JP7104119B2 - Manufacturing method and processing mold of resin frame member for fuel cell - Google Patents

Description

The present invention relates to a method for manufacturing a resin frame member for a fuel cell and a processing mold.

The power generation cell is formed, for example, by sandwiching an electrolyte membrane / electrode structure with a resin frame (MEA with a resin frame) between a pair of separators. The MEA with a resin frame includes an electrolyte membrane / electrode structure (MEA) in which an anode electrode is provided on one surface of the electrolyte membrane and a cathode electrode is provided on the other surface of the electrolyte membrane, and an electrolyte membrane / electrode structure. It is provided with a square annular resin frame member provided on the outer peripheral portion of the above.

The inner peripheral end portion of the resin frame member is joined to the electrolyte membrane in a state where it orbits the outer peripheral portion of the MEA and is arranged between the outer peripheral portion of the anode electrode and the outer peripheral portion of the cathode electrode. In such a resin frame member, if the cross section of the inner peripheral end portion along the thickness direction is square, a gap (electrolyte film and electrode are separated from each other) in the inner peripheral end portion of the resin frame member. Part) is formed. In the MEA with a resin frame, the gap formed inward of the inner peripheral end portion of the resin frame member becomes a non-power generation portion. Therefore, the power generation efficiency of the power generation cell is lowered.

For example, Patent Document 1 discloses a MEA with a resin frame in which the inner gap of the inner peripheral end portion of the resin frame member is reduced. At the inner peripheral end of the resin frame member of the MEA with a resin frame, an inclined surface inclined inward from one surface of the resin frame member toward the other surface is formed.

Japanese Unexamined Patent Publication No. 2018-97917

The present invention has been made in connection with the above-mentioned prior art, and an object of the present invention is to provide a method for manufacturing a resin frame member for a fuel cell and a processing mold capable of efficiently forming an inclined surface.

In the first aspect of the present invention, an inclined surface is formed on each side of an inner peripheral end portion surrounding a square opening formed in the central portion of the resin film, thereby forming an inclined surface on the outer periphery of the electrolyte membrane / electrode structure. A method for manufacturing a resin frame member for a fuel cell for manufacturing a resin frame member provided in a portion, wherein the resin film is placed on a mounting surface of a lower mold, and after the mounting step described above, By moving the upper mold toward the lower mold and shearing each side portion between the lower processing portion of the lower mold and the upper processing portion of the upper mold, the inclined surface is formed on each side portion. In the processing step, each side portion is inclined downward inward while maintaining a predetermined clearance between the lower processing portion and the upper processing portion. A resin for a fuel cell, which is subjected to the shearing process in a state where at least a part of each side portion is positioned in the notch portion in which the corner portion on the lower processed portion side of the above-described mounting surface is cut out. This is a method for manufacturing a frame member.

A second aspect of the present invention is a processing mold used in the above-described method for manufacturing a resin frame member for a fuel cell, comprising the lower mold and the upper mold which are arranged so as to be close to each other so as to be separated from each other. On the upper surface of the lower mold, a quadrangular insertion port, a previously described mounting surface on which the resin film is placed so as to surround the insertion port, and an extension along the outer periphery of the insertion port. The lower processed portion having a square ring shape and the cutout portion obtained by cutting out the corner portion on the lower processed portion side of the above-mentioned mounting surface are provided, and the upper mold has a square-shaped upper processed portion. Has a punch formed so as to be insertable into the insertion slot, and the lower processing portion and the upper processing portion are formed when the upper mold is moved toward the lower mold. It is a processing mold provided so that each side portion can be sheared by the lower processing portion and the upper processing portion while maintaining the clearance between the side processing portion and the upper processing portion. ..

According to the present invention, each side is made into a notch portion of the lower mold so that each side portion inclines downward while maintaining a predetermined clearance between the lower processed portion and the upper processed portion. Shearing of each side can be performed with at least a part of the part positioned. As a result, the cut surface of each side portion cut by the upper processed portion and the lower processed portion becomes an inclined surface inclined with respect to the thickness direction of the resin frame member. Therefore, the inclined surface can be efficiently formed.

It is a partially omitted disassembled perspective view of the fuel cell stack having the resin frame member obtained by the method of manufacturing the resin frame member for a fuel cell which concerns on one Embodiment of this invention. It is sectional drawing along the line II-II of FIG. 3A is a perspective view of the resin frame member of FIG. 2, and FIG. 3B is a cross-sectional view taken along the line IIIB-IIIB of FIG. 3A. It is a flowchart which shows the manufacturing method of the resin frame member shown in FIG. 3A. It is a perspective view of the processing mold for manufacturing a resin frame member, and a resin film. It is explanatory drawing of the mounting process. FIG. 7A is a first explanatory view of the processing process, and FIG. 7B is a second explanatory view of the processing process. FIG. 8A is a third explanatory view of the processing process, and FIG. 8B is an explanatory view of a modified example of the punch. FIG. 9A is a first explanatory view of the pinching process, and FIG. 9B is a second explanatory view of the pinching process. It is sectional drawing which shows the deformation example of the support surface of the lower mold. It is a perspective view of the processing die and a resin film which concerns on a modification. 12A is a cross-sectional view taken along the line XIIA-XIIA of FIG. 11, and FIG. 12B is a cross-sectional view showing a modified example of the support surface of the lower mold of FIG. 12A. It is a flowchart which shows the manufacturing method of the processing die shown in FIG. It is a perspective view of the lower mold member.

Hereinafter, a method for manufacturing a resin frame member for a fuel cell and a processing mold according to the present invention will be described with reference to the accompanying drawings with reference to suitable embodiments.

As shown in FIGS. 1 and 2, a plurality of power generation cells 10 are stacked in the thickness direction (arrow A direction) to form a fuel cell stack 12. The fuel cell stack 12 is mounted on a fuel cell electric vehicle (not shown) as, for example, an in-vehicle fuel cell stack. The stacking direction of the plurality of power generation cells 10 may be either the horizontal direction or the gravity direction.

In FIG. 1, the power generation cell 10 is formed in a horizontally long rectangular shape. However, the power generation cell 10 may be formed in a vertically long rectangular shape. As shown in FIGS. 1 and 2, the power generation cell 10 is arranged on both sides of the electrolyte membrane / electrode structure with a resin frame (hereinafter referred to as “MEA14 with a resin frame”) and the MEA14 with a resin frame. A separator 16 and a second separator 18 are provided. The MEA 14 with a resin frame has an electrolyte membrane / electrode structure (hereinafter referred to as “MEA 20”) and a resin frame member 22 (resin frame portion) provided on the outer peripheral portion of the MEA 20.

In FIG. 2, the MEA 20 includes an electrolyte membrane 24, an anode electrode 26 (first electrode) provided on one surface 24a of the electrolyte membrane 24, and a cathode electrode 28 (first electrode) provided on the other surface 24b of the electrolyte membrane 24 (1). It has a second electrode). The electrolyte membrane 24 is, for example, a solid polymer electrolyte membrane (cation exchange membrane). The solid polyelectrolyte membrane is, for example, a thin film of perfluorosulfonic acid containing water. As the electrolyte membrane 24, an HC (hydrocarbon) -based electrolyte can be used in addition to the fluorine-based electrolyte. The electrolyte membrane 24 is sandwiched between the anode electrode 26 and the cathode electrode 28.

Although not shown in detail, the anode electrode 26 has a first electrode catalyst layer bonded to one surface 24a of the electrolyte membrane 24 and a first gas diffusion layer laminated on the first electrode catalyst layer. The first electrode catalyst layer is formed by uniformly coating the entire surface of the first gas diffusion layer with porous carbon particles on which a platinum alloy is supported on the surface.

The cathode electrode 28 has a second electrode catalyst layer bonded to the other surface 24b of the electrolyte membrane 24 and a second gas diffusion layer laminated on the second electrode catalyst layer. The second electrode catalyst layer is formed by uniformly coating the entire surface of the second gas diffusion layer with porous carbon particles on which a platinum alloy is supported on the surface. Each of the first gas diffusion layer and the second gas diffusion layer is made of carbon paper, carbon cloth or the like.

The planar dimension (external dimension) of the anode electrode 26 is larger than the planar dimension of the cathode electrode 28. The planar dimensions of the electrolyte membrane 24 are the same as the planar dimensions of the anode electrode 26. The outer peripheral end 26o of the anode electrode 26 is located outside the outer peripheral end 28o of the cathode electrode 28. In the plane direction of the electrolyte membrane 24 (direction of arrow C in FIG. 2), the outer peripheral end 24o of the electrolyte membrane 24 is at the same position as the outer peripheral end 26o of the anode electrode 26.

The planar dimension of the anode electrode 26 may be smaller than the planar dimension of the cathode electrode 28. In this case, the outer peripheral end 26o of the anode electrode 26 is located inward from the outer peripheral end 28o of the cathode electrode 28. The planar dimension of the electrolyte film 24 may be the same as the planar dimension of the anode electrode 26, or may be the same as the planar dimension of the cathode electrode 28. The planar dimension of the anode electrode 26 may be the same as the planar dimension of the cathode electrode 28. In this case, in the plane direction of the electrolyte membrane 24, the outer peripheral end 24o of the electrolyte membrane 24, the outer peripheral end 26o of the anode electrode 26, and the outer peripheral end 28o of the cathode electrode 28 are at the same positions.

The resin frame member 22 is a single frame-shaped sheet that orbits the outer peripheral portion of the MEA 20. The resin frame member 22 has an electrical insulating property. Examples of the constituent materials of the resin frame member 22 include PPS (polyphenylene sulfide), PPA (polyphthalamide), PEN (polyethylene naphthalate), PES (polyether sulfone), LCP (liquid crystal polymer), and PVDF (polyfluoropolymer). Vinylidene sulfide), silicone resin, fluororesin, m-PPE (modified polyphenylene ether resin), PET (polyethylene terephthalate), PBT (polybutylene terephthalate), modified polyolefin and the like. A detailed description of the resin frame member 22 will be described later.

In FIG. 1, each of the first separator 16 and the second separator 18 is formed in a rectangular shape (square shape). Each of the first separator 16 and the second separator 18 is formed by pressing and forming a corrugated cross section of, for example, a steel plate, a stainless steel plate, an aluminum plate, a plated steel plate, or a thin metal plate whose metal surface is surface-treated for corrosion protection. It is composed of. However, each of the first separator 16 and the second separator 18 may be made of carbon or the like. The first separator 16 and the second separator 18 are integrally joined by welding, brazing, caulking, or the like on the outer periphery in a state where they are overlapped with each other.

An oxidant gas inlet communication hole 30a, a cooling medium inlet communication hole 32a, and a fuel gas outlet communication hole 34b are provided at one end edge portion in the arrow B direction (end edge portion in the arrow B1 direction), which is the long side direction of the power generation cell 10. , Are arranged in the short side direction (arrow C direction) of the power generation cell 10. The oxidant gas inlet communication hole 30a supplies an oxidant gas (for example, an oxygen-containing gas) in the direction of arrow A. The cooling medium inlet communication hole 32a supplies a cooling medium (for example, pure water, ethylene glycol, oil, etc.) in the direction of arrow A. The fuel gas outlet communication hole 34b discharges fuel gas (for example, hydrogen-containing gas) in the direction of arrow A.

A fuel gas inlet communication hole 34a, a cooling medium outlet communication hole 32b, and an oxidizer gas outlet communication hole 30b are provided at the other end edge portion of the power generation cell 10 in the arrow B direction (end edge portion in the arrow B2 direction) in the arrow C direction. It is provided arranged in. The fuel gas inlet communication hole 34a supplies fuel gas in the direction of arrow A. The cooling medium outlet communication hole 32b discharges the cooling medium in the direction of arrow A. The oxidant gas outlet communication hole 30b discharges the oxidant gas in the direction of arrow A.

The size and position of the oxidizer gas inlet communication hole 30a, the oxidizer gas outlet communication hole 30b, the fuel gas inlet communication hole 34a, the fuel gas outlet communication hole 34b, the cooling medium inlet communication hole 32a, and the cooling medium outlet communication hole 32b, respectively. , Shape and number are not limited to this embodiment, and may be appropriately set according to the required specifications.

As shown in FIGS. 1 and 2, a fuel gas flow path 36 communicating with the fuel gas inlet communication hole 34a and the fuel gas outlet communication hole 34b is provided on the surface 16a of the first separator 16 toward the MEA20. The fuel gas flow path 36 has a plurality of fuel gas flow path grooves 38 extending in the direction of arrow B. Each fuel gas flow path groove 38 may extend in a wavy shape in the direction of arrow B.

In FIG. 1, the first separator 16 has a first seal portion 40 that prevents fluid (fuel gas, oxidant gas, and cooling medium) from leaking to the outside from between the MEA 14 with a resin frame and the first separator 16. It is provided. The first seal portion 40 goes around the outer peripheral portion of the first separator 16 and goes around each communication hole (oxidizing agent gas inlet communication hole 30a or the like). The first seal portion 40 extends linearly when viewed from the separator thickness direction (arrow A direction). However, the first seal portion 40 may extend in a wavy shape when viewed from the separator thickness direction.

In FIG. 2, the first seal portion 40 has a first metal bead portion 42 integrally molded with the first separator 16 and a first resin material 44 provided on the first metal bead portion 42. The first metal bead portion 42 projects from the first separator 16 toward the resin frame member 22. The cross-sectional shape of the first metal bead portion 42 is a trapezoidal shape that tapers in the protruding direction of the first metal bead portion 42. The first resin material 44 is an elastic member fixed to the protruding end face of the first metal bead portion 42 by printing or coating. The first resin material 44 is made of, for example, polyester fibers.

As shown in FIGS. 1 and 2, an oxidant gas flow path 46 communicating with the oxidant gas inlet communication hole 30a and the oxidant gas outlet communication hole 30b is provided on the surface 18a of the second separator 18 toward the MEA20. Be done. The oxidant gas flow path 46 has a plurality of oxidant gas flow path grooves 48 extending linearly in the direction of arrow B. Each oxidant gas flow path groove 48 may extend in a wavy shape in the direction of arrow B.

The second separator 18 is provided with a second seal portion 50 for preventing leakage of fluid (oxidizing agent gas, fuel gas and cooling medium) from between the MEA 14 with a resin frame and the second separator 18 to the outside. .. The second seal portion 50 goes around the outer peripheral portion of the second separator 18 and goes around each communication hole (oxidizing agent gas inlet communication hole 30a, etc.). The second seal portion 50 extends linearly when viewed from the separator thickness direction (arrow A direction). However, the second seal portion 50 may extend in a wavy shape when viewed from the separator thickness direction.

In FIG. 2, the second seal portion 50 has a second metal bead portion 52 integrally molded with the second separator 18 and a second resin material 54 provided on the second metal bead portion 52. The second metal bead portion 52 projects from the second separator 18 toward the resin frame member 22. The cross-sectional shape of the second metal bead portion 52 is a trapezoidal shape that tapers toward the protruding direction of the second metal bead portion 52. The second resin material 54 is an elastic member fixed to the protruding end face of the second metal bead portion 52 by printing or coating. The second resin material 54 is made of, for example, polyester fibers.

The first seal portion 40 and the second seal portion 50 are arranged so as to overlap each other when viewed from the separator thickness direction. Therefore, with the tightening load (compressive load) applied to the fuel cell stack 12, each of the first metal bead portion 42 and the second metal bead portion 52 is elastically deformed (compressively deformed). Further, in this state, the protruding end surface (first resin material 44) of the first sealing portion 40 comes into airtight and liquid-tight contact with one surface 22a of the resin frame member 22, and the protruding end surface (first resin material 44) of the second sealing portion 50. 2 The resin material 54) comes into airtight and liquid-tight contact with the other surface 22b of the resin frame member 22.

The first resin material 44 may be provided on one surface 22a of the resin frame member 22 instead of the first metal bead portion 42. The second resin material 54 may be provided on the other surface 22b of the resin frame member 22 instead of the second metal bead portion 52. Further, at least one of the first resin material 44 and the second resin material 54 may be omitted. The first seal portion 40 and the second seal portion 50 may be formed of an elastic rubber seal member instead of the metal bead seal as described above.

In FIGS. 1 and 2, between the surface 16b of the first separator 16 and the surface 18b of the second separator 18, the cooling medium flow path 56 communicating with the cooling medium inlet communication hole 32a and the cooling medium outlet communication hole 32b. Is provided. The cooling medium flow path 56 is formed by the back surface shape of the oxidant gas flow path 46 and the back surface shape of the fuel gas flow path 36.

As shown in FIGS. 1 and 3A, the resin frame member 22 is formed in a square ring shape. That is, in FIG. 3A, a square opening 60 is formed in the central portion of the resin frame member 22. Therefore, as shown in FIGS. 1 to 3A, the inner peripheral end portion 23 of the resin frame member 22 is formed in a square ring shape so as to orbit the outer peripheral portion of the MEA 20. The inner peripheral end portion 23 of the resin frame member 22 is a portion constituting the inner end 22i of the resin frame member 22 and a region in the vicinity thereof.

As shown in FIG. 2, the inner peripheral end portion 23 of the resin frame member 22 is arranged between the outer peripheral portion 27 of the anode electrode 26 and the outer peripheral portion 29 of the cathode electrode 28. Specifically, the inner peripheral end portion 23 of the resin frame member 22 is sandwiched between the outer peripheral portion 25 of the electrolyte membrane 24 and the outer peripheral portion 29 of the cathode electrode 28. The inner peripheral end portion 23 of the resin frame member 22 may be sandwiched between the outer peripheral portion 25 of the electrolyte membrane 24 and the outer peripheral portion 27 of the anode electrode 26.

In FIG. 3A, the inner peripheral end portion 23 of the resin frame member 22 includes four linear side portions 62 and four corner portions 64. As shown in FIGS. 2 and 3A, each side portion 62 is formed in a tapered shape toward the inside of the resin frame member 22. In other words, the thickness (dimension in the direction of arrow A) of each side portion 62 decreases toward the inside of the resin frame member 22. Each side portion 62 has a triangular cross section. That is, each side portion 62 has an inclined surface 66 inclined inward from one surface 22a of the resin frame member 22 toward the other surface 22b, and a pair of side surfaces 68 connected to both sides of the inclined surface 66 (FIG. 3A) and are formed. The inclined surface 66 is formed flat.

As shown in FIG. 2, the inclination angle θ of the inclined surface 66 (the angle formed by the other surface 22b of the resin frame member 22 and the inclined surface 66) is, for example, preferably 45 ° or less, and 15 ° or more and 30 ° or less. More preferably, about 20 ° is even more preferable. The tilt angle θ can be set as appropriate. At the four sides 62, the inclination angles θ are the same as each other. However, the inclination angles θ of the four side portions 62 may be different from each other.

The inclined surface 66 extends over the entire length of each side portion 62 (see FIG. 3A). However, the inclined surface 66 may be provided only on a part of each side portion 62 in the extending direction. The inclined surface 66 faces the other surface 24b of the electrolyte membrane 24. In other words, the inclined surface 66 is in close proximity to or in contact with the other surface 24b of the electrolyte membrane 24. Each side portion 62 is formed thin toward the inside. Therefore, the gap S formed inward of each side portion 62 is smaller than the case where the inclined surface 66 is not formed on each side portion 62 (when the cross section of each side portion 62 is square). ..

In FIG. 3A, each side surface 68 is connected to the end of the inclined surface 66 in the extending direction. In other words, each side surface 68 is located at the end of each side portion 62 in the extending direction. The corners 64 are formed by side surfaces 68 adjacent to each other. The angle formed by the two side surfaces 68 forming the corner portion 64 is approximately 90 °. Each side surface 68 is formed in a triangular shape. Each corner portion 64 projects toward one surface 22a of the resin frame member 22 with respect to the inclined surface 66. Between the side portion 62 and the corner portion 64 adjacent to each other in the inner peripheral end portion 23, the portion of one surface 22a of the resin frame member 22 located at the corner portion 64 (first plane portion 65) and the inclined surface 66. A step (side surface 68) is formed in. The first flat surface portion 65 of the corner portion 64 is flush with the portion (second flat surface portion 67) of one surface 22a of the resin frame member 22 located outside the inner peripheral end portion 23. There is.

As shown in FIGS. 3A and 3B, the thickness of each corner portion 64 is substantially constant from the inside of the resin frame member 22 to the inner end 22i of the resin frame member 22. Each corner 64 has a square cross section (rectangular shape) (see FIG. 3B). Each corner portion 64 is formed to be thicker than the portion (slope portion) of the inner peripheral end portion 23 on which the inclined surface 66 is formed. At each corner 64, one surface 22a of the resin frame member 22 and the other surface 22b of the resin frame member 22 extend in parallel with each other. That is, the inclined surface 66 is not formed on each corner portion 64.

As shown in FIG. 2, the outer peripheral portion 25 of the electrolyte membrane 24 is provided with a first inclined region 70a at a portion of the resin frame member 22 facing the inclined surface 66. In the electrolyte membrane 24, the surface 70b on the anode electrode 26 side located outside the first inclined region 70a is a cathode electrode more than the surface 70c on the anode electrode 26 side located inside the first inclined region 70a. It is farther from 28.

A second inclined region 72a is provided on the outer peripheral portion 27 of the anode electrode 26 at a portion of the electrolyte membrane 24 facing the first inclined region 70a. The second inclined region 72a extends substantially parallel to the first inclined region 70a. In the anode electrode 26, the surface 72b on the first separator 16 side located outside the second inclined region 72a is larger than the surface 72c on the first separator 16 side located inside the second inclined region 72a. It is farther from the cathode electrode 28.

The outer peripheral portion 29 of the cathode electrode 28 is provided with a third inclined region 74a at a position overlapping the inclined surface 66 of the resin frame member 22 in the thickness direction (arrow A direction) of the resin frame member 22. The third inclined region 74a is inclined toward the outer peripheral end 28o of the cathode electrode 28 on the side opposite to the side where the resin frame member 22 is located. In the cathode electrode 28, the surface 74b on the side of the second separator 18 located outside the third inclined region 74a is larger than the surface 74c on the side of the second separator 18 located inside the third inclined region 74a. It is farther away from the anode electrode 26.

Next, the operation of the fuel cell stack 12 including the power generation cell 10 according to the present embodiment will be described below.

As shown in FIG. 1, an oxidant gas such as an oxygen-containing gas is supplied to the oxidant gas inlet communication hole 30a, and a fuel gas such as a hydrogen-containing gas is supplied to the fuel gas inlet communication hole 34a. To. Further, a cooling medium such as pure water, ethylene glycol, or oil is supplied to the cooling medium inlet communication hole 32a.

Therefore, the oxidant gas is introduced into the oxidant gas flow path 46 of the second separator 18 from the oxidant gas inlet communication hole 30a, moves in the direction of arrow B, and is supplied to the cathode electrode 28 of the MEA 20. On the other hand, the fuel gas is introduced from the fuel gas inlet communication hole 34a into the fuel gas flow path 36 of the first separator 16. The fuel gas moves in the direction of arrow B along the fuel gas flow path 36 and is supplied to the anode electrode 26 of the MEA 20.

Therefore, in the MEA 20, the oxidant gas supplied to the cathode electrode 28 and the fuel gas supplied to the anode electrode 26 are consumed by the electrochemical reaction to generate electricity.

Next, in FIG. 1, the oxidant gas supplied to and consumed by the cathode electrode 28 is discharged in the direction of arrow A along the oxidant gas outlet communication hole 30b. Similarly, the fuel gas supplied to and consumed by the anode electrode 26 is discharged in the direction of arrow A along the fuel gas outlet communication hole 34b.

Further, the cooling medium supplied to the cooling medium inlet communication hole 32a is introduced into the cooling medium flow path 56 between the first separator 16 and the second separator 18 and then flows in the direction of arrow B. After cooling the MEA 20, this cooling medium is discharged from the cooling medium outlet communication hole 32b.

Next, a method for manufacturing the MEA14 with a resin frame according to the present embodiment will be described below.

First, the resin frame member 22 described above is manufactured. Specifically, as shown in FIG. 4, the method for manufacturing the resin frame member 22 includes a preparation step, a mounting step, a processing step, and a sandwiching step. As shown in FIG. 5, the resin frame member 22 is formed by processing the resin film 100 with the processing mold 200.

As shown in FIG. 5, the processing die 200 includes a lower die 202 and an upper die 204 arranged so as to be close to each other and separated from each other. The lower mold 202 is a die having a square insertion port 206 (opening) formed on the upper surface thereof. The lower mold 202 is formed in a square ring shape when viewed from the upper surface. On the upper surface of the lower mold 202, a square annular mounting surface 208 for mounting the resin film 100 and an inner end of the upper surface of the lower mold 202 are located (extending along the outer periphery of the insertion port 206). A lower processing portion 210 (lower blade) is provided. The inner peripheral angle portion (corner portion on the lower processed portion 210 side) of the mounting surface 208 is provided with four notched portions 212 extending along each side of the lower processed portion 210. The cutout portion 212 is formed by, for example, C chamfering. In this case, the C chamfer is preferably set to C0.5 or more and C2 or less.

In other words, on the upper surface of the lower mold 202, four support surfaces 214 inclined downward from the mounting surface 208 toward the lower processed portion 210 are formed in the portion where the notch portion 212 is located. Each support surface 214 extends over the entire length of each side of the lower processed portion 210. Each support surface 214 is a flat surface 216a. The width dimension and the inclination angle (the angle formed by the line parallel to the mounting surface 208 and the inclined surface 66) of each support surface 214 are appropriately set according to the material, thickness, and the like of the resin film 100. The corner portions 218 having a square cross section are located between the support surfaces 214 adjacent to each other.

The upper mold 204 has an upper mold main body 220 provided so as to be movable in the vertical direction, and a punch 222 protruding downward from the lower surface of the upper mold main body 220. The punch 222 is formed in a rectangular cuboid shape. The punch 222 is inserted into the insertion port 206 of the lower mold 202 when the upper mold 204 is moved downward with respect to the lower mold 202.

A square upper processing portion 224 (upper blade) is provided at the outer peripheral end of the protruding end surface of the punch 222. The upper processed portion 224 is formed to be one size smaller than the lower processed portion 210. That is, as shown in FIG. 7A, when the punch 222 is inserted into the insertion port 206, a predetermined clearance CL is formed between the upper processing portion 224 and the lower processing portion 210. The clearance CL is set within the range of 10 μm or more and 60 μm or less. The size of the clearance CL is appropriately set according to the material and thickness of the resin film 100.

In the method for manufacturing the resin frame member 22, first, a preparation step (step S1 in FIG. 4) is performed. In the preparatory step, the square annular resin film 100 shown in FIG. 5 is produced. The resin film 100 is formed in a horizontally long rectangular shape. A square opening 60 is formed in the central portion of the resin film 100. That is, the resin film 100 is formed in a square ring shape. The inner peripheral end portion 102 of the resin film 100 has four side portions 104 and four corner portions 106.

An oxidant gas inlet communication hole 30a, a cooling medium inlet communication hole 32a, and a fuel gas outlet communication hole 34b are formed at one end edge of the resin film 100 in the long side direction. A fuel gas inlet communication hole 34a, a cooling medium outlet communication hole 32b, and an oxidant gas outlet communication hole 30b are formed at the other end edge of the resin film 100 in the longitudinal direction.

When the preparation step is completed, the mounting step (step S2 in FIG. 4) is performed. In the mounting step, as shown in FIGS. 5 to 7A, the other surface 100b is placed on the mounting surface 208 of the lower mold 202 with one surface 100a of the resin film 100 facing upward. The processing mold 200 includes a positioning mechanism (not shown) for positioning the resin film 100 on the lower mold 202. The positioning mechanism is, for example, a knock pin provided in the lower mold 202, in which case the knock pin is inserted into a positioning hole (not shown) formed in the resin film 100. At this time, in FIG. 6, the center of the resin film 100 is positioned at the center of the upper surface of the lower mold 202.

The opening 60 of the resin film 100 is one size smaller than the insertion port 206 of the lower mold 202. Therefore, the inner peripheral end 102 of the resin film 100 is located inside the lower processed portion 210 of the lower mold 202. In other words, at least a part of each side portion 104 of the inner peripheral end portion 102 of the resin film 100 is located in the cutout portion 212 of the lower mold 202 (see FIG. 7A). That is, the inner end 104i of each side portion 104 is located inside the lower processing portion 210.

When the mounting step is completed, the processing step (step S3 in FIG. 4) is performed. In the processing step, as shown in FIGS. 7A to 8A, the upper mold 204 is moved toward the lower mold 202, and the lower processing portion 210 and the upper processing portion 224 form each of the inner peripheral end portions 102 of the resin film 100. By shearing the side portions 104, inclined surfaces 66 are formed on each side portion 104 of the resin film 100. At this time, one surface 100a of the resin film 100 may be pressed against the mounting surface 208 by a pressing member (not shown).

When the upper mold 204 is lowered, as shown in FIG. 7B, the upper processed portion 224 comes into contact with one surface 100a of the resin film 100, and the resin film 100 is pushed downward. At this time, the other surface 100b of the resin film 100 contacts the support surface 214 and the lower processed portion 210. That is, at least a part of each side portion 104 of the resin film 100 is located at the cutout portion 212. Therefore, each side portion 104 is inclined downward toward the inward side. Further, the inner end 104i of each side portion 104 of the resin film 100 faces downward. Further, a predetermined clearance CL is maintained between the lower processing portion 210 and the upper processing portion 224.

Then, when the upper mold 204 is further lowered, as shown in FIG. 8A, each side portion 104 of the resin film 100 is sheared by the upper processing portion 224. At this time, the upper processing portion 224 cuts each side portion 104 of the resin film 100 in a direction intersecting the thickness direction of each side portion 104.

That is, the cutting length L of the resin film 100 by the upper processed portion 224 is longer than the thickness dimension of the resin film 100. The cut surface 110 of the resin film 100 cut by the upper processed portion 224 is the inclined surface 66 described above. As a result, the resin frame member 22 described above is formed. Regarding the structure of the inclination of the support surface 214 and the clearance CL, the inclination angle θ (see FIG. 2) of the inclined surface 66 is preferably within the above-mentioned range (preferably 45 ° or more, more preferably 15 ° or more and 30 ° or less, and about 20 °. It is set to be even more preferable).

As shown in FIG. 8B, the lower surface of the punch 222 may be inclined upward in a direction away from the upper processed portion 224. That is, the angle α formed by the lower surface of the punch 222 and the horizontal plane may be formed at an acute angle.

After the processing step, as shown in FIG. 9A, when the inner peripheral end portion 23 of the resin frame member 22 is curved toward the other surface 22b of the resin frame member 22 with respect to the outer peripheral portion 31, if necessary, The sandwiching step (step S4 in FIG. 4) may be performed. In the sandwiching step, as shown in FIGS. 9A and 9B, the resin frame member 22 obtained in the processing step is sandwiched and pressed by the planes 250a and 252a of the pair of press members 250 and 252. As a result, the inner peripheral end portion 23 and the outer peripheral portion 31 of the resin frame member 22 can be straightened into the same plane shape.

After the production of the resin frame member 22 is completed, the anode electrode 26 provided with the electrolyte membrane 24 and the cathode electrode 28 are prepared. Then, the inner peripheral end portion 23 of the resin frame member 22 is arranged between the outer peripheral portion 25 of the electrolyte membrane 24 and the outer peripheral portion 29 of the cathode electrode 28 and joined to each other. Specifically, the anode electrodes 26, the electrolyte membrane 24, the resin frame member 22, and the cathode electrodes 28, which are stacked in the thickness direction, are heated and a load is applied (hot press) to join them. As a result, MEA14 with a resin frame can be obtained. An adhesive may be applied between the electrolyte membrane 24 and the resin frame member 22.

The method for manufacturing the processing mold 200 and the resin frame member 22 according to the present embodiment has the following effects.

The method of manufacturing the resin frame member 22 (the method of using the processing mold 200) is as follows: a mounting step of mounting the resin film 100 on the mounting surface 208 of the lower mold 202, and a mounting step of placing the upper mold 204 below. By moving toward the mold 202 and shearing each side portion 104 between the lower processing portion 210 of the lower mold 202 and the upper processing portion 224 of the upper mold 204, an inclined surface 66 is formed on each side portion 104. Including the processing process to be performed.

In the machining step, the lower side of the mounting surface 208 is such that each side portion 104 is inclined downward inward while maintaining a predetermined clearance CL between the lower machining portion 210 and the upper machining portion 224. Shearing is performed in a state where at least a part of each side portion 104 is positioned in the cutout portion 212 in which the corner portion on the processed portion 210 side is cut out.

According to such a method, the lower mold 202 is such that each side portion 104 is inclined downward inward while maintaining a predetermined clearance CL between the lower processing portion 210 and the upper processing portion 224. Each side portion 104 is sheared with at least a part of each side portion 104 positioned in the notch portion 212 of the above and the inner surface of each side portion 104 facing downward. As a result, the cut surface 110 of each side portion 104 cut by the upper processed portion 224 and the lower processed portion 210 becomes an inclined surface 66 inclined with respect to the thickness direction of the resin frame member 22. Therefore, the inclined surface 66 can be efficiently formed.

The lower mold 202 is formed with a support surface 214 inclined downward from the mounting surface 208 toward the lower processed portion 210 at a portion where the notch portion 212 is located, and the support surface 214 is a flat surface 216a. .. In the processing process, each side portion 104 is brought into contact with the support surface 214.

According to such a method, the inclined surface 66 can be accurately formed on each side portion 104 of the resin film 100 by the upper processed portion 224.

The clearance CL is set within the range of 10 μm or more and 60 μm or less.

In this case, the inclined surface 66 can be accurately formed on each side portion 104 of the resin film 100 while reducing the sagging and burrs of the cut surface 110 of the resin film 100.

Further, in the processing mold 200, on the upper surface of the lower mold 202, a square insertion port 206, a mounting surface 208 on which the resin film 100 is placed so as to surround the insertion port 206, and an insertion port 206. A square annular lower processed portion 210 extending along the outer periphery of the surface and a notched portion 212 having a corner portion of the lower processed portion 210 on the mounting surface 208 are provided. The upper mold 204 has a punch 222 in which a square upper processed portion 224 is formed and the punch 222 is formed so as to be insertable into the insertion port 206. The lower processing portion 210 and the upper processing portion 224 maintain a predetermined clearance between the lower processing portion 210 and the upper processing portion 224 when the upper mold 204 is moved toward the lower mold 202. The lower processing portion 210 and the upper processing portion 224 are provided so that each side portion 104 can be sheared.

According to such a processing mold 200, the same operation and effect as the method for manufacturing the resin frame member 22 as described above can be obtained.

The cutout portion 212 of the lower mold 202 may be formed by, for example, R chamfering. In this case, the R chamfer is preferably set to R0.3 or more and R2 or less. Further, as shown in FIG. 10, the support surface 214 of the lower mold 202 is formed on the convex R surface 216b (convex curved surface). Even in this case, the same effect as that of the flat surface 216a described above is obtained.

(Modification example)
Next, the processing mold 200a and the manufacturing method of the processing mold 200a according to the modified example will be described. In this modification, the same reference numerals are given to the same configurations as the above-mentioned processing mold 200, and detailed description thereof will be omitted.

As shown in FIG. 11, the processing die 200a includes a lower die 202a and an upper die 204. The lower mold 202a has a lower mold member 203 having an insertion port 206 formed on the upper surface thereof. A square annular recess 230 (see FIG. 12A) formed along the outer circumference of the insertion port 206 is formed on the upper surface of the lower mold member 203. The inner surface of the recess 230 is coated with a covering member 232 (coating member). Further, a mounting surface 208 is provided on the upper surface of the lower mold member 203.

In FIG. 12A, the recess 230 communicates with the insertion slot 206. The recess 230 is formed by a first inner surface 231a and a second inner surface 231b. The first inner surface 231a extends substantially parallel to the mounting surface 208. The second inner surface 231b extends upward from the first inner surface 231a. The first inner surface 231a and the second inner surface 231b intersect at a right angle. However, the angle formed by the first inner surface 231a and the second inner surface 231b can be appropriately set. The four corners of the recess 230 are formed in an R shape (arc shape) when viewed from above (see FIG. 11).

As a constituent material of the covering member 232, a metal material, a ceramic material, or the like is used. Examples of the metal material include cemented carbide such as tungsten carbide (WC) and pure tungsten. Examples of the ceramic material include aluminum oxide (Al ₂ O ₃ ), silicon carbide (SiC), zirconium dioxide (ZrO ₂ ) and the like.

The thickness D (film thickness) of the covering member 232 is the same as the height dimension of the second inner surface 231b (depth dimension of the recess 230). The thickness D of the covering member 232 is preferably set to 100 μm or more and 300 μm or less. The covering member 232 extends in a square ring shape. The covering member 232 is provided so as to fill a part of the recess 230. That is, the portion of the recess 230 that is not filled with the covering member 232 is left as the cutout portion 212.

The covering member 232 is provided with a lower processed portion 210 and a support surface 214. In other words, each of the support surface 214 and the lower processed portion 210 is formed by coating the inner surface (first inner surface 231a and second inner surface 231b) of the recess 230 with the covering member 232. That is, the covering member 232 is coated on the inner surface (first inner surface 231a and second inner surface 231b) of the recess 230 so that the support surface 214 and the lower processed portion 210 are formed. Each support surface 214 is a flat surface 216a. However, each support surface 214 may be a convex R surface 216b (see FIG. 12B).

In FIG. 11, the lower processed portion 210 and the support surface 214 extend linearly along the outer circumference of the insertion port 206. A corner portion 234 having a square cross section is provided between the support surfaces 214 adjacent to each other. Each corner portion 234 of the covering member 232 has an R-shaped (arc-shaped) outer peripheral surface.

Next, the method for manufacturing the processing mold 200a described above will be described. As shown in FIG. 13, the method for manufacturing the processing mold 200a includes a lower mold member preparation step and a coating step.

In the lower mold member preparation step (step S10 in FIG. 13), the lower mold member 203 is prepared as shown in FIG. Specifically, the lower mold member 203 is formed in a rectangular cuboid shape. On the upper surface of the lower mold member 203, there are a square insertion port 206, a mounting surface 208 on which the resin film 100 (see FIG. 11) is placed so as to surround the insertion port 206, and the insertion port 206. A square annular recess 230 that communicates with the concave portion 230 is formed.

Subsequently, in the coating step (step S11 in FIG. 13), the coating member 232 is coated on the first inner surface 231a and the second inner surface 231b of the recess 230, so that the coating member 232 is provided with the lower processed portion 210 and the support surface 214. To form. At this time, as shown in FIG. 11, the covering member 232 is coated in a square ring shape over the entire first inner surface 231a and the second inner surface 231b. In FIGS. 11 and 12A, the upper surface 233a of the covering member 232 is smoothly connected to the mounting surface 208 without a step. The inner surface 233b (the surface located on the insertion port 206 side) of the covering member 232 is smoothly connected to the inner surface 206a forming the insertion port 206 of the lower mold member 203 (FIG. 12A).

In this modification, in the coating step, the coating member 232 is coated on the first inner surface 231a and the second inner surface 231b of the recess 230 by thermal spraying. In this case, either the metal material or the ceramic material described above can be used as the constituent material of the covering member 232.

The coating process is not limited to thermal spray coating. In the coating step, the covering member 232 may be coated on the first inner surface 231a and the second inner surface 231b of the recess 230 by overlaying. In this case, the above-mentioned metal material is used as the constituent material of the covering member 232.

The processing mold 200a according to this modification has the same effect as the processing mold 200 described above.

In the processing die 200a according to this modification, a square annular recess 230 is formed on the upper surface of the lower die 202a along the outer circumference of the insertion port 206. The first inner surface 231a and the second inner surface 231b of the recess 230 are coated with a covering member 232, and each of the support surface 214 and the lower processed portion 210 is provided on the covering member 232.

Further, the method for manufacturing the processing mold 200a according to this modification includes a lower mold member preparation step and a coating step. In the lower mold member preparation step, the square insertion port 206, the mounting surface 208 on which the resin film 100 is placed so as to surround the insertion port 206, and the insertion port 206 extend along the outer periphery of the insertion port 206. A lower mold member 203 having a square annular recess 230 formed on the upper surface thereof is prepared. In the coating step, after the lower mold member preparation step, the first inner surface 231a and the second inner surface 231b of the recess 230 are coated with the covering member 232 to form the lower processed portion 210 located along the outer periphery of the insertion port 206. Is formed on the covering member 232. In the coating step, the covering member 232 is coated on the first inner surface 231a and the second inner surface 231b of the recess 230 so that the cutout portion 212 is provided at the corner portion of the lower processed portion 210 on the mounting surface 208.

By the way, when the cutout portion 212 is formed by cutting the inner end of the lower mold member 203 on the side where the insertion port 206 is located, a great deal of time and cost are required. However, according to such a configuration and method, since the cutout portion 212 and the lower processed portion 210 are provided by coating the covering member 232, the cutout portion 212 and the lower processed portion 210 are provided with respect to the lower mold member 203. The time and cost for manufacturing the lower mold 202a can be reduced as compared with the case where the lower mold 202a is formed by cutting.

In the coating step, by coating the first inner surface 231a and the second inner surface 231b of the recess 230 with the covering member 232, the supporting surface 214 inclined downward from the mounting surface 208 toward the lower processed portion 210 is covered with the covering member 232. To form.

According to such a method, the support surface 214 can be easily and accurately formed on the lower mold 202a.

The covering member 232 is made of a metal material containing tungsten or a ceramic material.

According to such a configuration, the durability of the support surface 214 and the lower processed portion 210 can be improved.

In the method for manufacturing the processing mold 200a, in the coating step, the coating member 232 is coated on the first inner surface 231a and the second inner surface 231b of the recess 230 by thermal spraying.

According to such a method, the support surface 214 and the lower processed portion 210 can be formed easily and accurately.

In the coating step, the covering member 232 is coated on the first inner surface 231a and the second inner surface 231b of the recess 230 by overlaying.

According to such a method, the support surface 214 and the lower processed portion 210 can be formed easily and accurately.

The present invention is not limited to the above-described embodiment, and various modifications can be made without departing from the gist of the present invention.

The above embodiments can be summarized as follows.

In the above embodiment, inclined surfaces (66) are formed on each side portion (104) of the inner peripheral end portion (102) surrounding the rectangular opening (60) formed in the central portion of the resin film (100). This is a method for manufacturing a resin frame member for a fuel cell for manufacturing a resin frame member (22) provided on the outer peripheral portion of the electrolyte membrane / electrode structure (20), wherein the resin film is used as a lower mold (202, 202a). After the mounting step of mounting on the mounting surface (208) of ) And the upper processing portion (224) of the upper mold include a processing step of forming the inclined surface on each side portion by performing shearing processing of each side portion. While maintaining a predetermined clearance (CL) between the lower processed portion and the upper processed portion, the lower processed portion on the above-mentioned mounting surface so that each side portion inclines downward inward. A method for manufacturing a resin frame member for a fuel cell, which performs the shearing process in a state where at least a part of each of the side portions is positioned in the cutout portion (212) in which the corner portion on the side is cut out, is disclosed. ..

In the method for manufacturing a resin frame member for a fuel cell, the lower mold has a support surface (214) inclined downward from the above-described mounting surface toward the lower processed portion in a portion where the notch portion is located. ) Is formed, and the support surface is a flat surface (216a) or a convex R surface (216b). In the processing step, each side portion may be brought into contact with the support surface.

In the above method for manufacturing a resin frame member for a fuel cell, the clearance may be set within the range of 10 μm or more and 60 μm or less.

The embodiment is a processing die (200, 200a) used in the above-described method for manufacturing a resin frame member for a fuel cell, and includes the lower die and the upper die arranged so as to be close to each other and separated from each other. On the upper surface of the lower mold, a quadrangular insertion port (206), a previously described mounting surface on which the resin film is placed so as to surround the insertion port, and an outer periphery of the insertion port. The lower processed portion having a square ring shape extending from the front and the notched portion notched at the corner portion on the lower processed portion side of the above-mentioned mounting surface are provided, and the upper mold has a quadrangular shape. The upper processed portion has a punch (222) formed so as to be inserted into the insertion port, and the lower processed portion and the upper processed portion have the upper die directed toward the lower die. When the lower processing portion and the upper processing portion are moved, the lower processing portion and the upper processing portion are provided so that each side portion can be sheared while maintaining the clearance between the lower processing portion and the upper processing portion. The processing mold is disclosed.

In the above-mentioned processing mold, the lower mold is formed with a support surface inclined downward from the above-described mounting surface toward the lower processing portion at a portion where the notch portion is located, and the support surface is formed on the support surface. It may be a flat surface or a convex R surface.

In the above processing mold, a square annular recess (230) is formed on the upper surface of the lower mold along the outer circumference of the insertion port, and the inner surface of the recess is coated with a covering member (232). The support surface and the lower processed portion may be provided on the covering member.

In the above processing mold, the covering member may be made of a metal material containing tungsten or a ceramic material.

The above embodiment is provided on the outer peripheral portion of the electrolyte membrane / electrode structure by forming inclined surfaces on each side of the inner peripheral end portion surrounding the square opening formed in the central portion of the resin film. It is a processing type manufacturing method for manufacturing a resin frame member to be manufactured, that is, a quadrangular insertion port, a mounting surface on which the resin film is placed so as to surround the insertion port, and the insertion. A lower mold member preparation step for preparing a lower mold member (203) having a square annular recess extending along the outer periphery of the mouth and a lower mold member (203) formed on the upper surface, and the recess after the lower mold member preparation step. The coating step includes a coating step of forming a lower processed portion located along the outer periphery of the insertion port on the covering member by coating the inner surface of the covering member, and the coating step includes the step of forming the lower processed portion on the mounting surface described above. A method for manufacturing a processing mold is disclosed in which the coating member is coated on the inner surface of the recess so that a notch is provided at a corner on the lower processing portion side.

In the above-mentioned processing mold manufacturing method, in the coating step, by coating the inner surface of the recess with the covering member, a support surface inclined downward from the above-mentioned mounting surface toward the lower processed portion is described. It may be formed on a covering member.

In the above-mentioned processing mold manufacturing method, in the coating step, the coating member may be coated on the inner surface of the recess by thermal spraying.

In the above-mentioned processing mold manufacturing method, in the coating step, the covering member may be coated on the inner surface of the recess by overlaying.

20 ... MEA (electrolyte membrane / electrode structure)
60 ... Opening 66 ... Inclined surface 100 ... Resin film 102 ... Inner peripheral end 104 ... Sides 200, 200a ... Machining molds 202, 202a ... Lower mold 203 ... Lower mold member 204 ... Upper mold 206 ... Insertion port 208 ... Placement surface 210 ... Lower processed portion 212 ... Notched portion 214 ... Support surface 216a ... Flat surface 216b ... Convex R surface 224 ... Upper processed portion 230 ... Recessed portion 231a ... First inner surface 231b ... Second inner surface 232 ... Covering member CL …clearance

Claims (7)

By forming inclined surfaces on each side of the inner peripheral end portion surrounding the square opening formed in the central portion of the resin film, a resin frame member provided on the outer peripheral portion of the electrolyte film / electrode structure is manufactured. This is a method for manufacturing resin frame members for fuel cells.
The mounting step of mounting the resin film on the mounting surface of the lower mold, and
After the above-described setting step, the upper die is moved toward the lower die, and the lower machining portion of the lower die and the upper machining portion of the upper die perform shearing of each side portion. Including a processing step of forming the inclined surface on each side portion,
In the processing step, while maintaining a predetermined clearance between the lower processing portion and the upper processing portion, the lower portion on the above-mentioned mounting surface so that each side portion inclines downward inward. A method for manufacturing a resin frame member for a fuel cell, wherein the shearing process is performed in a state where at least a part of each side portion is positioned in the notch portion in which the corner portion on the side processed portion side is cut out. The method for manufacturing a resin frame member for a fuel cell according to claim 1.
In the lower mold, a support surface inclined downward from the previously described mounting surface toward the lower processed portion is formed in a portion where the notch portion is located.
The support surface is a flat surface or a convex R surface, and is
In the processing step, a method for manufacturing a resin frame member for a fuel cell, in which each side portion is brought into contact with the support surface. The method for manufacturing a resin frame member for a fuel cell according to claim 1 or 2.
A method for manufacturing a resin frame member for a fuel cell, wherein the clearance is set within a range of 10 μm or more and 60 μm or less. A processing mold used in the method for manufacturing a resin frame member for a fuel cell according to any one of claims 1 to 3.
The lower mold and the upper mold are arranged so as to be close to each other and separated from each other.
On the upper surface of the lower mold,
With a square insertion slot,
The previously described surface on which the resin film is placed so as to surround the insertion slot, and
The lower processing portion of the square ring extending along the outer circumference of the insertion port, and the lower processing portion.
The cutout portion is provided by cutting out the corner portion on the lower processed portion side of the above-mentioned mounting surface.
The upper mold has a punch formed so that the upper processed portion having a square shape is formed and can be inserted into the insertion port.
The lower processing portion and the upper processing portion are in a state where the clearance between the lower processing portion and the upper processing portion is maintained when the upper mold is moved toward the lower mold. A processing mold provided so that each side portion can be sheared at the lower processing portion and the upper processing portion. The processing type according to claim 4.
In the lower mold, a support surface inclined downward from the previously described mounting surface toward the lower processed portion is formed in a portion where the notch portion is located.
The support surface is a processing type that is a flat surface or a convex R surface. The processing type according to claim 5.
A square annular recess is formed on the upper surface of the lower mold along the outer circumference of the insertion port.
The inner surface of the recess is coated with a covering member.
The support surface and the lower processed portion are processed molds provided on the covering member. The processing type according to claim 6.
The coating member is a processing mold made of a metal material containing tungsten or a ceramic material.

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