KR101312971B1 - Hydrocarbon based polyelectrolyte separation membrane surface-treated with fluorinated ionomer, membrane electrode assembly, and fuel cell - Google Patents

Abstract

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a hydrocarbon-based polymer electrolyte separator, a membrane electrode assembly, and a fuel cell that have been surface-modified using fluorine-based iono, and having a hydrocarbon-based membrane and a fluorine-based iono coating layer coated on both surfaces of the membrane. Provided are a separator, a membrane electrode assembly and a fuel cell produced using the same.

Description

Hydrocarbon based polyelectrolyte separation membrane surface-treated with fluorinated ionomer, membrane electrode assembly, and fuel cell}

The present invention relates to a polymer electrolyte membrane for a fuel cell and a surface modification method thereof, and more particularly, to a hydrocarbon-based polymer electrolyte membrane for a fuel cell surface-modified using a fluorine iono, and a membrane electrode assembly and a fuel cell manufactured using the same. It is about.

A fuel cell is a power generation system that directly converts chemical energy generated by electrochemical reaction between fuel (hydrogen or methanol) and oxidant (oxygen) to electrical energy.It is an eco-friendly feature with high energy efficiency and low emission of pollutants. Research and development. The fuel cell can be used by selecting a fuel cell for high temperature and low temperature according to the application field, and is generally classified according to the type of electrolyte. For high temperature, a solid oxide fuel cell (SOFC) and molten carbonate are used. Fuel cell (Molten Carbonate Fuel Cell, MCFC) and the like, Alkaline Fuel Cell (AFC) and Polymer Electrolyte Membrane Fuel Cell (PEMFC) are being developed for low temperature.

Subdivided into a double polymer electrolyte fuel cell is a hydrogen ion exchange membrane fuel cell (PEMFC) that uses hydrogen gas as a fuel, and direct methanol that supplies liquid methanol directly to the anode as a fuel. Fuel cell (Direct Methanol Fuel Cell, DMFC). BACKGROUND OF THE INVENTION Polymer electrolyte fuel cells have been in the spotlight as portable, automotive, and home power supplies for their low operating temperatures of less than 100 ° C., elimination of leakage problems due to the use of solid electrolytes, fast startup and response characteristics, and excellent durability. In particular, as a high output fuel cell having a higher current density than other types of fuel cells, it is possible to miniaturize, and thus research into a portable fuel cell continues.

The unit cell structure of the fuel cell has a structure in which an anode (anode, fuel electrode) and a cathode (cathode, oxygen electrode) are coated on both sides of an electrolyte membrane made of a polymer material, which is a membrane-electrode assembly (Membrane). Electrode Assembly (MEA). The membrane-electrode assembly (MEA) is a portion in which an electrochemical reaction between hydrogen and oxygen occurs and is composed of a cathode, an anode, and an electrolyte membrane, that is, an ion conductive electrolyte membrane (eg, a hydrogen ion conductive electrolyte membrane). In the anode, hydrogen or methanol, which is a fuel, is supplied to generate an oxidation reaction of hydrogen to generate hydrogen ions and electrons. In the cathode, water is generated by a reduction reaction of oxygen by combining hydrogen ions and oxygen that have passed through the polymer electrolyte membrane. . The membrane-electrode assembly has a form in which the electrode catalyst layers of the anode and the cathode are coated on both sides of the ion conductive electrolyte membrane, and the material forming the electrode catalyst layer is Pt (platinum), Pt-Ru (platinum-ruthenium), or the like. The catalyst substance of is supported on the carbon carrier. Membrane-electrode assembly (MEA), which can be seen as a key component of the electrochemical reaction of fuel cells, is especially used for ion-conducting electrolyte membranes and platinum catalysts, which have a high price ratio. It is considered as the most important part in improving the performance and increasing the price competitiveness.

Conventional methods for producing MEAs that are commonly used include preparing a paste by mixing a catalytic material with a hydrogen ion conductive binder, such as a fluorine-based Nafion Ionomer, and water and / or an alcohol solvent. In addition, an electrode support for supporting the catalyst layer and a carbon cloth or carbon paper serving as a gas diffusion layer and the like are coated, and then dried and thermally fused to a hydrogen ion conductive electrolyte membrane.

Redox reaction of hydrogen and oxygen by the catalyst in the catalyst layer; Transfer of electrons by tightly bonded carbon particles; Securing passages for supplying hydrogen, oxygen and moisture and for discharging excess gas after the reaction; Movement of oxidized hydrogen ions must be carried out at the same time. Furthermore, in order to improve performance, the area of the triple phase boundary where the feed fuel, the catalyst and the ion conductive polymer electrolyte membrane meet must be increased to reduce the activation polarization, and the interface between the catalyst layer and the electrolyte membrane and the catalyst layer The interface between the gas diffusion layer and the gas diffusion layer must be uniformly bonded to reduce ohmic polarization at the interface. Therefore, in order to improve the performance of the fuel cell by reducing the interface resistance between the catalyst layer and the electrolyte membrane as much as possible, not only the bonding force between the catalyst layer and the electrolyte membrane should be provided during MEA production, but also the interface bonding between the catalyst layer and the electrolyte membrane during the fuel cell operation is required. It must be maintained.

In general, in the case of using a Nafion electrolyte membrane (Nafion) as an electrolyte membrane for a fuel cell, in order to improve the interfacial adhesion between the catalyst layer and the Nafion electrolyte membrane and increase the efficiency of the catalyst layer, a liquid phase such as a Nafion Ionomer solution The electrolyte is impregnated into the catalyst layer. In the actual reaction, the migration rate of hydrogen ions to the platinum (Pt) catalyst is much faster through the ionomer than to the water. In the method of impregnating the ionomer into the catalyst layer, a method of preparing a catalyst slurry by adding a Nafion ionomer solution together and applying it on a carbon cloth or carbon paper as an electrode support to form a catalyst layer, and then coating the Nafion ionomer solution thinly thereon Use Here, the components of the coating layer and the electrolyte membrane on the catalyst layer are all the same as Nafion, so that the adhesion between the membrane and the catalyst layer is improved because of excellent miscibility. Therefore, in order to improve the adhesion between the electrolyte membrane and the catalyst layer and further improve the performance of the fuel cell by reducing the interface resistance between the membrane and the electrode, it is important to use the same or similar coating layer components as those of the electrolyte membrane. .

In general, an electrolyte membrane used in a polymer electrolyte fuel cell may be divided into a fluorine polymer electrolyte and a hydrocarbon polymer electrolyte. Nafion, a product of Du Pont, USA, is a representative example of a fluorine-based polymer electrolyte membrane, and is currently being most commercialized due to its excellent ion conductivity, chemical stability, and ion selectivity. However, the fluorinated polymer electrolyte membrane has a low price due to its high performance, but has low industrial utility due to its high price, methanol has high methanol crossover, and the efficiency of the polymer membrane is reduced at 80 ° C. or higher. Therefore, research is being actively conducted on hydrocarbon-based polymer electrolyte membranes which can compete in terms of price. In particular, polyetherketone, polyethersulfone-based polyarylene ether polymers have been studied for their application to fuel cells due to their excellent chemical stability and mechanical properties.

The polymer electrolyte fuel cell is largely composed of an anode (anode), a cathode (cathode) and a separator. Here, the separator is a material having ion conductivity but no electron conductivity. Separation membranes of polymer electrolyte fuel cells can be divided into fluorine-based and hydrocarbon-based, mainly fluorine-based membranes, and low-cost hydrocarbon-based membranes are under development. Fluorine-based membranes exhibit favorable properties for humidification and non-humidification fatigue, and thus have good mechanical durability. However, fluorine-based membranes are poor in chemical durability because they have high gas crossover. Hydrocarbon-based membranes have good chemical durability due to their cost competitiveness and low gas permeability, while their mechanical brittleness is poor due to their brittle nature.

Korean Patent Laid-Open Publication No. 2007-98325 discloses a polymer including a moiety that can be swelled in a micro-domain size by a Cl solvent without dissolving in a Cl solvent. Characteristic polymers are disclosed. In this patent, the surface was modified using a fluorinating agent rather than a fluorine-based iono.

As in the present invention, the fluoro ionic iono having good toughness is coated on both sides of a brittle hydrocarbon separator, thereby preventing mechanical cracks in the hydrocarbon separator during MEA operation, thereby improving mechanical durability.

Korean Patent Laid-Open Publication No. 2008-101180 discloses an electrolyte membrane prepared by using a combination of a non-fluorine-based ion conductive polymer and a partial fluorine-based polymer. In this patent, a non-fluorine ion conductive polymer and a partial fluorine polymer are used in combination with the non-fluorine iono.

When the fluorine-based iono coating layer is formed than when the blend of the non-fluorine ion conductive polymer and the partial fluorine-based polymer is formed on both sides of the hydrocarbon-based electrolyte membrane, the interface resistance between the electrode and the hydrocarbon-based separator can be reduced, thereby improving performance.

Korean Patent Laid-Open Publication No. 2009-17838 discloses a catalyst line or catalyst by spraying an electrolyte membrane or a gas diffusion layer in an inkjet manner such that a plurality of first catalyst particles continuously contact an ionomer binder resin and ink droplets for forming a catalyst portion dispersed in a solvent. A catalyst unit forming a spot line and having a plurality of catalyst lines or catalyst spot lines in contact with each other; And a plurality of second catalyst particles are sprayed by an inkjet method to continuously contact the ionomer binder resin and the ink droplets for forming the ionomer portion dispersed in the solvent to form an ionomer line or an ionomer spotline, and the ink droplets for forming the ionomer portion are catalysts. The concentration of the catalyst particles is lower than that of the ink for forming the sub, and the ionomer line or ionomer spotline has an ionomer portion formed of a plurality of ionomer lines or ionomer spot lines configured to be stacked on a portion where the plurality of catalyst lines or catalyst spot lines are in contact with each other. A fuel cell electrode comprising a catalyst layer formed by alternately stacking a catalyst portion and an ionomer portion is disclosed. In this patent, one of the fluorine-based electrolyte membrane and the hydrocarbon-based electrolyte membrane was used, and there is no disclosure about the electrolyte separator structure having the fluorine-based iono coating layer coated on both sides of the hydrocarbon-based membrane as in the present invention.

Republic of Korea Patent Publication No. 2009-92592 discloses a step of casting a polymer solution for producing an electrolyte membrane on a substrate; Primary drying the polymer solution for preparing the cast electrolyte membrane so as not to be completely dried; And stacking a catalyst layer for the first electrode on the first dried electrolyte membrane and completely drying the catalyst layer on one surface of the first polymer electrolyte membrane; A fuel comprising the step of adhering the first polymer electrolyte membrane and the second polymer electrolyte membrane formed with the catalyst layer for the second electrode, prepared through the above steps, so that the surfaces on which the catalyst layers of each polymer electrolyte membrane are not formed abut each other. A method of manufacturing a battery electrode assembly for a battery is disclosed. In this patent, one of the fluorine-based electrolyte membrane and the hydrocarbon-based electrolyte membrane was used, and there is no disclosure about the electrolyte separator structure having the fluorine-based iono coating layer coated on both surfaces of the hydrocarbon-based membrane as in the present invention.

An object of the present invention is to maintain the advantages of the hydrocarbon-based membrane used as the polymer electrolyte membrane of the fuel cell, but to compensate for the disadvantages, both chemical and mechanical durability is excellent, and performance by reducing the interface resistance between the electrode and the membrane It is to provide an improved polymer electrolyte separator for fuel cells.

Another object of the present invention is to provide a membrane electrode assembly having the above-described polymer electrolyte membrane.

Still another object of the present invention is to provide a fuel cell having the membrane electrode assembly described above.

In order to achieve the above object, the present invention provides a polymer electrolyte membrane for a fuel cell having a hydrocarbon-based membrane and a fluorine-based iono coating layer coated on both sides of the membrane.

The present invention is characterized by surface modification by coating both surfaces of the hydrocarbon-based membrane with fluorine ionomo, to maintain the advantages of the hydrocarbon-based membrane, but to compensate for the disadvantages. With such a simple surface modification, performance can be improved by reducing the interface resistance with the electrode layer, and mechanical durability can also be expected. It also maintains the original chemical durability.

In the present invention, the fluorine-based ionomer (Perfluorinated ionomer) may be used at least one selected from Nafion (TM), Flemion (TM), Aciplex (TM).

Hydrocarbon membranes in the present invention are sulfonated polykitone, sulfonated poly (phenylene oxide), sulfonated poly (phenylene sulfide), sulfonated polysulfone, sulfonated polycarbonate, sulfonated polystyrene, It may consist of one or more selected from sulfonated polyimide, sulfonated polyquinoxaline, sulfonated (phosphonated) polyphosphazene, and sulfonated polybenzimidazole.

In the present invention, the thickness of the fluorine-based iono coating layer is preferably 2 to 15 µm, particularly 2 to 5 µm.

The thicker the fluorine-based iono coating layer is advantageous for mechanical durability, but if too thick, the electrical resistance increases, so 2 to 15 μm is preferable.

In the present invention, the thickness of the hydrocarbon-based film is preferably 15 to 35 mu m, especially 20 to 25 mu m.

The thicker the hydrocarbon-based membrane, the better the chemical durability. However, if the thickness is too thick, the electrical resistance increases, so 15 to 35 μm is preferable.

In addition, the present invention is a polymer electrolyte membrane; An anode electrode formed on one side of the polymer electrolyte separator and including a catalyst layer and a gas diffusion layer; And a cathode electrode formed on the other side of the polymer electrolyte separator, the cathode electrode including a catalyst layer and a gas diffusion layer.

The present invention also provides a stack comprising at least one membrane electrode assembly as described above and a separator interposed between the membrane electrode assembly; A fuel supply unit supplying fuel to the stack; And an oxidant supply unit for supplying an oxidant to the stack.

The present invention can improve the performance by reducing the interfacial resistance between the electrode and the separator by coating the surface of both surfaces of the hydrocarbon-based membrane with fluorine ionomo, and can maintain the stable chemical durability of the hydrocarbon-based membrane, the brittleness of the hydrocarbon-based membrane By improving the (brittle) properties can improve the mechanical durability.

1 schematically illustrates the principle of electricity generation of a fuel cell.
2 schematically shows the structure of a membrane electrode assembly for a fuel cell.
Figure 3 schematically shows the structure of a polymer electrolyte membrane for a fuel cell according to an embodiment of the present invention.
4 schematically illustrates the structure of a fuel cell.

Hereinafter, the present invention will be described in detail with reference to the accompanying drawings.

FIG. 1 schematically illustrates the principle of electricity generation of a fuel cell. In the fuel cell, the most basic unit for generating electricity is a membrane electrode assembly (MEA), which is an electrolyte separator (M) and the electrolyte separator (M). It consists of an anode (A) and a cathode (C) electrode formed on both sides of the. Referring to FIG. 1 and Reaction Formula 1 (reaction formula of a fuel cell when hydrogen is used as a fuel) showing the electricity generation principle of a fuel cell, a fuel (F) such as hydrogen or a hydrocarbon such as methanol or butane is used at the anode (A) electrode. up of the oxidation reaction of hydrogen ion (H ⁺⁾ and electron (e ^-) it is generated, and the hydrogen ions move to the cathode (C) electrode through the electrolyte membrane (M). In the cathode (C) electrode, water (W) is generated by the reaction between the hydrogen ions transferred through the electrolyte separation membrane (M), the oxidant (O) such as oxygen, and the electrons. This reaction causes the movement of electrons in the external circuit.

[Reaction Scheme 1]

The ^{_{anode: H 2 → 2H + + 2e}} -

^{_{Cathode: 1 / 2O 2 + 2H +}} + 2e - → H 2 O

Overall Scheme: H ₂ + 1 / 2O ₂ → H ₂ O

FIG. 2 schematically illustrates the structure of a membrane electrode assembly for fuel cells, wherein the membrane electrode assembly for a fuel cell includes an anode electrode positioned to face each other with a polymer electrolyte separator 10 and the polymer electrolyte separator 10 therebetween; And a cathode electrode.

The anode electrode is composed of an anode catalyst layer 20 and an anode gas diffusion layer 50, and the anode gas diffusion layer 50 is again composed of an anode microporous layer 30 and an anode electrode substrate 40.

The cathode electrode is composed of the cathode catalyst layer 21 and the cathode gas diffusion layer 51, and the cathode gas diffusion layer 51 is composed of the cathode microporous layer 31 and the cathode electrode substrate 41.

The polymer electrolyte separator 10 includes a hydrocarbon-based membrane 11 and fluorine-based iono coating layers 12 and 13 coated on both surfaces thereof, which will be described later.

The catalyst layers 20 and 21 are prepared by mixing the catalyst, ionomer, and solvent in an appropriate mixture, and then using the method such as spraying or screen printing, ink is applied to the polymer electrolyte separator 10 or the gas diffusion layers 50 and 51. Apply and form. The thickness of the catalyst layers 20 and 21 may be determined as necessary, and may be, for example, 5 to 20 μm.

As the catalyst, a metal catalyst supported on a metal catalyst or a carbon-based support may be used. Typical metal catalysts include platinum, ruthenium, osmium, platinum-ruthenium alloys, platinum-osmium alloys, platinum-palladium alloys, and platinum-transition metal alloys. Any one or a mixture of two or more selected from can be used. Carbon-based supports include graphite (graphite), carbon black, acetylene black, denka black, canyon black, activated carbon, mesoporous carbon, carbon nanotubes, carbon nanofibers, carbon nanohorns, carbon nanorings, carbon nanowires, and fullerenes One or a mixture of two or more selected from the group consisting of (C60) and Super P may be a preferred example.

As ionomers, sulfonated polymers such as nafion ionomers or sulfonated polytrifluorostyrene may be representatively used.

As the solvent, any one or a mixture of two or more selected from the group consisting of water, butanol, isopropanol, methanol, ethanol, n-propanol, n-butyl acetate and ethylene glycol may be preferably used.

The gas diffusion layers 50 and 51 serve as current conductors between the polymer electrolyte separator 10 and the catalyst layers 20 and 21, and serve as passages of reactant gas and product water. Therefore, the gas diffusion layers 50 and 51 have a porous (20 to 90% porosity) structure to allow gas to pass through well. The thickness of the gas diffusion layers 50 and 51 may be appropriately adopted as necessary, and may be, for example, 100 to 400 μm. If the thickness is too thin, the electrical contact resistance between the catalyst layer and the bipolar plate is too large and does not have enough force to compress. If the thickness is too thick, it is difficult to move the reactant gas, so the thickness must be maintained at an appropriate level.

The fine pore layers 30 and 31 may include a carbonaceous material and a fluorine resin. Carbonaceous materials include graphite (graphite), carbon black, acetylene black, denka black, canyon black, activated carbon, mesoporous carbon, carbon nanotubes, carbon nanofibers, carbon nanohorns, carbon nanorings, carbon nanowires, and fullerenes. Any one or a mixture of two or more selected from the group consisting of (C60) and Super P may be used, but is not limited thereto. Examples of the fluororesin include polytetrafluoroethylene, polyvinylidene fluoride (PVdF), polyvinyl alcohol, cellulose acetate, polyvinylidene fluoride-hexafluoropropylene copolymer (PVdF-HFP) or styrene-butadiene rubber ( SBR) any one or a mixture of two or more selected from the group consisting of can be used.

The electrode substrates 40 and 41 may use a conductive substrate selected from the group consisting of carbon paper, carbon cloth, and carbon felt.

Figure 3 schematically shows the structure of a polymer electrolyte membrane for a fuel cell according to an embodiment of the present invention, the polymer electrolyte membrane 10 is a hydrocarbon-based membrane 11 and the fluorine iono coating layer 12 coated on both sides (12) , 13).

Hydrocarbon-based membrane 11 is sulfonated polykitone, sulfonated poly (phenylene oxide), sulfonated poly (phenylene sulfide), Sulfonated polysulfone, sulfonated polycarbonate, sulfonated polystyrene, sulfonated polyimide, sulfonated polyquinoxaline, Sulfonated (phosphonated) polyphosphazene (sulfonated (phosphonated) polyphosphazene), and sulfonated polybenzimidazole (PBI) may be made of one or more selected from.

The thickness of the hydrocarbon-based film 11 is preferably 15 to 35 mu m, especially 20 to 25 mu m.

Fluorine-based ionomorphs used in the fluorine-based iono coating layers 12 and 13 include Nafion (manufactured by Nafion, Dupont), Flemion (manufactured by Ashahi Glass), and Aciplex (manufactured by Aciplex, Ashahi Chemical). One or more kinds selected may be used.

Nafion is a fluorine-based membrane of DuPont, which is a perfluorosulfonic acid polymer having PTFE (Poly Tetra Fluoro Ethylene) as the main chain and a sulfone group in the side chain.

It is preferable that the thickness of the fluorine-type iono coating layers 12 and 13 is 2-15 micrometers, especially 2-5 micrometers.

As the coating method of the fluorine-based iono coating layers 12 and 13, a screen printing method, an inkjet coating method, a spray coating method, a doctor blade method, a roll coating method, a slit die coating method, or the like can be used. Particularly, a spray coating method is preferable. .

4 schematically illustrates a structure of a fuel cell, in which a fuel cell includes a stack 60, an oxidant supply unit 70, and a fuel supply unit 80.

The stack 200 includes one or two or more membrane electrode assemblies described above, and includes two or more separators interposed therebetween when two or more membrane electrode assemblies are included. The separator serves to prevent the membrane electrode assemblies from being electrically connected and to transfer fuel and oxidant supplied from the outside to the membrane electrode assembly.

The oxidant supply unit 70 serves to supply the oxidant to the stack 60. Oxygen is typically used as the oxidizing agent, and may be used by injecting oxygen or air into the pump 70.

The fuel supply unit 80 serves to supply fuel to the stack 60, and to the fuel tank 81 storing fuel and the pump 82 supplying fuel stored in the fuel tank 81 to the stack 60. Can be configured. The fuel may be gas or liquid hydrogen or hydrocarbon fuel, and examples of the hydrocarbon fuel include methanol, ethanol, propanol, butanol or natural gas.

[Example]

Fluorine-based ionomo was coated on both sides of the hydrocarbon-based membrane to prepare a polymer electrolyte membrane according to the present invention. Sulfonated polyketone was used as the hydrocarbon-based membrane, Nafion was used as the fluorine iono, and spray coating was used as the coating method. The thickness of the hydrocarbon film was 20 µm and the thickness of the fluorine iono coating layer was 5 µm.

A 9 cm × 9 cm polymer electrolyte membrane prepared as described above, and an anode electrode and a cathode electrode on which a catalyst layer was applied were prepared on 5 cm × 5 cm carbon paper. After stacking in order of anode electrode, electrolyte separator and cathode electrode, this was sandwiched between plates of a hot press at 140 ° C., pressed for 3 minutes at a pressure of 1 ton, and then the bonded body was taken out and cooled in air. Was produced.

[Comparative Example]

As the electrolyte separator, a conventional hydrocarbon-based polymer electrolyte separator (sulfonated polyketone) was used.

[Test Example]

For the polymer electrolyte membrane prepared in Examples and Comparative Examples, the chemical durability, mechanical durability and the performance of the MEA were measured, the results are shown in Table 1.

Chemical durability was measured by OCV holding method,

Mechanical durability was measured by the RH cycling method,

MEA performance was measured by polarization curve.

The OCV holding method maintains the Open Cell Voltage (OCV) state while hydrogen is flowed through the anode gas and oxygen is flowed through the cathode gas, which can induce chemical degradation of the separator and until the OCV value reaches 0.85V. The time of was measured. RH (Relative Humidity) cycling method can induce mechanical deterioration of separator by periodically flowing nitrogen in humidified state and non-humidified state, and periodically measure LSV (Linear Sweep Voltage) Was evaluated. MEA's performance was obtained by applying a load at intervals of 100 mA / cm2 from low current to high current with hydrogen flowing through the anode gas and air flowing through the cathode gas, and measuring the voltage corresponding to each step to obtain a polarization curve. Performance comparisons were made at voltages at 600 mA / cm 2.

Example Comparative Example Chemical durability 300 hours 200 hours Mechanical durability 3000 times 1000 times MEA performance 0.692 V 0.675 V

As can be seen in Table 1, it can be seen that in the case of the examples, the chemical durability, the mechanical durability and the performance of the MEA are superior to the comparative example.

10: polymer electrolyte membrane
11: hydrocarbon-based membrane
12, 13: fluorine iono coating layer
20, 21: catalyst bed
30, 31: microporous layer
40, 41: electrode substrate
50, 51: gas diffusion layer
60: stack
70: oxidant supply
80: fuel supply
81: fuel tank
82: pump

Claims (7)

A polymer electrolyte separator for a fuel cell, comprising a hydrocarbon-based membrane into which an ion exchange group is introduced and a fluorine-based iono coating layer into which an ion-exchange group is introduced, and having a fluorine-based iono coating layer on both surfaces of the hydrocarbon-based membrane. The polymer electrolyte separator for a fuel cell according to claim 1, wherein the fluorine-based ionomo is at least one selected from Nafion, Flemion, and Aciplex. The method of claim 1, wherein the hydrocarbon-based membrane is sulfonated polyketone, sulfonated poly (phenylene oxide), sulfonated poly (phenylene sulfide), sulfonated polysulfone, sulfonated polycarbonate, sulfonane A fuel characterized by consisting of at least one selected from tide polystyrene, sulfonated polyimide, sulfonated polyquinoxaline, sulfonated (phosphonated) polyphosphazene, and sulfonated polybenzimidazole Polymer electrolyte separator for batteries. The polymer electrolyte separator for a fuel cell according to claim 1, wherein the fluorine iono coating layer has a thickness of 2 to 15 µm. The polymer electrolyte separator for a fuel cell according to claim 1, wherein the thickness of the hydrocarbon-based membrane is 15 to 35 µm. The polymer electrolyte membrane of any one of claims 1 to 5;
An anode electrode formed on one side of the polymer electrolyte separator and including a catalyst layer and a gas diffusion layer; And
A membrane electrode assembly for a fuel cell, formed on the other side of the polymer electrolyte separator and comprising a cathode electrode comprising a catalyst layer and a gas diffusion layer. A stack comprising at least one membrane electrode assembly of claim 6 and a separator interposed between the membrane electrode assembly;
A fuel supply unit supplying fuel to the stack; And
A fuel cell having an oxidant supply unit for supplying an oxidant to a stack.

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