JP2021049520A - Hydrogen permeation device - Google Patents

Abstract

To provide a hydrogen permeation device having a heightened hydrogen permeation performance.SOLUTION: A hydrogen permeation device having a hydrogen permeable metal film between a primary side which is a supply side of raw material gas, and a secondary side which is a taking-out side of permeated gas, has, on the primary side, a raw material supply pipe 13 for forming a raw material gas supply route, raw material gas discharge routes 16a, 16b for discharging the raw material gas not permeating the secondary side, and an aperture plate 14 to be combined with the tip side of the raw material supply pipe 13. A diameter of an exhaust nozzle 15 of the aperture plate 14 is formed smaller than an inner diameter of the raw material supply pipe 13.SELECTED DRAWING: Figure 1

Description

The present invention relates to a hydrogen permeation device, and more particularly to a technique suitable for permeating hydrogen through a hydrogen permeation metal membrane.

As a technique related to hydrogen permeation, the hydrogen separator described in Patent Document 1 is known.
As described in paragraph 0008 of Patent Document 1, the hydrogen separator comprises a hydrogen permeable film formed of a non-palladium-based metal that permeates hydrogen or an alloy containing a non-palladium-based metal as a main metal, and hydrogen. A raw material gas supply flow path for supplying the contained raw material gas to the surface on the primary side of the hydrogen permeable film, a hydrogen recovery flow path for recovering hydrogen permeated to the surface on the secondary side of the hydrogen permeable film, and a raw material gas. In order to form a channel having a predetermined width for distributing the raw material gas supplied from the supply channel along the surface on the primary side of the hydrogen permeable film, only a predetermined width from the surface on the primary side of the hydrogen permeable film. It is provided with a flow path forming portion arranged at a distance.

Paragraph 0045 of Patent Document 1 describes that high hydrogen permeability can be obtained by providing the flow distribution flange 60.

JP-A-2019-5684

An object of the present invention is to provide a means for obtaining high hydrogen permeability by a means completely different from the flow distribution flange.

The means for solving the problem of the present invention is as follows.

First,
A hydrogen permeation device having a hydrogen permeation metal film between the primary side, which is the supply side of the raw material gas, and the secondary side, which is the extraction side of the permeated gas.
On the primary side
The raw material supply pipe that forms the raw material gas supply path,
A raw material gas discharge path that discharges a raw material gas that does not permeate to the secondary side,
It has a perforated plate that engages with the tip side of the raw material supply pipe.
A hydrogen permeation device characterized in that the size of the ejection hole of the perforated plate is smaller than that of the raw material supply pipe.
Here, the size of the ejection hole means the diameter when the ejection hole is a circle.
Therefore, when the ejection hole is circular, the diameter of the ejection hole is smaller than the inner diameter of the raw material supply pipe.
Further, as the shape of the ejection hole, in addition to the circle, various shapes such as a polygon such as a triangle, a quadrangle, and a pentagon, and a star-shaped polygon can be adopted.
Here, in the case of a polygon or a star-shaped polygon, "the size of the ejection hole is smaller than that of the raw material supply pipe" means that the shape of the polygon or the star-shaped polygon itself forms the inner diameter of the raw material supply pipe. It means that it fits within the circle.

Second,
A hydrogen permeation device having a hydrogen permeation metal film between the primary side, which is the supply side of the raw material gas, and the secondary side, which is the extraction side of the permeated gas.
On the primary side
The raw material supply pipe that forms the raw material gas supply path,
A raw material gas discharge path that discharges a raw material gas that does not permeate to the secondary side,
It has a perforated plate that engages with the tip side of the raw material supply pipe.
A hydrogen permeation device characterized in that the diameter of the ejection hole of the perforated plate is smaller than the inner diameter of the raw material supply pipe.

Third,
The hydrogen permeation device according to the first or second aspect, wherein the ejection holes of the opening plate have a tapered shape from the primary side to the secondary side.
Here, having a tapered shape means forming a taper so that the shape of the ejection hole gradually decreases from the primary side to the secondary side, and also from the primary side to the secondary side. A case where a taper is formed so that the shape of the ejection hole gradually increases is also included.
The shape of the ejection hole when forming the taper is preferably a circle in consideration of workability, but even in the case of various shapes such as a polygon such as a triangle, a quadrangle, and a pentagon, and a star-shaped polygon. , Can be adopted.

Fourth,
The second type is characterized in that the diameter of the ejection hole of the opening plate is one-half or less, preferably one-third or less, more preferably about one-fourth of the inner diameter of the raw material supply pipe. Or the hydrogen permeation device according to the third.
Here, about one-fourth means that, in addition to the one-fourth value, a range having substantially the same action and effect as in the case of one-fourth is included.

The hydrogen-permeable metal film may be a pure metal of a Group 5 element such as V, Nb, or Ta, which has a property of transmitting hydrogen, or a group 5 metal formed of an alloy, but pure vanadium is preferable.
Further, it is desirable to sputter palladium or a palladium-based alloy as a catalyst on both surfaces of the hydrogen permeable metal film.

According to the present invention, hydrogen permeation performance can be enhanced.

It is a vertical sectional view of the main part which concerns on Example 1 of this invention. It is a vertical sectional view of the whole which concerns on Example 1 of this invention. It is a perspective view of the primary side which concerns on Example 1 of this invention. It is a perspective view of the whole vertical cross section which concerns on Example 1 of this invention. It is a vertical cross-sectional view of the main part which concerns on a comparative example. It is a perspective view of the whole vertical cross section which concerns on a comparative example. It is a graph which shows the result of the test example by the flow rate. It is a graph which shows the result of a test example by a transmission coefficient. It is a vertical cross-sectional view of the part of the ejection hole which concerns on Example 2 of this invention. It is a top view of the ejection hole which concerns on Example 3 of this invention.

Hereinafter, embodiments for carrying out the present invention will be specifically described with reference to the drawings.
Here, in the attached drawings, the same members are designated by the same reference numerals, and duplicate description is omitted.
Since the description here is one embodiment of the present invention, the present invention is not limited to the relevant embodiment.

[Example 1]

An example of the hydrogen permeation apparatus according to the present invention is a primary side cylinder 10 which is a supply side of a raw material gas such as a hydrogen-containing gas and a extraction side of hydrogen which is a permeation gas, as shown in FIG. It has a hydrogen permeable metal film 30 made of pure vanadium between it and the secondary cylinder 20.
Palladium silver (Pd-25% Ag) is sputtered on both sides of the hydrogen permeable metal film 30 as a catalyst.

A primary side flange 11 is integrally formed on the tip end side of the primary side cylindrical body 10.
A secondary side flange 21 is integrally formed on the tip end side of the secondary side cylindrical body 20.

Recesses are formed on the inner peripheral surface side of the primary side flange 11 and the secondary side flange 21, respectively.
A copper primary gasket 12 is located in the primary recess.
A copper secondary gasket 22 is located in the secondary recess.
The material of the gasket is not limited to copper, and may be formed of other materials such as stainless steel.

A hydrogen permeable metal film 30 is located between the primary side gasket 12 and the secondary side gasket 22.
The diameter of the hydrogen permeable metal film 30 is slightly larger than the outer diameters of the primary side gasket 12 and the secondary side gasket 22, and the hydrogen permeable metal film 30 is sandwiched between the gaskets to maintain the airtightness. The outer peripheral edge portion is formed so as to slightly protrude from the outer peripheral ends of the primary side gasket 12 and the secondary side gasket 22.
The sandwiching between the primary side gasket 12 and the secondary side gasket 22 is not shown, but by passing bolts through the four through holes formed in the primary side flange 11 and the secondary side flange 21 and tightening them with nuts. It is done.

As shown in FIGS. 1 and 2, a raw material supply pipe 13 forming a raw material gas supply path is arranged inside the primary side cylindrical body 10.
As shown in FIG. 3, a substantially circular opening plate 14 having a circular ejection hole 15 at the center is combined with the tip side of the raw material supply path 13.

As shown in FIGS. 1 and 2, the diameter of the ejection hole 15 is formed to be one-fourth the size of the inner diameter of the raw material supply pipe 13.
In the first embodiment, the raw material supply pipe 13 has an inner diameter of 4.4 mm, and the ejection hole 15 has a hole diameter of 1.1 mm.
The inner diameters of the primary side cylindrical body 10 and the secondary side cylindrical body 20 are 30 mm.

As shown in FIG. 3, the outer periphery of the perforated plate 14 is smaller than the inner diameter of the primary side cylindrical body 10 and has a notched shape forming a raw material gas discharge path 16a and a portion that fits in the recess of the primary side flange 11. It has a connecting edge portion 14a which is.
Although not shown, a part of the connection edge portion 14a is welded to a recess formed in the primary side flange 11.
As shown in FIGS. 1 and 2, the raw material gas discharge path 16a leads to a raw material gas discharge path 16b formed between the primary side cylinder 10 and the raw material supply pipe 13.
As shown in FIG. 2, the raw material gas discharge passage 16b leads to the raw material gas discharge passage 16c by the raw material gas discharge pipe 17 connected to the rear end side of the primary side cylinder 10.

As shown in FIG. 1, in the recess of the secondary side flange 21, a circular metal filter 23 and a circular perforated support plate 24 are arranged in order from the hydrogen permeable metal film 30 side together with the secondary side gasket 22. Has been done.
The perforated support plate 24 is formed with a plurality of permeated gas passage holes 25 for passing hydrogen that has permeated through the hydrogen permeation metal film 30.

As shown in FIGS. 1 and 2, a permeated gas take-out path 26b into which hydrogen that has passed through the permeated gas passing hole 25 flows is formed inside the secondary side cylindrical body 20.
As shown in FIG. 2, a permeated gas take-out pipe 27 having an inner diameter of 4.4 mm is connected to the rear end side of the secondary side cylindrical body 20.

A permeated gas take-out passage 26c is formed inside the permeated gas take-out pipe 27.
The corresponding gas take-out path 26c leads to the permeated gas take-out path 26b.

Next, the operation of the hydrogen permeation device will be described.

As shown in FIGS. 1 to 4, the hydrogen-containing gas is supplied from the raw material supply pipe 13 at an adjusted pressure.
As shown in FIG. 1, the supplied gas does not flow as it is because the flow path is restricted by the perforated plate 14 at the tip of the raw material supply pipe 13, and the gas has a diameter smaller than the inner diameter of the raw material supply pipe 13. When ejecting from the hole 15 toward the hydrogen permeable metal film 30, the flow velocity is increased.

The gas ejected at a high flow velocity hits the vicinity of the central portion of the hydrogen permeable metal film 30, and then flows out to the outer edge side of the hydrogen permeable metal film 30.
At this time, some hydrogen molecules are separated to form hydrogen atoms and enter the hydrogen permeable metal film 30, proceed to the secondary side due to the pressure difference, and finally permeate the hydrogen permeable metal film 30.

As shown in FIGS. 2 and 4, the gas that does not enter the hydrogen permeable metal film 30 on the primary side passes through the raw material gas discharge path 16a formed on the outer peripheral edge of the perforated plate 14, and further, the raw material gas discharge path. 16b, it is discharged through the raw material gas discharge path 16c.

On the secondary side, hydrogen having a theoretical purity of 100% that has permeated the hydrogen permeation metal film 30 passes through the permeation gas passage holes 25 of the metal filter 23 and the perforated support plate 24, as shown in FIG.
As shown in FIGS. 2 and 4, the ultra-high purity hydrogen that has passed through the permeated gas passage hole 25 passes through the permeated gas extraction paths 26b and 26c and is separated and recovered in a container (not shown).

[Comparison example]

As shown in FIGS. 5 and 6, a hydrogen permeation device provided with a supply pipe diameter ejection hole 18 having a hole diameter of 4.4 mm, which is equal to the inner diameter of the raw material supply pipe 13, was prepared.
Since the hydrogen permeation device of the comparative example has the same configuration as the hydrogen permeation device of the above embodiment except for the hole diameter of the supply pipe diameter ejection hole 18, the description thereof will be omitted.

[Comparative test]

The hydrogen permeation device of the above example and the hydrogen permeation device of the comparative example were subjected to a hydrogen permeation test under the same conditions.
Regarding the test results, the flow rate is shown in FIG. 7, and the transmission coefficient is shown in FIG.

Examining the results, it was confirmed that the 1.1 mm hole of the example showed better data than the 4.4 mm hole of the comparative example, and it was confirmed that it was effective to reduce the hole diameter.

[Example 2]

As shown in FIG. 9, the circular ejection hole 15 of the opening plate 14 in the second embodiment is different from the ejection hole 15 of the first embodiment, and is on the supply side of the raw material gas to which the raw material supply pipe 13 is attached. It is formed so as to have a tapered shape from the primary side toward the secondary side, which is the extraction side of the permeated gas.
That is, in the case of the second embodiment, the diameter of the circular ejection hole 15 is formed so as to change in a tapered shape.

In FIG. 9, (A) shows a circular ejection hole 15 having a taper formed so that the diameter gradually decreases from the primary side to the secondary side, and the hole diameter on the primary side is 3 .1 mm, the hole diameter on the secondary side is formed to 1.1 mm.
In FIG. 9, FIG. 9B shows a circular ejection hole 15 having a taper formed so that the diameter gradually increases from the primary side to the secondary side, and the hole diameter on the primary side is 1. The hole diameter on the secondary side is 3.1 mm and is formed to be 3.1 mm.

According to the circular ejection hole 15 according to the second embodiment, since the diameter is formed so as to change in a tapered shape, not only the flow velocity is increased, but also due to turbulence, speed change, etc., after passing through the ejection hole 15. Changes in the air flow are caused in many ways and are more effectively ejected onto the hydrogen permeable metal film 30 (see FIG. 1).
[Example 3]

As shown in FIG. 10, the shape of the ejection hole 15 of the opening plate 14 in the third embodiment is different from the circular ejection hole 15 (see FIG. 3) in the first embodiment, but the opening plate 14 The feature that the size of the ejection hole 15 is smaller than the inner diameter of the raw material supply pipe 13 (see FIGS. 1 to 3) is common to the first embodiment.

In FIG. 10, (A) shows an enlarged portion of the ejection hole 15 having a star-shaped pentagon shape, and is formed so that the entire portion fits within a circle having a diameter of 1.1 mm.
In FIG. 10, (B) shows an enlarged portion of the hexagonal shape of the ejection hole 15, and is formed so that the entire portion fits within a circle having a diameter of 1.1 mm.

According to the polygonal or star-shaped polygonal ejection hole 15 according to the third embodiment, since the shape itself is formed in a shape different from the circular shape, not only the flow velocity is increased, but also due to turbulence, partial speed change, and the like. , The change of the air flow after passing through the ejection hole 15 is caused more polygonally, and is ejected to the hydrogen permeable metal film 30 (see FIG. 1) even more effectively.

10 Primary side cylinder 11 Primary side flange 12 Primary side gasket 13 Raw material supply pipe 14 Opening plate 14a Connection edge 15 Injection hole 16a, 16b, 16c Raw material gas discharge path 17 Raw material gas discharge pipe 18 Supply pipe diameter ejection Hole 20 Secondary side cylinder 21 Secondary side flange 22 Secondary side gasket 23 Metal filter 24 Perforated support plate 25 Permeated gas passage holes 26b, 26c Permeated gas outlet 27 Permeable gas outlet pipe 30 Hydrogen permeable metal film

Claims (3)

A hydrogen permeation device having a hydrogen permeation metal film between the primary side, which is the supply side of the raw material gas, and the secondary side, which is the extraction side of the permeated gas.
On the primary side
The raw material supply pipe that forms the raw material gas supply path,
A raw material gas discharge path that discharges a raw material gas that does not permeate to the secondary side,
It has a perforated plate that engages with the tip side of the raw material supply pipe.
A hydrogen permeation device characterized in that the size of the ejection hole of the perforated plate is smaller than that of the raw material supply pipe. A hydrogen permeation device having a hydrogen permeation metal film between the primary side, which is the supply side of the raw material gas, and the secondary side, which is the extraction side of the permeated gas.
On the primary side
The raw material supply pipe that forms the raw material gas supply path,
A raw material gas discharge path that discharges a raw material gas that does not permeate to the secondary side,
It has a perforated plate that engages with the tip side of the raw material supply pipe.
A hydrogen permeation device characterized in that the diameter of the ejection hole of the perforated plate is smaller than the inner diameter of the raw material supply pipe. The hydrogen permeation device according to claim 1 or 2, wherein the ejection hole of the opening plate has a tapered shape from the primary side to the secondary side.

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