Separation membrane element and separation device

Abstract

To provide a plate and frame type separation membrane element which prevents a sealing part on a supply side from being peeled when gas is supplied thereto.SOLUTION: A plate and frame type separation membrane element has a sealing part between a supply side flow channel member and a permeation side flow channel member, wherein a compression deformation amount measured by JIS K 7181 of the permeation side flow channel member is 0.40 mm or less, and adhesive force measured by JIS K 6854 of the sealing part is 1.0 N or more.SELECTED DRAWING: Figure 3

Description

[Technical field]

[0001] The present invention relates to a separation membrane element and a separation device. [Background technology]

[0002] Plate-and-frame type separation membrane elements, which are made by stacking flat membranes, are known as separation membranes that separate specific fluid components from liquid or gaseous raw fluids (e.g., Patent Documents 1 to 3). In recent years, the performance of separation membranes has improved, making it possible to realize thinner separation membranes. Such thin separation membranes can be used to remove carbon dioxide and the like contained in gases such as exhaust gas. The plate-and-frame type separation membrane element can use thin separation membranes that are difficult to use with spiral type separation membrane elements. [Prior art documents] [Patent documents]

[0003] [Patent Document 1] JP 2017-000965 A [Patent Document 2] JP 2017-000964 A [Patent Document 3] US Application Publication No. 2019 / 0065091 Summary of the Invention [Problem to be solved by the invention]

[0004] However, when gas is supplied to a plate-and-frame type separation membrane element such as those described in Patent Documents 1 to 3 mentioned above, the membrane is pushed into the permeate side, which may cause the seal on the supply side to peel off.

[0005] The present invention has been made in consideration of the above-mentioned problems, and aims to provide a plate-and-frame type separation membrane element in which the sealing portion on the supply side is unlikely to peel off (and more preferably does not peel off) even when gas is supplied. [Means for solving the problem]

[0006] As a result of investigations aimed at solving the above-mentioned problems, the inventors found that the above-mentioned problems can be solved by a separation membrane element in which the amount of compressive deformation of the permeate side flow path member is equal to or less than a certain level and the peel strength of the feed side plugging portion is equal to or more than a certain level, and thus completed the present invention.

[0007] The present invention includes the following configurations. <1> A plate-and-frame type separation membrane element comprising a container and a separation membrane having a region arranged in the container in the form of a flat membrane, wherein the separation membrane has a separation functional layer that selectively separates a specific fluid component contained in a feed fluid, the container accommodates a laminate having at least two permeate-side flow path members through which a permeated fluid that has permeated the separation membrane flows, and a feed-side flow path member through which the separation membrane and the feed fluid flow, which is disposed between the two permeate-side flow path members, the separation membrane element having a feed-side plugging portion between the feed-side flow path member and the separation membrane, the permeate-side flow path member having a compressive deformation amount of 0.40 mm or less as measured in accordance with JIS K 7181, and the plugging portion having a peel strength of 1.0 N or more as measured in accordance with JIS K 6854. <2> the number of meshes of the permeate-side flow path member is 18 meshes or more, and when the permeate-side flow path member has a multi-layer structure having two or more layers, the number of meshes of each layer is the same; <1> The plate-and-frame type separation membrane element according to claim 1. <3> The mesh number of the permeation side flow path member is 50 mesh or more. <1> The plate-and-frame type separation membrane element according to claim 1. <4> The thickness of the separation membrane is 10 to 600 μm. <1> ~ <3> 13. The plate-and-frame type separation membrane element according to claim 12. <5> The raw material fluid is a gas. <1> ~ <4> 13. The plate-and-frame type separation membrane element according to claim 12. <6> The specific fluid component is an acid gas. <1> ~ <5> 13. The plate-and-frame type separation membrane element according to claim 12. <7> <1> ~ <6> a first supply section and a first discharge section communicating with the supply side flow path member, and a second discharge section communicating with the permeation side flow path member. Effect of the Invention

[0008] According to one aspect of the present invention, it is possible to provide a plate-and-frame type separation membrane element in which the seal on the supply side is unlikely to peel off (more preferably, does not peel off) even when a gas is supplied. [Brief description of the drawings]

[0009] [Figure 1] 1 is a perspective view that typically illustrates a separation membrane element according to one embodiment of the present invention. [Diagram 2] FIG. 2 is an exploded perspective view showing a stack of a separation membrane element according to one embodiment of the present invention. [Diagram 3] 1 is a cross-sectional view of a laminate included in a separation membrane element according to one embodiment of the present invention. [Figure 4] FIG. 2 is a perspective view illustrating a manufacturing process of a separation membrane element according to one embodiment of the present invention. [Diagram 5] FIG. 5 is a perspective view illustrating a continuation of the manufacturing process shown in FIG. [Figure 6] FIG. 6 is a perspective view illustrating a continuation of the manufacturing process shown in FIG. 5. [Figure 7] FIG. 2 is a schematic diagram illustrating a test device for an airtight test performed in the examples. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS

[0010] [1. Separation membrane element] A separation membrane element according to one embodiment of the present invention (hereinafter also referred to as the present separation membrane element) is a plate-and-frame type separation membrane element including a container and a separation membrane having a region arranged in the container in the form of a flat membrane, wherein the separation membrane has a separation functional layer that selectively separates a specific fluid component contained in a raw fluid, and the container accommodates a laminate having at least two permeate-side flow path members through which a permeated fluid that has permeated the separation membrane flows, and a supply-side flow path member through which the raw fluid flows, which is disposed between the permeate-side flow path members, and the separation membrane element has a supply-side plug between the supply-side flow path member and the separation membrane, and the amount of compressive deformation of the permeate-side flow path member measured according to JIS K 7181 is 0.40 mm or less, and the peel strength of the plug measured according to JIS K 6854 is 1.0 N or more.

[0011] Hereinafter, an embodiment of the present invention will be described with reference to the drawings, but the present invention is not limited to the following embodiment.

[0012] Fig. 1 is a perspective view showing a schematic diagram of a separation membrane element according to one embodiment of the present invention. Fig. 2 is a perspective view showing an exploded view of a laminate included in a separation membrane element according to one embodiment of the present invention. In Fig. 1, L represents the length direction of a container, W represents the width direction of the container, and H represents the height direction of the container.

[0013] The separation membrane element 1 includes a container 40 and a separation membrane 21 (FIG. 2) having a region arranged in a flat membrane shape within the container 40. A separation membrane having a region arranged in a flat membrane shape within the container 40 means that the separation membrane 21 is contained within the container 40 so as to include a region arranged in a flat state without being wound into a roll or cylindrical shape. The separation membrane 21 contained within the container 40 may have a folded portion so long as it has a region arranged in a flat membrane shape within the container 40, and as described below, may be contained within the container 40 in a folded state so as to form a flat membrane region. The separation membrane element 1 is a plate-and-frame type separation membrane element.

[0014] The separation membrane 21 has a separation functional layer that selectively separates a specific fluid component contained in the raw fluid. The separation membrane 21 may be composed of only a separation functional layer, but may also have a laminated structure of a separation functional layer and a porous membrane. The porous membrane can be provided on one or both sides of the separation functional layer, and can support or protect the separation functional layer.

[0015] The container 40 contains a laminate 10 having two permeate-side flow path members 22, and a separation membrane 21 and a supply-side flow path member 23 disposed between the two permeate-side flow path members 22. In Fig. 1, the height direction H of the container coincides with the stacking direction of the laminate 10. The separation membrane 21 included in the laminate 10 is stacked so as to have a region in which it is arranged in a flat membrane shape within the container 40. The permeate-side flow path member 22 and the supply-side flow path member 23 included in the laminate 10 are also usually stacked so as to have a region in which it is arranged in a flat membrane shape within the container 40.

[0016] The laminate 10 may have at least a portion in which a permeate-side flow path member 22, a separation membrane 21, a supply-side flow path member 23, and a permeate-side flow path member 22 are laminated in this order. For example, as shown in FIG. 2, the laminate 10 may have a membrane laminate section 20 in which a separation membrane 21, a supply-side flow path member 23, and a separation membrane 21 are laminated in this order. The laminate 10 preferably has a structure in which the membrane laminate section 20 is disposed between two permeate-side flow path members 22. The separation membrane 21 and the supply-side flow path member 23 may be bonded with a supply-side sealing material. In addition, the permeate-side flow path member 22 and the separation membrane 21 may be bonded with a permeate-side sealing material. As the supply-side sealing material and the permeate-side sealing material, a sealing material described later can be used.

[0017] In the laminate 10, the membrane stacking section 20 and the permeate side flow path member 22 stacked on the membrane stacking section 20 may constitute a membrane leaf. The membrane leaf is a laminate having a layer structure in which the permeate side flow path member 22, the separation membrane 21, the feed side flow path member 23, and the separation membrane 21 are stacked in this order. The laminate 10 may have only one membrane leaf, but preferably has a structure in which a plurality of membrane leaves are stacked. When the laminate 10 has a structure in which a plurality of membrane leaves are stacked, as shown in FIG. 2, each member and the separation membrane may be repeatedly stacked on the membrane stacking section 20 so that the permeate side flow path member 22, the separation membrane 21, etc. are formed. The number of membrane leaves included in the laminate 10 is not particularly limited, but may be, for example, 2 to 100, 5 to 50, or 10 to 30. The uppermost and lowermost surfaces of the laminate 10 are preferably the permeate side flow path member 22, and in this case, the uppermost permeate side flow path member 22 constitutes a membrane leaf.

[0018] 3 is a cross-sectional view of the laminate of the present separation membrane element cut in a direction parallel to the end 12. The laminate 10 has a supply-side plugging section 31 between a separation functional layer 53 included in a separation membrane 21 and a supply-side flow path member 23 (FIG. 3). The separation functional layer 53 forms a separation membrane together with a porous substrate 52. In the supply-side plugging section 31, the separation functional layer 53 and the supply-side flow path member 23 are bonded at an adhesive section 51 by a supply-side plugging material. Therefore, the peel strength of the supply-side plugging section 31 can be said to be the adhesive strength of the adhesive section 51. When a raw material fluid flows through the supply-side flow path member, pressure is generated in the direction of the separation membrane 21 (i.e., the direction of the block arrow shown in FIG. 3).

[0019] The supply-side plugs 31 also have the function of preventing mixing of the fluid flowing through the supply-side flow path member 23 and the fluid flowing through the permeate-side flow path member 22. The fluid flowing through the supply-side flow path member 23 is, for example, a raw material fluid and a non-permeated fluid that has not permeated the separation membrane 21. The fluid flowing through the permeate-side flow path member 22 is, for example, a permeated fluid that has permeated the separation membrane 21, and a sweep fluid that is supplied to the permeate-side flow path member 22 and discharged together with the permeated fluid. The sweep fluid is a fluid that is inactive with respect to the separation functional layer of the separation membrane.

[0020] The laminate may have a permeate-side plugging portion 32 provided so as to include a position corresponding to the stacking position of the permeate-side flow path member 22 in the stacking direction of the laminate 10 as required (FIG. 2). The position corresponding to the stacking position of the permeate-side flow path member 22 refers to a position occupied by the permeate-side flow path member 22, as well as a position occupied by an extended portion of the permeate-side flow path member 22 when the permeate-side flow path member 22 is extended in a direction along the plane of the laminate 10 (the direction in which the permeate-side plugging portions 32 in FIG. 2 exist). The permeate-side plugging portions 32 may be formed so as to include the permeated portions by permeating a permeate-side plugging material for forming the permeate-side plugging portions 32 shown in FIG. 2 into the permeate-side flow path member 22.

[0021] An end of the supply-side flow path member 23 may be provided with tape to prevent seepage of a permeate-side plugging material for forming a permeate-side plugging portion 32, which will be described later. The tape is preferably provided on the end of the supply-side flow path member 23 on the side facing the separation membrane 21, and may be provided on both sides of the end when the separation membrane 21 is disposed on both sides of the supply-side flow path member 23. Similarly, an end of the permeate-side flow path member 22 may be provided with tape to prevent seepage of a supply-side plugging material for forming a supply-side plugging portion 31. When the plugging material is a double-sided tape, it is not necessary to use tape to prevent seepage.

[0022] Although not shown, the permeate-side plugging parts 32 may be provided at the first end 11 in addition to the second end 12 of the laminate 10. The permeate-side plugging parts 32 are preferably provided along the entire one side of the laminate 10 constituting the first end 11 in plan view. The second plugging parts 32 provided at the first end 11 may also be provided at a position corresponding to the stacking position of the permeate-side flow path member 22 in the stacking direction of the laminate 10, and may be formed so that the plugging material permeates into the permeate-side flow path member 22 and includes this permeated portion. When the permeate-side plugging parts 32 are provided at the first end 11 as well, the permeate-side plugging parts 32 may be provided at two ends included in the second end 12 and one end of the first end 11, and may be formed in a state in which the permeate-side plugging parts 32 at the second end and the first end 11 are connected in plan view (for example, U-shaped).

[0023] The supply-side plugging portion 31 and the permeation-side plugging portion 32 are preferably bonded to each other at a position where the plugging portions intersect in a plan view (hereinafter, may be referred to as an "intersection position"). In the laminate 10 shown in Figs. 1 and 2, the intersection position can be provided at a corner portion of the laminate 10 in a plan view.

[0024] 1, the vessel 40 may have a first supply port 43 communicating with the supply-side flow path member 23 of the laminate 10 and for supplying a raw material fluid, a first discharge port 44 communicating with the supply-side flow path member 23 of the laminate 10 and for discharging a non-permeating fluid, and a second discharge port 46 communicating with the permeation-side flow path member 22 of the laminate 10 and for discharging a permeating fluid. The vessel 40 may further have a supply discharge port 45 communicating with the permeation-side flow path member 22 of the laminate 10. The supply discharge port 45 may be used as a second supply port for supplying a sweep fluid or as a third discharge port for discharging a permeating fluid.

[0025] In the separation membrane element 1, the second end 12 of the laminate 10 is disposed so as to face the side wall 49 in which the first supply port 43 and the first discharge port 44 of the container 40 are formed, and the first end 11 of the laminate 10 is disposed so as to face the side wall 49 in which the second discharge port 46 of the container 40 is formed (FIG. 1). When the supply and discharge port 45 of the container 40 is not used or the container 40 does not have the supply and discharge port 45, the permeate side plugging section 32 is formed at the first end 11 of the laminate 10. When the container 40 has the supply and discharge port 45 and this supply and discharge port 45 is used, by not forming the permeate side plugging section 32 at the first end 11 of the laminate 10, a sweep fluid can be supplied to the permeate side flow path member 22 from the supply and discharge port 45, or a permeated fluid can be discharged.

[0026] The separation membrane element 1 having the above structure can separate a specific fluid component as follows. First, the raw fluid is supplied from the first supply port 43 of the container 40 to the second end 12 side of the laminate 10, thereby supplying the raw fluid into the supply-side flow path member 23. The separation functional layer of the separation membrane 21 can selectively permeate a specific fluid component contained in the raw fluid flowing through the supply-side flow path member 23. As a result, the permeated fluid that has permeated the separation membrane 21 has a higher content of the specific fluid component than the raw fluid. Since the separation membrane element 1 is provided with the supply-side plug 31, the raw fluid supplied to the supply-side flow path member 23 and the non-permeated fluid that has not permeated the separation membrane 21 are prevented from mixing with the permeated fluid flowing through the permeate-side flow path member 22. On the other hand, since the separation membrane element 1 is provided with the permeate-side plug 32, the permeated fluid that has permeated the separation membrane 21 and flows through the permeate-side flow path member 22 is prevented from mixing with the raw fluid and the non-permeated fluid flowing through the supply-side flow path member 23. The non-permeated fluid that has not permeated the separation membrane 21 flows through the feed-side flow path member 23 and is discharged from the second end 12 of the laminate 10 on the first outlet 44 side of the vessel 40 to the outside of the separation membrane element 1 through the first outlet 44. The permeated fluid that has permeated the separation membrane 21 flows through the permeate-side flow path member 22 and is discharged from the first end 11 of the laminate 10 on the second outlet 46 side of the vessel 40 to the outside of the separation membrane element 1 through the second outlet 46. The permeated fluid flowing through the permeate-side flow path member 22 may be discharged from the first end 11 of the laminate 10 on the supply and outlet 45 side of the vessel 40 to the outside of the separation membrane element 1 through the supply and outlet in addition to the second outlet 46. This allows the raw material fluid to be separated into a permeated fluid and a non-permeated fluid.

[0027] When supplying a sweep fluid to the separation membrane element 1, the sweep fluid is supplied from the supply and discharge port 45 of the vessel 40 to the first end 11 side of the laminate 10, thereby supplying the sweep fluid to the permeate-side flow path member 22. The sweep fluid flows through the permeate-side flow path member 22, and is discharged from the first end 11 side of the laminate 10 on the second discharge port 46 side of the vessel 40 to the outside of the separation membrane element 1 via the second discharge port 46.

[0028] When a raw material fluid is supplied to the separation membrane element 1, internal pressure is generated in the supply-side space (i.e., in the direction of the block arrow in FIG. 3) formed by the supply-side flow path member 23 through which the raw material fluid flows. Conventionally, plate-and-frame type separation membrane elements have been used mainly for liquid permeation, and problems caused by the internal pressure have not been recognized. For example, the above-mentioned Patent Documents 1 and 2 describe plate-and-frame type separation membrane elements, but are intended to be used mainly for liquid permeation of wastewater, seawater, etc. Furthermore, Patent Document 3 describes the permeation of gas through a plate-and-frame type separation membrane element, but does not consider at all the permeation-side flow path member and the sealing portion, and only describes a low-cost plate-and-frame type separation membrane element.

[0029] However, when gas permeation is performed under normal pressure using a plate-and-frame type separation membrane element, the seals and the separation membrane are likely to peel off due to the influence of the internal pressure. When peeling occurs between the seals and the separation membrane, the airtightness of the seals decreases, making it difficult to perform good fluid separation. The fact that peeling occurs at the supply side seals and the airtightness of the separation membrane element decreases when a plate-and-frame type separation membrane element is subjected to gas permeation is a new problem discovered by the present inventors. With the present separation membrane element having the above configuration, it is possible to permeate gas without peeling off the supply side seals, even when gas is supplied.

[0030] Furthermore, according to the above configuration, it is possible to remove CO2 and the like from harmful gases such as exhaust gases. Such an effect also contributes to the achievement of, for example, Goal 7 "Affordable and clean energy for all," Goal 12 "Ensure sustainable consumption and production patterns," and Goal 13 "Take urgent action to combat climate change" of the Sustainable Development Goals (SDGs) advocated by the United Nations.

[0031] When the supply-side plug 31 and the permeation-side plug 32 are bonded to each other at the intersection of the first end 11 and the second end 12, the adhesion of the supply-side plug 31 can be improved at the intersection, making it easier to further improve the airtightness of the supply-side plug 31.

[0032] The supply-side plugging part 31 and the permeate-side plugging part 32 can be formed using a plugging material. The supply-side plugging part 31 and the permeate-side plugging part 32 may each independently use an adhesive or a double-sided tape as the plugging material. When an adhesive is used, the plugging material may be an adhesive layer obtained by drying or curing the adhesive.

[0033] The supply-side plugging section 31 can be formed, for example, by applying a plugging material at the first end 11 so as to fill a space formed between the permeate-side flow path members 22 arranged on both sides of the membrane stacking section 20 outside the end of the membrane stacking section 20, and then drying or curing the applied plugging material. When applying the plugging material, the plugging material may be applied to the end of the membrane stacking section 20 at the first end 11, or the plugging material may be allowed to penetrate into the separation membrane 21 or the porous membrane of the separation membrane 21 located at the end of the membrane stacking section 20 and the supply-side flow path member 23, and the plugging material may be dried or cured in this state to form the supply-side plugging section 31.

[0034] The feed side plugs 31 have a peel strength of 1.0 N or more, preferably 1.1 N or more, and more preferably 1.2 N or more, as measured according to JIS K 6854. There is no particular upper limit to the peel strength, but it may be, for example, 4.0 N or less. When the peel strength is 1.0 N or more, peeling of the feed side plugs 31 does not occur even when gas permeates the separation membrane element. The peel strength of the feed side plugs is measured by the method described in the examples below.

[0035] As the sealing material, double-sided tape, adhesives, etc. can be used. The resin contained in the adhesive is not particularly limited as long as it is an adhesive with a peel strength of 1.0 N or more, and examples thereof include epoxy resins, urethane resins, silicone resins, vinyl chloride copolymer resins, vinyl chloride-vinyl acetate copolymer resins, vinyl chloride-vinylidene chloride copolymer resins, vinyl chloride-acrylonitrile copolymer resins, butadiene-acrylonitrile copolymer resins, polyamide resins, polyvinyl butyral resins, polyester resins, cellulose derivative (nitrocellulose, etc.) resins, styrene-butadiene copolymer resins, various synthetic rubber (elastomer) resins, phenol resins, urea resins, melamine resins, phenoxy resins, urea formamide resins, etc. Among these, the sealing material is preferably an adhesive of epoxy resin (resin for epoxy adhesive), and more preferably a two-liquid mixed type epoxy adhesive. In the case of double-sided tape, a structural joining tape in which an acrylic adhesive is applied to an acrylic foam can be used. When using a double-sided tape, the double-sided tape can be applied onto the separation membrane, the release paper of the double-sided tape can be peeled off, and the other separation membrane can be further applied.

[0036] The supply-side plugging section 31 and the permeate-side plugging section 32 may be formed of the same plugging material or different plugging materials. That is, for example, the plugging material of the supply-side plugging section 31 may be a double-sided tape and the plugging material of the permeate-side plugging section 32 may be an adhesive, or the plugging material of the supply-side plugging section 31 may be an adhesive and the plugging material of the permeate-side plugging section 32 may be a double-sided tape. Furthermore, both the plugging materials of the supply-side plugging section 31 and the permeate-side plugging section 32 may be double-sided tapes or adhesives.

[0037] In the laminate 10 shown in FIG. 1 and FIG. 2, the ends of the two permeation side flow path members 22 arranged on both sides of the membrane stacking portion 20 are located outside the ends of the membrane stacking portion 20 at the first end 11, but the laminate according to one embodiment of the present invention is not limited to this. In a plan view of the laminate 10, the end of the separation functional layer arranged between the two permeation side flow path members 22 at the first end 11 may be outside the end of the separation functional layer. For example, in a plan view of the laminate 10, the end of the two permeation side flow path members 22 at the first end 11 may be outside the end of the separation membrane 21 (separation functional layer and porous membrane) and may be at the same position as the end of the supply side flow path member 23 arranged between the two permeation side flow path members 22. Alternatively, in a plan view of the laminate 10, the end of the two permeation side flow path members 22 at the first end 11 may be outside the end of the supply side flow path member 23 arranged between the two permeation side flow path members 22 and may be at the same position as the end of the porous membrane included in the separation membrane 21. In a plan view of the laminate 10, when the ends at the first end 11 of the two permeation side flow path members 22 are located at the same position as the ends of the porous membrane and / or the supply side flow path member 23, the supply side plug 31 may include a part (e.g., an end) of the porous membrane and / or the supply side flow path member 23.

[0038] The separation membrane element 1 can separate a specific fluid component from a feed fluid containing at least the specific fluid component. The feed fluid, the specific fluid component, the permeating fluid, the non-permeating fluid, and the sweep fluid may each independently be a gas or a liquid. The separation membrane element 1 is preferably a gas separation membrane element, and is preferably one that selectively allows a specific gas component to permeate from the feed gas.

[0039] The specific fluid component is preferably an acid gas. Acid gases include carbon dioxide (CO2), hydrogen sulfide (H2S), sulfur oxides (SO x ), nitrogen oxides (NO x) and the like. The specific gas component is preferably carbon dioxide or hydrogen sulfide, and more preferably carbon dioxide. Examples of the raw material gas include gases containing acidic gases such as residual exhaust gases of synthesis gases synthesized in plants that manufacture hydrogen, urea, and the like, natural gas, biogas, and combustion exhaust gases discharged from power plants, waste treatment plants, cement factories, and the like.

[0040] In an airtightness test, this separation membrane element had a pressure of 40 GPU (1 GPU = 3.35 × 10 -10 mol m -2 ·s -1 ·Pa -1 ) or less. If the separation membrane element of the present invention achieves the above performance, it can be said to be fully suitable for practical use. The upper limit of GPU is not particularly limited, but may be, for example, 100 GPU or less at 200 kPG. The airtightness test is the test described in the examples below.

[0041] (Method of manufacturing separation membrane element) 4 to 6 are perspective views illustrating a manufacturing process of a separation membrane element according to one embodiment of the present invention, in which L represents the length direction of the container, W represents the width direction of the container, and H represents the height direction of the container.

[0042] The separation membrane element 1 can be manufactured by using a container 40, a separation membrane 21, a permeate-side flow path member 22, and a supply-side flow path member 23, and stacking the permeate-side flow path member 22, the separation membrane 21, and the supply-side flow path member 23 in the accommodation space of the container 40 to form a laminate 10. Hereinafter, an example of a method for manufacturing a separation membrane element 1 in which a laminate 10 having a rectangular shape in a plan view is accommodated in a prismatic container 40 will be described.

[0043] First, a container 40 is prepared. The container 40 shown in Fig. 4(a) has a storage space for storing each member constituting the laminate 10, and is shown in a state where the top surface is open. The container 40 can have a guide portion 41 for positioning the member stored in the storage space. When the storage space of the container 40 is prismatic, the guide portion 41 is preferably provided at a corner of the container 40 (Fig. 4(a)).

[0044] A first tape 25 for preventing the seepage of the sealing material is attached to both sides of the end of the permeate-side flow path member 22 that will become the first end 11 of the laminate 10. In the permeate-side flow path member 22 shown in FIG. 4, the first tape 25 is attached to the ends along two opposing sides ((b) of FIG. 4). The permeate-side flow path member 22 to which the first tape 25 is attached is placed in the container 40 so that the side to which the first tape 25 is attached is parallel to the side extending parallel to the width direction W. Thereafter, a sealing material 33a is applied along the end (the end of the permeate-side flow path member 22 to which the first tape 25 is not attached (the end extending parallel to the length direction L)) that will become the second end 12 of the laminate 10 ((b) of FIG. 4). The sealing material 33a may be applied outside the end of the permeate-side flow path member 22 in a plan view of the container 40, or may be applied so as to cover the end.

[0045] Next, a separation membrane 21 (hereinafter, sometimes referred to as "first separation membrane 21a") is laminated on the permeate-side flow path member 22 (FIG. 4(c)). At this time, the first separation membrane 21a is laminated so that the end of the permeate-side flow path member 22 is located outside the end of the first separation membrane 21a in a plan view of the laminate 10 at an end (extending parallel to the width direction W) that will be the first end 11 of the laminate 10 (FIG. 4(c)). For example, the first separation membrane 21a is laminated so as not to cover the first tape 25 of the permeate-side flow path member 22. At an end (extending parallel to the length direction L) that will be the second end 12 of the laminate 10, the end of the permeate-side flow path member 22 may be located outside the end of the first separation membrane 21a in a plan view of the laminate 10, or may be located at the same position as the end of the first separation membrane 21a.

[0046] Thereafter, a sealing material 33b is applied to an end portion that will become the first end portion 11 of the laminate 10 (FIG. 5(a)). For example, the sealing material 33b is applied so as to cover the entire end portion of the permeate-side flow path member 22 that is located outside the end portion of the first separation membrane 21a in a plan view of the laminate 10. FIG. 5(a) shows a case in which the sealing material 33b is applied onto the first tape 25 of the permeate-side flow path member 22. The sealing material 33b is applied so that both ends (both ends in the width direction W) of the applied sealing material 33b overlap both ends (both ends in the length direction L) of the sealing material 33a.

[0047] Next, a second tape 26 for preventing seepage of the plugging material is attached to both sides of the end of the supply-side flow path member 23 that will become the second end 12 of the laminate 10. The supply-side flow path member 23 to which the second tape 26 is attached is laminated on the first separation membrane 21a in the container 40 (FIG. 5(b)). The supply-side flow path member 23 is laminated on the first separation membrane 21a so that the side to which the second tape 26 is attached is parallel to the side extending parallel to the length direction L. At this time, the supply-side flow path member 23 is laminated so that the end of the permeate-side flow path member 22 is located outside the end of the supply-side flow path member 23 in a plan view of the laminate 10 at the end (the end extending parallel to the width direction W) that will become the first end 11 of the laminate 10 (FIG. 5(b)). In FIG. 5(b), the supply-side flow path member 23 is laminated so as not to overlap the plugging material 33b applied on the permeate-side flow path member 22.

[0048] Thereafter, a separation membrane 21 (hereinafter, sometimes referred to as "second separation membrane 21b") is further laminated on the supply-side flow path member 23 in the container 40. At this time, the second separation membrane 21b is laminated so that the end of the permeate-side flow path member 22 is located outside the end of the second separation membrane 21b in a plan view of the laminate 10 at an end (extending parallel to the width direction W) that will become the first end 11 of the laminate 10 (FIG. 5(c)). At an end (extending parallel to the length direction L) that will become the second end 12 of the laminate 10, the end of the permeate-side flow path member 22 may be located outside the end of the second separation membrane 21b in a plan view of the laminate 10, but may be located at the same position as the end of the second separation membrane 21b. Next, a plugging material is applied to the end that will become the second end 12 of the laminate 10. It is preferable that the plugging material is applied to a position that overlaps the previously applied plugging material 33a via the supply-side flow path member 23. In this manner, the first separation membrane 21a, the supply side flow path member 23, and the second separation membrane 21b stacked on the permeate side flow path member 22 constitute a membrane stack 20.

[0049] Next, the permeate-side flow path member 22 is further laminated on the second separation membrane 21b in the container 40. The permeate-side flow path member 22 is laminated on the second separation membrane 21b at an end (an end extending parallel to the width direction W) that becomes the first end 11 of the laminate 10 so that the end of the permeate-side flow path member 22 is located outside the end of the membrane stack 20 in a plan view of the laminate 10. The membrane stack 20 (the first separation membrane 21a, the supply-side flow path member 23, and the second separation membrane 21b) and the permeate-side flow path member 22 laminated on the membrane stack 20 constitute a membrane leaf. The process of laminating the membrane leaves is repeated in the procedure described above to form the laminate 10 in the container 40 (FIG. 6(a)).

[0050] After forming the laminate 10 in the container 40, the gap between the guide portion 41 of the container 40 and the laminate 10 is sealed with a sealing material. Next, at the second end portion 12 of the laminate 10, the sealing material is applied onto the permeate-side flow path member 22 included in the uppermost membrane leaf of the laminate 10, and a top lid that will become the upper surface portion 47 of the container 40 is placed (FIG. 6(b)), and the sealing material is applied to the gap between the top lid and the side wall portion 49 of the container 40. Thereafter, the sealing material is dried or cured to obtain the separation membrane element 1 (FIG. 6(b)).

[0051] In the manufacturing method described above, two separation membranes (first separation membrane 21a and second separation membrane 21b) are used to form the membrane stack 20, but the membrane stack 20 may be formed by folding one separation membrane in half and sandwiching the supply-side flow path member 23 between the folded separation membranes. When using a separation membrane folded in half, the fold should be located at the end that will become the first end 11 of the stack 10. In the separation membrane element 1 shown in FIG. 6(b), it is preferable to arrange it so that it communicates with the second outlet 46 side for discharging the permeated fluid of the container 40. In this case, there is no need to provide a supply-side plug at the first end 11 where the fold of the separation membrane is located.

[0052] [2. Separation device] The separation apparatus may have one or more of the separation membrane elements. The arrangement and number of separation membrane elements to be provided in the separation apparatus may be selected depending on the required processing amount, the recovery rate of a specific fluid component, the size of the place where the separation apparatus is to be installed, etc.

[0053] The separation apparatus can include a first supply section and a first discharge section communicating with the supply-side flow path member 23 of the separation membrane element 1, and a second discharge section communicating with the permeate-side flow path member 22 of the separation membrane element 1. The separation apparatus may further include a supply / discharge section communicating with the permeate-side flow path member 22 of the separation membrane element 1.

[0054] The first supply section is an inlet for supplying a raw material fluid to the supply-side flow path member, and can be connected to the first supply port 43 of the separation membrane element 1. The first discharge section is an outlet for discharging a non-permeating fluid flowing through the supply-side flow path member, and can be connected to the first discharge port 44 of the separation membrane element 1. The second discharge section is an outlet for discharging a permeating fluid flowing through the permeate-side flow path member, and can be connected to the second discharge port 46 of the separation membrane element 1. The supply and discharge section can be used as a second supply section that is an inlet for supplying a sweep fluid to the permeate-side flow path member, or as a third discharge section for discharging a permeating fluid. The supply and discharge section can be connected to the supply and discharge port 45 of the separation membrane element 1.

[0055] Hereinafter, the separation membrane element 1 and each of the members constituting the separation device will be described in more detail.

[0056] (container) The container 40 contains the laminate 10. As shown in FIG. 1, the container 40 has an upper surface portion 47, a lower surface portion 48, and a side wall portion 49 connecting the upper surface portion 47 and the lower surface portion 48, and the upper surface portion 47, the lower surface portion 48, and the side wall portion 49 can partition the storage space. The upper surface portion 47 and the lower surface portion 48 extend in a direction perpendicular to the stacking direction of the laminate 10, and the side wall portion 49 extends in the stacking direction of the laminate. The shape of the container is not particularly limited, and the upper surface portion 47 and the lower surface portion 48 may be polygonal such as a rectangle, or may be circular. The side wall portion 49 may be prismatic or cylindrical.

[0057] 5(a), the container 40 may have a guide portion 41 for positioning each member constituting the laminate 10. When the side wall portion 49 of the container 40 has a prismatic shape, the guide portion 41 is preferably provided at a corner of the side wall portion 49.

[0058] The first supply port 43, supply and discharge port 45, first discharge port 44, and second discharge port 46 of the container 40 may all be provided on the side wall portion 49 of the container 40, or on the upper surface portion 47 or lower surface portion 48.

[0059] The above-mentioned members constituting the container 40 can be made of resin, glass, metal, ceramics, etc. Examples of resins include polycarbonate, acrylic resin, fluororesin, polybutylene succinate (PBS), polyethylene terephthalate (PET), polyvinyl chloride (PVC), polystyrene (PS), acrylonitrile-butadiene-styrene copolymer (ABS), polyphenylene sulfide (PPS), polyethersulfone (PES), polysulfone (PSF), polyacrylonitrile (PAN), polyphenylene oxide (PPO), polyamide (PA), polyimide (PI), polyetherimide (PEI), polyetheretherketone (PEEK), polypropylene (PP), etc., and fiber-reinforced resins obtained by mixing fibers such as glass with these resins. Examples of metals include stainless steel such as SUS, aluminum, copper, etc. The above-mentioned members constituting the container 40 may be made of the same material or different materials.

[0060] (separation membrane) The separation membrane 21 is not particularly limited as long as it is a known membrane that can selectively permeate a specific fluid component from the raw fluid. The separation membrane 21 can be, for example, an ultrafiltration membrane, a nanofiltration membrane, a reverse osmosis membrane, a dialysis membrane, a forward osmosis membrane, a solution-diffusion membrane, a facilitated transport membrane, or the like. A solution-diffusion membrane is a membrane that selectively permeates molecules by utilizing the difference in solubility and diffusibility of fluid molecules. A facilitated transport membrane is a membrane that contains a substance that promotes the solubility and / or diffusibility of fluid molecules. The separation membrane 21 is preferably a solution-diffusion membrane.

[0061] The separation membrane 21 may have a porous membrane and a separation functional layer. The separation membrane 21 may have one or more porous membrane layers, two or more porous membrane layers, or three or more porous membrane layers. The porous membrane may be provided on one or both sides of the separation functional layer. The porous membrane provided on one or both sides of the separation functional layer may be one or more porous membrane layers. The separation membrane 21 may also have a support layer for reinforcement, if necessary.

[0062] When the separation membrane has a porous membrane on only one side, in the membrane stacking section 20 described above, it is preferable to stack the separation membrane 21 and the supply side flow path member 23 so that the separation functional layer side of the separation membrane 21 faces the supply side flow path member 23.

[0063] The thickness of the separation membrane is preferably 10 to 600 μm, more preferably 10 to 550 μm, and even more preferably 10 to 510 μm. If the thickness of the separation membrane is within the above range, the membrane thickness is thin, and specific fluid components such as carbon dioxide can be sufficiently separated from the raw material fluid. Furthermore, if the thickness of the separation membrane is within the above range, it is difficult to use it in a spiral type separation membrane element, but it can be used in a plate-and-frame type separation membrane element.

[0064] (separation functional layer) The separation functional layer can be selected according to the type of the membrane. The separation functional layer is preferably a layer formed using a composition containing a resin. Examples of the resin include polyacrylic acid, polyamide, cellulose acetate, polysulfone, polyethersulfone, vinylidene fluoride, polyacrylonitrile, polyvinyl chloride-polyacrylonitrile copolymer, epoxy resin, polyimide, polyvinyl alcohol, polysiloxane, polyether block amide copolymer, polyethylene oxide, etc. The polyacrylic acid may be a crosslinked polyacrylic acid, or may be a non-crosslinked polyacrylic acid.

[0065] The separation functional layer may be a gel layer. The gel layer contains a hydrophilic resin such as polyacrylic acid, and may further contain an amino acid, an aminosulfonic acid, and / or an aminophosphonic acid. The gel layer may contain a surfactant for adjusting the wettability with respect to the porous membrane. When the specific fluid component is a gas, the gel layer may further contain an alkali metal compound, and / or a surfactant. Alternatively, the gas may contain a hydration catalyst for improving the reaction rate between a specific gas component and an alkali metal compound.

[0066] The separation functional layer can be manufactured, for example, by applying a coating solution containing the above-mentioned resin and medium onto a porous membrane. Methods for applying the coating solution onto a porous membrane include slot die coating, spin coating, bar coating, die coating, blade coating, air knife coating, gravure coating, roll coating, spray coating, dip coating, comma roll method, kiss coating method, screen printing, inkjet printing, etc.

[0067] The thickness of the separation functional layer is preferably 1 to 1000 nm, more preferably 10 to 500 nm, and even more preferably 100 to 400 nm. If the thickness of the separation functional layer is within the above range, specific fluid components such as carbon dioxide can be sufficiently separated from the raw material fluid.

[0068] (Porous membrane) The porous membrane can be a support layer for supporting the separation functional layer or a protective layer for protecting the separation functional layer. The porous membrane can be in direct contact with the separation functional layer. The porous membrane preferably has a high porosity for fluid permeability so as not to become a diffusion resistance of the raw fluid or a specific fluid component contained in the raw fluid supplied to the separation functional layer.

[0069] The porous membrane is preferably made of a resin material or an inorganic material. Examples of the resin material constituting the porous membrane include polyolefin resins such as polyethylene (PE) and polypropylene (PP); fluorine-containing resins such as polytetrafluoroethylene (PTFE), polyvinyl fluoride (PVF), and polyvinylidene fluoride (PVDF); polyester resins such as polyethylene terephthalate (PET) and polyethylene naphthalate; polystyrene (PS), polyethersulfone (PES), polyphenylene sulfide (PPS), polysulfone (PSF), polyacrylonitrile (PAN), polyphenylene oxide (PPO), polyamide (PA), polyimide (PI), polyetherimide (PEI), polyetheretherketone (PEEK), high molecular weight polyester, heat-resistant polyamide, aramid, polycarbonate, and mixtures of two or more of these resin materials. Among these, from the viewpoint of water repellency and heat resistance, it is preferable to include at least one of polyolefin resin and fluorine-containing resin, and more preferable to include at least one of polyethylene, polypropylene, and polytetrafluoroethylene. Examples of inorganic materials constituting the porous membrane include metal, glass, ceramics, etc.

[0070] The porous membrane is not particularly limited as long as it is a porous body. The porous membrane may be a porous sheet-like body such as a porous resin film, a nonwoven fabric, a woven fabric, a foam, a mesh, or a net. These porous bodies can also be used as a supporting layer for reinforcement.

[0071] The porous membrane of the separation membrane may be, for example, one or more layers of porous resin film laminated on one side of the separation functional layer and one or more layers of nonwoven fabric laminated on the other side of the separation functional layer.

[0072] (Feed-side flow path member and permeate-side flow path member) The feed-side flow path member 23 and the permeate-side flow path member 22 preferably have a function of promoting turbulence (surface renewal of the membrane surface) of the raw material fluid and the permeated fluid that has permeated the separation membrane 21 to increase the membrane permeation rate of the permeated fluid in the raw material fluid, and a function of minimizing the pressure loss of the raw material fluid supplied and the permeated fluid that has permeated the separation membrane 21. Since the feed-side flow path member 23 and the permeate-side flow path member 22 preferably have a function as a spacer that forms a flow path for the raw material fluid and the permeated fluid, and a function of generating turbulence in the raw material fluid and the permeated fluid, a mesh-like (net-like, mesh-like, etc.) one is preferably used. The shape of the unit lattice of the mesh is preferably selected from shapes such as a square, a rectangle, a rhombus, a parallelogram, etc., depending on the purpose, since the flow path of the fluid changes depending on the shape of the mesh.

[0073] The amount of compressive deformation of the permeate-side flow path member measured according to JIS K 7181 is 0.40 mm or less, preferably 0.35 mm or less, and more preferably 0.30 mm or less. The lower limit of the amount of compressive deformation is not particularly limited, but may be, for example, 0.10 mm or more. When the amount of compressive deformation is 0.40 mm or less, peeling of the feed-side plugs 31 is unlikely to occur even when gas permeates through this separation membrane element. The amount of compressive deformation of the permeate-side flow path member is measured by the method described in the Examples below.

[0074] The materials for the supply-side flow path member 23 and the permeate-side flow path member 22 are not particularly limited, but are preferably materials having heat resistance capable of withstanding the operating temperature conditions of a separation apparatus in which the separation membrane element 1 is provided. The supply-side flow path member 23 and the permeate-side flow path member 22 may each independently have a single-layer structure or a multilayer structure. The supply-side flow path member 23 and the permeate-side flow path member 22 having a multilayer structure preferably have a structure in which one or more types of mesh-like layers are laminated, and the laminated mesh-like layers may have different mesh structures. Preferably, the permeate-side flow path member 22 has a single-layer structure.

[0075] In this specification, the phrase "the permeate side flow path member 22 has a single layer structure" means that the permeate side flow path member 22 does not have multiple layers. In other words, this means that the permeate side flow path member 22 is made of a single mesh or net, and does not mean that the permeate side flow path member 22, the separation membrane 21, and the supply side flow path member 23 are not laminated in the separation membrane element 1. In addition, the phrase "the permeate side flow path member 22 has a multi-layer structure" means that the permeate side flow path member 22 is composed of multiple meshes or nets.

[0076] In one embodiment of the present invention, the permeate side flow path member is preferably in a mesh shape. When the permeate side flow path member is in a mesh shape and has a multilayer structure having two or more layers, it is preferable that the meshes of each layer of the permeate side flow path member are the same. If the meshes of each layer are the same, deformation of the permeate side flow path member due to one layer penetrating into the other layer is unlikely to occur, and the compressive strength of the permeate side flow path member is improved. When the permeate side flow path member has a single layer structure, and when the permeate side flow path member has a multilayer structure and the meshes of each layer are the same, the mesh number of the permeate side flow path member is preferably 18 meshes or more. The upper limit of the mesh number is not particularly limited, but may be, for example, 150 meshes or less.

[0077] In another embodiment of the present invention, when the permeate side flow path member is in a mesh shape and has a multilayer structure having two or more layers, the number of meshes of each layer of the permeate side flow path member may be different. In this case, the number of meshes of the permeate side flow path member is preferably 50 meshes or more. The upper limit of the number of meshes is not particularly limited, but may be, for example, 150 meshes or less. When the number of meshes of the permeate side flow path member is 50 meshes or more, the meshes between the meshes are sufficiently small, so that deformation of the permeate side flow path member due to one layer penetrating into the other layer is unlikely to occur.

[0078] (1st tape, 2nd tape) The first tape 25 and the second tape 26 are tapes used to prevent seepage of the sealing material. The first tape 25 and the second tape 26 can be made of a material impermeable to the sealing material. Examples of such materials include polypropylene, polyimide, polytetrafluoroethylene, glass fiber, polyester, and the like. The materials forming the first tape 25 and the second tape 26 may be the same or different. The first tape and the second tape are used during the manufacture of the separation membrane element, and may be removed or may remain when the separation membrane element is used.

[0079] The present invention is not limited to the above-described embodiments, and various modifications are possible within the scope of the claims. Embodiments obtained by appropriately combining the technical means disclosed in different embodiments are also included in the technical scope of the present invention. EXAMPLES

[0080] Example 1 (Preparation of separation membrane) The separation membrane is a composite membrane, and is composed of a separation functional layer (Pebax (registered trademark) polyether block amide copolymer), a porous substrate (polyacrylonitrile), and a PET nonwoven fabric serving as a reinforcing support layer, laminated in this order.

[0081] (Preparation of separation membrane element) The permeate side flow path member used was a PET mesh (mesh number: 18 meshes) with a fiber diameter of 263 μm and a thickness of 0.53 mm, length 119 mm x width 119 mm. The container used was a polycarbonate storage container with outer dimensions of length 150 mm x width 150 mm x height 85 mm and inner dimensions of the four corner guides of length 120 mm x width 120 mm. The separation membrane used was a length 119 mm x width 119 mm. The supply flow path member used was a polypropylene diamond net (manufactured by SWM Co., Ltd.; product name No. 1716) with a width of 119 mm x length 96 mm.

[0082] (Preparation of separation membrane element) Using the method shown in FIGS. 4 to 6, a separation membrane element was produced in the following procedure. 1 First, the permeate side flow path member was placed in the container, and then an adhesive (Nagase ChemteX: Denatite 2204) was applied to both ends (longitudinal L side) of the permeate side flow path member (Figure 4(b)). 2 The separation membrane was placed with the separation functional layer surface facing up (Figure 4(c)), and sealing material A (3M double-sided tape (Y-4930), width 10 mm × length 150 mm) was attached to the supply-side sealing parts, which are the two ends (i.e., the width direction W sides) opposite to where the adhesive was applied to the permeate-side flow path member (Figure 4(a)), and the supply-side flow path member was installed (Figure 4(b)). 3 After the separation membrane was placed with the separation functional layer facing down (Fig. 4(c)), adhesive was applied to both ends of the separation membrane on the side opposite the feed side plugs (i.e., the length direction L side). Next, the permeate side flow path member was placed (Fig. 5(a)). 4. The above steps 1 to 3 for stacking the permeate side flow path member, the separation membrane, and the feed side flow path member were repeated until the number of membrane leaves reached 20. The four corners of the membrane leaves and the guide parts in the container were sealed with the adhesive. 5 Adhesive was applied to both ends (i.e., the longitudinal L side) of the surface of the permeate side flow path member at the top of the membrane leaf, and after placing the top lid of the container, the gap between the top lid and the container was coated with adhesive (Fig. 5(b)). After that, seven flanges (10.2 kg) with a diameter of 12 cm and a thickness of 15 mm were placed on the top lid and dried at room temperature for 10 hours to harden the adhesive, thereby obtaining a separation membrane element. The effective membrane area of ​​the obtained separation membrane element was 0.2 m. 2 It was.

[0083] Example 2 A separation membrane element was obtained in the same manner as in Example 1, except that two overlapping meshes were used as the permeate side flow path member.

[0084] Example 3 A separation membrane element was obtained in the same manner as in Example 1, except that the mesh of the permeate side flow path member was made of polypropylene with a fiber diameter of 250 μm, a thickness of 0.50 mm, and a mesh number of 25 meshes.

[0085] Example 4 A separation membrane element was obtained in the same manner as in Example 3, except that two overlapping meshes were used as the permeate side flow path member.

[0086] Example 5 A separation membrane element was obtained in the same manner as in Example 1, except that the mesh of the permeate side flow path member had a fiber diameter of 70 μm, a thickness of 0.14 mm, and a mesh number of 50 meshes.

[0087] Example 6 A separation membrane element was obtained in the same manner as in Example 5, except that two meshes were used as the permeate side flow path member in a layered manner.

[0088] Example 7 A separation membrane element was obtained in the same manner as in Example 1, except that the mesh of the permeate side flow path member had a fiber diameter of 150 μm, a thickness of 0.30 mm, and a mesh number of 50 meshes.

[0089] Example 8 A separation membrane element was obtained in the same manner as in Example 7, except that two overlapping meshes were used as the permeate side flow path member.

[0090] Example 9 A separation membrane element was obtained in the same manner as in Example 1, except that the mesh of the permeate side flow path member had a fiber diameter of 70 μm, a thickness of 0.14 mm, and a mesh number of 80 meshes.

[0091] Example 10 A separation membrane element was obtained in the same manner as in Example 9, except that two overlapping meshes were used as the permeate side flow path member.

[0092] Example 11 A separation membrane element was obtained in the same manner as in Example 1, except that the mesh of the permeate side flow path member had a fiber diameter of 70 μm, a thickness of 0.14 mm, and a mesh number of 100 meshes.

[0093] Example 12 A separation membrane element was obtained in the same manner as in Example 1, except that the mesh used in Example 5 (fiber diameter 70 μm, mesh count 50 mesh) was sandwiched between the mesh used in Example 11 (fiber diameter 70 μm, mesh count 100 mesh) to form a mesh (thickness 0.21 mm) as the permeate side flow path member.

[0094] Example 13 A separation membrane element was obtained in the same manner as in Example 7, except that sealing material B (double-sided tape (Y-4920) manufactured by 3M, width 10 mm×length 150 mm) was used instead of sealing material A.

[0095] Comparative Example 1 A separation membrane element was obtained in the same manner as in Example 1, except that the permeation side flow path member was a mesh (thickness 0.76 mm) obtained by sandwiching the mesh of Example 1 (fiber diameter 263 nm, mesh number 18) between the mesh of Example 3 (fiber diameter 250 nm, mesh number 25).

[0096] Comparative Example 2 A separation membrane element was obtained in the same manner as in Example 1, except that the permeation side flow path member was a mesh (thickness 0.55 mm) obtained by sandwiching the mesh of Example 3 (fiber diameter 250 nm, mesh number 25) between the mesh of Example 5 (fiber diameter 70 nm, mesh number 50).

[0097] Comparative Example 3 A separation membrane element was obtained in the same manner as in Comparative Example 2, except that the sealing material B was used instead of the sealing material A.

[0098] Comparative Example 4 A separation membrane element was obtained in the same manner as in Example 7, except that sealing material C (two-component epoxy adhesive (90FL) manufactured by Henkel) was used instead of sealing material A.

[0099] [Measurement method] (Determination of peel strength at sealing part)

[0100] The average peel force (hereinafter also referred to as peel strength) at the feed side plug of the separation membrane elements prepared in the examples and comparative examples was determined by the following procedure, which conforms to JIS K 6854-1. 1. The container lid was removed from the separation membrane element, and the laminate was taken out. 2. A test piece was obtained by cutting out from the removed laminate so as to have a size of 100 mm length x 25 mm width, including the supply side sealing portion of the membrane leaf. 3. The average peel force [N] of the feed-side seal part between the separation membrane of the test piece and the feed-side flow path member (peel section 40 mm to 100 mm) was measured by a T-peel test. The T-peel test was performed at a temperature of 25°C using a test machine (Shimadzu Corporation's "Desktop Small Test Machine EZ-graph").

[0101] (Compression test) The amount of compressive deformation of the permeate-side flow path member of the separation membrane elements prepared in the Examples and Comparative Examples was determined by the following procedure, which conforms to JIS K 7181. 1. The container lid was removed from the separation membrane element, and the laminate was taken out. 2. A test piece was obtained by cutting the permeate side flow path member of the membrane leaf from the laminate so taken out, to a length of 80 mm x 80 mm. 3. The deformation of the test piece is the compressive deformation of the permeate side flow path material when a load of 900 N is applied at a speed of 0.1 mm / min. The compression test was performed at a temperature of 25°C using a testing machine (Shimadzu Corporation's "Desktop Small Testing Machine EZ-graph").

[0102] (Airtightness test) An airtightness test of the separation membrane elements prepared in the examples and comparative examples was carried out in the following procedure. Fig. 6 is a schematic diagram for explaining a test device for an airtightness test. In Fig. 6, two ends parallel to the width direction W of the separation membrane element 1 were respectively designated as a supply section 83 communicating with the first supply port 43 (Fig. 5(b)) and a discharge section 84 communicating with the first discharge port 44 (Fig. 5(b)). Two ends parallel to the length direction L of the separation membrane element 1 were respectively designated as a supply section 85 communicating with the supply and discharge port 45 (Fig. 6(b)) and a discharge section 86 communicating with the second discharge port 46 (Fig. 5(b)). 1. Using the device shown in Fig. 6, N2 gas at room temperature (20°C) was supplied into the separation membrane element, and a pressure of 200 kPG (G indicates gauge pressure) was applied to the supply part 83 of the separation membrane element. The pressure was confirmed with a pressure gauge, and the valves of the discharge parts 84 and 86 were closed. 2. The valve of the supply section 85 was closed and the valve of the exhaust section 86 was opened, and the flow rate of the permeated gas was measured using a high-precision membrane flowmeter (VP-U series manufactured by Horiba, Ltd.) and evaluated according to the following criteria. A: The N2 permeation rate indicated by the membrane flowmeter is 40 GPU or less. B: The N2 permeation rate indicated by the membrane flowmeter is greater than 40 GPU.

[0103] Table 1 shows the test results for the separation membrane elements of the examples and comparative examples.

[0104] [Table 1]

[0105] 〔result〕 Table 1 shows that the separation membrane elements of Examples 1 to 13, in which the compressive deformation amount of the permeate-side flow path member was 0.40 mm or less and the peel strength of the feed-side plugging portion was 1.0 N or more, all had excellent airtightness and the feed-side plugging portion did not peel off. Moreover, Example 13 showed that if the compressive deformation amount satisfies 0.40 mm or less and the peel strength is sufficient, the plugging portion will not peel off even if the plugging material is changed.

[0106] On the other hand, in Comparative Examples 1 to 3 in which the compressive deformation amount was more than 0.40 mm, even if the peel strength of the supply side sealing portion was high, the airtightness was poor and the supply side sealing portion peeled off. Moreover, Comparative Example 4 showed that even if the compressive deformation amount was 0.40 mm or less, the supply side sealing portion peeled off when the peel strength was less than 1.0 N. [Industrial Applicability]

[0107] One embodiment of the present invention can be widely used in a process for separating acid gases such as CO2 from mixed gases containing at least acid gases and water vapor, such as synthesis gas synthesized in a large-scale plant for producing hydrogen or urea, combustion exhaust gas discharged from a power plant, a waste treatment plant, a cement plant, etc., or natural gas or other exhaust gas. [Explanation of symbols]

[0108] 1 Separation membrane element, 10 Laminated body, 11 First end, 12 Second end, 20 Membrane stack, 21 Separation membrane, 21a First separation membrane (separation membrane), 21b Second separation membrane (separation membrane), 22 Permeation side flow path member, 23 Supply side flow path member, 25 First tape, 26 Second tape, 31 Supply side sealing portion, 32 Permeation side sealing portion, 33a Sealing material, 33b Sealing material, 40 Container, 41 Guide section, 43 First supply port, 44 First discharge port, 45 Supply and discharge port, 46 Second discharge port, 47 Top surface section, 48 Bottom surface section, 49 Side wall section, 51 Adhesive section, 52 Separation functional layer, 53 Porous base material, 81 Pressure gauge, 82 Flow meter, 83 Supply section, 84 Discharge section, 85 Supply section, 86 Discharge section.

Claims

1. A plate-and-frame type separation membrane element comprising a container and a separation membrane having a flat membrane-like region in the container, The separation membrane has a separation functional layer that selectively separates a specific fluid component contained in a raw material fluid, the container accommodates a laminate having at least two permeate-side flow path members through which a permeated fluid that has permeated the separation membrane flows, and a feed-side flow path member disposed between the two permeate-side flow path members through which the separation membrane and the raw material fluid flow, the separation membrane element has a supply-side plug between the supply-side flow path member and the separation membrane, The amount of compressive deformation of the permeate side flow path member measured according to JIS K 7181 is 0.40 mm or less, and The peel strength of the sealing portion measured according to JIS K 6854 is 1.0 N or more; Plate and frame type separation membrane element.

2. The mesh number of the permeate side flow path member is 18 meshes or more, 2. The plate-and-frame type separation membrane element according to claim 1, wherein when the permeate-side flow path member has a multilayer structure having two or more layers, the number of meshes in each layer is the same.

3. 2. The plate-and-frame type separation membrane element according to claim 1, wherein the mesh number of the permeate side flow path member is 50 meshes or more.

4. 4. The plate-and-frame type separation membrane element according to claim 1, wherein the separation membrane has a thickness of 10 to 600 μm.

5. 4. The plate-and-frame type separation membrane element according to claim 1, wherein the raw material fluid is a gas.

6. 4. The plate-and-frame type separation membrane element according to claim 1, wherein the specific fluid component is an acid gas.

7. A separation device comprising: the plate-and-frame type separation membrane element according to any one of claims 1 to 3; a first supply section and a first discharge section communicating with the supply-side flow path member; and a second discharge section communicating with the permeation-side flow path member.

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