WO2024247668A1 - ガス分離膜、ガス分離モジュール、ガス分離モジュールの製造方法、ガス分離回収システム、及びガス分離回収方法 - Google Patents

ガス分離膜、ガス分離モジュール、ガス分離モジュールの製造方法、ガス分離回収システム、及びガス分離回収方法 Download PDF

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WO2024247668A1
WO2024247668A1 PCT/JP2024/017505 JP2024017505W WO2024247668A1 WO 2024247668 A1 WO2024247668 A1 WO 2024247668A1 JP 2024017505 W JP2024017505 W JP 2024017505W WO 2024247668 A1 WO2024247668 A1 WO 2024247668A1
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region
gas
gas separation
membrane
recovery
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PCT/JP2024/017505
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English (en)
French (fr)
Japanese (ja)
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孝彦 大坪
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Dic株式会社
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Priority to JP2025501643A priority Critical patent/JP7732615B2/ja
Publication of WO2024247668A1 publication Critical patent/WO2024247668A1/ja

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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
    • B01D53/22—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 diffusion
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D63/00—Apparatus in general for separation processes using semi-permeable membranes
    • B01D63/02—Hollow fibre modules
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B01D69/02—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor characterised by their properties
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B01D69/08—Hollow fibre membranes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B01D69/10—Supported membranes; Membrane supports
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D69/00—Semi-permeable membranes for separation processes or apparatus characterised by their form, structure or properties; Manufacturing processes specially adapted therefor
    • B01D69/12—Composite membranes; Ultra-thin membranes

Definitions

  • the present invention relates to a gas separation membrane, a gas separation module, a method for manufacturing a gas separation module, a gas separation and recovery system, and a gas separation and recovery method.
  • Patent Document 1 describes a gas separation membrane for separating gas components such as carbon dioxide from a mixed raw gas.
  • the gas separation membrane includes a base membrane having many holes and a separation active layer.
  • the base membrane includes a porous layer having holes and a dense layer having no holes.
  • the gas separation membrane is provided on the dense layer of the base membrane.
  • Patent Document 1 also describes a gas separation module in which, when the base layer is made of hollow fibers, both ends of a hollow fiber bundle contained in a housing are fixed with an adhesive.
  • This gas separation membrane is manufactured by impregnating the base membrane with a viscous aqueous solution, applying a coating liquid consisting of an aqueous solution containing a gas separating polymer that forms a separation active layer to the surface of the base membrane, and drying and removing the solvent in the coating liquid from the base membrane.
  • the gas separation membrane in the manufacture of the gas separation module described in Patent Document 1, the gas separation membrane must be produced by carrying out the steps of impregnating the base membrane with a viscous aqueous solution, applying a coating liquid to the surface of the base membrane, and drying the solvent in the coating liquid, and then the gas separation membrane must be assembled into a housing. This creates the problem of complicated manufacturing.
  • the present invention aims to provide a gas separation membrane, a gas separation module, a method for manufacturing a gas separation module, a gas separation and recovery system, and a gas separation and recovery method that can improve the permeability and selectivity of acidic gases.
  • the gas separation membrane of the present invention comprises a hollow fiber membrane having a hollow portion formed on the inside, and a separation functional gel containing a carrier capable of chemically interacting with an acidic gas, the hollow fiber membrane having a porous layer adjacent to the hollow portion and a dense layer located on the outer periphery of the porous layer, and the separation functional gel being supported on the surface of the porous layer.
  • the separating gel is supported on the surface of the porous layer, so acidic gases can be selectively separated.
  • the porous layer adjacent to the hollow portion has open pores that open into the hollow portion, so the surface of the porous layer includes not only the inner peripheral surface of the porous layer, but also the pore forming surface that forms the open pores that open into the hollow portion. Therefore, the surface area of the separating gel can be increased to be greater than or equal to the area of the inner peripheral surface of the hollow fiber membrane. This can improve the permeability and selectivity of acidic gases.
  • the separation functional gel may be supported on the inner circumferential surface of the porous layer and on a pore forming surface that forms open pores that open to the hollow portion.
  • the separation functional gel is supported on the inner circumferential surface of the porous layer and on a pore forming surface that forms open pores that open to the hollow portion, so that the permeability and selectivity of acidic gases can be improved.
  • the separation functional gel may cover the surface of the porous layer.
  • the separation functional gel covers the surface of the porous layer, so that the permeability and selectivity of acidic gases can be improved.
  • the carrier may be capable of chemically interacting with carbon dioxide.
  • the carrier capable of chemically interacting with carbon dioxide is contained in the separation functional gel, so that carbon dioxide can be selectively separated.
  • the separation factor of carbon dioxide from nitrogen may be 2 or more and 100,000 or less.
  • the separation function gel is supported on the surface of the porous layer, so the separation factor of carbon dioxide from nitrogen can be increased.
  • the separation factor of carbon dioxide from nitrogen is 2 or more, it is possible to suppress the permeation of nitrogen accompanying carbon dioxide. This improves the carbon dioxide separation performance.
  • the separation factor of carbon dioxide from nitrogen is 100,000 or less, the gas separation membrane can be easily manufactured.
  • the carrier may be an ionic liquid.
  • the ionic liquid which is the carrier, is contained in the separation functional gel, so that it can appropriately chemically interact with acidic gases, particularly carbon dioxide.
  • the gas separation module of the present invention comprises a gas separation membrane according to any one of [1] to [6] above, a housing that contains the gas separation membrane, and a partition that divides the area within the housing into an intramembrane area that is connected to the hollow area and an extramembrane area that is not connected to the hollow area, and the housing has an intramembrane area port that is connected to the intramembrane area and an extramembrane area port that is connected to the extramembrane area.
  • the region within the housing is divided into an intra-membrane region that is connected to the hollow portion, and an extra-membrane region that is not connected to the hollow portion, so that by supplying a target gas containing an acidic gas to either the intra-membrane region or the extra-membrane region, the acidic gas can be selectively separated from the target gas and permeated through the gas separation membrane.
  • the housing has an intra-membrane region port that is connected to the intra-membrane region, and an extra-membrane region port that is connected to the extra-membrane region
  • the target gas can be supplied from either the intra-membrane region port or the extra-membrane region port, and the acidic gas can be recovered from the other of the intra-membrane region or the extra-membrane region.
  • the gas separation module is equipped with the above-mentioned gas separation membrane, the permeability and selectivity of acidic gas can be improved.
  • the intramembrane region port may have a first intramembrane region port and a second intramembrane region port located on opposite sides of the hollow portion.
  • the intramembrane region port has a first intramembrane region port and a second intramembrane region port located on opposite sides of the hollow portion, so that a flow path passing through the intramembrane region is formed between the first intramembrane region port and the second intramembrane region port. This can improve the flow of fluid in the intramembrane region.
  • the extramembrane region port may have a first extramembrane region port and a second extramembrane region port spaced apart from each other.
  • the extramembrane region port has a first extramembrane region port and a second extramembrane region port spaced apart from each other, so that a flow path passing through the extramembrane region is formed between the first extramembrane region port and the second extramembrane region port. This can improve the flow of fluid in the extramembrane region.
  • the method for producing a gas separation module of the present invention includes a preparation step of preparing a module intermediate in which the separation functional gel is not supported on the surface of the porous layer in the gas separation module described in any one of [7] to [9] above, a supply step of supplying a gel liquid containing the carrier to the intramembrane region of the module intermediate, a discharge step of discharging the gel liquid from the intramembrane region, and a gel generation step of gelling the gel liquid remaining in the intramembrane region.
  • a gel liquid can be supplied to the intramembrane region of a module intermediate, which is a gas separation module in which no separation functional gel is supported on the surface of the porous layer, so that the gel liquid can be attached to the surface of the porous layer. Therefore, the gel liquid can be discharged from the intramembrane region, and the gel liquid remaining in the intramembrane region can be gelled to produce a separation functional gel supported on the surface of the porous layer.
  • This makes it possible to produce a gas separation module in which a separation functional gel is supported on the surface of the porous layer. In other words, it is possible to produce a gas separation module that can improve the permeability and selectivity of acidic gases.
  • the separation functional gel can be supported on the surface of the porous layer after producing a module intermediate in which a hollow fiber membrane is housed in a housing, the gas separation module can be easily produced.
  • the gas separation and recovery system of the present invention comprises a gas separation module according to any one of the above [7] to [9], a target gas supply device that is connected to a target gas region, which is either the intramembrane region or the extramembrane region of the gas separation module, and supplies a target gas containing an acidic gas to the target gas region, and an acidic gas recovery device that is connected to a recovery region, which is the other of the intramembrane region or the extramembrane region of the gas separation module, and aspirates the recovery region.
  • the target gas is supplied to the target gas area, and the recovery area is suctioned, allowing the acid gas to be selectively separated from the target gas and permeate the gas separation membrane. This allows the acid gas to be recovered from the recovery area. Furthermore, since the system is equipped with the above-mentioned gas separation membrane, it is possible to improve the permeability and selectivity of the acid gas.
  • the gas separation and recovery system of the present invention comprises a first gas separation module which is a gas separation module described in any one of [7] to [9] above, and a second gas separation module which is a gas separation module described in any one of [7] to [9] above, and a target gas region which is either the intramembrane region or the extramembrane region of the second gas separation module is connected to a recovery region which is the other of the intramembrane region or the extramembrane region of the first gas separation module.
  • the target gas passes through the first gas separation and recovery system and then the second gas separation and recovery system, thereby increasing the concentration of the recovered acidic gas. Therefore, even if the separation performance of the acidic gas is insufficient in one gas separation module, the concentration of the recovered acidic gas can be sufficiently increased.
  • the gas separation and recovery system described in [12] above may further include a pump disposed in a flow path that communicates the recovery region of the first gas separation module and the target gas region of the second gas separation module.
  • a pump disposed in a flow path that communicates the recovery region of the first gas separation module and the target gas region of the second gas separation module by providing a pump disposed in a flow path that communicates the recovery region of the first gas separation module and the target gas region of the second gas separation module, the gas recovered in the recovery region of the first gas separation module can be pressurized and supplied to the target gas region of the second gas separation module.
  • the gas separation and recovery system described in [12] or [13] above may further include a target gas supply device that is connected to a target gas region, which is either the intramembrane region or the extramembrane region of the first gas separation module, and supplies a target gas containing an acidic gas to the target gas region, and an acidic gas recovery device that is connected to a recovery region, which is the other of the intramembrane region or the extramembrane region of the second gas separation module, and aspirates the recovery region. Since this gas separation and recovery system includes a target gas supply device and an acidic gas recovery device, it is possible to supply a target gas to the gas separation and recovery system and recover an acidic gas from the gas separation and recovery system without connecting other devices.
  • the gas separation and recovery method of the present invention is a gas separation and recovery method for separating and recovering an acidic gas from a target gas containing an acidic gas using the gas separation and recovery system described in [11] or [14] above, in which the target gas is supplied from the target gas supply device to the target gas region, and the recovery region is aspirated to recover the acidic gas from the recovery region.
  • the target gas is supplied from the target gas supply device to the target gas region, and the recovery region is aspirated to recover the acidic gas from the recovery region, thereby improving the permeability and selectivity of the acidic gas and improving the efficiency of separation and recovery of the acidic gas.
  • the present invention can improve the permeability and selectivity of acid gases.
  • FIG. 1 is a schematic cross-sectional view of a gas separation module according to an embodiment.
  • 2 is a schematic cross-sectional view taken along line II-II in FIG. 1.
  • 3 is a schematic cross-sectional view taken along line III-III shown in FIG. 2.
  • 3 is a schematic cross-sectional view showing a preparation step in a method for producing a gas separation module.
  • FIG. 5 is a schematic cross-sectional view taken along line VV shown in FIG. 4.
  • 4 is a schematic cross-sectional view showing a supplying step in a method for producing a gas separation module.
  • FIG. 7 is a schematic cross-sectional view taken along line VII-VII shown in FIG. 6.
  • FIG. 4 is a schematic cross-sectional view showing a discharging step in a method for producing a gas separation module.
  • FIG. 9 is a schematic cross-sectional view taken along line IX-IX shown in FIG. 8.
  • 1 is a schematic diagram of a gas separation and recovery system according to an embodiment.
  • FIG. 2 is a schematic cross-sectional view showing an enlarged portion of the inside of the gas separation module.
  • FIG. 2 is a schematic diagram of another gas separation and recovery system according to an embodiment.
  • FIG. 11 is a schematic cross-sectional view of a modified gas separation module.
  • FIG. 11 is a schematic cross-sectional view of a gas separation module according to another modified example.
  • FIG. 13 is a schematic diagram of a modified gas separation and recovery system.
  • FIG. 1 is a schematic cross-sectional view of a gas separation module according to an embodiment of the present invention.
  • the gas separation module 1 shown in Fig. 1 is a module for selectively separating acidic gas from a target gas containing acidic gas.
  • acidic gases examples include carbon dioxide (CO 2 ), nitrogen oxides (NOx) such as nitric oxide and nitrogen dioxide, sulfur oxides (SOx) such as sulfur dioxide and sulfur trioxide, hydrogen sulfide, chlorine, hydrogen chloride, etc.
  • CO 2 carbon dioxide
  • NOx nitrogen oxides
  • SOx sulfur oxides
  • the acidic gas is preferably carbon dioxide.
  • Target gases include, for example, exhaust gas from power plants such as thermal power plants and biomass power plants, exhaust gas from cement factories, exhaust gas from steel mills, exhaust gas from factories such as oil refineries and chemical plants, exhaust gas from facilities related to hydrogen and ammonia production, and natural gas.
  • the gas separation module 1 comprises one or more gas separation membranes 2, a housing 3, and a partition section 4.
  • Gas separation membrane 2 is a hollow fiber membrane. Gas separation membrane 2 has the function of selectively separating acidic gas from the target gas. Selective separation of acidic gas means, for example, that acidic gas has a faster permeation rate than gases other than acidic gas, and thus acidic gas is preferentially permeated.
  • the outer diameter of the gas separation membrane 2 is not particularly limited, but can be, for example, 100 ⁇ m to 3000 ⁇ m, 100 ⁇ m to 500 ⁇ m, or 100 ⁇ m to 300 ⁇ m.
  • the inner diameter of the gas separation membrane 2 is not particularly limited, but can be, for example, 10 ⁇ m to 500 ⁇ m, 50 ⁇ m to 300 ⁇ m, or 80 ⁇ m to 200 ⁇ m.
  • the membrane thickness of the gas separation membrane 2 is not particularly limited, but can be, for example, 5 ⁇ m to 200 ⁇ m, 10 ⁇ m to 100 ⁇ m, or 20 ⁇ m to 50 ⁇ m.
  • FIG. 2 is a schematic cross-sectional view taken along line II-II in FIG. 1.
  • the gas separation membrane 2 includes a hollow fiber membrane 21 and a separation functional gel 22.
  • the hollow fiber membrane 21 is a hollow fiber-shaped membrane with a hollow portion 21a formed on the inside.
  • the hollow fiber membrane 21 is a permeable membrane that allows gases such as acid gases to pass through but does not allow liquids such as gel liquids to pass through, as described below.
  • materials for the hollow fiber membrane 21 include polyolefin-based resins such as polypropylene, polyethylene, and polymethylpentene (also known as PMP, 4-methylpentene-1, and poly(4-methylpentene-1)), silicone-based resins such as polydimethylsiloxane and its copolymers, and fluororesins such as PTFE and vinylidene fluoride.
  • FIG. 3 is a schematic cross-sectional view taken along line III-III in FIG. 2.
  • the hollow fiber membrane 21 has a porous layer 211 and a dense layer 212.
  • the porous layer 211 is a layer adjacent to the hollow portion 21a. In other words, the porous layer 211 is located in the innermost layer of the hollow fiber membrane 21.
  • the porous layer 211 is formed in a ring shape and forms the inner surface of the hollow fiber membrane 21.
  • the porous layer 211 is porous. Porous means, for example, that it has a plurality of holes 211a through which the gel liquid can pass. In other words, the porous layer 211 has a plurality of holes 211a through which the gel liquid can pass.
  • the plurality of holes 211a includes a plurality of open holes 211b that are open to the hollow portion 21a.
  • the shape of the open holes 211b is not particularly limited.
  • the open hole 211b may be, for example, a single spherical hole, a hole in which a plurality of spherical holes are connected, a single slit-shaped hole, a hole in which a plurality of slit-shaped holes are connected, or a hole of various other shapes.
  • the porous layer 211 is formed, for example, in a sponge-like shape.
  • the porous layer 211 also functions as a layer that supports the dense layer 212.
  • the dense layer 212 is a layer located on the outer periphery of the porous layer 211 (the outer periphery of the hollow fiber membrane 21).
  • the dense layer 212 is formed in a ring shape and covers the porous layer 211 from the outer periphery.
  • the dense layer 212 may be located at any position of the hollow fiber membrane 21 as long as it is located on the outer periphery of the porous layer 211. From the viewpoint of easily forming the dense layer 212, the dense layer 212 may be located, for example, in the outermost layer of the hollow fiber membrane 21. Note that if the dense layer 212 is not located in the outermost layer of the hollow fiber membrane 21, a layer similar to the porous layer 211 may be formed on the outer periphery of the dense layer 212.
  • the dense layer 212 is a non-porous layer that has no porosity. Not having porosity means, for example, that it has no pores through which the gel liquid can pass. In other words, the dense layer 212 has no pores through which the gel liquid can pass. In this case, the dense layer 212 may have pores through which the gel liquid cannot pass.
  • the separation functional gel 22 is a gel containing a carrier capable of chemically interacting with acidic gas.
  • the separation functional gel 22 has the function of selectively separating acidic gas from the target gas by chemically interacting with the acidic gas.
  • the carriers contained in the separation functional gel 22 may be, for example, ionic liquids, deep eutectic solvents (DES), which are compounds that exhibit properties similar to ionic liquids, or organic amines.
  • Ionic liquids are salts whose molecules are designed to be liquid at room temperature.
  • Deep eutectic solvents are compounds that are a mixture of hydrogen bond donor compounds and hydrogen bond acceptor compounds, and are compounds that become liquid at room temperature, just like ionic liquids.
  • ionic liquids combining ammonium cations and fluorine-containing anions e.g., [N 1114 ][TFSA], [choline][TFSA], etc.
  • ionic liquids combining imidazolium cations and fluorine-containing anions e.g., [emim][TFSA], [emim][TfO], [emim][BF 4 ], [bmim][TFSA], [bmim][Tf 3 C], [bmim][TfO], [bmim][BF 4 ], [bmim][PF 6 ], [bmim][TFA], [hmim][TFSA], [omim][TFSA], [C 6 H 4 F 9 ionic liquids combining imidazolium cations and cyano group-containing anions (e.g., [emim][DCA], [emim][C(CN) 3 ], [emim][B
  • examples of deep eutectic solvents that can chemically interact favorably with carbon dioxide include hydrogen bond donors selected from amide, carboxylic acid, and alcohol compounds, and hydrogen bond acceptors selected from ammonium salts and phosphonium salts.
  • Specific examples include deep eutectic solvents made by mixing choline chloride and urea, and mixtures of choline chloride and ethylene glycol.
  • the separating gel 22 is supported on the surface 211c of the porous layer 211.
  • the surface of the porous layer 211 does not exist on the outer periphery of the porous layer 211, but exists only on the inner periphery (hollow portion 21a side) of the porous layer 211. Therefore, the surface of the porous layer 211 that leads to the hollow portion 21a becomes the surface 211c of the porous layer 211.
  • the surface 211c of the porous layer 211 is composed of the inner periphery 211d of the porous layer 211 and the hole forming surface 211e that forms each of the multiple open holes 211b that open to the hollow portion 21a.
  • the inner periphery 211d is also the inner periphery of the hollow fiber membrane 21.
  • the separating gel 22 is supported on the inner surface 211d of the porous layer 211 and on the hole forming surface 211e that forms each of the multiple open holes 211b that open into the hollow portion 21a.
  • the separation gel 22 covers the surface 211c of the porous layer 211. It is preferable that the separation gel 22 covers the entire surface 211c of the porous layer 211, but it is not necessary that the separation gel 22 covers the entire surface 211c of the porous layer 211.
  • the coverage rate of the surface 211c of the porous layer 211 by the separation gel 22 can be, for example, 50% or more, 75% or more, or 90% or more.
  • one of the indices for separating carbon dioxide from the target gas is the separation factor ⁇ of carbon dioxide with respect to nitrogen.
  • the separation factor ⁇ can be obtained, for example, by measuring the permeation rates of carbon dioxide and nitrogen based on ASTM D-1434, and then calculating the ratio of the permeation rate of carbon dioxide to the permeation rate of nitrogen (permeation rate of carbon dioxide/permeation rate of nitrogen).
  • Carbon dioxide can be separated from the target gas when the separation factor ⁇ of the gas separation membrane 2 for carbon dioxide with respect to nitrogen is greater than 1.
  • the separation function gel 22 is supported on the surface 211c of the porous layer 211, so that the separation factor ⁇ of the gas separation membrane 2 for carbon dioxide with respect to nitrogen is increased.
  • the separation factor ⁇ of the gas separation membrane 2 for carbon dioxide with respect to nitrogen may be, for example, 2 or more, 10 or more, 30 or more, or 50 or more.
  • the upper limit of the separation factor ⁇ of the gas separation membrane 2 for carbon dioxide with respect to nitrogen is the case where only carbon dioxide permeates, in which case it is infinite.
  • the separation factor ⁇ of the gas separation membrane 2 for carbon dioxide relative to nitrogen may be, for example, 100,000 or less, 30,000 or less, 5,000 or less, or 1,000 or less.
  • the separation factor ⁇ of the carbon dioxide relative to nitrogen in each of the multiple gas separation membranes 2 may be, for example, 2 or more and 100,000 or less, 10 or more and 30,000 or less, 30 or more and 5,000 or less, or 50 or more and 1,000 or less.
  • the housing 3 is formed in a cylindrical shape and contains multiple gas separation membranes 2.
  • the partition section 4 divides the area inside the housing 3 into an intra-membrane area A that is connected to the hollow section 21a, and an extra-membrane area B that is not connected to the hollow section 21a.
  • the area inside the housing 3 is divided by the partition section 4 into an intra-membrane area A and an extra-membrane area B.
  • the partition section 4 is composed of, for example, a first sealing section 41 that seals between the tip end of one side of one or more gas separation membranes 2 and the housing 3, and a second sealing section 42 that seals between the tip end of the other side of one or more gas separation membranes 2 and the housing 3.
  • the multiple gas separation membranes 2 are also referred to as a membrane bundle.
  • the first sealing portion 41 fills the entire area except for the one or more gas separation membranes 2 in a cross section perpendicular to the central axis of the housing 3. In other words, the first sealing portion 41 fills between one end of the one or more gas separation membranes 2 and the inner wall of the housing 3. When multiple gas separation membranes 2 are accommodated in the housing 3, the first sealing portion 41 also fills between the multiple gas separation membranes 2.
  • the hollow portion 21a of each of the one or more gas separation membranes 2 is not sealed by the first sealing portion 41 and is open from the first sealing portion 41.
  • the first sealing portion 41 is formed, for example, from a resin.
  • the second sealing portion 42 fills the entire area except for the one or more gas separation membranes 2 in a cross section perpendicular to the central axis of the housing 3. In other words, the second sealing portion 42 fills between the other end of the one or more gas separation membranes 2 and the inner wall of the housing 3. When multiple gas separation membranes 2 are accommodated in the housing 3, the second sealing portion 42 also fills between the multiple gas separation membranes 2.
  • the hollow portion 21a of each of the one or more gas separation membranes 2 is not sealed by the second sealing portion 42 and is open from the second sealing portion 42.
  • the second sealing portion 42 is formed, for example, from a resin.
  • the hollow portions 21a of the multiple gas separation membranes 2, the region a1 of the first sealing portion 41 opposite the second sealing portion 42, and the region a2 of the second sealing portion 42 opposite the first sealing portion 41 form the intra-membrane region A.
  • the region outside the multiple gas separation membranes 2 between the first sealing portion 41 and the second sealing portion 42 forms the extra-membrane region B.
  • the housing 3 has a first intramembrane region port 31 and a second intramembrane region port 32 that are connected to the intramembrane region A, and a first extramembrane region port 33 and a second extramembrane region port 34 that are connected to the extramembrane region B.
  • the first intramembrane region port 31 and the second intramembrane region port 32 are openings that open the intramembrane region A to the outside of the housing 3.
  • the first intramembrane region port 31 and the second intramembrane region port 32 are located on opposite sides of the hollow portion 21a.
  • the first intramembrane region port 31 is located on the opposite side of the second sealing portion 42 of the first sealing portion 41 so as to be adjacent to region a1 on the opposite side of the second sealing portion 42 of the first sealing portion 41 in the intramembrane region A.
  • the second intramembrane region port 32 is located on the opposite side of the first sealing portion 41 of the second sealing portion 42 so as to be adjacent to region a2 on the opposite side of the first sealing portion 41 of the second sealing portion 42 in the intramembrane region A.
  • the first extramembrane region port 33 and the second extramembrane region port 34 are openings that open the extramembrane region B to the outside of the housing 3.
  • the first extramembrane region port 33 and the second extramembrane region port 34 may be located in any position, but are preferably spaced apart from each other and are preferably located so as to sandwich one or more gas separation membranes 2.
  • the first extramembrane region port 33 is located near the second sealing portion 42
  • the second extramembrane region port 34 is located on the opposite side of the first extramembrane region port 33 across one or more gas separation membranes 2 near the first sealing portion 41.
  • FIG 4 is a schematic cross-sectional view showing a preparation step in the manufacturing method of a gas separation module.
  • Figure 5 is a schematic cross-sectional view taken along line V-V shown in Figure 4.
  • a preparation step is performed to prepare a module intermediate 11.
  • the module intermediate 11 is a gas separation module 1 in which no separation functional gel 22 is supported on the surface 211c of the porous layer 211.
  • the module intermediate 11 is similar to the gas separation module 1 described above, except that no separation functional gel 22 is supported on the surface 211c of the porous layer 211.
  • the module intermediate 11 is a module in which a hollow fiber membrane 21 in the form of a hollow fiber with a hollow portion 21a formed on the inside is housed in a housing 3, the hollow fiber membrane 21 has a porous layer 211 adjacent to the hollow portion 21a and a dense layer 212 located on the outer periphery of the porous layer 211, and the region inside the housing 3 is divided by a partition portion 4 into an intra-membrane region A that is connected to the hollow portion 21a and an extra-membrane region B that is not connected to the hollow portion 21a.
  • FIG. 6 is a schematic cross-sectional view showing the supplying step in the manufacturing method of the gas separation module.
  • FIG. 7 is a schematic cross-sectional view of the VII-VII line shown in FIG. 6.
  • a supplying step is performed in which gel liquid L containing a carrier capable of chemically interacting with acidic gas is supplied to the intramembrane region A of the module intermediate 11.
  • the gel liquid L is a precursor of the separation functional gel, and is a liquid that becomes the separation functional gel by gelling.
  • the gel liquid L is also called a sol.
  • the gel liquid L includes, for example, a carrier and a hydrophilic cross-linked polymer such as polyethylene glycol, polypropylene glycol, polyamine, polyethyleneimine, polyvinyl alcohol, polyacrylic acid, polyacrylamide, gelatin, polyglutamic acid, and polyaspartic acid. Any one of these hydrophilic cross-linked polymers may be used alone, or two or more may be mixed or copolymerized for use.
  • the gel liquid L is circulated from the first intramembrane region port 31 to the second intramembrane region port 32 so that the intramembrane region A is filled with the gel liquid L.
  • FIG. 8 is a schematic cross-sectional view showing the discharge step in the manufacturing method of the gas separation module.
  • FIG. 9 is a schematic cross-sectional view along line IX-IX shown in FIG. 8.
  • a discharge step is performed to discharge the gel liquid L from the intramembrane region A.
  • the supply of the gel liquid L to the intramembrane region A is stopped, and the gel liquid filled in the intramembrane region A is discharged from the second intramembrane region port 32.
  • a part of the gel liquid L remains in the intramembrane region A and is supported on the surface 211c of the porous layer 211.
  • the gel liquid L may be discharged from the second intramembrane region port 32 by gravity, by pushing out with a pressure device (not shown), or by suction with a suction device (not shown).
  • a gel generation process is performed to gel the gel liquid L remaining in the intra-membrane region A.
  • Gelation may be performed, for example, by drying the gel liquid L to volatilize the solvent contained in the gel liquid L, by heating the gel liquid L to promote cross-linking of the gel liquid L, or by UV irradiation when cross-linking of the gel liquid L is performed by UV irradiation.
  • a separation functional gel 22 supported on the surface 211c of the porous layer 211 is generated. In this way, the gas separation module 1 is manufactured.
  • FIG. 10 is a schematic diagram of a gas separation and recovery system according to an embodiment.
  • the gas separation and recovery system 101A shown in Fig. 10 is a system for selectively separating an acidic gas AG from a target gas TG.
  • the gas separation and recovery system 101A includes the above-mentioned gas separation module 1, a target gas supply device 102, and an acidic gas recovery device 103.
  • the target gas supply device 102 is a device that is connected to the intra-membrane region A of the gas separation module 1 and supplies the target gas TG to the intra-membrane region A.
  • the target gas supply device 102 has, for example, a compressor 104 that compresses and sends out the target gas TG, and the operation of this compressor 104 makes it possible to compress the target gas TG and supply it to the gas separation module 1.
  • the target gas supply device 102 is connected to the first intra-membrane region port 31 of the gas separation module 1 by the target gas supply path 105.
  • the target gas supply path 105 is formed, for example, by a tubular member such as a pipe.
  • the target gas supply device 102 is connected to the target gas supply path 105 and is thereby in communication with the intra-membrane region A. Therefore, the target gas TG sent out from the target gas supply device 102 is supplied to the intra-membrane region A of the gas separation module 1 through the target gas supply path 105.
  • the target gas TG supplied to the intra-membrane region A is discharged from the second intra-membrane region port 32 to the outside of the gas separation and recovery system 101A.
  • the second intra-membrane region port 32 is connected to a target gas discharge path 106 for discharging the target gas TG from the intra-membrane region A.
  • the gas discharged from the target gas discharge path 106 is ideally a gas from which acidic gases have been completely removed, but in reality, it is a target gas with a reduced concentration of acidic gases.
  • the target gas discharge path 106 is formed, for example, by a tubular member such as a pipe.
  • a flow rate control valve 107 is attached to the target gas discharge path 106 to adjust (limit) the flow rate of the target gas TG so that the target gas TG is maintained at a high pressure in the intra-membrane region A.
  • the acidic gas recovery device 103 is connected to the membrane extra-region B of the gas separation module 1, and is a device for sucking the membrane extra-region B and recovering the acidic gas AG from the membrane extra-region B.
  • the gas recovered by the acidic gas recovery device 103 is ideally only acidic gas, but in reality, it is a target gas with an increased concentration of acidic gas.
  • the acidic gas recovery device 103 has a suction device 108 such as a vacuum pump, and the operation of this suction device 108 makes it possible to suck the membrane extra-region B and recover the acidic gas from the membrane extra-region B.
  • the acidic gas recovery device 103 is connected to the second membrane extra-region port 34 of the gas separation module 1 by the acidic gas recovery line 109.
  • the acidic gas recovery line 109 is formed, for example, by a tubular member such as a pipe.
  • the acidic gas recovery device 103 is connected to the acidic gas recovery line 109 and is connected to the membrane extra-region B. Therefore, the suction force of the suction device 108 acts on the membrane extra-region B of the gas separation module 1 through the acidic gas recovery line 109.
  • the acidic gas that has permeated the gas separation membrane 2 is discharged outside the gas separation and recovery system 101A through the acidic gas recovery line 109 and is recovered in the acidic gas recovery device 103.
  • the first membrane extra-region port 33 is closed. However, in order to facilitate the discharge of the acid gas AG from the membrane extra-region B, a carrier gas supply device (not shown) that supplies a carrier gas (sweep gas) such as helium or argon to the membrane extra-region B may be connected to the first membrane extra-region port 33.
  • a carrier gas such as helium or argon
  • the intramembrane region A is the target gas region to which the target gas TG is supplied
  • the extramembrane region B is the recovery region to which the acid gas AG is sucked and recovered.
  • This gas separation and recovery method is a method for separating and recovering an acid gas AG from a target gas TG using a gas separation and recovery system 101A shown in FIG.
  • the target gas TG is supplied from the target gas supply device 102 to the intra-membrane region A. That is, by operating the compressor 104 of the target gas supply device 102, the target gas TG is compressed and supplied to the intra-membrane region A from the target gas supply path 105 and the first intra-membrane region port 31. At this time, it is preferable to adjust the flow rate of the target gas TG in the target gas discharge path 106 by the flow control valve 107 so that the target gas TG is maintained in a high-pressure state in the intra-membrane region A.
  • the extra-membrane region B is aspirated by the acidic gas recovery device 103. That is, by operating the aspirator 108, gas is sent from the gas separation module 1 side to the opposite side of the gas separation module 1 in the acidic gas recovery path 109, and the extra-membrane region B is aspirated.
  • FIG. 11 is a schematic cross-sectional view of an enlarged portion of the inside of the gas separation module.
  • the target gas TG from which the acidic gas AG has been separated is discharged from the intra-membrane region A to the target gas discharge path 106.
  • the acidic gas AG separated from the target gas TG and permeating the gas separation membrane 2 is discharged from the extra-membrane region B to the acidic gas recovery path 109.
  • the acidic gas AG is then recovered through the acidic gas recovery path 109.
  • Fig. 12 is a schematic diagram of another gas separation and recovery system according to an embodiment.
  • the gas separation and recovery system 101B shown in Fig. 11 is basically the same as the gas separation and recovery system 101A shown in Fig. 10, but differs from the gas separation and recovery system 101A in that the outer membrane region B is the target gas region to which the target gas TG is supplied, and the inner membrane region A is the recovery region to which the acid gas AG is sucked and recovered. Therefore, only the differences from the gas separation and recovery system 101A will be described below, and the same description as the gas separation and recovery system 101A will be omitted.
  • the gas separation and recovery system 101B includes the above-mentioned gas separation module 1, a target gas supply device 102, and an acid gas recovery device 103.
  • the target gas supply device 102 is connected to the first extra-membrane region port 33 of the gas separation module 1 by a target gas supply path 105, and is in communication with the extra-membrane region B. In other words, the target gas supply device 102 supplies the target gas TG to the extra-membrane region B.
  • the second extramembrane region port 34 is connected to a target gas exhaust passage 106.
  • a flow rate control valve 107 is attached to the target gas exhaust passage 106.
  • the acidic gas recovery device 103 is connected to the first intra-membrane region port 31 of the gas separation module 1 by an acidic gas recovery path 109, and is in communication with intra-membrane region A. In other words, the acidic gas recovery device 103 sucks intra-membrane region A and recovers acidic gas from intra-membrane region A.
  • the second intra-membrane region port 32 is closed. However, to facilitate discharging the acid gas AG from the intra-membrane region A, a carrier gas supply device (not shown) that supplies a carrier gas to the intra-membrane region A may be connected to the second intra-membrane region port 32.
  • This gas separation and recovery method is a method for separating and recovering an acid gas AG from a target gas TG using a gas separation and recovery system 101B shown in FIG.
  • the target gas TG is supplied from the target gas supply device 102 to the extra-membrane region B. That is, by operating the compressor 104 of the target gas supply device 102, the target gas TG is compressed and supplied to the extra-membrane region B from the target gas supply path 105 and the first extra-membrane region port 33. At this time, it is preferable to adjust the flow rate of the target gas TG in the target gas discharge path 106 by the flow control valve 107 so that the target gas TG is maintained in a high-pressure state in the extra-membrane region B.
  • the intra-membrane region A is aspirated by the acidic gas recovery device 103. That is, by operating the aspirator 108, gas is sent from the gas separation module 1 side to the opposite side of the gas separation module 1 in the acidic gas recovery path 109, and the intra-membrane region A is aspirated.
  • the acidic gas AG contained in the target gas TG supplied to the extra-membrane region B chemically interacts with the separation functional gel 22 and permeates the gas separation membrane 2.
  • part or all of the acidic gas AG is separated from the target gas TG.
  • the target gas TG from which the acidic gas AG has been separated is then discharged from the extra-membrane region B to the target gas discharge path 106.
  • the acidic gas AG separated from the target gas TG and permeating the gas separation membrane 2 is discharged from the intra-membrane region A to the acidic gas recovery path 109.
  • the acidic gas is then recovered through the acidic gas recovery path 109.
  • the separation gel 22 is supported on the surface 211c of the porous layer 211, so that the acidic gas AG can be selectively separated. Furthermore, since the porous layer 211 adjacent to the hollow portion 21a has open holes 211b that open to the hollow portion 21a, the surface 211c of the porous layer 211 includes not only the inner peripheral surface 211d of the porous layer 211, but also the hole forming surface 211e that forms the open holes 211b that open to the hollow portion 21a. Therefore, the surface area of the separation gel 22 can be increased to be greater than the area of the inner peripheral surface of the hollow fiber membrane 21. This can improve the permeability and selectivity of the acidic gas AG.
  • the separation functional gel 22 is supported on the inner surface 211d of the porous layer 211 and on the hole forming surface 211e that forms the open hole 211b that opens to the hollow portion 21a, so that the permeability and selectivity of the acid gas AG can be improved.
  • the separation functional gel 22 covers the surface 211c of the porous layer 211, which improves the permeability and selectivity of the acid gas AG.
  • this gas separation membrane 2 can selectively separate carbon dioxide because the separation functional gel 22 contains a carrier that can chemically interact with carbon dioxide.
  • the separation coefficient ⁇ of carbon dioxide relative to nitrogen can be increased.
  • the separation coefficient ⁇ of carbon dioxide relative to nitrogen is 2 or more, 10 or more, 30 or more, or 50 or more, it is possible to suppress the permeation of nitrogen accompanying carbon dioxide. This improves the carbon dioxide separation performance.
  • the separation coefficient ⁇ of carbon dioxide relative to nitrogen is 100,000 or less, 30,000 or less, 5,000 or less, or 1,000 or less, the gas separation membrane 2 can be easily manufactured.
  • the ionic liquid which acts as a carrier, is contained in the separation functional gel 22, so that it can appropriately chemically interact with acidic gases, especially carbon dioxide.
  • the region within the housing 3 is divided into an intra-membrane region A that is connected to the hollow portion 21a and an extra-membrane region B that is not connected to the hollow portion 21a. Therefore, by supplying a target gas TG containing an acidic gas AG to either the intra-membrane region A or the extra-membrane region B, the acidic gas AG can be selectively separated from the target gas TG and permeated through the gas separation membrane 2.
  • the housing 3 has a first intra-membrane region port 31 and a second intra-membrane region port 32 that are connected to the intra-membrane region A, and a first extra-membrane region port 33 and a second extra-membrane region port 34 that are connected to the extra-membrane region B. Therefore, the target gas TG can be supplied to any of these ports, and the acidic gas AG can be recovered from any of these ports. Moreover, since the gas separation module 1 includes the above-mentioned gas separation membrane 2, the permeability and selectivity of the acidic gas AG can be improved.
  • the first intra-membrane region port 31 and the second intra-membrane region port are located on opposite sides of the hollow portion 21a, so that a flow path passing through the intra-membrane region A is formed between the first intra-membrane region port 31 and the second intra-membrane region port 32. This can improve the flow of fluid in the intra-membrane region A.
  • the first extramembrane region port 33 and the second extramembrane region port 34 are spaced apart from each other, so that a flow path passing through the extramembrane region B is formed between the first extramembrane region port 33 and the second extramembrane region port 34. This can improve the flow of fluid in the extramembrane region B.
  • the gel liquid L can be attached to the surface 211c of the porous layer 211 by supplying the gel liquid L to the membrane region A of the module intermediate 11, which is the gas separation module 1 in which the separation functional gel 22 is not supported on the surface 211c of the porous layer 211. Therefore, the gel liquid L is discharged from the membrane region A, and the gel liquid L remaining in the membrane region A is gelled, thereby generating the separation functional gel 22 supported on the surface 211c of the porous layer 211.
  • a gas separation module 1 in which the separation functional gel 22 is supported on the surface 211c of the porous layer 211 can be manufactured.
  • a gas separation module 1 that can improve the permeability and selectivity of the acidic gas AG can be manufactured. Moreover, since the separation functional gel 22 can be supported on the surface 211c of the porous layer 211 after the module intermediate 11 in which the hollow fiber membrane 21 is accommodated in the housing 3 is manufactured, the gas separation module 1 can be easily manufactured.
  • the target gas TG is supplied to the intra-membrane region A, which is the target gas region, and the extra-membrane region B, which is the recovery region, is aspirated, thereby selectively separating the acidic gas AG from the target gas TG and allowing it to permeate through the gas separation membrane 2.
  • This allows the acidic gas AG to be recovered from the extra-membrane region B.
  • the gas separation membrane 2 described above is provided, the permeability and selectivity of the acidic gas AG can be improved.
  • the target gas TG is supplied to the extra-membrane region B, which is the target gas region, and the intra-membrane region A, which is the recovery region, is suctioned, thereby selectively separating the acidic gas AG from the target gas TG and allowing it to permeate through the gas separation membrane 2.
  • This allows the acidic gas AG to be recovered from the intra-membrane region A.
  • the system is provided with the gas separation membrane 2 described above, it is possible to improve the permeability and selectivity of the acidic gas AG.
  • the target gas TG is supplied from the target gas supply device 102 to a target gas region, which is either the intra-membrane region A or the extra-membrane region B, and the recovery region, which is the other of the intra-membrane region A or the extra-membrane region B, is aspirated to recover the acid gas AG from the recovery region, thereby improving the permeability and selectivity of the acid gas AG and improving the separation and recovery efficiency of the acid gas AG.
  • one of the two ports connected to the extra-membrane region of the gas separation module 1 is blocked and does not function. Therefore, for example, as in the gas separation module 1A shown in FIG. 13, there may be only one port connected to the extra-membrane region B. In the gas separation module 1A shown in FIG. 13, only one extra-membrane region port 35 is formed in the housing 3 as a port connected to the extra-membrane region B.
  • the housing is described as having two intramembrane region ports connected to the intramembrane region and two extramembrane region ports connected to the extramembrane region.
  • the target gas can be supplied and the acidic gas can be recovered, and further, the gel liquid can be supplied and discharged, as in the gas separation module 1B shown in FIG. 14, there may be only one intramembrane region port connected to the intramembrane region, and there may be only one extramembrane region port connected to the extramembrane region.
  • the second sealing portion 42 may also be filled in each hollow portion 21a of one or more gas separation membranes 2.
  • FIG. 15 is a schematic diagram of a modified gas separation and recovery system.
  • Gas separation and recovery system 101C shown in FIG. 15 is provided with multiple gas separation and recovery systems 101A described in FIG. 10, and multiple gas separation modules 1 are connected in series.
  • Multiple gas separation modules 1 connected in series means that multiple gas separation modules 1 are connected so that the target gas TG flows in series through the multiple gas separation modules 1.
  • the acid gas recovery device 103 of the first stage gas separation and recovery system 101A and the target gas supply device 102 of the second stage gas separation and recovery system 101A are used together, and the acid gas recovery device 103 of the second stage gas separation and recovery system 101A and the target gas supply device 102 of the third stage gas separation and recovery system 101A are used together.
  • the acid gas recovery device 103 of the front stage (upstream side) gas separation and recovery system 101A and the target gas supply device 102 of the rear stage (downstream side) gas separation and recovery system 101A may be configured with a single pump.
  • a pump may be disposed in a flow path that connects the recovery region (either the intramembrane region A or the extramembrane region B) of the gas separation module 1 (first gas separation module) in the front stage (upstream side) with the target gas region (either the intramembrane region A or the extramembrane region B) of the gas separation module 1 (second gas separation module) in the rear stage (downstream side).
  • the pump is a device that pressurizes the supplied gas and sends it out, and can be, for example, a device similar to the compressor 104 or the suction device 108.
  • the concentration of the recovered acid gas AG is increased each time the target gas TG passes through each stage of the gas separation and recovery system 101A. Therefore, even if the separation performance of the acid gas AG is insufficient in one gas separation module 1, the concentration of the recovered acid gas AG can be sufficiently increased.
  • 1...gas separation module 1A...gas separation module, 1B...gas separation module, 2...gas separation membrane, 3...housing, 4...compartment, 11...module intermediate, 21...hollow fiber membrane, 21a...hollow portion, 211...porous layer, 211a...hole, 211b...open hole, 211c...surface, 211d...inner surface, 211e...hole-forming surface, 212...dense layer, 22...separation functional gel, 31...first intramembrane region port, 32...second intramembrane region port, 33...first extramembrane region port, 34...second extramembrane region port, 35...extramembrane region port, 36...intramembrane region area port, 37...extramembrane area port, 41...first sealing section, 42...second sealing section, 101A...gas separation and recovery system, 101B...gas separation and recovery system, 102...target gas supply device, 103...acid gas recovery device, 104...compressor, 105...target gas supply line

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PCT/JP2024/017505 2023-05-31 2024-05-10 ガス分離膜、ガス分離モジュール、ガス分離モジュールの製造方法、ガス分離回収システム、及びガス分離回収方法 WO2024247668A1 (ja)

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS6090005A (ja) * 1983-10-22 1985-05-21 Agency Of Ind Science & Technol 気体分離膜
US8383026B1 (en) * 2010-10-21 2013-02-26 U.S Department Of Energy Fabrication of fiber supported ionic liquids and methods of use
JP2016000402A (ja) * 2011-12-01 2016-01-07 株式会社ルネッサンス・エナジー・リサーチ 促進輸送膜の製造方法
WO2018043053A1 (ja) * 2016-08-31 2018-03-08 旭化成株式会社 気体分離膜

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JP4965927B2 (ja) 2006-08-01 2012-07-04 株式会社ルネッサンス・エナジー・リサーチ Ｃｏ２促進輸送膜及びその製造方法
JP6156838B2 (ja) 2013-03-29 2017-07-05 富士フイルム株式会社 酸性ガス分離用複合体の製造方法
JP6966993B2 (ja) 2016-03-09 2021-11-17 株式会社ルネッサンス・エナジー・リサーチ 燃焼システム

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS6090005A (ja) * 1983-10-22 1985-05-21 Agency Of Ind Science & Technol 気体分離膜
US8383026B1 (en) * 2010-10-21 2013-02-26 U.S Department Of Energy Fabrication of fiber supported ionic liquids and methods of use
JP2016000402A (ja) * 2011-12-01 2016-01-07 株式会社ルネッサンス・エナジー・リサーチ 促進輸送膜の製造方法
WO2018043053A1 (ja) * 2016-08-31 2018-03-08 旭化成株式会社 気体分離膜

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