CN109621647A - A kind of method of separation and concentration carbon dioxide - Google Patents
A kind of method of separation and concentration carbon dioxide Download PDFInfo
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- CN109621647A CN109621647A CN201910037721.2A CN201910037721A CN109621647A CN 109621647 A CN109621647 A CN 109621647A CN 201910037721 A CN201910037721 A CN 201910037721A CN 109621647 A CN109621647 A CN 109621647A
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- 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
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- 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
- B01D53/32—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 electrical effects other than those provided for in group B01D61/00
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- 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
- B01D67/0079—Manufacture of membranes comprising organic and inorganic components
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
- B01D69/02—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor characterised by their properties
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D71/00—Semi-permeable membranes for separation processes or apparatus characterised by the material; Manufacturing processes specially adapted therefor
- B01D71/02—Inorganic material
- B01D71/021—Carbon
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D71/00—Semi-permeable membranes for separation processes or apparatus characterised by the material; Manufacturing processes specially adapted therefor
- B01D71/06—Organic material
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2256/00—Main component in the product gas stream after treatment
- B01D2256/22—Carbon dioxide
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2257/00—Components to be removed
- B01D2257/50—Carbon oxides
- B01D2257/504—Carbon dioxide
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- 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
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- 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
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Abstract
The present invention relates to gas separation technique fields, disclose a kind of method of separation and concentration carbon dioxide, it include: that separation and concentration is carried out to the mixed gas containing carbon dioxide using ionic liquid/two-dimensional slice material gas seperation film under 20~100 DEG C, 0.01~0.2MPa pressure, the current field condition that intensity is -7.5~7.5V/mm;Ionic liquid/two-dimensional slice material gas seperation film preparation method includes: that (1) disperses two-dimensional slice material to obtain two-dimensional slice material dispersion liquid in deionized water, two-dimensional slice material dispersion liquid is filtered onto perforated substrate by vacuum filtration, obtains two-dimensional slice material membrane;(2) ionic liquid is coated on to the two-dimensional slice material film surface, is kept for 1~8 hour in the case where being not less than 50KPa negative pressure, obtains ionic liquid/two-dimensional slice material gas seperation film.Method of the invention is by applying electric field to ionic liquid/two-dimensional slice material gas seperation film, so that ionic liquid/two-dimensional slice material gas seperation film has very excellent gas separating capacity.
Description
Technical field
The present invention relates to gas separation technique field more particularly to a kind of methods of separation and concentration carbon dioxide.
Background technique
The principle of gas separation membrane separation gas is mainly based upon transmission rate difference of the gas with various in film, usually may be used
It is divided into micropore flooding mechanism and dissolution flooding mechanism.Micropore flooding mechanism is mainly the hole or stratified material for utilizing porous material
Channel sieved;Dissolution flooding mechanism is then to have different solubilities to gas with various using such as some high molecular materials
It separates and is enriched with the characteristic of diffusion coefficient.
Membrane separation technique is in reply currently due to CO2Based on greenhouse gases a large amount of discharges caused by greenhouse effects etc.
Climate change bring negative effect aspect has very high utility value, has the advantages such as environmental protection, low energy consumption.It develops novel
Energy-efficient seperation film becomes important research direction.
Thin polymer film puts it into commercial operation already as gas separation membrane, but flux possessed by thin polymer film is low, stablizes
The disadvantages of property is poor significantly limits its application.And two-dimensional layer material such as graphene, graphene oxide etc., there is unique receive
Meter level channel makes gas separation membrane have new possibility in gas separation field.Graphene oxide has unique two-dimensional structure
With mature preparation process, the graphene oxide film as made of graphene oxide layer rule stacking has in multiple fields
Very big application potential, such as water process, electrochemistry, catalysis, gas separation etc..But in gas separation field, pure oxidation stone
The black thin membrane separation efficiency of alkene is far from reaching can be with the stage of practical application, it is therefore desirable to be modified.
Ionic liquid is a kind of salt being in a liquid state at room temperature, has steam forces down, thermal stability and chemical stability are good etc.
Advantage, and have very high solubility to carbon dioxide, therefore can be used to separate and carbon dioxide-enriched.But it is ionic liquid is straight
It connects for using that there are significant limitations, therefore usually ionic liquid is filled in porous media, composite membrane is made to make
With.
Under simple pressure difference driving, gas separation membrane to the separation and concentration efficiency of carbon dioxide in gas mixture still
It is to be improved.
Summary of the invention
The present invention provides a kind of methods of separation and concentration carbon dioxide, to the separating capacity and separative efficiency of carbon dioxide
It is higher.
Specific technical solution is as follows:
A kind of method of separation and concentration carbon dioxide, comprising:
Under 20~100 DEG C, 0.01~0.2MPa pressure, the current field condition that intensity is -7.5~7.5V/mm, using ion
Liquid/two-dimensional slice material gas seperation film carries out separation and concentration to the mixed gas containing carbon dioxide;
The ionic liquid/two-dimensional slice material gas seperation film preparation method includes:
(1) dispersion of two-dimensional slice material is obtained into two-dimensional slice material dispersion liquid in deionized water, passes through vacuum filtration
Two-dimensional slice material dispersion liquid is filtered onto perforated substrate, two-dimensional slice material membrane is obtained;
(2) ionic liquid is coated on to the two-dimensional slice material film surface, keeps 1 in the case where being not less than 50KPa negative pressure
~8 hours, obtain ionic liquid/two-dimensional slice material gas seperation film.
The two-dimensional slice material in two-dimensional slice material aqueous solution is filtered to perforated substrate in the way of vacuum filtration
On, the two-dimensional slice material film with regular layer structure is obtained, interlamellar spacing is at 1 nanometer or less in the film;By ionic liquid
After body is coated on two-dimensional slice material film surface, ionic liquid will receive the effect of capillary force, gradually penetrate into two-dimensional slice
Between the lamella of layer material film, and it is eventually restricted from wherein.
Compared to hydrogen, methane and nitrogen, ionic liquid has higher solubility to carbon dioxide, adds two-dimensional slice
The confinement of layer material nano pore acts on, and ionic liquid/two-dimensional slice material gas seperation film at this time has had preferably
Separating capacity, under the further effect of electric field, structure of the ionic liquid between two-dimensional slice material can be changed, thus
Change ionic liquid to the solubility and diffusion coefficient of gas.Under the action of electric field, ionic liquid/two-dimensional slice material gas
Seperation film is higher to the separative efficiency of carbon dioxide gas.In addition, by the electric field for applying varying strength, adjustable ionic liquid
Changes in distribution of the zwitterion of body between two-dimensional slice material, so as to reconcile ionic liquid/two-dimensional slice material gas
The separating property of seperation film.
In the present invention, the applying mode of electric field are as follows: in the ionic liquid/two-dimensional slice material gas seperation film two sides
Piece of metal capacitance sheet is respectively set, applies DC voltage in two panels metal capacitance on piece.
Preferably, the mixed gas containing carbon dioxide be in carbon dioxide and hydrogen, methane and nitrogen at least
A kind of gaseous mixture.
Flux difference of the ionic liquid/two-dimensional slice material gas seperation film to carbon dioxide and hydrogen, methane and nitrogen
Larger, the mixed gas containing carbon dioxide is the mixed of at least one of carbon dioxide and hydrogen, methane and nitrogen
When closing gas, ionic liquid/two-dimensional slice material gas seperation film is more efficient to the separation and concentration of carbon dioxide.
Preferably, in the two-dimensional slice material dispersion liquid, the mass percent concentration of two-dimensional slice material is 0.02
~0.2%.
Preferably, the two-dimensional slice material is at least one of graphene oxide, molybdenum disulfide and tungsten disulfide;
It is further preferred that the two-dimensional slice material is graphene oxide.Graphene oxide has unique Nanoscale channels, tool
There is preferable selectivity.
Preferably, the ionic liquid is 1- butyl -3- methyl imidazolium tetrafluoroborate ([BMIM] [BF4]).It should be from
Sub- liquid is higher to the selectivity of carbon dioxide, and cost is relatively low.
As film thickness increases, the flux of gas is declined, but the segregation ratio of carbon dioxide is risen, but works as film thickness
After reaching certain thickness, flux and segregation ratio are basically unchanged.The content of film intermediate ion liquid is higher, and flux can be declined, but
The segregation ratio of carbon dioxide will increase.
Preferably, the ionic liquid/two-dimensional slice material gas seperation film is with a thickness of 50~1500nm;Ionic liquid
In body/two-dimensional slice material gas seperation film, the mass percent of ionic liquid is 50~80%.
Preferably, the perforated substrate is polycarbonate perforated membrane or inorganic oxide aluminium perforated membrane.Polycarbonate is porous
Film or inorganic oxide aluminium perforated membrane mechanical strength are big, can provide more stable branch for ionic liquid/two-dimensional slice Material cladding layer
Support.
Compared with prior art, the invention has the benefit that
(1) in ionic liquid/two-dimensional slice material gas seperation film, using two-dimensional slice material as support substrate, have
Good stability, while ionic liquid can be limited in the layer gap of two-dimensional slice material, the ionic liquid under confinement is compared
The ionic liquid of liquid phase has certain raising to the separating property of gas;
(2) change distribution of the zwitterion between two-dimensional slice material of ionic liquid by electric field, thus change from
Sub- liquid enhances ionic liquid/two-dimensional slice material gas seperation film to carbon dioxide to the solubility and diffusion coefficient of gas
Separation and concentration ability so that ionic liquid/two-dimensional slice material gas seperation film have very excellent gas separating capacity.
Detailed description of the invention
Fig. 1 is the scanning electron microscope (SEM) photograph of graphene oxide film prepared by embodiment 1, wherein (a) is surface scan electron microscope,
It (b) is profile scanning electron microscope;
Fig. 2 is ionic liquid/graphene oxide film scanning electron microscope (SEM) photograph prepared by embodiment 1, wherein (a) sweeps for surface
Electron microscope is retouched, (b) is profile scanning electron microscope;
Fig. 3 is ionic liquid/graphene oxide film scanning electron microscope (SEM) photograph prepared by embodiment 4, wherein (a) sweeps for surface
Electron microscope is retouched, (b) is profile scanning electron microscope.
Specific embodiment
Embodiment 1
(1) at room temperature, the graphene oxide water solution that configuration graphene oxide mass percent concentration is 0.02%, will
0.5ml solution filters under 85KPa negative pressure to inorganic oxide aluminium perforated membrane, and the diameter of film is 25mm, aperture 200nm, is made
The graphene oxide film of 76nm thickness;
As shown in Figure 1, there are elongated fold, the well-regulated layer structure of section in graphene oxide film surface.
(2) then, 0.05ml [BMIM] [BF is coated on graphene oxide film surface4], it is maintained at 2 under 50KPa negative pressure
Hour, [BMIM] [BF of 170nm thickness is made4]/graphene oxide gas separation membrane, wherein graphene oxide and [BMIM] [BF4]
Mass ratio be 0.39.
As shown in Figure 2.After having added ionic liquid, the fold on graphene oxide film surface becomes short and thick, section
Layer structure also disappears, and film thickness significantly increases.
Room temperature, 0.06MPa pressure, intensity be -2.5V/mm current field condition under, measure the seperation film to carbon dioxide,
The flux of hydrogen, methane and nitrogen obtains the flux of carbon dioxide and hydrogen, carbon dioxide and methane, carbon dioxide and nitrogen
Ratio is respectively 14,67,85.
Comparative example 1
Under conditions of room temperature, 0.06MPa pressure, [BMIM] [BF made from embodiment 1 is measured4]/graphene oxide gas
Body seperation film obtains carbon dioxide and hydrogen, carbon dioxide and methane, two to the flux of carbon dioxide, hydrogen, methane and nitrogen
The flux ratio of carbonoxide and nitrogen is respectively 12,39,66.
Embodiment 2
Under room temperature, 0.06MPa pressure, the current field condition that intensity is 2.5V/mm, seperation film made from embodiment 1 is measured
To the flux of carbon dioxide, hydrogen, methane and nitrogen, obtain carbon dioxide and hydrogen, carbon dioxide and methane, carbon dioxide and
The flux ratio of nitrogen is respectively 20,72,132.
Embodiment 3
Under room temperature, 0.06MPa pressure, the current field condition that intensity is 5V/mm, seperation film pair made from embodiment 1 is measured
Carbon dioxide, hydrogen, methane and nitrogen flux, obtain carbon dioxide and hydrogen, carbon dioxide and methane, carbon dioxide and nitrogen
The flux ratio of gas is respectively 33,192,405.
Embodiment 4
(1) at room temperature, the graphene oxide water solution that configuration graphene oxide mass percent concentration is 0.02%, will
0.8ml solution filters under 85KPa negative pressure to inorganic oxide aluminium perforated membrane, and the diameter of film is 25mm, aperture 200nm, is made
The graphene oxide film of 125nm thickness;
(2) then, 0.08ml [BMIM] [BF is coated on graphene oxide film surface4], [BMIM] of 280nm thickness is made
[BF4]/graphene oxide gas separation membrane, wherein graphene oxide and [BMIM] [BF4] mass ratio be 0.45.
It should [BMIM] [BF4The surface of]/graphene oxide gas separation membrane and the structure of section are as shown in Figure 3.
Under room temperature, 0.06MPa, the current field condition that intensity is 5V/mm, the seperation film is measured to carbon dioxide, hydrogen, first
The flux of alkane and nitrogen obtains the flux ratio difference of carbon dioxide and hydrogen, carbon dioxide and methane, carbon dioxide and nitrogen
It is 39,238,479.
Technical solution of the present invention and beneficial effect is described in detail in embodiment described above, it should be understood that
Above is only a specific embodiment of the present invention, it is not intended to restrict the invention, it is all to be done in spirit of the invention
Any modification, supplementary, and equivalent replacement etc., should all be included in the protection scope of the present invention.
Claims (8)
1. a kind of method of separation and concentration carbon dioxide characterized by comprising
Under 20~100 DEG C, 0.01~0.2MPa pressure, the current field condition that intensity is -7.5~7.5V/mm, using ionic liquid
Body/two-dimensional slice material gas seperation film carries out separation and concentration to the mixed gas containing carbon dioxide;
The ionic liquid/two-dimensional slice material gas seperation film preparation method includes:
(1) dispersion of two-dimensional slice material is obtained into two-dimensional slice material dispersion liquid in deionized water, by being filtered by vacuum two
It ties up sheet layer material dispersion liquid to filter onto perforated substrate, obtains two-dimensional slice material membrane;
(2) ionic liquid is coated on to the two-dimensional slice material film surface, small not less than holding 1~8 under 50KPa negative pressure
When, obtain ionic liquid/two-dimensional slice material gas seperation film.
2. the method for separation and concentration carbon dioxide according to claim 1, which is characterized in that the applying mode of electric field are as follows:
Piece of metal capacitance sheet is respectively set in the ionic liquid/two-dimensional slice material gas seperation film two sides, in two panels metal
Apply DC voltage on capacitance sheet.
3. the method for separation and concentration carbon dioxide according to claim 1, which is characterized in that described containing carbon dioxide
Mixed gas is the gaseous mixture of at least one of carbon dioxide and hydrogen, methane and nitrogen.
4. the method for separation and concentration carbon dioxide according to claim 1, which is characterized in that the two-dimensional slice material
For at least one of graphene oxide, molybdenum disulfide and tungsten disulfide.
5. the method for separation and concentration carbon dioxide according to claim 4, which is characterized in that the two-dimensional slice material
For graphene oxide.
6. the according to claim 1, method of separation and concentration carbon dioxide described in 4 or 5, which is characterized in that the ionic liquid
Body is 1- butyl -3- methyl imidazolium tetrafluoroborate.
7. the method for separation and concentration carbon dioxide according to claim 1, which is characterized in that ionic liquid/bis-
Tie up sheet layer material gas separation membrane with a thickness of 50~1500nm;In ionic liquid/two-dimensional slice material gas seperation film, ion
The mass percent of liquid is 50~80%.
8. the method for separation and concentration carbon dioxide according to claim 1, which is characterized in that the perforated substrate is poly-
Carbonic ester perforated membrane or inorganic oxide aluminium perforated membrane.
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Cited By (4)
Publication number | Priority date | Publication date | Assignee | Title |
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CN111603945A (en) * | 2020-06-08 | 2020-09-01 | 天津工业大学 | Ionic liquid functionalized cerium fluoride porous nanosheet, preparation method and application thereof, mixed matrix membrane, preparation method and application thereof |
CN112646613A (en) * | 2019-10-12 | 2021-04-13 | 中石化南京化工研究院有限公司 | Absorbent and method for separating and recovering carbon dioxide in blast furnace gas |
CN113457467A (en) * | 2021-08-04 | 2021-10-01 | 中国矿业大学 | High-stability GO-confinement ionic liquid supported liquid membrane and preparation method and application thereof |
WO2022059368A1 (en) * | 2020-09-17 | 2022-03-24 | 日東電工株式会社 | Separation membrane, separation membrane production method, and coating fluid for producing separation membrane |
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CN106975370A (en) * | 2017-04-01 | 2017-07-25 | 浙江大学 | Ionic liquid/transition metal dichalcogenide gas separation membrane and its application are prepared using capillary effect |
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Cited By (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CN112646613A (en) * | 2019-10-12 | 2021-04-13 | 中石化南京化工研究院有限公司 | Absorbent and method for separating and recovering carbon dioxide in blast furnace gas |
CN111603945A (en) * | 2020-06-08 | 2020-09-01 | 天津工业大学 | Ionic liquid functionalized cerium fluoride porous nanosheet, preparation method and application thereof, mixed matrix membrane, preparation method and application thereof |
WO2022059368A1 (en) * | 2020-09-17 | 2022-03-24 | 日東電工株式会社 | Separation membrane, separation membrane production method, and coating fluid for producing separation membrane |
CN113457467A (en) * | 2021-08-04 | 2021-10-01 | 中国矿业大学 | High-stability GO-confinement ionic liquid supported liquid membrane and preparation method and application thereof |
CN113457467B (en) * | 2021-08-04 | 2022-08-02 | 中国矿业大学 | High-stability GO-confinement ionic liquid supported liquid membrane and preparation method and application thereof |
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