WO2014030388A1 - Co2回収装置およびco2回収方法 - Google Patents
Co2回収装置およびco2回収方法 Download PDFInfo
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- WO2014030388A1 WO2014030388A1 PCT/JP2013/061403 JP2013061403W WO2014030388A1 WO 2014030388 A1 WO2014030388 A1 WO 2014030388A1 JP 2013061403 W JP2013061403 W JP 2013061403W WO 2014030388 A1 WO2014030388 A1 WO 2014030388A1
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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
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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
- B01D53/1456—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
- B01D53/18—Absorbing units; Liquid distributors therefor
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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
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/75—Multi-step processes
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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
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/77—Liquid phase processes
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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
- B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
- B01D53/77—Liquid phase processes
- B01D53/78—Liquid phase processes with gas-liquid contact
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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
- B01D53/96—Regeneration, reactivation or recycling of reactants
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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
- B01D2251/00—Reactants
- B01D2251/30—Alkali metal compounds
- B01D2251/304—Alkali metal compounds of sodium
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01D—SEPARATION
- B01D2251/00—Reactants
- B01D2251/60—Inorganic bases or salts
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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
- B01D2252/10—Inorganic absorbents
- B01D2252/103—Water
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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
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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
- B01D2257/00—Components to be removed
- B01D2257/70—Organic compounds not provided for in groups B01D2257/00 - B01D2257/602
- B01D2257/704—Solvents not covered by groups B01D2257/702 - B01D2257/7027
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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
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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
- 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
Definitions
- the present invention relates to a CO 2 recovery device and a CO 2 recovery method that simultaneously reduce the concentrations of a basic amine compound and an aldehyde compound that are released and remain in a decarbonized exhaust gas from which CO 2 has been removed by contact with an absorbing solution.
- Patent Document 1 the amine compound entrained in the decarbonized exhaust gas is recovered by bringing the cleaning water into gas-liquid contact with the decarbonized exhaust gas from which CO 2 has been absorbed and removed by gas-liquid contact with the absorbent. It is shown that a plurality of water washing sections are provided, and the recovery process of the amine accompanying the decarbonation exhaust gas is sequentially performed in the plurality of water washing sections. Washing water of Patent Document 1, in a process of reproducing the amine absorbing solution to remove CO 2 from the amine-based absorbing solution that has absorbed CO 2, the condensed water separated by condensing the moisture contained in the CO 2 is It is used.
- Patent Document 2 it is shown that the washing efficiency is further improved by providing a plurality of water washing sections and washing with acidic water at the uppermost water washing section of the plurality of stages. .
- the amine compound that is the absorbing liquid contains an aldehyde compound that is generated due to oxidative deterioration over time while being recycled in the absorption tower and the regeneration tower. Since this aldehyde compound is a kind of volatile organic substance (VOC), there is a concern that this volatile organic substance is released from the absorption tower to the outside of the system, leading to an increase in environmental impact load.
- VOC volatile organic substance
- the present invention has been made to solve the problems described above, CO 2 to reduce the concentration of the basic amine compound and the aldehyde compound released remains in the decarbonated flue gas that has been removed of CO 2 in contact with the absorption liquid at the same time It is an object to provide a recovery device and a CO 2 recovery method.
- the first aspect of the present invention to solve the problems described above, CO 2 absorption to absorb CO 2 in the flue gas by contacting the flue gas with the basic amine compound absorbent to the basic amine compound absorbent A CO 2 absorption tower, and a CO 2 absorption tower having a CO 2 absorption unit and a dewatering exhaust gas from which CO 2 has been removed in the CO 2 absorption unit and a washing water to remove entrained substances accompanying the decarbonation exhaust gas, An absorption liquid regeneration tower that separates CO 2 from a rich solution that has absorbed 2 to regenerate a basic amine compound absorption liquid to obtain a lean solution, and a lean solution from which CO 2 has been removed by the absorption liquid regeneration tower a CO 2 is reused as a basic amine compound absorbent in 2 absorber, the wash water in the circulating wash water line for circulating the washing section, aldehyde-removing agent supplying section for supplying the aldehyde compound removers
- the CO 2 recovery apparatus characterized by having.
- the CO 2 recovery apparatus according to the first aspect, further comprising an acid supply means for supplying an acid to the circulating washing water line.
- a third invention provides the aldehyde compound remover to the circulating washing water line of the washing unit close to the top side of the CO 2 absorption tower by providing a plurality of stages of the washing unit in the first or second invention. And a CO 2 recovery device having an aldehyde removing agent supply unit.
- an alkali is provided in contact with the exhaust gas containing CO 2, nitrogen oxides and sulfur oxides provided on the upstream side of the CO 2 absorption tower.
- the CO 2 recovery apparatus includes a gas cooling means that uses cleaning water to which water is added, and a supply line that supplies the alkali-added cooling water after contact to the circulating cleaning water line.
- a fifth invention is the separation and the CO 2 absorber to remove CO 2 by contacting the CO 2 containing exhaust gas and the basic amine compounds containing CO 2, the CO 2 from the basic amine compound that has absorbed CO 2 a by using the absorbent regenerator to regenerate the CO 2 absorbing solution, CO 2 recovery method of reusing a lean solution from which CO 2 has been removed by the absorbing solution regeneration tower in the CO 2 absorption tower, removing A method for recovering CO 2, wherein the carbon dioxide exhaust gas is washed with water in a water washing section, and at the time of this water washing, an aldehyde compound removing agent is supplied to the washing water to simultaneously remove the basic amine compound and the aldehyde compound. It is in.
- a sixth invention is the CO 2 recovery method according to the fifth invention, characterized in that an acid is supplied to the washing water.
- a seventh invention is characterized in that, in the fifth or sixth invention, the rinsing section is provided in a plurality of stages, and the aldehyde compound remover is supplied in a rinsing section close to a tower top side of the CO 2 absorption tower. In the CO 2 recovery method.
- any one invention of the fifth to 7 in the upstream side of the CO 2 absorption tower, and flue gas containing CO 2 and nitrogen oxides and sulfur oxides, cooling water by adding an alkali In the CO 2 recovery method, wherein the exhaust gas is cooled with gas and the alkali-added cooling water after contact is used as circulating water in the washing section.
- the basic amine compound and the aldehyde compound entrained in the decarbonation exhaust gas can be simultaneously recovered and removed, so that the basic amine compound and the volatile organic substance are released from the absorption tower outside the system. Is greatly suppressed.
- FIG. 1 is a schematic diagram of a CO 2 recovery apparatus according to the first embodiment.
- FIG. 2 is a schematic diagram of a CO 2 recovery apparatus according to the second embodiment.
- FIG. 3 is a schematic diagram of a CO 2 recovery apparatus according to the third embodiment.
- FIG. 4 is a schematic diagram of a CO 2 recovery device according to the fourth embodiment.
- FIG. 5-1 is a graph showing the results of amine compound removal rate (recovery rate)% in Test Example 1.
- FIG. 5-2 is a graph showing the results of the removal rate (recovery rate)% of the aldehyde compound of Test Example 1.
- FIG. 6 is a diagram in which the ionic form of sulfurous acid changes due to the change in pH.
- 7-1 is a graph showing the results of the removal rate (recovery rate)% of the amine compound of Test Example 2.
- 7-2 is a graph showing the results of% removal rate (recovery rate) of the aldehyde compound of Test Example 2.
- FIG. 8 is a diagram showing the relationship between the pH of the washing water in the washing section and the recovery rate of the aldehyde compound.
- FIG. 9-1 is a graph showing the results of amine compound removal rate (recovery rate)% in Test Example 3.
- 9-2 is a graph showing the results of the removal rate (recovery rate)% of the aldehyde compound of Test Example 3.
- FIG. 10 is a diagram showing a reduction ratio of the addition amount of the sulfite compound.
- FIG. 1 is a schematic diagram of a CO 2 recovery apparatus according to the first embodiment.
- CO 2 recovery apparatus 10A by contacting the CO 2 absorbing liquid 12 is CO 2 containing exhaust gas 11A and the basic amine compound absorbent containing CO 2 CO 2
- the CO 2 absorption part 13A for removing CO 2 , the decarbonation exhaust gas 11B from which CO 2 has been removed by the CO 2 absorption part 13A, and the washing water 20 are brought into contact with each other to remove entrained substances accompanying the decarbonation exhaust gas 11B.
- an aldehyde removal agent supply unit 23 supplying at least one aldehyde-removing agent 22 of bisulfite compound or a mixture thereof.
- the washing unit 21 is washed by countercurrent contact with the decarbonation exhaust gas 11B where the washing water 20 falls from the tower top side through the nozzle and rises, and the washing water 20 is collected by the liquid storage unit 24.
- the collected washing water 20 is circulated and used by a circulation pump 25 interposed in the circulation washing water line L 1 . Also been cooled to a predetermined temperature by the cooling unit 26 interposed circulating wash water line L 1.
- a rich / lean solution heat exchanger 52 is provided to exchange heat between the rich solution 12A and the lean solution 12B from which CO 2 has been released.
- reference numeral 13 a is a tower top
- 13 b is a tower bottom
- 19 is a mist eliminator that captures mist in gas
- 51 is a rich solution pump
- 54 is a lean solution pump
- L 11 is a rich solution supply pipe
- L 12 is Each of the lean solution supply tubes is illustrated.
- the CO 2 -containing exhaust gas 11 A is in countercurrent contact with an amine-based CO 2 absorption liquid 12 based on, for example, alkanolamine, in a CO 2 absorption section 13 A provided on the lower side of the absorption tower 13.
- CO 2 in the CO 2 containing exhaust gas 11A is absorbed by the CO 2 absorbing liquid 12 by a chemical reaction (R-NH 2 + H 2 O + CO 2 ⁇ R-NH 3 HCO 3).
- R-NH 2 + H 2 O + CO 2 ⁇ R-NH 3 HCO 3 a chemical reaction
- the CO 2 removal exhaust gas 11B rises to the washing unit 21 side via the chimney tray 16, comes into gas-liquid contact with the washing water 20 supplied from the top side of the washing unit 21, and accompanies the decarbonized exhaust gas 11B.
- the CO 2 absorbent 12 is recovered by circulating cleaning.
- the washing water 20 stored in the liquid storage section 24 of the chimney tray 16 is circulated through the circulation washing water line L 1 for circulation washing.
- the circulating washing water line L 1 is provided with a cooling unit 26 for cooling to a predetermined temperature (for example, 40 ° C. or lower).
- At least one aldehyde removing agent 22 of, for example, a sulfite compound, a hydrogen sulfite compound or a mixture thereof is supplied to the circulating washing water line L 1 , dewatering exhaust gas in the washing portion 21. Since 11B and the washing water 20 containing a sulfite compound, a bisulfite compound, or a mixture thereof are brought into contact with each other, simultaneous recovery of the amine compound and the aldehyde compound in the decarbonized exhaust gas 11B can be achieved. As a result, it is possible to reduce the concentration of entrained substances in the outlet gas 11C discharged from the tower top 13a of the absorption tower 13.
- Examples of the sulfite compound that is the aldehyde removing agent 22 include sodium sulfite, ammonium sulfite, and potassium sulfite.
- Examples of the hydrogen sulfite compound include sodium bisulfite, ammonium bisulfite, and potassium bisulfite. The invention is not limited to this, and any substance that can decompose and remove aldehydes may be used.
- Rich solution 12A that has absorbed CO 2 in the absorption tower 13 is withdrawn from the bottom portion 13b, is boosted by the rich solution pump 51 interposed in the rich solution supply pipe L 11, supplied to the top side of the regenerator 14 Is done.
- the rich solution 12A released into the tower from the top side of the regeneration tower 14 releases most of the CO 2 by heating with water vapor from the bottom of the tower.
- the CO 2 absorbent 12 that has released part or most of the CO 2 in the regeneration tower 14 is referred to as a “semi-lean solution”.
- the semi-lean solution (not shown) flows down to the bottom of the regeneration tower 14, it becomes a lean solution 12B from which almost all of the CO 2 has been removed.
- This lean solution 12B is saturated steam 62 in the regeneration heater 61 interposed in the circulation line L 20, obtained is heated.
- the saturated steam 62 after heating becomes steam condensed water 63.
- the CO 2 gas 41 accompanied by water vapor dissipated from the rich solution 12A and a semi-lean solution (not shown) is released from the top 14a of the regeneration tower 14 in the tower.
- CO 2 gas 41 accompanied by water vapor is derived by the gas discharge line L 21
- the water vapor is condensed by the cooling unit 42 interposed in the gas discharge line L 21
- condensed water 44 is separated in the separation drum 43
- the CO 2 gas 45 is discharged out of the system from the separation drum 43 and separately subjected to post-processing such as compression recovery.
- Condensed water 44 separated in the separation drum 43 is supplied to the upper portion of the regeneration tower 14 by the condensed water circulation pump 46 interposed in condensate line L 22.
- a part of the condensed water 44 may be supplied to the circulating cleaning water line L 1 and used as the cleaning water 20 for the CO 2 absorbent 12 accompanying the outlet gas 11C.
- the regenerated CO 2 absorbent (lean solution 12B) is sent to the absorption tower 13 side by the lean solution pump 54 via the lean solution supply pipe L 12 and circulated and used as the CO 2 absorbent 12. At this time, the lean solution 12B is cooled to a predetermined temperature by the cooling unit 55 and is supplied into the CO 2 absorbing unit 13A through the nozzle 56.
- the CO 2 absorbent 12 forms a closed path that circulates between the absorption tower 13 and the regeneration tower 14 and is reused in the CO 2 absorption section 13A of the absorption tower 13.
- the CO 2 absorbent 12 is supplied from a replenishment line (not shown) as necessary, and the CO 2 absorbent 12 is regenerated by a reclaimer (not shown) as needed.
- the CO 2 -containing exhaust gas 11A supplied to the absorption tower 13 is cooled by the cooling water 71 in the cooling tower 70 provided on the upstream side thereof, and then introduced into the absorption tower 13.
- a part of the cooling water 71 is also supplied to the top of the water washing section 21 as the washing water 20 of the absorption tower 13 and may be used for washing the CO 2 absorbent 12 accompanying the decarbonation exhaust gas 11B.
- Reference numeral 72 is a circulating pump, 73 a cooler, L 30 illustrates the circulation line.
- FIG. 5A and 5B are graphs showing the results of the removal rate (recovery rate)% of the amine compound and the removal rate (recovery rate)% of the aldehyde compound in Test Example 1.
- FIG. FIG. 6 is a diagram in which the ionic form of sulfurous acid changes due to the change in pH.
- sodium sulfite was used as an aldehyde remover (the same applies to the following test examples).
- the case of “None” in the conventional method is a case where the sulfite compound / bisulfite compound is not added to the cleaning water 20.
- the sulfite compound / bisulfite compound is added to the washing water 20.
- “Yes” (1) is a case where sodium sulfite is added to the washing water 20 at a standard 1 molar concentration.
- “Yes” (73) is the case where 73 molar concentration of sodium sulfite is added to the washing water 20 which is 73 times the standard.
- the ionic form of sulfurous acid changes depending on the pH of the existing solution. From the low pH side, sulfurous acid (H 2 SO 3 ), hydrogen sulfite ion (HSO 3 ⁇ ), sulfite ion ( SO 3 2- ).
- sulfurous acid H 2 SO 3
- hydrogen sulfite ion HSO 3 ⁇
- SO 3 2- sulfite ion
- FIG. 2 is a schematic diagram of a CO 2 recovery apparatus according to the second embodiment.
- CO 2 recovery apparatus 10B according to this embodiment, the CO 2 recovery apparatus 10A of the first embodiment shown in FIG. 1, further circulating wash water line L acid supply unit for supplying acid 27 to 1 28 is provided to control the pH in the wash water 20 to the acidic side.
- reference numeral 29 denotes a pH meter that measures pH.
- the water washing section 21 has a desired pH for recovering the aldehyde compound in the decarbonized exhaust gas 11B, and the aldehyde recovery efficiency. Will improve. Therefore, in the water washing part 21, in addition to making it contact with the decarbonation waste gas 11B and the washing water 20 containing a sulfite compound, a bisulfite compound, or those mixtures, the pH of the washing water 20 of the water washing part 21 is adjusted to the appropriate range of an acidic side. By doing so, the concentration of the entrained substance in the exit gas 11C discharged from the absorption tower 13 can be further reduced.
- FIGS. 7-1 and 7-2 are graphs showing the results of the amine compound removal rate (recovery rate)% and the aldehyde compound removal rate (recovery rate)% in Test Example 2.
- FIGS. 7-1 and 7-2 are graphs showing the results of the amine compound removal rate (recovery rate)% and the aldehyde compound removal rate (recovery rate)% in Test Example 2.
- the case of “None” in the conventional method is a case where the sulfite compound / bisulfite compound is not added to the cleaning water 20.
- the sulfite compound / bisulfite compound is added to the washing water 20.
- dilute sulfuric acid was added to obtain a standard pH having a high hydrogen sulfite ion concentration ratio.
- “Yes” (1) is the case where sodium sulfite is added to the washing water 20 at a standard concentration of 1 mol.
- the recovery rate was improved. Therefore, it was confirmed that the addition of the sulfite compound can efficiently remove at least the aldehyde compound by adding the acid 27 so as to obtain an appropriate pH with a high proportion of hydrogen sulfite ion.
- FIG. 8 is a diagram showing the relationship between the pH of the washing water in the washing section and the recovery rate of the aldehyde compound. As shown in FIG. 8, it was confirmed that when the pH is raised above the standard pH (the hydrogen sulfite ion concentration ratio is large), the hydrogen sulfite ion concentration is lowered, so that the recovery efficiency of the aldehyde compound is lowered.
- FIG. 3 is a schematic diagram of a CO 2 recovery apparatus according to the third embodiment.
- the CO 2 recovery apparatus 10C according to the present embodiment is located above the CO 2 absorption section 13A installed in the absorption tower 13 in the CO 2 recovery apparatus 10B of the second embodiment shown in FIG.
- the provided flushing section has a plurality of stages.
- the preliminary flushing section 21A, the first flushing section 21B, the second flushing section 21C, and the third flushing section 21D are performed from the CO 2 absorbing section 13A toward the tower top section 13a.
- the third washing section 21D was described in Example 2, an aldehyde-removing agent 22 and acid 27, is supplied to the circulating washing water line L 1, it is set to finish washing means for recovering aldehyde compound.
- a mist eliminator 19 is interposed between the third water washing section 21D exit, between the third water washing section 21D and the second water washing section 21C, and between the first water washing section 21B and the preliminary water washing section 21A, respectively. The mist is removed.
- the washing water 20 to be introduced into the second washing section 21C is a condensed water 44 is separated from the separation drum 43, via a washing water line L 23 branched from the condensate line L 22, using I am doing so.
- the supplied wash water 20 falls in the second water wash section 21C and the first water wash section 21B and is collected in the liquid storage section 24 on the bottom side of the first water wash section 21B. Wash water 20 recovered in the liquid reservoir 24, the circulating wash water line L 1 was dropped from the top of the first water-washing section 21B, and washed.
- a portion 20a of the washing water 20 is supplied to a pre-washing section 21A side branch line L 2 branched from the circulating wash water line L 1 is performing a preliminary washing of the decarbonated exhaust gas 11B.
- Wash water 20 after the preliminary washing with water, dropped the CO 2 absorbing section 13A, with rich solution 12A, is reproduced by a reproducing tower 14, as condensed water 44 is withdrawn again, the washing water branched from the condensate line L 22 via line L 23, to supply to the second washing section 21C, so that achieve the recycling in a closed system.
- the washing water from the separately outside the system into the wash water line L 23 may be supplied.
- the decarbonized exhaust gases 11B, 11C, and 11D pass through the preliminary water washing section 21A, the first water washing section 21B to the third water washing section 21D, and are discharged to the outside as the outlet gas 11E. Then, the accompanying basic amine compound is removed in the preliminary washing section 21A, the first washing section 21B to the second washing section 21C, and the aldehyde compound is removed simultaneously with the removal of the basic amine compound in the third washing section 21D. As a result, the release of the volatile organic substance from the absorption tower 13 to the outside of the system is greatly suppressed.
- the absorption tower 13 by installing a plurality of water washing sections (in this embodiment, two stages: the first water washing section to the second water washing section / the third water washing section, four layers 21A to 21D), the absorption tower 13 The entrained substance concentration diffused into the outlet gas 11E can be further greatly reduced.
- the case of “None” in the conventional method is a case where the sulfite compound / bisulfite compound is not added to the cleaning water 20.
- the sulfite compound / bisulfite compound is added to the washing water 20.
- dilute sulfuric acid was added to obtain a standard pH having a high hydrogen sulfite ion concentration ratio.
- the addition of the sulfite compound can efficiently remove at least the aldehyde compound by adding the acid 27 so that the water washing part is multistage and the pH is high so that the ratio of hydrogen sulfite ion is high. It was.
- FIG. 4 is a schematic diagram of a CO 2 recovery device according to the fourth embodiment.
- the CO 2 recovery apparatus 10D according to the present embodiment, the CO 2 recovery system 10C of the third embodiment shown in FIG. 3, was placed in the preceding stage of the absorption tower 13, the CO 2 containing exhaust gas 11A
- a cooling tower 80 for recovering SO 2 in the exhaust gas is provided.
- the cooling tower 80 of the present embodiment is provided with a liquid reservoir 81 for collecting the cooling water 71 inside the tower, and the inside has a two-stage configuration.
- Upper side like the cooling tower 70, CO 2 containing exhaust gas 11A is cooled by cooling water 71 circulating through the circulation line L 30.
- the part 71a of the cooling water 71 is fed into the circulation line L 32 that circulates through the lower stage side via the feed line L 31.
- sodium hydroxide 83 is supplied as an alkaline agent to the circulation line L 32 to remove SO 2 present in the CO 2 -containing exhaust gas 11A so that the sulfurous acid compound is taken into the cooling water 71a.
- the cooling water 71b containing the sulfite compound into the third water washing section 21D, it is possible to reduce the addition amount of the aldehyde removing agent 22 supplied from the outside.
- FIG. 10 is a diagram showing a reduction ratio of the addition amount of the sulfite compound. As shown in FIG. 10, when Example 3 is set to 1, when the cooling water in which the sulfur oxide in the exhaust gas is recovered by the cooling tower 80 is partially used as an aldehyde remover, the addition ratio is 0. It is possible to save about 30% or more on the cost of chemicals.
Abstract
Description
特に、将来予想される処理ガス流量の多い火力発電所などの排ガスに対して、CO2回収装置を設置する場合、排ガスの放出量が多量であることから、脱炭酸排ガスに残存して放出される同伴物質の放出量が増加する傾向にあり、放出される同伴物質の濃度をより一層低減することが必要である。
図1に示すように、本実施例に係るCO2回収装置10Aは、CO2を含有するCO2含有排ガス11Aと塩基性アミン化合物吸収液であるCO2吸収液12とを接触させてCO2を除去するCO2吸収部13Aと、前記CO2吸収部13AでCO2を除去された脱炭酸排ガス11Bと洗浄水20とを接触させて前記脱炭酸排ガス11Bに同伴する同伴物質を除去する水洗部21とを有するCO2吸収塔(以下「吸収塔」という)13と、CO2を吸収したCO2吸収液(リッチ溶液12A)を再生する吸収液再生塔(以下「再生塔」という)14と、前記再生塔14でCO2が除去されたリーン溶液12Bを2吸収塔13で再利用するCO2回収装置であって、前記水洗部21に洗浄水20を循環させる循環洗浄水ラインL1に、例えば亜硫酸化合物、亜硫酸水素化合物又はこれらの混合物の少なくとも一種のアルデヒド除去剤22を供給するアルデヒド除去剤供給部23を有する。
回収された洗浄水20は、循環洗浄水ラインL1に介装された循環ポンプ25で循環利用されている。また、循環洗浄水ラインL1に介装された冷却部26で所定温度に冷却している。
図1中、符号13aは塔頂部、13bは塔底部、19はガス中のミストを捕捉するミストエリミネータ、51はリッチ溶液ポンプ、54はリーン溶液ポンプ、L11はリッチ溶液供給管、L12はリーン溶液供給管を各々図示する。
この結果、CO2吸収部13Aを通過して、吸収塔13の内部を上昇する脱炭酸排ガス11Bには、CO2が殆ど残存しないものとなる。
なお、循環洗浄水ラインL1には冷却部26を設け、所定の温度(例えば40℃以下)まで冷却している。
この結果、吸収塔13の塔頂部13aから排出される出口ガス11C中の同伴物質濃度の低減を図ることができる。
そして、水蒸気を伴ったCO2ガス41がガス排出ラインL21により導出され、ガス排出ラインL21に介装された冷却部42により水蒸気が凝縮され、分離ドラム43にて凝縮水44が分離される。その後、CO2ガス45が分離ドラム43から系外に放出されて、別途圧縮回収等の後処理がなされる。
分離ドラム43にて分離された凝縮水44は凝縮水ラインL22に介装された凝縮水循環ポンプ46にて再生塔14の上部に供給される。
なお、図示していないが、一部の凝縮水44は循環洗浄水ラインL1に供給され、出口ガス11Cに同伴するCO2吸収液12の洗浄水20として用いるようにしてもよい。
図5-1、5-2は、試験例1のアミン化合物の除去率(回収率)%と、アルデヒド化合物の除去率(回収率)%との結果を示す図である。
図6は、亜硫酸がpHの変動によりその存在イオン形態が変化する図である。
本試験例では、アルデヒド除去剤として、亜硫酸ナトリウムを用いた(以下の試験例でも同様)。
実施例1の「有」の場合は、亜硫酸化合物/亜硫酸水素化合物を、洗浄水20中に添加した場合である。
この添加の際、図5-2に示すように、有(1)は、洗浄水20に亜硫酸ナトリウムを標準である1モル濃度添加した場合である。
この添加の際、図5-2に示すように、有(73)は、標準の73倍である洗浄水20に亜硫酸ナトリウムを73モル濃度添加した場合である。
洗浄水のpHが高い(アルカリ性)場合には、亜硫酸イオンが支配しているので、アルデヒド化合物の反応吸収に寄与する亜硫酸水素イオンの存在量が少ないものとなる。
図2に示すように、本実施例に係るCO2回収装置10Bは、図1に示す実施例1のCO2回収装置10Aにおいて、さらに循環洗浄水ラインL1に酸27を供給する酸供給部28を設けており、洗浄水20中のpHを酸性側に制御するようにしている。なお、図中、符号29はpHを計測するpH計である。
この酸27として例えば希硫酸を供給することで、水洗部21の洗浄水20が酸性となる。
よって水洗部21において、脱炭酸排ガス11Bと亜硫酸化合物又は亜硫酸水素化合物又はそれらの混合物を含む洗浄水20と接触させることに加え、水洗部21の洗浄水20のpHを酸性サイドの適切範囲に調節することにより、吸収塔13から放出する出口ガス11C中の同伴物質濃度の低減をさらに図ることができる。
図7-1、7-2は、試験例2のアミン化合物の除去率(回収率)%と、アルデヒド化合物の除去率(回収率)%との結果を示す図である。
実施例2の「有」の場合は、亜硫酸化合物/亜硫酸水素化合物を、洗浄水20中に添加した場合である。この際、希硫酸を添加して亜硫酸水素イオン濃度割合が多い標準pHとなるようにした。
この添加の際、図7-2に示すように、有(1)は、洗浄水20に亜硫酸ナトリウムを標準である1モル濃度添加した場合であるが、試験例1の場合よりも、アルデヒド化合物の回収率の向上となった。
よって、亜硫酸水素イオンの割合が多い適正なpHとなるように酸27を添加することで、亜硫酸化合物の添加が少なくとも、アルデヒド化合物を効率的に除去できることが確認された。
図8に示すように、標準pH(亜硫酸水素イオン濃度割合が多い)よりもpHを上昇させると、亜硫酸水素イオン濃度が低下するので、アルデヒド化合物の回収効率が低下するのが確認された。
図3に示すように、本実施例に係るCO2回収装置10Cは、図2に示す実施例2のCO2回収装置10Bにおいて、吸収塔13内に設置したCO2吸収部13Aの上方側に設けた水洗部を複数段としている。
そして、第3水洗部21Dは、実施例2で説明した、アルデヒド除去剤22と酸27とを、循環洗浄水ラインL1に供給して、アルデヒド化合物を回収する仕上げ水洗手段としている。
この供給された洗浄水20は、第2水洗部21C及び第1水洗部21Bを落下し、第1水洗部21B底部側の液貯留部24で回収されている。
液貯留部24で回収された洗浄水20は、循環洗浄水ラインL1で第1水洗部21Bの頂部から落下させて、洗浄している。
なお、洗浄水20が不足する場合には、洗浄水ラインL23へ別途系外より洗浄水を供給するようにしてもよい。
脱炭酸排ガス11B、11C、11Dは、予備水洗部21A、第1水洗部21B~第3水洗部21Dを通過し、出口ガス11Eとして、塔頂部13aから外部へ排出されている。
そして、予備洗浄部21A、第1水洗部21B~第2水洗部21Cにおいて、同伴する塩基性アミン化合物を除去すると共に、第3水洗部21Dにおいて、塩基性アミン化合物の除去と同時にアルデヒド化合物を除去するので、揮発性有機物質が吸収塔13から系外に放出されることが大幅に抑制される。
図9-1、9-2は、試験例3のアミン化合物の除去率(回収率)%と、アルデヒド化合物の除去率(回収率)%との結果を示す図である。
なお、水洗部の段数は2段(4層)とした。
実施例3の「有」の場合は、亜硫酸化合物/亜硫酸水素化合物を、洗浄水20中に添加した場合である。この際、希硫酸を添加して亜硫酸水素イオン濃度割合が多い標準pHとなるようにした。
図4に示すように、本実施例に係るCO2回収装置10Dは、図3に示す実施例3のCO2回収装置10Cにおいて、吸収塔13の前段側に設置し、CO2含有排ガス11Aを冷却する冷却手段として、排ガス中のSO2を回収する冷却塔80を設けている。
上段側は、冷却塔70と同様に、CO2含有排ガス11Aは、循環ラインL30を循環する冷却水71により冷却されている。そして、この冷却水71の一部71aは、送液ラインL31を介して下段側を循環する循環ラインL32に供給される。この循環ラインL32には、例えばアルカリ剤として水酸化ナトリウム83が供給され、CO2含有排ガス11Aに存在するSO2を除去して、亜硫酸化合物を冷却水71a中に取り込むようにしている。
この結果、第3水洗部21Dに、亜硫酸化合物が含まれる冷却水71bを導入することで、別途外部から供給するアルデヒド除去剤22の添加量の節減を図ることができる。
図10に示すように、実施例3の場合を1とした場合、冷却塔80で排ガス中の硫黄酸化物を回収した冷却水を、アルデヒド除去剤として一部用いた場合、添加量比が0.65と少なく、約30%以上の薬品代の節約を図ることができる。
11A CO2含有排ガス
11B 脱炭酸排ガス
12 CO2吸収液
13 CO2吸収塔
13A CO2吸収部
20 洗浄水
21 水洗部
21A 予備水洗部
21B 第1水洗部
21C 第2水洗部
21D 第3水洗部
22 アルデヒド除去剤
23 アルデヒド除去剤供給部
27 酸
28 酸供給部
Claims (8)
- 排ガスと塩基性アミン化合物吸収液とを接触させて前記排ガス中のCO2を前記塩基性アミン化合物吸収液に吸収させるCO2吸収部と、前記CO2吸収部でCO2を除去された脱炭酸排ガスと洗浄水とを接触させて前記脱炭酸排ガスに同伴する同伴物質を除去する水洗部とを有するCO2吸収塔と、
CO2を吸収したリッチ溶液からCO2を分離して塩基性アミン化合物吸収液を再生してリーン溶液とする吸収液再生塔と、
前記吸収液再生塔でCO2が除去されたリーン溶液を前記CO2吸収塔で塩基性アミン化合物吸収液として再利用するCO2回収装置であって、
前記水洗部に洗浄水を循環させる循環洗浄水ラインに、アルデヒド化合物除去剤を供給するアルデヒド除去剤供給部を有することを特徴とするCO2回収装置。 - 請求項1において、
前記循環洗浄水ラインに酸を供給する酸供給手段を有することを特徴とするCO2回収装置。 - 請求項1又は2において、
前記水洗部を複数段設け、
前記CO2吸収塔の塔頂部側に近い水洗部の前記循環洗浄水ラインに、前記アルデヒド化合物除去剤を供給するアルデヒド除去剤供給部を有することを特徴とするCO2回収装置。 - 請求項1乃至3のいずれか一つにおいて、
前記CO2吸収塔の前流側に設けられ、CO2及び窒素酸化物及び硫黄酸化物を含む排ガスとの接触に、アルカリを添加した洗浄水を使用するガス冷却手段と、
接触後のアルカリ添加冷却水を、前記循環洗浄水ラインに供給する供給ラインとを有することを特徴とするCO2回収装置。 - CO2を含有するCO2含有排ガスと塩基性アミン化合物とを接触させてCO2を除去するCO2吸収塔と、CO2を吸収した塩基性アミン化合物からCO2を分離してCO2吸収液を再生する吸収液再生塔とを用い、前記吸収液再生塔でCO2が除去されたリーン溶液を前記CO2吸収塔で再利用するCO2回収方法であって、
脱炭酸排ガスを水洗部で水洗浄すると共に、この水洗浄の際に、アルデヒド化合物除去剤を洗浄水に供給し、塩基性アミン化合物とアルデヒド化合物とを同時除去することを特徴とするCO2回収方法。 - 請求項5において、
前記洗浄水に酸を供給することを特徴とするCO2回収方法。 - 請求項5又は6において、
前記水洗部を複数段設け、
前記CO2吸収塔の塔頂部側に近い水洗部において、前記アルデヒド化合物除去剤を供給することを特徴とするCO2回収方法。 - 請求項5乃至7のいずれか一つにおいて、
前記CO2吸収塔の前流側で、CO2及び窒素酸化物及び硫黄酸化物を含む排ガスと、アルカリを添加した冷却水とを接触させて前記排ガスをガス冷却すると共に、
接触後のアルカリ添加冷却水を、前記水洗部の循環水に用いることを特徴とするCO2回収方法。
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US9789437B2 (en) | 2017-10-17 |
CA2878910A1 (en) | 2014-02-27 |
EP2886183A1 (en) | 2015-06-24 |
EP2886183A4 (en) | 2015-08-26 |
AU2013307050A1 (en) | 2015-02-05 |
NO2886183T3 (ja) | 2018-07-21 |
EP2886183B1 (en) | 2018-02-21 |
JP5968159B2 (ja) | 2016-08-10 |
AU2013307050B2 (en) | 2015-11-26 |
CA2878910C (en) | 2016-10-11 |
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