WO2007018444A1

WO2007018444A1 - Hydrogen purification membrane, filtering element and membrane device

Info

Publication number: WO2007018444A1
Application number: PCT/RU2005/000407
Authority: WO
Inventors: Dmitry Ippolitovich Slovetskiy; Evgeny Michailovich Chistov
Original assignee: Dmitry Ippolitovich Slovetskiy; Evgeny Michailovich Chistov
Priority date: 2005-08-09
Filing date: 2005-08-09
Publication date: 2007-02-15
Also published as: WO2007018444A8; RU2416460C2; RU2008108094A

Abstract

The invention relates to pure hydrogen membrane extraction from hydrogen-containing gas mixtures. The aim of said invention is to increase the performance and service life of membranes. The inventive flat sealed filtering element comprises two walls, a separating porous element arranged therebetween and a hydrogen-removing pipe. The walls consist of water permeable membranes made of a palladium alloy and sealingly connected to each other in frames. The wall membrane is shaped in the form of the relief consisting of protrusions and recesses, which are uniformly distributed along the working surface thereof. The ratio between the protrusion length (L) in a normal cross-section and the projection (D) thereof ranges from 1.05 to 1+δ, wherein δ is the membrane material plasticity. The relief makes it possible to increase the strength, reliability, service life and the performance of the membrane due to the modification of the surface area and thickness thereof. The membrane device comprises a body, a set of parallel filtering elements, gas supplying and gas removing elements, which enable an initial mixture to flow from the periphery to the center, a weak mixture to be discharged from the membrane center, prevent the formation of dead zones and make it possible to attain the maximum degree of hydrogen extraction.

Description

HYDROGEN RESISTANT MEMBRANE, FILTERING ELEMENT

AND MEMBRANE APPARATUS

FIELD OF THE INVENTION

The invention relates to the field of membrane extraction of pure hydrogen from gas mixtures containing hydrogen, and can be used in the electronic, micro - and nanoelectronic, chemical, petrochemical, metallurgical industries, the production of pure materials, hydrogen energy and other industries using high-purity hydrogen (> 99.999 %).

State of the art

Analogs of the invention are membranes, membrane elements (ME) and apparatuses described in articles V.Z. Mordkóvish, Yu.K. Waishtosk, M.N. Sospa, Platipum Metals Rev. 36, p.90-97, 1992 [I]; R.Wuhbaum apt H. Lei, J. Rogue Sugs, 2003. - p. 5467 [2]; Tolchinsky A.P., Sorokin VG, Shishkov G.B., Makarov V.M. Production and use of ultrapure hydrogen. - Sverdlovsk, Ural Branch of the Academy of Sciences of the USSR, 1989. P. 93 [3] and patents, for example: R. Vuhbaum US Patents 6,461,408, Ostober 8, 2002; 6,168,650, Japan 2, 2001 [4] Ogawa, US Pat. 5, 782,960, JuIy 21, 1998 [5]; Edlud, US Pat. 6.419, 728; PCT WO 01/70376 [6]; Juda et al. DJ Rattept 5,904, 754, Mau 18, 1999 [7].

To extract high-purity hydrogen, membranes and membrane elements are used in the form of capillary tubes with a diameter of 0.8 to 5 mm and a wall thickness of 80-120 μm [1, 2] from PdAg palladium alloys and Bl-VZ series alloys containing precious alloys other than silver metals, nickel, aluminum and rare-earth elements [l, 2]. In the analogue of [3], membranes and membrane elements (MEs) in the form of flags of the Bl alloy are described. The tight connection of membranes with structural materials (usually with stainless steel of different grades) is ensured by microplasma welding [3], soldering with various solders [4,5], gluing with high-temperature adhesives [6], diffusion welding [7], and the sealing of ME parts by gluing, argon-arc, laser or microplasma welding [3,5]. The extraction of hydrogen from gas mixtures containing from 15 to 99.8% hydrogen is carried out at a temperature of 300-600 ⁰ C and a pressure drop across the membrane from 0.1 to 17 MPa. Membranes and membrane elements are placed in a sealed enclosure, into which a mixture of gases containing hydrogen is supplied through an inlet fitting. It passes over the surface of the membranes through which pure hydrogen diffuses, and the hydrogen-depleted gas mixture is discharged after the extraction of pure hydrogen from the housing. The tubular elements [1, 2, 4] are hermetically sealed on one side, and pure hydrogen is discharged from the other end, for which they are soldered to tubular or flat collectors - the so-called tube boards. In flat membrane elements, membranes are directly welded to each other along the perimeter [3], welded or glued to porous substrates [5, 6] or frames made of structural materials [7]. The disadvantages of the analogues are the high cost of the precious metal - palladium [1, 3], due to the large thickness and low permeability of the membranes, the low yield for the manufacture of MEs [1, 3] and the insufficient life of the MEs and apparatuses, due to their depressurization due to the difference the coefficients of thermal expansion of palladium alloys and structural materials - usually stainless steel, and to a greater extent due to the high coefficients of thermoconcentration expansion of palladium alloys in a hydrogen atmosphere [8- 10].

Closest to the invention are a hydrogen-permeable membrane based on a palladium alloy with a raised outer surface with alternating protrusions and depressions surrounding each protrusion (USSR Patent jN ° 310430 from 07.26.1971 [8]); filter element for the evolution of pure hydrogen (USSR Author's Certificate N ° 1611421 of January 25, 1989 [9]), and the assembly of the filter filter for pure gases - a membrane apparatus (Assemblоf rugas gas рреаmаtпг seраратор, Patent GB 1060451,1967 and US Pat. 3534531 , 10.20.1970 [10]).

In order to increase the strength and performance of known hydrogen-permeable membranes, a relief is formed on their working surface by stamping. Stamping is carried out by pressing using a hydraulic press at room temperature on Dutch woven nets under a pressure of 100-400 kg / cm ² [8] lying on a metal or rubber substrate. The surface relief is obtained in the form of waves arranged in concentric circles with alternating convex and concave sections, with a wave period of 0.08-0.6 mm, convex heights and concave sections from 0.04 to 0.3 mm deep [8], or concentric circular waves with a cross section in the form of a semicircle (h = R), an ellipse and a parabola and a period of 5-10 mm [10], or in the form of radial rays at an angle to the radius from 5 to 30 ° [9].

Due to a slight increase in the true surface area of the membranes due to the relief in [8, 9], only an increase in the strength and stability of the membranes was achieved. When creating a deeper relief with a cross section in the form of a semicircle [10], it was shown that the membrane productivity also increases due to an increase in the true working surface area of the membranes and a decrease in the average thickness due to the stretching of the membrane material. However, our attempts to repeat the results described in [10] were unsuccessful. On the surface of the membranes, hermetically connected to the frames, 50 μm thick of Bl alloy, the composition of which is PdAgI 6% Aul, 7% PtO.7% RuO.7% AY, 15% did not differ much from the PdAg20% Au5% Ru0.5% alloy used in [10], a relief was created by pressing in the form of concentric circles with a cross section in the form of a semicircle (R = h = l, 6 mm). The same relief was created on samples with a thickness of 50 μm from a PdInRu alloy that did not contain silver. All membranes on the samples cracked during the pressing process. The relief on membranes with frames in the form of concentric circles was only possible with a cross section in the form of a circle segment with a height h <R. However, as a result of cyclic heating and cooling of the samples in a mixture of 70% H ₂ + 30% Ag at a pressure of SHPa from 25O ⁰ C up to 600 ⁰ C with a rate of 110 ° C / min on a circular concentric relief of the working surface after 40-70 cycles, radial straight folds were clearly formed on the periphery, clearly visible in the photograph (Fig. 14). In this case, the samples warped and lost their tightness. A theoretical analysis of the result confirmed that the relief in the form of concentric circles is unstable with respect to the thermoconcentration expansion of membranes and frames with very different expansion coefficients. The relief turned out to be more stable in the form of straight corrugations located at angles from 5 to 30 ° to the radius [9], which provided 10 times longer operation compared to smooth Bl alloy membranes withstanding less than 40 cycles.

The disadvantages of the described methods of forming membranes are the small depth of the corrugations [8, 9], uneven coverage of the surface area, the occurrence of an increased stress concentration at the points of convergence of the corrugations to the center, as well as at the edges of the membrane elements near the sealing zones with frames or calipers in which in the end, the appearance of cracks, leading to a loss of tightness, the failure of the filter elements,

. reducing the resource of their work [9] and the instability of the resulting membranes [10]. Flat filter elements are described in the prototypes [9, 10].

A double-sided filter element (FEL) [9] contains two flat disc-shaped palladium alloy membranes, hermetically connected to two ring frames made of stainless steel, representing FEL walls, between which a porous separation element is placed. The frames have mirrored annular corrugations and radial recesses, which, after sealing the two frames around the perimeter, form an annular collector for collection and a round hole for the pipe for removing pure hydrogen, which is hermetically connected to the frames. In this case, the outer edge of the separator is located in the collector, without injuring the membrane during assembly, sealing and operation of the ME. To compensate for the difference in thermal expansion of the membranes and rings, straight corrugations are made on the surface of the membranes at an angle of 5 to 30 degrees to the radial direction. When the FEL is heated to a working temperature of 400 ⁰ C in a vacuum or in an inert gas, the frames having a greater coefficient of thermal expansion than the membranes stretch the membranes, and when the gas mixture contains hydrogen is subsequently expanded, the membranes expand, forming folds, wrinkles due to the large thermoconcentration expansion and other surface irregularities. As the membrane temperature decreases, wrinkles, wrinkles, and other surface irregularities increase even more. The presence of corrugations on the membrane in the absence of communication between the membranes and the porous separator provides damping of tensile and compression stresses of the membranes, partially eliminating warping. As a result, the tightness and operability of the membrane element at a temperature of 500 ⁰ C and a pressure drop across the UMP membranes in a mixture with a 75% hydrogen concentration is maintained for 500 hours, withstanding more than 300 cycles of cooling and heating at variable pressures (thermobarocycles), whereas analogues that do not have corrugations, under the same conditions with membranes of the same alloy, remained airtight and operable for less than 50 hours and withstood less than 40 such cycles. Flat filter elements of several different designs [10] consist of one or two of the above-described hydrogen-permeable membranes in the form of a disk with a relief made by pressing, in the form of annular corrugations with a cross section in the form of a semicircle. The first design is a solid disk, in the middle of which a blind channel is drilled along the radius and a pipe is inserted into it to remove pure hydrogen. Holes (channels for hydrogen removal) perpendicular to its axis were drilled along the length of the channel, communicating with the radial channel, and on both surfaces of the disk there are the flat membranes described above with circular annular corrugations with a cross section in the form of a semicircle, peripherally hermetically connected to the disk so that each corrugation is convex up or down to the surface of the support (disk with channels) above two diametrically opposite holes in the disks. A hydrogen-containing gas mixture is supplied to the surface of the membranes, hydrogen diffuses through the membranes, enters the vertical channels, and through them passes into the radial channel and is discharged through the pipe.

The second design also contains the two flat membranes described above, located on two calipers, having round holes in the center, which are hermetically connected to the calipers along the outer perimeter and to the central rings through which the tubular manifold passes to remove pure hydrogen. A hydrogen-containing gas mixture is supplied to the surface of the membranes, hydrogen diffuses through the membranes and enters through vertical corrugated channels in the calipers through the corrugations, and through them passes into the space between the calipers, connected with the internal cavity of the collector and is discharged through it. The third design also contains the two flat membranes described above, located on two calipers with channels perpendicular to their plane, in communication with the pipes for removing pure hydrogen diffused through the membranes. Calipers are tightly connected to each other friend on the periphery. A hydrogen-containing gas mixture is supplied separately to the surface of each of the membranes through two radially diametrically opposite nozzles, hydrogen diffuses through the membrane into the corrugations and is removed from their volume into radial channels in the caliper, enters the radial channel located inside the caliper and nozzle, and the lean gas mixture is discharged from the periphery of the surface of each membrane separately through two diametrically opposed nozzles, the axis of which is perpendicular to the axis of the supply nozzles similar mixture.

The disadvantages of the above-described membrane elements are the lack of performance and stability due to the above-described disadvantages of the methods of creating a relief on the surface of the membranes, as well as the complexity of the design and the large dimensions and weight due to the design of the calipers.

The main component of the membrane apparatus [10] are filter units, consisting of several of the third type of filter elements described above. Between them are heaters that provide heating of the membranes during the preparation and subsequent operation of the apparatus, thermocouples for temperature control and pressure sensors. A hydrogen-containing gas mixture is supplied separately to each membrane element on the surface of each membrane through two radially diametrically opposed nozzles, hydrogen diffuses through the membranes into the corrugations and is removed from their volume into radial channels in the calipers, and enters the radial channels located inside the calipers and is diverted from each membrane separately through its nozzles, and the lean gas mixture is diverted from the periphery of the surface of each membrane separately through two diametrically opposed falsely located nozzle, the axis of which is perpendicular to the axis of the nozzles for supplying the initial mixture.

A modernized design is also described in which the supply of the initial gas mixture containing hydrogen is supplied to each membrane element through two diametrically arranged nozzles to the surface of one of the membranes, and the gas mixture depleted as a result of hydrogen diffusion through this membrane is supplied to the surface of the second membranes, where part of the hydrogen contained in it as a result of diffusion through it passes into the channels of the second part of the membrane element and is discharged through the second pipe of pure hydrogen, and an additional depleted gas mixture is discharged through two similar pipes of the mixture removal from the periphery of the surface of the second membrane. Thus, in this design, the sequential operation of two membranes of each membrane element is realized.

The disadvantages of the above-described designs of membrane apparatuses include the sum of the above-described disadvantages of hydrogen-permeable membranes and filter elements of the prototypes, supplemented by the complex nature of the flow along the surface of each membrane with the formation of stagnant zones due to the supply of the initial mixture through two diametrically oppositely located nozzles for supplying and discharging the lean mixture through two diametrically oppositely located nozzle on the same surface in the first structure or inlet and outlet and gas mixtures on different surfaces of the membranes - in the second. An additional disadvantage of the second design is associated with an additional decrease in the efficiency of hydrogen extraction due to a decrease in the partial pressure of hydrogen above the surface of the second membrane in each membrane element.

Disclosure of invention

The objective of the invention is to increase the specific productivity and service life of hydrogen-permeable membranes, filter elements and membrane devices, reduce the size of the membrane devices, the weight and specific costs of palladium for the extraction of pure hydrogen from gas mixtures, simplify the assembly and maintenance of filter units during operation and regeneration of palladium from old filter nodes and devices, increasing their maintainability.

The technical result of the invention is to ensure the constancy of the composition, pressure and speed of the feed mixture to the periphery of the surface of all membranes, changes in the radius of the membranes of the velocities and concentrations of all components, including hydrogen, as well as the pressure, composition and flow rate of the lean mixture discharged from the center of the membranes, turbulent vortices in the feed gas stream and accelerate the mixing of the flow, supply and hydrogen removal to and from the membrane surface. In addition, simplifying the connection of the individual parts of the patented elements and the membrane apparatus.

These task and technical result achieved vodor ^{'odopronitsaemoy} membrane based on palladium alloy with an embossed outer surface with alternating ridges and around each protrusion troughs, thus, a palladium alloy contains one or more elements of I, III, IV and VIII of the Periodic Table of the Elements, and the ratio of the length of the arc L on the surface of the protrusions in their cross section to the length of its projection onto the base area D is in the range from 1.05 to 1 + δ, where δ is the ductility of the membrane material.

And also the fact that these protrusions are made with a convex surface. And also the fact that these protrusions are made in the form of a spherical, parabolic or ellipsoidal segment.

And also the fact that these protrusions are evenly spaced on the surface of the membrane.

And also by the fact that these depressions are interconnected. And also because it has a metal frame on the supply side of the gas mixture, hermetically connected to it around the perimeter, the internal size of the frame is smaller, and the external size is larger than the outer size of the membrane. And also the fact that said frame is made of metal with a coefficient of thermal expansion different from the coefficient of thermal expansion of the palladium alloy of which the membrane is made.

And also the fact that the specified frame is made of structural material. And also the fact that it is made in the form of a plate with the shape of a flat figure. And also the fact that the plate is made in the form of a circle, ellipse, square or rectangle.

The indicated problem and technical result are achieved by a filter element comprising two walls with a separating element placed between them, the gas outlet channels of which are in communication with an annular collector for collecting hydrogen and with a discharge pipe. One of the walls is made in the form of a hydrogen-permeable palladium alloy membrane tightly connected to the frame, and the other wall is made in the same form or in the form of a continuous metal substrate, each hydrogen-permeable membrane is made with a relief outer surface with alternating protrusions and depressions surrounding each protrusion, moreover, the palladium alloy contains one or more elements from groups I ⁶ , III, IV, and VIII of the Periodic Table of Elements, and the ratio of the maximum protrusion surface length L is the ratio of the arc length L on the protrusion surface in their cross section to the length of its projection onto the base area D to the maximum length of the base of the protrusion D is in the range from 1.05 to 1+ δ, where δ is the ductility of the membrane material, while the separation gas discharge element t is made porous with the smallest possible hydraulic resistance to pure hydrogen, each membrane is hermetically connected on the supply side of the gas mixture with a frame whose internal size is smaller and the external size is larger than the external size of the membrane or equal to the external size of a solid metal substrate, and the frame between each other or frame and a continuous metal substrate is hermetically connected around the perimeter to form an annular collector for collecting hydrogen. And also the fact that the separating gas outlet element is made in the form of a set of woven grids coated with an inert material, which excludes its welding with membranes in a hydrogen medium, and its linear dimensions are greater than or equal to the linear dimensions of the membrane, but smaller than the linear dimensions of the frame or solid metal substrate . And also the fact that these protrusions of the hydrogen-permeable membrane are made with a convex surface, which faces the supply mixture.

And also the fact that these protrusions of the hydrogen permeable membrane are made in the form of a spherical, parabolic or ellipsoidal segment. And also the fact that these protrusions of the hydrogen-permeable membrane are evenly distributed over the surface of the membrane.

And also by the fact that these troughs of the hydrogen permeable membrane are interconnected.

And also the fact that said frame is made of metal with a coefficient of thermal expansion different from the coefficient of thermal expansion of the palladium alloy from which the membranes are made.

And also the fact that the specified frame is made of structural material. And also the fact that the hydrogen permeable membrane is made in the form of a plate with the shape of a flat figure.

And also the fact that the plate is made in the form of a circle, ellipse, square or rectangle. The aforementioned task and technical result are achieved by a membrane apparatus comprising a housing with one or more filtering elements located therein with gas exhaust and gas supply elements placed on both sides thereof and having an input of the initial gas mixture, hydrogen and ^" lean gas mixture, characterized in that it equipped with collectors for the removal of hydrogen and the exhaust of the lean gas mixture, hermetically connected, respectively, with the leads of hydrogen and the lean gas mixture, each filter element in is filled in the form of the filter element described above, the gas outlet elements are made in the form of gas outlet pipes hermetically connected to the exhaust manifold outlet manifold, the gas supply elements are made in the form of deflectors directing the initial gas mixture along the outer surface of the hydrogen-permeable membrane of the filter elements from their periphery to the center, and the outlet pipes of the peripheral annular collectors for collecting hydrogen of the filter elements are hermetically connected to the collector of the hydrogen outlet. And also the fact that the deflector is made of two identical profiled disks fastened to each other along the periphery and made with a central hole, with protrusions on their outer sides, extending from the periphery to the center, and with protrusions on the inner sides of these disks forming the channel in which the exhaust pipe is placed.

And also the fact that the deflector is made in the form of a flat disk located in the slot of the gas outlet pipe, extending from the center of the hydrogen-permeable membrane and having an inner diameter greater than the thickness of the disk.

And also the fact that the protrusions of the hydrogen permeable membrane of the filter elements are made with a convex surface.

And also by the fact that these troughs of the hydrogen permeable membrane are interconnected. And also the fact that the hydrogen permeable membrane is made in the form of a plate with the shape of a flat figure.

And also the fact that the plates are made in the form of a circle, ellipse, square or rectangle.

And also due to the fact that the permeable hydrogen membrane has a metal frame sealed to it.

And also the fact that the specified frame is made of structural material. And also the fact that the supply of the original gas mixture and the conclusions of hydrogen and depleted gas mixture are made in the form of fittings.

And also the fact that the sealed connections of these outlet pipes with a collector of hydrogen removal are made in the form of threaded connections with ball-cone seals. And also the fact that the sealed connections of these outlet pipes with a collector of hydrogen removal are made in the form of welded joints.

And also by the fact that the filter elements are combined into a module, which is an assembly of elements on the hydrogen removal manifold, made in the form of a segment of a helix covering the specified assembly around the circumference with a rotation of up to 270 degrees.

And also the fact that these outlet pipes of the filter elements combined into a module are hermetically connected to the above collector with rotation around an axis passing through the centers of the membranes perpendicular to their plane, relative to each other by an angle of 10-20 degrees. And also by the fact that the filter elements are combined into one or more of these modules, and their outlet pipes are hermetically connected to a common hydrogen output collector by a threaded ball-cone connection. And also the fact that the filter elements are combined into one or more of these modules, and their outlet pipes are hermetically connected to a common hydrogen output manifold by a welded joint.

The invention is illustrated by the following drawings and drawings. In Fig. 1, a hydrogen permeable membrane (top view) of a PdInRu alloy in the form of a disk with convex protrusions in the form of sphere segments (h <R), located uniformly on the working surface.

Figure 2 is a cross section of the membrane along the line A-A shown in figure 1. In Fig.3 - a hydrogen-permeable membrane made of PdInRu alloy in the form of a disk with convex protrusions in the form of sphere segments (h <R), arranged uniformly along the working surface (Figs. 1-2), hermetically connected to the frame, in section along the line A-A.

Figure 4 is a top view of the filter element in the form of a flat disk. Figure 5 is a section along the line A-A of figure 4. Figure 6 - membrane apparatus.

7 - deflector flow of a hydrogen-containing mixture of gases (view from the side of the membrane).

On Fig - deflector in the form of a disk embedded in the exhaust pipe of the exhaust gas mixture from the center of the filter elements (section, side view).

In Fig.9 is a view along the axis A of the exhaust pipe of the deflector (Fig.8). Figure 10 is a top view of the deflector (Figure 8).

Figure 11 is a view of a module of a filtering assembly, which is an assembly of filtering elements on a pure hydrogen discharge manifold in the form of a segment of a helix covering the assembly around a circle with a rotation of 270 degrees, with the arrangement of the filter elements with a rotation of 20 degrees relative to each other and hermetically connected to the collector by threaded ball-cone connections.

In Fig.12 - filter element (one-sided, the second embodiment is a top view);

In FIG. 13 is a section along line A-A of FIG. 12.

On Fig - photograph of a hydrogen-permeable membrane of alloy Bl with a relief on the surface in the form of circular concentric waves, similar proposed in the patent [10], with a frame, after testing at T = 500 ° C, a pressure of 1 MPa for 6 hours with periodic cycles of lowering temperatures to 35O ⁰ C and rising to 500 ⁰ C for every hour.

In accordance with the invention, a hydrogen permeable membrane 1 (Fig.1-2) made of palladium alloys with one or more elements from groups I ⁶ , III, IV, VI of the Periodic system of elements (e.g. PdCu, PdAg, PdAu, PdY, PdRu, PdInRu, PdCuPb, PdAgAuRu, PdAgAuAlNi and multicomponent alloys of the Bj-B ₄ series containing Pd, Ag, Pt, Au, Al, Ru in different concentrations) has a high selectivity of permeability to hydrogen and its isotopes with respect to all other gases and has a shape, for example , flat disk or any other flat shape (circle, ellipse, square or rectangle), on the working the surface of which by pressing has created a deep relief of protrusions 2 arranged, for example, evenly, on the membrane surface with a convex surface in the form of segments of a sphere (h> R), an ellipsoid or paraboloid, and valleys 3 surrounding each protrusion, which can communicate with each other. The height of the convex sections (protrusions 2) of the relief is selected so that the ratio of the length of the arc L on the surface of the protrusions 2 in their cross section to the length of its projection onto the base area D is within l, 05 <L / D <l + δ, (1 ) where δ is the ductility of the membrane material.

The radius of the sphere can vary from 0.5 to 10 mm, and the distance between the protrusions is the smallest possible. The mechanical properties of some alloys annealed in vacuum are shown in table 1.

An example of a membrane with a surface relief in the form of convex sections in the form of sphere segments (h / r = 0.5) is shown in FIGS. 1-2.

Such a relief ensures uniform compensation of mechanical stresses arising due to the difference in the thermoconcentration expansion of the frames and membranes, in any direction at any point on the surface of the membranes for any form of membranes. It almost completely eliminates the possibility of wrinkles, wrinkles, and other defects on the surface of the membranes, provides additional rigidity to the structure of the membranes and walls of the ME, increasing the life of the ME. Moreover, the proposed molding of membranes increases their productivity in pure hydrogen by increasing the true surface and the decrease in membrane thickness, the greater, the higher the plasticity of the membrane material with the same operating parameters, the initial thickness and surface area of the membrane to create a relief.

The membrane 1 on the supply side of the gas mixture can be hermetically connected around the perimeter with a metal frame 4, the inner size of which is smaller, and the outer dimension is larger than the outer dimension of the membrane 1 (Fig.Z).

Frame 4 is a structural element that ensures the strength and integrity of the membrane during its use, as well as facilitating the tight connection of the membrane with other structural elements of the membrane apparatus. The frame can be made of any structural material having a coefficient of thermal (thermal) expansion other than the coefficient of thermal (thermal) expansion of the material of the membrane, for example, stainless steel, nickel and nickel alloys, titanium.

The filter element 5 is preferably in the form of a flat disk (Fig. 4-5) contains (according to the first embodiment) the two membranes 1 described above, tightly connected around the perimeter with two frames 4 on the supply side of the gas mixture, the inner size of which is smaller and the outer dimension - larger than the outer size of the membrane 1. Between them is a porous separation element 6, the size of which is equal to or greater than the size of the membrane 1, but smaller than the outer size of the frame 4. The frames 4 have annular 7 and radial 8 corrugations, which, after tight connection I form a ring collector 9 around the perimeter for collecting pure hydrogen and a radial channel 10 into which a pipe 11 for removing pure hydrogen is placed, hermetically connected to the frames 4. The separation element 6 has minimal hydraulic resistance to ensure unhindered transport of pure hydrogen passing through the membranes 1, and communicates with the annular collector 9 to collect pure hydrogen passing through the membrane 1. The size of the separation element 6 may be equal to or greater than the size of the membrane 1 to Oh, so it can not damage the membrane 1 during assembly and operation. Figure 4 shows for example a filter element in the form of a flat disk, and figure 5 its cross section. But the filter element can have any other flat shape, for example, a square or rectangle, including with rounded corners, an ellipse, a flag, etc.

The filter element 5 may contain only one membrane 1 (one-sided filter element of FIGS. 12-13) connected hermetically to the frame 4 and forming the membrane wall 12, and a continuous metal wall (substrate) 13 with an external dimension equal to the outer dimension of the membrane wall frame 4 12, having the same annular 7 and radial 8 corrugations as the frame 4, a porous venting element 6 placed between the walls 12 and 13 and communicating with the peripheral annular collector 9 for collecting hydrogen. An annular collector 9 is formed after a tight connection of the frame 4 and the substrate 13 around the perimeter, as well as the radial channel 10, in which the pipe 11 for removing pure hydrogen is placed, hermetically connected to the frame 4 and the substrate 13.

The membrane apparatus (FIG. 6) includes a housing 14 with one or more filter elements 5 (FIGS. 4-5) placed therein. On both sides of the filter elements 5 there are gas exhaust 15 and gas supply 16 elements. On the housing 14 there are nozzles for supplying the initial gas mixture 17, the outlet of pure hydrogen 18 and the depleted gas mixture 19. The filter elements together with the gas supply and gas removal elements, the collectors of the hydrogen removal 20 and the depleted gas mixture 21 constitute the filter assembly of the membrane apparatus. The collectors are hermetically connected, respectively, with the conclusions of the hydrogen 18 and the lean gas mixture 19. The gas outlet elements 15 are made in the form of gas outlet pipes 22, hermetically connected to the exhaust manifold of the exhaust gas mixture 21. The gas supply elements 16 are made in the form of plates. The assembly of the gas supply elements 16 and gas exhaust elements 15 forms a deflector 23 (Figs. 7, 8-10), directing the initial gas mixture along the outer surface of the hydrogen-permeable membranes 1 and filter elements 5 from the periphery to the center and exhausting the gas mixture depleted from the center of their membranes, depleted after extraction of hydrogen passing through the membrane. Pipes 11, discharging pure hydrogen, passed through the membrane into the filter elements 5, are hermetically connected to the collector of hydrogen removal 20. The deflector 23 according to the first embodiment (Fig. 7) is made of two identical profiled disks 24, fastened together at the periphery and made with a central hole 25, with protrusions 26 on their outer sides extending from the periphery to the center, and with protrusions 27, forming on the inner side sides of said disks 24 a channel 28 in which a gas outlet pipe 22 is located.

The deflector 23 according to the second embodiment (Figs. 8-10) is made in the form of a flat disk 29 (Fig. 10) located in the slot of the gas outlet pipe 22 (Figs. 8, 9) extending from the center of the hydrogen permeable membrane and having an inner diameter larger than the thickness disk 29 (Fig. 8).

The filter elements 5 can be combined into a module of the filter unit, which is an assembly of filter elements 5 on the collector of pure hydrogen 19, and two or more modules of the filter unit with a common collector of hydrogen of the filter unit connected to the nozzle 18. In the same way, the branch pipes the depleted mixture 22 from the filter unit module can be combined by assembly on the collector 21, and the collector of all modules 21 with a common collector connected to the fitting 19.

The tightness of the connection of the nozzles 11 with the collector 20 and the collector 20 with the nozzle 18 of the drain of pure hydrogen, as well as the nozzles 22 with the collector 21 and the collector 21 with the nozzle 19 of the exhaust lean mixture is provided by welded joints. Welded joints can be ensured tightness of all of the above elements.

The nozzles 11 of the drain of pure hydrogen from the filter elements 5 can be replaced by fittings with ball-cone seals 31, as shown in Fig. 11, which shows the module of the filter unit.

The filtering elements 5 in this case are combined into a module 30, which is an assembly of filtering elements 5 on the collector of hydrogen removal 19, made in the form of a segment of a helix covering the specified assembly around the circle with rotation up to 270 degrees. These outlet nozzles with seals 31 of the filter elements 5 integrated into the module 30 are hermetically connected to the above collector 19 with rotation about an axis passing through the centers of their membranes 1 perpendicular to their plane, relative to each other by an angle of 10-20 degrees. The collector of module 19 in its the queue is hermetically connected by the same connection Зl to the common collector 20, and the collector 20 with the outlet fitting on the housing (not shown in Fig. 1).

The filter elements 5 can be combined into one or more of these modules, and the manifolds of the modules are hermetically connected to the common output collector of hydrogen 20 by a threaded connection of the ball-cone 32 type or by a welded connection (not shown).

The gas outlet pipes 22 can be hermetically connected to the depletion mixture manifolds 21 with welded joints or ball-cone threaded connections 31 (not shown), and the manifold 21 with a fitting 22 leading the lean mixture out of the housing, a ball-cone threaded joint or welded joint (not shown).

On the membrane 1 (according to the closest analogue - Fig. 14) with the initial circular corrugations 33 and frame 4, the radial folds 34 formed as a result of the tests are visible. They lead to rapid depressurization of the filter elements and their failure. Moreover, as follows from the data of Tables 1-4 below, the creation of corrugations with a cross-section in the form of a semicircle inevitably leads to rupture of membranes from currently known palladium alloys due to the failure of ratio 1. Thus, the use of such corrugations does not fulfill the intended functions - increase productivity and service life of the membranes.

The membrane apparatus (Fig.6) with patentable filtering elements (Fig.4, 5) works as follows.

The initial gas mixture containing hydrogen is supplied to the housing 14 through the fitting 17 and passes into the slotted channels between the surfaces of the membrane 1 and the disks 24 (Fig. 7) of the deflector 23 and flows over the surface of the membranes from the periphery to the center. In this case, hydrogen passes through the membranes 1 into the filter elements 5 and is discharged through the separation element 6, the outlet pipe 11 into the collector of clean hydrogen 20 and is discharged from the housing 14 through the fitting 18, and the lean gas mixture is discharged from the center of the membrane 1 through the hole 25 in the center the disk 24 of the deflector 23 (Fig.7) into the gas outlet pipe 22 and the collector of its outlet 21 and is removed from the housing through the fitting 19.

By varying the height of the protrusions 26 on the surface of the disks 24 of the deflector 23, the supply parameters and the flow of the initial mixture are adjusted along the surface of the membranes 1, such as speed and flow rate, and by changing the diameter of the hole 25 in the center of the deflectors 23 and the pressure at the terminal 19 from the housing 14, the flow rate of the exhaust lean gas mixture is adjusted.

The deflector 23 can also be made according to the second embodiment (Figs. 8-10). In this case, the outer diameter of the gas outlet pipe 22 determines the width of the slot channel for supplying the initial gas mixture, and the gas mixture depleted as a result of the selection of pure hydrogen through the membranes 1 is discharged from the center of the membranes 1 through two slots formed by the inner wall of the pipe 22 and the disk 29. By varying these Parameters provides adjustment of the flow parameters of the initial mixture and removal of the lean gas mixture. The nozzles 22 of the deflectors 23 are hermetically connected to the exhaust manifold exhaust manifold 21.

The described design ensures the constancy of the composition, pressure and velocity of the feed mixture to the periphery of the surface of all membranes installed in the filtering unit, changes in the radius of the membranes of the velocities and concentrations of all components, including hydrogen, as well as the pressure, composition and flow rate of the lean mixture discharged from the center of the membranes .

The presence of a convex regular relief on the surface of the membranes due to their molding with a height commensurate with the width of the channels leads to the formation of turbulent vortices in the gas flow and accelerates the mixing of the flow and the supply of hydrogen to the surface of the membranes, increasing their productivity. Both described designs of deflectors (Figs. 7 and 8-10) completely exclude the occurrence of stagnant zones, inconstancy of the concentration of hydrogen in the initial mixture along the height of the filter assembly, typical for analogues and prototypes.

By replacing the outlet pipes 11 for discharging pure hydrogen into fittings that are sealed with a collector 20 by using threaded connections with a ball-cone seal instead of welding (Fig. 11), the assembly and disassembly of the filter assembly are simplified, the maintainability is increased by disconnecting each defective filter element from the collector of the removal of pure hydrogen and its replacement with a new one. In this design, it is easier to implement the modular principle of forming filter units, and the regeneration of palladium from defective filter elements is also facilitated. The implementation of the invention

Example 1. Four groups of identical samples of membranes with a diameter of 50 mm, 5 samples in each group, were cut from a 50 μm thick PdInRu alloy foil. Three groups of samples were annealed in vacuum, and the fourth was left without annealing. All samples were molded by pressing at a pressure of 16 kg / mm ² with the creation of a relief in the form of segments of a sphere located uniformly on the surface, with a radius of spheres R = 2.5 mm and different heights. The results of the leak test before and after molding are shown in table 2, where the number of sealed samples of different groups after surface forming is presented.

Thus, the tightness of the membranes after molding is maintained in 100% of cases when condition (1) is met, and is broken in 100% of cases if this condition is not fulfilled.

Example 2

Three identical samples of membranes with a diameter of 50 mm were cut from foils of alloys PdY6%, PdCu40%, and PdCuPb 50 μm thick, obtained by cold rolling. Two samples from each alloy were annealed in vacuum, and one was left without annealing. All samples were molded by pressing at a pressure of 16 kg / mm to create a relief in the form of segments of a sphere located uniformly on the surface with a radius of spheres R = 2.5 mm and different heights. The results of leak testing before and after molding are shown in Table 3. Thus , the tightness of the membranes after molding is maintained in 100% of cases under condition (1), and is violated in 100% of cases if this condition is not met for all membranes with different compositions of the palladium alloy.

Example 3 Three identical samples of membranes with a diameter of 50 mm were cut from a PdInRu alloy foil 50 μm thick. The surface of one of them is molded by creating corrugations in the form of radial rays at an angle of 30 °, the second by pressing at a pressure of 16 kg / cm ^{2 the} surface of the membrane in the form of spherical segments of radius R = 2.5 mm and a height h = 0.5 mm, arranged uniformly on the surface, and the third left without molding. After that, the membranes are hermetically connected to the frames. A check was carried out to confirm the tightness of all three membranes with frames. After that, they were tested under conditions typical for the operation of membrane filter elements and filter units. For this, they were placed in a vacuum chamber, where they were heated at a residual air pressure of 10 mm Hg. Art. to a temperature of 35O ⁰ C, then hydrogen was admitted to a pressure of 0.5 MPa, the temperature increased to 600 ⁰ C and the walls were kept under these conditions for an hour, then they were cooled to 35O ⁰ C in hydrogen, then the chamber volume was pumped out to 10 ^"4 mm Hg and cooled to room temperature. This procedure was repeated five times. Subsequent inspection of the surface and the tightness of the membranes with frames after removing them to the atmosphere showed that the wall with the unformed membrane is strongly warped and leaky. somewhat distorted, but its tightness is not broken.The wall with a membrane molded by creating a deep relief in the form of segments of a sphere is also tight and also has not changed its appearance. Thus, it is shown that full compensation of the stresses of the membranes with frames due to thermal and concentration expansion in a hydrogen atmosphere, only membrane formation is possible by creating a relief in the form of sphere segments evenly spaced along the surface while maintaining the condition L / D <1 + δ (1).

Example 4

Three identical membranes were cut from a 50 μm thick PdInRu alloy foil. The surface of one of them is molded by pressing at a pressure of lbqr / cm ² with the creation of a deep relief in the form of segments of a sphere with a radius of 2.5 mm and a height of 0.5 mm, and the second with a height of 0.7 mm located uniformly on the membrane surface. The surface of the third is left unchanged. Of these, samples were cut with a diameter of 28 mm, which were installed in airtight cells for measuring the flow rate of hydrogen passing through the membrane with a diameter of the geometric working surface of 20 mm, and measurements were taken of the flow rate of hydrogen passing through the membrane with the same parameters. The measurement results are shown in table 4. As follows from the data in table 4, the molding of the membrane surface increased the consumption of pure hydrogen at the same parameters by 1.3-1.5 times in comparison with the unformed sample.

Example 5. Three identical membranes are cut from a PdY6% foil with a thickness of 50 μm. The surface of one of them is molded by pressing at a pressure of lkg / cm with the creation of a deep relief in the form of segments of a sphere with a radius of 2.5 mm and a height of 0.5 mm, the second - with a height of 0.7 mm, located uniformly on the surface of the membranes. The surface of the third is left unchanged. Samples of 28 mm diameter were cut from them, which were installed in sealed cells for measuring the flow rate of hydrogen passing through the membrane with a diameter of the geometric working surface of 20 mm, and measurements were taken of the flow rate of hydrogen passing through the membrane with the same parameters. The measurement results are shown in table 5. As follows from the data in table 5, the molding of the surface of the membranes increased the consumption of pure hydrogen at the same parameters by 1.3-1.5 times in comparison with the unformed sample.

Example 6. Three filtering bilateral elements with membranes from Bl alloy with a thickness of 50 μm and a membrane working area of 0.0032 m are installed in sealed enclosures with various schemes for supplying the initial gas mixture and removing the gas mixture depleted after hydrogen extraction:

- in the chamber N ° l, the supply of the initial mixture and the removal of the depleted were carried out through fittings located diametrically opposite to each other in the side wall;

- in the chamber N ° 2, the supply of the initial mixture was carried out through a tubular manifold, covering half the perimeter of the filter element and having radial holes uniformly spaced along the length, directed toward the surface of the membranes, and the discharge of the lean mixture through a fitting located diametrically opposite to the supply fitting of the initial mixture;

- in the chamber N ° 3, the initial mixture was supplied into the chamber volume through the fitting located in the lid, and the depleted mixture was discharged through two nozzles with inlet openings located above the centers of the membranes and hermetically connected to the outlet fitting.

A gas mixture was supplied to all chambers from the outlet of the catalytic conversion reactor of methanol with a flow rate of 0.32 Nm ³ / h, containing 68% hydrogen, at a pressure of P ₁ with a temperature of 490C. The pressure of pure hydrogen passing through the membranes (P ₂ ) was slightly higher than atmospheric. The extraction parameters and the results of measuring the consumption of pure hydrogen (GH ₂ ) of the lean mixture (Gout) and the hydrogen extraction coefficient (η Щ) are given in Table 6.

From the data obtained it follows that the coefficient of extraction of pure hydrogen with the same parameters and composition of the initial mixture when feeding it from the periphery of the membranes and removing the lean mixture from the center (N ° 3) exceeds by 35% the coefficient of extraction when feeding and removing from the edges of the membranes (NsI) and 16% - when feeding from half the periphery and draining the lean mixture through the pipe from the edge

(N ° 2). The increase in efficiency is due to the elimination of stagnant zones and uneven flows.

Example 7

In the membrane apparatus (Fig. 7) containing 10 filtering elements 5 in the form of a flat disk (Fig. 5) with membranes with a working diameter of 144 mm and an initial thickness of 0.05 mm from PdCu40% alloy, on the surface of which a relief is created in the form of convex segments of a sphere R = 4 mm, height h = 0.8 mm, the deflectors placed between them in the form of stamped disks (Fig. 9) were supplied through a nozzle 17 under a pressure of 3.0 MPa, a gas mixture with a temperature of 35O ⁰ C, containing 70% hydrogen, 9.36% CH ₄ , 6.73% CO ₂ , 3.69% CO and 10.22% H ₂ O, with a consumption of 53.6 Nm ³ / h. Hydrogen passing through the membranes was sampled at a pressure of 0.15 MPa through nozzle 19, and the lean gas mixture was discharged from the apparatus through nozzle 18. The measured flow rate of pure hydrogen (> 99.9999%) was 30 Nm ³ / h, and the degree of hydrogen extraction was 80% . After that, the initial gas mixture was supplied through the nozzle 19 to the same apparatus with the same parameters. Thus, the flow direction of the initial gas mixture above the surface of the membranes 1 reversed - the mixture was supplied in the center of the membranes 1, and the depleted mixture was discharged from the periphery of the membranes . In this case, the measured consumption of pure hydrogen was 22 Nm ³ / h, and the degree of hydrogen extraction was 59%. Thus, changing only the direction of flow of the initial gas mixture above the membrane and taking the lean gas mixture from the periphery of the membranes led to a decrease in the degree of hydrogen extraction equal conditions almost 1, 3 times.

Example 8

In the membrane apparatus (Fig. 7) containing 10 filtering elements in the form of a flat disk (Fig. 5) with membranes with a working diameter of 144 mm and an initial thickness of 0.05 mm from PdY6% alloy, on the surface of which a relief is created in the form of convex segments of the sphere R = 2.5 mm in height h = 0.5 mm, and deflectors placed between them in the form of plates with a diameter of 150 mm and a thickness of 1.5 mm, cut into a 6x1 mm pipe (Fig. 7), were supplied through a nozzle 18 under a pressure of 3.0 MPa with a gas mixture with a temperature of 45O ⁰ C, containing 70% hydrogen, 9.36% CH ₄ , 6.73% CO ₂ , 3.69% CO and 10.22% H ₂ O, with a flow rate of 90 Nm ³ / h. Hydrogen passing through the membranes was sampled at a pressure of 0.15 MPa through the nozzle 17, and the lean gas mixture was removed from the apparatus through the nozzle 19. The measured flow rate of pure hydrogen (> 99.9999%) was 43 Nm ³ / h, and the degree of hydrogen extraction was 68 %

Table 1

Table 2

Table 3

Table4

Table 5

Table6

Claims

Claim.

1. A hydrogen-permeable membrane based on a palladium alloy with a raised outer surface with alternating protrusions and depressions surrounding each protrusion, characterized in that the palladium alloy contains one or more elements from groups I ⁶ , III, IV and VIII of the Periodic Table of the Elements, and the ratio of the arc length L on the surface of the protrusions in their cross section to the length of its projection onto the base area D is in the range from 1.05 to 1 + δ, where δ is the ductility of the membrane material.

2. A hydrogen permeable membrane according to claim 1, characterized in that said protrusions are made with a convex surface.

3. A hydrogen permeable membrane according to claim 1, characterized in that said protrusions are made in the form of a spherical, parabolic or ellipsoidal segment.

4. A hydrogen permeable membrane according to claim 1, characterized in that said protrusions are arranged uniformly on the surface of the membrane.

5. A hydrogen permeable membrane according to claim 1, characterized in that said depressions are interconnected.

6. A hydrogen permeable membrane according to claim 1, characterized in that it has a metal frame on the supply side of the gas mixture tightly connected to it along the perimeter, the internal size of the frame is smaller, and the external size is larger than the external size of the membrane.

7. A hydrogen permeable membrane according to claim 1, characterized in that said frame is made of metal with a coefficient of thermal expansion different from the coefficient of thermal expansion of the palladium alloy of which the membrane is made.

8. Hydrogen-permeable membrane according to claim 7, characterized in that said frame is made of structural material.

9. A hydrogen permeable membrane according to claim 1, characterized in that it is made in the form of a plate with the shape of a flat figure.

10. Hydrogen-permeable membrane according to claim 9, characterized in that the plate is made in the form of a circle, ellipse, square or rectangle.

11. A filter element comprising two walls, one of which is made in the form of a hydrogen-permeable membrane of palladium alloy, with a separating gas outlet element located between them, the gas outlet channels of which are connected to the annular collector for collecting hydrogen with a discharge nozzle, characterized in that the other wall is made in the form of a hydrogen-permeable membrane or a continuous metal substrate, each hydrogen-permeable membrane is made with a relief external surface with alternating protrusions and surrounding yuschimi each protrusion troughs, wherein, palladium alloy contains one or more elements from ⁶ I, III, IV and VIII of the Periodic Table of the Elements, and the ratio of the maximum projection length L to the maximum length of the surface projection base of D ranges from 1.05 to 1 + δ, where δ is the ductility of the membrane material, while the gas separation element is made porous with the smallest possible hydraulic resistance to clean hydrogen, each membrane is hermetically connected on the supply side of the gas mixture to the frame, inside Nij size is smaller, and the outer size - size larger than the outer membrane or equal to the outer size of the solid metal substrate and the frame or between the frame and a solid metal substrate is hermetically joined at the perimeter to form a ring collector for collecting hydrogen.

12. The filter element according to item ll, characterized in that the separating gas outlet element is made in the form of a set of woven grids coated with an inert material, excluding its welding with membranes in a hydrogen medium, and its linear dimensions are larger or equal to the linear dimensions of the membrane, but smaller linear dimensions of the frame or solid metal substrate.

13. The filter element according to claim 1, characterized in that said protrusions of the hydrogen-permeable membrane are made with a convex surface that faces the feed mixture.

14. The filter element according to claim 1, wherein said protrusions of the hydrogen permeable membrane are made in the form of a spherical, parabolic or ellipsoid segment.

15. The filter element according to item ll, characterized in that said protrusions of the hydrogen permeable membrane are evenly distributed over the surface of the membrane.

16. The filter element according to claim 11, characterized in that said troughs of the hydrogen permeable membrane are interconnected.

17. The filter element according to claim 11, characterized in that said frame is made of metal with a thermal expansion coefficient different from the thermal expansion coefficient of the palladium alloy from which the membranes are made.

18. The filter element according to claim l l, characterized in that said frame is made of structural material.

19. The filter element according to claim l l, characterized in that the hydrogen permeable membrane is made in the form of a plate with the shape of a flat figure.

20. The filter element according to claim 19, characterized in that the plate is made in the form of a circle, ellipse, square or rectangle.

21. The membrane apparatus, comprising a housing with one or more filter elements placed in it with gas exhaust and gas supply elements placed on both sides thereof and having an input of the initial gas mixture, leads of hydrogen and a lean gas mixture, characterized in that it is provided with collectors of hydrogen removal and depletion of the lean gas mixture, hermetically connected, respectively, with the conclusions of hydrogen and depleted gas mixture, each filter element is made in the form of a filter element according to item ll, gas These elements are made in the form of gas outlet pipes sealed to the drain manifold of the lean gas mixture, gas supply elements are made in the form of deflectors directing the initial gas mixture along the outer surface of the hydrogen-permeable membranes of the filter elements from their periphery to the center, and outlet pipes of the peripheral ring collectors for collecting hydrogen filter elements are hermetically connected to the collector of hydrogen removal.

22. The membrane apparatus according to item 21, wherein the deflector is made of two identical profiled disks fastened together at the periphery and made with a central hole, with protrusions on their outer sides extending from the periphery to the center, and with protrusions on the inner sides of said disks forming a channel in which a gas outlet pipe is located.

23. The membrane apparatus according to item 21, wherein the deflector is made in the form of a flat disk located in the slot of the exhaust pipe, extending from the center of the hydrogen-permeable membrane and having an inner diameter greater than the thickness of the disk.

24. The membrane apparatus according to item 21, wherein the protrusions of the hydrogen permeable membrane of the filter elements are made with a convex surface.

25. The membrane apparatus according to item 21, wherein the said protrusions of the hydrogen permeable membrane are made in the form of a spherical, parabolic or ellipsoid segment.

26. The membrane apparatus according to item 21, characterized in that the said protrusions of the hydrogen permeable membrane are evenly distributed over the surface of the membrane.

27. The membrane apparatus according to item 21, wherein the said troughs of the hydrogen permeable membrane are interconnected.

28. The membrane apparatus according to item 21, wherein the hydrogen permeable membrane is made in the form of a plate with the shape of a flat figure.

29. The membrane apparatus according to item 21, wherein the plates are made in the form of a circle, ellipse, square or rectangle.

30. The membrane apparatus according to item 21, wherein the permeable hydrogen membrane has a metal frame sealed to it.

31. The membrane apparatus according to claim 3, characterized in that said frame is made of metal with a thermal expansion coefficient different from the thermal expansion coefficient of the palladium alloy from which the membranes are made.

32. Membrane apparatus according to claim 3, characterized in that said frame is made of structural material.

33. The membrane apparatus according to item 21, wherein the supply of the source gas mixture and the conclusions of hydrogen and lean gas mixture are made in the form of fittings.

34. The membrane apparatus according to item 21, wherein the sealed connections of these outlet pipes with a collector of hydrogen removal are made in the form of threaded connections with ball-cone seals.

35. The membrane apparatus according to item 21, characterized in that the sealed connections of these outlet pipes with a collector of hydrogen removal are made in the form of welded joints.

36. The membrane apparatus according to item 21, characterized in that the filter elements are combined into a module, which is an assembly of elements on the collector of hydrogen removal, made in the form of a segment of a helix covering the specified assembly around the circumference with a rotation of up to 270 degrees.

37. The membrane apparatus according to clause 36, wherein said outlet pipes of filter elements combined into a module are hermetically connected to the above collector with rotation about an axis passing through the centers of the membranes perpendicular to their plane, at an angle of 10-20 degrees relative to each other .

38. The membrane apparatus according to clause 36, wherein the filter elements are combined into one or more of these modules, and their outlet pipes are hermetically connected to a common hydrogen output manifold by a ball-cone threaded connection.

39. The membrane apparatus according to clause 35, wherein the filter elements are combined into one or more of these modules, and their outlet pipes are hermetically connected to a common output hydrogen collector by a welded joint.