External pressure type high-purity hydrogen purifier and preparation method thereof

Abstract

This invention discloses an external pressure high-purity hydrogen purifier, comprising an outer cylinder with a membrane tube welded flange inserted at one end and an upper end cap inserted at the other end. The end of the membrane tube welded flange inserted into the outer cylinder is closed and has several uniformly distributed through holes, each through hole having a palladium membrane tube welded into it. The end of the palladium membrane tube away from the membrane tube welded flange is closed. An inner cylinder, sealed to the upper end cap, is also provided within the outer cylinder. A support plate with vent holes is provided within the inner cylinder. An end face flange, with a pure hydrogen interface, is sealed to the end of the membrane tube welded flange away from the outer cylinder. A raw material gas interface is provided on the outer cylinder, and a tail gas emission interface is provided on the upper end cap. The external pressure high-purity hydrogen purifier also includes a temperature measuring sleeve extending into the inner cylinder. The external pressure high-purity hydrogen purifier of this invention has a simple structure, compact layout, small device size, excellent resistance to gas impact and vibration, high hydrogen purification and separation efficiency, and a large gas throughput per unit volume.

Description

Technical Field

[0001] This invention belongs to the field of hydrogen purification equipment and its manufacturing technology, specifically relating to an external pressure high-purity hydrogen purifier and its preparation method. Background Technology

[0002] High-purity hydrogen has wide applications in petrochemical, electronics, metallurgical, and aerospace industries. In recent years, the rapid development of the new energy industry has spurred research into high-purity hydrogen production and separation technologies. Methods for purifying hydrogen include catalytic methods, pressure swing adsorption (PSA), metal hydride methods, and palladium alloy membrane diffusion. Palladium membrane diffusion, due to its unique purification performance, can obtain high-purity hydrogen with a purity of over 99.9999%. Furthermore, this technology features compact equipment, small size and weight, and convenient operation, making it suitable for small- and medium-scale high-purity hydrogen purification and possessing broad application prospects.

[0003] Palladium membrane diffusion is a method that uses a palladium membrane hydrogen purifier to separate and purify high-purity hydrogen from a mixed hydrogen gas. A palladium membrane purifier typically consists of a palladium membrane tube assembly, an external sealing shell, and piping interfaces. According to the working principle of hydrogen purifiers, the hydrogen permeation rate and purification efficiency of the palladium membrane are related to the composition, thickness, and hydrogen partial pressure across the membrane. In addition, the structural form and parameters of the purifier significantly affect hydrogen purification and separation performance, including the distribution of the palladium membrane tubes, their aspect ratio, and the size and location of the interfaces. Furthermore, existing membrane tube assemblies are usually sealed to the shell by welding, which has the disadvantage of being difficult to replace and repair if the palladium membrane tubes are damaged. Additionally, existing external pressure palladium membrane tube purifiers have poor resistance to airflow impact and vibration, leading to deformation and damage to the palladium membrane, thus affecting the service life of the palladium membrane purifier. Summary of the Invention

[0004] The technical problem to be solved by this invention is to address the shortcomings of the prior art by providing an external pressure high-purity hydrogen purifier. This purifier purifies the input hydrogen gas by setting an outer cylinder and installing a membrane tube welding flange and a palladium membrane tube within it. It provides an external pressure high-purity hydrogen purifier with a simple structure, compact layout, small device size, excellent resistance to gas impact and vibration, high hydrogen purification and separation efficiency, and a large gas throughput per unit volume.

[0005] To solve the above-mentioned technical problems, the technical solution adopted by the present invention is: an external pressure high-purity hydrogen purifier, characterized in that the external pressure high-purity hydrogen purifier includes an outer cylinder, one end of which is inserted into a sealed membrane tube welding flange, and the other end is inserted into a sealed upper end cap. The membrane tube welding flange inserted into the outer cylinder is closed and has a plurality of through holes evenly distributed. A palladium membrane tube is sealed and welded into each through hole. The end of the palladium membrane tube away from the membrane tube welding flange is closed. The outer cylinder also has an inner cylinder to accommodate all the palladium membrane tubes. The inner cylinder is sealed and connected to the upper end cap. The inner cylinder has a support plate for the palladium membrane tubes to pass through. The support plate also has a vent hole. The end of the membrane tube welding flange away from the outer cylinder is sealed and connected to an end face flange. A pure hydrogen interface is provided on the end face flange. A raw material gas interface is provided on the outer cylinder. A tail gas emission interface is provided on the upper end cap. The external pressure high-purity hydrogen purifier also has a temperature measuring sleeve extending into the inner cylinder.

[0006] The aforementioned external pressure high-purity hydrogen purifier is characterized in that the palladium membrane tube is a self-supporting dense palladium tube or a composite tube coated with a palladium film on a porous metal; the dense palladium tube and the palladium film are composed of pure Pd or a palladium alloy with a mass purity greater than 99%, wherein the palladium alloy contains, in addition to Pd, one or more of Cu, Au, Ag, Pt, Ru, Re, Ni, Fe, Ta, V, Zr, Nb, and Y; the diameter of the dense palladium tube is 1 mm to 10 mm, the wall thickness is 0.005 mm to 0.2 mm, and the length is 100 mm to 1000 mm; the porous metal tube coated with a palladium film composite tube has a diameter of 4 mm to 10 mm, a wall thickness of 0.5 mm to 2 mm, a coating thickness of 0.005 mm to 0.02 mm, and a length of 100 mm to 1000 mm; the number of palladium membrane tubes is 1 to 200.

[0007] The above-mentioned external pressure high-purity hydrogen purifier is characterized in that the through holes on the closed end of the membrane tube welding flange satisfy the following: the edge spacing between adjacent through holes is 1mm to 20mm; and the through holes on the closed end of the membrane tube welding flange are all provided with countersunk holes with a depth of 0.5mm to 2mm.

[0008] The aforementioned external pressure high-purity hydrogen purifier is characterized in that the support plate has a through hole in the center that is adapted to the temperature measuring sleeve, and the diameter of the vent hole is 0.5mm to 10mm.

[0009] The aforementioned external pressure high-purity hydrogen purifier is characterized in that the temperature measuring sleeve extends into the inner cylinder and is sealed at one end.

[0010] The aforementioned external pressure high-purity hydrogen purifier is characterized in that the end flange, outer cylinder, inner cylinder, membrane tube welded flange, and upper end cap are made of stainless steel, heat-resistant steel, nickel-based alloy, or copper-based alloy.

[0011] The aforementioned external pressure high-purity hydrogen purifier is characterized in that the inner cylinder is composed of a cap and a body, the outer diameter of the cap is larger than the outer diameter of the body, and the cap is provided with a plurality of evenly distributed U-shaped grooves, the width of the U-shaped grooves being 2mm to 5mm and the depth being 2mm to 10mm; the combined gap between the outer cylinder and the body of the inner cylinder is 2mm to 10mm.

[0012] The aforementioned external pressure high-purity hydrogen purifier is characterized in that the palladium membrane tube and the membrane tube welding flange are connected by vacuum brazing or self-fusion welding, and the end face flange and the membrane tube welding flange end are connected by a detachable flange sealing connection.

[0013] In addition, the present invention also provides a method for preparing an external pressure high-purity hydrogen purifier, characterized in that the method includes the following steps:

[0014] Step 1: Determine the specifications and quantity of palladium membrane tubes based on the gas processing capacity of the purifier, and then prepare palladium membrane tubes to obtain multiple palladium membrane tubes; the palladium membrane tubes are self-supporting dense palladium tubes or composite tubes coated on porous metal.

[0015] Step 2: Determine the diameter, arrangement and number of through holes on the welding flange and support plate of the palladium membrane tube according to the specifications and quantity of the palladium membrane tube. Make consistent through holes on the welding flange and support plate respectively. At the same time, make a through hole with the same outer diameter as the temperature measuring sleeve in the center of the support plate to obtain the welding flange and support plate of the membrane tube.

[0016] Step 3: Seal one end of the multiple palladium membrane tubes prepared in Step 1, insert the other end into the through hole of the membrane tube welding flange obtained in Step 2, and seal the two ends by welding to obtain the palladium membrane tube bundle assembly.

[0017] Step 4: Insert the temperature measuring sleeve into the center hole of the support plate and fix it in an appropriate position. Then, assemble each palladium membrane tube in the palladium membrane tube bundle assembly obtained in Step 3 with the corresponding through hole of the support plate according to the arrangement of the membrane tube welding flange. Finally, seal and connect it with the inner cylinder, outer cylinder, upper end cap and end face flange to obtain the external pressure high-purity hydrogen purifier.

[0018] This invention involves preparing a palladium membrane tube, assembling the palladium membrane tube and the membrane tube welded flange and support plate, and then sequentially installing a temperature measuring sleeve, inner cylinder, outer cylinder, upper end cap and end face flange for sealing connection, to obtain an external pressure high-purity hydrogen purifier.

[0019] The above method is characterized in that the welding in step three satisfies the following conditions: when the palladium film tube is a self-supporting dense palladium tube, brazing is used; when the palladium film tube is a composite tube coated on a porous metal, fusion welding is used. The fusion welding is laser welding, argon arc welding, or plasma welding. This invention employs different welding methods depending on the shape of the film tube; dense palladium tubes are brazed, and composite tubes are fusion welded, i.e., laser welding, argon arc welding, or plasma welding.

[0020] Compared with the prior art, the present invention has the following advantages:

[0021] 1. This invention provides a purification space by setting an outer cylinder and using a membrane tube welding flange and upper end cap for sealing. It facilitates the introduction of hydrogen to be purified and the discharge of impurity gases by setting a raw material gas interface and a tail gas discharge interface. An end face flange with a pure hydrogen interface is welded and sealed to the membrane tube welding flange, serving as the product output end of the purified high-purity hydrogen. A palladium membrane tube is installed on the membrane tube welding flange to purify the input hydrogen. An inner cylinder surrounds all the palladium membrane tubes in the center for easy hydrogen purification. A support plate supports the palladium membrane tubes. Ventilation holes allow unpermeated hydrogen and impurity gases to pass through. A temperature measuring sleeve and thermometer facilitate the monitoring of the internal temperature of the external pressure high-purity hydrogen purifier. This invention provides an external pressure high-purity hydrogen purifier with a simple structure, compact layout, small device size, excellent resistance to gas impact and vibration, high hydrogen purification and separation efficiency, and a large gas throughput per unit volume.

[0022] 2. When the external pressure high-purity hydrogen purifier of the present invention is working, the raw material hydrogen is introduced into the raw material gas interface, and after passing through the combination gap between the outer and inner cylinders and the U-shaped groove of the cylinder cap, it comes into contact with the palladium membrane tube. The hydrogen permeates from the outside of the palladium membrane tube to the inside, while the impurity gas remains on the outside of the palladium membrane tube. The purified high-purity hydrogen is output through the pure hydrogen port, while the unpermeated hydrogen and impurity gas are discharged from the tail gas emission port. The hydrogen purification and separation efficiency is high, and the gas processing capacity per unit volume is large.

[0023] 3. This invention prepares a palladium membrane tube, then assembles the palladium membrane tube with a welded flange and a support plate, and then sequentially installs the temperature measuring sleeve, inner cylinder, outer cylinder, upper end cap, and end face flange for sealing connection, thus obtaining an external pressure high-purity hydrogen purifier. The process is simple and easy to promote and use.

[0024] The technical solution of the present invention will be further described in detail below with reference to the accompanying drawings and embodiments. Attached Figure Description

[0025] Figure 1 This is a schematic diagram of the structure of the external pressure high-purity hydrogen purifier of the present invention.

[0026] Figure 2This is a schematic diagram of the inner cylinder of the external pressure high-purity hydrogen purifier of the present invention.

[0027] Figure 3 This is a schematic diagram of the structure of the cap of the inner cylinder of the external pressure high-purity hydrogen purifier of the present invention.

[0028] Explanation of reference numerals in the attached figures:

[0029] 1—Outer cylinder; 2—Membrane tube welding flange; 3—Upper end cap;

[0030] 4—Palladium film tube; 5—Inner cylinder; 5-1—Cylinder cap;

[0031] 5-2—Cylinder body; 6—Support plate; 7—End flange;

[0032] 8—Pure hydrogen inlet; 9—Feed gas inlet; 10—Exhaust gas emission inlet;

[0033] 11—Temperature measuring sleeve. Detailed Implementation

[0034] An external pressure high-purity hydrogen purifier of the present invention is described in detail through Example 1.

[0035] Example 1

[0036] like Figure 1 As shown, the external pressure high-purity hydrogen purifier of this embodiment includes an outer cylinder 1. A membrane tube welding flange 2 with a sealing connection is inserted into one end of the outer cylinder 1, and an upper end cap 3 with a sealing connection is inserted into the other end. The membrane tube welding flange 2, inserted into the outer cylinder 1, is closed at one end and has several uniformly spaced through holes. A palladium membrane tube 4 is sealed and welded into each through hole. The end of the palladium membrane tube 4 away from the membrane tube welding flange 2 is closed. An inner cylinder 5 is also provided inside the outer cylinder 1 to accommodate all the palladium membrane tubes 4. The inner cylinder 5 is sealed to the upper end cap 3. A support plate 6 is provided in the inner cylinder 5 for the palladium membrane tube 4 to pass through. The support plate 6 is also provided with a vent hole. The end of the membrane tube welding flange 2 away from the outer cylinder 1 is sealed to an end face flange 7. A pure hydrogen interface 8 is provided on the end face flange 7. A raw material gas interface 9 is provided on the outer cylinder 1. A tail gas emission interface 10 is provided on the upper end cap 3. A temperature measuring sleeve 11 extending into the inner cylinder 5 is also provided in the external pressure high-purity hydrogen purifier.

[0037] It should be noted that the outer cylinder 1 serves as the outer shell of the external pressure high-purity hydrogen purifier. A membrane tube welding flange 2 and an upper end cap 3 seal both ends of the outer cylinder 1, providing a purification space. A raw material gas inlet 9 on the outer cylinder 1 facilitates the introduction of hydrogen to be purified, and a tail gas outlet 10 on the upper end cap 3 facilitates the discharge of impurity gases. A membrane tube welding flange 2 is inserted into one end of the outer cylinder 1, and an end face flange 7 is welded and sealed onto the membrane tube welding flange 2, with a pure hydrogen inlet 8 provided for the production of purified high-purity hydrogen. At the output end, the membrane tube welding flange 2 is inserted into the outer cylinder 1, one end is closed and several through holes are evenly opened for installing palladium membrane tubes 4 and preventing gas leakage. The palladium membrane tubes 4 are used to purify the input hydrogen gas that needs to be purified. The inner cylinder 5 surrounds all the palladium membrane tubes 4 in the center to facilitate hydrogen gas purification. The palladium membrane tubes 4 are supported by a support plate 6. The vent holes allow unpermeated hydrogen gas and impurity gases to pass through. The temperature measuring sleeve 11 is installed with a thermometer to facilitate the detection of the internal temperature of the external pressure high-purity hydrogen purifier.

[0038] It should be noted that the pure hydrogen interface 8, the exhaust gas interface 10, and the raw material gas interface 9 use compression fittings or VCR connectors.

[0039] It should be noted that the diameters of the raw material gas inlet 9 and the exhaust gas outlet 10 are 4mm to 25mm.

[0040] In this embodiment, the palladium film tube 4 is a self-supporting dense palladium tube or a composite tube with a palladium film deposited on a porous metal. The dense palladium tube and the palladium film are composed of pure Pd or a palladium alloy with a mass purity greater than 99%. In addition to Pd, the palladium alloy contains one or more of Cu, Au, Ag, Pt, Ru, Re, Ni, Fe, Ta, V, Zr, Nb, and Y. The diameter of the dense palladium tube is 1 mm to 10 mm, the wall thickness is 0.005 mm to 0.2 mm, and the length is 100 mm to 1000 mm. The porous metal tube with a palladium film is a composite tube in which the diameter of the porous metal tube is 4 mm to 10 mm, the wall thickness is 0.5 mm to 2 mm, the film thickness is 0.005 mm to 0.02 mm, and the length is 100 mm to 1000 mm. The number of palladium film tubes 4 is 1 to 200.

[0041] It should be noted that the palladium membrane tube 4 comes in two forms: one is a self-supporting dense palladium tube, which is a palladium tube made of palladium or palladium alloy; the other is a composite tube formed by plating a layer of palladium or palladium alloy onto a porous metal tube. The effect of hydrogen purification can be controlled by controlling the composition and size of the dense palladium tube or palladium membrane, and the efficiency of hydrogen purification can be controlled by controlling the palladium membrane. The choice can be made according to actual needs.

[0042] In this embodiment, the through holes on the closed end of the membrane tube welding flange 2 satisfy the following conditions: the edge spacing between adjacent through holes is 1mm to 20mm; and all through holes on the closed end of the membrane tube welding flange 2 are provided with countersunk holes with a depth of 0.5mm to 2mm. By controlling the spacing of the through holes, the spacing of the palladium membrane tubes 4 is controlled, ensuring that there is a suitable distance between the palladium membrane tubes 4, so that the hydrogen in the purifier is purified uniformly.

[0043] In this embodiment, the support plate 6 has a through hole in its center that is compatible with the temperature measuring sleeve 11, and the diameter of the vent hole is 0.5mm to 10mm. By having a through hole in the center of the support plate 6 that is compatible with the temperature measuring sleeve 11, it is easy for the temperature measuring sleeve 11 to extend into the center of the purifier, making it easy to detect the temperature inside the purifier.

[0044] In this embodiment, the end of the temperature measuring sleeve 11 that extends into the inner cylinder 5 is sealed. Sealing the end of the temperature measuring sleeve 11 that extends into the inner cylinder 5 prevents air leakage.

[0045] In this embodiment, the end flange 7, outer cylinder 1, inner cylinder 5, membrane tube welded flange 2, and upper end cap 3 are made of stainless steel, heat-resistant steel, nickel-based alloy, or copper-based alloy. By controlling the materials of the end flange 7, outer cylinder 1, inner cylinder 5, membrane tube welded flange 2, and upper end cap 3, the hydrogen purification effect is ensured, as well as the service life of the purifier.

[0046] like Figure 2 and Figure 3 As shown, in this embodiment, the inner cylinder 5 consists of a cap 5-1 and a body 5-2. The outer diameter of the cap 5-1 is larger than the outer diameter of the body 5-2. The cap 5-1 has multiple evenly distributed U-shaped grooves, the width of which is 2mm to 5mm and the depth is 2mm to 10mm. The combined gap between the outer cylinder 1 and the body 5-2 of the inner cylinder 5 is 2mm to 10mm. The larger outer diameter of the cap 5-1 facilitates the formation of a combined gap between the outer cylinder 1 and the body 5-2 of the inner cylinder 5. This allows the raw material hydrogen to pass through the combined gap between the outer cylinder 1 and the body 5-2, and through the U-shaped grooves, to contact the palladium membrane tube 4, improving the purification effect. By controlling the size of the U-shaped grooves, the amount of raw material hydrogen contacting the palladium membrane tube 4 can be controlled, ensuring the purification effect.

[0047] In this embodiment, the palladium membrane tube 4 and the membrane tube welding flange 2 are connected by vacuum brazing or self-fusion welding, and the end face flange 7 and the membrane tube welding flange 2 are connected by a detachable flange.

[0048] The preparation method of an external pressure high-purity hydrogen purifier of the present invention is described in detail through Examples 2 to 4.

[0049] Example 2

[0050] This embodiment includes the following steps:

[0051] Step 1: Determine the specifications and quantity of palladium membrane tubes 4 based on the gas processing capacity of the purifier, and then prepare palladium membrane tubes 4 to obtain 50 palladium membrane tubes 4; the palladium membrane tubes 4 are self-supporting dense palladium-yttrium alloy tubes prepared by melting, rolling and drawing, with a diameter of 2mm, a wall thickness of 0.08mm and a length of 500mm.

[0052] Step 2: Based on the specifications and quantity of the palladium membrane tubes 4, determine the diameter, arrangement, and number of through holes on the membrane tube welding flange 2 and the support plate 6. Drill identical through holes on both the membrane tube welding flange 2 and the support plate 6. Simultaneously, drill a through hole in the center of the support plate 6 with the same outer diameter as the temperature measuring sleeve 11, thus obtaining the membrane tube welding flange 2 and the support plate 6. The membrane tube welding flange 2 has 50 evenly distributed through holes with a diameter of 2.05 mm, matching the outer diameter of the palladium membrane tubes 4, with a 3 mm distance between adjacent through holes. Each through hole has a 0.5 mm deep countersunk hole. The support plate 6 has a 6 mm diameter through hole in its center, matching the diameter of the temperature measuring sleeve 11, and 50 through holes with a diameter of 2.2 mm, matching the palladium membrane tubes 4. The support plate 6 also has a number of vent holes with diameters of 1 mm and 2 mm. The palladium membrane tubes 4 are evenly distributed around the axis of the membrane tube welding flange 2.

[0053] Step 3: Seal one end of the multiple palladium membrane tubes 4 prepared in Step 1, insert the other end into the through hole of the membrane tube welding flange 2 obtained in Step 2, and seal the two ends by brazing to obtain the palladium membrane tube bundle assembly.

[0054] Step 4: Insert the temperature measuring sleeve 11 into the center hole of the support plate 6 and fix it in an appropriate position. Then, assemble each palladium membrane tube 4 in the palladium membrane tube bundle assembly obtained in Step 3 with the corresponding through hole of the support plate 6 according to the arrangement of the membrane tube welding flange 2. Finally, seal and connect it with the inner cylinder 5, outer cylinder 1, upper end cap 3 and end face flange 7 to obtain an external pressure high-purity hydrogen purifier. The outer cylinder 1, inner cylinder 5, upper end cap 3, temperature measuring sleeve 11, membrane tube welding flange 2 and end face flange 7 are made of 316 stainless steel. The combination gap between the outer cylinder 1 and the inner cylinder 5 body 5-2 is 2mm. The width and depth of the U-shaped groove on the cap 5-1 of the inner cylinder 5 are 5mm. The diameter of the temperature measuring sleeve 11 is 6mm. The tail gas emission interface 10, pure hydrogen interface 8 and raw material gas interface 9 in the external pressure high-purity hydrogen purifier all adopt 1 / 4-inch VCR connectors.

[0055] In this embodiment, the dense palladium-yttrium alloy tube may also be composed of pure Pd or palladium alloy with a mass purity greater than 99%. The palladium alloy, in addition to Pd, may also contain one or more of the following: Cu, Au, Ag, Pt, Ru, Re, Ni, Fe, Ta, V, Zr, and Nb.

[0056] Example 3

[0057] This embodiment includes the following steps:

[0058] Step 1: Determine the specifications and quantity of palladium membrane tube 4 based on the gas processing capacity of the purifier, and then prepare palladium membrane tube 4 to obtain 5 palladium membrane tubes 4; the palladium membrane tube 4 is a composite tube with a palladium silver film chemically plated on the surface of a porous stainless steel tube, with a diameter of 8mm, a wall thickness of 1mm, a palladium silver film thickness of 0.005mm, and a length of 200mm.

[0059] Step 2: Based on the specifications and quantity of the palladium membrane tubes 4, determine the diameter, arrangement, and number of through holes on the membrane tube welding flange 2 and the support plate 6. Drill identical through holes on both the membrane tube welding flange 2 and the support plate 6. Simultaneously, drill a through hole in the center of the support plate 6 with the same outer diameter as the temperature measuring sleeve 11, thus obtaining the membrane tube welding flange 2 and the support plate 6. The membrane tube welding flange 2 has five evenly distributed through holes with a diameter of 8.1 mm, matching the outer diameter of the palladium membrane tubes 4, with a 20 mm distance between adjacent through holes. Each through hole has a 2 mm deep countersunk hole. The support plate 6 has a through hole in its center with a diameter of 8 mm, matching the diameter of the temperature measuring sleeve 11, and five through holes with a diameter of 8.2 mm, matching the palladium membrane tubes 4. The support plate 6 also has a number of vent holes with diameters of 4 mm and 6 mm. The palladium membrane tubes 4 are evenly distributed around the axis of the membrane tube welding flange 2.

[0060] Step 3: Seal one end of the multiple palladium membrane tubes 4 prepared in Step 1, insert the other end into the through hole of the membrane tube welding flange 2 obtained in Step 2, and seal the connection between the two by argon arc welding to obtain the palladium membrane tube bundle assembly.

[0061] Step 4: Insert the temperature measuring sleeve 11 into the center hole of the support plate 6 and fix it in an appropriate position. Then, assemble each palladium membrane tube 4 in the palladium membrane tube bundle assembly obtained in Step 3 with the corresponding through hole of the support plate 6 according to the arrangement of the membrane tube welding flange 2. Finally, seal and connect it with the inner cylinder 5, outer cylinder 1, upper end cap 3 and end face flange 7 to obtain an external pressure high-purity hydrogen purifier. The outer cylinder 1, inner cylinder 5, upper end cap 3, temperature measuring sleeve 11, membrane tube welding flange 2 and end face flange 7 are made of 310 heat-resistant steel. The combination gap between the outer cylinder 1 and the inner cylinder 5 body 5-2 is 5mm. The width of the U-shaped groove on the cap 5-1 of the inner cylinder 5 is 4mm and the depth is 4mm. The diameter of the temperature measuring sleeve 11 is 8mm. The tail gas emission interface 10, pure hydrogen interface 8 and raw material gas interface 9 in the external pressure high-purity hydrogen purifier all adopt 8mm compression fittings.

[0062] In this embodiment, the palladium-silver film in the composite tube can also be composed of pure Pd or a palladium alloy with a purity greater than 99%. The palladium alloy, in addition to Pd, also contains one or more of Cu, Au, Pt, Ru, Re, Ni, Fe, Ta, V, Zr, Nb, and Y.

[0063] Example 4

[0064] This embodiment includes the following steps:

[0065] Step 1: Determine the specifications and quantity of palladium membrane tube 4 based on the gas processing capacity of the purifier, and then prepare palladium membrane tube 4 to obtain 200 palladium membrane tubes 4; the palladium membrane tube 4 is a self-supporting dense palladium-copper alloy tube prepared by melting, rolling and drawing, with a diameter of 1mm, a wall thickness of 0.06mm and a length of 1000mm.

[0066] Step 2: Based on the specifications and quantity of the palladium membrane tubes 4, determine the diameter, arrangement, and number of through holes on the membrane tube welding flange 2 and the support plate 6. Drill identical through holes on both the membrane tube welding flange 2 and the support plate 6. Simultaneously, drill a through hole in the center of the support plate 6 with the same outer diameter as the temperature measuring sleeve 11, thus obtaining the membrane tube welding flange 2 and the support plate 6. The membrane tube welding flange 2 has 200 through holes evenly distributed with a diameter of 1.02 mm, matching the outer diameter of the palladium membrane tubes 4, with a 1 mm spacing between adjacent through holes. Each through hole has a 1 mm deep countersunk hole. The support plate 6 has a 4 mm diameter through hole in its center, matching the diameter of the temperature measuring sleeve 11, and 200 through holes with a diameter of 1.1 mm, matching the palladium membrane tubes 4. The support plate 6 also has a number of vent holes with diameters of 0.5 mm and 1 mm. The palladium membrane tubes 4 are evenly distributed around the axis of the membrane tube welding flange 2.

[0067] Step 3: Seal one end of the multiple palladium membrane tubes 4 prepared in Step 1, insert the other end into the through hole of the membrane tube welding flange 2 obtained in Step 2, and seal the two ends by brazing to obtain the palladium membrane tube bundle assembly.

[0068] Step 4: Insert the temperature measuring sleeve 11 into the center hole of the support plate 6 and fix it in an appropriate position. Then, assemble each palladium membrane tube 4 in the palladium membrane tube bundle assembly obtained in Step 3 with the corresponding through hole of the support plate 6 according to the arrangement of the membrane tube welding flange 2. Finally, seal and connect it with the inner cylinder 5, outer cylinder 1, upper end cap 3 and end face flange 7 to obtain an external pressure high-purity hydrogen purifier. The outer cylinder 1, inner cylinder 5, upper end cap 3, temperature measuring sleeve 11, membrane tube welding flange 2 and end face flange 7 are made of Monel 400 alloy. The combination gap between the outer cylinder 1 and the inner cylinder 5 body 5-2 is 5mm. The width of the U-shaped groove on the cap 5-1 of the inner cylinder 5 is 3mm and the depth is 10mm. The diameter of the temperature measuring sleeve 11 is 4mm. The tail gas emission interface 10, pure hydrogen interface 8 and raw material gas interface 9 in the external pressure high-purity hydrogen purifier all adopt 1 / 2-inch VCR connectors.

[0069] Example 5

[0070] This embodiment includes the following steps:

[0071] Step 1: Determine the specifications and quantity of palladium membrane tube 4 based on the gas processing capacity of the purifier, and then prepare palladium membrane tube 4 to obtain one palladium membrane tube 4; the palladium membrane tube 4 is a composite tube with a palladium-silver film chemically plated on the surface of a porous stainless steel tube, with a diameter of 10mm, a wall thickness of 2mm, a palladium-silver film thickness of 0.01mm, and a length of 100mm.

[0072] Step 2: Based on the specifications and quantity of the palladium membrane tube 4, determine the diameter, arrangement, and number of through holes on the membrane tube welding flange 2 and the support plate 6. Drill identical through holes on both the membrane tube welding flange 2 and the support plate 6. Simultaneously, drill a through hole in the center of the support plate 6 with the same outer diameter as the temperature measuring sleeve 11, thus obtaining the membrane tube welding flange 2 and the support plate 6. The membrane tube welding flange 2 has one through hole evenly distributed with a diameter of 8.1 mm, matching the outer diameter of the palladium membrane tube 4, and each through hole has a 1 mm deep countersunk hole. The support plate 6 has a through hole in the center with a diameter of 5 mm, matching the diameter of the temperature measuring sleeve 11, and also has one through hole with a diameter of 8.2 mm, matching the palladium membrane tube 4. The support plate 6 also has a number of vent holes with diameters of 1 mm and 2 mm distributed on it.

[0073] Step 3: Seal one end of the multiple palladium membrane tubes 4 prepared in Step 1, insert the other end into the through hole of the membrane tube welding flange 2 obtained in Step 2, and seal the connection between the two by argon arc welding to obtain the palladium membrane tube bundle assembly.

[0074] Step 4: Insert the temperature measuring sleeve 11 into the center hole of the support plate 6 and fix it in an appropriate position. Then, assemble each palladium membrane tube 4 in the palladium membrane tube bundle assembly obtained in Step 3 with the corresponding through hole of the support plate 6 according to the arrangement of the membrane tube welding flange 2. Finally, seal and connect it with the inner cylinder 5, outer cylinder 1, upper end cap 3 and end face flange 7 to obtain an external pressure high-purity hydrogen purifier. The outer cylinder 1, inner cylinder 5, upper end cap 3, temperature measuring sleeve 11, membrane tube welding flange 2 and end face flange 7 are made of 310 heat-resistant steel. The combination gap between the outer cylinder 1 and the inner cylinder 5 body 5-2 is 10mm. The width of the U-shaped groove on the cap 5-1 of the inner cylinder 5 is 2mm and the depth is 2mm. The diameter of the temperature measuring sleeve 11 is 5mm. The tail gas emission interface 10, pure hydrogen interface 8 and raw material gas interface 9 in the external pressure high-purity hydrogen purifier all adopt 8mm compression fittings.

[0075] Example 6

[0076] This embodiment includes the following steps:

[0077] Step 1: Determine the specifications and quantity of palladium membrane tubes 4 based on the gas processing capacity of the purifier, and then prepare palladium membrane tubes 4 to obtain 100 palladium membrane tubes 4; the palladium membrane tube 4 is a composite tube with a palladium-silver film chemically plated on the surface of a porous stainless steel tube, with a diameter of 4mm, a wall thickness of 0.5mm, a palladium-silver film thickness of 0.02mm, and a length of 1000mm.

[0078] Step 2: Based on the specifications and quantity of the palladium membrane tubes 4, determine the diameter, arrangement, and number of through holes on the membrane tube welding flange 2 and the support plate 6. Drill identical through holes on both the membrane tube welding flange 2 and the support plate 6. Simultaneously, drill a through hole in the center of the support plate 6 with the same outer diameter as the temperature measuring sleeve 11, thus obtaining the membrane tube welding flange 2 and the support plate 6. The membrane tube welding flange 2 has 100 through holes evenly distributed with a diameter of 8.1 mm, matching the outer diameter of the palladium membrane tubes 4, with a 10 mm distance between adjacent through holes. Each through hole has a 2 mm deep countersunk hole. The support plate 6 has a 6 mm diameter through hole in its center, matching the diameter of the temperature measuring sleeve 11, and 100 through holes with a diameter of 8.2 mm, matching the palladium membrane tubes 4. The support plate 6 also has a number of vent holes with diameters of 8 mm and 10 mm distributed throughout. The palladium membrane tubes 4 are evenly distributed around the axis of the membrane tube welding flange 2.

[0079] Step 3: Seal one end of the multiple palladium membrane tubes 4 prepared in Step 1, insert the other end into the through hole of the membrane tube welding flange 2 obtained in Step 2, and seal the connection between the two by argon arc welding to obtain the palladium membrane tube bundle assembly.

[0080] Step 4: Insert the temperature measuring sleeve 11 into the center hole of the support plate 6 and fix it in an appropriate position. Then, assemble each palladium membrane tube 4 in the palladium membrane tube bundle assembly obtained in Step 3 with the corresponding through hole of the support plate 6 according to the arrangement of the membrane tube welding flange 2. Finally, seal and connect it with the inner cylinder 5, outer cylinder 1, upper end cap 3 and end face flange 7 to obtain an external pressure high-purity hydrogen purifier. The outer cylinder 1, inner cylinder 5, upper end cap 3, temperature measuring sleeve 11, membrane tube welding flange 2 and end face flange 7 are made of 310 heat-resistant steel. The combination gap between the outer cylinder 1 and the inner cylinder 5 body 5-2 is 8mm. The width of the U-shaped groove on the cap 5-1 of the inner cylinder 5 is 2mm and the depth is 8mm. The diameter of the temperature measuring sleeve 11 is 6mm. The tail gas emission interface 10, pure hydrogen interface 8 and raw material gas interface 9 in the external pressure high-purity hydrogen purifier all adopt 8mm compression fittings.

[0081] Example 7

[0082] The difference between this implementation and Example 4 is that the palladium film tube 4 is a self-supporting dense palladium-copper alloy tube prepared by melting, rolling and drawing, with a diameter of 10 mm, a wall thickness of 0.005 mm and a length of 100 mm.

[0083] Example 8

[0084] The difference between this implementation and Example 4 is that the palladium film tube 4 is a self-supporting dense palladium-copper alloy tube prepared by melting, rolling and drawing, with a diameter of 6 mm, a wall thickness of 0.2 mm and a length of 200 mm.

[0085] The above description is merely a preferred embodiment of the present invention and is not intended to limit the invention in any way. Any simple modifications, alterations, and equivalent changes made to the above embodiments based on the inventive essence shall still fall within the protection scope of the present invention.

Claims

1. An outer pressure type high purity hydrogen purifier characterized by comprising: The outer pressure type high-purity hydrogen purifier comprises an outer cylinder (1), a sealingly connected membrane tube welding flange (2) is inserted into one end of the outer cylinder (1), and an upper head (3) is inserted into the other end of the outer cylinder (1); a plurality of through holes are uniformly arranged on the sealingly connected membrane tube welding flange (2) inserted into one end of the outer cylinder (1); a palladium membrane tube (4) is sealingly welded in each through hole; the palladium membrane tube (4) is closed at one end away from the membrane tube welding flange (2); an inner cylinder (5) for accommodating all the palladium membrane tubes (4) is arranged in the outer cylinder (1); the inner cylinder (5) is sealingly connected with the upper head (3); a support disc (6) for the palladium membrane tube (4) to pass through is arranged in the inner cylinder (5); the support disc (6) is further provided with a gas permeable hole; an end face flange (7) is sealingly connected to one end of the membrane tube welding flange (2) away from the outer cylinder (1); a pure hydrogen interface (8) is arranged on the end face flange (7); a raw material gas interface (9) is arranged on the outer cylinder (1); the upper head (3) is provided with a tail gas discharge interface (10); a temperature measuring sleeve (11) is further arranged in the inner cylinder (5); the inner cylinder (5) is composed of a cylinder cap (5-1) and a cylinder body (5-2); the outer diameter of the cylinder cap (5-1) is larger than that of the cylinder body (5-2); a plurality of uniformly distributed U-shaped grooves are arranged on the cylinder cap (5-1); the width of the U-shaped groove is 2mm-5mm, and the depth is 2mm-10mm; the combined gap between the outer cylinder (1) and the cylinder body (5-2) of the inner cylinder (5) is 2mm-10mm.

2. The external pressure type high-purity hydrogen gas purifier according to claim 1, characterized by The palladium membrane tube (4) is a self-supporting dense palladium tube or a composite tube with a palladium film plated on a porous metal tube; the composition of the dense palladium tube and the palladium film is pure Pd or a palladium alloy with a mass purity greater than 99%; the palladium alloy contains one or more than two of Cu, Au, Ag, Pt, Ru, Re, Ni, Fe, Ta, V, Zr, Nb and Y in addition to Pd; the diameter of the dense palladium tube is 1mm-10mm, the wall thickness is 0.005mm-0.2mm, and the length is 100mm-1000mm; the composite tube with a palladium film plated on a porous metal tube has a diameter of 4mm-10mm, a wall thickness of 0.5mm-2mm, a film plating thickness of 0.005mm-0.02mm, and a length of 100mm-1000mm; the number of the palladium membrane tubes (4) is 1-200.

3. The external pressure type high-purity hydrogen gas purifier according to claim 1, characterized by The through holes on the closed end of the membrane tube welding flange (2) satisfy that the edge distance between adjacent through holes is 1mm-20mm; the through holes on the closed end of the membrane tube welding flange (2) are all provided with a counterbore with a depth of 0.5mm-2mm.

4. The external pressure type high-purity hydrogen gas purifier according to claim 1, characterized by The support disc (6) is provided with a through hole in the center, which is adapted to the temperature measuring sleeve (11); the diameter of the gas permeable hole is 0.5mm-10mm.

5. The external pressure type high-purity hydrogen gas purifier according to claim 1, characterized by The temperature measuring sleeve (11) is inserted into one end of the inner cylinder (5).

6. The external pressure type high-purity hydrogen gas purifier according to claim 1, characterized by The material of the end face flange (7), the outer cylinder (1), the inner cylinder (5), the membrane tube welding flange (2) and the upper head (3) is stainless steel, heat-resistant steel, nickel-based alloy or copper-based alloy.

7. The external pressure type high-purity hydrogen gas purifier according to claim 1, characterized by The palladium membrane tube (4) and the membrane tube welding flange (2) are connected by vacuum brazing or self-fusion welding sealing, and the end face flange (7) and the membrane tube welding flange (2) are connected by detachable flange sealing.

8. A method of manufacturing the external pressure type high-purity hydrogen gas purifier according to any one of claims 1 to 7, characterized by, The method comprises the following steps: Step one, according to the gas treatment capacity of the purifier, the specification and quantity of the palladium membrane tube (4) are determined, and then the palladium membrane tube (4) is prepared to obtain a plurality of palladium membrane tubes (4); the palladium membrane tube (4) is a self-supporting dense palladium tube or a composite tube plated on a porous metal; Step two, according to the specification and quantity of the palladium membrane tube (4), the hole diameter of the through hole on the membrane tube welding flange (2) and the support disc (6) and the arrangement mode and quantity of the through hole are determined, and the consistent through holes are opened on the membrane tube welding flange (2) and the support disc (6), and a through hole with the same diameter as the outer diameter of the temperature measuring sleeve (11) is opened in the center of the support disc (6), thereby obtaining the membrane tube welding flange (2) and the support disc (6); Step three, one end of the plurality of palladium membrane tubes (4) prepared in step one is sealed, and the other end is inserted into the through hole of the membrane tube welding flange (2) obtained in step two, and the two are sealed and connected by welding, thereby obtaining a palladium membrane tube bundle assembly; Step four, the temperature measuring sleeve (11) is inserted into the center hole of the support disc (6) and fixed in place, then each palladium membrane tube (4) in the palladium membrane tube bundle assembly obtained in step three is assembled according to the arrangement mode of the membrane tube welding flange (2) and the corresponding through hole of the support disc (6), and finally sealed and connected with the inner cylinder (5), the outer cylinder (1), the upper head (3) and the end face flange (7), thereby obtaining an external pressure type high-purity hydrogen purifier.

9. The method of claim 8, wherein, The welding in step three satisfies that when the palladium membrane tube (4) is a self-supporting dense palladium tube, the brazing method is used, and when the palladium membrane tube (4) is a composite tube plated on a porous metal, the fusion welding method is used, and the fusion welding is laser welding, argon arc welding or plasma welding.

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