WO2019073866A1 - Procédé de séparation/récupération de co2 et équipement de séparation/récupération de co2 - Google Patents

Procédé de séparation/récupération de co2 et équipement de séparation/récupération de co2 Download PDF

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Publication number
WO2019073866A1
WO2019073866A1 PCT/JP2018/036977 JP2018036977W WO2019073866A1 WO 2019073866 A1 WO2019073866 A1 WO 2019073866A1 JP 2018036977 W JP2018036977 W JP 2018036977W WO 2019073866 A1 WO2019073866 A1 WO 2019073866A1
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Prior art keywords
adsorption
separation
cooling
recovery
adsorbent
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PCT/JP2018/036977
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English (en)
Japanese (ja)
Inventor
佐々木　崇
朋子 鈴木
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株式会社日立製作所
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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
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/74—General processes for purification of waste gases; Apparatus or devices specially adapted therefor
    • B01D53/81—Solid phase processes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
    • B01J20/02—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material
    • B01J20/06—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof comprising inorganic material comprising oxides or hydroxides of metals not provided for in group B01J20/04
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J20/00—Solid sorbent compositions or filter aid compositions; Sorbents for chromatography; Processes for preparing, regenerating or reactivating thereof
    • B01J20/30—Processes for preparing, regenerating, or reactivating
    • B01J20/34—Regenerating or reactivating
    • 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
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02C—CAPTURE, STORAGE, SEQUESTRATION OR DISPOSAL OF GREENHOUSE GASES [GHG]
    • Y02C20/00—Capture or disposal of greenhouse gases
    • Y02C20/40—Capture or disposal of greenhouse gases of CO2
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/151—Reduction of greenhouse gas [GHG] emissions, e.g. CO2

Definitions

  • the present invention relates to a CO 2 separation method and a CO 2 separation and recovery facility.
  • CO2 carbon dioxide
  • the sources of carbon dioxide (CO2) emissions are diverse, such as thermal power generation, steel, natural gas mining, various chemical industries, etc.
  • CO2 recovery technology from these sources has been developed since the late 20th century.
  • a membrane separation method that selectively allows CO2 permeation and liquefaction temperature difference of mixed gas are used.
  • cryogenic separation method etc. CO 2 separation and recovery technology has technical and cost advantages respectively, but as a CO 2 separation and recovery technology from a large-scale plant, it is considered that the chemical absorption method or physical absorption method using CO2 absorbent is suitable There is.
  • Patent Document 3 describes an example of a CO 2 separation and recovery method using a solid adsorbent.
  • This patent has an adsorption step of adsorbing CO2 in exhaust gas to the adsorbent and a desorption step of desorbing CO2 adsorbed by the adsorbent, and the desorption step is a step of CO2 when adsorbing the CO2 to the adsorbent.
  • This is a CO2 separation and recovery method using a purge gas exhibiting a CO2 partial pressure lower than the pressure, for example, a steam extracted on the way or after leaving the turbine of a thermal power plant.
  • Patent Document 4 aims to separate and recover CO2 from boiler exhaust gas, a CO2 adsorption process for capturing CO2 with an adsorbent, a purge process for purging a CO2 adsorption tower with high purity CO2, and thermal energy such as water vapor
  • Patent No. 5468562 gazette Patent No. 5725992 Unexamined-Japanese-Patent No. 2010-69398 JP, 2013-061088, A
  • Patent Documents 3 and 4 can not all say that “low energy input,” “high CO 2 recovery rate,” and “high CO 2 purity” are all satisfied.
  • a CO2 adsorption step of adsorbing and separating CO2 contained in exhaust gas with an adsorbent, and the exhaust gas present in the CO2 adsorption tower after the adsorption step By introducing a gas containing CO 2 at a temperature lower than the temperature in the purge step of discharging the carbon dioxide, the desorption step of desorbing the adsorbed CO 2 by heating the adsorbent, and the desorption step. And a cooling step of cooling the adsorbent, wherein the gas discharged in the cooling step is cooled and pressurized to return to the adsorption step.
  • high CO2 recovery rate and high CO2 purity can be achieved with less energy.
  • FIG. 1 is a process flow of the present invention shown in Example 1; It is an example of the system block diagram of this invention shown in Example 2.
  • FIG. FIG. 16 is an example of a system configuration diagram of the present invention shown in the third embodiment.
  • FIG. 16 is an example of a system configuration diagram of the present invention shown in the fourth embodiment. It is an example of the system block diagram of this invention shown in Example 5.
  • FIG. 16 is an example of a system configuration diagram of the present invention shown in Example 1; It is an example of the system block diagram of this invention shown in Example 2.
  • FIG. 16 is an example of a system configuration diagram of the present invention shown in the third embodiment.
  • FIG. 16 is an example of a system configuration diagram of the present invention shown in the fourth embodiment. It is an example of the system block diagram of this invention shown in Example 5.
  • FIG. 1 shows a conceptual diagram of the CO2 separation and recovery method according to the present invention.
  • the gas species to be supplied to the adsorption tower in the four steps of adsorption, purge, desorption, and cooling will be described for one adsorption tower packed with a CO 2 solid adsorbent, and the state in the adsorption tower at that time.
  • an exhaust gas containing CO 2 is supplied to the adsorption tower.
  • the exhaust gas 2 containing no CO2 is discharged from the outlet of the adsorption tower.
  • the temperature of the exhaust gas 1 supplied to the adsorbent depends on the type of adsorbent to be charged. The appropriate temperature is also considered to be different depending on whether the adsorbent captures CO 2 by physical adsorption or chemical adsorption.
  • the supply of the exhaust gas 1 is stopped when the CO2 adsorption to the adsorbent reaches saturation in the adsorption step. At that time, the exhaust gas 1 containing CO 2 remains in the air gap in the adsorption tower.
  • the exhaust gas 1 remaining in the void is discharged in the purge step.
  • a suction facility such as a rotary pump is installed at the outlet of the adsorption tower, and the exhaust gas 1 remaining in the gap of the adsorption tower is exhausted to the outside of the tower by gas suction.
  • desorbs among CO2 which adsorb
  • CO2 in the adsorbent is desorbed in the desorption step to regenerate the adsorbent.
  • TSA Temperatur Swing Adsorption
  • PSA Pressure Swing Adsorption
  • the present invention is directed to TSA.
  • the heating temperature depends on the characteristics of the adsorbent to be packed into the adsorption column, but the temperature from 100 ° C to 250 ° C, the CO2 desorption characteristic, the regeneration temperature of the chemical absorption method using the aforementioned absorbent, the adsorbent in the next step 100 ° C. to 200 ° C. is desirable in consideration of the time required for cooling, etc.
  • a heating method for example, there is a method of heating using a heater from the outside of the adsorption tower, but any method may be used as long as the adsorbent can be heated regardless of external heating and internal heating.
  • CO2 is desorbed from the adsorbent, but since the inside of the adsorption tower is maintained at a negative pressure in the purge step of the previous step, the temperature is heated to a predetermined temperature and then the rotary pump installed at the gas outlet of the adsorption tower The CO2 in the adsorption tower is discharged to the outside of the tower and recovered by a suction facility such as At this time, CO2 is not adsorbed to the adsorbent. In addition, it is considered that some CO2 remains in the void.
  • the adsorbent (tower) heated in the desorption step is cooled.
  • Exhaust gas 1 is used as the cooling gas.
  • CO2 remaining in the air gap is not only discharged to the outside of the column at the beginning of the supply of exhaust gas 1, but also CO2 is contained in exhaust gas 1, so most of the CO2 is captured by the adsorbent when the temperature of the adsorbent is high. It is discharged out of the tower without being If the cooling gas is exhausted as it is, the gas containing CO 2 is exhausted, which causes a decrease in the CO 2 recovery rate of the target facility and the plant. Therefore, the gas discharged from the adsorption tower in the cooling step is recycled to the adsorption step in the gas circulating step.
  • high purity CO2 can be recovered while maintaining high CO2 recovery.
  • the present embodiment shows an example of a system according to the present invention.
  • An example of a system configuration diagram is shown in FIG.
  • the system shown in FIG. 2 comprises an adsorption tower 1 filled with an adsorbent, an electric heater 2 for external heating, a rotary pump 3, a cooler 4 and a compressor 5.
  • the fixed bed adsorption tower has four columns. The adsorption, purge, desorption, and cooling operations are performed in the four adsorption towers, respectively.
  • an exhaust gas supply pipe to which gas is supplied from a CO 2 exhaust gas generation source and a recycle pipe for returning the gas from the adsorption column outlet pipe to the inlet pipe are connected.
  • the outlet side of the adsorption tower is branched into four lines.
  • the exhaust pipe exhausting the exhaust gas at the time of adsorption operation, the purge pipe exhausting the exhaust gas at the time of purge, the CO2 pipe recovering CO2 generated at the time of desorption, and the cooling gas at the time of cooling It is a recycling pipe.
  • the rotary pump 3 is installed in the purge pipe and the CO 2 pipe.
  • the pipes branched at the outlet of each adsorption tower are collected and sent to the exhaust or CO 2 storage step.
  • the system performs adsorption operation in the first adsorption column (R1), purge in the second adsorption column (R2), desorption in the third adsorption column (R3), and cooling operation in the fourth adsorption column (R4). Indicates the status.
  • the valve V011 installed in the exhaust gas supply pipe is opened to supply the exhaust gas.
  • the adsorbent to be packed into the adsorption column may be any solid that absorbs CO2, such as activated carbon, zeolite, or cerium oxide, but if exhaust gas contains water, CO2 adsorption is inhibited by the adsorption of water onto the adsorbent.
  • a cerium oxide-based adsorbent that is less affected by moisture is preferable.
  • the filling method may be any form as long as it can be filled in a fixed layer such as granular, honeycomb or plate-like.
  • a gas for example, a gas containing N2 and O2 as a main component in the case of a boiler exhaust gas
  • CO2 a gas containing N2 and O2 as a main component in the case of a boiler exhaust gas
  • the valve V11 installed in the exhaust line is opened.
  • CO2 is desorbed from the adsorbent by heating the adsorption tower (adsorbent).
  • adsorption tower adsorbent
  • an external heating electric heater 2 was installed in the adsorption tower.
  • any heating method may be used either external / internal heating type, and the heating method may be any medium having heat such as water vapor other than electric heaters, for example. It may be a method.
  • the adsorption tower In the desorption operation, the adsorption tower is heated by a heater, and when the temperature reaches a predetermined temperature, the valve V33 installed in the CO 2 pipe at the outlet of the adsorption tower is opened to start the rotary pump 3b to discharge the released CO 2 to the outside of the adsorption tower Do.
  • the valve V041 installed in the exhaust gas supply pipe and the valve V44 installed in the recycle pipe are opened to supply the exhaust gas from the exhaust gas supply pipe.
  • CO 2 which could not be discharged partially remains in the void.
  • the cooling gas is returned to the adsorption tower performing the adsorption operation through a recycle line for the purpose of recovering CO 2 remaining in the void during the cooling operation.
  • the exhaust gas discharged from the adsorption tower Since the exhaust gas discharged from the adsorption tower has a higher temperature than the exhaust gas supplied to the adsorption operation, it is cooled by the cooler 4a installed in the recycle pipe, and then boosted by the compressor 5 to perform the adsorption tower during the adsorption operation. Will be returned to Here, what is boosted by the compressor 5 is considered that the exhaust gas supplied to the adsorption tower in the cooling operation is slightly lower than the supply pressure due to the pressure loss. A compressor will be installed to compensate for this pressure loss. In addition, the adiabatic compression of the gas may increase the temperature.
  • cooler 4b is installed downstream of the compressor 5 is to cool the gas when the temperature of the recycle gas rises above the adsorption temperature due to adiabatic compression, but the ⁇ T, which rises at the pressure increase of the pressure loss, is neglected If the size is as small as possible, the installation of the cooler 4b is unnecessary.
  • high purity CO2 can be recovered while maintaining high CO2 recovery.
  • FIG. 3 shows the state of the system when the first adsorption column (R1) is purged, the second adsorption column (R2) is desorbed, the third adsorption column (R3) is cooled, and the fourth adsorption column (R4) performs adsorption operation
  • the configuration in which the CO 2 analyzer 6a is installed in the recycle pipe is the same as in Example 2, and thus the details are omitted.
  • the feature of this embodiment is that a CO2 analyzer is installed in the recycle pipe.
  • the cooling operation is performed using an exhaust gas containing CO2.
  • CO2 When the temperature of the adsorbent is high, CO2 is exhausted from the outlet without adsorbing to the adsorbent, and it is recycled to the adsorbing tower during adsorption through the recycle pipe, but when the temperature of the adsorbent falls in the cooling process CO2 is adsorbed and the concentration of CO2 in the outlet exhaust gas decreases.
  • the CO 2 concentration in the outlet exhaust gas is sufficiently low, for example, below the detection limit of the CO 2 analyzer, the temperature of the adsorbent becomes a temperature at which the adsorption operation can be shifted, and the cooling operation is completed.
  • the CO2 analyzer installed in this embodiment is used to measure the concentration of CO2 in the gas in the recycle pipe and to measure the timing of transition from the cooling operation to the adsorption operation.
  • FIG. 4 shows the state of the system at the time of desorption in the first adsorption column (R1), cooling in the second adsorption column (R2), adsorption in the third adsorption column (R3), and purging in the fourth adsorption column (R4)
  • a CO 2 analyzer 6 b is installed in the purge pipe at the outlet of the adsorption column.
  • the conditions of the adsorption towers performing the adsorption, purge, desorption, and cooling operations are the same as in Example 2, and thus the details are omitted.
  • the exhaust gas remaining in the gap of the adsorption tower after the adsorption operation is sucked by the rotary pump 3a, and the exhaust gas in the gap is discharged by depressurizing the inside of the adsorption tower.
  • CO 2 adsorbed to the adsorbent in particular, the physically adsorbed component is desorbed from the adsorbent as described in the second embodiment.
  • the CO2 recovery rate decreases.
  • a CO2 analyzer is installed in the purge pipe, and when the CO2 concentration in the purge exhaust gas reaches a predetermined concentration or more, the suction by the rotary pump is stopped to complete the purge operation.
  • the present embodiment it is possible to prevent the CO2 that is once adsorbed on the adsorbent in the adsorption operation from being discharged in the purge operation, and it is possible to suppress the decrease in the CO2 recovery rate.
  • FIG. 5 shows the state of the system when the first adsorption column (R1) is cooled, the second adsorption column (R2) is adsorbed, the third adsorption column (R3) is purged, and the fourth adsorption column (R4) is desorbed.
  • a CO2 analyzer 6c is installed in the exhaust gas pipe at the outlet of the adsorption tower. The conditions of the adsorption towers performing the adsorption, purge, desorption, and cooling operations are the same as in Example 2, and thus the details are omitted.
  • the outlet exhaust gas does not contain CO2, but the amount of CO2 that can be adsorbed on the adsorbent is saturated in the process of the adsorption operation. It is thought that the concentration of CO2 in the medium will gradually increase. Since the exhaust gas at the outlet of the adsorption tower at the time of the adsorption operation is likely to be exhausted to the atmosphere, if CO2 is contained in the exhaust gas at the outlet, the CO2 recovery rate is reduced.
  • a CO 2 analyzer is installed in the exhaust gas pipe at the outlet of the adsorption tower, and the supply of the exhaust gas to the adsorption tower is stopped when the CO 2 concentration in the gas flowing in the exhaust gas pipe becomes a predetermined concentration or more.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Analytical Chemistry (AREA)
  • Environmental & Geological Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Biomedical Technology (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Treating Waste Gases (AREA)
  • Carbon And Carbon Compounds (AREA)
  • Solid-Sorbent Or Filter-Aiding Compositions (AREA)

Abstract

Dans un système qui sépare le CO2 d'un gaz contenant du CO2 en utilisant un matériau d'adsorption à l'état solide, le taux de récupération de CO2 et la pureté du CO2 récupéré sont dans une relation de compromis, et améliorer le taux de récupération du CO2 tout en maintenant la pureté du CO2 constitue un problème dans un tel système. Dans la présente invention, afin de récupérer le CO2 restant dans un espace après la désorption du CO2 à partir d'un matériau d'adsorption dans une étape de désorption, un gaz est purgé pour forcer le CO2 restant à sortir lors du refroidissement (constituant également l'étape de purge), et ce gaz est renvoyé pour être utilisé dans une étape d'adsorption, ce qui améliore le taux de récupération du CO2.
PCT/JP2018/036977 2017-10-10 2018-10-03 Procédé de séparation/récupération de co2 et équipement de séparation/récupération de co2 WO2019073866A1 (fr)

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JP2017196532A JP2021035654A (ja) 2017-10-10 2017-10-10 Ｃｏ２分離方法及び設備

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2024048566A1 (fr) * 2022-09-01 2024-03-07 日本碍子株式会社 Procédé de collecte de gaz acide

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20100135009A (ko) * 2009-06-16 2010-12-24 한국에너지기술연구원 연소배가스에서 온도변동 흡착공정을 이용한 이산화탄소를 회수 장치 및 그 운전방법
JP2013061088A (ja) * 2011-09-12 2013-04-04 Hitachi Ltd Ｃｏ２回収装置を備えたボイラーの熱回収システム
JP2013059703A (ja) * 2011-09-12 2013-04-04 Hitachi Ltd 二酸化炭素捕捉材
JP2013147386A (ja) * 2012-01-20 2013-08-01 Hitachi Ltd Ｃｏ２分離回収装置

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR20100135009A (ko) * 2009-06-16 2010-12-24 한국에너지기술연구원 연소배가스에서 온도변동 흡착공정을 이용한 이산화탄소를 회수 장치 및 그 운전방법
JP2013061088A (ja) * 2011-09-12 2013-04-04 Hitachi Ltd Ｃｏ２回収装置を備えたボイラーの熱回収システム
JP2013059703A (ja) * 2011-09-12 2013-04-04 Hitachi Ltd 二酸化炭素捕捉材
JP2013147386A (ja) * 2012-01-20 2013-08-01 Hitachi Ltd Ｃｏ２分離回収装置

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2024048566A1 (fr) * 2022-09-01 2024-03-07 日本碍子株式会社 Procédé de collecte de gaz acide

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