JP6252377B2 - Multi-tube separation membrane module - Google Patents

Description

  The present invention relates to a multi-tubular separation membrane module used for separating some components from a fluid such as a solution or a mixed gas, and a tubular separation membrane connector.

  A multi-tubular separation membrane module is known as an apparatus for separating components in a solution or mixed gas. The tubular separation membrane used in this multitubular separation membrane module has a tubular porous ceramic support and a porous separation membrane made of zeolite or the like provided on the outer peripheral surface of the support. In order to separate a specific component from a fluid such as a solution or a mixed gas, the fluid of the solution is brought into contact with one (outer surface) of the separation membrane element, and the other (inner surface) is depressurized, whereby the specific component is A method of vaporizing and separating, a method of vaporizing a solution and bringing it into contact with a separation membrane in a gaseous state, and depressurizing a non-contact surface side to separate a specific component, and bringing a pressurized mixed gas into contact with the separation membrane Methods for separating specific components are known (Patent Documents 1 and 2).

JP 2013-39546 A JP 2010-247107 A

  In order to increase the separation efficiency of the multitubular separation membrane module, it is preferable to increase the length of the tubular separation membrane. However, it is difficult to manufacture a single long long ceramic separator. For example, in the example of Patent Document 1, the length of the tubular separation membrane is 1020 mm, and in Patent Document 2, it is 500 mm.

  The present invention provides a multi-tubular separation membrane module having a high separation efficiency by including a long tubular separation membrane connector in which a plurality of tubular separation membranes are connected, and the tubular separation membrane connector. Objective.

The multi-tubular separation membrane module of the present invention has a cylindrical housing and a plurality of tubular separation membrane connectors disposed in the housing in the longitudinal direction of the housing, and a fluid to be treated passes through the housing. A multi-tubular separation membrane module in which a communication fluid that flows from one end side to the other end side and permeates through a tubular separation membrane is taken out through the tubular separation membrane. It is connected via a joint pipe, and a seal ring is interposed on the contact surface between the joint pipe and the tubular separation membrane.
The tubular separation membrane connector of the present invention is characterized in that the tubular separation membranes are connected to each other through a joint tube, and a seal ring is interposed on the contact surface between the joint tube and the tubular separation membrane. .

  In the present invention, the tubular separation membrane has a tubular porous ceramic support and a ceramic separation membrane provided on the outer peripheral surface of the porous support, and the joint tube has one end on one side. The other end is inserted into the other tubular separation membrane, and the first seal ring is interposed between the outer peripheral surface of the joint tube and the inner peripheral surface of the tubular separation membrane. The joint pipe is provided with ridges on the outer peripheral surface in the middle of the longitudinal direction, and both end sides in the longitudinal direction of the ridge are stepped surfaces perpendicular to the outer peripheral surface of the joint pipe. Preferably, a second seal ring is interposed between the end surface of the tubular separation membrane and the step surface.

  In the multi-tubular separation membrane module of the present invention, a plurality of tubular separation membranes are connected by a joint tube to form a long tubular separation membrane connector, so that the membrane area is increased and the fluid is efficiently membrane-separated. be able to.

  Providing a seal ring between the end face of the tubular separation membrane and the stepped surface of the protrusions of the joint pipe prevents fluid from flowing into the porous ceramic support from the end face of the tubular separation membrane.

  The inflow of fluid into the porous ceramic support is further sufficiently prevented by coating the end face of the tubular separation membrane with glass or the like.

It is sectional drawing which follows the housing axial center line direction of the multi-tubular separation membrane module which concerns on embodiment. It is the II-II sectional view taken on the line of FIG. It is the III-III sectional view taken on the line of FIG. It is an expanded sectional view of the connection part of tubular separation membranes. It is an expanded sectional view of the connection part of a tubular separation membrane and an end pipe.

  With reference to FIGS. 1-5, the multitubular-type separation membrane module which concerns on one embodiment of this invention, and its tubular separation membrane coupling body are demonstrated.

  The multi-tubular separation membrane module 1 includes a cylindrical housing 2 having a cylindrical axis direction as a vertical direction, a connection body of a plurality of tubular separation membranes 3 arranged in a direction parallel to the axial line of the housing 2, and a housing. 2, a support plate 5 provided at the top and a support plate 15 provided at the bottom, a top cover 6A attached to the upper end of the housing 2 and a bottom cover 6B attached to the lower end, and support plates 5 and 15. A first baffle (rectifying plate) 7 and a second baffle (rectifying plate) 8 are arranged in parallel at the upper and lower portions in the housing 2. The first baffle 7 is disposed below the support plate 5, and the second baffle 8 is disposed above the support plate 15.

  In this embodiment, two tubular separation membranes 3 are connected by a joint pipe 17 to form a tubular separation membrane coupled body. An end tube 4 is connected to the upper end of the upper tubular separation membrane 3. An end plug 20 is connected to the lower end of the lower tubular separation membrane 3.

  A fluid inlet 9 is provided on the outer peripheral surface of the upper part of the housing 2, and a fluid outlet 10 is provided on the outer peripheral surface of the lower part. The inflow port 9 is provided so as to face the chamber 11 between the support plate 5 and the first baffle 7. The outlet 10 is provided so as to face the chamber 12 between the support plate 15 and the second baffle 8. Between the baffles 7 and 8 is a main chamber 13 for performing membrane separation.

  The flow in the main chamber 13 and the flow in the tubular separation membrane 3 may be cocurrent or counterflow, and the inflow port 9 and the outflow port 10 of the fluid to be processed may be interchanged.

  The multi-tubular separation membrane module 1 may be used with the top cover 6A side up as shown in FIG. 1 or may be used with the bottom cover 6B side up.

  The baffles 7 and 8 are provided with circular insertion holes 7a and 8a through which the tubular separation membrane 3 is inserted, and the connection body of the tubular separation membrane 3 is inserted through the insertion holes 7a and 8a. The diameters of the insertion holes 7 a and 8 a are larger than the diameter (outer diameter) of the tubular separation membrane 3, and there is a gap over the entire circumference between the inner peripheral surface of the insertion holes 7 a and 8 a and the outer peripheral surface of the tubular separation membrane 3. ing.

  The support plate 5 is provided with an opening 5 a for supporting the end tube 4 connected to the tubular separation membrane 3. The end tube 4 is inserted into the opening 5a, and the outer peripheral surface of the end tube 4 and the inner peripheral surface of each opening 5a are hermetically sealed by welding or the like. The end pipe 4 may be attached to the support plate 5 by screwing the end pipe 4 by cutting the outer periphery of the end pipe 4 and the opening 5a of the support plate 5.

  The upper end side of each end pipe 4 is open toward the outflow chamber 16 between the top cover 6 </ b> A and the support plate 5. The top cover 6A is provided with an outlet 6a for the separated permeated fluid.

  In this embodiment, outward flanges 2a, 2b, 6b, 6c are provided at the upper and lower ends of the housing 2 and the outer peripheral edges of the top cover 6A and the bottom cover 6B, and these are fixed by bolts (not shown). Has been. The peripheral edge of the support plate 5 is sandwiched between the flanges 2a and 6b via a gasket (not shown).

  A plurality of rods 14 are erected from the bottom support plate 15, and the baffles 7 and 8 are supported by the rods 14. The upper end of the rod 14 is fixed to the support plate 5 with a nut or the like. The baffles 7 and 8 are supported at a predetermined height with respect to the rod 14 by a locking member (not shown) such as a pin.

  Seal members such as an O-ring, a V-packing, and a C-ring are interposed between the outer peripheral surfaces of the baffles 7 and 8 and the inner peripheral surface of the housing 2.

  The tubular separation membrane 3 has a tubular porous support and a zeolite membrane as a ceramic separation membrane formed on the outer peripheral surface of the porous support. In the present invention, a plurality (two in this embodiment, as described above) of tubular separation membranes 3 are connected via a joint pipe 17 to form a tubular separation membrane connector.

  As shown in FIG. 4, the joint pipe 17 has a through hole 17a penetrating in the pipe axis direction. On the outer peripheral surface in the middle of the joint pipe 17 in the longitudinal direction, a ridge 17b is provided around. Both end sides of the ridge 17b are standing surfaces 17c perpendicular to the outer peripheral surface of the tubular separation membrane 7. A plurality of grooves 17d are provided around the outer peripheral surface of the joint pipe 17 other than the protrusions 17b. A first seal ring 18 is attached to the groove 17d, and the first seal ring 18 is in airtight contact with the inner peripheral surface of the tubular separation membrane 3. A second seal ring 19 is interposed between the rising surface 17c of the ridge 17b and the end surface of the tubular separation membrane 3, and the seal ring 19 is tubular in the vicinity of the rising surface 17c, the end surface of the tubular separation membrane 3, and the ridge 17b. Each of them is in airtight contact with the outer peripheral surface of the separation membrane 3.

  A baffle 7 may be provided at the joint pipe 17 as in FIG.

  An end plug 20 is connected to the lower end of the lower tubular separation membrane 3. The end plug 20 is cylindrical and seals the lower end of the tubular separation membrane 3. The end tube 4 and the end plug 20 are connected to the tubular separation membrane 3 by a heat shrink film 21 (FIG. 5).

  Examples of the material of the end tube 4 and the end plug 20 include, but are not limited to, metals and ceramics that do not allow fluid to permeate.

  Examples of the material of the tubular porous support include an inorganic porous support of a ceramic sintered body containing silica, α-alumina, γ-alumina, mullite, zirconia, titania, yttria, silicon nitride, silicon carbide, and the like. It is done. Among these, an inorganic porous support containing at least one of alumina, silica, and mullite is preferable. The average pore diameter of the surface of the porous support is not particularly limited, but those having a controlled pore diameter are preferred, usually 0.02 μm or more, preferably 0.05 μm or more, more preferably 0.1 μm. The above is usually in the range of 20 μm or less, preferably 10 μm or less, more preferably 5 μm or less.

Zeolite is crystallized on the surface of the porous support to form a zeolite membrane.
The main zeolite constituting the zeolite membrane usually contains a zeolite having an oxygen 6-10 membered ring structure, and preferably contains a zeolite having an oxygen 6-8 membered ring structure.

  Here, the value of n of the zeolite having an oxygen n-membered ring indicates the one having the largest number of oxygen among the pores composed of oxygen and T element forming the zeolite skeleton. For example, when there are 12-membered and 8-membered pores of oxygen, such as MOR type zeolite, it is regarded as a 12-membered ring zeolite.

  An example of a zeolite having an oxygen 6-10 membered ring structure is AEI, AEL, AFG, ANA, BRE, CAS, CDO, CHA, DAC, DDR, DOH, EAB, EPI, ESV, EUO, FAR, FRA, FER, GIS, GIU, GOO, HEU, IMF, ITE, ITH, KFI, LEV, LIO, LOS, LTN, MAR, MEP, MER, MEL, MFI, MFS, MON, MSO, MTF, MTN, MTT, MWW, NAT, NES, NON, PAU, PHI, RHO, RRO, RTE, RTH, RUT, SGT, SOD, STF, STI, STT, TER, TOL, TON, TSC, TUN, UFI, VNI, VSV, WEI, YUG, etc. There is.

  The zeolite membrane may be a single membrane of the zeolite, or the zeolite powder is dispersed in a binder such as a polymer to form a membrane, and the zeolite is fixed in a film form on various supports. A zeolite membrane composite may be used. The zeolite membrane may partially contain an amorphous component or the like.

  The thickness of the zeolite membrane is not particularly limited, but is usually 0.1 μm or more, preferably 0.6 μm or more, more preferably 1.0 μm or more. Moreover, it is 100 micrometers or less normally, Preferably it is 60 micrometers or less, More preferably, it is the range of 20 micrometers or less.

  However, the present invention may use a tubular separation membrane having a separation membrane other than the zeolite membrane.

  In the multi-tube separation membrane module 1 configured as described above, the fluid to be treated is introduced into the chamber 11 of the housing 2 from the inlet 9, and the inner peripheral surface of the insertion hole 7 a of the baffle 7 and the outer peripheral surface of the end tube 4. It flows into the main chamber 13 through the gap between and the main chamber 13, and then flows out into the chamber 12 through the gap between the insertion hole 8 a of the baffle 8 and the end plug 20. While flowing through the main chamber 13, some components of the fluid to be treated permeate the tubular separation membrane 3 and are taken out from the tubular separation membrane 3 through the outflow chamber 16 and the outlet 6a. The fluid that has not permeated flows out of the multi-tubular separation membrane module 1 from the outlet 10.

  In this embodiment, a large number of connected bodies of tubular separation membranes 3 are arranged in parallel and the membrane area is large, so that membrane separation is performed efficiently. In addition, since the joint pipe 17 is used for the connection part of the tubular separation membranes 3 and 3, and the sealing between the tubular separation membrane 3 and the joint pipe 17 is performed by the seal rings 18 and 19, the sealing characteristics are good. . In particular, since the seal ring 19 is interposed between the end face of the tubular separation membrane 3 and the standing surface 17c, the flow of fluid that attempts to permeate the inside of the porous support from the end face of the tubular separation membrane 3 is prevented. be able to.

  In this embodiment, the end pipe 4 and the end plug 20 connected to the upper and lower ends of the tubular separation membrane 3 are inserted into the insertion holes 7a and 8a of the baffles 7 and 8, respectively. Therefore, even if the tubular separation membrane 3 vibrates or swings so that the end tube 4 and the end plug 20 come into contact with the inner peripheral surfaces of the insertion holes 7a and 8a, the zeolite membrane is not damaged and is stably operated over a long period of time. It can be performed.

  The outer diameter C of the tubular separation membrane 3 is preferably 3 mm or more, more preferably 6 mm or more, further preferably 10 mm or more, preferably 20 mm or less, more preferably 18 mm or less, and further preferably 16 mm or less. If the outer diameter C is too small, the strength of the tubular separation membrane may be insufficient and may be easily broken, and if it is too large, the membrane area per module is reduced.

  The length of the portion of the tubular separation membrane 3 covered with the zeolite membrane is preferably 20 cm or more, and preferably 150 cm or less. If the length is shorter than this, the ratio of the portion covered with the heat shrink film 21 is increased, so that the ratio of the exposed portion that can be used for the separation of the membrane is reduced, and if it is longer than this, the handling may be difficult. .

  The seal rings 18 and 19 are preferably made of fluorine rubber or fluorine resin such as PTFE.

  The material of the baffles 7 and 8 and the joint tube 17 is usually a metal material such as stainless steel, but is not particularly limited as long as it has heat resistance and supply under separation conditions and resistance to a permeation component. It can be changed to other materials.

  In the multitubular separation membrane module of the present invention, it is preferable that 2 to 850 tubular separation membrane assemblies are usually arranged, and the shortest distance between the tubular separation membrane assemblies is 2 mm to 10 mm. The size of the housing and the number of connected tubular separation membranes are appropriately changed depending on the amount of fluid to be processed.

  In the multi-tubular separation membrane module of the present invention, the fluid to be separated or concentrated is not particularly limited as long as it is a gas or liquid mixture composed of a plurality of components that can be separated or concentrated by the separation membrane. Any mixture may be used, but it is preferably used for a gas mixture.

  In the case where the mixture to be separated or concentrated is, for example, a mixture of an organic compound and water (hereinafter sometimes referred to as “hydrated organic compound”), the water permeability to the zeolite membrane is high. Therefore, a separation or concentration method called a pervaporation method (pervaporation method) or a vapor permeation method (vapor permeation method) in which water is separated from the mixture and the organic compound is concentrated in the original mixture can be used. The pervaporation method is a separation or concentration method in which a liquid mixture is directly introduced into a separation membrane, so that a process including separation or concentration can be simplified.

  In the present invention, when the mixture to be separated or concentrated is a gas mixture composed of a plurality of components, examples of the gas mixture include carbon dioxide, oxygen, nitrogen, methane, ethane, ethylene, propane, and propylene. And those containing at least one component selected from normal butane, isobutane, 1-butene, 2-butene, isobutene, sulfur hexafluoride, helium, carbon monoxide, nitrogen monoxide, water and the like. Among the mixture of these gas components, the gas component having a high permeance passes through the separation membrane and is separated, and the gas component having a low permeance is concentrated on the supply gas side.

  The multi-tubular separation membrane module of the present invention can be used by being connected depending on the amount of fluid or the desired degree of separation and concentration. If the amount of fluid is large or the target separation / concentration is high and processing cannot be performed sufficiently with one module, connect the piping so that the fluid from the outlet enters the inlet of another module. It is preferable. Moreover, it can be further linked according to the degree of separation and the degree of concentration to obtain the desired degree of separation and concentration.

  The multi-tubular separation membrane module of the present invention may be installed in parallel to branch the fluid and supply gas. At this time, it is also possible to install modules in series with the modules in parallel. When the parallel modules are connected in series, the amount of gas to be supplied decreases in the serial direction and the linear velocity decreases. Therefore, it is preferable to reduce the number of parallel installations so as to keep the linear velocity appropriately.

  The permeated components when the modules are arranged in series may be discharged for each module, or the modules may be connected together to be discharged.

DESCRIPTION OF SYMBOLS 1 Multitubular separation membrane module 2 Housing 3 Tubular separation membrane 4 End pipe 5 Support plate 6A Top cover 6B Bottom cover 6a Outlet 7,8 Baffle 7a, 8a Insertion hole 9 Inlet 10 Outlet 11,12 Chamber 13 Main chamber 14 Rod 16 Outflow chamber 17 Joint pipe 17b Projection 17c Standing surface 17d Groove 18, 19 Seal ring 20 End plug 21 Heat shrink film

Claims (3)

A tubular housing;
A plurality of tubular separation membrane connectors disposed in the housing in the longitudinal direction of the housing;
A multi-tubular separation membrane module in which a fluid to be treated flows from one end side to the other end in the housing, and a communication fluid that has permeated the tubular separation membrane is taken out through the tubular separation membrane;
The tubular separation membrane connector is obtained by connecting tubular separation membranes via a joint tube, and a seal ring is interposed on a contact surface between the joint tube and the tubular separation membrane ,
A multi-tubular separation membrane module , wherein a baffle having an insertion hole through which the tubular separation membrane connector is inserted is provided at a portion of the joint pipe . In Claim 1, the tubular separation membrane has a tubular porous ceramic support and a ceramic separation membrane provided on the outer peripheral surface of the porous support,
The joint pipe has one end inserted into one tubular separation membrane and the other end inserted into the other tubular separation membrane.
A first seal ring is interposed between the outer peripheral surface of the joint pipe and the inner peripheral surface of the tubular separation membrane;
The joint pipe is provided with ridges on the outer peripheral surface in the middle of the longitudinal direction, and both end sides in the longitudinal direction of the ridge are stepped surfaces perpendicular to the outer peripheral surface of the joint pipe,
A multi-tubular separation membrane module, wherein a second seal ring is interposed between an end face of the tubular separation membrane and the stepped surface.   In Claim 1 or 2, the above-mentioned housing makes the cylinder axial direction the up-and-down direction,
  A support plate that supports the upper end side of the tubular separation membrane connector is provided at the top of the housing,
  The baffle provided at the joint pipe is a third baffle;
  A first baffle having an insertion hole through which an upper part of the tubular separation membrane connector is inserted is disposed below the support plate;
  A second baffle having an insertion hole through which a lower part of the tubular separation membrane connector is inserted;
  An inflow port is provided so as to introduce a fluid to be processed into one of the chamber between the support plate and the first baffle and the chamber below the second baffle. A multi-tubular separation membrane module, characterized in that an outlet is provided so as to flow out.

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