JP2005145786A - Gas flow control structure of oxygen separation apparatus or diaphragm reactor using mixed conductive solid electrolyte - Google Patents

Abstract

<P>PROBLEM TO BE SOLVED: To provide a gas flow control structure capable of solving the problem of efficiency deterioration in the supply of gas to a highly integrated Tammann tube in the field of the oxygen separation or diaphragm reactor technology using a Tammann tube-shaped mixed conductive solid electrolyte. <P>SOLUTION: In the oxygen separation apparatus or the diaphragm reactor apparatus provided at least with a pressure vessel provided with a gas introducing port and a discharge port, the plurality of Tammann tubes having the mixed conductive solid electrolyte at least on one side surface, a manifold plate holding the Tammann tube and having a gas leading port and a box housing the whole of the plurality of Tammann tubes arranged on the manifold plate and having the gas introducing port, the gas flow control structure of the oxygen separation or the diaphragm reactor using the mixed conductive solid electrode is provided with a gas storage chamber for supplying a gas to the plurality of Tammann tubes in the vertical direction from the gas introducing port inside the box and a gas discharge port on a surface opposed to the gas storage chamber in the box. <P>COPYRIGHT: (C)2005,JPO&NCIPI

Description

  The present invention relates to a gas flow control structure in the technical field of an oxygen separation device or a diaphragm reactor using a plurality of Tamman tube (one-end sealed cylindrical tube) -shaped separation tubes or reactor tubes made of a mixed conductive solid electrolyte.

Oxygen separation and membrane reactors using mixed conductive solid electrolytes have been actively researched with the development of materials having high oxide ion conductivity.
Oxygen separation is based on the principle of diffusing the interior of a solid electrolyte in the form of oxide ions using the difference in oxygen partial pressure as the driving force. For example, high-purity oxygen is separated from compressed air in one step. I can do it. In addition, although it is necessary to operate at a high temperature (for example, 850 to 900 ° C) in order to increase the diffusion rate of oxide ions, PSA using the adsorption phenomenon by increasing the energy utilization rate by combining heat recovery and pressure recovery Compared with the cryogenic separation method using the difference in the vapor pressure characteristics (boiling point), it is expected that the unit energy consumption of oxygen can be lowered. This is one of the reasons why research for practical application in recent years is vigorous.

  On the other hand, with respect to the diaphragm reactor, when a solid electrolyte is used as a diaphragm, for example, when methane gas and air are introduced, oxygen diffuses from the air side to the methane gas side on the same principle as oxygen separation, and the catalyst disposed on the solid electrolyte surface on the methane gas side Methane is partially oxidized to obtain a mixed gas (synthesis gas) of hydrogen and carbon monoxide. There is great expectation for technological development because hydrogen, which is a raw material for polymer electrolyte fuel cells, can be extracted from natural gas (mainly methane gas). Further, since the synthesis gas can be converted into various hydrocarbon compounds by Fischer-Tropsch synthesis (FT synthesis), it becomes possible to transport from the natural gas field not in gas but in liquid, resulting in cost merit.

  Despite this background, it is said that it will still take a considerable amount of time to put it into practical use. It is a very hurdle to realize a high temperature seal technology that maximizes the integration of the membrane area through which oxide ions permeate within a certain space and that completely separates two different gases. Because.

  Among these, the other technical problem of how to control the gas flow is related to the former technical problem. This is because when the gas is supplied to the highly integrated ion permeable membrane, the gas flow greatly affects the permeation performance. Techniques related to conventional gas flow control methods can be found in the field of fuel cells using the ion permeation phenomenon of solid electrolytes.

  In the case of a flat fuel cell, it is common to provide a plurality of gas flow passages in one stack. (Patent Document 1). In each of Patent Documents 2, fuel gas and air (oxidizing gas) passages are provided in a module for a fuel cell to improve efficiency and improve reliability. However, there is no disclosure regarding overall gas flow control when a plurality of modules are integrated.

  In the case of a Tamman tube type fuel cell, for example, Patent Document 3 discloses a gas flow control method in which a plurality of supply holes are provided in a gas supply tube for one Tamman tube. There is no disclosure regarding overall gas flow control when a plurality of Tamman tubes are integrated.

  Patent Document 4, Patent Document 5 and Patent Document 6 disclose technical disclosure using a plurality of Tamman tubes, but none of them disclose a gas flow control method, and the gas flow is parallel to the Tamman tube. It has become.

  In order for the gas flow control method to be effective in improving efficiency, it is important to consider the influence of the gas flow on the permeation performance. Taking oxygen separation as an example, it is as follows. When supplying an oxygen-containing gas (for example, air) to a forested Tamman tube, oxygen is selectively deprived from the oxygen-containing gas, so that the oxygen concentration changes depending on the location. The transmission efficiency is greatly reduced. If a stagnant region occurs in the gas flow on the oxygen supply side, a driving force sufficient to transmit oxide ions cannot be obtained in that region. Further, when a part of the oxygen-containing gas flows in a region outside the oxygen separation region, oxygen cannot be recovered from the oxygen-containing gas at all, and the efficiency is greatly impaired. In the prior art, there has been no attempt to control the gas flow from such a viewpoint.

JP-A-6-1888008 JP 2002-208417 A Japanese Patent Laid-Open No. 5-94830 JP 7-29590 A JP 2001-43887 JP 2001-273915 A

  The above-mentioned problems have not been so obvious until now. This is because a fuel cell using a solid electrolyte has not yet matured in terms of integration. Furthermore, with regard to oxygen separation and membrane reactors, the technology for integrating the Tammann tube type has just begun. In fact, the present inventors made the shape of the mixed conductive solid electrolyte into a Tamman tube type, and used it as a large number to act as an oxygen separation or a membrane reactor, and compared it with the value expected from the measurement with a single tube. Only a much lower efficiency could be measured, and this led to the recognition of the importance of gas flow control for the first time.

  The present invention solves the problem of efficiency reduction when supplying gas to a highly integrated Tamman tube in the field of oxygen separation using a mixed conductive solid electrolyte in the form of a Tamman tube or diaphragm reactor. An object of the present invention is to increase oxygen separation efficiency and reactor yield by providing a gas flow control structure.

The inventors of the present invention have completed the present invention by constructing a simulator for gas flow and oxygen absorption, and conducting studies for improving efficiency, while simultaneously finding out the effect by experiments.
That is, in order to achieve the above object, the present invention provides a gas flow control structure for an oxygen separation or diaphragm reactor using a mixed conductive solid electrolyte, a pressure vessel having a gas inlet and a discharge port, A plurality of Tamman tubes having a porous solid electrolyte on at least one surface, a manifold plate holding the Tamman tube and having a gas outlet, and containing all of the plurality of Tamman tubes installed on the manifold plate, In an oxygen separation apparatus or a diaphragm reactor apparatus having at least a box having an inlet, a gas storage chamber for supplying gas in the box from the gas inlet to the plurality of Tamman tubes in the vertical direction; A gas discharge port is provided on the opposing surface of the gas storage chamber of the box.

  At this time, a structure in which gas is introduced from the gas storage chamber into the box through a porous plate, or a structure in which the discharge port installed in the box is a porous plate is desirable. More preferably, the perforated plate is provided on the entire surface of one surface of the box.

  Further, the plurality of Tamman tubes are arranged in a plurality of Tamman tube rows, and more preferably, the Tamman tube row is arranged in a gas flow structure arranged in a direction perpendicular to the gas flow. At this time, the Tamman tube arranged perpendicularly to the gas flow is in a position satisfying the relationship of 3.0> d / r> 1.2, where d is the Tamman tube interval and r is the outer diameter of the Tamman tube. It is desirable to be placed.

Further, the Tamman tubes arranged in the direction perpendicular to the gas flow are arranged such that each Tamman tube is arranged at a position where the center of the Tamman tube in the next row and the center of the Tamman tube in the previous row are not parallel to the gas flow. desirable.
Further, it is most desirable that the Tamman tubes aligned in the direction perpendicular to the gas flow are arranged so that each Tamman tube is arranged at a position behind the center of the two Tamman tubes arranged in the front row. In addition, the Tamman tube rows aligned in the direction perpendicular to the gas flow are expressed as 2d>D> 0.5r, where D is the Tamman tube row interval, d is the Tamman tube interval, and r is the Tamman tube outer diameter. It is preferable to be arranged at a position satisfying this relationship.

Furthermore, a structure in which a plurality of protrusions are provided on the surface of the box where the perforated plate is not provided is more desirable in terms of the gas flow structure. Furthermore, it is a more desirable structure that the protrusion is a plate-like body. At this time, it is most desirable that the plate-like body is installed on the wall surface of the box where the perforated plate is not provided in a direction that is not parallel to the gas flow and parallel to the Tamman tube. .
Similarly, a structure in which the plate-like body is installed on the ceiling surface of the box in a direction non-parallel to the gas flow is also most desirable.

  According to the present invention, the gas supplied from the gas inlet provided in the pressure vessel is once stored in the storage chamber provided in the box, and then supplied vertically and uniformly to the plurality of Tamman tubes. As a result, gas efficiently flows between the plurality of Tamman tubes. Thereby, the gas flow efficiency is improved, and the oxygen separation efficiency and the reactor yield can be dramatically increased.

  First, as a best mode for carrying out the present invention, specific examples are shown in FIGS. Fig. 1 shows the structure of an example of a separation furnace of an oxygen separation device. However, even in a diaphragm reactor, the gas introduction pipe is inserted into the inside of the Tamman pipe, and there are significant differences in the structural features. There is no. In FIG. 1, a pressure vessel 1 having a gas inlet 5 and a gas outlet 12, a plurality of Tamman tubes 10 made of a mixed conductive solid electrolyte, a manifold plate 11 for holding it, and a manifold plate Fig. 2 shows an overall view of a separation furnace composed of a box 6 (hereinafter referred to as a rectifying box) that houses all of the plurality of Tamman tubes, and in Fig. 2, gas is introduced vertically from the gas inlet to the Tamman tube group. A gas storage chamber 7 having a perforated plate 8 disposed inside the box so that it can be supplied is provided, and a side wall of the box facing the perforated plate has a structure of a rectifying box provided with a perforated plate 9 for discharging gas. Show.

  The gas supplied from the gas inlet 5 provided in the pressure vessel 1 is stored in the gas storage chamber 7 and then supplied perpendicularly to the Tamman tube through the outer perforated plate 8. The gas flow passes through the perforated plate 9 provided in the opposite direction while colliding with the Tamman tube, and is finally discharged from the discharge port 12 provided in the pressure vessel.

  The gas flow efficiency differs greatly between the case where the gas is supplied vertically and uniformly to the Tamman tube as in the present invention and the case where the gas is supplied in parallel to the Tamman tube, and especially as the gas flow rate increases. The difference is noticeable.

  When the oxygen-containing gas is supplied in parallel to the Tamman tube, oxygen selectively permeates from a limited region flowing in the vicinity of the Tamman tube. Although oxygen is supplied to the vicinity of the Tamman tube by diffusion from a distance from the Tamman tube, this region becomes an oxygen-poor region as a result of the limited amount, and in other regions It will be discharged without contributing to permeation. This situation becomes more noticeable as the gas flow becomes faster. On the other hand, this situation does not occur with vertical supply.

  The number of through holes and the hole diameter provided in the porous plate 8 are determined in consideration of pressure loss when passing through the porous plate. For example, if the pressure loss is too small, the gas is preferentially supplied from the hole close to the gas introduction port 14, and the gas flow rate varies depending on the location of the hole. On the other hand, if the pressure loss is too large, the gas flow non-uniformity depending on the location is eliminated, but the pressure is increased beyond the actual pressure, leading to energy loss.

  Since the pressure loss varies greatly depending on the amount of gas passing through the perforated plate per unit time, it is necessary to first determine the gas supply rate in advance. After that, a simulation on pressure loss and flow uniformity is performed to obtain knowledge that uniformity can be secured with a pressure loss of a certain value or more. Thereafter, the position and number of through holes provided in the perforated plate are determined. For example, (m × n) through holes are provided at positions regularly arranged in m rows and n columns. Although it is desirable that the interval between the through holes in one row is set so as to match the interval between the Tamman tubes, the interval is not necessarily required unless the interval is larger than the interval between the Tamman tubes. Moreover, it is desirable to provide the interval between the through holes in one row within a range of 5 to 50 mm, for example. Finally, the hole diameter of the through hole is determined so as to be a target pressure loss. Although the hole diameter varies depending on the number of holes, for example, it is desirable to provide in the range of 1 to 10 mmφ.

  The number of through holes provided in the porous plate 9 and the hole diameter are determined based on the same concept as the porous plate 8. If the pressure loss when passing through the perforated plate is too small, the gas is preferentially discharged from the hole close to the discharge port 12 and the gas flow uniformity is lost. This is because the uniformity is eliminated, but it leads to energy loss.

Next, an embodiment of the present invention relating to the arrangement of the Tamman tube will be described.
The arrangement of the Tamman tubes is made such that a plurality of Tamman tubes are arranged in a plurality of Tamman tube rows. It is desirable to arrange the Tamman tube row in a direction perpendicular to the gas flow. Further, the center of the Tamman tube in the next row and the center of the Tamman tube in the previous row are arranged so as not to be parallel to the gas flow (hereinafter referred to as a staggered arrangement). When each Tamman tube is placed in a position where the center of the Tamman tube in the next row and the center of the Tamman tube in the front row are parallel to the gas flow (hereinafter referred to as series arrangement), This is because the gas flow (invalid gas flow) that passes between the Tamman tubes without interaction is generated to the extent that it cannot be ignored.

  In order to suppress the ineffective gas flow most effectively, each Tamman tube is arranged at a position behind the center of the two Tamman tubes arranged in the front row. (Denoted as a staggered arrangement). By adopting a regular zigzag arrangement, the entire gas flow is supplied to all Tamman pipes in a balanced manner, and the amount of ineffective gas flow is minimized.

  An example of the best mode regarding the arrangement of the Tamman tube is shown in FIG. FIG. 3 shows a bird's-eye view of a plurality of Tamman tubes made of mixed conductive solid electrolyte.All Tamman tubes 10 stand perpendicular to the gas flow direction 15 and are in the front row. Are arranged so that the next row of Tamman tubes comes behind the center of the two Tamman tubes. In order to make this arrangement easy to understand, FIG. 4 shows a view of the Tamman tube viewed from above.

  As shown in FIG. 4, if the distance between the Tamman tubes is d, the outer diameter of the Tamman tubes is r, and the distance between the Tamman tube rows is D, the relationship between the sizes greatly affects the efficiency of the gas flow. Further, this relationship is related to the gas flow velocity, and there is an optimum value for each flow velocity.

  First, the relationship between d and r is preferably in the range of 3.0> d / r> 1.2. When the d / r value is 3.0 or more, even if the Tamman pipes are arranged as in the present invention, the interval between the Tamman pipes is too large and the invalid gas flow cannot be ignored, and the d / r value is 1.2 or less. This is because a large resistance is required for gas to pass between the Tamman tubes, and a smooth flow cannot be achieved in the rear row. Incidentally, Tamman tubes contact each other at d / r = 1, and the gas flow is completely inhibited.

  The relationship between D and r is preferably in the range of 2d> D> 0.5r. This is because odd-numbered columns or even-numbered columns interfere with each other when D is 0.5r or less, and cannot be physically arranged. When D is 2d or more, the original integration cannot be achieved. It is.

  As described above, the reactive gas flow passing between the plurality of Tamman tubes can be minimized by improving the arrangement of the Tamman tubes. On the other hand, the reactive gas flow that flows in the vicinity of the Tamman tube arranged at the extreme end, specifically between the Tamman tube located at the extreme end and the wall of the rectifying box, can be improved by improving the arrangement method. Absent. Also, the reactive gas flow that flows between the top of the Tamman tube and the ceiling of the rectifying box cannot be improved by improving the arrangement method.

  In order to improve these, it is effective to provide a plurality of protrusions on the surface of the rectifying box where the perforated plate is not provided. In particular, it is the simplest method to provide a plate-like protrusion. At least two or more projections of the plate-like body are arranged in parallel to the gas flow and parallel to the Tamman tube in the gap between the side wall of the rectification box where the porous plate is not provided and the Tamman tube group. Is desirable. In addition, the effect of the reactive gas flow that flows between the top of the Tamman tube and the ceiling of the rectifying box can be reduced by matching the ceiling height of the rectifying box according to the height of the Tamman tube. If the tube heights are slightly different, it is also effective to install a plate-like protrusion between the rectifying box ceiling and the top of the Tamman tube in a direction that is not parallel to the gas flow. .

  FIG. 5 shows an example in which a plate-like protrusion 16 is added to FIG. 2, and four protrusions are provided on each side wall. For ease of viewing, only one tamman tube is drawn in FIG. 5, but naturally a plurality of tamman tubes are erected.

FIG. 6 is a top view of FIG. 5 (in the case of a plurality of Tamman tubes).
Protrusions provided on the side walls of the rectification box are for effective use of gas that does not reach the reaction region because it flows in a laminar flow along the side walls, but is also effective for improving workability at the same time. Works. In other words, if the gas that escapes as a laminar flow along the side wall is minimized, the gap between the Tamman tube group and the side wall becomes extremely small, but this makes the setting method very difficult. is there. In the method of providing the protrusions, such difficulty is reduced if the protrusions are set after setting the rectification box having a margin for the plurality of Tamman tubes.

  Various variations can be considered for the number and shape of protrusions on the plate-like body. An example is shown in FIG. Although (a) is the same as that illustrated in FIG. 6, for example, (b) to (d) are also conceivable. In each example, only the vicinity of the protrusion is illustrated, and the whole can be expressed by repetition and repetition of what is illustrated. Also, the shape of the projections of the plate-like body provided on the ceiling of the rectifying box can be variously changed as in FIG. An example is shown in FIG.

Hereinafter, the present invention will be described with reference to examples and comparative examples.
(Example 1)
-Study on gas flow rate and perforated plate pressure loss-
With the shape shown in Fig. 9, the air flow rate is set to 10,100,500 Nm ³ / Hr (volume per hour, N is converted to the standard state of gas (0.1 MPa, 25 ° C)), and perforated plate The uniformity of the flow rate passing through was examined. The analysis model used the symmetry of the internal structure of the rectification box, and targeted the actual half area. The number of analysis lattices was X = 160, Y = 65, Z = 40 (total 416000), and the individual through holes and plate thickness of the porous plate were not modeled as shapes. The analysis tool used was a structured grid thermal fluid analysis code “STREAM Ver.3.11” from Software Cradle. The analysis conditions and analysis results are summarized in the following tables (Tables 1 and 2).

Table, for example, in a flow rate of 100 Nm ³ / Hr about the perforated plate pressure drop 500 Pa, the flow rate of 10 Nm ³ / Hr was found that may be used perforated plate of about 5 Pa. Although not shown in the table, it was also found that in each experiment, the passage flow velocity tends to increase at the upper part of the perforated plate, and the nonuniformity due to this tendency becomes stronger as the flow rate increases.

In this simulation, the individual through-holes and plate thickness of the perforated plate were not modeled as shapes, so we assumed the hypothetical that the perforated plate had infinitely many through-holes with infinitely small hole diameters. Actually, for example, 15 rows x 11 columns (165 total) with through holes with a hole diameter of about ³ mmφ at the flow rate of 100 Nm ³ / Hr, the rectification shown in FIG. It was found that it could be used on the entire surface of the perforated plate of the box.

(Example 2)
When gas was supplied from a gas storage chamber to a plurality of Tamman tubes in the vertical direction, the gas supply method was changed and an oxygen separation experiment was actually performed. In the experiment, 53 oxygen separation tubes with an outer diameter of 18 mm and an average length of 20 cm were arranged in a staggered manner in 11 odd rows, 10 even rows, and 5 rows in total, separating oxygen from 1.0 MPa air at 850 ° C. I went under the conditions to do. In both experiments, the pressure loss was set to about 500 Pa on both the introduction side and the discharge side. The air flow rate was 100 Nm3 / Hr. Further, the separation tube interval d was 34 mm, and no protrusions were provided in the rectification box. The results are summarized in Table 3.

  As can be seen from the table, a structure in which gas is introduced from the gas storage chamber into the box through the perforated plate or a structure in which the discharge port installed in the box is a perforated plate is desirable, and the structure in which both are perforated plates is the most. desirable.

(Example 3)
-Examination of Tamman tube arrangement method-
In the gas flow control structure of the present invention, the arrangement of the Tamman tubes was set to the series arrangement and the normal zigzag arrangement, and the gas flow was compared by the difference in arrangement method. The analysis tool was FLUENT's thermal fluid general-purpose analysis code "FLUENT Ver.5.5", and the analysis was performed using a two-dimensional analysis grid. As in Example 1, since a large number of lattice points are required, the individual through holes and plate thickness of the perforated plate were not modeled as shapes. The analysis conditions are summarized in Table 4. Assuming an air temperature of 850 ° C and a pressure of 1.0 MPa, an air density of 3.143 kg / m ³ , an air viscosity of 46.464 × 10 ^-6 Pas (Pascal second) was used, and gas disappearance due to oxygen permeation was not considered. .

  The analysis results are shown in FIGS. 10 and 11 show the gas flow velocity in contour lines. In both results, a low-velocity region appears behind the Tamman tube, but in the case of the series arrangement, that region extends to the front of the next Tamman tube, whereas in the case of the regular zigzag arrangement, There was no such situation, and it turned out that it was clearly an efficient flow.

(Example 4)
Using the same method as in Example 3, the effect of the projection of the plate-like body illustrated in FIG. 7 was simulated. As a comparison, a study was also made on the absence of protrusions. The analysis conditions are summarized in Table 5. As common conditions, the air temperature was 900 ° C., the air flow rate was 100 Nm ³ / Hr, and the Tamman tube arrangement was a staggered arrangement.

The results are summarized in Fig. 12, paying attention to the flow velocity of the air hitting the surface of the Tamman tube arranged in a zigzag pattern. In FIG. 12, the horizontal axis represents the position of the Tamman tube row (1 is the most upstream, 16 is the most downstream), and the vertical axis is the average value of the flow velocity of the air hitting the surface of the Tamman tube in that row. In Experiment No. 10 without protrusions, the average flow velocity gradually decreases as going downstream, whereas in other cases where protrusions are provided, the average flow velocity is almost constant except for the first row, and It turns out to keep a high level. This indicates that the gas is efficiently supplied to the Tamman tube by providing the protrusions.
(Example 5)
In the gas flow control structure of the present invention, 53 oxygen separation tubes having an outer diameter of Tamman tube of 18 mm and an average length of 20 cm are arranged in a staggered manner in 11 odd rows, 10 even rows, and 5 rows in total, and 1.0 at 850 ° C. Experiments were conducted to separate oxygen from MPa air. The used porous plate is provided with through holes having a hole diameter of 3.0 mmφ and a number of holes of 165 (15 rows × 11 columns). The distance d between the separation tubes was 34 mm. Table 6 shows the results of providing protrusions on the ceiling and side walls, Table 7 shows the results with protrusions only on the side walls, and Table 8 shows the results without protrusions. The shape of the protrusion on the side wall is shown in FIG. 7 (a), and the shape of the protrusion on the ceiling is shown in FIG. 8 (a).

  When Tables 6 to 8 were compared, it was found that the oxygen separation efficiency was clearly improved when the protrusions were provided.

(Example 6)
With the gas flow control structure of the present invention, experiments were conducted to separate oxygen from 1.0 MPa air at 850 ° C. under various conditions. The air flow rate was 100 Nm ³ / Hr in all cases. The results are summarized in Table 9. Comparing the experiments of No. 27, No. 28, and 29, No. 27 whose d / r ratio is within the desirable range of the present invention has a higher transmission rate. In the experiment on the shape of the protrusion, all the shapes exemplified in the present invention showed a high transmission rate (No. 27, 30 to 32). It was also found that the decrease in average transmission rate was not so noticeable even when the number of Tamman tubes was increased (No. 33). In the case of the arrangement arranged in series with respect to the normal zigzag arrangement, the transmission rate was lowered to some extent even when any projection was used, and it was confirmed that the normal zigzag arrangement was more desirable (No. 34 to 37).

(Comparative example)
An experiment was conducted in which oxygen was separated from 1.0 MPa air at 850 ° C. in accordance with Example 5 with no gas storage chamber provided in the rectifying box. Further, no protrusion was provided. The experimental results are summarized in Table 10.

  As can be seen from Table 10, in the state where no gas storage chamber was provided in the rectifying box, the gas flow control was insufficient, and the permeation rate was extremely reduced.

It is an illustration figure of the desirable structure of the separation furnace in an oxygen separator. It is the schematic of the rectification | straightening box structure of this invention which accommodates a some Tammann pipe | tube. It is a bird's-eye view of a mode that a plurality of Tamman tubes which consist of mixed conductive solid electrolytes are arranged in a regular staggered manner. FIG. 4 is a diagram when FIG. 3 is viewed from above. FIG. 2 is a diagram in which protrusions of a plate-like body are additionally described on the wall surface of the rectification box. FIG. 6 is a diagram when FIG. 5 is viewed from above. It is the figure (figure seen from the upper part of a rectification box) which showed the specific example regarding the shape of the projection of the plate-shaped object provided in a rectification box wall surface. It is the figure (figure seen from the horizontal direction of a rectification box) which showed the specific example regarding the shape of the projection of the plate-shaped object provided in a rectification box ceiling. It is a figure which shows the magnitude | size of the rectification | straightening box assumed when simulating the uniformity of the flow rate which passes a perforated plate. It is the figure which put together the result of the gas flow analysis at the time of supplying gas to the several Tamman pipe arranged in series. It is the figure which put together the result of the gas flow analysis at the time of supplying gas to the several Tamman pipe arrange | positioned in a zigzag pattern. It is a figure which shows the row | line | column average value of the Tamman tube surface average flow velocity arrange | positioned in the zigzag pattern in each protrusion shape.

Explanation of symbols

DESCRIPTION OF SYMBOLS 1 Pressure vessel 2 Insulation wall 3 Pressure vessel flange 4 Fastening means (bolt & nut)
5 Gas inlet 6 Rectification box 7 Gas storage chamber 8 Perforated plate (supply side)
9 Perforated plate (discharge side)
DESCRIPTION OF SYMBOLS 10 Tamman pipe 11 Manifold plate 12 Exhaust port 13 Separation oxygen exhaust port 14 Service port for gas introduction 15 Gas flow 16 Protrusion A Area | region where gas flow rate is large B Area | region in gas flow velocity area C Gas flow velocity area | region small

Claims (14)

A pressure vessel having a gas inlet and a gas outlet; a plurality of Tamman tubes having a mixed conductive solid electrolyte on at least one surface; a manifold plate holding the Tamman tubes and having a gas outlet; and the manifold plate In the oxygen separation device or the membrane reactor device that contains all of the plurality of Tamman tubes installed on the top and has at least a box having a gas inlet,
A gas storage chamber for supplying gas in a direction perpendicular to the plurality of Tamman tubes from the gas inlet in the box, and a gas discharge port is provided on the opposing surface of the gas storage chamber of the box. A gas flow control structure of an oxygen separator or a diaphragm reactor using a mixed conductive solid electrolyte.   The gas flow control structure according to claim 1, wherein gas is introduced from the gas storage chamber into the box through a perforated plate.   The gas flow control structure according to claim 1, wherein the gas discharge port installed in the box is a perforated plate.   The gas flow control structure according to claim 2 or 3, wherein the perforated plate is provided on the entire surface of one surface of the box.   The gas flow control structure according to claim 1, wherein the plurality of Tamman tubes are arranged in the plurality of Tamman tube rows.   6. The gas flow control structure according to claim 5, wherein the Tamman tube row is disposed in a direction perpendicular to the gas flow.   The Tamman tube arranged in the direction perpendicular to the gas flow is arranged at a position satisfying a relationship of 3.0> d / r> 1.2, where d is the distance between the Tamman tubes and r is the outer diameter of the Tamman tube. The gas flow control structure according to claim 6, wherein the gas flow control structure is provided.   The Tamman tubes aligned in the direction perpendicular to the gas flow are characterized in that each Tamman tube is disposed at a position where the center of the Tamman tube in the next row and the center of the Tamman tube in the previous row are not parallel to the gas flow. The gas flow control structure according to claim 7.   9. The gas flow according to claim 8, wherein the Tamman tubes arranged in a direction perpendicular to the gas flow are disposed at positions behind the center of the two Tamman tubes arranged in the front row. Control structure.   When the Tamman tube row aligned in the direction perpendicular to the gas flow has a distance of the Tamman tube row as D, a space between the Tamman tubes as d, and a diameter of the Tamman tube as r, 2d> D> 0.5r The gas flow control structure according to any one of claims 6 to 9, wherein the gas flow control structure is arranged at a position satisfying the relationship.   The gas flow control structure according to claim 4, wherein a plurality of protrusions are provided on a surface of the box on which the perforated plate is not provided.   The gas flow control structure according to claim 11, wherein the protrusion is a plate-like body.   The plate-like body is installed on a wall surface of the box where a perforated plate is not provided in a direction that is non-parallel to the gas flow and parallel to the Tamman tube. Item 13. A gas flow control structure according to Item 12. The gas flow control structure according to claim 12, wherein the plate-like body is installed on the ceiling surface of the box in a direction that is not parallel to the gas flow.

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