WO2005086267A1 - Separator for fuel cell, manufacturing method thereof, and fuel cell having such a separator - Google Patents

Separator for fuel cell, manufacturing method thereof, and fuel cell having such a separator Download PDF

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Publication number
WO2005086267A1
WO2005086267A1 PCT/KR2004/001950 KR2004001950W WO2005086267A1 WO 2005086267 A1 WO2005086267 A1 WO 2005086267A1 KR 2004001950 W KR2004001950 W KR 2004001950W WO 2005086267 A1 WO2005086267 A1 WO 2005086267A1
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WO
WIPO (PCT)
Prior art keywords
fuel cell
separator
graphite foil
flow field
forming
Prior art date
Application number
PCT/KR2004/001950
Other languages
French (fr)
Inventor
Ho-Suk Kim
Byung-Sun Hong
Mee-Nam Shinn
Original Assignee
Fuelcell Power, Inc.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Fuelcell Power, Inc. filed Critical Fuelcell Power, Inc.
Priority to JP2007502697A priority Critical patent/JP4971972B2/en
Priority to US10/598,729 priority patent/US8865372B2/en
Priority to EP04748506.5A priority patent/EP1723688B1/en
Publication of WO2005086267A1 publication Critical patent/WO2005086267A1/en
Priority to US14/487,212 priority patent/US10109865B2/en
Priority to US16/139,429 priority patent/US10998557B2/en

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Classifications

    • HELECTRICITY
    • H02GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
    • H02JCIRCUIT ARRANGEMENTS OR SYSTEMS FOR SUPPLYING OR DISTRIBUTING ELECTRIC POWER; SYSTEMS FOR STORING ELECTRIC ENERGY
    • H02J7/00Circuit arrangements for charging or depolarising batteries or for supplying loads from batteries
    • H02J7/0042Circuit arrangements for charging or depolarising batteries or for supplying loads from batteries characterised by the mechanical construction
    • H02J7/0044Circuit arrangements for charging or depolarising batteries or for supplying loads from batteries characterised by the mechanical construction specially adapted for holding portable devices containing batteries
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/02Details
    • H01M8/0202Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204Non-porous and characterised by the material
    • H01M8/0213Gas-impermeable carbon-containing materials
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M50/00Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/40Separators; Membranes; Diaphragms; Spacing elements inside cells
    • H01M50/403Manufacturing processes of separators, membranes or diaphragms
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/02Details
    • H01M8/0202Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204Non-porous and characterised by the material
    • H01M8/0206Metals or alloys
    • H01M8/0208Alloys
    • H01M8/021Alloys based on iron
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/02Details
    • H01M8/0202Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204Non-porous and characterised by the material
    • H01M8/0223Composites
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/02Details
    • H01M8/0202Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0204Non-porous and characterised by the material
    • H01M8/0223Composites
    • H01M8/0228Composites in the form of layered or coated products
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/02Details
    • H01M8/0202Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0258Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/02Details
    • H01M8/0202Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0258Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
    • H01M8/026Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant characterised by grooves, e.g. their pitch or depth
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/02Details
    • H01M8/0202Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/0258Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
    • H01M8/0263Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant having meandering or serpentine paths
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/02Details
    • H01M8/0271Sealing or supporting means around electrodes, matrices or membranes
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/02Details
    • H01M8/0271Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0273Sealing or supporting means around electrodes, matrices or membranes with sealing or supporting means in the form of a frame
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/24Grouping of fuel cells, e.g. stacking of fuel cells
    • H01M8/2465Details of groupings of fuel cells
    • H01M8/2483Details of groupings of fuel cells characterised by internal manifolds
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/02Details
    • H01M8/0271Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/0286Processes for forming seals
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/10Fuel cells with solid electrolytes
    • H01M8/1009Fuel cells with solid electrolytes with one of the reactants being liquid, solid or liquid-charged
    • H01M8/1011Direct alcohol fuel cells [DAFC], e.g. direct methanol fuel cells [DMFC]
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10Energy storage using batteries
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30Hydrogen technology
    • Y02E60/50Fuel cells
    • YGENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50Manufacturing or production processes characterised by the final manufactured product

Definitions

  • the present invention relates to a fuel cell. More
  • the present invention relates to a separator for a fuel cell using a
  • the anode and the cathode are formed with a catalyst layer having platinum or
  • fuel gas for example, hydrogen
  • a fuel cell stack is
  • the water formed at the cathode is usually formed as vapor or liquid
  • FIG. 1 is a schematic sectional view of an exemplary fuel cell stack
  • a fuel cell stack is formed by stacking a plurality of unit cells
  • Such a unit cell 100 includes a proton exchange membrane 110 (for
  • proton exchange membrane 110 and electrodes 121 and 122 form a
  • MEA membrane electrode assembly
  • layers 125 are formed to the exterior of the electrodes 121 and 122 of the
  • MEA 130 MEA 130. MEAs 130 of adjacent unit cells are separated and supported by a
  • the separator 150 is formed with a flow field 151 for
  • fuel gas e.g., hydrogen, or methanol in the case of a direct
  • the separator 150 is also formed
  • a gasket 160 is applied between the
  • the unit cells 100 including the MEA 130, the separator 150, and the gasket 160 are stacked in series to form a high voltage.
  • cells are conjoined by, e.g., current collectors and end plates 170 disposed
  • reaction gases i.e., fuel gas and reduction gas
  • the fuel cell stack separates a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g., hydrogen or methanol) and a fuel gas (e.g.,
  • reduction gas e.g., oxygen or air
  • the separator has a heat exhaust structure for
  • the polymer electrolyte membrane should be hydrated to contain
  • polymer electrolyte membrane is excessively hydrated, small pores forming a
  • patent No. 4,988,583 have serpentine flow fields for fuel and reduction gases. This is mainly for utilizing a pressure drop along the flow fields for efficient exhaust of water formed at the cathodes.
  • the water formed at the cathodes is in the form of vapor, near the entry of reduction gas flow-field channel.
  • it becomes of two phased, as mixed liquid and vapor.
  • liquefied water drops fill the pores of the cathodes, and accordingly, the effective active areas of the catalyst layers become reduced.
  • liquefied water requires a high pressure of reduction gas for exhaust thereof.
  • thermosetting or thermoplastic resin is usually added to the separator
  • the separator and also for easy forming during the molding process.
  • the resin included in the separator causes an increase of volume resistance with respect to movement of electrons, and thereby deteriorates
  • Patent Publication No. EP1253657A1 discloses a method in which rib
  • present invention is a separator for a fuel cell that is capable of closely
  • the separator comprises a
  • the lamellar structure graphite foil may include a stainless steel layer therewithin.
  • the stainless steel layer is exteriorly exposed, interposing the hydrophobic layer.
  • the graphite foil is substantially free from thermosetting or thermoplastic resin.
  • a bulk density of the graphite foil preferably lies in the range of
  • a thickness of the graphite foil preferably lies in the range of 0.5mm to 3mm.
  • a thickness of the hydrophobic layer preferably lies in the range of 30 ⁇ m to 100 ⁇ m. It is preferable that at least one manifold is formed in the separator, and a sealing member is unified to the separator along each circumference of the at least one manifold and an area for contacting the fluid diffusion layer. It is preferable that the sealing member encloses, respectively along a closed curve, each of the at least one manifold and the area for contacting the fluid diffusion layer.
  • a method for manufacturing a separator according to the present invention is a method for manufacturing a separator for a fuel cell that is capable of closely contacting either an anode or a cathode of an MEA
  • the method includes: preparing a graphite foil of a predetermined size; forming a mask pattern on the graphite foil corresponding to the flow field channel; forming the flow field channel on the graphite foil by etching the graphite foil formed with the mask pattern thereon; forming a hydrophobic layer on an interior side of the flow field channel by impregnation; and removing the mask pattern from the graphite foil.
  • the forming of a mask pattern on the graphite foil includes: coating the graphite foil with a dry film resist; exposing the coated graphite foil; and developing the dry film resist on the graphite foil by moving a spray nozzle of a spray-type developing apparatus thereover.
  • the forming of a mask pattern on the graphite foil includes attaching a mask on the graphite foil, the mask being provided with a pattern corresponding to the flow field channel and being made of rubber or stainless steel. It is preferable that the forming of the flow field channel on the graphite foil includes at least one of sandblasting and ultrasonic etching. It is preferable that the forming of a hydrophobic layer on the interior side of the flow field channel by impregnation includes: forming a hydrophobic layer on the graphite foil attached with the mask pattern and formed with the flow field channel; and drying the graphite foil formed with the hydrophobic layer, in a
  • the mask pattern includes a front mask pattern and a rear mask
  • At least one aligning hole is formed through the graphite foil corresponding to the aligning holes of the mask patterns; and the aligning holes of the mask patterns and the aligning holes of the
  • graphite foil are aligned by using at least one pair of aligning bars
  • At least one pair of aligning bars respectively include a plurality of pairs thereof
  • a fuel cell stack according to the present invention is a fuel cell stack
  • the at least one unit cell includes: an MEA including a polymer electrolyte membrane, and an anode and a cathode formed on both sides thereof; a pair of fluid diffusion layers contiguously disposed to the anode and
  • At least one of the pair of separators includes a lamellar structure
  • the lamellar structure graphite foil may include a stainless steel layer
  • the stainless steel layer is exteriorly
  • the graphite foil is substantially free from thermosetting or
  • thermoplastic resin thermoplastic resin
  • a bulk density of the graphite foil preferably lies in the range of 1 .5g/cm 3 to 2.0g/cm 3 .
  • a thickness of the graphite foil preferably lies in the range of 0.5mm
  • a thickness of the hydrophobic layer preferably lies in the range of 30 ⁇ m to 100 ⁇ m. It is preferable that a sealing member is unified to the separator along
  • FIG. 1 is a schematic sectional view of an exemplary fuel cell stack.
  • FIG. 2 is an exploded perspective view of a fuel cell stack according
  • FIG. 3 a sectional view showing a detailed junction structure of an
  • FIG. 4 shows a front side 400 (i.e., a side toward a cathode) of a cathode side separator 260 of a unit cell 200 of a fuel cell stack according to an embodiment of the present invention.
  • FIG. 5 shows a rear side 500 (i.e., a side opposite to a cathode) of a
  • cathode side separator 260 of a unit cell 200 of a fuel cell stack according to
  • FIG. 6 shows a rear side 600 (i.e., a side toward an anode) of an
  • FIG. 7 is a sectional view of FIG. 4 along a line VII-VII.
  • FIG. 8 is a sectional view of FIG. 6 along a line VIII-VIII.
  • FIG. 9 is a flowchart showing a method for manufacturing a separator
  • FIG. 10 is a drawing for illustrating a process for attaching a mask to a graphite foil in a method for manufacturing a separator according to an embodiment of the present invention.
  • FIG. 11 is a sectional view of FIG. 6 along a line XI-XI according to a second embodiment of the present invention.
  • FIG. 2 is an exploded perspective view of a fuel cell stack according to an embodiment of the present invention.
  • a fuel cell stack according to an embodiment of the present invention includes a stack of a plurality of unit cells 200.
  • the stack of the unit cells 200 are conjoined by end plates 290 disposed at ends thereof.
  • connection holes 270 are formed for supplying and exhausting reaction gas etc. to/from the fuel cell stack.
  • the connection holes 270 include a hydrogen supply hole 271 , a coolant supply hole 272, an air supply hole 273, an air exhaust hole 274, a coolant exhaust hole 275, and a hydrogen exhaust hole 276.
  • Each of the connection holes 271-276 is connected to a corresponding manifold in the fuel cell stack 100.
  • fluid diffusion layers 225 are attached to front and rear of an MEA 230, and separators 250 and 260 are disposed to front and rear of the MEA 230 and attached to the fluid diffusion layers 225.
  • separators 250 and 260 are disposed to front and rear of the MEA 230 and attached to the fluid diffusion layers 225.
  • the left side of FIG. 2 is referred to as frontward of the unit cells 200
  • the right side of FIG. 2 is referred to as rearward of the unit cells 200.
  • the above-described fluid diffusion layer 225 is usually called a gas
  • GDL diffusion layer
  • fluid diffusion layer 225 through the fluid diffusion layer 225 is not necessarily a gas, so the term fluid diffusion layer is hereinafter used instead of the usual term gas diffusion
  • FIG. 3 is a sectional view showing a detailed junction structure of an
  • an anode 221 and a cathode 222 are respectively formed, by
  • the fluid diffusion layer 225 is formed to each exterior of the anode 221 and
  • a cathode side separator 260 is in close contact with the cathode of the MEA 230 having the fluid diffusion layer 225, and an anode side separator 250 is in close contact with the anode.
  • the anode side separator 250 is described to be of a monopolar structure
  • the cathode side separator 260 is described to be of a bipolar structure.
  • the protection scope of the present invention should not be understood to be limited thereto, because the spirit of the present invention may be applied to various other schemes of disposing separators at the front and rear of the MEA 230.
  • the separators 250 and 260 are closely conjoined to exterior surfaces of the fluid diffusion layers 225, and have a plurality of flow field channels on their surface closely facing the fluid diffusion layers.
  • the flow field channels of the separators 250 and 260 are used as passages of reaction gas between the fluid diffusion layers 225 and the separators 250 and 260.
  • the separators 250 and 260 distribute reaction gases through the fuel cell stack, separate a fuel gas and a reduction gas, and electrically connect adjacent unit cells by providing an electron passage between an anode and a cathode of adjacent unit cells.
  • the separators have
  • the separators 250 and 260 according to an embodiment of the
  • FIG. 4 shows a front side 400 (i.e., a side toward a cathode) of a
  • cathode side separator 260 of a unit cell 200 of a fuel cell stack according to
  • air supply manifold 473 are formed through the separator 260, respectively
  • exhaust manifold 476 are formed through the separator 260, respectively
  • channels 410 for supplying air to the MEA 230 are formed by ribs 420
  • Such air flow-field channels 410 are formed as grooves of
  • FIG. 4 illustrates that the air flow-field channels 410 of the separator
  • 260 according to an embodiment of the present invention are of a serpentine
  • the air supplied to the air supply manifold 473 is supplied to the air
  • hole 460 is exhausted to the air exhaust manifold 474 through air exhaust
  • passages 560 (refer to FIG. 5) formed at the rear side of the separator 260.
  • groove 480 is formed for application of sealant for preventing air leakage
  • sealant grooves 480-486 are in the form of closed loops that
  • At least one pair of aligning holes are formed through the separator 260, for
  • the at least one pair of aligning holes are formed as a plurality of
  • aligning holes 431 and 432 enables rough alignment (i.e., allowing easy
  • FIG. 4 illustrates that the pair of the larger diameter
  • aligning holes 431 and 432 are formed at upper and lower portions of the
  • FIG. 4 illustrates that the aligning holes 431
  • FIG. 5 shows a rear side 500 (i.e., a side opposite to a cathode) of a
  • cathode side separator 260 of a unit cell 200 of a fuel cell stack according to
  • hole 450 are interconnected through the air supply passages 550, and the air
  • exhaust manifold 474 and air exhaust hole 460 are interconnected through
  • the air exhaust passages 560 The air supply passages 550 and the air
  • exhaust passages 560 are formed on the rear side 500 of the separator 260 in the form of grooves.
  • hydrogen supply passages 555 are formed to be
  • passage 565 are formed to be connected to the hydrogen exhaust manifold 476.
  • Sealant grooves 581 , 583, 584, and 586 for application of sealant are formed on the rear side 500 of separator 260 in the form of grooves. Sealant grooves 581 , 583, 584, and 586 for application of sealant are
  • coolant At a central portion on the rear side 500 of the separator, coolant
  • supply manifold 472 are formed by ribs 520 defining the route. Such coolant
  • flow-field channels 510 on the rear side 500 of the separator are formed to
  • the fuel cell coolant is supplied to the coolant flow-field channels 510
  • FIG. 6 shows a rear side 600 (i.e., a side toward an anode) of an
  • anode side separator 250 of a unit cell 200 of a fuel cell stack according to an embodiment of the present invention.
  • the rear side of the anode side separator 250 is structured similarly
  • supply manifold 673 are formed through the separator 250.
  • the separator 250 In addition, at a
  • hydrogen flow-field channels 610 for supplying hydrogen to the MEA 230 are formed by ribs 620 defining the route.
  • the hydrogen supplied to the hydrogen supply manifold 671 is the hydrogen supplied to the hydrogen supply manifold 671.
  • reaction region sealant groove 680 is formed for application of sealant for
  • Aligning holes 631 , 632, 633, and 634 are formed through the anode
  • the unit cells 200 may be eased due to the aligning holes 431 , 432, 631 , and
  • separators 250 and 260 are described in detail.
  • FIG. 7 is a sectional view of FIG. 4 along a line Vll-Vll
  • FIG. 8 is
  • FIG. 6 a sectional view of FIG. 6 along a line VIII-VIII.
  • graphite foil 700 and 800 is used as a material for the separators 250 and 260. Manufacturing of a graphite foil is usually accompanied by a pressing
  • the enlarged portion A of FIG. 7 and portion B of FIG. 8 may be
  • heat conductivity thereof is more than 250
  • thermosetting resin or thermoplastic resin
  • an operating temperature range of a fuel cell may be
  • separators 250 and 260 may have high formability for, e.g.,
  • a separator of a fuel cell should maintain uniform pressure without
  • production cost of a graphite foil i.e., production cost of a separator.
  • graphite foil used for separators 250 and 260 of an embodiment of the present invention may have a bulk density less than 2.0g/cm 3 .
  • a minimum depth for the flow field channels is usually about 0.2mm.
  • the thickness d2 of the flow field channels becomes less than 0.3mm.
  • membrane fuel cell is less than 100 ° C and about 80 ° C , efficient and steady exhaust of reaction products, i.e., heat and water, is very important.
  • reaction products i.e., heat and water
  • hydrophobic layers 710 and 810 are formed by
  • the hydrophobic layers 710 and 810 are
  • hydrophobic layer is simply coated on a surface of a workpiece. In this case,
  • the coated hydrophobic layer may be easily scraped or removed.
  • hydrophobic layers 710 and 810 are formed
  • hydrophobic layers 710 and 810 to the interior surface of the flow field channels 410 and 610 is enhanced and thereby durability of the hydrophobic
  • impregnation into the flow field channels preferably lies in a range of 30 ⁇ m to
  • the thickness of the hydrophobic layers 710 and 810 is preferably
  • hydrophobic layers 710 and 810 are thicker than 100 ⁇ m
  • hydrophobic solution used for the hydrophobic layer is excessively
  • lamellas may occur due to, e.g., bubbles formed at the lamellar structure graphite foil, when heat treatment for hydrophobic effect (for example, heat
  • grooves 481-486, 681-686, 480, and 680 are formed around the manifolds
  • sealing members 790 and 890 are
  • FIGs. 7 and 8 illustrate that sealing
  • rubber liquid of, e.g., silicon series, fluorine series, and olefin series may be
  • sealing members 790 and 890 are used as the sealing members 790 and 890.
  • FIG. 9 is a flowchart showing a method for manufacturing a separator
  • step S930 the manifolds, the sealant grooves, and the flow
  • step S950 the mask pattern is removed from the graphite
  • flow-field channels etc. i.e., the manifolds
  • sealant grooves, and the flow field channels are formed by executing the
  • step S910 of preparing the graphite foil the prepared
  • graphite foil has a thickness of 1 .0mm, an overall density of 1.78g/cm3, and
  • the step S920 of forming the mask pattern may be further embodied
  • a dry film may be used.
  • a dry film for example, BF410
  • a dry film for example, BF410
  • the upper roller temperature is about 70 ° C
  • the lower roller temperature is about
  • a film mask formed with a pattern for flow-field channels etc. is laid in
  • a spray nozzle moves while spraying a liquid
  • developer e.g., 1 -2% solution of Na2C03
  • the developing conditions of the spray-type developing machine is preferably set to be the temperature of the liquid developer being about 25 °C ,
  • the spray pressure being about 2.7Kg/cm2, and the nozzle moving speed
  • the step S920 of forming a mask pattern includes a step of attaching
  • working plate 1 100 is formed as a transparent plate such that an exposure
  • a prepared mask 1010 is formed with aligning holes 101 1 , 1012,
  • aligning holes 631 , 632, 633, and 634 are formed at the graphite foil at
  • a thickness of the mask 10 0 is usually less than 0.2mm, and it
  • the mask 1010 is laid on the working plate 1 100 such that the
  • protruded aligning bars 1021 , 1022, 1023, and 1024 may be inserted into the
  • aligning holes 101 1 , 1012, 1013, and 1014 In this case, the aligning bars
  • holes 631 , 632, 633, and 634 are inserted by aligning bars 1021 , 1022, 1023,
  • front and rear sides of the separator are precisely aligned.
  • processed with the mask pattern process is dry-etched using, e.g., a sand
  • the sand blast condition is preferably set to be the separator moving
  • the spraying pressure of the nozzle being about 3.0kg/cm2
  • the distance between the separator and the nozzle being about 60mm.
  • SiC may be used as an abrasive such that surface roughness on
  • An ultrasonic etching process that is, an etching process using an
  • abrasive may be performed instead of or together with the sand blast
  • hydrophobic solution e.g., a 20% PTFE (polytetrafluoroethylene) solution
  • PTFE polytetrafluoroethylene
  • the mask pattern is
  • the graphite foil used for the separator includes a stainless
  • FIG. 11 is a sectional view of FIG. 6 along a line XI-XI according to a
  • Such graphite foil 1 140 including the stainless steel layer 1160 may be easily manufactured e.g., by pressing graphite layers of predetermined thickness to front and rear of the stainless steel layer 1160.
  • the stainless steel layer 1160 may be of, e.g., SUS304 or SUS316, and its thickness t is preferably 0.1mm to 0.3mm.
  • the separator 1150 uses the graphite foil 1140 formed with, e.g., the stainless layer 1160 of 0.1 mm thickness at its center and graphite layers of 0.2mm thickness at each of front and rear sides of the stainless layer 1160 (therefore, total thickness D3 of the graphite foil becomes 0.5mm).
  • the flow- field channels 610 are formed by dry-etching one side (e.g., upper side in FIG. 11) of the graphite foil 1140.
  • a method for manufacturing the separator 1150 using the graphite foil 1140 including the stainless steel layer 1160 therein is the same as a method for manufacturing the separators 250 and 260 according to the first embodiment of the present invention that has been described with reference to FIG. 10.
  • the graphite layer is etched such that the stainless steel layer 1160 is exposed.
  • the stainless steel layer 1 160 has a substantially
  • the abrasive used in the etching process may easily form a roughness thereon, e.g., to the degree of several decades of micrometers
  • the hydrophobic layer 810 is formed while the
  • stainless steel layer 1160 is exposed in the flow-field channels 610.
  • hydrophobic layer 810 is formed while the stainless steel layer 1 160 is
  • fuel gas should be understood in a collective
  • MEA polymer electrolyte fuel cell
  • lamellar structure graphite foil is used as a material for a separator
  • hydrophobic layer is formed by impregnation on an interior
  • hydrophobic layer is formed by impregnation on
  • thermosetting or thermoplastic resin from resins such as thermosetting or thermoplastic resin and a hydrophobic
  • the cooling effect of a fuel cell stack is enhanced and temperature distribution of a fuel cell stack becomes uniform. Furthermore, since the lamellar structure graphite foil used as a

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Abstract

A lamellar structure graphite foil is used as a material for a separator for a fuel cell, and a hydrophobic layer is formed by impregnation on flow-field channels of the graphite foil. Such a separator is manufactured by forming the flow field channel by etching the graphite foil formed with the mask pattern thereon and forming a hydrophobic layer by impregnation. According to such a separator, performance of a fuel cell stack is enhanced and the manufacturing process of a separator is simplified.

Description

TITLE OF THE INVENTION
SEPARATOR FOR FUEL CELL, MANUFACTURING METHOD THEREOF, AND FUEL CELL HAVING SUCH A SEPARATOR
BACKGROUND OF THE INVENTION
(a) Field of the Invention
Generally, the present invention relates to a fuel cell. More
particularly, the present invention relates to a separator for a fuel cell using a
graphite foil, a manufacturing method thereof, and a fuel cell stack including
such a separator.
(b) Description of the Related Art
As is well known in the art, a fuel cell produces electric power by an
oxidation reaction at an anode and a reduction reaction at a cathode. The anode and the cathode are formed with a catalyst layer having platinum or
platinum-ruthenium metal for accelerating the oxidation and reduction
reactions.
At the anode, fuel gas (for example, hydrogen) is supplied thereto
and is divided into ions (for example, protons) and electrons through the
oxidation reaction. At the cathode, the divided ion bonds with a reduction gas
(for example, oxygen) to form water. Final products of such reactions are
electricity (i.e., electron movement from the anode to the cathode), water (i.e.,
a chemical bond of hydrogen and oxygen), and heat. A fuel cell stack is
usually provided with a cooling device for removing such heat. The water formed at the cathode is usually formed as vapor or liquid,
and such water is removed by a strong stream of reduction gas (oxygen or
air) flowing at a cathode side.
FIG. 1 is a schematic sectional view of an exemplary fuel cell stack
according to the prior art.
Usually, a fuel cell stack is formed by stacking a plurality of unit cells
100. Such a unit cell 100 includes a proton exchange membrane 110 (for
example, a polymer electrolyte membrane). An anode 121 and a cathode
122 are formed at both sides of the proton exchange membrane 1 10. The
proton exchange membrane 110 and electrodes 121 and 122 form a
membrane electrode assembly (MEA) 130 by hot pressing. Fluid diffusion
layers 125 are formed to the exterior of the electrodes 121 and 122 of the
MEA 130. MEAs 130 of adjacent unit cells are separated and supported by a
separator 150. The separator 150 is formed with a flow field 151 for
supplying fuel gas (e.g., hydrogen, or methanol in the case of a direct
methanol fuel cell) to the anode. In addition, the separator 150 is also formed
with a flow field 152 for supplying oxygen or air as a reduction gas to the
cathode, and also for exhausting water. A gasket 160 is applied between the
separator 150 and the MEA 130, for preventing leakage of gas/liquid flowing
through the flow fields 151 and 152.
The unit cells 100 including the MEA 130, the separator 150, and the gasket 160 are stacked in series to form a high voltage. The stacked unit
cells are conjoined by, e.g., current collectors and end plates 170 disposed
at ends thereof.
As can be understood from the above description, a separator in a
fuel cell distributes reaction gases (i.e., fuel gas and reduction gas) through
the fuel cell stack, separates a fuel gas (e.g., hydrogen or methanol) and a
reduction gas (e.g., oxygen or air), and electrically connects adjacent unit
cells by providing an electron passage between an anode and a cathode of
adjacent unit cells. In addition, the separator has a heat exhaust structure for
exhausting heat produced by the oxidation-reduction reaction of the fuel cell
stack, and provides mechanical strength for supporting the stacked unit cells. In order to accelerate movement of hydrogen ions (i.e., protons)
produced at the anode to the cathode through a polymer electrolyte
membrane, the polymer electrolyte membrane should be hydrated to contain
an appropriate amount of moisture. The hydrated polymer electrolyte
membrane prevents movement of electrons therethrough while allowing
movement of hydrogen ions.
When the polymer electrolyte membrane is not sufficiently hydrated,
ion conductivity of the polymer electrolyte membrane is lowered, and
therefore performance of a fuel cell is deteriorated. To the contrary, when the
polymer electrolyte membrane is excessively hydrated, small pores forming a
triple-phase boundary of reaction are blocked (which is usually called
flooding), and thereby the reaction area of the electrodes reduces, resulting in deterioration in performance of the fuel cell. Therefore, in the case that the water formed at cathodes is not promptly exhausted, reaction gas is not sufficiently supplied to the catalyst layer, and therefore performance of a fuel cell is deteriorated. Many separators, including an exemplary one disclosed by U.S.
patent No. 4,988,583, have serpentine flow fields for fuel and reduction gases. This is mainly for utilizing a pressure drop along the flow fields for efficient exhaust of water formed at the cathodes. The water formed at the cathodes is in the form of vapor, near the entry of reduction gas flow-field channel. However, as it flows through the reduction gas flow-field channel, it becomes of two phased, as mixed liquid and vapor. In this case, liquefied water drops fill the pores of the cathodes, and accordingly, the effective active areas of the catalyst layers become reduced. In addition, liquefied water requires a high pressure of reduction gas for exhaust thereof. Therefore, energy loss occurs by a pressure drop of reduction gas between entry and exit of flow fields, and reaction gas is much consumed for stable realization of the reduction reaction at a high flow speed. Therefore, if water exhaust of a separator having serpentine flow fields becomes more stable and efficient, it will promise a reduction of energy loss by the pressure drop of reduction gas between the entry and exit of the flow fields and reduction of consumption of reaction gas. Graphite or carbon composite materials are widely used for a separator for a polymer electrolyte membrane fuel cell. The graphite and the
carbon composite material show strong anti-corrosiveness to the oxidation-
reduction reaction of a fuel cell, and also have a merit of low bulk density in
comparison with metallic materials (e.g., stainless steel). When the graphite or the carbon composite material is used as a
material for a separator, according to the prior art, a resin such as
thermosetting or thermoplastic resin is usually added to the separator
material in order to prevent movement of hydrogen by filling micropores of
the separator, and also for easy forming during the molding process.
However, the resin included in the separator causes an increase of volume resistance with respect to movement of electrons, and thereby deteriorates
performance of a fuel cell. Furthermore, the resin increases contact
resistance between cells.
As an exemplary method for reducing an increase of contact
resistance between cells cause by the resin in the separator, European
Patent Publication No. EP1253657A1 discloses a method in which rib
surfaces of flow fields of a separator are etched in an alkaline solution such
that the resin in the surface area of the rib may be removed.
According to the prior art, the manufacturing process for a stable and
useful separator using a graphite or a carbon composite material has been
very complex, non-productive, and non-efficient. Therefore, if a separator
using graphite or a carbon composite material can result in higher
performance and be appropriate for mass production, it promises a substantial decrease in production cost of a separator and in turn production
cost of a fuel cell, as well as enhancement of performance of a separator.
The information disclosed in this Background of the Invention section
is only for enhancement of understanding of the background of the invention
and should not be taken as an acknowledgement or any form of suggestion
that this information forms the prior art that is already known in this country
to a person of ordinary skill in the art.
SUMMARY OF THE INVENTION
Therefore, the present invention has been made in an effort to solve
the above-described problem. The motivation for the present invention is to
provide a separator for a fuel cell, a manufacturing method thereof, and a
fuel cell including such a separator, providing an enhanced water exhaust
performance, enhanced durability, and being more appropriate for mass
production. From such motivation, a separator for a fuel cell according to the
present invention is a separator for a fuel cell that is capable of closely
contacting either an anode or a cathode of an MEA (membrane electrode
assembly) of a fuel cell and interposing a fluid diffusion layer, the separator
having a flow field channel for allowing a fluid to flow between the separator
and the fluid diffusion layer, characterized in that: the separator comprises a
lamellar structure graphite foil; and a hydrophobic layer is formed by
impregnation on an interior side of the flow field channel.
The lamellar structure graphite foil may include a stainless steel layer therewithin. Preferably in this case, the stainless steel layer is exteriorly exposed, interposing the hydrophobic layer. Preferably, the graphite foil is substantially free from thermosetting or thermoplastic resin. A bulk density of the graphite foil preferably lies in the range of
1.5g/cm3 to 2.0g/cm3. A thickness of the graphite foil preferably lies in the range of 0.5mm to 3mm. A thickness of the hydrophobic layer preferably lies in the range of 30μm to 100μm. It is preferable that at least one manifold is formed in the separator, and a sealing member is unified to the separator along each circumference of the at least one manifold and an area for contacting the fluid diffusion layer. It is preferable that the sealing member encloses, respectively along a closed curve, each of the at least one manifold and the area for contacting the fluid diffusion layer. In addition, a method for manufacturing a separator according to the present invention is a method for manufacturing a separator for a fuel cell that is capable of closely contacting either an anode or a cathode of an MEA
of a fuel cell and interposing a fluid diffusion layer, and has a flow field
channel for allowing a fluid to flow between the separator and the fluid
diffusion layer, characterized in that the method includes: preparing a graphite foil of a predetermined size; forming a mask pattern on the graphite foil corresponding to the flow field channel; forming the flow field channel on the graphite foil by etching the graphite foil formed with the mask pattern thereon; forming a hydrophobic layer on an interior side of the flow field channel by impregnation; and removing the mask pattern from the graphite foil. It is preferable that the forming of a mask pattern on the graphite foil includes: coating the graphite foil with a dry film resist; exposing the coated graphite foil; and developing the dry film resist on the graphite foil by moving a spray nozzle of a spray-type developing apparatus thereover. As another example, it is also preferable that the forming of a mask pattern on the graphite foil includes attaching a mask on the graphite foil, the mask being provided with a pattern corresponding to the flow field channel and being made of rubber or stainless steel. It is preferable that the forming of the flow field channel on the graphite foil includes at least one of sandblasting and ultrasonic etching. It is preferable that the forming of a hydrophobic layer on the interior side of the flow field channel by impregnation includes: forming a hydrophobic layer on the graphite foil attached with the mask pattern and formed with the flow field channel; and drying the graphite foil formed with the hydrophobic layer, in a
temperature range of 50°C-90°C.
It is preferable that, in the forming of a hydrophobic layer on the
graphite foil, a hydrophobic. solution is spray coated on a surface of the
graphite foil, or the graphite foil is dipped in the hydrophobic solution.
As for a bipolar separator in which the flow field channel is formed on
each of front and rear sides thereof, it is preferable that: the mask pattern includes a front mask pattern and a rear mask
pattern; at least one pair of aligning holes are formed at each of the front and
rear mask patterns; at least one aligning hole is formed through the graphite foil corresponding to the aligning holes of the mask patterns; and the aligning holes of the mask patterns and the aligning holes of the
graphite foil are aligned by using at least one pair of aligning bars
corresponding thereto.
It is preferable that the at least one pair of aligning holes and the at
least one pair of aligning bars respectively include a plurality of pairs thereof,
corresponding to different sizes.
A fuel cell stack according to the present invention is a fuel cell stack
including at least one unit cell, wherein the at least one unit cell includes: an MEA including a polymer electrolyte membrane, and an anode and a cathode formed on both sides thereof; a pair of fluid diffusion layers contiguously disposed to the anode and
the cathode at both sides of the MEA; and a pair of separators for closely contacting the pair of fluid diffusion
layers, forming flow field channels on sides thereof facing the fluid diffusion
layers so as to form a reaction region, and forming manifold regions
peripheral to the reaction region, characterized in that at least one of the pair of separators includes a lamellar structure
graphite foil, and a hydrophobic layer is formed by impregnation on an interior side of
the flow field channels of the at least one of the pair of separators.
The lamellar structure graphite foil may include a stainless steel layer
therewithin. Preferably in this case, the stainless steel layer is exteriorly
exposed, interposing the hydrophobic layer.
Preferably, the graphite foil is substantially free from thermosetting or
thermoplastic resin.
A bulk density of the graphite foil preferably lies in the range of 1 .5g/cm3 to 2.0g/cm3. A thickness of the graphite foil preferably lies in the range of 0.5mm
to 3mm.
A thickness of the hydrophobic layer preferably lies in the range of 30μm to 100μm. It is preferable that a sealing member is unified to the separator along
each circumference of the manifold and the reaction region. BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1 is a schematic sectional view of an exemplary fuel cell stack. FIG. 2 is an exploded perspective view of a fuel cell stack according
to an embodiment of the present invention.
FIG. 3 a sectional view showing a detailed junction structure of an
MEA and fluid diffusion layers in a unit cell of a fuel cell stack according to an
embodiment of the present invention. FIG. 4 shows a front side 400 (i.e., a side toward a cathode) of a cathode side separator 260 of a unit cell 200 of a fuel cell stack according to an embodiment of the present invention.
FIG. 5 shows a rear side 500 (i.e., a side opposite to a cathode) of a
cathode side separator 260 of a unit cell 200 of a fuel cell stack according to
an embodiment of the present invention.
FIG. 6 shows a rear side 600 (i.e., a side toward an anode) of an
anode side separator 250 of a unit cell 200 of a fuel cell stack according to
an embodiment of the present invention.
FIG. 7 is a sectional view of FIG. 4 along a line VII-VII. FIG. 8 is a sectional view of FIG. 6 along a line VIII-VIII.
FIG. 9 is a flowchart showing a method for manufacturing a separator
for a fuel cell according to an embodiment of the present invention.
FIG. 10 is a drawing for illustrating a process for attaching a mask to a graphite foil in a method for manufacturing a separator according to an embodiment of the present invention. FIG. 11 is a sectional view of FIG. 6 along a line XI-XI according to a second embodiment of the present invention. DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS
An embodiment of the present invention will hereinafter be described in detail with reference to the accompanying drawings. In the description below, terms such as upper portion/lower portion and front side/rear side implying directions are used for convenience of explanation. However, such terms are only for convenience of description and better understanding, so it should not be understood that specific elements should be disposed at such directions according to the present invention. FIG. 2 is an exploded perspective view of a fuel cell stack according to an embodiment of the present invention. As shown in FIG. 2, a fuel cell stack according to an embodiment of the present invention includes a stack of a plurality of unit cells 200. The stack of the unit cells 200 are conjoined by end plates 290 disposed at ends thereof. The end plates 290 are formed with current collectors 295, and thereby supply electricity produced through the entire fuel cell stack. At the end plate 290 applying a conjoining pressure to the fuel cell stack, a multiplicity of connection holes 270 are formed for supplying and exhausting reaction gas etc. to/from the fuel cell stack. The connection holes 270 include a hydrogen supply hole 271 , a coolant supply hole 272, an air supply hole 273, an air exhaust hole 274, a coolant exhaust hole 275, and a hydrogen exhaust hole 276. Each of the connection holes 271-276 is connected to a corresponding manifold in the fuel cell stack 100. For each unit cell 200, fluid diffusion layers 225 are attached to front and rear of an MEA 230, and separators 250 and 260 are disposed to front and rear of the MEA 230 and attached to the fluid diffusion layers 225. Hereinafter, the left side of FIG. 2 is referred to as frontward of the unit cells 200, and the right side of FIG. 2 is referred to as rearward of the unit cells 200. The above-described fluid diffusion layer 225 is usually called a gas
diffusion layer (GDL) in the art. However, the material diffused/distributed
through the fluid diffusion layer 225 is not necessarily a gas, so the term fluid diffusion layer is hereinafter used instead of the usual term gas diffusion
layer.
FIG. 3 is a sectional view showing a detailed junction structure of an
MEA 230 and fluid diffusion layers 225 in a unit cell 200 of a fuel cell stack
according to an embodiment of the present invention.
As shown in FIG. 3, according to an embodiment of the present
invention, an anode 221 and a cathode 222 are respectively formed, by
pressing, to front and rear sides of a polymer electrolyte membrane 210, and
the fluid diffusion layer 225 is formed to each exterior of the anode 221 and
the cathode 222 Referring back to FIG. 2, a cathode side separator 260 is in close contact with the cathode of the MEA 230 having the fluid diffusion layer 225, and an anode side separator 250 is in close contact with the anode. In the following description of an embodiment of the present invention, the anode side separator 250 is described to be of a monopolar structure, and the cathode side separator 260 is described to be of a bipolar structure. However, the protection scope of the present invention should not be understood to be limited thereto, because the spirit of the present invention may be applied to various other schemes of disposing separators at the front and rear of the MEA 230. The separators 250 and 260 are closely conjoined to exterior surfaces of the fluid diffusion layers 225, and have a plurality of flow field channels on their surface closely facing the fluid diffusion layers. The flow field channels of the separators 250 and 260 are used as passages of reaction gas between the fluid diffusion layers 225 and the separators 250 and 260. The separators 250 and 260 distribute reaction gases through the fuel cell stack, separate a fuel gas and a reduction gas, and electrically connect adjacent unit cells by providing an electron passage between an anode and a cathode of adjacent unit cells. In addition, the separators have
a heat exhaust structure for exhausting heat produced by the oxidation-
reduction reaction of the fuel cell stack, and provide mechanical strength for
supporting the stacked unit cells. The separators 250 and 260 according to an embodiment of the
present invention are hereinafter described in further detail.
FIG. 4 shows a front side 400 (i.e., a side toward a cathode) of a
cathode side separator 260 of a unit cell 200 of a fuel cell stack according to
an embodiment of the present invention.
As shown in FIG. 4, at an upper portion of the cathode side separator
260, a hydrogen supply manifold 471 , a coolant supply manifold 472, and an
air supply manifold 473 are formed through the separator 260, respectively
corresponding to the hydrogen supply hole 271 , the coolant supply hole 272,
and the air supply hole 273.
In addition, at a lower portion of the cathode side separator 260, an air exhaust manifold 474, a coolant exhaust manifold 475, and a hydrogen
exhaust manifold 476 are formed through the separator 260, respectively
corresponding to the air exhaust hole 274, the coolant exhaust hole 275, and
the hydrogen exhaust hole 276.
For preventing leakage of reaction gas/coolant from the manifolds
471-476, manifold sealant grooves 481-486 for application of sealant are
respectively formed around each of the manifolds 471-476.
At a fuel cell reaction region (i.e., a region contacting the fluid
diffusion layer 225) in front of the cathode side separator 260, air flow-field
channels 410 for supplying air to the MEA 230 are formed by ribs 420
defining the route. Such air flow-field channels 410 are formed as grooves of
a predetermined depth. FIG. 4 illustrates that the air flow-field channels 410 of the separator
260 according to an embodiment of the present invention are of a serpentine
shape. However, this is only an exemplary shape of which the spirit of the
present invention may be applied, and accordingly the protection scope of
the present invention should not be understood to be limited thereto.
At entry ends of the air flow-field channels 410, an air supply hole
450 for supplying air to the air flow-field channels 410 is formed through the
separator 260, and at exit ends of the air flow-field channels 410, air exhaust
hole 460 for exhausting air from the air flow-field channels 410 is formed
through the separator 260.
The air supplied to the air supply manifold 473 is supplied to the air
supply hole 450 through air supply passages 550 (refer to FIG. 5) formed at
the rear side of the separator 260. The air exhausting from the air exhaust
hole 460 is exhausted to the air exhaust manifold 474 through air exhaust
passages 560 (refer to FIG. 5) formed at the rear side of the separator 260.
Around the reaction region having the air flow-field channels 410, the
air supply hole 450, and the air exhaust hole 460, a reaction region sealant
groove 480 is formed for application of sealant for preventing air leakage
from the reaction region. The sealant grooves 480-486 are in the form of closed loops that
respectively enclose the manifolds and the region closely contacting the fluid
diffusion layer.
In an area between sealant grooves 480-486 on the separator 260, at least one pair of aligning holes are formed through the separator 260, for
alignment of flow field channels on front and rear sides of the separator 260. The at least one pair of aligning holes are formed as a plurality of
aligning hole pairs (pairs of 431 and 432, and 433 and 434) having different
sizes. By forming the aligning hole pairs with different sizes, larger diameter
aligning holes 431 and 432 enables rough alignment (i.e., allowing easy
alignment), and smaller diameter aligning holes 433 and 434 enable a
precise alignment.
As an example, FIG. 4 illustrates that the pair of the larger diameter
aligning holes 431 and 432 are formed at upper and lower portions of the
separator, and the pair of the smaller diameter aligning holes 433 and 434
are formed interior to the larger diameter aligning holes 431 and 433.
Again as an example, FIG. 4 illustrates that the aligning holes 431
and 433 at the upper portion are formed between the sealant groove 481 of
the hydrogen supply manifold 471 and the sealant groove 482 of the coolant
supply manifold 472, and the aligning holes 432 and 434 at the lower portion
are formed between the sealant groove 486 for the hydrogen exhaust
manifold 476 and the sealant groove 485 for the coolant exhaust manifold
475. Aligning of the flow field channels on the front and rear sides 400 and
500 of the bipolar separator 260 using the aligning holes 431 , 432, 433, and
434 is described in further detail in the description regarding a manufacturing
method of a separator according to an embodiment of the present invention. FIG. 5 shows a rear side 500 (i.e., a side opposite to a cathode) of a
cathode side separator 260 of a unit cell 200 of a fuel cell stack according to
an embodiment of the present invention.
As shown in FIG. 5, the air supply manifold 473 and the air supply
hole 450 are interconnected through the air supply passages 550, and the air
exhaust manifold 474 and air exhaust hole 460 are interconnected through
the air exhaust passages 560. The air supply passages 550 and the air
exhaust passages 560 are formed on the rear side 500 of the separator 260 in the form of grooves. In addition, hydrogen supply passages 555 are formed to be
connected to the hydrogen supply manifold 471 , and hydrogen exhaust
passage 565 are formed to be connected to the hydrogen exhaust manifold 476. The hydrogen supply passages 555 and hydrogen exhaust passage
565 are formed on the rear side 500 of separator 260 in the form of grooves. Sealant grooves 581 , 583, 584, and 586 for application of sealant are
respectively formed around each of the manifolds 471 , 473, 474, and 476, in
the form of closed loops that respectively enclose the manifolds and
passages connected thereto.
At a central portion on the rear side 500 of the separator, coolant
flow-field channels 510 for circulating the coolant supplied from the coolant
supply manifold 472 are formed by ribs 520 defining the route. Such coolant
flow-field channels 510 on the rear side 500 of the separator are formed to
be aligned with the air flow-field channels 410 on the front side 400 of the separator.
The fuel cell coolant is supplied to the coolant flow-field channels 510
through the coolant supply manifold 472, is circulated on the rear side of the
separator 260, and is then exhausted through the coolant exhaust manifold
475. A sealant groove 580 for application of sealant for preventing leakage
of coolant is formed enclosing the coolant supply manifold 472, the coolant
flow-field channel 510, and the coolant exhaust manifold 475.
FIG. 6 shows a rear side 600 (i.e., a side toward an anode) of an
anode side separator 250 of a unit cell 200 of a fuel cell stack according to an embodiment of the present invention.
The rear side of the anode side separator 250 is structured similarly
to the front side 400 of the cathode side separator 260.
That is, as shown in FIG. 6, at an upper portion of the separator 250,
a hydrogen supply manifold 671 , a coolant supply manifold 672, and an air
supply manifold 673 are formed through the separator 250. In addition, at a
lower portion of the separator 250, an air exhaust manifold 674, a coolant
exhaust manifold 675, and a hydrogen exhaust manifold 676 are formed
through the separator 250. In addition, manifold sealant grooves 681-686 for
application of sealant are respectively formed around each of the manifolds
671-676.
At a fuel cell reaction region in rear of the anode side separator 250,
hydrogen flow-field channels 610 for supplying hydrogen to the MEA 230 are formed by ribs 620 defining the route.
At entry ends of the hydrogen flow-field channels 610, a hydrogen
supply hole 650 for supplying hydrogen to the hydrogen flow-field channels
610 is formed through the separator 250, and at exit ends of the hydrogen
flow-field channels 610, a hydrogen exhaust hole 660 for exhausting
hydrogen from the hydrogen flow-field channels 610 is formed through the
separator 260.
The hydrogen supplied to the hydrogen supply manifold 671 is
supplied to the hydrogen supply hole 650 through hydrogen supply passages
555 (refer to FIG. 5) formed at the rear side of the cathode side separator
260 of an adjacent unit cell. The hydrogen exhausting from the hydrogen exhaust hole 660 is exhausted to the hydrogen exhaust manifold 676
through hydrogen exhaust passages 565 (refer to FIG. 5) formed at the rear
side of the cathode side separator 260 of an adjacent unit cell. Around the reaction region having the hydrogen flow-field channels
610, the hydrogen supply hole 650, and the hydrogen exhaust hole 660, a
reaction region sealant groove 680 is formed for application of sealant for
preventing hydrogen leakage from the reaction region.
Aligning holes 631 , 632, 633, and 634 are formed through the anode
side separator 250 at the same positions and same sizes with the aligning
holes 431 , 432, 433, and 434 of the cathode side separator 260. Stacking of
the unit cells 200 may be eased due to the aligning holes 431 , 432, 631 , and
632. In the above description, exterior features of and reaction gas/coolant
communication through the separators 250 and 260 according to an
embodiment of the present invention were main topics.
Hereinafter, materials, interior structure, and manufacturing method
of separators 250 and 260 are described in detail.
FIG. 7 is a sectional view of FIG. 4 along a line Vll-Vll, and FIG. 8 is
a sectional view of FIG. 6 along a line VIII-VIII.
According to an embodiment of the present invention, graphite foil 700 and 800 is used as a material for the separators 250 and 260. Manufacturing of a graphite foil is usually accompanied by a pressing
step, and a graphite foil pressed with a high pressure has an internal lamellar
structure. Therefore, according to an embodiment of the present invention, the
material for the separators 250 and 260 may be called a lamellar structure
graphite foil. The enlarged portion A of FIG. 7 and portion B of FIG. 8 may be
referred to for the lamellar structure of the graphite foils 700 and 800 used
for materials of the separators 250 and 260 according to an embodiment of
the present invention, For a usual graphite foil, heat conductivity thereof is more than 250
W/mK in the stacking direction of unit cells. Therefore, it may contribute to an
enhancement of heat exhaust performance of a fuel cell stack and also to
uniformity in temperature distribution of a fuel cell stack. In a separator of a graphite/carbon composite material according to
the prior art, a resin such as thermosetting resin or thermoplastic resin is
included in the separator, for preventing leakage of reaction gas or for easier
molding of graphite material. However, according to the separators 250 and 260 according to an
embodiment of the present invention, the graphite foil used for the
separators is substantially free from such resin. Lamellar structure graphite
foils are currently mass produced, and if the resin of the prior art does not
need to be contained, mass productivity of the graphite foils further increases. Therefore, if such lamellar structure graphite foil is used for manufacturing a
separator, it contributes to a reduction of production cost of a separator.
Furthermore, the separator of graphite material containing resin
according to the prior art is rarely used for a fuel cell operating at a
temperature higher than about 100°C because heat deflection temperature of most of the resins is below about 100 °C .
Therefore, in the case that a graphite foil free from the resin may be
used for a separator, an operating temperature range of a fuel cell may be
broadened, and durability of the fuel cell may be enhanced against the case
that the fuel cell is overheated more than 100°C . In fact, separators 250 and 260 may have high formability for, e.g.,
forming flow fields on the separators 250 and 260, without containing resin
therein. Furthermore, leakage prevention of reaction gases and a
hydrophobic effect may be preserved,, while enhancing the durability. A method for manufacturing a stable and high-performance separator using a
graphite foil without containing resin is described later.
A separator of a fuel cell should maintain uniform pressure without
deformation during stacking of a fuel cell stack, and it should provide
sufficient electric conductivity.
Therefore, it is preferable that the graphite foil used as a material for
the separators 260 and 250 of an embodiment of the present invention
shows a bulk density higher than 1.5g/cm3. As an experimental result, in the
case that the bulk density of the graphite foil is lower than 1 .5g/cm3, reaction
gas leakage or a contact resistance increase has been found to possibly
occur due to excessive deformation of the separator when stacked in the fuel
cell stack. In addition, an excessively high bulk density causes an increase of
production cost of a graphite foil, i.e., production cost of a separator.
Therefore, graphite foil used for separators 250 and 260 of an embodiment of the present invention may have a bulk density less than 2.0g/cm3.
In the case that a separator is excessively thin, performance and
durability of a fuel cell stack may be deteriorated due to an increase of gas
permeability of the separator. Considering such a point, it is preferable that
thicknesses D1 and D2 of graphite foils used for the separators 250 and 260
according to an embodiment of the present invention are greater than 0.5mm.
A minimum depth for the flow field channels is usually about 0.2mm.
Therefore, in the case that the thickness of a graphite foil is less than 0.5mm, the thickness d2 of the flow field channels becomes less than 0.3mm. In this
case, it has been found that gas permeability of the graphite foils 700 and
800 becomes excessively high.
Therefore, by forming the separator of graphite foil at a thickness of
at least 0.5mm, enhancement of durability and performance is expected,
guaranteeing such minimum thickness.
However, if the separator becomes excessively thick, production cost
increases without any increase in performance and durability. As an
experimental result, it has been found that the thickness of the graphite foil
used for the separator according to an embodiment of the present invention does not need to be more than 3mm.
Since a normal operating temperature of a polymer electrolyte
membrane fuel cell is less than 100°C and about 80 °C , efficient and steady exhaust of reaction products, i.e., heat and water, is very important. For such purpose, hydrophobic layers 710 and 810 are formed by
impregnation on interior surfaces of the flow field channels 410 and 610 of
the separators 260 and 250 according to an embodiment of the present
invention. The hydrophobic layers formed on the flow field channels 410 and
610 also contribute to efficient supplying of reaction gases to electrodes
through the fluid diffusion layers 225.
As shown in FIGs. 7 and 8, the hydrophobic layers 710 and 810 are
not formed on the surfaces of the ribs 420 and 620. Therefore, contact
resistance between the fluid diffusion layers 225 and the separators 260 and 250 does not increase because of the hydrophobic layers 710 and 810.
For conventional hydrophobic treatment according to the prior art, a
hydrophobic layer is simply coated on a surface of a workpiece. In this case,
the coated hydrophobic layer may be easily scraped or removed. However, according to hydrophobic layers 710 and 810 of an
embodiment of the present invention, interior sides of the flow field channels
410 and 610 are firstly modified to a roughness of several decades of
micrometers (μm), and then the hydrophobic layers 710 and 810 are formed
by impregnation on the roughened surface. Therefore, since hydrophobic
layers 710 and 810 are formed on the roughened surface, cohesion strength
hydrophobic layers 710 and 810 to the interior surface of the flow field channels 410 and 610 is enhanced and thereby durability of the hydrophobic
layers 710 and 810 is enhanced.
Thickness of the hydrophobic layers 710 and 810 formed by
impregnation into the flow field channels preferably lies in a range of 30μm to
100μm. The thickness of the hydrophobic layers 710 and 810 is preferably
above 30μm to durably provide the hydrophobic effect of the hydrophobic
layer 710 and 810, considering the reaction gases and the coolant flow
under the conjoining force of the fuel cell stack. To the contrary, in the case
that the hydrophobic layers 710 and 810 are thicker than 100μm, the
hydrophobic solution used for the hydrophobic layer is excessively
impregnated into the flow field channels 410 and 610. In this case, dividing of
lamellas may occur due to, e.g., bubbles formed at the lamellar structure graphite foil, when heat treatment for hydrophobic effect (for example, heat
treatment at 330 °C ).
As has already been described with reference to FIGs. 4 to 6, sealant
grooves 481-486, 681-686, 480, and 680 are formed around the manifolds
471 -476 and 671-676 and the area contacting the fluid diffusion layers.
As shown in FIGs. 7 and 8, sealing members 790 and 890 are
applied to the sealant grooves of the separators 260 and 250, and become
integral with the separators 260 and 250. FIGs. 7 and 8 illustrate that sealing
members 790 and 890 are applied only to specific portions, however, the sealing member 790 and 890 are actually applied to each of the sealant
grooves 480-486, 580-586, and 680-686 of the separators 260 and 250. A
rubber liquid of, e.g., silicon series, fluorine series, and olefin series may be
used as the sealing members 790 and 890.
Since the sealing member is applied to the separators 260 and 250
on the sealant groove and becomes integral therewith, the assembly process
of a fuel cell stack may be simplified.
Hereinafter, an embodiment of the present invention is described in
detail regarding a method for manufacturing a separator made of a lamellar
structure graphite foil and having a hydrophobic layer formed by
impregnation on its flow field channels.
FIG. 9 is a flowchart showing a method for manufacturing a separator
for a fuel cell according to an embodiment of the present invention.
As shown in FIG. 9, according to a method for manufacturing a separator for a fuel cell according to an embodiment of the present invention,
a graphite foil of a predetermined thickness and bulk density is firstly
prepared at step S910. Then at step S920, a mask pattern is formed on the prepared
graphite foil corresponding to manifolds, sealant grooves, and flow field
channels.
Then at step S930, the manifolds, the sealant grooves, and the flow
field channels are formed on the graphite foil by selectively dry-etching the graphite foil formed with the mask pattern thereon. Subsequently at step S940, a hydrophobic layer is formed on each
interior side of the flow field channels by impregnation.
Finally at step S950, the mask pattern is removed from the graphite
foil having the impregnated hydrophobic layer, and then the graphite foil is cleaned and heat-treated such that a separator is finalized. A monopolar separator is finished by such a process.
For a bipolar separator, flow-field channels etc. (i.e., the manifolds,
sealant grooves, and the flow field channels) are formed by executing the
steps of S920 and S930 with respect to one side of the prepared graphite foil,
and then the steps of S920 and S930 are also executed to the other side of
the graphite foil such that the flow-field channels etc. are also formed to the
other side.
Then, the graphite foil having the flow-field channels etc. on both
sides thereof is processed according to the steps of S940 and S950, and accordingly the bipolar separator is completed.
A manufacturing method for a bipolar separator will be obviously
understood from a description of a manufacturing method for a monopolar
separator. Hereinafter, the above-mentioned steps S910-S950 are described in
further detail, with respect to an exemplary monopolar separator 250.
Firstly at step S910 of preparing the graphite foil, the prepared
graphite foil has a thickness of 1 .0mm, an overall density of 1.78g/cm3, and
dimensions of 10cm x 15cm. Moisture is removed from the prepared graphite foil by drying the foil in a dryer for 5 minutes at 100 °C . The aligning holes 631 ,
632, 633, and 634 are formed at the prepared graphite foil. In this stage, only
the diameters of the aligning holes 631 , 632, 633, and 634 and the distance
therebetween need be paid attention to in order to be formed in accordance with a predetermined specification, since the flow-fields channels etc. are not
yet formed thereon.
The step S920 of forming the mask pattern may be further embodied
in various ways. For example, a mask of a rubber or stainless steel material
with a pattern corresponding to the flow field channels etc. may be attached
to the graphite foil. For another example, a dry film may be used.
In the case that a dry film (for example, BF410) is used, a dry film
(e.g., BF410) of a thickness of 100μm is coated on the graphite foil using a
laminator apparatus. For the laminating process, it is preferable that the upper roller temperature is about 70 °C , the lower roller temperature is about
65 °C, and the rolling speed is about 60mm/sec.
A film mask formed with a pattern for flow-field channels etc. is laid in
contact with the graphite foil, and then the graphite foil with the film mask is
exposed at an exposure machine for about 18-23 seconds with an energy
density of about 20mW/cm2.
In the case of a dry film, it may bulge when it is dipped in a liquid
developer. Therefore, in order for develop a graphite foil coated with a dry
film, it is preferable that a spray nozzle moves while spraying a liquid
developer (e.g., 1 -2% solution of Na2C03) in a spray-type developing machine.
The developing conditions of the spray-type developing machine is preferably set to be the temperature of the liquid developer being about 25 °C ,
the spray pressure being about 2.7Kg/cm2, and the nozzle moving speed
being about 80mm/sec. When developed as such, it is preferably baked in
an oven for about 5 minutes at about 100 °C .
The step S920 of forming a mask pattern includes a step of attaching
the mask on the graphite foil. For such a purpose, the aligning holes 631 ,
632, 633, and 634 and aligning bars are used. Attaching the mask on the
graphite foil using the aligning holes 631 , 632, 633, and 634 is hereinafter
described in further detail.
As shown in FIG. 10, a pair of larger diameter aligning bars 1021 and
1022 and a pair of smaller diameter aligning bars 1023 and 1024 are formed protruding on a working plate 1 100 on an exposure machine 1000. The
working plate 1 100 is formed as a transparent plate such that an exposure
light generated at a light source 1005 of the exposure machine 1000 may
penetrate therethrough. A prepared mask 1010 is formed with aligning holes 101 1 , 1012,
1013, and 1014 at positions corresponding to the aligning bars 1021 , 1022,
1023, and 1024. In addition, at the step S910 of preparing the graphite foil,
aligning holes 631 , 632, 633, and 634 are formed at the graphite foil at
positions corresponding to the aligning bars 1021 , 1022, 1023, and 1024. Since a thickness of the mask 10 0 is usually less than 0.2mm, and it
suffices that a protruding height h of the aligning bars 1021 , 1022, 1023, and
1024 from the working plate 1 100 is 0.2mm. The larger diameter aligning
bars 1021 and 1022 protrude slightly more than the smaller diameter aligning bars 1023 and 1024. Therefore, a separator may be precisely aligned in the
correct position using the smaller diameter aligning bars 1023 and 1024 after
it is positioned in a rough alignment position using the larger diameter
aligning bars 1021 and 1022.
The mask 1010 is laid on the working plate 1 100 such that the
protruded aligning bars 1021 , 1022, 1023, and 1024 may be inserted into the
aligning holes 101 1 , 1012, 1013, and 1014. In this case, the aligning bars
1021 , 1022, 1023, and 1024 fully penetrate the mask 1010 and protrude
therefrom, since the protruding height h of the aligning bars 1021 , 1022,
1023, and 1024 is greater than the thickness of the mask 1010. Therefore, front and rear sides of the separator may be precisely
aligned by simply disposing the prepared graphite foil such that the aligning
holes 631 , 632, 633, and 634 are inserted by aligning bars 1021 , 1022, 1023,
and 1024. By attaching masks on the graphite foil according to such an
aligning process, front and rear sides of the separator are precisely aligned.
At the step S930 of forming the flow field channels, the graphite foil
processed with the mask pattern process is dry-etched using, e.g., a sand
blast apparatus, such that the depth of the flow field channels may become
about 500 μm. The sand blast condition is preferably set to be the separator moving
speed being about 40mm/minute, the nozzle moving speed being about
20m/minute, the spraying pressure of the nozzle being about 3.0kg/cm2, and
the distance between the separator and the nozzle being about 60mm. For example, SiC may be used as an abrasive such that surface roughness on
the bottom of the flow field channels may become several decades of
micrometers. An ultrasonic etching process, that is, an etching process using an
abrasive, may be performed instead of or together with the sand blast
process. At the step S950 of forming the hydrophobic layer by impregnation,
the graphite foil having the flow-field channels and having the mask pattern
attached thereon is dried in a range of 50 °C to 90 °C after dipping it in a
hydrophobic solution (e.g., a 20% PTFE (polytetrafluoroethylene) solution) for 2 to 4 seconds, or processing by spray coating.
At the step S950 of finishing the separator, the mask pattern is
removed in acetone using an ultrasonic cleaner such that the dry film
attached to the graphite foil is removed, and then the graphite foil is cleaned
and heat-treated to finalize the separator. The process of cleaning and heat-
treating the graphite foil is obvious to a person of ordinary skill in the art. As
for a mask of a rubber or a stainless steel material, it may be removed by
simply dividing it. In the above description of an embodiment of the present invention, a
separator is described to use a graphite foil having a uniform structure.
However, the protection scope of the present invention should not be
understood to be limited thereto, since variations of embodiments may be
possible, such as the case that a stainless steel layer is inserted inside the
graphite foil used for the separator. Hereinafter, a second embodiment of the present invention related to
the case that the graphite foil used for the separator includes a stainless
steel layer therein is described with reference to FIG. 1 1 .
FIG. 11 is a sectional view of FIG. 6 along a line XI-XI according to a
second embodiment of the present invention. As shown in FIG. 1 1 , a lamellar structure graphite foil 1 140 used for a
separator 1 150 according to a second embodiment of the present invention
includes a stainless steel layer 1 160 therein.
Such graphite foil 1 140 including the stainless steel layer 1160 may be easily manufactured e.g., by pressing graphite layers of predetermined thickness to front and rear of the stainless steel layer 1160. The stainless steel layer 1160 may be of, e.g., SUS304 or SUS316, and its thickness t is preferably 0.1mm to 0.3mm. The thickness d3 of the graphite layers formed at front and rear sides of the stainless steel layer
1160 is preferably more than 0.2mm considering the depth of flow-field channels 610, and is preferably less than 3mm considering the production cost. That is, the separator 1150 according to such a second embodiment of the present invention uses the graphite foil 1140 formed with, e.g., the stainless layer 1160 of 0.1 mm thickness at its center and graphite layers of 0.2mm thickness at each of front and rear sides of the stainless layer 1160 (therefore, total thickness D3 of the graphite foil becomes 0.5mm). The flow- field channels 610 are formed by dry-etching one side (e.g., upper side in FIG. 11) of the graphite foil 1140. A method for manufacturing the separator 1150 using the graphite foil 1140 including the stainless steel layer 1160 therein is the same as a method for manufacturing the separators 250 and 260 according to the first embodiment of the present invention that has been described with reference to FIG. 10.
In the process of dry-etching for forming the flow-field channels 610, the graphite layer is etched such that the stainless steel layer 1160 is exposed. As for the process of dry-etching (e.g., the above-described sand blasting etching process), the stainless steel layer 1 160 has a substantially
smaller etch rate than the graphite layers formed to front and rear of the
stainless steel layer 1 160. Therefore, such stainless steel layer 1 160
functions as an etch stop in the process of etching. According to such a feature, the manufacturing process of a
separator becomes easier, and a manufacturing device of lower precision
may be used to produce a separator with equally high performance and
precision.
Although rigidity of the stainless steel layer 1 160 is higher than that of
the graphite layer, the abrasive used in the etching process may easily form a roughness thereon, e.g., to the degree of several decades of micrometers
described in connection with the first embodiment.
In addition, in the process of forming the hydrophobic layer (refer to
the step S940 in FIG. 9), the hydrophobic layer 810 is formed while the
stainless steel layer 1160 is exposed in the flow-field channels 610.
Therefore, as for a finished separator 1 150, the stainless steel layer 1 160
becomes exteriorly exposed interposing the hydrophobic layer 810, since the
hydrophobic layer 810 is formed while the stainless steel layer 1 160 is
exposed in the flow-field channels 610. In the above description, the present invention has been exemplarily
described in connection with a polymer electrolyte fuel cell. However, the
protection scope of the present invention should not be understood to be
limited thereto. To the contrary, the spirit of the present invention may be applied to an arbitrary fuel cell of which a normal operating temperature lies
in a range below a heat deflection temperature of the graphite foil (e.g.,
below 250 °C). As an example, the spirit of the present invention may also be
applied to a DMFC (direct methanol fuel cell). Therefore, in the above description and also in the appended claims,
the terms related to a polymer electrolyte fuel cell should not be understood
to strictly refer to the specific element of the polymer electrolyte fuel cell.
For example, the term fuel gas should be understood in a collective
meaning that covers methanol fuel supplied in the form of liquid as well as
hydrogen in the form of gas. In addition, as for a fuel cell other than a
polymer electrolyte fuel cell, the term MEA should be understood to be
referring to a corresponding element of the fuel cell. As described above, according to an embodiment of the present
invention, lamellar structure graphite foil is used as a material for a separator
for a fuel cell, and hydrophobic layer is formed by impregnation on an interior
wall of flow field channels of the separator.
Therefore, water produced at cathodes may be efficiently exhausted,
and thereby performance of the fuel cell may be enhanced, by, e.g.,
accelerating diffusion of reaction gases to catalyst layers. Accordingly, power
density per unit volume of a fuel cell stack may be enhanced.
In addition, since the hydrophobic layer is formed by impregnation on
an interior wall of flow-field channels of a separator that has been formed by
dry-etching, durability of the hydrophobic layer is enhanced, and consequently, durability and reliability of a fuel cell is enhanced.
Furthermore, since an interior of the graphite foil is substantially free
from resins such as thermosetting or thermoplastic resin and a hydrophobic
layer is prevented from forming on the separator surface contacting an MEA
by a mask pattern, additional processes for reducing contact resistance
between cells are not required.
Furthermore, since such graphite foil exhibits high heat conductivity,
the cooling effect of a fuel cell stack is enhanced and temperature distribution of a fuel cell stack becomes uniform. Furthermore, since the lamellar structure graphite foil used as a
material of a separator may be mass-produced, production cost of a separator and accordingly a fuel cell may be reduced.
Furthermore, since the manufacturing process of a separator may be
simplified and be more adaptive to mass-production, the production cost of a separator and accordingly a fuel cell may be reduced.
While this invention has been described in connection with what is
presently considered to be the most practical and preferred embodiment, it is
to be understood that the invention is not limited to the disclosed
embodiments, but, on the contrary, is intended to cover various modifications
and equivalent arrangements included within the spirit and scope of the
appended claims.
Throughout this specification and the claims that follow, unless
explicitly described to the contrary, the word "comprise" or variations such as "comprises" or "comprising" will be understood to imply the inclusion of stated elements but not the exclusion of any other elements.

Claims

WHAT IS CLAIMED IS: 1. A separator for a fuel cell that is capable of closely contacting either an anode or a cathode of an MEA (membrane electrode assembly) of a fuel cell and interposing a fluid diffusion layer, the separator having a flow field channel for allowing a fluid to flow between the separator and the fluid diffusion layer, characterized in that: the separator comprises a lamellar structure graphite foil; and a hydrophobic layer is formed by impregnation on an interior side of
the flow field channel.
2. The separator for a fuel cell as claimed in claim 1 , wherein the lamellar structure graphite foil comprises a stainless steel layer therewithin.
3. The separator for a fuel cell as claimed in claim 2, wherein the stainless steel layer is exteriorly exposed, interposing the hydrophobic layer.
4. The separator for a fuel cell as claimed in claim 1 , wherein the
graphite foil is substantially free from thermosetting or thermoplastic resin.
5. The separator for a fuel cell as claimed in claim 1 , wherein a bulk
density of the graphite foil lies in the range of 1.5g/cm3 to 2.0g/cm3.
6. The separator for a fuel cell as claimed in one of claims 1 -5, wherein thickness of the graphite foil lies in the range of 0.5mm to 3mm.
7. The separator for a fuel cell as claimed in one of claims 1-5, wherein thickness of the hydrophobic layer lies in the range of 30μm to 100μm.
8. The separator for a fuel cell as claimed in one of claims 1-5, wherein: at least one manifold is formed in the separator; and a sealing member is unified to the separator along each circumference of the at least one manifold and an area for contacting the fluid diffusion layer.
9. The separator for a fuel cell as claimed in claim 8, wherein the sealing member encloses, respectively along a closed curve, each of the at least one manifold and the area for contacting the fluid diffusion layer.
10. A method for manufacturing a fuel cell having a separator for a
fuel cell that is capable of closely contacting either an anode or a cathode of
an MEA (membrane electrode assembly) of a fuel cell and interposing a fluid
diffusion layer, the separator having a flow field channel for allowing a fluid to
flow between the separator and the fluid diffusion layer, the method
comprising: preparing a graphite foil of a predetermined size; forming a mask pattern on the graphite foil corresponding to the flow field channel; forming the flow field channel on the graphite foil by etching the graphite foil formed with the mask pattern thereon; forming a hydrophobic layer on an interior side of the flow field channel by impregnation; and removing the mask pattern from the graphite foil.
11. The method for manufacturing a fuel cell as claimed in claim 10, wherein the forming of a mask pattern on the graphite foil comprises: coating the graphite foil with a dry film resist; exposing the coated graphite foil; and developing the dry film resist on the graphite foil by moving a spray nozzle of a spray-type developing apparatus thereover.
12. The method for manufacturing a fuel cell as claimed in claim 10,
wherein the forming of a mask pattern on the graphite foil comprises
attaching a mask on the graphite foil, the mask being provided with a pattern
corresponding to the flow field channel and being made of rubber or
stainless steel.
13. The method for manufacturing a fuel cell as claimed in claim 10, wherein the forming of the flow field channel on the graphite foil comprises at least one of sandblasting and ultrasonic etching.
14. The method for manufacturing a fuel cell as claimed in one of claims 10-13, wherein the forming a hydrophobic layer on the interior side of the flow field channel by impregnation comprises: forming a hydrophobic layer on the graphite foil attached with the mask pattern and formed with the flow field channel; and drying the graphite foil formed with the hydrophobic layer, in a temperature range of 50°C-90°C.
15. The method for manufacturing a fuel cell as claimed in claim 14, wherein, in the forming of a hydrophobic layer on the graphite foil, a hydrophobic solution is spray coated on a surface of the graphite foil, or the graphite foil is dipped in the hydrophobic solution.
16. The method for manufacturing a fuel cell as claimed in claim 10,
wherein: the flow field channel is formed on each of front and rear sides of the
separator; the mask pattern comprises a front mask pattern and a rear mask
pattern; at least one pair of aligning holes are formed at each of the front and rear mask patterns; at least one aligning hole is formed through the graphite foil corresponding to the aligning holes of the mask patterns; and the aligning holes of the mask patterns and the aligning holes of the graphite foil are aligned by using at least one pair of aligning bars corresponding thereto.
17. The method for manufacturing a fuel cell as claimed in claim 16, wherein the at least one pair of aligning holes and the at least one pair of aligning bars respectively comprise a plurality of pairs thereof, corresponding to different sizes.
18. A fuel cell stack comprising at least one unit cell, wherein the at least one unit cell comprises: an MEA (membrane electrode assembly) comprising a polymer electrolyte membrane, and an anode and a cathode formed on both sides thereof; a pair of fluid diffusion layers contiguously disposed to the anode and the cathode at both sides of the MEA; and a pair of separators for closely contacting the pair of fluid diffusion layers, forming flow field channels on sides thereof facing the fluid diffusion layers so as to form a reaction region, and forming manifold regions peripheral to the reaction region, wherein at least one of the pair of separators comprises a lamellar structure graphite foil, and a hydrophobic layer is formed by impregnation on an interior side of the flow field channels of the at least one of the pair of separators.
19. The fuel cell stack as claimed in claim 18, wherein the lamellar structure graphite foil comprises a stainless steel layer therewithin.
20. The fuel cell stack as claimed in claim 19, wherein the stainless steel layer is exteriorly exposed, interposing the hydrophobic layer.
21. The fuel cell stack as claimed in claim 18, wherein the graphite foil is substantially free from thermosetting or thermoplastic resin.
' 22. The fuel cell stack as claimed in claim 18, wherein a bulk density of the graphite foil lies in the range of 1.5g/cm3 to 2.0g/cm3.
23. The fuel cell stack as claimed in one of claims 18-22, wherein thickness of the graphite foil lies in the range of 0.5mm to 3mm.
24. The fuel cell stack as claimed in one of claims 18-22, wherein thickness of the hydrophobic layer lies in the range of 30μm to 100μm.
25. The fuel cell stack as claimed in one of claims 18-22, wherein a sealing member is unified to the separator along each circumference of the manifold and the reaction region.
PCT/KR2004/001950 2004-03-10 2004-08-03 Separator for fuel cell, manufacturing method thereof, and fuel cell having such a separator WO2005086267A1 (en)

Priority Applications (5)

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JP2007502697A JP4971972B2 (en) 2004-03-10 2004-08-03 Separator for fuel cell, method for producing the same, and fuel cell having the separator
US10/598,729 US8865372B2 (en) 2004-03-10 2004-08-03 Separator for fuel cell, manufacturing method thereof, and fuel cell having such a separator
EP04748506.5A EP1723688B1 (en) 2004-03-10 2004-08-03 Separator for fuel cell, manufacturing method thereof, and fuel cell having such a separator
US14/487,212 US10109865B2 (en) 2004-03-10 2014-09-16 Separator for fuel cell, manufacturing method thereof, and fuel cell having such a separator
US16/139,429 US10998557B2 (en) 2004-03-10 2018-09-24 Separator for fuel cell, manufacturing method thereof, and fuel cell having such a separator

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KR1020040016162A KR100545992B1 (en) 2004-03-10 2004-03-10 Separator and manufacturing method for fuel cell, and fuel cell stack comprising such separator

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US14/487,212 Division US10109865B2 (en) 2004-03-10 2014-09-16 Separator for fuel cell, manufacturing method thereof, and fuel cell having such a separator

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US20150004516A1 (en) 2015-01-01
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US8865372B2 (en) 2014-10-21
KR20050090876A (en) 2005-09-14
JP4971972B2 (en) 2012-07-11
CN100490232C (en) 2009-05-20
US10109865B2 (en) 2018-10-23
CN101325260B (en) 2010-10-06
CN101325260A (en) 2008-12-17
EP1723688B1 (en) 2013-12-25
EP1723688A4 (en) 2009-07-29
US20190027763A1 (en) 2019-01-24
CN1926704A (en) 2007-03-07
EP1723688A1 (en) 2006-11-22
US20070190392A1 (en) 2007-08-16
JP2007528112A (en) 2007-10-04

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