WO2012070523A1 - 燃焼排ガス中の二酸化炭素除去装置 - Google Patents
燃焼排ガス中の二酸化炭素除去装置 Download PDFInfo
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- WO2012070523A1 WO2012070523A1 PCT/JP2011/076789 JP2011076789W WO2012070523A1 WO 2012070523 A1 WO2012070523 A1 WO 2012070523A1 JP 2011076789 W JP2011076789 W JP 2011076789W WO 2012070523 A1 WO2012070523 A1 WO 2012070523A1
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- combustion exhaust
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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
- B01D53/14—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
- B01D53/1418—Recovery of products
-
- 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
-
- 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
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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
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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
- 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 present invention carbon dioxide in the combustion exhaust gas (CO 2) removal apparatus and a method, in particular CO 2 removing device that prevents the release of the amine compound from CO 2 absorber using an aqueous solution of an amine compound as a CO 2 absorbing solution And methods.
- CO 2 removing device that prevents the release of the amine compound from CO 2 absorber using an aqueous solution of an amine compound as a CO 2 absorbing solution And methods.
- Patent Document 1 proposes a method of performing decarboxylation by using an aqueous solution of an amine compound as a CO 2 absorbent.
- the reaction between CO 2 and the amine compound is an exothermic reaction, the temperature of the absorbing solution in the CO 2 absorption portion increases and the vapor pressure of the amine compound increases. That is, since a large amount of the absorbing solution evaporates as the temperature rises, the amount of amine compound accompanying the decarbonation gas increases.
- Patent Document 2 proposes a method in which the water washing section has a multistage structure.
- FIG. 2 shows an example of such a conventional CO 2 removal device, which is a contact portion (filling portion) 2 for bringing the combustion exhaust gas and an amine compound aqueous solution into countercurrent contact, and is included in the combustion exhaust gas.
- a decarboxylation tower 1 that removes carbon dioxide (CO 2 )
- a regeneration tower 13 that regenerates the aqueous solution of the amine compound by heating the aqueous solution of the amine compound discharged from the decarboxylation tower 1, and the regeneration tower 13
- a recirculation means (reflux water supply line) 21 is provided for recirculating the regenerated aqueous solution of the amine compound to the decarboxylation tower 1 through the cooler 19.
- 3 is a combustion exhaust gas supply line
- 4 is a de-CO 2 combustion exhaust gas
- 5 is an amine compound aqueous solution supply line
- 6, 9, 14, and 20 are nozzles
- 7 is a water circulation pump
- 8 is a cooler
- 10 is CO 2 absorbing amine compound extraction line
- 11 is a gas to be treated
- 12 is a blower
- 15 is a lower packing section of a regeneration tower
- 16 is a pump
- 17 is a CO 2 separator
- 18 is exhausted CO 2
- 22 is a heat exchanger.
- 23 is a reboiler
- 24 is a washing section
- 25 is an upper packing section of the regeneration tower.
- a carbon dioxide removing apparatus comprising a regeneration tower for regenerating an aqueous solution of an amine compound by heating an aqueous solution, and a reflux means for refluxing the aqueous solution of the amine compound regenerated in the regeneration tower to the decarboxylation tower through a cooler.
- the contact portion where the reflux water of the regeneration tower and the combustion exhaust gas from which CO 2 has been removed is counter-contacted has a two-stage configuration
- the cooler on the downstream side of the regeneration tower has a two-stage configuration.
- the reflux water from the first cooler is supplied to the first-stage contact portion
- the reflux water from the second-stage cooling tower is supplied to the second-stage contact portion.
- Carbon dioxide removal equipment (2)
- the amount of the amine compound aqueous solution refluxed from the cooler to the decarbonation tower is adjusted so that the temperature of the combustion exhaust gas is as equal as possible at the decarbonation tower inlet and outlet.
- the reflux water from the cooler at the top of the amine regeneration tower can be efficiently used for removing the amine at the top of the absorption tower, and the concentration of amine released from the de-CO 2 tower can be reduced.
- Illustration of CO 2 removing device according to an embodiment of the present invention Illustration of a conventional CO 2 removal device.
- the amine compound used in the CO 2 absorbing solution includes monoethanolamine, alcoholic hydroxyl group-containing primary amines such as 2-amino-2-methyl-1-propanol, diethanolamine, and 2-methylaminoethanol.
- carbon dioxide absorption accelerators or corrosion inhibitors, and methanol, polyethylene glycol, sulfolane, etc. can be added to the absorbing solution as other media.
- de-CO 2 column 1 established a demister at the exit of the washing section 24, part of the washing water mist fed to a part or the washing section 24 of the absorption liquid mist is supplied to the de-CO 2 column 1 is removed It may be released together with the CO 2 exhaust gas to prevent loss of moisture and amine compounds.
- the water washing section 24 may be a packed tower or a tray tower.
- the pressure of the carbon dioxide-containing gas to be decarboxylated may be pressurized or normal pressure, the temperature may be low or high, and there is no particular limitation. .
- it is an atmospheric pressure combustion exhaust gas.
- FIG. 1 is an explanatory view of a carbon dioxide removing apparatus showing an embodiment of the present invention.
- the cooler 19 on the downstream side of the regeneration tower 13 has a two-stage structure, and the dewatered tower is supplied with the reflux water from the first stage cooler via the pump 16 and the line 21A. That is, the first stage of the first washing unit 24 and the reflux water from the second stage cooler are respectively supplied to the second stage of the washing unit 24 of the decarbonation tower 1 via the line 21B. That is, when the water-washing part on the downstream side of the de-CO 2 tower is divided into a plurality of stages, the amine concentration in the de-CO 2 combustion exhaust gas decreases toward the rear stage side.
- the temperature at the outlet of the regeneration tower 13 of the combustion exhaust gas containing the amine compound vapor that has been de-CO 2 is about 100 ° C., and contains the amine compound of the saturated vapor pressure.
- the gas temperatures at the inlets of the first and second stage coolers 19 are about 100 ° C. and about 70 ° C., respectively, and the concentration of amine compounds contained in the condensed water from the cooler is more than five times that of the second stage. It becomes.
- the amine concentration in the de-CO 2 combustion exhaust gas is low and the amine concentration in water is high, the amine may move from water to gas, which may have the opposite effect.
- the present invention supplies a higher water of amine concentration from the first stage of the cooler to a high washing section preceding stage of amine concentration of de-CO 2 combustion exhaust gas, a low amine concentration of de-CO 2 combustion exhaust gas washing
- the lower amine concentration water from the second stage cooler is supplied to the rear stage of the section to improve the amine removal efficiency in the decarbonation tower water washing section.
- the combustion exhaust gas 11 is supplied to the de-CO 2 tower 1 by a blower 12 and is brought into countercurrent contact with an aqueous solution of a fixed concentration amine compound supplied from a nozzle 6 at a contact portion (filling portion) 2.
- CO 2 in the combustion exhaust gas is absorbed and removed by an aqueous solution of an amine compound, removing CO 2 combustion exhaust gas directed to the washing section 24.
- the aqueous solution of the amine compound supplied to the de-CO 2 tower 1 absorbs CO 2, and due to the heat of reaction due to the absorption, it becomes higher than the temperature at the supply port 3, sent to the heat exchanger 22, heated and regenerated. Guided to tower 13.
- the temperature of the aqueous solution of the amine compound supplied to the de-CO 2 tower 1 is adjusted by the cooler 19 or, if necessary, the heat exchanger 22 provided between the cooler 19 and the aqueous solution supply port 6 of the amine compound. Can do. After the system reaches a steady state, the temperature of the aqueous solution of the amine compound in the de-CO 2 tower 1 is usually constant.
- the temperature of the combustion exhaust gas hardly rises due to the reaction heat, and the de-CO 2 tower 1 is raised and discharged at substantially the same temperature as the supply temperature of the combustion exhaust gas supply port 3.
- the de-CO 2 tower 1 is raised and discharged at substantially the same temperature as the supply temperature of the combustion exhaust gas supply port 3.
- the same are included in substantially the same range in some states a temperature difference of water balance of the de CO 2 column 1 below is maintained even if.
- the combustion exhaust gas temperature is the same at the entrance and exit of the de CO 2 column 1, by adjusting the temperature of the aqueous solution of the amine compound fed from the solution feed opening 6 of the amine compound, removing CO 2 column 1, further The water balance of the whole system of FIG. 1 will be maintained. Further, even if the temperature of the combustion exhaust gas discharged from the de-CO 2 tower 1 is high, the amine compound system is used by the apparatus and method of the present invention in which the reflux water from the regeneration tower 13 is used for the de-CO 2 tower 1 as described later. Emission to the outside can be effectively prevented.
- the aqueous solution of the amine compound is regenerated by heating with the reboiler 23, extracted from the bottom of the tower, cooled by the heat exchanger 22, and then returned to the de-CO 2 tower 1.
- the CO 2 separated from the aqueous solution of the amine compound comes into contact with the reflux water supplied from the nozzle 20, exits the top of the tower, and is further cooled by the regeneration tower reflux cooler 19.
- the water vapor accompanying the CO 2 is separated from the condensed reflux water by the two separator 17 and led to the CO 2 recovery step through the line 18.
- a part of the reflux water is refluxed to the regeneration tower 13 by the reflux water pump 16.
- a part of the reflux water is supplied to the de-CO 2 tower 1 through the nozzle 9 by the regeneration tower reflux water supply line 21A as described above.
- the cooler on the downstream side of the regeneration tower 13 is used. 19 has a two-stage structure, and the reflux water from the first-stage cooler is supplied to the first stage of the water washing section 24 of the decarbonation tower 1 via the pump 16 and the line 21A, and the reflux water from the second-stage cooler is supplied to the first stage. Each is supplied to the second stage of the water washing section 24 of the decarbonation tower 1 via the line 21B.
- Combustion exhaust gas containing amine compound vapor de-CO 2 is brought into countercurrent contact with the reflux water at the portion constituted by the filling portion or tray 24 to reduce the amine compound vapor in the combustion exhaust gas to almost zero.
- the water having the higher amine concentration from the first stage cooler is supplied to the upstream side of the water washing section having a higher amine concentration in the combustion exhaust gas de-CO 2 as described above, and the combustion is de-CO 2.
- the amine removal efficiency in the decarbonation tower water washing section can be significantly improved. it can.
- Example 1 Using the apparatus shown in FIG. 1, combustion exhaust gas 30Nm 3 / h containing 10% CO 2 is supplied to the contact part of the decarbonation tower 1, and an aqueous solution (absorbing liquid) of an alcoholic hydroxyl group-containing secondary amine is used as an absorbing liquid. Carbon dioxide was absorbed by contact. The remaining decarbonized exhaust gas was brought into counter-current contact with the wash water at a liquid / gas ratio of 2 L / Nm 3 from the outlet of the contact part in the first stage water washing part.
- the CO 2 exhaust gas was brought into counter-current contact with the cleaning water at a liquid / gas ratio of 2 L / Nm 3 in the second stage washing section, passed through the demister at the outlet of the second stage washing section, and then discharged out of the system.
- the cooler 19 on the downstream side of the regeneration tower 13 has a two-stage configuration, and the inlet temperatures of the first and second stage coolers are 100 ° C. and 70 ° C., respectively, and the condensed water from the first stage cooler Was supplied to the first-stage flushing section at 0.5 L / h, and the condensed water from the second-stage cooler was fed to the second-stage flushing section at 0.6 L / h.
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- Oil, Petroleum & Natural Gas (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Health & Medical Sciences (AREA)
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Abstract
Description
(1)燃焼排ガスとアミン化合物の水溶液を向流接触させる接触部で、燃焼排ガス中に含まれる二酸化炭素(CO2)を除去する脱炭酸塔と、該脱炭酸塔から排出されたアミン化合物の水溶液を加熱してアミン化合物の水溶液を再生する再生塔と、該再生塔で再生されたアミン化合物の水溶液を冷却器を経て前記脱炭酸塔に還流させる還流手段とを有する二酸化炭素除去装置であって、前記再生塔の還流水とCO2が除去された燃焼排ガスが向流接触する接触部を2段構成とし、さらに前記再生塔後流側の前記冷却器を2段構成とし、1段目の冷却器からの還流水は1段目の接触部に供給し、2段目の冷却塔からの還流水は2段目の接触部に供給するように構成したことを特徴とする燃焼排ガス中の二酸化炭素除去装置。
(2)燃焼排ガスの温度が、脱炭酸塔入口と出口とで可及的に同一となるように、前記冷却器から脱炭酸塔に還流されるアミン化合物水溶液の量を調節することを特徴とする(1)記載の装置を用いた燃焼排ガス中の二酸化炭素除去方法。
また、脱炭酸処理の対象となる二酸化炭素含有ガスの圧力は加圧であっても、常圧であってもよく、温度は低温であっても、高温であってもよく、特に制限はない。好ましくは、常圧の燃焼排ガスである。
[実施例1]
図1の装置を用い、CO2を10%含む燃焼排ガス30Nm3/hを脱炭酸塔1の接触部に供給し、吸収液としてアルコール性水酸基含有2級アミンの水溶液(吸収液)と向流接触させて二酸化炭素を吸収した。残りの脱炭酸排ガスを前記接触部出口から、一段目の水洗部にて洗浄水と液/ガス比2L/Nm3で向流接触させた。更に、二段目の水洗部にて脱CO2排ガスを洗浄水と液/ガス比2L/Nm3で向流接触させ、二段水洗部出口のデミスタを通過させた後に系外へ放出した。この際、再生塔13の後流側の冷却器19は二段構成とし、一段目、二段目の冷却器入口温度はそれぞれ100℃,70℃であり、一段目の冷却器からの凝縮水を0.5L/hで一段目の水洗部に供給し、二段目の冷却器からの凝縮水を0.6L/hで二段目の水洗部に供給した。このとき、一段目の水洗部出口ガス温度及び二段目の水洗部出口ガス温度が共に42℃なるように運転した。その結果、吸収塔から系外に放出された脱CO2排ガス中のアミン化合物濃度は8ppmであった。
[比較例1]
実施例1において、再生塔の後流側の冷却器を一段構成とし、凝縮水1.1L/hを二段目の水洗部に供給した以外は実施例1と同様にして運転した結果、吸収塔から系外に放出された脱CO2ガス中のアミン濃度は12ppmであった。
Claims (2)
- 燃焼排ガスとアミン化合物の水溶液を向流接触させる接触部で、燃焼排ガス中に含まれる二酸化炭素(CO2)を除去する脱炭酸塔と、該脱炭酸塔から排出されたアミン化合物の水溶液を加熱してアミン化合物の水溶液を再生する再生塔と、該再生塔で再生されたアミン化合物の水溶液を冷却器を経て前記脱炭酸塔に還流させる還流手段とを有する二酸化炭素除去装置であって、前記再生塔の還流水とCO2が除去された燃焼排ガスが向流接触する接触部を2段構成とし、さらに前記再生塔後流側の前記冷却器を2段構成とし、1段目の冷却器からの還流水は1段目の接触部に供給し、2段目の冷却塔からの還流水は2段目の接触部に供給するように構成したことを特徴とする燃焼排ガス中の二酸化炭素除去装置。
- 燃焼排ガスの温度が、脱炭酸塔入口と出口とで可及的に同一となるように、前記冷却器から脱炭酸塔に還流されるアミン化合物水溶液の量を調節することを特徴とする請求項1記載の装置を用いた燃焼排ガス中の二酸化炭素除去方法。
Priority Applications (5)
Application Number | Priority Date | Filing Date | Title |
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US13/988,898 US9399188B2 (en) | 2010-11-22 | 2011-11-21 | Apparatus for removing carbon dioxide in combustion exhaust gas |
JP2012545738A JP5597260B2 (ja) | 2010-11-22 | 2011-11-21 | 燃焼排ガス中の二酸化炭素除去装置 |
EP11842554.5A EP2644255B1 (en) | 2010-11-22 | 2011-11-21 | Device for removing carbon dioxide in combustion exhaust gas |
PL11842554T PL2644255T3 (pl) | 2010-11-22 | 2011-11-21 | Urządzenie do usuwania dwutlenku węgla w wylotowych gazach spalinowych |
CA2819272A CA2819272C (en) | 2010-11-22 | 2011-11-21 | Apparatus for removing carbon dioxide in combustion exhaust gas |
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JP2010259711 | 2010-11-22 | ||
JP2010-259711 | 2010-11-22 |
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US (1) | US9399188B2 (ja) |
EP (1) | EP2644255B1 (ja) |
JP (1) | JP5597260B2 (ja) |
CA (1) | CA2819272C (ja) |
PL (1) | PL2644255T3 (ja) |
WO (1) | WO2012070523A1 (ja) |
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WO2014045797A1 (ja) * | 2012-09-24 | 2014-03-27 | 三菱重工業株式会社 | 二酸化炭素回収システムおよび方法 |
JP2018001086A (ja) * | 2016-06-30 | 2018-01-11 | 株式会社東芝 | 二酸化炭素回収システムおよび排ガス処理方法 |
CN109562318A (zh) * | 2016-07-05 | 2019-04-02 | 英力士美国有限公司 | 用于回收酸性气体处理中的吸收剂的方法和设备 |
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EP3072869B1 (en) * | 2013-11-22 | 2018-01-31 | LG Chem, Ltd. | Method for recovering absorption solvent in process for preparing butadiene through oxidative dehydrogenation |
JP6581768B2 (ja) * | 2014-11-04 | 2019-09-25 | 三菱重工エンジニアリング株式会社 | Co2回収装置およびco2回収方法 |
US10375901B2 (en) | 2014-12-09 | 2019-08-13 | Mtd Products Inc | Blower/vacuum |
CN108360450B (zh) * | 2018-02-08 | 2021-05-04 | 宁夏旭升建设工程有限公司 | 一种高自动化新型水利安全环保装置 |
US11207634B2 (en) | 2018-07-02 | 2021-12-28 | University Of Kentucky Research Foundation | Apparatus and method for recovering an amine solvent from an acid gas stream |
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2011
- 2011-11-21 PL PL11842554T patent/PL2644255T3/pl unknown
- 2011-11-21 EP EP11842554.5A patent/EP2644255B1/en active Active
- 2011-11-21 WO PCT/JP2011/076789 patent/WO2012070523A1/ja active Application Filing
- 2011-11-21 CA CA2819272A patent/CA2819272C/en active Active
- 2011-11-21 JP JP2012545738A patent/JP5597260B2/ja active Active
- 2011-11-21 US US13/988,898 patent/US9399188B2/en active Active
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WO2014037214A1 (de) * | 2012-09-05 | 2014-03-13 | Basf Se | Verfahren zur abtrennung von sauergasen aus einem wasserhaltigen fluidstrom |
RU2637549C2 (ru) * | 2012-09-05 | 2017-12-05 | Басф Се | Способ отделения кислых газов от содержащего воду потока текучей среды |
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JP2018001086A (ja) * | 2016-06-30 | 2018-01-11 | 株式会社東芝 | 二酸化炭素回収システムおよび排ガス処理方法 |
US10737213B2 (en) | 2016-06-30 | 2020-08-11 | Kabushiki Kaisha Toshiba | Carbon dioxide capturing system and exhaust gas processing method |
CN109562318A (zh) * | 2016-07-05 | 2019-04-02 | 英力士美国有限公司 | 用于回收酸性气体处理中的吸收剂的方法和设备 |
KR20190044057A (ko) * | 2016-07-05 | 2019-04-29 | 이네오스 아메리카스 엘엘씨 | 산성 가스 처리에서 흡수제를 회수하기 위한 방법 및 장치 |
EP3481536A4 (en) * | 2016-07-05 | 2019-12-04 | Ineos Americas, LLC | METHOD AND DEVICE FOR RECOVERING ABSORBENTS IN ACID GAS TREATMENT |
US10646818B2 (en) | 2016-07-05 | 2020-05-12 | Ineos Americas, Llc | Method and apparatus for recovering absorbing agents in acid gas treatment |
KR102406584B1 (ko) * | 2016-07-05 | 2022-06-08 | 이네오스 아메리카스 엘엘씨 | 산성 가스 처리에서 흡수제를 회수하기 위한 방법 및 장치 |
US11433347B2 (en) | 2016-07-05 | 2022-09-06 | Ineos Americas, Llc | Method and apparatus for recovering absorbing agents in acid gas treatment |
AU2017291680B2 (en) * | 2016-07-05 | 2022-12-22 | Ineos Americas, Llc | Method and apparatus for recovering absorbing agents in acid gas treatment |
Also Published As
Publication number | Publication date |
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JP5597260B2 (ja) | 2014-10-01 |
PL2644255T3 (pl) | 2016-06-30 |
EP2644255A1 (en) | 2013-10-02 |
US9399188B2 (en) | 2016-07-26 |
CA2819272A1 (en) | 2012-05-31 |
CA2819272C (en) | 2019-01-29 |
EP2644255A4 (en) | 2014-10-08 |
US20130284021A1 (en) | 2013-10-31 |
EP2644255B1 (en) | 2015-12-09 |
JPWO2012070523A1 (ja) | 2014-05-19 |
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