CN105056715A - Hydrogen separation device - Google Patents
Hydrogen separation device Download PDFInfo
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- CN105056715A CN105056715A CN201510512732.3A CN201510512732A CN105056715A CN 105056715 A CN105056715 A CN 105056715A CN 201510512732 A CN201510512732 A CN 201510512732A CN 105056715 A CN105056715 A CN 105056715A
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Abstract
The invention discloses a hydrogen separation device. The hydrogen separation device comprises a tubular hydrogen separation membrane, a closure plate, a shell, a hydrogen exhaust opening, an embedded part, an outer surface of an inner tube of the embedded part, the inner tube, a gas delivery tube, a gas flow path, a hydrogen separation membrane assembly, a gas supply opening and a gas exhaust opening; the tubular hydrogen separation membrane can selectively allow hydrogen to permeate and is provided with through holes; the hydrogen exhaust opening is formed in the shell; the gas supply opening can deliver unprocessed gas to the interior of the hydrogen separation membrane; the gas exhaust opening can deliver the gas which cannot permeate through the hydrogen separation membrane; the hydrogen exhaust opening can exhaust the hydrogen which permeates through the hydrogen separation membrane, and hydrogen molecules can permeate to the other side of the hydrogen separation membrane after making contact with the hydrogen separation membrane due to the through holes formed in the hydrogen separation membrane; the embedded part is provided with the gas delivery tube, and the gas supply opening and the gas exhaust opening are divided by the gas delivery tube; an opening in the tail end of the tubular hydrogen separation membrane is next to the closure plate, and the outer surface of the embedded part extends to the position near the closure plate.
Description
Technical field
The present invention relates to a kind of hydrogen separation membrane device, described a kind of hydrogen separation device can make hydrogen separate from containing the mist of hydrogen, and relates to a kind of Hydrogen Separation method.
Background technology
Along with the environmental problems such as global warming in the last few years receive much concern, the research and development form little to environmental pressure is also more and more taken seriously.These start to be used as the equal energy source such as hydrogen and hydrogen fuel cell.Hereinafter patent document 1 describes the technology be separated from the gas body of hydrogen by hydrogen, more particularly, is a kind of hydrogen purification device with tubulose palladium alloy membrane.
Hydrogen generates by reacting (see formula (1)) in water vapour as methane, and can accelerate the generation (see formula (2)) of hydrogen when adding carbon monoxide.
(1)CH4+H2O→CO+3H2
(2)CO+H2O→CO2+H2
By supplying urban atmospheres kerosene in incinerator, usually mist can be produced in the incinerator containing hydrogen and other gases.These mists comprise carbon dioxide, methane and steam.Although different with the type of reaction condition according to raw material composition, in mist, the large appointment of hydrogen accounts for cumulative volume 70%, and carbon dioxide concentration wherein accounts for 30% of cumulative volume.
According to the research of present inventor, when being such as separated the above-mentioned mist containing a large amount of hydrogen with traditional Hydrogen Separation membrane module, even if hydrogen purity is very high, continues to use single measure and efficiency can not be allowed to increase.Namely problem is how to solve low separative efficiency, and this may be because traditional separation membrane device only requires the critical piece by improving the pending gas purity of density of hydrogen more than 99% further.
The invention provides a kind of hydrogen separation device, hydrogen can be isolated expeditiously from pending mist, described hydrogen separation device comprises: outer surface, interior pipe, air shooter, gas flow paths, hydrogen separation membrane assembly, air supply opening, the gas discharge outlet of pipe in the inner surface of tubulose Hydrogen Separation film, Hydrogen Separation film, the outer surface of Hydrogen Separation film, shrouding, shell, hydrogen discharge, insert, insert, the described selectively permeable hydrogen of tubulose Hydrogen Separation film, described Hydrogen Separation film contains through hole; Described hydrogen discharge in the enclosure.Described air supply opening can carry untreated gas inner to Hydrogen Separation film; Described gas discharge outlet can be carried can not through the gas of Hydrogen Separation film; Described hydrogen discharge can discharge the hydrogen of permeate through hydrogen gas diffusion barrier, and the through hole on described Hydrogen Separation film makes hydrogen molecule can penetrate into the another side of Hydrogen Separation film after contact Hydrogen Separation film; Described insert has an air shooter, and air supply opening and outlet are shunted by air shooter; The opening of described tubulose Hydrogen Separation film end is close to shrouding, and the outer surface of insert extends near shrouding.
In the present invention, the outlet of the end of described tubular separation membrane is provided with a shrouding, and the outer surface of described insert stretches out shrouding outward mutually.According to this structure, described gas flow paths makes pending mist flow to outlet along the inner surface of tubular separation membrane, increases the area of mist to be separated and described tubular separation membrane with this, thus improves the separative efficiency of hydrogen.
The present invention also provides a kind of Hydrogen Separation method using above-mentioned hydrogen separation device, comprise and a kind of tubulose Hydrogen Separation film is provided, flow in the gas flow paths that described tubulose Hydrogen Separation film makes gas form at the outer surface of the inner surface of tubular separation membrane and insert, and hydrogen can be gone out by tubulose Hydrogen Separation membrane filtration from pending hydrogeneous mist.
According to described Hydrogen Separation method and hydrogen separation device, pending mist makes pending mist flow along the inner surface of Hydrogen Separation film by described air flow path, to guarantee that the mist containing hydrogen molecule fully contacts Hydrogen Separation film, further, pending mist is adjusted to the state of laminar flow with increased efficiency, thus obtain highly purified hydrogen.
Summary of the invention
The object of the invention is to overcome in prior art not enough, provide a kind of Hydrogen Separation equipment, according to a kind of hydrogen separation device of the present invention, user can isolate high-purity hydrogen and have containing good hydrogen production efficiency from pending gas.For achieving the above object, present invention employs following technical scheme:
A kind of hydrogen separation device, described a kind of hydrogen separation device comprises: described hydrogen separation device comprises outer surface, interior pipe, air shooter, gas flow paths, hydrogen separation membrane assembly, air supply opening, the gas discharge outlet of pipe in tubulose Hydrogen Separation film, the inner surface of Hydrogen Separation film, the outer surface of Hydrogen Separation film, shrouding, shell, hydrogen discharge, insert, insert.The described selectively permeable hydrogen of tubulose Hydrogen Separation film, described Hydrogen Separation film contains through hole; Described hydrogen discharge in the enclosure.Described air supply opening can carry untreated gas to arrive film inside; Described gas discharge outlet can be carried can not through the gas of Hydrogen Separation film; Described hydrogen discharge can discharge the hydrogen of permeate through hydrogen gas diffusion barrier, and the through hole on described Hydrogen Separation film makes hydrogen molecule can penetrate into the another side of Hydrogen Separation film after contact Hydrogen Separation film.
Preferably, described insert has a carrier pipe, and gas supply opening and outlet are shunted by air shooter.
Preferably, the opening of described tubulose Hydrogen Separation film end is close to shut, and the outer surface of insert extends near shut.
A kind of Hydrogen Separation method, described hydrogen separation device comprises the flow path that untreated mist is formed along tubulose Hydrogen Separation film and insert outer surface, and the hydrogen in the untreated gas of hydrogen can through Hydrogen Separation film.
Preferably, the wherein adjacent shut of the opening of the end of tubular separation membrane, and insert outer surface extends near shut.
The present invention has following advantage: according to a kind of hydrogen separation device of the present invention, and user can isolate high-purity hydrogen and have containing good hydrogen production efficiency from pending gas.
Accompanying drawing explanation
Fig. 1 is the sectional view of a hydrogen separation device based on prior art.
Fig. 2 is the sectional view of another embodiment of the invention.
Fig. 3 is the hydrogen separation device with multiple Hydrogen Separation film of the present invention.
Fig. 4 is the top view after a kind of hydrogen separation device of Fig. 3 removes shell.
Fig. 5 is the sectional view of traditional hydrogen separation device.
Wherein, 1, Hydrogen Separation film; The inner surface of 1a, Hydrogen Separation film; The outer surface of 1b, Hydrogen Separation film; 2, shrouding; 5, sleeve pipe; SA, hydrogen discharge; 8,18, insert; The outer surface of 8F, 18F, interior pipe; 8a, 18, interior pipe; 8b, 18b, air shooter; 9,19, gas flow paths; 10,20,30, hydrogen separation membrane assembly; 10A, 20A, air supply opening; 10b, 20b, gas discharge outlet; 28, insert.
Detailed description of the invention
With the drawings and specific embodiments, the present invention is further detailed explanation below.
Hydrogen separation device
Embodiment 1
Shown in Fig. 1 is a kind of hydrogen separation membrane assembly (being called simply " assembly ") 10, assembly 10 provides a kind of cylindrical hydrogen diffusion barrier 1 selected through hydrogen, one is arranged on the shell 5 on Hydrogen Separation film 1, the insert 8 of Hydrogen Separation film 1 inside is arranged on one, wherein, the material of shell 5 and insert 8 comprises stainless steel, inconel and hastelloy.
Hydrogen Separation film 1 has the selective performance through hydrogen molecule.This Hydrogen Separation film can differential permeability be because the hydrogen molecule of the inner surface of Hydrogen Separation film arrives at 2000 DEG C
Hydrogen atom has been dispersed at the temperature of 6000 DEG C, hydrogen atom is subject to the driving force produced at Hydrogen Separation film outer surface 1b due to Hydrogen Separation film 1 surfaces externally and internally pressure difference when moving to Hydrogen Separation film outer surface 1b, hydrogen atom and other hydrogen atoms tie the Surface Creation hydrogen being incorporated in Hydrogen Separation film at the outer surface 1b of Hydrogen Separation membrane module 1.
The material of Hydrogen Separation film 1 comprises palladium, copper palldium alloy and silver palladium alloy.In above-mentioned alloy, add other elements can suppress the hydrogen permeability of Hydrogen Separation film to reduce.Other elements comprise: Mg, Ti, Mn, Fe, Co, Ni, Cu, Nb, Mo, Ag, Ai, Pt, Rh, Ru, I, S, Pr, Sm and Gd.
Hydrogen Separation film 1 can be a dense film be only made up of above-mentioned material, or the film that fine and close, and this film comprises the above-mentioned permeable material mentioned.In the case of the former, the thickness of Hydrogen Separation film 1 is for ease of processing preferably 2 μm or thicker, 5 μm to 25 μm.
In shell, Hydrogen Separation film 1 comprises the dense film be made up of above-mentioned material and through hole, at the screening gaseous species of through hole, and makes pending mist isolate hydrogen by described film.
Hydrogen Separation film 1 is columniform, and interior diameter is 10mm or thicker, as 25mm to 40mm.The length of Hydrogen Separation film is 50mm or longer, as 80mm to 1000mm.
Further, by shrouding 2, the distal openings being positioned at Hydrogen Separation film 1 is closed.On the other hand, plate 3 has a through hole 3a and is connected with the proximal openings 1d of Hydrogen Separation film 1.It is inner that pending mist delivers to Hydrogen Separation film 1 by this through hole 3a.The material of shrouding and plate 3 comprises stainless steel, inconel and hastelloy.Hydrogen Separation film 1 is connected with shrouding 2 and plate 3 makes it airtight, and this connected mode can be welding or electron beam welding.
Insert 8 has an interior pipe 8a, the internal diameter of described interior pipe 8a is slightly less than the external diameter of Hydrogen Separation film 1, described insert 9 embeds the air shooter 8b of shrouding 3 through hole 3a, with the far-end being positioned at shrouding 2, with respectively by shrouding 8c with envelope version 8d close into an annular by pipe 8a in far-end with near-end and air shooter 8b.By the inner side that will the insert 8 of such said structure had to be placed in Hydrogen Separation film 1, the gas flow paths 9 at pending mist place is made to be in the outer surface 8F of interior pipe 8a and the inner surface 1a of Hydrogen Separation film 1.
The interior pipe 8a of insert 8 is extended near shrouding 2.The upper surface of interior pipe 8a(shut 8c) and the spacing of shrouding 2 be 0.1mm to 10mm, preferably 0.1mm to 5mm.
The outer surface 8F of interior pipe 8a and the spacing of Hydrogen Separation film 1 are 0.1mm to 30mm, are preferably 1mm to 25mm, can be even 1mm to 20mm.If this spacing is less than 0.1mm, Hydrogen Separation efficiency will decline when pending mist flow velocity is large, and if distance exceeds 30mm, the pending mist containing hydrogen molecule and the contact of Hydrogen Separation film 1 just will tail off.
Gas air supply opening far-end is provided with a breach 8e, will be converted to gas discharge outlet 10b by breach 8e by the non-infiltration gas of gas flow paths 9.In the present embodiment, the proximal end of air shooter 8b accepts gas supply opening 10a, and the annular element between through hole 3a and air shooter 8b accepts gas outlet pipe 10b.As shown in Figure 1, although insert 8 is hollow between interior pipe 8a and air shooter 8b, this part can not be hollow.
Shell 5 comprises described Hydrogen Separation film 1, and the upper end face of shell 5 is provided with a hydrogen discharge 5a.The hydrogen gone out from Hydrogen Separation UF membrane can be discharged by hydrogen discharge 5a.Assembly 10 by said structure is set forth effect below: in assembly 10, as illustrated by the arrows in fig. 1, untreated gas can in the inner surface 1a of Hydrogen Separation film 1 and insert 8 pipe 8a outer surface between flow along gas flow paths 9.Therefore, the amounts of hydrogen of discharging from hydrogen discharge will increase greatly, obtain highly purified hydrogen when high-recovery.In addition, in assembly 10, gas supply opening 10a and gas discharge outlet 10b is embedded into the air shooter 8b of part 8 separately.Like this, the mist cross-current to be separated from gas supply pipe 10a to gas flow outlet is made to be blocked.
Further, in assembly 10, at the opening 1c of the far-end of Hydrogen Separation film 1 this shrouding 2 adjacent, and the interior pipe 8a of insert 8 extends to the near-end of shrouding 2.Owing to adopting this structure, gas flow paths 9 makes mist to be separated flow to outlet along the inner surface of Hydrogen Separation film 1, increases the area of mist to be separated and described Hydrogen Separation film 1 with this, thus improves the separative efficiency of hydrogen.
Embodiment 2
As shown in Figure 2, assembly 20 comprises can the selective cylindric Hydrogen Separation film 1 through hydrogen, holds the shell 5 of hydrogen diffusion barrier 1, and an insert 18 be arranged in Hydrogen Separation film 1.The insert 18 of assembly 20 is different from the insert 8 of above-mentioned assembly 10, replaces, and the insert 18 in assembly 20 has structure as described below.The concrete difference of insert 18 will be introduced below.
As shown in Figure 2, as shown in Figure 2, insertion parts 18 is near-end by interior pipe 18a and feed tube 18b to the described insert 18 be made up of interior pipe 18a and air shooter 18b.In the present embodiment, untreated mist can flow along gas flow paths 19 between the inner surface 1a of Hydrogen Separation film 1 and the outer surface 18b of interior pipe 18a.Interior pipe 18a has an external diameter larger than air shooter 18b.The near-end of interior pipe 18a extends near plate 3, and this makes at impermeable gas by reaching gas delivery port 20b between insert 18 and plate 3.In the present embodiment, the near-end of air shooter 18b accepts supply opening 20a, and in addition, the annulus between through hole 3a and air shooter 18b accepts gas delivery port 20b.
The interior pipe 8a of insert 8 is extended near shrouding 2.The spacing of interior pipe 18a and shrouding 2 is 0.1mm to 10mm, preferably 0.1 to 5mm.The outer surface 18F of interior pipe 18a and the spacing of Hydrogen Separation film 1 are 0.1mm to 30mm, are preferably 1mm to 25mm, can be even 1mm to 20mm.Assembly 20 by said structure is set forth by effect below.Specifically, in assembly 20, as illustrated by the arrows in fig. 1, untreated gas can in the inner surface 1a of Hydrogen Separation film 1 and insert 18 pipe 18a outer surface between flow along gas flow paths 19.Therefore, the amounts of hydrogen of discharging from hydrogen discharge will increase greatly, obtain highly purified hydrogen when high-recovery.In addition, in assembly 20, gas supply opening and gas discharge outlet 20b are embedded into the air shooter 18b of part 18 separately.Like this, the mist cross-current to be separated from gas supply pipe 20a to gas discharge outlet 20b is made to be blocked.
Further, in assembly 20, at the opening 1c of the far-end of Hydrogen Separation film 1 this shrouding 2 adjacent, and the interior pipe 18a of insert 18 extends to the near-end of shrouding 2.Owing to adopting this structure, gas flow paths 19 makes mist to be separated flow to outlet along the inner surface of Hydrogen Separation film 1, increases the area of mist to be separated and described Hydrogen Separation film 1 with this, thus improves the separative efficiency of hydrogen.
A kind of Hydrogen Separation method
Below according to the invention provides the Hydrogen Separation method that adopts Hydrogen Separation membrane module, using the assembly 10 in the first embodiment to carry out separating hydrogen gas here, assembly 20 can be used equally to carry out separating hydrogen gas.
According to the Hydrogen Separation method described in the present embodiment, pending mist by the flow path 9 between the inner surface 1a of Hydrogen Separation film 1 and the outer surface 8F of insert 8, and is that the mist that the is mixed with hydrogen inside from cylindrical hydrogen diffusion barrier 1 is to outside.Although have no particular limits the density of hydrogen of untreated gas, the clear gas concentration in mist can be 50% to 100% or 70% to 100%.According to a kind of hydrogen separation device of the present invention, it is characterized in that: described hydrogen separation device still can isolate highly purified hydrogen when hydrogen concentration is low.Such as, in untreated mist, the concentration of hydrogen can be 95% or less, as 85% or be less than or equal to 80%.
In pending mist, other gases are as carbon dioxide, carbon monoxide, methane, nitrogen and steam.Such as, in hydrogen required for water gas reaction and the mist of carbon monoxide, hydrogen is 20% to 30%, this kind of described mist can contain the carbon monoxide of 0.1vol% to 5vol% and the methane of 0.1vol% to 5vol% further, also comprises the steam of 0.1vol% to 5vol% in addition in pending gas.
According to kind and the performance of Hydrogen Separation film 1, the temperature of Hydrogen Separation film is in use 2000 DEG C to 6000 DEG C, can be maybe 3000 DEG C to 5000 DEG C, pressure in Hydrogen Separation film 1 is 0.1MPa to 5MPa, can be maybe 0.5Mpa to 4MPa, on the other hand, the pressure outside Hydrogen Separation film 1 is at least low 0.1MPa to 5MPa than the pressure in Hydrogen Separation film 1, or lower than 2MPa.
From realizing the high angle of organic efficiency, the region A(cm2 of the inner surface 1a of Hydrogen Separation film 1) be 0.05 or more with the ratio of amounts of hydrogen within the unit interval of the untreated mist of hydrogen, as 0.09 to 0.11.If the value of A/B is more than 0.11, the rate of recovery of hydrogen will reduce.This shows that the performance of assembly 10 is excessive relative to untreated gas.
In the flow path 9 of assembly 10, the flowing of untreated mist is laminar flow, under the high rate of recovery, obtain high-purity hydrogen.According to circumstances flow path flow path cross sectional area 9 is suitably set.
According to Hydrogen Separation method of the present invention, by thinking that flow path 9 carries pending mist to make pending mist flow along the inner surface of Hydrogen Separation film 1, fully the contacting of hydrogen molecule and Hydrogen Separation film 1 in mist in ensureing like this.
Although be explained in detail the present invention above, the present invention is not limited to above-mentioned requirement.Such as, although show in embodiment to be provided with a Hydrogen Separation film 1 in shell 5, but as Fig. 3 and Fig. 4, multiple Hydrogen Separation film 1 can be had to be mounted to (see figure 4) in shell 5, and insert 28 is embedded into the inside of each Hydrogen Separation film 1, insert 28 has the structure being similar to insert 8 in first embodiment, and extends to shut 2 on the upper end of Hydrogen Separation film 1, and the quantity being arranged on the Hydrogen Separation film 1 in shell 5 is not limit; In addition, according to the second embodiment, the structure of insert 28 can be identical with insert 18, or insert 28 is that insert 18 combines the structure formed mutually with insert 8.
In addition, the structure flowing into flow path 9 and 19 place from the far-end of insert 8 or 18 to shrouding 2 according to gas in the present invention has provided such as hereinafter about a preferred embodiment of the invention of Hydrogen Separation film 1 far-end.Such as, one may be made up of the far-end of Hydrogen Separation film 1 relative to Hydrogen Separation film 1 length direction providing the mouth of pipe of hydrogen.Therefore, untreated mist by flow path 9 or 19 formed spiral flow, from but hydrogen recovery rate reaches desired value.
In the present invention, Hydrogen Separation film can be used for both ends open, and the outer surface of Hydrogen Separation film inner surface and insert and the flow path that forms in device described in adopting.In addition, the rightabout to above-described embodiment flows by the direction of untreated mist, and the shape of hydrogen isolation component is not limited to cylindrical, and its cross section can also be rectangle or polygon.
It should be noted last that, above embodiment is only in order to illustrate technical scheme of the present invention and unrestricted.Although with reference to embodiment to invention has been detailed description, will be understood by those skilled in the art that, modify to technical scheme of the present invention or equivalent replacement, do not depart from the spirit and scope of technical solution of the present invention, it all should be encompassed in the middle of right of the present invention.
Claims (5)
1. a hydrogen separation device, it is characterized in that: described hydrogen separation device comprises outer surface, interior pipe, air shooter, gas flow paths, hydrogen separation membrane assembly, air supply opening, the gas discharge outlet of pipe in tubulose Hydrogen Separation film, the inner surface of Hydrogen Separation film, the outer surface of Hydrogen Separation film, shrouding, shell, hydrogen discharge, insert, insert, the described selectively permeable hydrogen of tubulose Hydrogen Separation film, described Hydrogen Separation film contains through hole; In the enclosure, described air supply opening can carry untreated gas to arrive film inside to described hydrogen discharge; Described gas discharge outlet can be carried can not through the gas of Hydrogen Separation film; Described hydrogen discharge can discharge the hydrogen of permeate through hydrogen gas diffusion barrier, and the through hole on described Hydrogen Separation film makes hydrogen molecule can penetrate into the another side of Hydrogen Separation film after contact Hydrogen Separation film.
2. a kind of hydrogen separation device according to claim 1, is characterized in that: described insert has a carrier pipe, and gas supply opening and outlet are shunted by air shooter.
3. according to claim 2 hydrogen separation device, it is characterized in that: the opening of described tubulose Hydrogen Separation film end is close to shut, and the outer surface of insert extends near shut.
4. a kind of hydrogen separation device according to claim 1, it is characterized in that: comprise the flow path that untreated mist is formed along tubulose Hydrogen Separation film and insert outer surface, further, the hydrogen in the untreated gas of hydrogen can through Hydrogen Separation film.
5. a kind of hydrogen separation device according to claim 4, is characterized in that: the adjacent shut of opening of the end of described tubular separation membrane, and insert outer surface extends near shut.
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CN201510512732.3A CN105056715A (en) | 2015-08-20 | 2015-08-20 | Hydrogen separation device |
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Cited By (2)
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CN110526211A (en) * | 2019-09-25 | 2019-12-03 | 浙江高成绿能科技有限公司 | A kind of portable chemical hydrogen generating system |
CN115138186A (en) * | 2022-06-29 | 2022-10-04 | 中国石油大学(华东) | Hydrogen separation device with spiral structure membrane module |
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