Gas separation pipe, gas separation apparatus, and method for manufacturing a gas separation pipe

Abstract

This invention provides a technology to improve the internal airtightness of gas separation pipes. [Solution] The gas separation tube comprises a cylindrical member formed of a tubular ceramic having pores, a gas separation membrane disposed on the outer circumference of the cylindrical member for separating the target gas from a mixed gas containing the target gas, a pair of metal members disposed at each end of the cylindrical member, each having a through hole in at least one of them that connects the inside and outside of the cylindrical member, and a joint that joins the cylindrical member to each of the pair of metal members, each of the pair of metal members having an annular recess into which the end of the cylindrical member is inserted, the recess having a first opposing surface facing the outer circumferential surface of the end of the cylindrical member and a second opposing surface facing the inner circumferential surface of the end of the cylindrical member, and the joint is disposed between the outer circumferential surface of the end of the cylindrical member and the first opposing surface, and between the inner circumferential surface of the end of the cylindrical member and the second opposing surface.

Description

Technical Field

[0001] The present invention relates to a gas separation tube, a gas separation device, and a method for manufacturing a gas separation tube.

Background Art

[0002] Conventionally, a gas separation tube provided with a gas separation membrane has been known (for example, Patent Documents 1 to 3).

Prior Art Documents

Patent Documents

[0003]

Patent Document 1

Patent Document 2

Patent Document 3

Summary of the Invention

[0008] In this configuration, the joint that connects the cylindrical member and the metal member is located in an annular recess of the metal member into which the end of the cylindrical member is inserted, between the outer circumferential surface of the end of the cylindrical member and the first opposing surface of the recess facing the outer circumferential surface, and between the inner circumferential surface of the end of the cylindrical member and the second opposing surface of the recess facing the inner circumferential surface. As a result, even if a gap is formed between the outer circumferential surface of the cylindrical member and the first opposing surface of the recess, or between the inner circumferential surface of the cylindrical member and the second opposing surface of the recess, due to the difference in thermal expansion between the cylindrical member formed of ceramic and the metal member, the joint between the cylindrical member and the metal member can be maintained in the other of the two spaces. Therefore, the airtightness inside the cylindrical member can be improved.

[0009] (2) In the gas separation pipe of the above form, in a temperature range of 280°C to 650°C, the coefficient of thermal expansion of the material forming the metal member is ±40 × 10⁻¹⁰ of the coefficient of thermal expansion of the ceramic forming the cylindrical member. -7It may be within / K. With this configuration, in the temperature range in which the gas separation tube is used, 280°C to 650°C, the difference in thermal expansion coefficients between the cylindrical member formed of ceramic and the metal member is ±40 × 10 -7 The temperature is within / K. This makes it easier to maintain the joint between the cylindrical member and the metal member at the joint throughout the period from when the gas separation pipe is manufactured to when it is used, thereby improving the airtightness inside the cylindrical member.

[0010] (3) In the gas separation pipe of the above form, the metal member may be formed from any one of SUS403, SUS405, SUS410, SUS430, SUS434, SUS436L, SUS443J1, SUS444, SUS409, SUS409L, 42 alloy, or Kovar. With this configuration, the metal member is formed from a material whose coefficient of thermal expansion is relatively close to that of the ceramic forming the cylindrical member. As a result, the difference in thermal expansion between the cylindrical member and the metal member makes it less likely for a gap to form between the outer surface of the cylindrical member and the first opposing surface of the recess, or between the inner surface of the cylindrical member and the second opposing surface of the recess. Therefore, the airtightness inside the cylindrical member can be improved.

[0011] (4) In the gas separation pipe of the above form, the thickness of the joint may be 0.1 mm or more and 1.0 mm or less. With this configuration, since the joint has a thickness within a certain range, the airtightness inside the cylindrical member can be improved without being affected by the difference in thermal expansion between the cylindrical member and the metal member or the dimensional variation of the cylindrical member formed by ceramic.

[0012] (5) In the gas separation pipe of the above form, the length of the joint in the depth direction of the recess may be 2 mm or more and 20 mm or less. With this configuration, the length of the joint in the depth direction of the recess into which the end of the cylindrical member is inserted is within a certain range. This makes it possible to maintain airtightness inside the cylindrical member while suppressing damage to the joint due to the difference in thermal expansion between the cylindrical member and the metal member.

[0013] (6) According to another embodiment of the present invention, a gas separation apparatus is provided. This gas separation apparatus comprises the gas separation tube described above, a container housing the gas separation tube, and a catalyst disposed outside the gas separation tube inside the container, which promotes a chemical reaction for generating the target gas from a raw material gas supplied to the inside of the container. With this configuration, the gas separation apparatus houses a gas separation tube, in which the airtightness of the inside of the cylindrical member is improved, within the container. As a result, the target gas can be generated from the raw material gas using a catalyst disposed outside the gas separation tube, and the target gas can be separated from the mixed gas containing the target gas by a gas separation membrane, thereby recovering a target gas with relatively high purity.

[0014] (7) The gas separation apparatus of the above form further comprises a pair of support parts that support each of the pair of metal members, the support parts being fixed inside the container, and the material forming at least one of the support parts of the pair may be the same material as the material forming the metal member supported by the one support part. With this configuration, at least one of the pair of support parts that support each of the pair of metal members of the gas separation pipe is made of the same material as the material forming the metal member. As a result, the thermal expansion coefficients of the metal member and at least one of the pair of support parts are the same, so that a difference in thermal expansion is unlikely to occur even if the temperature of the gas separation apparatus changes. Therefore, the gas separation pipe can be reliably supported inside the container.

[0015] (8) According to yet another embodiment of the present invention, a method for manufacturing a gas separation pipe is provided. The method for manufacturing this gas separation tube comprises the steps of: preparing a cylindrical member, a gas separation membrane, a pair of metal members, and an adhesive capable of joining the cylindrical member and the pair of metal members; placing the adhesive between the bottom surface of a recess in one of the pair of metal members and the tip surface of one end of the cylindrical member, and placing the adhesive between the bottom surface of a recess in the other of the pair of metal members and the tip surface of the other end of the cylindrical member; and melting the adhesive while applying force to at least one of the pair of metal members so as to shorten the distance between the pair of metal members, thereby moving the melted adhesive between the outer circumferential surface of the end of the cylindrical member and the first opposing surface of the recess facing the outer circumferential surface, and between the inner circumferential surface of the end of the cylindrical member and the second opposing surface of the recess facing the inner circumferential surface, and then cooling to join the cylindrical member and the pair of metal members at the joint. According to this configuration, in the process of joining a cylindrical member to each of the pair of metal members with an adhesive, the adhesive is melted and moved between the outer circumferential surface of the end of the cylindrical member and the first opposing surface of the recess facing the outer circumferential surface, and between the inner circumferential surface of the end of the cylindrical member and the second opposing surface of the recess facing the inner circumferential surface, and then cooled. As a result, even if a gap is formed between the outer circumferential surface of the end of the cylindrical member and the first opposing surface of the recess, or between the inner circumferential surface of the end of the cylindrical member and the second opposing surface of the recess, due to the difference in thermal expansion between the cylindrical member and the metal member, the joint between the cylindrical member and the metal member can be maintained by the joint in the other of the two spaces. Therefore, it is possible to manufacture a gas separation pipe that can improve the airtightness inside the cylindrical member.

[0016] Furthermore, the present invention can be realized in various forms, for example, as an apparatus equipped with a gas separation pipe, a method for manufacturing a gas separation pipe, a method for controlling an apparatus equipped with a gas separation pipe, or a computer program that causes the apparatus equipped with a gas separation pipe to perform the separation of a specific gas.

Brief Description of the Drawings

[0017] [Figure 1] It is a cross-sectional view of the gas separation tube of the first embodiment. [Figure 2] It is a first cross-sectional view of the gas separation tube of the first embodiment. [Figure 3] It is a second cross-sectional view of the gas separation tube of the first embodiment. [Figure 4] It is a diagram for explaining the manufacturing method of the gas separation tube of the first embodiment. [Figure 5] It is a first diagram for explaining the function of the gas separation tube of the first embodiment. [Figure 6] It is a second diagram for explaining the function of the gas separation tube of the first embodiment. [Figure 7] It is a schematic diagram of the gas separation device of the first embodiment.

Modes for Carrying Out the Invention

[0018] <Embodiment> FIG. 1 is a cross-sectional view of the gas separation tube 1 of the first embodiment. FIG. 2 is a first cross-sectional view of the gas separation tube 1 of this embodiment. FIG. 3 is a second cross-sectional view of the gas separation tube 1 of this embodiment. The gas separation tube 1 is a member capable of separating a target gas from a mixed gas containing the target gas. The gas separation tube 1 of this embodiment separates, for example, methanol and water as the target gases and other gases from a mixed gas containing methanol and water. The gas separation tube 1 includes a gas separation part 10, a pair of metal members 21 and 22, a connecting member 23, and joining parts 31 and 32. Note that, in FIG. 1, the size relationships of the gas separation part 10, the pair of metal members 21 and 22, the connecting member 23, and the joining parts 31 and 32 are illustrated to be different from the actual size relationships for the sake of explanation. Also, in FIG. 1, in the cross-sectional view of the gas separation tube 1 shown in FIG. 1, the longitudinal direction of the gas separation tube 1 is taken as the x-axis direction, and among the short-side directions of the gas separation tube 1, the direction perpendicular to the x-axis direction is taken as the y-axis direction, and the direction orthogonal to each of the x-axis direction and the y-axis direction is taken as the z-axis direction.

[0019] The gas separation section 10 is a cylindrical member. The gas separation section 10 comprises a cylindrical member 11 and a gas separation membrane 12.

[0020] The cylindrical member 11 is formed from a tubular ceramic having pores. In this embodiment, the cylindrical member 11 is made of alumina (Al2O3). In this embodiment, the cylindrical member 11 is a porous ceramic substrate with a porosity of 40%, and the cylindrical member 11 has through holes 11a inside. In this embodiment, the dimensions of the cylindrical member 11 are, for example, an outer diameter of 12 mm, an inner diameter of 9 mm, and a total length of 1200 mm. Details of the relationship between the material forming the cylindrical member 11 and the materials forming the pair of metal members 21 and 22, which will be described later, will be described later.

[0021] The gas separation membrane 12 is positioned on the outer circumference of the cylindrical member 11. In this embodiment, the gas separation membrane 12 is positioned on the side surface 11b of the cylindrical member 11 and has a cylindrical shape. The gas separation membrane 12 in this embodiment is a zeolite membrane that allows methanol molecules and water molecules to pass through, but does not allow hydrogen molecules, carbon monoxide molecules, and carbon dioxide molecules to pass through. As a result, the gas separation membrane 12 can separate methanol and water from a mixed gas containing methanol, water, hydrogen, carbon monoxide, and carbon dioxide.

[0022] A pair of metal members 21 and 22 are positioned at each of the two ends 111 and 112 of the cylindrical member 11. Each of the pair of metal members 21 and 22 has a substantially cylindrical shape. In this embodiment, the dimensions of each of the pair of metal members 21 and 22 are an outer diameter of 14 mm, an inner diameter of 12.4 mm, and a total length of 10 mm. Of the pair of metal members 21 and 22, metal member 21 has a through hole 21a that connects the inside (through hole 11a) of the cylindrical member 11 to the outside. Each of the pair of metal members 21 and 22 in this embodiment is made of SUS403. In a temperature range of 280°C to 650°C, the thermal expansion coefficient of the material forming the metal members 21 and 22 is ±40 × 10⁻¹⁰ of the thermal expansion coefficient of the alumina forming the cylindrical member 11.-7 The temperature is within / K. Each of the pair of metal members 21 and 22 may be formed from one of the following: SUS403, SUS405, SUS410, SUS430, SUS434, SUS436L, SUS443J1, SUS444, SUS409, SUS409L, 42 alloy, or Kovar.

[0023] Each of the pair of metal members 21 and 22 has annular recesses 211 and 221 into which the ends 111 and 112 of the cylindrical member 11 are inserted. The recess 211 is formed on the side of the cylindrical member 11 in the metal member 21. The recess 211 has a first opposing surface 211a that faces the outer circumferential surface 111a of the end 111 of the cylindrical member 11, a second opposing surface 211b that faces the inner circumferential surface 111b of the end 111 of the cylindrical member 11, and a bottom surface 211c that connects to the first opposing surface 211a and the second opposing surface 211b and faces the front end surface 111c of the end 111 of the cylindrical member 11. The recess 221 is formed on the side of the cylindrical member 11 in the metal member 22. The recess 221 has a first opposing surface 221a facing the outer circumferential surface 112a of the end 112 of the cylindrical member 11, a second opposing surface 221b facing the inner circumferential surface 112b of the end 112 of the cylindrical member 11, and a bottom surface 221c connected to the first opposing surface 221a and the second opposing surface 221b and facing the front end surface 112c of the end 112 of the cylindrical member 11.

[0024] The connecting member 23 is a tubular member provided on the metal member 21 of the pair of metal members 21 and 22, on the side opposite to the cylindrical member 11. The through hole 23a of the connecting member 23 communicates with the through hole 11a of the cylindrical member 11 via the through hole 21a of the metal member 21. In this embodiment, the outer diameter of the connecting member 23 is 12 mm, the inner diameter is 10 mm, and the total length is 50 mm. The connecting member 23 is made of SUS316.

[0025] Each of the joints 31 and 32 connects the cylindrical member 11 to the pair of metal members 21 and 22, respectively. The joint 31 is located between the outer circumferential surface 111a of the end 111 of the cylindrical member 11 and the first opposing surface 211a, and between the inner circumferential surface 111b of the end 111 of the cylindrical member 11 and the second opposing surface 211b. For the sake of explanation, the joint 31 located between the outer circumferential surface 111a of the end 111 of the cylindrical member 11 and the first opposing surface 211a will be referred to as joint 311, and the joint 31 located between the inner circumferential surface 111b of the end 111 of the cylindrical member 11 and the second opposing surface 211b will be referred to as joint 312 (see Figure 2). The joint portion 32 is located between the outer circumferential surface 112a of the end portion 112 of the cylindrical member 11 and the first opposing surface 221a, and between the inner circumferential surface 112b of the end portion 112 of the cylindrical member 11 and the second opposing surface 221b. For the sake of explanation, the joint portion 32 located between the outer circumferential surface 112a of the end portion 112 of the cylindrical member 11 and the first opposing surface 221a will be referred to as joint portion 321, and the joint portion 32 located between the inner circumferential surface 112b of the end portion 112 of the cylindrical member 11 and the second opposing surface 221b will be referred to as joint portion 322 (see Figure 3). Each of the joint portions 31 and 32 in this embodiment has a thickness of 0.1 mm or more and 1.0 mm or less. The thickness of each joint 31 and 32 is preferably about 0.1 mm, considering only the difference in thermal expansion between the cylindrical member 11 and the pair of metal members 21 and 22. However, considering the dimensional variations and roundness of the cylindrical member 11, it is preferable that the thickness be 1.0 mm or less. The length of the joint 31 in the depth direction of the recess 211 is 2 mm or more and 20 mm or less, and the length of the joint 32 in the depth direction of the recess 221 is 2 mm or more and 20 mm or less.

[0026] Each of the joints 31 and 32 in this embodiment includes inorganic glass as a base. The inorganic glass included in each of the joints 31 and 32 in this embodiment has a coefficient of thermal expansion of 72 × 10⁻⁶. -7It has a coefficient of thermal expansion of 560°C or higher and a softening point of 700°C or lower. An example of the inorganic glass contained in each of the joints 31 and 32 in this embodiment is ASF-6004A manufactured by AGC Inc., which has a softening point of 585°C. In the gas separation pipe 1 of this embodiment, since the cylindrical member 11 is formed of alumina, examples of materials used to form the joints 31 and 32 corresponding to the thermal expansion coefficient of the alumina forming the cylindrical member 11 include ASF-1094, ASF-1097, ASF-1109, ASF-2511C, YFT-531E, ASF-6004A, FP67, FP74, and KP312E, all manufactured by AGC Inc. Furthermore, in the gas separation pipe 1 of this embodiment, since the pair of metal members 21 and 22 are formed of SUS403, which has a thermal expansion coefficient greater than that of the alumina forming the cylindrical member 11, examples of materials for forming the joints 31 and 32 corresponding to the SUS403 forming the metal members 21 and 22 include ASF-1199, ASF-1100B, ASF-4001B, ASF-1941B, K-301, K-304, LS-5-300M, KF9173, KFI0115B, ASF-1898, and SG354, all manufactured by AGC Inc. Furthermore, when using a 42 alloy, which has a lower coefficient of thermal expansion than the alumina used to form the cylindrical member 11, as the material for forming the metal members 21 and 22, AGC Inc.'s ASF-1098, ASF-1099, 7574, and FP74 are examples of joints 31 and 32 whose coefficients of thermal expansion are matched to those of the metal members 21 and 22.

[0027] Next, the manufacturing method of the gas separation tube 1 of this embodiment will be described. In the manufacturing method of the gas separation tube 1, first, a gas separation section 10 comprising a cylindrical member 11 and a gas separation membrane 12, a pair of metal members 21 and 22, and a bonding agent capable of joining the cylindrical member 11 and the pair of metal members 21 and 22 are prepared.

[0028] In the fabrication of the gas separation unit 10, first, a clay mold for extrusion molding is prepared by mixing and kneading 100 parts by weight of alumina powder with an average particle size of 3 μm with 10 parts by mass of methylcellulose, 30 parts by mass of water, and 5 parts by mass of lubricant in a mixer. Next, a tubular molded body is produced by extruding the prepared clay molded body into a tubular shape using an extrusion molding machine. Next, the prepared tubular molded body is dried using a roller dryer in a temperature range of room temperature to 80°C to produce a dried molded body. Next, a cylindrical member 11, which is a ceramic porous substrate with a porosity of 40%, is produced by firing the dried molded body in an air atmosphere at a temperature of 1400°C to 1500°C for 3 hours. The prepared cylindrical member 11 is immersed vertically in a slurry of Na-ZSM-5 type crystals (Si / Al=11.9) (concentration 2.40 g / L) for 1 minute, then pulled out at 30 mm / s and dried (temperature: 180°C, time: 30 minutes). This immersion in the slurry and drying of the cylindrical member 11 is repeated twice to support seed crystals on the cylindrical member 11. Next, crystallization is performed using a hydrothermal synthesis method (temperature: 180°C, time: 6 hours) with raw materials (10Na2O:0.15Al2O3:36SiO2:960H2O) that have been aged at 50°C for 4 hours, and a zeolite film is formed on the cylindrical member 11. After the zeolite film is formed on the cylindrical member 11, it is washed with distilled water, air-dried, and then dried at 150°C to produce the gas separation unit 10.

[0029] Figure 4 is a diagram illustrating the manufacturing method of the gas separation pipe 1 according to this embodiment. In the manufacturing method of the gas separation pipe 1 according to this embodiment, the prepared adhesive is then placed between the bottom surface 211c of the recess 211 of metal member 21 of the pair of metal members 21, 22 and the front surface 111c of one end 111 of the cylindrical member 11, and the adhesive is then placed between the bottom surface 221c of the recess 221 of metal member 22 of the pair of metal members 21, 22 and the front surface 111c of the other end 112 of the cylindrical member 11. Specifically, in the gas separation pipe manufacturing apparatus M1 shown in Figure 4, each of the pair of ends 111 and 112 of the cylindrical member 11 is inserted into the recesses 211 and 221 of the pair of metal members 21 and 22. At this time, as shown in Figure 4, the prepared adhesive G1 is placed between the bottom surface 211c of the recess 211 of the metal member 21 and the tip surface 111c of one end 111 of the cylindrical member 11, and the adhesive G2 is placed between the bottom surface 221c of the recess 221 of the metal member 22 and the tip surface 111c of the other end 112 of the cylindrical member 11. After placing the adhesives G1 and G2, the cylindrical member 11 to which the pair of metal members 21 and 22 are attached is sandwiched from both sides using the Inconel springs M11 and M12 provided in the gas separation pipe manufacturing apparatus M1.

[0030] In the manufacturing method of the gas separation pipe 1 of this embodiment, the adhesive is melted and then cooled while applying force to at least one of the pair of metal members 21 and 22 so as to shorten the distance between them, thereby joining the cylindrical member 11 of the gas separation section 10 and the pair of metal members 21 and 22, respectively, at the joints 31 and 32. In Figure 4, from before joining to after joining, the biasing force of the Inconel spring M12 is used to shorten the distance between the pair of metal members 21 and 22. When a force is applied to at least one of the pair of metal members 21 and 22 such that the distance between them is shortened, the bonding agent G1 that melts in the recess 211 moves between the outer circumferential surface 111a of the end 111 of the cylindrical member 11 and the first opposing surface 211a of the recess 211 that is opposite the outer circumferential surface 111a, and between the inner circumferential surface 111b of the end 111 of the cylindrical member 11 and the second opposing surface 211b of the recess 211 that is opposite the inner circumferential surface 111b. Furthermore, the bonding agent G2 that melts within the recess 221 moves between the outer circumferential surface 112a of the end 112 of the cylindrical member 11 and the first opposing surface 221a of the recess 221 facing the outer circumferential surface 112a, and between the inner circumferential surface 112b of the end 112 of the cylindrical member 11 and the second opposing surface 221b of the recess 221 facing the inner circumferential surface 112b. After this, by cooling the bonding agents G1 and G2, the gas separation unit 10 and the pair of metal members 21 and 22 are joined by the joints 31 and 32. In the manufacturing method of the gas separation pipe 1 of this embodiment, the joining of the cylindrical member 11 and the pair of metal members 21 and 22 is performed in an atmospheric environment at a temperature of 580°C for a heat treatment time of 30 minutes.

[0031] In the manufacturing method of the gas separation tube 1 of this embodiment, the cylindrical member 11 of the gas separation section 10 and the pair of metal members 21 and 22 are joined by joints 31 and 32, and then a vacuum pump is connected so that the inside of the cylindrical member 11 (through hole 11a) becomes a vacuum. The change in the vacuum level is observed by measuring the vacuum level inside the cylindrical member 11 after 1 hour using a vacuum pressure gauge, and it is confirmed that the airtightness inside the cylindrical member 11 is maintained. After that, it is set in a forced-air constant temperature incubator, and a thermal cycle test is performed in which the maintenance at room temperature and maintenance at 300°C are repeated 20 times. After the thermal cycle test, a vacuum pump is connected so that the inside of the cylindrical member 11 becomes a vacuum. The change in the vacuum level is observed by measuring the vacuum level inside the cylindrical member 11 after 1 hour using a vacuum pressure gauge, and it is confirmed that the airtightness inside the cylindrical member 11 is maintained. This completes the gas separation tube 1 of this embodiment.

[0032] Next, the features of the gas separation pipe 1 of this embodiment will be described. In the gas separation pipe 1 of this embodiment, the joint portion 31 is located between the outer circumferential surface 111a of the end portion 111 of the cylindrical member 11 and the first opposing surface 211a, and between the inner circumferential surface 111b of the end portion 111 of the cylindrical member 11 and the second opposing surface 211b. The joint portion 32 is located between the outer circumferential surface 112a of the end portion 112 of the cylindrical member 11 and the first opposing surface 221a, and between the inner circumferential surface 112b of the end portion 112 of the cylindrical member 11 and the second opposing surface 221b.

[0033] Figure 5 is the first diagram illustrating the function of the gas separation pipe 1 of this embodiment. Figure 6 is the second diagram illustrating the function of the gas separation pipe 1 of this embodiment. In the gas separation pipe 1 of this embodiment, the relationship between the thermal expansion coefficient of the material forming the cylindrical member 11, the thermal expansion coefficient of the materials forming the metal members 21 and 22, and the thermal expansion coefficient of the materials forming the joints 31 and 32 can be assumed to follow four patterns. Here, in order to avoid making the explanation complicated, we will use the relationship between the cylindrical member 11, the metal member 21, and the joint 31 for explanation, but the same applies to the relationship between the cylindrical member 11, the metal member 22, and the joint 32. Pattern A: A pattern in which the thermal expansion coefficient of the metal member 21 is smaller than that of the cylindrical member 11, and the thermal expansion coefficient of the joint 31 is close to that of the cylindrical member 11. • Pattern B: A pattern in which the thermal expansion coefficient of the metal member 21 is smaller than that of the cylindrical member 11, and the thermal expansion coefficient of the joint 31 is close to that of the metal member 21. Pattern C: A pattern in which the thermal expansion coefficient of the metal member 21 is greater than that of the cylindrical member 11, and the thermal expansion coefficient of the joint 31 is close to that of the cylindrical member 11. • Pattern D: A pattern in which the thermal expansion coefficient of the metal member 21 is greater than that of the cylindrical member 11, and the thermal expansion coefficient of the joint 31 is close to that of the metal member 21.

[0034] For the four patterns described above, after the cylindrical member 11 and the metal member 21 are joined by melting the bonding agent G1 during the manufacturing of the gas separation pipe 1, when the temperature of the gas separation pipe 1 drops to room temperature, tensile and compressive stresses act on the portion joined by the joint 31. Figure 6 shows the relationship between the tensile and compressive stresses acting on the gas separation pipe 1 from the time of manufacture until the temperature reaches room temperature for each of the four patterns described above. Pattern A: A tensile force acts on the interface between the metal member 21 and the joint 311, while a compressive stress is applied to the joint 312, thus strengthening the seal between the inner circumferential surface 111b of the cylindrical member 11 and the second opposing surface 211b of the metal member 21. Pattern B: A tensile force acts on the interface between the cylindrical member 11 and the joint 311, while a compressive stress is applied to the joint 312. As a result, the seal between the inner circumferential surface 111b of the cylindrical member 11 and the second opposing surface 211b of the metal member 21 is strengthened. Pattern C: A tensile force acts on the interface between the metal member 21 and the joint 312, while a compressive stress is applied to the joint 311. This strengthens the seal between the outer surface 111a of the cylindrical member 11 and the first opposing surface 211a of the metal member 21. Pattern D: A tensile force acts on the interface between the cylindrical member 11 and the joint 312, while a compressive stress is applied to the joint 311. As a result, the seal between the outer surface 111a of the cylindrical member 11 and the first opposing surface 211a of the metal member 21 is strengthened.

[0035] Furthermore, for the four patterns described above, when the temperature of the gas separation pipe 1, which is at room temperature, is raised to the operating temperature range of 250°C to 350°C, tensile force and compressive stress act on the portion joined by the joint 31. Figure 7 shows the relationship between the tensile force and compressive stress acting on the gas separation pipe 1 from room temperature to the operating temperature for each of the four patterns described above. Pattern A: A tensile force acts on the interface between the metal member 21 and the joint 312, while a compressive stress is applied to the joint 311. As a result, the seal between the outer surface 111a of the cylindrical member 11 and the first opposing surface 211a of the metal member 21 is strengthened. Pattern B: A tensile force acts on the interface between the cylindrical member 11 and the joint 312, while a compressive stress is applied to the joint 311. As a result, the seal between the outer surface 111a of the cylindrical member 11 and the first opposing surface 211a of the metal member 21 is strengthened. Pattern C: A tensile force acts at the interface between the metal member 21 and the joint 311, while a compressive stress is applied to the joint 312, thus strengthening the seal between the inner circumferential surface 111b of the cylindrical member 11 and the second opposing surface 211b of the metal member 21. Pattern D: A tensile force acts on the interface between the cylindrical member 11 and the joint 311, while a compressive stress is applied to the joint 312. As a result, the seal between the inner circumferential surface 111b of the cylindrical member 11 and the second opposing surface 211b of the metal member 21 is strengthened.

[0036] As described above, in the gas separation pipe 1 of this embodiment, the joint portion 31 is located between the cylindrical member 11 and the metal member 21, between the outer peripheral surface 111a and the first opposing surface 211a, and between the inner peripheral surface 111b and the second opposing surface 211b. The joint portion 32 is located between the cylindrical member 11 and the metal member 22, between the outer peripheral surface 112a and the first opposing surface 221a, and between the inner peripheral surface 112b and the second opposing surface 221b. As a result, as shown in Figures 6 and 7, in the gas separation pipe 1 of this embodiment, even when the temperature changes, the seal between the cylindrical member 11 and the metal members 21 and 22 becomes stronger, thereby improving the airtightness of the through hole 11a of the cylindrical member 11.

[0037] Figure 7 is a cross-sectional view of a gas separation apparatus 100 equipped with a gas separation tube 1 according to the first embodiment. The gas separation apparatus 100 produces methanol from a raw material gas containing hydrogen, carbon monoxide, and carbon dioxide, and separates and recovers the produced methanol and the by-product water. The gas separation apparatus 100 comprises a plurality of gas separation tubes 1, a container 110 that houses the plurality of gas separation tubes 1, a catalyst 120 that produces methanol and water from the raw material gas, and a support part 130 that supports the gas separation tubes 1. For the convenience of explaining the positional relationship of each part of the gas separation apparatus 100, in the cross-sectional view of the gas separation apparatus 100 shown in Figure 7, the longitudinal direction of the plurality of gas separation tubes 1 housed in the container 110 is defined as the x-axis direction, the direction in which the plurality of gas separation tubes 1 are arranged side by side and perpendicular to the x-axis direction is defined as the y-axis direction, and the direction perpendicular to the x-axis direction and the y-axis direction is defined as the z-axis direction.

[0038] The container 110 is a container having a substantially rectangular parallelepiped shape, and houses a plurality of gas separation pipes 1, a plurality of catalysts 120, etc. The container 110 in this embodiment is made of SUS316. The container 110 has a raw material gas inlet 110a, a used gas outlet 110b, and a generated gas outlet 110c.

[0039] As shown in Figure 7, the raw material gas inlet 110a is located on the positive side in the x-axis direction of the gas separation device 100. The raw material gas inlet 110a supplies raw material gas containing hydrogen, carbon monoxide, and carbon dioxide into the container 110 (white arrow F1 shown in Figure 7). In this embodiment, the raw material gas supplied via the raw material gas inlet 110a has a temperature of approximately 250°C and a pressure of 2 MPa to 3 MPa. The maximum temperature of the raw material gas is 300°C, and the maximum pressure of the raw material gas is 5 MPa.

[0040] As shown in Figure 7, the spent gas outlet 110b is located on the negative side in the z-axis direction of the gas separation device 100. The spent gas outlet 110b discharges the spent gas from inside the container 110 after methanol and water, which are produced by the catalyst 120 (described later), have been separated by the gas separation pipe 1 (white arrow F2 shown in Figure 7). The spent gas contains unreacted hydrogen, carbon monoxide, and carbon dioxide that were not used in the production of methanol and water by the catalyst 120.

[0041] As shown in Figure 7, the generated gas outlet 110c is located on the negative side in the x-axis direction of the gas separation device 100. The generated gas outlet 110c removes the gas (generated gas) containing methanol and water that is generated inside the container 110 from inside the container 110 (white arrow F3 shown in Figure 7).

[0042] The catalyst 120 is positioned outside each of the multiple gas separation tubes 1 inside the containment 110. In this embodiment, the catalyst 120 is formed to have a cylindrical shape and is positioned outside the gas separation membrane 12 provided by the gas separation tube 1. The catalyst 120 is, for example, a Cu / ZnO-based catalyst and promotes a reaction to produce methanol from the raw material gas supplied into the containment 110 via the raw material gas inlet 110a. The methanol produced in the catalyst 120 passes through the gas separation membrane 12 of the gas separation tube 1 and flows into the through-hole 11a of the cylindrical member 11.

[0043] The support portion 130 supports each of the pair of metal members 21 and 22. The support portion 130 is fixed inside the container 110. The support portion 130 in this embodiment has a first support portion 131 and a second support portion 132. The first support portion 131 and the second support portion 132 are made of the same material (SUS403) as the material that forms each of the pair of metal members 21 and 22. The first support portion 131 is connected to a connecting member 23 provided on each of the plurality of gas separation pipes 1. The second support portion 132 has a through hole 132a through which the metal member 22 provided on each of the plurality of gas separation pipes 1 is inserted. A catalyst 120 is arranged between the first support portion 131 and the second support portion 132, as shown in Figure 7.

[0044] In the gas separation apparatus 100 of this embodiment, when raw material gas is supplied to the inside of the container 110 from the raw material gas inlet 110a, it flows through the through hole 132a formed in the second support part 132 and into the space between the first support part 131 and the second support part 132. Between the first support part 131 and the second support part 132, a catalyst 120 is placed on the outside of the gas separation membrane 12 of the gas separation pipe 1, and a reaction to produce methanol from the raw material gas proceeds. The mixed gas containing methanol produced with the involvement of the catalyst 120 is separated into methanol, water and other gases in the gas separation membrane 12 of the gas separation pipe 1.

[0045] The methanol and water separated from the mixed gas by the gas separation membrane 12 pass through the through-hole 11a of the cylindrical member 11, the through-hole 21a of the metal member 21, and the through-hole 23a of the connecting member 23, and move towards the generated gas outlet 110c side of the first support part 131, where they are taken out of the container 110 via the generated gas outlet 110c. The mixed gas from which methanol and water have been separated is discharged to the outside of the container 110 as spent gas via the spent gas outlet 110b.

[0046] As described above, according to the gas separation pipe 1 of this embodiment, the joint portion 31 that joins the cylindrical member 11 and the metal member 21 is located in the annular recess 211 of the metal member 21 into which the end portion 111 of the cylindrical member 11 is inserted, between the outer peripheral surface 111a of the end portion 111 of the cylindrical member 11 and the first opposing surface 211a of the recess 211 that faces the outer peripheral surface 111a, and between the inner peripheral surface 111b of the end portion 111 of the cylindrical member 11 and the second opposing surface 211b of the recess 211 that faces the inner peripheral surface 111b. The joint portion 32 that joins the cylindrical member 11 and the metal member 22 is located in an annular recess 221 of the metal member 22 into which the end portion 112 of the cylindrical member 11 is inserted. The joint portion 32 is positioned between the outer circumferential surface 112a of the end portion 112 of the cylindrical member 11 and the first opposing surface 221a of the recess 221 that faces the outer circumferential surface 112a, and between the inner circumferential surface 112b of the end portion 112 of the cylindrical member 11 and the second opposing surface 221b of the recess 221 that faces the inner circumferential surface 112b. As a result, even if a gap is formed between the outer circumferential surfaces 111a, 112a of the cylindrical member 11 and the first opposing surfaces 211a, 221a of the recesses 211, 221, or between the inner circumferential surfaces 111b, 112b of the cylindrical member 11 and the second opposing surfaces 211b, 221b of the recesses 211, 221, due to the difference in thermal expansion between the cylindrical member 11 formed by ceramic and the metal members 21, 22, the joint state between the cylindrical member 11 and the metal members 21, 22 by the joints 31, 32 can be maintained in the other of the two of the two of the two of the two of the two of the two of the two of the recesses 211a, 221, or between the inner circumferential surfaces 111b, 112b of the cylindrical member 11 and the second opposing surfaces 211b, 221b of the recesses 211, 221. Therefore, the airtightness of the through hole 11a of the cylindrical member 11 can be improved.

[0047] Furthermore, according to the gas separation pipe 1 of this embodiment, in the temperature range in which the gas separation pipe 1 is used, 280°C to 650°C, the difference in thermal expansion coefficients between the cylindrical member 11 made of ceramic and the metal members 21 and 22 is ±40 × 10 -7The temperature is within / K. This makes it easier to maintain the joint state between the cylindrical member 11 and the metal members 21 and 22 by the joints 31 and 32 throughout the period from when the gas separation pipe 1 is manufactured to when it is used, thereby improving the airtightness of the through hole 11a of the cylindrical member 11.

[0048] Furthermore, according to the gas separation pipe 1 of this embodiment, the metal members 21 and 22 are made of a material whose coefficient of thermal expansion is relatively close to that of the ceramic forming the cylindrical member 11. As a result, the difference in thermal expansion between the cylindrical member 11 and the metal members 21 and 22 makes it less likely for a gap to form between the outer circumferential surfaces 111a and 112a of the cylindrical member 11 and the first opposing surfaces 211a and 221a of the recesses 211 and 221, or between the inner circumferential surfaces 111b and 112b of the cylindrical member 11 and the second opposing surfaces 211b and 221b of the recesses 211 and 221. Therefore, the airtightness of the through hole 11a of the cylindrical member 11 can be improved.

[0049] Furthermore, according to the gas separation pipe 1 of this embodiment, since the joint portions 31 and 32 have a thickness of 0.1 mm or more and 1.0 mm or less, the airtightness of the through-hole 11a of the cylindrical member 11 can be improved without being affected by the difference in thermal expansion between the cylindrical member 11 and the metal members 21 and 22, or by dimensional variations in the cylindrical member 11 formed of ceramic.

[0050] Furthermore, according to the gas separation pipe 1 of this embodiment, the joint portions 31 and 32 have a length in the depth direction of the recesses 211 and 221 into which the ends 111 and 112 of the cylindrical member 11 are inserted, which is between 2 mm and 20 mm. This makes it possible to maintain the airtightness of the through hole 11a of the cylindrical member 11 while suppressing damage to the joint portions 31 and 32 due to the difference in thermal expansion between the cylindrical member 11 and the metal members 21 and 22.

[0051] Furthermore, according to the gas separation apparatus 100 of this embodiment, the gas separation apparatus 100 houses a gas separation tube 1, in which the airtightness inside the cylindrical member 11 is improved, within a container 110. As a result, a catalyst 120 placed outside the gas separation tube 1 is used to generate the target gas from the raw material gas, and methanol is separated from the methanol-containing mixed gas by the gas separation membrane 12, thereby recovering methanol with relatively high purity.

[0052] Furthermore, in the gas separation device 100 of this embodiment, the pair of support parts 131 and 132 that support each of the pair of metal members 21 and 22 of the gas separation pipe 1 are made of the same material as the material that forms the metal members 21 and 22. As a result, the thermal expansion coefficients of the metal members 21 and 22 and the pair of support parts 131 and 132 are the same, so that a difference in thermal expansion is unlikely to occur even if the temperature of the gas separation device 100 changes. Therefore, the gas separation pipe 1 can be reliably supported inside the container 110.

[0053] Furthermore, according to the manufacturing method of the gas separation pipe 1 of this embodiment, in the step of joining the cylindrical member 11 and the pair of metal members 21 and 22 with adhesives G1 and G2, the adhesives G1 and G2 are melted and moved between the outer circumferential surfaces 111a and 112a of the cylindrical member 11 and the first opposing surfaces 211a and 221a of the recesses 211 and 221, and between the inner circumferential surfaces 111b and 112b of the cylindrical member 11 and the second opposing surfaces 211b and 221b of the recesses 211 and 221, and then cooled. As a result, even if a gap is formed between the outer circumferential surfaces 111a, 112a of the cylindrical member 11 and the first opposing surfaces 211a, 221a of the recesses 211, 221, or between the inner circumferential surfaces 111b, 112b of the cylindrical member 11 and the second opposing surfaces 211b, 221b of the recesses 211, 221, due to the difference in thermal expansion between the cylindrical member 11 formed by ceramic and the metal members 21, 22, the joint state between the cylindrical member 11 and the metal members 21, 22 by the joints 31, 32 can be maintained in the other of the two of the two of the two of the two of the two of the two of the two of the recesses 211a, 221, or between the inner circumferential surfaces 111b, 112b of the cylindrical member 11 and the second opposing surfaces 211b, 221b of the recesses 211, 221. Therefore, it is possible to manufacture a gas separation pipe 1 that can improve the airtightness of the through hole 11a of the cylindrical member 11.

[0054] <Modified form of this embodiment> The present invention is not limited to the embodiments described above, and can be implemented in various forms without departing from its spirit, for example, the following modifications are also possible.

[0055] [Example 1] In the above-described embodiment, the gas separation membrane 12 was assumed to be a zeolite membrane that permeates methanol molecules and water molecules, but does not permeate hydrogen molecules, carbon monoxide molecules, and carbon dioxide molecules. The properties of the gas separation membrane are not limited to this. For example, it can also be applied to a zeolite membrane that selectively permeates only water molecules from a mixed gas containing methanol, water, hydrogen, carbon monoxide, and carbon dioxide, or a zeolite membrane that selectively permeates ammonia molecules from a mixed gas containing hydrogen, nitrogen, and ammonia.

[0056] [Differentiation 2] In the above embodiment, in the temperature range in which the gas separation tube 1 is used, 280°C to 650°C, the difference in thermal expansion coefficients between the ceramic cylindrical member 11 and the metal members 21 and 22 is ±40 × 10 -7 It was assumed that the temperature was within / K. The difference in thermal expansion coefficients between the tubular member 11 formed of ceramic and the metal members 21 and 22 is not limited to this, but a smaller difference in thermal expansion coefficients is desirable because it reduces the tensile and compressive stresses acting on the joint.

[0057] [Difference 3] In the above-described embodiment, the metal members 21 and 22 were assumed to be formed of SUS403, whose thermal expansion coefficient is close to that of the alumina forming the cylindrical member 11. The relationship between the thermal expansion coefficient of the material forming the metal members and the thermal expansion coefficient of the ceramic forming the cylindrical member is not limited to this.

[0058] [Differentiation Example 4] In the above-described embodiment, the joints 31 and 32 were assumed to have a thickness of 0.1 mm to 1.0 mm. The thickness of the joints is not limited to this, but considering the difference in thermal expansion between the cylindrical member 11 and the metal members 21 and 22, and the dimensional variations of the cylindrical member 11 formed from ceramic, a thickness of 0.1 mm to 1.0 mm is desirable.

[0059] [Difference 5] In the above embodiment, the length of the joints 31 and 32 in the depth direction of the recesses 211 and 221 into which the ends 111 and 112 of the cylindrical member 11 are inserted is 2 mm or more and 20 mm or less. The length of the joints 31 and 32 is not limited to this, but it is desirable that it be 2 mm or more and 20 mm or less in order to maintain the airtightness of the through hole 11a of the cylindrical member 11 and to suppress damage to the joints 31 and 32 due to the difference in thermal expansion between the cylindrical member 11 and the metal members 21 and 22.

[0060] [Modification 6] In the above embodiment, the pair of support parts 131 and 132 that support each of the pair of metal members 21 and 22 of the gas separation pipe 1 are assumed to be made of the same material as the material forming the metal members 21 and 22. One of the pair of support parts 131 and 132 may be made of the same material as the material forming the metal members 21 and 22. Alternatively, the material forming each of the pair of support parts 131 and 132 may be different from the material forming the metal members 21 and 22, but it is preferable that the coefficients of thermal expansion are similar.

[0061] [Difference 7] In the above-described embodiment, the gas separation device is provided with a catalyst. However, the catalyst may not be necessary, and the gas separation device may simply separate the target gas from the mixed gas supplied to the container.

[0062] The embodiments of this specification have been described above based on the embodiments and modifications described above. The embodiments described above are for the purpose of facilitating understanding of this specification and do not limit it. This specification may be modified and improved without departing from its spirit and the scope of the claims, and equivalents thereof are included in this specification. Furthermore, any technical features that are not described as essential in this specification may be deleted as appropriate.

[0063] <Application Example 1> It is a gas separation pipe, A cylindrical member formed from a tubular ceramic having pores, A gas separation membrane is arranged on the outer circumference of the cylindrical member and separates the target gas from a mixed gas containing the target gas, A pair of metal members arranged at each end of the cylindrical member, the pair of metal members having a through hole formed in at least one of them that connects the inside and outside of the cylindrical member, A joint portion that connects the cylindrical member and each of the pair of metal members, Equipped with, The metal member has an annular recess into which the end of the cylindrical member is inserted. The recess has a first opposing surface facing the outer circumferential surface of the end of the cylindrical member, and a second opposing surface facing the inner circumferential surface of the end of the cylindrical member. The joint is characterized in that it is positioned between the outer circumferential surface of the end of the cylindrical member and the first opposing surface, and between the inner circumferential surface of the end of the cylindrical member and the second opposing surface. Gas separation pipe. <Application Example 2> The gas separation pipe described in Application Example 1, In a temperature range of 280°C to 650°C, the thermal expansion coefficient of the material forming the metal member is ±40 × 10⁻¹⁰ of the thermal expansion coefficient of the ceramic forming the cylindrical member. -7 Characterized by being within / K, Gas separation pipe. <Application Example 3> A gas separation pipe as described in Application Example 1 or Application Example 2, The aforementioned metal member is characterized by being formed from one of the following: SUS403, SUS405, SUS410, SUS430, SUS434, SUS436L, SUS443J1, SUS444, SUS409, SUS409L, 42 alloy, or Kovar. Gas separation pipe. <Application Example 4> A gas separation pipe described in any one of the examples from Application Example 1 to Application Example 3, The thickness of the joint is characterized by being 0.1 mm or more and 1.0 mm or less. Gas separation pipe. <Application Example 5> A gas separation pipe described in any one of the examples from Application Example 1 to Application Example 4, The length of the joint in the depth direction of the recess is characterized to be 2 mm or more and 20 mm or less. Gas separation pipe. <Application Example 6> A gas separation device, A gas separation pipe described in any one of Application Examples 1 to 5, A container for housing the aforementioned gas separation pipe, The present invention is characterized by comprising a catalyst disposed outside the gas separation pipe within the containment, which promotes a reaction for generating the target gas from the raw material gas supplied inside the containment, Gas separation device. <Application Example 7> The gas separation apparatus described in Application Example 6 further includes: A pair of support parts for supporting each of the pair of metal members, comprising a pair of support parts fixed inside the container, The material forming at least one of the pair of support parts is the same material as the material forming the metal member supported by the one support part. Gas separation device. <Application Example 8> A method for manufacturing a gas separation pipe, A step of preparing a cylindrical member, a gas separation membrane, a pair of metal members, and a bonding agent capable of joining the cylindrical member and the pair of metal members, The steps include: placing the adhesive between the bottom surface of a recess in one of the pair of metal members and the tip surface of one end of the cylindrical member; and placing the adhesive between the bottom surface of a recess in the other of the pair of metal members and the tip surface of the other end of the cylindrical member; The method is characterized by comprising the step of joining the cylindrical member and each of the pair of metal members by a joint by applying force to at least one of the pair of metal members such that the distance between the pair of metal members is shortened, while melting the bonding agent, thereby moving the melted bonding agent between the outer circumferential surface of the end of the cylindrical member and the first opposing surface of the recess facing the outer circumferential surface, and between the inner circumferential surface of the end of the cylindrical member and the second opposing surface of the recess facing the inner circumferential surface, and then cooling. A method for manufacturing gas separation pipes. [Explanation of Symbols]

[0064] 1...Gas separation pipe 11…Cylindrical member 12…Gas separation membrane 21, 22… Metal components 21a...Through hole 31,32,311,312,321,322...Joint part 100... Gas separation device 110...container 111,112…ends 111a, 112a...outer surface 111b,112b…Inner peripheral surface 111c,112c…Tip surface 120... Catalyst 130...Support part 211,221… recessed 211a, 221a... First opposing surface 211b, 221b... Second opposing surface 211c, 221c…Bottom surface G1, G2… Bonding agent

Claims

1. It is a gas separation pipe, A cylindrical member formed from a tubular ceramic having pores, A gas separation membrane is arranged on the outer circumference of the cylindrical member and separates the target gas from a mixed gas containing the target gas, A pair of metal members arranged at each end of the cylindrical member, the pair of metal members having a through hole formed in at least one of them that connects the inside and outside of the cylindrical member, A joint portion that connects the cylindrical member and each of the pair of metal members, Equipped with, The metal member has an annular recess into which the end of the cylindrical member is inserted. The recess has a first opposing surface facing the outer circumferential surface of the end of the cylindrical member, and a second opposing surface facing the inner circumferential surface of the end of the cylindrical member. The joint is characterized in that it is positioned between the outer circumferential surface of the end of the cylindrical member and the first opposing surface, and between the inner circumferential surface of the end of the cylindrical member and the second opposing surface. Gas separation pipe.

2. A gas separation pipe according to claim 1, In a temperature range of 280°C to 650°C, the thermal expansion coefficient of the material forming the metal member is ±40 × 10⁻¹⁰ of the thermal expansion coefficient of the ceramic forming the cylindrical member. -7 Characterized by being within / K, Gas separation pipe.

3. A gas separation pipe according to claim 1 or claim 2, The metal member is characterized by being made of one of the following: SUS403, SUS405, SUS410, SUS430, SUS434, SUS436L, SUS443J1, SUS444, SUS409, SUS409L, 42 alloy, or Kovar. Gas separation pipe.

4. A gas separation pipe according to claim 1 or claim 2, The thickness of the joint is characterized by being 0.1 mm or more and 1.0 mm or less. Gas separation pipe.

5. A gas separation pipe according to claim 1 or claim 2, The length of the joint in the depth direction of the recess is characterized to be 2 mm or more and 20 mm or less. Gas separation pipe.

6. A gas separation device, A gas separation pipe according to claim 1 or claim 2, A container for housing the aforementioned gas separation pipe, The present invention is characterized by comprising a catalyst disposed outside the gas separation pipe within the containment, which promotes a reaction for generating the target gas from the raw material gas supplied inside the containment, Gas separation device.

7. The gas separation apparatus described in claim 6 further includes: A pair of support parts for supporting each of the pair of metal members, comprising a pair of support parts fixed inside the container, The material forming at least one of the pair of support parts is the same material as the material forming the metal member supported by the one support part. Gas separation device.

8. A method for manufacturing a gas separation pipe, A step of preparing a cylindrical member, a gas separation membrane, a pair of metal members, and a bonding agent capable of joining the cylindrical member and the pair of metal members, The steps include: placing the adhesive between the bottom surface of a recess in one of the pair of metal members and the tip surface of one end of the cylindrical member; and placing the adhesive between the bottom surface of a recess in the other of the pair of metal members and the tip surface of the other end of the cylindrical member; The method is characterized by comprising the step of joining the cylindrical member and each of the pair of metal members by a joint by applying force to at least one of the pair of metal members such that the distance between the pair of metal members is shortened, while melting the bonding agent, thereby moving the melted bonding agent between the outer circumferential surface of the end of the cylindrical member and the first opposing surface of the recess facing the outer circumferential surface, and between the inner circumferential surface of the end of the cylindrical member and the second opposing surface of the recess facing the inner circumferential surface, and then cooling. A method for manufacturing gas separation pipes.

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