Membrane sealing assembly

Abstract

The present invention provides a membrane sealing assembly comprising a central region, inner and outer peripheral boundary regions and an outer peripheral boundary region, wherein the inner and outer peripheral boundary regions and the outer peripheral boundary region comprise different sealing materials.

Description

Technical Field

[0001] The present invention relates to a membrane sealing assembly and use thereof in an electrochemical device, in particular to use thereof in a proton exchange membrane fuel cell. Background Art

[0002] A fuel cell is an electrochemical cell comprising two electrodes separated by an electrolyte. A fuel (e.g., hydrogen, an alcohol (such as methanol or ethanol) or formic acid) is supplied to the anode, and an oxidant (e.g., oxygen or air) is supplied to the cathode. An electrochemical reaction occurs at the electrodes, and the chemical energy of the fuel and oxidant is converted into electrical energy and heat. An electrocatalyst is used to promote the electrochemical oxidation of the fuel at the anode and the electrochemical reduction of oxygen at the cathode.

[0003] Fuel cells are generally classified according to the nature of the electrolyte used. The electrolyte is typically a solid polymer membrane that is electrically insulating but ionically conductive. In a proton exchange membrane fuel cell, the ion-conducting membrane is proton-conducting and transports protons generated at the anode across the membrane to the cathode, where they combine with oxygen to form water.

[0004] The main component of a proton exchange membrane fuel cell is a five-layer structure conventionally referred to as a membrane electrode assembly. The middle layer is a polymer ion conductive membrane. There is a catalyst layer on either side of the ion conductive membrane, which contains an electrocatalyst designed for a specific electrolysis reaction. The catalyst layer generally also includes a proton conductive material, such as a proton conductive polymer, to facilitate the transfer of protons from the anode electrocatalyst to the ion conductive membrane and / or from the ion conductive membrane to the cathode electrocatalyst. There is a gas diffusion layer adjacent to each catalyst layer. The gas diffusion layer must allow reactants to reach the catalyst layer and must conduct the current generated by the electrochemical reaction. Therefore, the gas diffusion layer must be porous and conductive. This five-layer structure is conventionally referred to as a membrane electrode assembly.

[0005] Conventionally, the membrane electrode assembly is constructed so that the central polymer ion conductive membrane extends to the edge of the membrane electrode assembly, wherein the area of the gas diffusion layer and the catalyst layer is less than the area of the membrane, so that there is a region including only the ion conductive membrane around the periphery of the membrane electrode assembly. The region where the catalyst layer is not present is a non-electrochemically active region. A separate membrane layer formed by a non-ion conductive polymer, such as a subgasket, is typically positioned around the edge region of the membrane electrode assembly on the exposed surface of the ion conductive membrane, where there is no catalyst layer (usually overlapping the edge of the catalyst layer). These membranes provide a seal to prevent reactant and product gases from escaping, strengthen and reinforce the edge of the membrane electrode assembly, and provide a suitable surface to support subsequent components, such as subgaskets or elastic gaskets. An adhesive layer may be present on one or both surfaces of the sealing membrane layer. The layers or components in the membrane electrode assembly are typically combined by a lamination process. Alternatively, the sealing material may be deposited in a picture frame type arrangement around the central ion conductive membrane, for example as disclosed in WO 2015 / 145127. Summary of the Invention

[0006] In conventional membrane electrode assembly configurations, which involve using separate sealing membranes and ion conductive membranes or catalyst coated ion conductive membranes and combining them together, there are still durability issues. These problems may be due to, for example, mechanical stresses that may be built up in the ion conductive membrane and at the edges of the ion conductive membrane electrode assembly, at the interface where the seal overlaps or frames the ion conductive membrane. Such mechanical stresses may arise due to dimensional changes caused by changes in fuel cell operating conditions during hydration and dehydration. Specifically, these stresses cause the ion conductive membrane to weaken, which may cause the ion conductive membrane to tear in the edge area near the interface with the seal, and ultimately cause the membrane electrode assembly and fuel cell to fail. Therefore, there is a need to improve the durability and life of the membrane electrode assembly.

[0007] Thus, in a first aspect, the present invention provides a membrane sealing assembly comprising a first side and a second side, the membrane sealing assembly comprising:

[0008] (i) a central region having a first side and a second side, the first side and the second side corresponding to the first side and the second side of the membrane sealing assembly, respectively, the central region comprising an ionically conductive material;

[0009] (ii) inner and outer peripheral boundary regions, the inner and outer peripheral boundary regions having a first side and a second side, the first side and the second side corresponding to the first side and the second side of the membrane sealing assembly, respectively, the inner and outer peripheral boundary regions comprising a first sealing material, wherein the inner and outer peripheral boundary regions surround the central region;

[0010] (iii) an outer peripheral border region having a first side and a second side, the first side and the second side corresponding to the first side and the second side of the membrane sealing assembly, respectively, the outer peripheral border region comprising a second sealing material, wherein the outer peripheral border region surrounds the inner and outer peripheral border regions;

[0011] The first sealing material and the second sealing material are different.

[0012] The use of two different sealing materials in the inner and outer peripheral boundary regions and the outer peripheral boundary region can have different chemical and mechanical properties, which allows the targeted use of materials that are more chemically robust and may be more expensive and more difficult to handle. Specifically, the sealing material can be used in the inner and outer peripheral boundary regions, which avoids problems associated with mechanical stresses at the interface with the central region. At the same time, a material that is more easily handled can be used in the outer peripheral boundary region. In specific aspects, the inventors have found that it may be beneficial to use a first material for the inner and outer peripheral boundary regions, the first material having a Young's modulus that is less than the Young's modulus of the second sealing material in the outer peripheral boundary region. The benefit of this arrangement is that the inner and outer peripheral boundary regions can absorb mechanical stresses from the interface with the ion-conducting central region while maintaining the stiffness required to support, for example, a subgasket in the outer peripheral boundary region.

[0013] In a second aspect, the present invention provides a membrane sealing assembly with a sub-gasket, which comprises the membrane sealing assembly according to the first aspect of the present invention, a first sub-gasket located at a first side of the membrane sealing assembly, and a second sub-gasket located at a second side of the membrane sealing assembly, wherein the first sub-gasket contacts the first surface of the outer peripheral boundary area, and the second sub-gasket contacts the second surface of the outer peripheral boundary area.

[0014] In a third aspect, the present invention provides a catalytic membrane sealing assembly, which comprises the membrane sealing assembly according to the first aspect of the present invention and a first catalyst layer located on the first surface of the central area, wherein the catalyst layer has a first surface and a second surface, wherein the second surface of the catalyst layer is in contact with the first surface of the central area.

[0015] In a fourth aspect, the present invention provides a catalytic membrane sealing assembly with a sub-gasket, the catalytic membrane sealing assembly with a sub-gasket comprising the catalytic membrane sealing assembly according to the third aspect of the present invention, a first sub-gasket located at a first side of the catalytic membrane sealing assembly, and a second sub-gasket located at a second side of the catalytic membrane sealing assembly, wherein the first sub-gasket contacts the first surface of the outer peripheral boundary area, and the second sub-gasket contacts the second surface of the outer peripheral boundary area.

[0016] In the fifth aspect, the present invention provides a membrane-sealed electrode assembly with a sub-gasket, which includes a catalytic membrane sealing assembly with a sub-gasket according to the fourth aspect of the present invention, a first gas diffusion layer located at the first side of the catalytic membrane sealing assembly with a sub-gasket, and a second gas diffusion layer located at the second side of the catalytic membrane sealing assembly with a sub-gasket.

[0017] In the sixth aspect, the present invention provides a fuel cell, which includes the membrane sealing assembly according to the first aspect of the present invention, the membrane sealing assembly with a tape gasket according to the second aspect of the present invention, the catalytic membrane sealing assembly according to the third aspect of the present invention, the catalytic membrane sealing assembly with a tape gasket according to the fourth aspect of the present invention, or the membrane sealing electrode assembly with a tape gasket according to the fifth aspect of the present invention.

[0018] In a seventh aspect, the present invention provides a method for preparing the membrane sealing assembly according to the first aspect of the present invention, the method comprising the following steps:

[0019] (a) depositing an ion-conducting material and forming a central region;

[0020] (b) depositing a first sealing material and forming inner and outer peripheral boundary regions;

[0021] (c) Depositing a second sealing material and forming an outer peripheral border region.

[0022] In an eighth aspect, the present invention provides a method for preparing the catalytic membrane sealing assembly according to the third aspect of the present invention, the method comprising the following steps:

[0023] (d) preparing a membrane sealing assembly by the method of the seventh aspect of the present invention;

[0024] (e) depositing a catalyst assembly on the central region and forming a first catalyst layer on the central region.

[0025] In a ninth aspect, the present invention provides a method for preparing the catalytic membrane sealing assembly according to the third aspect of the present invention, the method comprising the following steps:

[0026] (f) depositing a catalyst assembly on the support material and forming a first catalyst layer;

[0027] (g) depositing an ion conductive material on the catalyst layer and forming a central region;

[0028] (i) depositing a first sealing material and forming inner and outer peripheral boundary regions;

[0029] (j) Depositing a second sealing material and forming an outer peripheral border region. BRIEF DESCRIPTION OF THE DRAWINGS

[0030] Figure 1a is a plan view of a membrane sealing assembly according to the present invention.

[0031] Figure 1b yes Figure 1a A cross-sectional view of the membrane seal assembly is shown.

[0032] Figure 2a and Figure 2b is a cross-sectional view of a membrane sealing assembly with a tape gasket according to the present invention.

[0033] Figures 3a to 3d is a cross-sectional view of a catalytic membrane sealing assembly according to the present invention.

[0034] Figure 4a and Figure 4b is a cross-sectional view of a catalytic membrane sealing assembly with a gasket according to the present invention.

[0035] Figure 5a is a cross-sectional view of a membrane-sealed electrode assembly with a gasket according to the present invention. DETAILED DESCRIPTION

[0036] The preferred and / or optional features of the present invention will now be described. Unless the context otherwise requires, any aspect of the present invention may be combined with any other aspect of the present invention. Unless the context otherwise requires, any of the preferred or optional features of any aspect may be combined with any aspect of the present invention, either individually or in combination.

[0037] The central region is an ion-conducting membrane. The ion-conducting material is suitably a proton-conducting polymer or an anion-conducting polymer, such as a hydroxy anion-conducting polymer. Preferably, the ion-conducting material is a proton-conducting polymer, suitably a perfluorinated sulfonic acid material. Examples of suitable proton-conducting polymers include perfluorinated sulfonic acid materials, such as Nafion TM (Chemours Company), (Solvay Specialty Polymers)、 (AsahiGlass Group) and Aciplex TM (Asahi Kasei Chemicals corp.), and Alternatively, the ion-conducting material may be based on a sulfonated hydrocarbon membrane, such as that available from FuMA-Tech GmbH (as E or K series products), or those available from JSR Corporation, Toyobo Corporation, etc.

[0038] The central region may include one or more hydrogen peroxide decomposition catalysts. Examples of suitable hydrogen peroxide decomposition catalysts are known to those skilled in the art and include metal oxides such as cerium oxide, manganese oxide, titanium oxide, beryllium oxide, bismuth oxide, tantalum oxide, niobium oxide, hafnium oxide, vanadium oxide, and lanthanum oxide; suitable cerium oxide, manganese oxide, or titanium oxide; preferably cerium dioxide (ceria). The central region may include a recombination catalyst, specifically a catalyst for recombination of unreacted hydrogen and oxygen, which can diffuse from the anode and cathode, respectively, into the central region to produce water. Suitable recombination catalysts include metals (such as platinum) supported on high surface area oxide support materials (such as silicon dioxide, titanium dioxide, zirconium oxide). Further examples of recombination catalysts are disclosed in EP0631337 and WO00 / 24074.

[0039] Both the first sealing material and the second sealing material should be non-ionically conductive. Thus, the inner and outer peripheral boundary regions are seals, and the outer peripheral boundary region is a seal. Preferably, the inner and outer peripheral boundary regions do not include the second sealing material, and the outer peripheral boundary region does not include the first sealing material. The first and second sealing materials are suitably different in that they have different chemical compositions. In other words, they are different chemical species. Preferably, the first sealing material has a Young's modulus that is less than that of the second material. Young's modulus defines the relationship between stress and strain when a material is within the elastic regime, and this property can be measured using equipment such as a tensiometer or dynamic mechanical analyzer. Preferably, the Young's modulus is obtained using a Houndsfield tensiometer using the measurement method defined in ASTM E111–17. The relationship between the materials must be correct within the operating temperature range of the fuel cell, suitably between -20°C and 180°C, preferably between -20°C and 120°C. The first sealing material may also suitably have a Young's modulus that is greater than the Young's modulus of the ionically conductive material in the central region. Suitably, the Young's modulus of the first sealing material does not exceed 3GPa, typically does not exceed 2.5GPa, for example does not exceed 2GPa. Suitably, the Young's modulus of the first sealing material is at least 200MPa. The first sealing material should also be compatible with the fuel cell environment. For example, the first sealing material must be able to withstand temperatures in the range of -20°C to 180°C, and including -20°C to 180°C, suitably -20°C to 120°C, and the presence of water, hydrogen and / or oxygen. Under fuel cell operating conditions, the first sealing material suitably has a gas permeability lower than that of the ion conductive material, and preferably, under fuel cell operating conditions, it is airtight. The first sealing material should be compatible with the ion conductive material and the second sealing material. For example, the first sealing material must be able to form an airtight seal with the ion conductive material in the central region and the second sealing material in the outer peripheral boundary region. Technicians know the interactions that must be considered when producing an airtight seal. For example, an airtight seal can be formed by van der Waals interactions, as long as the applied material forms a tight fit. The edge of the center area, inner and outer peripheral boundary area and outer peripheral boundary area that form the interface between these regions can be shaped separately to optimize contact, thereby forming airtight seal.At the interface between the center area and the inner and outer peripheral boundary area and / or at the interface between the inner and outer peripheral boundary area and outer peripheral boundary area, there can be a blending region in plane (x and / or y) direction.In the blending region, if material is miscible, then two materials can exist and mix completely so that the distribution of component in whole blending region is uniform.Alternatively, if material is immiscible, there can be one or more " islands " of a kind of material in the blending region.

[0040] Suitable first sealing materials include silicone rubbers, including polysiloxanes and polydimethylsiloxanes. Suitable first sealing materials also include polyvinylidene fluoride (PVDF) homopolymers and copolymers. A preferred PVDF copolymer is poly(vinylidene fluoride-hexafluoropropylene copolymer), otherwise known as PVDF-HFP. The PVDF-HFP copolymer may have the formula (-CH2CF2-) x [-CF2CF(CF3)-] y , wherein x is suitably in the range of 0.2 to 0.8 and inclusive, preferably 0.4 to 0.6, and y is suitably in the range of 0.8 to 0.2 and inclusive, preferably 0.6 to 0.4. Advantageously, the characteristics of the inner and outer peripheral boundary regions can be adjusted by varying the ratio of x and y.

[0041] The second sealing material is suitably a polymer material that is conventionally used as a sealing material in a fuel cell membrane electrode assembly. Suitable second sealing materials include: polyetherimide (PEI), polyimide (PI), polyethersulfone (PES), fluorinated ethylene propylene (FEP), ethylene tetrafluoroethylene (ETFE), Polyethylene oxide (PEO), polyphenylene ether (PPE), polyethylene terephthalate (PET), polyethylene naphthalate (PEN), polyacrylonitrile (PAN), polyphenylene sulfide (PPS), polyolefins and silicones. UV-curable acrylic resins and UV-curable cationic materials can also be used.

[0042] The central region is suitably a planar region in the Cartesian x, y direction, also referred to as the in-plane direction, which extends through the thickness of the membrane sealing assembly in the Cartesian z direction, also referred to as the through-plane direction between the first and second faces. The inner and outer peripheral boundary regions are suitably planar regions in the Cartesian x, y direction, which extend around the periphery of the central region and extend through the thickness of the membrane sealing assembly in the Cartesian z direction between the first and second faces. The outer peripheral boundary region is suitably a planar region in the Cartesian x, y direction, which extends around the periphery of the inner and outer peripheral boundary regions and extends through the thickness of the membrane sealing assembly in the Cartesian z direction between the first and second faces. The central region, the inner and outer peripheral boundary regions, and the outer peripheral boundary region typically each independently have a substantially uniform thickness, which suitably means that the thickness of each region independently varies by no more than 0.5 μm in the x, y plane, typically 0.25 μm. Preferably, the thickness of each region is independently the same at any point in the x, y plane. There is no particular limitation on the thickness of the membrane sealing assembly and will depend on the intended application. For example, a typical fuel cell membrane sealing assembly will have a central region thickness of at least 5 μm, suitably at least 10 μm. A typical fuel cell membrane sealing assembly will have a central region thickness of no more than 100 μm, suitably no more than 80 μm, typically no more than 20 μm.

[0043] Suitably, the central region has a quadrilateral geometry, such as a rectangle or a square, and the inner and outer peripheral border regions create a frame around the central region. However, it should be understood that the central region can have any geometry; the inner edges of the inner and outer peripheral border regions will have the same geometry as the central region. The outer edges of the inner and outer peripheral border regions do not necessarily have to have a geometry corresponding to the shape of the inner edges; for example, the inner edge can be circular and the outer edge can be square. It should also be understood that the inner edge of the outer peripheral border region can have the same geometry as the outer edges of the inner and outer peripheral border regions. The outer edge of the outer peripheral border region does not necessarily have to have a geometry corresponding to the shape of the inner edge; for example, the inner edge can be square and the outer peripheral edge can be a more complex geometry.

[0044] Figure 1a shows a plan view of the membrane sealing assembly of the present invention, and Figure 1b The same membrane sealing assembly is shown in cross-section. The membrane sealing assembly 1 has a first side 3 and a second side 5. The central region 6 has a first face 7 and a second face 9, which correspond to the first side 3 and the second side 5 of the membrane sealing assembly, respectively. Inner and outer peripheral boundary regions 11 surround the central region 6 and have a first face 13 and a second face 15, which correspond to the first side 3 and the second side 5 of the membrane sealing assembly, respectively. An outer peripheral boundary region 17 surrounds the inner and outer peripheral boundary regions and has a first face 19 and a second face 21, which correspond to the first side 4 and the second side 5 of the membrane sealing assembly, respectively.

[0045] exist Figure 1a and Figure 1b In the shown film sealing assembly, the central area, the inner and outer peripheral boundary areas and the outer peripheral boundary area have uniform thickness independently of each other. In addition, the first and second faces 7, 13 and 19 of the central area, the inner and outer peripheral boundary areas and the outer peripheral boundary area are flush respectively. Suitably, the first and second faces of each region in these regions are respectively in the same xy plane. Alternatively, the first and second faces of the central area may not be flush with the first and second faces of the inner and outer peripheral boundary areas respectively. In the described case, the thickness of the central area is less than the thickness of the inner and outer peripheral boundary areas. In addition, the first and second faces of the inner and outer peripheral boundary areas may not be flush with the first and second faces of the outer peripheral boundary areas respectively. In the described case, the thickness of the inner and outer peripheral boundary areas is less than the thickness of the outer peripheral boundary areas.

[0046] Figure 1a and Figure 1b The following alternative configurations to the configuration shown are typical, wherein the central region, the inner and outer peripheral border regions, and the outer peripheral border region each independently have a uniform thickness:

[0047] The first and second surfaces of the central region are not flush with the first and second surfaces of the inner and outer peripheral boundary regions, respectively, and the first and second surfaces of the inner and outer peripheral boundary regions are flush with the first and second surfaces of the outer peripheral boundary region, respectively, and the thickness of the central region is less than the thickness of the inner and outer peripheral boundary regions. The first and second surfaces of the inner and outer peripheral regions and the outer peripheral region are respectively in the same x,y plane, which is different from the x,y plane of the first and second surfaces of the central region.

[0048] The first and second surfaces of the central region are flush with the first and second surfaces of the inner and outer peripheral boundary regions, respectively, and the first and second surfaces of the inner and outer peripheral boundary regions are not flush with the first and second surfaces of the outer peripheral boundary region, respectively, and the thickness of the central region and the inner and outer peripheral boundary regions is the same and less than the thickness of the outer peripheral boundary region. The first and second surfaces of the central region and the inner and outer peripheral boundary regions are respectively in the same x,y plane, which is different from the x,y plane of the first and second surfaces of the outer peripheral boundary region, respectively;

[0049] The first and second surfaces of the central region are not flush with the first and second surfaces of the inner and outer peripheral boundary regions, respectively, and the first and second surfaces of the inner and outer peripheral boundary regions are not flush with the first and second surfaces of the outer peripheral boundary region, respectively. The thickness of the central region is less than the thickness of the inner and outer peripheral boundary regions, and the thickness of the inner and outer peripheral boundary regions is less than the thickness of the outer peripheral boundary region. The first and second surfaces of the central region, the inner and outer peripheral boundary regions, and the outer peripheral boundary region are all in different x,y planes.

[0050] The total plane area of the membrane sealing assembly will depend on the end use of the membrane sealing assembly, and the selection of suitable total plane area will be within the capabilities of the technician. In addition, the size of the central area and the inner and outer peripheral boundary areas, the outer peripheral boundary areas will be determined by the total plane area, and will also depend on the end use of the enhanced membrane sealing assembly, and the selection of suitable size will be within the capabilities of the technician. For example, in the case of a fuel cell, the outer peripheral boundary area has a width that can depend on the design of the fuel cell stack using the area, and can include ports or manifold holes that allow fuel cell reactant inlet and product outlet. The inner and outer peripheral boundary areas are usually narrower than the outer peripheral boundary area.

[0051] There may be a configuration in which the inner and outer peripheral boundary regions do not have uniform thickness. In the case described, there is a step suitably in the first face, the second face, or the first and second face of the inner and outer peripheral boundary regions. If there is a step in the first face and the second face, the step is preferably aligned in the Cartesian z direction of the through plane. When the inner and outer peripheral boundary regions do not have uniform thickness, the inner and outer peripheral boundary regions are divided into two regions, an inner region adjacent to the central region and an outer region adjacent to the outer peripheral boundary region, wherein the outer region preferably has a thickness greater than the inner region. Therefore, the first face, the second face, or the first and second face of the inner and outer peripheral boundary regions can be flush with the first face, the second face, or the first and second face of the central region and the first face, the second face, or the first and second face of the outer peripheral boundary region respectively, and the first face, the second face, or the first and second face of the central region and the outer peripheral boundary region are not in identical x, y planes respectively.

[0052] A second aspect of the present invention provides a membrane sealing assembly with a subgasket, which includes the membrane sealing assembly of the present invention and a subgasket applied on one or both sides of the outer peripheral boundary area or on both the inner and outer peripheral boundary areas. Figure 2a An example of a membrane sealing assembly 31 of such subgaskets is shown, wherein a first subgasket 33 is present on a first side 3 of the membrane sealing assembly and a second subgasket 36 is present on a second side 5 of the membrane sealing assembly. In this case, the first and second subgaskets are in contact with and adhere to the outer peripheral border region 17 and do not overlap with the inner and outer peripheral border regions 11. Figure 2b In the embodiment, the first subgasket 33 and the second subgasket 36 overlap the inner and outer peripheral boundary regions 11 and adhere to both the inner and outer peripheral regions 11 and the outer peripheral region 17. Figure 2a As shown in FIG. 1 and FIG. 2 , the film sealing assembly of the tape gasket of the present invention may include a film sealing assembly having any configuration within the scope of the present invention.

[0053] The subgasket is designed to provide additional strength and robustness to the edges of the membrane seal assembly. The subgasket can be made of any material compatible with the fuel cell environment. For example, the subgasket must be able to withstand temperatures in the range of -20°C to 180°C, inclusive, and suitably -20°C to 120°C, as well as the presence of water, hydrogen, and / or oxygen. Suitable materials include polyester, polyimide, polyethylene naphthalate, and polyethylene terephthalate. The thickness of the subgasket is not particularly limited, but can suitably be in the range of 10 μm to 100 μm, inclusive. The subgaskets do not need to have the same properties. For example, the subgaskets can have different thicknesses and / or be made of different materials. The subgaskets can also include features that facilitate handling or fuel cell operation. For example, the subgaskets can include holes in their respective peripheral edge regions. These holes can, for example, facilitate gas migration in the fuel cell stack. These holes can also facilitate handling of the membrane seal assembly with the subgasket. The shape of the subgasket is not particularly limited. In other words, the peripheral edges of the first and second subgaskets may define any shape, and the shape is generally determined by the arrangement of the components in a particular fuel cell stack.

[0054] Using a coating process well known to those skilled in the art, the subgasket can be applied as a coating of a solution or dispersion, or as beads of a viscous mixture applied to the border area, or can be applied as a pre-formed picture frame film to the outside or both the inner and outer peripheral border areas and the outer peripheral border area. An adhesive layer can be used to help the adhesion of the subgasket. The adhesive layer can be an integral part of the subgasket so that the subgasket and the adhesive layer are applied in a single step, or the adhesive layer can first be applied to the outer peripheral border area or both the inner and outer peripheral border areas and the outer peripheral border area of the membrane sealing assembly, and the subgasket is then applied to the adhesive layer. Use any suitable adhesive, such as a pressure-sensitive adhesive, a heat-sensitive adhesive, a UV-activated adhesive or other adhesive to adhere the subgasket. For example, the adhesive layer can include an acrylic pressure-sensitive adhesive, a rubber-based adhesive, an ethylene maleic anhydride copolymer, an olefin adhesive, a nitrile-based adhesive, an epoxy-based adhesive, and a urethane-based adhesive.

[0055] Figure 3a A cross section of a catalytic membrane seal assembly 22 is shown wherein a first catalyst layer 23 and a second catalyst layer 25 have been applied to the membrane seal assembly 22. Figure 1a and Figure 1b The central region 6 of the membrane sealing assembly is shown. These first catalyst layer 23 and second catalyst layer 25 do not overlap with the inner and outer peripheral boundary regions 11. Figure 3b An alternative configuration is shown in which the first catalyst layer 23 and the second catalyst layer 25 do overlap the inner and outer peripheral boundary regions 11 . Figure 3aThe configuration shown has the advantage that, since all layers are in contact with the electrolyte material, all applied catalyst material is active. Figure 3b A design where the central catalyst layer overlaps the inner and outer peripheral boundary regions will have lower catalyst utilization, but the step height caused by the termination of the catalyst layer is moved to the inner and outer peripheral boundary regions, and therefore any stress caused by the step height will have a reduced effect on the interface between the central region and the inner and outer peripheral boundary regions. Figure 3a and Figure 3b compared to, Figure 3c and Figure 3d The catalytic membrane sealing assembly shown has different configurations of a central region, inner and outer peripheral boundary regions, and an outer peripheral boundary region. Figure 3c , the first surface 7 and the second surface 9 of the central region 6 are not flush with the first surface 13 and the second surface 15 of the inner and outer peripheral boundary regions 11, and the thickness of the central region 6 is less than the thickness of the inner and outer peripheral boundary regions 11. In addition, the first surface 13 and the second surface 15 of the inner and outer peripheral boundary regions 11 are flush with the first surface 19 and the second surface 21 of the outer peripheral boundary region 17, and the thickness of the inner and outer peripheral boundary regions and the outer peripheral boundary region are the same. Therefore, the first surface and the second surface of the inner and outer peripheral boundary regions and the outer peripheral boundary region are respectively in the same x, y plane. Compared with the inner and outer peripheral boundary regions 11, the reduced thickness of the central region 6 allows the first catalyst layer 23 and the second catalyst layer 25 to be applied to the central region 6 so that the first surfaces 27 and 29 of the first catalyst layer and the second catalyst layer are flush with the first surface 13 and the second surface 15 of the inner and outer peripheral boundary regions 11, respectively.

[0056] exist Figure 3d , the first and second faces 7 and 9 of the central region 6 are flush with the first and second faces 13 and 15 of the inner and outer peripheral boundary regions 11. Thus, the first and second faces of the central region and the inner and outer peripheral boundary regions are respectively in the same x, y plane. However, the first and second faces 13 and 15 of the inner and outer peripheral boundary regions 11 are not flush with the first and second faces 19 and 21 of the outer peripheral boundary region 17, and the thickness of the inner and outer peripheral boundary regions 11 is less than the thickness of the outer peripheral boundary region 17. The reduced thickness of the central region 6 and the inner and outer peripheral boundary regions 11 relative to the outer peripheral boundary region 17 allows the first and second catalyst layers 23 and 25 to be applied to the central region 6 such that the first faces 27 and 29 of the first and second catalyst layers 23 and 25 are respectively flush with the first and second faces 13 and 15 of the outer peripheral boundary region 17. Figure 3c and Figure 3dThe configurations shown all have the advantage of no step height between the catalyst layer and the sealing material. This means that when the gas diffusion layer is applied, it will be supported by the membrane sealing assembly across its entire width. In other words, there will be no gap above the unsupported step where the gas diffusion layer bridges between the catalyst layer and the membrane sealing assembly. This prevents the membrane sealing assembly material from twisting into the gap. Figure 3c The configuration shown has the additional advantage that no catalyst material is present outside the active area of the assembly, ie outside the periphery of the central area. Figures 3a to 3d In the configuration shown, the catalytic membrane seal assembly of the present invention may include a membrane seal assembly having any configuration within the scope of the present invention.

[0057] The catalyst layer in the catalytic membrane sealing assembly of the present invention includes one or more electrocatalysts. The one or more electrocatalysts are independently finely divided non-supported metal powders, or supported catalysts in which small catalyst nanoparticles are dispersed on a conductive high surface area support, such as a granular carbon black material. The exact electrocatalyst used will depend on the reaction it is intended to catalyze, and its selection is within the capabilities of the technician. The electrocatalyst can be a cathode or anode electrocatalyst, preferably a cathode or anode electrocatalyst of a fuel cell or electrolyzer, more preferably a proton exchange membrane fuel cell or electrolyzer. The thickness of the catalyst layer is not particularly limited and will depend on the intended application. In the fuel cell anode, the catalyst layer thickness is suitably at least 1 μm, typically at least 5 μm. In the fuel cell anode, the catalyst layer thickness is suitably no more than 15 μm, typically no more than 10 μm. In the fuel cell cathode, the catalyst layer thickness is suitably at least 2 μm, typically at least 5 μm. In the fuel cell cathode, the catalyst layer thickness is suitably no more than 20 μm, typically no more than 15 μm.

[0058] The electrocatalyst is suitably selected from:

[0059] (i) platinum group metals (platinum, palladium, rhodium, ruthenium, iridium and osmium);

[0060] (ii) gold or silver;

[0061] (iii) base metals;

[0062] Or an alloy or mixture comprising one or more of these metals or their oxides. The base metal is tin or a transition metal that is not a noble metal. The noble metal is a platinum group metal (platinum, palladium, rhodium, ruthenium, iridium or osmium) or gold. Preferred base metals are copper, cobalt, nickel, zinc, iron, titanium, molybdenum, vanadium, manganese, niobium, tantalum, chromium and tin. Typically, the electrocatalyst comprises an alloy of a platinum group metal or a platinum group metal, preferably with a base metal (preferred base metal as defined above). Specifically, the electrocatalyst comprises an alloy of platinum or platinum with a base metal (preferred base metal as defined above, more preferably nickel or cobalt, most preferably nickel). The atomic ratio of platinum to the alloy metal is typically in the range of 3:1 to 1:3 and includes 3:1 to 1:3. If the electrocatalyst is a supported catalyst, the loading of the metal particles on the support material is in the range of 10 wt % to 90 wt %, suitably 15 wt % to 75 wt % of the weight of the resulting electrocatalyst.

[0063] The catalyst layer preferably comprises an ionically conductive polymer, such as a proton conducting ionomer, to improve the ionic conductivity of the layer. Thus, the ionically conductive material may comprise an ionomer, such as a perfluorosulfonic acid material (e.g. (ChemoursCompany), (Asahi Kasei)、 (Solvay Specialty Polymer), (Asahi Glass Co.) and perfluorosulfonic acid ionomer materials supplied by fluorinated polymers), or ionomers based on partially fluorinated or non-fluorinated hydrocarbon sulfonated or phosphinated polymers, such as those available from FuMA-Tech GmbH (as P, E or K series products), those of JSR Corporation, Toyobo Corporation, etc. Suitably, the ionomer is perfluorosulfonic acid, specifically available from Chemours Company. series (especially 1100EW), and purchased from Solvay series (especially 830EW).

[0064] The catalyst layer may include additional components. Such components include, but are not limited to, oxygen evolution catalysts; hydrogen peroxide decomposition catalysts; hydrophobic additives (e.g., polymers with or without surface treatment (such as polytetrafluoroethylene (PTFE) or inorganic solids) or hydrophilic additives to control the transport characteristics of reactants and water. The choice of additional components will depend on whether the catalyst layer is for an anode or a cathode, and determining which additional components are appropriate is within the ability of the skilled person.

[0065] The fourth aspect of the present invention provides a catalytic membrane sealing assembly with a subgasket, comprising the catalytic membrane sealing assembly of the present invention, a first subgasket located at a first side of the catalytic membrane sealing assembly, and a second subgasket located at a second side of the catalytic membrane sealing assembly. Figure 4a An example of such a catalytic membrane seal assembly 32 with subgaskets is shown, wherein a first subgasket 33 is present on the first side 3 of the catalytic membrane seal assembly and a second subgasket 36 is present on the second side 5 of the membrane seal assembly. In this case, the first and second subgaskets are in contact with and adhere to the outer peripheral border region 17 and do not overlap with the inner and outer peripheral border regions 11. Figure 4b , the first subgasket 33 and the second subgasket 36 overlap the inner and outer peripheral boundary areas 11, so that the first subgasket 33 is also in contact with the first face 13 of the inner and outer peripheral boundary areas, and the second subgasket 36 is also in contact with the second face 15 of the inner and outer peripheral boundary areas. In this case, the first subgasket 33 and the second subgasket 36 are adhered to both the inner and outer peripheral areas 11 and the outer peripheral area 17.

[0066] Figure 5a An example of a membrane-seal electrode assembly with a subgasket according to the fifth aspect of the present invention is shown. This particular membrane-seal electrode assembly with a subgasket 32 has a first gas diffusion layer 38 and a second gas diffusion layer 40 at the first and second sides of the catalytic membrane seal assembly with a subgasket. Figure 5a It can be seen that the catalyst layers 23 and 25 are combined with the above Figure 3c and Figure 3d The lack of a step height between the membrane seal assemblies discussed means that the gas diffusion layer is fully supported by the membrane seal assemblies. This particular tape-gasket membrane seal electrode assembly 36 also includes a planar reinforcement assembly 42 that extends to both the inner and outer peripheral boundary regions and the outer outer peripheral boundary region and does not span the entire thickness of the tape-gasket membrane seal electrode assembly.

[0067] The gas diffusion layer comprises a gas diffusion substrate and preferably a microporous layer. Typical gas diffusion substrates include nonwoven paper or webs comprising a carbon fiber web and a thermosetting resin binder (e.g., TGP-H series carbon fiber paper available from Toray Industries Inc., Japan, or H2315 series available from Freudenberg FCCT KG, Germany, or GL Technologies GmbH, Germany). series, or from Ballard Power Systems Inc. series), or woven carbon cloth. Prior to manufacturing the electrodes and incorporating them into the membrane sealed electrode assembly, the carbon paper, mesh or cloth may be provided with a pre-treatment to make it more wettable (hydrophilic) or more water-repellent (hydrophobic). The nature of any treatment will depend on the type of fuel cell and the operating conditions to be used. The substrate may be made more wettable by incorporating a material such as amorphous carbon black via impregnation from a liquid suspension, or the substrate may be made more hydrophobic by impregnating the pore structure of the substrate with a colloidal suspension of a polymer such as PTFE or polyfluoroethylene propylene (FEP), followed by drying and heating to above the melting point of the polymer. A typical microporous layer comprises a mixture of carbon black and a polymer such as polytetrafluoroethylene (PTFE).

[0068] In the membrane-sealed electrode assembly with a gasket of the fifth aspect of the present invention, the first gas diffusion layer and the second gas diffusion layer preferably do not overlap the outer peripheral boundary region. An adhesive may be used to facilitate adhesion to the inner and outer peripheral boundary regions (and the outer peripheral boundary region, if applicable). The adhesive may be an integral part of the gas diffusion layer, allowing the gas diffusion layer and the adhesive layer to be applied in a single step, or the adhesive layer may be applied first to the inner and outer peripheral boundary regions (and the outer peripheral boundary region, if applicable), and the gas diffusion layer subsequently applied to the adhesive layer.

[0069] The fuel cell of the sixth aspect of the present invention is preferably a proton exchange membrane fuel cell. Although the present invention is described primarily with respect to a proton exchange membrane fuel cell, it should be understood that the membrane sealing assembly can be used in other electrochemical systems, such as an electrolyzer. In a proton exchange membrane electrolyzer, a voltage is applied across the membrane sealing electrode assembly so that the water supplied to the device is separated into hydrogen and oxygen at the cathode and anode, respectively. The membrane sealing electrode assembly may require different catalyst components for a proton exchange membrane fuel cell, such as an Ir-based material and a Ru-based material at the anode, but is otherwise very similar to the construction of the proton exchange membrane of a fuel cell.

[0070] In the method for a seventh aspect of the present invention, by any technology well known to those skilled in the art, ion conductive material, the first sealing material and the second sealing material are suitably deposited as liquid or dispersion respectively.This type of technology comprises gravure coating, slot die (groove, extrusion) coating (coating is extruded onto substrate via groove under pressure thus), screen printing, rotary screen printing, inkjet printing, spraying, painting, rod coating, roll coating, gap coating technology, such as the knife or scraper on roller (coating is applied to substrate thus, then passes through the crack between knife and support roller), and metering rod coating, such as with Meyer rod.Each in ion conductive material, the first sealing material and the second sealing material can be deposited in twice or more times by.Preferably, ion conductive material and the first sealing material are deposited by inkjet printing, and can be deposited simultaneously to contribute to the alignment of central area and inner and outer peripheral boundary area.

[0071] The ion conductive material and the sealing material are dried separately after deposition of each material, or may be dried after deposition of both the ion conductive material and the first sealing material, or after deposition of all three of the ion conductive material, the first sealing material and the second sealing material. If two or more passes are used to deposit any material, there may be a drying step after each pass. Drying to substantially remove the solvent from the ion conductive or sealing material coating dispersion may be achieved by any suitable heating technique well known to those skilled in the art, such as air impingement, infrared, etc. Suitably, the drying step is carried out at a temperature in the range of 70°C to 120°C, inclusive, but may be up to or in excess of 200°C depending on the nature of the solvent.

[0072] In addition to being dried, the first sealing material, the second sealing material and the ion conductive material can be cured to provide mechanical and chemical strength to the material. Curing is a chemical reaction that achieves changes (such as cross-linking) and can be thermally activated (for example, by heat or IR) or by UV activation. In addition, in addition to being dried (and optionally cured), the ion conductive material can be annealed to change and strengthen the crystal structure of the ion conductive material. Any annealing step will use a high temperature, for example up to 200°C, compared to the drying step. The curing step and / or annealing step can be performed after each drying step or at the end of the deposition process. Depending on the materials used for the sealing material and the ion conductive material, curing and annealing can be achieved in a single process.

[0073] The ion conductive material, the first sealing material and the second sealing material may be deposited on a carrier material that does not form part of the final membrane sealing assembly but is intended to be removed in a subsequent step; this step may be performed immediately after the membrane sealing assembly is formed, or may be performed at some point downstream in the production process when the membrane sealing assembly is combined with other components, such as a subgasket. The carrier material provides support for the membrane sealing assembly during manufacture and, if not removed immediately, may provide support and strength during any subsequent storage and / or transport. The material from which the carrier material is made should provide the required support, be compatible with the ion conductive material and the sealing material, be impermeable to the ion conductive material and the sealing material, be able to withstand the process conditions of producing the membrane sealing assembly, and be able to be easily removed without damaging the membrane sealing assembly. Examples of materials suitable for use include fluoropolymers (such as polytetrafluoroethylene (PTFE), ethylene tetrafluoroethylene (ETFE), perfluoroalkoxy polymers (PFA), fluorinated ethylene propylene (FEP - a copolymer of hexafluoropropylene and tetrafluoroethylene)) and polyolefins (such as biaxially oriented polypropylene (BOPP)). Other examples include laminates, multilayer extrusions, and coated films / foils that can maintain their mechanical strength / integrity at elevated temperatures, such as temperatures up to 200°C. Examples include laminates of poly(ethylene tetrafluoroethylene) (ETFE) and polyethylene naphthalate (PEN); polymethylpentene (PMP) and PEN; polyperfluoroalkoxy (PFA) and polyethylene terephthalate (PET) and polyimide (PI). Laminates can have two or more layers, such as ETFE-PEN-ETFE, PMP-PEN-PMP, PFA-PET-PFA, PEN-PFA, FEP-PI-FEP, PFA-PI-PFA, and PTFE-PI-PTFE. These layers can be bonded using adhesives such as acrylic or polyurethane.

[0074] If there is a planar reinforcement component in the membrane sealing assembly, this can be suitably applied to the ion conductive material before forming the central area after deposition. Suitable reinforcement component materials include a planar porous material embedded in the thickness of the membrane sealing assembly, such as expanded polytetrafluoroethylene (ePTFE), such as described in USRE37307, to provide improved mechanical strength of the membrane sealing assembly, such as enhanced tear resistance and reduced hydration and dehydration dimensional changes, and therefore further increase the durability of the membrane sealing electrode assembly and the life of the fuel cell incorporating the membrane sealing assembly of the present invention. The reinforcement component material and the first sealing material are suitably different in the sense that they have different chemical compositions. In other words, they are suitably different chemical substances. For example, the planar reinforcement component is suitably made of a material different from the first sealing material. Similarly, the reinforcement component material and the second sealing material are suitably different in the sense that they have different chemical compositions. For example, the planar reinforcement component is suitably made of a material different from the second sealing material. Any planar reinforcement component present can extend over the entire thickness of the membrane sealing assembly, or can extend over only a portion of the membrane sealing assembly thickness. The planar reinforcement component can extend into the inner and outer peripheral boundary regions, and can also extend into the outer peripheral boundary region.

[0075] In the method of the eighth aspect of the invention, the catalyst layer is suitably deposited on the central region as an organic or aqueous (but preferably aqueous) ink. Alternatively, the first catalyst layer can be applied by transferring a previously prepared catalyst layer; for example, the catalyst layer is applied to a decal transfer substrate film (e.g., PTFE) and then transferred to the membrane sealing assembly of the invention by techniques involving pressure and temperature well known to those skilled in the art.

[0076] In the optional step (k) of the method of the ninth aspect of the invention, the catalyst component is suitably deposited on the central area as an organic or aqueous (but preferably aqueous) ink. Alternatively, the second layer can be applied by transferring a previously prepared catalyst layer; for example, the catalyst layer is applied to a decal transfer substrate film (e.g., PTFE), and then the catalyst layer is transferred to the membrane sealing assembly of the present invention by techniques involving pressure and temperature well known to those skilled in the art.

[0077] The invention will now be further described with reference to the following examples, which are intended to be illustrative rather than limiting of the invention.

[0078] like Figure 1a and Figure 1bThe membrane sealing assembly of the present invention is shown as follows. A liquid dispersion of perfluorosulfonic acid (PFSA) ion conductive material is applied as a thin layer to a release film of a carrier material simultaneously with a PVDF / HFP copolymer solution. These materials are distributed using an inkjet system that allows two liquids to align with each other, with the PFSA material occupying a central area and the PVDF / HFP copolymer surrounding the area and forming an inner and outer peripheral boundary area. Once dried, the two liquids form a continuous film 3 μm thick. The second layer of each material is coated on top of the first layer, and when the second layer is still wet, the ePTFE reinforcement is placed on top of the second layer, and the reinforcement is held under tension. The reinforcement is drawn down into the wet PFSA and PVDF / HFP layers so that once dried, all holes in the holes in the reinforcement are completely filled with PFSA or PVDF / HFP from the second coating. After drying, the final coating of the PFSA dispersion and PVDF / HFP solution is applied to the upper surface of the reinforcement, and dried to ensure that the central area of the reinforcement is completely encapsulated by the material in the coated area. Finally, a UV-curable polymer material, poly(4-vinylphenol-co-methyl methacrylate) (PVP-co-PMMA), was dispensed using an inkjet to form an outer peripheral border region around the PVDF / HFP inner and outer peripheral border regions and cured using UV radiation. Once cured, the outer peripheral border region had the same thickness as the central region and the inner and outer peripheral border regions.

Claims

1. A membrane sealing assembly, comprising a first side and a second side, the membrane sealing assembly comprising: (i) a central region having a first face and a second face, the first face and the second face corresponding to the first side and the second side of the membrane sealing assembly, respectively, the central region comprising an ionically conductive material; (ii) inner and outer peripheral boundary regions, the inner and outer peripheral boundary regions having a first side and a second side, the first side and the second side corresponding to the first side and the second side of the membrane sealing assembly, respectively, the inner and outer peripheral boundary regions comprising a first sealing material, wherein the inner and outer peripheral boundary regions surround the central region; (iii) an outer peripheral border region having a first side and a second side, the first side and the second side corresponding to the first side and the second side of the membrane sealing assembly, respectively, the outer peripheral border region comprising a second sealing material, wherein the outer peripheral border region surrounds the inner and outer peripheral border regions; wherein the first sealing material and the second sealing material are different; wherein the first sealing material and the second sealing material are non-ion conductive; wherein the first sealing material has a Young's modulus that is less than the Young's modulus of the second sealing material; and The first surface and the second surface of the inner and outer peripheral boundary areas are flush with the first surface and the second surface of the outer peripheral boundary area, respectively. 2 . The membrane sealing assembly of claim 1 , wherein the first sealing material has a Young's modulus that is greater than the Young's modulus of the ion-conducting material in the central region.

3. The membrane sealing assembly according to any one of claims 1 to 2, wherein the first and second faces of the central region are flush with the first and second faces of the inner and outer peripheral boundary regions, respectively.

4. The membrane sealing assembly according to any one of claims 1 to 2, wherein the first surface and the second surface of the central area are not flush with the first surface and the second surface of the inner and outer peripheral boundary areas, respectively, and the thickness of the central area is less than the thickness of the inner and outer peripheral boundary areas.

5. The membrane sealing assembly of any one of claims 1 to 2, further comprising a planar reinforcement assembly in the central region.

6. The membrane sealing assembly of claim 5, wherein the planar reinforcement assembly extends into the inner and outer peripheral boundary regions.

7. The membrane sealing assembly of claim 6, wherein the planar reinforcement assembly extends into the outer peripheral boundary region.

8. A membrane sealing assembly with a sub-gasket, comprising a membrane sealing assembly according to any one of claims 1 to 2, a first sub-gasket located at the first side of the membrane sealing assembly, and a second sub-gasket located at the second side of the membrane sealing assembly, wherein the first sub-gasket contacts the first surface of the outer peripheral boundary area, and the second sub-gasket contacts the second surface of the outer peripheral boundary area.

9. A membrane sealing assembly with sub-gaskets according to claim 8, wherein the first sub-gasket and the second sub-gasket overlap with the inner and outer peripheral boundary areas, the first sub-gasket contacts the first surface of the inner and outer peripheral boundary areas, and the second sub-gasket contacts the second surface of the inner and outer peripheral boundary areas.

10. A catalytic membrane sealing assembly, comprising a membrane sealing assembly according to any one of claims 1 to 2 and a first catalyst layer located on the first surface of the central region, wherein the catalyst layer has a first surface and a second surface, wherein the second surface of the catalyst layer is in contact with the first surface of the central region. 11 . The catalytic membrane sealing assembly according to claim 10 , wherein the first catalyst layer overlaps the inner and outer peripheral boundary regions, and the second surface of the first catalyst layer contacts the first surface of the inner and outer peripheral boundary regions.

12. The catalytic membrane sealing assembly according to claim 10 further comprises a second catalyst layer located on the second surface of the central region, wherein the second catalyst layer has a first surface and a second surface, wherein the second surface of the second catalyst layer contacts the second surface of the central region. 13 . The catalytic membrane sealing assembly according to claim 12 , wherein the second catalyst layer overlaps the inner and outer peripheral boundary regions, and the second surface of the second catalyst layer contacts the second surface of the inner and outer peripheral boundary regions. 14 . The catalytic membrane sealing assembly according to claim 10 , wherein the first surface of the first catalyst layer is flush with the first surface of the inner and outer peripheral boundary regions. 15 . The catalytic membrane sealing assembly according to claim 12 , wherein the first surface of the second catalyst layer is flush with the second surface of the inner and outer peripheral boundary regions.

16. A catalytic membrane sealing assembly with a sub-gasket, the catalytic membrane sealing assembly with a sub-gasket comprising a catalytic membrane sealing assembly according to claim 10, a first sub-gasket located at the first side of the catalytic membrane sealing assembly, and a second sub-gasket located at the second side of the catalytic membrane sealing assembly, wherein the first sub-gasket contacts the first surface of the outer peripheral boundary area, and the second sub-gasket contacts the second surface of the outer peripheral boundary area.

17. A catalytic membrane sealing assembly with sub-gaskets according to claim 16, wherein the first sub-gasket and the second sub-gasket overlap with the inner and outer peripheral boundary areas, the first sub-gasket contacts the first surface of the inner and outer peripheral boundary areas, and the second sub-gasket contacts the second surface of the inner and outer peripheral boundary areas.

18. A membrane-sealed electrode assembly with a sub-gasket, the membrane-sealed electrode assembly with a sub-gasket comprising a catalytic membrane-sealed assembly with a sub-gasket according to claim 16, a first gas diffusion layer located at the first side of the catalytic membrane-sealed assembly with a sub-gasket, and a second gas diffusion layer located at the second side of the catalytic membrane-sealed assembly with a sub-gasket.

19. The gasketed membrane-sealed electrode assembly of claim 18, wherein the first gas diffusion layer and the second gas diffusion layer do not overlap with the outer peripheral border region. 20 . The gasket-taped membrane-sealed electrode assembly of claim 18 , wherein the first gas diffusion layer and the second gas diffusion layer are bonded to the first face and the second face of the inner and outer peripheral boundary regions, respectively.

21. A fuel cell comprising the membrane sealing assembly according to any one of claims 1 to 2.

22. The fuel cell according to claim 21, wherein the fuel cell is a proton exchange membrane fuel cell.

23. A method for preparing the membrane sealing assembly according to any one of claims 1 to 2, the method comprising the following steps: (a) depositing an ion conductive material and forming the central region; (b) depositing a first sealing material and forming the inner and outer peripheral boundary areas; (c) Depositing a second sealing material and forming the outer peripheral border region.

24. A method for preparing the catalytic membrane sealing assembly according to claim 10, the method comprising the following steps: (d) preparing a membrane sealing assembly by the method according to claim 23; (e) depositing a catalyst assembly on the central region and forming the first catalyst layer on the central region.

25. A method for preparing the catalytic membrane sealing assembly according to claim 10, the method comprising the following steps: (f) depositing a catalyst assembly on the support material and forming a first catalyst layer; (g) depositing an ion conductive material on the catalyst layer and forming the central region; (i) depositing a first sealing material and forming the inner and outer peripheral boundary regions; (j) Depositing a second sealing material and forming the outer peripheral border region.

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