KR102598546B1 - Manufacturing device of membrane electrode assembly restraining deformation of both membrane electrode assembly and electrolyte membrane, and manufacturing method of membrane electrode assembly using the same - Google Patents

Abstract

The present invention relates to a membrane-electrode assembly manufacturing device that suppresses deformation of the electrolyte membrane and membrane-electrode assembly and a membrane-electrode assembly manufacturing method using the same, which uses a fixing part in a roll to roll process to produce an electrolyte membrane And it is characterized by providing a device and a manufacturing method for continuously manufacturing a membrane-electrode assembly without deformation of the membrane-electrode assembly.

Description

Manufacturing device of membrane electrode assembly restraining deformation of both membrane electrode assembly and electrolyte membrane, and manufacturing method of membrane electrode assembly using the same}

The present invention relates to a device for continuously manufacturing a membrane-electrode assembly without deformation of the electrolyte membrane and membrane-electrode assembly in a roll-to-roll process and a method for manufacturing a membrane-electrode assembly using the device.

Fuel cells produce electricity through electrochemical reactions between hydrogen and oxygen. These fuel cells are capable of continuous power generation by receiving chemical reactants from outside without a separate charging process.

A fuel cell can be constructed by placing a separator (separation plate) on both sides of a membrane-electrode assembly. These fuel cells are arranged in series and can be configured as a fuel cell stack.

The membrane-electrode assembly, a core component of a fuel cell, forms a hydrogen electrode and an air electrode as electrode layers on both sides of the electrolyte membrane through which hydrogen ions move. Additionally, the membrane-electrode assembly is provided with a sub-gasket to protect the electrode layer and electrolyte membrane and ensure assembly of the fuel cell.

The membrane-electrode assembly was manufactured by unwinding the electrolyte membrane wound into a roll and using a decal method to transfer the electrode layer to both sides of the electrolyte membrane.

In addition, a membrane-electrode assembly and a gas diffusion layer (GDL) are bonded to each other at a high temperature, and the bonded assembly is alternately stacked with a separator plate to manufacture a fuel cell.

Figure 1 shows a method of manufacturing a membrane-electrode assembly using a pair of pressure rollers in a roll-to-roll method. Referring to FIG. 1, a first release paper (2) coated with an anode and a second release paper (2') coated with a cathode are formed on the upper and lower surfaces of the electrolyte membrane (1) supplied through the electrolyte membrane supply roller (10). are stacked, and the electrodes stacked on both sides of the electrolyte membrane 1 are joined through a pair of pressure rollers 20 to form a membrane-electrode assembly 3, which is recovered by the recovery roller 30.

The above method has the disadvantage that the process speed cannot be increased due to the characteristics of the electrolyte membrane having a low tensile strength, and there is a limitation in forming the thickness of the electrolyte membrane into a thin film.

Another method is to form electrodes on both sides of the electrolyte membrane and heat-press them on a hot press plate. In this case, additional processing time of about 150 to 600 seconds is required due to hot pressing, and continuous processing, mass production, and automated processing are difficult. there is a problem.

In addition, it is generally important to manufacture the membrane-electrode assembly while maintaining the same transfer speed of the electrolyte membrane, creating a difference in the tension of the recovery roller and the electrolyte membrane supply roller. As the process progresses, the electrolyte membrane supply roller and the recovery roller Due to changes in the thickness of the wound electrolyte membrane, the transfer speed of the electrolyte membrane changes, and as a result, it becomes difficult to obtain a membrane-electrode assembly of uniform thickness, width, and quality.

Korean Patent Publication No. 10-2017-0133715 relates to a manufacturing apparatus and method of an electrode membrane assembly for fuel cells, which involves equipping electrodes on both sides of an electrolyte membrane supplied through an electrolyte membrane supply roller and laminating them with a thermocompression roller. The method is disclosed. However, there is a difference in the transfer speed of the electrolyte membrane supplied from the electrolyte membrane supply roller and the transfer speed of the membrane-electrode assembly recovered by the winding roller, and changes in thickness due to partial elongation of the electrolyte membrane and membrane-electrode assembly by the thermocompression roller. There is no way to fundamentally block it.

Korean Patent Publication No. 10-2017-0133715

The present invention is intended to solve the above problems, and its specific purpose is as follows.

The purpose of the present invention is to ensure dimensional stability of the electrolyte membrane by minimizing deformation of the weak electrolyte membrane when manufacturing a membrane-electrode assembly.

The purpose of the present invention is to manufacture a high-quality membrane-electrode assembly even when using a thin film or an electrolyte membrane with low tensile strength.

The purpose of the present invention is to provide a manufacturing method that can continuously manufacture a membrane-electrode assembly without interruption.

The purpose of the present invention is to improve the speed of the process of manufacturing a membrane-electrode assembly.

According to the present invention, it includes a supply part, a pressurizing part, a recovery part, and a fixing part, wherein the supply part supplies an electrolyte membrane, a first release paper coated with an anode, and a second release paper coated with a cathode, and the pressurizing part is supplied from the supply part. It includes a pair of pressure rollers for producing a membrane-electrode assembly by pressing the transferred electrolyte membrane, the first release paper coated with the anode, and the second release paper coated with the cathode, wherein the recovery unit produces the membrane-electrode assembly. It includes a winding recovery roller, a first release paper recovery roller for winding the first release paper from which the positive electrode has been removed, and a second release paper recovery roller for winding the second release paper from which the negative electrode has been removed, wherein the fixing part is configured to separate the electrolyte membrane from the front and rear ends of the pressing unit. and a tension-blocking membrane-electrode assembly manufacturing device, which is provided on both sides of the membrane-electrode assembly.

The fixing part includes a clip part including tongs that apply pressure to the upper and lower surfaces of both sides of the electrolyte membrane and membrane-electrode assembly to be transported; And it may include a body part fastened to the clip part.

Clamps are mounted on the front of the clip, the rear of the clip is fastened to the body, and a plurality of clips are fastened to the body at regular intervals along the outer surface of the body, and the clips are fastened to the body. It can move along the outer surface of the unit.

A plurality of clip parts fastened to the body part move at a constant speed along the body part, and the clip part is formed at a starting point parallel to the transfer direction (MD direction) of the electrolyte membrane or membrane-electrode assembly. The electrolyte membrane or membrane-electrode assembly is pulled by picking the membrane-electrode assembly with tongs, and the electrolyte membrane or membrane-electrode assembly is held at an end point that is horizontal to the transfer direction (MD direction) of the electrolyte membrane or membrane-electrode assembly. The tongs can be dismantled.

The moving speed and traction speed of the clip unit may be the same.

The supply unit may include an electrolyte membrane supply roller that supplies the electrolyte membrane.

The electrolyte membrane may be made of expanded polytetrafluoroethylene (ePTFE) as a support and impregnated with a fluorine-based ionomer.

It includes a first area between a fixing part provided on both sides of the electrolyte membrane at the front end of the pressing part and a fixing part provided on both sides of the membrane-electrode assembly at the rear end of the pressing part, wherein the first area is of the pressing part. It may include a second area between a pressing roller and a fixing part provided on both sides of the membrane-electrode assembly at a rear end of the pressing part.

The first area may not receive tension transmitted from the recovery roller.

The second region is not stretched in the MD and TD directions and can maintain constant tension in the MD and TD directions.

A pair of press rollers in the press unit can apply heat and pressure.

According to the present invention, a supply step of supplying an electrolyte membrane, a first release paper coated with an anode, and a second release paper coated with a cathode; A transfer step of transferring the electrolyte membrane, the first release paper, and the second release paper; A recovery step of winding the membrane-electrode assembly with a recovery roller, winding the first release paper from which the positive electrode has been removed with the first release paper recovery roller, and winding the second release paper from which the cathode has been removed with the second release paper recovery roller; and the transfer. The step includes a first transfer step of transferring the electrolyte membrane by the tension of the fixing part; A second transfer step of pulling the electrolyte membrane and membrane-electrode assembly through the fixing unit; And a third transfer step of transferring the membrane-electrode assembly by the tension of the recovery roller; In the second transfer step, the fixing unit exerts pressure on the upper and lower surfaces of both sides of the electrolyte membrane and the membrane-electrode assembly to be transferred. a clip portion including tongs that secure the electrolyte membrane and the membrane-electrode assembly to each fixing portion; and a body part fastening the clip part; wherein the clip part of the fixing part secures and tows the electrolyte membrane and the membrane-electrode assembly, respectively, and the second transfer step is performed by using a pair of pressure rollers to form the electrolyte membrane and the anode. A method of manufacturing a tension-blocking membrane-electrode assembly is provided, further comprising a pressurizing step of manufacturing a membrane-electrode assembly by pressing the coated first release paper and the cathode-coated second release paper.

The traction speed (w4) of the fixing part that fixes the electrolyte membrane and the membrane-electrode assembly in the second transfer step may be the same as the electrolyte membrane transfer speed in the first transfer step and the membrane-electrode assembly transfer speed in the third transfer step. .

In the second transfer step, the fixing part may be provided on both sides of the electrolyte membrane at the front end of the pressure roller and on both sides of the membrane-electrode assembly at the rear end of the pressure roller.

Fixing parts provided on both sides of the membrane-electrode assembly at the rear end of the pressure roller may be located at a point where deformation of the towed membrane-electrode assembly is minimal.

It includes a first area between fixing parts provided on both sides of the electrolyte membrane at the front end of the pressing part and fixing parts provided on both sides of the membrane-electrode assembly at the rear end of the pressing part, wherein the first area is pressed by the pressing part. It may include a second area between the roller and the fixing part provided on both sides of the membrane-electrode assembly at the rear end of the pressing part.

The first area may not receive tension transmitted from the recovery roller.

The electrolyte membrane and membrane-electrode assembly included in the second region are not stretched in the MD and TD directions and can maintain a constant tension in the MD and TD directions.

The transfer speed of the electrolyte membrane and the membrane-electrode assembly in the first transfer step, the second transfer step, and the third transfer step are all the same, and there may be no change in the transfer speed of the electrolyte membrane and the membrane-electrode assembly over time. there is.

In the pressing step, the pair of pressure rollers may apply heat and pressure to the supplied electrolyte membrane, the first release paper coated with the anode, and the second release paper coated with the cathode.

According to the present invention, when manufacturing a membrane-electrode assembly, deformation of the electrolyte membrane and the membrane-electrode assembly can be minimized.

According to the present invention, a high-quality membrane-electrode assembly can be manufactured even when a thin film or an electrolyte membrane with low tensile strength is used.

According to the present invention, a membrane-electrode assembly can be made in a continuous process using a thin film and a low tensile strength electrolyte membrane.

According to the present invention, the speed of the process of manufacturing a membrane-electrode assembly can be improved.

The effects of the present invention are not limited to the effects mentioned above. The effects of the present invention should be understood to include all effects that can be inferred from the following description.

Figure 1 shows a method of manufacturing a membrane-electrode assembly using a conventional roll-to-roll method.
Figure 2 schematically shows the process diagram of the membrane-electrode assembly manufacturing apparatus of the present invention.
Figure 3 briefly shows the formation process of a membrane-electrode assembly formed at regular intervals.
Figure 4 schematically shows the fixing part of the present invention.
Figure 5 shows the driving method of the fixing part and the clip part that pull the electrolyte membrane.
Figure 6 represents the area of the electrolyte membrane pulled by the fixing part.
Figure 7 shows the transfer steps of the electrolyte membrane divided by zone.
Figure 8 is a photograph observing the electrolyte membrane prepared in Comparative Example 1 and Example 1.

The above objects, other objects, features and advantages of the present invention will be easily understood through the following preferred embodiments related to the attached drawings. However, the present invention is not limited to the embodiments described herein and may be embodied in other forms. Rather, the embodiments introduced herein are provided so that the disclosed content will be thorough and complete and so that the spirit of the present invention can be sufficiently conveyed to those skilled in the art.

While describing each drawing, similar reference numerals are used for similar components. In the attached drawings, the dimensions of the structures are enlarged from the actual size for clarity of the present invention. Terms such as first, second, etc. may be used to describe various components, but the components should not be limited by the terms. The above terms are used only for the purpose of distinguishing one component from another. For example, a first component may be named a second component, and similarly, the second component may also be named a first component without departing from the scope of the present invention. Singular expressions include plural expressions unless the context clearly dictates otherwise.

In this specification, terms such as “comprise” or “have” are intended to designate the presence of features, numbers, steps, operations, components, parts, or combinations thereof described in the specification, but are not intended to indicate the presence of one or more other features. It should be understood that this does not exclude in advance the possibility of the existence or addition of elements, numbers, steps, operations, components, parts, or combinations thereof. Additionally, when a part of a layer, membrane, region, plate, etc. is said to be “on” another part, this includes not only being “directly above” the other part, but also cases where there is another part in between. Conversely, when a part of a layer, membrane, region, plate, etc. is said to be "underneath" another part, this includes not only being "immediately below" the other part, but also cases where there is another part in between.

Unless otherwise specified, all numbers, values, and/or expressions used herein expressing quantities of components, reaction conditions, polymer compositions, and formulations are intended to represent, among other things, how such numbers inherently occur in obtaining such values. Since they are approximations reflecting the various uncertainties of measurement, they should be understood in all cases as being qualified by the term "approximately". Additionally, where a numerical range is disclosed herein, such range is continuous and, unless otherwise indicated, includes all values from the minimum to the maximum of such range inclusively. Furthermore, when such range refers to an integer, all integers from the minimum value up to and including the maximum value are included, unless otherwise indicated.

In this specification, when a range is stated for a variable, the variable will be understood to include all values within the stated range, including the stated endpoints of the range. For example, the range "5 to 10" includes the values 5, 6, 7, 8, 9, and 10, as well as any subranges such as 6 to 10, 7 to 10, 6 to 9, 7 to 9, etc. It will be understood that it also includes any values between integers that fall within the scope of the stated range, such as 5.5, 6.5, 7.5, 5.5 to 8.5, and 6.5 to 9, etc. Also, for example, the range "10% to 30%" includes values such as 10%, 11%, 12%, 13%, etc. and all integers up to and including 30%, as well as 10% to 15%, 12% to 12%, etc. It will be understood that it includes any subranges, such as 18%, 20% to 30%, etc., and any value between reasonable integers within the range of the stated range, such as 10.5%, 15.5%, 25.5%, etc.

The present invention relates to an apparatus for manufacturing a membrane-electrode assembly that suppresses deformation of the electrolyte membrane (1) and a method for manufacturing a membrane-electrode assembly using the same. It is characterized by providing an apparatus and manufacturing method for continuously manufacturing a membrane-electrode assembly without deformation of the membrane 1 and the membrane-electrode assembly 3. The membrane-electrode assembly manufacturing apparatus and manufacturing method will be described below using the drawings of the present invention.

Membrane-electrode conjugate manufacturing device

According to the present invention, it includes a supply part (A1), a pressurizing part (A2), a recovery part (A3), and a fixing part (A4), and the supply part (A1) includes an electrolyte membrane (1) and a first release paper coated with an anode. (2) and the second release paper (2') coated with the cathode is supplied, and the pressurizing part (A2) supplies the electrolyte membrane (1) transferred from the supply part (A1) and the first release paper (2') coated with the anode. And a pair of pressure rollers (20) that pressurize the second release paper (2') coated with the cathode to produce the membrane-electrode assembly (3), and the recovery unit (A3) is configured to press the second release paper (2') coated with the cathode. It includes a recovery roller 30 for winding the bonded body 3, a first release paper recovery roller for winding the first release paper 4 from which the positive electrode has been removed, and a second release paper recovery roller for winding the second release paper 4' from which the negative electrode has been removed. And the fixing part (A4) is a tension-blocking membrane-electrode assembly, characterized in that it is provided on both sides of the electrolyte membrane (1) and the membrane-electrode assembly (3) at the front and rear ends of the pressing portion (A2). Manufacturing equipment is provided.

Figure 2 briefly shows in plan view the configuration and driving method of the membrane-electrode assembly manufacturing apparatus of the present invention. Each part and configuration of the membrane-electrode assembly manufacturing apparatus of the present invention will be described with reference to FIG. 2 with FIG. 1 as the basic base.

The membrane-electrode assembly manufacturing apparatus of the present invention largely includes a supply part (A1), a pressurizing part (A2), and a recovery part (A3). It is characterized in that it further includes a fixing part (A4), wherein the fixing part (A4) controls the amount of the electrolyte membrane (1) and the membrane-electrode assembly (3) at the front and rear ends of the pressing part (A2). It is provided on the side. Specifically, the fixing part (A4) located at the front end is provided between the supply part (A1) and the pressing part (A2), and the fixing part (A4) located at the rear end is provided between the pressing part (A2) and the recovery part ( It is provided between A3).

The supply unit A1 includes an electrolyte membrane supply roller 10 that supplies the electrolyte membrane 1. Typically, the electrolyte membrane supply roller 10 creates a tension difference with the recovery roller 30 of the recovery unit A3, thereby allowing the electrolyte membrane 1 to be completely transferred and wound around the recovery roller 30. Typically, when the fixing part (A4) is excluded, the tension of the supply part (A1) and the pressing part (A2) is usually 10N or more, and the tension of the pressing part (A2) and the recovery part (A3) is 12N or more, and the tension The difference is transmitted through the electrolyte membrane (1). However, in the present invention, the tension of the recovery roller 30 is transmitted to the electrolyte membrane 1 passing through the fixing part A4 located at the rear end of the pressure roller 20, and the tension of the electrolyte membrane supply roller 10 is transmitted to the front end of the pressure roller 20. It is transmitted only up to the fixing part (A4) located at, and the tension of the electrolyte membrane (1) is not transmitted at the front end (A4) of the fixing part and the pressurizing part (A2), and the tension of the electrolyte membrane (1) is not transmitted at the pressurizing part (A2) and the rear end of the fixing part (A4). -The tension of the electrode assembly (3) is not transmitted. The electrolyte membrane supply roller 10 supplies and transports the electrolyte membrane 1 due to a tension difference with the fixing part A4 located at the front of the pressure roller 20. The transfer speed of the electrolyte membrane 1 can be adjusted while maintaining the difference in tension constant.

The electrolyte membrane 1 that can be used in the present invention is not particularly limited as long as it is an electrolyte membrane material that can be used in a fuel cell. Due to the nature of the present invention, materials with a thickness of 20 μm or less and a tensile strength of 100 MPa or less can be used. In the present invention, an electrolyte membrane impregnated with a fluorine-based ionomer using expanded polytetrafluoroethylene (ePTFE) as a support was used as the electrolyte membrane (1). Typically, the electrolyte membrane 1 is supplied at room temperature.

The supply unit (A1) includes an anode supply roller (not shown) that supplies the anode-coated first release paper 2 so as to supply electrodes to the upper and lower parts of the electrolyte membrane 1, and a cathode-coated second release paper. It further includes a cathode supply roller (not shown) that supplies (2'). It is common to interpose the electrolyte membrane supply roller 10 between the anode supply roller and the cathode supply roller. At this time, the anode supply roller and the cathode supply roller can change their up and down positions as needed. Therefore, the anode can be attached to the top or the bottom of the electrolyte membrane 1, and the same applies to the cathode.

In the description and drawings of the present invention, for convenience, the anode and the cathode are formed continuously on the first release paper 2 and the second release paper 2', and are continuously formed on the top and bottom of the electrolyte membrane 1 like this. Although it is depicted as an attached shape, it is not limited to this. For example, Figure 3 shows a membrane-electrode assembly in which the anode and cathode are formed at regular, discontinuous intervals.

Since the anode supply roller and the cathode supply roller are driven for the purpose of attaching the anode and cathode to the upper and lower parts of the electrolyte membrane 1, they are generally operated at the same rotational speed as the electrolyte membrane supply roller 10.

The anode material of the anode-coated release paper (2) supplied from the anode supply roller is formed on the surface of the anode-coated release paper (2) facing the electrolyte membrane (1), and the anode material supplied from the cathode supply roller is formed on the surface of the anode-coated release paper (2) facing the electrolyte membrane (1). The negative electrode material of the negative electrode-coated release paper 2' is formed on the side of the negative electrode-coated release paper 2' facing the electrolyte membrane 1.

The pressing part (A2) is located between the supply part (A1) and the recovery part (A3), and includes an electrolyte membrane (1), a first release paper (2) coated with the anode, and a second release paper (2) coated with the cathode. ') and a pressure roller 20 capable of applying heat and pressure. Specifically, the anode and cathode and the electrolyte membrane 1 respectively laminated on the upper and lower surfaces of the electrolyte membrane 1 supplied from the supply unit A1 through release paper can be rotated and pressed with heat and constant pressure. At this time, the heat and pressure vary depending on the material and stacking environment of the electrolyte membrane 1 used, and are typically applied at a temperature of 80 to 200°C and a pressure of 5 to 100 MPa. It is possible to continuously manufacture the membrane-electrode assembly 3 by rotating the pressure roller 20. (The method of stacking the anode and cathode is not specifically specified because it deviates from the characteristics of the present invention to select the method of stacking the anode and the cathode. However, this does not exclude that the anode, electrolyte membrane 1, and cathode are pressed and joined through a pair of pressure rollers 20.)

The recovery unit (A3) includes a recovery roller (30) that winds and recovers the membrane-electrode assembly (3) manufactured in the pressing unit (A2), and a first release paper recovery roller that winds the first release paper (4) from which the positive electrode has been removed. and a second release paper recovery roller (not shown) that winds the second release paper 4' from which the cathode has been removed.

The recovery roller 30 transmits a certain tension to the membrane-electrode assembly 3 through rotational movement, and the pressure roller 20 is moved by the tension of the recovery roller 30 transmitted through the membrane-electrode assembly 3. ) The membrane-electrode assembly (3) that has passed through the fixing part (A4) at the rear end is completely transferred and goes through the process. The difference in tension is generally 2N or more.

The first release paper recovery roller and the second release paper recovery roller are provided above and below the recovery roller 30 for recovering the membrane-electrode assembly 3. The first release paper recovery roller and the second release paper recovery roller attach the electrode material to the electrolyte membrane 1 by the pressure roller 20 and wind the first release paper and the second release paper from which the anode and cathode have been removed.

Figure 4 briefly shows the configuration of the fixing part A4 of the present invention. The fixing part (A4) includes a clip part (41) including clamps that apply pressure to the upper and lower surfaces of both sides of the electrolyte membrane (1) to be transferred (only one side is shown in FIG. 4 for convenience). and a body part to which the clip part 41 is fastened (the specific drawing of the body part is omitted, and only the rail 42, which is a part of the body part, is shown in FIG. 4). At this time, the tongs are opened or closed with a rotating pin (not shown) serving as a rotation axis at the end of the tongs as the central point. However, the shape of the tongs is not particularly limited by this.

The tongs of the present invention include a pair of pressing members that can apply enough pressure to fix a generally flat sheet at a desired time at the top and bottom of the sheet. This is sufficient to have the shape of a normal tongs or a shape that can perform the role of tongs, and in addition, the pair of pressure members are spaced at a certain interval so that the sheet can be unfastened or placed at a desired time. It is enough to be able to dismantle it.

The body portion is basically fixed without movement in its provided position.

The tongs are mounted on the front of the clip part 41, and the clip part 41 on which the tongs are mounted is fastened to the body part. The side of the body part may be equipped with a belt-shaped or strip-shaped rail 42. A bearing mounted on the rear side of the clip part 41 contacts the rail 42 and rotates the bearing to form the clip part 41. ) can move along the side of the body. If necessary, the rail 42 may be selected in a chain shape, but there is no particular limitation as long as the clip portion 41 has a shape that can move along the side of the body.

A plurality of clip parts 41 are fastened at regular intervals along the outer surface of the body, and the plurality of clip parts 41 move sequentially along the outer surface, that is, the side, of the body. At this time, the plurality of clip parts 41 can move while maintaining a constant speed (w4), and the power source for moving the clip parts 41 is supplied from a separate external power source.

Figure 5 schematically shows the driving method of the fixing part A4. Referring to this, the clip portion 41 is formed at a starting point B1 that is horizontal to the transport direction (machine direction, MD direction) of the electrolyte membrane 1 and the membrane-electrode assembly 3. ) and the membrane-electrode assembly 3 are picked up with tongs to pull the electrolyte membrane 1 and the membrane-electrode assembly 3, and the transfer direction of the electrolyte membrane 1 and the membrane-electrode assembly 3 ( The tongs holding the electrolyte membrane 1 and the membrane-electrode assembly 3 are dismantled and placed at the end point B2 (MD direction) and horizontal end point. At this time, the moving speed (w4) of the clip portion 41 that does not hold the electrolyte membrane (1) and the membrane-electrode assembly (3) or the clip portion (41) that holds the electrolyte membrane (1) and the membrane-electrode assembly (3) ) of the traction speed (w4) is the same as the transfer speed of the electrolyte membrane (1) or membrane-electrode assembly (3) in all sections.

The plurality of clip parts 41 fastened to the body are located on the left side of the electrolyte membrane 1 (for convenience of understanding, the explanation will be centered on the electrolyte membrane) that is transferred when the body moves from the supply part A1 to the recovery part A3. If it is provided on the right side, it moves counterclockwise along the outer surface of the body, and if it is provided on the right side, it moves clockwise along the outer surface of the body.

The starting point (B1) and the ending point (B2) of both sides of the electrolyte membrane (1) are fixed with the clamps of a plurality of clip portions (41), and the clip portions (41) clamp the electrolyte contained in the section. It also plays a role in continuously suppressing the membrane 1 from shrinking in the MD and TD directions.

Figure 6 shows the area of the electrolyte membrane 1 pulled by the fixing part A4. Referring to this, the electrolyte membrane 1 is formed by a fixing part A4 provided on both sides of the electrolyte membrane 1 at the front end of the pressing part A2 and the membrane-electrode assembly ( 3) Fixing parts (A4) provided on both sides of the membrane-electrode assembly (3) where the anode and cathode (2) are joined by exactly a pair of pressure rollers (20) or a sub-gasket is additionally joined. It includes a first area (P1) between the pressing roller (20) of the pressing part (A2) and the membrane-electrode assembly (3) at the rear end of the pressing part (A2). It includes a second area (P2) between the fixing parts (A4) provided on both sides. At this time, the position of the fixing part A4 located at the front of the pressure roller 20 of the pressure part A2, which is the reference of the first area P1, can be adjusted according to the purpose and convenience of the process, but the pressure roller 20 The position of the fixing part (A4) located at the rear end must be located at a point where the deformation of the membrane-electrode assembly (3) is minimal. Specifically, even if the membrane-electrode assembly 3, whose tensile strength has decreased due to heat and pressure from the pressurizing roller 20, passes through the fixing part A4 and directly receives the tension of the recovery roller 30, the membrane-electrode assembly ( It is desirable that the last fixing part (A4) is provided in a range where the deformation of 3) does not occur. This is to provide time for the reduced tensile strength of the membrane-electrode assembly (3) to recover while being transported, and the type of electrolyte membrane (1) material included in the membrane-electrode assembly (3) is transferred through the pressure roller (20). It may vary depending on the transferred heat, pressure, and transfer speed of the electrolyte membrane (1) and membrane-electrode assembly (3).

The first area P1 is characterized in that it does not receive tension transmitted from the recovery roller 30. Specifically, the electrolyte membrane 1 and the membrane-electrode assembly 3 are fixed through the tongs included in the fixing part A4, which is the standard for forming the partition of the first area P1. At this time, the electrolyte membrane 1 and the membrane-electrode assembly 3 are fixed. (1) and the membrane-electrode assembly 3 are fixed with tongs attached to the clip portion 41, so that the first region P1 is not affected by external forces. The transfer of the electrolyte membrane 1 fixed with the tongs proceeds based on the movement of the clip portion 41.

The first area (P1) includes a pressure roller 20 of the pressure part (A2), and the electrolyte membrane 1 moving in the first area (P1) is applied by heat and pressure by the pressure roller 20. Although the tensile strength is lowered due to pressure, it is not affected by external tension, so it is not stretched in the MD and TD directions, and maintains the shape of the electrolyte membrane 1 before entering the pressure roller 20. do. In FIG. 6, the membrane-electrode assembly 3 passing through the second region P2 maintains a constant tension and is pulled by the clip portion 41.

Membrane-electrode assembly manufacturing method

According to the present invention, a supply step of supplying an electrolyte membrane (1), a first release paper (2) coated with an anode, and a second release paper (2') coated with a cathode; A transfer step of transferring the electrolyte membrane (1), the first release paper (2) coated with the anode, the second release paper (2') coated with the cathode, and the membrane-electrode assembly (3); A recovery step of winding the membrane-electrode assembly with a recovery roller, winding the first release paper from which the positive electrode has been removed with the first release paper recovery roller, and winding the second release paper from which the negative electrode has been removed with the second release paper recovery roller; The transfer step includes a first transfer step of transferring the electrolyte membrane (1) by the tension of the fixing part (A4); A second transfer step (S2) of pulling the electrolyte membrane (1) and the membrane-electrode assembly (3) through the fixing part (A4); And a third transfer step (S3) of transferring the membrane-electrode assembly 3 by the tension of the recovery roller 30; In the second transfer step (S2), the fixing part A4 is the electrolyte membrane to be transferred. (1) and the clamps that secure the electrolyte membrane (1) and the membrane-electrode assembly (3) to the fixing portion (A4) by applying pressure to the upper and lower surfaces of both sides of the membrane-electrode assembly (3). A clip portion (41) including; and a body part fastening the clip part 41, wherein the clip part 41 of the fixing part A4 secures and pulls the electrolyte membrane 1 and the membrane-electrode assembly 3, respectively. , the second transfer step (S2) presses the electrolyte membrane 1, the anode-coated first release paper 2, and the cathode-coated second release paper 2' with a pair of pressure rollers 20. A method for manufacturing a tension-blocking membrane-electrode assembly is provided, further comprising a pressurizing step.

In the membrane-electrode assembly manufacturing method, parts that overlap with the features of the present invention described in the membrane-electrode assembly manufacturing apparatus will be omitted.

The transfer step of the present invention includes a first transfer step (S1) of transferring the electrolyte membrane (1) by the tension of the fixing part (A4); A second transfer step (S2) of pulling the electrolyte membrane (1) and the membrane-electrode assembly (3) through the fixing part (A4); and a third transfer step (S3) of transferring the membrane-electrode assembly 3 by the tension of the recovery roller 30. The division of the step of transferring the electrolyte membrane 1 and the membrane-electrode assembly 3 into three stages as described above is due to a change in the subject transporting the electrolyte membrane 1 and the membrane-electrode assembly 3. .

In Figure 7, the transfer steps of the electrolyte membrane 1 are shown for each section. The first transfer step (S1) is a step in which the electrolyte membrane (1) is transferred by tension transmitted through the electrolyte membrane (1), which is fixed and towed by the tongs of the fixing part (A4). The second transfer step (S2) is a step in which the electrolyte membrane (1) and the membrane-electrode assembly (3) are transferred by pulling the clip unit (41) operated through an external power source. The third transfer step (S3) is a step in which the tension generated from the recovery roller 30 is transferred to the membrane-electrode assembly 3 that has passed through the clip portion 41, and the membrane-electrode assembly 3 is transferred.

Typically, as the process progresses, the amount of electrolyte membrane wound around the electrolyte membrane supply roller (exactly the total thickness of the electrolyte membrane wound around the supply roller) decreases, and the amount of membrane-electrode assembly wound around the recovery roller (exactly the membrane wound around the recovery roller) decreases. The total thickness of the electrode assembly increases, and due to the above change in thickness, a difference occurs in the rotation speed of the electrolyte membrane supply roller and the recovery roller. Due to the above subtle differences, uneven tension occurs in the electrolyte membrane or membrane-electrode assembly or differences in transfer speed occur in the first transfer step (S1), the second transfer step (S2), and the third transfer step (S3). This occurs, and as a result, it has a negative impact on the quality (specifically, the effect of wrinkles occurring or elongation in the electrolyte membrane or membrane-electrode assembly) in continuously manufacturing the membrane-electrode assembly. However, in the case of the present invention, the speed (v1) of the electrolyte membrane (1) in the first transfer step (S1), the electrolyte membrane (1) and the membrane-electrode assembly (3) pulled in the second transfer step (S2) It is characteristic that the speed (v2) and the speed (v3) of the membrane-electrode assembly (3) transferred in the third transfer step (S3) are all the same.

That is, as the process progresses, the thickness of the membrane-electrode assembly 3 wound around the recovery roller 30 and the thickness of the electrolyte membrane 1 wound around the electrolyte membrane supply roller 10 change. ) and the transfer speed of the membrane-electrode assembly 3 may vary, but in the present invention, the electrolyte membrane 1 and the membrane-electrode assembly 3 are connected between the recovery roller 30 and the electrolyte membrane supply roller 10. The presence of the pulling fixing part A4 can control the change in transfer speed of the electrolyte membrane 1 and the membrane-electrode assembly 3.

If the above is further explained with reference to FIG. 7, the rotational speed (w2) of the recovery roller 30 is usually greater than the rotational speed (w1) of the electrolyte membrane supply roller 10 at the beginning of the process, but the recovery roller 30 ) After the thickness of the membrane-electrode assembly (3) wound on the electrolyte membrane supply roller (10) becomes thicker than the thickness of the electrolyte membrane (1) wound on the electrolyte membrane supply roller (10), the rotational speed (w2) of the recovery roller (30) increases. It becomes smaller than the rotational speed (w1) of the electrolyte membrane supply roller (10).

However, according to the present invention, the fixing part A4 (exactly the clip part 41 included in the fixing part A4) fixed the electrolyte membrane 1 and the membrane-electrode assembly 3 in the second transfer step (S2). ) of the traction speed (w4) is the same as the transfer speed (V1) of the electrolyte membrane (1) in the first transfer step (S1), and the transfer speed of the membrane-electrode assembly (3) in the third transfer step (S3) It has the same features as (V3). In other words, the process of manufacturing the membrane-electrode assembly can proceed at a constant speed.

Hereinafter, the present invention will be described in more detail through specific examples. The following examples are merely examples to aid understanding of the present invention, and the scope of the present invention is not limited thereto.

Comparative Example 1

A pair of pressure rollers rotated at a speed of 0.1 m/min and pressed the transported electrolyte membrane at a temperature of 100°C and a pressure of 13 MPa. The electrolyte membrane used at this time is PFSA-based with a thickness of 20㎛ and a width of 160㎜. The electrolyte membrane was transferred while controlling the tension to be 10N at the electrolyte membrane supply roller and 12N at the recovery roller.

In Figure 8, the electrolyte membrane on the left is the electrolyte membrane of Comparative Example 1. Looking at this, you can see that many wrinkles have occurred in the non-joint area. Overall, the electrolyte membrane width was reduced from 160 mm to 157 mm. This can be seen as a result of the non-bonded portion of the electrolyte membrane, whose tensile strength has decreased due to heat and pressure from the pressurizing roller, being stretched in the MD direction due to the tension of the recovery roller, resulting in shrinkage in the TD direction. In addition, it is expected that the formation of unequal tensile strength between the joints joined by the pressure roller and the non-joint parts not joined by the pressure roller will cause deformation of the entire electrolyte membrane, causing a substantial deterioration in the quality of the membrane-electrode assembly. In other words, the changes in the wrinkles and dimensions of the electrolyte membrane of Comparative Example 1 as described above appear to be because some of the tension generated from the recovery roller was used as energy to stretch the electrolyte membrane whose tensile strength was lowered by the pressure roller.

Example 1

The electrolyte membrane was transferred under the same conditions as in Comparative Example 1, but the electrolyte membrane was fixed and pulled by using fixing parts of the present invention on both sides of the electrolyte membrane before and after the pressure roller. At this time, the traction speed (w4) of the fixed part is 0.1 m/min.

The right side of Figure 8 is the electrolyte membrane of Example 1. Compared to Comparative Example 1, it can be confirmed with the naked eye that almost no wrinkles occur in the non-bonded portion. The width of the electrolyte membrane in Example 1 is 159.5 mm. Looking at the width strain rate, Comparative Example 1 is about 6%, while Example 1 is about 0.3%, which is expected to produce a very high quality membrane-electrode assembly even in a process at a speed of 0.1 m/min. As described above, the reason that the electrolyte membrane was produced stably without change in dimensions compared to Comparative Example 1 appears to be because the transfer of tension generated from the recovery roller to the electrolyte membrane, whose tensile strength was lowered by the pressure roller, was effectively excluded.

1: Electrolyte membrane w1: Rotation speed of electrolyte membrane supply roller
2: First release paper coated with anode w2: Rotation speed of recovery roller
2': Second release paper coated with cathode w3: Rotation speed of pressure roller
3: Membrane-electrode assembly w4: Clip part movement speed (=electrolyte membrane traction speed)
4: First release paper with anode removed v1: Electrolyte membrane movement speed in the first transfer step
4': Second release paper v2 with the cathode removed: Electrolyte membrane movement speed in the second transfer step
10: Electrolyte membrane supply roller v3: Electrolyte membrane moving speed in the third transfer step
20: Pressure roller P1: First area
30: Recovery roller P2: Second area
40: Clip part, body part
41: Clip part
42: Rail of body part
A1: Supply Department
A2: Pressurizing part
A3: Recovery Department
A4: Fixed part
B1: starting point
B2: Endpoint

Claims (20)

It includes a supply part, a pressurizing part, a recovery part, and a fixing part,
The supply unit supplies an electrolyte membrane, a first release paper coated with an anode, and a second release paper coated with a cathode,
The pressing unit includes a pair of press rollers that press the electrolyte membrane, the anode-coated first release paper, and the cathode-coated second release paper transferred from the supply unit to produce a membrane-electrode assembly,
The recovery unit includes a recovery roller that winds the manufactured membrane-electrode assembly,
A first release paper recovery roller that winds the first release paper from which the anode has been removed, and
It includes a second release paper recovery roller that winds the second release paper from which the cathode has been removed,
The fixing portion is provided on both sides of the electrolyte membrane and the membrane-electrode assembly at the front and rear ends of the pressurizing portion,
Comprising a first area between a fixing part provided on both sides of the electrolyte membrane at the front end of the pressing part and a fixing part provided on both sides of the membrane-electrode assembly at the rear end of the pressing part,
The first area is a tension-blocking membrane-electrode characterized in that it includes a second area between the pressing roller of the pressing unit and the fixing parts provided on both sides of the membrane-electrode assembly at the rear end of the pressing unit. Conjugate manufacturing device. According to paragraph 1,
The fixing part includes a clip part including tongs that apply pressure to the upper and lower surfaces of both sides of the electrolyte membrane and membrane-electrode assembly to be transported; and
A tension-blocking membrane-electrode assembly manufacturing apparatus comprising a body part fastened to the clip part. According to paragraph 2,
A clamp is mounted on the front of the clip portion,
The rear of the clip portion is fastened to the body portion,
A plurality of clip parts are fastened to the body at regular intervals along the outer surface of the body,
A tension-blocking membrane-electrode assembly manufacturing device, characterized in that the clip portion can move along the outer surface of the body portion. According to paragraph 3,
A plurality of clip parts fastened to the body move at a constant speed along the body,
The clip portion picks up the electrolyte membrane or membrane-electrode assembly with tongs at a starting point that is horizontal to the transfer direction (MD direction) of the electrolyte membrane or membrane-electrode assembly and pulls the electrolyte membrane or membrane-electrode assembly,
A tension-blocking membrane-electrode assembly manufacturing device, characterized in that dismantling the tongs holding the electrolyte membrane or membrane-electrode assembly at an end point that is horizontal to the transfer direction (MD direction) of the electrolyte membrane or membrane-electrode assembly. According to paragraph 4,
Tension-blocking membrane-electrode assembly manufacturing device, characterized in that the moving speed and traction speed of the clip part are the same. According to paragraph 1,
The supply unit is a tension-blocking membrane-electrode assembly manufacturing device, characterized in that it includes an electrolyte membrane supply roller for supplying the electrolyte membrane. According to paragraph 1,
The electrolyte membrane is a tension-blocking membrane-electrode assembly manufacturing device, characterized in that expanded polytetrafluoroethylene (ePTFE) is used as a support and impregnated with a fluorine-based ionomer. delete According to paragraph 1,
A tension-blocking membrane-electrode assembly manufacturing device, characterized in that the first region does not receive tension transmitted from the recovery roller. According to paragraph 1,
A tension-blocking membrane-electrode assembly manufacturing apparatus, characterized in that the second region is not stretched in the MD and TD directions and maintains a constant tension in the MD and TD directions. According to paragraph 1,
A tension-blocking membrane-electrode assembly manufacturing device, characterized in that a pair of press rollers in the press unit applies heat and pressure. A supply step of supplying an electrolyte membrane, a first release paper coated with an anode, and a second release paper coated with a cathode;
A transfer step of transferring the electrolyte membrane, the first release paper coated with the anode, the second release paper coated with the cathode, and the membrane-electrode assembly;
A recovery step of winding the membrane-electrode assembly with a recovery roller, winding the first release paper from which the positive electrode has been removed with the first release paper recovery roller, and winding the second release paper from which the negative electrode has been removed with the second release paper recovery roller;
The transfer step includes a first transfer step of transferring the electrolyte membrane by tension of the fixing part;
A second transfer step of pulling the electrolyte membrane and membrane-electrode assembly through the fixing part; and
A third transfer step of transferring the membrane-electrode assembly using the tension of the recovery roller,
In the second transfer step, the fixing part applies pressure to the upper and lower surfaces of both sides of the electrolyte membrane and the membrane-electrode assembly to be transferred, and the clip includes a tong for fixing the electrolyte membrane and the membrane-electrode assembly to the fixing part, respectively. wealth; and
It includes a body part fastened to the clip part,
The clip portion of the fixing unit secures and pulls the electrolyte membrane and the membrane-electrode assembly, respectively,
The second transfer step further includes a pressing step of manufacturing a membrane-electrode assembly by pressing the electrolyte membrane, the anode-coated first release paper, and the cathode-coated second release paper with a pair of pressure rollers,
In the second transfer step, the fixing part is provided on both sides of the electrolyte membrane at the front end of the pressure roller and on both sides of the membrane-electrode assembly at the rear end of the pressure roller,
Comprising a first area between a fixing part provided on both sides of the electrolyte membrane at the front end of the pressing part and a fixing part provided on both sides of the membrane-electrode assembly at the rear end of the pressing part,
The first area is a tension-blocking membrane-electrode assembly manufacturing method, characterized in that it includes a second area between the pressing roller of the pressing unit and the fixing parts provided on both sides of the membrane-electrode assembly at the rear end of the pressing unit. According to clause 12,
The traction speed (w4) of the fixing part that fixes the electrolyte membrane and the membrane-electrode assembly in the second transfer step is the same as the electrolyte membrane transfer speed in the first transfer step and the membrane-electrode assembly transfer speed in the third transfer step. Method for manufacturing a tension-blocking membrane-electrode assembly. delete According to clause 12,
A method of manufacturing a tension-blocking membrane-electrode assembly, characterized in that the fixing portions provided on both sides of the membrane-electrode assembly at the rear end of the pressure roller are located at a point where deformation of the towed membrane-electrode assembly is minimized. delete According to clause 12,
A method of manufacturing a tension-blocking membrane-electrode assembly, characterized in that the first region does not receive tension transmitted from the recovery roller. According to clause 12,
A method of manufacturing a tension-blocking membrane-electrode assembly, characterized in that the electrolyte membrane and membrane-electrode assembly included in the second region are not stretched in the MD and TD directions and maintain a constant tension in the MD and TD directions. According to clause 12,
In the first transfer step, second transfer step, and third transfer step, the transfer speeds of the electrolyte membrane and the membrane-electrode assembly are all the same,
A method of manufacturing a tension-blocking membrane-electrode assembly, characterized in that there is no change in the transfer speed of the electrolyte membrane and the membrane-electrode assembly over time. According to clause 12,
In the pressing step, the pair of pressure rollers applies heat and pressure to the supplied electrolyte membrane, the anode-coated first release paper, and the cathode-coated second release paper.