at at least one predetermined location in the circumferential direction of the cylindrical cooling surface 53A satisfies 500 mm. 2 As a result, the cumulative value is less than 500 mm in the 100% area in the circumferential direction of the cylindrical cooling surface 53A. 2 Compared with the reaction device of the present invention, even if the condition parameters are the same, the reaction yield of the product can be improved. The condition parameters include the pressure, temperature and the ratio of the catalyst amount to the raw material supply rate (W / F) in the reaction system.

[0097] In the conventional reaction device, the cumulative value is 500 mm. 2 When the internal structure is changed in the above manner, the change can be achieved by, for example, increasing the diameter of the inner cylinder 40A without changing the diameter of the outer cylinder 20A. First, consider the case where the filling amount of the catalyst 30 and the density of the catalyst 30 in the catalyst layer 3A (the dilution ratio of the catalyst 30) are the same. In this case, in the reaction tube 10A, when the diameter of the inner cylinder 40A is increased, the height H of the catalyst layer 3A is X The sum of the above-mentioned cumulative value of 500 mm can be achieved. 2 The above reaction device 100A. In other words, this change is a change to increase the contact area between the catalyst layer 3A and the inner tube 40A.

[0098] In the above reaction in which the chemical equilibrium is shifted to the product side by condensing the product and recovering it from the reaction container, the overall reaction speed is controlled by any one of the reaction speed of the reaction occurring in the catalyst layer 3, the diffusion speed of the product to the cooling surface 53, and the condensation speed at the cooling surface 53. When the overall reaction speed is controlled by the diffusion speed, it is considered that increasing the distance L XThis will reduce the driving force that moves the chemical equilibrium toward the product side, thereby reducing the overall reaction rate. Therefore, it is usually not necessary to increase the distance L. X However, the inventors have found through experiments that by forming the internal structure of the reaction device 100A so that the cumulative value is 500 mm 2 The above structure can actually increase the reaction yield of the product.

[0099] In addition, the above cumulative value is 500mm 2 The above changes in the internal structure can also be achieved by increasing the height H X For example, the height H can be reduced by diluting the catalyst 30 in the catalyst layer 3A. X In order to further increase the above-mentioned cumulative value, the diameter of the inner cylinder 40A may be increased and the catalyst 30 may be diluted.

[0100] On the other hand, as mentioned above, from an economic point of view, the distance L X Preferably less than 500 mm, height H X The sum of is preferably 20,000 mm or less. Therefore, the above cumulative value is preferably 10,000,000 mm 2 the following.

[0101] (Reaction process)

[0102] The raw gas 31 is supplied from the raw gas inlet 35A and supplied to the catalyst layer 3A in the reaction tube 10A through the opening 38A. The reaction proceeds by contacting the raw gas 31 with the catalyst 30 in the catalyst layer 3A. The reaction gas 32 generated by the reaction passes through the inner tube 40A and enters the space 4A, and is cooled to below the dew point of the reaction gas 32 on the cooling surface 53A, thereby condensing the product. The condensed and liquefied product falls to the condensate storage part 47A through the space 4A and the condensate flow pipe 42A. The condensate 41 stored in the condensate storage part 47A is recovered through the condensate recovery port 46A.

[0103] The reaction gas 32 passing through the inner tube 40A from the catalyst layer 3A side also contains unreacted raw gas. However, the main components contained in the unreacted raw gas are not condensed on the cooling surface 53A. In addition, the lower end of the condensate circulation pipe 42A is immersed in the condensate 41 stored in the condensate storage section 47A, so that the unreacted raw gas moving inside the condensate circulation pipe 42A is hindered by the liquid level of the condensate 41 and returns to the catalyst layer 3A again. In the gas recovery area 49A, a prescribed pressure is applied due to the injection of the raw gas 31, and the pressure is also applied to the liquid level of the condensate 41 in the condensate storage section 47A. Therefore, the liquid level prevents the unreacted raw gas from being discharged from the lower end of the condensate circulation pipe 42A without returning to the catalyst layer 3A. Here, it is preferred that the liquid height h of the condensate storage section 47A is 0.177°. A Keep within the range that satisfies the following relationship.

[0104] h A =αΔP / ρg

[0105] 1.0<α<10

[0106] h A : Liquid height of storage part [m],

[0107] ΔP: Pressure loss of the reaction gas passing through the catalyst layer [Pa]

[0108] ρ: Density of condensate [kg / m 3 ]

[0109] g: Gravitational acceleration (=9.8 [m / s 2 ]),

[0110] α: coefficient [-]

[0111] In h A If the h is too small, part of the reaction gas passes through the space 4A and the condensate storage section 47A and flows out from the condensate recovery port 46A together with the condensate, and the contact efficiency with the catalyst 30 may be reduced. A If it is too large, the height of the reaction container increases, and the pressure of the space 4A becomes higher than the pressure of the catalyst layer 3A, which may hinder the movement of the product from the catalyst layer 3A to the space 4A.

[0112] The uncondensed gas 32A including the raw material that has not reacted in the catalyst layer 3A is recovered to the gas recovery region 49A, and is recovered from the uncondensed gas recovery port 36A formed in the upper portion of the storage portion 48A.

[0113] (Recovery of reaction heat and condensation heat)

[0114] The first heat medium 21 is supplied to the first heat exchange part 22A from the first heat medium supply port 25A. The reaction heat generated in the catalyst layer 3A is heat exchanged through the outer cylinder 20A and recovered by the first heat medium 21. The first heat medium 21 is recovered to the high-pressure steam separation drum (not shown) through the first heat medium recovery port 26A. Then, the high-pressure steam obtained by performing gas-liquid separation is used as a power source for compressing raw materials, for example.

[0115] The second heat medium 51 is supplied from the second heat medium supply port 55A to the second heat medium supply part 57A, and then supplied to the second heat exchange part 52A. The second heat medium 51 performs heat exchange via the second heat exchange wall 50A, thereby reducing the temperature of the reaction gas 32 in the space 4A to below the dew point at the cooling surface 53A, thereby recovering the heat of the reaction gas 32. The second heat medium 51 is recovered to the low-pressure steam separation drum (not shown) through the second heat medium recovery port 56A. Then, the low-pressure steam obtained by performing gas-liquid separation is used, for example, as a heat source in the refining process of the product.

[0116] (Effects of Embodiment 2)

[0117] As described above, the reaction device 100A has a reaction container 1A, and the reaction container 1A includes at least one multi-structure reaction tube 10A, and the multi-structure reaction tube 10A performs a reaction in which the product includes a component having a higher boiling point than the component in the raw material gas and the reaction in the gas phase is subject to the chemical equilibrium between the raw material and the product. Each of the at least one reaction tube 10A respectively includes: an inner tube 40A extending in the Z-axis direction and through which the reaction gas 32 generated in the above reaction can pass, an outer tube 20A in which the inner tube 40A is arranged, a second heat exchange part 52A (cooling tube) arranged in the inner tube 40A, and a catalyst layer 3A arranged between the inner tube 40A and the outer tube 20A. The distance L between the surface of the catalyst layer 3A in contact with the inner tube 40A and the cooling surface 53 is set to X and with a distance L X The height H of the catalyst layer 3A corresponding to the cooling surface 53 X The cumulative value obtained by accumulating the product from one end to the other end of the cooling surface 53 in the height direction is 500 mm. 2 The temperature of the cooling surface 53 is maintained at a temperature lower than the dew point of the reaction gas 32, and part of the product is condensed in the space 4A formed between the second heat exchange section 52A and the inner tube 40A.

[0118] According to the reaction apparatus 100A configured as described above and the chemical reaction method using the reaction apparatus 100A, the product is recovered from the reaction apparatus 100A in the form of the condensate 41 , thereby making it possible to cause the reaction to proceed at a conversion rate exceeding the equilibrium conversion rate.

[0119] In addition, the cumulative value of the reaction device 100A accumulated from one end to the other end of the cooling surface 53A in the Z-axis direction at at least one predetermined point in the circumferential direction of the cylindrical cooling surface 53A satisfies 500 mm. 2 Therefore, the cumulative value is less than 500 mm in the 100% area of ​​the cylindrical cooling surface 53A in the circumferential direction. 2 Compared with the reaction apparatus of the present invention, the reaction apparatus 100A and the chemical reaction method using the reaction apparatus 100A can improve the reaction yield of the product.

[0120] [Implementation method 3]

[0121] Another embodiment of the present invention is described below. Figure 3 It is understood that Embodiment 2 can utilize a larger amount of the first heat medium 21 for recovering the heat of reaction than the second heat medium 51 for recovering the heat of condensation. That is, the reaction apparatus 100A of Embodiment 2 is an advantageous structure in a reaction system where the removal of the heat of reaction is important.

[0122] On the other hand, the reaction apparatus 100B of the third embodiment described in detail below is a structure that is advantageous in a reaction system in which the removal of condensation heat is important. The basic principle of the reaction apparatus 100B is the same as that of the reaction apparatus 100A.

[0123] The reaction apparatus 100B can also be suitably used as an apparatus for a chemical reaction in which the raw material gas 31 contains carbon oxides and hydrogen and the product contains methanol, similarly to the reaction apparatus 100. The reaction apparatus 100B can also be used for a reaction in which dimethyl ether or ammonia is produced as a product.

[0124] Figure 5 This is a cross-sectional view when the reaction apparatus 100B is cut along a plane perpendicular to the bottom surface. Figure 6 This is a cross-sectional view when the reaction tube 10B included in the reaction apparatus 100B is cut along a parallel plane perpendicular to the long axis of the reaction tube 10B.

[0125] (Reaction device 100B)

[0126] like Figure 5 and Figure 6As shown, the reaction device 100B has a plurality of reaction tubes 10B inside the reaction container 1B. The number of reaction tubes 10B arranged inside the reaction container 1B is not particularly limited and may be one or more. When considering the efficiency of the reaction, the number of reaction tubes 10B is preferably multiple. On the upper side of the plurality of reaction tubes 10B, a raw gas supply section 37B is formed, and the raw gas supply section 37B is filled with the raw gas 31 supplied to each reaction tube 10B. A condensate storage section 47B (liquid storage section) is formed on the lower side of the plurality of reaction tubes 10B, and the condensate storage section 47B is used to store the liquid condensed inside the reaction tube 10B. A gas recovery section 48B is formed on the lower side of the condensate storage section 47B, and the gas recovery section 48B stores the gas that has passed through the catalyst layer 3B. A first heat medium recovery section 28B is formed on the lower side of the gas recovery section 48B, and the first heat medium recovery section 28B stores the first heat medium 21 discharged from the first heat exchange section 22B described later. Furthermore, a first heat medium supply unit 27B is formed below the first heat medium supply unit 27B for storing the first heat medium 21 supplied to the first heat exchange unit 22B. The above-mentioned units are formed by partitioning the internal space of the reaction container 1B with metal plates, for example, stainless steel plates.

[0127] The reaction tube 10B has, from the outside, an outer tube 50B, an inner tube 40B arranged to be separated from the inner wall of the outer tube 50B by a space 4B (first space), a cylindrical catalyst layer 3B in contact with the inner wall of the inner tube 40B, and a first heat exchanger 22B (heat source) provided inside the catalyst layer 3B. The catalyst layer 3B has the same material and structure as the catalyst layer 3A. The inner tube 40B is a tube through which the reaction gas 32 can pass, and has the same material and structure as the inner tube 40A.

[0128] The second heat exchange section 52B is a heat exchanger composed of a part of the inner wall surface of the reaction container 1A, the outer wall surface of the outer tube 50B, and the metal plate 11B / 12B. Inside the second heat exchange section 52B, a second heat medium area 5B common to a plurality of reaction tubes 10B is formed. The second heat medium 51 flows in the second heat medium area 5B. The outer tube 50B includes a member through which a fluid cannot pass, and the cooling surface 53B of the outer tube 50B (the inner surface of the outer tube 50B) functions as a second heat exchange surface.

[0129] A second heat medium supply port 55B for supplying the second heat medium 51 to the second heat medium region 5B and a second heat medium recovery port 56B for discharging the second heat medium 51 from the second heat medium region 5B are formed on the side wall of the reaction container 1B. The second heat exchange unit 52B allows the second heat medium 51 to flow through the second heat medium region 5B, thereby maintaining the outer tube 50B and the cooling surface 53B at a temperature below the dew point of the reaction gas 32.

[0130] like Figure 5 and Figure 6 As shown, the first heat exchange part 22B is a heat exchanger having a first heat exchange wall 20B and an inner tube 29B and having a heat transfer surface 23B on the catalyst layer 3B side. A first heat medium region 2B is formed between the first heat exchange wall 20B and the inner tube 29B. The first heat medium region 2B is a region where the first heat medium 21 flows.

[0131] The first heat exchange part 22B has a double tube structure. The first heat medium 21 in the first heat medium supply part 27B is supplied to the first heat exchange part 22B through the inner tube 29B. On the other hand, the flow path between the outer wall surface of the inner tube 29B and the inner wall surface of the first heat exchange wall 20B is connected to the inside of the first heat medium recovery part 28B. The first heat medium 21 that has passed through the inner tube 29B passes through the above-mentioned flow path and is discharged to the first heat medium recovery part 28B through the outlet 24B formed on the upper wall surface of the first heat medium recovery part 28B.

[0132] The catalyst layer 3B extends in the Z-axis direction and has a distance L from B The height H corresponding to the cooling surface 53B B . Distance L B The distance L is the distance between the surface of the catalyst layer 3B in contact with the inner tube 40B and the cooling surface 53B. B , distance L X , height H B and the length from the upper end to the lower end of the catalyst layer 3B (height H X The distance L is the same as that in the second embodiment. X It is preferably 0.5 mm or more and 500 mm or less. When the partial area of ​​the cooling surface 53B facing the catalyst layer 3B is added together, the distance L X The range is preferably achieved in an area of ​​80% or more of the length of the vertical direction of the total area after the addition, and more preferably achieved in an area of ​​95% or more.

[0133] The space 4B is a space formed between the inner cylinder 40B and the outer cylinder 50B. In the present embodiment, a condensate storage portion 47B is provided on the lower side of the space 4B in the vertical direction. In addition, a condensate flow pipe 42B (extension pipe) is provided inside the condensate storage portion 47B in such a manner as to extend the outer cylinder 50B downward in the vertical direction. The lower end of the condensate flow pipe 42B is positioned so as to be immersed in the condensate 41 stored in the condensate storage portion 47B. The condensate flow pipe 42B forms a space (second space) 6B continuous with the space 4B inside the condensate storage portion 47B.

[0134] The liquid (condensate 41) condensed in the space 4B passes through the space 6B inside the condensate flow pipe 42B and is stored in the condensate storage section 47B. The condensate 41 stored in the condensate storage section 47B is recovered through the condensate recovery port 46B. Here, the discharge control of the fluid from the condensate recovery port 46B is performed in a manner that the reaction gas 32 is not recovered from the condensate recovery port 46B.

[0135] A gas recovery section 48B (gas storage section) is provided below the catalyst layer 3B in the vertical direction, into which the gas passing through the catalyst layer 3B flows. The gas recovery section 48B has an uncondensed gas recovery port 36B (exhaust section).

[0136] In this way, the condensate storage part 47B and the gas recovery part 48B form separate spaces. The condensate storage part 47B forms a closed space for the gas, so the raw gas 31 descending in the space 4B has nowhere to go and returns to the catalyst layer 3B. Therefore, the possibility of the raw gas 31 passing through the space 4B and being directly discharged to the outside can be reduced.

[0137] The first heat exchange part 22B penetrates the gas recovery part 48B, and the lower end of the inner tube 29B of the first heat exchange part 22B is open to the internal space of the first heat medium supply part 27B. The flow path between the outer wall surface of the inner tube 29B and the inner wall surface of the first heat exchange wall 20B is connected to the inside of the first heat medium recovery part 28B. The first heat medium 21 that comes out of the first heat medium supply part 27B and reaches the upper end of the inner tube 29B passes through the above-mentioned flow path and is discharged to the first heat medium recovery part 28B through the outlet 24B formed on the upper wall surface of the first heat medium recovery part 28B.

[0138] (About cumulative value)

[0139] Regarding the reaction device 100B of this embodiment, the distance L X , height H X The product of the accumulated value from one end to the other end of the cooling surface 53B in the height direction is 500 mm. 2 When the reaction apparatus 100B is a multi-tube reactor including a plurality of reaction tubes 10B, the above-mentioned cumulative value is 500 mm for each reaction tube 10B. 2 above.

[0140] In the present invention, the cumulative value accumulated from one end to the other end of the cooling surface 53B in the predetermined direction is 500 mm. 2 It means that the cumulative value accumulated from one end to the other end of the cooling surface 53B in the Z-axis direction at at least one predetermined point satisfies 500 mm. 2In the case where the cumulative value varies depending on the specified position in the X-axis direction, the cumulative value accumulated from one end to the other end of the cooling surface 53B in the Z-axis direction in an area of ​​more than 50%, preferably more than 80%, more preferably more than 95%, and particularly preferably 100% in the X-axis direction can be 500 mm. 2 It should be noted that the X-axis direction in the present embodiment refers to the circumferential direction of the cooling surface 53B having a cylindrical shape.

[0141] In the conventional reaction device, the cumulative value is 500 mm. 2 When the internal structure is changed in the above manner, the change can be achieved, for example, by reducing the diameter of the inner tube 40B. First, consider the case where the filling amount of the catalyst 30 and the density of the catalyst 30 in the catalyst layer 3B (the dilution ratio of the catalyst 30) are the same. In this case, when the diameter of the inner tube 40B is reduced in the reaction tube 10B, the height H of the catalyst layer 3B is X The sum of the above-mentioned cumulative value of 500 mm can be achieved. 2 The above reaction device 100B. In other words, this change is a change to increase the contact area between the catalyst layer 3B and the inner tube 40B.

[0142] In addition, the above cumulative value is 500mm 2 Such a change in the internal structure can be achieved, for example, by diluting the catalyst 30 in the catalyst layer 3B. In order to further increase the above-mentioned integrated value, the diameter of the inner tube 40A may be increased and the catalyst 30 may be diluted.

[0143] On the other hand, as mentioned above, from an economic point of view, the distance L X Preferably less than 500 mm, height H X The sum of is preferably 20,000 mm or less. Therefore, the above cumulative value is preferably 10,000,000 mm 2 the following.

[0144] (Reaction process)

[0145] The raw gas 31 is supplied from the raw gas inlet 35B, through the opening 38B, and supplied to the catalyst layer 3B in the reaction tube 10B. The raw gas 31 contacts the catalyst 30 in the catalyst layer 3B, and the reaction proceeds. The reaction gas 32 generated by the reaction passes through the inner tube 40B and enters the space 4B, and is cooled to below the dew point of the reaction gas 32 on the inner wall surface (second heat exchange surface) of the outer tube 50B, thereby condensing the product. The condensed and liquefied product passes through the space 4B and falls into the condensate storage section 47B. The condensate 41 stored in the condensate storage section 47B is recovered via the condensate recovery port 46B.

[0146] The reaction gas 32 passing through the inner cylinder 40B from the catalyst layer 3B side to the outer cylinder 50B also contains unreacted raw gas. However, the main components contained in the unreacted raw gas are not condensed in the outer cylinder 50B. In addition, the condensate storage part 47B forms a closed space for the gas, so the unreacted raw gas descending in the space 4B has no place to go, and its movement is hindered by the liquid level of the condensate 41, and it returns to the catalyst layer 3B again. Here, the liquid height h of the condensate storage part 47B is B It is preferable to maintain it in the range satisfying the following relationship.

[0147] h B =αΔP / ρg

[0148] 1.0<α<10

[0149] h B : Liquid height of storage part [m],

[0150] ΔP: Pressure loss of the reaction gas passing through the catalyst layer [Pa]

[0151] ρ: Density of condensate [kg / m 3 ]

[0152] g: Gravitational acceleration (=9.8 [m / s 2 ]),

[0153] α: coefficient [-]

[0154] In h B If the h is too small, part of the reaction gas 32 passes through the space 4B and the condensate storage section 47B and then flows out from the condensate recovery port 46B together with the condensate, and the contact efficiency with the catalyst 30 may be reduced. B If it is too large, the height of the reaction container increases, and the pressure in the space 4B becomes higher than the pressure in the catalyst layer 3B, which may hinder the material movement of the product from the catalyst layer 3B to the space 4B.

[0155] The uncondensed gas 32B including the raw material that has not reacted in the catalyst layer 3B and has descended in the catalyst layer 3B is recovered to the gas recovery unit 48B and recovered from the uncondensed gas recovery port 36B formed in the gas recovery unit 48B.

[0156] (Recovery of reaction heat and condensation heat)

[0157] The first heat medium 21 is supplied from the first heat medium supply port 25B to the first heat medium supply section 27B, and then to the first heat exchange section 22B. The reaction heat generated in the catalyst layer 3B is heat exchanged via the first heat exchange wall 20B and recovered by the first heat medium 21. The first heat medium 21 is recovered to the high-pressure steam separation drum (not shown) through the first heat medium recovery port 26B. Then, the high-pressure steam obtained by performing gas-liquid separation is used, for example, as a power source for compressing raw materials.

[0158] The second heat medium 51 is supplied to the second heat exchange part 52B from the second heat medium supply port 55B. The second heat medium 51 performs heat exchange via the outer cylinder 50B, thereby reducing the temperature of the reaction gas 32 in the space 4B to below the dew point, and recovering the heat of the reaction gas 32. The second heat medium 51 is recovered to the low-pressure steam separation drum (not shown) through the second heat medium recovery port 56B. Then, the low-pressure steam obtained by performing gas-liquid separation is used, for example, as a heat source in the refining process for the product.

[0159] (Effects of Embodiment 3)

[0160] As described above, the reaction device 100B has a reaction container 1B, which includes at least one multi-structured reaction tube 10B, and the multi-structured reaction tube 10B performs a reaction in which a component having a higher boiling point than that in the raw material gas 31 is included in the product and the progress of the reaction in the gas phase is subject to the chemical equilibrium between the raw material and the product. Each of the at least one reaction tube 10B includes an inner cylinder 40B extending in the Z-axis direction and through which the reaction gas 32 generated in the above reaction can pass, an outer cylinder 50B in which the inner cylinder 40B is arranged, and a catalyst layer 3B arranged in the inner cylinder 40B. The distance L between the surface of the catalyst layer 3B in contact with the inner cylinder 40B and the cooling surface 53B is set to X and with a distance L X The height H of the catalyst layer 3B corresponding to the cooling surface 53B X The product of the sum of the sums from one end to the other end of the cooling surface 53B in the Z-axis direction is 500 mm. 2 The temperature of the cooling surface 53B of the outer cylinder 50B is maintained at a temperature lower than the dew point of the reaction gas 32, and part of the product is condensed in the space 4 formed between the outer cylinder 50B and the inner cylinder 40B.

[0161] According to the reaction apparatus 100B configured as described above and the chemical reaction method using the reaction apparatus 100B, the product is recovered from the reaction apparatus 100B in the form of the condensate 41 , thereby making it possible to cause the reaction to proceed at a conversion rate exceeding the equilibrium conversion rate.

[0162] In addition, the cumulative value of the reaction device 100B accumulated from one end to the other end of the cooling surface 53B in the Z-axis direction at at least one predetermined point in the circumferential direction of the cylindrical cooling surface 53B satisfies 500 mm. 2 Therefore, the reaction device 100B and the chemical reaction method using the reaction device 100B can be used even if the cooling surface 53B having a cylindrical shape is used in an area of ​​100% of the circumference direction and the cumulative value is less than 500 mm. 2 Under the same reaction conditions and parameters of the reaction device, the reaction yield of the product can also be improved.

[0163] (Comparative Example and Examples 1 to 5)

[0164] (Actual verification test)

[0165] In this actual verification test, in order to examine the relationship between the above-mentioned cumulative value and the methanol production rate, the methanol synthesis reaction was carried out using the reaction device 100A described in Embodiment 2. The above-mentioned cumulative value was less than 500 mm in the circumferential 100% area of ​​the cylindrical cooling surface. 2 Table 1 shows the conditions of the internal structures of the comparative examples and Examples 1 to 5, and the obtained results. Figure 7 The distance L is shown for the comparative example and Examples 1 to 5. A With height H A of graph of relationship. Figure 8 The graph shows the relationship between the above-mentioned integrated value and the methanol production rate of the comparative example and Examples 1 to 5. In this actual verification test, the common condition parameters between the comparative example and Examples 1 to 5 are as follows.

[0166] Raw material flow rate…115 [Ncc (standard milliliter) / minute]

[0167] Raw gas composition: H2 72%, CO2 24%, N2 4%

[0168] Catalyst: "Copper based methanol synthesis catalyst" purchased from Alfa Aesar

[0169] Catalyst filling amount…122[g]

[0170] Ratio of catalyst amount to raw material supply rate (W / F) ... 412 [g / (mole / hour)]

[0171] Pressure…0.85[MPaG]

[0172] Reaction temperature…240[℃]

[0173] Cooling water temperature…-10[℃]

[0174] Table 1 below shows the conditions of the comparative examples and the examples.

[0175] Table 1

[0176]

[0177] Examples 1 and 3 are examples in which the above-mentioned cumulative value is increased by increasing the height H by diluting the catalyst 30 relative to the comparative example. Example 2 is an example in which the above-mentioned cumulative value is increased by increasing the distance L relative to Example 1. Examples 4 and 5 are examples in which the above-mentioned cumulative value is further increased by increasing the distance L relative to Example 1 and increasing the height H by diluting the catalyst 30.

[0178] like Figure 8 As shown in FIG. 1 , it can be seen that the cumulative value is less than 500 mm in the 100% area of ​​the cylindrical cooling surface in the circumferential direction. 2 Compared with the comparative example, the above cumulative value is 500mm 2 The methanol production rate of the above embodiments is improved. Figure 7 It is understood that the higher the value of the cumulative value is, the higher the methanol production rate is.

[0179] That is, it was actually verified that even if the condition parameters were the same, by changing the internal structure, the above cumulative value would be 500mm. 2 The above can also increase the yield of the product.

[0180] (Other embodiments)

[0181] The following Examples 6 and 7 are examples that have different condition parameters from the above Examples 1 to 5 but are within the scope of the present invention. Examples 6 and 7 are examples in which the above integrated value is larger than that of Examples 1 to 5.

[0182] (Example 6)

[0183] The condition parameters of Example 6 are as follows. Raw material flow rate: 1,000 [Ncc / min], raw material gas composition: H2 71%, CO2 25%, N2 4%, catalyst: "Copper based methanol synthesis catalyst" purchased from Alfa Aesar, catalyst filling amount: 1746 [g], catalyst dilution rate: 1.0 [times], catalyst amount to raw material supply rate ratio (W / F): 679 [g / (mol / hour)], pressure: 0.85 [MPaG], reaction temperature: 200 [°C], cooling water temperature: -10 [°C], distance L: 7.8 [mm], height H: 1,500 [mm], cumulative value: 11,700 [mm 2 ]. The methanol production rate in Example 6 was 87.3%.

[0184] (Example 7)

[0185] The condition parameters of Example 7 are as follows. Raw material flow rate 1,000 [Ncc / min], raw material gas composition: H2 71%, CO2 25%, N2 4%, catalyst: "Copper based methanol synthesis catalyst" purchased from Alfa Aesar, catalyst filling amount: 2580 [g], catalyst dilution rate: 1.0 [times], catalyst amount to raw material supply rate ratio (W / F): 1003 [g / (mol / hour)], pressure: 0.85 [MPaG], reaction temperature: 200 [°C], cooling water temperature: -10 [°C], distance L: 3.8 [mm], height H: 1,500 [mm], cumulative value: 5,700 [mm 2 ]. The methanol production rate in Example 7 was 88.1%.

[0186] Description of symbols

[0187] 1. 1A, 1B… reaction vessel

[0188] 3. 3A, 3B…Catalyst layer

[0189] 4, 4A, 4B…Space

[0190] 10A, 10B…reaction tube

[0191] 20A…Outer barrel

[0192] 23, 23A, 23B…heat transfer surface

[0193] 30…Catalyst

[0194] 31…Raw gas

[0195] 32…Reaction gas

[0196] 40…Through the Wall

[0197] 40A, 40B…Inner tube

[0198] 50B…outer cylinder

[0199] 53, 53A, 53B cooling surface

[0200] 100, 100A, 100B…Reaction device

[0201] 300, 300A, 300B…filler

Claims

1. A chemical reaction method, wherein the product contains a component having a higher boiling point than a component in a raw material gas and the progress of the reaction in the gas phase is controlled by a chemical equilibrium between the raw material and the product, wherein: The feed gas comprises carbon oxides and hydrogen, and the product comprises methanol. A chemical reaction device is used, wherein the chemical reaction device has: a catalyst layer, the catalyst layer comprising a catalyst that promotes the reaction; a cooling surface spaced apart from the catalyst layer, maintained at a temperature below a dew point of a reaction gas generated in the reaction, and extending in a predetermined direction; and a permeable wall, the permeable wall being arranged at a boundary between the catalyst layer and the space, and the reaction gas being able to permeate the permeable wall, The distance between the surface of the catalyst layer in contact with the permeable wall and the cooling surface is 0.5 mm or more and 500 mm or less. The catalyst layer has a height of 1,000 mm or more and 20,000 mm or less, The product of the distance between the surface of the catalyst layer in contact with the permeable wall and the cooling surface and the height of the catalyst layer corresponding to the cooling surface having the distance is accumulated from one end to the other end of the cooling surface in the predetermined direction, and the cumulative value is 618 mm. 2 above, By supplying the raw material gas to the catalyst layer, a chemical reaction is carried out. A portion of the product produced in the chemical reaction is condensed on the cooling surface and in the space.

2. The chemical reaction method according to claim 1, wherein The cumulative value is 10,000,000 mm 2 the following.

3. A chemical reaction device, which is a chemical reaction device used in the chemical reaction method according to claim 1, wherein the chemical reaction device is a chemical reaction device for carrying out a reaction in which a component having a higher boiling point than a component in a raw material gas is contained in the product and the progress of the reaction in the gas phase is restricted by the chemical equilibrium between the raw material and the product, wherein: The feed gas comprises carbon oxides and hydrogen, and the product comprises methanol. The chemical reaction device has a catalyst layer to which the raw material gas is supplied and which contains a catalyst that promotes the reaction; a cooling surface spaced apart from the catalyst layer, maintained at a temperature below the dew point of the reaction gas, and extending in a predetermined direction; and a permeable wall, the permeable wall being arranged at a boundary between the catalyst layer and the space, and the reaction gas generated in the reaction being able to permeate through the permeable wall, The distance between the surface of the catalyst layer in contact with the permeable wall and the cooling surface is 0.5 mm or more and 500 mm or less. The catalyst layer has a height of 1,000 mm or more and 20,000 mm or less, The product of the distance between the surface of the catalyst layer in contact with the permeable wall and the outer surface of the cooling surface and the height of the catalyst layer corresponding to the outer surface having the distance is accumulated from one end to the other end of the cooling surface in the predetermined direction, and the cumulative value is 618 mm. 2 above, A portion of the product is condensed on the surface of the cooling surface and in the space.

4. The chemical reaction device according to claim 3, wherein: The cumulative value is 10,000,000 mm 2 the following.

5. The chemical reaction device according to claim 3, wherein: The chemical reaction device has a heat transfer surface maintained at a higher temperature than the cooling surface on the side opposite to the permeable wall across the catalyst.

6. A chemical reaction device, which is a chemical reaction device used in the chemical reaction method according to claim 1, wherein the chemical reaction device has a reaction container, the reaction container includes at least one multi-structured reaction tube, and the multi-structured reaction tube performs a reaction inside thereof so that the product contains a component with a higher boiling point than the component in the raw material gas and the progress of the reaction in the gas phase is restricted by the chemical equilibrium between the raw material and the product, wherein: The feed gas comprises carbon oxides and hydrogen, and the product comprises methanol. Each of the at least one reaction tube has: an inner cylinder through which the reaction gas generated in the reaction can pass, An outer cylinder having the inner cylinder arranged therein, a cooling pipe disposed inside the inner tube and extending in a predetermined direction, and A catalyst layer is disposed between the inner tube and the outer tube, The distance between the surface of the catalyst layer in contact with the inner cylinder and the outer surface of the cooling tube is 0.5 mm or more and 500 mm or less. The catalyst layer has a height of 1,000 mm or more and 20,000 mm or less, The product of the distance between the surface of the catalyst layer in contact with the inner cylinder and the outer surface of the cooling tube and the height of the catalyst layer corresponding to the outer surface having the distance is accumulated from one end to the other end of the cooling tube in the specified direction, and the cumulative value is 618 mm. 2 above, The temperature of the outer surface of the cooling tube is maintained at a temperature below the dew point of the reaction gas, A portion of the product is condensed in a space formed between the cooling tube and the inner cylinder.

7. The chemical reaction device according to claim 6, wherein: The cumulative value is 10,000,000 mm 2 the following.

8. The chemical reaction device according to claim 6, wherein: A heat medium is arranged in a space defined by the inner wall of the reaction container and the outer wall of the reaction tube.

9. A chemical reaction device used in the chemical reaction method according to claim 1, wherein the chemical reaction device comprises a reaction vessel, wherein the reaction vessel comprises at least one multi-structured reaction tube, wherein the multi-structured reaction tube performs a reaction in which a component having a higher boiling point than a component in a raw material gas is included in the product and the progress of the reaction in the gas phase is controlled by a chemical equilibrium between the raw material and the product, The feed gas comprises carbon oxides and hydrogen, and the product comprises methanol. Each of the at least one reaction tube has: an inner cylinder through which the reaction gas generated in the reaction can pass, an outer cylinder having the inner cylinder disposed therein and extending in a predetermined direction, and A catalyst layer is disposed inside the inner cylinder, The distance between the surface of the catalyst layer in contact with the inner tube and the inner surface of the outer tube is 0.5 mm or more and 500 mm or less. The catalyst layer has a height of 1,000 mm or more and 20,000 mm or less, The product of the distance between the surface of the catalyst layer in contact with the inner cylinder and the inner surface of the outer cylinder and the height of the catalyst layer corresponding to the inner surface having the distance is accumulated from one end to the other end of the inner surface in the predetermined direction, and the cumulative value is 618 mm. 2 Above, among them, The temperature of the inner surface of the outer cylinder is maintained at a temperature below the dew point of the reaction gas, A portion of the product is condensed in a space formed between the outer cylinder and the inner cylinder.

10. The chemical reaction device according to claim 9, wherein: The cumulative value is 10,000,000 mm 2 the following.

11. The chemical reaction device according to claim 9 or 10, wherein: A heat source is also provided inside the catalyst layer.

Citation Information

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