WO2013091439A1 - 一种捕集电站烟气中二氧化碳的方法及其设备 - Google Patents
一种捕集电站烟气中二氧化碳的方法及其设备 Download PDFInfo
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- WO2013091439A1 WO2013091439A1 PCT/CN2012/083575 CN2012083575W WO2013091439A1 WO 2013091439 A1 WO2013091439 A1 WO 2013091439A1 CN 2012083575 W CN2012083575 W CN 2012083575W WO 2013091439 A1 WO2013091439 A1 WO 2013091439A1
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- flue gas
- carbon dioxide
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- 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
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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
- B01D53/14—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 absorption
- B01D53/1425—Regeneration of liquid absorbents
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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
- B01D53/34—Chemical or biological purification of waste gases
- B01D53/46—Removing components of defined structure
- B01D53/62—Carbon oxides
-
- 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
- B01D53/14—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 absorption
-
- 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
- B01D53/14—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 absorption
- B01D53/1456—Removing acid components
- B01D53/1475—Removing carbon dioxide
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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
- B01D53/14—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 absorption
- B01D53/1493—Selection of liquid materials for use as absorbents
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
- B01D2252/20—Organic absorbents
- B01D2252/204—Amines
- B01D2252/20436—Cyclic amines
- B01D2252/20473—Cyclic amines containing an imidazole-ring
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
- B01D2252/20—Organic absorbents
- B01D2252/204—Amines
- B01D2252/20478—Alkanolamines
- B01D2252/20484—Alkanolamines with one hydroxyl group
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
- B01D2252/20—Organic absorbents
- B01D2252/204—Amines
- B01D2252/20478—Alkanolamines
- B01D2252/20489—Alkanolamines with two or more hydroxyl groups
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
- B01D2252/30—Ionic liquids and zwitter-ions
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2252/00—Absorbents, i.e. solvents and liquid materials for gas absorption
- B01D2252/50—Combinations of absorbents
- B01D2252/504—Mixtures of two or more absorbents
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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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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2258/00—Sources of waste gases
- B01D2258/02—Other waste gases
- B01D2258/0283—Flue gases
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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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02A—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE
- Y02A50/00—TECHNOLOGIES FOR ADAPTATION TO CLIMATE CHANGE in human health protection, e.g. against extreme weather
- Y02A50/20—Air quality improvement or preservation, e.g. vehicle emission control or emission reduction by using catalytic converters
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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
- 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
Definitions
- the invention relates to the technical field of carbon dioxide emission reduction and resource utilization in a power plant boiler flue gas, and specifically relates to a method and a device for capturing carbon dioxide in a power station flue gas.
- C0 2 capture methods There are many C0 2 capture methods.
- the industrial application is more chemical absorption.
- the principle is that C0 2 in the flue gas reacts with the chemical solvent and is absorbed.
- the chemical solvent that absorbs C0 2 reaches equilibrium and becomes rich.
- the rich liquid enters the regeneration tower to release the C0 2 gas and becomes the lean liquid.
- the lean liquid then circulates and absorbs the C0 2 in the flue gas, so that the absorption solution is circulated in the absorption tower and the regeneration tower, and the C0 2 in the flue gas It was separated and purified and captured.
- the chemical absorption method for absorbing CO 2 with an alcohol amine solution is the most widely used, mainly including MEA, MDEA and mixed organic amines.
- the object of the present invention is to provide a method and a device for capturing carbon dioxide in flue gas of a power station with high efficiency and low energy consumption, and the method has the characteristics of high collection efficiency, low energy consumption and simple process flow.
- a method for efficiently capturing carbon dioxide in a power plant flue gas with high efficiency and low energy consumption characterized in that it comprises the following steps:
- the molar ratio of the organic amine to the ionic liquid is (1 to 1.1): 1, the organic amine, the ionic liquid and water are mixed to obtain a composite absorbent aqueous solution, wherein the concentration of the composite absorbent aqueous solution is 20 to 40% by weight. ;
- An aqueous solution of a composite absorbent composed of an organic amine and an ionic liquid is used as a CO 2 absorbent, and the aqueous solution of the composite absorbent is uniformly sprayed into the flue gas of the power plant boiler after the conventional dust removal and desulfurization treatment, so that the upward moving smoke and the downward movement Sprayed
- the composite absorbent aqueous solution is sufficiently reversely contacted, and the co 2 gas in the flue gas is absorbed by the gas-liquid two-phase chemical reaction with the composite absorbent, and the mechanism of the composite absorbent absorbing C0 2 is as follows; (A-organic amine; B - ionic liquid; the following reaction formula does not represent the actual reaction process, which includes physical adsorption and chemical absorption);
- Liquid gas ratio control in 5 ⁇ 25L / m 3 range, C0 2 in the flue gas and the absorbent composite aqueous reaction temperature may be preferably in the range of 40 ⁇ 55 ° C, reaction pressure of 0. 01 ⁇ 10atm;
- compound The aqueous solution of the absorbent can be fully and completely reacted with CO 2 in the flue gas at a suitable temperature and pressure to form a liquid rich in A ⁇ C0 2 and B ⁇ C0 2 ;
- the separated mixed liquid rich in A ⁇ C0 2 and B ⁇ C0 2 is subjected to heat exchange, and a part of C0 2 gas dissolved or adsorbed by the aqueous solution of the composite absorbent in the mixed liquid rich in A ⁇ C0 2 and B ⁇ C0 2 is Evaporation, heat exchange to obtain a mixed liquid rich in A ⁇ (: 0 2 and B ⁇ C0 2 ;
- step 5 cooling the high-concentration C0 2 gas separated in step 3) to cause condensation of hot water vapor contained therein;
- Step 5) The high-concentration C0 2 gas cooled and treated is subjected to gas-liquid separation treatment to remove the condensed water therein to obtain C0 2 gas with a purity of 99% (high purity (: 0 2 gas);
- the high-purity CO 2 gas obtained in the step 6) is further dried (drying temperature is 110 ° C, time is 0. l ⁇ 5 min), and then compressed and condensed to be liquid, and made into a high-concentration industrial grade. Liquid carbon dioxide finished product.
- the ionic liquid may be any one of a conventional ionic liquid, a functionalized ionic liquid, a polymeric ionic liquid, or a mixture of any two or more (including two), and any two or more (including two). When mixing, it is an arbitrary ratio.
- the conventional ionic liquid contains any one of an imidazolium salt, a pyrrole salt, a pyridinium salt, an ammonium salt, and a sulfonate ionic liquid, or a mixture of two or more kinds (including two kinds), and any two or more thereof (including Two kinds) When mixing, it is an arbitrary ratio.
- the functionalized ionic liquid is an ionic liquid that introduces an amino group.
- the conventional ionic liquid is 1-butyl-3-methylimidazolium tetrafluoroborate, 1-butyl-3-methylimidazolium hexafluorophosphate, 1-hexyl-3-methylimidazolium difluoride Any one or a mixture of two or more kinds (including two kinds) of methanesulfonimide salt, 1-hexyl-3-methylimidazolium hexafluorophosphate, or the like, and when two or more kinds (including two kinds) are mixed For any ratio.
- the introduced amino ionic liquid is any one of 1-(1-aminopropyl)-3-methylimidazolium bromide, 1-(3propylamino)-3-butylimidazolium tetrafluoroborate, and the like. Any kind of mixture of two or more kinds (including two kinds), and any two or more types (including two types) may be any ratio.
- the polymeric ionic liquid is poly-1_(4-styryl)-3-methylimidazolium tetrafluoroborate, poly-1_(4-styryl)-3-methylimidazolium hexafluorophosphate, poly 1 - (4-styryl)-3-methylimidazolium benzylsulfonimide salt, poly-1_(4-styryl)-3-methylimidazolium trifluoromethanesulfonimide salt and poly 1_ ( Any one or a mixture of two or more (including two kinds) of 4-styryl)-3-methylimidazolium tetrafluoroborate, and any combination of two or more (including two) ratio.
- the organic amine is any one of an alcohol amine such as ethanolamine (methanol) or hydrazine-methyldiethanolamine (MDEA), or a mixture of two or more kinds (including two kinds), and any two or more kinds thereof. (including two kinds) When mixing, it is an arbitrary ratio.
- an alcohol amine such as ethanolamine (methanol) or hydrazine-methyldiethanolamine (MDEA), or a mixture of two or more kinds (including two kinds), and any two or more kinds thereof. (including two kinds)
- MDEA hydrazine-methyldiethanolamine
- the heating analysis process is performed at a temperature of 80 to 110 ° C and a pressure of 0.01 to 10 atm, and the analysis time is 1 to 5 min, and A ⁇ C0 2 is rapidly decomposed first, that is, A ⁇ C0 2 is decomposed and generated.
- A, and release C0 2 , B ⁇ C0 2 is not easy to release C0 2 under this condition ; since A will easily absorb the absorption in solution B: 0 2 in C 2 2 to generate A - C0 2 , then A - C0 2 continue to decompose to release C0 2 .
- the cooling treatment is performed by cooling the separated high-concentration CO 2 gas to an optimum temperature range of 20 to 35 ° C, and the cooling time is 1 to 5 min. In this way, most of the water vapor can be condensed out and then returned to the analytical column for recycling.
- An apparatus for efficiently and low-energy capture of carbon dioxide in a power plant flue gas by the above method comprising an absorption tower 1, a sloping plate clarification tank 7, a regeneration tower 22, a gas-liquid separator 19, a dryer 18, a compressor 17, and condensation
- the rich liquid at the bottom of the absorption tower 1 is stratified from the inflow swash plate clarification tank 7, and the gas outlet of the gas-liquid separator 19 is sequentially connected in series with the dryer 18, the compressor 17, the condenser 16, and the liquid carbon dioxide storage tank 15.
- the bottom outlet of the swash plate clarifier 7 is connected to the first medium (mixed condensate) input port of the second heat exchanger 23 through a pipe (for the first temperature rise), and the pipe is provided with a rich
- the liquid pump 8 the supernatant overflow port of the swash plate clarifier 7 is connected to the input port of the circulating absorbent tank 10 through a pipe; the outlet of the circulating absorbent tank 10 is sprayed through the pipe and the absorption tower 1
- the spray pipe of the layer 2 is connected, the pipe is provided with an absorption liquid circulation pump 9;
- the first medium (mixed condensate) output port of the second heat exchanger 23 is connected to the first medium (mixed condensate) input port of the first heat exchanger 21 through a pipe (for the second temperature rise), the first change
- the first medium (mixed condensate) output port of the heat exchanger 21 communicates with the inlet of the upper portion of the regeneration tower 22 through a pipe, and the gas discharge port at the top of the second heat exchanger 23 passes through the pipe and the first heat exchanger 21 and the cooler 20
- the connected pipes are connected to each other, and the gas outlet at the upper portion of the regeneration tower 22 communicates with the second medium (gas, heating first medium) input port of the first heat exchanger 21 through the pipe, and the second heat exchanger 21 is second.
- the medium output port is connected to the input port of the cooler 20 through a pipe, and the output port of the cooler 20 is connected to the inlet of the gas-liquid separator 19 through a pipe;
- the liquid outlet in the lower portion of the regeneration tower 22 is connected to the second medium input port of the second heat exchanger 23 through a pipe, the pipe a poor liquid pump 13 is disposed on the road, and a second medium output port of the second heat exchanger 23 is connected to an input port of the circulating absorbent tank 10 through a pipe, and the pipe is provided with a filter 24; the gas-liquid separator
- the condensate overflow port of 19 is connected to the input port of the circulating absorbent tank 10 through a pipe;
- the solution tank 12 for storing the aqueous solution of the composite absorbent is connected to the input port of the circulating absorbent tank 10 through a pipe.
- a solution pump 11 is provided on the pipe.
- the absorption tower 1 is a pneumatic bubble column, and a sieve plate 5 is arranged in the absorption tower 1 between the flue gas inlet 6 at the lower portion of the absorption tower 1 and the flue gas outlet 27 at the top of the absorption tower 1 from bottom to top.
- the pneumatic bubbling layer 4, the packing layer 3 and the demisting device 26, the spray tower 2 is further provided with a spray layer 2, and the spray layer 2 is provided with 2 to 4 spray pipes, each of which is provided with a spray pipe a plurality of nozzles (sprinklers) 25, the ratio of the circular through-hole area of the sieve plate 5 to the plate area is 30 to 40%, and the demisting device 26 is composed of upper and lower two layers of demisting filters and is located at the upper and lower sides.
- the cleaning spray component is formed between the layer demisting filters.
- the internal transfer promotes decomposition and can rapidly regenerate and release carbon dioxide gas. This method has the characteristics of high collection efficiency.
- the aqueous solution of the composite absorbent easily aggregates with each other to form a different liquid layer with water, and the liquid layer of the product containing carbon dioxide is separated and returned to the regeneration tower for regeneration, thereby reducing the amount of the aqueous solution entering the interior of the regeneration tower, thereby greatly reducing the amount of liquid.
- the second heat exchanger (lean-rich liquid heat exchanger) part of the gas dissolved or adsorbed by the composite absorbent in the rich liquid is heated and evaporated by the lean liquid, which reduces the quality of the heated rich liquid entering the regeneration tower. , thereby reducing energy consumption; at the same time, the low-temperature rich liquid from the absorption tower is heated twice by the high-temperature lean liquid at the bottom of the regeneration tower and the high-temperature carbon dioxide gas at the top to increase the temperature of the rich liquid, further reducing the system energy consumption; The heat exchange of the rich liquid cools down, reducing the cooling water consumption of the subsequent cooler and reducing the energy consumption again.
- the method has simple process flow, simple equipment structure, low investment and operation cost.
- the invention overcomes the disadvantages of severe corrosion of the organic amine method, high energy consumption for regeneration, and almost no vapor pressure by using the ionic liquid, thereby reducing the disadvantages of easy loss of the simple organic amine as an absorbent.
- Figure 1 is a schematic view showing the structure of the apparatus of the present invention.
- a method for capturing carbon dioxide in flue gas of a power station with high efficiency and low energy consumption comprising the following steps:
- molar ratio of amine to the organic ionic liquid is 1.01: 1, the organic amines, mixed ionic liquid and water to obtain an aqueous solution of an absorbent composite, wherein the concentration of the complex aqueous absorption of 20wt%;
- the ionic liquid is 1-butyl-3-methylimidazolium tetrafluoroborate in a conventional ionic liquid;
- the organic amine is ethanolamine (MEA);
- An aqueous solution of a composite absorbent composed of an organic amine and an ionic liquid is used as a CO 2 absorbent, and the aqueous solution of the composite absorbent is uniformly sprayed into the flue gas of the power plant boiler after the conventional dust removal and desulfurization treatment, so that the upward moving smoke and the downward movement
- the sprayed composite absorbent aqueous solution is sufficiently reversely contacted, and the CO 2 gas in the flue gas is chemically reacted with the composite absorbent to be absorbed by the gas-liquid two-phase chemical reaction;
- the control liquid-gas ratio is 20L/m 3 (liquid refers to the composite absorbent aqueous solution, the gas refers to the flue gas), and the reaction temperature of the flue gas (the combination of 0 2 and the composite absorbent aqueous solution is 50 ° C, and the inlet pressure of the absorption tower is 1. 2atm ; thus, the aqueous composite absorbent solution can react fully and completely with CO 2 in the flue gas at a suitable temperature and pressure to form a liquid rich in A ⁇ (: 0 2 and B ⁇ C0 2 , A is Organic amine; B is a functionalized ionic liquid;
- a ⁇ C0 2 is rapidly decomposed first, that is, A ⁇ C0 2 decomposes to generate eight, and releases C0 2 , B * (: 0 2 is not easy to release C0 2 under this condition ; since A will easily absorb in solution B ⁇ C0 2 in C0 2 generates A ⁇ C0 2 , then A ⁇ C0 2 continues to decompose to release C0 2; regeneration to obtain a high concentration of CO 2 gas and a composite absorbent aqueous solution;
- step 5 The high-concentration C0 2 gas separated in step 3) is cooled to coagulate the hot water vapor contained therein; the cooling treatment is to cool the separated high-concentration CO 2 gas to 30 ° C ( The cooling time is L 5min) ; in this way, most of the water vapor can be condensed out and then returned to the analytical tower for recycling;
- Step 5) The high concentration of the cooling treatment (: 0 2 gas passes through the gas-liquid separator, gas-liquid separation treatment, and the condensed water vapor is separated to obtain C0 2 gas having a purity higher than 99%;
- step 6) The high purity obtained in step 6) (: 0 2 gas is further dried (drying temperature is 110 ° C, time is 2 min), and then subjected to compressor compression and heat exchange condensation treatment to 20 ° C, 72 atm, which becomes Liquid C0 2 can be used to produce high-concentration industrial grade liquid carbon dioxide products. , measured by experiment:
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- an apparatus for efficiently capturing carbon dioxide in a power plant flue gas with high efficiency and low energy consumption comprising an absorption tower 1, a sloping plate clarification tank 7, a second heat exchanger 23, and a first heat exchanger 21 , regeneration tower 22, gas-liquid separator 19, dryer 18, compressor 17 and condenser 16;
- the absorption tower 1 is a pneumatic bubble column, the upper part of the absorption tower 1 is a packing layer, the middle part is a pneumatic bubbling layer, the lower layer is a sieve plate; the regeneration tower 22 is a sieve plate tower;
- the spray tower 2 is further provided with a spray layer 2, and the spray layer 2 is provided with a total of 2 to 4 spray pipes (three in Fig.
- each nozzle has a plurality of nozzles (sprinklers) 25 (the specific number is determined according to the flow rate, generally each spray pipe) 2-20 nozzles are provided), the ratio of the circular through hole area of the sieve plate 5 to the plate area is 30 to 40%, and the demisting device 26 is composed of upper and lower two layers of demisting filters and upper and lower layers.
- the cleaning spray component between the demisting filters is configured to completely remove the composite absorbent droplets entrained in the flue gas;
- the rich liquid outlet at the bottom of the absorption tower 1 is connected to the input port of the swash plate clarification tank 7 through a pipe, and the rich liquid at the bottom of the absorption tower 1 is stratified from the inflow swash plate clarification tank 7, and the supernatant in the swash plate clarification tank 7 is stratified.
- the underflow in the swash plate clarification tank 7 is mainly a product mixed condensate
- the bottom outlet of the swash plate clarifier 7 passes through the pipe and the first medium of the second heat exchanger 23 ( Mixed condensate liquid)
- the input port is connected to each other (for the first temperature rise), the pipeline is provided with a rich liquid pump 8, and the supernatant overflow port of the swash plate clarifier 7 is passed through the pipeline and the circulating absorbent tank 10
- the inlet port is connected to the outlet; the outlet of the circulating absorbent tank 10 is connected to the spray pipe of the spray layer 2 in the absorption tower 1 through a pipe, and the pipe is provided with an absorption liquid circulation pump 9;
- the first medium (mixed condensate) output port of the second heat exchanger 23 is connected to the first medium (mixed condensate) input port of the first heat exchanger 21 through a pipe (for the second temperature rise), the first change
- the first medium (mixed condensate) output port of the heat exchanger 21 communicates with the inlet of the upper portion of the regeneration tower 22 through a pipe, and the gas discharge port at the top of the second heat exchanger 23 passes through the pipe and the first heat exchanger 21 and the cooler 20
- the connected pipes are connected to each other, and the gas outlet at the upper portion of the regeneration tower 22 communicates with the second medium (gas, heating first medium) input port of the first heat exchanger 21 through the pipe, and the second heat exchanger 21 is second.
- the medium output port is connected to the input port of the cooler 20 through a pipe, and the output port of the cooler 20 is connected to the inlet of the gas-liquid separator 19 through a pipe;
- the reboiler 14 associated with the regeneration tower 22 is disposed outside the bottom of the regeneration tower, and the outlet of the reboiler 14 is connected to the bottom reservoir of the regeneration tower through a pipeline, and the inlet of the reboiler 14 passes through the pipeline and the bottom of the regeneration tower.
- the liquid storage tank is connected; the regeneration tower ,
- the liquid outlet of the lower portion of the 22 is connected to the second medium inlet of the second heat exchanger 23 through a pipe, the pipe is provided with a lean liquid pump 13, and the second medium output port of the second heat exchanger 23 is passed through the pipe and the circulation
- the input port of the absorbing liquid tank 10 is connected, and the pipe is provided with a filter 24;
- the gas outlet of the gas-liquid separator 19 is sequentially connected in series with the dryer 18, the compressor 17, the condenser 16, and the liquid carbon dioxide storage tank 15; the condensate overflow port of the gas-liquid separator 19 passes through the pipeline and the circulating absorption liquid tank
- the input ports of 10 are connected;
- the solution tank 12 for storing the aqueous solution of the composite absorbent is connected to the input port of the circulating absorbent tank 10 through a pipe, and the pipe is provided with a solution pump 11 (the supplementary aqueous solution of the composite absorbent and water are added to the solution tank) 12).
- a sieve plate for uniformly distributing the flue gas and contacting the gas and liquid is disposed above the flue gas inlet of the lower portion of the absorption tower, and the ratio of the pore area to the plate area of the sieve plate is 30 to 40%.
- the airflow distribution is more uniform, effectively eliminating the dead angle of the flue gas flow, and facilitating the full contact between the flue gas and the absorbent solution; on the other hand, under the interaction of multiple sets of spray pipes
- the spray coverage of the cross section of the absorption tower can reach 300% or more, and the carbon dioxide in the flue gas can be sufficiently contacted with the absorption liquid to be fully and completely reacted and absorbed.
- the lean-rich liquid heat exchanger is arranged, and the rich liquid outlet at the bottom of the swash plate clarification tank is connected to the upper inlet of the regeneration tower through the rich liquid pump, the second (poor and rich liquid) heat exchanger, and the regeneration tower lean liquid
- the outlet is connected to the upper inlet of the circulating absorbent tank through a lean pump and a second (lean-rich) heat exchanger.
- the flue gas inlet 6 at the lower part of the absorption tower 1 enters the absorption tower 1, and the air flow distribution through the sieve plate 5, the pneumatic bubbling layer 4, and the packing layer 3 rise.
- the aqueous solution of the composite absorbent is sprayed downward through the spray layer 2, and the ratio of the control liquid to gas is in the range of 5 to 25 L/m 3 , and the reaction temperature of the CO 2 in the flue gas and the aqueous solution of the composite absorbent may preferably be 40 to 40. 01 ⁇ 10atm ⁇ The reaction pressure is 0. 01 ⁇ 10atm.
- the CO 2 gas in the flue gas is sufficiently in reverse contact with the aqueous solution of the composite absorbent at the filler layer 3 and the pneumatic bubble layer 4, and C0 2 is chemically absorbed or adsorbed into the solution.
- the defogging device 26 disposed at the top of the absorption tower 1 removes the absorbent droplets, the clean flue gas is directly discharged into the atmosphere, and the absorption of C0 2 is generated.
- the rich liquid falls into the bottom of the absorption tower 1, and is condensed and stratified from the inflow swash plate clarification tank 7, the supernatant liquid is a solution containing a small amount of composite absorbent, and the bottom stream is mainly composed of agglomerated composite absorbent product slurry.
- the bottom flow of the tank is transported by the rich liquid pump 8 through the tube of the second heat exchanger (lean rich liquid heat exchanger) 23 for one temperature rise, the second heat is raised in the first heat exchanger 21, and then sent from the upper portion of the regeneration tower 22 the column-rich liquid through a second heat exchanger (heat exchanger liquid wealth) 23 after heating, partially dissolved or adsorbed C0 2 gas is released.
- the second heat exchanger lean rich liquid heat exchanger
- the absorbed or adsorbed C0 2 rich liquid is sprayed to the regeneration tower 22, passes through each sieve plate in turn, and the product of the composite absorbent is applied.
- the liter of steam is heated and decomposed, co 2 is released, and the decomposed composite absorbent product slurry falls into the bottom of the column, and is heated to 80 to 110 ° C through the bottom reboiler 14 to further analyze the high concentration of C0 2 gas.
- the composite absorbent product is completely resolved.
- the resolved (: 0 2 gas flows out from the upper gas outlet of the regeneration tower 22 along with a large amount of water vapor, enters the first heat exchanger 21, and is rich after being heated by the second heat exchanger (lean rich liquid heat exchanger) 23
- the liquid is heated again, and after the heat exchange, the gas is mixed with the gas released by the second heat exchanger (the rich and the thin liquid heat exchanger) 23, and then enters the cooler 20, where the C0 2 gas stream is cooled to 25 to 35 ° C.
- Most of the water vapor is condensed out.
- the composite absorbent solution generated by the decomposition of the regeneration tower 22 is lifted by the lean liquid pump 13 and then introduced into the second heat exchanger (lean rich liquid heat exchanger). The heat of the tube is released and cooled, and then enters the filter 24 to remove the flue gas.
- the dissolved heavy metal or the reaction-generated impurities, the pure composite absorbent solution is processed from the high level into the circulating absorbent tank 10, the supplementary composite absorbent and the process water are added to the solution storage tank 12, and the solution storage tank 12 is passed.
- the solution pump 11 is replenished to the circulating absorbent tank 10.
- the circulating absorption liquid is transported to the spray layer 2 in the absorption tower through the absorption liquid circulation pump for spray absorption.
- a method for capturing carbon dioxide in flue gas of a power station with high efficiency and low energy consumption comprising the following steps:
- the functionalized ionic liquid is an ionic liquid to which an amino group is introduced, and the functionalized ionic liquid is ⁇ - ⁇ -aminopropyl)-3-methylimidazolium bromide;
- the organic amine is ⁇ -methyldiethanolamine (MDEA);
- An aqueous solution of a composite absorbent composed of an organic amine and an ionic liquid is used as a CO 2 absorbent, and the aqueous solution of the composite absorbent is uniformly sprayed into the flue gas of the power plant boiler after the conventional dust removal and desulfurization treatment, so that the upward moving smoke and the downward movement
- the sprayed composite absorbent aqueous solution is sufficiently reversely contacted, and the CO 2 gas in the flue gas is chemically reacted with the composite absorbent to be absorbed by the gas-liquid two-phase chemical reaction;
- the control liquid-gas ratio is 20L/m 3 (liquid refers to the composite absorbent aqueous solution, the gas refers to the flue gas), and the reaction temperature of the flue gas (the combination of 0 2 and the composite absorbent aqueous solution is 50 ° C, and the inlet pressure of the absorption tower is 1. 2atm ; thus, the aqueous composite absorbent solution can react fully and completely with CO 2 in the flue gas at a suitable temperature and pressure to form a liquid rich in A ⁇ (: 0 2 and B ⁇ C0 2 , A is Organic amine; B is a functionalized ionic liquid;
- a ⁇ C0 2 is rapidly decomposed first, that is, A ⁇ C0 2 decomposes to generate eight, and releases C0 2 , B * (: 0 2 is not easy to release C0 2 under this condition ; since A will easily absorb in solution B ⁇ C0 2 in C0 2 generates A ⁇ C0 2 , then A ⁇ C0 2 continues to decompose to release C0 2; regeneration to obtain a high concentration of CO 2 gas and a composite absorbent aqueous solution;
- step 5 The high-concentration C0 2 gas separated in step 3) is cooled to coagulate the hot water vapor contained therein; the cooling treatment is performed to cool the separated high concentration (: 0 2 gas to 30 °) C (cooling time is L 5min) ; in this way, most of the water vapor can be condensed out and then returned to the analytical tower for recycling;
- Step 5) The high concentration of the cooling treatment (: 0 2 gas passes through the gas-liquid separator, gas-liquid separation treatment, and the condensed water vapor is separated to obtain C0 2 gas having a purity higher than 99%;
- the high-purity CO 2 gas obtained in the step 6) is further dried (drying temperature is 110 ° C, time is 2 min), and then subjected to compressor compression and heat exchange condensation treatment to 20 ° C, 72 atm, which becomes liquid C0. 2 , can be made into high-concentration industrial grade liquid carbon dioxide products.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 46 X 10 7 kJ / h , 30.5% reduction in energy consumption.
- a method for capturing carbon dioxide in flue gas of a power station with high efficiency and low energy consumption comprising the following steps:
- the ionic liquid is a polymeric ionic liquid, and the polymeric ionic liquid is poly 1_(4-styryl)-3-methylimidazole tetrafluoroborate;
- the organic amines are ethanolamine (MEA) and N-methyldiethanolamine (MDEA), ethanolamine (MEA) and N-methyldiethanolamine (MDEA) each occupy 1/2;
- An aqueous solution of a composite absorbent composed of an organic amine and an ionic liquid is used as a CO 2 absorbent, and the aqueous solution of the composite absorbent is uniformly sprayed into the flue gas of the power plant boiler after the conventional dust removal and desulfurization treatment, so that the upward moving smoke and the downward movement
- the sprayed composite absorbent aqueous solution is sufficiently reversely contacted, and the CO 2 gas in the flue gas is chemically reacted with the composite absorbent to be absorbed by the gas-liquid two-phase chemical reaction;
- control liquid-gas ratio is 20L / m 3 (liquid refers to composite absorbent aqueous solution, gas refers to flue gas), in the flue gas (: 0 2 and the composite absorbent aqueous solution reaction temperature is 50 ° C range, absorption tower inlet pressure 1.
- the aqueous solution of the composite absorbent can be fully and completely reacted with CO 2 in the flue gas at a suitable temperature and pressure to form a liquid rich in A ⁇ (: 0 2 and B ⁇ C0 2 , A Is an organic amine; B is a functionalized ionic liquid;
- a ⁇ C0 2 is rapidly decomposed first, that is, A ⁇ C0 2 decomposes to generate eight, and releases C0 2 , B * (: 0 2 is not easy to release C0 2 under this condition ; since A will easily absorb in solution B ⁇ C0 2 in C0 2 generates A ⁇ C0 2 , then A ⁇ C0 2 continues to decompose to release C0 2; regeneration to obtain a high concentration of CO 2 gas and a composite absorbent aqueous solution;
- step 5 The high-concentration C0 2 gas separated in step 3) is cooled to coagulate the hot water vapor contained therein; the cooling treatment is to cool the separated high-concentration CO 2 gas to 30 ° C ( The cooling time is L 5min) ; in this way, most of the water vapor can be condensed out and then returned to the analytical tower for recycling;
- step 5) in step 5) a high concentration of cooling process (: 02 through the gas-liquid separator, gas-liquid separation process, the separated condensed water vapor, C0 2 gas to obtain a purity higher than 99%;
- step 6) The high purity obtained in step 6) (: 0 2 gas is further dried (drying temperature is 110 ° C, time is 2 min), and then subjected to compressor compression and heat exchange condensation treatment to 20 ° C, 72 atm, which becomes Liquid C0 2 can be used to produce high-concentration industrial grade liquid carbon dioxide products.
- the absorption gas inlet C0 2 content of the absorption tower is 12%, the absorption tower outlet flue gas C0 2 content is 0.6%, the carbon dioxide absorption efficiency is 95%; the conventional MEA absorption C0 2 regeneration energy consumption is 2. 1 X 10 7 kJ/h, The energy consumption was reduced by 1.49 X 10 7 kJ/h, and the energy consumption was reduced by 29.1%.
- Example 2 It is basically the same as Example 1, except that the molar ratio of organic amine to ionic liquid is 1:1, and the organic amine, ionic liquid and water are mixed to obtain a composite absorbent aqueous solution, wherein the concentration of the composite absorbent aqueous solution is 30wt%.
- step 1) the control liquid-gas ratio is 5 L/m 3
- the reaction temperature of C0 2 in the flue gas and the aqueous solution of the composite absorbent is 40 ° C
- the reaction pressure is 0. 01atm o
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- step 1) the control liquid-gas ratio is 25 L/m 3 , and the reaction temperature in the flue gas (: 0 2 and the composite absorbent aqueous solution is 55 ° C, and the reaction pressure is 10atm.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- the heating analysis process is performed under the conditions of temperature 80 to V and pressure O. Olatm, and the analysis time is lmin.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- Example 2 It is basically the same as Example 1, except that in the above step 3), the heating analysis process is analyzed at a temperature of 110 V and a pressure of 10 atm, and the analysis time is 5 min.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- Example 9 It is basically the same as Example 1, except that in the above step 5), the cooling treatment is performed by cooling the separated high concentration (0 2 gas to 20 ° C, and the cooling time is 1 min.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- Example 2 Basically the same as Example 1, except that in the above step 5), the cooling treatment was carried out by cooling the separated high concentration (: 0 2 gas to 35 ° C, and the cooling time was 5 min.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- step 7 the drying temperature is 110 ° C, the time is 0. lmin. Tested by experiment:
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- step 7 the drying temperature is 110 ° C and the time is 5 min. Tested by experiment:
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- Example 2 It is basically the same as Example 1, except that the ionic liquid is 1-butyl-3-methylimidazolium hexafluorophosphate in a conventional ionic liquid.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- Example 2 It is basically the same as Example 1, except that the ionic liquid is 1-hexyl-3-methylimidazolium bistrifluoromethanesulfonimide salt in a conventional ionic liquid.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- Example 2 It is basically the same as Example 1, except that the ionic liquid is 1-hexyl-3-methylimidazolium hexafluorophosphate in a conventional ionic liquid.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- the ionic liquid is 1-butyl-3-methylimidazolium hexafluorophosphate, 1-hexyl-3-methylimidazolium trifluorophosphate in a conventional ionic liquid.
- Methanesulfonimide salt and 1-hexyl-3-methylimidazolium hexafluorophosphate are each used in an amount of 1/3.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- the ionic liquid is a conventional ionic liquid and a functionalized ionic liquid, each of which accounts for 1/2;
- the traditional ionic liquid is 1-butyl-3-methylimidazolium tetrafluoroborate; the functionalized ionic liquid is iota- ⁇ -aminopropyl , benzyl)-3-methylimidazolium bromide.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- the ionic liquid is a conventional ionic liquid, a functionalized ionic liquid and a polymeric ionic liquid, each of which accounts for 1/3;
- the conventional ionic liquid is 1-butyl-3-methylimidazolium tetrafluoroborate; the functionalized ionic liquid is iota- ⁇ -aminopropyl)-3-methylimidazolium bromide; The liquid is poly 1_(4-styryl)-3-methylimidazolium tetrafluoroborate.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 52 X 10 7 kJ / h , 27.6% reduction in energy consumption.
- Example 2 It is basically the same as in Example 2 except that the functionalized ionic liquid is 1-(3propylamino)-3-butylimidazole tetrafluoroborate.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 46 X 10 7 kJ / h , 30.5% reduction in energy consumption.
- the functionalized ionic liquid is i- ⁇ -aminopropyl)-3-methylimidazolium bromide and 1-(3propylamino)-3-butylimidazole Tetrafluoroborate, the amount of each accounted for 1/2.
- MEA conventional C0 2 absorption of energy regeneration 2. 1 X 10 7 kJ / h , measured experimentally reproducing this energy consumption 1. 46 X 10 7 kJ / h , 30.5% reduction in energy consumption.
- Example 21 It is basically the same as Example 3 except that the polymerized ionic liquid is poly-1-(4-styryl)-3-methylimidazolium hexafluorophosphate.
- the absorption gas inlet C0 2 content of the absorption tower is 12%, the absorption tower outlet flue gas C0 2 content is 0.6%, the carbon dioxide absorption efficiency is 95%; the conventional MEA absorption C0 2 regeneration energy consumption is 2. 1 X 10 7 kJ/h, The energy consumption was reduced by 1.49 X 10 7 kJ/h, and the energy consumption was reduced by 29.1%.
- Example 3 It is basically the same as Example 3 except that the polymerized ionic liquid is poly-1-(4-styryl)-3-methylimidazolium benzalsulfonimide salt.
- the absorption gas inlet C0 2 content of the absorption tower is 12%, the absorption tower outlet flue gas C0 2 content is 0.6%, the carbon dioxide absorption efficiency is 95%; the conventional MEA absorption C0 2 regeneration energy consumption is 2. 1 X 10 7 kJ/h, The energy consumption was reduced by 1.49 X 10 7 kJ/h, and the energy consumption was reduced by 29.1%.
- polymerized ionic liquid is poly-1_(4-styryl)-3-methylimidazolium trifluoromethanesulfonimide salt and poly-1-(4-styrene).
- Base -3-methylimidazolium tetrafluoroborate, each in an amount of 1/2.
- the absorption gas inlet C0 2 content of the absorption tower is 12%, the absorption tower outlet flue gas C0 2 content is 0.6%, the carbon dioxide absorption efficiency is 95%; the conventional MEA absorption C0 2 regeneration energy consumption is 2. 1 X 10 7 kJ/h, The energy consumption was reduced by 1.49 X 10 7 kJ/h, and the energy consumption was reduced by 29.1%.
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SG11201403509SA SG11201403509SA (en) | 2011-12-23 | 2012-10-26 | Method for capturing carbon dioxide in power station flue gas and device therefor |
AP2014007785A AP2014007785A0 (en) | 2011-12-23 | 2012-10-26 | Method for capturing carbon dioxide in power station flue gas and device therefor |
CA2859841A CA2859841A1 (en) | 2011-12-23 | 2012-10-26 | Method for capturing carbon dioxide in power station flue gas and device therefor |
EP12859719.2A EP2796183B1 (en) | 2011-12-23 | 2012-10-26 | Method for capturing carbon dioxide in power station flue gas and device therefor |
DK12859719.2T DK2796183T3 (en) | 2011-12-23 | 2012-10-26 | Process for the collection of carbon dioxide in flue gas in a power plant and apparatus therefor |
RU2015101990/05A RU2600348C2 (ru) | 2011-12-23 | 2012-10-26 | Способ улавливания углекислого газа из дымового газа электростанции и установка для его осуществления |
KR1020147018985A KR101545604B1 (ko) | 2011-12-23 | 2012-10-26 | 발전소 연도 가스의 이산화탄소 포집 방법 및 그 장치 |
BR112014015304A BR112014015304A2 (pt) | 2011-12-23 | 2012-10-26 | método para capturar dióxido de carbono em uma central elétrica de gás de combustão e um dispositivo para o mesmo |
JP2014547682A JP5945333B2 (ja) | 2011-12-23 | 2012-10-26 | 発電所排煙の二酸化炭素回収方法および装置 |
AU2012357358A AU2012357358B2 (en) | 2011-12-23 | 2012-10-26 | Method for capturing carbon dioxide in power station flue gas and device therefor |
MX2014007608A MX359692B (es) | 2011-12-23 | 2012-10-26 | Método para capturar dióxido de carbono en gas de combustión de estación de energía y dispositivo para ello. |
US14/311,379 US9669354B2 (en) | 2011-12-23 | 2014-06-23 | Method and apparatus for collecting carbon dioxide from flue gas |
ZA2014/05332A ZA201405332B (en) | 2011-12-23 | 2014-07-21 | Method for capturing carbon dioxide in power station flue gas and device therefor |
US15/593,294 US10155194B2 (en) | 2011-12-23 | 2017-05-11 | Method and apparatus for collecting carbon dioxide from flue gas |
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EP2796183A4 (en) | 2015-10-28 |
RU2015101990A (ru) | 2016-08-10 |
KR101545604B1 (ko) | 2015-08-19 |
EP2796183A1 (en) | 2014-10-29 |
EP2796183B1 (en) | 2018-07-04 |
US20140301929A1 (en) | 2014-10-09 |
JP2015507526A (ja) | 2015-03-12 |
SG11201403509SA (en) | 2014-09-26 |
AP2014007785A0 (en) | 2014-07-31 |
DK2796183T3 (en) | 2018-10-08 |
RU2600348C2 (ru) | 2016-10-20 |
MX359692B (es) | 2018-10-08 |
US9669354B2 (en) | 2017-06-06 |
US10155194B2 (en) | 2018-12-18 |
MX2014007608A (es) | 2015-05-15 |
CN102553396B (zh) | 2014-06-04 |
US20170274319A1 (en) | 2017-09-28 |
JP5945333B2 (ja) | 2016-07-05 |
ZA201405332B (en) | 2015-10-28 |
AU2012357358A1 (en) | 2014-07-17 |
CN102553396A (zh) | 2012-07-11 |
AU2012357358B2 (en) | 2016-05-26 |
KR20140109426A (ko) | 2014-09-15 |
MY170461A (en) | 2019-08-02 |
BR112014015304A2 (pt) | 2017-07-04 |
CA2859841A1 (en) | 2013-06-27 |
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