JP2011072958A - Inspection method and inspection device of hydrogen separation film, and method and apparatus for manufacturing hydrogen separation film module - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide an inspection method of hydrogen separation film capable of reliably removing a hydrogen separation film having a film defect by detecting a pinhole being the film defect with high precision in order to manufacture a high-quality hydrogen separation film module, and capable of improving the efficiency of manufacturing the hydrogen separation film module. <P>SOLUTION: The inspection method for inspecting leak of gas of the hydrogen separation films 2, 22 includes: a step of mounting the hydrogen separation films 2, 22 onto the surface 4a of a plate-shape member 4 provided with a plurality of pore parts 4b corresponding to a leak inspection part of the hydrogen separation films 2, 22; a step of applying a tension to the hydrogen separation films 2, 22; a step of pressing the outer circumference of the leak inspection part of the hydrogen separation film 2, 22 to the plate-shape member 4; a step of performing evacuation through pore parts 4b of the plate-shape member 4; and a step of measuring the amount of leak of gas which permeates the hydrogen separation films 2, 22 and enters the pore parts 4b of the plate-shape member 4 by spraying the gas onto the surface of the hydrogen separation films 2, 22 of the opposite side of the contacting surface with the plate-shape member 4. <P>COPYRIGHT: (C)2011,JPO&INPIT

Description

  The present invention relates to a hydrogen separation membrane inspection method and inspection apparatus for inspecting a leak (leakage) of a gas that permeates a hydrogen separation membrane. Furthermore, the present invention relates to a method and apparatus for manufacturing a hydrogen separation membrane module that inspects for a leak of gas that permeates the hydrogen separation membrane and manufactures a hydrogen separation membrane module using the hydrogen separation membrane.

  Hydrogen is increasingly produced at hydrogen stations for fuel cell vehicles, semiconductor manufacturing plants, and the like. For example, in a fuel cell vehicle, power is generated by a chemical reaction between hydrogen and oxygen in the fuel cell. Therefore, the fuel cell vehicle needs to take in oxygen from the air and be supplied with hydrogen. In order to supply hydrogen to this fuel cell vehicle, a hydrogen station is required. At present, this hydrogen station is in the stage of starting the demonstration test, but it is considered that many hydrogen stations will be constructed over a wide area by the spread of fuel cell vehicles in the future. There are two types of hydrogen stations: an off-site method and an on-site method. In the off-site system, hydrogen is transported and stored in a hydrogen station tank or the like, and this hydrogen is supplied to the fuel cell vehicle. In the on-site method, hydrogen is produced in a hydrogen station, and this hydrogen is supplied to a fuel cell vehicle. The on-site system is superior to the off-site system in that it does not require the transport of hydrogen. Currently, on-site system hydrogen stations are widely studied. Also, in semiconductor manufacturing factories, ultra-high purity hydrogen is required as a material gas for semiconductors, and such ultra-high purity hydrogen is being purified.

  Regarding hydrogen, generally 99.99 vol. % (4N) or higher purity is required, but 99.999 vol. % (5N) or higher purity may be required. As typical methods for producing such hydrogen, there are a PSA (Pressure Swing Adsorption) method and a membrane reformer method. In the PSA system, hydrogen is produced by removing a gas other than hydrogen from a reformed gas such as city gas with an adsorbent. On the other hand, in the membrane reformer method, hydrogen is produced by allowing a reformed gas such as city gas to permeate through a hydrogen separation membrane that allows only hydrogen to permeate. The membrane reformer method is considered to be superior to the PSA method in terms of hydrogen production efficiency. Currently, it is widely studied to produce hydrogen by the membrane reformer method.

  Here, regarding a method for producing a hydrogen separation membrane used in the membrane reformer method, hydrogen separation is performed by plating and vapor-depositing a Pd (palladium) alloy or the like on a thin film made of a porous material having gas permeability. It is known to produce membranes. In this manufacturing method, the thickness of the hydrogen separation membrane can be formed to about 5 μm to about 10 μm. However, in this manufacturing method, when reducing membrane defects such as leaks, it is necessary to close the pores of the porous substrate, so that the thickness of the hydrogen separation membrane becomes thicker and the hydrogen separation membrane becomes thinner. It becomes difficult. Therefore, when the hydrogen separation membrane is thinned, the hydrogen separation membrane contains many membrane defects, and the purity of hydrogen produced by such a hydrogen separation membrane is 99.99 vol. % (4N) or less.

  Therefore, as another method for producing a hydrogen separation membrane, a method of producing a hydrogen separation membrane having a thickness of about 20 μm by rolling a Pd alloy material or the like into a thin film may be used. When a hydrogen separation membrane is produced by this production method, the purity of hydrogen produced by the hydrogen separation membrane is 99.99 vol. % (4N) or more. However, in this manufacturing method, when inclusions having a particle size of 10 μm are included in the material, the Pd alloy material is rolled together with the inclusions to generate pinholes based on the inclusions in the hydrogen separation membrane. There is a risk. This pinhole causes problems such as gas leakage, a decrease in purity of hydrogen produced by the hydrogen separation membrane, and a decrease in durability of the hydrogen separation membrane.

  In order to solve such a problem, Patent Document 1 and Patent Document 2 disclose that an ingot is removed from the ingot obtained by melting after cold-floating and melting the Pd alloy material. It is disclosed to reduce the number of inclusions and reduce the generation of pinholes in the hydrogen separation membrane.

  It is also conceivable to remove the hydrogen separation membrane having a film defect by inspecting for the presence of a film defect such as a pinhole. Regarding such inspection, Patent Document 3 and Patent Document 4 disclose inspection of a metal membrane (corresponding to a hydrogen separation membrane) by an optical method. Patent Document 3 confirms the presence or absence of a defect hole (corresponding to a pinhole) generated in a metal film by reflecting light emitted from a light source to the metal film and detecting the reflected light with a light receiving sensor. Is disclosed. Patent Document 4 discloses that light emitted from a light source is transmitted through a metal film, and the transmitted light is detected by a light receiving sensor, thereby confirming the presence or absence of a defect hole generated in the metal film. Yes.

  Further, for the hydrogen separation membrane inspection, the He leak inspection for determining the presence or absence of membrane defects by measuring the amount of He (helium) leakage that passes through the hydrogen separation membrane, and the presence or absence of membrane defects from the pressure resistance of the hydrogen separation membrane. It is conceivable to perform an airtight test such as a pressure test to judge. However, it is difficult to perform a He leak test, a pressure resistance test, etc. on a single hydrogen separation membrane composed of a thin film. Therefore, as in Patent Document 5, the hydrogen separation membrane is inspected in the state of a hydrogen separation membrane module combined with a support having a hole through which hydrogen permeates. By this inspection, the amount of He leaks through the hydrogen separation membrane module is measured, and the hydrogen separation membrane module having a membrane defect is discarded.

JP 2006-175379 A JP 2008-223119 A JP 2003-057189 A JP 2002-257740 A JP 2009-011978 A

  However, in Patent Document 1 and Patent Document 2, only the reduction of pinholes generated by removing inclusions in the ingot is considered, and when the hydrogen separation membrane is produced by rolling the ingot In addition, it is difficult to reduce pinholes generated by the inclusion of foreign matter.

  In the inspection by optical methods such as Patent Document 3 and Patent Document 4, it is difficult to detect a pinhole having a diameter of about 5 μm generated in a thin film having a thickness of 20 μm or less. It is also difficult to detect pinholes that penetrate diagonally.

  Further, as in Patent Document 5, when a He leak test is performed on a hydrogen separation membrane module, it is necessary to assemble a hydrogen separation membrane having a membrane defect into the hydrogen separation membrane module. Since such a hydrogen separation membrane module is finally discarded, the production efficiency of the hydrogen separation module deteriorates, which causes a problem.

  The present invention has been made in view of such a situation, and its purpose is to detect pinholes that cause membrane defects with high accuracy in order to manufacture high-quality hydrogen separation membrane modules, and to detect membrane defects. To provide a hydrogen separation membrane inspection method and inspection apparatus, and a hydrogen separation membrane module manufacturing method that can reliably exclude the hydrogen separation membrane from the production of the hydrogen separation membrane and improve the production efficiency of the hydrogen separation membrane module It is in.

  In order to solve the problem, an inspection method for a hydrogen separation membrane according to the present invention is an inspection method for inspecting a gas leakage of a hydrogen separation membrane, and includes a plurality of holes corresponding to the leak inspection portion of the hydrogen separation membrane. A step of placing the hydrogen separation membrane on the surface of the plate-like member provided with a step, a step of applying tension to the hydrogen separation membrane, and an outer periphery of a leak inspection section of the hydrogen separation membrane against the plate-like member. Applying the gas to the surface of the hydrogen separation membrane on the opposite side of the contact surface with the plate-like member, and the step of evacuating the hole from the plate-like member. Measuring the amount of leak of the gas that permeates the membrane and enters the hole of the plate-like member.

  An inspection apparatus for a hydrogen separation membrane according to the present invention is an inspection apparatus for inspecting a leak of a gas that permeates a hydrogen separation membrane, is configured to be capable of mounting the hydrogen separation membrane, and mounts the hydrogen separation membrane A plate-like member having a plurality of holes in a portion, a holding plate configured to be able to press the hydrogen separation membrane against the plate-like member, and having an opening corresponding to a leak inspection portion of the hydrogen separation membrane; A seal member provided so as to seal between the hydrogen separation membrane and the pressing plate; tension applying means for applying tension to the hydrogen separation membrane; and a vacuum pump configured to be evacuated from a hole of the plate-like member; The gas blowing means for blowing the gas to the surface of the hydrogen separation membrane opposite to the contact surface with the plate-like member, and the hole that penetrates the hydrogen separation membrane and enters the hole of the plate-like member Gas measurement to measure the amount of gas leak Means for evacuating from the hole of the plate-like member by the vacuum pump, applying tension to the hydrogen separation membrane placed on the plate-like member by the tension applying means, and After the outer periphery of the leak inspection part of the hydrogen separation membrane is pressed against the plate-like member, the gas is blown onto the hydrogen separation membrane by the gas blowing means, passes through the hydrogen separation membrane and passes through the hydrogen separation membrane. The amount of leakage of the gas entering the hole is measured by the gas measuring means.

  The method for manufacturing a hydrogen separation membrane module of the present invention is a manufacturing method for inspecting a gas leakage of a hydrogen separation membrane and manufacturing the hydrogen membrane module using the hydrogen separation membrane, wherein the hydrogen separation membrane leaks. Placing the hydrogen separation membrane on the surface of a plate-like member having a plurality of holes corresponding to the inspection portion and attached to the base plate; applying tension to the hydrogen separation membrane; A step of pressing an outer periphery of a leak inspection portion of the hydrogen separation membrane against the plate-like member, a step of evacuating the hole from the plate-like member, and the hydrogen opposite to the contact surface with the plate-like member Measuring the amount of leakage of the gas that permeates the hydrogen separation membrane and enters the hole of the plate-like member by blowing the gas onto the surface of the separation membrane; and the amount of leakage is equal to or less than a threshold value. Above And a step of mounting the element separation film in the plate-like member and said base plate.

  An apparatus for manufacturing a hydrogen separation membrane module according to the present invention is a manufacturing apparatus for inspecting a gas leakage of a hydrogen separation membrane and manufacturing the hydrogen membrane module using the hydrogen separation membrane, wherein the hydrogen separation membrane is mounted. A plate-like member configured to be able to be placed and having a plurality of holes in a portion on which the hydrogen separation membrane is placed; and a base plate attached to the plate-like member and configured to be able to attach the hydrogen separation membrane; A pressure plate configured to be able to press the hydrogen separation membrane against the plate-like member and having an opening corresponding to a leak inspection portion of the hydrogen separation membrane, and to seal between the hydrogen separation membrane and the pressure plate A contact surface between the sealing member provided, tension applying means for applying tension to the hydrogen separation membrane, a vacuum pump configured to be evacuated from the hole of the plate-like member, and the plate-like member Is a gas spraying means for spraying the gas from the surface of the hydrogen separation membrane on the opposite side, and a gas measuring means for measuring the leak amount of the gas that passes through the hydrogen separation membrane and enters the hole of the plate-like member; And evacuating from the hole of the plate-like member by the vacuum pump, applying tension to the hydrogen separation membrane placed on the plate-like member by the tension applying means, and After pressing the outer periphery of the leakage inspection portion of the separation membrane against the plate-like member, the gas is blown onto the hydrogen separation membrane by the gas blowing means, and passes through the hydrogen separation membrane to pass through the hole of the plate-like member The amount of leakage of the gas entering is measured by the gas measuring means, and the hydrogen separation membrane having the leakage amount equal to or less than a threshold is attached to the plate member and the base plate.

According to the present invention, the following effects can be obtained.
An inspection method for a hydrogen separation membrane according to the present invention is an inspection method for inspecting a gas leak in a hydrogen separation membrane, wherein a plate-like member provided with a plurality of holes corresponding to the leak inspection portion of the hydrogen separation membrane is provided. Placing the hydrogen separation membrane on the surface; applying tension to the hydrogen separation membrane; pressing an outer periphery of a leak inspection portion of the hydrogen separation membrane against the plate-like member; Evacuating from the hole of the member, and blowing the gas onto the surface of the hydrogen separation membrane on the side opposite to the contact surface with the plate-like member, thereby passing through the hydrogen separation membrane and the plate Measuring the leak amount of the gas entering the hole of the member.
The hydrogen separation membrane inspection apparatus according to the present invention is an inspection device for inspecting a leak of a gas that permeates the hydrogen separation membrane, is configured to be capable of mounting the hydrogen separation membrane, and mounts the hydrogen separation membrane. A plate-like member having a plurality of holes in the portion to be placed, a holding plate configured to be able to press the hydrogen separation membrane against the plate-like member, and having an opening corresponding to a leak inspection portion of the hydrogen separation membrane; A seal member provided so as to seal between the hydrogen separation membrane and the pressing plate, tension applying means for applying tension to the hydrogen separation membrane, and a vacuum configured to be evacuated from the hole of the plate-like member. A gas spraying means for spraying the gas onto the surface of the hydrogen separation membrane opposite to the contact surface between the pump and the plate-like member; and the holes of the plate-like member through the hydrogen separation membrane Measure the leak amount of the gas entering Measuring means, and evacuating from the hole of the plate-like member by the vacuum pump, applying tension to the hydrogen separation membrane placed on the plate-like member by the tension applying means, and After pressing the outer periphery of the leak inspection part of the hydrogen separation membrane to the plate-like member by a plate, the gas is blown to the hydrogen separation membrane by the gas blowing means and permeates the hydrogen separation membrane to form the plate The gas measurement means measures the leak amount of the gas entering the hole of the member.
Therefore, even if the hydrogen separation membrane module is not in a state where the hydrogen separation membrane is attached to a support or the like, it is possible to perform a leak inspection with high membrane defect detection accuracy on the hydrogen separation membrane alone that is difficult to handle. In particular, during the leak test, the hydrogen separation membrane is held while being applied with tension, so that generation of wrinkles on the hydrogen separation membrane can be prevented. Therefore, it is possible to perform a leak inspection of the hydrogen separation membrane while preventing deterioration of the quality of the hydrogen separation membrane.
After such a leak inspection, for example, if a hydrogen separation membrane module is manufactured using the hydrogen separation membrane that does not include membrane defects, after inspecting the presence or absence of membrane defects in the state of the hydrogen separation membrane module as in the past, It is possible to reduce useless work for attaching a hydrogen separation membrane having a membrane defect to a support. In particular, when producing a hydrogen separation membrane module for producing high-purity hydrogen, a large number of the hydrogen separation membranes having membrane defects are generated, so that many of the hydrogen separation membranes having membrane defects are attached to a support. This wasteful work can be greatly reduced. In addition, there is no need to wastefully discard the support attached to the hydrogen separation membrane having membrane defects. Therefore, the yield and manufacturing efficiency of the hydrogen separation membrane module can be improved, and consequently the manufacturing cost of the hydrogen separation membrane module can be reduced. Further, for example, if the hydrogen separation membrane alone is made of a recyclable material, the hydrogen separation membrane alone having a membrane defect can be collected and recycled.

The method for manufacturing a hydrogen separation membrane module of the present invention is a manufacturing method for inspecting a gas leakage of a hydrogen separation membrane and manufacturing the hydrogen membrane module using the hydrogen separation membrane, wherein the hydrogen separation membrane leaks. Placing the hydrogen separation membrane on the surface of a plate-like member having a plurality of holes corresponding to the inspection portion and attached to the base plate; applying tension to the hydrogen separation membrane; A step of pressing an outer periphery of a leak inspection portion of the hydrogen separation membrane against the plate-like member, a step of evacuating the hole from the plate-like member, and the hydrogen opposite to the contact surface with the plate-like member Measuring the amount of leakage of the gas that permeates the hydrogen separation membrane and enters the hole of the plate-like member by blowing the gas onto the surface of the separation membrane; and the amount of leakage is equal to or less than a threshold value. Above And a step of mounting the element separation film in the plate-like member and said base plate.
An apparatus for manufacturing a hydrogen separation membrane module according to the present invention is a manufacturing apparatus for inspecting a gas leakage of a hydrogen separation membrane and manufacturing the hydrogen membrane module using the hydrogen separation membrane, wherein the hydrogen separation membrane is mounted. A plate-like member configured to be able to be placed and having a plurality of holes in a portion on which the hydrogen separation membrane is placed; and a base plate attached to the plate-like member and configured to be able to attach the hydrogen separation membrane; A pressure plate configured to be able to press the hydrogen separation membrane against the plate-like member and having an opening corresponding to a leak inspection portion of the hydrogen separation membrane, and to seal between the hydrogen separation membrane and the pressure plate A contact surface between the sealing member provided, tension applying means for applying tension to the hydrogen separation membrane, a vacuum pump configured to be evacuated from the hole of the plate-like member, and the plate-like member Is a gas spraying means for blowing the gas from the surface of the hydrogen separation membrane on the opposite side, and a gas measuring means for measuring the leak amount of the gas that passes through the hydrogen separation membrane and enters the hole of the plate-like member; And evacuating from the hole of the plate-like member by the vacuum pump, applying tension to the hydrogen separation membrane placed on the plate-like member by the tension applying means, and After pressing the outer periphery of the leakage inspection portion of the separation membrane against the plate-like member, the gas is blown onto the hydrogen separation membrane by the gas blowing means, and passes through the hydrogen separation membrane to pass through the hole of the plate-like member The amount of leak of the gas entering is measured by the gas measuring means, and the hydrogen separation membrane having the leak amount equal to or less than a threshold is attached to the plate member and the base plate.
Therefore, even if the hydrogen separation membrane module is not in a state where the hydrogen separation membrane is attached to a support or the like, it is possible to perform a leak inspection with high membrane defect detection accuracy on the hydrogen separation membrane alone that is difficult to handle. In particular, during the leak test, the hydrogen separation membrane is held while being applied with tension, so that generation of wrinkles on the hydrogen separation membrane can be prevented. Therefore, it is possible to perform a leak inspection of the hydrogen separation membrane while preventing deterioration of the quality of the hydrogen separation membrane.
After such a leak inspection, the hydrogen separation membrane that does not contain membrane defects is attached to the plate member and the base plate as they are to manufacture the hydrogen separation membrane module. After inspecting the presence or absence of membrane defects, it is possible to reduce wasteful work of attaching the hydrogen separation membrane having membrane defects to the plate member and the base plate. In particular, when producing the hydrogen separation membrane module for producing high-purity hydrogen, many of the hydrogen separation membranes that are judged to have membrane defects are generated, so that many of the hydrogen separation membranes having membrane defects are generated. Can be removed before attaching to the plate-like member and the base plate, and this wasteful work can be greatly reduced. In addition, it is not necessary to wastefully discard the plate member and the base plate attached to the hydrogen separation membrane having membrane defects. Therefore, the yield and manufacturing efficiency of the hydrogen separation membrane module can be improved, and consequently the manufacturing cost of the hydrogen separation membrane module can be reduced. Furthermore, if the hydrogen separation membrane alone is made of a recyclable material, the hydrogen separation membrane alone having a membrane defect can be recovered and recycled.

It is a schematic perspective view which shows the inspection apparatus in 1st Embodiment of this invention. In 1st Embodiment of this invention, it is the schematic side view which looked at the test | inspection apparatus from the longitudinal direction of the hydrogen separation membrane in the state which is conveying the hydrogen separation membrane shown by the cross section. In 1st Embodiment of this invention, it is the schematic side view which looked at the test | inspection apparatus from the longitudinal direction of the hydrogen separation membrane in the state in which the hydrogen separation membrane shown by the cross section is in leak inspection. It is a schematic perspective view which shows the inspection apparatus in 2nd Embodiment of this invention.

[First Embodiment]
The hydrogen separation membrane inspection apparatus and inspection method in the first embodiment of the present invention will be described below.
The inspection apparatus 1 in the first embodiment of the present invention will be described. The inspection apparatus 1 shown in FIGS. 1 and 2 is configured to inspect a leak of gas generated in the hydrogen separation membrane 2. The hydrogen separation membrane 2 is configured to selectively permeate hydrogen and is produced by rolling raw materials. As shown in FIG. 1 and FIG. 2, the hydrogen separation membrane 2 is formed in a band shape, and both end portions in the longitudinal direction of the hydrogen separation membrane 2 are each wound up by a cylindrical roll 3. The roll 3 is configured to wind up and unwind the hydrogen separation membrane 2. Therefore, the hydrogen separation membrane 2 can be transported along its longitudinal direction.

  A plate-like member 4 and a base plate 5 are disposed below the hydrogen separation membrane 2 located between the two rolls 3. The plate-like member 4 is attached on the surface 5 a of the base plate 5. The surface 4a of the plate-like member 4 located on the hydrogen separation membrane 2 side and the surface 5a of the base plate 5 are configured so that the hydrogen separation membrane 2 can be mounted and attached. By attaching the hydrogen separation membrane 2 to the plate member 4 and the base plate 5 as described above, a hydrogen separation membrane module can be manufactured. Here, in the state where the hydrogen separation membrane 2 is conveyed, the plate-like member 4 and the base plate 5 are positioned so as to be spaced apart from each other in the vertical direction with respect to the hydrogen separation membrane 2. In a state where the hydrogen separation membrane 2 is placed on the plate-like member 4 and the base plate 5, the hydrogen separation membrane 2 is disposed on the surface 4 a of the plate-like member 4, and a plurality of holes 4 b of the plate-like member 4 are provided. The part of the hydrogen separation membrane 2 located on the part becomes a leak inspection part.

  The plate-like member 4 is provided with a plurality of holes 4b. Further, the side 5b of the base plate 5 located on the longitudinal direction side of the hydrogen separation membrane 2 and on the surface 5a side of the base plate 5 is formed to be curved. A plurality of grooves 5c extending along the longitudinal direction of the hydrogen separation membrane 2 are provided on the surface 5a of the base plate 5 corresponding to the plate-like member 4, and the plurality of grooves 5c communicate with each other. . The base plate 5 is provided with a vent hole 5d, and the vent hole 5d communicates with the plurality of grooves 5c.

  The inspection apparatus 1 is provided with a vacuum pump 6 for evacuating the hydrogen separation membrane 2 on the plate-like member 4 side, and a gas measuring means 7 for measuring the amount of gas that passes through the hydrogen separation membrane 2. Yes. A first vent pipe 8 is attached to the vent hole 5 d of the base plate 5, and the vent hole 5 d and the vacuum pump 6 are connected by the first vent pipe 8. A vacuum gauge 9 is disposed in the first vent pipe 8, and a vacuum exhaust valve 10 is disposed between the vacuum pump 6 and the vacuum gauge 9 of the first vent pipe 8. Further, a second vent pipe 11 is attached to the first vent pipe 8 so as to branch the gas flow between the vacuum gauge 9 and the vacuum exhaust valve 10. 11, the gas measuring means 7 and the first vent pipe 8 are connected. A gas measurement valve 12 is disposed in the second vent pipe 11.

  A pressing plate 13 is provided above the hydrogen separation membrane 2 located between the two rolls 3. The pressing plate 13 is arranged corresponding to the base plate 5. The holding plate 13 has an opening 13a corresponding to the leak inspection portion. Such a pressing plate 13 is configured to be movable up and down. A seal member 14 is provided between the hydrogen separation membrane 2 and the pressing plate 13. The seal member 14 is formed corresponding to the shape of the presser plate 13, and the seal member 14 is formed with an opening 14 a corresponding to the leak inspection part, similarly to the presser plate 13. Here, as an example, the seal member 14 may be attached to the surface of the pressing plate 13 located on the hydrogen separation membrane 2 side. As another example, the sealing member 14 is independent of the pressing plate 13. It may be provided.

  When the pressing plate 13 and the sealing member 14 are raised, the pressing plate 13 and the sealing member 14 are positioned so as to be spaced apart from the hydrogen separation membrane 2 in the vertical direction, and the hydrogen separation membrane 2 can be transported. It has become. In a state where the pressing plate 13 and the sealing member 14 are lowered, the pressing plate 13 and the sealing member 14 press the outer periphery of the leak inspection portion of the hydrogen separation membrane 2 against the plate-like member 4 and the base plate 5. Seals the space between the hydrogen separation membrane 2 and the pressing plate 13.

  A gas spraying means 15 is provided in the vicinity of the opening 13 a of the pressing plate 13. This gas spraying means 15 is configured to spray a gas for leak measurement onto the surface of the hydrogen separation membrane 2 on the opposite side of the contact surface with the surface 4 a of the plate-like member 4.

  A tension applying means 16 is attached to the lower part of the base plate 5. The tension applying means 16 is configured to make the base plate 5 movable in the vertical direction. Therefore, the tension applying means 16 is configured to apply tension to the hydrogen separation membrane 2 by moving the base plate 5 upward and pressing the plate member 4 and the base plate 5 against the hydrogen separation membrane 2 from below. . At this time, the hydrogen separation membrane 2 contacts the surface 4a of the plate-like member 4, the surface 5a and the side portion 5b of the base plate 5, but the side portion 5b of the base plate 5 is curved. It is hard to get hurt.

Here, although an example of a further preferable form is demonstrated about the inspection apparatus 1, the structure of the inspection apparatus 1 is not limited.
As a raw material used for the hydrogen separation membrane 2, it is preferable to use a metal such as Pd (palladium), Ta (tantalum), Nb (niobium), or V (vanadium), an alloy containing these as a main component, or metallic glass. . The thickness of the hydrogen separation membrane 2 is preferably 20 μm or less, and the width of the hydrogen separation membrane 2 is preferably 1 cm to 20 cm.
As the gas for measuring the leak, a gas capable of measuring the leak amount of the gas that permeates the hydrogen separation membrane 2 may be used. As an example of this gas, it is preferable to use He (helium) gas.

The plate-like member 4 is preferably made of metal, but as another example, the plate-like member 4 may be made of a material other than metal as long as the hydrogen separation membrane 2 can be supported. The surface roughness of the plate-like member 4 is preferably Ry 10 μm or less, and optimally Ry 1.6 μm or less.
The vacuum pump 6 may be configured to be evacuated from atmospheric pressure, and is preferably a rotary pump, a drive pump, or the like, for example.
The gas measuring means 7 is preferably a residual gas analyzer (Q mass) with a leak detector and a differential exhaust function, and can further measure a gas leak amount to a minimum of 1 × 10 ⁻¹⁰ Pa · m ³ / sec. Preferably there is.
The evacuation valve 10 and the gas measurement valve 12 may be flow rate adjustment valves.
The sealing member 14 may be an elastic member capable of sealing the space between the hydrogen separation membrane 2 and the pressing plate 13, and is preferably a silicon sheet, a rubber sheet, or the like.
The gas spraying means 15 is preferably configured to be able to spray gas in small amounts, and is preferably configured as an air gun, for example. In this case, the gas spraying means 15 may be configured to be movable so as to spray gas over the entire leak inspection part of the hydrogen separation membrane 2.

An inspection method for a hydrogen separation membrane in the first embodiment of the present invention will be described.
(Step 1) As shown in FIGS. 1 and 2, the plate member 4 and the base plate 5 are spaced apart from the hydrogen separation membrane 2 in the vertical direction. The holding plate 13 and the seal member 14 are in a state spaced apart from the hydrogen separation membrane 2 in the vertical direction. The evacuation valve 10 and the gas measurement valve 12 are closed.
(Step 2) The hydrogen separation membrane 2 is transported by the roll 3, and the leak inspection part of the hydrogen separation membrane 2 is moved above the plate-like member 4 and the base plate 5 and below the pressing plate 13.
(Step 3) The base plate 5 is raised by the tension applying means 16, and the hydrogen separation membrane 2 is placed on the surface 4a of the plate-like member 4 and the surface 5a of the base plate 5.
(Step 4) Further, the base plate 5 is lifted by the tension applying means 16, the plate member 4 and the base plate 5 are pressed against the hydrogen separation membrane 2, and a tension is applied to the hydrogen separation membrane 2. At this time, the hydrogen separation membrane 2 comes into contact with the surface 4a of the plate-like member 4, the surface 5a of the base plate 5, and the curved side portion 5b.
(Step 5) The pressing plate 13 is lowered together with the seal member 14, and the outer periphery of the leak inspection portion of the hydrogen separation membrane 2 is pressed against the plate-like member 4 and the base plate 5 by the pressing plate 13 and the sealing member 14. At this time, the sealing member 14 seals the space between the hydrogen separation membrane 2 and the pressing plate 13. At this time, the inspection apparatus 1 is in a state as shown in FIG.
(Step 6) While the vacuum exhaust valve 10 is opened, the vacuum pump 6 is operated to perform vacuum exhaust from the plurality of holes 4b of the plate member 4 on the plate member 4 side of the hydrogen separation membrane 2.
(Step 7) When the vacuum gauge 9 indicates a threshold value or less, the vacuum exhaust valve 10 is closed. As an example, this threshold is preferably 10 Pa.
(Step 8) The gas measurement valve 12 is opened, and a gas for leak measurement is sprayed onto the hydrogen separation membrane 2 by the gas spraying means 15. The sprayed gas passes through the hydrogen separation membrane 2 and enters the hole 4b of the plate-like member 4 and is sent to the gas measuring means 7. Thus, the total leak amount of the gas is measured by the leak detection device 7.

[Second Embodiment]
An inspection apparatus and inspection method for a hydrogen separation membrane in the second embodiment of the present invention will be described below. The basic configuration of the inspection apparatus and inspection method in the second embodiment is the same as that of the inspection apparatus and inspection method in the first embodiment. Elements similar to those in the first embodiment will be described using the same symbols and names as those in the first embodiment. Here, a configuration different from the first embodiment will be described.

The inspection device 21 in the second embodiment of the present invention will be described.
As shown in FIG. 4, the hydrogen separation membrane 22 is formed in a sheet shape corresponding to the plate-like member 4 and the base plate 5. The tension applying means for applying tension to the hydrogen separation membrane 22 is not shown, but it is preferable to temporarily fix the hydrogen separation membrane 22 with a tension applying means such as a pin or clip while applying tension to the hydrogen separation membrane 22.

An inspection method in the second embodiment of the present invention will be described.
Unlike the (Step 1) to (Step 4) in the inspection method of the first embodiment, the inspection method of the second embodiment has the following steps.
(Step 1 ′) As shown in FIG. 4, the pressing plate 13 and the sealing member 14 are spaced apart from the plate-like member 4 and the base plate 5 in the vertical direction. The evacuation valve 10 and the gas measurement valve 12 are closed.
(Step 2 ′) The hydrogen separation membrane 22 is formed in a sheet shape corresponding to the plate-like member 4 and the base plate 5.
(Step 3 ′) The hydrogen separation membrane 22 is placed on the surface 4 a of the plate-like member 4 and the surface 5 a of the base plate 5.
(Step 4 ') While applying tension to the hydrogen separation membrane 22, the hydrogen separation membrane 22 is temporarily fixed by tension applying means such as pins and clips.

[Third Embodiment]
An apparatus and a method for manufacturing a hydrogen separation membrane module according to the third embodiment of the present invention will be described below. The basic configuration of the inspection apparatus and the inspection method used in the manufacturing apparatus and the manufacturing method according to the third embodiment is the same as that of the inspection apparatus and the inspection method according to the first embodiment. Elements similar to those in the first embodiment will be described using the same symbols and names as those in the first embodiment. Here, a configuration different from the first embodiment will be described.

A manufacturing apparatus according to a third embodiment of the present invention will be described.
The manufacturing apparatus according to the third embodiment includes an inspection apparatus 1. Further, when the total amount of gas leaking through the hydrogen separation membrane 2 is equal to or less than the threshold value, the manufacturing apparatus is configured to attach the inspected hydrogen separation membrane 2 to the plate member 4 and the base plate 5 as they are. Yes.

  On the other hand, when the total leak amount of the gas passing through the hydrogen separation membrane 2 exceeds the threshold value, the manufacturing apparatus is configured to operate as follows. After raising the pressing plate 13 and the sealing member 14, the base plate 5 is lowered by the tension applying means 16. As a result, the pressing plate 13 and the seal member 14 are spaced apart from the hydrogen separation membrane 2 in the vertical direction, and the plate member 4 and the base plate 5 are spaced apart from the hydrogen separation membrane 2 in the vertical direction. It becomes a state. Further, the hydrogen separation membrane 2 is transported, and the leak inspection section of the new hydrogen separation membrane 2 is moved above the plate-like member 4 and the base plate 5 and below the pressing plate 13.

A manufacturing method in the third embodiment of the present invention will be described.
The manufacturing method of the third embodiment includes the following steps in addition to (Step 1) to (Step 8) in the inspection method of the first embodiment.
(Step 9a) When the total amount of gas leaks measured by the leak detector 7 is equal to or less than the threshold value, the inspected hydrogen separation membrane 2 is attached to the plate member 4 and the base plate 5 as they are.

(Step 9b) When the total amount of gas leaks measured by the leak detector 7 exceeds the threshold value, the base plate 5 is lowered by the tension applying means 16 after the presser plate 13 and the seal member 14 are raised. As a result, the pressing plate 13 and the seal member 14 are spaced apart from the hydrogen separation membrane 2 in the vertical direction, and the plate member 4 and the base plate 5 are spaced apart from the hydrogen separation membrane 2 in the vertical direction. It becomes a state. At this time, the hydrogen separation membrane 2 is transported, and the leak inspection part of the new hydrogen separation membrane 2 is moved above the plate-like member 4 and the base plate 5 and below the pressing plate 13.
(Step 10b) The same steps as (Step 2) to (Step 8) of the first embodiment are performed.

As an example of the manufacturing apparatus and the manufacturing method of the third embodiment, the threshold value of the total leak amount can be changed in accordance with the purity of hydrogen manufactured by the hydrogen separation membrane 2. For example, it is preferably 1 × 10 ⁻⁶ Pa · m ³ / sec and optimally 1 × 10 ⁻¹⁰ Pa · m ³ / sec, but is not limited thereto.

[Fourth Embodiment]
An apparatus and a method for manufacturing a hydrogen separation membrane module according to the fourth embodiment of the present invention will be described below. The basic configuration of the inspection apparatus and the inspection method used in the manufacturing apparatus and the manufacturing method according to the fourth embodiment is the same as that of the inspection apparatus and the inspection method according to the second embodiment. The same elements as those of the second embodiment will be described using the same symbols and names as those of the second embodiment. Here, a configuration different from the second embodiment will be described.

A manufacturing apparatus according to a fourth embodiment of the present invention will be described.
The manufacturing apparatus according to the fourth embodiment includes an inspection apparatus 21. Further, when the total amount of gas leaking through the hydrogen separation membrane 22 is less than or equal to the threshold value, the manufacturing apparatus is configured to attach the inspected hydrogen separation membrane 22 to the plate member 4 and the base plate 5 as they are. Yes.

  On the other hand, when the total leak amount of the gas passing through the hydrogen separation membrane 22 exceeds the threshold, the manufacturing apparatus is configured to operate as follows. The pressing plate 13 and the sealing member 14 are raised, and the pressing plate 13 and the sealing member 14 are in a state of being spaced apart from the hydrogen separation membrane 22 in the vertical direction. Further, the hydrogen separation membrane 22 is removed from the temporarily fixed state, and a new hydrogen separation membrane 22 is placed on the surface 4 a of the plate-like member 4 and the surface 5 a of the base plate 5, and the new hydrogen separation membrane 22 is placed on the new hydrogen separation membrane 22. While applying tension, the new hydrogen separation membrane 22 is temporarily fixed by tension applying means such as pins and clips.

A manufacturing method according to the fourth embodiment of the present invention will be described.
The manufacturing method according to the fourth embodiment includes the following steps in addition to (Step 1 ′) to (Step 4 ′) and (Step 5) to (Step 8) in the inspection method according to the second embodiment.
(Step 9a) When the total amount of gas leaks measured by the leak detector 7 is equal to or less than the threshold value, the inspected hydrogen separation membrane 22 is attached to the plate member 4 and the base plate 5 as they are.

(Step 9b) When the total amount of gas leaks measured by the leak detector 7 exceeds the threshold, the presser plate 13 and the seal member 14 are raised. As a result, the presser plate 13 and the seal member 14 are spaced apart from the hydrogen separation membrane 22 in the vertical direction.
(Step 10b) The hydrogen separation membrane 22 temporarily fixed to the plate-like member 4 and the base plate 5 is removed.
(Step 11b) For the new hydrogen separation membrane 22, the same steps as (Step 2 ′) to (Step 4 ′) and (Step 5) to (Step 8) in the inspection method of the second embodiment are performed.

As an example of the manufacturing apparatus and the manufacturing method of the fourth embodiment, the threshold value of the total leak amount can be changed according to the purity of hydrogen manufactured by the hydrogen separation membrane 22. For example, it is preferably 1 × 10 ⁻⁶ Pa · m ³ / sec and optimally 1 × 10 ⁻¹⁰ Pa · m ³ / sec, but is not limited thereto.

As described above, according to the first to fourth embodiments of the present invention, it is difficult to handle even if the hydrogen separation membranes 2 and 22 are not in the state of the hydrogen separation membrane module attached to the plate-like member 4 and the base plate 5. Leak inspection with high detection accuracy of membrane defects can be performed on the hydrogen separation membrane units 2 and 22. In particular, during the leak inspection, the hydrogen separation membranes 2 and 22 are held while being applied with tension, so that generation of wrinkles on the hydrogen separation membranes 2 and 22 can be prevented. Therefore, the leak inspection of the hydrogen separation membranes 2 and 22 can be performed while preventing the quality of the hydrogen separation membranes 2 and 22 from being deteriorated.
In particular, after such a leak test, the hydrogen separation membranes 2 and 22 that do not contain membrane defects are directly attached to the plate member 4 and the base plate 5 to manufacture the hydrogen separation membrane module. After inspecting for the presence or absence of membrane defects in this state, it is possible to reduce useless work of attaching the hydrogen separation membrane having membrane defects to the plate member and the base plate. In particular, when producing a hydrogen separation membrane module for producing high-purity hydrogen, a large number of hydrogen separation membranes 2 and 22 having membrane defects are generated. Therefore, many of the hydrogen separation membranes 2 and 22 having membrane defects are produced. It can be removed before being attached to the plate-like member 4 and the base plate 5, and this wasteful work can be greatly reduced. In addition, there is no need to wastefully discard the plate-like member 4 and the base plate 5 attached to the hydrogen separation membranes 2 and 22 having membrane defects. Therefore, the yield and manufacturing efficiency of the hydrogen separation membrane module can be improved, and consequently the manufacturing cost of the hydrogen separation membrane module can be reduced. Furthermore, if the hydrogen separation membranes 1 and 22 are made of a recyclable material, the hydrogen separation membranes 2 and 22 having membrane defects can be recovered and recycled.

  The first to fourth embodiments of the present invention have been described so far. However, the present invention is not limited to the above-described embodiments, and various modifications and changes can be made based on the technical idea of the present invention. Is possible.

  For example, as a modification of the first embodiment and the third embodiment of the present invention, a guide roll for guiding the transport of the hydrogen separation membrane 2 is provided for the tension applying means 16 so that the guide roll can be moved in the vertical direction. A configuration may be adopted in which tension is applied to the hydrogen separation membrane 2 by pressing the hydrogen separation membrane 2 against the plate-like member 4 and the base plate 5. The same effects as those of the first embodiment and the third embodiment of the present invention can be obtained.

[Example 1]
Example 1 of the present invention will be described. In Example 1, a hydrogen separation membrane module is manufactured using the manufacturing apparatus and manufacturing method of the third embodiment including the inspection apparatus and inspection method of the first embodiment. The manufactured hydrogen separation membrane module has a length of 50 cm and a width of 5 cm. The hydrogen separation membrane 2 for one lot used for manufacturing the hydrogen separation membrane module has a length of 60 m, a width of 6 cm, and a thickness of 20 μm, and is used in a state where the hydrogen separation membrane 2 is wound around a roll 3. . In Example 1, when all the hydrogen separation membranes 2 for one lot are used for the production of the hydrogen separation membrane module, 120 hydrogen separation membrane modules can be produced. The gas for leak measurement is He gas. Hydrogen purity 99.999 vol. With the goal of producing a hydrogen separation membrane module of% (5N) or more, the threshold value of the gas leakage amount for judging the presence or absence of membrane defects is set to 1 × 10 ⁻¹⁰ Pa · m ³ / sec.

  An airtight test is performed on the hydrogen separation membrane module manufactured under such conditions. The airtight test is a pressure test with nitrogen (differential pressure is 1 MPaG). In this airtight test, the amount of gas leaking through the hydrogen separation membrane module is measured with a precision soap membrane flow meter. In addition, the hydrogen purity in the hydrogen separation membrane module is confirmed.

  Regarding the hydrogen separation membrane modules manufactured using one lot of hydrogen separation membranes 2, the number of manufactured hydrogen separation membrane modules is counted, and the manufactured hydrogen separation membrane modules are ranked and evaluated. Regarding the rank evaluation, the leak amount is ND (Non Detected, measurement is impossible due to a small numerical value), and the hydrogen purity is 99.999 vol. If it is larger than% (5N), the evaluation is “rank A”. The leak amount is less than 0.2 Ncc / min, and the hydrogen purity is 99.999 vol. If it is% (5N) or less, the evaluation is “rank B”. The leak amount is 0.2 Ncc / min or more and less than 2 Ncc / min, and the hydrogen purity is 99.99 vol. If it is% (4N) or less, the evaluation is “rank C”. The amount of leak is larger than 2 Ncc / min, and the hydrogen purity is 99.9 vol. If it is equal to or less than% (3N), the evaluation is “rank D”.

[Example 2]
A second embodiment of the present invention will be described. In Example 2, a hydrogen separation membrane module is manufactured using the manufacturing apparatus and manufacturing method of the fourth embodiment including the inspection apparatus and inspection method of the second embodiment. In the second embodiment, the basic conditions for manufacturing the hydrogen separation membrane module are the same as those in the first embodiment, but the second embodiment is different from the first embodiment in that the hydrogen separation membrane 22 is formed in a sheet shape. Different from 1. For the hydrogen separation membrane module manufactured under such conditions, as in Example 2, the amount of gas leakage was measured, the hydrogen purity was confirmed, and the number of manufactured hydrogen separation membrane modules was further determined. Count and evaluate the manufactured hydrogen separation membrane modules.

[Comparative example]
A comparative example of the present invention will be described. In the comparative example, a hydrogen separation membrane module is manufactured by attaching all the hydrogen separation membranes of one lot as in Example 1 to the plate-like member and the base plate. In the comparative example, when all the hydrogen separation membranes for one lot are used for the production of the hydrogen separation membrane module, 100 hydrogen separation membrane modules can be produced. For the hydrogen separation membrane module manufactured under such conditions, as in Example 1, the amount of gas leakage was measured, the hydrogen purity was confirmed, and the number of produced hydrogen separation membrane modules was further determined. Count, confirm the yield, and rank the manufactured hydrogen separation membrane modules.

Table 1 shows the confirmation results of Example 1, Example 2, and Comparative Example.

  In Example 1 and Example 2, all of the manufactured hydrogen separation membrane modules were rated as Rank A. On the other hand, in the comparative example, the manufactured hydrogen separation membrane module included those evaluated as rank B, rank C, and rank D. Therefore, it has been confirmed that the present invention can provide a hydrogen separation membrane module with high quality and high production efficiency.

DESCRIPTION OF SYMBOLS 1,21 Inspection apparatus 2,22 Hydrogen separation membrane 4 Plate-like member 4a Surface 4b Hole 5 Base plate 6 Vacuum pump 7 Gas measuring means 12 Gas measuring valve 13 Holding plate 13a Opening 15 Gas spraying means 16 Tension applying means

Claims (4)

An inspection method for inspecting gas leakage of a hydrogen separation membrane,
Placing the hydrogen separation membrane on the surface of a plate-like member provided with a plurality of holes corresponding to the leak inspection portion of the hydrogen separation membrane;
Applying tension to the hydrogen separation membrane;
Pressing the outer periphery of the leak inspection part of the hydrogen separation membrane against the plate-like member;
Evacuating from the hole in the plate member;
Leakage of the gas that permeates the hydrogen separation membrane and enters the hole of the plate-like member by blowing the gas onto the surface of the hydrogen separation membrane opposite to the contact surface with the plate-like member A method for inspecting a hydrogen separation membrane comprising the steps of: measuring the amount. An inspection apparatus for inspecting a leak of gas that permeates a hydrogen separation membrane,
A plate-like member configured to be capable of placing the hydrogen separation membrane and having a plurality of holes in a portion on which the hydrogen separation membrane is placed;
A holding plate configured to be capable of pressing the hydrogen separation membrane against the plate-like member, and having an opening corresponding to a leak inspection portion of the hydrogen separation membrane;
A seal member provided so as to seal between the hydrogen separation membrane and the pressing plate;
Tension applying means for applying tension to the hydrogen separation membrane;
A vacuum pump configured to be evacuated from the hole of the plate member;
A gas spraying means for spraying the gas onto the surface of the hydrogen separation membrane opposite to the contact surface with the plate-like member;
Gas measuring means for measuring the amount of leakage of the gas that permeates the hydrogen separation membrane and enters the hole of the plate-like member, and
The vacuum pump evacuates from the hole of the plate-like member, and adds tension to the hydrogen separation membrane placed on the plate-like member by the tension applying means, and the holding plate removes the hydrogen separation membrane. After the outer periphery of the leak inspection part is pressed against the plate-like member, the gas is blown onto the hydrogen separation membrane by the gas blowing means, passes through the hydrogen separation membrane and enters the hole of the plate-like member. An apparatus for inspecting a hydrogen separation membrane configured to measure a gas leak amount by the gas measuring means. Inspecting the gas leakage of the hydrogen separation membrane, and manufacturing the hydrogen membrane module using the hydrogen separation membrane,
Placing the hydrogen separation membrane on the surface of a plate-like member having a plurality of holes corresponding to the leak inspection portion of the hydrogen separation membrane and attached to a base plate;
Applying tension to the hydrogen separation membrane;
Pressing the outer periphery of the leak inspection part of the hydrogen separation membrane against the plate-like member;
Evacuating from the hole in the plate member;
Leakage of the gas that permeates the hydrogen separation membrane and enters the hole of the plate-like member by blowing the gas onto the surface of the hydrogen separation membrane opposite to the contact surface with the plate-like member Measuring the quantity;
Attaching the hydrogen separation membrane to the plate member and the base plate, wherein the leak amount is equal to or less than a threshold value. Inspecting the gas leakage of the hydrogen separation membrane, and manufacturing the hydrogen membrane module using the hydrogen separation membrane,
A plate-like member configured to be capable of placing the hydrogen separation membrane and having a plurality of holes in a portion on which the hydrogen separation membrane is placed;
A base plate attached to the plate-like member and configured to attach the hydrogen separation membrane;
A holding plate configured to be capable of pressing the hydrogen separation membrane against the plate-like member, and having an opening corresponding to a leak inspection portion of the hydrogen separation membrane;
A seal member provided so as to seal between the hydrogen separation membrane and the pressing plate;
Tension applying means for applying tension to the hydrogen separation membrane;
A vacuum pump configured to be evacuated from the hole of the plate member;
A gas spraying means for spraying the gas from the surface of the hydrogen separation membrane opposite to the contact surface with the plate-like member;
Gas measuring means for measuring the amount of leakage of the gas that permeates the hydrogen separation membrane and enters the hole of the plate-like member, and
The vacuum pump evacuates from the hole of the plate-like member, and adds tension to the hydrogen separation membrane placed on the plate-like member by the tension applying means, and the holding plate removes the hydrogen separation membrane. After the outer periphery of the leak inspection part is pressed against the plate-like member, the gas is blown onto the hydrogen separation membrane by the gas blowing means, passes through the hydrogen separation membrane and enters the hole of the plate-like member. An apparatus for manufacturing a hydrogen separation membrane module configured to measure a gas leak amount by the gas measuring means and attach the hydrogen separation membrane to the plate member and the base plate, wherein the leak amount is equal to or less than a threshold value.

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