CN1019454B - The film unit and the film device that from hydrogeneous gaseous mixture, separate special pure hydrogen - Google Patents
The film unit and the film device that from hydrogeneous gaseous mixture, separate special pure hydrogenInfo
- Publication number
- CN1019454B CN1019454B CN 88107278 CN88107278A CN1019454B CN 1019454 B CN1019454 B CN 1019454B CN 88107278 CN88107278 CN 88107278 CN 88107278 A CN88107278 A CN 88107278A CN 1019454 B CN1019454 B CN 1019454B
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- CN
- China
- Prior art keywords
- film unit
- film
- cylinder
- fairlead
- pipe
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Abstract
The film unit (1) that separates special pure hydrogen has hydrogen-permeable membrane (2), fairlead (4), ventilation liner plate.It is middle near one of them end limit (3) that the part of fairlead (4) is placed in film (2), in fact, is to surround from the outside on whole length of ventilation liner plate and by liner plate, constitutes the thick section from pipe (4) at a segment distance.
Film device has the cylinder (9) of tube grid (14), and is mounted with the cylinder 15 of perforated wall (16) in its lower section.The gatherer (20) and the film unit (1) that pass its bottom have been installed in cylinder, each film unit with itself away from inside, the end limit (21) of fairlead (4) towards cylinder 15.
Description
The present invention relates to separate from hydrogeneous gaseous mixture the film unit and the film device of special pure hydrogen, it is with selecting the method for diffusion to carry out by the hydrogen of metal (palladium) film.It can be used for metallurgical industry, for example, will heat-treat in the pure hydrogen medium of spy when preparing the steel material by high-alloy steel, also can be used for chemical industry, mechanical industry, food industry and electronics industry.
The equipment (US.A.3779711) of the special pure hydrogen of separation known is tubular-shaped structures, wherein uses by the made seamless capillary of palladium-base alloy as film unit.
Equipment has shell, has the air inlet pipe of supplying with hydrogeneous gaseous mixture, in order to blast pipe that discharges special pure hydrogen and the blast pipe that discharges useless current stabilization gas.The inner chamber of equipment is divided into high pressure and two chambers of low pressure with the pipe grid, bunchy is installed wherein and the seamless capillary that is placed in the hyperbaric chamber is fixed with the end of itself.
Enter high pressure (～10-15MPa) all compositions of hydrogeneous gaseous mixture of chamber are adsorbed on the outer surface of each film unit (pipe), at this moment, on palldium alloy, have only hydrogen molecule to resolve into atom, lose electronics, be dissolved in the solid kind plate and under the effect of concentration gradient by the outer surface of pipe to diffusion inside, the process of combination and desorb takes place at this.
The special pure hydrogen that obtains like this enters low-pressure chamber along pipe, delivers the user then.
In this equipment, because pipe close packing bunchy, it is very complicated changing a pipe that loses sealing.Therefore, must or weld damaged pipe down, perhaps change whole whole tube bank, like this, can cause reducing widely the productivity ratio of entire equipment certainly.As a rule, such film unit will damage by 2-3 thermal cycle.Fixedly the binding site of light-wall pipe will stand very big stress in operating process (high pressure-temperature) on the steel unit of pipe grid, causes above-mentioned binding site gas leakage, and its reason is that these Mechanical Properties of Materials have very big difference under the condition of transformation temperature.In order to increase the service life of this equipment, the temperature that must limit technology is up to 350～400 ℃, and this also makes its productivity ratio descend.Employed thin-walled palladium tube diameter is little, and therefore the equipment for the assembling high productive capacity needs a large amount of palladium tubes.
The film device (US.A.3367504) that uses penetration theory to prepare distilled water also is known.
Equipment has the cylinder cell, and the indoor hollow gatherer that coaxial device is arranged, the shell of being made by semi-permeable diaphragm are reeled on it twist, and semipermeable membrane by the ventilation lining plate separately.Along the whole width of shell antipriming pipe is housed, links to each other with the device of supplying with the water of wanting purifying.The gatherer of being furnished with shell moves by the film unit principle.
Want the water (for example seawater) of purifying to send into space in the shell, and remove salinity by film by said pipe.The water of having strengthened enters gatherer, gives the user then.
Obtaining under the necessary high pressure-temperature condition of special pure hydrogen, film unit is a poor efficiency.At first, because the seam on the long distance between the material of homogenous quantities loses sealing very soon, the second, to this structure, it is characterized in that high fluid resistance and inefficient " direct current " mass transfer mode, this just can not set up high efficiency equipment and operation reliably.
The hydrogen-permeable membrane (fixing with welding along the limit) made by palladium-base alloy and the delivery pipe of special pure hydrogen are equipped with in the two sides that known film unit (GB.A.1140952) is included in the nickel flat board, and this pipe communicates with space between the film.Film has waved surface.Film unit has high fluid resistance, and the equipment that can not guarantee has the high production rate of producing special pure hydrogen.
Basic task of the present invention is to improve the film unit that separates special pure hydrogen, settle the pipeline and the liner plate of the special pure hydrogen of discharging to make it have low fluid resistance therein like this to guarantee the separation of hydrogen of maximal efficiency under its service condition, and improve the film device of the special pure hydrogen of separation from hydrogeneous gaseous mixture with these film units, these film units be so mutual arrangement guarantee to realize adverse current mass transfer mode, this mode causes improving widely the productivity ratio of equipment.
Task is to solve like this, the film unit that separates special pure hydrogen is provided, and it comprises the hydrogen-permeable membrane of being made by palladium-base alloy that is placed in ventilation liner plate two sides, and this film is fixed along the limit, with the fairlead that is used to discharge hydrogen, it communicates with intermembranous space, wherein, and according to the present invention, the part that fairlead is furnished with perforation is placed between the film, near it on one side, in fact be placed on whole length of ventilation liner plate and surrounded by this liner plate from the outside, constitute the thick section at a segment distance from fairlead.
The film unit that this structure realizes, the first, can realize discharging hydrogen by the film inner surface to fairlead by the shortest distance even from the distal-most end of unit.Second, on the liner plate thick section, the area of cell cross-section (admission passage) increases to twice, this has just reduced the movement velocity of hydrogen on contiguous fairlead section of being separated, these two factors have reduced the fluid resistance of film unit, have guaranteed the maximal efficiency of separation of hydrogen and have caused improving its specific productivity.
Certainly, be damaged under the film unit service condition of high pressure and alternating temperature for preventing film, flat is made in fairlead perforated section end.Preferably, be damaged with prevention film under frequent thermal cycle conditions to flat end dress protecting sheathing.
Simultaneously, also provide by the film device that separates special pure hydrogen in the hydrogeneous gaseous mixture, it comprises the cylinder that has the pipeline of supplying with hydrogeneous gaseous mixture and discharge the pipeline of special pure hydrogen, there are the pipe grid its inside and are placed on the film unit of pipe below the grid, fairlead is fixed in the pipe grid along cylinder longitudinal axis orientation and with its free end in each film unit, communicate with the outlet of hydrogen, according to invention, wherein column body is settled the cylinder with perforated wall below the pipe grid, this perforated wall forms the circular passage with cylinder wall and is used to pass through admixture of gas, in cylinder, be mounted with exhaust-gas mixture gatherer and above-mentioned film unit by its bottom, each film unit with self away from the end limit of fairlead towards cylinder interior.
The equipment that this structure is implemented can be realized adverse current mass transfer mode, and according to the number and the service condition of film unit, this mode can cause increasing the hydrogen productivity ratio of present device to 1000M
3/ hour.
According to the hydrogen concentration in required equipment productivity and the material gas mixture that will process, in tube, preferably film unit to be installed like this, make its fairlead at least along around settle a row, and away from their end limit towards gatherer, this gatherer is to lay by the longitudinal axis of cylinder.Same purpose, one row's film unit is preferably arranged with the chessboard order for another row's film unit, perhaps advise film unit is listed as into several rows, at this moment, in the row of contiguous gatherer, film unit away from the end limit of fairlead towards gatherer, this gatherer is laid by the cylinder longitudinal axis, and whenever the end limit of next row's film unit makes film unit form spiral helicine passage towards the fairlead of last row's adjacent cells.
Under the situation that this film unit is settled, the displacement volume of film device has been set up the mass transfer optimum condition according to the present invention.
Describe film unit and the film device by the special pure hydrogen of separation in the hydrogeneous gaseous mixture of the present invention in detail below by quoted figures the present invention is described, wherein:
The sketch of Fig. 1-film unit of the present invention has part section;
The larger scale map of Fig. 2-Fig. 1 ㄇ-ㄇ section;
The larger scale map of Fig. 3-Fig. 1 mountain-mountain section;
The film device of Fig. 4-special pure hydrogen of separation of the present invention is an equal proportion, and section is arranged;
Fig. 5-Fig. 4 V-V diagrammatic sectional view;
Fig. 6,7-Fig. 4 VI-VI, in VII-VII section, other scheme sketch that the film unit in tube is arranged.
Film unit 1(Fig. 1 of the present invention) comprise the hydrogen-permeable membrane 2 of being made by palladium-base alloy on the two sides that is installed in ventilation liner plate 1a, with being weldingly fixed on the end limit 3 and being used for discharging the fairlead 4 of hydrogen, this pipe communicates with space between the film 2. Porose 5 on part fairlead 4, and pipe placed between the film 2, near an end of film, be actually on the overall length of ventilation liner plate 1a. The perforated portion of fairlead 4 is surrounded from the outside by liner plate 1a and makes from managing 4 at segment distance formation thick section 6(Fig. 2).
Optimum is to assemble like this film unit of the present invention, by inciting somebody to action A film 2 is folded into the stacked film 2 of double method, and places the pipe 4 that surrounds with liner plate 1a at bending part. In this case, film is as long as connect rather than 4 end limits by 3 end side welds. This scheme is shown in Fig. 2.
The fairlead 4 of finishing like this and settling when discharging hydrogen by film 2 inner surfaces to the fairlead 4 that plays collecting action, has guaranteed the shortest route, and it is no more than the width of film unit. In this case, fluid resistance is actually and has reduced, and on the thick section 6 of ventilation liner plate 1a, the cross-sectional area of film unit doubles, can reduce like this movement velocity (in pipe 4 hydrogen stream maximum) of hydrogen to pipe 4 discharging the time, thereby generally speaking reduce the fluid resistance of unit.
Undermined in order to prevent under high pressure thermal cycle of film 2 and when operation, the terminal 7 of the perforated section of pipe 4 makes it into flat and to it protecting sheathing 8 is installed, as shown in Figure 3. Because the ratio of diffusion impedance and dynamic impedance (determining that hydrogen migration is to the intensity of the process of film unit) depends on the thickness of film 2, its thickness suggestion is equal to or less than 0.1 millimeter. The material of pipe 4 and protecting sheathing 8, its coefficient of cubical expansion should be close to the coefficient of corresponding film 2 materials. So just guaranteed the reliability of whole film units.
According to the present invention, comprise cylinder 9(Fig. 4 by the film device that separates special pure hydrogen in the hydrogeneous gaseous mixture), its top cover 10 and bottom 11. Top cover 10 is equipped with the blast pipe 12 of the special pure hydrogen of discharging, and the air supply pipe 13 of supplying with hydrogeneous gaseous mixture is equipped with in bottom 11.
Pipe grid 14 are housed in the chamber of cylinder 9, the cylinder 15 with perforated wall 16 is installed below the pipe grid, the post jamb 17 of this perforated wall 16 and cylinder 9 forms circular passage 18 together, in order to pass through hydrogeneous gaseous mixture. The collector 20 that passes its bottom 19 is housed in cylinder 15, guarantees from the useless gaseous mixture of cylinder 15 dischargings. In the scheme of advising, collector 20 is to install by the longitudinal axis of cylinder 9, and plays simultaneously the blast pipe of the said gaseous mixture of discharging, and it is cylindrical and along cylinder 15 length perforated wall is being arranged. Film unit 1 of the present invention is housed in cylinder 15, each film unit from it away from the inside towards cylinder 15, the end limit 21 of fairlead 4. The direction of the pipe 4 of each film unit 1 is along the longitudinal axis of cylinder 9, and uses transition spool piece (not expressing in Fig. 4) to be fixed in the pipe grid 14 with the free end 22 of itself. End 22 is communicated with blast pipe 12 by the cell 23 that is formed by top cover 10 and pipe grid 14, and pipe 12 is used for discharging special pure hydrogen to the user. The shape of cylinder 9 and collector 20, the width of the latter's assembling and passage 18 all only depends on conveniently to install and be convenient in the best condition liver mass and shifts, simultaneously this dispensable condition. Recommendering folder equipment in a small amount production and when in by gaseous mixture, extracting the little extraction coefficient of special pure hydrogen, wherein the film unit in cylinder 15 1 will be installed like this, make fairlead along being arranged in a row at least 24(Fig. 5 all around), at this moment, away from the end limit 21 of fairlead towards the recipient 20 of pressing cylinder 9 longitudinal axis and settling.
The outer surface of the adjacent membranes unit 1 among one row forms transfer passage 25, has guaranteed that the hydrogeneous gaseous mixture in cylinder 15 moves to collector 20 along its film 2. This scheme is shown in Fig. 4 and sketch 5. For have high production rate with by the equipment that separates special pure hydrogen in the admixture of gas and have big extraction coefficient, recommend other scheme, film unit 1 is listed as into its fairlead 4 of several rows by circumferential arrangement.
At Fig. 6, film unit 1 is listed as into two rows 24,26, and at this moment, row 24 film unit 1 is arranged by the chessboard order another row's 26 film unit 1. Away from the end limit 21 of the unit 1 of fairlead 4 towards the collector 20 of pressing cylinder 9 longitudinal axis and settling.
The outer surface of the adjacent membranes unit 1 among the row of being listed in 24 and the row 26 forms passage 27, has guaranteed that the hydrogeneous gaseous mixture in cylinder 15 does not represent in Fig. 6 along their film 2() to collector 20 motions.
At Fig. 7, recommend film unit 1 is listed as into three rows 24,28,29.Near among the row 24 of gatherer 20, away from the end limit 21 of fairlead 4 towards the gatherer 20 of press the arrangement of cylinder 9 longitudinal axis.The end limit 21 of every next row's 28,29 film unit 1 is towards the pipe 4 of a last row's 24,28 adjacent cells 1, and like this, the film unit 1 formation helical duct 30(predetermined direction of passage 30 is in the drawings represented by the A arrow).
According to the present invention, the film device that comprises film unit 1 in the following manner.
The hydrogeneous gaseous mixture that will be heated to 600～630 ℃ of temperature under 1～1.8MPa pressure infeeds circular passage 18 by air supply pipe 13 towards equipment eminence constant speed.The aperture of the perforated wall 16 by cylinder 15 makes hydrogeneous gaseous mixture along the film 2 of transfer passage 25,27,30 along film unit 1 then, manages 4 directions from it and flows into to gatherer 20.Because select absorption hydrogen by the film 2 that palldium alloy is made, only produce on its surface hydrogen molecule is decomposed into atom.
The atom that loses electronics forwards in the solid solution of film 2 materials (composition of film 2 materials, lattice will be selected to such an extent that can only pass through hydrogen) under the effect of concentration gradient, inwardly (1 volume) diffusion of outer surface by film 2 from the unit, hydrogen atom takes place here be combined into hydrogen molecule again, from the process of film unit 1 volume inner surface parsing.Special pure hydrogen in unit 1 volume enters fairlead 4 and enters in its chamber by the aperture in its wall 5 then, introduces cell 23 then and gives the user by blast pipe 12.After extracting hydrogen partial with film unit 1, the remainder of hydrogeneous gaseous mixture also is sent to the user by the gatherer of installing 20.
Determined as us, on the unit are of selective membrane 2, depend at the tissue of the air-flow of the hydrogeneous gaseous mixture in the transfer passage 25,27,30 and playing hydrogen in the inner chamber of unit 1 of discharge-channel effect by separated hydrogen amount in the gaseous mixture.
Under the fluid resistance of low discharge-channel and along transfer passage 25,27, under the condition of the motor tissue of 30 mixture, use the adverse current hydrogen in the passing away (inner chamber of unit 1), the amounts of hydrogen of extraction is very big.The efficient of adverse current mixture increases along with the minimizing of the hydrogen content in raw mix and comes across to a great extent in the equipment that highly extracts hydrogen.
In our scheme, at transfer passage 25,27, the gaseous mixture in 30 is to gatherer 20 motions, and is in the direction facing to it in mentioned passing away.When film unit 1 is listed as into a few row (Fig. 6,7), the length of said transfer passage 25,27,30 surpasses the length of said passing away, and this influences mass transfer effectively, and equipment can be worked expeditiously when guaranteeing that hydrogen concentration is low in gaseous mixture.
Embodiment:
Technology according to the present invention separates special pure hydrogen in film device is listed as into one with film unit 1 and arranges (as Fig. 4), totally 30 in cylinder 15.The area of each unit 1 is 980cm
2The consumption of hydrogeneous gaseous mixture (75% cracked ammonium) is 250M
3/ hour.Technological temperature is 600 ℃, and pressure is 1.2MPa.Equipment productivity (by hydrogen) is 25M
3/ hour.The commercial plant of special pure hydrogen has 6 such equipment, all connects with public gatherer.
The feature of film unit of the present invention is to have the high-seal reliability under the service condition of the pressure of 600～630 ℃ temperature and 10MPa, and the productivity ratio that guarantees each film unit is at 1-1.8M
3In/hour the scope.
According to the present invention, the feature with film device of unit is a high efficiency, and this is owing to due to the rational mass transfer method tissue, can be made into strong disperser, guarantees that hydrogen purity is not less than 99.9999%.Device structure can be allowed the film unit of realizing changing fast damage.
Claims (8)
1, the film unit that separates special pure hydrogen, has the hydrogen-permeable membrane of settling on the two sides of ventilation liner plate (1a) of making by palladium-base alloy (2), fixing along end limit (3), with the fairlead that is used to discharge hydrogen (4), it communicates with space between the film (2), it is characterized in that the part that fairlead (4) is furnished with perforation is placed between the film (2), near an one end limit (3), be actually on the whole length of ventilation liner plate (1a) and and surround from the outside, constitute the thick section at a segment distance from pipe (4) by liner plate (1a).
2,, it is characterized in that the end (7) of managing (4) perforated section makes flat according to the film unit of claim 1.
3,, it is characterized in that the end (7) of the pipe (4) that flattened is equipped with protecting sheathing (8) according to the film unit of claim 2.
4, arbitrary comprising by the film device that separates special pure hydrogen in the hydrogeneous gaseous mixture according to claim 1-3: have the pipe (13 of supplying with hydrogeneous gaseous mixture and the special pure hydrogen of discharging with film unit (1), 12) in cylinder (9) cylinder pipe grid (14) are arranged, and film unit (1) is installed in its lower section, in each film unit, the direction of fairlead (4) is along the longitudinal axis of cylinder (9), and be fixed in pipe grid (14) with its free end (22), communicate with the pipe (12) of discharging hydrogen, it is characterized in that, in cylinder (9), the cylinder (15) of perforated wall (16) is installed below pipe grid (14), the wall (17) of this perforated wall and cylinder (9) forms circular passage (18), in order to pass through gaseous mixture, and exhaust-gas mixture gatherer (20) and the above-mentioned film unit (1) that passes its bottom (19) be installed in cylinder (15), each film unit with itself away from inside, the end limit (21) of fairlead (4) towards cylinder (15).
5, according to the film device of claim 4, it is characterized in that the film unit (1) in cylinder (15) is to install like this, fairlead (4) is at least along being listed as into a row (24) all around.
6,, it is characterized in that each film unit (1) is to install like this, the gatherer (20) that it is installed towards the longitudinal axis of pressing cylinder (9) away from the end limit (21) of fairlead (4) according to the film device of claim 5.
7, according to claim 5,6 film device is characterized in that film unit is listed as into two rows (24,26), and at this moment, a row (24) film unit (1) is settled with the chessboard order the film unit (1) of another row (26).
8, according to the film device of claim 5, it is characterized in that film unit (1) is listed as into several rows (24,28,29), at this moment at the gatherer of installing towards the longitudinal axis of cylinder (9) near the end limit (21) away from fairlead (4) of film unit (1) among the row (24) of gatherer (20), and every next row (28, the end limit (21) of film unit 29) (1) is towards a last row (24, the pipe (4) of adjacent membranes unit (1) 28), film unit (1) forms spirality channel (30) like this.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN 88107278 CN1019454B (en) | 1988-05-20 | 1988-10-05 | The film unit and the film device that from hydrogeneous gaseous mixture, separate special pure hydrogen |
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| PCT/SU1988/000108 WO1989011328A1 (en) | 1988-05-20 | 1988-05-20 | Membrane element and membrane apparatus for extracting super-pure hydrogen from gaseous hydrogen-containing mixtures |
| CN 88107278 CN1019454B (en) | 1988-05-20 | 1988-10-05 | The film unit and the film device that from hydrogeneous gaseous mixture, separate special pure hydrogen |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1041538A CN1041538A (en) | 1990-04-25 |
| CN1019454B true CN1019454B (en) | 1992-12-16 |
Family
ID=25742498
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN 88107278 Expired CN1019454B (en) | 1988-05-20 | 1988-10-05 | The film unit and the film device that from hydrogeneous gaseous mixture, separate special pure hydrogen |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN1019454B (en) |
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101318110B (en) * | 2002-07-25 | 2011-06-08 | 大日本印刷株式会社 | Thin film support substrate for use in hydrogen production filter and production method of hydrogen production filter |
Families Citing this family (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112708487B (en) * | 2020-12-16 | 2022-02-15 | 山东师范大学 | Rotating membrane separation device and system and method for preparing synthesis gas by converting methane |
-
1988
- 1988-10-05 CN CN 88107278 patent/CN1019454B/en not_active Expired
Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101318110B (en) * | 2002-07-25 | 2011-06-08 | 大日本印刷株式会社 | Thin film support substrate for use in hydrogen production filter and production method of hydrogen production filter |
Also Published As
| Publication number | Publication date |
|---|---|
| CN1041538A (en) | 1990-04-25 |
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