CN113184850B - High-purity carbon dioxide gas purification method and device thereof - Google Patents
High-purity carbon dioxide gas purification method and device thereof Download PDFInfo
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- CN113184850B CN113184850B CN202110531940.3A CN202110531940A CN113184850B CN 113184850 B CN113184850 B CN 113184850B CN 202110531940 A CN202110531940 A CN 202110531940A CN 113184850 B CN113184850 B CN 113184850B
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- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 title claims abstract description 240
- 229910002092 carbon dioxide Inorganic materials 0.000 title claims abstract description 120
- 239000001569 carbon dioxide Substances 0.000 title claims abstract description 120
- 238000000034 method Methods 0.000 title claims abstract description 42
- 238000000746 purification Methods 0.000 title claims description 16
- 239000007789 gas Substances 0.000 claims abstract description 243
- 238000001179 sorption measurement Methods 0.000 claims abstract description 157
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 39
- 239000003463 adsorbent Substances 0.000 claims abstract description 37
- 229910001868 water Inorganic materials 0.000 claims abstract description 34
- 238000000926 separation method Methods 0.000 claims abstract description 31
- 239000002912 waste gas Substances 0.000 claims abstract description 27
- 238000005057 refrigeration Methods 0.000 claims abstract description 21
- 239000007788 liquid Substances 0.000 claims abstract description 11
- 238000011084 recovery Methods 0.000 claims abstract description 9
- 238000005516 engineering process Methods 0.000 claims abstract description 7
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 30
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 18
- 239000001301 oxygen Substances 0.000 claims description 17
- 229910052760 oxygen Inorganic materials 0.000 claims description 17
- 239000002994 raw material Substances 0.000 claims description 16
- 229910052757 nitrogen Inorganic materials 0.000 claims description 15
- 238000003795 desorption Methods 0.000 claims description 10
- 239000000203 mixture Substances 0.000 claims description 10
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 claims description 9
- 239000003507 refrigerant Substances 0.000 claims description 9
- 239000003546 flue gas Substances 0.000 claims description 8
- 230000006835 compression Effects 0.000 claims description 7
- 238000007906 compression Methods 0.000 claims description 7
- 238000007599 discharging Methods 0.000 claims description 7
- 239000012530 fluid Substances 0.000 claims description 6
- 239000002808 molecular sieve Substances 0.000 claims description 6
- URGAHOPLAPQHLN-UHFFFAOYSA-N sodium aluminosilicate Chemical compound [Na+].[Al+3].[O-][Si]([O-])=O.[O-][Si]([O-])=O URGAHOPLAPQHLN-UHFFFAOYSA-N 0.000 claims description 6
- PNEYBMLMFCGWSK-UHFFFAOYSA-N aluminium oxide Inorganic materials [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 5
- 238000004519 manufacturing process Methods 0.000 claims description 5
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 4
- 230000003139 buffering effect Effects 0.000 claims description 4
- 238000001816 cooling Methods 0.000 claims description 4
- 229930195733 hydrocarbon Natural products 0.000 claims description 4
- 150000002430 hydrocarbons Chemical class 0.000 claims description 4
- 239000012535 impurity Substances 0.000 claims description 4
- 238000011069 regeneration method Methods 0.000 claims description 4
- 239000000741 silica gel Substances 0.000 claims description 4
- 229910002027 silica gel Inorganic materials 0.000 claims description 4
- 239000004215 Carbon black (E152) Substances 0.000 claims description 3
- 239000002826 coolant Substances 0.000 claims description 3
- 230000008929 regeneration Effects 0.000 claims description 3
- 229920006395 saturated elastomer Polymers 0.000 claims description 3
- 239000000112 cooling gas Substances 0.000 claims description 2
- 238000005520 cutting process Methods 0.000 claims description 2
- 238000012544 monitoring process Methods 0.000 claims description 2
- 239000000047 product Substances 0.000 description 42
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 8
- 239000012071 phase Substances 0.000 description 6
- 229910052786 argon Inorganic materials 0.000 description 4
- 238000001514 detection method Methods 0.000 description 4
- -1 for example Substances 0.000 description 4
- 239000000463 material Substances 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- 229910021536 Zeolite Inorganic materials 0.000 description 2
- 238000002485 combustion reaction Methods 0.000 description 2
- 230000001276 controlling effect Effects 0.000 description 2
- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 2
- 239000012466 permeate Substances 0.000 description 2
- 230000000704 physical effect Effects 0.000 description 2
- 230000003584 silencer Effects 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 239000010457 zeolite Substances 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 238000010521 absorption reaction Methods 0.000 description 1
- 150000001335 aliphatic alkanes Chemical class 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 229910002091 carbon monoxide Inorganic materials 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
- 230000005494 condensation Effects 0.000 description 1
- 230000018044 dehydration Effects 0.000 description 1
- 238000006297 dehydration reaction Methods 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 239000000945 filler Substances 0.000 description 1
- 239000005431 greenhouse gas Substances 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000007791 liquid phase Substances 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 239000003345 natural gas Substances 0.000 description 1
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen(.) Chemical compound [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 description 1
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 1
- 239000013618 particulate matter Substances 0.000 description 1
- 238000004321 preservation Methods 0.000 description 1
- 238000007670 refining Methods 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 230000009919 sequestration Effects 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 239000002594 sorbent Substances 0.000 description 1
- 238000009628 steelmaking Methods 0.000 description 1
- 238000003860 storage Methods 0.000 description 1
- 230000026676 system process Effects 0.000 description 1
Classifications
-
- 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
-
- 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
- B01D53/02—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 adsorption, e.g. preparative gas chromatography
- B01D53/04—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 adsorption, e.g. preparative gas chromatography with stationary adsorbents
- B01D53/047—Pressure swing adsorption
- B01D53/053—Pressure swing adsorption with storage or buffer vessel
-
- 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
- C01B2210/0001—Separation or purification processing
- C01B2210/0009—Physical processing
- C01B2210/0014—Physical processing by adsorption in solids
-
- 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
- C01B2210/0045—Oxygen
-
- 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
- C01B2210/0046—Nitrogen
-
- 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
- C01B2210/0062—Water
-
- 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
-
- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/151—Reduction of greenhouse gas [GHG] emissions, e.g. CO2
Abstract
The invention belongs to the technical field of gas separation, and particularly relates to a method and a device for purifying high-purity carbon dioxide gas. The invention adopts the pressure swing adsorption technology of carbon dioxide adsorbent with equilibrium adsorption mechanism, obtains high-purity carbon dioxide from adsorption phase under lower pressure, and couples pressurization, refrigeration, water removal and carbon dioxide liquefaction to obtain high-purity liquid carbon dioxide as product gas; the gas phase components in the bed layer are replaced by circularly feeding carbon dioxide product gas so as to obtain the mixed gas of the carbon dioxide with higher purity and the water vapor; a gas recovery loop is designed between two or more groups of beds which are symmetrically operated, and part of waste gas generated in the adsorption separation process is returned to the symmetrical separation beds so as to improve the recovery rate of the system; a portion of the product gas will flow back to the feed end of the adsorbent bed to displace the impure gas in the gas phase. The invention can purify and obtain 60-99.9% carbon dioxide gas from the carbon dioxide mixed gas containing about 15%.
Description
Technical Field
The invention belongs to the technical field of gas separation, and particularly relates to a method and a device for purifying a low-partial-pressure carbon dioxide mixed gas.
Background
Pressure Swing Adsorption (PSA) is an important and widely used gas separation process, such as pressure swing adsorption drying, pressure swing adsorption oxygen production, nitrogen production, etc., and typically, different adsorbents are used to separate different mixtures based on equilibrium adsorption or kinetic separation characteristics to obtain the desired components.
Carbon dioxide (CO) 2 ) Is the main greenhouse gas, CO, responsible for global climate change 2 The capture, utilization and sequestration of (c) has become one of the hot issues of international social concern. A large amount of CO exists in the industrial fields of steelmaking, cement, chemical industry (such as synthetic ammonia, hydrogen production, natural gas purification) and the like 2 And (5) discharging. At present, china generates CO in flue gas generated by combustion 2 The recovery measure is to recycle CO in the flue gas by a chemical absorption and temperature-changing regeneration method 2 Separating, compressing, liquefying, refining to obtain industrial or food grade CO 2 The product, the system process is complex, the investment is large, the equipment occupation is large, and particularly the miniaturized system has no simple, feasible and effective solution.
Disclosure of Invention
In view of the above, the present invention provides a method and apparatus for removing nitrogen, oxygen and moisture in flue gas generated in combustion chemical reaction process by non-cryogenic air separation technology to obtain high purity carbon dioxide.
The purification method of high-purity carbon dioxide provided by the invention adopts a pressure swing adsorption technology of a carbon dioxide adsorbent based on an equilibrium adsorption mechanism, obtains high-purity carbon dioxide from an adsorption phase under lower pressure, and couples pressurization, refrigeration, water removal and carbon dioxide liquefaction to obtain high-purity liquid carbon dioxide as product gas, wherein:
the pressure swing adsorption technology based on the equilibrium adsorption mechanism is that a carbon dioxide adsorbent is filled in an adsorption bed layer, and compared with nitrogen and oxygen components, the adsorbent has stronger adsorption capacity to moisture and carbon dioxide in raw material gas, and high-purity mixed gas of carbon dioxide and water vapor is obtained through desorption after the adsorption saturation of the bed layer;
and the gas phase components in the bed layer are replaced by circularly feeding the carbon dioxide product gas with higher purity, and the mixed gas of the carbon dioxide with higher purity and the water vapor can be obtained by desorption after the adsorption saturation of the bed layer;
in addition, in the invention, a gas recovery loop is designed between two or more groups of beds which are symmetrically operated, so that the loss of target gas is reduced to the maximum extent and the recovery rate is improved;
in addition, at least one part of waste gas generated in the adsorption separation process is returned to the symmetrical separation bed layer, so that the pressure boosting process of the symmetrical separation bed layer is facilitated, the power consumption in the desorption process is reduced, and the recovery rate of the system is improved;
also, in the present invention, at least a portion of the product gas will flow back to the feed end of the adsorbent bed to displace the impure gas in the gas phase;
in the present invention, the purification process is preferably used to obtain a carbon dioxide purity of 60 to 99.9%, more preferably 60 to 85%, from a carbon dioxide mixture gas containing about 15% of typical flue gas;
in addition, in the invention, the subsequent coupled product carbon dioxide gas pressurizing process adopts two-stage refrigeration to respectively achieve the purpose of removing moisture and liquefied carbon dioxide, wherein, the moisture in the product is preferably removed by the first-stage refrigeration (typically, a freeze dryer) under the pressure of 3-7.5 MPa so as to achieve the technical purpose of normal pressure dew point of-65 ℃, and the invention combines the pressure boosting process required by the carbon dioxide itself to remove the moisture at the station unlike the dehydration process which is mainly carried out on raw material gas at the front end in the prior art;
in addition, in the invention, the pressurizing process of the carbon dioxide gas of the product which is coupled subsequently adopts two-stage refrigeration to respectively achieve the purposes of removing moisture and liquefying carbon dioxide, wherein, preferably, under the pressure of 3-7.5 MPa, the mixed gas with the purity of 60-85 percent and obtained by a purification system is liquefied under the conditions of 1-15 ℃ and 3-7.5 MPa by selecting the second-stage refrigeration (typically, the heat exchange of chilled water), and the non-condensable gas in the mixed gas is discharged out of the system.
Based on the method, the purification device of the high-purity carbon dioxide provided by the invention comprises the following components:
(1) At least one compression device for providing the necessary feed gas under pressure, preferably but not necessarily including the means (not shown in the figures) required for the pretreatment, such as oxygen-, nitrogen-, water-containing carbon dioxide mixtures having a pressure of 15 to 100kpa (gauge);
(2) At least one set of pressure swing adsorption device which is known in the prior art and at least comprises an adsorption tower, wherein a carbon dioxide adsorbent is arranged in the adsorption tower; typically, such as with 13X or other modified regenerable carbon dioxide sorbents having equilibrium adsorption characteristics. One or more combination of molecular sieves capable of adsorbing water such as activated alumina and silica gel can be compositely filled at the air inlet end of the raw material gas to remove the impurity gases such as water and total hydrocarbon contained in the mixed gas; the device also comprises an air inlet valve for feeding raw material gas into each adsorption tower and necessary connecting pipelines thereof, an exhaust valve for feeding waste gas into the waste gas buffer tank and necessary connecting pipelines thereof, and a gas production valve for feeding product gas into the product gas buffer tank and necessary connecting pipelines thereof; the control valve for fluid exchange between the symmetrical operation towers and the necessary pipelines are used for adjusting and cutting off the gas flow between the adsorption towers; product gas enters an air inlet valve of each adsorption tower and a necessary pipeline thereof;
(3) At least one exhaust buffer tank connected to the exhaust end of each separator through a control valve and necessary connecting lines thereof for receiving exhaust gas from the separator and feeding the temporarily stored exhaust gas into the separator in which the pre-pressurizing process is being performed by the exhaust end of the separator;
(4) At least one product gas buffer tank connected to the feed end of each separator via a desorption vacuum pump via a control valve and its necessary connecting line, for receiving product gas from the separator, and for feeding the product gas in the product buffer tank via the control valve and its necessary connecting line to the feed end of the separator for repressurizing the separator undergoing the adsorption process;
(5) At least one product gas booster that boosts the product gas in the product gas surge tank to a predetermined pressure;
(6) At least one refrigerant heat exchanger and one filter, cool the gas, condense the moisture in the gas into liquid state, and dispel and discharge the system through the filter;
(7) At least one heat exchanger for cooling the carbon dioxide mixed gas from which the moisture is removed to a liquefaction triple point of the mixed gas, liquefying carbon dioxide in the mixed gas as a product, and discharging the non-condensable gas out of the system;
(8) And a complete control assembly for controlling the valve in the loop and the compression equipment, vacuum pump, refrigerating equipment, heat exchanger, etc.
The invention can be used for separating the gas which is difficult to be adsorbed from the gas which is difficult to be adsorbed/permeated by adopting one or a plurality of adsorbents, and the component which is easy to be adsorbed/permeated or the component which is difficult to be adsorbed/permeated can be used as the required product gas independently or simultaneously. The present invention is preferably applied to PSA processes based on equilibrium adsorption theory rather than kinetic separation theory, but it is not excluded that PSA processes based on kinetic separation theory may be employed to achieve the object of the present invention. The disclosed principles are applicable to many other separation applications. Typical examples of separations that can be achieved by the present invention include:
by selective adsorption of N 2 Is used for recovering N from air 2 ；
By selective adsorption of O 2 Is used for recovering O from air 2 ；
Enriching CO from a carbon monoxide mixture with an adsorbent material that selectively adsorbs CO;
by selective adsorption of CO 2 Is used for enriching CO from carbon dioxide mixed gas 2 ；
Realization of CO 2 /CH 4 Separation of CO 2 /N 2 Separation, H of 2 /N 2 And olefin/alkane separation.
From O-containing 2 Separation of O from a gas mixture of Ar (e.g., produced by pressure swing adsorption coupled membrane separation air separation) 2 Or Ar;
any combination of one or more suitable adsorbents may also be used for separation, for example, caA zeolite, liX zeolite, or any other specific separation material to recover oxygen or nitrogen; the gas that is difficult to adsorb/permeate is enriched from the non-feed end and the component that is more easily selectively adsorbed/permeate is enriched from the other end.
In the present invention, the product gas refers to a gas which is difficult to be adsorbed by an adsorbent, for example, nitrogen is easy to be adsorbed by a nitrogen adsorbent, oxygen and argon are difficult to be adsorbed by an oxygen adsorbent, oxygen is easy to be adsorbed by an argon is difficult to be adsorbed by an argon adsorbent.
In the present invention, the exhaust gas refers to a gas that is more easily adsorbed by the adsorbent than the product gas, such as nitrogen, oxygen, and the like, and is more easily adsorbed by the nitrogen adsorbent and the oxygen adsorbent than argon.
In the present invention, the adsorbent, also called molecular sieve, is used for pressure swing adsorption of dried molecular sieves such as 13X, activated alumina, silica gel, etc., and nitrogen adsorbents such as CaA, caX, naX, liX type are generally used in conventional PSA processes for producing oxygen from air streams to produce oxygen based on equilibrium adsorption theory.
In the present invention, the term "adsorption column" may be also referred to as an adsorber, an adsorbent bed or a separator "means a vessel filled with at least one kind of adsorbent such as the one described above, and the adsorbent has a strong adsorption capacity for components that are more easily adsorbed in the mixed gas.
In the present invention, the terms pressure swing adsorption, adsorption separation, PSA, and the like are understood by those skilled in the art to refer to not only PSA processes, but also similar processes such as vacuum pressure swing adsorption (Vacuum Swing Adsorption-VSA) or mixed pressure swing adsorption (Mixed Pressure Swing Adsorption-MPSA) processes, and the like, and are understood in a broader sense, that is, for the cyclical adsorption pressure, a higher pressure is a higher pressure relative to the desorption step and may include greater than or equal to atmospheric pressure, while the cyclical desorption pressure, a lower pressure is a lower pressure relative to the adsorption step and includes less than or equal to atmospheric pressure.
The above-described method and apparatus of the present invention do not preclude the use of multiple sets of side-by-side adsorption separators for separation, and the gas flow patterns of the adsorption separators may be axial, radial, lateral, or other patterns. Those skilled in the art will appreciate that even three or more types of separators may be employed for separation by providing the necessary additional lines and switching valves.
The product gas buffer tank may be filled with the necessary filler material as described in the prior art to achieve a more economical buffer volume.
The method and the device can be provided with necessary gas detection equipment at the feed gas inlet, the intermediate process and the product gas outlet, and necessary pressure detection equipment, dew point detection equipment and purity detection equipment are arranged on the separator and the buffer tank, so that a system which runs completely according to the required pressure and purity is formed, and the system is controlled by an intelligent control program. The implementation in the technical field is not difficult, and the experienced technicians can know that the debugging process of the equipment is almost the process of self-adapting to the stability of the system, and on the basis of fault judgment, the control program gives more sufficient information to maintenance staff, and even directly designates the fault point.
Regarding liquefaction of the product gas carbon dioxide, basic physical property data of carbon dioxide are shown in the following table 1:
TABLE 1 basic physical Property data of carbon dioxide
。
Obviously, the lower the temperature is, the smaller the pressure required by the gas-liquid phase change is, but the achievement of the temperature and the pressure all needs to consume a large amount of refrigeration and compression energy, the invention preferably adopts the cold water as a cold source, and is generally easy to obtain with low cost, for example, the typical water supply temperature of 3 ℃ (if the temperature can be lower, the water return temperature of the water is better) is adopted for liquefaction, the compression power consumption of the liquefaction can be reduced to the greatest extent, and the effects of low-temperature liquefaction and storage are comprehensively considered.
In Table 2 below, at 10℃the carbon dioxide gas content was 30% and 70%, the pressure required to achieve carbon dioxide condensation was 15MPa and 6.5MPa, respectively, with a great difference; with the increase of the concentration of the carbon dioxide, the typical liquefaction pressure of 70 percent of the carbon dioxide is close to that of the pure component carbon dioxide, namely 6.5/4.5MPa, the purity of the purification system is as high as possible, the liquefaction operation pressure can be greatly reduced, and the liquefaction of 6.5MPa is selected, so that the effects of low-temperature refrigeration and high-pressure compression are considered.
TABLE 2 comparison of carbon dioxide concentration and operating pressure
。
Therefore, the purification system preferably obtains the mixed gas with the purity of 60-85% at first, and selects the condition of 1-15 ℃ and 3-7.5 MPa for liquefaction, so that good economy can be obtained.
In the device described above, various modifications may be made without departing from the scope of the invention.
Drawings
FIG. 1 is a schematic flow chart of a method and apparatus for purifying a low partial pressure carbon dioxide mixture according to the present invention.
The symbols in the drawings are as follows: 101A and 101B are adsorption towers, B01 is a boosting device, C01 is a boosting device, and PV01 is a product gas buffer tank; PV02 is an exhaust buffer tank; TC01 is a refrigerant heat exchanger, F01 is a filter; YHQ01 is a liquefier, XYQ01 is a muffler, 01A,02A,03A,04A,01B,02B,03B,04B are automatic control valves, and TV01 is an automatic control valve with flow control regulation performance.
Detailed Description
A typical purification device for low partial pressure carbon dioxide mixed gas has a structure shown in figure 1. Comprising the following steps:
two groups of pressure swing adsorption devices (also called adsorption towers, separators) 101A and 101B are connected in parallel to form two groups of symmetrically-operated adsorption components; two sets of pressure swing adsorption units are charged with carbon dioxide adsorbent, typically, 13X, other modified regenerable carbon dioxide adsorbent with equilibrium adsorption characteristics;
in addition, water adsorbents (such as one or more combinations of molecular sieves for adsorbing water, such as activated alumina, silica gel and the like) are compositely filled at the feed gas inlet ends of the two groups of pressure swing adsorption devices so as to remove impurity gases, such as moisture, total hydrocarbon and the like, contained in the feed gas mixture;
the pressure boosting device B01 is used for extracting gas in the adsorption tower and sending the gas into the product gas buffer tank PV01; the pressure boosting device B01 may be a vacuum pump;
the pressure boosting device C01 is used for boosting the product carbon dioxide mixed gas to the pressure required by the three-phase point of water removal and liquefaction;
a product gas buffer tank PV01 for buffering carbon dioxide product gas;
a waste gas buffer tank PV02 for buffering and discharging waste gas;
the refrigerant heat exchanger TC01 can be various refrigeration equipment used for cooling down the mixed gas so as to reduce the water content in the gas;
a filter F01 for removing liquid water droplets contained in a gas state and discharging the liquid water droplets out of the system;
the liquefier YHQ01 can be various refrigeration equipment and heat exchange equipment, is used for cooling gas, meets the requirement of the liquefaction triple point of the carbon dioxide mixed gas, and is typically a pressure-bearing container (containing heat preservation) for heat exchange by adopting chilled water; the liquefier YHQ01 comprises an air inlet, a liquefied carbon dioxide outlet, a non-condensable gas outlet, a coolant water supply outlet and a water outlet, and can also comprise necessary temperature and pressure monitoring;
the silencer XYQ01 is used for eliminating the fluid discharge noise and can be a silencer of all types;
the control valve is also included: 01A,02A,03A, 01B,02B,03B,04B, automatic control valve with flow control regulating capability: TV01. Wherein:
the raw material gas pipeline is respectively connected with the gas inlets of the adsorption devices 101A and 101B through pipelines, and the control valves 01A and 01B are correspondingly arranged on the two connecting pipelines;
the boosting device B01 is connected with the product air ports of the adsorption devices 101A and 101B through pipelines, and the control valves 02A and 02B are correspondingly arranged on the two connecting pipelines; the other end of the pressure boosting device B01 is connected with the inlet end of the product gas buffer tank PV01 through a pipeline;
the inlet end of the product gas buffer tank PV01 is respectively connected with the product gas ports of the adsorption devices 101A and 101B through pipelines, and the control valves 04A and 04B are correspondingly arranged on the two connecting pipelines;
the inlet end of the waste gas buffer tank PV02 is respectively connected with the waste gas outlets of the adsorption devices 101A and 101B through pipelines, and the control valves 03A and 03B are correspondingly arranged on the two connecting pipelines; the outlet end of the exhaust buffer tank PV02 is connected with a muffler XYQ01 for exhausting the exhaust;
the automatic control valve TV01 is arranged on a connecting pipeline of the waste gas outlets of the adsorption devices 101A and 101B;
the inlet end of the refrigerant heat exchanger TC01 is connected with the outlet end of the product gas buffer tank PV01 through a pipeline, and the boosting equipment C01 is arranged on the connecting pipeline; the outlet end of the refrigerant heat exchanger TC01 is connected with the filter F01 and the liquefier YHQ01 in sequence through pipelines.
Typically, the unit receives a relatively clean feed gas that has been pretreated, typically by removal of entrained solid particulate impurities and total hydrocarbons such as oil; as is known in the art, these are very necessary for gas separation systems.
After entering the pressure swing adsorption separation device of the known technology described in the attached figure 1, the treated raw gas is output from the outlet of the vacuum pump B01 to enrich carbon dioxide components which are easier to adsorb, and the carbon dioxide with higher purity is output from the product gas buffer tank PV 01.
The pressure swing adsorption device is a typical double-tower adsorption system, an adsorption tower 101A adsorbs and removes gases which are difficult to adsorb, such as nitrogen, oxygen and the like, in a mixed gas, an adsorption tower 101B generates enriched carbon dioxide mixed gas and sends the enriched carbon dioxide mixed gas into a product gas buffer tank PV01 when the adsorption tower 101A is in adsorption saturation, namely, the adsorption tower 101B which is already regenerated is switched to perform the processes of oxygen removal and nitrogen removal, the adsorption tower 101A generates enriched carbon dioxide mixed gas and sends the enriched carbon dioxide mixed gas into the product gas buffer tank PV01 when performing the regeneration process, and the pressure swing adsorption process based on the equilibrium adsorption mechanism adopts heterogeneous sequence operation when adopting the double-tower device, and typical operation flow is as follows:
(1) Opening a control valve TV01, adjusting to a certain opening degree, simultaneously opening control valves 02A and 02B, boosting the pressure of the adsorption tower 101A, and decompressing the adsorption tower 101B;
(2) Opening control valves 01A and 03A, enabling raw material gas and waste gas of a waste gas buffer tank PV102 to enter an adsorption tower 101A at the same time, and pre-pressurizing the adsorption tower 101A; simultaneously, the control valve 02B is opened, and the adsorption tower 101B starts to produce gas and sends the gas into the product gas buffer tank PV101;
(3) Opening a control valve 01A, and enabling raw material gas to enter an adsorption tower 101A to continue pre-pressurizing; simultaneously, the control valve 02B is opened, and the adsorption tower 101B generates gas;
(4) The control valves 01A and 03A are opened, the adsorption tower 101A is used for normal feeding and adsorption, and the gas difficult to adsorb enters the waste gas buffer tank PV102 and is discharged out of the system; simultaneously, the control valve 02B is opened, and the adsorption tower 101B generates gas;
(5) Opening control valves 04A and 03A, and enabling product gas in the buffer tank PV101 to enter the buffer tank PV 101A for replacing the gas phase; simultaneously, the control valve 02B is opened, and the adsorption tower 101B generates gas;
(6) Opening a control valve TV01 and adjusting to a certain opening degree, and simultaneously opening control valves 01A and 03A, wherein the adsorption tower 101A is used for feeding and adsorbing; simultaneously, the control valve 02B is opened, and the adsorption tower 101B generates gas;
(7) Opening a control valve TV01, adjusting to a certain opening degree, simultaneously opening control valves 02A and 02B, depressurizing an adsorption tower 101A, and pressurizing the adsorption tower 101B;
(8) Opening a control valve 02A, generating gas by the adsorption tower 101A and sending the gas into a product gas buffer tank PV101; simultaneously, the control valves 01B and 03B are opened, and the raw material gas and the waste gas of the waste gas buffer tank PV102 enter the adsorption tower 101B for pre-pressurizing;
(9) Opening a control valve 02A, and generating gas by the adsorption tower 101A; simultaneously, the control valve 01B is opened, and raw material gas enters the adsorption tower 101B to be continuously pre-pressurized;
(10) Opening a control valve 02A, and generating gas by the adsorption tower 101A; simultaneously, the control valves 01B and 03B are opened, the adsorption tower 101B normally adsorbs gases difficult to adsorb, and the gases difficult to adsorb enter the exhaust buffer tank PV102 and are discharged out of the system;
(11) Opening a control valve 02A, and generating gas by the adsorption tower 101A; simultaneously, the control valves 04B and 03B are opened, and the product gas in the buffer tank PV101 enters the buffer tank PV 101B to replace the gas phase;
(12) Opening a control valve 02A, and generating gas by the adsorption tower 101A; simultaneously, the control valve TV01 is opened and adjusted to a certain opening degree, and meanwhile, the control valves 01B and 03B are opened for feeding and adsorbing, and the adsorption tower 101B is used for feeding and adsorbing.
In the above steps, except for the appointed opening valve, all the other valves are in the closed state, and the opening and flow rate of the valves can be controlled by adjusting the TV01.
In the above steps, when one group of adsorption is saturated, the fluid is controlled to enter the symmetrical adsorption groups by controlling the switching fluid control valve, and the adsorption saturated adsorption groups are regenerated and produce gas, so that the carbon dioxide mixed gas containing oxygen, nitrogen and water can be purified to high-purity carbon dioxide with the purity of 99% or even more than 99.99% and continuously sent into a later-stage system.
In the present invention, it is preferable to purify the carbon dioxide mixture gas containing about 15% of carbon dioxide in a typical flue gas to obtain a purity of 60 to 99.9%, and it is more preferable to obtain a purity of 60 to 85% of carbon dioxide and continuously send the carbon dioxide mixture gas to a subsequent system.
In addition, the product carbon dioxide gas continuously extracted through the steps is pressurized to a pressure of 3-7.5 MPa by adopting a booster C01, and the purposes of removing moisture and liquefying carbon dioxide are respectively achieved through two-stage coupled refrigeration, wherein:
preferably, the water in the water is removed by primary refrigeration TC01 under the pressure of 3-7.5 MPa, so as to achieve the technical purpose of normal pressure dew point of-65 ℃.
The provided pipe filter F01 traps particulate matter, liquid droplets which may be present, transported through the pipe and out of the system via the filter.
Preferably, the mixed gas with the purity of 60-85% obtained by the purification system is liquefied under the conditions of 1-15 ℃ and 3-7.5 MPa in YHQ01 with a second-stage cold source (second-stage refrigeration, typically, chilled water can exchange heat), and the non-condensable gas is discharged out of the system.
Thus, the flue gas containing about 15% of carbon dioxide can be continuously extracted, and the carbon dioxide in the flue gas can be purified and liquefied into liquid carbon dioxide.
The embodiments described above illustrate only some important features of the invention and all other variations which do not depart from the essence of the invention which is illustrated are intended to be within the scope of the invention which is limited only by the scope of the claims.
Claims (8)
1. A purification method of high-purity carbon dioxide gas is characterized in that a pressure swing adsorption technology of a carbon dioxide adsorbent based on an equilibrium adsorption mechanism is adopted, high-purity carbon dioxide is obtained from an adsorption phase under lower pressure, pressurization, refrigeration, water removal and carbon dioxide liquefaction are coupled to obtain high-purity liquid carbon dioxide as product gas, wherein:
the pressure swing adsorption technology based on the equilibrium adsorption mechanism is that a carbon dioxide adsorbent is filled in an adsorption bed layer, and compared with nitrogen and oxygen components, the adsorbent has stronger adsorption capacity to moisture and carbon dioxide in raw material gas, and high-purity mixed gas of carbon dioxide and water vapor is obtained through desorption after the adsorption saturation of the bed layer;
and the gas phase components in the bed layer are replaced by circularly feeding the carbon dioxide product gas with higher purity, and the mixed gas of the carbon dioxide with higher purity and the water vapor is obtained by desorption after the adsorption saturation of the bed layer;
in addition, a gas recovery loop is designed between two or more groups of beds which are symmetrically operated, so that the loss of target gas is reduced to the maximum extent, and the recovery rate is improved;
at least one part of waste gas generated in the adsorption separation process is returned to the symmetrical separation bed layer, so that the pressure boosting process of the symmetrical separation bed layer is facilitated, the power consumption in the desorption process is reduced, and the recovery rate of the system is improved;
and, at least a portion of the product gas will flow back to the feed end of the adsorbent bed to displace impure gas in the gas phase;
the subsequent coupled product carbon dioxide gas pressurizing process adopts two-stage refrigeration to respectively remove moisture and liquefied carbon dioxide, wherein the moisture in the product is removed by first-stage refrigeration under the pressure of 3-7.5 MPa to realize the normal pressure dew point of-65 ℃; and (3) liquefying the mixed gas with the purity of 60-85% obtained by the purification system under the conditions of the temperature of 1-15 ℃ and the pressure of 3-7.5 MPa by using second-stage refrigeration.
2. The high-purity carbon dioxide gas purifying apparatus based on the purifying method according to claim 1, comprising:
(1) At least one compression device for providing a feed gas under pressure;
(2) At least one set of pressure swing adsorption device, which at least comprises an adsorption tower, wherein the adsorption tower is filled with carbon dioxide adsorbent; the device also comprises an air inlet valve for feeding raw material gas into each adsorption tower and necessary connecting pipelines thereof, an exhaust valve for feeding waste gas into the waste gas buffer tank and necessary connecting pipelines thereof, and a gas production valve for feeding product gas into the product gas buffer tank and necessary connecting pipelines thereof; the control valve for fluid exchange between the symmetrical operation towers and the necessary pipelines are used for adjusting and cutting off the gas flow between the adsorption towers; product gas enters an air inlet valve of each adsorption tower and a necessary pipeline thereof;
(3) At least one exhaust buffer tank connected to the exhaust end of each separator through a control valve and necessary connecting lines thereof for receiving exhaust gas from the separator and feeding the temporarily stored exhaust gas into the separator in which the pre-pressurizing process is being performed by the exhaust end of the separator;
(4) At least one product gas buffer tank connected to the feed end of each separator via a desorption vacuum pump via a control valve and its necessary connecting line, for receiving product gas from the separator, and for feeding the product gas in the product buffer tank via the control valve and its necessary connecting line to the feed end of the separator for repressurizing the separator undergoing the adsorption process;
(5) At least one product gas booster that boosts the product gas in the product gas surge tank to a predetermined pressure;
(6) At least one refrigerant heat exchanger and one filter, cool the gas, condense the moisture in the gas into liquid state, and dispel and discharge the system through the filter;
(7) At least one heat exchanger for cooling the carbon dioxide mixed gas from which the moisture is removed to a liquefaction triple point of the mixed gas, liquefying carbon dioxide in the mixed gas as a product, and discharging the non-condensable gas out of the system;
(8) A complete control assembly is used for carrying out necessary operation control on valve elements on the loop and necessary control operation on compression equipment, vacuum pumps, refrigeration and heat exchanger equipment.
3. The apparatus for purifying high purity carbon dioxide gas according to claim 2, wherein the carbon dioxide adsorbent is 13X or other modified regenerable adsorbent having equilibrium adsorption characteristics.
4. The high-purity carbon dioxide gas purification apparatus according to claim 2, wherein a water adsorbent is compositely filled in the feed gas inlet end of the pressure swing adsorption apparatus for removing moisture and total hydrocarbon impurity gas contained in the mixed gas; the water adsorbent is one of active alumina and molecular sieve for adsorbing water by silica gel, or the combination of a plurality of the active alumina and the molecular sieve.
5. The purification apparatus of high purity carbon dioxide gas according to claim 2, wherein said pressure swing adsorption apparatus is also called an adsorption tower or a separator, and has two groups, denoted as 101A, 101B, in parallel structure, forming two groups of symmetrically operated adsorption modules; the two groups of pressure swing adsorption devices are filled with carbon dioxide adsorbent; further comprises:
the pressure boosting device B01 is used for extracting gas in the adsorption tower and sending the gas into the product gas buffer tank PV01;
the pressure boosting device C01 is used for boosting the product carbon dioxide mixed gas to the pressure required by the three-phase point of water removal and liquefaction;
a product gas buffer tank PV01 for buffering carbon dioxide product gas;
a waste gas buffer tank PV02 for buffering and discharging waste gas;
the refrigerant heat exchanger TC01 is used for cooling down the mixed gas so as to reduce the water content in the gas;
a filter F01 for removing liquid water droplets contained in a gas state and discharging the liquid water droplets out of the system;
the liquefier YHQ01 is used for cooling gas, meets the requirement of the liquefaction triple point of the carbon dioxide mixed gas, and is typically a pressure-bearing container for heat exchange by adopting chilled water; the liquefier YHQ01 comprises an air inlet, a liquefied carbon dioxide outlet, a non-condensable gas outlet, a coolant water supply outlet, a coolant water outlet, and necessary temperature and pressure monitoring;
a muffler XYQ01 for eliminating fluid discharge noise;
also comprises control valves 01A,02A,03A,04A,01B,02B,03B,04B and an automatic control valve TV01 with flow control regulation performance; wherein:
the raw material gas pipeline is respectively connected with the gas inlets of the adsorption devices 101A and 101B through pipelines, and the control valves 01A and 01B are correspondingly arranged on the two connecting pipelines;
the boosting device B01 is connected with the product air ports of the adsorption devices 101A and 101B through pipelines, and the control valves 02A and 02B are correspondingly arranged on the two connecting pipelines; the other end of the pressure boosting device B01 is connected with the inlet end of the product gas buffer tank PV01 through a pipeline;
the inlet end of the product gas buffer tank PV01 is respectively connected with the product gas ports of the adsorption devices 101A and 101B through pipelines, and the control valves 04A and 04B are correspondingly arranged on the two connecting pipelines;
the inlet end of the waste gas buffer tank PV02 is respectively connected with the waste gas outlets of the adsorption devices 101A and 101B through pipelines, and the control valves 03A and 03B are correspondingly arranged on the two connecting pipelines; the outlet end of the exhaust buffer tank PV02 is connected with a muffler XYQ01 for exhausting the exhaust;
the automatic control valve TV01 is arranged on a connecting pipeline of the waste gas outlets of the adsorption devices 101A and 101B;
the inlet end of the refrigerant heat exchanger TC01 is connected with the outlet end of the product gas buffer tank PV01 through a pipeline, and the boosting equipment C01 is arranged on the connecting pipeline; the outlet end of the refrigerant heat exchanger TC01 is connected with the filter F01 and the liquefier YHQ01 in sequence through pipelines.
6. The apparatus for purifying high-purity carbon dioxide gas according to claim 5, wherein the treated raw gas is introduced into the pressure swing adsorption separation apparatus and enriched in carbon dioxide components which are easily adsorbed by the outlet of the pressure increasing apparatus B01, and the high-purity carbon dioxide is discharged from the product gas buffer tank PV01; the adsorption tower 101A adsorbs and removes the gas which is difficult to adsorb by nitrogen and oxygen in the mixed gas, the adsorption tower 101B finishes the regeneration process of the adsorbent and simultaneously produces enriched carbon dioxide mixed gas which is sent to the product gas buffer tank PV01, when the adsorption tower 101A is saturated in adsorption, the adsorption tower 101B which is already regenerated is switched to perform the process of removing oxygen and nitrogen, the adsorption tower 101A performs the regeneration process and simultaneously produces enriched carbon dioxide mixed gas which is sent to the product gas buffer tank PV01, and the pressure swing adsorption process based on the equilibrium adsorption mechanism adopts heterogeneous sequence operation when a double-tower device is adopted; the typical operation flow is as follows:
(1) Opening a control valve TV01, adjusting to a certain opening degree, simultaneously opening control valves 02A and 02B, boosting the pressure of the adsorption tower 101A, and decompressing the adsorption tower 101B;
(2) Opening control valves 01A and 03A, enabling raw material gas and waste gas of a waste gas buffer tank PV102 to enter an adsorption tower 101A at the same time, and pre-pressurizing the adsorption tower 101A; simultaneously, the control valve 02B is opened, and the adsorption tower 101B starts to produce gas and sends the gas into the product gas buffer tank PV101;
(3) Opening a control valve 01A, and enabling raw material gas to enter an adsorption tower 101A to continue pre-pressurizing; simultaneously, the control valve 02B is opened, and the adsorption tower 101B generates gas;
(4) The control valves 01A and 03A are opened, the adsorption tower 101A is used for normal feeding and adsorption, and the gas difficult to adsorb enters the waste gas buffer tank PV102 and is discharged out of the system; simultaneously, the control valve 02B is opened, and the adsorption tower 101B generates gas;
(5) Opening control valves 04A and 03A, and enabling product gas in the buffer tank PV101 to enter the buffer tank PV 101A for replacing the gas phase; simultaneously, the control valve 02B is opened, and the adsorption tower 101B generates gas;
(6) Opening a control valve TV01 and adjusting to a certain opening degree, and simultaneously opening control valves 01A and 03A, wherein the adsorption tower 101A is used for feeding and adsorbing; simultaneously, the control valve 02B is opened, and the adsorption tower 101B generates gas;
(7) Opening a control valve TV01, adjusting to a certain opening degree, simultaneously opening control valves 02A and 02B, depressurizing an adsorption tower 101A, and pressurizing the adsorption tower 101B;
(8) Opening a control valve 02A, generating gas by the adsorption tower 101A and sending the gas into a product gas buffer tank PV101; simultaneously, the control valves 01B and 03B are opened, and the raw material gas and the waste gas of the waste gas buffer tank PV102 enter the adsorption tower 101B for pre-pressurizing;
(9) Opening a control valve 02A, and generating gas by the adsorption tower 101A; simultaneously, the control valve 01B is opened, and raw material gas enters the adsorption tower 101B to be continuously pre-pressurized;
(10) Opening a control valve 02A, and generating gas by the adsorption tower 101A; simultaneously, the control valves 01B and 03B are opened, the adsorption tower 101B normally adsorbs gases difficult to adsorb, and the gases difficult to adsorb enter the exhaust buffer tank PV102 and are discharged out of the system;
(11) Opening a control valve 02A, and generating gas by the adsorption tower 101A; simultaneously, the control valves 04B and 03B are opened, and the product gas in the buffer tank PV101 enters the buffer tank PV 101B to replace the gas phase;
(12) Opening a control valve 02A, and generating gas by the adsorption tower 101A; simultaneously, the control valve TV01 is opened and adjusted to a certain opening, and meanwhile, the control valves 01B and 03B are opened for feeding and adsorbing, and the adsorption tower 101B is used for feeding and adsorbing;
in the above steps, except for the appointed opening valve, all the other valves are in the closed state, and the opening and flow rate of the valves are controlled by adjusting the control valve TV01.
7. The apparatus for purifying high-purity carbon dioxide gas according to claim 6, wherein said step is performed to obtain a carbon dioxide gas having a purity of 60 to 99.9% from a carbon dioxide gas mixture containing about 15% of flue gas.
8. The high purity carbon dioxide gas purifying apparatus according to claim 6, wherein the subsequent coupled product carbon dioxide gas pressurizing process adopts two-stage refrigeration to achieve removal of moisture and liquefied carbon dioxide, respectively, wherein the moisture is removed by one-stage refrigeration under a pressure of 3 to 7.5MPa to achieve an atmospheric dew point of-65 ℃; and (3) liquefying the mixed gas with the purity of 60-85% obtained by the purification system under the conditions of the temperature of 1-15 ℃ and the pressure of 3-7.5 MPa by using second-stage refrigeration.
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