CN116059801B - Gas membrane separation device and gas selective separation method - Google Patents
Gas membrane separation device and gas selective separation method Download PDFInfo
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- CN116059801B CN116059801B CN202310035947.5A CN202310035947A CN116059801B CN 116059801 B CN116059801 B CN 116059801B CN 202310035947 A CN202310035947 A CN 202310035947A CN 116059801 B CN116059801 B CN 116059801B
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- 239000012528 membrane Substances 0.000 title claims abstract description 222
- 238000000926 separation method Methods 0.000 title claims abstract description 164
- 239000007789 gas Substances 0.000 claims abstract description 258
- 239000007788 liquid Substances 0.000 claims abstract description 53
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims abstract description 42
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims abstract description 42
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims abstract description 33
- 239000000654 additive Substances 0.000 claims abstract description 27
- LNTHITQWFMADLM-UHFFFAOYSA-N gallic acid Chemical compound OC(=O)C1=CC(O)=C(O)C(O)=C1 LNTHITQWFMADLM-UHFFFAOYSA-N 0.000 claims abstract description 24
- 239000001569 carbon dioxide Substances 0.000 claims abstract description 21
- 229910002092 carbon dioxide Inorganic materials 0.000 claims abstract description 21
- GUJOJGAPFQRJSV-UHFFFAOYSA-N dialuminum;dioxosilane;oxygen(2-);hydrate Chemical compound O.[O-2].[O-2].[O-2].[Al+3].[Al+3].O=[Si]=O.O=[Si]=O.O=[Si]=O.O=[Si]=O GUJOJGAPFQRJSV-UHFFFAOYSA-N 0.000 claims abstract description 20
- 229910052901 montmorillonite Inorganic materials 0.000 claims abstract description 20
- 230000000996 additive effect Effects 0.000 claims abstract description 18
- 239000001257 hydrogen Substances 0.000 claims abstract description 16
- 229910052739 hydrogen Inorganic materials 0.000 claims abstract description 16
- 229910052757 nitrogen Inorganic materials 0.000 claims abstract description 16
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 16
- 238000000034 method Methods 0.000 claims abstract description 15
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims abstract description 14
- 238000002360 preparation method Methods 0.000 claims abstract description 14
- 229940074391 gallic acid Drugs 0.000 claims abstract description 12
- 235000004515 gallic acid Nutrition 0.000 claims abstract description 12
- 239000007791 liquid phase Substances 0.000 claims abstract description 11
- 239000012466 permeate Substances 0.000 claims abstract description 10
- 238000001914 filtration Methods 0.000 claims description 16
- 238000011068 loading method Methods 0.000 claims description 14
- 238000002156 mixing Methods 0.000 claims description 8
- 239000011148 porous material Substances 0.000 claims description 6
- 238000007789 sealing Methods 0.000 claims description 4
- 238000001471 micro-filtration Methods 0.000 claims description 3
- 230000000052 comparative effect Effects 0.000 description 20
- 239000005431 greenhouse gas Substances 0.000 description 18
- 238000004891 communication Methods 0.000 description 12
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 description 9
- 229910052622 kaolinite Inorganic materials 0.000 description 8
- 229920002678 cellulose Polymers 0.000 description 5
- 238000001878 scanning electron micrograph Methods 0.000 description 4
- 238000001612 separation test Methods 0.000 description 4
- 239000006228 supernatant Substances 0.000 description 4
- 238000012360 testing method Methods 0.000 description 4
- 239000001913 cellulose Substances 0.000 description 3
- 150000002431 hydrogen Chemical class 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 238000010586 diagram Methods 0.000 description 2
- 238000000227 grinding Methods 0.000 description 2
- 239000012535 impurity Substances 0.000 description 2
- 229920001343 polytetrafluoroethylene Polymers 0.000 description 2
- 239000004810 polytetrafluoroethylene Substances 0.000 description 2
- 230000008569 process Effects 0.000 description 2
- 239000000047 product Substances 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 239000005995 Aluminium silicate Substances 0.000 description 1
- 239000000020 Nitrocellulose Substances 0.000 description 1
- 239000002033 PVDF binder Substances 0.000 description 1
- 206010040844 Skin exfoliation Diseases 0.000 description 1
- FJWGYAHXMCUOOM-QHOUIDNNSA-N [(2s,3r,4s,5r,6r)-2-[(2r,3r,4s,5r,6s)-4,5-dinitrooxy-2-(nitrooxymethyl)-6-[(2r,3r,4s,5r,6s)-4,5,6-trinitrooxy-2-(nitrooxymethyl)oxan-3-yl]oxyoxan-3-yl]oxy-3,5-dinitrooxy-6-(nitrooxymethyl)oxan-4-yl] nitrate Chemical compound O([C@@H]1O[C@@H]([C@H]([C@H](O[N+]([O-])=O)[C@H]1O[N+]([O-])=O)O[C@H]1[C@@H]([C@@H](O[N+]([O-])=O)[C@H](O[N+]([O-])=O)[C@@H](CO[N+]([O-])=O)O1)O[N+]([O-])=O)CO[N+](=O)[O-])[C@@H]1[C@@H](CO[N+]([O-])=O)O[C@@H](O[N+]([O-])=O)[C@H](O[N+]([O-])=O)[C@H]1O[N+]([O-])=O FJWGYAHXMCUOOM-QHOUIDNNSA-N 0.000 description 1
- 230000009471 action Effects 0.000 description 1
- 235000012211 aluminium silicate Nutrition 0.000 description 1
- 229920002301 cellulose acetate Polymers 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 239000003795 chemical substances by application Substances 0.000 description 1
- 230000008094 contradictory effect Effects 0.000 description 1
- 229910001873 dinitrogen Inorganic materials 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000012510 hollow fiber Substances 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 239000002440 industrial waste Substances 0.000 description 1
- 238000009434 installation Methods 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012544 monitoring process Methods 0.000 description 1
- 229920001220 nitrocellulos Polymers 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 239000013618 particulate matter Substances 0.000 description 1
- 239000012071 phase Substances 0.000 description 1
- -1 polytetrafluoroethylene Polymers 0.000 description 1
- 229920002981 polyvinylidene fluoride Polymers 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 238000009423 ventilation Methods 0.000 description 1
Classifications
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/22—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by diffusion
- B01D53/228—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by diffusion characterised by specific membranes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/22—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by diffusion
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D67/00—Processes specially adapted for manufacturing semi-permeable membranes for separation processes or apparatus
- B01D67/0081—After-treatment of organic or inorganic membranes
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B21/00—Nitrogen; Compounds thereof
- C01B21/04—Purification or separation of nitrogen
- C01B21/0405—Purification or separation processes
- C01B21/0433—Physical processing only
- C01B21/0438—Physical processing only by making use of membranes
- C01B21/0444—Physical processing only by making use of membranes characterised by the membrane
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
- C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
- C01B3/501—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by diffusion
- C01B3/503—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by diffusion characterised by the membrane
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/50—Carbon dioxide
-
- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07C—ACYCLIC OR CARBOCYCLIC COMPOUNDS
- C07C7/00—Purification; Separation; Use of additives
- C07C7/144—Purification; Separation; Use of additives using membranes, e.g. selective permeation
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
- B01D53/22—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by diffusion
- B01D2053/221—Devices
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2311/00—Details relating to membrane separation process operations and control
- B01D2311/12—Addition of chemical agents
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0405—Purification by membrane separation
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0465—Composition of the impurity
- C01B2203/0475—Composition of the impurity the impurity being carbon dioxide
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
- C01B2203/04—Integrated processes for the production of hydrogen or synthesis gas containing a purification step for the hydrogen or the synthesis gas
- C01B2203/0465—Composition of the impurity
- C01B2203/048—Composition of the impurity the impurity being an organic compound
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2210/00—Purification or separation of specific gases
- C01B2210/0043—Impurity removed
- C01B2210/0051—Carbon dioxide
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B2210/00—Purification or separation of specific gases
- C01B2210/0043—Impurity removed
- C01B2210/0068—Organic compounds
- C01B2210/007—Hydrocarbons
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
- Y02C20/00—Capture or disposal of greenhouse gases
- Y02C20/40—Capture or disposal of greenhouse gases of CO2
Landscapes
- Chemical & Material Sciences (AREA)
- Organic Chemistry (AREA)
- Engineering & Computer Science (AREA)
- Analytical Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Inorganic Chemistry (AREA)
- Oil, Petroleum & Natural Gas (AREA)
- General Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Combustion & Propulsion (AREA)
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- Separation Using Semi-Permeable Membranes (AREA)
Abstract
The invention provides a method for selectively separating gas, which comprises the following steps: s1, providing mixed gas; the mixed gas contains a first component and a second component; the first component comprises one or two of hydrogen and nitrogen, and the second component comprises one or two of methane and carbon dioxide; s2, introducing the mixed gas into a gas membrane separation device provided with a gas separation membrane, and enabling the mixed gas to permeate the gas separation membrane; the gas separation membrane is loaded with an additive, and the preparation method of the additive comprises the following steps: s21, dispersing montmorillonite and gallic acid in water together to obtain a liquid to be treated; s22, carrying out ultrasonic liquid phase stripping treatment on the liquid to be treated to obtain treated liquid; and S33, carrying out solid-liquid separation on the treated liquid to obtain the load liquid containing the additive.
Description
Technical Field
The present invention relates to gas separation, and more particularly, to a gas membrane separation apparatus and a method for selectively separating gas.
Background
Hydrogen, nitrogen, methane, carbon dioxide and the like are all common components in industrial waste gas; among them, methane and carbon dioxide belong to greenhouse gases, and the emission of a large amount of greenhouse gases may cause harm to the environment and climate.
Currently, there has been a great deal of research focusing on the separation of greenhouse gases. For example, chinese patent publication No. CN113577964a discloses a method for separating greenhouse gases from hollow fiber membrane materials based on PTFE/PVDF. However, although this patent performs separation of greenhouse gases, it only achieves separation of large-particle impurities from greenhouse gases, and does not achieve effective separation of greenhouse gases from other gases in the mixed gas, resulting in not high applicability of the above patent to mixed gases.
In view of the foregoing, it is desirable to provide a gas membrane separation device and a method for selectively separating gases, which solve or at least alleviate the above-mentioned technical drawbacks of not being able to effectively separate greenhouse gases from mixed gases.
Disclosure of Invention
The invention mainly aims to provide a gas membrane separation device and a gas selective separation method, and aims to solve the technical problem that greenhouse gases cannot be effectively separated from mixed gases.
To achieve the above object, the present invention provides a method for selectively separating gas, comprising the steps of:
s1, providing mixed gas;
The mixed gas contains a first component and a second component; the first component comprises one or two of hydrogen and nitrogen, and the second component comprises one or two of methane and carbon dioxide;
S2, introducing the mixed gas into a gas membrane separation device provided with a gas separation membrane, enabling the mixed gas to permeate the gas separation membrane, and intercepting the second component in the mixed gas so as to selectively separate the second component;
the gas separation membrane is loaded with an additive, and the preparation method of the additive comprises the following steps:
S21, mixing montmorillonite and gallic acid together into water to obtain a liquid to be treated;
The mass ratio of the montmorillonite to the gallic acid is 1:0.2-2, and the mass volume ratio of the montmorillonite to the water is 60-150mg:30mL;
s22, carrying out ultrasonic liquid phase stripping treatment on the liquid to be treated to obtain treated liquid;
And S33, carrying out solid-liquid separation on the treated liquid to obtain the load liquid containing the additive.
Further, the ultrasonic liquid phase peeling treatment includes: and stripping the liquid to be treated for 12-24 hours under the ultrasonic power of 300-500W.
Further, the preparation process of the gas separation membrane comprises the following steps: and (3) allowing the loading liquid to permeate through the microporous filtering membrane in a vacuum loading mode to obtain the gas separation membrane loaded with the additive.
Further, the volume of the loading liquid: the cross-sectional area of the microporous filtering membrane is 1-2mL, 1cm 2.
Further, the pore size of the microporous filtering membrane is 0.2um.
The invention also provides a gas membrane separation device for use in a method of effecting selective separation of a gas as described in any one of the preceding claims.
Further, the gas membrane separation device comprises at least one separation module comprising a housing and a membrane mounting assembly;
An air accommodating chamber is formed in the shell;
An air inlet communicated with the air accommodating cavity is formed in the air inlet end of the shell; the exhaust end of the shell is provided with a first exhaust port communicated with the air accommodating cavity; the gas collecting end of the shell is provided with a gas collecting port communicated with the gas accommodating cavity;
The membrane mounting assembly includes a membrane cover plate and the gas separation membrane;
the membrane cover plate is provided with a second exhaust port, and the second exhaust port and the first exhaust port form a gas exhaust channel; the gas separation membrane is fixed between the membrane cover plate and the exhaust end and is simultaneously in sealing arrangement with the membrane cover plate and the exhaust end; the gas separation membrane also covers both the first and second exhaust ports to selectively separate the gas entering the gas exhaust passage.
Further, the gas membrane separation device comprises a plurality of separation modules which are sequentially communicated, and the second exhaust ports and the air inlets of two adjacent separation modules are communicated.
Further, the membrane mounting assembly further comprises a first membrane clamp plate secured between the membrane cover plate and the gas separation membrane, and a second membrane clamp plate secured between the gas separation membrane and the exhaust end;
one side of the first membrane clamping plate is attached to the membrane cover plate, and the other side of the first membrane clamping plate is attached to the gas separation membrane;
One side of the second membrane clamping plate is attached to the gas separation membrane, and the other side of the second membrane clamping plate is attached to the exhaust end.
Further, the gas membrane separation device further comprises a gas collection pipeline, one end of the gas collection pipeline is communicated with the gas collecting port, the other end of the gas collection pipeline is communicated with an external container, and zigzag protrusions are distributed on the inner wall of the gas collection pipeline.
Compared with the prior art, the invention has at least the following advantages:
according to the invention, non-greenhouse gases (hydrogen and nitrogen) and greenhouse gases (methane and carbon dioxide) can be selectively separated, so that the purity of the hydrogen and the nitrogen can be improved on the basis of recovering the methane and the carbon dioxide, and the utilization rate of the hydrogen and the nitrogen can be improved. Specifically, the practical research of the invention shows that the additive based on montmorillonite, gallic acid and water does not retain hydrogen and nitrogen, but only retains methane and carbon dioxide, thereby providing a guarantee for the gas selectivity of the invention, being capable of separating greenhouse gases from mixed gases and having great application value.
Drawings
In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings that are required in the embodiments or the description of the prior art will be briefly described, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and other drawings may be obtained according to the structures shown in these drawings without inventive effort for a person skilled in the art.
FIG. 1 is a schematic view of a gas membrane separation device having three separation modules according to the present invention;
FIG. 2 is a schematic view showing the structure of a gas membrane separation device in example 1 and comparative examples 1 to 3 of the present invention when not installed;
FIG. 3 is an SEM image of the montmorillonite after grinding in example 1 and comparative examples 1-3 of the present invention;
FIG. 4 is an SEM image of the kaolin after grinding in example 1 and comparative examples 1-3 of the present invention.
Reference numerals: 1. a housing; 2. a membrane mounting assembly; 3. an air inlet; 4. a first exhaust port; 5. a membrane cover plate; 6. a gas separation membrane; 7. a second exhaust port; 8. a first membrane splint; 9. a second membrane splint; 10. a communication port; 11. a gas collection line; 12. and a gas pipeline.
The achievement of the object, functional features and advantages of the present invention will be further described with reference to the drawings in connection with the embodiments.
Detailed Description
The following description of the embodiments of the present invention will be made clearly and fully with reference to the accompanying drawings, in which it is evident that the embodiments described are only some, but not all embodiments of the invention. All other embodiments, based on the embodiments of the invention, which are apparent to those of ordinary skill in the art without inventive faculty, are intended to be within the scope of the invention.
Moreover, the technical solutions of the embodiments of the present invention may be combined with each other, but it is necessary to be based on the fact that those skilled in the art can implement the embodiments, and when the technical solutions are contradictory or cannot be implemented, it should be considered that the combination of the technical solutions does not exist, and is not within the scope of protection claimed by the present invention.
It should be understood that gas membrane separation is a process of separating components by using differences in permeation rates of the components in a gas mixture in the gas separation membrane 6 under the action of a pressure difference as a pushing force. The gas membrane separation technology has the characteristics of no phase change in separation operation and no addition of separating agent. The key to the gas membrane separation process is the membrane material, and the ideal gas separation membrane 6 material should be selective for a particular type of gas.
In order to selectively separate methane and carbon dioxide, the present invention provides a gas selective separation method, which can be understood as a method for selectively separating methane and carbon dioxide gas, comprising the steps of:
S1, providing mixed gas.
The mixed gas contains a first component and a second component or consists of the first component and the second component.
The first component comprises or is one or two of hydrogen and nitrogen, and the second component comprises or is one or two of methane gas and carbon dioxide gas.
And S2, introducing the mixed gas into a gas membrane separation device provided with a gas separation membrane 6, enabling the mixed gas to permeate (partially permeate) the gas separation membrane 6, and intercepting all or part of the second component in the mixed gas so as to selectively separate the second component.
That is, the second component may be totally or partially trapped during the permeation of the mixed gas through the gas separation membrane 6, and may not permeate the gas separation membrane 6, thereby being separated from other gases that permeate the gas separation membrane 6.
In order to achieve selective separation of methane gas and carbon dioxide gas, it is necessary to load an additive on the gas separation membrane 6, the additive preparation method comprising the steps of:
S21, mixing montmorillonite and gallic acid together into water to obtain the liquid to be treated.
The mass ratio of the montmorillonite to the gallic acid is 1:0.2-2, and the mass volume ratio of the montmorillonite to the water is 60-150mg:30mL.
S22, carrying out ultrasonic liquid phase stripping treatment on the liquid to be treated to obtain treated liquid.
The ultrasonic liquid phase stripping treatment may include or be: and stripping the liquid to be treated for 12-24 hours under the ultrasonic power of 300-500W.
S33, carrying out solid-liquid separation on the treated liquid to obtain a load liquid containing the additive; wherein, the solid-liquid separation mode can be standing.
As a preferred way, the process for preparing the gas separation membrane 6 may comprise or be: and allowing the loading liquid to permeate through the microporous filtering membrane in a vacuum loading mode, so that the additive is loaded on the microporous filtering membrane, and the gas separation membrane 6 loaded with the additive is obtained.
Specifically, the microporous filtering membrane is placed at the bottom of the loading liquid, and then a vacuum pump is used to vacuumize (under a closed condition) from the lower part of the microporous filtering membrane, so that the loading liquid penetrates through the microporous filtering membrane from top to bottom, and the additives in the loading liquid are loaded in the microporous filtering membrane.
In carrying out the loading, the volume of the loading liquid: the cross-sectional area of the microporous filtration membrane can be 1-2mL:1cm 2. The cross-sectional area of the microporous filtering membrane is the ventilation surface area of the microporous filtering membrane. Illustratively, the cross-section of the microfiltration membrane may be a circular face, which may be 50mm in diameter; the pore size of the microfiltration membrane may be 0.2um.
The microporous filtering Membrane is a Mixed Cellulose (MCE) Membrane (Mixed Cellulose Ester (MCE) Membrane) which is derived from Tianjin Jiuteng laboratory equipment Co., ltd; it should be appreciated by those skilled in the art that Mixed Cellulose (MCE) films are common aqueous films, which are formed by mixing cellulose nitrate and cellulose acetate.
Referring to fig. 1-2, the present invention also provides a gas membrane separation device for use in a method of effecting selective separation of a gas as described in any of the above embodiments.
In particular, the gas membrane separation device may comprise at least one separation module comprising a housing 1 and a membrane mounting assembly 2.
The inside of the shell 1 is provided with a gas containing cavity which is isolated from the outside.
An air inlet 3 communicated with the air accommodating cavity is formed in the air inlet end of the shell 1; the exhaust end of the shell 1 is provided with a first exhaust port 4 communicated with the air accommodating cavity; the gas collecting end of the shell 1 is provided with a gas collecting port communicated with the gas containing cavity.
The air inlet end of the casing 1 and the air outlet end of the casing 1 may be side ends, and the air inlet end of the casing 1 and the air outlet end of the casing 1 may be disposed opposite to each other; the gas collecting end of the housing 1 may be an upper end of the housing 1.
The membrane mounting assembly 2 comprises a membrane cover plate 5 and the gas separation membrane 6.
The membrane cover plate 5 is provided with a second exhaust port 7, and the second exhaust port 7 and the first exhaust port 4 form a gas exhaust channel. The gas separation membrane 6 is fixed between the membrane cover plate 5 and the exhaust end and is arranged in a sealing way with the membrane cover plate 5 and the exhaust end; that is, there is no gap for gas to escape between the gas separation membrane 6 and the end face of the membrane cover 5, and there is no gap for gas to escape between the gas separation membrane 6 and the end face of the exhaust end. The gas separation membrane 6 also covers both the first gas outlet 4 and the second gas outlet 7 to selectively separate the gas entering the gas outlet passage.
In order to enhance the sealability of the gas separation membrane 6 and protect the gas separation membrane 6, the membrane mounting assembly 2 may further include a first membrane clamping plate 8 fixed between the membrane cover plate 5 and the gas separation membrane 6, and a second membrane clamping plate 9 fixed between the gas separation membrane 6 and the exhaust end; the membrane splint in the invention can be made of polytetrafluoroethylene.
The first membrane clamping plate 8 and the second membrane clamping plate 9 are respectively provided with a communication port 10, and can be specifically arranged in the middle of the membrane clamping plate. The communication ports 10 of the first membrane holder plate 8 and the second membrane holder plate 9 are part of the gas discharge passage, and do not block the flow of gas in the gas discharge passage. Illustratively, the dimensions of the communication ports 10 of the first vent port 4, the first membrane clamping plate 8, and the second membrane clamping plate 9, and the second vent port 7 may be identical and, after installation, mutually coincide.
Illustratively, the communication ports 10 of the first vent port 4, the first membrane clamping plate 8, and the second membrane clamping plate 9, the second vent port 7, and the gas separation membrane 6 may all be circular; the size of the gas separation membrane 6 is larger than the sizes of the first gas outlet 4, the communication ports 10 of the first membrane clamping plate 8 and the second membrane clamping plate 9, and the second gas outlet 7; the first exhaust port 4, the communication ports 10 of the first and second membrane clamping plates 8 and 9, and the second exhaust port 7 may be the same size.
In order to ensure air tightness, one side of the first membrane clamping plate 8 is attached to the membrane cover plate 5, and the other side of the first membrane clamping plate 8 is attached to the gas separation membrane 6. One side of the second membrane clamping plate 9 is attached to the gas separation membrane 6, and the other side of the second membrane clamping plate 9 is attached to the exhaust end.
In order to facilitate the input of the mixed gas, the gas inlet 3 of the separation module is communicated with a gas supply device, the gas supply device provides the mixed gas to the gas accommodating chamber of the separation module, and a gas flowmeter can be arranged in the gas supply device so as to monitor the flow of the mixed gas. When the number of the separation modules is plural, only the air inlet 3 of the first separation module is provided in communication with the air supply device.
In order to realize the collection of methane and carbon dioxide, the gas membrane separation device further comprises a gas collection pipeline 11, wherein one end of the gas collection pipeline 11 is communicated with the gas collection port, and the other end of the gas collection pipeline 11 is communicated with an external container; the gas collecting pipeline 11 is provided with a valve body for controlling the gas flow so as to ensure the normal operation of gas separation, and the pressure of the gas accommodating cavity can be relieved when the air pressure is too high.
In order to reduce particulate matter and other impurities in the recovered gas, the inner wall of the gas collection pipe 11 may have a plurality of zigzag protrusions.
In order to facilitate the improvement of the separation rate of methane and carbon dioxide in a certain period of time, the gas membrane separation device comprises a plurality of separation modules (connected in series) which are sequentially communicated, and the second exhaust ports 7 and the air inlets 3 of two adjacent separation modules are communicated. That is, the second exhaust port 7 of the last separation module may be provided in communication with the intake port 3 of the next separation module. For example, referring to fig. 1, the separation modules may be three.
The second exhaust ports 7 and the air inlets 3 of two adjacent separation modules can be specifically communicated through air pipelines 12, and each air pipeline 12 can be provided with an air pressure monitoring meter. Through the arrangement of a plurality of separation modules in a sequential communication mode, the pressure difference of two sides of the gas separation membrane 6 can be reduced, and therefore the service life of the gas separation membrane 6 is prolonged.
To facilitate a detailed understanding of the invention by those skilled in the art, reference will now be made to the accompanying drawings, in which:
example 1
1. Preparation of additives (montmorillonite + water + gallic acid):
Mixing 60mg montmorillonite and 60mg gallic acid into 30mL water; wherein, the SEM diagram of montmorillonite is shown in figure 3, the montmorillonite is ground by a grinder before use, and sieved by a 60-mesh screen, and the undersize product is taken.
After ultrasonic liquid phase stripping for 16 hours under the condition of 400W ultrasonic power, solid-liquid separation is carried out by adopting a mode of standing for 20min, and supernatant is taken as load liquid containing additives.
2. Preparation of gas separation membrane 6:
All the loading liquid is filtered by a vacuum pump, and the additive in the loading liquid is loaded in the micro-pore filter membrane through the micro-pore filter membrane, and the gas separation membrane 6.
Wherein the microporous filtering Membrane is a Mixed Cellulose (MCE) Membrane (Mixed Cellulose Ester (MCE) Membrane, has a pore size of 0.2um, a diameter of 50mm, and a round shape, and is from Tianjin Jiuteng laboratory equipment Co., ltd.
3. Assembling a gas membrane separation device:
Referring to fig. 2, the gas membrane separation apparatus has a separation module including a housing 1 and a membrane mounting assembly 2.
The housing 1 has an air chamber formed therein.
An air inlet 3 communicated with the air accommodating cavity is formed in the air inlet end of the shell 1, and the air inlet 3 is also communicated with the air supply device so as to receive mixed gas to be treated; the exhaust end of the shell 1 is provided with a first exhaust port 4 communicated with the air accommodating cavity; the gas collecting end of the shell 1 is provided with a gas collecting port communicated with the gas containing cavity. The air inlet end and the air outlet end are both side ends and are oppositely arranged; the gas collecting end is the upper end;
the membrane mounting assembly 2 includes a membrane cover plate 5 and a gas separation membrane 6 prepared in this embodiment.
The membrane cover plate 5 is provided with a second exhaust port 7, and the second exhaust port 7 and the first exhaust port 4 form a gas exhaust channel; the gas separation membrane 6 is fixed between the membrane cover plate 5 and the exhaust end and is arranged in a sealing way with the membrane cover plate 5 and the exhaust end; the gas separation membrane 6 also covers both the first gas outlet 4 and the second gas outlet 7 to selectively separate the gas entering the gas outlet passage.
The membrane mounting assembly 2 further comprises a first membrane clamping plate 8 fixed between the membrane cover plate 5 and the gas separation membrane 6, and a second membrane clamping plate 9 fixed between the gas separation membrane 6 and the exhaust end.
One side of the first membrane clamping plate 8 is attached to the membrane cover plate 5, and the other side of the first membrane clamping plate 8 is attached to the gas separation membrane 6; one side of the second membrane clamping plate 9 is attached to the gas separation membrane 6, and the other side of the second membrane clamping plate 9 is attached to the exhaust end. The first membrane clamping plate 8 and the second membrane clamping plate 9 are respectively provided with a communication port 10, and the communication ports 10 of the first membrane clamping plate 8 and the second membrane clamping plate 9 are all part of a gas discharge channel, so that the flow of gas in the gas discharge channel is not blocked.
4. Separation test of mixed gas:
The gas membrane separation device assembled by the embodiment is adopted to separate the mixed gas, and specifically comprises the following components:
Introducing mixed gas into the gas containing chamber, wherein the mixed gas consists of hydrogen, nitrogen, methane and carbon dioxide, and the volume contents of the hydrogen, the nitrogen, the methane and the carbon dioxide in the mixed gas are 5.05%, 85.08%, 4.91% and 4.96% respectively; the mixed gas enters the gas containing cavity from the gas inlet 3 of the separation module, the flow is 40mL/min, and the introducing duration of the mixed gas is 60min.
During the introduction of the mixed gas, the gas flowing out of the gas collecting port (trapped gas) and the gas flowing out of the second gas discharging port (gas passing through the gas separation membrane 6) are collected.
Test results:
in this example, the rejection rate of hydrogen gas was 0%, the rejection rate of nitrogen gas was 0%, the rejection rate of methane was 16.62%, and the rejection rate of carbon dioxide was 39.82%, so that greenhouse gases could be selectively trapped. In the practical application process, a plurality of separation modules which are communicated in sequence can be arranged for further improving the separation efficiency of methane and carbon dioxide, so that the mixed gas is simultaneously trapped for a plurality of times.
Comparative example 1
1. Preparation of additives (montmorillonite + water):
mixing 60mg of montmorillonite into 30mL of water; wherein, the SEM diagram of montmorillonite is shown in figure 3, the montmorillonite is ground by a grinder before use, and sieved by a 60-mesh screen, and the undersize product is taken.
After ultrasonic liquid phase stripping for 16 hours under the condition of 400W ultrasonic power, solid-liquid separation is carried out by adopting a mode of standing for 20min, and supernatant is taken as load liquid containing additives.
2. Preparation of gas separation membrane 6:
Other conditions were the same as in example 1 except that the supporting liquid was replaced with the supporting liquid prepared in this comparative example as in example 1.
3. Assembling a gas membrane separation device:
Other conditions were the same as in example 1 except that the gas separation membrane 6 was replaced with the gas separation membrane 6 prepared in this comparative example as compared with example 1.
4. Separation test of mixed gas:
In comparison with example 1, only the gas membrane separation device was replaced with the gas membrane separation device assembled in this comparative example, and other conditions were the same as those in example 1.
Test results:
The comparative example has a hydrogen rejection rate of 31.64%, a nitrogen rejection rate of 6.9%, a methane rejection rate of 31.87%, a carbon dioxide rejection rate of 59.68%, and a low applicability, and cannot selectively reject greenhouse gases.
Comparative example 2
1. Preparation of additives (kaolinite+water+gallic acid):
Mixing 60mg of kaolinite and 60mg of gallic acid into 30mL of water; wherein, the SEM image of the kaolinite is shown in FIG. 4, the kaolinite is ground by a grinder before use, and sieved by a 60-mesh sieve, and the undersize is taken.
After ultrasonic liquid phase stripping for 16 hours under the condition of 400W ultrasonic power, solid-liquid separation is carried out by adopting a mode of standing for 20min, and supernatant is taken as load liquid containing additives.
2. Preparation of gas separation membrane 6:
Other conditions were the same as in example 1 except that the supporting liquid was replaced with the supporting liquid prepared in this comparative example as in example 1.
3. Assembling a gas membrane separation device:
Other conditions were the same as in example 1 except that the gas separation membrane 6 was replaced with the gas separation membrane 6 prepared in this comparative example as compared with example 1.
4. Separation test of mixed gas:
In comparison with example 1, only the gas membrane separation device was replaced with the gas membrane separation device assembled in this comparative example, and other conditions were the same as those in example 1.
Test results:
The comparative example has a hydrogen rejection rate of 10.66%, a nitrogen rejection rate of 0%, a methane rejection rate of 22.45%, a carbon dioxide rejection rate of 14.65%, and a low applicability, and cannot selectively reject greenhouse gases.
Comparative example 3
1. Preparation of additives (kaolinite+water):
Mixing 60mg of kaolinite into 30mL of water; wherein, the SEM image of the kaolinite is shown in FIG. 4, the kaolinite is ground by a grinder before use, and sieved by a 60-mesh sieve, and the undersize is taken.
After ultrasonic liquid phase stripping for 16 hours under the condition of 400W ultrasonic power, solid-liquid separation is carried out by adopting a mode of standing for 20min, and supernatant is taken as load liquid containing additives.
2. Preparation of gas separation membrane 6:
Other conditions were the same as in example 1 except that the supporting liquid was replaced with the supporting liquid prepared in this comparative example as in example 1.
3. Assembling a gas membrane separation device:
Other conditions were the same as in example 1 except that the gas separation membrane 6 was replaced with the gas separation membrane 6 prepared in this comparative example as compared with example 1.
4. Separation test of mixed gas:
In comparison with example 1, only the gas membrane separation device was replaced with the gas membrane separation device assembled in this comparative example, and other conditions were the same as those in example 1.
Test results:
The comparative example has a hydrogen rejection rate of 1.79%, a nitrogen rejection rate of 1.46%, a methane rejection rate of 0%, and a carbon dioxide rejection rate of 0%; although the comparative example can selectively intercept non-greenhouse gases, only partial hydrogen and nitrogen are intercepted, the greenhouse gases can be doped with hydrogen and nitrogen, the comparative example has low interception rate of the non-greenhouse gases, and the applicability is not high.
In the above technical solution of the present invention, the above is only a preferred embodiment of the present invention, and therefore, the patent scope of the present invention is not limited thereto, and all the equivalent structural changes made by the description of the present invention and the content of the accompanying drawings or the direct/indirect application in other related technical fields are included in the patent protection scope of the present invention.
Claims (9)
1. A method for the selective separation of gases, comprising the steps of:
s1, providing mixed gas;
The mixed gas contains a first component and a second component; the first component comprises one or two of hydrogen and nitrogen, and the second component comprises one or two of methane and carbon dioxide;
S2, introducing the mixed gas into a gas membrane separation device provided with a gas separation membrane, enabling the mixed gas to permeate the gas separation membrane, and intercepting the second component in the mixed gas so as to selectively separate the second component;
the gas separation membrane is loaded with an additive, and the preparation method of the additive comprises the following steps:
S21, mixing montmorillonite and gallic acid together into water to obtain a liquid to be treated;
The mass ratio of the montmorillonite to the gallic acid is 1:0.2-2, and the mass volume ratio of the montmorillonite to the water is 60-150 mg:30 mL;
s22, carrying out ultrasonic liquid phase stripping treatment on the liquid to be treated to obtain treated liquid;
s33, carrying out solid-liquid separation on the treated liquid to obtain a load liquid containing the additive;
The preparation process of the gas separation membrane comprises the following steps: and (3) allowing the loading liquid to permeate through the microporous filtering membrane in a vacuum loading mode to obtain the gas separation membrane loaded with the additive.
2. The method of gas-selective separation of claim 1, wherein the ultrasonic liquid phase stripping treatment comprises: and stripping the liquid to be treated under the ultrasonic power of 300-500W by 12-24 h.
3. The method of gas selective separation according to claim 1, wherein the volume of the carrier liquid: the cross-sectional area of the microporous filtering membrane is 1-2 mL:1 cm 2.
4. The method of claim 1, wherein the pore size of the microfiltration membrane is 0.2 um.
5. A gas membrane separation device for carrying out the method of selective separation of a gas according to any one of claims 1 to 4.
6. The gas membrane separation device of claim 5, wherein the gas membrane separation device comprises at least one separation module comprising a housing and a membrane mounting assembly;
An air accommodating chamber is formed in the shell;
An air inlet communicated with the air accommodating cavity is formed in the air inlet end of the shell; the exhaust end of the shell is provided with a first exhaust port communicated with the air accommodating cavity; the gas collecting end of the shell is provided with a gas collecting port communicated with the gas accommodating cavity;
The membrane mounting assembly includes a membrane cover plate and the gas separation membrane;
the membrane cover plate is provided with a second exhaust port, and the second exhaust port and the first exhaust port form a gas exhaust channel; the gas separation membrane is fixed between the membrane cover plate and the exhaust end and is simultaneously in sealing arrangement with the membrane cover plate and the exhaust end; the gas separation membrane also covers both the first and second exhaust ports to selectively separate the gas entering the gas exhaust passage.
7. The gas membrane separation device according to claim 6, wherein the gas membrane separation device comprises a plurality of separation modules which are sequentially communicated, and the second exhaust ports and the gas inlets of two adjacent separation modules are communicated.
8. The gas membrane separation device of claim 6, wherein the membrane mounting assembly further comprises a first membrane clamp plate secured between the membrane cover plate and the gas separation membrane, and a second membrane clamp plate secured between the gas separation membrane and the gas discharge end;
one side of the first membrane clamping plate is attached to the membrane cover plate, and the other side of the first membrane clamping plate is attached to the gas separation membrane;
One side of the second membrane clamping plate is attached to the gas separation membrane, and the other side of the second membrane clamping plate is attached to the exhaust end.
9. The gas membrane separation device according to any one of claims 6 to 8, further comprising a gas collecting pipe, wherein one end of the gas collecting pipe is communicated with the gas collecting port, the other end of the gas collecting pipe is communicated with an external container, and zigzag protrusions are distributed on the inner wall of the gas collecting pipe.
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| WO2005007725A1 (en) * | 2003-07-11 | 2005-01-27 | Pemeas Gmbh | Asymmetric polymer film, method for the production and the utilization thereof |
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